WO2019004022A1 - 熱可塑性ポリエステル樹脂組成物およびその成形品 - Google Patents
熱可塑性ポリエステル樹脂組成物およびその成形品 Download PDFInfo
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- WO2019004022A1 WO2019004022A1 PCT/JP2018/023459 JP2018023459W WO2019004022A1 WO 2019004022 A1 WO2019004022 A1 WO 2019004022A1 JP 2018023459 W JP2018023459 W JP 2018023459W WO 2019004022 A1 WO2019004022 A1 WO 2019004022A1
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- polyester resin
- thermoplastic polyester
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- LOAWHQCNQSFKDK-UHFFFAOYSA-N triethyltin Chemical compound CC[Sn](CC)CC.CC[Sn](CC)CC LOAWHQCNQSFKDK-UHFFFAOYSA-N 0.000 description 1
- OLBXOAKEHMWSOV-UHFFFAOYSA-N triethyltin;hydrate Chemical compound O.CC[Sn](CC)CC OLBXOAKEHMWSOV-UHFFFAOYSA-N 0.000 description 1
- QLAGHGSFXJZWKY-UHFFFAOYSA-N triphenylborane;triphenylphosphane Chemical compound C1=CC=CC=C1B(C=1C=CC=CC=1)C1=CC=CC=C1.C1=CC=CC=C1P(C=1C=CC=CC=1)C1=CC=CC=C1 QLAGHGSFXJZWKY-UHFFFAOYSA-N 0.000 description 1
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- JIKOHGNZNKFYHF-UHFFFAOYSA-N tris(2-tert-butyl-4-phenylphenyl) phosphite Chemical compound CC(C)(C)C1=CC(C=2C=CC=CC=2)=CC=C1OP(OC=1C(=CC(=CC=1)C=1C=CC=CC=1)C(C)(C)C)OC(C(=C1)C(C)(C)C)=CC=C1C1=CC=CC=C1 JIKOHGNZNKFYHF-UHFFFAOYSA-N 0.000 description 1
- SZPHBONKPMLMCA-UHFFFAOYSA-N tris(2-tert-butylphenyl) phosphite Chemical compound CC(C)(C)C1=CC=CC=C1OP(OC=1C(=CC=CC=1)C(C)(C)C)OC1=CC=CC=C1C(C)(C)C SZPHBONKPMLMCA-UHFFFAOYSA-N 0.000 description 1
- WXAZIUYTQHYBFW-UHFFFAOYSA-N tris(4-methylphenyl)phosphane Chemical compound C1=CC(C)=CC=C1P(C=1C=CC(C)=CC=1)C1=CC=C(C)C=C1 WXAZIUYTQHYBFW-UHFFFAOYSA-N 0.000 description 1
- QEDNBHNWMHJNAB-UHFFFAOYSA-N tris(8-methylnonyl) phosphite Chemical compound CC(C)CCCCCCCOP(OCCCCCCCC(C)C)OCCCCCCCC(C)C QEDNBHNWMHJNAB-UHFFFAOYSA-N 0.000 description 1
- ZMPODEGAECKFEA-UHFFFAOYSA-N tris[2,4-bis(2-methylbutan-2-yl)phenyl] phosphite Chemical compound CCC(C)(C)C1=CC(C(C)(C)CC)=CC=C1OP(OC=1C(=CC(=CC=1)C(C)(C)CC)C(C)(C)CC)OC1=CC=C(C(C)(C)CC)C=C1C(C)(C)CC ZMPODEGAECKFEA-UHFFFAOYSA-N 0.000 description 1
- LDZXOZYBYWMGIT-UHFFFAOYSA-N tris[2-(2-methylbutan-2-yl)phenyl] phosphite Chemical compound CCC(C)(C)C1=CC=CC=C1OP(OC=1C(=CC=CC=1)C(C)(C)CC)OC1=CC=CC=C1C(C)(C)CC LDZXOZYBYWMGIT-UHFFFAOYSA-N 0.000 description 1
- 229940124543 ultraviolet light absorber Drugs 0.000 description 1
- 239000006097 ultraviolet radiation absorber Substances 0.000 description 1
- 235000021122 unsaturated fatty acids Nutrition 0.000 description 1
- 239000010455 vermiculite Substances 0.000 description 1
- 229910052902 vermiculite Inorganic materials 0.000 description 1
- 235000019354 vermiculite Nutrition 0.000 description 1
- 239000013585 weight reducing agent Substances 0.000 description 1
- 239000010456 wollastonite Substances 0.000 description 1
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- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
- 229910000166 zirconium phosphate Inorganic materials 0.000 description 1
- LEHFSLREWWMLPU-UHFFFAOYSA-B zirconium(4+);tetraphosphate Chemical compound [Zr+4].[Zr+4].[Zr+4].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O LEHFSLREWWMLPU-UHFFFAOYSA-B 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G63/00—Macromolecular compounds obtained by reactions forming a carboxylic ester link in the main chain of the macromolecule
- C08G63/02—Polyesters derived from hydroxycarboxylic acids or from polycarboxylic acids and polyhydroxy compounds
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Definitions
- the present invention relates to a thermoplastic polyester resin composition and a molded article obtained by molding the same.
- thermoplastic polyester resins are used in a wide range of fields such as mechanical and mechanical parts, electric / electronic parts and automobile parts, by taking advantage of various properties such as excellent injection moldability and mechanical properties.
- thermoplastic polyester resins are likely to lose mechanical strength due to thermal oxidative degradation at high temperatures, so they are generally used for industrial materials such as mechanical and mechanical parts, electric / electronic parts and automobile parts.
- it is also required to have long-term heat aging resistance at high temperature.
- thermoplastic polyester resins are easily degraded by hydrolysis, long-term hydrolysis resistance is required to be used for the above applications.
- thermoplastic polyester resin for example, a thermoplastic resin composition in which a compound having an isocyanate and / or a carbodiimide is added to a polybutylene terephthalate resin (see, for example, Patent Document 1)
- a thermoplastic resin composition in which a polyhydric alcohol, a reinforcing agent and a polymer reinforcing agent are added to a thermoplastic resin selected from the group consisting of polyamides, polyesters and mixtures thereof see, for example, Patent Document 2 ing.
- thermoplastic resin compositions in which a hydroxyl group-containing resin and / or an epoxy compound are added to a polyester resin are proposed.
- Patent Documents 1 and 2 have insufficient heat aging resistance and mechanical properties.
- Patent Documents 3 to 7 improve thermal properties and mechanical strength by containing a hydroxyl group-containing resin, but are sufficient to meet the recent demand for materials I could not say that.
- thermoplastic resin composition and a molded product which can be used, and further, a thermoplastic resin composition and a molded product capable of suppressing bleeding out on the surface of the molded product during dry and wet heat treatment.
- thermoplastic polyester resin composition which satisfy
- thermoplastic polyester resin (A) epoxy compound (B) having an epoxy equivalent of 200 to 3,000 g / eq, and number average molecular weight of 2,000 to 500,000 and halogen element content of 1,000 ppm or less
- a thermoplastic polyester resin composition comprising a certain hydroxy group-containing resin (C), comprising 70 to 99.9 parts by weight of the thermoplastic polyester resin (A) and 0.1 to 30 hydroxy group-containing resin (C)
- a thermoplastic polyester resin composition comprising 0.05 to 10 parts by weight of an epoxy compound (B) with respect to a total of 100 parts by weight of parts by weight.
- the present invention is compatible with long-term hydrolysis resistance and heat aging resistance at a high level, and can suppress bleed-out to the surface of a molded article even during dry and wet heat treatment.
- a plastic resin composition and a molded article can be obtained.
- thermoplastic polyester resin composition of the present invention will be described in detail.
- thermoplastic polyester resin composition of the present invention is a thermoplastic polyester resin (A), an epoxy compound having an epoxy equivalent of 200 to 3,000 g / eq.
- a thermoplastic polyester resin composition comprising (B) and a hydroxy group-containing resin (C) having a number average molecular weight of 2,000 to 500,000 and a halogen element content of 1,000 ppm or less, which is thermoplastic 0.05 to 10 parts by weight of epoxy compound (B) is compounded with respect to 100 parts by weight in total of 70 to 99.9 parts by weight of polyester resin (A) and 0.1 to 30 parts by weight of hydroxy group-containing resin (C) Thermoplastic polyester resin composition.
- thermoplastic polyester resin composition of the present invention contains a reaction product in which the (A) component, the (B) component and the (C) component react, but the reaction product is a product produced by a complicated reaction.
- the present invention specifies the invention by the components to be blended.
- the thermoplastic polyester resin (A) is (1) a residue of a dicarboxylic acid or an ester-forming derivative thereof and a residue of a diol or an ester-forming derivative thereof, (2) a residue of a hydroxycarboxylic acid or an ester-forming derivative thereof And (3) a polymer or copolymer having as a main structural unit at least one residue selected from the group consisting of residues of lactones.
- "as a main structural unit” refers to having at least 50% by mole of at least one residue selected from the group consisting of (1) to (3) in all structural units, and those residues It is preferable to have 80 mol% or more.
- a polymer or copolymer having a residue of a dicarboxylic acid or an ester-forming derivative thereof and a residue of a diol or an ester-forming derivative thereof as a main structural unit is excellent in mechanical properties and heat resistance It is preferable in point.
- thermoplastic polyester (A) preferably has a melting point higher than 200 ° C.
- the melting point is higher than 200 ° C.
