AU2013275206A1

AU2013275206A1 - Flying-insect pest repellent product and method for repelling flying insect pest

Info

Publication number: AU2013275206A1
Application number: AU2013275206A
Authority: AU
Inventors: Seiichi Kashima; Yumi Kawajiri; Koji Nakayama; Ryoko Ukita
Original assignee: Dainihon Jochugiku Co Ltd
Current assignee: Dainihon Jochugiku Co Ltd
Priority date: 2012-06-15
Filing date: 2013-06-13
Publication date: 2015-01-22
Anticipated expiration: 2033-06-13
Also published as: HK1222511A1; TWI478666B; JP5832649B2; CN104135860B; CN105900980B; CN104135860A; AU2013275206B2; CN105900980A; TW201400015A; WO2013187463A1; JPWO2013187463A1; KR20140126392A; KR101774896B1

Abstract

Provided are a flying-insect pest repellent product having excellent repelling effect on flying insect pests while utilizing characteristics of silicone rubber, and a method for repelling flying insect pests. In the flying-insect pest repellent product of the present invention, obtained by retaining a flying-insect pest repellent fragrance composition containing a flying-insect pest repellent fragrance component on a rubber molded article containing silicone rubber and having a hardness of 50 or less, the rubber molded article is an annular rubber molded article provided with an expandable annular part into which a part of the human body or an object is inserted or fitted, and the flying-insect pest repellent fragrance component is volatilized for 5-15 hours from a surface of the annular rubber molded article in a state in which a part of the human body or an object is inserted or fitted in the annular part.

Description

DESCRIPTION FLYING-INSECT PEST REPELLENT PRODUCT AND METHOD FOR REPELLING FLYING INSECT PEST 5 TECHNICAL FIELD [0001] The present invention relates to flying-insect pest repellent products and methods for repelling flying insect 10 pests. BACKGROUND ART [0002] Conventionally, repellents containing DEET (N,N-diethyl 15 toluamide) are commonly applied to a surface of the skin against flying insect pests of Culicidae, Simuliidae, Chironomidae, Brachycera, etc. However, DEET has a volatility somewhat lower than that of typical aroma chemical components, and therefore, cannot be expected to provide a spatial 20 repellent effect. On the other hand, although the effect of repelling flying insect pest may be achieved by causing an insecticide component which vaporizes at room temperature, such as empenthrin of the family of pyrethroids, etc., to vaporize and diffuse into space, the use of an insecticide 25 component which vaporizes at room temperature needs to be 1 avoided in not a few situations. [0003] Therefore, several attempts to use volatile naturally occurring essential oils, or components thereof, as a 5 repellent component have been proposed. For example, it is well known that citronella oil, or citronellal, which is a major component thereof, has a repellent effect against mosquitoes. In the United States of America, candles containing citronella oil as an active component were on the 10 market. However, the method of diffusing citronellal by means of heat of the candle is not efficient in vaporizing or diffusing citronellal, and therefore, has not a practical repellent effect. [0004] 15 Japanese Unexamined Patent Application Publication No. 2002-173407 (Patent Document 1) describes a flying-insect pest repellent containing a naturally-occurring essential oil selected from orange oil, cassia oil, etc., in addition to citronella oil, as active components. Patent Document 1 also 20 describes various examples of a solvent for use in a liquid formulation, including alcohols such as methyl alcohol, ethyl alcohol, etc., esters such as diethyl phthalate, isopropyl myristate, etc., aliphatic hydrocarbons such as hexane, kerosene, paraffin, etc., aromatic hydrocarbons, ethers, and 25 the like. 2 [0005] In addition, Japanese Unexamined Patent Application Publication No. 2003-201203 (Patent Document 2) describes a volatile insect pest repellent composition containing, as an 5 insect pest repellent component (A), one or more selected from citronellal, terpineol, menthol, limonene, geraniol, citronellol, camphene, etc., where the content of citronellal in the insect pest repellent component (A) is 2-10% by mass. However, these repellents are advertised as being naturally 10 occurring and safe, but are not necessarily satisfactory, because their repellent effects are inferior in terms of sustainability. [0006] Moreover, Japanese Unexamined Patent Application 15 Publication No. S61-289002 (Patent Document 3) proposes a "repellent for arthropods, mollusks, and reptiles containing glycol ethers as an active component." Patent Document 3 states that glycol ethers have a good repellent effect against cockroaches and ticks. However, the effect is in no way 20 sufficient. In addition, Patent Document 3 does not mention any effect of repelling flying insect pests. [0007] Thus, there is not yet a known useful aroma chemical composition for repelling flying insect pests, that is aimed 25 at achieving a flying-insect pest repellent effect, and in 3 addition to this, an improved sustainability of fragrance. There is a demand for the development of such a composition. [0008] Incidentally, it is known that silicone rubber has good 5 adsorptivity and gas permeability, stable physical properties, and good ability to discharging aroma chemicals. Because of such properties, air fresheners which are silicone rubber containing an aroma chemical are commercially available. Silicone rubber containing an aroma chemical is typically 10 produced by mixing a silicone compound or liquid silicone with the aroma chemical, followed by vulcanization (cross-linking) using a vulcanizing agent such as sulfur, etc., an additive, and the like. However, the aroma chemical easily separates from the rubber polymer or the additive during kneading, and 15 moreover, a chemical change such as decomposition, degeneration, etc., occurs in the aroma chemical due to heat or sulfur during molding. Therefore, it has been difficult to obtain a molded article having fragrance and stable physical properties. 20 [0009] Therefore, as a means for solving the above problems, Japanese Unexamined Patent Application Publication No. H08 311216 (Patent Document 4) and Japanese Unexamined Patent Application Publication No. 2011-26462 (Patent Document 5) 25 employ a method of adding an aroma chemical to silicone rubber 4 after molding instead of kneading silicone rubber together with an aroma chemical before molding. However, neither of these documents mentions the compatibility of the nature of the aroma chemical composition with silicone rubber. 5 Therefore, it is not unclear that the techniques of these documents are applicable to the flying-insect pest repellent aroma chemical composition, which has different functionality. CITATION LIST 10 PATENT LITERATURE [0010] Patent Document 1: Japanese Unexamined Patent Application Publication No. 2002-173407 Patent Document 2: Japanese Unexamined Patent 15 Application Publication No. 2003-201203 Patent Document 3: Japanese Unexamined Patent Application Publication No. S61-289002 Patent Document 4: Japanese Unexamined Patent Application Publication No. H08-311216 20 Patent Document 5: Japanese Unexamined Patent Application Publication No. 2011-26462 SUMMARY OF INVENTION TECHNICAL PROBLEM 25 [0011] 5 Thus, there has been a situation where, in order to develop a useful flying-insect pest repellent product using silicone rubber, it would be necessary to find a flying-insect pest repellent aroma chemical composition which has a high 5 repellent effect and good compatibility with silicone rubber, through trial and error, and conduct various tests. [0012] With the above problems in mind, the present invention has been made. It is an object to the present invention to 10 provide a product and method for repelling flying insect pests which have a good repellent effect against flying insect pests while utilizing properties of silicone rubber. SOLUTION TO PROBLEM 15 [0013] The present invention has found that the following configurations have a good effect in order to achieve the above object. [0014] 20 (1) A flying-insect pest repellent product which is a molded rubber article containing silicone rubber and having a hardness of no more than 50 degrees, the molded rubber article holding a flying-insect pest repellent aroma chemical composition containing a flying-insect pest repellent aroma 25 chemical component. 6 [0015] (2) The flying-insect pest repellent product of (1) , in which the molded rubber article is an annular molded rubber 5 article having an elastic annular portion configured to be put around or attached to a portion of the human body or an object, and the flying-insect pest repellent aroma chemical component vaporizes and discharges from a surface of the annular molded rubber article. 10 [0016] (3) The flying-insect pest repellent product of (2), in which when the annular portion is put around or attached to the portion of the human body or the object, the flying-insect 15 pest repellent aroma chemical component vaporizes and discharges over 5-15 hours. [0017] (4) The flying-insect pest repellent product of (3), in which 20 an average rate of vaporization and discharge of the flying-insect pest repellent aroma chemical component is 0.05 1.0 mg/cm2 -h throughout all surface area of the annular molded rubber article. [0018] 25 (5) The flying-insect pest repellent product of (3) or 7 (4), in which when the annular portion is put around or attached to the portion of the human body or the object, the area of the annular portion where the annular portion is in contact with 5 the portion of the human body or the object is no more than 80% of the area of an inner surface of the annular portion. [0019] (6) The flying-insect pest repellent product of any one of (1)-(5), in which 10 the flying-insect pest repellent aroma chemical composition contains, as the flying-insect pest repellent aroma chemical component, a component (a) and a component (b), the component (a) is a single acetic acid ester compound or a mixture of acetic acid ester compounds, the acetic acid 15 ester compound being represented by:

