JP2008239898A - Heat-radiating resin composition and molded article containing the same - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a heat-radiating resin excellent in heat radiation, heat deformation resistance, color-toning property, glossiness, impact resistance and bending distortion characteristics, and a molded article containing the same. <P>SOLUTION: This heat-radiating resin composition is provided by containing a thermoplastic resin containing at least 20 mass% copolymer type polybutylene terephthalate and a thermoconductive filler, and having ≥2.0 W/(m×K) heat conductivity, ≥0.7 heat emissivity and ≥30% whiteness. <P>COPYRIGHT: (C)2009,JPO&INPIT

Description

  The present invention relates to a heat-dissipating resin composition excellent in heat dissipation, heat-resistant deformation, toning, gloss, impact resistance, and bending strain characteristics, and a molded article containing the same.

  As the integration density of semiconductor elements such as LSIs increases, the operation speed increases, and electronic components are mounted with high density, heat radiation countermeasures for products having heat-generating components have become major issues. For example, metals and ceramics with high thermal conductivity have been used for housings of electronic components, but in recent years, heat-dissipating resin compositions that have a high degree of freedom in shape selection and are easy to reduce in weight and size are used. ing. In addition, as a result of its application in a wide range of fields, a material having high design properties and excellent glossiness and toning properties on the surface is desired. And high heat-resistant deformation property is also calculated | required.

  As the heat-dissipating resin composition, Patent Document 1 discloses a composition containing graphite particles, and Patent Document 2 discloses a composition containing boron nitride.

JP 2001-60413 A JP-A-8-283456

Since the heat-dissipating resin composition of Patent Document 1 contains graphite particles, the molded product exhibits a black color, and even if a colorant is added, it cannot be colored other than black, Low reflectivity (gloss) and poor electrical insulation.
On the other hand, a molded product using the heat-dissipating resin composition of Patent Document 2 is white, and can be adjusted to a white color or another color by adding a colorant. Moreover, it is excellent in light reflectivity (gloss). And when a polyester-type resin is used as a thermoplastic resin component, it is excellent in heat-resistant deformation property. Thus, the boron nitride-based heat-dissipating resin composition using the polyester-based resin as the thermoplastic resin is excellent in heat distortion resistance, designability, and electrical insulation. However, mechanical strength such as impact resistance and bending strain characteristics is not sufficient, and improvement is required.
An object of the present invention is to provide a heat-dissipating resin composition excellent in heat dissipation, heat-resistant deformation, toning, gloss, impact resistance and bending strain characteristics, and a molded product containing the same.

  As a result of intensive studies to solve the above problems, the inventors of the present invention contain a thermoplastic resin containing at least 20% by mass of copolymerized polybutylene terephthalate and a thermally conductive filler, and have a thermal conductivity of 2. A composition having a thermal emissivity of 0.7 W or more and a whiteness of 30% or more having a heat dissipation, heat distortion resistance, toning property, glossiness, 0 W / (m · K) or more. The inventors found out that they were excellent in impact resistance and bending strain characteristics, and completed the present invention.

The present invention is shown below.
1. It contains a thermoplastic resin containing at least 20% by mass of copolymerized polybutylene terephthalate, and a thermally conductive filler, has a thermal conductivity of 2.0 W / (m · K) or more, and a thermal emissivity of 0.7. It is above, and the heat dissipation resin composition characterized by whiteness being 30% or more.
2. The copolymer polybutylene terephthalate is a polymer obtained by polycondensation of a dicarboxylic acid component comprising a dicarboxylic acid containing terephthalic acid and / or a derivative thereof and a dihydroxy component containing 1,4-butanediol. 2. The heat dissipating resin composition as described in 1 above.
3. The heat dissipation according to 1 or 2 above, wherein the thermoplastic resin is composed of the copolymerized polybutylene terephthalate and the homopolybutylene terephthalate, and the ratio of both is 20 to 95% by mass and 5 to 80% by mass, respectively. Resin composition.
4). The heat dissipation resin according to any one of 1 to 3 above, wherein the content of the heat conductive filler is 20 to 90% by mass when the total of the thermoplastic resin and the heat conductive filler is 100% by mass. Composition.
5. 5. The heat-dissipating resin composition as described in any one of 1 to 4 above, wherein the thermally conductive filler has a scale shape.
6). 6. The heat-dissipating resin composition according to any one of 1 to 5, wherein the thermally conductive filler is boron nitride.
7). Furthermore, the heat dissipation resin composition in any one of said 1 thru | or 6 containing a flame retardant.
8). Furthermore, the heat dissipation in any one of said 1 thru | or 7 which contains a coloring agent and content of this coloring agent is 0.05-30 mass parts when the said thermoplastic resin is 100 mass parts. Resin composition.
9. Furthermore, it contains an ultraviolet absorber and a light stabilizer, and the content ratio of the ultraviolet absorber and the light stabilizer is 5 to 95% by mass and 95 to 5%, respectively, when the total of these is 100% by mass. 9. The heat-dissipating resin composition according to any one of 1 to 8 above, which is% by mass.
10. 10. The heat radiating resin composition according to any one of 1 to 9 above, wherein the light reflectance is 20% or more.
11. A molded product comprising the heat-dissipating resin composition according to any one of 1 to 10 above.

The heat dissipating resin composition of the present invention is excellent in heat dissipating property, heat distortion resistance, toning property, glossiness, impact resistance and bending strain characteristics.
In particular, when the thermoplastic resin is composed of the copolymer type polybutylene terephthalate and the homo type polybutylene terephthalate, and the ratio of both is 20 to 95% by mass and 5 to 80% by mass, respectively, Excellent in resistance and impact resistance.
When the heat conductive filler is boron nitride, heat dissipation, insulation, heat resistance, and light reflection characteristics are more excellent.
According to the composition containing the ultraviolet absorber and the light stabilizer, the light resistance is excellent, and discoloration and a decrease in light reflectance when receiving light are suppressed.

  The molded article of the present invention is excellent in heat dissipation, heat distortion resistance, toning, gloss, impact resistance, and bending distortion characteristics, so that it can be used for telephones (mobile phones, facsimiles), copying machines, printers, computers, electronic dictionaries. OA equipment such as hair dryers; beauty equipment such as dryers; (digital) cameras, (digital) video cameras, projectors, liquid crystal televisions, plasma televisions and other image display / recording equipment; acoustic equipment; indoor lighting equipment; pachinko and other game machines; It is suitable for in-vehicle electronic devices such as lamps, car stereos, and car navigations; various power supply devices; drive devices such as stepping motors; housings for toys such as home game machines; In particular, since it is excellent in toning properties and glossiness, it is suitable for the above-mentioned casing, and also suitable for heat-radiating parts that require high thermal conductivity.

The present invention will be described in detail below.
In the present invention, “(co) polymerization” means homopolymerization and copolymerization, and “(meth) acryl” means acrylic and methacrylic.

1. Heat-dissipating resin composition The heat-dissipating resin composition of the present invention (hereinafter referred to as “the composition of the present invention”) includes a thermoplastic resin containing at least 20% by mass of copolymerized polybutylene terephthalate, a heat-conductive filler, The thermal conductivity is 2.0 W / (m · K) or more, the thermal emissivity is 0.7 or more, and the whiteness is 30% or more.

1-1. Thermoplastic Resin This thermoplastic resin contains at least 20% by mass of copolymerized polybutylene terephthalate. That is, the thermoplastic resin may be only copolymerized polybutylene terephthalate, or may be a mixture of copolymerized polybutylene terephthalate and other thermoplastic resins.

