WO2013161843A1 - Light-diffusing resin composition and part molded using same - Google Patents

Abstract

This light-diffusing resin composition contains a transparent resin (X) and cross-linked resin microparticles (Y). The absolute value of the difference between the refraction index of the transparent resin (X) and the refraction index of the cross-linked resin microparticles (Y) is 0.095-0.115. The volume-average grain diameter of the cross-linked resin microparticles (Y) is 1.5-3.3 µm. The variation coefficient when the volume-average grain diameter is measured is no more than 20%. When the cross-linked resin microparticles (Y) are pyrolyzed in a nitrogen-gas environment with the temperature increasing by 10°C/minute. The temperature at which the mass is reduced by half is at least 320°C.

Description

Light diffusing resin composition and molded article thereof

The present invention relates to a light diffusing resin composition and a molded product thereof. More specifically, the present invention relates to a light diffusing resin composition that exhibits good light diffusibility and diffusion efficiency, and is excellent in heat resistance, impact resistance, and flame retardancy, and a molded product thereof.

In a luminaire cover or a liquid crystal display device, a diffusion plate in which a light diffusing agent is dispersed in a matrix made of a transparent resin such as polymethyl methacrylate, polystyrene, and polycarbonate in order to uniformly diffuse light from a light source. It is used. Conventionally, inorganic particles such as crystalline silica, amorphous silica, calcium carbonate, barium sulfate, aluminum hydroxide, and titanium oxide, or inorganic fibers such as glass fibers have been used as the light diffusing agent. However, when a light diffusing agent made of inorganic particles or inorganic fibers is used, there are problems such as a decrease in impact resistance and a problem that light transmittance in the diffusion plate is lowered due to the high reflectance of the light diffusing agent. there were.
On the other hand, a method using polymer fine particles having a refractive index different from that of a transparent resin and having a crosslinked structure as an organic light diffusing agent is also known. As the organic light diffusing agent, for example, crosslinked acrylic particles, crosslinked silicone particles, and crosslinked styrene particles are known.
Organic light diffusing agents are widely used as light diffusing agents because they are superior in surface smoothness of molded articles and have good light diffusibility compared to inorganic light diffusing agents. However, when the addition amount is large, there is a problem that impact resistance and flame retardancy are lowered, and conversely, when the addition amount is reduced considering the cost, the light diffusibility may be insufficient. Are known.

Technologies using organic light diffusing agents have been proposed. Patent Document 1 discloses a light diffusing plate using polymer particles having an average particle size of 3 to 20 μm and a narrow particle size distribution with a CV value of 20% or less as a light diffusing agent. Patent Document 2 discloses that the average particle diameter is 0.6 to 1.5 μm, the standard deviation of the particle diameter is 0.01 μm to 0.5 μm, and the styrene monomer / methacrylic acid copolymer and A light diffusing plate containing a diffusing agent having an absolute value of the refractive index difference of 0.05 or more is disclosed.
Patent Document 3 discloses a composition in which acrylic resin-based fine particles having an average particle size of 1 to 4 μm as a light diffusing agent and having a specific particle size distribution are dispersed in a polycarbonate resin. Further, Patent Document 4 discloses a composition containing crosslinked polymer fine particles having a refractive index different from that of polycarbonate resin and having an average particle diameter in the range of 0.5 to 100 μm.
Patent Document 5 discloses a composition in which polymer fine particles having a refractive index in the range of 1.495 to 1.504 are dispersed in a polycarbonate resin.
Patent Document 6 discloses a composition containing crosslinked resin fine particles comprising a specific (meth) acrylate ester resin having a volume average particle size of 0.7 to 2.5 μm and a narrow particle size distribution. Has been.

JP-A-7-234304 JP 2008-292969 A JP 2011-157536 A JP-A-3-143950 JP 2011-57925 A International Publication No. 2010/24167 Pamphlet

However, with the recent increase in performance of lighting fixtures and displays, there has been an increasing demand for components relating to light diffusion, such as lighting fixture covers and display diffusion plates. In particular, regarding a cover for a lighting fixture, there is a demand for a molding material that exhibits good light diffusibility in a wide range of total light transmittance. Furthermore, there is a demand for a molding material containing a light diffusing agent that can achieve a target light diffusibility (dispersion degree) with a small amount of addition. Here, “dispersion degree” means the amount of transmitted light (emitted light) at θ = 0 (degrees) when a light beam is emitted perpendicularly from the light source 2 onto the surface of the molded body 1 as shown in FIG. Is the θ when the amount of transmitted light (emitted light) is 50.
The light diffusibility of a resin composition in which a light diffusing agent particle is blended with a transparent resin and a molded product made from the resin composition are the refractive index difference between the resin and the light diffusing agent particle, the particle size of the light diffusing agent particle, and the light diffusing agent particle. As the refractive index difference between the resin and the light diffusing agent particle is larger, and the particle size of the light diffusing agent particle is larger, the light from one light diffusing agent particle is known. The diffusion coefficient increases. However, if the particle size of the light diffusing agent particles is large, the mass of the light diffusing agent particles becomes large. Therefore, when the mass ratio of the light diffusing agent particles in the resin is constant, the large particles contained in the resin The number of light diffusing agent particles having a smaller diameter is reduced, and the overall light diffusibility based on the product of the light diffusion coefficient of each light diffusing agent particle and the number of light diffusing agent particles contained in the resin is not necessarily high. Don't be. On the other hand, if the particle size of the light diffusing agent particles contained in the transparent resin is too small, the light diffusion coefficient decreases exponentially, so that sufficient light diffusibility cannot be obtained.

2 and 3 show the influence on the light diffusibility by the content of the light diffusing agent. In general, as the content of the light diffusing agent increases, the light diffusibility (dispersion degree) improves (see FIG. 2). However, as the content of the light diffusing agent increases, the amount of reflected light from the molded body also increases, so the ratio of the amount of transmitted light to the amount of incident light, that is, the total light transmittance decreases. Therefore, the relationship between the total light transmittance and the degree of dispersion is as shown in FIG. In regions where the total light transmittance is high, the degree of dispersion tends to decrease, but a material exhibiting a high degree of dispersion in a wide range of total light transmittance is preferable, and the light diffusing agent has a total light transmittance of, for example, There is a demand for performance that shows a high degree of dispersion even in a high region of 85% and that can be used in a wide range of total light transmittance.

Moreover, if the difference between the refractive index of the transparent resin and the refractive index of the light diffusing agent particles becomes too large, the amount of reflected light from the molded body increases. Then, the total light transmittance is reduced, and for example, sufficient brightness cannot be obtained in a light diffusing plate of a display, a transmissive screen, a cover of a lighting fixture, an electric signboard, and the like.
Furthermore, since the light diffusing plate may be molded under a high temperature condition exceeding 300 ° C., the light diffusing agent has excellent heat resistance such that decomposition or the like hardly occurs even under a high temperature condition. Is also required.

However, conventionally, a light diffusing resin composition that satisfies all of the above requirements has not been obtained.
The technique disclosed in Patent Document 1 is not practical because it requires a relatively large amount of light diffusing agent in the formation of the diffusion plate. The technique described in Patent Document 2 shows good light diffusibility with a relatively small amount of light diffusing agent, but the light diffusibility in a region where the total light transmittance is 70% or more is not sufficient. For this reason, it cannot be used for applications that require high light transmission, such as covers for lighting fixtures. In addition, the light diffusing agents described in Patent Documents 3 to 5 need to be added in an amount in order to obtain good light diffusibility in a region where the total light transmittance is less than 80%. There was a problem from the aspect.
In the technique described in Patent Document 6, although it is possible to express good light diffusibility in a wide range of total light transmittance with a small amount of light diffusing agent, there is room for improvement in terms of heat resistance.

An object of the present invention is to provide a light diffusing resin composition that exhibits high dispersion in a wide range of total light transmittance, has excellent light diffusibility, and has excellent heat resistance, impact resistance, and flame retardancy, and a molded product thereof. It is to be.

As a result of intensive studies in view of the above problems, the present inventors have used light-diffusing properties, heat resistance, impact resistance by using crosslinked resin fine particles having a specific particle size, particle size distribution, refractive index and the like as a light diffusing agent. It has been found that a light diffusing resin composition having excellent properties and the like can be obtained.

