Resin composition, pellet, molded article, method for improving appearance, and appearance improver

A resin composition with polyalkylene terephthalate resin and recycled glass fibers, supplemented with other resins or flame retardants, addresses poor appearance and mechanical property issues by suppressing alkaline reactions, ensuring excellent performance post-moist heat test.

JP2026031234APending Publication Date: 2026-02-24MITSUBISHI CHEM CORP
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Patent Information

Application Number
JP2024134634
Authority / Receiving Office
JP · JP
Patent Type
Applications
Current Assignee / Owner
Filing Date
2024-08-09
Publication Date
2026-02-24

AI Technical Summary

Technical Problem

Recycled glass fibers, such as A-glass and C-glass fibers, when blended with polyalkylene terephthalate resins, result in poor appearance due to powdery matter adherence after a moist heat test, compromising mechanical properties.

Method used

A resin composition is formulated with a blend of polyalkylene terephthalate resin, recycled glass fibers, and additional resins or flame retardants to suppress the reaction of alkaline components in the glass fibers with the resin, maintaining mechanical properties and appearance.

Benefits of technology

The resin composition achieves excellent mechanical properties and appearance after a moist heat test by balancing the polyalkylene terephthalate resin content and incorporating other resins or flame retardants to prevent powdery matter precipitation.

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Abstract

To provide a resin composition which is obtained by blending a polyalkylene terephthalate resin with an A glass fiber and / or a C glass fiber as a recycled product and gives a molded article excellent in mechanical properties and appearance after a wet heat test, and to provide a pellet, a molded article, a method for improving appearance, and an appearance improver.SOLUTION: The resin composition according to the present disclosure comprises a polyalkylene terephthalate resin and at least one of a C-glass fiber and / or an A-glass fiber, wherein the C-glass fiber and / or the A-glass fiber comprises a recycled glass fiber, and the content of the polyalkylene terephthalate resin in the resin composition is 50-95 parts by mass based on 100 parts by mass of the total components excluding the glass fiber.SELECTED DRAWING: None
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Description

[Technical Field]

[0001] The present invention relates to a resin composition, a pellet, a molded article, a method for improving appearance, and an appearance improver, and more particularly to a resin composition containing a polyalkylene terephthalate resin as a main component. [Background technology]

[0002] Polyalkylene terephthalate resins, typified by polybutylene terephthalate resin and polyethylene terephthalate resin, are widely used in electrical and electronic equipment parts, automotive interior and exterior parts, other electrical parts, machine parts, etc., because of their excellent mechanical strength, chemical resistance, electrical insulation properties, etc. Here, in order to improve the mechanical strength of the polyalkylene terephthalate resin, glass fibers (usually E-glass fibers) are sometimes blended into the polyalkylene terephthalate resin (Patent Document 1, Patent Document 2). [Prior art documents] [Patent documents]

[0003] [Patent Document 1] Japanese Patent Application Laid-Open No. 2012-087234 [Patent Document 2] Japanese Patent Publication No. 2022-8175 Summary of the Invention [Problem to be solved by the invention]

[0004] In recent years, recycling of glass fibers has been considered from the viewpoint of effective utilization of resources, and therefore, it is considered to blend recycled glass fibers into polyalkylene terephthalate resins. Here, recycled glass fibers are often made from inexpensive glass used for glass bottles and building materials. Therefore, recycled glass fibers are often A-glass fibers or C-glass fibers. However, the inventors' investigations revealed that when a molded product is manufactured by blending A-glass fibers or C-glass fibers with a polyalkylene terephthalate resin, poor appearance occurs after a moist heat test. Specifically, it was found that powdery matter adheres to the surface of the molded product. Naturally, such molded articles are also required to have excellent mechanical properties. The present invention aims to solve these problems, and provides a resin composition comprising a polyalkylene terephthalate resin blended with recycled A-glass fiber and / or C-glass fiber, which, when molded into a molded article, has excellent mechanical properties and appearance after a moist heat test, as well as pellets, a molded article, a method for improving appearance, and an appearance improver. [Means for solving the problem]

