WO2023112546A1 - Resin additive masterbatch, synthetic resin composition, and molded object - Google Patents

Abstract

This resin additive masterbatch contains a surface-treated silica, and a hindered amine compound with which the surface-treated silica is impregnated. With respect to a total of 100 parts by mass of the surface-treated silica and the hindered amine compound, the amount of the surface-treated silica is 25-99 parts by mass. The hindered amine compound is represented by general formula (1). The surface-treated silica is surface-treated by a polyol compound.　The polyol compound is preferably at least one selected from the group consisting of alkylene glycols and polyalkylene glycols. (For definitions of R¹ and R², see the description.)

Description

Resin additive masterbatch, synthetic resin composition, and molding

The present invention relates to a resin additive masterbatch containing silica and a hindered amine compound, a synthetic resin composition containing the resin additive masterbatch, and a molded article.

Various resin additives are added to synthetic resins for the purpose of suppressing deterioration and modifying resin properties. Among them, hindered amine compounds obtained by reacting 2,2,6,6-tetramethylpiperidinols with carboxylic acids are effective in suppressing resin deterioration due to light and heat and imparting flame retardancy. It has been known.

However, hindered amine compounds with small molecular weights tend to become liquid. When compounding a liquid resin additive or a resin additive that tends to become liquid into a synthetic resin, special equipment is required to handle the liquid substance, which is more difficult to handle than solid additives. rice field.

As a method for improving the handling of such liquid resin additives or resin additives that tend to become liquid, a technique of manufacturing a masterbatch containing a high concentration of resin additives is known. For example, polyolefin resin, low-melting resin additive, resin additive masterbatch (Patent Document 1) containing specific amounts of organic acid metal salt and fatty acid metal salt, photostabilization by mixing silica and hindered amine compound in a specific procedure A method for producing an agent masterbatch (Patent Document 2) and a light stabilizer composition in which a hindered amine compound is impregnated in silica having a specific water content (Patent Document 3) have been proposed, and the handling of resin additives has been improved. Examples are given.

US2018/0105653A1 US2018/0094108A1 US2016/0237241A1

However, with the technique described in Patent Document 1, only resins that have good compatibility with the resin used in the masterbatch can be blended, and there is a problem that the range of resin selection is narrow. The silica-based masterbatches described in Patent Documents 2 and 3 have the advantage of being able to be mixed with any type of resin. It turned out that there was room.

Therefore, the problem to be solved by the present invention is to provide a resin additive masterbatch containing silica and a hindered amine compound and having good heat resistance.

The present inventors have made intensive studies to solve the above problems, and found that a resin additive masterbatch containing silica surface-treated with a polyol compound and a hindered amine compound having a specific structure solves the above problems. The discovery led to the completion of the present invention.

According to the invention,
A resin additive masterbatch containing surface-treated silica and a hindered amine compound impregnated in the surface-treated silica,
The amount of the surface-treated silica is 25 to 99 parts by mass with respect to a total of 100 parts by mass of the surface-treated silica and the hindered amine compound,
The hindered amine compound is represented by the following general formula (1),
A resin additive masterbatch is provided in which the surface-treated silica is obtained by surface-treating silica with a polyol compound.

In general formula (1), R ¹ is a hydrogen atom, a hydroxy group, an alkyl group having 1 to 30 carbon atoms, a hydroxyalkyl group having 1 to 30 carbon atoms, an alkoxy group having 1 to 30 carbon atoms, or a carbon atom. represents a hydroxyalkoxy group or an oxy radical having a number of 1 to 30, and R ² is an alkyl group having 1 to 30 carbon atoms, an alkenyl group having 2 to 30 carbon atoms, or a group represented by the following general formula (2); show.

In general formula (2), R ³ is a hydrogen atom, a hydroxy group, an alkyl group having 1 to 30 carbon atoms, a hydroxyalkyl group having 1 to 30 carbon atoms, an alkoxy group having 1 to 30 carbon atoms, or a carbon atom. represents a hydroxyalkoxy group or an oxy radical of numbers 1 to 30, and * represents a bond.

In the resin additive masterbatch of the present invention, the polyol compound is preferably one or more selected from the group consisting of alkylene glycol and polyalkylene glycol.

In the resin additive masterbatch of the present invention, the polyol compound preferably contains polyethylene glycol.

In the resin additive masterbatch of the present invention,
The hindered amine compound is preferably a compound represented by the following general formula (3).

In general formula (3), R ⁴ and R ⁵ each independently represent an alkyl group having 1 to 30 carbon atoms or a hydroxyalkyl group having 1 to 30 carbon atoms.

In the resin additive masterbatch of the present invention,
Further, the benzoate compound represented by the following general formula (4) is added to the benzoate compound in which the mass ratio (former/latter) of the hindered amine compound represented by the general formula (1) and the benzoate compound is 1/4 to 4/1. It is preferable to contain so as to fall within the range.

In general formula (4), R ⁶ and R ⁷ each independently represent a hydrogen atom, a linear or branched alkyl group having 1 to 12 carbon atoms or an arylalkyl group having 7 to 30 carbon atoms, R ⁸ represents an alkyl group having 8 to 30 carbon atoms.

The present invention also provides a synthetic resin composition obtained by blending the resin additive masterbatch into a synthetic resin.

In the synthetic resin composition of the present invention,
The content of the hindered amine compound is preferably 0.01 to 10 parts by mass with respect to 100 parts by mass of the synthetic resin.

The present invention also provides a molded article obtained by molding the synthetic resin composition.

According to the present invention, it is possible to provide a resin additive masterbatch containing silica and a hindered amine compound and having good heat resistance. Further, it is possible to provide a synthetic resin composition containing the resin additive masterbatch, and a molded article obtained by molding the synthetic resin composition.

BEST MODE FOR CARRYING OUT THE INVENTION Hereinafter, embodiments of the present invention will be described in detail.
<Resin additive masterbatch>
The resin additive masterbatch of the present invention is obtained by impregnating surface-treated silica with a hindered amine compound. The term "impregnation" as used in the present invention means impregnation of solid pores with a liquid or adherence of fine particles to solid pores. Impregnating the pores of the solid with a liquid includes permeating the pores of the solid with the liquid or filling the pores of the solid with the liquid.

The surface-treated silica contained in the resin additive masterbatch of the present invention is such that silica (hereinafter also referred to as "(a1) component" or "(a1) silica") is a polyol compound (hereinafter "(a2) component" or Also referred to as "(a2) polyol compound"). The surface-treated silica is hereinafter also referred to as "(A) component" or "(A) surface-treated silica".