The present invention is as follows.
1. An absolute value of a difference between the refractive index of the transparent resin (X) and the refractive index of the crosslinked resin fine particles (Y) (hereinafter referred to as “Δn”) including the transparent resin (X) and the crosslinked resin fine particles (Y). 0.095 to 0.115, the volume average particle diameter of the crosslinked resin fine particles (Y) is 1.5 to 3.3 μm, and the coefficient of variation of the particle diameter of the crosslinked resin fine particles (Y) is 20%. The cross-linked resin fine particles (Y) are characterized in that the temperature at which the mass is halved is 320 ° C. or higher when pyrolyzed in a nitrogen gas atmosphere at a temperature rising rate of 10 ° C./min. A light diffusing resin composition.
2. 2. The light diffusing resin composition as described in 1 above, wherein the crosslinked resin fine particles (Y) contain a structural unit derived from a (meth) acrylic acid ester.
3. A sheet of 1.5 mm thickness produced using the light diffusing resin composition, which has a total light transmittance of 85% for white light, is irradiated with light in a vertical direction using a goniometer. 3. The light diffusing resin composition according to 1 or 2 above, wherein an angle at which the emitted light having a luminance of 50% with respect to the emitted light at 0 degree is 20 degrees or more when the incident light is incident.
4). The surface of a 1.5 mm thick sheet prepared using a light-scattering resin composition in which the mass ratio of the transparent resin (X) and the crosslinked resin fine particles (Y) is 100 parts by mass and 0.5 parts by mass, respectively. The light diffusion according to 1 or 2 above, wherein, when light is incident in a vertical direction using a goniometer, the angle at which the emitted light having a luminance of 50% with respect to the emitted light at 0 degree is 22 degrees or more Resin composition.
5. 5. The light diffusing resin composition as described in any one of 1 to 4 above, wherein the transparent resin (X) is a polycarbonate resin.
6). 6. The light diffusing resin composition according to any one of 1 to 5, comprising 0.1 to 2.0 parts by mass of the crosslinked resin fine particles (Y) with respect to 100 parts by weight of the transparent resin (X).
7). 7. The light diffusing resin composition as described in any one of 1 to 6 above, wherein the crosslinked resin fine particles (Y) are produced by dispersion polymerization.
8). 8. The light diffusing resin according to any one of 1 to 7 above, wherein the crosslinked resin fine particles (Y) are crosslinked resin fine particles obtained by silane-crosslinking a (meth) acrylic acid ester-based resin having a hydrolyzable silyl group. Composition.
9. A molded article comprising the light diffusing resin composition according to any one of 1 to 8 above.
10. 10. The molded product according to 9 above, wherein the molded product is disposed in a lighting device or a display device.

The light diffusing resin composition of the present invention exhibits a high degree of dispersion in a wide range of total light transmittance and is excellent in light diffusibility. Moreover, the light diffusable resin composition of this invention is excellent also in heat resistance, impact resistance, and a flame retardance.

It is the figure which showed the measurement principle of dispersion degree typically. In a light diffusable resin composition, it is the figure which showed typically the relationship between the addition amount of a light diffusing agent, and dispersion degree. It is the figure which showed typically the relationship between a total light transmittance and dispersion degree.

The light diffusing resin composition of the present invention comprises crosslinked resin fine particles (Y) having a specific particle size, particle size distribution, refractive index, composition and the like as a light diffusing agent, and a transparent resin (X). The present invention relates to a light diffusing resin composition that exhibits good light diffusivity and diffusion efficiency and is excellent in heat resistance and the like, and a molded body using the same. In the light diffusing resin composition of the present invention, the crosslinked resin fine particles (Y) have an action as a light diffusing agent.
The present invention will be described in detail below.

The transparent resin (X) according to the present invention is not particularly limited, and examples thereof include acrylic resins such as polymethyl methacrylate (PMMA), styrene resins such as polystyrene and styrene / methacrylic acid copolymers, Polycarbonate resin etc. are mentioned. Of these, styrene resins are preferred when importance is placed on cost, but polycarbonate resins are preferred when impact resistance and flame retardancy are required.

As the styrenic resin, the content ratio of the structural unit derived from the styrenic monomer from the viewpoint of the melt fluidity, moldability, heat resistance, moisture absorption resistance, refractive index, etc. of the composition is styrene resin. It is preferable to use a resin that is 80% by mass or more with respect to a total amount of 100% by mass of all the structural units to be configured. More preferred is 90% by mass or more, and particularly preferred is 95 to 100% by mass.

Examples of the styrene monomer forming the styrene resin include styrene, α-methyl styrene, p-methyl styrene, o-methyl styrene, m-methyl styrene, vinyl toluene, p-ethyl styrene, p-tert. -Butyl-styrene, pn-butylstyrene, pn-hexylstyrene, p-octylstyrene, 2,4-dimethylstyrene, p-methoxystyrene, p-phenylstyrene, o-chlorostyrene, m-chlorostyrene , P-chlorostyrene, 2,4-dichlorostyrene and the like. The styrenic resin may contain only one type of structural unit derived from these styrenic monomers, or may contain two or more types.
Of these, styrene is preferable from the viewpoint of availability of styrene-based resin, cost, polymerizability, and the like.

The styrenic resin may be either a homopolymer or a copolymer. In the latter case, a copolymer obtained by copolymerizing a monomer containing a styrene monomer and methacrylic acid can be used. The content of the styrene monomer unit constituting the copolymer is preferably 80 to 95 mol%, more preferably 85 to 95 mol% from the viewpoint of heat resistance.

The copolymer may contain a structural unit derived from another monomer copolymerizable with these, in addition to the styrene monomer and methacrylic acid. Other monomers include methyl (meth) acrylate, ethyl (meth) acrylate, butyl (meth) acrylate, 2-ethylhexyl (meth) acrylate, cyclohexyl (meth) acrylate, (meth) acrylic acid (Meth) acrylic acid esters such as benzyl and 2-hydroxyethyl (meth) acrylate; acrylic acid, maleic anhydride, (meth) acrylonitrile and the like. Other monomers can be used alone or in combination of two or more.

The molecular weight of the styrene resin is not particularly limited. The weight average molecular weight (Mw) in terms of polystyrene measured by gel permeation chromatography (GPC) is 50,000 to 1 in terms of the moldability of the composition, particularly melt moldability, and the strength of the resulting molded product. It is preferably 1,000,000, more preferably 100,000 to 500,000.
The molecular weight distribution (Mw / Mn) of the styrenic resin is preferably 1.5 to 3.5 from the viewpoint of the strength of the obtained molded article.

Examples of the polycarbonate resin include aromatic polycarbonate resin, aliphatic polycarbonate resin, and aromatic-aliphatic copolymer polycarbonate resin. An aromatic polycarbonate resin is often used for the light diffusing resin composition. Specifically, it is an aromatic polycarbonate resin obtained by a reaction between a divalent phenol compound and phosgene or diphenyl carbonate.

Specific examples of the divalent phenol include 2,2- (4-hydroxyphenyl) propane (bisphenol A), 2,2- (4-hydroxyphenyl) butane, and 2,2- (4-hydroxyphenyl). Examples include pentane, 4,4′-biphenol, hydroquinone, resorcinol and the like. Of these, 2,2- (4-hydroxyphenyl) propane (bisphenol A) is preferred because of its good impact resistance and the like.
The polycarbonate resin may be a polycarbonate resin obtained by any method of interfacial polymerization and melt transesterification.

The viscosity average molecular weight of the polycarbonate resin is not particularly limited, but is preferably 1 × 10 ⁴ to 1 × 10 ⁵ , more preferably 1.3 × 10 ⁴ to from the viewpoint of mechanical properties and fluidity during injection molding. 3 × 10 ⁴ .

Polycarbonate resin is excellent in transparency, impact resistance, heat resistance, flame retardancy, etc., and is relatively inexpensive for its performance, so it is widely used in optical applications such as lighting equipment and displays. . Accordingly, the transparent resin (X) according to the present invention is particularly preferable.

The cross-linked resin fine particles (Y) are not limited as long as they are fine particles made of a resin having a cross-linked structure. Since the selectivity of the monomer to be used is high and the refractive index can be easily adjusted, the fine particles are composed of a (meth) acrylate crosslinked resin containing a structural unit derived from (meth) acrylate. preferable. The crosslinked structure contained in the fine particles can be based on cleavage by polymerization of a polyfunctional polymerizable unsaturated compound containing a plurality of carbon-carbon double bonds, or can be based on a siloxane bond.

The content ratio of the structural unit derived from the (meth) acrylic acid ester constituting the (meth) acrylic acid ester-based crosslinked resin is preferably 50% by mass or more, more preferably 80% by mass or more, and further preferably 90% by mass. % Or more, particularly preferably 95 to 100% by mass. In particular, when the content of the structural unit derived from (meth) acrylic acid ester is 80% by mass or more, the refractive index of the crosslinked resin fine particles (Y) is easily adjusted to the range of 1.460 to 1.510. This is preferable because it can be performed.

The method for producing the crosslinked resin fine particles (Y) used in the present invention is not particularly limited, but the following methods can be exemplified.
(I) A method in which a vinyl monomer (m2) containing a crosslinkable monomer is absorbed in seed particles made of resin fine particles produced by dispersion polymerization, and then the vinyl monomer (m2) is polymerized. .
(Ii) A method of carrying out a crosslinking reaction between hydrolyzable silyl groups after obtaining resin fine particles having hydrolyzable silyl groups by dispersion polymerization.
In the present invention, the crosslinked resin fine particles obtained by the above methods (i) and (ii) may be used alone or in combination.

The method for producing (meth) acrylic ester-based crosslinked resin fine particles is generally suspension polymerization, but in the case of suspension polymerization, it is necessary to produce crosslinked resin fine particles having a narrow particle size distribution and uniform size. Is generally difficult. On the other hand, in the dispersion polymerization, crosslinked resin fine particles having a narrow particle size distribution and a uniform size can be produced smoothly by polymerization in an alcohol solvent, particularly a mixed solvent of alcohol and water. Further, the particle size and particle size distribution can be controlled by adjusting the ratio of alcohol and water. From this point, in the present invention, the above methods (i) and (ii) are preferably used.

In the case of the above method (i), the seed particle is preferably a (meth) acrylic acid ester resin and is produced by subjecting the vinyl monomer (m1) to dispersion polymerization in a water / alcohol polar solvent. can do. At this time, when a carboxyl group-containing macromonomer is used as a dispersion stabilizer, dispersion polymerization proceeds more smoothly.
The carboxyl group-containing macromonomer is not particularly limited as long as it has a radical polymerizable unsaturated bond at the molecular end or side chain. Examples of the radical polymerizable unsaturated bond include a terminal vinylidene group, a terminal (meth) acryloyl group, a side chain (meth) acryloyl group, and a terminal styryl group.

