JP7476281B2 - Methods for spraying water-borne pesticide formulations - Google Patents

Description

The present invention relates to a water-floating pesticide formulation that exhibits good floatability and diffusibility when applied to paddy fields, particularly when applied by flooding in shallow water conditions, and that maintains its performance even after long-term storage, and has excellent diffusibility and preservability.

Known formulations of pesticides for paddy rice include granules, powders, wettable powders, tablets, packs, flowables, water-soluble agents, liquids, and emulsions. In recent years, to reduce the labor required for spraying pesticides, pesticide formulations that can be sprayed simply by pouring them into the paddy field from the ridges (jumbo formulations, flowable formulations for flood-spraying of undiluted solutions, etc.) have been developed and are in use. However, because such pesticide formulations spray the pesticide active ingredient locally at a high concentration, it takes a long time for the pesticide active ingredient to diffuse evenly into the water on the paddy field surface, and there are problems with the pesticide damage to paddy rice or ineffectiveness due to the localized uneven distribution of the pesticide active ingredient. To solve these problems, it is required that the pesticide active ingredient disperse quickly and evenly after the pesticide formulation is poured into a flooded paddy field.

Various methods have been proposed to meet the above requirements, for example, see the following patent documents:

International Publication No. 2016-129466 (Patent Document 1) describes a method for producing a granular pesticide composition, which contains an active ingredient in pesticides, a surfactant, hollow bodies, and a solid carrier, has a particle size distribution in which 80% or more of the particles have a particle size of 3 mm or more, has the property of floating on the water surface, and disintegrates on the water surface within 30 minutes, and includes the steps of: (a) kneading a mixture containing a portion of the active ingredient in pesticides, a portion of the surfactant, a portion of the hollow bodies, a portion of the solid carrier, and water; (b) granulating the kneaded mixture obtained in step (a) using an extrusion granulator; and (c) granulating the mixture obtained in step (b). A method for producing a granular pesticide composition is proposed, which includes the steps of: (a) drying the granules obtained in step (c) to obtain granules; (b) crushing the granules obtained in step (c); (c) kneading a mixture containing the crushed material obtained in step (d), the remaining pesticide active ingredient, the remaining surfactant, the remaining hollow bodies, the remaining solid carrier, and water; (d) granulating the kneaded material obtained in step (e) by discharging it through a screen with a hole diameter of 3 mm or more using an extrusion granulator; and (e) drying the granules obtained in step (f).

International Publication WO 2016-114200 (Patent Document 2) proposes a water-floating large granular pesticide composition containing a water-containing raw material, which has a particle size distribution in which 80% or more of the particles are 3 mm or larger, has the property of floating on the water surface, and disintegrates on the water surface within 30 minutes, and a method for producing the same, characterized in that the composition is obtained by extruding and granulating a water-containing mixture containing one or more pesticide active ingredients, a poorly water-soluble polysaccharide that has water retention and is inhibited from swelling in water, a surfactant, a hollow body, a solid carrier, and water, and then drying to remove the water.

International Publication WO 2015-159906 (Patent Document 3) proposes a water-floating large granular pesticide formulation that contains a pesticide active ingredient, a floating carrier, and 0.3 to 3 mass% water, has a particle size distribution in which 80% or more of particles are 3 mm or larger in diameter, has the property of floating on the water surface, and disintegrates on the water surface within 30 minutes of being dropped into water, and proposes a water-floating large granular pesticide formulation and a method for producing the same, in which the value X defined by formula (1) is in the range of 0.5 to 2 for a total of n raw materials, which are all of the pesticide active ingredients and auxiliary ingredients (excluding water) that make up the pesticide formulation.

JP 2012-116788 A (Patent Document 4) proposes a water-floating pesticide formulation that uses in combination (a) a fungicidal active ingredient and/or an insecticidal active ingredient, (b) a specific polyoxyethylene alkyl ether, (c) a specific sodium alkylnaphthalene sulfonate, (d) isoparaffin with a distillation point of 277°C to 353°C, and (e) a water-floating hollow body.

JP 2012-116787 A (Patent Document 5) proposes a water-floating herbicidal formulation that uses in combination (a) a herbicidal active ingredient, (b) a specific polyoxyethylene alkyl ether represented by general formula (1), (c) a specific sodium alkylnaphthalenesulfonate, (d) isoparaffin with a distillation point of 277°C to 353°C, and (e) a water-floating hollow body.

International Publication WO 2005-29956 (Patent Document 6) proposes a non-disintegrating pesticide granule that contains an acidic pesticide active ingredient, a cationic surfactant, and a basic substance and does not disintegrate in water within 30 minutes, a surfactant, and a floating component, a particle size distribution in which the mass ratio of particles with a diameter of 3 mm or more is 80 mass% or more, and the formulation floats on the water surface immediately after being dropped on the water surface, but disintegrates on the water surface within 30 minutes.

JP 2002-179507 A (Patent Document 7) proposes a uniformly dispersible granular pesticide formulation that contains an active ingredient in a pesticide, has a particle size distribution in which 80% of the particles are 3 mm or larger, has the property of floating on the water surface, and disintegrates on the water surface within 30 minutes, and also proposes a uniformly dispersible granular pesticide formulation that is dispersed over an area of 5% to 50% of the total paddy field area at a distance of 1 m or more from the ridge of a flooded paddy field.

JP 2002-128605 A (Patent Document 8) proposes an agrochemical formulation for application to water surfaces, which is characterized by the use of an agrochemical active ingredient, a floating hollow body, and a specific polyoxyalkylene alkyl ether phosphate ester or its salt.

JP 2000-351701 A (Patent Document 9) proposes a water-floating pesticide solid formulation that contains one or more water surface spreaders consisting of C2-C4 alkylene oxide adducts of C4-C10 alkyl alcohols and their derivatives, and an active pesticide ingredient.

JP 2001-114603 A (Patent Document 10) proposes a solid pesticide composition that contains a pesticide active ingredient and one or more water-soluble substances selected from inorganic salts, organic salts, organic acids, sugars, and urea, the particle size of which is 1/10 to 1/2 the minor axis of the solid pesticide composition.

JP 2000-319103 A (Patent Document 11) proposes a water-floating granular pesticide formulation, which contains an active pesticide ingredient, a surfactant, a solid carrier, a water-floating agent, and water, and in which the water content after molding is 0.3 to 6 parts per 100 parts by weight of the water-floating granular pesticide formulation, and a method for producing the same.

JP 2000-319102 A (Patent Document 12) proposes a water-drop type pesticide formulation in which a water-floating granular pesticide containing an active pesticide ingredient, a surfactant, a solid carrier, and a water-floating agent is packaged in a water-soluble film bag that has a dissolution time of 1/5 or less of the disintegration time of the water-floating granular pesticide.

JP 2000-302602 A (Patent Document 13) proposes a water-floating granular pesticide formulation that contains an active pesticide ingredient, a surfactant, a solid carrier, a water-floating agent, water, and other auxiliary agents as necessary, and is characterized in that (1) each particle weighs 0.03 g to 0.3 g, each particle has a density of 0.4 to less than 1.0, (2) each particle has a ratio of minor axis to major axis of 1 to 3, and has an external shape composed of curved surfaces, and (3) the time it takes for the particles floating on the water surface to disintegrate and disperse is within 30 minutes, as well as a method for producing the same.

JP-A-11-310503 (Patent Document 14) proposes an agrichemical pack for throwing into paddy fields, which floats and spreads on the water surface, contains no foaming agent, and is packaged in a water-soluble film with holes to prevent solidification over time.

Although the diffusibility is improved in all the prior arts, this is the diffusibility under the condition that the water depth (water volume) is guaranteed. On the other hand, there are also fields that can only maintain a shallow water depth (less than 3 cm) due to reasons such as leakage and natural water reduction. Under such conditions, the distance between the water surface and the soil is close, so if the buoyancy is small, the formulation may run aground or be buried in the soil when sprayed, and a large amount of it may settle at the spraying point, which may cause damage to the phytosanitary agent at the spraying point or cause insufficient effectiveness due to poor diffusion. In addition, shallow water depth is synonymous with a small amount of water, and in a formulation in which the active ingredient diffuses through the water surface or underwater, the range in which it can diffuse is limited compared to a normal water depth (about 5 cm). In such fields, better floatation and diffusibility are required, and the prior art was not sufficient. Furthermore, the prior art does not mention maintaining these performances even after long-term storage, and a formulation with excellent floatation, diffusibility, and storage stability is required.

International Publication No. 2016/129466 International Publication No. 2016/114200 International Publication No. 2015/159906 JP 2012-116788 A JP 2012-116787 A International Publication No. 2005/29956 JP 2002-179507 A JP 2002-128605 A JP 2000-351701 A JP 2001-114603 A JP 2000-319103 A JP 2000-319102 A JP 2000-302602 A Japanese Patent Application Laid-Open No. 11-310503

In view of the above-mentioned conventional shortcomings, the present invention aims to provide a water-floating pesticide formulation with excellent diffusibility in flooding treatment under shallow water conditions, more specifically, a water-floating pesticide formulation that has excellent buoyancy and diffuses on the water surface without settling below the water surface when sprayed, and that exhibits excellent diffusibility in water even after disintegration in water over time, and that maintains its performance even after long-term storage.

The present inventors have conducted extensive research to solve the above problems, and have found that the object can be achieved by a water-floating pesticide formulation that is characterized in that it comprises a pesticide active ingredient, a floating carrier, and at least one anionic surfactant selected from sodium alkylnaphthalenesulfonate and sodium dialkylsuccinatesulfonate, the major axis/minor axis ratio of the base of the particles being 1.1 to 1.4, 80% by weight or more of the particle size being in the range of 2.80 mm to 1.70 mm, and the number of particles per gram being 50 to 150.
They also found that a water-floating pesticide formulation containing a polyoxyalkylene alkyl ether phosphate salt as an active ingredient, a floating carrier, and an anionic surfactant together with a water-soluble alkylene glycol such as propylene glycol, and further containing one or more anionic surfactants selected from sodium alkylnaphthalenesulfonate and sodium dialkylsuccinatesulfonate, has excellent diffusibility.
It has been found that the diffusibility of the water-floating pesticide formulation is particularly excellent when the content of the water-floating pesticide is 0% by weight or more and the number of particles per gram is 50 to 200.
Furthermore, the inventors have found that it is more preferable that the water-floating pesticide formulation has a particle size of 90% by weight or more in the range of 2.80 mm to 1.70 mm, the floating carrier is a shirasu balloon having an average particle size of 90 to 120 μm, and further contains, as an anionic surfactant, one or more selected from alkylnaphthalenesulfonate formaldehyde condensate Na, naphthalenesulfonate formaldehyde condensate Na, and partially desulfonated sodium ligninsulfonate (sodium ligninsulfonate in the case where a polyoxyalkylene alkyl ether phosphate salt and a water-soluble alkylene glycol are contained), and further contains, as a binder, sodium carboxymethylcellulose (sodium carboxymethylcellulose and polyvinyl alcohol in the case where a polyoxyalkylene alkyl ether phosphate salt and a water-soluble alkylene glycol are contained), and thus have completed the present invention.

[式中、Ｒは、炭素数８～１０の直鎖状または分岐鎖状のアルキル基を示し、Ａは炭素数
２～４のアルキレン基を示し、ｎは１～２０の整数を示し、ｐおよびｑは、ｐ＋ｑ＝３かつｐ＝１または２である整数を示し、Ｍは水素原子、アルカリ金属原子、アンモニウム基、または有機アンモニウム基を示す。なお、Ｒ、Ａ、Ｍがそれぞれ複数ある場合は、それらの種類は同じでも異なってもよい。]
［７］水溶性アルキレングリコールがプロピレングリコールである［６］に記載の水面浮遊性農薬製剤。
［８］以下の特徴を有する、［６］または［７］に記載の水面浮遊性農薬製剤：
ｄ）粒の底面の長径/短径比が１．１～１．６、
ｅ）粒度が２．８０ｍｍ～１．７０ｍｍの範囲に８０重量％以上、および
ｆ）１gあたりの粒数が５０～２００。
［９］ｅ）前記粒度が２．８０ｍｍ～１．７０ｍｍの範囲に９０重量％以上であることを特徴とする［８］に記載の水面浮遊性農薬製剤。
［１０］前記浮遊性担体としての中空体が平均粒子径９０～１２０μｍのシラスバルーンであることを特徴とする［６］～［９］のいずれかに記載の水面浮遊性農薬製剤。
［１１］更に、陰イオン性界面活性剤としてアルキルナフタレンスルホン酸ホルムアルデヒド縮合物Ｎａ、ナフタレンスルホン酸ホルムアルデヒド縮合物Ｎａ、およびリグニンスルホン酸Ｎａから選ばれる１種以上を含有することを特徴とする［６］～［１０］のいずれかに記載の水面浮遊性農薬製剤。
［１２］更に、結合剤としてカルボキシメチルセルロースＮａおよびポリビニルアルコールから選ばれる１種以上を含有することを特徴とする［６］～［１１］のいずれかに記載の水面浮遊性農薬製剤。 That is, the gist of the present invention is as follows.
[1] A water-floating pesticide formulation comprising: a) a pesticide active ingredient; b) a hollow body as a floating carrier; and c) one or more anionic surfactants selected from sodium alkylnaphthalenesulfonate and sodium dialkylsuccinatesulfonate, the water-floating pesticide formulation having the following characteristics:
d) The ratio of the major axis to the minor axis of the base of the grain is 1.1 to 1.4;
e) the particle size is in the range of 2.80 mm to 1.70 mm at least 80% by weight, and f) the number of particles per gram is 50 to 150.
[2] e) The water-floating pesticide formulation according to [1], characterized in that 90% by weight or more of the particle size is in the range of 2.80 mm to 1.70 mm.
[3] The water-floating pesticide formulation according to either [1] or [2], characterized in that the hollow bodies as the floating carriers are shirasu balloons having an average particle size of 90 to 120 μm.
[4] The water-floating pesticide formulation according to any one of [1] to [3], further comprising one or more anionic surfactants selected from the group consisting of alkylnaphthalenesulfonic acid formaldehyde condensates Na, naphthalenesulfonic acid formaldehyde condensates Na, and partially desulfonated lignosulfonic acid Na.
[5] The water-floating pesticide formulation according to any one of [1] to [4], further comprising carboxymethylcellulose Na as a binder.
[6] A water-floating pesticide formulation comprising: a) a pesticide active ingredient; b) a hollow body as a floating carrier; and c) a polyoxyalkylene alkyl ether phosphate salt represented by the following general formula (I) and a water-soluble alkylene glycol, and one or more anionic surfactants selected from sodium alkylnaphthalenesulfonate and sodium dialkylsuccinatesulfonate:

[In the formula, R represents a linear or branched alkyl group having 8 to 10 carbon atoms, A represents an alkylene group having 2 to 4 carbon atoms, n represents an integer from 1 to 20, p and q represent integers such that p+q=3 and p=1 or 2, and M represents a hydrogen atom, an alkali metal atom, an ammonium group, or an organic ammonium group. When there are multiple R, A, and M, the types of these may be the same or different.]
[7] The water-floating pesticide formulation according to [6], wherein the water-soluble alkylene glycol is propylene glycol.
[8] The water-floating pesticide formulation according to [6] or [7], having the following characteristics:
d) The ratio of the major axis to the minor axis of the base of the grain is 1.1 to 1.6;
e) at least 80% by weight of the particle size is in the range of 2.80 mm to 1.70 mm, and f) the number of particles per gram is between 50 and 200.
[9] e) The water-floating pesticide formulation according to [8], characterized in that 90% by weight or more of the particle size is in the range of 2.80 mm to 1.70 mm.
[10] The water-floating pesticide formulation according to any one of [6] to [9], characterized in that the hollow bodies as the floating carriers are shirasu balloons having an average particle size of 90 to 120 μm.
[11] The water-floating pesticide formulation according to any one of [6] to [10], further comprising one or more anionic surfactants selected from the group consisting of alkylnaphthalenesulfonic acid formaldehyde condensates, naphthalenesulfonic acid formaldehyde condensates, and ligninsulfonic acid sodium.
[12] The water-floating pesticide formulation according to any one of [6] to [11], further comprising one or more binders selected from carboxymethylcellulose Na and polyvinyl alcohol.