- dicarboxylic acids or ester-forming derivatives thereof include terephthalic acid, isophthalic acid, phthalic acid, 2,6-naphthalenedicarboxylic acid, 1,5-naphthalenedicarboxylic acid, bis (p-carboxyphenyl) methane, anthracene
- Aromatic dicarboxylic acids such as dicarboxylic acids, 4,4'-diphenylether dicarboxylic acid, 5-tetrabutylphosphonium isophthalic acid, 5-sodium sulfoisophthalic acid; oxalic acid, succinic acid, adipic acid, sebacic acid, azelaic acid, dodecanedione
- Aliphatic dicarboxylic acids such as acid, malonic acid, glutaric acid and dimer acid
- alicyclic dicarboxylic acids such as 1,3-cyclohexanedicarboxylic acid and 1,4-cyclohexanedicarboxylic
- diol or its ester-forming derivative for example, ethylene glycol, propylene glycol, 1,4-butanediol, neopentyl glycol, 1,5-pentanediol, 1,6-hexanediol, decamethylene glycol And aliphatic or alicyclic glycols having 2 to 20 carbon atoms such as cyclohexanedimethanol, cyclohexanediol and dimerdiol; molecular weights of 200 to 100,000 such as polyethylene glycol, poly-1,3-propylene glycol and polytetramethylene glycol Long-chain glycols; aromatic dioxy compounds such as 4,4'-dihydroxybiphenyl, hydroquinone, t-butyl hydroquinone, bisphenol A, bisphenol S, bisphenol F; Such as ester forming derivatives thereof. Two or more of these may be used.
- a polymer or copolymer which makes a dicarboxylic acid or its ester formation derivative and diol or its ester formation derivative a structural unit For example, a polyethylene terephthalate, a polypropylene terephthalate, a polybutylene terephthalate, a polypropylene isophthalate, a polybutylene isophthalate , Polybutylene naphthalate, polypropylene isophthalate / terephthalate, polybutylene isophthalate / terephthalate, polypropylene terephthalate / naphthalate, polybutylene terephthalate / naphthalate, polybutylene terephthalate / decanedicarboxylate, polypropylene terephthalate / 5-sodium sulfoisophthalate, poly Butylene terephthalate / 5-sodium sulfoisophthalate Polypropylene terephthalate
- a polymer having a residue of an aromatic dicarboxylic acid or an ester-forming derivative thereof and a residue of an aliphatic diol or an ester-forming derivative thereof as main structural units Or a copolymer is more preferable, and a residue of a dicarboxylic acid selected from terephthalic acid and naphthalene dicarboxylic acid or an ester-forming derivative thereof, and an aliphatic diol selected from ethylene glycol, propylene glycol and 1,4-butanediol Further preferred is a polymer or copolymer having as its main structural unit the residue of its ester-forming derivative.
- Aromatic polyester resins are particularly preferred, polybutylene terephthalate, polypropylene terephthalate and polybutylene naphthalate are more preferred, and polybutylene terephthalate is more preferred in terms of excellent moldability and crystallinity.
- these 2 or more types can also be used by arbitrary content.
- the ratio of terephthalic acid or an ester-forming derivative thereof to all the dicarboxylic acids constituting the above-mentioned polymer is preferably 30 mol% or more, more preferably 40 mol% or more.
- thermoplastic polyester resin (A) a liquid crystalline polyester resin which can form anisotropy upon melting can also be used.
- a structural unit of liquid crystalline polyester resin an aromatic oxycarbonyl unit, an aromatic dioxy unit, an aromatic and / or aliphatic dicarbonyl unit, an alkylene dioxy unit, an aromatic imino oxy unit etc. are mentioned, for example.
- the carboxyl end group content of the thermoplastic polyester resin (A) is preferably 50 eq / t or less from the viewpoint of flowability, hydrolysis resistance and heat aging resistance. More preferably, it is 40 eq / t or less, still more preferably 30 eq / t or less.
- the carboxy group acts as an acid catalyst under wet heat environment and high temperature dry heat environment, and the hydrolysis resistance and the heat aging resistance decrease.
- the change in molecular weight of the thermoplastic polyester (A) becomes large, and the retention stability is deteriorated.
- the lower limit value of the amount of carboxyl terminal group is 0 eq / t.
- the carboxyl end group amount of the thermoplastic polyester resin (A) is a value measured by dissolving the thermoplastic polyester resin (A) in o-cresol / chloroform solvent and then titration with ethanolic potassium hydroxide. .
- the thermoplastic polyester resin (A) preferably has a weight average molecular weight (Mw) of 8,000 or more from the viewpoint of further improving the mechanical properties. Moreover, when the weight average molecular weight (Mw) is 500,000 or less, it is preferable because the balance between mechanical physical properties and molding processability (melt viscosity) is excellent.
- the weight average molecular weight is more preferably 300,000 or less, still more preferably 250,000 or less.
- Mw of the (A) thermoplastic polyester resin is a value in terms of polymethyl methacrylate (PMMA) measured by gel permeation chromatography (GPC) using hexafluoroisopropanol as a solvent.
- the intrinsic viscosity of the thermoplastic polyester resin (A) is preferably in the range of 0.36 to 1.60 dl / g when measured at 25 ° C. in o-chlorophenol solution from the viewpoint of moldability, More preferably, it is in the range of 0.50 to 1.50 dl / g.
- the blending amount of the thermoplastic polyester resin (A) is 70 to 99. to 100 parts by weight in total of the thermoplastic polyester resin (A) and the hydroxy group-containing resin (C). 9 parts by weight. In this range, it is possible to simultaneously achieve high heat aging resistance and hydrolysis resistance. If the compounding amount exceeds 99.9 parts by weight, the heat aging resistance improvement effect is not sufficient.
- the compounding amount is more preferably 99.8 parts by weight or less, still more preferably 99.5 parts by weight or less, and particularly preferably 99 parts by weight or less. On the other hand, if the compounding amount is less than 70 parts by weight, hydrolysis resistance and mechanical properties tend to deteriorate, which is not preferable.
- the compounding amount is more preferably 80 parts by weight or more, still more preferably 90 parts by weight or more.
- thermoplastic polyester resin (A) can be produced by a known polycondensation method or ring-opening polymerization method.
- the production method may be either batch polymerization or continuous polymerization, and any of transesterification reaction and direct polymerization reaction can be applied. From the viewpoint of productivity, continuous polymerization is preferable, and direct polymerization is preferably used.
- thermoplastic polyester resin (A) is a polymer or copolymer obtained by a condensation reaction containing dicarboxylic acid or its ester-forming derivative and diol or its ester-forming derivative as main components, dicarboxylic acid Alternatively, it can be produced by subjecting an ester-forming derivative thereof and a diol or an ester-forming derivative thereof to an esterification reaction or a transesterification reaction and then a polycondensation reaction.
- the polymerization reaction catalyst include methyl ester, tetra-n-propyl ester, tetra-n-butyl ester, tetraisopropyl ester, tetraisobutyl ester, tetra-tert-butyl ester, cyclohexyl ester, phenyl ester of titanic acid Organotitanium compounds such as benzyl ester, tolyl ester or mixed esters thereof; dibutyltin oxide, methylphenyltin oxide, tetraethyltin, hexaethylditin oxide, cyclohexyhexylditin oxide, didodecyltin oxide, triethyltin hydroxide, Triphenyl tin hydrox
- organic titanium compounds and tin compounds are preferable, and tetra-n-butyl ester of titanic acid is more preferably used.
- the addition amount of the polymerization reaction catalyst is preferably in the range of 0.01 to 0.2 parts by weight with respect to 100 parts by weight of the thermoplastic polyester resin.
- thermoplastic polyester resin composition of the present invention is formed by blending an epoxy compound (B) and a hydroxy group-containing resin (C) with a thermoplastic polyester resin (A).
- the thermoplastic polyester resin (A) is decomposed by thermal oxidative degradation to cause decomposition of the main chain, resulting in a decrease in molecular weight and an increase in the amount of carboxy terminal groups.
- the mechanical properties of the molded article made of the thermoplastic polyester resin composition decrease.
- the thermoplastic polyester resin (A) is hydrolyzed to cleave ester bonds in the main chain to form a carboxy terminal group and a hydroxy terminal group.
- the carboxy terminal group generated by this hydrolysis is a factor to further accelerate the cleavage of the ester bond, and as a result of accelerating the cleavage of the main chain, the molecular weight decreases, and the mechanical properties of the molded article made of the thermoplastic polyester resin composition Decreases.
- thermoplastic polyester resin (A) By blending the epoxy compound (B) and the hydroxy group-containing resin (C) with the thermoplastic polyester resin (A), the above-mentioned decomposition reaction is suppressed, and the hydrolysis resistance and heat aging resistance of the thermoplastic polyester resin composition Can be improved.
- the epoxy compound (B) has an epoxy equivalent of 200 to 3,000 g / eq.
- the epoxy equivalent (g / eq) of the epoxy compound (B) is a value obtained by dividing the molecular weight per mole of the epoxy compound by the number of epoxy groups per molecule of the epoxy compound.
- the epoxy equivalent is obtained by adding acetic acid and triethylammonium bromide / acetic acid solution to a solution in which epoxy compound (B) is dissolved in chloroform according to JIS K 7236: 2001, and performing potentiometric titration with 0.1 mol / L acetic acid perchloric acid. It can be measured.
- the epoxy equivalent is preferably 200 to 2,000 g / eq, more preferably 200 to 1,500 g / eq, and still more preferably 200 to 1,000 g / eq.
- the epoxy compound (B) preferably contains an epoxy compound having two or more epoxy groups in one molecule.
- epoxy compounds having two or more epoxy groups in one molecule include bisphenol A, resorcinol, hydroquinone, pyrocatechol, bisphenol F, saligenin, bisphenol S, 4,4'-dihydroxybiphenyl, 1,5-dihydroxynaphthalene 1,4-Dihydroanthracene-9,10-diol, 6-hydroxy-2-naphthoic acid, 1,1-methylenebis-2,7-dihydroxynaphthalene, 1,1,2,2-tetrakis-4-hydroxyphenyl
- Glycidyl ether epoxy compounds which are polycondensates of epichlorohydrin with phenol compounds such as ethane and cashew phenol;
- Glycidyl ester epoxy compounds such as glycidyl phthalate esters; N, N'-methylenebis (N-glycidyl aniline Glycidyl
- liquid or solid can be used.