Examples of the vinyl monomer (m1) forming the seed particles include (meth) acrylic acid esters and aromatic vinyl compounds. Specific monomers include methyl (meth) acrylate, (meta ) Ethyl acrylate, propyl (meth) acrylate, n-butyl (meth) acrylate, isobutyl (meth) acrylate, tert-butyl (meth) acrylate, pentyl (meth) acrylate, (meth) acrylic acid 2 -Alkyl esters of (meth) acrylic acid such as ethylhexyl, lauryl (meth) acrylate and stearyl (meth) acrylate; alicyclics of (meth) acrylic acid such as cyclohexyl (meth) acrylate and isobornyl (meth) acrylate Group-containing ester; (meth) such as glycidyl (meth) acrylate and tetrahydrofurfuryl (meth) acrylate Heterocyclic group-containing esters of crylic acid; 2-hydroxyethyl (meth) acrylate, 2-hydroxypropyl (meth) acrylate, 3-hydroxypropyl (meth) acrylate, 4-hydroxybutyl (meth) acrylate, etc. Examples include hydroxyalkyl esters of (meth) acrylic acid; alkoxyalkyl esters of (meth) acrylic acid such as 2-methoxyethyl (meth) acrylate. These compounds may be used alone or in combination of two or more. The vinyl monomer (m1) preferably contains a (meth) acrylic acid ester, and methyl methacrylate and isobutyl methacrylate are particularly preferable.
The amount of the (meth) acrylic acid ester used for the formation of the seed particles is preferably 50 to 100% by mass, more preferably 80 to 100% by mass, based on the total mass of the vinyl monomer (m1). It is.
The seed particles are preferably 60% by mass or more, more preferably 65% by mass or more, and particularly preferably 70 to 100% by mass based on 100% by mass of the total amount of structural units constituting the seed particles. It is preferable from the point of the heat-resistant blocking property of a particle | grain, a weather resistance, and a refractive index that it is a methacrylic ester resin which consists of a structural unit derived from (2) and / or a structural unit derived from isobutyl methacrylate.

When producing the seed particles, the macromonomer is used in an amount of preferably 0.5 to 50 parts by mass, more preferably 1.0 to 20 parts by mass with respect to 100 parts by mass of the vinyl monomer (m1). Part.

The weight average molecular weight (Mw) of the seed particles is preferably 1,000 to 2,000,000 in terms of polystyrene measured by gel permeation chromatography (GPC), preferably 5,000 to 1,000. 1,000 is more preferable.

In addition, the vinyl monomer (m2) to be polymerized after being absorbed in the seed particles obtained by dispersion polymerization contains a polyfunctional vinyl monomer in order to form the crosslinked resin fine particles (Y). As this polyfunctional vinyl monomer, a polyfunctional (meth) acrylate compound excellent in polymerizability is preferably used. Specific examples include ethylene glycol di (meth) acrylate, propylene glycol di (meth) acrylate, 1,6-hexanediol di (meth) acrylate, polyethylene glycol di (meth) acrylate, polypropylene glycol di (meth) acrylate and the like. Di (meth) acrylate of dihydric alcohol; trimethylolpropane tri (meth) acrylate, trimethylolpropane ethylene oxide modified tri (meth) acrylate, glycerol tri (meth) acrylate, pentaerythritol tri (meth) acrylate, pentaerythritol Examples include tri (meth) acrylates of trihydric or higher polyhydric alcohols such as tetra (meth) acrylate and poly (meth) acrylates such as tetra (meth) acrylate. Only 1 type may be used for a polyfunctional (meth) acrylate compound, and 2 or more types can be used for it.
Among these, ethylene glycol di (meth) acrylate and trimethylolpropane tri (meth) acrylate can be easily absorbed into seed particles made of (meth) acrylic ester resin, and can increase the crosslinking density. It is preferably used in terms of being possible and excellent in polymerization stability.

The vinyl monomer (m2) to be absorbed and polymerized in the seed particles contains a monofunctional vinyl monomer together with the polyfunctional vinyl monomer described above. This is preferable because the polymerization stability is advantageous. This monofunctional vinyl monomer is a monomer that is the same as or similar to the monomer such as (meth) acrylic acid ester constituting the seed particle, for example, methyl methacrylate and isobutyl methacrylate. Is preferred. By using such a vinyl monomer containing a monofunctional vinyl monomer, the seed particles are well swelled, thereby promoting the absorption of the vinyl monomer (m2) into the seed particles. Thus, crosslinked resin fine particles (Y) that are sufficiently crosslinked are obtained. In addition, for example, when a styrene resin is used as the transparent resin (X), in order to increase the refractive index difference from the crosslinked resin fine particles (Y) and obtain higher light diffusibility, the refractive resin is more refracted. It is preferable to select a monofunctional vinyl monomer that forms a polymer having a low rate, and for example, isobutyl methacrylate, tert-butyl methacrylate and the like are preferably used.

The ratio of the preferred amount of seed particles and vinyl monomer (m2) used in the production of the crosslinked resin fine particles (Y) is not particularly limited, but the crosslinking structure is imparted to the particles and the monomer is absorbed into the seed particles. From the point of view, it is shown below. The vinyl monomer (m2) is preferably 0.5 to 10 parts by mass and more preferably 0.7 to 5 parts by mass with respect to 1 part by mass of the seed particles.
The amount of the polyfunctional vinyl monomer used is preferably 3 to 95% by mass, particularly preferably 5 to 75% by mass, based on the total mass of the vinyl monomer (m2).

Next, in the case of the above method (ii), the resin fine particles having a hydrolyzable silyl group are subjected to dispersion polymerization using a vinyl monomer having a hydrolyzable silyl group and (meth) acrylic acid ester or the like. It is preferable that it is the fine particle obtained by performing. The hydrolyzable silyl group means a functional group that can be crosslinked by forming a siloxane bond by hydrolysis condensation reaction, and includes methoxysilane, ethoxysilane, and the like.

Any vinyl compound having at least one hydrolyzable silyl group can be used as the vinyl monomer having a hydrolyzable silyl group. For example, vinyl silane such as vinyltrimethoxysilane, vinyltriethoxysilane, vinylmethyldimethoxysilane, vinyldimethylmethoxysilane, etc .; hydrolysis of trimethoxysilylpropyl acrylate, triethoxysilylpropyl acrylate, methyldimethoxysilylpropyl acrylate, etc. Hydrolyzable silyl group-containing acrylic acid ester; hydrolyzable silyl group-containing methacrylate ester such as trimethoxysilylpropyl methacrylate, triethoxysilylpropyl methacrylate, methyldimethoxysilylpropyl methacrylate, dimethylmethoxysilylpropyl methacrylate; Hydrolyzable silyl group-containing vinyl ethers such as propyl vinyl ether; Hydrolyzable silyl group-containing vinyl ethers such as vinyl trimethoxysilylundecanoate Mention may be made of the ether and the like. These vinyl monomers may be used alone or in combination of two or more.
Among these, as the vinyl monomer having a hydrolyzable silyl group, a hydrolyzable silyl group-containing acrylate ester and a hydrolyzable silyl group-containing methacrylate ester are preferable. These monomers are preferable because they are excellent in copolymerizability with (meth) acrylic acid esters and the like, and fine particles excellent in heat resistance and weather resistance are obtained. As the vinyl monomer, trimethoxysilylpropyl methacrylate (also known as trimethoxysilylpropyl methacrylate) is excellent in copolymerization with (meth) acrylic acid ester, stability during dispersion polymerization, and crosslinkability. Is particularly preferably used.

The amount of vinyl monomer having a hydrolyzable silyl group is generally based on the total mass of monomers (including macromonomers) used for the production of resin fine particles having hydrolyzable silyl groups. Thus, it is preferably 2 to 50% by mass, particularly 5 to 30% by mass.

Examples of monomers other than vinyl monomers having hydrolyzable silyl groups used in the production of resin fine particles having hydrolyzable silyl groups include (meth) acrylic acid esters. The monomer is as described above.

In addition, in the dispersion polymerization for producing resin fine particles having a hydrolyzable silyl group, it is preferable to use a macromonomer type dispersion stabilizer having a (meth) acryloyl group. When a macromonomer type dispersion stabilizer having a (meth) acryloyl group is used, a (meth) acrylic acid ester system having a target particle size and a hydrolyzable silyl group having a narrow particle size distribution with a small amount of use. Resin fine particles can be obtained smoothly. Furthermore, the macromonomer type dispersion stabilizer more preferably has a carboxyl group.
The (meth) acryloyl group may be bonded to any position of the end of the polymer chain and the side chain. In particular, a macromonomer type dispersion stabilizer with a (meth) acryloyl group bonded to the side chain stably produces (meth) acrylic ester resin fine particles having the desired hydrolyzable silyl group with a smaller amount of use. It is preferable from the point which can be performed.
As a method for producing a macromonomer type dispersion stabilizer having a (meth) acryloyl group in the side chain and having a carboxyl group, a carboxyl group-containing prepolymer is synthesized by emulsion polymerization, and then the carboxyl group of this prepolymer, A method of reacting with an epoxy group in an epoxy group-containing (meth) acrylate such as glycidyl (meth) acrylate to give a (meth) acryloyl group can be mentioned. At this time, a part of the carboxyl group of the prepolymer may remain. With this method, a high-performance macromonomer can be easily produced. In the case of using an epoxy group-containing (meth) acrylate, it is preferable to add 0.6 to 2.0 per polymer chain, whereby fine particles having a narrower particle size distribution and a uniform particle size can be produced. .