The water-floating pesticide formulation of the present invention has good floatability and diffusibility, and therefore, even in flooded paddy fields with shallow water conditions of less than 3 cm, the formulation itself has excellent water surface movement and diffusibility after the formulation disintegrates, and can maintain its performance even after long-term storage. Therefore, spraying does not necessarily require a spraying machine such as a powered sprayer or a spraying tool such as a granulator, and manual spraying is also possible. In addition, since the formulation spreads even when sprayed from one side of the ridge, there are no limitations on the scene of use. Furthermore, since quality deterioration is suppressed even after long-term storage, it can be stored in advance as a reserve. Therefore, the water-floating pesticide formulation of the present invention is a labor-saving formulation that reduces the physical, time, and economic burden on the applicator.

The water-floating pesticide formulation of the present invention is described in more detail below.

<A. Compositional Components>
The pesticide active ingredient that can be used in the present invention may be any ingredient that is applicable to paddy rice. Examples of such pesticide active ingredients include the following:

Insecticidally active ingredients
For example, as an insecticidal active ingredient, there may be mentioned organophosphate (MEP, diazinon, etc.), carbamate (BPMC, carbosulfan, etc.), pyrethroid (cycloprothrin, etc.), nereistoxin (thiocyclam, etc.), neonicotinoid (imidacloprid, thiamethoxam, clothianidin, dinotefuran, etc.), diamide (flubendiamide, chlorantraniliprole, cyantraniliprole, etc.), phenylpyrazole (fipronil, ethiprole, etc.), spinosyn (spinosad, spinetoram, etc.) insecticides, insect growth regulators (tebufenozide, chromafenozide, methoxyfenozide, buprofezin, etc.), other synthetic insecticides (pymetrozine, triflumezopyrim, etc.), biological pesticides, etc.

<Antibacterial active ingredient>
Examples of fungicidal active ingredients include inorganic copper, organic copper, inorganic sulfur, organic sulfur, organophosphorus (IBP, etc.), melanin biosynthesis inhibitors (pyroquilon, tricyclazole, carpropamid, diclocymet, fenoxanil, etc.), benzimidazoles (benomyl, thiophanate methyl, diethofencarb, etc.), amides (mepronil, flutolanil, furametpyr, penflufen, fluxapyroxad, thifluzamide, thiadinil, isotianil, etc.), sterol biosynthesis inhibitors (pefurazoate, ipconazole, simeconazole, etc.), strobilurins (azoxystrobin, metominostrobin, orysastrobin, etc.), antibiotic fungicides (kasugamycin, validamycin, etc.), other synthetic fungicides, biological pesticides, etc.

Herbicidal active ingredient
Examples of herbicidal active ingredients include phenoxy acids (MCPA thioethyl, MCPB ethyl, etc.), carbamates, acid amides (thenylchlor, butachlor, bromobutide, etc.), acetanilides, ureas, sulfonylureas (bensulfuron methyl, propyrisulfuron, etc.), benzofuranyl alkylsulfonic acids (benfuresate, etc.), pyrimidyloxybenzoic acids (penoxsulam, etc.), triazines (simetryn, etc.), diazines, diazoles (pyrazolate, benzofenap, etc.), bipyridyliums, dinitroanilines, aromatic carboxylic acids, imidazolinols, etc. Examples of herbicides include arylsulfates, fatty acids, organophosphates, amino acids, tetrazolinones (such as fentrazamide), diphenyl ethers (such as bifenox), oxazolidinediones (such as pentoxazone), nitriles, phenylphthalimides, cineoles, indanediones, benzofurans, triazolopyrimidines, oxazinones (such as oxaziclomefone), aryltriazolinones, isourazoles, pyrimidinylthiophthalides, triazolinones (such as ipfencarbazone), triketones (such as tefuryltrione, mesotrione, benzobicyclon), and inorganic herbicides.

Plant growth regulators
Examples of plant growth regulators include ethylene-based, auxin-based, cytokinin-based, and gibberellin-based regulators.

The specific pesticide active ingredients contained therein are described, for example, in "Pesticide Handbook 2016 Edition" (published by the Japan Plant Protection Association), "SHIBUYA INDEX 13th Edition" (published by the SHIBUYA INDEX Research Group), and "The Pesticide Manual Sixteenth Edition" (published by the British Crop Protection Council).

In addition, the pesticide active ingredient used in the present invention may be any other pesticide active ingredient that is known or will be developed in the future, as long as it achieves the same purpose as the present invention and is applicable as a water-floating pesticide formulation.

The above pesticide active ingredients may be used alone or in combination of two or more. The amount added is usually 0.01 to 60% by weight, preferably 0.05 to 50% by weight, in the formulation.

Floating Carrier
The floating carrier used in the present invention has a hollow body, which generates buoyancy, and therefore can float on the water surface, and also functions as a disintegration aid by generating minute gaps in the formulation, contributing to diffusibility from the viewpoint of floating and disintegrating properties. Examples of floating carriers include those having hollow bodies such as shirasu balloons, fly ash balloons, ceramic balloons, and synthetic resin hollow bodies. In addition, since the formulation hardness tends to become brittle if the average particle size of these components is too large, those having an average particle size of 200 μm or less are preferred.

Considering the balance between buoyancy, disintegration, and formulation hardness, Shirasu balloons with an average particle size of 90 to 120 μm are particularly preferred.

The amount of the buoyant carrier usable in the present invention to be added may be sufficient to make the formulation float on the water surface, and is usually 2.0 to 80% by weight, preferably 5.0 to 70% by weight. One or more of the above types may be used.

Sodium alkylnaphthalenesulfonate and sodium dialkylsuccinatesulfonate (anionic surfactants)
The sodium alkylnaphthalenesulfonate and sodium dialkylsuccinatesulfonate used in the present invention are anionic surfactants with a good balance between wettability and dispersibility, and thus the inclusion of one or more of these anionic surfactants contributes to the disintegration and dispersibility of the formulation, and this function is maintained even after long-term storage. In addition, due to their wetting ability, less water is required for granulation during production, and the load during granulation is also reduced.

The amount of sodium alkylnaphthalenesulfonate and sodium dialkylsuccinatesulfonate that can be used in the present invention is 0.5 to 30% by weight, preferably 1 to 20% by weight, in the formulation.

{Alkylnaphthalenesulfonic acid formaldehyde condensate Na, naphthalenesulfonic acid formaldehyde condensate Na, partially desulfonated lignosulfonate Na, and lignosulfonate Na} (additional anionic surfactants)
The water-floating pesticide formulation of the present invention further contains one or more selected from the group consisting of sodium alkylnaphthalenesulfonate formaldehyde condensates, sodium naphthalenesulfonate formaldehyde condensates, and sodium partially desulfonated ligninsulfonates, thereby enhancing the diffusibility and storage stability functions.

All of these ingredients are polymeric sulfonic acid surfactants with molecular weights ranging from several thousand to several tens of thousands. When used in combination with sodium alkylnaphthalenesulfonate and sodium dialkylsuccinatesulfonate, their dispersibility is enhanced, and this effect is maintained even after long-term storage.

In addition, when the polyoxyalkylene alkyl ether phosphate ester salt and water-soluble alkylene glycol described below are contained, the diffusibility and storage stability functions are enhanced by adding one or more selected from sodium alkylnaphthalenesulfonate formaldehyde condensate, sodium naphthalenesulfonate formaldehyde condensate, and sodium ligninsulfonate.

The amount of the alkylnaphthalenesulfonate formaldehyde condensate Na, naphthalenesulfonate formaldehyde condensate Na, partially desulfonated lignosulfonate Na, and lignosulfonate Na that can be used in the present invention is 0.5 to 30% by weight, preferably 1 to 20% by weight, in the formulation.

[式中、Ｒは、炭素数８～１０の直鎖状または分岐鎖状のアルキル基を示し、Ａは炭素数
２～４のアルキレン基を示し、ｎは１～２０の整数を示し、ｐおよびｑは、ｐ＋ｑ＝３かつｐ＝１または２である整数を示し、Ｍは水素原子、アルカリ金属原子、アンモニウム基、または有機アンモニウム基を示す。なお、Ｒ、Ａ、Ｍがそれぞれ複数ある場合は、それらの種類は同じでも異なってもよい。]
で表されるポリオキシアルキレンアルキルエーテルリン酸エステル塩は、すぐれた拡展力、湿潤性、分散性および水と接触することでゲル化する能力を有する。製剤が水に接触することで該成分が農薬活性成分あるいは浮遊性担体を取り込んだ形でゲル化することで、浮遊性担体により浮力を強化された状態で農薬活性成分をより遠くまで拡散させることが可能となる。また、ゲルが水に溶解する際、農薬活性成分の周囲には該成分が高濃度で存在するため、農薬活性成分に該成分が効率的に吸着し、ゲル状態解除後もさらに遠くまで農薬活性成分が拡散する。また、ゲル化能力は劣化することがないため、製剤への拡展力、分散力の付与効果および浮遊補助は長期保管後も継続される。 Polyoxyalkylene alkyl ether phosphate ester salt (anionic surfactant)
The compound represented by the following general formula (I) is used in the present invention.

[In the formula, R represents a linear or branched alkyl group having 8 to 10 carbon atoms, A represents an alkylene group having 2 to 4 carbon atoms, n represents an integer from 1 to 20, p and q represent integers such that p+q=3 and p=1 or 2, and M represents a hydrogen atom, an alkali metal atom, an ammonium group, or an organic ammonium group. When there are multiple R, A, and M, the types of these may be the same or different.]
The polyoxyalkylene alkyl ether phosphate salt represented by the formula (I) has excellent spreading power, wettability, dispersibility, and the ability to gel when it comes into contact with water. When the formulation comes into contact with water, the component gels in a form incorporating the pesticide active ingredient or the floating carrier, and the pesticide active ingredient can be diffused farther in a state in which the buoyancy is enhanced by the floating carrier. In addition, when the gel dissolves in water, the pesticide active ingredient is present in high concentration around the pesticide active ingredient, so that the component is efficiently adsorbed to the pesticide active ingredient, and the pesticide active ingredient diffuses farther even after the gel state is released. In addition, since the gelling ability does not deteriorate, the effect of imparting spreading power and dispersing power to the formulation and the floating assistance continue even after long-term storage.

In the present invention, examples of the alkylene group represented by A in the phosphate salt represented by general formula (I) include an ethylene group having two carbon atoms, a propylene group having three carbon atoms, and a butylene group having four carbon atoms.
In order to exert the spreading force and gelling ability in the present invention, the alkylene group preferably contains an ethylene group having a carbon number of 2. The alkylene group represented by A may be only an ethylene group having a carbon number of 2, or may contain, together with the ethylene group having a carbon number of 2, either a propylene group having a carbon number of 3 or a butylene group having a carbon number of 4, or both.
In the present invention, the alkyl group represented by R in the phosphate salt represented by general formula (I) must have a linear or branched structure having 8 to 10 carbon atoms in order to balance the solubility in water and the spreading force on the water surface. Examples of the alkyl group include an n-octyl group, an n-decyl group, an isodecyl group, and a 2-ethylhexyl group.
In the present invention, in the phosphate ester salt represented by general formula (I), the cation (M in the formula) which is paired with the phosphate ion is not particularly limited as long as it does not impair the functions of the present invention. Examples of the atom represented by M include an alkali metal atom such as a hydrogen atom, a lithium atom, a sodium atom, or a potassium atom, and examples of the substituent include an organic ammonium group such as an ammonium group, a methylammonium group, or a dimethylammonium group.
Since the preparation is produced through a heat drying process, the cation (M in the formula) is preferably K ⁺ , Na ⁺ , or H ⁺ , which is unlikely to volatilize even during the heat drying process.
In the present invention, the number of phosphate bonds in the phosphate salt represented by general formula (I) must be 1 (monoester) or 2 (diester) in order to balance the solubility in water and the spreading force on the water surface. When the phosphate salt is a monoester, p=1 and q=2, in which case the alkyl groups represented by R may be the same or different, and when the phosphate salt is a diester, p=2 and q=1, in which case the atoms represented by M may be the same or different.
In the present invention, the phosphoric acid monoester salt and phosphoric acid diester salt represented by the general formula (I) may be used alone or in combination.

The amount of polyoxyalkylene alkyl ether phosphate ester salt that can be used in the present invention is 1 to 40% by weight, preferably 3 to 25% by weight, in the formulation, and there is no problem in using one or more types in combination.

<Water-soluble alkylene glycol>
The water-soluble alkylene glycol used in the present invention is essential for the polyoxyalkylene alkyl ether phosphate salt to exert its functions. The water-soluble alkylene glycol has both hydrophilicity and lipophilicity, and when used in combination with a polyoxyalkylene alkyl ether, it adjusts the water dissolution time of the gel that is generated upon contact with water. This not only maximizes the spreading and dispersing power of the polyoxyalkylene alkyl ether phosphate salt, but also provides a secondary effect of providing the formulation with a floating aid effect by the gel holding the floating carrier.

The water-soluble alkylene glycol that can be used in the present invention may be any alkylene glycol that is miscible with water, such as ethylene glycol, propylene glycol, butylene glycol, pentylene glycol, and hexylene glycol, and there is no problem in using one or more of these in combination.

The amount of water-soluble alkylene glycol that can be used in the present invention is 0.5 to 20% by weight, preferably 1 to 10% by weight, in the formulation.

Binder
Examples of the auxiliary binder include, but are not limited to, dextrin (roasted dextrin, enzyme-modified dextrin, etc.), processed starches such as acid-decomposed starch, oxidized starch, pregelatinized starch, etherified starch (carboxymethyl starch, hydroxyalkyl starch, etc.), esterified starch (starch acetate, starch phosphate, etc.), crosslinked starch, grafted starch, and other such modified starches; natural substances such as sodium alginate, gum arabic, gelatin, tragacanth gum, locust bean gum, and casein; cellulose derivatives such as sodium carboxymethylcellulose, hydroxyethylcellulose, hydroxypropylcellulose, hydroxypropylmethylcellulose, methylcellulose, ethylcellulose, and acetylcellulose; and polyvinyl alcohol and polyvinylpyrrolidone. These may be used alone or in combination with one or more of them.

From the viewpoint of disintegration and dispersibility, sodium carboxymethylcellulose is preferred.
When a polyoxyalkylene alkyl ether phosphate salt and a water-soluble alkylene glycol are contained, sodium carboxymethyl cellulose or polyvinyl alcohol is preferred from the standpoint of disintegration and dispersibility.
The content of the binder usable in the present invention is preferably 0.1 to 10% by weight.

Other supplements
In addition to the above-mentioned components, the water-floating pesticide formulation of the present invention may contain the following components as adjuvants to the extent that the effect of the present invention is not lost.

For example, surfactants include nonionic surfactants, anionic surfactants other than those mentioned above, cationic surfactants, and amphoteric surfactants.

Nonionic surfactants include polyoxyethylene alkyl aryl ethers, polyoxyethylene alkyl ethers, polyoxyethylene aryl aryl ethers, polyoxyethylene alkyl esters, and alkyl esters of sorbitan.

Examples of anionic surfactants other than those mentioned above include dodecylbenzenesulfonate, alkylsulfonate, lauryl sulfate, α-olefinsulfonate, polyoxyethylene alkylsulfosuccinate, polyoxyethylene alkyl ether sulfate, polyoxyethylene alkylaryl ether sulfate, polyoxyethylene arylphenyl ether phosphate, polyoxyethylene styryl phenyl ether phosphate, and sodium and potassium salts of (co)polymers of carboxylic acids such as acrylic acid and maleic acid, and copolymers of these with styrenesulfonic acid, vinyl groups, and the like.
In addition, the sodium and potassium salts of (co)polymers of carboxylic acids such as acrylic acid and maleic acid, and copolymers of these with styrenesulfonic acid, vinyl groups, etc., are expected to contribute to the disintegration and dispersibility of preparations.

Cationic surfactants include alkyltrimethylammonium salts, alkyldimethylbenzylammonium salts, and alkylpyridinium salts.

Examples of amphoteric surfactants include dialkylaminoethyl betaine and alkyldimethylbenzyl betaine.

The surfactants that can be used in the present invention are not limited to these examples, and one or more types may be used in combination. The content of the surfactant in the formulation is preferably 0.1 to 20% by weight.