Silica comes in natural and synthetic products, each with crystalline and amorphous properties. Examples of natural crystalline silica include quartz, crystal, and silica sand, and examples of natural amorphous silica include diatomaceous earth and acid clay. Synthetic products include amorphous silica such as dry silica, wet silica and silica gel. As (a1) silica in the present invention, silica having a neutral pH of about 6 to 8 is preferable from the viewpoint of being inexpensive and not inhibiting the performance of additives blended together with the resin. In addition, synthetic silica is preferable because it is easy to control the average particle size and pore volume.

Although the water content of (a1) silica is not particularly limited, it is preferably 7% by mass or less. If it is more than 7% by mass, foaming may occur during molding of a resin composition or the like containing them. The water content of silica can be easily adjusted by placing it in a humidity-controlled environment, but it can also be adjusted by drying with a vacuum or heat source.

(a1) The average particle size of silica varies depending on the use of the molded article, but is preferably 0.1 to 100 μm, more preferably 0.3 to 50 μm, and still more preferably 0.5 to 30 μm. If the average particle size is larger than the above range, the dispersibility in the resin may deteriorate and the physical properties of the resin may be reduced. be. According to ISO-13320 standard, the sample is dispersed with ultrasonic waves built into the device, the volume particle size distribution is measured by laser diffraction method, and the 50% cumulative particle size (D50) is taken as the average particle size.

(a1) The method for synthesizing silica is not particularly limited, but silica obtained by a known synthesis method can be used. Specific synthesis methods include, for example, a method of burning silicon tetrachloride in an oxygen or hydrogen flame, a method of obtaining silicon tetrachloride from by-products generated during the production of metallic silicon, and a method of using sodium silicate and mineral acids (sulfuric acid, hydrochloric acid, etc.). Examples include a method of neutralization reaction, a method of hydrolysis of alkoxysilane, and the like. Silica with different particle size, surface structure, pore state, etc. can be obtained by selecting reaction conditions.

(a2) The polyol compound is a compound having two or more hydroxy groups in the molecule.
Examples of the (a2) polyol compound include 1,2-propylene glycol, 1,3-propylene glycol, 1,2-butylene glycol, 1,3-butylene glycol, 1,4-butylene glycol, and 1,6-hexanediol. , 1,12-dodecamethylene glycol; polyalkylene glycols such as diethylene glycol, triethylene glycol, polyethylene glycol, dipropylene glycol, tripropylene glycol, polypropylene glycol, dibutylene glycol, polybutylene glycol, polyethylene polypropylene glycol; trihydric or higher polyhydric alcohols such as glycerin, diglycerin, triglycerin, polyglycerin, trimethylolpropane, pentaerythritol, dipentaerythritol, sorbitol, and sorbitan; fats such as 1,4-cyclohexanedimethanol and hydrogenated bisphenol A; Cyclic diols; bisphenols such as bisphenol A, bisphenol F and bisphenol S; and the like, and alkylene oxide adducts thereof may also be used. Among these, alkylene glycol or polyalkylene glycol is preferable from the viewpoint of excellent heat resistance and flame retardancy, and alkylene glycol having 2 to 4 carbon atoms or polyalkylene glycol having an alkylene group having 2 to 4 carbon atoms. is more preferred, and polyethylene glycol is particularly preferred. The (a2) polyol compound may be used alone or in combination of two or more.

The surface treatment method is not particularly limited, and examples thereof include a method of mixing (a1) silica and (a2) a polyol compound, a method of spray-drying (a2) a polyol compound to (a1) silica, and then adding and mixing the mixture. mentioned.

Apparatuses used for surface treatment are not particularly limited, and examples thereof include tumbler mixers, Henschel mixers, ribbon blenders, V-type mixers, W-type mixers, super mixers, Nauta mixers, and food mixers.
You may heat when surface-treating. The temperature of the (a2) polyol compound during the surface treatment is not particularly limited. It is more preferable that the temperature is higher than 5°C. Thereby, surface treatment can be performed efficiently and uniformly. The temperature during surface treatment is preferably 250° C. or lower, more preferably 200° C. or lower, and even more preferably 150° C. or lower. Thereby, decomposition and volatilization of the (a2) polyol compound can be suppressed.

(A) As the surface-treated silica, for example, a commercially available product such as Carplex CS-701 (manufactured by Evonik) may be used.

In the present invention, excellent flame retardancy can be achieved by impregnating (A) the surface-treated silica with a hindered amine compound represented by the following general formula (1). In the present invention, the hindered amine compound represented by the following general formula (1) is hereinafter also referred to as "component (B)" or "(B) hindered amine compound".

In general formula (1), R ¹ is a hydrogen atom, a hydroxy group, an alkyl group having 1 to 30 carbon atoms, a hydroxyalkyl group having 1 to 30 carbon atoms, an alkoxy group having 1 to 30 carbon atoms, or a carbon atom. represents a hydroxyalkoxy group or an oxy radical having a number of 1 to 30, and R ² is an alkyl group having 1 to 30 carbon atoms, an alkenyl group having 2 to 30 carbon atoms, or a group represented by the following general formula (2); show.

In general formula (2), R ³ is a hydrogen atom, a hydroxy group, an alkyl group having 1 to 30 carbon atoms, a hydroxyalkyl group having 1 to 30 carbon atoms, an alkoxy group having 1 to 30 carbon atoms, or a carbon atom. represents a hydroxyalkoxy group or an oxy radical of numbers 1 to 30, and * represents a bond.

Examples of alkyl groups having 1 to 30 carbon atoms represented by R ¹ and R ² in general formula (1) and R ³ in general formula (2) include methyl, ethyl, propyl and isopropyl. group, butyl group, isobutyl group, sec-butyl group, tert-butyl group, pentyl group, isopentyl group, neopentyl group, tert-pentyl group, hexyl group, isohexyl group, tert-hexyl group, heptyl group, isoheptyl group, tert -heptyl group, octyl group, isooctyl group, tert-octyl group, 2-ethylhexyl group, nonyl group, isononyl group, decyl group, isodecyl group, 2-propylheptyl group, undecyl group, isoundecyl group, dodecyl group, isododecyl group, tridecyl group, isotridecyl group, tetradecyl group, hexadecyl group, octadecyl group, nonadecyl group, eicosyl group, henicosyl group, docosyl group, tricosyl group, tetracosyl group, pentacosyl group, hexacosyl group, heptacosyl group, octacosyl group, nonacosyl group, triacontyl group linear or branched alkyl groups such as

Examples of hydroxyalkyl groups having 1 to 30 carbon atoms represented by R ¹ in general formula (1) and R ³ in general formula (2) include 2-hydroxyethyl group, 2-hydroxypropyl group, Hydroxyalkyl groups corresponding to the above alkyl groups, such as 3-hydroxypropyl group and 2-hydroxy-2-methylpropyl group.