CH

3 -COO-R1 (I) where R1 is an alcohol residue having 6-12 carbons, and the component (b) is a monoterpene alcohol and/or an aromatic alcohol having 10 carbons. 20 [0020] (7) The flying-insect pest repellent product of (6), in which the flying-insect pest repellent aroma chemical composition further contains, as the component (a), a single 25 allyl ester compound or a mixture of allyl ester compounds, 8 the allyl ester compound being represented by: R2-CH 2

-COO-CH

2

-CH=CH

2 (II) where R2 is an alkyl, alkoxy, cycloalkyl, cycloalkoxy, or phenoxy group having 4-7 carbons, and 5 the component (a) is at least one selected from the acetic acid ester compounds and the allyl ester compounds. [0021] (8) The flying-insect pest repellent product of (6) or (7), in which 10 the blend ratio of the component (a) to the component (b) is 0.1-2.0. [0022] (9) The flying-insect pest repellent product of any one of (6)-(8), in which 15 the acetic acid ester compound is at least one selected from the group consisting of p-tert-butylcyclohexyl acetate, o-tert-butylcyclohexyl acetate, p-tert-pentylcyclohexyl acetate, tricyclodecenyl acetate, benzyl acetate, phenylethyl acetate, styralyl acetate, anisyl acetate, cinnamyl acetate, 20 terpinyl acetate, dihydroterpinyl acetate, linalyl acetate, ethyllinalyl acetate, citronellyl acetate, geranyl acetate, neryl acetate, bornyl acetate, and isobornyl acetate. [0023] (10) The flying-insect pest repellent product of any one 25 of (6)-(9), in which 9 the allyl ester compound is at least one selected from the group consisting of allyl hexanoate, allyl heptanoate, allyl octanoate, allyl n-amyloxyacetate, allyl cyclohexylacetate, allyl cyclohexyloxyacetate, and allyl 5 phenoxyacetate. [0024] (11) The flying-insect pest repellent product of any one of (6)-(10), in which the monoterpene alcohol and/or the aromatic alcohol 10 having 10 carbons are at least one selected from the group consisting of terpineol, geraniol, dihydromyrcenol, borneol, menthol, citronellol, nerol, linalool, ethyl linalool, thymol, eugenol, and p-menthane-3,8-diol. [0025] 15 (12) The flying-insect pest repellent product of any one of (6)-(11), in which the flying-insect pest repellent aroma chemical composition further contains a glycol and/or glycol ether having a vapor pressure of 0.2-20 Pa at 20 0 C as a repellent 20 effect sustaining component for the flying-insect pest repellent aroma chemical component during vaporization and discharge. [0026] (13) The flying-insect pest repellent product of (12), 25 in which 10 the glycol and/or the glycol ether are at least one selected from the group of consisting of benzyl glycol, propylene glycol, dipropylene glycol, tripropylene glycol, 1,3-butylene glycol, hexylene glycol, diethylene glycol 5 monobutyl ether, dipropylene glycol monobutyl ether, and tripropylene glycol monomethyl ether. [0027] (14) The flying-insect pest repellent product of (12) or (13), in which 10 the glycol is dipropylene glycol. [0028] (15) The flying-insect pest repellent product of any one of (1)-(14), in which the annular portion has a contour of a graphic shape or 15 figure. [0029] (16) The flying-insect pest repellent product of (15), in which the annular portion has a branch portion extending 20 outward from the annular portion at at least one point on the contour. [0030] (17) A flying-insect pest repellent method of using a flying-insect pest repellent product which is a molded rubber 25 article containing silicone rubber and having a hardness of no 11 more than 50 degrees, the molded rubber article holding a flying-insect pest repellent aroma chemical composition containing a flying-insect pest repellent aroma chemical component. 5 ADVANTAGEOUS EFFECTS OF INVENTION [0031] According to the flying-insect pest repellent product and method of the present invention, a flying-insect pest 10 repellent aroma chemical component is allowed to suitably vaporize and discharge from a molded rubber article containing silicone rubber and having a hardness of no more than 50 degrees, resulting in a good flying-insect pest repellent effect over a predetermined period of time. When a component 15 which can provide fragrance is used as the flying-insect pest repellent aroma chemical component, the initial fragrance type can be sustained over a long period of time, and therefore, the usefulness is considerably high. 20 BRIEF DESCRIPTION OF DRAWINGS [0032] [FIG. 1] FIG. 1 is a schematic diagram of a molded silicone rubber article which looks like a bear. FIG. 1(a) shows the molded silicone rubber article as it is not 25 attached. FIG. 1 (b) shows the molded silicone rubber article 12 as it is attached to the wrist. [FIG. 2] FIG. 2 is a schematic diagram of a molded silicone rubber article which looks like a rabbit. FIG. 2(a) shows the molded silicone rubber article as it is not 5 attached. FIG. 2(b) shows the molded silicone rubber article as it is attached to the wrist. [FIG. 3] FIG. 3 is a schematic diagram of a molded silicone rubber article which looks like a squirrel. FIG. 3(a) shows the molded silicone rubber article as it is not 10 attached. FIG. 3(b) shows the molded silicone rubber article as it is attached to the wrist. [FIG. 4] FIG. 4 is a schematic diagram of a molded silicone rubber article which looks like a bear, where branch portions extending outward are formed on the molded silicone 15 rubber article. FIG. 4(a) shows the molded silicone rubber article as it is not attached. FIG. 4(b) shows the molded silicone rubber article as it is attached to the wrist. DESCRIPTION OF EMBODIMENTS 20 [0033] Embodiments of a flying-insect pest repellent product according to the present invention will now be described. A flying-insect pest repellent method according to the present invention will be described together with the flying-insect 25 pest repellent product. Note that the present invention is not 13 intended to be limited to configurations described in the embodiments described below and the accompanying drawings. [0034] The flying-insect pest repellent product of the present 5 invention is a molded rubber article which contains silicone rubber and has a hardness of no more than 50 degrees (hereinafter also referred to as a "molded rubber article"), and holds an aroma chemical composition for repelling flying insect pests (hereinafter also referred to as a "flying-insect 10 pest repellent aroma chemical composition"), that contains an aroma chemical component for repelling flying insect pests (hereinafter also referred to as a "flying-insect pest repellent aroma chemical component") . A specific type of flying-insect pest repellent aroma chemical component suitable 15 for the molded rubber article is used. The flying-insect pest repellent aroma chemical component will be described in detail below. [0035] Silicone rubber, which is used in the molded article, 20 has good gas permeability and stable physical properties, and good ability to adsorb and discharge aroma chemicals. This may be because the molecular structure of aroma chemicals has a carbon backbone, and the three-dimensionally cross-linked molecular structure of the rubber allows aroma chemical 25 molecules to easily enter voids in the structure. In order to 14 utilize the properties of silicone rubber, it is preferable to adjust the hardness of the molded rubber article to no more than 50 degrees. For example, a silicone rubber having a hardness of no more