The following are examples of solid carriers that can be used in the present invention:

For example, natural minerals such as clay, quartz, calcite, sepiolite, dolomite, chalk, kaolin, pyrophyllite, sericite, halloysite, metahaloysite, wood-bush clay, frog-eye clay, pottery stone, ziglite, allophane, shirasu, kira, talc, pumice, sepiolite, bentonite, hectorite, zeolite, and diatomaceous earth; calcined products of natural minerals such as calcined clay, perlite, vermiculite, attapulgas clay, and calcined diatomaceous earth; magnesium carbonate, calcium carbonate, sodium carbonate, etc. Examples of suitable materials include inorganic salts such as thorium, sodium bicarbonate, ammonium sulfate, sodium sulfate, magnesium sulfate, diammonium hydrogen phosphate, ammonium dihydrogen phosphate, and potassium chloride; sugars such as glucose, fructose, sucrose, and lactose; polysaccharides such as starch, powdered cellulose, and dextrin; organic substances such as urea, urea derivatives, benzoic acid, and salts of benzoic acid; and plants such as wood flour, corn cobs, walnut shells, and tobacco stalks, and white carbon.

The amount of solid carrier that can be used in the present invention is 3 to 95% by weight, preferably 5 to 90% by weight, in the formulation.

Examples of preservatives and antiseptics include potassium sorbate, p-chloro-m-xylenol, butyl p-oxybenzoate, 1,2-benzisothiazolin-3-one, 5-chloro-2-methyl-4-isothiazolin-3-one, and 2-methyl-4-isothiazolin-3-one. Examples of pH adjusters include hydrochloric acid, sulfuric acid, citric acid, phosphoric acid, and magnesium carbonate. Examples of stabilizers for the pesticide active ingredients include antioxidants, ultraviolet light inhibitors, and crystal precipitation inhibitors, but they are not limited to the adjuvants exemplified here.

The amount of these adjuvants that can be used in the present invention is 0.01 to 15% by weight in the formulation, and preferably 0.1 to 10% by weight.

<B. Physical properties of the formulation>
In order for the water-floating pesticide formulation of the present invention to exhibit good floating and diffusibility as well as excellent shelf life, not only the formulation components but also the physical properties of the pesticide formulation such as the ratio of long diameter to short diameter at the base of the particle, particle size, and number of particles per gram, which will be described below, are required.

<Ratio of major axis to minor axis at the base of the grain>
In the water-floating pesticide formulation of the present invention, the bottom surface of the granule refers to the surface resulting from the screen holes during granulation, and the long and short diameters of the bottom surface refer to the maximum diameter when a straight line (diameter) is drawn passing through the center of the bottom surface, and the short diameter is the minimum diameter.

Therefore, the long/short axis ratio of the base of a particle refers to the value obtained by cutting the base of the formulation with a cutter so that it forms a cross section, measuring the maximum diameter (long axis) and minimum diameter (short axis) of the cross section with a microscope, and calculating the ratio of the long axis to the short axis as the average value for 10 particles of the formulation.

In the water-floating pesticide formulation of the present invention, adjusting the long diameter/short diameter ratio at the bottom of the particle contributes to the floating, diffusibility, and storage stability (the distance the formulation reaches after long-term storage, the diffusion distance) of the formulation. In order to impart the effect of improving floating and diffusibility, it is essential to adjust the long diameter/short diameter ratio to the range of 1.1 to 1.4. The long diameter/short diameter ratio is a parameter that expresses the shape of the formulation, and when it is 1.0 (the minimum value), the shape of the bottom is a perfect circle, and as the value increases, the particle approaches a flat shape. When the long diameter/short diameter ratio is 1.0, the movement of the formulation on the water surface is slow, leading to a decrease in diffusion, and when it exceeds 1.4, the movement on the water surface is fast, but the formulation quickly disintegrates and disperses, resulting in a short diffusion distance of the active ingredient.
In addition, when polyoxyalkylene alkyl ether phosphate salt and propylene glycol are contained, the gel generated when contacting with water increases the time for disintegration of the formulation in water, so the upper limit of the long axis/short axis ratio can be up to 1.6. In addition, regarding the distance the formulation reaches and the diffusion distance after long-term storage, when the long axis/short axis ratio is 1.1 or more, the quality deterioration after long-term storage is suppressed. It is presumed that the reason for this is that with an increase in the long axis/short axis ratio, the area of the formulation in contact with the water surface increases, making it more susceptible to the influence of the buoyancy of water, or the release rate of the surfactant on the water surface increases, improving the efficiency of disintegration and dispersion on the water surface.

The long diameter/short diameter ratio can be adjusted by adjusting the extrusion hole diameter during granulation in the extrusion granulation process, and then using a machine that rotates granules, such as a drum type granulator or a Marumerizer, in the granulation process to rotate the granules before drying and control the centrifugal force to control the long diameter/short diameter ratio.
In addition, the granulated material before drying is soft because the binder contains water and is in a swollen state, and if the particle size (extrusion hole diameter) is large, it will be affected by its own weight. Therefore, when rotational motion is applied, centrifugal force and its own weight act, and the cross section of the granulated material becomes flattened (generating major and minor diameters).

Granularity
In the water-floating pesticide formulation of the present invention, the particle size is calculated from the following formula (1) based on the weight of the formulation remaining on the 1.70 mm sieve when 100 g of the formulation is sieved through test sieves with openings of 2.80 mm and 1.70 mm.

In the water-floating pesticide formulation of the present invention, adjusting the particle size contributes to the floatability and diffusibility of the formulation. In terms of the balance between floatability and diffusibility, it is essential that the particle size is in the range of 2.80 mm to 1.70 mm for 80% by weight or more, and more preferably 90% by weight or more. Particles smaller than this particle size range have less floating carrier and therefore less buoyancy, making them more likely to sink, while particles with a larger particle size have a larger weight per particle, which slows down movement on the water surface and reduces diffusibility.

One method for adjusting the particle size is to adjust the extrusion hole diameter during granulation in the extrusion granulation process, and then, in the sieving process, appropriately adjust the length of the granules of the granulated material before drying to control the particle size. The sieving machine used to adjust the particle size is not particularly limited, but may be a drum sieving machine or a rotary sieving machine such as a Marmerizer, or a crushing type sieving machine such as a pin mill, oscillator, Randel mill, or nebulizer. From the standpoint of economy and labor saving during production, a rotary sieving machine such as a drum sieving machine that can simultaneously adjust the long axis/short axis ratio of the bottom surface of the particles is preferred.

Number of grains per gram
In the water-floating pesticide formulation of the present invention, the number of particles per 1 g is expressed as the number of particles in 5.0 g of the formulation weighed out using a particle counter, and the measured value is divided by 5 (rounded off to the nearest whole number).

In the water-floating pesticide formulation of the present invention, adjusting the number of particles per 1 g contributes to the floatability and diffusibility of the formulation. In terms of the balance between floatability and diffusibility, it is essential that the number of particles per 1 g is 50 to 150. For the same reason as for the particle size described above, particles with a number of particles greater than 150 per 1 g are small and have less buoyancy, making them more likely to sink, while particles with a number of particles less than 50 have a large weight per particle, which slows down the movement on the water surface and reduces diffusibility.
In addition, when polyoxyalkylene alkyl ether phosphate ester salt and propylene glycol are contained, the enhanced diffusivity allows even particles with low buoyancy to diffuse farther, so the upper limit of the number of particles per gram can be up to 200.

One method for adjusting the number of particles per gram is to crush the granulated material before drying in the sieving process, thereby controlling the number of particles per gram. The sieving machine used to adjust the number of particles is not particularly limited, but may be a drum type sieving machine, a rotary type sieving machine such as a Marmerizer, or a crushing type sieving machine such as a pin mill, oscillator, Randel mill, or nebulizer. From the standpoint of economy and labor saving during production, a rotary type sieving machine such as a drum type sieving machine is preferred, as it is possible to simultaneously adjust the long/short diameter ratio of the base of the particles and the particle size.

<Method of manufacturing water-floating pesticide formulation>
The water-floating pesticide formulation of the present invention is produced by an extrusion granulation method, which is advantageous in terms of economy and production efficiency.

In the manufacturing process, the pesticide active ingredient, the floating carrier, one or more selected from alkylnaphthalenesulfonate Na and dialkylsuccinatesulfonate Na, if necessary, polyoxyalkylene alkyl ether phosphate salt, if necessary, alkylnaphthalenesulfonate formaldehyde condensate Na, naphthalenesulfonate formaldehyde condensate Na, partially desulfonated ligninsulfonate Na, and ligninsulfonate Na, and various auxiliary agents are added, and mixed uniformly using a juice mixer, hammer mill, Loedige mixer, ribbon mixer, etc. Water is added to this mixture and kneaded using a double-arm kneader or ribbon mixer, etc. In addition, when the pesticide active ingredient is wet-pulverized and added to the slurry for reasons such as mixing accuracy, it is added together with water during kneading.

The physical properties of the water-floating pesticide formulation of the present invention are adjusted in the granulation and sizing processes that follow the kneading process. In the sizing process, the major axis/minor axis ratio of the base of the particles, particle size, and particle number may be adjusted all at once, or the major axis/minor axis ratio of the base of the particles may be adjusted and then the particle size and particle number may be adjusted. It is preferable to adjust them all at once, as this eliminates the number of steps and improves the economic efficiency of production.

In the granulation and sieving process, the mixture is first granulated using an extrusion granulator such as a basket granulator or a screw granulator. The extrusion hole diameter during granulation is preferably 2.8 to 3.0 mm in order to adjust the physical properties of the water-floating pesticide formulation of the present invention. With this extrusion hole diameter, the water-floating pesticide formulation of the present invention can be sized by sieving the obtained granules with a machine that applies centrifugal force to the particles, such as a drum sieving machine or a marumerizer, so that the major axis/minor axis ratio at the bottom is 1.1 to 1.4, and the particle size is 80% or more by weight in the range of 2.80 mm to 1.70 mm, and the number of particles per gram is 50 to 150. After sieving, the water-floating pesticide formulation used in the present invention is obtained by drying using a fluidized bed dryer or a bed dryer, and then sieving.

When using an agrochemical active ingredient whose dissolution is to be accelerated, it is possible to add a coating step to the extent that the effect of the present invention is not lost.

<How water-floating pesticide formulations are used>
The water surface floating pesticide formulation of the present invention is directly sprayed without entering the paddy field. Spraying methods include manual spraying, spraying in a container such as a cup, mechanical spraying with a power sprayer, aerial spraying using a radio-controlled helicopter or drone, and water inlet spraying into the water flowing into the paddy field. In consideration of avoiding exposure to radiation by the sprayer, a spraying method that does not directly touch the formulation is preferred. The application amount is usually 50 to 500 g, preferably 75 to 300 g per 10 ares.

The present invention will be described in detail below with reference to examples, but the present invention is not limited to these.

In the following examples and comparative examples, "parts" means "parts by weight" and "%" means "% by weight."

In the following examples and comparative examples, the instruments (microscope, sieve shaker, particle number measuring instrument) used to measure the major axis/minor axis ratio, particle size, and particle number of the water-floating pesticide formulations were VHX-5000 (manufactured by Keyence Corporation), a sieve shaker low tap type (manufactured by Iida Manufacturing Co., Ltd.), and a multi-auto counter KC-1M5 type (manufactured by Fujiwara Manufacturing Co., Ltd.), respectively.

[Example 1]
24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasuballoon (average particle size 70-90 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 5.0 parts of dextrin, 10.0 parts of bentonite, 30.0 parts of perlite, and 3.0 parts of clay were pulverized and mixed with a hammer mill (Sample Mill KIIW-1, manufactured by Dalton Co., Ltd.) to obtain a powder mixture. The obtained powder mixture was placed in a double-arm kneader (KDHJ, manufactured by Dalton Co., Ltd.), and kneaded for 15 minutes after adding water. Next, this water-kneaded mixture was granulated with an extrusion granulator equipped with a basket-type screen with a hole diameter of 3.0 mm. The obtained granulated product was pre-dried, sized with a drum-type granulator, and dried with a fluidized bed dryer. This was sieved at 3.35 mm to 2.00 mm to obtain a water-floating pesticide formulation. The particle size of the obtained preparation was 85% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 98.

[Example 2]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium carboxymethyl cellulose, 35.0 parts of perlite, 7.5 parts of clay, and 2.8 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 105.

[Example 3]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 2.0 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium polyacrylate, 2.0 parts of sodium carboxymethylcellulose, 57.0 parts of perlite, 10.0 parts of clay, and a particle size of 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per gram was 113.

[Example 4]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium carboxymethylcellulose, 36.0 parts of diatomaceous earth, 10.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 93% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per gram was 83.

[Example 5]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of shirasuballoon (average particle size 70-90 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 10.0 parts of bentonite, 20.0 parts of perlite, 4.5 parts of white carbon, 5.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 88.

[Example 6]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 33.0 parts of diatomaceous earth, 5.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 88% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 96.

[Example 7]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium polyacrylate, 3.0 parts of sodium carboxymethylcellulose, 37.0 parts of diatomaceous earth, 6.5 parts of clay, and 3.0 mm of particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 87% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 110.

[Example 8]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 32.0 parts of perlite, 5.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 96% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 98.

[Example 9]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium acrylic acid-vinyl sulfonic acid copolymer, 2.0 parts of sodium carboxymethyl cellulose, 34.5 parts of perlite, 6.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 97% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per gram was 87.

[Example 10]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of shirasuballoon (average particle size 70-90 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 2.0 parts of sodium carboxymethylcellulose, 28.5 parts of perlite, 7.5 parts of clay, and 2.8 mm particle size. A water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 76.

[Example 11]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 2.0 parts of sodium polyacrylate, 2.0 parts of sodium carboxymethyl cellulose, 10.0 parts of bentonite, 18.5 parts of perlite, 5.0 parts of white carbon, 4.0 parts of clay, and 3.0 mm in particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 87% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 93.

[Example 12]
The formulation composition is 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of ceramic balloon (average particle size 20 to 150 μm) (floating carrier), and sodium alkylnaphthalenesulfonate.
A water-floating pesticide formulation was prepared in accordance with Example 1 using 3.0 parts of naphthalenesulfonic acid formaldehyde condensate Na 3.0 parts of acrylic acid-vinylsulfonic acid copolymer Na 2.0 parts of carboxymethylcellulose Na, 10.0 parts of bentonite, 21.0 parts of diatomaceous earth, 5.0 parts of clay, and a particle size of 2.8 mm. The particle size of the resulting formulation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per gram was 85.

[Example 13]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 2.0 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 2.0 parts of sodium acrylic acid-maleic acid copolymer, 2.0 parts of sodium carboxymethyl cellulose, 55.5 parts of diatomaceous earth, 10.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 68.

[Example 14]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of acrylic acid-vinylsulfonic acid copolymer Na, 2.0 parts of carboxymethylcellulose Na, 10.0 parts of bentonite, 22.0 parts of perlite, 3.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 88% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 111.

[Example 15]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 1.5 parts of dialkyl succinate sulfonate Na, 3.0 parts of naphthalene sulfonic acid formaldehyde condensate Na, 3.0 parts of acrylic acid-methacrylic acid copolymer Na, 3.0 parts of carboxymethylcellulose Na, 10.0 parts of bentonite, 10.0 parts of perlite, 7.5 parts of white carbon, 8.0 parts of clay, and 3.0 mm in particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 105.

[Example 16]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 29.0 parts of perlite, 5.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 94% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 121.

[Example 17]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 30.0 parts of shirasuballoon (average particle size 90 to 120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium alkyl naphthalene sulfonate formaldehyde condensate, 3.0 parts of sodium polyacrylic acid, 3.0 parts of sodium carboxymethyl cellulose, 30.5 parts of diatomaceous earth,
Using 5.0 parts of clay and a particle size of 2.8 mm, a water-floating pesticide formulation was prepared in accordance with Example 1. The particle size of the resulting formulation was 93% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per gram was 83.

[Example 18]
12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of polyvinyl alcohol, 47.0 parts of perlite, and 10.0 parts of clay were pulverized and mixed with a hammer mill (Sample Mill KIIW-1, Dalton Co., Ltd.) to obtain a powder mixture. The obtained powder mixture was placed in a double-arm kneader (KDHJ, Dalton Co., Ltd.), and kneaded for 15 minutes after adding water. Next, this water-kneaded mixture was granulated with an extrusion granulator equipped with a basket-type screen with a hole diameter of 3.0 mm. The obtained granulated product was pre-dried, sized with a drum-type granulator, and dried with a fluidized bed dryer. This was sieved at 3.35 mm to 2.00 mm to obtain a water-floating pesticide formulation. The particle size of the obtained preparation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 89.

[Example 19]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium carboxymethyl cellulose, 48.5 parts of perlite, 10.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 97.