The polystyrene equivalent weight average molecular weight (Mw) of the macromonomer measured by gel permeation chromatography (GPC) is preferably 500 to 50,000, more preferably 1,000 to 10,000.

The macromonomer type dispersion stabilizer having a (meth) acryloyl group and a carboxyl group used for the production of resin fine particles having a hydrolyzable silyl group is preferably neutralized. This makes it possible to stably produce resin fine particles having hydrolyzable silyl groups due to the electrostatic repulsion effect of the neutralized carboxy anion. The amount of alkali used for neutralization is preferably not more than twice the equivalent of the carboxyl group. If it exceeds 2 equivalents, the alkalinity of the reaction solution becomes strong, and a hydrolyzable silyl group may react during polymerization to cause aggregation. Examples of the alkali for neutralization include ammonia and triethylamine. Among these, ammonia that can be easily removed is preferably used.

In the dispersion polymerization method using the macromonomer type dispersion stabilizer, a known polymerization initiator used in dispersion polymerization can be used. Specific examples include benzoyl peroxide, lauroyl peroxide, orthochlorobenzoyl peroxide, orthomethoxybenzoyl peroxide, 3,5,5-trimethylhexanoyl peroxide, tert-butylperoxy-2-ethylhexanoate , Organic peroxides such as di-tert-butyl peroxide, di-tert-hexyl peroxide, di-tert-amyl peroxide, tert-butyl peroxypivalate; azobisisobutyronitrile, azobiscyclohexa Examples thereof include azo compounds such as carbonitrile and azobis (2,4-dimethylvaleronitrile); persulfate compounds such as potassium persulfate.

In the case of the method (ii), since it is preferable to copolymerize a vinyl monomer having a hydrolyzable silyl group and a (meth) acrylic acid ester in the presence of the macromonomer type dispersion stabilizer, By these dispersion polymerizations, structural units derived from vinyl monomers having hydrolyzable silyl groups, structural units derived from (meth) acrylic acid esters, and structural units derived from macromonomer type dispersion stabilizers. A dispersion containing the (meth) acrylic acid ester resin fine particles having hydrolyzable silyl groups is obtained.

Thereafter, the hydrolyzable silyl groups in the (meth) acrylic acid ester resin fine particles having hydrolyzable silyl groups obtained above are subjected to a crosslinking reaction to produce crosslinked resin fine particles (Y).
The cross-linking reaction can be performed by adding a cross-linking catalyst to a dispersion containing (meth) acrylic ester resin fine particles having a hydrolyzable silyl group. With the crosslinking catalyst, a hydrolyzable silyl group can be subjected to a condensation reaction to form a siloxane bond. As the crosslinking catalyst, an alkaline material is preferable, and in particular, ammonia that can be easily removed after the crosslinking reaction or a low-boiling amine is preferably used.
The amount of the alkali material used is preferably 3 times equivalent or more and 6 times equivalent or more with respect to the silyl group in the resin fine particles having a hydrolyzable silyl group from the viewpoint of increasing the degree of silyl crosslinking. More preferred.

Among the methods for producing the crosslinked resin fine particles (Y) shown in the above methods (i) and (ii), the method (ii) for carrying out the crosslinking reaction after obtaining the resin fine particles having hydrolyzable silyl groups by dispersion polymerization, It is preferable because it can be produced simply and at low cost.

In addition, the light diffusable resin composition of this invention can contain an additive so that it may mention later. In the present invention, the crosslinked resin fine particles (Y) may be particles containing an antioxidant, a light stabilizer and the like. A light diffusing resin composition containing these additives is a preferable embodiment because it is particularly excellent in heat decomposition stability and weather resistance.
Examples of the antioxidant include phosphorus antioxidants, phenolic antioxidants, sulfur antioxidants, and the like.
Of these, examples of phosphorus antioxidants include phosphite compounds.

Examples of the phosphite compound include triphenyl phosphite, trisnonylphenyl phosphite, tris (2,4-di-tert-butylphenyl) phosphite, tris [2-tert-4- (3-tert- 4-hydroxy-5-methylphenylthio) -5-methylphenyl] phosphite, trioctyl phosphite, tridecyl phosphite, trioctadecyl phosphite, octyl diphenyl phosphite, di (decyl) monophenyl phosphite, dioctyl mono Phenyl phosphite, diisopropyl monophenyl phosphite, di (tridecyl) pentaerythritol diphosphite, distearyl pentaerythritol diphosphite, monobutyl diphenyl phosphite, monodecyl diphenyl phosphite Ite, monooctyl diphenyl phosphite, di (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) pentaerythritol diphosphite, 2,2-methylenebis (4,6-di-tert-butylphenyl)- 2-ethylhexyl phosphite, 2,2'-methylenebis (4,6-di-tert-butylphenyl) -2-octadecyl phosphite, 2,2'-ethylidenebis (4,6-di-tert-butylphenyl) Fluorophosphite, tetra (tridecyl) isopropylidene di Phenol diphosphite, tetra (tridecyl) -4,4-n-butylidenebis (2-tert-butyl-5-methylphenol) diphosphite, hexa (tridecyl) -1,1,3-tris (2-methyl-4- Hydroxy-5-tert-butylphenyl) butane triphosphite.

Examples of the phenolic antioxidant include n-octadecyl-β- (4′-hydroxy-3 ′, 5′-di-tert-butylphenyl) propionate, tetrakis [methylene-3- (3-tert-butyl- 4-hydroxy-5-methylphenyl) propionate] methane, octadecyl-3- (3,5-di-tert-butyl-4-hydroxyphenyl) propionate, 2-tert-butyl-6- (3′-tert-butyl -5′-methyl-2′-hydroxybenzyl) -4-methylphenyl acrylate, 2,6-di-tert-butyl-4- (N, N-dimethylaminomethyl) phenol, 3,5-di-tert- Butyl-4-hydroxybenzylphosphonate diethyl ester, 2,2′-methylenebis (4-methyl-6) tert-butylphenol), 2,2'-methylenebis (4-ethyl-6-tert-butylphenol), 4,4'-methylenebis (2,6-di-tert-butylphenol), 2,2'-methylenebis (4- Methyl-6-cyclohexylphenol), 2,2′-dimethylene-bis (6-α-methyl-benzyl-p-cresol), 2,2′-ethylidene-bis (4,6-di-tert-butylphenol), 2,2′-butylidene-bis (4-methyl-6-tert-butylphenol), 4,4′-butylidenebis (3-methyl-6-tert-butylphenol), triethylene glycol-N-bis-3- (3 -Tert-butyl-4-hydroxy-5-methylphenyl) propionate, 1,6-hexanediol bis [ -(3,5-di-tert-butyl-4-hydroxyphenyl) propionate], bis [2-tert-butyl-4-methyl 6- (3-tert-butyl-5-methyl-2-hydroxybenzyl) phenyl ] Terephthalate, 3,9-bis {2- [3- (3-tert-butyl-4-hydroxy-5-methylphenyl) propionyloxy] -1,1, -dimethylethyl} -2,4,8,10 -Tetraoxaspiro [5,5] undecane, 4,4'-thiobis (6-tert-butyl-m-cresol), 4,4'-thiobis (3-methyl-6-tert-butylphenol), 2,2 '-Thiobis (4-methyl-6-tert-butylphenol), bis (3,5-di-tert-butyl-4-hydroxybenzyl) sulfide, 4, '-Di-thiobis (2,6-di-tert-butylphenol), 4,4'-tri-thiobis (2,6-di-tert-butylphenol), 2,2-thiodiethylenebis- [3- (3 , 5-di-tert-butyl-4-hydroxyphenyl) propionate], 2,4-bis (n-octylthio) -6- (4-hydroxy-3 ′, 5′-di-tert-butylanilino) -1, 3,5-triazine, N, N′-hexamethylenebis- (3,5-di-tert-butyl-4-hydroxyhydrocinnamide), N, N′-bis [3- (3,5-di- tert-butyl-4-hydroxyphenyl) propionyl] hydrazine, 1,1,3-tris (2-methyl-4-hydroxy-5-tert-butylphenyl) butane, 1,3,5-trimethyl -2,4,6-tris (3,5-di-tert-butyl-4-hydroxybenzyl) benzene, tris (3,5-di-tert-butyl-4-hydroxyphenyl) isocyanurate, tris (3 5-di-tert-butyl-4-hydroxybenzyl) isocyanurate, 1,3,5-tris (4-tert-butyl-3-hydroxy-2,6-dimethylbenzyl) isocyanurate, 1,3,5- Tris [(3,5-di-tert-butyl-4-hydroxyphenyl) propionyloxyethyl] isocyanurate and tetrakis [methylene-3- (3 ′, 5′-di-tert-butyl-4-hydroxyphenyl) Propionate] Examples include methane, vitamin E, α-tocopherol, butylhydroxytoluene, and sinapyr alcohol. It is possible. Of these, hindered phenol compounds are preferred.

Examples of sulfur-based antioxidants include pentaerythritol tetrakis (3-mercaptopropionate), pentaerythritol tetrakis (3-laurylthiopropionate), and glycerol-3-stearylthiopropionate. .
The said antioxidant can be used 1 type or in combination of 2 or more types.