Examples of alkoxy groups having 1 to 30 carbon atoms represented by R ¹ in general formula (1) and R ³ in general formula (2) include methoxy, ethoxy, propoxy, butoxy, octoxy, linear or branched alkoxy groups corresponding to the aforementioned alkyl groups, such as groups, 2-ethylhexyloxy groups, undecanoxy groups, octadecanoxy groups, and the like.

Examples of hydroxyalkoxy groups having 1 to 30 carbon atoms represented by R ¹ in general formula (1) and R ³ in general formula (2) include hydroxyethoxy, 2-hydroxypropoxy, 3- Hydroxypropoxy group, 4-hydroxybutoxy group, 2-hydroxy-2-methylpropoxy group, 6-hydroxyhexyloxy group and the like.

Examples of the alkenyl group having 2 to 30 carbon atoms represented by R ² in the general formula (1) include vinyl group, propenyl group, butenyl group, hexenyl group and oleyl group. The position of the double bond may be α-position, internal or ω-position.

From the viewpoint of performance as a resin additive, R ¹ in general formula (1) and R ³ in general formula (2) are a hydrogen atom, an alkyl group having 1 to 30 carbon atoms, or a An alkoxy group of 30 is preferred, a hydrogen atom, an alkyl group having 1 to 22 carbon atoms or an alkoxy group having 1 to 22 carbon atoms is more preferred, and a hydrogen atom, a methyl group and an alkoxy group having 1 to 14 carbon atoms are further preferred. more preferred.

R ² in general formula (1) is preferably an alkyl group having 1 to 26 carbon atoms or a group represented by general formula (2), and an alkyl group having 8 to 22 carbon atoms or general formula A group represented by (2) is more preferable.
R ¹ and R ² may be the same or different. R ¹ and R ³ may be the same or different.

The hindered amine compound (B) is preferably a compound represented by the following general formula (3).

In general formula (3), R ⁴ and R ⁵ each independently represent an alkyl group having 1 to 30 carbon atoms or a hydroxyalkyl group having 1 to 30 carbon atoms.

The alkyl group having 1 to 30 carbon atoms or the hydroxyalkyl group having 1 to 30 carbon atoms represented by R ⁴ and R ⁵ in general formula (3) is R ¹ in general formula (1). Examples thereof include the same alkyl groups and hydroxyalkyl groups to be obtained. R ⁴ and R ⁵ may be the same or different.

R ⁴ and R ⁵ in general formula (3) are preferably alkyl groups having 1 to 22 carbon atoms, more preferably alkyl groups having 1 to 14 carbon atoms, from the viewpoint of performance as a resin additive.

More specifically, as the component (B) in the present invention, the following compound No. 1 to No. 7 is mentioned. However, the present invention is not limited by the following compounds.

The (B) component in the present invention is the compound No. 1 to No. It is preferably one or more selected from the group of 7. Among these, compound No. 1 is preferred because it can sufficiently obtain the effects of weather resistance and flame retardancy when blended in a synthetic resin composition. 1, No. 2, No. 3, and no. more preferably one or more selected from the group No. 6; 6 is even more preferred.

Although the melting point of the component (B) is not particularly limited, it is preferably 60° C. or lower, more preferably 55° C. or lower, in order to sufficiently obtain the effect of facilitating impregnation with silica, and is liquid at room temperature. It is even more preferable to have 25 degreeC is mentioned as normal temperature. The melting point is measured as an endothermic peak temperature when the temperature is raised at 2° C./min in a nitrogen atmosphere using a differential scanning calorimeter (DSC).

A conventionally known method can be used as a method for producing the hindered amine compound which is the component (B) in the present invention. A method of reacting with an alcohol having a nol skeleton is included. Further, for example, direct esterification of acid and alcohol, reaction of acid halide and alcohol, esterification by transesterification reaction, etc. can also be mentioned, and purification methods include distillation, recrystallization, using a filtering material or an adsorbent. A method or the like can be used as appropriate.

The resin additive masterbatch of the present invention may contain one or more hindered amine compounds as component (B).

The content of components (A) and (B) in the resin additive masterbatch of the present invention is 25 to 99 parts by mass of component (A), with the total of components (A) and (B) being 100 parts by mass. parts, and component (B) is 1 to 75 parts by mass. Component (A) is preferably 30 parts by mass or more, more preferably 35 parts by mass or more, in 100 parts by mass of the total amount of components (A) and (B) in the resin additive masterbatch. Further, component (B) is preferably 20 parts by mass or more, more preferably 25 parts by mass or more, in 100 parts by mass of the total amount of components (A) and (B) in the resin additive masterbatch. From these points, the total amount of 100 parts by mass of components (A) and (B) in the resin additive masterbatch is preferably 30 to 80 parts by mass of component (A) and 20 to 70 parts by mass of component (B). more preferably 35 to 75 parts by mass of component (A) and 25 to 65 parts by mass of component (B). By setting the contents of component (A) and component (B) within this range, it is possible to obtain a resin additive masterbatch that contains component (B) at a sufficiently high concentration and is difficult to bleed. By combining component A) and component (B), an excellent effect of improving heat resistance and flame retardancy can be exhibited.

The resin additive masterbatch of the present invention may contain components other than (A) the surface-treated silica and (B) the hindered amine compound within a range that does not impair the effects of the present invention. As the other component, any additive described later as a component that can be blended in the synthetic resin composition of the present invention can be used.

The resin additive masterbatch of the present invention preferably contains a benzoate compound represented by the following general formula (4) as the (C) component. Thereby, the effect of the (B) hindered amine compound as a light stabilizer can be improved.

In general formula (4), R ⁶ and R ⁷ each independently represent a hydrogen atom, a linear or branched alkyl group having 1 to 12 carbon atoms or an arylalkyl group having 7 to 30 carbon atoms, R ⁸ represents an alkyl group having 8 to 30 carbon atoms.

In the general formula (4), the alkyl group having 1 to 12 carbon atoms represented by R ⁶ and R ⁷ includes groups having 1 to 12 carbon atoms among the groups exemplified as the alkyl group represented by R ¹ above. Examples of arylalkyl groups having 7 to 30 carbon atoms include benzyl, phenylethyl and 1-methyl-1-phenylethyl groups.