- a bisphenol epoxy compound or a novolac epoxy compound which is a polycondensate of bisphenol and epichlorohydrin is preferable. By using these, it is possible to obtain a polyester resin composition excellent in the balance between durability and retention stability at high temperature.
- bisphenol-A epoxy resin As a bisphenol-type epoxy compound, bisphenol-A epoxy resin is preferable. Among them, bisphenol A epoxy resin having an epoxy equivalent of 300 to 2,000 g / eq is preferable. When the epoxy equivalent is 300 g / eq or more, the gas generation amount at the time of melt processing can be suppressed.
- the epoxy equivalent is more preferably 500 g / eq or more. When the epoxy equivalent is 2,000 g / eq or less, hydrolysis resistance and high temperature melt retention stability can be compatible at a higher level.
- the epoxy equivalent is more preferably 1,500 g / eq or less, and still more preferably 1,000 g / eq or less.
- novolac epoxy compounds include phenol novolac epoxy compounds, cresol novolac epoxy compounds, naphthol novolac epoxy compounds, bisphenol A novolac epoxy compounds, dicyclopentadiene-phenol-added novolac epoxy compounds, dimethylene Examples thereof include phenylene-phenol-added novolac epoxy compounds and dimethylene biphenylene-phenol-added novolac epoxy compounds.
- the epoxy compound (B) can also contain an epoxy compound having only one epoxy group in one molecule.
- an epoxy compound having only one epoxy group in one molecule.
- a glycidyl ether type compound, a glycidyl ester type compound, an epoxidized fatty acid ester compound, a glycidyl imide compound, an alicyclic epoxy compound etc. are mentioned. Two or more of these may be used in combination.
- Examples of glycidyl ester compounds contained in an epoxy compound having only one epoxy group in one molecule include cyclohexanecarboxylic acid glycidyl ester, stearic acid glycidyl ester, lauric acid glycidyl ester, neodecanoic acid glycidyl ester, palmitic acid glycidyl ester , Versatic acid glycidyl ester, oleic acid glycidyl ester, linoleic acid glycidyl ester, linolenic acid glycidyl ester, acrylic acid glycidyl ester, methacrylic acid glycidyl ester, benzoic acid glycidyl ester, 4-t-butylbenzoic acid glycidyl ester, p-toluoyl Acid glycidyl ester is exemplified.
- examples of glycidyl ether compounds include monohydric alcohols having only one hydroxyl group and glycidyl ethers of phenols.
- examples of glycidyl ethers of monohydric alcohols include butyl glycidyl ether, 2-ethylhexyl glycidyl ether, stearyl glycidyl ether, allyl glycidyl ether, benzyl glycidyl ether, ethylene oxide lauryl alcohol glycidyl ether and the like.
- glycidyl ethers of monohydric phenols include phenyl glycidyl ether, p-t-butylphenyl glycidyl ether, p-sec-butylphenyl glycidyl ether, ethylene oxide phenol glycidyl ether, o-methylphenyl glycidyl ether and the like . Two or more of these may be used.
- epoxidized fatty acid ester compound the compound which epoxidized the unsaturated bond of unsaturated fatty acid ester, such as soybean oil and linseed oil, is mentioned, Specifically, epoxidized fatty acid octyl ester, epoxidized soybean oil, epoxidation Flaxseed oil etc. can be illustrated.
- glycidyl imide compounds include N-glycidyl phthalimide, N-glycidyl-4-methyl phthalimide, N-glycidyl-4,5-dimethyl phthalimide, N-glycidyl-3-methyl phthalimide, N-glycidyl-3,6 -Dimethylphthalimide, N-glycidyl-4-ethoxyphthalimide, N-glycidyl-4-chlorophthalimide, N-glycidyl-4,5-dichlorophthalimide, N-glycidyl-3,4,5,6-tetrabromophthalimide, N-glycidyl-4-n-butyl-5-bromophthalimide, N-glycidylsuccinimide, N-glycidyl hexahydrophthalimide, N-glycidyl-1,2,3,6-tetrahydrophthalimide, N-glycidyl maleimide, N -G
- alicyclic epoxy compounds include 3,4-epoxycyclohexylmethyl-3,4-epoxycyclohexylcarboxylate, bis (3,4-epoxycyclohexylmethyl) adipate, vinylcyclohexene diepoxide, N-methyl-4 , 5-Epoxycyclohexane-1,2-dicarboximide, N-ethyl-4,5-epoxycyclohexane-1,2-dicarboximide, N-phenyl-4,5-epoxycyclohexane-1,2-dicarboxylic acid Imide, N-naphthyl-4,5-epoxycyclohexane-1,2-dicarboximide, N-tolyl-3-methyl-4,5-epoxycyclohexane-1,2-dicarboximide and the like can be mentioned.
- an epoxy compound (B) a glycidyl ether type compound, a glycidyl ester type compound, a novolac type epoxy compound, an epoxidized fatty acid ester compound, a glycidyl imide compound from a viewpoint which can suppress reaction of epoxies and can control a deterioration of retention stability.
- glycidyl ether compounds, glycidyl ester compounds, novolac epoxy compounds, and glycidyl imide compounds are more preferable, and since the heat aging resistance and hydrolysis resistance can be further improved, glycidyl ether compounds, novolac epoxy compounds, and glycidyl are preferable.
- Imide compounds are particularly preferred.
- the compounding amount of the epoxy compound (B) is 0.05 to 10 parts by weight to 100 parts by weight in total of the thermoplastic polyester resin (A) and the hydroxy group-containing resin (C). It is a department.
- the compounding quantity of an epoxy compound (B) component is less than 0.05 weight part, hydrolysis resistance falls. More preferably, it is 0.1 parts by weight or more, still more preferably 0.3 parts by weight or more.
- the compounding quantity of an epoxy compound (B) component exceeds 10 weight part, heat resistance and retention stability will deteriorate. More preferably, it is 8 parts by weight or less, still more preferably 5 parts by weight or less.
- the thermoplastic polyester resin composition of the present invention comprises a thermoplastic polyester resin (A) and a hydroxy group-containing resin (C) having a number average molecular weight of 2,000 to 500,000 and a halogen element content of 1,000 ppm or less. It mixes (it may describe as "hydroxy group-containing resin (C)" hereafter). By blending a hydroxy group-containing resin (C) having a halogen element content of 1,000 ppm or less with the thermoplastic polyester resin (A), the heat aging resistance against long-term exposure in a dry heat environment can be obtained. It can be improved.
- the content of the halogen element contained in the hydroxy group-containing resin (C) is greater than 1,000 ppm, the dispersibility in the thermoplastic polyester resin tends to decrease during melt processing, and as a result, the thermoplastic polyester resin composition The mechanical strength and heat aging resistance of the resulting molded article are reduced.
- a gas derived from a halogen element may be generated at the time of melt processing or at the time of using a molded product, which causes deterioration of moldability and mold deposit.
- the halogen content in the hydroxy group-containing resin (C) is preferably 800 ppm or less, more preferably 500 ppm, still more preferably 300 ppm or less, and most preferably 0 ppm.
- said halogen element content shows the sum total of the quantity of the halogen element contained in hydroxyl group containing resin (C). That is, the total amount of the halogen element contained as a constituent element in the molecule of the hydroxy group-containing resin (C) and the halogen element in the inorganic halogen compound contained in the hydroxy group-containing resin (C) is shown.
- the method of quantifying the content of the halogen element can be carried out by an analysis method in accordance with IEC62321-3-2. That is, combustion is performed at 1,000 ° C.
- the generated halogen gas is absorbed by the alkaline adsorption solution, and the absorption solution is analyzed by ion chromatography, and the halogen element content Can be quantified.
- the hydroxy group-containing resin (C) is a resin having a number average molecular weight of 2,000 to 500,000 and having hydroxy groups in the molecule.
- the number average molecular weight of the hydroxy group-containing resin (C) is a value in terms of polystyrene measured by gel permeation chromatography (GPC) using tetrahydrofuran as a solvent.
- the number average molecular weight of the hydroxy group-containing resin (C) is smaller than 2,000, the molecular weight tends to decrease due to the progress of transesterification with the thermoplastic polyester resin (A) when exposed to a dry heat environment, and heat aging resistance It is inferior to. If the number average molecular weight exceeds 500,000, the retention stability at the time of melting tends to deteriorate, which is not preferable. It is preferably 3,000 to 200,000, more preferably 4,000 to 100,000, and still more preferably 5,000 to 50,000.
- the hydroxy group value of the hydroxy group-containing resin (C) is preferably 3 to 20 eq / kg.
- the hydroxy group value (eq / kg) of the hydroxy group-containing resin (C) is acetylated with an acetylating reagent of the hydroxy group of the hydroxy group-containing resin (C) according to JIS K 0070 and JIS K 155-1 to give an indicator It is a value measured by adding a phenolphthalein solution and titrating with a potassium hydroxide ethanol solution.
- the thermoplastic polyester resin composition containing a hydroxy group-containing resin (C) having a hydroxy group value in the above range can exhibit excellent heat aging resistance and retention stability at the time of melting.
- the reaction with the carboxy group terminal of the thermoplastic polyester resin (A) can be promoted to improve the heat aging resistance.
- the hydroxyl value By setting the hydroxyl value to 20 eq / kg or less, retention stability at the time of melting can be maintained.
- the hydroxyl value is preferably 3 to 17 eq / kg, more preferably 3 to 15 eq / kg.