Examples of the light stabilizer include 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-butanetetracarboxylate, tetrakis (1,2,2,6,6-pentamethyl-4-piperidyl) -1,2 , 3,4-Butanetetracarboxylate, poly {[6- (1,1,3,3-tetramethylbutyl) amino-1,3,5-triazine-2,4-diyl] [(2,2, 6,6-tetramethylpiperidyl) imino] hexamethylene [(2,2,6,6-tetramethylpiperidyl) imino]}, polymethylpropyl 3-oxy- [4- (2,2,6,6-tetra Methyl) piperi Sulfonyl] hindered amine compounds such siloxanes, and the like.
The said light stabilizer can be used 1 type or in combination of 2 or more types.

The volume average particle diameter (dv) of the crosslinked resin fine particles (Y) according to the present invention is 1.5 to 3.3 μm, preferably 1.8 to 2.8 μm, more preferably 2.1 to 2.5 μm. It is.
When the volume average particle diameter (dv) is less than 1.5 μm, the ratio of diffuse light per particle decreases, so the ratio of regular transmitted light that does not diffuse increases, and the total light transmittance is high. This is not preferable because the diffusibility (dispersion degree) decreases. On the other hand, when the volume average particle diameter (dv) exceeds 3.3 μm, the number of particles at the same mass decreases, and the amount added to obtain the same total light transmittance increases, which is not preferable. Moreover, when the particle | grains of crosslinked resin microparticles | fine-particles (Y) are large, since diffused transmission light increases more straightness, it is not preferable.

In the particle size distribution of the crosslinked resin fine particles (Y), the coefficient of variation (CV) is 20% or less, preferably 10% or less. When the CV value exceeds 20%, the degree of dispersion in the high transmittance region tends to decrease.
Note that the coefficient of variation (CV) can be used as an index representing the spread of the particle size distribution. The smaller the coefficient of variation (CV), the narrower the particle size distribution. If it is 20% or less, it can be said that the distribution width is very narrow. When all the particles have the same particle size and a true spherical particle, the coefficient of variation (CV) is 0, but about 2% is considered to be the lower limit as what is actually obtained.

Here, the volume average particle diameter (dv) and coefficient of variation (CV) of the crosslinked resin fine particles (Y) in the present specification are measured or measured using a laser diffraction scattering type particle size distribution meter and a scanning electron microscope, respectively. It is calculated and its detailed method is as described in the examples described later.

Further, in the present invention, when the crosslinked resin fine particles (Y) are thermally decomposed under a nitrogen gas atmosphere at a temperature rising rate of 10 ° C./min, the temperature at which the mass becomes half, that is, 50% by weight. The temperature reduction (Td ₅₀ ) is 320 ° C. or higher, preferably 350 ° C. or higher. The upper limit temperature is 400 ° C. for general acrylic fine particles. When Td ₅₀ is less than 320 ° C., the crosslinked resin fine particles are decomposed by heat applied at the time of kneading, which may cause problems such as change in particle diameter, generation of gas, and coloring. Td ₅₀ can be measured, for example, using a thermogravimetric / differential thermal analyzer.
In general, methacrylic polymers are known to have a higher decomposition rate when heated compared to other polymer materials, and the Td _{50 of} crosslinked resin fine particles consisting only of methacrylic monomers is low. However, the copolymerization of acrylic monomer, styrene monomer, etc. by about several mass% reduces the decomposition rate at the time of heating, so that the value of Td ₅₀ can be increased.

The light diffusing resin composition of the present invention includes the transparent resin (X) and the crosslinked resin fine particles (Y), and the refractive index of the transparent resin (X) and the refractive index of the crosslinked resin fine particles (Y) The absolute value (Δn) of the difference is 0.095 to 0.115, preferably 0.100 to 0.110.
When Δn is large, the ratio of scattered light per light diffusing agent particle is increased, and the necessary amount of diffusing agent added is reduced, which is basically preferable. However, if Δn is too large, the ratio of reflected light increases, which is not preferable. In addition, if the amount of the light diffusing agent added is too small, it is not preferable because the regular transmitted light that does not hit the particles in the resin composition and is transmitted increases and the diffuse transmitted light decreases. In such a case, the degree of dispersion tends to decrease in a region where the total light transmittance is high. If Δn exceeds 0.115, these problems may occur.
On the other hand, when Δn is less than 0.095, the ratio of the diffused light per particle is reduced, so that it is necessary to increase the amount of the light diffusing agent, which is not preferable.

The content ratio of the transparent resin (X) and the crosslinked resin fine particles (Y) in the light diffusing resin composition of the present invention is shown. The content of the crosslinked resin fine particles (Y) is preferably 0.1 to 2.0 parts by mass, more preferably 0.3 to 1.5 parts by mass, and still more preferably 100 parts by mass of the transparent resin (X). Is 0.3 to 1.0 part by mass. When the content of the crosslinked resin fine particles (Y) exceeds 2.0 parts by mass, impact resistance and flame retardancy tend to be lowered. Moreover, when it is less than 0.1 parts by mass, the light diffusibility tends to be insufficient.

Further, the light diffusing resin composition of the present invention may contain fine particles other than the crosslinked resin fine particles (Y) (hereinafter referred to as “other fine particles”) as necessary. The light diffusibility can be finely adjusted by including other fine particles. Examples of the other fine particles include cross-linked (meth) acrylate-based fine particles, cross-linked polystyrene-based fine particles, cross-linked polyorganosiloxane-based fine particles, and silica fine particles. These other fine particles may be used alone or in combination of two or more.

The light diffusing resin composition of the present invention can contain additives as long as the object of the present invention is not impaired. Examples of additives include light stabilizers, ultraviolet absorbers, antioxidants, antistatic agents, lubricants, flame retardants, colorants (dyes, pigments), fluorescent brighteners, selective wavelength absorbers, plasticizers, and the like. Can do.
Here, as the antioxidant and the light stabilizer, the compounds described above that can be added to the crosslinked resin fine particles (Y) can be used.

The light diffusing resin composition of the present invention can be produced by melt-kneading a raw material containing transparent resin (X) and crosslinked resin fine particles (Y). Examples of the production apparatus include a melt extruder, a kneader, a mill, and the like. The temperature is equal to or higher than the melting temperature of the transparent resin (X) and lower than the thermal decomposition temperature of the transparent resin (X) and the crosslinked resin fine particles (Y). Melt and knead.

In the case of producing the light diffusing resin composition of the present invention, the whole amount of the transparent resin (X) and the whole amount of the crosslinked resin fine particles (Y) can be used. Further, a master batch having a high content ratio of the crosslinked resin fine particles (Y) is prepared in advance using a part of the transparent resin (X) and the total amount of the crosslinked resin fine particles (Y). The batch and the remaining transparent resin (X) may be kneaded.

The preferred light diffusibility of the light diffusing resin composition of the present invention is shown below. A sheet having a thickness of 1.5 mm and produced using the light diffusing resin composition of the present invention, wherein the total light transmittance of white light is 85%, and a vertical direction using a goniometer When light is incident on the light, the angle (hereinafter referred to as “dispersion degree (I)”) at which the emitted light has a luminance of 50% with respect to the emitted light at 0 degree is preferably 20 degrees or more, more preferably 23 degrees. That's it.
This property indicates that the light diffusing resin composition exhibiting a degree of dispersion of a certain level or higher in a region where the total light transmittance is high indicates that the light diffusibility is good, and the degree of dispersion (I) is 20 degrees or more. As a result, sufficient brightness and good light diffusibility can be achieved at the same time. Therefore, the light diffusing resin composition of the present invention is also suitable as a molding material for members such as displays and lighting fixtures. The degree of dispersion is adjusted by balancing the difference in refractive index (Δn) between the transparent resin (X) and the crosslinked resin fine particles (Y), the particle diameter of the crosslinked resin fine particles (Y), the particle size distribution, and the amount added. Is done.

In the present invention, a 1.5 mm thick sheet prepared using a light diffusing resin composition in which the transparent resin (X) and the crosslinked resin fine particles (Y) are 100 parts by mass and 0.5 parts by mass, respectively. The angle (hereinafter referred to as “dispersion degree (II)”) at which the emitted light has a luminance of 50% with respect to the emitted light at 0 degree when the light is incident on the surface in the vertical direction using a goniometer is preferable. Is 22 degrees or more, more preferably 23 degrees or more.
If the degree of dispersion (II) is 22 degrees or more, it is preferable because light diffusion is excellent.

For the dispersities (I) and (II), a goniometer (variable photometer) was used to irradiate parallel light in the thickness direction perpendicular to one surface of a 1.5 mm thick sheet. It is obtained by measuring the light distribution of transmitted light on the other surface side. Specifically, the luminance Bθ is obtained from the following equation (1) using the luminous intensity Iθ at each emission angle θ, and the angle at which the luminance becomes 50% with respect to the luminance B ₀ when θ = 0 ° is set as the degree of dispersion. It was.
Bθ = Iθ / cos θ (1)

The method for forming the sheet is not particularly limited, and can be obtained, for example, by subjecting the light diffusing resin composition to compression molding using a compression molding machine or the like. Moreover, since the value obtained by dispersion | distribution differs with the thickness of a sheet | seat, it is preferable to use for a measurement, after confirming that the thickness of a sheet | seat exists in the range of 1.50 +/- 0.05mm.

Using the light diffusing resin composition of the present invention, a molded article can be produced by various molding methods conventionally employed for molding resin compositions such as polycarbonate resins. The molding method for producing the molded body is appropriately selected according to the purpose of use and application, and is not particularly limited. For example, extrusion molding, injection molding, compression molding, extrusion blow molding, injection blow molding, flow Examples include melt molding such as rolling, calendar molding, and casting. Moreover, the molded body obtained by melt molding may be subjected to secondary molding processing such as bending, vacuum molding, blow molding, press molding, or the like, if necessary, to obtain a target molded body. In the case of an optical application, a processing method in which a lens shape and an embossed shape are formed on the surface of the molded body can be performed according to the purpose of use and application to adjust the optical characteristics.