In general formula (4), the alkyl group having 8 to 30 carbon atoms represented by R ⁸ includes those having 8 to 30 carbon atoms among the groups exemplified as the alkyl group represented by R ¹ above. is mentioned.

The content of component (C) is such that the mass ratio of component (B) to component (C) (former/latter) is preferably in the range of 1/4 to 4/1, preferably 1/3 to 3/1. A range of amounts is more preferred.

The (C) component may be impregnated with the (A) component, or may be mixed with the (A) component impregnated with the (B) component.

As described above in the resin additive masterbatch of the present invention, the component (C) may or may not be contained, but the components (A), (B) and (C) in the resin additive masterbatch ) is preferably 50 parts by mass or more, more preferably 75 parts by mass or more, and even more preferably 85 parts by mass or more, based on 100 parts by mass of the resin additive masterbatch, Particularly preferably, it is 95 parts by mass or more. When the resin additive masterbatch does not contain component (C), the total content referred to herein is the total content of components (A) and (B). As a result, deterioration of the mechanical properties of the synthetic resin composition containing the resin additive masterbatch can be suppressed.

In addition, the resin additive masterbatch of the present invention can contain commonly used resin additives. Examples of the resin additives include phenol antioxidants, phosphorus antioxidants, thioether antioxidants, ultraviolet absorbers, hindered amine light stabilizers other than component (B), nucleating agents, flame retardants, Flame retardant aids, lubricants, fillers, metal soaps, hydrotalcites, antistatic agents, pigments, dyes, neutralizers and the like can be used. These resin additives may be contained in the resin additive masterbatch of the present invention, or may be added to the synthetic resin separately from the resin additive masterbatch of the present invention. These resin additives may be impregnated with the component (A) or may be mixed with the component (A) impregnated with the component (B).

Phenolic antioxidants include, for example, 2,6-di-tert-butyl-p-cresol, 2,6-diphenyl-4-octadecyloxyphenol, distearyl (3,5-di-tert-butyl- 4-hydroxybenzyl)phosphonate, 1,6-hexamethylenebis[(3,5-di-tert-butyl-4-hydroxyphenyl)propionamide], 4,4′-thiobis(6-tert-butyl-m -cresol), 2,2′-methylenebis(4-methyl-6-tert-butylphenol), 2,2′-methylenebis(4-ethyl-6-tert-butylphenol), 4,4′-butylidenebis(6-tert -butyl-m-cresol), 2,2′-ethylidenebis(4,6-di-tert-butylphenol), 2,2′-ethylidenebis(4-sec-butyl-6-tert-butylphenol), 1, 1,3-tris(2-methyl-4-hydroxy-5-tert-butylphenyl)butane, 1,3,5-tris(2,6-dimethyl-3-hydroxy-4-tert-butylbenzyl)isocyanurate , 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl) isocyanurate, 1,3,5-tris(3,5-di-tert-butyl-4-hydroxybenzyl) -2,4,6-trimethylbenzene, 2-tert-butyl-4-methyl-6-(2-acryloyloxy-3-tert-butyl-5-methylbenzyl)phenol, stearyl (3,5-di-tert -butyl-4-hydroxyphenyl) propionate, pentaerythritol tetrakis [3-(3,5-di-tert-butyl-4-hydroxyphenyl) propionate], thiodiethylene glycol bis [(3,5-di-tert-butyl- 4-hydroxyphenyl)propionate], 1,6-hexamethylenebis[(3,5-di-tert-butyl-4-hydroxyphenyl)propionate], bis[3,3-bis(4-hydroxy-3-tert -butylphenyl)butyric acid]glycol ester, bis[2-tert-butyl-4-methyl-6-(2-hydroxy-3-tert-butyl-5-methylbenzyl)phenyl]terephthalate, 1,3,5 -tris[(3,5-di-tert-butyl-4-hydroxyphenyl)propionyloxyethyl]isocyanurate, 3,9-bis[1,1-dimethyl-2-{(3-tert-butyl-4- Hydroxy-5-methylphenyl)propionyloxy}ethyl]-2,4,8,10-tetraoxaspiro[5,5]undecane, triethylene glycol bis[(3-tert-butyl-4-hydroxy-5-methyl phenyl) propionate] and the like. When using these phenolic antioxidants, the content of the phenolic antioxidant is 0.001 per 100 parts by mass of the synthetic resin that is the component (D) when the synthetic resin composition described later is produced. It is preferably in an amount of up to 10 parts by mass, and more preferably in an amount of 0.01 to 0.5 parts by mass.

Examples of phosphorus antioxidants include tris(nonylphenyl) phosphite, tris[2-tert-butyl-4-(3-tert-butyl-4-hydroxy-5-methylphenylthio)-5-methylphenyl ] Phosphite, tridecylphosphite, octyldiphenylphosphite, didecylmonophenylphosphite, bis(tridecyl)pentaerythritol diphosphite, bis(nonylphenyl)pentaerythritol diphosphite, bis(2,4-di- tert-butylphenyl)pentaerythritol diphosphite, bis(2,6-di-tert-butyl-4-methylphenyl)pentaerythritol diphosphite, bis(2,4,6-tri-tert-butylphenyl)penta Erythritol diphosphite, bis(2,4-dicumylphenyl)pentaerythritol diphosphite, tetrakis(tridecyl)isopropylidene diphenol diphosphite, tetrakis(tridecyl)-4,4'-n-butylidene bis(2-tert -butyl-5-methylphenol) diphosphite, hexakis(tridecyl)-1,1,3-tris(2-methyl-4-hydroxy-5-tert-butylphenyl)butane triphosphite, tetrakis(2,4-di- tert-butylphenyl)biphenylenediphosphonite, 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide, 2,2′-methylenebis(4,6-tert-butylphenyl)-2 -ethylhexylphosphite, 2,2'-methylenebis(4,6-tert-butylphenyl)-octadecylphosphite, 2,2'-ethylidenebis(4,6-di-tert-butylphenyl)fluorophosphite, tris (2-[(2,4,8,10-tetrakis-tert-butyldibenzo[d,f][1,3,2]dioxaphosphepin-6-yl)oxy]ethyl)amine, 2-ethyl Phosphite of -2-butylpropylene glycol and 2,4,6-tri-tert-butylphenol. The amount of these phosphorus antioxidants used is 0.001 to 10 parts by mass of the phosphorus antioxidant with respect to 100 parts by mass of the synthetic resin that is the component (D) when the synthetic resin composition described later is produced. The amount is preferably 0.01 to 0.5 parts by mass, more preferably 0.01 to 0.5 parts by mass.