- hydroxy group-containing resin (C) polyhydroxy polyethers such as phenoxy resin, acrylic resin containing hydroxyalkyl (meth) acrylate as a structural unit, EVOH resin which is ethylene-vinyl alcohol copolymer, paravinyl phenol resin , Carbinol modified or diol modified silicone oil, polycarbonate diol and the like.
- an acrylic resin containing a phenoxy resin and / or a hydroxyalkyl (meth) acrylate as a structural unit is preferable from the viewpoint of the heat resistance of the hydroxy group-containing resin itself and the dispersibility in the thermoplastic polyester resin (A).
- compatibility and dispersibility with the thermoplastic polyester resin are improved.
- polyhydroxy polyethers include hydroquinone, resorcine, 2,2'-biphenol, 4,4-biphenol, 4,4'-dihydroxybiphenyl, 4,4'-dihydroxydiphenyl ether, bis (hydroxyaryl) ) Aromatic dihydroxys such as alkanes, bis (hydroxyaryl) cycloalkanes, 4,4'-dihydroxydiphenylsulfone, 4,4'-dihydroxydiphenyl sulfide, 4,4'-dihydroxydiphenyl ketone, and 2,6-dihydroxynaphthalene
- the phenoxy resin obtained by condensing a compound and epichlorohydrin can be illustrated.
- bis (hydroxyaryl) alkanes bis (4-hydroxyphenyl) methane: bisphenol F, 2,2-bis (4-hydroxyphenylpropane): bisphenol A, 1,1-bis (4-hydroxyphenylethane): Bisphenol AD, 2,2-bis (4-hydroxyphenyl) butane and the like can be exemplified.
- Examples of bis (hydroxyaryl) cycloalkanes include 1,1-bis (hydroxyphenyl) pentane, 1,1-bis (4-hydroxyphenyl) hexane, 1,1-bis (hydroxyphenyl) heptane and the like. These phenoxy resins can be used alone or in combination of two or more.
- hydroxyalkyl (meth) acrylate As the hydroxyalkyl (meth) acrylate, 2-hydroxyethyl (meth) acrylate, 3-hydroxypropyl (meth) acrylate, 4-hydroxybutyl (meth) acrylate 5-hydroxypentyl (meth) acrylate, 6-hydroxyhexyl (meth) acrylate, hydroxyoctyl (meth) acrylate, cyclohexane dimethanol mono (meth) acrylate and the like.
- alkyl or aryl esters such as acrylic acid and methacrylic acid other than the above; olefin compounds such as ethylene, propylene, 1-butene and butadiene; vinyl aromatic compounds such as styrene; acrylonitrile Acrylamide, methacrylamide, etc. may be contained.
- hydroxy group-containing acrylic resins can be used alone or in combination of two or more.
- the compounding amount of the hydroxy group-containing resin (C) is 0.1 to 30 parts by weight with respect to 100 parts by weight in total of the thermoplastic polyester resin (A) and the hydroxy group-containing resin (C). In this range, it is possible to simultaneously achieve high heat aging resistance and hydrolysis resistance. If the amount is less than 0.1 parts by weight, the heat aging resistance improvement effect is not sufficient.
- the amount is more preferably 0.2 parts by weight or more, still more preferably 0.5 parts by weight or more, and particularly preferably 1 part by weight or more.
- the compounding amount exceeds 30 parts by weight, hydrolysis resistance and mechanical properties tend to be lowered, which is not preferable. More preferably, it is 20 parts by weight or less, still more preferably 10 parts by weight or less.
- the hydroxy group concentration (eq / kg) of the hydroxy group-containing resin (C) in the thermoplastic polyester resin composition is 3 to 600 eq / kg from the viewpoints of heat aging resistance and improvement of retention stability at melting. preferable.
- the hydroxy group concentration (eq / kg) of the hydroxy group-containing resin (C) in the thermoplastic polyester resin composition means the hydroxy group equivalent derived from the hydroxy group-containing resin (C) in 1 kg of the thermoplastic polyester resin composition (Eq) is shown. This value can be calculated from the blending amount of the hydroxy group-containing compound (C) blended with the thermoplastic polyester resin and the hydroxy group value of the hydroxy group-containing compound (C).
- the hydroxy group concentration of the hydroxy group-containing resin (C) in the thermoplastic polyester resin composition is 3 eq / kg or more, the reaction with the carboxy group terminal of the thermoplastic polyester resin (A) is promoted to achieve heat aging. It is possible to improve the quality.
- the hydroxyl group concentration is more preferably 3 to 400 eq / kg, still more preferably 3 to 200 eq / kg.
- phosphorus compound (D) a phosphorus compound represented by (D) the following general formula (1) into the thermoplastic polyester resin composition of the present invention.
- phosphorus compound (D) By blending the phosphorus compound represented by the general formula (1), the organic peroxide generated by oxidative deterioration in a high temperature environment is reduced by the reducing phosphorus compound (D) to form a decomposition product It is possible to suppress the increase of the carboxyl group and to further improve the heat aging resistance and the hydrolysis resistance.
- R 1 and R 2 are independently hydrogen (except when R 1 and R 2 are both hydrogen), OM (where O is negatively charged oxygen) And M is a positively charged counter ion), an alkyl group having 1 to 20 carbon atoms, an alkylene group having 2 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, and an alkyl having 1 to 20 carbon atoms It is selected from an oxy group, a polyoxyalkylene group consisting of an alkylene of 2 to 4 carbon atoms, and an aryloxy group of 6 to 20 carbon atoms.
- the alkyl group, the alkylene group, the aryl group, the alkyloxy group, the polyoxyalkylene group, and the aryloxy group are an OH group, a halogen, a COOH group, a COOR 3 group (wherein R 3 is an alkyl having 1 to 4 carbon atoms) It may be substituted by a substituent selected from the group) and NH 2 group.
- the substitution number in this case is 1 or 2.
- R 1 and R 2 may be linked.
- phosphorus compound represented by the general formula (1) examples include phosphonate compounds and phosphinate compounds.
- Examples of phosphonate compounds include phosphonic acid, phosphonic acid alkyl ester, phosphonic acid aryl ester, and metal salts thereof. Specifically, dimethyl phosphonate, diethyl phosphonate, diphenyl phosphonate, metal salts of phosphonic acid and the like can be mentioned.
- phosphinate compounds include phosphinic acid, phosphinic acid alkyl esters, phosphinic acid aryl esters, alkylated phosphinic acids, arylated phosphinic acids, alkyl esters or aryl esters thereof, metal salts thereof, and the like.
- phosphinic acid methyl phosphinic acid, ethyl phosphinic acid, propyl phosphinic acid, isopropyl phosphinic acid, butyl phosphinic acid, phenyl phosphinic acid, tolyl phosphinic acid, xylyl phosphinic acid, biphenylyl phosphinic acid, naphthyl phosphinic acid, Anthryl phosphinic acids, their alkyl esters or aryl esters, and their metal salts and the like can be mentioned.
- the oxidative deterioration of the epoxy compound (B) can be suppressed, and the hydrolysis resistance of the molded article and the color tone can be further improved.
- Metal salts of phosphonic acid or metal salts of phosphinic acid are preferred, metal salts of phosphinic acid are more preferred, and sodium salts of phosphinic acid are particularly preferred.
- the compounding amount of the phosphorus compound (D) represented by the general formula (1) is 0.01 to 1 with respect to a total of 100 parts by weight of the thermoplastic polyester resin (A) and the hydroxy group-containing resin (C). Parts by weight are preferred.
- Oxidation resistance deterioration resistance can be improved as the compounding quantity of a phosphorus compound (D) is 0.01 weight part or more.
- the compounding amount is more preferably 0.02 parts by weight or more, still more preferably 0.05 parts by weight or more.
- the compounding amount is more preferably 0.5 parts by weight or less, still more preferably 0.3 parts by weight or less.
- thermoplastic polyester resin composition of the present invention preferably further contains a fiber reinforcement (E).
- a fiber reinforcement (E) By blending the fiber reinforcement (E), mechanical strength and heat resistance can be further improved.
- glass fiber As a fiber reinforcement (E), glass fiber, aramid fiber, carbon fiber, alumina fiber, silicon carbide fiber etc. can be illustrated, Preferably glass fiber can be used. As glass fiber, chopped strand type or roving type glass fiber is preferably used.
- a silane coupling agent such as an aminosilane compound or an epoxysilane compound and / or a copolymer consisting of a urethane, an acrylic acid such as an acrylic acid / styrene copolymer, a methyl acrylate / methyl methacrylate / maleic anhydride copolymer, etc.
- Glass fibers treated with a sizing agent containing a copolymer of maleic anhydride, one or more epoxy compounds such as vinyl acetate, bisphenol A diglycidyl ether and novolak epoxy compounds are also preferably used.
- a glass fiber treated with a convergent agent containing a copolymer of maleic anhydride is more preferable because the hydrolysis resistance can be further improved.
- the silane coupling agent and / or the sizing agent may be used by being mixed with the emulsion liquid.
- the fiber diameter of the fiber reinforcement is preferably in the range of 1 to 30 ⁇ m.
- the lower limit value is preferably 5 ⁇ m from the viewpoint of the dispersibility of the fiber reinforcement in the resin.
- the upper limit is preferably 15 ⁇ m from the viewpoint of mechanical strength.
- the fiber cross section is usually circular, a fiber reinforced material having an arbitrary cross section such as oval glass fiber, flat glass fiber and cocoon-shaped glass fiber of any aspect ratio can also be used, This has the effect of improving the flowability and obtaining a molded article with little warpage.
- the compounding amount of the fiber reinforcing material (E) is 1 to 100 parts by weight with respect to 100 parts by weight in total of the thermoplastic polyester resin (A) and the hydroxy group-containing resin (C).