[Example 20]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 2.0 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium polyacrylate, 2.0 parts of sodium carboxymethylcellulose, 60.0 parts of perlite, 18.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 88% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 106.

[Example 21]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium carboxymethylcellulose, 43.0 parts of diatomaceous earth, 10.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 93% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 82.

[Example 22]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 1.5 parts of dialkyl succinate sulfonic acid Na, 2.0 parts of acrylic acid-maleic acid copolymer Na, 2.0 parts of carboxymethyl cellulose Na, 10.0 parts of bentonite, 30.0 parts of perlite, 5.0 parts of white carbon, 7.5 parts of clay, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 96% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 88.

[Example 23]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of acrylic acid-methacrylic acid copolymer Na, 3.0 parts of sodium carboxymethylcellulose, 40.0 parts of diatomaceous earth, 10.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 93.

[Example 24]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium polyacrylate, 3.0 parts of sodium carboxymethyl cellulose, 45.0 parts of diatomaceous earth, 6.5 parts of clay, and 3.0 mm of particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 97.

[Example 25]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium acrylic acid-maleic acid copolymer, 2.0 parts of sodium carboxymethylcellulose, 45.0 parts of perlite, 10.0 parts of clay, and a particle size of 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 94% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 95.

[Example 26]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium acrylic acid-vinyl sulfonic acid copolymer, 3.0 parts of sodium carboxymethyl cellulose, 48.5 parts of perlite, 7.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 97% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 107.

[Example 27]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 28.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of acrylic acid-methacrylic acid copolymer Na, 3.0 parts of carboxymethylcellulose Na, 38.0 parts of perlite, 10.0 parts of clay, and 2.8 mm particle size. A water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 91.

[Example 28]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 28.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 1.5 parts of dialkyl succinate sulfonate Na, 3.0 parts of partially desulfonated lignin sulfonate Na, 3.0 parts of polyacrylic acid Na, 2.0 parts of carboxymethyl cellulose Na, 10.0 parts of bentonite, 30.0 parts of perlite, 5.0 parts of white carbon, 5.5 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 87% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 83.

[Example 29]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of naphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of acrylic acid-vinylsulfonic acid copolymer Na, 3.0 parts of carboxymethylcellulose Na, 10.0 parts of bentonite, 36.0 parts of diatomaceous earth, 5.0 parts of clay, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 98% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 86.

[Example 30]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 2.0 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 1.5 parts of dialkyl succinate sulfonate Na, 3.0 parts of partially desulfonated lignin sulfonate Na, 2.0 parts of acrylic acid-maleic acid copolymer Na, 2.0 parts of carboxymethyl cellulose Na, 35.0 parts of perlite, 35.0 parts of diatomaceous earth, 7.5 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 93% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 95.

[Example 31]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 28.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of acrylic acid-vinylsulfonic acid copolymer Na, 2.0 parts of carboxymethylcellulose Na, 10.0 parts of bentonite, 30.0 parts of perlite, 9.0 parts of clay, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 108.

[Example 32]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of dialkyl succinate sulfonate Na, 3.0 parts of naphthalene sulfonic acid formaldehyde condensate Na, 3.0 parts of acrylic acid-methacrylic acid copolymer Na, 2.0 parts of carboxymethyl cellulose Na, 10.0 parts of bentonite, 19.5 parts of perlite, 15.0 parts of white carbon, 4.0 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 90.

[Example 33]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of partially desulfonated ligninsulfonic acid Na, 2.0 parts of acrylic acid-maleic acid copolymer Na, 2.0 parts of carboxymethylcellulose Na, 40.0 parts of perlite, 8.0 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 88.

[Example 34]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium alkyl naphthalene sulfonate formaldehyde condensate, 2.0 parts of sodium polyacrylate, 2.0 parts of sodium carboxymethyl cellulose, 44.5 parts of diatomaceous earth, 5.0 parts of clay, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 96% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 99.

[Example 35]
10.0 parts of ipfencarbazone (herbicidal active ingredient), 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water were mixed, and then wet-pulverized in a Dyno Mill (manufactured by Shinmaru Enterprises) until the average particle size reached 1.0 μm, to obtain a slurry. In addition, 25.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 2.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of polyvinyl alcohol, 5.0 parts of bentonite, 42.0 parts of perlite, and 13.0 parts of clay were pulverized and mixed in a hammer mill (Sample Mill KIIW-1, manufactured by Dalton Co., Ltd.) to obtain a powder mixture. The obtained slurry and powder mixture were placed in a double-arm kneader (KDHJ, manufactured by Dalton Co., Ltd.), and after adding water, they were kneaded for 15 minutes. Next, this water-kneaded mixture was granulated in an extrusion granulator equipped with a basket-type screen with a hole diameter of 3.0 mm. The obtained granules were pre-dried, sized using a drum-type sieving machine, and dried using a fluidized bed dryer. The granules were sieved at 3.35 mm to 2.00 mm to obtain a water-floating pesticide formulation. The particle size of the obtained formulation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.4, and the number of particles per gram was 109.

[Example 36]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 28.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium carboxymethylcellulose, 51.5 parts of perlite, 7.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water), and the particle size was 2.8 mm. A water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 115.

[Example 37]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 2.0 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium polyacrylate, 3.0 parts of sodium carboxymethylcellulose, 70.0 parts of perlite, 10.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 88% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 123.

[Example 38]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 28.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium polyacrylate, 3.0 parts of sodium carboxymethylcellulose, 48.0 parts of diatomaceous earth, 8.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), and the particle size was 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 92% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 103.

[Example 39]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of acrylic acid-maleic acid copolymer Na, 3.0 parts of sodium carboxymethyl cellulose, 10.0 parts of bentonite, 33.5 parts of perlite, 10.0 parts of white carbon, 5.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium dialkyl succinate sulfonate, and 14.0 parts of water), with a particle size of 2.8 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 95% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 100.

[Example 40]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of acrylic acid-methacrylic acid copolymer Na, 2.0 parts of sodium carboxymethylcellulose, 43.0 parts of diatomaceous earth, 10.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), with a particle size of 2.8 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 87% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 123.

[Example 41]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium polyacrylate, 3.0 parts of sodium carboxymethylcellulose, 50.0 parts of diatomaceous earth, 7.5 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water), with a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 109.

[Example 42]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalene sulfonate, 3.0 parts of sodium acrylic acid-maleic acid copolymer, 2.0 parts of sodium carboxymethylcellulose, 45.0 parts of perlite, 7.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalene sulfonate, and 14.0 parts of water), with a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 96% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 103.

[Example 43]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 28.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of acrylic acid-vinyl sulfonic acid copolymer Na, 3.0 parts of sodium carboxymethyl cellulose, 50.0 parts of perlite, 4.5 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium dialkyl succinate sulfonate, and 14.0 parts of water), with a particle size of 2.8 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 95% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 126.

[Example 44]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 28.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 3.0 parts of sodium acrylic acid-methacrylic acid copolymer, 2.0 parts of sodium carboxymethylcellulose, 46.0 parts of perlite, 5.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), and the particle size was 2.8 mm. A water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 113.

[Example 45]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 28.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 2.0 parts of sodium polyacrylate, 2.0 parts of sodium carboxymethyl cellulose, 10.0 parts of bentonite, 20.0 parts of perlite, 15.0 parts of white carbon, 8.5 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium dialkyl succinate sulfonate, 14.0 parts of water), and the particle size was 3.0 mm. A water surface floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 99.

[Example 46]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 28.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of naphthalenesulfonic acid formaldehyde condensate Na, 2.0 parts of acrylic acid-vinylsulfonic acid copolymer Na, 3.0 parts of carboxymethylcellulose Na, 10.0 parts of bentonite, 38.0 parts of diatomaceous earth, 6.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of alkylnaphthalenesulfonic acid Na, 14.0 parts of water), and the particle size was 2.8 mm. A water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 96% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 108.

[Example 47]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 2.0 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 2.0 parts of sodium acrylic acid-maleic acid copolymer, 2.0 parts of sodium carboxymethyl cellulose, 10.0 parts of perlite, 61.5 parts of diatomaceous earth, 8.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium dialkyl succinate sulfonate, 14.0 parts of water), and the particle size was 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 93% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 103.

[Example 48]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 2.0 parts of sodium acrylic acid-vinylsulfonic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 10.0 parts of bentonite, 38.0 parts of perlite, 6.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium alkylnaphthalenesulfonate, 14.0 parts of water), and the particle size was 2.8 mm. A water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 113.

[Example 49]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 28.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium naphthalenesulfonate formaldehyde condensate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 3.0 parts of sodium carboxymethyl cellulose, 10.0 parts of bentonite, 25.0 parts of perlite, 10.0 parts of white carbon, 7.5 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water), with a particle size of 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained preparation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.1, and the number of particles per gram was 96.

[Example 50]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalene sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium acrylic acid-maleic acid copolymer, 2.0 parts of sodium carboxymethylcellulose, 45.0 parts of perlite, 9.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium alkylnaphthalene sulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water surface floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 94% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 97.

[Example 51]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 28.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium alkyl naphthalene sulfonate formaldehyde condensate, 3.0 parts of sodium polyacrylate, 3.0 parts of sodium carboxymethyl cellulose, 48.0 parts of diatomaceous earth, 3.5 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium dialkyl succinate sulfonate, and 14.0 parts of water), with a particle size of 2.8 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 97% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 90.

[Example 52]
Simetryn 12.0 parts (herbicidal active ingredient), Shirasu balloon (average particle size 70-90 μm) (floating carrier) 30.0 parts, alkyl naphthalene sulfonate Na 3.0 parts, dextrin 5.0 parts, bentonite 10.0 parts, perlite 38.0 parts, clay 2.0 parts were pulverized and mixed with a hammer mill (sample mill KIIW-1, Dalton Co., Ltd.) to obtain a powder mixture. The obtained powder mixture was placed in a double-arm kneader (KDHJ, Dalton Co., Ltd.), water was added, and the mixture was kneaded for 15 minutes. Next, this water-kneaded mixture was granulated with an extrusion granulator equipped with a basket-type screen with a hole diameter of 3.0 mm. The obtained granulated product was pre-dried, sized with a drum-type granulator, and dried with a fluidized bed dryer. This was sieved at 3.35 mm to 2.00 mm to obtain a water-floating pesticide formulation. The particle size of the obtained preparation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.4, and the number of particles per gram was 93.

[Example 53]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 28.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium carboxymethyl cellulose, 43.0 parts of perlite, 12.5 parts of clay, and 2.8 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 88.

[Example 54]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 2.0 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium polyacrylate, 2.0 parts of sodium carboxymethylcellulose, 65.0 parts of perlite, 14.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 87% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per gram was 97.

[Example 55]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 28.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium carboxymethylcellulose, 45.0 parts of diatomaceous earth, 9.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 93% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 96.

[Example 56]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 28.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of sodium carboxymethyl cellulose, 10.0 parts of bentonite, 30.0 parts of perlite, 8.0 parts of white carbon, 5.5 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 96% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 108.

[Example 57]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 28.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 47.0 parts of diatomaceous earth, 5.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 87% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 95.

[Example 58]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 30.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium polyacrylate, 3.0 parts of sodium carboxymethylcellulose, 45.0 parts of diatomaceous earth, 5.5 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 97.

[Example 59]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 30.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium acrylic acid-maleic acid copolymer, 2.0 parts of sodium carboxymethylcellulose, 46.0 parts of perlite, 4.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 96% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 93.

[Example 60]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 30.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium acrylic acid-vinyl sulfonic acid copolymer, 2.0 parts of sodium carboxymethyl cellulose, 47.5 parts of perlite, 5.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 94% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 98.

[Example 61]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 2.0 parts of sodium carboxymethylcellulose, 40.0 parts of perlite, 8.0 parts of clay, and 2.8 mm particle size. A water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 108.

[Example 62]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 28.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium polyacrylate, 2.0 parts of sodium carboxymethyl cellulose, 10.0 parts of bentonite, 25.0 parts of perlite, 10.0 parts of white carbon, 5.5 parts of clay, and a particle size of 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 100.

[Example 63]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 30.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of naphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of acrylic acid-vinylsulfonic acid copolymer Na, 2.0 parts of carboxymethylcellulose Na, 10.0 parts of bentonite, 30.0 parts of diatomaceous earth, 7.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 97.

[Example 64]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 2.0 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 2.0 parts of sodium acrylic acid-maleic acid copolymer, 2.0 parts of sodium carboxymethyl cellulose, 67.5 parts of diatomaceous earth, 10.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 94% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 96.

[Example 65]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of acrylic acid-vinylsulfonic acid copolymer Na, 2.0 parts of carboxymethylcellulose Na, 10.0 parts of bentonite, 30.0 parts of perlite, 7.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 93.

[Example 66]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 30.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of dialkyl succinate sulfonate Na, 3.0 parts of naphthalene sulfonic acid formaldehyde condensate Na, 2.0 parts of acrylic acid-methacrylic acid copolymer Na, 2.0 parts of carboxymethyl cellulose Na, 10.0 parts of bentonite, 20.0 parts of perlite, 15.0 parts of white carbon, 4.5 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 101.

[Example 67]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 30.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 39.0 parts of perlite, 7.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 93% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 94.

[Example 68]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium alkyl naphthalene sulfonate formaldehyde condensate, 2.0 parts of sodium polyacrylate, 3.0 parts of sodium carboxymethyl cellulose, 48.5 parts of diatomaceous earth, 5.0 parts of clay, and 2.8 mm particle size. A water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 97% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 98.

[Example 69]
Benfuresate 18.0 parts (herbicidal active ingredient), Shirasu balloon (average particle size 70-90 μm) (floating carrier) 30.0 parts, alkylnaphthalenesulfonic acid Na 3.0 parts, dextrin 3.0 parts, polyvinyl alcohol 1.0 parts, bentonite 5.0 parts, perlite 30.0 parts, clay 10.0 parts were pulverized and mixed with a hammer mill (sample mill KIIW-1, Dalton Co., Ltd.) to obtain a powder mixture. The obtained powder mixture was placed in a double-arm kneader (KDHJ, Dalton Co., Ltd.), water was added, and the mixture was kneaded for 15 minutes. Next, the water-kneaded mixture was granulated with an extrusion granulator equipped with a basket-type screen with a hole diameter of 3.0 mm. The obtained granulated product was pre-dried, sized with a drum-type granulator, and dried with a fluidized bed dryer. This was sieved at 3.35 mm to 2.00 mm to obtain a water-floating pesticide formulation. The particle size of the obtained preparation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 93.

[Example 70]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 28.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium carboxymethyl cellulose, 45.5 parts of perlite, 5.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 87% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per gram was 83.

[Example 71]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 2.0 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium polyacrylate, 2.0 parts of sodium carboxymethylcellulose, 63.0 parts of perlite, 10.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per gram was 86.

[Example 72]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 30.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium carboxymethylcellulose, 39.0 parts of diatomaceous earth, 7.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 94% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 97.

[Example 73]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 28.0 parts of shirasuballoon (average particle size 70-90 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 10.0 parts of bentonite, 25.0 parts of perlite, 7.5 parts of white carbon, 5.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 93% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 82.

[Example 74]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 30.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 2.0 parts of sodium carboxymethylcellulose, 40.0 parts of diatomaceous earth, 5.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 85.

[Example 75]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 30.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium polyacrylate, 2.0 parts of sodium carboxymethylcellulose, 40.0 parts of diatomaceous earth, 5.5 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 80.

[Example 76]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 28.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium acrylic acid-maleic acid copolymer, 2.0 parts of sodium carboxymethylcellulose, 38.0 parts of perlite, 8.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 93% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 91.

[Example 77]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium acrylic acid-vinyl sulfonic acid copolymer, 2.0 parts of sodium carboxymethyl cellulose, 46.5 parts of perlite, 5.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 97% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per gram was 79.

[Example 78]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 28.0 parts of shiras balloon (average particle size 70-90 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 2.0 parts of sodium carboxymethylcellulose, 39.0 parts of perlite, 5.0 parts of clay, and 2.8 mm particle size. A water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 75.

[Example 79]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 30.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 2.0 parts of sodium polyacrylate, 2.0 parts of sodium carboxymethyl cellulose, 10.0 parts of bentonite, 18.5 parts of perlite, 10.0 parts of white carbon, 5.0 parts of clay, and 3.0 mm in particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 98.