The molded body comprising the light diffusing resin composition of the present invention can be effectively used for optical applications such as a light diffusing plate, a Fresnel lens, a lenticular lens, a lighting fixture, and an electric signboard in a liquid crystal display device.

Hereinafter, the present invention will be specifically described based on examples, but the present invention is not limited to the following examples. In the following description, “parts” and “%” mean “parts by mass” and “% by mass”, respectively.

1. Evaluation Method of Physical Properties Evaluation methods carried out on the macromonomer, the crosslinked resin fine particles (Y), a molded product produced from the light diffusing resin composition, and the like are as follows.

(1) Number average molecular weight (Mn) and weight average molecular weight (Mw)
From a calibration curve prepared in advance using a polystyrene having a known molecular weight as a reference substance, a macromonomer or a prepolymer that is a raw material for production thereof is subjected to gel permeation chromatography (GPC). , “Mn”) and weight average molecular weight (hereinafter “Mw”).
Measurement was performed using “HLC-8220GPC” manufactured by Tosoh Corporation as the GPC apparatus and “TSK-GEL MULTIPIORE HXL-M” (four) manufactured by Tosoh Corporation as the column. The polymer is dissolved in tetrahydrofuran (THF) to prepare a 0.2% concentration solution, and 100 μL of the solution is injected into the column. The eluent is THF, the column temperature is 40 ° C., and the eluent (THF) flow rate is 1. Measurement was performed at 0 mL / min.

(2) Volume average particle diameter (dv)
Methanol was added to the slurry containing the crosslinked resin fine particles obtained in Production Examples 1 to 13 shown in Table 1 to adjust the concentration of the fine particles to 5%, and the mixture was sufficiently shaken and dispersed uniformly. The dispersion was irradiated with ultrasonic waves for 10 minutes, and then particle size distribution measurement was performed using a laser diffraction scattering type particle size distribution analyzer “MT-3000” manufactured by Nikkiso Co., Ltd. Ion exchange water or acetone was used as a circulating dispersion medium at the time of measurement. Further, the crosslinked resin fine particles of the commercial products 1 to 3 were put into acetone so that the concentration of the dry powder was 5%, and were sufficiently shaken to be uniformly dispersed. This dispersion was irradiated with ultrasonic waves for 10 minutes, and then particle size distribution measurement was performed. The median diameter (μm) was calculated from the volume-based particle size distribution obtained by the particle size distribution measurement, and was defined as the volume average particle size (dv).

(3) Coefficient of variation (CV)
The crosslinked resin fine particles (A1) to (A9) and (B1) to (B7) shown in Table 1 were observed with a field emission scanning electron microscope (FE-SEM) “JSM-6330F” manufactured by JEOL. After photographing at a magnification at which about 50 to 100 particles can be observed on one sheet, the particle diameter (di) (equivalent circle diameter) of 0.2 μm or more crosslinked resin fine particles (200 or more) that can clearly confirm the particle image ) Was measured. Next, the standard deviation (σ) was calculated by the following formula (3), and the coefficient of variation (CV) was calculated by the following formula (2) using this.
CV (%) = 100 × (σ / dn) (2)
σ = (Σ (di-dn) ² / ΣNi) ^1/2 (3)
Here, the number average particle diameter (dn) for obtaining the coefficient of variation (CV) and the standard deviation (σ) is the particle diameter (di) obtained by the SEM observation and the number of particles having the particle diameter (Ni). It was calculated from the following formula (4).
dn = (ΣNidi / ΣNi) (4)

(4) Refractive index (n)
The refractive index of the crosslinked resin fine particles is determined by using the refractive index (ni) of the homopolymer of each structural unit constituting the crosslinked resin and the mass ratio (wi) of each structural unit to the total amount of the structural units constituting the crosslinked resin. It was calculated from the following formula (5).
n = Σniwi (5)
In addition, the refractive index of each homopolymer used the value described in "POLYMER HANDBOOK 4th edition" (John Wiley & Sons, Inc. issue). For polymers whose refractive index is not described in the literature, homopolymers were synthesized by solution polymerization or photopolymerization, and measured with an Abbe refractometer “DR-M2” manufactured by Atago Co., Ltd., at a temperature of 25 ° C. and with a wavelength of 589 nm. .

(5) Thermal decomposition temperature (Td ₅₀ )
The thermal decomposition temperature of the crosslinkable fine particles was measured with a differential thermothermal gravimetric simultaneous measurement apparatus (TG-DTA) “SII EXSTAR6000” manufactured by SII Nanotechnology. Under a nitrogen gas atmosphere, the temperature was increased from 25 ° C. to 500 ° C. at a temperature increase rate of 10 ° C./min, and the weight change was measured. The temperature at which the measurement before the mass was halved was measured, which was used as Td _50.

(6) Total light transmittance of molded body Using the light diffusable resin composition, a sheet having a thickness of 1.5 mm was prepared, and this was cut into an appropriate size to obtain a measurement sample. The total light transmittance (Tt) was measured using a Nippon Denshoku haze meter “Haze meter NDH2000” (model name).

(7) Dispersion of molded product The same sheet as the total light transmittance was used as a measurement sample. As shown in FIG. 1, as a device including a light source 2, a variable angle photometer “GP-200” manufactured by Murakami Color Research Laboratory Co., Ltd. is used to irradiate a light beam perpendicularly to the surface of the sheet 1. The distribution of transmitted light (emitted light) was measured on the side to determine the degree of dispersion. Specifically, after measuring the luminous intensity Iθ at the outgoing angle θ of each transmitted light (outgoing light), the luminance Bθ is obtained from the following formula (6), and the luminance B ₀ when θ = 0 is set to 100 The angle θ when the luminance of the light becomes 50 was calculated, and this θ was defined as the degree of dispersion.
Bθ = Iθ / cos θ (6)

2. Synthesis of Macromonomer First, macromonomers MM-1 and MM-2 were produced in order to produce crosslinked resin fine particles.

Synthesis Example 1 (Production of Macromonomer MM-1)
200 parts of ion-exchanged water was charged into a glass reaction vessel equipped with a stirrer, a reflux condenser, a thermometer, a nitrogen gas introduction pipe, and a liquid feed pipe connecting part. Next, the water temperature in the reaction vessel was adjusted to 80 ° C. while stirring and introducing nitrogen gas. Meanwhile, 36.35 parts of methyl methacrylate (hereinafter referred to as “MMA”), 36.35 parts of isobutyl methacrylate (hereinafter referred to as “IBMA”), methacrylic acid (hereinafter referred to as “MAA”) ”) And 20 parts of 2-ethylhexyl thioglycolate (hereinafter“ OTG ”) were charged and stirred to prepare a monomer mixture (100 parts). After confirming that the water temperature in the glass reaction vessel was stabilized at 80 ° C., 0.8 parts of ammonium persulfate (hereinafter referred to as “APS”), which is a polymerization initiator, was added to the ion exchange water 3.0 in the glass reaction vessel. The initiator aqueous solution dissolved in the part was added and stirred. Then, 5 minutes later, the supply of the monomer mixture was started from the glass container connected to the glass reaction container via the liquid feeding pipe connecting part using a metering pump. The monomer mixture was supplied at a constant rate over 240 minutes. After completing the supply of the monomer mixture, the temperature inside the reaction vessel was raised to 90 ° C. over 30 minutes. And it maintained at 90 degreeC for 4.5 hours, and obtained the dispersion liquid of the prepolymer. When a part of the dispersion was sampled and the prepolymer after removing the medium by drying was subjected to GPC measurement, Mn in terms of polystyrene was 2,700 and Mw was 4,600.
After the temperature of the prepolymer dispersion obtained above was lowered to 80 ° C. over 30 minutes, the introduced gas was changed from nitrogen gas to air, and 0.03 part of methoxyhydroquinone was immediately added. Five minutes after adding methoxyhydroquinone, 9.4 parts of triethylamine was supplied to the reaction vessel at a constant rate over 30 minutes. After 15 minutes, 6.1 parts of glycidyl methacrylate (hereinafter, “GMA”) was supplied to the reaction vessel at a constant rate over 30 minutes and heated at a temperature of 80 ° C. for 3 hours. As a result, the carboxyl group of the prepolymer and the glycidyl group contained in GMA were reacted to obtain a dispersion containing macromonomer MM-1 having a methacryloyl group derived from GMA (NV 34%).