Examples of thioether antioxidants include dialkylthiodipropionates such as dilauryl thiodipropionate, dimyristyl thiodipropionate, and distearyl thiodipropionate, and pentaerythritol tetrakis (β-alkylmercaptopropionates These thioether-based antioxidants are used in an amount of 0.00 to 100 parts by mass of the synthetic resin as component (D) when the synthetic resin composition described later is produced. 001 to 10 parts by mass, and more preferably 0.01 to 0.5 parts by mass.

UV absorbers include, for example, 2,4-dihydroxybenzophenone, 2-hydroxy-4-methoxybenzophenone, 2-hydroxy-4-octoxybenzophenone, 5,5′-methylenebis(2-hydroxy-4-methoxybenzophenone) 2-hydroxybenzophenones such as; 2-(2′-hydroxy-5′-methylphenyl)benzotriazole, 2-(2′-hydroxy-3′,5′-di-tert-butylphenyl)-5-chloro benzotriazole, 2-(2'-hydroxy-3'-tert-butyl-5'-methylphenyl)-5-chlorobenzotriazole, 2-(2'-hydroxy-5'-tert- octylphenyl)benzotriazole, 2-(2'-hydroxy-3',5'-dicumylphenyl)benzotriazole, 2,2'-methylenebis(4-tert-octyl-6-(benzotriazolyl) 2-(2'-hydroxyphenyl)benzotriazoles such as phenol), 2-(2'-hydroxy-3'-tert-butyl-5'-carboxyphenyl)benzotriazole; phenyl salicylate, resorcinol monobenzoate, 2, 4-di-tert-butylphenyl-3,5-di-tert-butyl-4-hydroxybenzoate, 2,4-di-tert-amylphenyl-3,5-di-tert-butyl-4-hydroxybenzoate and the like benzoates of; substituted oxanilides such as 2-ethyl-2'-ethoxyoxanylide and 2-ethoxy-4'-dodecyloxanilide; ethyl-α-cyano-β, β-diphenylacrylate, methyl-2- Cyanoacrylates such as cyano-3-methyl-3-(p-methoxyphenyl)acrylate; 2-(2-hydroxy-4-octoxyphenyl)-4,6-bis(2,4-di-tert-butyl phenyl)-s-triazine, 2-(2-hydroxy-4-methoxyphenyl)-4,6-diphenyl-s-triazine, 2-(2-hydroxy-4-propoxy-5-methylphenyl)-4,6 -Triaryltriazines such as bis(2,4-di-tert-butylphenyl)-s-triazine. The amount of these ultraviolet absorbers to be used is 0.001 to 10 parts by mass of the ultraviolet absorber with respect to 100 parts by mass of the synthetic resin that is the component (D) when the synthetic resin composition described later is produced. and more preferably 0.01 to 0.5 parts by mass.

Examples of hindered amine light stabilizers other than component (B) include 2,2,6,6-tetramethyl-4-piperidyl benzoate and bis(2,2,6,6-tetramethyl-4-piperidyl) sebacate. , bis(1,2,2,6,6-pentamethyl-4-piperidyl) sebacate, tetrakis(2,2,6,6-tetramethyl-4-piperidyl)-1,2,3,4-butanetetracarboxy tetrakis(1,2,2,6,6-pentamethyl-4-piperidyl)-1,2,3,4-butanetetracarboxylate, bis(2,2,6,6-tetramethyl-4-piperidyl) )·bis(tridecyl)-1,2,3,4-butanetetracarboxylate, bis(1,2,2,6,6-pentamethyl-4-piperidyl)·bis(tridecyl)-1,2,3, 4-butane tetracarboxylate, bis(1,2,2,6,6-pentamethyl-4-piperidyl)-2-butyl-2-(3,5-di-tert-butyl-4-hydroxybenzyl)malonate, 1-(2-hydroxyethyl)-2,2,6,6-tetramethyl-4-piperidinol/diethyl succinate polycondensate, 1,6-bis(2,2,6,6-tetramethyl- 4-piperidylamino)hexane/2,4-dichloro-6-morpholino-s-triazine polycondensate, 1,6-bis(2,2,6,6-tetramethyl-4-piperidylamino)hexane/2, 4-dichloro-6-tert-octylamino-s-triazine polycondensate, 1,5,8,12-tetrakis[2,4-bis(N-butyl-N-(2,2,6,6-tetra methyl-4-piperidyl)amino)-s-triazin-6-yl]-1,5,8,12-tetraazadodecane, 1,5,8,12-tetrakis[2,4-bis(N-butyl- N-(1,2,2,6,6-pentamethyl-4-piperidyl)amino)-s-triazin-6-yl]-1,5,8-12-tetraazadodecane, 1,6,11-tris [2,4-bis(N-butyl-N-(2,2,6,6-tetramethyl-4-piperidyl)amino)-s-triazin-6-yl]aminoundecane, 1,6,11-tris [2,4-bis(N-butyl-N-(1,2,2,6,6-pentamethyl-4-piperidyl)amino)-s-triazin-6-yl]aminoundecane, bis(2,2, 6,6-tetramethyl-1-octyloxy-4-piperidyl)decanedioate, BASF TINUVIN NOR 371, and the like. The amount of these hindered amine light stabilizers used is preferably 0.001 to 30 parts by mass, more preferably 0.01 to 10 parts by mass, with respect to 100 parts by mass of the synthetic resin that is component (D). is more preferred.

In the resin additive masterbatch of the present invention, when components other than (A) to (C) are blended, the total blending amount should be 200 parts by mass or less per 100 parts by mass of component (A). is preferred.
From the viewpoint of maximizing the concentration of active ingredients in the resin additive masterbatch of the present invention, the resin additive masterbatch of the present invention contains substantially only components (A) and (B), preferably contains only components (A), (B) and (C). Substantially only (A) component and (B) component, and substantially only (A) component, (B) component and (C) component are components other than (A), (B) and (C) It is preferred to mean that the amount of the components is for example 1% by weight or less in total, more preferably 0.1% by weight or less in the masterbatch. Most preferably, the resin additive masterbatch contains only components (A) and (B), or contains only components (A), (B) and (C).