[Example 80]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 30.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of naphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of acrylic acid-vinylsulfonic acid copolymer Na, 2.0 parts of carboxymethylcellulose Na, 10.0 parts of bentonite, 28.0 parts of diatomaceous earth, 4.0 parts of clay, and a particle size of 2.8 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 97% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 89.

[Example 81]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 2.0 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 2.0 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of sodium carboxymethyl cellulose, 60.5 parts of diatomaceous earth, 10.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 95% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 86.

[Example 82]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 28.0 parts of shiras balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 3.0 parts of sodium acrylic acid-vinylsulfonic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 10.0 parts of bentonite, 28.0 parts of perlite, 4.0 parts of clay, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per gram was 98.

[Example 83]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 30.0 parts of silas balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium naphthalene sulfonate formaldehyde condensate, 3.0 parts of sodium acrylic acid-methacrylic acid copolymer, 3.0 parts of sodium carboxymethyl cellulose, 10.0 parts of bentonite, 15.0 parts of perlite, 12.0 parts of white carbon, 4.5 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 101.

[Example 84]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 28.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 37.0 parts of perlite, 5.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 95% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 96.

[Example 85]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 30.0 parts of shiras balloon (average particle size 90-120 μm) (floating carrier), 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium alkyl naphthalene sulfonate formaldehyde condensate, 3.0 parts of sodium polyacrylate, 3.0 parts of sodium carboxymethyl cellulose, 36.5 parts of diatomaceous earth, 5.0 parts of clay, and 2.8 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 93% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 93.

[Comparative Example 1]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium carboxymethylcellulose, 40.0 parts of perlite, 6.0 parts of clay, 3.0 mm particle size, 3.35 mm and 0.85 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 72% in the range of 2.80-1.70 mm (the remainder was 28% below the particle size of 1.70 mm), the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 179, so that a formulation with many particles smaller than 1.70 mm in particle size was prepared.

[Comparative Example 2]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 36.0 parts of perlite, 7.0 parts of clay, 1.7 mm particle size, 2.00 mm and 0.85 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 5% in the range of 2.80-1.70 mm (the remainder was 95% below the particle size of 1.70 mm), the major axis/minor axis ratio at the bottom was 1.0, and the number of particles per 1 g was 259, and a formulation with many small particles of 1.70 mm or less was prepared.

[Comparative Example 3]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 2.0 parts of sodium carboxymethylcellulose, 35.0 parts of perlite, 8.0 parts of clay, 4.0 mm particle size, 4.76 mm and 2.36 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 23% in the range of 2.80-1.70 mm (the remainder was 77% above 2.80 mm), the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 36, so a formulation with many particles larger than 2.80 mm was prepared.

[Comparative Example 4]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 37.0 parts of perlite, 6.0 parts of clay, and 3.0mm particle size. The formulation was not sized by a drum sieving machine, and the cross section was dried in a circular shape to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 83% in the range of 2.80-1.70mm, the major axis/minor axis ratio at the bottom was 1.0, and the number of particles per gram was 112.

[Comparative Example 5]
The formulation consisted of 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium carboxymethylcellulose, 38.0 parts of perlite, 8.0 parts of clay, and a particle size of 3.0 mm. The particles were sized using a drum sieving machine, and further sized by pounding up and down in a plastic bag, which was then dried to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.6, and the number of particles per gram was 108.

[Comparative Example 6]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 33.0 parts of perlite, 10.0 parts of clay, and a particle size of 3.0 mm. The product was sized by a drum sieving machine and then smashed up and down in a plastic bag, which was then dried to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.8, and the number of particles per gram was 119.

[Comparative Example 7]
The formulation contained 24.0 parts of kasugamycin (fungicidal active ingredient), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 60.0 parts of perlite, 7.0 parts of clay, and a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 1. The particle size of the resulting formulation was 82% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 103.

[Comparative Example 8]
The formulation contained 24.0 parts of kasugamycin (fungicidal active ingredient), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 18.0 parts of perlite, 49.0 parts of clay, and a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 1. The particle size of the resulting formulation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per gram was 43.

[Comparative Example 9]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium carboxymethylcellulose, 39.0 parts of perlite, 6.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 108.

[Comparative Example 10]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium alkyl sulfate, 3.0 parts of sodium carboxymethylcellulose, 34.0 parts of perlite, 8.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 98.

[Comparative Example 11]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium alkylbenzene sulfonate, 2.0 parts of sodium carboxymethylcellulose, 38.0 parts of perlite, 5.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per gram was 100.

[Comparative Example 12]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of polyoxyethylene alkyl ether, 2.0 parts of carboxymethylcellulose Na, 36.0 parts of perlite, 7.0 parts of clay, and 3.0 mm of particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per gram was 95.

[Comparative Example 13]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of polyoxyethylene arylphenyl ether, 3.0 parts of carboxymethylcellulose Na, 39.0 parts of perlite, 6.0 parts of clay, and 3.0 mm of particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 1. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 113.

[Comparative Example 14]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium carboxymethylcellulose, 47.0 parts of perlite, 10.0 parts of clay, 3.0 mm of particle size, 3.35 mm and 0.85 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 65% in the range of 2.80-1.70 mm (the remainder was 35% below the particle size of 1.70 mm), the major axis/minor axis ratio at the bottom was 1.2, the number of particles per 1 g was 195, and a formulation with many particles smaller than 1.70 mm in particle size was prepared.

[Comparative Example 15]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalene sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium carboxymethylcellulose, 48.0 parts of perlite, 6.0 parts of clay, 1.7 mm particle size, 2.00 mm and 0.85 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 1% in the range of 2.80 to 1.70 mm (the remainder was 99% below the particle size of 1.70 mm), the major axis/minor axis ratio at the bottom was 1.0, and the number of particles per 1 g was 283, and a formulation with many small particles of 1.70 mm or less was prepared.

[Comparative Example 16]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of Na alkyl naphthalene sulfonate, 3.0 parts of Na alkyl naphthalene sulfonate formaldehyde condensate, 3.0 parts of Na carboxymethyl cellulose, 47.0 parts of perlite, 7.0 parts of clay, 4.0 mm particle size, 4.76 mm and 2.36 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 15% in the range of 2.80 to 1.70 mm (the remainder was 85% above 2.80 mm), the major axis/minor axis ratio at the bottom was 1.2, the number of particles per 1 g was 40, and a formulation with many particles larger than 2.80 mm was prepared.

[Comparative Example 17]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalene sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium carboxymethylcellulose, 47.0 parts of perlite, 7.0 parts of clay, and a particle size of 3.0 mm. The formulation was not sized using a drum sieving machine, and the cross section was dried in a circular state to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.0, and the number of particles per gram was 105.

[Comparative Example 18]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium carboxymethylcellulose, 51.0 parts of perlite, 6.0 parts of clay, and a particle size of 3.0 mm. In addition to sizing with a drum sizing machine, the sizing was further carried out by smashing the sizing agent up and down in a plastic bag, and the resulting product was dried to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 82% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.6, and the number of particles per gram was 96.

[Comparative Example 19]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 47.0 parts of perlite, 7.0 parts of clay, and a particle size of 3.0 mm. In addition to sizing with a drum sizing machine, the sizing was further carried out by smashing the sizing agent up and down in a plastic bag, and the resulting product was dried to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.8, and the number of particles per gram was 108.

[Comparative Example 20]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 69.0 parts of perlite, 10.0 parts of clay, and a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 85% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 93.

[Comparative Example 21]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 21.0 parts of perlite, 58.0 parts of clay, and a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 85% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per gram was 38.

[Comparative Example 22]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 2.0 parts of sodium carboxymethylcellulose, 51.0 parts of perlite, 7.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 106.

[Comparative Example 23]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium alkyl sulfate, 2.0 parts of sodium carboxymethylcellulose, 48.0 parts of perlite, 7.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 93.

[Comparative Example 24]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium alkylbenzene sulfonate, 2.0 parts of sodium carboxymethyl cellulose, 46.0 parts of perlite, 9.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 95.

[Comparative Example 25]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of polyoxyethylene alkyl ether, 3.0 parts of carboxymethylcellulose Na, 50.0 parts of perlite, 4.0 parts of clay, and 3.0 mm of particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 83.

[Comparative Example 26]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of polyoxyethylene arylphenyl ether, 3.0 parts of carboxymethylcellulose Na, 49.0 parts of perlite, 8.0 parts of clay, and 3.0 mm of particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 18. The particle size of the obtained formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 99.

[Comparative Example 27]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium carboxymethylcellulose, 52.0 parts of perlite, 8.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), with a particle size of 3.0 mm and sieves of 3.35 mm and 0.85 mm used for sieving. A water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the resulting formulation was 68% in the range of 2.80-1.70 mm (the remainder was a particle size of 1.
32%) below 70 mm, the long axis/short axis ratio at the base was 1.2, and the number of particles per gram was 175, meaning that a preparation was prepared in which most of the particles were smaller than 1.70 mm in size.

[Comparative Example 28]
A water-floating pesticide formulation was prepared in accordance with Example 35 using the formulation composition of 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 48.0 parts of perlite, and 9.0 parts of clay (of which the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), with a particle size of 1.7 mm and sieves of 2.00 mm and 0.85 mm. The particle size of the obtained preparation was 10% in the range of 2.80 to 1.70 mm (the remainder was 90% below the particle size of 1.70 mm), the long axis/short axis ratio at the base was 1.0, and the number of particles per gram was 354, indicating that the preparation was composed of many small particles below 1.70 mm.

[Comparative Example 29]
A water-floating pesticide formulation was prepared in accordance with Example 35 with a formulation composition of 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 2.0 parts of sodium carboxymethylcellulose, 51.0 parts of perlite, and 6.0 parts of clay (of which the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), with a particle size of 4.0 mm and sieves of 4.76 mm and 2.36 mm. The particle size of the obtained preparation was 38% in the range of 2.80 to 1.70 mm (the remainder was 62% above 2.80 mm), the long axis/short axis ratio at the base was 1.2, and the number of particles per gram was 41, indicating that the preparation contained a large number of particles larger than 2.80 mm.

[Comparative Example 30]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalene sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium carboxymethylcellulose, 49.0 parts of perlite, 7.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 parts of sodium alkylnaphthalene sulfonate, and 14.0 parts of water), with a particle size of 3.0 mm. The formulation was not sized using a drum sizing machine, and the formulation was dried in a state where the cross section was a perfect circle to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.0, and the number of particles per gram was 98.

[Comparative Example 31]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium carboxymethylcellulose, 52.0 parts of perlite, 7.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), with a particle size of 3.0 mm. The particles were sized using a drum sizing machine, and further sized by pounding up and down in a plastic bag, which was then dried to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.6, and the number of particles per gram was 89.

[Comparative Example 32]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalene sulfonate, 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium carboxymethylcellulose, 49.0 parts of perlite, 7.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalene sulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. The particles were sized using a drum sizing machine, and further sized by pounding up and down in a plastic bag, which was then dried to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.8, and the number of particles per gram was 83.

[Comparative Example 33]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 65.0 parts of perlite, 17.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), with a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the resulting formulation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per gram was 96.

[Comparative Example 34]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 30.0 parts of perlite, 51.0 parts of clay (of which the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), with a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the resulting formulation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per gram was 33.

[Comparative Example 35]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium carboxymethylcellulose, 50.0 parts of perlite, 9.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of partially desulfonated sodium lignin sulfonate, and 14.0 parts of water), with a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 105.

[Comparative Example 36]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium alkyl sulfate, 2.0 parts of sodium carboxymethylcellulose, 48.0 parts of perlite, 9.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of partially desulfonated sodium lignin sulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 90.

[Comparative Example 37]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium alkylbenzene sulfonate, 3.0 parts of sodium carboxymethylcellulose, 51.0 parts of perlite, 5.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of partially desulfonated sodium lignin sulfonate, 14.0 parts of water), and a particle size of 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 82% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 110.

[Comparative Example 38]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of polyoxyethylene alkyl ether, 3.0 parts of carboxymethylcellulose Na, 49.0 parts of perlite, 7.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of polyoxyethylene alkyl ether, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 87% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 99.

[Comparative Example 39]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of polyoxyethylene arylphenyl ether, 2.0 parts of carboxymethylcellulose Na, 54.0 parts of perlite, 6.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of polyoxyethylene arylphenyl ether, and 14.0 parts of water), with a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 35. The particle size of the resulting formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 86.

[Comparative Example 40]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium carboxymethylcellulose, 51.0 parts of perlite, 6.0 parts of clay, 3.0 mm particle size, 3.35 mm and 0.85 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 55% in the range of 2.80-1.70 mm (the remainder was 45% below the particle size of 1.70 mm), the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 203, so that a formulation with many particles smaller than 1.70 mm in particle size was prepared.

[Comparative Example 41]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 47.0 parts of perlite, 8.0 parts of clay, 1.7 mm particle size, 2.00 mm and 0.85 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 8% in the range of 2.80-1.70 mm (the remainder was 92% below the particle size of 1.70 mm), the major axis/minor axis ratio at the bottom was 1.0, and the number of particles per 1 g was 236, and a formulation with many small particles of 1.70 mm or less was prepared.

[Comparative Example 42]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 3.0 parts of sodium carboxymethylcellulose, 49.0 parts of perlite, 5.0 parts of clay, 4.0 mm particle size, 4.76 mm and 2.36 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 18% in the range of 2.80-1.70 mm (the remainder was 82% above 2.80 mm), the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 43, so a formulation with many particles larger than 2.80 mm was prepared.

[Comparative Example 43]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 49.0 parts of perlite, 6.0 parts of clay, and 3.0 mm particle size. The formulation was not sized using a drum sizing machine, and the cross section was dried in a circular shape to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.0, and the number of particles per gram was 90.

[Comparative Example 44]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium carboxymethylcellulose, 51.0 parts of perlite, 6.0 parts of clay, and a particle size of 3.0 mm. The product was sized in a drum sizing machine and further sized by pounding up and down in a plastic bag, and then dried to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.6, and the number of particles per gram was 84.

[Comparative Example 45]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of shiras balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 47.0 parts of perlite, 7.0 parts of clay, and a particle size of 3.0 mm. The product was sized in a drum granulator and further sized by pounding up and down in a plastic bag, and then dried to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.8, and the number of particles per gram was 95.

[Comparative Example 46]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 68.0 parts of perlite, 12.0 parts of clay, and a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per gram was 99.

[Comparative Example 47]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 25.0 parts of perlite, 55.0 parts of clay, and 3.0 mm particle size, and a water-floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 82% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 31.

[Comparative Example 48]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 49.0 parts of perlite, 8.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 86% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 98.

[Comparative Example 49]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium alkyl sulfate, 3.0 parts of sodium carboxymethylcellulose, 48.0 parts of perlite, 6.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per gram was 107.

[Comparative Example 50]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium lignin sulfonate, 3.0 parts of sodium alkylbenzene sulfonate, 3.0 parts of sodium carboxymethylcellulose, 48.0 parts of perlite, 6.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 110.

[Comparative Example 51]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of polyoxyethylene alkyl ether, 2.0 parts of carboxymethylcellulose Na, 47.0 parts of perlite, 8.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per gram was 106.

[Comparative Example 52]
The formulation composition was 12.0 parts of simetryn (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of polyoxyethylene arylphenyl ether, 2.0 parts of carboxymethylcellulose Na, 50.0 parts of perlite, 8.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 52. The particle size of the obtained formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 114.

[Comparative Example 53]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium carboxymethylcellulose, 46.0 parts of perlite, 6.0 parts of clay, 3.0 mm particle size, and 3.35 mm and 0.85 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 63% in the range of 2.80-1.70 mm (the remainder was 37% below the particle size of 1.70 mm), the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 188, so that a formulation with many particles smaller than 1.70 mm in particle size was prepared.

[Comparative Example 54]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 40.0 parts of perlite, 8.0 parts of clay, 1.7 mm particle size, 2.00 mm and 0.85 mm sieves for sieving, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 5% in the range of 2.80-1.70 mm (the remainder was 95% below the particle size of 1.70 mm), the major axis/minor axis ratio at the bottom was 1.0, and the number of particles per 1 g was 313, so a formulation with many small particles of 1.70 mm or less was prepared.

[Comparative Example 55]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shiras balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 3.0 parts of sodium carboxymethylcellulose, 40.0 parts of perlite, 8.0 parts of clay, particle size 4.0 mm, sieves for sieving were 4.76 mm and 2.36 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 13% in the range of 2.80-1.70 mm (the remainder was 87% above 2.80 mm), the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 39, so a formulation with many particles larger than 2.80 mm was prepared.