- the mechanical strength and the heat resistance can be further improved by blending the fiber reinforcing material (E) in an amount of 1 part by weight or more. 20 parts by weight or more is more preferable, and 30 parts by weight or more is more preferable.
- a composition excellent in the balance between mechanical strength and moldability can be obtained. 95 parts by weight or less is more preferable, and 90 parts by weight or less is more preferable.
- a reinforcing material other than the fiber reinforcing material can be blended within the range not impairing the effects of the present invention.
- a reinforcing material other than the fiber reinforcing material it is possible to improve part of the crystallization characteristics, arc resistance, anisotropy, mechanical strength, flame retardancy or heat distortion temperature of the molded article.
- needle-like, granular, powdery and layered inorganic fillers may be mentioned, and specific examples include glass beads, milled fibers, glass flakes, potassium titanate whiskers, calcium sulfate whiskers, Wollastonite, silica, kaolin, talc, calcium carbonate, zinc oxide, magnesium oxide, aluminum oxide, a mixture of magnesium oxide and aluminum oxide, finely powdered silica, aluminum silicate, silicon oxide, smectite clay mineral (montmorillonite, hectorite) And vermiculite, mica, fluoroteniolite, zirconium phosphate, titanium phosphate, and dolomite. Two or more of these may be blended.
- the average particle diameter of the granular, powdery and layered inorganic fillers is preferably 0.1 to 20 ⁇ m in terms of impact strength.
- the average particle diameter is particularly preferably 0.2 ⁇ m or more from the viewpoint of the dispersibility of the inorganic filler in the resin, and preferably 10 ⁇ m or less from the viewpoint of mechanical strength.
- the blending amount of the inorganic filler other than the fiber reinforcing material is a thermoplastic polyester resin (A) and the blending amount of the fiber reinforcing material from the viewpoint of flowability at the time of molding and durability of the molding machine and mold. 100 parts by weight or less is preferable with respect to a total of 100 parts by weight of the hydroxyl group-containing resin (C).
- the amount of the inorganic filler other than the fiber reinforcing material is preferably 1 to 50 parts by weight with respect to 100 parts by weight in total of the thermoplastic polyester resin (A) and the hydroxy group-containing resin (C).
- the compounding quantity of inorganic fillers other than a fiber reinforcement is 1 weight part or more, anisotropy can be reduced and residence stability can be improved more.
- the blending amount is more preferably 2 parts by weight or more, further preferably 3 parts by weight or more.
- the compounding quantity of inorganic fillers other than a fiber reinforcement is 50 weight part or less, mechanical strength can be improved.
- thermoplastic polyester resin composition of the present invention further contains a reaction accelerator, a phosphorus-based stabilizer, an ultraviolet light absorber, a light stabilizer, a mold release agent, a plasticizer and an antistatic agent, as long as the object of the present invention is not impaired.
- a reaction accelerator a phosphorus-based stabilizer
- an ultraviolet light absorber a light stabilizer
- the reaction of the carboxy group of the thermoplastic polyester resin (A) and the epoxy compound (B) can be further promoted, and the long-term hydrolysis resistance and heat aging resistance can be further improved.
- hindered amine compounds containing nitrogen or phosphorus, organic phosphines and salts thereof, amidine compounds, imidazoles and the like are examples of hindered amine compounds containing nitrogen or phosphorus, organic phosphines and salts thereof, amidine compounds, imidazoles and the like.
- hindered amine compound examples include 4-benzoyloxy-2,2,6,6-tetramethylpiperidine, bis- (2,2,6,6-tetramethyl-4-piperidyl) adipate, bis- (2, 2,6,6-Tetramethyl-4-piperidyl) suberate, bis- (2,2,6,6-tetramethyl-4-piperidyl) sebacate, bis- (2,2,6,6-tetramethyl-4) -Piperidyl) phthalate, bis- (2,2,6,6-tetramethyl-4-piperidyl) terephthalate, bis- (1,2,2,6,6-pentamethyl-4-piperidyl) sebacate, bis- (1 2,2,2,6,6-pentamethyl-4-piperidyl) terephthalate, N, N'-bis- (2,2,6,6-tetramethyl-4-piperidyl) isophthalamide, N N'-bis- (2,2,6,6-tetramethyl-4-piperidyl) iso
- hindered amine compounds it is an active hydrogen-containing, strongly basic secondary amine, and (2, B) a 2,2,6,6-tetramethyl-4-piperidyl structure capable of promoting the reaction between an epoxy compound and a carboxyl group.
- NH type hindered amines are preferred.
- amidine compounds include 1,8-diazabicyclo (5,4,0) undecene-7, 1,5-diazabicyclo (4,3,0) nonene-5,5,6-dibutylamino-1,8 diazabicyclo (5,4,0) undecene-7, 7-methyl-1,5,7-triazabicyclo (4,4,0) decene-5 and the like.
- the above-mentioned amidine compounds can also be used in the form of salts with inorganic acids or organic acids such as 1,8-diazabicyclo (5,4,0) undecen-7 tetraphenylborate.
- organic phosphines and salts thereof include triparatolyl phosphine, tris-4-methoxyphenyl phosphine, tetrabutylphosphonium bromide, butyltriphenylphosphonium bromide, benzyltriphenylphosphonium bromide, tetraphenylphosphonium bromide, and tetraphenylphosphonium tetraphenylborate.
- triparatolyl phosphine tris-4-methoxyphenyl phosphine
- tetrabutylphosphonium bromide butyltriphenylphosphonium bromide
- benzyltriphenylphosphonium bromide tetraphenylphosphonium bromide
- tetraphenylphosphonium tetraphenylborate tetraphenylphosphonium tetraphenylborate.
- triphenyl phosphine trip
- imidazole for example, 2-methylimidazole, 2-aminoimidazole, 2-methyl-1-vinylimidazole, 2-ethyl-4-methylimidazole, 2-heptadecylimidazole, 2-phenylimidazole, 2-undecylimidazole 1-allylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2-undecylimidazolium trimellitate, 1-benzyl-2-methylimidazole, 1- Cyanoethyl-2-ethyl-4-methylimidazole, 1-cyanoethyl-2-phenylimidazolium trimellitate, 1-dodecyl-2-methyl-3-benzylimidazolium chloride, 2-methylimidazolium isocyanurate 2-phenylimidazolium isocyanurate, 2,4-did
- the compounding amount of the reaction accelerator is preferably 0.001 to 1 part by weight with respect to 100 parts by weight in total of the thermoplastic polyester resin (A) and the hydroxy group-containing resin (C).
- the compounding amount of the reaction accelerator is 0.001 parts by weight or more, long-term hydrolysis resistance can be further improved.
- the compounding amount is 1 part by weight or less, long-term hydrolysis resistance can be further improved while maintaining mechanical properties.
- blend phosphorus stabilizer as said additive.
- blending a phosphorus stabilizer the crosslinking reaction of epoxy compounds (B) can be suppressed and the retention stability at the time of high temperature 270 degreeC or more can further be improved.
- the phosphorus-based stabilizer in the present invention is a compound including a structure in which two or more oxygen atoms are bonded to a phosphorus atom having a noncovalent electron pair.
- a structure in which two or more oxygen atoms are bonded to a phosphorus atom having a noncovalent electron pair.
- it can be coordinated to the phenoxy radical or quinone which is the coloring cause derived from the novolac type epoxy resin, and can be decomposed or decolorized.
- bonded with the phosphorus atom which has an unshared electron pair is three pieces.
- a phosphorus-based stabilizer as a compound containing a structure in which two oxygen atoms are bonded to a phosphorus atom having a non-covalent electron pair, a phosphonite compound, and three oxygen atoms to phosphorus atoms having a phosphorus atom having a non-covalent electron pair
- a phosphite compound etc. can be mentioned as a compound containing the structure couple
- phosphinite compounds include phosphonous acid compounds such as phenylphosphonous acid and 4,4'-biphenyldiphospholine acid, aliphatic alcohols having 4 to 25 carbon atoms and / or 2,6-di-t- Examples thereof include condensates with phenol compounds such as butylphenol and 2,4-di-t-butyl-5-methylphenol.
- tetrakis (2,4-di-t-butyl-5-methylphenyl) -4,4'-biphenylene diphosphonite tetrakis (2,4--) from the viewpoint of the thermal stability of the phosphorus-based stabilizer.
- Di-t-butylphenyl) -4,4'-biphenylene diphosphonite is preferred.
- phosphite compounds include phosphorous acid, aliphatic alcohols having 4 to 25 carbon atoms, polyhydric alcohols such as glycerol and pentaerythritol, and / or 2,6-di-t-butylphenol and 2,4-di And condensates with phenol compounds such as t-butylphenol.
- triisodecyl phosphite tris nonylphenyl phosphite, diphenyl isodecyl phosphite, phenyldiisodecyl phosphite, 2,2-methylenebis (4,6-di-t-butylphenyl) octyl phosphite, 4 4,4'-Butylidenebis (3-methyl-6-t-butylphenyl) ditridecyl phosphite, tris (2,4-di-t-butylphenyl) phosphite, tris (2-t-butyl-4-methylphenyl) ) Phosphite, tris (2,4-di-t-amylphenyl) phosphite, tris (2-t-butylphenyl) phosphite, tris [2- (1,1-dimethylpropyl) -phenyl]
- bis (alkylaryl) pentaerythritol diphosphite is preferable from the viewpoint of the heat resistance stability of the phosphorus-based stabilizer, and bis (2,4-di-t-butyl-4-methylphenyl) pentaerythritol diphosphite is preferable. More preferred is bis (2,6-di-t-butyl-4-methylphenyl) pentaerythritol diphosphite.