1-1-1. Copolymerized polybutylene terephthalate The copolymerized polybutylene terephthalate is not particularly limited as long as it is a resin having an ester bond in the main chain of the molecule, and may be a saturated polyester resin or an unsaturated polyester resin. There may be. Of these, saturated polyester resins are preferred. Further, the copolymer polybutylene terephthalate may be a crystalline resin or an amorphous resin.

  Examples of the copolymerized polybutylene terephthalate include dicarboxylic acid components containing terephthalic acid and / or derivatives thereof (lower alkyl esters such as dimethyl ester, acid halides such as acid anhydrides and acid chlorides), and 1,4 -What was obtained by polycondensation with the dihydroxy component containing butanediol etc. can be used. Such copolymerized polybutylene terephthalate is substantially more flexible than homopolybutylene terephthalate (PBT) produced from terephthalic acid and / or its derivatives and 1,4-butanediol. It is known to exist and is also called “soft PBT”.

The dicarboxylic acid component preferably contains 30% by mass or more, more preferably 40% by mass or more, and still more preferably 50% by mass or more of terephthalic acid and / or a derivative thereof based on the total amount thereof. Other dicarboxylic acid components other than terephthalic acid and its derivatives include isophthalic acid, phthalic acid, naphthalenedicarboxylic acid (2,6-naphthalenedicarboxylic acid, etc.), diphenyldicarboxylic acid, diphenyletherdicarboxylic acid, diphenylmethanedicarboxylic acid, diphenylethane Aromatic dicarboxylic acids having about 8 to 16 carbon atoms such as dicarboxylic acid, diphenyl ketone dicarboxylic acid, 4,4′-diphenylsulfone dicarboxylic acid or derivatives thereof, cyclohexanedicarboxylic acid (1,2-cyclohexanedicarboxylic acid, 1,3 -Cyclohexanedicarboxylic acid, 1,4-cyclohexanedicarboxylic acid), hexahydrophthalic acid, hexahydroisophthalic acid, hexahydroterephthalic acid, hymic acid, etc. Examples thereof include aliphatic dicarboxylic acids having about 2 to 40 carbon atoms such as adipic acid, pimelic acid, suberic acid, azelaic acid, sebacic acid, dodecanedicarboxylic acid, hexadecanedicarboxylic acid, and dimer acid, or derivatives thereof.
The derivatives of the other dicarboxylic acid components include derivatives capable of forming an ester, for example, lower alkyl esters such as dimethyl ester, acid halides such as acid anhydride and acid chloride, and the like.
The said other dicarboxylic acid component can be used individually by 1 type or in combination of 2 or more types.

The dihydroxy component preferably contains 10% by mass or more, more preferably 30% by mass or more, and still more preferably 50% by mass or more of 1,4-butanediol, based on the total amount. Other dihydroxy components other than 1,4-butanediol include 1,3-butanediol, ethylene glycol, 1,2-propanediol, 1,3-propanediol, 1,5-pentanediol, and neopentyl glycol. , 1,6-hexanediol, 1,8-octanediol, decanediol and the like linear or branched aliphatic alkylene glycol such as alkylene glycol having about 2 to 12 carbon atoms; 1,2-cyclohexanediol, Alicyclic diols such as 1,4-cyclohexanediol, 1,1-cyclohexanedimethylol, 1,4-cyclohexanedimethylol, hydrogenated bisphenol A; hydroquinone, resorcin, dihydroxybiphenyl, naphthalenediol, dihydroxydiphenyl ether, bisphenol A Aromatic diols such as adducts (diethoxylated bisphenol A, etc.) added with alkylene oxide such as ethylene oxide and propylene oxide to bisphenol A; diethylene glycol, triethylene glycol, polyoxyethylene glycol, ditetramethylene glycol, polytetra Examples thereof include polyoxyalkylene glycols such as methylene glycol, dipropylene glycol, tripropylene glycol, polyoxypropylene glycol, and polytetramethylene ether glycol.
In addition, the compound illustrated as these other dihydroxy components may have substituents, such as an alkyl group, an alkoxy group, and a halogen.
The said other dihydroxy component can be used individually by 1 type or in combination of 2 or more types.

  In the polycondensation of the dicarboxylic acid component and the dihydroxy component, as necessary, glycolic acid, m-hydroxybenzoic acid, p-hydroxybenzoic acid, 6-hydroxy-2-naphthalenecarboxylic acid, p-β-hydroxy. Hydroxycarboxylic acids and alkoxycarboxylic acids such as ethoxybenzoic acid, and monofunctional components such as stearyl alcohol, benzyl alcohol, stearic acid, benzoic acid, tert-butylbenzoic acid, benzoylbenzoic acid or ester derivatives thereof; tricarballylic acid, Multifunctional carboxylic acids such as trimellitic acid, trimesic acid, pyromellitic acid; polyhydric alcohols such as glycerin, trimethylolethane, trimethylolpropane, glycerol, pentaerythritol; Ester derivatives It may be used singly or in combination.

In the present invention, preferred copolymer-type polybutylene terephthalate is exemplified below, but a dicarboxylic acid component containing 50% by mass or more of terephthalic acid and / or a derivative thereof, 1,4-butanediol and other dihydroxy components. And a polymer obtained by polycondensation with a dihydroxy component containing 1,4-butanediol, preferably 50 to 90% by mass, more preferably 60 to 90% by mass, and the other dihydroxy component described above As such, polyoxyalkylene glycols containing oxyalkylene units having a poly (oxy-alkylene) unit such as diethylene glycol and polytetramethylene glycol and having a repeating number of about 2 to 4 are preferred.
(1) A dicarboxylic acid component comprising terephthalic acid and / or a derivative thereof, 1,4-butanediol and another dihydroxy component, and 1,4-butanediol is preferably 50 to 90% by mass, more preferably Is a polymer obtained by polycondensation with 60 to 90% by mass of a dihydroxy component.
(2) Preferably from 50% by weight or more, more preferably from 70% by weight or more of terephthalic acid and / or derivatives thereof, and preferably from 50% by weight or less, more preferably from 30% by weight or less of isophthalic acid and / or derivatives thereof. And a dihydroxy component containing 1,4-butanediol and other dihydroxy components, and preferably containing 1,4-butanediol in an amount of 50 to 90% by mass, more preferably 60 to 90% by mass. A polymer obtained by polycondensation.

  The glass transition temperature of the copolymerized polybutylene terephthalate is preferably 0 to 75 ° C. The lower limit temperature is more preferably 0 ° C. The upper limit temperature is more preferably less than 70 ° C, still more preferably less than 65 ° C, particularly preferably less than 60 ° C, and most preferably less than 50 ° C. If the glass transition temperature is too low, the mechanical strength and heat resistance of the molded article containing the composition of the present invention are not sufficient, while if too high, the flexibility is inferior. The glass transition temperature can be obtained by a dynamic viscoelasticity measurement method.

  The copolymer type polybutylene terephthalate has a melt viscosity of 250 ° C., a shear rate of 91.2 (1 / second), a nozzle diameter of 1 mmφ, and a nozzle channel length of 30 mm (L / D = 30) from the viewpoint of molding processability. When measured under conditions, it is preferably 400 to 2500 Pa · s, more preferably 600 to 1300 Pa · s.