than 50 degrees is used as a material for 5 the molded rubber article. As a result, the finished molded rubber article has a hardness of no more than 50 degrees. If the hardness of the molded rubber article is no more than 50 degrees, the silicone rubber does not have very dense molecular structure, and therefore, the molecular structure of 10 the rubber allows aroma chemical molecules to enter voids in the structure. Note that the hardness of the molded rubber article is measured using a method or device compliant with Japanese Industrial Standards (JIS K6253). In the present invention, the hardness of the molded rubber article is 15 measured using a durometer compliant with the above standards. [0036] Any of the types of silicone rubber, such as the room temperature curable type, the thermosetting type, the condensation type, the addition type, etc., can be used. 20 Typically, a silicone compound or liquid silicone is vulcanized (cross-linked) using a vulcanizing agent such as sulfur, etc., an additive such as silica, etc., and the like, followed by molding. Note that, by adjusting the cross-link density of silicone rubber, or by adjusting the amount of a 25 silicone oil or filler which is used and added as an additive, 15 the rate of vaporization and discharge of a flying-insect pest repellent aroma chemical composition which is subsequently added, can be controlled. [0037] 5 The molded rubber article used in the present invention may contain other types of rubber. For example, the molded rubber article containing fluorine-based rubber in addition to silicone rubber is expected to have improved durability. [0038] 10 The molded rubber article may be formed as an annular molded rubber article including an elastic annular portion which is put around or attached to a portion of the human body or an object. If the annular molded rubber article holding the flying-insect pest repellent aroma chemical composition is put 15 around or attached to a portion of the human body such as the wrist, ankle, etc., or an object such as the handle, etc., of a buggy, etc., the handlebars, etc., of a bicycle, etc., the handle, etc., of a handbag, rucksack, bag, etc., a chinstrap, a shoelace, etc., the flying-insect pest repellent aroma 20 chemical component gradually vaporizes and discharges through the surface of the annular molded rubber article. For example, if the flying-insect pest repellent product sustains the vaporization and discharge state over 5-15 hours, the average rate of vaporization and discharge of the flying-insect pest 25 repellent aroma chemical component is preferably 0.05-1.0 16 mg/cm 2 -h throughout all surface area of the annular molded rubber article in order to maintain the vaporization and discharge performance. If the average rate of vaporization and discharge of the flying-insect pest repellent aroma chemical 5 component is within this range, the bleeding of the flying insect pest repellent aroma chemical component in the annular molded rubber article stably smoothly proceeds over 5-15 hours, preferably 8-12 hours. If the average rate of vaporization and discharge of the flying-insect pest repellent 10 aroma chemical component is less than 0.05 mg/cm2-h, the flying-insect pest repellent effect is not sufficient. If the average rate of vaporization and discharge of the flying insect pest repellent aroma chemical component exceeds 1.0 mg/cm 2 -h, the sustained period of the repellent effect may 15 decrease, or the amount of the flying-insect pest repellent aroma chemical component or the flying-insect pest repellent aroma chemical composition which is held in the molded silicone rubber article may be excessively large, so that the surface is unavoidably likely to become wet and sticky. Note 20 that, in the present invention, the average rate of vaporization and discharge refers to an average value calculated over a period of time during which the rate of vaporization and discharge is at least 0.02 mg/cm 2 -h. [0039] 25 The molded rubber article is in the shape of a single 17 strand with one end joined to the other to form a circle (strand diameter: 1-3 mm, length: about 10-20 cm) so that the molded rubber article can be easily put around or attached to a portion of the human body such as the wrist, ankle, etc., or 5 the above objects, and forms a graphic shape or a figure. FIGS. 1-4 are schematic diagrams of a molded silicone rubber article 1 which looks like an animal, particularly a figure thereof. In each diagram, (a) shows the molded rubber article 1 as it is not attached, and (b) shows the molded rubber 10 article 1 as it is attached to a wrist 2. The molded silicone rubber article 1 is an annular molded rubber article including an elastic annular portion which is put around or attached to a portion of the human body or an object. As shown in (a) of each of FIGS. 1-4, the contour of the annular portion has a 15 graphic shape or a figure (profile). Examples of the graphic shape or figure include, but are not limited to, animals, insects, vehicles, alphabets, etc. When the molded rubber article 1 is attached to the wrist, ankle, etc., with a portion thereof being expanded, the original shape of the 20 molded rubber article 1 can preferably stretch so that at least 20%, preferably 30%, of that portion is separated from the skin of the wrist, ankle, etc. This is because not only the separation portion contributes to an improvement in vaporization and discharge of the repellent aroma chemical 25 component, but also it is desirable to keep even the aroma 18 chemical component away from the skin to the extent possible. In each of FIGS. 1-4, (b) shows a separation portion 3 which is formed by a portion of the molded rubber article 1 being separated from the wrist 2. 5 [0040] A main portion of the flying-insect pest repellent product of the present invention is the single strand-like article which forms a graphic shape or a figure. As shown in FIG. 4, the molded rubber article may be caused to branch at 10 one or more portions of the strand-like article to form a branch portion(s) 4, i.e., an attached accessory(s) . Thus, decorativeness is imparted, and the weight of the molded rubber article is increased, so that the amount of the flying insect pest repellent aroma chemical component which is held 15 can be increased, and therefore, the number of the flying insect pest repellent products of the present invention which are attached to the wrist, ankle, etc., can be advantageously reduced. The shape and size of the accessory are not particularly limited, unless the performance of vaporization 20 and discharge of the aroma chemical component of the accessory is excessively large or small than that of the main portion having the graphic shape or figure. [0041] The flying-insect pest repellent aroma chemical 25 composition used in the flying-insect pest repellent product 19 of the present invention does not substantially use an insecticide component, and uses an aroma chemical component as a flying-insect pest repellent component. Such an aroma chemical component is referred to as a "flying-insect pest 5 repellent aroma chemical component." The flying-insect pest repellent aroma chemical component contains the following components (a) and (b). [0042] Examples of the component (a) include a single acetic 10 acid ester compound or a mixture of acetic acid ester compounds, the acetic acid ester compound being represented by:

CH

3 -COO-R1 (I) where R1 is an alcohol residue having 6-12 carbons. 15 Examples of the component (b) include monoterpene alcohols and/or aromatic alcohols having 10 carbons. [0043] Of the flying-insect pest repellent aroma chemical components, a single allyl ester compound or a mixture of 20 allyl ester compounds may be additionally contained as the component (a), the allyl ester compound being represented by: R2-CH 2

-COO-CH

2

-CH=CH

2 (II) where R2 is an alkyl, alkoxy, cycloalkyl, cycloalkoxy, or phenoxy group having 4-7 carbons. In this case, the component 25 (a) is at least one selected from the acetic acid ester 20 compounds and the allyl ester compounds. [0044] The flying-insect pest repellent aroma chemical composition preferably further contains a glycol and/or glycol 5 ether having a vapor pressure of 0.2-20 Pa at 20 0 C as a repellent effect sustaining component during vaporization and discharge of the flying-insect pest repellent aroma chemical component. [0045] 10 The amount of the flying-insect pest repellent aroma chemical component or the flying-insect pest repellent aroma chemical composition which is added to (held in) the molded rubber article may be suitably determined based on the purpose of use or period of use of the flying-insect pest repellent 15 product, and the type or specification of the molded rubber article, etc. For example, in the case of a repellent product which is used for 8-12 hours at a time, the weight of the product is typically about 0.5-2.5 g, and the flying-insect pest repellent aroma chemical component which is held is 20 suitably within the range of 5-50 mg (i.e., 1-10% by mass) per molded rubber article. [0046] Also, according to the result of testing by the present inventors described below, it was found that the vaporization 25 and discharge state of the flying-insect pest repellent aroma 21 chemical component from the molded rubber article is affected by the prescription of the flying-insect pest repellent aroma chemical composition. For the flying-insect pest repellent aroma chemical composition used in the present invention, the 5 glycol and/or glycol ether which is mixed as a repellent effect sustaining component during vaporization and discharge, significantly contributes to stabilization of vaporization and discharge of the aroma chemical component from the molded silicone rubber article. On the other hand, in the case of the 10 flying-insect pest repellent aroma chemical composition which does not contain a glycol and/or a glycol ether, it was found that the amount of the composition which vaporizes and discharges in an early period tends to be somewhat large (eventually, the sustained period might be less than 5 hours, 15 and the average rate of vaporization and discharge might exceed 1.0 mg/cm 2 -h). [0047] The flying-insect pest repellent aroma chemical component contained in the flying-insect pest repellent aroma 20 chemical composition used in the flying-insect pest repellent product of the present invention will be specifically described. [0048] Specific examples of the acetic acid ester compound 25 represented by the general formula (I) which is the component 22 (a), of the flying-insect pest repellent aroma chemical components, include p-tert-butylcyclohexyl acetate, o-tert butylcyclohexyl acetate, p-tert-pentylcyclohexyl acetate, tricyclodecenyl acetate, benzyl acetate, phenylethyl acetate, 5 styralyl acetate, anisyl acetate, cinnamyl acetate, terpinyl acetate, dihydroterpinyl acetate, linalyl acetate, ethyllinalyl acetate, citronellyl acetate, geranyl acetate, neryl acetate, bornyl acetate, isobornyl acetate, etc. These acetic acid ester compounds may be used alone or in 10 combination. [0049] The specific examples of the allyl ester compound represented by the general formula (II) which is the component (a), of the flying-insect pest repellent aroma chemical 15 components, include allyl hexanoate, allyl heptanoate, allyl octanoate, allyl isobutyloxyacetate, allyl n-amyloxyacetate, allyl cyclohexylacetate, allyl cyclohexylpropionate, allyl cyclohexyloxyacetate, allyl phenoxyacetate, etc. These allyl ester compounds may be used alone or in combination. Also, 20 these allyl ester compounds may be used in combination with any of the acetic acid ester compounds. [0050] Specific examples of the monoterpene alcohol and/or the aromatic alcohol having 10 carbons which are the component 25 (b), of the flying-insect pest repellent aroma chemical 23 components, include terpineol, geraniol, dihydromyrcenol, borneol, menthol, citronellol, nerol, linalool, ethyl linalool, thymol, eugenol, p-menthane-3,8-diol, etc. These monoterpene alcohols and/or aromatic alcohols having 10 5 carbons may be used alone or in combination. [0051] In the flying-insect pest repellent product of the present invention, the components (a) and (b) which are the flying-insect pest repellent aroma chemical components are 10 preferably used in conjunction with each other. In this case, the results of the extensive study conducted by the present inventors demonstrated that if blend ratio of the component (a) to the component (b) is set to 0.1-2.0, a particularly good flying-insect pest repellent effect is achieved. 15 [0052] In the flying-insect pest repellent product of the present invention, the following additives may be suitably added as a flying-insect pest repellent aroma chemical component, in addition to the above aroma chemical components: 20 for example, ester compounds such as benzyl benzoate, cinnamyl formate, geranyl formate, etc.; monoterpene hydrocarbons such as limonene, etc.; monoterpene ketones such as menthone, carvone, pulegone, camphor, damascone, etc.; monoterpene aldehydes such as citral, citronellal, neral, perillaldehyde, 25 etc.; phenylethyl alcohol; diphenyl oxide; indol aroma 24 (dihydroindenyl-2,4-dioxane); etc. Moreover, the following various essential oils containing the above aroma chemical component may be suitably added: for example, jasmine oil, neroli oil, peppermint oil, bergamot oil, orange oil, geranium 5 oil, petitgrain oil, lemon oil, citronella oil, lemongrass oil, cinnamon oil, eucalyptus oil, lemon eucalyptus oil, thyme oil, etc. [0053] In the flying-insect pest repellent product of the 10 present invention, the flying-insect pest repellent aroma chemical composition held by the molded rubber article preferably further contains a repellent effect sustaining component during vaporization and discharge of the flying insect pest repellent aroma chemical component. The repellent 15 effect sustaining component is, for example, a glycol and/or glycol ether having a vapor pressure of 0.2-20 Pa at 20 0 C. Such a glycol and/or glycol ether are exemplified as a solvent together with ethanol, isopropanol, lamp oil, etc., in Patent Document 2. Also, Patent Document 3 states that such a glycol 20 and/or glycol ether has a good repellent effect against cockroaches and ticks, but does not mention a effect on flying insect pests. Therefore, the present inventors were the first to find that the glycol and/or glycol ether not only serves as a solvent, but also has the action of specifically sustaining 25 the repellent effect of the flying-insect pest repellent aroma 25 chemical, and when a flying-insect pest repellent aroma chemical which can provide fragrance is used, also allows the flying-insect pest repellent aroma chemical to sustain the initial fragrance type. 5 [0054] Specific examples of the glycol and/or glycol ether (followed by the vapor pressure at 20 0 C) include propylene glycol (10.7 Pa), dipropylene glycol (1.3 Pa), tripropylene glycol (0.67 Pa), diethylene glycol (3 Pa), triethylene glycol 10 (1 Pa), 1,3-butylene glycol, hexylene glycol (6.7 Pa), benzyl glycol (2.7 Pa), diethylene glycol monobutyl ether (3 Pa), dipropylene glycol monobutyl ether, and tripropylene glycol monomethyl ether. Of them, dipropylene glycol is preferable to the spirit of the present invention. Note that the above 15 glycols and/or glycol ethers may be used alone or in combination. The blend ratio of the glycol and/or glycol ether to the flying-insect pest repellent aroma chemical is suitably about 0.05-5. [0055] 20 The flying-insect pest repellent aroma chemical composition may be blended with other functional components unless the advantages of the present invention are impaired. Examples of other functional components include insecticide components, air freshener components, antibacterial and 25 antifungal components, etc. Examples of the insecticide 26 component include empenthrin, profluthrin, transfluthrin, metofluthrin, etc., which are of the family of pyrethroids which vaporize at room temperature. When an insecticide component is blended, the amount of the insecticide component 5 is preferably limited to as small an amount as possible because of the spirit of the present invention. A representative example of the air freshener component is an extract of a plant selected from Poaceae, Theaceae, Ginkgoaceae, Oleaceae, Moraceae, Rutaceae, Malpighiaceae, and 10 Ebenaceae. Also, leaf alcohol, leaf aldehyde, etc., which are called "green odor," may be added to impart a relaxing effect. These functional components may be used alone or in combination. [0056] 15 The flying-insect pest repellent aroma chemical composition may be optionally suitably blended with a solvent, surfactant, solubilizer, dispersant, stabilizer, pH adjuster, colorant, etc., unless the advantages of the present invention are impaired. Also, the flying-insect pest repellent aroma 20 chemical composition may be encapsulated into microcapsules or several of the flying-insect pest repellent aroma chemical components may be bound together into a cyclodextrin-like structure, so that the flying-insect pest repellent aroma chemical composition can be stabilized or the performance of 25 vaporization and discharge of the flying-insect pest repellent 27 aroma chemical component can be adjusted. [0057] Examples of the solvent used in formulation of the flying-insect pest repellent product include water, lower 5 alcohols such as ethanol, isopropanol, etc., ketone solvents, ester solvents, hydrocarbon solvents such as normal