[0005] In light of the above-mentioned problems, the present inventors have conducted research and have found that the above-mentioned problems can be solved by blending a resin other than polyester resin into a resin composition in which recycled A-glass fiber and / or C-glass fiber is blended with a polyalkylene terephthalate resin. Specifically, the above problems were solved by the following means. [1] A polyalkylene terephthalate resin, At least one of C glass fiber and / or A glass fiber is included, and the C glass fiber and / or A glass fiber includes recycled glass fiber. A resin composition comprising: A resin composition, wherein the content of the polyalkylene terephthalate resin in the resin composition is 50 to 95 parts by mass per 100 parts by mass of the total of the components excluding the glass fiber. [2] The resin composition according to [1], wherein the polyalkylene terephthalate resin contains a polybutylene terephthalate resin. [3] The resin composition according to [1] or [2], wherein the polyalkylene terephthalate resin has a terminal carboxyl group concentration of 1 eq / ton or more. [4] The resin composition according to any one of [1] to [3], wherein the resin composition contains a thermoplastic resin other than a polyester resin. [5] The resin composition according to [4], wherein the mass ratio of the polyalkylene terephthalate resin to the thermoplastic resin other than the polyester resin is 10:90 to 90:10. [6] The resin composition according to [4] or [5], wherein the thermoplastic resin other than the polyester resin comprises at least one selected from the group consisting of polyolefin resin, polyamide resin, styrene-based resin, polycarbonate resin, silicone resin, and polyarylene sulfide resin. [7] The resin composition according to any one of [4] to [6], wherein the thermoplastic resin other than the polyester resin includes a styrene-based resin and / or a polycarbonate resin. [8] The resin composition according to any one of [1] to [7], wherein the resin composition contains a flame retardant. [9] The resin composition according to [8], wherein the flame retardant comprises at least one selected from the group consisting of brominated phthalimide, brominated poly(meth)acrylate, brominated polycarbonate, brominated epoxy, and brominated polystyrene.

[10] The resin composition according to any one of [1] to [9], wherein the C glass fiber and / or the A glass fiber contains 1 mass % or more of recycled glass fiber.

[11] The resin composition according to any one of [1] to

[10] , wherein the C glass fiber and / or A glass fiber contains sodium oxide and / or potassium oxide in a total amount of 1 part by mass or more per 100 parts by mass of the C glass fiber and / or A glass fiber.

[12] The resin composition according to any one of [1] to

[11] , wherein the polyalkylene terephthalate resin comprises a polybutylene terephthalate resin, and the polyalkylene terephthalate resin has a terminal carboxyl group concentration of 1 eq / ton or more, the resin composition comprises a thermoplastic resin other than a polyester resin and / or a flame retardant, the thermoplastic resin other than a polyester resin comprises a styrene-based resin and / or a polycarbonate resin, the flame retardant comprises at least one selected from the group consisting of brominated phthalimide, brominated poly(meth)acrylate, brominated polycarbonate, brominated epoxy, and brominated polystyrene, the C-glass fiber and / or A-glass fiber contain 1 mass% or more of recycled glass fiber, and the C-glass fiber and / or A-glass fiber contain 1 mass% or more of sodium oxide and / or potassium oxide in total, per 100 mass parts of the C-glass fiber and / or A-glass fiber.

[13] Pellets of the resin composition according to any one of [1] to

[12] .

[14] A molded article molded from the resin composition according to any one of [1] to

[12] .

[15] A molded article molded from the pellets described in

[13] .

[16] A method for improving the appearance of a resin composition containing a polyalkylene terephthalate resin and at least one of C-glass fiber and / or A-glass fiber, wherein the C-glass fiber and / or A-glass fiber contains recycled glass fiber, the method comprising blending a resin other than polyester resin and / or a flame retardant.