As a method for producing the copolymer-type polybutylene terephthalate, raw material components such as a dicarboxylic acid component containing terephthalic acid and / or a derivative thereof and a dihydroxy component containing 1,4-butanediol are used as one or a plurality of esterification reaction vessels. In the presence of an esterification reaction catalyst, the temperature is usually 150 to 280 ° C., preferably 180 to 265 ° C., and usually 50 to 1000 Torr (6666 to 133322 Pa), preferably 70 to 760 Torr (9333 to 101325 Pa). ) Under the condition of pressure), the esterification reaction is carried out for 2 to 5 hours with stirring, and the resulting esterification reaction product (oligomer) is transferred to a polycondensation reaction tank and in one or a plurality of polycondensation reaction tanks. In the presence of a polycondensation reaction catalyst, usually 210 to 280 ° C, preferably 220 to 265 ° C Temperature, and, typically, 200Torr (26664Pa) or less, preferably 150Torr (19998Pa) following pressure, in conditions, can be stirring 2-5 hours polycondensation reaction. The reaction format may be any of continuous type, semi-continuous type or batch type.
In addition, the resin obtained by the polycondensation reaction is usually transferred from the bottom of the polycondensation reaction tank to a polymer extraction die and extracted into a strand shape, cooled with water, or after being cooled with water and cut with a cutter to give pellets. And a granular material such as a chip.

  Examples of the esterification reaction catalyst include titanium compounds, tin compounds, magnesium compounds, calcium compounds, and zirconium compounds.

1-1-2. Other thermoplastic resins Other thermoplastic resins are not particularly limited as long as they include a polymer having thermoplasticity; polyester resins other than copolymerized polybutylene terephthalate; polycarbonate resins; ABS resins, ASA resins Rubber-reinforced resin such as AES resin; polystyrene, styrene / acrylonitrile copolymer, styrene / maleic anhydride copolymer, styrene-based (co) polymer such as (meth) acrylic acid ester / styrene copolymer; polyethylene, Polyolefin resins such as polypropylene; Polyarylate resins; Polyamide polymers; Polyacetal resins; Vinyl chloride resins such as polyvinyl chloride, ethylene / vinyl chloride polymers and polyvinylidene chloride; Polymethyl methacrylate (PMMA) and the like ( One or more of (meth) acrylic acid esters were used ( Co) polymer and other acrylic resins; polyphenylene ether; polyphenylene sulfide; fluorine resins such as polytetrafluoroethylene and polyvinylidene fluoride; liquid crystal polymers; imide resins such as polyimide, polyamideimide, and polyetherimide; polyether ketone, Ketone resins such as polyether ether ketone; Sulfone resins such as polysulfone and polyether sulfone; Urethane resins; Polyvinyl acetate; Polyethylene oxide; Polyvinyl alcohol; Polyvinyl ether; Polyvinyl butyral; Phenoxy resin; And other plastics. These can be used alone or in combination of two or more. Of these, polyester resins such as homopolybutylene terephthalate, polycarbonate resins and rubber reinforced resins are preferred.

  The homopolybutylene terephthalate is a heavy polymer obtained from terephthalic acid and / or a derivative thereof (lower alkyl ester such as dimethyl ester, acid halide such as acid anhydride or acid chloride) and 1,4-butanediol. It is a condensate. The homopolybutylene terephthalate is usually a crystalline resin.

When the thermoplastic resin constituting the composition of the present invention is composed of copolymerized polybutylene terephthalate and homopolybutylene terephthalate, these contents are 20% when the total of both is 100% by mass. It is -95 mass% and 5-80 mass%, Preferably it is 50-90 mass% and 10-50 mass%. If these content ratios are in the above range, the balance between physical properties of heat distortion resistance and impact resistance is particularly excellent.
In addition, when the said thermoplastic resin consists only of copolymerization type polybutylene terephthalate, impact resistance and a bending distortion characteristic are still more excellent.

1-2. Thermally conductive filler As this thermally conductive filler, the thermal conductivity at 25 ° C is preferably 30 W / (m · K) or more, more preferably 80 W / (m · K) or more, and further preferably 100 W / (m. · K) or more, particularly preferably a material of 150 W / (m · K) or more. Examples of the heat conductive filler according to the present invention include boron nitride, aluminum nitride, silicon nitride, zinc oxide, aluminum oxide, magnesium oxide, calcium titanate and the like because of excellent insulation. In addition, a composite filler formed by forming a shell by coating the above compound with inorganic particles or organic particles made of a substance other than the above as a core can also be used. Further, by using an insulating heat conductive filler, it is possible to obtain a heat-dissipating resin composition having insulation properties, and the surface resistivity (insulation index, value of the molded product containing this composition increases as the value increases. The insulating property is preferably 1 × 10 ¹³ Ω or more, more preferably 1 × 10 ¹⁴ Ω or more. Within this range, the insulation is excellent.
Furthermore, the thermal conductive filler is preferably a white material from the viewpoint of light reflectivity, and among these, boron nitride and zinc oxide are preferable, and boron nitride is particularly preferable. When a material made of boron nitride is used as the heat conductive filler, a heat dissipating resin composition having a high level of physical balance among heat dissipation, heat resistance and reflection characteristics can be obtained.

As boron nitride, a plurality of stable structures such as c-BN (zinc blende structure), w-BN (wurtzite structure), h-BN (hexagonal crystal structure), r-BN (rhombohedral crystal structure) are known. It has been. In the present invention, any boron nitride can be used, but hexagonal boron nitride is preferred. By using hexagonal structure boron nitride, the wear of the molding machine and the mold used for obtaining the molded product can be reduced.
Hexagonal boron nitride has a layered crystal structure, and the shape thereof is a flat plate (scale-like). In boron nitride having this layered structure, the thermal conductivity in the direction parallel to the layer (a-axis direction) is said to be about 30 times that in the direction perpendicular to the layer (c-axis direction).

  Moreover, as a zinc oxide, a well-known thing can be used, The shape is not specifically limited, Either spherical shape and an indefinite shape may be sufficient. The zinc oxide may be one coated with a silicone resin, one treated with a coupling agent such as a silane coupling agent, a titanate coupling agent, or an aluminum coupling agent.

  The shape of the heat conductive filler is not particularly limited, and may be spherical, linear (fibrous), flat (scale-like), curved, needle-like, etc. (Single-grain agglomerates) may be used. Use of a scaly product is preferable because a molded product having excellent thermal conductivity can be obtained and the mechanical properties can be improved. Moreover, if this heat conductive filler is scale-like and is a white color, the composition of this invention is excellent in the reflective characteristic with respect to light.

The average particle diameter (or average value of the maximum length) of the heat conductive filler is preferably 1 to 350 μm, more preferably 2 to 200 μm. Moreover, an aspect ratio becomes like this. Preferably it is 3 or more, More preferably, it is 5 or more, More preferably, it is 6-20. Furthermore, the purity is preferably 98% or more, more preferably 99% or more. By setting it as said range, it is excellent in heat dissipation and whiteness. Further, the bulk density is preferably 0.8 g / cm ² or less, more preferably 0.7 g / cm ² or less. By setting it as each said range, the resin composition excellent in heat dissipation can be obtained. The specific surface area is not particularly limited.

  The content of iron oxide in the thermally conductive filler is preferably 0.01% by mass or less, more preferably 0.001% by mass or less. When this content is too large, the whiteness of the molded product tends to be inferior.