paraffin, isoparaffin, etc., and the like. Examples of the surfactant include non-ionic surfactants such as polyoxyethylene hydrogenated castor oil, polyoxyethylene higher alkyl ethers 10 (polyoxyethylene lauryl ether, polyoxyethylene oleyl ether, etc.), polyoxyethylene alkyl phenyl ethers, polyoxyethylene higher fatty acid esters, polyoxyethylene sorbitan fatty acid esters, polyoxyethylene glycerin fatty acid esters, polyoxyethylene polyoxypropylene alkyl ethers, etc., and 15 higher alkyl amine oxide surfactants such as lauryl amine oxide, stearyl amine oxide, lauric acid amide propyldimethylamine oxide, etc. These surfactants may be used alone or in combination. [0058] 20 The above flying-insect pest repellent aroma chemical composition is added to a molded rubber article containing silicone rubber and having a hardness of no more than 50 degrees, followed by a predetermined treatment, so that the molded rubber article holds the flying-insect pest repellent 25 aroma chemical composition, whereby the production of the 28 flying-insect pest repellent product of the present invention is completed. By using the flying-insect pest repellent product of the present invention, the flying-insect pest repellent method of the present invention can be carried out. 5 [0059] The flying-insect pest repellent aroma chemical composition can be added to the molded rubber article using a conventionally known suitable technique. For example, if the molded rubber article has a large surface area, the molded 10 rubber article is caused to carry the flying-insect pest repellent aroma chemical composition by a solution dispensing technique or an application technique. If the molded rubber article has a small surface area, a large number of the molded rubber articles are placed in a closed container, and the 15 flying-insect pest repellent aroma chemical composition and, optionally, a solvent are added to the container by spraying or dropping, and allowed to permeate the molded rubber articles. Alternatively, the molded rubber article may be immersed in a solution of the flying-insect pest repellent 20 aroma chemical composition for a suitable period of time. Alternatively, the molded rubber article containing a high concentration of the flying-insect pest repellent aroma chemical composition and the non-treated molded rubber article are placed together in a closed container, and allowed to 25 stand for a suitable period of time so that the concentration 29 of the aroma chemical composition is caused to be uniform in the entire molded rubber article. The flying-insect pest repellent product can be manufactured using these techniques. [0060] 5 The amount of the flying-insect pest repellent aroma chemical composition which is contained in the flying-insect pest repellent product of the present invention may be suitably determined based on the purpose of use or period of use of the flying-insect pest repellent product, and the type 10 or specification of the molded rubber article, etc. For example, in the case of a flying-insect pest repellent product which is used for 8-12 hours at a time, about 10-50 mg of the flying-insect pest repellent aroma chemical composition is preferably contained in each molded rubber article. In the 15 case of a flying-insect pest repellent product which is used for 15-30 days, about 100-2000 mg of the flying-insect pest repellent aroma chemical composition is preferably contained in each molded rubber article. [0061] 20 According to the flying-insect pest repellent product of the present invention, the molded rubber article itself may be a flying-insect pest repellent product. Examples of the flying-insect pest repellent product include a wrist ring, wrist band, etc. The flying-insect pest repellent product may 25 also be in the form of a watch strap. In this case, an 30 accommodation portion for accommodating a small piece of molded rubber article may be formed in a portion of the watch strap so that the molded rubber article can be replaced with a new one. Note that, in this case, the flying-insect pest 5 repellent product has the advantage of allowing the molded rubber article not to be in direct contact with the skin of the arm. [0062] When one to five of the flying-insect pest repellent 10 products of the present invention thus obtained are attached to a site such as the wrist, ankle, etc., in a room such as a front door, kitchen, bathroom, living room, bedroom, etc., space such as a warehouse, car, etc., a garden, or the open air as required, the flying-insect pest repellent product 15 provides a good flying-insect pest repellent effect against flying insect pests of Culicidae (Culex pipiens pallens, Culex pipiens molestus, Aedes albopictus, etc.), Simuliidae, Chironomidae, Brachycera, small flies (Drosophilidae, Phoridae, etc.), Psychodidae, Tineidae, and the like, over a 20 predetermined period of time. When a flying-insect pest repellent aroma chemical which can provide fragrance is used, the initial fragrance type is sustained over a period of time without being changed. In addition, the present product does not substantially contain an insecticide component, and 25 therefore, can be used by people who do not like to use 31 insecticides, without hesitation, and therefore, the practical utility is considerably high. Examples [0063] 5 To demonstrate the effectiveness of the flying-insect pest repellent product of the present invention, the following examples and comparative examples were carried out. [0064] (Example 1) 10 A flying-insect pest repellent aroma chemical composition of the present invention was formulated which contained: 8.0% by mass of p-tert-butylcyclohexyl acetate and 3.2% by mass of phenylethyl acetate as an acetic acid ester compound represented by the general formula (I) which is the 15 component (a) of the flying-insect pest repellent aroma chemical component; 14.3% by mass of terpineol, 9.8% by mass of geraniol, and 12.0% by mass of dihydromyrcenol as an monoterpene alcohol and/or an aromatic alcohol having 10 carbons which is the component (b) of the flying-insect pest 20 repellent aroma chemical component; 38.0% by mass of dipropylene glycol as a repellent effect sustaining component; and 14.7% by mass of other flying-insect pest repellent aroma chemicals (including 7.1% by mass of phenylethyl alcohol and 1.6% by mass of cinnamyl formate). In this flying-insect pest 25 repellent aroma chemical composition, the blend ratio of the 32 component (a) to the component (b) is 0.32. [0065] Next, a vulcanizing agent was added to liquid silicone, followed by molding, to form a strand ring-shaped molded 5 silicone rubber article (strand diameter: about 2 mm, weight: 1.6 g, and hardness: 32). A hundred of the molded rubber articles were placed in a closed container with a spray device. The flying-insect pest repellent aroma chemical composition was sprayed over the molded rubber articles using 10 the spray device in an amount such that the amount of the composition which was adsorbed by each molded rubber article was 30 mg. The molded rubber articles were allowed to stand for one day so that the flying-insect pest repellent aroma chemical composition permeated uniformly the entire molded 15 rubber article. As a result, the flying-insect pest repellent product of the present invention which was in the shape of a wristband and had an effective sustained period of 8-12 hours, was obtained. Note that, alternatively, a molded silicone rubber article having a hardness of 80 degrees was tested in a 20 similar manner. However, the flying-insect pest repellent aroma chemical composition was adsorbed in only a small amount. [0066] When an experimenter wore the wristband thus obtained on 25 the arm and stayed outdoor, the experimenter was not annoyed 33 by flying insect pests such as mosquitos, small flies, etc., over 8-12 hours, so that a practical repellent effect was demonstrated. Fragrance still having the initial fragrance type wafted in space around the body, so that the experimenter 5 enjoyed a pleasantly fresh smell. [0067] <Sustainability Evaluation Test 1> As in Example 1, a flying-insect pest repellent aroma chemical composition which can be used in the flying-insect 10 pest repellent product of the present invention was formulated which contained: 12 mg of styralyl acetate as an acetic acid ester compound represented by the general formula (I) which is the component (a) of the flying-insect pest repellent aroma chemical component; 28 mg of geraniol as a monoterpene alcohol 15 and/or an aromatic alcohol having 10 carbons which is the component (b) of the flying-insect pest repellent aroma chemical component; and each repellent effect sustaining component. A sustainability evaluation test 1 described below was performed on the flying-insect pest repellent aroma 20 chemical composition thus obtained. In this test, the knockdown activity against adults of Culex pipiens pallens (female (?)) was used as an index for sustainability evaluation. [0068] 25 Filter paper having a diameter of 15 cm was impregnated 34 with 0.5 mL of acetone solution (specimen reagent) containing 70 mg of the flying-insect pest repellent aroma chemical and the repellent effect sustaining components, followed by air drying, to formulate each piece of specimen reagent-treated 5 filter paper. A plastic cylinder (inner diameter: 20 cm, and height: 43 cm) was installed, in which each piece of specimen reagent-treated filter paper was then placed. A 12-mesh wire mesh was provided on top of the plastic cylinder to separate upper and lower spaces. A second cylinder (inner diameter: 20 10 cm, and height: 20 cm) in which 20 specimen adults of Culex pipiens pallens were released was placed on top of the plastic cylinder. A third cylinder (inner diameter: 20 cm, and height: 43 cm) was placed on top of the second cylinder. The number of specimen insects which were knocked down as time passed was 15 counted to obtain a value KT 5 o (a time it takes to knock down half of the specimen insects) . Note that, in order to evaluate the sustainability of each specimen reagent, two pieces of specimen reagent-treated filter paper, i.e., specimen reagent treated filter paper immediately after air drying (0 h in 20 Table 1), and specimen reagent-treated filter paper which had been placed in another room for four hours for vaporization and discharge after air drying (4 h in Table 1), were tested. The results of the sustainability evaluation test 1 are shown in Table 1. 