(B) The method for impregnating (A) the surface-treated silica with the hindered amine compound includes, for example, the following method. However, the present invention is not limited by these methods. Also, (B) the hindered amine compound may be mixed with (C) the benzoate compound.
Method 1. A method of mixing the (B) hindered amine compound, which is optionally heated to a liquid state, with the (A) surface-treated silica under atmospheric pressure or vacuum to impregnate the (A) surface-treated silica.
Method 2. A method of mixing a solid (B) hindered amine compound with (A) a surface-treated silica and allowing the solid to be adsorbed/sorbed onto the (A) surface-treated silica under atmospheric pressure or vacuum.
Method 3. (B) A method of mixing a solution of a hindered amine compound in a solvent with (A) surface-treated silica, impregnating (A) surface-treated silica under atmospheric pressure or vacuum, and then distilling off the solvent.
Method 4. (B) A method in which a hindered amine compound is carried on the surface of (A) the surface-treated silica, and pressure is applied to move and adsorb the (B) hindered amine compound inside the pores of the (A) surface-treated silica.
Method 5. (B) A method of evaporating a hindered amine compound and adsorbing and impregnating (A) the surface-treated silica in a gaseous state. Method 6. (A) A method of synthesizing (B) a hindered amine compound in the presence of a surface-treated silica and impregnating (A) the surface-treated silica with the (B) hindered amine compound as a product.

Among the above, methods 1, 2, and 3 are preferred, methods 1 and 2 are more preferred, and method 1 is even more preferred, since the operation is simple.

In the present invention, (A) surface-treated silica is preferably impregnated with (B) hindered amine compound as uniformly as possible. In addition, (A) the surface-treated silica is preferably subjected to pretreatment such as drying and classification so that it can be easily impregnated with (B) the hindered amine compound. Impregnation may also be performed under vacuum so that there is no air in the pores of the silica.

The apparatus for producing the resin additive masterbatch of the present invention is not particularly limited, and various types of mixers, stirring tanks, tumbling tanks, and the like can be used. These devices may be accompanied by a heating/cooling device, a decompression device, a stirring device, a raw material recovery mechanism, an inert gas supply device, and the like.
Impregnation can be carried out batchwise, semi-batchwise or continuously.

The 3% weight loss temperature of the resin additive masterbatch is preferably higher than 230°C, preferably 235°C or higher, more preferably 240°C or higher, particularly preferably 250°C or higher, and 260°C or higher. Most preferred. It is preferable that the upper limit is 400° C. or less. The 3% weight loss temperature of the resin additive masterbatch can be measured by the method described in Examples.

<Synthetic resin composition>
The synthetic resin composition is obtained by blending the resin additive masterbatch of the present invention with component (D): a synthetic resin, particularly preferably a thermoplastic resin.

Specific examples of the thermoplastic resin include polypropylene, high-density polyethylene, low-density polyethylene, linear low-density polyethylene, crosslinked polyethylene, ultra-high molecular weight polyethylene, polybutene-1, poly-3-methylpentene, poly-4- α-olefin polymers such as methylpentene, polyolefin resins and olefin copolymers such as ethylene-vinyl acetate copolymer, ethylene-ethyl acrylate copolymer, ethylene-propylene copolymer; polyvinyl chloride, polyvinylidene chloride , chlorinated polyethylene, chlorinated polypropylene, polyvinylidene fluoride, chlorinated rubber, vinyl chloride-vinyl acetate copolymer, vinyl chloride-ethylene copolymer, vinyl chloride-vinylidene chloride copolymer, vinyl chloride-vinylidene chloride-vinyl acetate Halogen-containing resins such as terpolymers, vinyl chloride-acrylate copolymers, vinyl chloride-maleate copolymers, vinyl chloride-cyclohexylmaleimide copolymers; petroleum resins, coumarone resins, polystyrene, polyacetic acid Copolymers (e.g., AS resins, ABS (Acrylonitrile-butadiene-styrene copolymer) resin, ACS resin, SBS resin, MBS resin, heat-resistant ABS resin, MABS resin, etc.); polymethyl methacrylate, polyvinyl alcohol, polyvinyl formal, polyvinyl butyral; polyethylene terephthalate, polybutylene terephthalate, polycyclohexane Aromatic polyesters such as polyalkylene terephthalates such as dimethylene terephthalate, polyethylene naphthalate, polyalkylene naphthalates such as polybutylene naphthalate, and linear polyesters such as polytetramethylene terephthalate; polyhydroxybutyrate, polycaprolactone, polybutylene succinate degradable aliphatic polyesters such as polylactic acid, polyethylene succinate, polylactic acid, polymalic acid, polyglycolic acid, polydioxane, and poly(2-oxetanone); polyamides and polycarbonates such as polyphenylene oxide, polycaprolactam and polyhexamethylene adipamide , Polycarbonate/ABS resin, branched polycarbonate, polyacetal, polyphenylene sulfide, polyurethane, cellulose resin, polyimide resin, polysulfone, polyphenylene ether, polyetherketone, polyetheretherketone, liquid crystal polymer and other thermoplastic resins and blends thereof can be mentioned. Thermoplastic resins include isoprene rubber, butadiene rubber, acrylonitrile-butadiene copolymer rubber, styrene-butadiene copolymer rubber, fluororubber, silicone rubber, polyolefin thermoplastic elastomer, styrene thermoplastic elastomer, and polyester thermoplastic elastomer. , a nitrile-based thermoplastic elastomer, a nylon-based thermoplastic elastomer, a vinyl chloride-based thermoplastic elastomer, a polyamide-based thermoplastic elastomer, a polyurethane-based thermoplastic elastomer, and the like. In the present invention, these thermoplastic resins may be used alone or in combination of two or more. Also, the thermoplastic resin may be alloyed.

These thermoplastic resins have molecular weight, degree of polymerization, density, softening point, ratio of insolubles in solvents, degree of stereoregularity, presence or absence of catalyst residue, type and blending ratio of raw material monomers, type of polymerization catalyst (eg, Ziegler catalyst, metallocene catalyst, etc.) and the like can be used. Among these thermoplastic resins, one or more selected from the group consisting of polyolefin-based resins, polystyrene-based resins, and olefin- or styrene-copolymers is preferable because the effect of the component (B) is stably exhibited. It is also preferable to use them in combination with a thermoplastic elastomer.

When a polyolefin resin is used as the synthetic resin of the synthetic resin composition of the present invention, a known neutralizing agent is added to neutralize the catalyst residue in the polyolefin resin within a range that does not impair the effects of the present invention. It is preferable to contain. Examples of neutralizing agents include fatty acid metal salts such as calcium stearate, lithium stearate, sodium stearate and magnesium stearate, ethylenebis(stearic acid amide), ethylenebis(12-hydroxystearic acid amide), and stearic acid amide. or inorganic compounds such as hydrotalcite. These neutralizing agents may be used alone or in combination of two or more. The amount of these neutralizing agents used is preferably 0.001 to 3 parts by mass, more preferably 0.01 to 1 part by mass, per 100 parts by mass of the synthetic resin.