Synthesis Example 2 (Production of macromonomer MM-2)
A 500 ml pressurized stirred tank reactor equipped with a hot oil heating device was filled with ethyl 3-ethoxypropionate. The reactor was then warmed to about 250 ° C. Meanwhile, 20 parts of MMA, 55 parts of cyclohexyl acrylate (hereinafter “CHA”), 25 parts of acrylic acid (hereinafter “AA”) and 0.1 part of di-tert-butyl peroxide (hereinafter “DTBP”) are mixed. Then, a monomer mixed solution was prepared and stored in a raw material tank.
Next, the monomer mixed solution is continuously supplied from the raw material tank to the reactor while keeping the pressure in the reactor constant by the pressure regulator above the vapor pressure of ethyl 3-ethoxypropionate. Polymerization was carried out at 0 ° C. At this time, the feed rate was set so that the average residence time of the monomer mixture in the reactor was 12 minutes. A reaction solution corresponding to the supply amount of the monomer mixture was continuously taken out from the outlet of the reactor. The temperature in the reactor was maintained at 230 ° C. ± 2 ° C. while supplying the monomer mixture.
After 90 minutes from the start of supplying the monomer mixture, the reaction liquid taken out from the outlet of the reactor is introduced into a thin film evaporator to remove volatile components such as unreacted monomers in the reaction liquid, Monomer MM-2 was obtained. The macromonomer MM-2 was collected for 60 minutes and then cooled to obtain a solid macromonomer MM-2. When the macromonomer MM-2 was subjected to GPC measurement, Mn in terms of polystyrene was 3,100 and Mw was 10,600. Further, the concentration of terminal ethylenically unsaturated bonds contained in the macromonomer MM-2 was measured by nuclear magnetic resonance spectrum (hereinafter referred to as ¹ H-NMR). The terminal ethylenically unsaturated bond introduction rate (hereinafter referred to as F value) of the macromonomer MM-2 calculated from the number average molecular weight and the concentration of the terminal ethylenically unsaturated bond was 98%.
Next, 100 parts of pulverized solid macromonomer MM-2, 260 parts of water and 22.5 parts of 25% aqueous ammonia were charged into a glass flask with a condenser tube, and a warm bath was used. The internal temperature was 90 ° C. Then, stirring was performed to make the macromonomer MM-2 water-soluble. After confirming that the macromonomer MM-2 was dissolved, water was added so that the solid content was 25% to obtain an aqueous solution of the macromonomer MM-2.

3. Crosslinked resin fine particles The crosslinked resin fine particles used in the production of the light diffusing resin composition are a synthetic product and a commercial product, and are shown below.

Production Example 1 (Production of crosslinked resin fine particles A1)
In a glass reaction vessel equipped with a stirrer, a reflux condenser, a thermometer, a nitrogen gas introduction pipe and a liquid feed pipe connection part, 100.4 parts of ion exchange water, 475.6 parts of methanol, 0.12 part of 25% ammonia water Then, 5.86 parts of a dispersion containing the macromonomer MM-1 obtained in Synthesis Example 1, 15.0 parts of MMA, 50.0 parts of IBMA, and 10.0 parts of 2-ethylhexyl acrylate (hereinafter “HA”) were charged. It is. Next, the internal temperature of the reaction vessel was adjusted to 55 ° C. while stirring and introducing nitrogen gas.
After confirming that the internal temperature was stable at 55 ° C., 25.0 parts of trimethoxysilylpropyl methacrylate (hereinafter “TMOS-PMA”) was supplied to the reaction vessel. Further, 10 minutes later, 2.4 parts of a 70% solution of tert-butyl peroxypivalate (trade name “Perbutyl PV” manufactured by NOF Corporation) was added as a polymerization initiator to initiate polymerization. As soon as this polymerization initiator was added, the reaction solution became turbid and gradually whitened to become milky white. That is, it was confirmed that polymer fine particles were generated. From the start of addition of the polymerization initiator, the internal temperature was maintained at 55 ° C., and after 6 hours, the polymerization was terminated to obtain a dispersion of polymer fine particles having hydrolyzable silyl groups.
Next, 32.8 parts of 25% aqueous ammonia was added to the dispersion as a basic catalyst for crosslinking hydrolyzable silyl groups, the internal temperature was 62 ° C., and the mixture was held for 3 hours with stirring. As a result, fine particles having a crosslinked structure were formed. When 2.5 hours had elapsed since the addition of the ammonia water, 1.0 part of an antioxidant (trade name “Irganox 245” manufactured by BASF Corporation) was added.
After cooling the reaction solution, it was filtered through a 200-mesh polynet to collect a filtrate (a dispersion of crosslinked resin fine particles). And this dispersion liquid was dried at 60 degreeC until the non volatile matter at the time of heating at 155 degreeC for 30 minutes became 98% or more. After drying, crushing was performed to obtain powdered crosslinked resin fine particles A1. Thereafter, dv, CV, refractive index and Td ₅₀ were obtained by the above method (see Table 1).

Production Examples 2 to 6 and 9 to 13 (Production of crosslinked resin fine particles A2 to A6 and A9 and B1 to B4)
The same procedure as in Production Example 1 was carried out except that the types and amounts of monomers used in the presence of the macromonomer, and the amounts of ion-exchanged water and methanol used were changed as shown in Table 1. Fine particles A2 to A6, A9 and B1 to B4 were obtained. Table 1 shows the physical properties of the obtained crosslinked resin fine particles.

Production Example 7 (Production of crosslinked resin fine particles A7)
The types and amounts of monomers used in the presence of the macromonomer, and the amounts of ion-exchanged water and methanol used are as shown in Table 1, and 9/10 of the monomers used are initially charged, and the rest Was added in 10 minutes after adding the polymerization initiator, and the same operation as in Production Example 1 was performed to obtain crosslinked resin fine particles A7. The physical properties of the obtained A7 are shown in Table 1.

Production Example 8 (Production of crosslinked resin fine particles A8)
The crosslinked resin fine particles A8 were obtained by preparing seed particles SD-1 made of resin fine particles and then polymerizing a vinyl monomer containing a crosslinkable monomer in the presence of the seed particles SD-1. Fine particles.

(1) Production of seed particles SD-1 In a glass reaction vessel equipped with a stirrer, a reflux condenser, a thermometer, a nitrogen gas introduction pipe and a liquid feed pipe connection section, 250 parts of ion-exchanged water, 750 parts of methanol, 40 parts of MMA , 50 parts of IBMA, 10 parts of isobutyl acrylate (hereinafter “IBA”), and 40 parts of an aqueous solution containing the macromonomer (MM-2) obtained above. Subsequently, the temperature of the liquid mixture in the reaction vessel was adjusted to 60 ° C. while stirring and introducing nitrogen gas.
After confirming that the temperature of the mixed solution was stable at 60 ° C., 2.4 parts of a polymerization initiator “perbutyl PV” was added to a glass reaction vessel, and polymerization was started with stirring. As soon as this polymerization initiator was added, the reaction solution became turbid and gradually whitened to become milky white. That is, it was confirmed that polymer fine particles were generated. From the start of addition of the polymerization initiator, the internal temperature was kept at 60 ° C., and after 6 hours, it was cooled to 50 ° C. Thereafter, methanol and water were distilled off under reduced pressure to adjust the solid content to 35.0% to obtain a dispersion containing seed particles SD-1.
The obtained dispersion of seed particles SD-1 was subjected to centrifugal separation, and the supernatant was removed. The volume average particle diameter (dv) of the collected fine particles was measured with a laser diffraction / scattering particle size distribution analyzer. .65 μm.

(2) Production of crosslinked resin fine particles A8 In a glass reaction vessel equipped with a stirrer, reflux condenser, thermometer and nitrogen gas introduction tube, 299 parts of ion-exchanged water, 3.0 parts of 10% KOH aqueous solution, and the above A dispersion of 285.7 parts of the produced seed particle SD-1 was charged. Then, the temperature in reaction container was adjusted to 20 degreeC, stirring these.
On the other hand, 40 parts of MMA, 40 parts of IBMA and 20 parts of trimethylolpropane triacrylate (manufactured by Toagosei Co., Ltd., trade name “Aronix M-309”) were charged into a SUS container and mixed with stirring. Thereafter, an emulsifier aqueous solution in which 1.5 parts of sodium lauryl sulfate as an emulsifier (trade name “Emar 2F-30”) as an emulsifier is dissolved in 100 parts of ion-exchanged water is added to the obtained mixture, followed by emulsification. The mixture was emulsified using a vessel to prepare an emulsion of vinyl monomer.
Next, the vinyl monomer emulsion prepared above is added to the reaction vessel containing the seed particles SD-1, and 2,2′-azobis (2,4-dimethylvalero) as a polymerization initiator is further added. Nitrile) (trade name “V-65”, manufactured by Wako Pure Chemical Industries, Ltd.) 1 part was added, and the mixture was stirred at 20 ° C. for 12 hours to allow the seed monomer SD-1 to absorb the vinyl monomer and the polymerization initiator. .
Thereafter, nitrogen gas was introduced into the gas phase portion in the reaction vessel through a nitrogen gas introduction pipe. And the vinyl monomer absorbed by the seed particle was polymerized by heating up internal temperature over 2 hours from 20 degreeC to 70 degreeC. After reaching 70 ° C., the mixture was further stirred for 2 hours while maintaining the temperature at 70 ° C. Next, 1 part of triethylene glycol bis [3- (3-tert-butyl-4-hydroxy-5-methylphenyl)] propionate (trade name “AO-70” manufactured by ADEKA) as an antioxidant is added to methanol 19. The liquid which melt | dissolved in the part was added and it hold | maintained for 30 minutes at 70 degreeC under stirring. Thereafter, the mixture was cooled to obtain a dispersion containing crosslinked resin fine particles A8.
Next, the dispersion was centrifuged and the supernatant was removed to obtain a precipitated cake containing crosslinked resin fine particles A8. The obtained precipitated cake was mixed with the same mass of ion-exchanged water and redispersed. Then, the centrifugation process was performed again, the supernatant was removed, and the sedimentation cake was obtained. The obtained precipitated cake was dried at 80 ° C. until the non-volatile content reached 98% or more when heated at 155 ° C. for 30 minutes. After drying, crushing was performed to obtain powdered crosslinked resin fine particles A8. Table 1 shows the physical properties of the obtained A8.