25 [0069] 35 Table 1 Repellent effect Vapor KT 5 o (min) sustaining component in pressure 0 h 4h specimen reagent (Pa/20 0 C) 1 Tripropylene glycol 0.67 62.7 101.5 2 Triethylene glycol 1 76.1 118.4 3 Dipropylene glycol 1.3 19.3 42.0 4 Benzyl glycol 2.7 42.8 75.9 Glycol/ 5 Diethylene glycol 3 38.5 76.7 glycol 6 Hexylene glycol 6.7 59.0 83.2 ether 7 Propylene glycol 10.7 36.4 59.8 8 Diethylene glycol 3 22.9 51.3 monobutyl ether 1 Myristate isopropyl 0.012 83.2 > 120 Other 2 Neochiozol 2.7 86.3 > 120 compounds 3 Isobutyl alcohol 1200 32.8 > 120 4 - 36.1 > 120 [0070] According to the results of Table 1, it was demonstrated 5 that a glycol and/or glycol ether having a vapor pressure of 0.2-20 Pa at 20 0 C has the action of sustaining the knockdown effect, i.e., is useful as a repellent effect sustaining component. Note that the comparison between ethylene glycols and propylene glycols showed that the latter is generally 36 preferable. In contrast to this, myristate isopropyl and Neochiozol, which are not a glycol or a glycol ether, had a poor knockdown effect sustaining action even when the vapor pressure was within the range of 0.2-20 Pa at 20 0 C. 5 [0071] Based on the results of Table 1, a sustainability evaluation test similar to that described above was next performed on hexylene glycol and dipropylene glycol while changing the type and content of the flying-insect pest 10 repellent aroma chemical component. The results are shown in Table 2. [0072] 37 Table 2 Repellent Flying-insect pest repellent KT 5 o (min) effect aroma chemical sustaining (a) (b) (a)/ 0 h 4 h component (b) (a) 1 Hexylene Benzyl Menthol 0.25 41.8 47.1 and glycol acetate 10 mg 40 mg (b) 2 75 mg Benzyl Menthol 0.05 54.0 61.7 acetate 2 mg 45 mg 3 Dipropylene Benzyl Thymol 0.25 22.3 36.2 glycol acetate 10 mg 40 mg 4 75 mg Benzyl Thymol 0.04 37.9 43.0 acetate 2 mg 45 mg 5 Benzyl Thymol 2.5 35.3 41.6 acetate 30 mg 12 mg (a) 1 Hexylene Benzyl - - 61.5 78.8 or glycol acetate 10 mg (b) 2 75 mg - Menthol - 83.2 101.5 40 mg 3 Dipropylene Benzyl - - 44.7 68.3 glycol acetate 10 mg 4 75 mg - Thymol - 65.3 109.4 40 mg [0073] According to the results of Table 2, it was found that 38 the repellent effect sustaining component used in the present invention has a more efficient knockdown effect sustaining action when an acetic acid ester compound represented by the general formula (I) which is the component (a) of the flying 5 insect pest repellent aroma chemical component, and a monoterpene alcohol and/or an aromatic alcohol having 10 carbons which is the component (b) of the flying-insect pest repellent aroma chemical component, are used in combination, and the blend ratio of the component (a) to the component (b) 10 is 0.1-2.0. [0074] (Examples 2-10) As in Example 1, strand ring-shaped molded silicone rubber articles (strand diameter: about 2 mm, weight: 1.6 g, 15 and hardness: 30) were molded. Flying-insect pest repellent aroma chemical compositions described in Table 3 were each added to the molded articles in an amount of 30 mg per molded article, to obtain flying-insect pest repellent products of the present invention having an effective sustained period of 20 about 8-12 hours. In a testing room (about 6 M 3 ), two plastic cups (about 1 L) whose lids were taken off and therefore were open, were placed. A Drosophilidae attractant and a specimen flying-insect pest repellent product were placed in one of the two cups (treatment zone), and only the Drosophilidae 25 attractant was placed in the other plastic cup (control zone) 39 After four hours of use, adults of Drosophilidae (the number of them was about 100) were released in the room. The number of insects entering each zone plastic cup was counted. The repellency rate was calculated by: 5 Repellency rate = [(the number of insects entering the control zone - the number of insects entering the treatment zone)/the number of insects entering the control zone] x 100 [0075] 40 Table 3 Flying-insect pest repellent product (% Repelle by mass) ncy Flying-insect pest repellent Repelle rate aroma chemical nt (%) (a) (b) (a)/ effect (b) sustain ing compone nt Example 1 p-tert- Terpineol 0.32 Dipropy 100 butylcycloh 14.3 lene exyl Geraniol 9.8 glycol acetate 8 Dihydromyrce 38 Phenylethyl nol 12 acetate 3.2 2 p-tert- Geraniol 40 0.65 Dipropy 100 butylcycloh lene exyl glycol acetate 26 20 3 Styralyl Linalool 15 0.32 Benzyl 98 acetate 8 Eugenol 10 glycol 34 41 (Continuation of Table 3) 4 Tricyclodec Terpineol 20 1.0 Dipropy 96 enyl lene acetate 20 glycol 40 5 Cinnamyl Geraniol 60 0.07 Triethy 87 acetate 4 lene glycol 14 6 Benzyl p-menthane- 1.1 Diethyl 82 acetate 36 3,8-diol 20 ene Menthol 14 glycol monobut yl ether 9 7 p-tert- Geraniol 24 0.58 - 53 butylcycloh exyl acetate 14 8 Tricyclodec Borneol 20 0.82 Polyeth 60 enyl Ethyl ylene acetate 16 linalool 14 glycol Anisyl (< 0.01 acetate 12 Pa/20 0 C) 29 42 (Continuation of Table 3) 9 Tricyclodec Nerol 21 0.69 Propyle 51 enyl Citronellol ne acetate 18 15 glycol Geranyl monomet acetate 7 yl ether (1660 Pa/20 0 C) 12 10 Dihydroterp Borneol 11 2.3 Hexylen 64 inyl e acetate 25 glycol 16 Comparat 77 Styralyl Linalool 15 0.32 Benzyl 37 ive acetate 8 Eugenol 10 glycol Example 34 2 Mint oil 50 - Dipropy 19 lene glycol 40 * Molded silicon rubber article having hardness of 80 degrees [0076] According to the results of Table 3, it was demonstrated 5 that the flying-insect pest repellent product of the present 43 invention (containing the flying-insect pest repellent aroma chemical, and preferably additionally a glycol and/or glycol ether having a vapor pressure of 0.2-20 Pa at 20 0 C as a repellent effect sustaining component after vaporization and 5 discharge), has a good flying-insect pest repellent effect over four hours after vaporization and discharge. Also, when an acetic acid ester compound represented by the general formula (I) which is the component (a) of the flying-insect pest repellent aroma chemical component, and a monoterpene 10 alcohol and/or an aromatic alcohol having 10 carbons which is the component (b) of the flying-insect pest repellent aroma chemical component, were used in combination, and the blend ratio of the component (a) to the component (b) was 0.1-2.0, the repellent effect sustaining component had a more efficient 15 action, and not only the repellency rate but also the fragrance sustainability were satisfactory. [0077] In contrast to this, in Comparative Example 1 in which a molded silicone rubber article having a hardness exceeding 50 20 degrees was used, the repellent effect was low. Also, in Comparative Example 2 in which mint oil, which is not considered to be a flying-insect pest repellent aroma chemical, is used, the repellent effect was not sufficient. [0078] 25 Therefore, the flying-insect pest repellent product of 44 the present invention which contains a combination of a flying-insect pest repellent aroma chemical, and preferably additionally a repellent effect sustaining component, has good practical utility. 5 [0079] (Example 11) A flying-insect pest repellent aroma chemical composition of the present invention was formulated which contained: 10.5% by mass of tricyclodecenyl acetate and 3.0% 10 by mass of benzyl acetate as an acetic acid ester compound represented by the general formula (I) which is the component (a) of the flying-insect pest repellent aroma chemical component; 27.2% by mass of geraniol and 3.4% by mass of thymol as a monoterpene alcohol and/or an aromatic alcohol 15 having 10 carbons which is the component (b) of the flying insect pest repellent aroma chemical component; 40.6% by mass of dipropylene glycol as a repellent effect sustaining component; and further 15.3% by mass of other flying-insect pest repellent aroma chemicals (4.0% by mass of eucalyptus 20 oil, and 1.5% by mass of benzyl benzoate). The blend ratio of the component (a) to the component (b) in this flying-insect pest repellent aroma chemical composition was 0.44. [0080] Next, a band ring-shaped molded silicone rubber article 25 (width: 10 mm, length: 20 cm, weight: 5.2 g, and hardness: 27) 45 containing a silicone compound was molded. The inner surface (a surface which is made contact with the skin) of the molded rubber article was coated with polyethylene film. Moreover, the flying-insect pest repellent aroma chemical composition 5 was applied to the outer surface of the molded rubber article at four portions in a total amount of 700 mg. The band ring shaped molded silicone rubber article was allowed to stand in a closed space for two days so that the flying-insect pest repellent aroma chemical composition permeated uniformly the 10 entire molded rubber article. As a result, a flying-insect pest repellent product of the present invention which is in the form of a wristband and has an effective sustained period of about one month, was provided. [0081] 15 When an experimenter wore the wristband thus obtained on the arm and stayed outdoor, the experimenter was not annoyed by flying insect pests such as mosquitos, small flies, etc., over about 30 days. Also, in the case of this product, the repellent aroma chemical carrier was not in direct contact 20 with the skin, and therefore, was also preferable in terms of consideration for safety. [0082] (Example 12) A flying-insect pest repellent aroma chemical 25 composition of the present invention was formulated which 46 contained: 8.6% by mass of p-tert-butylcyclohexyl acetate and 3.2% by mass of phenylethyl acetate as an acetic acid ester compound represented by the general formula (I) which is the component (a) of the flying-insect pest repellent aroma 5 chemical component; 2.3% by mass of allyl heptanoate as an allyl ester compound represented by the general formula (II) which is the component (a) of the flying-insect pest repellent aroma chemical component; 14.5% by mass of terpineol, 9.4% by mass of geraniol, and 11.0% by mass of dihydromyrcenol as