  When the thermal conductive filler contains scaly boron nitride, the boron nitride itself is excellent in whiteness, so that it is easy to obtain a molded product with high whiteness by the composition of the present invention, and excellent in reflection characteristics with respect to light. . In addition, if the average particle size of boron nitride used in the composition of the present invention is preferably in the range of 1 to 350 μm, more preferably in the range of 2 to 200 μm, heat dissipation, insulation, and light reflection characteristics. Can be obtained. If the average particle size is in the above range, boron nitrides having different particle sizes may be used in combination.

  Moreover, when the said heat conductive filler contains zinc oxide, since it is excellent in whiteness, it is easy to obtain a molded article with high whiteness with the composition of this invention, and it is excellent in the reflective characteristic with respect to light. Moreover, if the average particle diameter of the zinc oxide used when setting it as the composition of this invention becomes like this. Preferably it is 1-50 micrometers, More preferably, it is 2-30 micrometers, It was excellent in heat dissipation and the reflective characteristic with respect to light. A molded product can be obtained.

  The content ratio of the heat conductive filler in the composition of the present invention is preferably 20 to 90% by weight, more preferably, when the total of the thermoplastic resin and the heat conductive filler is 100% by weight. It is 25-90 mass%, More preferably, it is 30-70 mass%, Most preferably, it is 31-60 mass%. If the content of the heat conductive filler is too large, the moldability, impact resistance and bending strain characteristics tend to be inferior. On the other hand, if the content is too small, the heat dissipation tends to be inferior.

1-3. Additives The composition of the present invention may contain additives depending on the purpose and application. These additives include flame retardants, UV absorbers, light stabilizers, colorants, transesterification inhibitors, fillers, thermal stabilizers, antioxidants, anti-aging agents, antistatic agents, plasticizers, lubricants, release agents. Examples include molds, antibacterial agents, crystal nucleating agents, flow modifiers, impact modifiers, and the like.

Examples of the flame retardant include organic flame retardants, inorganic flame retardants, and reactive flame retardants. These can be used alone or in combination of two or more.
Organic flame retardants include brominated epoxy compounds, brominated alkyltriazine compounds, brominated bisphenol epoxy resins, brominated bisphenol phenoxy resins, brominated bisphenol polycarbonate resins, brominated polystyrene resins, brominated crosslinked polystyrene resins Halogenated flame retardants such as brominated bisphenol cyanurate resin, brominated polyphenylene ether, decabromodiphenyl oxide, tetrabromobisphenol A and oligomers thereof; trimethyl phosphate, triethyl phosphate, tripropyl phosphate, tributyl phosphate, tripentyl phosphate, toki Hexyl phosphate, tricyclohexyl phosphate, triphenyl phosphate, tricresyl phosphate, trixylenyl phosphate Phosphate esters such as phosphate, cresyl diphenyl phosphate, dicresyl phenyl phosphate, dimethyl ethyl phosphate, methyl dibutyl phosphate, ethyl dipropyl phosphate, hydroxyphenyl diphenyl phosphate, compounds modified with these substituents, various condensed types Phosphorus ester compounds, phosphorus flame retardants such as phosphazene derivatives containing phosphorus element and nitrogen element; polytetrafluoroethylene, guanidine salts, silicone compounds, phosphazene compounds, and the like. These can be used alone or in combination of two or more.

Examples of the inorganic flame retardant include aluminum hydroxide, antimony oxide, magnesium hydroxide, zinc borate, zirconium compound, molybdenum compound, and zinc stannate. These can be used alone or in combination of two or more.
Reactive flame retardants include tetrabromobisphenol A, dibromophenol glycidyl ether, brominated aromatic triazine, tribromophenol, tetrabromophthalate, tetrachlorophthalic anhydride, dibromoneopentyl glycol, poly (pentabromobenzyl polyacrylate) , Chlorendic acid (hett acid), chlorendic anhydride (hett acid anhydride), brominated phenol glycidyl ether, dibromocresyl glycidyl ether and the like. These can be used alone or in combination of two or more.

The content of the flame retardant is usually 5 to 30 parts by mass, preferably 5 to 20 parts by mass when the amount of the thermoplastic resin is 100 parts by mass.
In addition, when making the composition of this invention contain a flame retardant, it is preferable to use a flame retardant adjuvant. As this flame retardant aid, antimony trioxide, antimony tetroxide, antimony pentoxide, sodium antimonate, antimony tartrate and other antimony compounds, zinc borate, barium metaborate, hydrated alumina, zirconium oxide, Examples include ammonium polyphosphate and tin oxide. These can be used alone or in combination of two or more.

  Examples of the ultraviolet absorber include 2,4-dihydroxybenzophenone, 2-hydroxy-4-methoxybenzophenone, 2,2′-dihydroxy-4-methoxybenzophenone, 2,2′-dihydroxy-4,4′-dimethoxybenzophenone, Mixtures of 2,2′-dihydroxy-4,4′-dimethoxybenzophenone with other 4-substituted benzophenones, 2-hydroxy-4-methoxy-2′-carboxybenzophenone, 2-hydroxy-4-methoxy-5-sulfobenzophenone Trihydrate, 2-hydroxy-4-n-octoxybenzophenone, 2,2 ′, 4,4′-tetrahydroxybenzophenone, 4-dodecyloxy-2-hydroxybenzophenone, bis (5-benzoyl-4-hydroxy-) 2-methoxyphenyl) methane, benzof Benzophenones such as non-compounds; 2- (2′-hydroxy-5′-methylphenyl) benzotriazole, 2- (2′-hydroxy-3 ′, 5′-di-tert-butylphenyl) benzotriazole, 2- (2′-hydroxy-3′-tert-butyl-5′-methylphenyl) -5-chlorobenzotriazole, 2- (2′-hydroxy-3 ′, 5′-di-tert-butylphenyl) -5 Chlorobenzotriazole, 2- (2′-hydroxy-5′-tert-octylphenyl) benzotriazole, 2- (2′-hydroxy-3 ′, 5′-di-tert-amylphenyl) benzotriazole, 2- ( 2'-hydroxy-3 ', 5'-di-tert-butylphenyl) benzotriazole, 2- [2'-hydroxy-3'- 3 ", 4", 5 ", 6" -tetrahydrophthalimidomethyl) -5'-methylphenyl] benzotriazole, 2,2'-methylenebis [4- (1,1,3,3-tetramethylbutyl) -6 -(2H-benzotriazol-2-yl) phenol], benzotriazole derivatives such as benzotriazole derivatives; salicylic acid esters such as phenyl salicylate and p-tert-butylphenyl salicylate; nickel bis-octylphenylsulfamide, [2, 2′-thiobis (4-tert-octylphenolate)]-n-butylamine nickel, [2,2′-thiobis (4-tert-octylphenolate)]-2-ethylhexylamine nickel, nickel dibutyldithiocarbamate, ethyl -3,5-di-tert-butyl-4-hydride Metal complex salts such as nickel salt of oxybenzyl phosphate and nickel thiobisphenol complex; Shu such as 2-ethoxy-5-tert-butyl-2′-ethyl oxalate bisanilide, 2-ethoxy-2-ethyl oxalate bisanilide Acid anilide derivatives; benzoic acid derivatives such as methyl o-benzoylbenzoate, resorcinol-monobenzoate, 2,4-di-tert-butylphenyl-3,5-di-tert-butyl-4-hydroxybenzoate; 2-ethylhexyl 2-cyano-3,3-diphenyl acrylate, 1,3-bis- (4-benzoyl-3-hydroxyphenoxy) -2-propyl acrylate, 1,3-bis- (4-benzoyl-3-hydroxyphenoxy) 2-propyl methacrylate, 2-hydroxy-4-methoxyben Examples include zophenone-5-sulfonic acid and ethyl-2-cyano-3,3-diphenyl acrylate. These can be used alone or in combination of two or more.