[Comparative Example 56]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shiras balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 38.0 parts of perlite, 10.0 parts of clay, and a particle size of 3.0 mm. The formulation was not sized using a drum sieving machine, and the cross section was dried in a circular shape to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 82% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.0, and the number of particles per gram was 108.

[Comparative Example 57]
The formulation consisted of 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium carboxymethylcellulose, 45.0 parts of perlite, 7.0 parts of clay, and a particle size of 3.0 mm. The product was sized in a drum sieving machine and further sized by pounding up and down in a plastic bag, and then dried to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 82% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.6, and the number of particles per gram was 98.

[Comparative Example 58]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shiras balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 39.0 parts of perlite, 10.0 parts of clay, and a particle size of 3.0 mm. The product was sized in a drum granulator and further sized by pounding up and down in a plastic bag, and then dried to prepare a water-floating pesticide formulation. The particle size of the resulting formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.8, and the number of particles per gram was 93.

[Comparative Example 59]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 67.0 parts of perlite, 7.0 parts of clay, and a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per gram was 102.

[Comparative Example 60]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 3.0 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of partially desulfonated sodium ligninsulfonate, 2.0 parts of sodium carboxymethylcellulose, 19.0 parts of perlite, 55.0 parts of clay, and a particle size of 3.0 mm, and a water-floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per gram was 35.

[Comparative Example 61]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium carboxymethylcellulose, 42.0 parts of perlite, 9.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 35. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 96.

[Comparative Example 62]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium alkyl sulfate, 3.0 parts of sodium carboxymethylcellulose, 41.0 parts of perlite, 7.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 85% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 93.

[Comparative Example 63]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of partially desulfonated sodium ligninsulfonate, 3.0 parts of sodium alkylbenzenesulfonate, 2.0 parts of sodium carboxymethylcellulose, 43.0 parts of perlite, 6.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 84% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per gram was 83.

[Comparative Example 64]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of polyoxyethylene alkyl ether, 2.0 parts of carboxymethylcellulose Na, 42.0 parts of perlite, 7.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 82% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per gram was 78.

[Comparative Example 65]
The formulation composition was 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of polyoxyethylene arylphenyl ether, 3.0 parts of carboxymethylcellulose Na, 43.0 parts of perlite, 8.0 parts of clay, and 3.0 mm particle size, and a water surface floating pesticide formulation was prepared in accordance with Example 69. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per gram was 88.

[Example 86]
24.0 parts of kasugamycin (bactericidal active ingredient), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: n-octyl, ester bond number: 1, cation: Na ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of methylcellulose, 25.0 parts of perlite, and 8.5 parts of clay were pulverized and mixed with a hammer mill (Sample Mill KIIW-1, Dalton Co., Ltd.) to obtain a powder mixture. The obtained powder mixture and 25.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier) were mixed with a twin-arm kneader (KDHJ, Dalton Co., Ltd.) for 10 minutes, then water was added and kneaded for 15 minutes. Next, this water-kneaded mixture was granulated with an extrusion granulator equipped with a basket-type screen with a hole diameter of 3.0 mm. The obtained granules were pre-dried, sized with a drum-type sieving machine, and dried with a fluidized bed dryer. The resulting product was sieved through a 3.35-2.00 mm sieve to obtain a water-floating pesticide formulation. The particle size of the resulting formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 113.

[Example 87]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 28.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-octyl, ester bond number: 2, cation: Na ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of alkylnaphthalene sulfonate Na, 2.0 parts of acrylic acid-vinyl sulfonic acid copolymer Na, 6.0 parts of dextrin, 20.0 parts of white carbon, 11.5 parts of bentonite, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained formulation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 103.

[Example 88]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 6.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 1.5 parts of propylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 2.0 parts of polyacrylic acid Na, 3.0 parts of methylcellulose, 25.0 parts of perlite, 11.0 parts of bentonite, and a particle size of 3.0 mm. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained formulation was 85% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.6, and the number of particles per 1 g was 175.

[Example 89]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 2.5 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 12.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ⁺ ), 3.0 parts of propylene glycol, 2.5 parts of Na alkylnaphthalenesulfonate, 3.0 parts of methylcellulose, 30.0 parts of white carbon, 23.0 parts of bentonite, and a water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained formulation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.5, and the number of particles per 1 g was 132.

[Example 90]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-decyl, ester bond number: 1, cation: H ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 2.0 parts of polyacrylic acid Na, 6.0 parts of dextrin, 20.0 parts of perlite, 8.5 parts of bentonite, and a particle size of 3.0 mm. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained formulation was 85% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 115.

[Example 91]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 2.5 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-decyl, ester bond number: 2, cation: H ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of alkylnaphthalene sulfonate Na, 2.0 parts of acrylic acid-vinyl sulfonic acid copolymer Na, 6.0 parts of dextrin, 30.0 parts of white carbon, 23.0 parts of bentonite, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained formulation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 102.

[Example 92]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 8.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: isodecyl, ester bond number: 1, cation: K ⁺ ), 2.5 parts of butylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 2.0 parts of acrylic acid-vinyl sulfonic acid copolymer Na, 6.0 parts of dextrin, 17.0 parts of perlite, 13.0 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained formulation was 82% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 59.

[Example 93]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 28.0 parts of shirasubaroon (average particle size 70-90 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: isodecyl, ester bond number: 2, cation: K ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of alkylnaphthalenesulfonic acid Na, 2.0 parts of acrylic acid-vinylsulfonic acid copolymer Na, 3.0 parts of methylcellulose, 18.0 parts of white carbon, 10.5 parts of bentonite, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained formulation was 87% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 121.

[Example 94]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalene sulfonate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 3.0 parts of methylcellulose, 20.0 parts of diatomaceous earth, 11.0 parts of clay, and 3.0 mm of particle size. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained preparation was 82% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.5, and the number of particles per gram was 135.

[Example 95]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: n-octyl, ester bond number: 1, cation: Na ⁺ ), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: isodecyl, ester bond number: 2, cation: K ^{+ ).} A water-floating pesticide formulation was prepared in accordance with Example 86 using 4.0 parts of propylene glycol, 2.0 parts of sodium alkylnaphthalenesulfonate, 2.5 parts of sodium polyacrylate, 3.0 parts of methylcellulose, 20.0 parts of perlite, 8.5 parts of clay, and a particle size of 3.0 mm. The particle size of the resulting formulation was 82% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per gram was 127.

[Example 96]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 6.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-octyl, ester bond number: 2, cation: Na ⁺ ), 6.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalene sulfonate, 2.0 parts of sodium acrylic acid-vinyl sulfonic acid copolymer, 6.0 parts of dextrin, 20.0 parts of perlite, 6.0 parts of bentonite, and 3.0 mm particle size. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained preparation was 94% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 161.

[Example 97]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 28.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-decyl, ester bond number: 2, cation: H ⁺ ), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: isodecyl, ester bond number: 1, cation: K ⁺ ), 1.5 parts of propylene glycol, 2.5 parts of sodium dialkyl succinate sulfonate, 2.5 parts of sodium polyacrylate, 3.0 parts of methylcellulose, 18.0 parts of diatomaceous earth, 10.5 parts of bentonite, and 3.0 mm particle size. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained preparation was 82% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 115.

[Example 98]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 8.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-decyl, ester bond number: 1, cation: H ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 2.0 parts of acrylic acid-vinyl sulfonic acid copolymer Na, 3.0 parts of methylcellulose, 25.0 parts of perlite, 8.5 parts of bentonite, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained formulation was 92% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 105.

[Example 99]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: isodecyl, ester bond number: 1, cation: K ⁺ ), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: isodecyl, ester bond number: 2, cation: K ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalenesulfonate, 5.0 parts of sodium naphthalenesulfonate formaldehyde condensate, 3.0 parts of sodium polyacrylate, 6.0 parts of dextrin, 20.0 parts of diatomaceous earth, 4.0 parts of clay, and 3.0 mm of particle size. A water-floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained preparation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 183.

[Example 100]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 28.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: isodecyl, ester bond number: 1, cation: K ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 2.0 parts of acrylic acid-maleic acid copolymer Na, 6.0 parts of dextrin, 17.0 parts of perlite, 5.5 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained formulation was 94% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 127.

[Example 101]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 6.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-octyl, ester bond number: 2, cation: Na ⁺ ), 6.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-decyl, ester bond number: 2, cation: H ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 3.0 parts of sodium carboxymethyl cellulose, 20.0 parts of diatomaceous earth, 9.0 parts of bentonite, and 2.8 mm particle size. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained preparation was 82% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 118.

[Example 102]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ⁺ ), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-decyl, ester bond number: 1, cation: H ⁺ ), 3.0 parts of propylene glycol, 3.0 parts of sodium ligninsulfonate, 2.0 parts of sodium polyacrylate, 3.0 parts of polyvinyl alcohol, 20.0 parts of perlite, 9.5 parts of clay, and 3.0 mm of particle size. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained preparation was 96% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 116.

[Example 103]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-octyl, ester bond number: 2, cation: Na ⁺ ), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-decyl, ester bond number: 2, cation: H ⁺ ), 2.5 parts of sodium alkyl naphthalene sulfonate, 3.0 parts of sodium alkyl naphthalene sulfonate formaldehyde condensate, 2.0 parts of sodium polyacrylate, 3.0 parts of sodium carboxymethylcellulose, 12.5 parts of diatomaceous earth, 18.0 parts of bentonite, and 3.0 mm of particle size. A water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained preparation was 94% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 61.

[Example 104]
The formulation composition was 24.0 parts of kasugamycin (bactericidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of propylene glycol, 2.5 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of naphthalenesulfonic acid formaldehyde condensate Na, 2.0 parts of acrylic acid-vinylsulfonic acid copolymer Na, 3.0 parts of carboxymethylcellulose Na, 25.0 parts of diatomaceous earth, 12.5 parts of bentonite, and a particle size of 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 86. The particle size of the obtained formulation was 92% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 105.

[Example 105]
12.0 parts of pymetrozine (insecticidal active ingredient), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: n-octyl, ester bond number: 1, cation: Na ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of alkylnaphthalenesulfonic acid Na, 6.0 parts of dextrin, 27.0 parts of perlite, and 15.0 parts of bentonite were pulverized and mixed with a hammer mill (Sample Mill KIIW-1, Dalton Co., Ltd.) to obtain a powder mixture. The obtained powder mixture and 25.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier) were mixed with a twin-arm kneader (KDHJ, Dalton Co., Ltd.) for 10 minutes, then water was added and kneaded for 15 minutes. Next, this water-kneaded mixture was granulated with an extrusion granulator equipped with a basket-type screen with a hole diameter of 2.8 mm. The obtained granules were pre-dried, sized using a drum-type sieving machine, and dried using a fluidized bed dryer. The granules were sieved at 3.35 mm to 2.00 mm to obtain a water-floating pesticide formulation. The particle size of the obtained formulation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 138.

[Example 106]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 4.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 4, alkyl group: n-octyl, ester bond number: 2, cation: Na ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 1.5 parts of acrylic acid-vinyl sulfonic acid copolymer Na, 6.0 parts of dextrin, 28.0 parts of diatomaceous earth, 19.0 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 87% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 105.

[Example 107]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 6.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 2.0 parts of acrylic acid-vinyl sulfonic acid copolymer Na, 3.0 parts of methylcellulose, 25.0 parts of diatomaceous earth, 17.5 parts of bentonite, and a water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 85% in the range of 2.80 to 1.70 mm, the major axis / minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 182.

[Example 108]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 12.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ⁺ ), 2.5 parts of hexylene glycol, 2.5 parts of alkyl naphthalene sulfonate Na, 7.0 parts of dextrin, 17.0 parts of white carbon, 17.0 parts of bentonite, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 83% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 159.

[Example 109]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: n-decyl, ester bond number: 1, cation: H ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of alkylnaphthalene sulfonate Na, 2.0 parts of acrylic acid-methacrylic acid copolymer Na, 3.0 parts of methylcellulose, 25.0 parts of perlite, 18.5 parts of clay, and a particle size of 3.0 mm. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 108.

[Example 110]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 2.5 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-decyl, ester bond number: 2, cation: H ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 6.0 parts of dextrin, 35.0 parts of diatomaceous earth, 29.5 parts of bentonite, and the particle size was 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 85% in the range of 2.80 to 1.70 mm, the major axis / minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 125.

[Example 111]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: isodecyl, ester bond number: 1, cation: K ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of alkylnaphthalene sulfonate Na, 2.0 parts of acrylic acid-methacrylic acid copolymer Na, 3.0 parts of methylcellulose, 23.0 parts of white carbon, 15.0 parts of clay, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 113.

[Example 112]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: isodecyl, ester bond number: 2, cation: K ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 1.0 parts of polyacrylic acid Na, 3.0 parts of methylcellulose, 25.0 parts of diatomaceous earth, 19.5 parts of clay, and a particle size of 3.0 mm. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 87% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 113.

[Example 113]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of sodium alkyl naphthalene sulfonate, 3.0 parts of sodium acrylic acid-methacrylic acid copolymer, 3.0 parts of methylcellulose, 25.0 parts of diatomaceous earth, 17.0 parts of clay, and 3.0 mm of particle size. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained preparation was 85% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.1, and the number of particles per gram was 124.

[Example 114]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 30.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: n-octyl, ester bond number: 1, cation: Na ⁺ ), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalene sulfonate, 3.0 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of methylcellulose, 23.0 parts of white carbon, 17.5 parts of bentonite, and 3.0 mm of particle size. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained preparation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.6, and the number of particles per gram was 105.

[Example 115]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 2.5 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 6.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-octyl, ester bond number: 2, cation: Na ⁺ ), 6.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 3.0 parts of propylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 1.5 parts of acrylic acid-vinyl sulfonic acid copolymer Na, 6.0 parts of dextrin, 30.0 parts of perlite, 30.5 parts of bentonite, and 2.8 mm of particle size. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained preparation was 94% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 95.

[Example 116]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 28.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-decyl, ester bond number: 2, cation: H ⁺ ), 1.5 parts of propylene glycol, 2.5 parts of Na alkylnaphthalene sulfonate, 2.0 parts of Na polyacrylate, 3.0 parts of methylcellulose, 22.0 parts of diatomaceous earth, 19.0 parts of bentonite, and a water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 83% in the range of 2.80 to 1.70 mm, the major axis / minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 93.

[Example 117]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 28.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-octyl, ester bond number: 2, cation: Na ⁺ ), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ⁺ ), 1.5 parts of propylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 2.0 parts of acrylic acid-vinyl sulfonic acid copolymer Na, 3.0 parts of methylcellulose, 22.0 parts of diatomaceous earth, 21.0 parts of clay, and 3.0 mm of particle size. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained preparation was 97% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 109.

[Example 118]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 12.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-decyl, ester bond number: 2, cation: H ⁺ ), 3.0 parts of propylene glycol, 2.5 parts of alkyl naphthalene sulfonate Na, 3.0 parts of alkyl naphthalene sulfonate formaldehyde condensate Na, 3.0 parts of polyacrylic acid Na, 6.0 parts of dextrin, 25.0 parts of perlite, 8.5 parts of bentonite, and a particle size of 2.8 mm. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 82% in the range of 2.80-1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 111.

[Example 119]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: n-decyl, ester bond number: 1, cation: H ⁺ ), 1.5 parts of propylene glycol, 2.5 parts of alkylnaphthalenesulfonic acid Na, 3.0 parts of naphthalenesulfonic acid formaldehyde condensate Na, 2.5 parts of acrylic acid-methacrylic acid copolymer Na, 3.0 parts of methylcellulose, 25.0 parts of perlite, 15.5 parts of clay, and 3.0 mm of particle size. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained preparation was 96% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.1, and the number of particles per gram was 128.

[Example 120]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: n-octyl, ester bond number: 1, cation: Na ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of dialkyl succinate sulfonic acid Na, 2.0 parts of acrylic acid-vinyl sulfonic acid copolymer Na, 2.0 parts of carboxymethyl cellulose Na, 25.0 parts of white carbon, 19.5 parts of bentonite, and a water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 85% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 110.