[17] An appearance improver for a resin composition containing a polyalkylene terephthalate resin and at least one of C-glass fiber and / or A-glass fiber, wherein the C-glass fiber and / or A-glass fiber contains recycled glass fiber, and the appearance improver contains a resin other than a polyester resin and / or a flame retardant. [Effects of the Invention]

[0006] The present invention makes it possible to provide a resin composition comprising a polyalkylene terephthalate resin blended with A-glass fiber and / or C-glass fiber, which, when molded into a molded article, exhibits excellent mechanical properties and excellent appearance after a moist heat test, as well as pellets, a molded article, a method for improving appearance, and an appearance improver. DETAILED DESCRIPTION OF THE INVENTION

[0007] Hereinafter, an embodiment for carrying out the present invention (hereinafter simply referred to as "the present embodiment") will be described in detail. Note that the present embodiment is an example for explaining the present invention, and the present invention is not limited to only this embodiment. In this specification, the symbol "to" is used to mean that the numerical values ​​before and after it are included as upper and lower limits. "A to B" means that the range is A or more and B or less. In addition, any combination of the upper and lower limit values ​​of the numerical values ​​in this specification is an example of this embodiment. In this specification, various physical properties and characteristic values ​​are those at 23°C unless otherwise specified. If the measurement methods, etc. described in the standards shown in this specification change from year to year, they will be based on the standards in effect as of January 1, 2024, unless otherwise specified. If the measurement methods, etc. described in the standards shown in this specification are abolished as of January 1, 2024, they will be based on the standards in effect at the time of abolition. When a component that can be contained in the resin composition of this embodiment (such as a resin other than polyester resin or a flame retardant) corresponds to two or more components and the component is explicitly stated in this specification, it is classified as the explicitly stated component. On the other hand, when a component that can be contained in the resin composition of this embodiment and corresponds to two or more components but is not explicitly stated in this specification, it is classified as a component previously described in this specification.

[0008] The resin composition of the present embodiment is a resin composition containing a polyalkylene terephthalate resin and at least one of C-glass fiber and / or A-glass fiber, wherein the C-glass fiber and / or A-glass fiber contains recycled glass fiber, and is characterized in that the content of the polyalkylene terephthalate resin in the resin composition is 50 to 95 parts by mass per 100 parts by mass of the total of all components excluding the glass fiber. By adopting such a constitution, it is possible to provide a resin composition which, when molded into a molded article, has excellent mechanical properties and appearance after a moist heat test. That is, because C-glass fiber and / or A-glass fiber contain a large amount of alkaline components, it was speculated that when they are blended with a polyalkylene terephthalate resin to form a molded article, the carboxylic acid terminals of the polyalkylene terephthalate resin react with the alkaline components contained in the C-glass fiber and / or A-glass fiber during wet heat treatment, resulting in the precipitation of alkali metal salts. It was also speculated that these alkali metal salts adhere to the surface of the molded article as powder, resulting in a poor appearance of the molded article. Under these circumstances, the resin composition of the present embodiment is formulated with components other than the polyalkylene terephthalate resin (for example, a resin other than polyester resin or a flame retardant). By formulating components other than the polyalkylene terephthalate resin, the proportion of the polyalkylene terephthalate resin in the resin composition becomes relatively small, and it is presumed that this makes it possible to suppress the precipitation of powdery matter. On the other hand, if components other than the polyalkylene terephthalate resin are blended and the blending amount of the polyalkylene terephthalate resin is too small, the inherent advantages of the polyalkylene terephthalate resin, such as strength and heat resistance, are reduced, and the mechanical properties of the resulting molded product are deteriorated. Therefore, in this embodiment, it has been found that the above problem can be solved by precisely adjusting the proportion of the polyalkylene terephthalate resin in the resin composition.

[0009] In particular, in this embodiment, it is preferable that the component other than the polyalkylene terephthalate resin and the C-glass fiber and / or the A-glass fiber contains at least one selected from the group consisting of amorphous resins such as styrene-based resins and polycarbonate resins, fillers such as epoxy compounds, elastomers, and talc, and brominated flame retardants, because even if the blending amount of these components is large, they are unlikely to adversely affect the mechanical properties of the resulting molded article.