  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, 1- [2 -{3- (3,5-di-tert-butyl-4-hydroxyphenyl) propionyloxy} ethyl] -4- {3- (3,5-di-tert-butyl-4-hydroxyphenyl) propionyloxy} -2,2,6,6-tetramethylpiperidine, 8-benzyl-7,7,9,9-tetramethyl-3-octyl-1,2,3-triazaspiro [4,5] undecane-2,4- Dione, 4-benzoyloxy-2,2,6,6-tetramethylpiperidine, dimethyl-1- (2-hydroxyethyl) -4-hydroxy-2,2,6,6-tetramethylpiperidine succinate Polycondensate, poly [[6- (1,1,3,3-tetramethylbutyl) imino-1,3,5-triazine-2,4-diyl] [(2,2,6,6-tetra Methyl-4-piperidyl) imino] hexamethylene [[(2,2,6,6-tetramethyl-4-piperidyl) imino]], 2- (3,5-di-tert-butyl-4-hydroxybenzyl) 2-n-butyl-bis (1,2,2,6,6-pentamethyl-4-piperidyl) malonate, tetrakis (2,2,6,6-tetramethyl-4-piperidyl) -1,2,3 , 4-butanetetracarboxylate, 1,2,3,4-butanetetracarboxylic acid, 1,2,2,6,6-pentamethyl-4-piperidinol and tridecyl alcohol condensate, 2,2 , 6,6-tetramethyl-4-pi Condensation product of lizinol and tridecyl alcohol, 1,2,3,4-butanetetracarboxylic acid, 1,2,2,6,6-pentamethyl-4-piperidinol, β, β, β ′, β A condensate with '-tetramethyl-3,9- (2,4,8,10-tetraoxaspiro [5.5] undecane) diethanol, 1,2,3,4-butanetetracarboxylic acid, 2,6,6-tetramethyl-4-piperidinol and β, β, β ′, β′-tetramethyl-3,9- (2,4,8,10-tetraoxaspiro [5.5] undecane) Condensate with diethanol, 1,2,2,6,6-pentamethyl-4-piperidyl methacrylate, 2,2,6,6-tetramethyl-4-piperidyl methacrylate, bis (1-octyloxy-2,2, 6,6-tetramethyl- -Piperidyl) sebacate, 2- (3,5-di-tert-butyl-4-hydroxyphenyl) -2-n-butyl-bis (2,2,6,6-tetramethyl-4-piperidyl) malonate, 2 -(3,5-di-tert-butyl-4-hydroxyphenyl) -2-n-butyl-bis (1,2,2,6,6-pentamethyl-4-piperidyl) malonate, 2- (3,5 -Di-tert-butyl-4-hydroxybenzyl) -2-n-butyl-bis (2,2,6,6-tetramethyl-4-piperidyl) malonate, tetrakis (1,2,2,6,6- Pentamethyl-4-piperidyl) -1,2,3,4-butanetetracarboxylate, 1,2-bis (3-oxo-2,2,6,6-tetramethyl-4-piperidyl) ethane, 1- ( 3,5-di-t ert-butyl-4-hydroxyphenyl) -1,1-bis (2,2,6,6-tetramethyl-4-piperidyloxycarbonyl) pentane, poly [1-oxyethylene (2,2,6,6- Tetramethyl-1,4-piperidyl) oxysuccinyl], poly [2- (1,1,4-trimethylbutylimino) -4,6-triazinediyl- (2,2,6,6-tetramethyl-4- Piperidyl) iminohexamethylene- (2,2,6,6-tetramethyl-4-piperidyl) imino], N, N′-bis (3-aminopropyl) ethylenediamine-2,4-bis [N-butyl-N -(2,2,6,6-tetramethyl-4-piperidyl) amino] -6-chloro-1,3,5-triazine condensate and hindered amines such as N-methyl compounds thereof; Semicarbazones such as hexamethylenebis- (N, N-dimethylsemicarbazide)) and (1,1,1 ′, 1′-tetramethyl-4,4 ′-(methylenedi-p-phenylene) disemicarbazide) It is done. These can be used alone or in combination of two or more.

When the ultraviolet absorber and the light stabilizer described above are used, the light resistance is excellent, and it is possible to suppress discoloration and decrease in light reflectance when receiving light from sunlight or the like.
The content of the ultraviolet absorber and / or light stabilizer is preferably 0.05 to 10 parts by mass, more preferably 0.1 to 5 parts by mass, when the amount of the thermoplastic resin is 100 parts by mass. Part, more preferably 0.2 to 5 parts by mass. In addition, by using the ultraviolet absorber and the light stabilizer in combination, the effect of improving the defect phenomenon becomes remarkable, and the mass ratio in that case is preferably respectively when the total of both is 100 mass%. 5 to 95% by mass and 5 to 95% by mass, more preferably 10 to 90% by mass and 90 to 10% by mass, further preferably 15 to 85% by mass and 85 to 15% by mass, particularly preferably 40 to 60% by mass. And 60 to 40% by mass.

As the colorant, any of dyes, inorganic pigments, and organic pigments may be used. Moreover, you may use combining these. The color of the colorant is not particularly limited, and may be white, red, yellow, blue, green, or other chromatic colors.
As dyes, nitroso dyes, nitro dyes, azo dyes, stilbene azo dyes, ketoimine dyes, triphenylmethane dyes, xanthene dyes, acridine dyes, quinoline dyes, methine / polymethine dyes, thiazole dyes, indamine / indophenol dyes, azine dyes Oxazine dye, thiazine dye, sulfur dye, aminoketone / oxyketone dye, anthraquinone dye, indigoid dye, phthalocyanine dye and the like.

Examples of inorganic pigments include white inorganic pigments, red inorganic pigments, yellow inorganic pigments, green inorganic pigments, and blue inorganic pigments. These may be used alone or in combination of two or more. Can do.
Examples of the white inorganic pigment include TiO ₂ , Al ₂ O ₃ .nH ₂ O, [ZnS + BaSO ₄ ], CaSO ₄ .2H ₂ O, BaSO ₄ , CaCO ₃ , 2PbCO ₃ .Pb (OH) _{2 and the} like. .
Examples of the red inorganic pigment include CdS · nCdSe, PbCrO ₄ · mPbMoO ₄ · nPbSO ₄ , TiO ₂ · Sb ₂ O ₃ · NiO, Zn-Fe composite oxide (ZnO · Fe ₂ O ₃ etc.), Zn- Fe-Cr-based composite oxide _{(ZnO · Fe 2 O 3 ·} Cr 2 O 3 , etc.) and the like.
Examples of the yellow inorganic pigment include TiO ₂ · BaO · NiO, TiO ₂ · NiO · Sb ₂ O ₃ , Fe ₂ O ₃ · H ₂ O, PbCrO ₄ , Pb (SbO ₃ ) ₂ , Pb ₃ (SbO ₄ ). ₂ , Ti-Sb-Ni composite oxide, Ti-Sb-Cr composite oxide, and the like.
Examples of the green inorganic pigment include Cu (C ₂ H ₃ O ₂ ) ₃ , Cu (AsO ₂ ) ₂ , CoO · nZnO, BaMnO ₂ , Cu ₂ (OH) ₂ (CO ₃ ), and Ti—Co—Ni—. Examples thereof include Zn-based composite oxides.
Examples of the blue inorganic _{pigments, CoO · nAl 2 O 3,} CoO · nSnO · mMgO, Na 6 Al 6 (SiO 4) 6 · 2Na 3 SO 4 , and the like.