[Example 121]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-octyl, ester bond number: 2, cation: Na ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of alkylnaphthalenesulfonic acid Na, 2.5 parts of ligninsulfonic acid Na, 2.0 parts of polyacrylic acid Na, 2.0 parts of polyvinyl alcohol, 26.0 parts of perlite, 15.5 parts of bentonite, and a particle size of 2.8 mm was prepared according to Example 105. The particle size of the obtained formulation was 97% in the range of 2.80 to 1.70 mm, the major axis / minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 119.

[Example 122]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 2.5 parts of alkylnaphthalenesulfonic acid Na, 2.5 parts of alkylnaphthalenesulfonic acid formaldehyde condensate Na, 2.0 parts of polyacrylic acid Na, 3.0 parts of carboxymethylcellulose Na, 23.0 parts of perlite, 15.0 parts of bentonite, 5.0 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 93% in the range of 2.80 to 1.70 mm, the major axis / minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 102.

[Example 123]
The formulation composition was 12.0 parts of pymetrozine (insecticidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 3.0 parts of propylene glycol, 2.5 parts of alkylnaphthalenesulfonic acid Na, 2.5 parts of naphthalenesulfonic acid formaldehyde condensate Na, 3.0 parts of acrylic acid-vinylsulfonic acid copolymer Na, 3.0 parts of carboxymethylcellulose Na, 26.0 parts of perlite, 10.0 parts of bentonite, 13.0 parts of clay, and 3.0 mm in particle size. A water surface floating pesticide formulation was prepared in accordance with Example 105. The particle size of the obtained formulation was 91% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 79.

[Example 124]
10.0 parts of ipfencarbazone (herbicidal active ingredient), 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water were mixed and wet-ground in a Dyno Mill (manufactured by Shinmaru Enterprises) until the average particle size reached 1.0 μm to obtain a slurry. Also, 8.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-octyl, ester bond number: 1, cation: H ⁺ ), 2.0 parts of propylene glycol, 1.5 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of methylcellulose, 29.0 parts of perlite, and 17.5 parts of bentonite were ground and mixed in a hammer mill (Sample Mill KIIW-1, manufactured by Dalton Co.) to obtain a powder mixture. The slurry, powder mixture, and 28.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier) were mixed for 10 minutes in a twin-arm kneader (KDHJ, Dalton Co., Ltd.), then water was added and kneaded for 15 minutes. Next, this water-kneaded mixture was granulated in an extrusion granulator equipped with a basket-type screen with a hole diameter of 3.0 mm. The obtained granulated product was pre-dried, sized in a drum-type granulator, and dried in a fluidized bed dryer. This was sieved at 3.35 mm to 2.00 mm to obtain a water-floating pesticide formulation. The particle size of the obtained formulation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 132.

[Example 125]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of ceramic balloons (average particle size 20-150 μm) (floating carrier), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-octyl, ester bond number: 2, cation: H ⁺ ), 1.5 parts of propylene glycol, 2.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 6.0 parts of dextrin, 30.0 parts of perlite, 19.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water), with a particle size of 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 102.

[Example 126]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 30.0 parts of fly ash balloons (average particle size 20-150 μm) (floating carrier), 6.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 3.0 parts of propylene glycol, 2.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium acrylic acid-vinyl sulfonate copolymer, 3.0 parts of methylcellulose, 27.0 parts of perlite, 16.5 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 87% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.4, and the number of particles per gram was 105.

[Example 127]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 2.5 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalene sulfonate, 2.0 parts of sodium acrylic acid-vinyl sulfonate copolymer, 3.0 parts of methylcellulose, 40.0 parts of perlite, 30.0 parts of bentonite (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalene sulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 118.

[Example 128]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of ceramic balloons (average particle size 20-150 μm) (floating carrier), 8.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-decyl, ester bond number: 1, cation: Na ⁺ ), 2.0 parts of butylene glycol, 2.5 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium acrylic acid-maleic acid copolymer, 6.0 parts of dextrin, 26.0 parts of diatomaceous earth, 18.5 parts of bentonite (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 99.

[Example 129]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 30.0 parts of fly ash balloons (average particle size 80-120 μm) (floating carrier), 12.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-decyl, ester bond number: 2, cation: Na ⁺ ), 3.0 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of methylcellulose, 26.0 parts of diatomaceous earth, 13.5 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 87% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.5, and the number of particles per gram was 143.

[Example 130]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of shirasubaroon (average particle size 70-90 μm) (floating carrier), 12.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: isodecyl, ester bond number: 1, cation: K ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium polyacrylate, 6.0 parts of dextrin, 25.0 parts of white carbon, 15.0 parts of bentonite (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water), with a particle size of 2.8 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 85% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 85.

[Example 131]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of fly ash balloons (average particle size 80-120 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: isodecyl, ester bond number: 2, cation: K ⁺ ), 3.0 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 6.0 parts of dextrin, 25.0 parts of diatomaceous earth, 16.5 parts of bentonite (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), with a particle size of 2.8 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.6, and the number of particles per gram was 180.

[Example 132]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 6.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 1.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ^{+ ).} ) 6.0 parts, propylene glycol 2.5 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, acrylic acid-vinylsulfonic acid copolymer Na 2.0 parts, methylcellulose 3.0 parts, perlite 25.0 parts, clay 18.0 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 parts, water 14.0 parts), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained formulation was 82% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 103.

[Example 133]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of ceramic balloons (average particle size 20-150 μm) (floating carrier), 3.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-octyl, ester bond number: 1, cation: H ⁺ ), 3.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 3.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: isodecyl, ester bond number: 2, cation: K ^{+ ).} ) 3.0 parts, propylene glycol 3.0 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, acrylic acid-methacrylic acid copolymer Na 2.5 parts, methylcellulose 3.0 parts, white carbon 25.0 parts, bentonite 20.0 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 parts, water 14.0 parts), particle size 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained formulation was 82% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 93.

[Example 134]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of ceramic balloons (average particle size 20-150 μm) (floating carrier), 8.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-decyl, ester bond number: 1, cation: Na ⁺ ), 1.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: n-decyl, ester bond number: 2, cation: Na ^{+ ).} ) 4.0 parts, propylene glycol 2.0 parts, dialkyl succinate sulfonic acid Na 2.5 parts, polyacrylic acid Na 2.0 parts, dextrin 6.0 parts, perlite 25.0 parts, clay 15.5 parts (the composition used for the slurry was ipfencarbazone 10.0 parts, dialkyl succinate sulfonic acid Na 1.0 part, water 14.0 parts), and the particle size was 2.8 mm, and a water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained formulation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 108.

[Example 135]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: isodecyl, ester bond number: 1, cation: K ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalenesulfonate, 2.0 parts of sodium acrylic acid-maleic acid copolymer, 6.0 parts of dextrin, 25.0 parts of diatomaceous earth, 17.5 parts of bentonite (of which the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), with a particle size of 2.8 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.4, and the number of particles per gram was 117.

[Example 136]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 30.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 8.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: isodecyl, ester bond number: 2, cation: K ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium polyacrylate, 6.0 parts of dextrin, 23.0 parts of perlite, 16.5 parts of clay (of which the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water), with a particle size of 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 96% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 116.

[Example 137]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of ceramic balloons (average particle size 20-150 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium alkylnaphthalenesulfonate formaldehyde condensate, 2.0 parts of sodium acrylic acid-vinylsulfonic acid copolymer, 3.0 parts of methylcellulose, 25.0 parts of perlite, 17.5 parts of bentonite (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.1, and the number of particles per gram was 108.

[Example 138]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 6.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-octyl, ester bond number: 1, cation: H ⁺ ), 1.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ^{+ ).} ) 6.0 parts, propylene glycol 2.5 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, naphthalenesulfonic acid formaldehyde condensate Na 3.0 parts, acrylic acid-methacrylic acid copolymer Na 2.5 parts, dextrin 6.0 parts, diatomaceous earth 25.0 parts, clay 11.5 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 parts, water 14.0 parts), particle size 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained formulation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 156.

[Example 139]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 70-90 μm) (floating carrier), 5.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 1.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: Na ^{+ ).} ) 5.0 parts, propylene glycol 2.5 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, acrylic acid-vinylsulfonic acid copolymer Na 2.0 parts, polyvinyl alcohol 3.0 parts, white carbon 25.0 parts, bentonite 20.0 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 parts, water 14.0 parts), particle size 2.8 mm, and a water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained formulation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.5, and the number of particles per 1 g was 178.

[Example 140]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 7.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 4, alkyl group: n-decyl, ester bond number: 1, cation: Na ⁺ ), 1.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 4, alkyl group: n-decyl, ester bond number: 2, cation: Na ^{+ ).} ) 3.0 parts, propylene glycol 2.5 parts, dialkyl succinate sulfonic acid Na 2.5 parts, lignin sulfonic acid Na 3.0 parts, acrylic acid-maleic acid copolymer Na 1.5 parts, carboxymethyl cellulose Na 2.0 parts, diatomaceous earth 25.0 parts, bentonite 18.5 parts (the composition used in the slurry is ipfencarbazone 10.0 parts, dialkyl succinate sulfonic acid Na 1.0 parts, water 14.0 parts), the particle size was 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained formulation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 125.

[Example 141]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of shirasubaroon (average particle size 90-120 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: Na ⁺ ), 2.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium alkyl naphthalene sulfonate formaldehyde condensate, 1.5 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of sodium carboxymethyl cellulose, 22.0 parts of diatomaceous earth, 23.0 parts of bentonite (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 124. The particle size of the obtained preparation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 58.

[Example 142]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90 to 120 μm) (floating carrier), 2.5 parts of propylene glycol, 2.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of sodium alkyl naphthalene sulfonate formaldehyde condensate, 2.0 parts of sodium acrylic acid-vinyl sulfonic acid copolymer,
A water-floating pesticide formulation was prepared in accordance with Example 124 using 3.0 parts of carboxymethylcellulose Na, 35.0 parts of diatomaceous earth, 17.0 parts of bentonite (of which the composition used in the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water) with a particle size of 3.0 mm. The particle size of the resulting formulation was 91% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per gram was 112.

[Example 143]
10.0 parts of ipfencarbazone (herbicidal active ingredient), 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water were mixed and wet-milled in a Dyno Mill (manufactured by Shinmaru Enterprises) until the average particle size reached 1.0 μm to obtain a slurry. In addition, 18.0 parts of benfuresate (herbicidal active ingredient), 12.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-octyl, ester bond number: 1, cation: Na ⁺ ), 2.5 parts of propylene glycol, 1.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of methylcellulose, 18.0 parts of white carbon, and 9.0 parts of bentonite were pulverized and mixed in a hammer mill (Sample Mill KIIW-1, manufactured by Dalton Co.) to obtain a powder mixture. The slurry, powder mixture, and 25.0 parts of fly ash balloons (average particle size 80-120 μm) (floating carrier) were mixed in a twin-arm kneader (KDHJ, Dalton) for 10 minutes, then water was added and kneaded for 15 minutes. Next, this water-kneaded mixture was granulated in an extrusion granulator equipped with a basket-type screen with a hole diameter of 3.0 mm. The obtained granules were pre-dried, sized in a drum-type granulator, and dried in a fluidized bed dryer. The granules were sieved at 3.35 mm to 2.00 mm to obtain a water-floating pesticide formulation. The particle size of the obtained formulation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 78.

[Example 144]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 28.0 parts of shirasubaroon (average particle size 70-90 μm) (floating carrier), 6.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-octyl, ester bond number: 2, cation: Na ⁺ ), 2.0 parts of hexylene glycol, 2.5 parts of sodium alkylnaphthalene sulfonate, 2.0 parts of sodium polyacrylate, 6.0 parts of dextrin, 15.0 parts of calcium silicate, 10.5 parts of bentonite (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalene sulfonate, and 14.0 parts of water), with a particle size of 2.8 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained preparation was 87% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 89.

[Example 145]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 28.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 6.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: K ⁺ ), 3.0 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalene sulfonate, 1.5 parts of sodium acrylic acid-vinyl sulfonic acid copolymer, 6.0 parts of dextrin, 18.0 parts of calcium silicate, 7.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalene sulfonate, and 14.0 parts of water), and the particle size was 2.8 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained preparation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.5, and the number of particles per gram was 96.

[Example 146]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: K ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of sodium dialkyl succinate sulfonate, 3.0 parts of methylcellulose, 18.0 parts of white carbon, 11.5 parts of bentonite (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water), with a particle size of 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained preparation was 85% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 105.

[Example 147]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 28.0 parts of ceramic balloon (average particle size 20-150 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-decyl, ester bond number: 1, cation: Na ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of sodium dialkyl succinate sulfonate, 1.0 part of acrylic acid-vinyl sulfonic acid copolymer Na, 3.0 parts of methylcellulose, 18.0 parts of white carbon, 7.5 parts of bentonite (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained preparation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.4, and the number of particles per gram was 118.

[Example 148]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasubaroon (average particle size 70-90 μm) (floating carrier), 12.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-decyl, ester bond number: 2, cation: Na ⁺ ), 2.5 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of methylcellulose, 20.0 parts of calcium silicate, 7.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained preparation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.2, and the number of particles per gram was 93.

[Example 149]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 12.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 3, 4, alkyl group: isodecyl, ester bond number: 1, cation: H ⁺ ), 3.0 parts of propylene glycol, 2.5 parts of sodium dialkyl succinate sulfonate, 2.0 parts of sodium acrylic acid-maleic acid copolymer, 3.0 parts of methylcellulose, 18.0 parts of white carbon, 6.5 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium dialkyl succinate sulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained preparation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 82.

[Example 150]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 2.5 parts of acrylonitrile resin balloon (average particle size 20-40 μm) (floating carrier), 12.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: isodecyl, ester bond number: 2, cation: H ⁺ ), 2.0 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalene sulfonate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 6.0 parts of dextrin, 20.0 parts of calcium silicate, 25.0 parts of bentonite (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalene sulfonate, and 14.0 parts of water), with a particle size of 2.8 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained preparation was 85% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.4, and the number of particles per gram was 73.

[Example 151]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20 to 150 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: K ⁺ ), 10.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, alkyl group: 2-ethylhexyl, ester bond number: 2, cation: K ^{+ )} . ) 2.0 parts, propylene glycol 2.0 parts, dialkyl succinate sulfonic acid Na 2.5 parts, acrylic acid-vinyl sulfonic acid copolymer Na 1.5 parts, methylcellulose 3.0 parts, white carbon 18.0 parts, bentonite 8.0 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, dialkyl succinate sulfonic acid Na 1.0 parts, water 14.0 parts), and the particle size was 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained formulation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 75.

[Example 152]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of ceramic balloon (average particle size 20 to 150 μm) (floating carrier), 3.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, alkyl group: n-octyl, ester bond number: 1, cation: Na ⁺ ), 3.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: K ⁺ ), 3.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: isodecyl, ester bond number: 2, cation: H ^{+ ).} ) 3.0 parts, propylene glycol 3.0 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, acrylic acid-maleic acid copolymer Na 1.0 part, methylcellulose 3.0 parts, white carbon 18.0 parts, bentonite 10.5 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 part, water 14.0 parts), particle size 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained formulation was 82% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.6, and the number of particles per 1 g was 78.

[Example 153]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 10.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-octyl, ester bond number: 2, cation: Na ⁺ ), 1.5 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalene sulfonate, 2.0 parts of sodium polyacrylate, 6.0 parts of dextrin, 18.0 parts of white carbon, 7.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalene sulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained preparation was 93% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.1, and the number of particles per gram was 83.

[Example 154]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 28.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: K ⁺ ), 4.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-decyl, ester bond number: 2, cation: Na ^{+ )} . ) 6.0 parts, propylene glycol 1.5 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, acrylic acid-vinylsulfonic acid copolymer Na 2.0 parts, methylcellulose 3.0 parts, calcium silicate 18.0 parts, bentonite 7.0 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 parts, water 14.0 parts), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained formulation was 83% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 86.

[Example 155]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 5.0 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-octyl, ester bond number: 1, cation: Na ⁺ ), 2.5 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-decyl, ester bond number: 1, cation: Na ⁺ ), 1.5 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: isodecyl, ester bond number: 2, cation: H ^{+ )} , ) 2.5 parts, propylene glycol 2.0 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, polyacrylic acid Na 2.5 parts, methylcellulose 3.0 parts, calcium silicate 18.0 parts, clay 9.0 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 part, water 14.0 parts), and the particle size was 2.8 mm. A water-floating pesticide formulation was prepared according to Example 143. The particle size of the obtained formulation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.1, and the number of particles per 1 g was 85.