a 10 monoterpene alcohol and/or an aromatic alcohol having 10 carbons which is the component (b) of the flying-insect pest repellent aroma chemical component; 36.3% by mass of dipropylene glycol as a repellent effect sustaining component; and 14.7% by mass of other flying-insect pest repellent aroma 15 chemicals (4.5% by mass of phenylethyl alcohol, and 6.7% by mass of benzyl benzoate). The blend ratio of the component (a) to the component (b) in this flying-insect pest repellent aroma chemical composition was 0.40. [0083] 20 Next, a molded silicone rubber article (strand diameter: 2 mm, length: 15 cm, surface area: 9.42 cm2 , and hardness: 32) was produced by adding a vulcanizing agent to liquid silicone and molding the liquid silicone into a closed single strand like article which looks like a figure of a dragonfly. A 25 hundred of the molded rubber articles were placed in a closed 47 container with a spray device. The above flying-insect pest repellent aroma chemical composition was sprayed over the molded rubber articles using the spray device in an amount such that the amount of the composition which was adsorbed by 5 each molded rubber article was 30 mg (19.1 mg of the flying insect pest repellent aroma chemical) . The molded rubber articles were allowed to stand for one day so that the flying insect pest repellent aroma chemical composition permeated uniformly the entire molded rubber article. As a result, the 10 flying-insect pest repellent product of the present invention which was in the shape of a wristband and had an effective sustained period of about 10 hours, was obtained. Note that, alternatively, a molded silicone rubber article having a hardness of 80 degrees was tested in a similar manner. 15 However, the flying-insect pest repellent aroma chemical composition was adsorbed in only a small amount, and therefore, was not applicable to the present invention. [0084] The average rate of vaporization and discharge of the 20 flying-insect pest repellent aroma chemical component was 0.21 mg/cm 2 -h throughout all surface area of the flying-insect pest repellent product. When this product was put around the wrist, about 45% of the wrist ring was separated from the skin. [0085] 25 When an experimenter wore two of the wrist rings thus 48 obtained on each of the left and right wrists, and stayed outdoor, the experimenter was not annoyed by flying insect pests such as mosquitos, small flies, etc., over about 10 hours, so that a practical repellent effect was demonstrated. 5 Also, it was fun to wear the product having a figure of an animal, and fragrance still having the initial fragrance type wafted in space around the body, so that the experimenter enjoyed a pleasantly fresh smell. [0086] 10 <Sustainability Evaluation Test 2> As in Example 12, a flying-insect pest repellent aroma chemical composition which can be used in the flying-insect pest repellent product of the present invention was formulated which contained: 12 mg of styralyl acetate as an acetic acid 15 ester compound represented by the general formula (I) which is the component (a) of the flying-insect pest repellent aroma chemical component; 6 mg of allyl octanoate as an allyl ester compound represented by the general formula (II) which is the component (a) of the flying-insect pest repellent aroma 20 chemical component; 25 mg of geraniol as a monoterpene alcohol and/or an aromatic alcohol having 10 carbons which is the component (b) of the flying-insect pest repellent aroma chemical component; and each repellent effect sustaining component. A sustainability evaluation test 2 described below 25 was performed on the flying-insect pest repellent aroma 49 chemical composition thus obtained. In this test, the knockdown activity against adults of Culex pipiens pallens (female (0)) was used as an index for sustainability evaluation. 5 [0087] Filter paper having a diameter of 15 cm was impregnated with 0.5 mL of acetone solution (specimen reagent) containing 70 mg of the flying-insect pest repellent aroma chemical and the repellent effect sustaining components, followed by air 10 drying, to formulate each piece of specimen reagent-treated filter paper. A plastic cylinder (inner diameter: 20 cm, and height: 43 cm) was installed, in which each piece of specimen reagent-treated filter paper was then placed. A 12-mesh wire mesh was provided on top of the plastic cylinder to separate 15 upper and lower spaces. A second cylinder (inner diameter: 20 cm, and height: 20 cm) in which 20 specimen adults of Culex pipiens pallens were released was placed on top of the plastic cylinder. A third cylinder (inner diameter: 20 cm, and height: 43 cm) was placed on top of the second cylinder. The number of 20 specimen insects which were knocked down as time passed was counted to obtain a value KT 50 (a time it takes to knock down half of the specimen insects) . Note that, in order to evaluate the sustainability of each specimen reagent, two pieces of specimen reagent-treated filter paper, i.e., specimen reagent 25 treated filter paper immediately after air drying (0 h in 50 Table 4), and specimen reagent-treated filter paper which had been placed in another room for four hours for vaporization and discharge after air drying (4 h in Table 4), were tested. The results of the sustainability evaluation test 2 are shown 5 in Table 1. [0088] 51 Table 4 Repellent effect Vapor KT 5 o (min) sustaining component in pressure 0 h 4h specimen reagent (Pa/20 0 C) 1 Tripropylene glycol 0.67 62.4 101.2 2 Triethylene glycol 1 75.8 116.7 3 Dipropylene glycol 1.3 19.1 42.3 4 Benzyl glycol 2.7 42.6 75.0 Glycol/ 5 Diethylene glycol 3 37.9 76.4 glycol 6 Hexylene glycol 6.7 58.5 82.8 ether 7 Propylene glycol 10.7 36.0 59.6 8 Diethylene glycol 3 22.7 51.1 monobutyl ether 1 Myristate isopropyl 0.012 82.9 > 120 Other 2 Neochiozol 2.7 86.2 > 120 compounds 3 Isobutyl alcohol 1200 32.3 > 120 4 - 36.4 > 120 [0089] According to the results of Table 4, it was demonstrated 5 that a glycol and/or glycol ether having a vapor pressure of 0.2-20 Pa at 20 0 C has the action of sustaining the knockdown effect, i.e., is useful as a repellent effect sustaining component. Note that the comparison between ethylene glycols and propylene glycols showed that the latter is generally 52 preferable. In contrast to this, myristate isopropyl and Neochiozol, which are not a glycol or a glycol ether, had a poor knockdown effect sustaining action even when the vapor pressure was within the range of 0.2-20 Pa at 20 0 C. 5 [0090] Based on the result of Table 4, a sustainability evaluation test similar to that described above was next performed on hexylene glycol and dipropylene glycol while changing the type and content of the flying-insect pest 10 repellent aroma chemical component. The results are shown in Table 5. [0091] 53 Table 5 Repellent Flying-insect pest repellent KT 5 o (min) effect aroma chemical sustaining (a) (b) (a)/ 0 h 4 h component (b) (a) 1 Hexylene Benzyl Menthol 0.25 41.7 48.4 and glycol acetate 10 mg 40 mg (b) 2 70 mg Benzyl Menthol 0.05 54.2 62.3 acetate 2 mg 45 mg 3 Dipropylene Benzyl Thymol 0.25 22.5 36.9 glycol acetate 10 mg 40 mg 4 70 mg Benzyl Thymol 0.04 37.8 43.6 acetate 2 mg 45 mg 5 Benzyl Thymol 2.5 35.5 41.3 acetate 38 mg 15 mg (a) 1 Hexylene Benzyl - - 61.6 79.5 or glycol acetate 10 mg (b) 2 70 mg - Menthol - 83.3 102.0 40 mg 3 Dipropylene Benzyl - - 44.9 68.8 glycol acetate 10 mg 4 70 mg - Thymol - 65.7 110.1 40 mg [0092] According to the results of Table 5, it was found that 54 the repellent effect sustaining component used in the present invention has a more efficient knockdown effect sustaining action when an acetic acid ester compound represented by the general formula (I) which is the component (a) of the flying 5 insect pest repellent aroma chemical component, and a monoterpene alcohol and/or an aromatic alcohol having 10 carbons which is the component (b) of the flying-insect pest repellent aroma chemical component, are used in combination, and the blend ratio of the component (a) to the component (b) 10 was 0.1-2.0. [0093] (Examples 13-22) As in Example 12, strand-like molded silicone rubber articles (strand diameter: 2 mm, length: 10-20 cm, and 15 hardness: 30) which looked like a figure of an animal were produced which contained flying-insect pest repellent aroma chemical compositions described in Table 6 in an amount of 25 mg per molded article as follows: each flying-insect pest repellent aroma chemical composition was added to six non 20 treated molded articles in a total amount of 1500 mg (25 mg x 6 x 10) which was 10 times the content of the flying-insect pest repellent aroma chemical composition in the products, thereby producing the high concentration liquid-containing molded articles. Next, the 6 high concentration liquid-containing 25 molded articles and 54 non-treated molded silicone rubber 55 articles were placed in an aluminum bag whose inner surface was coated with polyester film. The bag was sealed and allowed to stand for 7-10 days. The flying-insect pest repellent aroma chemical composition was uniform in the entire bag. A flying 5 insect pest repellent product of the present invention (a figure name is additionally shown below a specimen number) was obtained which had a flying-insect pest repellent aroma chemical composition content per molded article of 25 mg and an effective sustained period of about 8-12 hours. In a 10 testing room (about 6 M 3 ), two plastic cups (about 1 L) whose lids were taken off and therefore were open, were placed. A Drosophilidae attractant and a specimen flying-insect pest repellent product were placed in one of the two cups (treatment zone), and only the Drosophilidae attractant was 15 placed in the other plastic cup (control zone) . After five hours of use, adults of Drosophilidae (the number of them was about 100) were released in the room. The number of insects entering each zone plastic cup was counted. The repellency rate was calculated by: 20 Repellency rate = [(the number of insects entering the control zone - the number of insects entering the treatment zone)/the number of insects entering the control zone] x 100 [0094] 56 4-) CD o o D -H 0) 0 4-H co