  Examples of organic pigments include azo lake pigments, benzoimidazolone pigments, diarylide pigments, azo pigments such as condensed azo pigments, phthalocyanine pigments such as phthalocyanine blue and phthalocyanine green, isoindolinone pigments, quinophthalone pigments, quinacridone pigments, Examples include perylene pigments, anthraquinone pigments, perinone pigments, and condensed polycyclic pigments such as dioxazine violet.

  When the chromatic colorant is a dark colorant alone, it can be used after being lightened with a white colorant in order to achieve a target whiteness.

  The content of the colorant is preferably 0.05 to 30 parts by mass, more preferably 0.1 to 15 parts by mass, and still more preferably 0.1 when the amount of the thermoplastic resin is 100 parts by mass. -10 parts by mass.

The transesterification inhibitor is not particularly limited, but a phosphoric acid compound having a PO bond is preferably used. Specific examples thereof include phosphoric acid, phosphorous acid, phosphonic acid, hypophosphorous acid and pyrophosphoric acid, derivatives thereof, silyl phosphate, and the like.
The content of the transesterification inhibitor is preferably 0.01 to 5 parts by mass, more preferably 0.02 to 3 parts by mass, and still more preferably 0 when the amount of the thermoplastic resin is 100 parts by mass. 0.03 to 1 part by mass. When the transesterification inhibitor is used in this range, deterioration due to heat during the molding process is suppressed, and a molded article excellent in impact resistance, whiteness and glossiness can be obtained.

Examples of the filler include talc, mica, clay, wollastonite, silica, calcium carbonate, glass fiber, glass beads, glass balloon, milled fiber, glass flake, aramid fiber, polyarylate fiber, and the like. These can be used alone or in combination of two or more.
The content of the filler is usually 3 to 30 parts by mass when the amount of the thermoplastic resin is 100 parts by mass.

Examples of the heat stabilizer include phosphites, hindered phenols, thioethers, and the like. These can be used alone or in combination of two or more.
Content of the said heat stabilizer is 0.1-5 mass parts normally, when the quantity of the said thermoplastic resin is 100 mass parts.

Examples of the antioxidant include hindered amines, hydroquinones, hindered phenols, and sulfur-containing compounds. These can be used alone or in combination of two or more.
The content of the antioxidant is usually 0.1 to 5 parts by mass when the amount of the thermoplastic resin is 100 parts by mass.

Examples of the antiaging agent include naphthylamine compounds, diphenylamine compounds, p-phenylenediamine compounds, quinoline compounds, hydroquinone derivative compounds, monophenol compounds, bisphenol compounds, trisphenol compounds, polyphenol compounds. Thiobisphenol compound, hindered phenol compound, phosphite compound, imidazole compound, nickel dithiocarbamate salt compound, phosphate compound and the like. These can be used alone or in combination of two or more.
The content of the anti-aging agent is usually 0.1 to 5 parts by mass when the amount of the thermoplastic resin is 100 parts by mass.

Examples of the plasticizer include phthalates such as dimethyl phthalate, diethyl phthalate, dibutyl phthalate, diisobutyl phthalate, dioctyl phthalate, butyl octyl phthalate, di- (2-ethylhexyl) phthalate, diisooctyl phthalate, and diisodecyl phthalate; dimethyl adipate , Diisobutyl adipate, di- (2-ethylhexyl) adipate, diisooctyl adipate, diisodecyl adipate, octyl decyl adipate, di- (2-ethylhexyl) azelate, diisooctyl azelate, diisobutyl azelate, dibutyl sebacate, di- Fatty acid esters such as (2-ethylhexyl) sebacate, diisooctyl sebacate; trimellitic acid isodecyl ester, trimellitic acid octy Esters, trimellitic acid esters such as trimellitic acid n-octyl ester, trimellitic acid isononyl ester; di- (2-ethylhexyl) fumarate, diethylene glycol monooleate, glyceryl monoricinolate, trilauryl phosphate, tristearyl phosphate , Tri- (2-ethylhexyl) phosphate, epoxidized soybean oil, polyether ester and the like. These can be used alone or in combination of two or more.
Content of the said plasticizer is 0.1-15 mass parts normally, when the quantity of the said thermoplastic resin is 100 mass parts.

Examples of the lubricant include fatty acid ester, hydrocarbon resin, paraffin, higher fatty acid, oxy fatty acid, fatty acid amide, alkylene bis fatty acid amide, aliphatic ketone, fatty acid lower alcohol ester, fatty acid polyhydric alcohol ester, fatty acid polyglycol ester, aliphatic Examples include alcohol, polyhydric alcohol, polyglycol, polyglycerol, metal soap, silicone, and modified silicone. These can be used alone or in combination of two or more.
The content of the lubricant is usually 0.1 to 5 parts by mass when the amount of the thermoplastic resin is 100 parts by mass.

Examples of the antibacterial agents include zeolite antibacterial agents such as silver zeolite and silver-zinc zeolite, silica gel antibacterial agents such as complexed silver-silica gel, glass antibacterial agents, calcium phosphate antibacterial agents, and zirconium phosphate antibacterial agents. Silicate antibacterial agents such as silver-magnesium aluminate, titanium oxide antibacterial agents, ceramic antibacterial agents, whisker antibacterial agents, etc .; formaldehyde releasing agents, halogenated aromatic compounds, road Organic antibacterial agents such as propargyl derivatives, thiocyanate compounds, isothiazolinone derivatives, trihalomethylthio compounds, quaternary ammonium salts, biguanide compounds, aldehydes, phenols, pyridine oxide, carbanilide, diphenyl ether, carboxylic acid, organometallic compounds; inorganic and organic Hybrid antibacterial agent; natural anti Agent, and the like. These can be used alone or in combination of two or more.
Content of the said antibacterial agent is 0.05-5 mass parts normally, when the quantity of the said thermoplastic resin is 100 mass parts.

  Examples of the impact modifier include graft rubber.

1-4. Method for Producing Composition The composition of the present invention is produced by supplying the raw material components weighed so as to have the above predetermined content to an extruder, a Banbury mixer, a kneader, a roll, a feeder ruder, and kneading. be able to. The method for supplying the raw material components is not particularly limited, and the respective components may be mixed and kneaded in a lump, or may be kneaded in multiple stages and divided.
In addition, although kneading | mixing temperature is selected by the kind of the said thermoplastic resin, and content of the said heat conductive filler, it is 200-300 degreeC normally.