[Example 156]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 70 to 90 μm) (floating carrier), 25.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation: K ⁺ ) 10.0 parts, propylene glycol 2.5 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, naphthalenesulfonic acid formaldehyde condensate Na 3.0 parts, acrylic acid-maleic acid copolymer Na 1.5 parts, methylcellulose 3.0 parts, white carbon 18.0 parts, bentonite 6.5 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 parts, water 14.0 parts), particle size 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained formulation was 86% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 93.

[Example 157]
The formulation composition is 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 25.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-octyl, ester bond number: 2, cation Na ⁺ ) 8.0 parts, propylene glycol 3.0 parts, dialkyl succinate sulfonic acid Na 2.5 parts, alkyl naphthalene sulfonic acid formaldehyde condensate Na 3.0 parts, acrylic acid - methacrylic acid copolymer Na 1.0 parts, methyl cellulose 3.0 parts, white carbon 18.0 parts, bentonite 8.5 parts (the composition used in the slurry is ipfencarbazone 10.0 parts, dialkyl succinate sulfonic acid Na 1.0 parts, water 14.0 parts), the particle size was 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained formulation was 94% in the range of 2.80 to 1.70 mm, the major axis / minor axis ratio at the bottom was 1.3, and the number of particles per 1 g was 120.

[Example 158]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of fly ash balloon (average particle size 80-120 μm) (floating carrier), 5.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-octyl, ester bond number: 2, cation Na ⁺ ), 5.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 4, alkyl group: 2-ethylhexyl, ester bond number: 1, cation K ^{+ ).} ) 5.0 parts, propylene glycol 3.0 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, acrylic acid-vinylsulfonic acid copolymer Na 3.0 parts, polyvinyl alcohol 3.0 parts, white carbon 18.0 parts, clay 7.5 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 parts, water 14.0 parts), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained formulation was 84% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 100.

[Example 159]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 4.5 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, alkyl group: 2-ethylhexyl, ester bond number: 2, cation K ⁺ ), 4.5 parts of polyoxyalkylene alkyl ether phosphate salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-decyl, ester bond number: 1, cation Na ⁺ ). ) 4.5 parts, propylene glycol 2.0 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, ligninsulfonic acid Na 3.0 parts, acrylic acid-methacrylic acid copolymer Na 2.0 parts, carboxymethylcellulose Na 3.0 parts, white carbon 18.0 parts, bentonite 7.5 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 parts, water 14.0 parts), particle size 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained formulation was 97% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.2, and the number of particles per 1 g was 90.

[Example 160]
The formulation composition is 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of Shirasu balloon (average particle size 90-120 μm) (floating carrier), 25.0 parts of polyoxyalkylene alkyl ether phosphate ester salt (alkylene group: carbon number 2, 3, 4, alkyl group: n-decyl, ester bond number: 2, cation Na ⁺ ) 10.0 parts, alkylnaphthalenesulfonic acid Na 2.5 parts, naphthalenesulfonic acid formaldehyde condensate Na 3.0 parts, acrylic acid-vinylsulfonic acid copolymer Na 2.0 parts, carboxymethylcellulose Na 3.0 parts, white carbon 17.0 parts, bentonite 9.5 parts (the composition used in the slurry was ipfencarbazone 10.0 parts, alkylnaphthalenesulfonic acid Na 1.0 parts, water 14.0 parts), particle size 3.0 mm, and a water surface floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained formulation was 93% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the bottom was 1.4, and the number of particles per 1 g was 102.

[Example 161]
The formulation composition was 10.0 parts of ipfencarbazone (herbicidal active ingredient), 18.0 parts of benfuresate (herbicidal active ingredient), 25.0 parts of shirasuballoon (average particle size 90-120 μm) (floating carrier), 3.0 parts of propylene glycol, 2.5 parts of sodium alkylnaphthalenesulfonate, 3.0 parts of sodium naphthalenesulfonate formaldehyde condensate, 2.0 parts of sodium acrylic acid-methacrylic acid copolymer, 3.0 parts of sodium carboxymethylcellulose, 21.5 parts of white carbon, 12.0 parts of clay (the composition used for the slurry was 10.0 parts of ipfencarbazone, 1.0 part of sodium alkylnaphthalenesulfonate, and 14.0 parts of water), and the particle size was 3.0 mm. A water-floating pesticide formulation was prepared in accordance with Example 143. The particle size of the obtained preparation was 95% in the range of 2.80 to 1.70 mm, the major axis/minor axis ratio at the base was 1.3, and the number of particles per gram was 86.

（３）次いで、処理４８時間後に試験区の散布地点を起点とし、１ｍ間隔で２０ｍＬ採水
した採水液、および別途作成した１平方メートル（１ｍ×１ｍ、湛水深２ｃｍ）試験区に上記製剤試料０．２５ｇを均一散布したものの４８時間後の採水液中の有効成分濃度を高速液体クロマトグラフィー（ＨＰＬＣ）あるいはガスクロマトグラフィー（ＧＣ）などにより定量し（分解物が生成した場合には、分解物も定量し、農薬活性成分濃度に換算して合算する）、各地点における拡散率（％）を下記式（２）により算出した。

Next, the usefulness of the water-floating pesticide formulation of the present invention will be demonstrated by test examples.
<Diffusion test 1 (Confirmation of diffusion in shallow water and tailwind conditions)>
After rice transplantation, the paddy field was divided into sections with corrugated iron so that each section had an area of 100 square meters (4 m x 25 m, water depth of 2 cm). 25 g of samples prepared according to the examples and comparative examples were treated on one side of the 4 m side under a tailwind of 2 to 3 m/s, and the following three items were investigated.
(1) The longest visual distance the formulation reached 15 minutes after spraying. (2) The presence or absence of sediment at the spray point 15 minutes after spraying. Sediment was evaluated according to the following criteria table.

(3) Next, 48 hours after the treatment, 20 mL of water was collected at 1 m intervals starting from the spraying point in the test area, and 0.25 g of the above formulation sample was uniformly sprayed in a separately prepared test area of 1 square meter (1 m x 1 m, flooding depth 2 cm). The active ingredient concentration in the collected water was quantified by high performance liquid chromatography (HPLC) or gas chromatography (GC) or the like (if decomposition products were produced, they were also quantified and converted into the concentration of the pesticide active ingredient and added together), and the diffusion rate (%) at each point was calculated using the following formula (2).

The maximum distance at which the diffusion rate was 90% or more was taken as the diffusion distance, and diffusion was evaluated. This test was also carried out on products immediately after preparation and on products stored at 40°C for 90 days (equivalent to storage at room temperature for 3 years).

<Diffusion test 2 (diffusion confirmation in shallow water and no wind conditions)>
The area was divided into sections with corrugated iron so that each section had an area of 120 square meters (4 m x 30 m, water depth 2 cm). Under windless conditions, 30 g of sample prepared in accordance with the examples was treated on one side of the 4 m side, and the following three items were investigated.
(1) The longest distance the formulation reached visually 15 minutes after spraying. (2) The presence or absence of sediment at the spray point 15 minutes after spraying. Sediment was evaluated according to the above-mentioned criteria table.
(3) Next, 24 hours after the treatment, 20 mL of water was collected at 1.5 m intervals starting from the spraying point in the test area, and 0.25 g of the above formulation sample was uniformly sprayed in a separately prepared test area of 1 square meter (1 m x 1 m, water depth 2 cm). The active ingredient concentration in the collected water was quantified by high performance liquid chromatography (HPLC) or gas chromatography (GC) or the like (if decomposition products were produced, they were also quantified and converted into the concentration of the pesticide active ingredient and added together), and the diffusion rate (%) at each point was calculated using the above formula (2).

The maximum distance at which the diffusion rate was 90% or more was taken as the diffusion distance, and the diffusivity was evaluated. This test was also carried out on products immediately after preparation and on products stored at 40°C for 150 days (equivalent to storage at room temperature for 5 years).

As a result of the diffusibility test, a formulation can be evaluated as having excellent buoyancy and diffusibility when there is less sediment at the point of application, and when the distance the formulation reaches is long and the point where the diffusivity is 90% or more extends further.
The test results are shown in Tables 2-1 to 2-9 (Examples) and Tables 3-1 to 3-5 (Comparative Examples).

<Table explanation>
(1) Diffusion test 1 (Confirmation of diffusion in shallow water and tailwind conditions)
The sedimentation was affected by the floating carrier, sodium alkylnaphthalenesulfonate or sodium dialkylsuccinatesulfonate, particle size, major axis/minor axis ratio at the base of the particle, and number of particles per gram. In Tables 2-1 to 2-5, Examples 1 to 85, which satisfied all the requirements, had sedimentation, formulation reach, and diffusion distance within practically acceptable ranges. On the other hand, Comparative Examples, in which any of the components were omitted or replaced with alternatives, showed results in which sedimentation during preparation or after storage at 40°C for 90 days was problematic for practical use.
In each of the Examples, the formulations containing either alkylnaphthalenesulfonic acid formaldehyde condensate Na, naphthalenesulfonic acid formaldehyde condensate Na, or partially desulfonated ligninsulfonic acid Na were prevented from decreasing in performance (sediment, formulation reach distance, diffusion distance) after 90 days at 40° C. In addition, the formulations containing carboxymethylcellulose Na as a binder showed improved sedimentation and diffusion distance compared to the Examples using other binders. The overall diffusibility was evaluated for Examples 16, 17, 33, and 34, in which the floating carrier contained shirasu balloons having an average particle size of 90 to 120 μm, sodium alkylnaphthalenesulfonate or sodium dialkylsuccinatesulfonate, and either sodium alkylnaphthalenesulfonate formaldehyde condensate, sodium naphthalenesulfonate formaldehyde condensate, or sodium partially desulfonated ligninsulfonate, contained sodium carboxymethylcellulose as a binder, had a particle size of 2.80 mm to 1.70 mm in an amount of 90% by weight or more, had a major axis/minor axis ratio of the base surface of the particle of 1.1 to 1.4, and had a particle number of 50 to 150 per gram.
, 50, 51, 67, 68, 84, and 85 were the most excellent, including immediately after preparation and after 90 days at 40°C.

From the above, in order for a water-floating pesticide formulation to fully demonstrate diffusibility, which takes into account sediment, formulation reach, and diffusion distance, not only immediately after preparation but also after long-term storage, it is necessary that the pesticide active ingredient, floating carrier, sodium alkyl naphthalene sulfonate or sodium dialkyl succinate sulfonate, the particle size be in the range of 2.80 mm to 1.70 mm for 80% by weight or more, and the long axis/short axis ratio at the base of the particle be 1.
Effective means are that the particle size is 90% by weight or more in the range of 2.80 mm to 1.70 mm, the floating carrier is a shirasu balloon having an average particle size of 90 to 120 μm, the mixture contains any one of sodium alkylnaphthalenesulfonate formaldehyde condensate, sodium naphthalenesulfonate formaldehyde condensate, or sodium partially desulfonated ligninsulfonate, and contains sodium carboxymethylcellulose as a binder.

(2) Diffusion test 2 (diffusion confirmation in shallow water and no wind conditions)
Examples 86 to 102, 105 to 121, 124 to 140, and 143 to 159 containing a polyoxyalkylene alkyl ether phosphate salt and a water-soluble alkylene glycol such as propylene glycol showed better sedimentation, formulation reach distance, and diffusion distance at the time of preparation and after 150 days at 40°C, and thus improved diffusivity, as compared with Examples 16, 17, 33, 34, 50, 51, 67, 68, 84, 85, 103, 104, 122, 123, 141, 142, 160, and 161 not containing said components (Tables 2-1 to 2-9).
Furthermore, among the Examples containing polyoxyalkylene alkyl ether phosphate salt and propylene glycol, the formulations using Shirasu balloons having a particle size of 90% or more by weight in the range of 2.80 mm to 1.70 mm and a floating carrier having an average particle size of 90 to 120 μm, the formulations to which any of alkylnaphthalenesulfonate formaldehyde condensates, naphthalenesulfonate formaldehyde condensates, or ligninsulfonate sodium was added, and the formulations containing carboxymethylcellulose sodium or polyvinyl alcohol as a binder showed superior results in terms of sedimentation, formulation reach, and diffusion distance during preparation or after storage at 40° C. for 150 days. The overall diffusibility was best in Examples 102, 121, 140 and 159, in which the buoyant carrier contained shirasu balloons with an average particle size of 90 to 120 μm, sodium alkylnaphthalenesulfonate or sodium dialkylsuccinatesulfonate, and either sodium alkylnaphthalenesulfonate formaldehyde condensate, sodium naphthalenesulfonate formaldehyde condensate, or sodium ligninsulfonate, contained sodium carboxymethylcellulose or polyvinyl alcohol as a binder, had a particle size of 90% or more by weight in the range of 2.80 mm to 1.70 mm, and had a major axis/minor axis ratio at the base of the particle of 1.1 to 1.6, both immediately after preparation and after 150 days at 40°C.

From the above, in order for a water-floating pesticide formulation to effectively exhibit the diffusibility, which is a combination of sediment, formulation reach, and diffusion distance, not only immediately after preparation but also after long-term storage, it is necessary to have a pesticide active ingredient, a floating carrier, a polyoxyalkylene alkyl ether phosphate ester salt, and sodium alkylnaphthalenesulfonate or sodium dialkylsuccinatesulfonate, a particle size of 80% or more by weight in the range of 2.80 mm to 1.70 mm, and a long axis/short axis ratio of 1.1 to 1.6 at the base of the particle.
It is effective to have 50 to 200 grains per gram, and the grain size is 2
More effective means include having 90% by weight or more in the range of 80 mm to 1.70 mm, the floating carrier being a shirasu balloon with an average particle size of 90 to 120 μm, containing either sodium alkylnaphthalenesulfonate formaldehyde condensate, sodium naphthalenesulfonate formaldehyde condensate, or sodium ligninsulfonate, and containing sodium carboxymethylcellulose or polyvinyl alcohol as a binder.

Claims (8)

A water-floating pesticide formulation comprising: a) 0.01-60% by weight of a pesticidal active ingredient; b) 2.0-80% by weight of a hollow body as a floating carrier; and c) 0.5-30% by weight of one or more anionic surfactants selected from sodium alkylnaphthalenesulfonate and sodium dialkylsuccinatesulfonate , the water-floating pesticide formulation having the following characteristics:
d) The ratio of the major axis to the minor axis of the base of the grain is 1.1 to 1.4;
e) 80% by weight or more of the grain size is in the range of 2.80 mm to 1.70 mm; and
f) The number of grains per gram is 50 to 150;
The method for spraying a pesticide formulation is characterized in that the sprayer directly sprays the pesticide formulation without entering the paddy field. The spraying method according to claim 1, characterized in that the spraying method is either manual spraying, mechanical spraying using a powered sprayer, or aerial spraying using a drone. The spraying method according to claim 1, characterized in that the spraying method is a water inlet spraying method in which the spraying is performed on water flowing into a paddy field. The method of spreading according to claim 1, characterized in that the spreading method is a method of spreading by hand from only one side of the ridge. The present invention relates to a method for spraying a water-floating pesticide formulation, the method comprising the steps of: a) 0.01 to 60% by weight of a pesticide active ingredient; b) 2.0 to 80 % by weight of a hollow body as a floating carrier; and c) 1 to 40% by weight of a polyoxyalkylene alkyl ether phosphate ester salt represented by the following general formula (I), 0.5 to 20% by weight of a water-soluble alkylene glycol, and 0.5 to 30% by weight of one or more anionic surfactants selected from sodium alkylnaphthalenesulfonate and sodium dialkylsuccinatesulfonate, the method comprising the steps of: spraying a water-floating pesticide formulation directly into a paddy field without the sprayer entering the paddy field;

[In the formula, R represents a linear or branched alkyl group having 8 to 10 carbon atoms, A represents an alkylene group having 2 to 4 carbon atoms, n represents an integer from 1 to 20, p and q represent integers such that p+q=3 and p=1 or 2, and M represents a hydrogen atom, an alkali metal atom, an ammonium group, or an organic ammonium group. When there are multiple R, A, and M, the types of these may be the same or different.] The spraying method according to claim 5, characterized in that the spraying method is either manual spraying, mechanical spraying using a powered sprayer, or aerial spraying using a drone. The spraying method according to claim 5, characterized in that the spraying method is a water inlet spraying method in which the spraying is performed on water flowing into a paddy field. The method of spreading according to claim 5, characterized in that the spreading method is a method of spreading by hand from only one side of the ridge.