The lower limit of the content of component (B) in the synthetic resin composition of the present invention is preferably 0.001 parts by mass or more, preferably 0.01 parts by mass or more, relative to 100 parts by mass of the synthetic resin. More preferably, it is still more preferably 0.03 parts by mass or more. Thereby, the effect of the component (B) is stably exhibited. On the other hand, the upper limit of the content of component (B) is preferably 10 parts by mass or less, more preferably 5 parts by mass or less, and 3 parts by mass or less per 100 parts by mass of the synthetic resin. Even more preferred. As a result, bleeding is less likely to occur on the surface of the synthetic resin composition or the molding described later.

<Molded body>
The molded article of the present invention is obtained by molding the synthetic resin composition of the present invention. The molding method and molding conditions are not particularly limited, and known molding methods and molding conditions can be used. Specific molding methods include extrusion, calendering, injection molding, roll molding, compression molding, blow molding, and rotational molding. can be produced.

The synthetic resin composition of the present invention and its molded article can be used in electricity, electronics, communications, agriculture, forestry and fisheries, mining, construction, food, textiles, clothing, medicine, coal, petroleum, rubber, leather, automobiles, precision equipment, lumber, and building materials. , civil engineering, furniture, printing, musical instruments, etc. More specifically, printers, personal computers, word processors, keyboards, PDAs (small information terminals), telephones, copiers, facsimiles, ECRs (electronic cash registers), calculators, electronic notebooks, cards, holders, stationery, etc. Office equipment, OA equipment, washing machines, refrigerators, vacuum cleaners, microwave ovens, lighting equipment, game machines, irons, household appliances such as kotatsu, TVs, VTRs, video cameras, radio cassette players, tape recorders, mini discs, CD players, speakers, AV equipment such as liquid crystal displays, connectors, relays, capacitors, switches, printed circuit boards, coil bobbins, semiconductor encapsulation materials, LED encapsulation materials, electric wires, cables, transformers, deflection yokes, distribution boards, electrical and electronic parts such as clocks It is also used for housings (frames, cases, covers, exteriors) and parts of communication equipment, OA equipment, etc., and interior and exterior materials for automobiles.

Furthermore, the synthetic resin composition of the present invention and its molded product can be used for seats (filling, outer material, etc.), belts, ceiling coverings, compatible tops, armrests, door trims, rear package trays, carpets, mats, sun visors, foil covers, mattresses. Covers, airbags, insulating materials, straps, straps, wire covering materials, electrical insulating materials, paints, coating materials, facing materials, floor materials, corner walls, carpets, wallpaper, wall covering materials, exterior materials, interior materials Materials, roofing materials, decking materials, wall materials, pillar materials, floorboards, fence materials, frames and moldings, windows and door shapes, shingles, siding, terraces, balconies, soundproofing boards, heat insulating boards, window materials, etc. , automobiles, hybrid cars, electric vehicles, vehicles, ships, aircraft, buildings, housing or construction materials, civil engineering materials, clothing, curtains, sheets, plywood, synthetic fiber boards, carpets, entrance mats, sheets, buckets, hoses, It is used for various purposes such as containers, spectacles, bags, cases, goggles, skis, rackets, tents, musical instruments and other daily necessities, and sporting goods.

Hereinafter, the present invention will be described in detail by way of examples. However, the present invention is by no means limited to the following examples.

Details of each component in Table 1 are shown below.
(A)-1: Synthetic silica (surface treatment: polyethylene glycol, trade name: Carplex CS-701, manufacturer name: Evonik, average particle size: 6.2 μm, water content: 7% by mass or less)
(A)-C1: synthetic silica (surface treatment: none, trade name: Carplex #80, manufacturer name: Evonik, average particle size: 15.0 μm)
(A)-C2: synthetic silica (surface treatment: none, trade name: Carplex CS-7, manufacturer name: Evonik, average particle size: 6.0 μm)
(A)-C3: synthetic silica (surface treatment: dimethyl silicone oil, trade name: Sipernat D10, manufacturer name: Evonik, average particle size: 6.5 μm)
(A)-C4: synthetic silica (surface treatment: dimethyl silicone oil, trade name: Sipernat D17, manufacturer name: Evonik, average particle size: 10.0 μm)
(A)-C5: synthetic silica (surface treatment: organosilicon compound, trade name: Sylophobic 200, manufacturer name: Fuji Silysia Chemical, average particle size: 3.9 μm)
(B)-1: bis(1-undecanoxy-2,2,6,6-tetramethylpiperidin-4-yl) carbonate (liquid at room temperature)
(C)-1: hexadecyl 3,5-bis-tert-butyl-4-hydroxybenzoate (melting point 62° C.)

[Examples 1 to 4, Comparative Examples 1 to 6]
<Production of Resin Additive Masterbatch>
The (B) component was heated to 70°C. For Example 4 and Comparative Example 2, the components (B) and (C) were mixed in the amounts shown in Table 1 and heated to 70° C. to obtain a liquid state. After putting the (A) component in a food mixer, the (B) component or the mixture of the (B) component and the (C) component, which had been preheated to 70° C., was added. The amount of each component was according to the compounding amounts shown in Table 1. After mixing for 60 seconds at 10,500 revolutions/minute, the mixer was stopped, the inner wall of the mixer and the stirring blades were scraped off with a spatula, and the mixture was mixed again for 60 seconds. It was confirmed that the silica particles after mixing were in the form of powder, and that there were no lumps or stickiness. As a result, a resin additive masterbatch comprising the component (B) or the component (B) and the component (C) and the component (A) impregnated with the component was obtained. Those produced with the compositions of Examples 1-4 were designated as "Masterbatches 1-4", respectively, and those produced with the compositions of Comparative Examples 1-6 were designated as "Comparative Masterbatches 1-6", respectively. All of the compounding amounts shown in Table 1 are based on parts by mass.

<Heat resistance evaluation>
For each resin additive masterbatch obtained above, using a thermogravimetric/differential thermal analyzer (Thermo plus EVO, manufactured by Rigaku), under the conditions of a nitrogen flow rate of 200 ml / min and a temperature increase rate of 10 ° C. / min, 30 ° C. to 400° C., and the temperatures at which the weight loss rates reached −3% and −5% were determined. Table 1 shows the results.