-H

(d 0 - -H 1 0 u 0 4-) 0, -0 U oc C; i 4- rH 4- U0 0d 0 0 > 2- g) a -- 2I ~ (0 4-) o 2 4-) ) 4-) 4 a)) >1 0) 4- Ui Q (1) 4- S 4U) 0 a4 o oco U u~ 5 ~ a) >1 a 4- 0 Fi )a) ( -H 4.-H 0 - 1 nH a)U (d Q i-4 -- H 21 4-) 4-) c Cd 0 4-) N) Q0 0 >M 0 >1 0 >D > C; 0; r-; C; o1 0 >1 0 0 >1 0 N1> 0 1 4-) LC)D co oQ0 a -H 0 0 0 0 0 I >1 =d r-H ) =d a) a) 4-) u 4-) u 4-) u 4-) r-Hl 4-) - co ( >1 co >1 co >1 co c (1) >1 n-d 4I-) 0 n-d 4-) 0 n-d 4-) N 4-~)P 4-) 4-) >1 a1) -H >1 a1) -H >1 a1) - a1)4 I- LO co 0 0 0 0 a m co L) C Q 44 xC 0 > 0 4-) 4-) 0 u (N (N coLO (N (N >1 a >1 r- a5 -(1 0 Q r- 0 4-) u 0 >1 I mi (NN S 0 0 0 4~ H 0 =dH 0 0 CC) -(I >1>1Sd 1 4-) >1 0 0 >1 (1) co =d co - co c (1a) =d Q2 =d 4-) >1 (1) -H =d n-H ) U- u4) u u 5d 52 0 U O-4 -H) - r-H CDO H~ 0 -H U~ ) - -1 U) a) N u 4-) -H 4-) 0 u M(N Q0u (YD (YN 0 CD C;H C; ; co w 0 0 r-H a)~ ) >1 0 0 >1> 00 > >1 0 0 r-H m2L 0 0 a) 0 >1 Q >1 CD - a) r- v- 0I 0co S ( C; a; C; LC) (1) LO >1 a)0) 0 0 0 0J 4 0 >1 >1 1 ~>> ~~~> co ~- > u~~ 4-) -H- 4)C 4-) 4-)) 4-) >1)_ ~ I)-I) a 0 d -H) (N (1) -H o- HC 0 =d a)u Cd m 0 S a) Cd -)> U~~~- 0H[4 ~H ( ~ [0095] According to the results of Table 6, it was demonstrated that the flying-insect pest repellent product of the present invention (a molded silicone rubber product with a hardness of 5 no more than 50 degrees which contains the flying-insect pest repellent aroma chemical composition containing the flying insect pest repellent aroma chemical, and preferably additionally a repellent effect sustaining component, with the average rate of vaporization and discharge of the flying 10 insect pest repellent aroma chemical component being about 0.05-1.0 mg/cm 2 -h throughout all surface area of the molded silicone rubber article when the molded silicone rubber article was put on a portion of the human body, such as the wrist, ankle, etc., while a portion of the molded silicone 15 rubber article was expanded), has a good flying-insect pest repellent effect in the test after five hours of vaporization and discharge. Also, when an acetic acid ester compound represented by the general formula (I) which is the component (a) of the flying-insect pest repellent aroma chemical 20 component, and/or an allyl ester compound represented by the general formula (II) which is the component (a) of the flying insect pest repellent aroma chemical component, and a monoterpene alcohol and/or an aromatic alcohol having 10 carbons which is the component (b) of the flying-insect pest 25 repellent aroma chemical component, were used in combination, 61 and the blend ratio of the component (a) to the component (b) was 0.1-2.0, the repellent effect sustaining component had a more efficient action, and not only the repellency rate but also the fragrance sustainability were satisfactory. 5 [0096] Moreover, the molded silicone rubber article is configured so that when the molded silicone rubber article is put on a portion of the human body, such as the wrist, ankle, etc., while a portion of the molded silicone rubber article 10 was expanded, the area of the molded rubber article where the molded rubber article is in contact with a portion of the human body is no more than 80% of the area of the inner surface of the molded rubber article, preferably no more than 70%. Therefore, the molded rubber article was put on the wrist 15 or ankle while at least 20%, preferably 30%, of the molded rubber article was separated from the skin of the wrist or ankle, which was preferable in terms of stability of an improvement in vaporization and discharge. [0097] 20 Note that if, as in Example 21, the average rate of vaporization and discharge is less than 0.05 mg/cm 2 -h, the repellent effect is low. On the other hand, if, as in Example 22, the average rate of vaporization and discharge exceeds 1.0 mg/cm 2 -h, the sustainability of the repellent effect tends to 25 decrease. Therefore, it was demonstrated that the vapor 62 pressure of the glycol and/or glycol ether repellent effect sustaining component at 20 0 C is preferably within the range of 0.2-20 Pa. [0098] 5 In contrast to this, in Comparative Example 3 in which a molded silicone rubber article having a hardness of more than 50 degrees was used, the repellent effect was poor. Also, in Comparative Example 4 in which mint oil, which is not considered to be a flying-insect pest repellent aroma 10 chemical, was used, the repellent effect was not sufficient. [0099] Therefore, it is clear that the flying-insect pest repellent product of the present invention which is a molded silicone rubber article containing a combination of a flying 15 insect pest repellent aroma chemical component, and preferably additionally a repellent effect sustaining component, has good practical utility. INDUSTRIAL APPLICABILITY 20 [0100] The flying-insect pest repellent product and method of the present invention can be used for the purpose of controlling a wide variety of insect pests in addition to flying insect pests. 25 63 REFERENCE SIGNS LIST [0101] 1 MOLDED SILICONE RUBBER ARTICLE 2 WRIST 5 3 SEPARATION PORTION 4 BRANCH PORTION 64

Claims

1. A flying-insect pest repellent product which is a molded rubber article containing silicone rubber and having a 5 hardness of no more than 50 degrees, the molded rubber article holding a flying-insect pest repellent aroma chemical composition containing a flying-insect pest repellent aroma chemical component. 10

2. The flying-insect pest repellent product of claim 1, wherein the molded rubber article is an annular molded rubber article having an elastic annular portion configured to be put around or attached to a portion of the human body or an 15 object, and the flying-insect pest repellent aroma chemical component vaporizes and discharges from a surface of the annular molded rubber article.

3. The flying-insect pest repellent product of claim 20 2, wherein when the annular portion is put around or attached to the portion of the human body or the object, the flying-insect pest repellent aroma chemical component vaporizes and discharges over 5-15 hours. 25 65

4. The flying-insect pest repellent product of claim 3, wherein an average rate of vaporization and discharge of the flying-insect pest repellent aroma chemical component is 0.05 5 1.0 mg/cm2 -h throughout all surface area of the annular molded rubber article.

5. The flying-insect pest repellent product of claim 3 or 4, wherein 10 when the annular portion is put around or attached to the portion of the human body or the object, the area of the annular portion where the annular portion is in contact with the portion of the human body or the object is no more than 80% of the area of an inner surface of the annular portion. 15

6. The flying-insect pest repellent product of any one of claims 1-5, wherein the flying-insect pest repellent aroma chemical composition contains, as the flying-insect pest repellent 20 aroma chemical component, a component (a) and a component (b), the component (a) is a single acetic acid ester compound or a mixture of acetic acid ester compounds, the acetic acid ester compound being represented by: CH 3 -COO-R1 (I) 25 where R1 is an alcohol residue having 6-12 carbons, and 66 the component (b) is a monoterpene alcohol and/or an aromatic alcohol having 10 carbons.

7. The flying-insect pest repellent product of claim 5 6, wherein the flying-insect pest repellent aroma chemical composition further contains, as the component (a) , a single allyl ester compound or a mixture of allyl ester compounds, the allyl ester compound being represented by: 10 R2-CH 2 -COO-CH 2 -CH=CH 2 (II) where R2 is an alkyl, alkoxy, cycloalkyl, cycloalkoxy, or phenoxy group having 4-7 carbons, and the component (a) is at least one selected from the acetic acid ester compounds and the allyl ester compounds. 15

8. The flying-insect pest repellent product of claim 6 or 7, wherein the blend ratio of the component (a) to the component (b) is 0.1-2.0. 20

9. The flying-insect pest repellent product of any one of claims 6-8, wherein the acetic acid ester compound is at least one selected from the group consisting of p-tert-butylcyclohexyl acetate, 25 o-tert-butylcyclohexyl acetate, p-tert-pentylcyclohexyl 67 acetate, tricyclodecenyl acetate, benzyl acetate, phenylethyl acetate, styralyl acetate, anisyl acetate, cinnamyl acetate, terpinyl acetate, dihydroterpinyl acetate, linalyl acetate, ethyllinalyl acetate, citronellyl acetate, geranyl acetate, 5 neryl acetate, bornyl acetate, and isobornyl acetate.

10. The flying-insect pest repellent product of any one of claims 6-9, wherein the allyl ester compound is at least one selected from 10 the group consisting of allyl hexanoate, allyl heptanoate, allyl octanoate, allyl n-amyloxyacetate, allyl cyclohexylacetate, allyl cyclohexyloxyacetate, and allyl phenoxyacetate. 15

11. The flying-insect pest repellent product of any one of claims 6-10, wherein the monoterpene alcohol and/or the aromatic alcohol having 10 carbons are at least one selected from the group consisting of terpineol, geraniol, dihydromyrcenol, borneol, 20 menthol, citronellol, nerol, linalool, ethyl linalool, thymol, eugenol, and p-menthane-3,8-diol.

12. The flying-insect pest repellent product of any one of claims 6-11, wherein 25 the flying-insect pest repellent aroma chemical 68 composition further contains a glycol and/or glycol ether having a vapor pressure of 0.2-20 Pa at 20 0 C as a repellent effect sustaining component for the flying-insect pest repellent aroma chemical component during vaporization and 5 discharge.

13. The flying-insect pest repellent product of claim 12, wherein the glycol and/or the glycol ether are at least one 10 selected from the group of consisting of benzyl glycol, propylene glycol, dipropylene glycol, tripropylene glycol, 1,3-butylene glycol, hexylene glycol, diethylene glycol monobutyl ether, dipropylene glycol monobutyl ether, and tripropylene glycol monomethyl ether. 15

14. The flying-insect pest repellent product of claim 12 or 13, wherein the glycol is dipropylene glycol. 20

15. The flying-insect pest repellent product of any one of claims 1-14, wherein the annular portion has a contour of a graphic shape or figure. 25

16. The flying-insect pest repellent product of claim 69 15, wherein the annular portion has a branch portion extending outward from the annular portion at at least one point on the contour. 5

17. A flying-insect pest repellent method of using a flying-insect pest repellent product which is a molded rubber article containing silicone rubber and having a hardness of no more than 50 degrees, the molded rubber article holding a 10 flying-insect pest repellent aroma chemical composition containing a flying-insect pest repellent aroma chemical component. 70