- the compounding amount of the phosphorus-based stabilizer can be adjusted by the kind and compounding amount of the epoxy compound (B), but a total of 100 weight of the thermoplastic polyester resin (A) and the hydroxy group-containing resin (C) 0.01 to 1 part by weight is preferable.
- the color tone can be improved.
- the compounding amount is more preferably 0.05 parts by weight or more.
- hydrolysis resistance and mechanical physical properties can be further improved by setting the compounding amount of the phosphorus-based stabilizer to 1 part by weight or less. 0.5 parts by weight or less is more preferable.
- thermoplastic resins other than the component (A) may be added to the resin composition of the present invention as long as the object of the present invention is not impaired, and the moldability, dimensional accuracy, molding shrinkage, toughness and the like are improved. be able to.
- thermoplastic resins other than the component (A) include olefin resins, vinyl resins, polyamide resins, polyacetal resins, polyurethane resins, aromatic or aliphatic polyketone resins, polyphenylene sulfide resins, polyetheretherketone resins, polyimides Resin, thermoplastic starch resin, polyurethane resin, aromatic polycarbonate resin, polyarylate resin, polysulfone resin, polyethersulfone resin, phenoxy resin, polyphenylene ether resin, poly-4-methylpentene-1, polyetherimide resin, cellulose acetate Resin, polyvinyl alcohol resin, etc. can be mentioned.
- the olefin resin examples include ethylene / propylene copolymer, ethylene / propylene / non-conjugated diene copolymer, ethylene-butene-1 copolymer, ethylene / glycidyl methacrylate copolymer, ethylene / butene-1 / Maleic anhydride copolymer, ethylene / propylene / maleic anhydride copolymer, ethylene / maleic anhydride copolymer and the like.
- vinyl resin examples include methyl methacrylate / styrene resin (MS resin), methyl methacrylate / acrylonitrile resin, polystyrene resin, acrylonitrile / styrene resin (AS resin), styrene / butadiene resin, styrene / N- Vinyl-based (co) polymers such as phenylmaleimide resin, styrene / acrylonitrile / N-phenylmaleimide resin, acrylonitrile / butadiene / styrene resin (ABS resin), acrylonitrile / butadiene / methyl methacrylate / styrene resin (MABS resin), high Impact-Styrene resin modified with rubbery polymer such as polystyrene resin; styrene / butadiene / styrene resin, styrene / isoprene
- MS resin
- the blending amount of the olefin resin is preferably 0.1 to 30 parts by weight with respect to 100 parts by weight in total of the thermoplastic polyester resin (A) and the hydroxy group-containing resin (C).
- the amount is 0.1 parts by weight or more, the toughness and the hydrolysis resistance are further improved.
- a compounding quantity 0.5 weight part or more is more preferable, More preferably, it is 1 weight part or more.
- the compounding amount is 30 parts by weight or less, mechanical physical properties are further improved.
- the blending amount is more preferably 20 parts by weight or less, still more preferably 10 parts by weight or less.
- the resin composition of the present invention is described as a multifunctional compound having a molecular weight of less than 2,000 (hereinafter referred to as "polyfunctional compound") having three or four functional groups and containing one or more alkylene oxide units. May be formulated.
- the functional group include hydroxy group, aldehyde group, carboxylic acid group, sulfo group, amino group, isocyanate group, carbodiimide group, carbodiimide group, oxazoline group, oxazine group, ester group, amide group, silanol group, silyl ether group and the like.
- a compound containing an ethylene oxide unit or a propylene oxide unit as an alkylene oxide unit, from the viewpoint of being excellent in fluidity, recyclability, durability, heat resistance and mechanical properties.
- a compound containing a propylene oxide unit in that it is excellent in long-term hydrolysis resistance and toughness (tensile breaking elongation).
- the number of alkylene oxide units is preferably 0.1 or more, more preferably 0.5 or more, and still more preferably 1 or more, from the viewpoint of being more excellent in fluidity. is there.
- the alkylene oxide unit per one functional group is preferably 20 or less, more preferably 10 or less, and still more preferably 5 or less, in terms of more excellent mechanical properties.
- a flame retardant can be blended with the thermoplastic polyester resin composition of the present invention as long as the effects of the present invention are not impaired.
- the flame retardant include phosphorus flame retardants, halogen flame retardants such as brominated flame retardants, salts of triazine compounds with cyanuric acid or isocyanuric acid, silicone flame retardants and inorganic flame retardants. Two or more of these may be blended.
- the resin composition of the present invention is further blended with one or more of carbon black, titanium oxide, and pigments and dyes of various colors, toning to various colors, weatherability (light) resistance and conductivity. It is also possible to improve Examples of carbon black include channel black, furnace black, acetylene black, anthracene black, oil smoke, pine smoke, and graphite. Carbon black has an average particle size of 500nm or less, and dibutyl phthalate oil absorption amount is 50 ⁇ 400cm 3 / 100g is preferably used.
- titanium oxide titanium oxide having a crystal form such as rutile type or anatase type and having an average particle diameter of 5 ⁇ m or less is preferably used.
- carbon black, titanium oxide and pigments and dyes of various colors may be treated with aluminum oxide, silicon oxide, zinc oxide, zirconium oxide, polyol, and a silane coupling agent.
- it may be used as a mixed material which is melt-blended or simply blended with various thermoplastic resins.
- the blending amount of the pigment and the dye is preferably 0.01 to 3 parts by weight with respect to 100 parts by weight in total of the thermoplastic polyester resin (A) and the hydroxy group-containing resin (C). From the viewpoint of preventing uneven coloring, 0.03 parts by weight or more is more preferable, and from the viewpoint of mechanical strength, 1 part by weight or less is more preferable.
- the molded article of the present invention preferably has a tensile strength retention of 75% or more after exposure to the atmosphere in an atmosphere at a temperature of 190 ° C. for 500 hours in order to suppress oxidative decomposition of the polyester resin due to thermal degradation.
- the tensile strength retention is less than 75%, it means that the main chain decomposition and the molecular weight decrease due to the oxidative deterioration of the polyester resin are in progress.
- the tensile strength retention is preferably 80% or more, more preferably 85% or more, and still more preferably 90% or more. As the value of the tensile strength retention ratio approaches 100%, it indicates that the thermal oxidation deterioration of the polyester resin is not progressing, and indicates that the heat aging resistance is high.
- the molded article of the present invention has a tensile strength retention of 90% or more after exposure for 50 hours in an atmosphere with a relative humidity of 100% and a temperature of 121 ° C. to suppress a decrease in molecular weight due to hydrolysis of the polyester resin. Is preferred.
- the tensile strength retention is less than 90%, it means that the carboxyl terminal group is increased by the hydrolysis of the polyester resin and the decrease in molecular weight is in progress.
- the carboxyl terminal group is increased by the hydrolysis of the polyester resin and the decrease in molecular weight is in progress.
- the molecular weight reduction of the polyester resin is further promoted and the mechanical properties are reduced.
- 92% or more is preferable and 95% or more of the said tensile strength retention is more preferable.
- the value of the tensile strength retention rate approaches 100%, it is shown that the decrease in molecular weight due to the progress of hydrolysis of the polyester resin is suppressed, and it is shown that the hydrolysis resistance is high.
- thermoplastic polyester resin composition of the present invention can be obtained, for example, by melt-kneading the components (A) to (C) and, if necessary, other components.
- melt-kneading method for example, a thermoplastic polyester resin (A), an epoxy compound (B), a hydroxy group-containing resin (C), a reaction accelerator, and various additives and the like as necessary are preliminarily mixed, There is a method of supplying to an extruder or the like to sufficiently melt and knead it, or a method of supplying each component to an extruder or the like by a predetermined amount using a quantitative feeder such as a weight finder and the like to sufficiently melt and knead.
- a quantitative feeder such as a weight finder and the like
- Examples of the above-mentioned pre-mixing include a method of dry blending and a method of mixing using a mechanical mixing device such as a tumbler, a ribbon mixer and a Henschel mixer.
- a mechanical mixing device such as a tumbler, a ribbon mixer and a Henschel mixer.
- inorganic fillers other than the fiber reinforcement (E) and the fiber reinforcement may be added by installing a side feeder in the middle of the loading portion and the vent portion of a multi-screw extruder such as a twin-screw extruder. .
- a method of installing a liquidation nozzle in the middle of the loading and unloading parts of a multi-screw extruder such as a twin-screw extruder and adding using a plunger pump, or loading It is also possible to use a method of supplying a metering pump from a part or the like.
- the thermoplastic polyester resin composition of the present invention is preferably pelletized and then subjected to molding processing.
- a method of pelletizing for example, a single screw extruder equipped with a screw of “unimelt” or “dalmage” type, a twin screw extruder, a triple screw extruder, a conical extruder, a kneader of kneader type, etc. can be used. It discharges in the shape of a strand, and the method of cutting with a strand cutter is mentioned.
- thermoplastic polyester resin composition of the present invention By melt-molding the thermoplastic polyester resin composition of the present invention, molded articles of films, fibers and other various shapes can be obtained.
- melt molding method include injection molding, extrusion molding and blow molding, and injection molding is particularly preferably used.
- injection molding As a method of injection molding, gas assist molding, two-color molding, sandwich molding, in-mold molding, insert molding, injection press molding, etc. are known besides the usual injection molding method, but any molding method is applied. it can.
- the molded articles of the present invention are excellent in long-term heat aging resistance and hydrolysis resistance, and take advantage of features such as tensile strength and elongation and excellent mechanical properties and heat resistance to form mechanical and mechanical parts, electric parts, electronic parts and automobiles. It can be used as a molded article of parts.
- the molded article of the present invention is particularly useful for exterior component applications because long-term heat aging resistance and hydrolysis resistance can be simultaneously achieved at high levels.