[Examples 5 to 8, Comparative Examples 7 to 9]
<Production of synthetic resin composition>
Stearyl (3,5 ^- di- tert-butyl-4-hydroxyphenyl)propionate 0.05 parts by mass, tris(2,4-di-tert-butylphenyl)phosphite 0.05 parts by mass as a phosphorus antioxidant, and calcium stearate as a neutralizing agent 0.05 part by mass was mixed to obtain a polyethylene composition 1.

Each component was mixed in the blending amounts shown in Table 2, and a twin-screw extruder (product name: 2D15W) was connected to Laboplastomill μ manufactured by Toyo Seiki Seisakusho. / min to obtain a resin strand. The resulting resin strand was cut with a pelletizer to obtain a synthetic resin composition in the form of pellets. All of the compounding amounts shown in Table 2 are based on parts by mass.

<Production of test piece>
A cast film having a thickness of 200 μm was produced using the obtained pellet-shaped synthetic resin composition. The film was created using a device in which a single-screw extruder (product name: D1220B) and a T-die (product name: MT60B) were connected to Labo Plastomill μ manufactured by Toyo Seiki Seisakusho Co., Ltd., with a melting temperature of 200 ° C. and a screw speed of The conditions were 30 revolutions/minute, a T-die extrusion temperature of 200°C, a chill roll temperature of 60°C, and a roll rotation speed of 0.40 to 0.45 revolutions/minute. A test piece of 200 mm×50 mm was cut out from the obtained film, left to stand at 23±2° C. and 50±5% RH for 48 hours, and then subjected to the following flame retardancy test.

<Flame Retardancy Evaluation: Horizontal Burning Test>
The test piece prepared above is held horizontally, a Bunsen burner with an inner diameter of 9.5 mm and a flame length of 38 mm is used as a heating source, and an indirect flame is applied to the center of the short side of the film for 15 seconds, and the long side until the flame disappears from the test piece. Directional distance was measured. Each test piece was measured with n=3, and the average value was calculated. Table 2 shows the results.

<Flame retardant evaluation: UL-94VTM>
The test piece prepared above was wound in a cylindrical shape so that the lower ends did not overlap, and the lower end of the sample was separated from the burner by 10 mm and held vertically. A Bunsen burner with an inner diameter of 9.5 mm and a flame length of 20 mm was used as a heating source, and the lower end of the test piece was flamed for 3 seconds, and then the number of burning seconds was measured. After the flame was extinguished, it was again flamed for 3 seconds, and the number of burning seconds was measured. Evaluate flame retardancy according to the evaluation criteria of VTM-0, VTM-1, and VTM-2, and the rank of the test piece that meets the lowest criteria among the number of measurements of n = 5 is the evaluation rank of the resin composition. and Those that did not correspond to any of the ranks of VTM-0 to VTM-2 were given NR (No Rating). Table 2 shows the results.

From the evaluation results of Examples 1 to 4 shown in Table 1, it was found that the resin additive masterbatch of the present invention has excellent heat resistance. The resin additive masterbatches of Comparative Examples 1-6 had a lower weight loss temperature and inferior heat resistance compared to Examples 1-4. In particular, the resin additive masterbatch using non-surface-treated silica (Comparative Examples 1 to 3) had a −3% weight loss temperature of less than 230° C., and was clearly inferior in heat resistance. Such a low heat-resistant resin additive masterbatch causes decomposition and volatilization of the contained components at the processing temperature of polyolefin resin, which is usually 180 to 230 ° C. Not suitable for blending with synthetic resins because it causes processing troubles.

Also, from the evaluation results of Examples 5 to 8 shown in Table 2, it was found that the film produced using the masterbatch of the present invention has excellent flame retardancy. When a resin additive masterbatch using silica with a surface treatment agent different from that of the present invention was blended (Comparative Examples 7 to 9), the flame retardancy was inferior. 

Claims (8)

1. A resin additive masterbatch containing surface-treated silica and a hindered amine compound impregnated in the surface-treated silica,
   The amount of the surface-treated silica is 25 to 99 parts by mass with respect to a total of 100 parts by mass of the surface-treated silica and the hindered amine compound,
   The hindered amine compound is represented by the following general formula (1),
   The resin additive masterbatch, wherein the surface-treated silica is obtained by surface-treating silica with a polyol compound.
   

   

   In general formula (1), R ¹ is a hydrogen atom, a hydroxy group, an alkyl group having 1 to 30 carbon atoms, a hydroxyalkyl group having 1 to 30 carbon atoms, an alkoxy group having 1 to 30 carbon atoms, or a carbon atom. represents a hydroxyalkoxy group or an oxy radical having a number of 1 to 30, and R ² is an alkyl group having 1 to 30 carbon atoms, an alkenyl group having 2 to 30 carbon atoms, or a group represented by the following general formula (2); show.
   

   

   In general formula (2), R ³ is a hydrogen atom, a hydroxy group, an alkyl group having 1 to 30 carbon atoms, a hydroxyalkyl group having 1 to 30 carbon atoms, an alkoxy group having 1 to 30 carbon atoms, or a carbon atom. represents a hydroxyalkoxy group or an oxy radical of numbers 1 to 30, and * represents a bond.
2. The resin additive masterbatch according to claim 1, wherein the polyol compound is one or more selected from the group consisting of alkylene glycol and polyalkylene glycol.
3. The resin additive masterbatch according to claim 2, wherein the polyol compound contains polyethylene glycol.
4. The resin additive masterbatch according to any one of claims 1 to 3, wherein the hindered amine compound represented by the general formula (1) is a compound represented by the following general formula (3).
   

   

   In general formula (3), R ⁴ and R ⁵ each independently represent an alkyl group having 1 to 30 carbon atoms or a hydroxyalkyl group having 1 to 30 carbon atoms.
5. Further, a benzoate compound represented by the following general formula (4) is contained so that the mass ratio (former/latter) of the hindered amine compound and the benzoate compound is in the range of 1/4 to 4/1. Item 5. The resin additive masterbatch according to any one of Items 1 to 4.
   

   

   In general formula (4), R ⁶ and R ⁷ each independently represent a hydrogen atom, a linear or branched alkyl group having 1 to 12 carbon atoms or an arylalkyl group having 7 to 30 carbon atoms, R ⁸ represents an alkyl group having 8 to 30 carbon atoms.
6. A synthetic resin composition obtained by blending the resin additive masterbatch according to any one of claims 1 to 5 with a synthetic resin.
7. The synthetic resin composition according to claim 6,
   A synthetic resin composition, wherein the content of the hindered amine compound is 0.001 to 10 parts by mass with respect to 100 parts by mass of the synthetic resin.
8. A molded article obtained by molding the synthetic resin composition according to claim 6 or 7.