1-5. Properties of Composition In the composition of the present invention, the thermal conductive filler is uniformly dispersed using the thermoplastic resin as a matrix. Therefore, the molded article containing the composition of the present invention is excellent in heat dissipation, heat resistance and light resistance. In addition, when the said heat conductive filler consists of boron nitride, it is excellent also in insulation and the reflective property with respect to light.
In the composition of the present invention, the thermal conductivity at 25 ° C. is 2.0 W / (m · K) or more, preferably 3.0 to 10.0 W / (m · K), more preferably 4.0. It is -5.0W / (m * K). If the said heat conductivity is the said range, it will be excellent in the physical property balance of heat dissipation and mechanical strength. When the thermal conductivity is less than 2.0 W / (m · K), the heat dissipation tends to be inferior. In addition, the said heat conductivity is the value measured with respect to the flow direction of the composition when a molded article is manufactured, and a measuring method is demonstrated in [Example] mentioned later.
This thermal conductivity can be adjusted by appropriately selecting the type, shape and content of the thermal conductive filler.
The thermal emissivity is 0.7 or more, preferably 0.75 or more, more preferably 0.8 or more. If the thermal emissivity is less than 0.7, the heat dissipation is not sufficient. A method for measuring the thermal emissivity will be described later in [Example].
This thermal emissivity can be adjusted by appropriately selecting the type and content of the thermally conductive filler.
Further, the whiteness is 30% or more, preferably 40% or more, more preferably 50% or more, and particularly preferably 70% or more. The higher the whiteness is, the more excellent the light reflection property is. However, even when the molded product is colored, the light reflection property is excellent if it is 30% or more. The whiteness can be measured with a hunter-type colorimetric color difference meter.
This whiteness can be adjusted by appropriately selecting the type and content of the thermoplastic resin, the type and content of the thermally conductive filler, and the type and content of the colorant.

In the composition of the present invention, the light reflectance is preferably 20% or more, more preferably 30% or more, still more preferably 50% or more, and particularly preferably 60% or more. The higher the light reflectance, the better the glossiness. In addition, the measuring method of a light reflectivity is demonstrated in below-mentioned [Example].
Furthermore, the heat distortion temperature according to ISO75 (load 1.80MPa) is 120 degreeC or more, Preferably it is 130-300 degreeC, More preferably, it is 130-280 degreeC. When this heat distortion temperature is in the above range, the heat distortion resistance is excellent.
This heat distortion temperature can be adjusted by appropriately selecting the type and content of the thermoplastic resin, the type, shape and content of the thermally conductive filler.
The bending strain according to ISO 178 is preferably 1.0% or more, more preferably 1.2 to 8%, and still more preferably 1.5 to 8%. If the said bending strain is the said range, the physical property balance of a bending strain characteristic and rigidity is in a high level, and it is preferable. When this bending strain is less than 1.0%, cracks tend to occur when various members, which are molded articles containing the composition of the present invention, are assembled and operations such as assembling are performed.
This bending strain can be adjusted by appropriately selecting the type and content of the thermoplastic resin, the type, shape and content of the thermally conductive filler.
Regarding the insulation of the composition, the surface specific resistance (insulation index, the higher the value, the better the insulation) of the molded article containing the composition of the present invention is preferably 1 × 10 ¹³ Ω or more, more preferably 1. × 10 ¹⁴ Ω or more. Within this range, the insulation is excellent.

2. Molded Article The molded article of the present invention is characterized by including the composition of the present invention.
Since the composition of the present invention has excellent properties as described above, the molded product of the present invention includes OA equipment such as a telephone (mobile phone, facsimile), copying machine, printer, computer, electronic dictionary; Beauty equipment such as dryers; acoustic equipment; indoor lighting equipment; pachinko and other game machines; in-vehicle electronic equipment such as lamps, car stereos, and car navigation systems; various power supply devices; driving devices such as stepping motors; toys such as home game machines It is suitable for a heat dissipation component such as a casing, a substrate, and the like. In particular, since it is excellent in toning properties and glossiness, it is suitable for the above-mentioned casing, and also suitable for heat-radiating parts that require high thermal conductivity. In addition, it does not apply to LED related members, such as a LED mounting substrate and a reflector disposed on the LED mounting substrate.

  Hereinafter, the present invention will be described in more detail with reference to examples. However, the present invention is not limited to such examples as long as the gist of the present invention is not exceeded. In the following, parts and% are Unless otherwise specified, it is based on mass.

The raw material components of the compositions used in the following examples and comparative examples are shown.
1. Thermoplastic resin (1) A1; copolymerized polybutylene terephthalate (modified PBT with flexibility; copolymer of dimethyl terephthalate, 1,4-butanediol and polytetramethylene glycol)
“NOVADURAN 5505S” (trade name) manufactured by Mitsubishi Engineering Plastics was used. The glass transition temperature is 27 ° C.
(2) A2: Homo-type polybutylene terephthalate “NOVADURAN 5007” (trade name) manufactured by Mitsubishi Engineering Plastics was used. The glass transition temperature is 30 ° C.
(3) A3: Homo-type polyethylene terephthalate “NOVAPEX GM700Z” (trade name) manufactured by Mitsubishi Chemical Corporation was used. The weight average molecular weight is 18000. The glass transition temperature is 67 ° C.
(4) A4: Polycarbonate “NOVAREX 7022PJ-LH1” (trade name) manufactured by Mitsubishi Engineering Plastics was used. The weight average molecular weight is 18000.

2. Thermally conductive filler (1) B1; boron nitride “DENCABORON NITRIDE POWDER SGP” (trade name) manufactured by Denki Kagaku Kogyo Co., Ltd. was used. It has a hexagonal structure, an average particle size of 18.0 μm, and an iron oxide content of 0%.
(2) B2: Zinc oxide “ZINC OXIDE No. 2” (trade name) manufactured by Sakai Chemical Industry Co., Ltd. was used. The average particle size is 3 μm (laser diffraction method) and the amount of iron oxide is 0.0007%.
(3) B3: Graphite particles “HF-150A” (trade name) manufactured by Chuetsu Graphite Industries Co., Ltd. was used. The shape is scaly, the aspect ratio is 16, and the weight average particle diameter is 161 μm (electron microscopy).

3. Ultraviolet absorber (1) C1; 2- (2′-hydroxy-5′-methylphenyl) benzotriazole “TINUVIN P” (trade name) manufactured by Ciba Specialty Chemicals was used.
(2) C2; 2,2′-methylenebis [4- (1,1,3,3-tetramethylbutyl) -6- (2H-benzotriazol-2-yl) phenol]
“ADEKA STAB LA-31” (trade name) manufactured by Adeka Company was used.

4). Light stabilizer (1) D1; bis (2,2,6,6-tetramethyl-4-piperidyl) sebacate “Adekastab LA-77” (trade name) manufactured by Adeka Company was used.
(2) D2; Poly [[6- (1,1,3,3-tetramethylbutyl) imino-1,3,5-triazine-2,4-diyl] [(2,2,6,6-tetra Methyl-4-piperidyl) imino] hexamethylene [[(2,2,6,6-tetramethyl-4-piperidyl) imino]]
“CHIMASSORB 944LD” (trade name) manufactured by Ciba Specialty Chemicals was used.

5. Inorganic white pigment (E1)
Titanium oxide (trade name “Taipeke PF691”, manufactured by Ishihara Sangyo Co., Ltd.) was used.

6). Flame retardant (F1)
A halogen-based flame retardant (trade name “Epicoat 5203”, manufactured by Tohto Kasei Co., Ltd.) was used.

7). Colorant (G1)
A blue pigment (trade name “Diaresin Blue G”, manufactured by Mitsubishi Chemical Corporation) was used.