- mechanical parts, electrical parts, electronic parts and automobile parts include breakers, electromagnetic switches, focus cases, flyback transformers, molded articles for fixing machines for copying machines and printers, general household appliances, OA Housings for equipment, Varicon case parts, various terminal boards, transformers, printed wiring boards, housings, terminal blocks, coil bobbins, connectors, relays, disk drive chassis, transformers, switch parts, socket parts, motor parts, sockets, plugs , Capacitors, various cases, resistors, electric / electronic parts incorporating metal terminals and wires, computer parts, audio parts such as acoustic parts, lighting parts, telegraph equipment parts, telephone equipment parts, air conditioner parts, VTR Home appliance parts such as TVs, etc., parts for copying machines, Kushimiri parts, parts for optical instruments, automotive ignition system parts, automotive connectors, and various electrical components for automobiles and the like.
- thermoplastic polyester resin composition of the present invention will be specifically described by way of examples.
- the raw material used for an Example and a comparative example is shown next.
- % and parts all mean weight% and parts by weight.
- "/" In the following resin names means copolymerization.
- Epoxy compound (B) ⁇ B-1> Bisphenol A Type Epoxy: “jER” (registered trademark) 1004 K manufactured by Mitsubishi Chemical Corporation was used (epoxy equivalent weight: 926 g / eq).
- N-glycidyl phthalimide Nagase ChemteX Co., Ltd. product "Denacol" (registered trademark) EX-731 was used (epoxy equivalent weight: 216 g / eq).
- Glycidyl phenyl ether A glycidyl phenyl ether manufactured by Tokyo Chemical Industry Co., Ltd. was used (epoxy equivalent: 152 g / eq).
- Hydroxy group-containing resin (C) having a halogen element content of 1,000 ppm or less ⁇ C-1> Bisphenol A Type Phenoxy Resin: “jER” (registered trademark) 1010 manufactured by Mitsubishi Chemical Corporation was used (hydroxy group number: 3.3 eq / kg, number average molecular weight: 5,500).
- ⁇ C-4> Ethylene-vinyl alcohol copolymer: "EVAL" (registered trademark) F171B manufactured by Kuraray Co., Ltd. (hydroxy group value: 17 eq / kg, number average molecular weight: 25,000). The content of the halogen element in each of ⁇ C-1> to ⁇ C-4> was 1,000 ppm or less.
- ⁇ C'-1> Dipentaerythritol: Using dipentaerythritol manufactured by Hiroei Chemical Industry Co., Ltd. (hydroxy group value: 24 eq / kg, number average molecular weight: 254.3, content of halogen element: 1000 ppm or less) ).
- Fiber reinforcement (E) Glass fiber treated with a sizing agent containing a copolymer consisting of maleic anhydride: ECS03T-253 manufactured by Nippon Electric Glass Co., Ltd., with a diameter of 13 ⁇ m in cross section and a fiber length of 3 mm.
- component (A) When a polybutylene terephthalate resin is used as component (A) using an IS55 EPN injection molding machine manufactured by Toshiba Machine Co., Ltd., it is used as a component (A) at a molding temperature of 250 ° C. or 270 ° C. and a mold temperature of 80 ° C. When polyethylene terephthalate resin is used, injection molding is performed under molding cycle conditions of molding temperature 270 ° C or 290 ° C, mold temperature 80 ° C, injection time and holding time total 10 seconds, cooling time 10 seconds The test piece of 1/8 inch (about 3.2 mm) in thickness was obtained.
- the tensile maximum point strength (tensile strength) and the tensile maximum point elongation (tensile elongation) were measured according to ASTM D 638 (2005), using the obtained test pieces for tensile property evaluation. The value was an average value of 5 measured values. It was judged that a material having a large tensile strength value is excellent in mechanical strength, and a material having a large tensile elongation value is judged to be excellent in toughness.
- the above-mentioned 1. was carried out using IS55 EPN injection molding machine manufactured by Toshiba Machine. Injection molding was performed under the same conditions as the test pieces for measuring mechanical physical properties described in Section 1 to obtain test pieces for evaluation of ASTM No. 1 dumbbell of 1/8 inch (about 3.2 mm) thickness. The obtained test piece for evaluation was placed in a hot air oven at 190 ° C. under atmospheric pressure, and heat treatment was performed for 500 hours. About the test piece for evaluation after heat processing, the said 1st. The tensile maximum point strength was measured under the same conditions as the item. The value was an average value of three measured values.
- Tensile maximum point strength of the test piece for evaluation after heat treatment The tensile strength retention was calculated from the following equation from the tensile maximum point strength of the test piece for evaluation before heat treatment measured in the section. It was judged that the higher the tensile strength retention, the better the heat aging resistance, and the particularly excellent at 75% or more.
- Tensile strength retention (%) (maximum tensile strength after heat treatment / maximum tensile strength before heat treatment) ⁇ 100.
- Tensile maximum point strength of the test specimen for evaluation after wet heat treatment and From the tensile maximum point strength of the test piece for evaluation before the wet heat treatment measured in Section, the tensile strength retention was determined by the following equation. The larger the tensile strength retention, the better the hydrolysis resistance, and it was judged that the material of 90% or more is particularly excellent in the hydrolysis resistance.
- Tensile strength retention (%) (Tension maximum point strength after wet heat treatment / Tension maximum point strength before wet heat treatment) ⁇ 100.
- the resulting pellets were dried in a hot air drier at a temperature of 110 ° C. for 12 hours, and then molded and evaluated in the manner described above.
- Tables 1 to 9 show the results.
- the hydroxy group concentration (eq / kg) of the hydroxy group-containing resin in the thermoplastic polyester resin composition described in Tables 1 to 9 is equivalent to the hydroxy group equivalent derived from the hydroxy group-containing resin in 1 kg of the thermoplastic polyester resin composition (eq ) Is shown.