Commercially available crosslinked resin fine particles B5 to B7 are shown below. Table 1 shows the volume average particle diameter (dv), coefficient of variation (CV), refractive index, and thermal decomposition temperature (Td ₅₀ ).
B5: Cross-linked polymethyl methacrylate fine particles “GM-0105” (trade name) manufactured by Ganz Kasei Co., Ltd.
B6: Cross-linked polymethyl methacrylate fine particles “GM-0401S” (trade name) manufactured by Ganz Kasei Co., Ltd.
B7: Silicone resin fine particle “Tospearl 120” (trade name) manufactured by Momentive Performance Materials.

The abbreviations of the compounds used in Table 1 and the refractive index values of the respective homopolymers used for calculating the refractive index of the obtained crosslinked resin fine particles are described below.
MMA: Methyl methacrylate (refractive index 1.4900)
IBMA: Isobutyl methacrylate (refractive index: 1.4770)
IBA: Isobutyl acrylate (refractive index 1.4608)
HA: 2-ethylhexyl acrylate (refractive index: 1.4625)
TMOS-PMA: Trimethoxysilylpropyl methacrylate (refractive index 1.4800)
TMPTA: Trimethylolpropane triacrylate (refractive index 1.5135)
St: Styrene (refractive index 1.5900)

4). Example 1 Production of Light Diffusing Resin Composition and Its Molded Product
In this example, the production and evaluation of a composition containing a polycarbonate resin (trade name “Iupilon S-3000F”, refractive index 1.585) manufactured by Mitsubishi Engineering Plastics Co., Ltd.) and a crosslinked resin fine particle A1 are carried out. It was.
After mixing 0.3 g of the crosslinked resin fine particles A1, 59.64 g of the polycarbonate resin, and 0.06 g of an antioxidant (trade name “Irganox B225” manufactured by BASF Corp.), Laboplast mill (manufactured by Toyo Seiki Co., Ltd., LABO PLASTOMILL) was melt-kneaded for 9 minutes at 250 ° C. and 50 rpm to obtain a light diffusing resin composition containing 0.5% of crosslinked resin fine particles A1 (see (3) in Table 2).
The light diffusing resin composition was compression-molded at 4 MPa with a compression molding machine (“SFA-37” manufactured by Shinto Metal Industries Co., Ltd.) using a mold having a cavity having a predetermined shape and size. A flat plate molded product (120 mm long × 120 mm wide × 1.5 mm thick) was produced. Thereafter, the thickness of the flat plate was measured using a micrometer and confirmed to be in the range of 1.50 mm ± 0.05 mm.
Separately, the light-diffusing resin composition was prepared in the same manner as described above except that the blending amounts of the crosslinked resin fine particles A1 and the polycarbonate resin were changed as shown in (1), (2) or (4) of Table 2. And a flat plate molded article was manufactured.
About each molded article obtained by the above, total light transmittance and dispersion degree were measured. The results are shown in Table 2. The absolute value Δn of the refractive index difference between the transparent resin and the crosslinked resin fine particles is also shown.

Example 2
Example 1 except that a GP polystyrene resin (manufactured by Dongbu Chemicals, trade name “SOLARENE GPPS G-116HV”, refractive index 1.590) was used instead of the polycarbonate resin, and the kneading temperature was 200 ° C. The light diffusing resin composition and the flat plate molded product were obtained. Separately, two types of compositions in which the content ratios of the polystyrene resin and the crosslinked resin fine particles A1 were changed were produced. About each obtained molded article, the total light transmittance and dispersion degree were measured. The results are shown in Table 2.

Examples 3 to 10
A light diffusing resin composition and a flat molded article were obtained in the same manner as in Example 1 using the polycarbonate resin and the crosslinked resin fine particles A2 to A9 with the formulation shown in Table 2. About each obtained molded article, the total light transmittance and dispersion degree were measured. The results are shown in Table 2.

Comparative Examples 1-7
A light diffusing resin composition and a flat molded product were obtained in the same manner as in Example 1 using the polycarbonate resin and the crosslinked resin fine particles B1 to B7 with the formulation shown in Table 3. About each obtained molded article, the total light transmittance and dispersion degree were measured. The results are shown in Table 3.

As is clear from Examples 1 to 10, the addition amount of the crosslinked resin fine particles (light diffusing agent) necessary for obtaining a degree of dispersion (light diffusibility) of about 20 degrees is as small as 0.5% or less. Thus, a result showing good diffusion efficiency was obtained. In addition, from the results of Example 1, it can be confirmed that good diffusibility is exhibited in a wide total light transmittance region of approximately 60 to 90% within a range of the addition amount of the crosslinked resin fine particles up to 2.0%. It was.
Focusing on the average volume particle diameter (dv), in Examples 1 to 9 using crosslinked resin fine particles having a dv of 1.8 μm or more, the degree of dispersion at a total light transmittance of about 85% is 20 degrees or more. It was recognized that good diffusivity was exhibited even in a region having a high total light transmittance. In Examples 1 to 4 and 6 to 10 where dv is 2.8 μm or less, the degree of dispersion when the addition amount of the crosslinkable resin fine particles to the transparent resin is 0.5% is 22 degrees or more, Results with better diffusion efficiency were obtained.

On the other hand, Comparative Example 1 in which the refractive index difference Δn between the transparent resin and the crosslinked resin fine particles is small, Comparative Example 3 in which the volume average particle size (dv) of the crosslinked resin fine particles is large, Comparative Example 5 in which the particle size distribution is wide, and Large particle size In Comparative Example 6 having a wide particle size distribution, the dispersion degree is less than 20 degrees when the addition amount of the crosslinked resin fine particles (light diffusing agent) is 0.5%, and the diffusion efficiency is inferior. there were. Further, from the result of Comparative Example 1, it is estimated that the region exhibiting diffusibility with a degree of dispersion of 20 degrees or more is about 70 to 90% or so in the range of the addition amount of the crosslinked resin fine particles up to 2.0%. As a result, the total light transmittance region showing good diffusibility compared with Example 1 was narrow.
In addition, in Comparative Example 2 in which the volume average particle diameter (dv) of the crosslinked resin fine particles is small and in Comparative Example 7 in which the silicone-based crosslinked resin fine particles are used, the dispersion in a high total light transmittance region having a total light transmittance of about 85%. It has been found that the total light transmittance region that can be applied is limited.
Furthermore, Comparative Example 4 in which the monomer components constituting the crosslinkable fine particles are all methacrylic acid ester monomers has a high thermal decomposition rate, and when the crosslinked resin fine particles are used for a light diffusion plate or the like, The result of concern about heat resistance was obtained.

According to the present invention, it is possible to obtain a light diffusing resin composition having good light diffusibility and showing a high degree of dispersion in a wide range of total light transmittance. Moreover, the molded object excellent also in heat resistance etc. can be obtained. For this reason, the light diffusing resin composition of the present invention is used for applications such as light diffusing plates, transmissive screens, liquid crystal panels, and electric signboards for displays that require sufficient luminance and light diffusibility, and a wide range of total light transmission. It is useful for applications such as a cover of a lighting fixture that requires light diffusibility in the rate region.

Claims (10)

1. Including a transparent resin (X) and crosslinked resin fine particles (Y), the absolute value of the difference between the refractive index of the transparent resin (X) and the refractive index of the crosslinked resin fine particles (Y) is 0.095 to 0.115. The volume average particle diameter of the crosslinked resin fine particles (Y) is 1.5 to 3.3 μm, the coefficient of variation of the particle diameter of the crosslinked resin fine particles (Y) is 20% or less, and the crosslinked resin fine particles The light diffusing resin composition is characterized in that, when (Y) is thermally decomposed under a nitrogen gas atmosphere at a temperature rising rate of 10 ° C./min, the temperature at which the mass becomes half is 320 ° C. or higher. .
2. The light diffusing resin composition according to claim 1, wherein the crosslinked resin fine particles (Y) include a structural unit derived from a (meth) acrylic acid ester.
3. A sheet of 1.5 mm thickness produced using the light diffusing resin composition and having a total light transmittance of white light of 85%, a light is vertically applied using a goniometer. The light diffusing resin composition according to claim 1, wherein an angle at which the emitted light having a luminance of 50% with respect to the emitted light at 0 degree is 20 degrees or more when the incident light is incident.
4. The surface of a 1.5 mm thick sheet produced using a light diffusing resin composition in which the mass ratio of the transparent resin (X) and the crosslinked resin fine particles (B) is 100 parts by mass and 0.5 parts by mass, respectively. The light according to claim 1 or 2, wherein when light is incident in a vertical direction using a goniometer, the angle at which the emitted light having a luminance of 50% with respect to the emitted light at 0 degree is 22 degrees or more. A diffusible resin composition.
5. The light diffusing resin composition according to any one of claims 1 to 4, wherein the transparent resin (X) is a polycarbonate resin.
6. 6. The light diffusing resin composition according to claim 1, comprising 0.1 to 2.0 parts by mass of the crosslinked resin fine particles (Y) with respect to 100 parts by weight of the transparent resin (X).
7. The light diffusing resin composition according to any one of claims 1 to 6, wherein the crosslinked resin fine particles (Y) are produced by a dispersion polymerization method.
8. The light diffusibility according to any one of claims 1 to 7, wherein the crosslinked resin fine particles (Y) are crosslinked resin fine particles obtained by silane-crosslinking a (meth) acrylic acid ester-based resin having a hydrolyzable silyl group. Resin composition.
9. A molded article comprising the light diffusing resin composition according to any one of claims 1 to 8.
10. The molded product according to claim 9, wherein the molded product is disposed in a lighting device or a display device.

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