8). Production and Evaluation of Heat Dissipating Resin Composition Examples 1 to 13 and Comparative Examples 1 to 5
(1) Manufacturing method of heat-dissipating resin composition A thermoplastic resin, a thermally conductive filler, and the like are put into a mixer at a ratio shown in Tables 1 to 3 and mixed for 5 minutes, and then an extruder (“BT- 40-S2-30-L type "(manufactured by Plastics Engineering Laboratory), using a weakly kneaded screw, melt kneading and extrusion at a screw rotation speed of 100 rpm and a cylinder temperature of 260 ° C, and pellets (heat dissipating resin composition) Obtained.

(2) Evaluation method Using the pellets obtained above, tests on the following evaluation items were performed. The results are shown in Tables 1 to 3.
[1] Thermal emissivity Using a pellet made of a heat-dissipating resin composition, a test piece having a size of 150 × 150 × 3 mm was prepared by injection molding (mold temperature: 50 to 80 ° C.), and a thermo spot sensor (“ Using “TSS-5X type” (manufactured by Japan Sensor Co., Ltd.), the measurement was performed at an ambient temperature of 25 ° C. by a reflection energy measurement method using infrared detection.

[2] Thermal conductivity (unit: W / (m · K))
The pellet made of the heat-dissipating resin composition was used, and the melt was injected from below the mold (mold temperature: 50 to 80 ° C.) having a cavity space having a diameter of 10 mm and a length of 50 mm. A cylindrical body having a thickness of 50 mm was produced. Then, it cut out so that it might become a disk with a thickness of 1.5 mm in the substantially central part, and this was made into the test piece (diameter 10mm and thickness 1.5mm). In order to measure the thermal conductivity with respect to the flow direction of the heat-dissipating resin composition, a probe is applied to each of the upper and lower surfaces of the test piece, and a laser flash method thermal constant measuring device (“TR-7000R type”). , Manufactured by ULVAC-RIKO) and measured at 25 ° C.

[3] Thermal deformation temperature (unit: ° C)
Using pellets made of a heat-dissipating resin composition, a test piece having a predetermined shape and size was produced by injection molding (mold temperature: 50 to 80 ° C.), and the load was 1.80 MPa according to ISO75. It was measured.

[4] Bending strain (unit:%)
Using pellets made of a heat-dissipating resin composition, a test piece having a size of 150 × 150 × 3 mm was prepared by injection molding (mold temperature: 50 to 80 ° C.), and a precision universal testing machine (“ Using “Autograph AG-10KNI type” (manufactured by Shimadzu Corporation), the measurement was performed by a three-point bending strength measurement method. The measurement conditions are a test piece span interval of 64 mm and a bending speed of 1 mm / min.

[5] Charpy impact strength (unit: kJ / m ² )
Notched data was measured according to ISO179.

[6] Surface resistivity (unit: Ω)
Using a pellet made of a heat-dissipating resin composition, a circular test piece having a diameter of 200 mm and a thickness of 2 mm was prepared by injection molding (mold temperature: 50 to 80 ° C.), and a high resistance meter (“4339B type”) , Agilent Technologies).

[7] Whiteness (unit:%)
About the same test piece as said [2], Lab (L; brightness, a; redness, b: yellowness) was measured for the whiteness before and after a light resistance test with the Hunter-type measurement color difference meter, and it computed with following Formula.
W = 100−√ {(100−L) ² + a ² + b ² }
The light resistance test was performed continuously for 1000 hours under the conditions of no rain and a temperature of 63 ° C. using a weather light tester “Sunshine Weather Meter” (manufactured by Suga Test Instruments Co., Ltd.).

[8] Light reflectance (unit:%)
For the same test piece as in [2] above, the reflectivity for ultraviolet light (wavelength 550 nm) before and after the light resistance test under the same conditions as in [7] above was measured using an ultraviolet-visible near-infrared spectrophotometer ("V-670 type", JASCO). Measured by an incident angle of 60 degrees.

[9] MFR (unit: g / 10 minutes)
The MFR of the heat-dissipating resin composition was measured according to ISO 1133 under the conditions of a temperature of 250 ° C. and a load of 2 kg.

From Tables 1 to 3, Example 1 is an example using only copolymer type polybutylene terephthalate as a thermoplastic resin, Comparative Example 1 using only homo type polybutylene terephthalate, and only homo type polyethylene terephthalate. As compared with Comparative Example 2 used and Comparative Example 3 using polycarbonate, it is understood that the bending strain and the Charpy impact strength are excellent.
Examples 6 to 11 are examples containing an ultraviolet absorber and a light stabilizer, and are particularly excellent in whiteness and light reflectance after the light resistance test. Example 7 is an example containing a colorant and was excellent in toning properties.

  The heat-dissipating resin composition of the present invention is excellent in heat-dissipation property, heat-resistant deformation property, toning property, glossiness, impact resistance, and bending strain properties. OA equipment such as electronic dictionaries; beauty equipment such as dryers; (digital) cameras, (digital) video cameras, projectors, liquid crystal televisions, plasma televisions and other image display / recording equipment; acoustic equipment; indoor lighting equipment; Suitable for game machines; in-vehicle electronic devices such as lamps, car stereos, car navigations, etc .; various power supply devices; drive devices such as stepping motors; housings for toys such as home game machines; In particular, since it is excellent in toning properties and glossiness, it is suitable for the above-mentioned casing, and also suitable for heat-radiating parts that require high thermal conductivity.

Claims (11)

  It contains a thermoplastic resin containing at least 20% by mass of copolymerized polybutylene terephthalate, and a thermally conductive filler, has a thermal conductivity of 2.0 W / (m · K) or more, and a thermal emissivity of 0.7. It is above, and the heat dissipation resin composition characterized by whiteness being 30% or more.   The copolymer polybutylene terephthalate is a polymer obtained by polycondensation of a dicarboxylic acid component comprising a dicarboxylic acid containing terephthalic acid and / or a derivative thereof and a dihydroxy component containing 1,4-butanediol. The heat-radiating resin composition according to claim 1.   When the thermoplastic resin is composed of the copolymerized polybutylene terephthalate and the homopolybutylene terephthalate, and the total of both is 100% by mass, the content of both is 20 to 95% by mass and 5% to 5%, respectively. The heat-radiating resin composition according to claim 1 or 2, wherein the heat-radiating resin composition is 80% by mass.   The heat dissipation according to any one of claims 1 to 3, wherein the content ratio of the thermally conductive filler is 20 to 90 mass% when the total of the thermoplastic resin and the thermally conductive filler is 100 mass%. Resin composition.   The heat-dissipating resin composition according to any one of claims 1 to 4, wherein the thermally conductive filler is scaly.   The heat-dissipating resin composition according to any one of claims 1 to 5, wherein the thermally conductive filler is boron nitride.   Furthermore, the heat-radiating resin composition according to any one of claims 1 to 6, further comprising a flame retardant.   The heat dissipation according to any one of claims 1 to 7, further comprising a colorant, wherein the content of the colorant is 0.05 to 30 parts by mass when the thermoplastic resin is 100 parts by mass. Resin composition.   Furthermore, it contains an ultraviolet absorber and a light stabilizer, and the content ratio of the ultraviolet absorber and the light stabilizer is 5 to 95% by mass and 5 to 95%, respectively, when the total of these is 100% by mass. The heat-dissipating resin composition according to claim 1, wherein the heat-dissipating resin composition is mass%.   The heat radiation resin composition according to any one of claims 1 to 9, wherein the light reflectance is 20% or more.   A molded article comprising the heat-dissipating resin composition according to any one of claims 1 to 10.