- the number average molecular weight is out of the specific range by blending the hydroxy group-containing resin (C) having the specific number average molecular weight in the specific range.
- the bleed out property was also improved while maintaining the mechanical properties, and the heat aging resistance was improved without reducing the hydrolysis resistance. As a result, it can be seen that a material having both high heat aging resistance and hydrolysis resistance can be obtained.
- thermoplastic polyester resin (A) and the hydroxy group-containing resin (C) in a specific range. Aging resistance and hydrolysis resistance were improved, and a material having both heat aging resistance and hydrolysis resistance was obtained.
Abstract
Description
[1]熱可塑性ポリエステル樹脂(A)、200~3,000g/eqのエポキシ当量を有するエポキシ化合物(B)および数平均分子量2,000~500,000かつハロゲン元素含有量が1,000ppm以下であるヒドロキシ基含有樹脂(C)を配合してなる熱可塑性ポリエステル樹脂組成物であって、熱可塑性ポリエステル樹脂(A)70~99.9重量部およびヒドロキシ基含有樹脂(C)0.1~30重量部の合計100重量部に対し、エポキシ化合物(B)を0.05~10重量部配合してなる熱可塑性ポリエステル樹脂組成物。
[2]上記の熱可塑性ポリエステル樹脂組成物を溶融成形してなる成形品。
また、(D)前記一般式(1)で表されるリン化合物の配合量は、熱可塑性ポリエステル樹脂(A)およびヒドロキシ基含有樹脂(C)の合計100重量部に対し、0.01~1重量部が好ましい。リン化合物(D)の配合量が0.01重量部以上であると、耐酸化劣化性を向上できる。配合量は、より好ましくは0.02重量部以上であり、さらに好ましくは0.05重量部以上である。一方、リン化合物(D)の配合量を1重量部以下とすることで、機械物性、耐加水分解性および耐ブリードアウト性が向上できる。配合量は、より好ましくは0.5重量部以下であり、さらに好ましくは0.3重量部以下である。
<A-1>ポリブチレンテレフタレート樹脂:東レ(株)製、融点225℃、o-クロロフェノールを溶媒として25℃で測定した固有粘度が0.80dL/gのポリブチレンテレフタレート樹脂を用いた。
<A-2>ポリエチレンテレフタレート樹脂:東レ(株)製、融点255℃、o-クロロフェノールを溶媒として25℃で測定した固有粘度が0.63dL/gのポリエチレンテレフタレート樹脂を用いた。
<B-1>ビスフェノールA型エポキシ:三菱ケミカル(株)製の“jER”(登録商標)1004Kを用いた(エポキシ当量:926g/eq)。
<B-2>ジシクロペンタジエン型ノボラックエポキシ:DIC(株)製“EPICLON”HP-7200Hを用いた(エポキシ当量:275g/eq)。
<B-3>ネオデカン酸グリシジルエステル:モメンティブ・パフォーマンス・マテリアルズ社製“CARDURA”(登録商標)E-10Pを用いた(エポキシ当量:239g/eq)。
<B-4>N-グリシジルフタルイミド:ナガセケムテックス(株)製“デナコール”(登録商標)EX-731を用いた(エポキシ当量:216g/eq)。
<B’-5>グリシジルフェニルエーテル:東京化成工業(株)製のグリシジルフェニルエーテルを用いた(エポキシ当量:152g/eq)。
<C-1>ビスフェノールA型フェノキシ樹脂:三菱ケミカル(株)製の“jER”(登録商標)1010を用いた(ヒドロキシ基価:3.3eq/kg、数平均分子量:5,500)。
<C-2>ビスフェノールA型フェノキシ樹脂:Gabriel社製のPKHBを用いた(ヒドロキシ基価:3.6eq/kg、数平均分子量:10,000)。
<C-3>ヒドロキシ基含有アクリルポリマー:東亞合成(株)製“ARUFON”(登録商標)UH-2170を用いた(ヒドロキシ基価:7.7eq/kg、数平均分子量:6,500)。
<C-4>エチレン-ビニルアルコール共重合ポリマー:(株)クラレ製“EVAL”(登録商標)F171Bを用いた(ヒドロキシ基価:17eq/kg、数平均分子量:25,000)。
なお、<C-1>~<C-4>はいずれも、ハロゲン元素含有量は1000ppm以下であった。
<C’-1>ジペンタエリストール:広栄化学工業(株)製のジペンタエリストールを用いた(ヒドロキシ基価:24eq/kg、数平均分子量:254.3、ハロゲン元素含有量:1000ppm以下)。
<C’-2>ハロゲン含有エポキシ樹脂系難燃剤:DIC(株)製のテトラブロモビスフェノールA-エポキシポリマー(ECX-30)を用いた(ヒドロキシ基価:1.7eq/kg、数平均分子量:3,000、ハロゲン元素含有量:580000ppm)。
前記一般式(1)で表されるリン化合物(D)
<D-1>ホスフィン酸ナトリウム:東京化成工業(株)製のホスフィン酸ナトリウム(試薬)を用いた。
繊維強化材(E)
<E-1>無水マレイン酸からなる共重合体を含有する集束剤により処理されたガラス繊維:日本電気硝子(株)製ECS03T-253、断面の直径13μm、繊維長3mmを用いた。
<E-2>エポキシ化合物を含有する集束剤により処理されたガラス繊維:日本電気硝子(株)製ガラス繊維ECS03T-187、断面の直径13μm、繊維長3mmを用いた。
実施例、比較例においては、次に記載する測定方法によって、その特性を評価した。
東芝機械製IS55EPN射出成形機を用いて、(A)成分としてポリブチレンテレフタレート樹脂を使用した場合は、成形温度250℃もしくは270℃、金型温度80℃の温度条件で、また(A)成分としてポリエチレンテレフタレート樹脂を使用した場合は成形温度270℃もしくは290℃、金型温度80℃の温度条件で、射出時間と保圧時間は合わせて10秒、冷却時間10秒の成形サイクル条件で射出成形を行い、試験片厚み1/8インチ(約3.2mm)のASTM1号ダンベルの引張物性評価用試験片を得た。得られた引張物性評価用試験片を用い、ASTM D638(2005年)に従い、引張最大点強度(引張強度)および引張最大点伸び(引張伸度)を測定した。値は5本の測定値の平均値とした。引張強度の値が大きい材料を機械強度に優れていると判断し、引張伸度の値が大きい材料を靭性に優れていると判断した。
東芝機械製IS55EPN射出成形機を用いて、上記1.項の機械物性測定用の試験片と同一の条件で射出成形を行い、1/8インチ(約3.2mm)厚みのASTM1号ダンベルの評価用試験片を得た。得られた評価用試験片を190℃の大気圧下の熱風オーブン中に置き、500時間加熱処理を行った。加熱処理後の評価用試験片について、上記第1.項と同一の条件で引張最大点強度を測定した。値は3本の測定値の平均値とした。加熱処理後の評価用試験片の引張最大点強度と、上記第1.項で測定した加熱処理前の評価用試験片の引張最大点強度から、下記式より引張強度保持率を算出した。引張強度保持率が大きいほど耐熱老化性に優れ、75%以上では特に優れていると判断した。
引張強度保持率(%)=(加熱処理後の引張最大点強度/加熱処理前の引張最大点強度)×100。
東芝機械製IS55EPN射出成形機を用いて、上記1.項の機械物性測定用の試験片と同一の条件で射出成形を行い、試験片厚み1/8インチ(約3.2mm)のASTM1号ダンベルの引張物性評価用試験片を得た。得られたASTM1号ダンベルを121℃×100%RHの温度と湿度に設定されたエスペック(株)社製高度加速寿命試験装置EHS-411に投入し、50時間加圧湿熱処理を行った。湿熱処理後の成形品について、上記1.項と同一の条件で引張最大点強度を測定した。値は3本の測定値の平均値とした。湿熱処理後の評価用試験片の引張最大点強度と、上記第1.項で測定した湿熱処理前の評価用試験片の引張最大点強度から、下記式により引張強度保持率を求めた。引張強度保持率が大きいほど耐加水分解性に優れ、90%以上の材料は耐加水分解性に特に優れていると判断した。
引張強度保持率(%)=(湿熱処理後の引張最大点強度/湿熱処理前の引張最大点強度)×100。
東芝機械製IS55EPN射出成形機を用いて、上記1.項の機械物性測定用の試験片と同一の条件で射出成形を行い、試験片厚み1/8インチ(約3.2mm)のASTM1号ダンベルのブリードアウト評価用試験片を得た。得られたASTM1号ダンベルを、170℃の大気圧下の熱風オーブン中に置き、1000時間乾熱処理を行った。また、同様に得られたASTM1号ダンベルを121℃×100%RHの温度と湿度に設定されたエスペック(株)社製高度加速寿命試験装置EHS-411に50時間投入し湿熱処理を行った。乾熱処理後および湿熱処理後の成形品外観を目視観察し、次の基準によりブリードアウトの判定を行った。
A:いずれの成形品にも液状もしくは白粉状のブリードアウトが観察されない。
B:成形品の一部もしくは随所に液状または白粉状のブリードアウトが観察される。
スクリュー径30mm、L/D35の同方向回転ベント付き二軸押出機(日本製鋼所製、TEX-30α)を用いて、熱可塑性ポリエステル樹脂(A)、エポキシ化合物(B)、ヒドロキシ基含有樹脂(C)、必要に応じてその他の材料を表1~表9に示した組成で混合し、二軸押出機の元込め部から添加した。なお、繊維強化材(E)は、元込め部とベント部の途中にサイドフィーダーを設置して添加した。混練温度250℃、スクリュー回転200rpmの押出条件で溶融混合を行い、溶融混合された樹脂をストランド状に吐出し、冷却バスを通した後、ストランドカッターによりペレット化した。
Claims (12)
- 熱可塑性ポリエステル樹脂(A)、200~3,000g/eqのエポキシ当量を有するエポキシ化合物(B)および数平均分子量2,000~500,000かつハロゲン元素含有量が1,000ppm以下であるヒドロキシ基含有樹脂(C)を配合してなる熱可塑性ポリエステル樹脂組成物であって、熱可塑性ポリエステル樹脂(A)70~99.9重量部およびヒドロキシ基含有樹脂(C)0.1~30重量部の合計100重量部に対し、エポキシ化合物(B)を0.05~10重量部配合してなる熱可塑性ポリエステル樹脂組成物。
- 前記熱可塑性ポリエステル(A)が200℃より高い融点を有する請求項1に記載の熱可塑性ポリエステル樹脂組成物。
- 前記エポキシ化合物(B)が、一分子内に二つ以上のエポキシ基を有するエポキシ化合物を含有する請求項1または2に記載の熱可塑性ポリエステル樹脂組成物。
- 前記ヒドロキシ基含有樹脂(C)のヒドロキシ基価が3~20eq/kgである請求項1~3のいずれかに記載の熱可塑性ポリエステル樹脂組成物。
- 前記ヒドロキシ基含有樹脂(C)が、フェノキシ樹脂および/またはヒドロキシアルキル(メタ)アクリレートを構造単位として含むアクリル樹脂である請求項1~4のいずれかに記載の熱可塑性ポリエステル樹脂組成物。
- 前記熱可塑性ポリエステル樹脂(A)および前記ヒドロキシ基含有樹脂(C)の合計100重量部に対し、さらに(D)下記一般式(1)で表されるリン化合物0.01~1重量部を配合してなる請求項1~5のいずれかに記載の熱可塑性ポリエステル樹脂組成物:
- 前記(D)上記一般式(1)で表されるリン化合物がホスホン酸の金属塩またはホスフィン酸の金属塩である請求項6に記載の熱可塑性ポリエステル樹脂組成物。
- 前記熱可塑性ポリエステル樹脂(A)が、ポリブチレンテレフタレート、ポリプロピレンテレフタレートおよびポリブチレンナフタレートから選ばれた樹脂である請求項1~7のいずれかに記載のポリエステル樹脂組成物。
- 前記熱可塑性ポリエステル樹脂(A)が、ポリブチレンテレフタレートである請求項1~8のいずれかに記載の熱可塑性ポリエステル樹脂組成物。
- 前記熱可塑性ポリエステル樹脂(A)および前記ヒドロキシ基含有樹脂(C)の合計100重量部に対し、繊維強化材(E)をさらに1~100重量部含有する請求項1~9のいずれかに記載の熱可塑性ポリエステル樹脂組成物。
- ASTM D638(2005年)に準じて成形した1/8インチ試験片を大気中、温度190℃の雰囲気下で500時間暴露した後の引張強度保持率(%)=(暴露後の引張強度/暴露前の引張強度)×100が75%以上であり、かつ、ASTM D638(2005年)に準じて成形した1/8インチ試験片を、相対湿度100%、温度121℃の雰囲気下で50時間暴露した後の引張強度保持率(%)=(暴露後の引張強度/暴露前の引張強度)×100が90%以上である請求項1~10のいずれかに記載の熱可塑性ポリエステル樹脂組成物。
- 請求項1~11のいずれかに記載の熱可塑性ポリエステル樹脂組成物を溶融成形してなる成形品。
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WO2021200793A1 (ja) * | 2020-03-30 | 2021-10-07 | 日鉄ケミカル&マテリアル株式会社 | 繊維強化プラスチック成形材料 |
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US20220283393A1 (en) * | 2021-03-08 | 2022-09-08 | Corning Research & Development Corporation | Flame retardant compositions for buffer tubes and method of making same |
CN114213819B (zh) * | 2022-02-21 | 2022-05-03 | 广东顺德顺炎新材料股份有限公司 | 一种耐磨免底涂pbt复合材料 |
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