[0010] Hereinafter, the embodiments of the present invention will be described in detail. However, the explanation of the constituent elements described below is an example of an embodiment of the present invention, and the present invention is not limited to these contents.

[0011] <Polyalkylene terephthalate resin> The resin composition of the present embodiment contains a polyalkylene terephthalate resin. In this embodiment, the polyalkylene terephthalate resin preferably contains a polyethylene terephthalate resin and / or a polybutylene terephthalate resin, and more preferably contains at least a polybutylene terephthalate resin.

[0012] More specifically, the polyalkylene terephthalate resin is a polyester obtained by polycondensation of terephthalic acid as a dicarboxylic acid compound and a diol, and may be either a homopolyester or a copolyester.

[0013] As the dicarboxylic acid compound constituting the polyalkylene terephthalate resin, a terphthalic acid compound or an ester-forming derivative thereof is preferably used. Aromatic dicarboxylic acids other than terephthalic acid can also be used in combination. Examples include isophthalic acid, orthophthalic acid, 1,5-naphthalenedicarboxylic acid, 2,5-naphthalenedicarboxylic acid, 2,6-naphthalenedicarboxylic acid, biphenyl-2,2'-dicarboxylic acid, biphenyl-3,3'-dicarboxylic acid, biphenyl-4,4'-dicarboxylic acid, diphenylether-4,4'-dicarboxylic acid, diphenylmethane-4,4'-dicarboxylic acid, diphenylsulfone-4,4'-dicarboxylic acid, diphenylisopropylidene-4,4'-dicarboxylic acid, 1,2-bis(phenoxy)ethane-4,4'-dicarboxylic acid, anthracene-2,5-dicarboxylic acid, anthracene-2,6-dicarboxylic acid, p-terphenylene-4,4'-dicarboxylic acid, and pyridine-2,5-dicarboxylic acid. These can be used in the polycondensation reaction as ester-forming derivatives such as dimethyl esters in addition to free acids. Of the above, isophthalic acid or its ester-forming derivatives are particularly preferred.

[0014] In addition, a small amount of terephthalic acid or the above-mentioned aromatic dicarboxylic acid may be used in combination with one or more aliphatic dicarboxylic acids such as adipic acid, azelaic acid, dodecanedioic acid, and sebacic acid, or alicyclic dicarboxylic acids such as 1,2-cyclohexanedicarboxylic acid, 1,3-cyclohexanedicarboxylic acid, and 1,4-cyclohexanedicarboxylic acid.

[0015] Examples of dihydroxy compounds constituting the polyalkylene terephthalate resin include aliphatic diols such as ethylene glycol, propylene glycol, butanediol, hexylene glycol, neopentyl glycol, 2-methylpropane-1,3-diol, diethylene glycol, and triethylene glycol, alicyclic diols such as cyclohexane-1,4-dimethanol, and mixtures thereof. Among these, butanediol and ethylene glycol are particularly preferred.

[0016] It is also possible to copolymerize one or more long-chain diols having a molecular weight of 400 to 6,000, such as polyethylene glycol, poly-1,3-propylene glycol, polytetramethylene glycol, etc. Also usable are aromatic diols such as hydroquinone, resorcinol, naphthalenediol, dihydroxydiphenyl ether, and 2,2-bis(4-hydroxyphenyl)propane.

[0017] In addition to the above-mentioned bifunctional monomers, a small amount of a trifunctional monomer such as trimellitic acid, trimesic acid, pyromellitic acid, pentaerythritol, or trimethylolpropane can be used in combination to introduce a branched structure, or a monofunctional compound such as a fatty acid can be used in combination to adjust the molecular weight.

[0018] The polyalkylene terephthalate resin is preferably one formed by polycondensation of terephthalic acid and a diol, i.e., one in which the polycondensate accounts for more than 50% by mass of the entire resin, preferably 70% by mass or more, more preferably 80% by mass or more, even more preferably 90% by mass or more, still more preferably 95% by mass or more, and even more preferably 99% by mass or more. The diol is preferably an aliphatic diol, preferably 1,4-butanediol or ethylene glycol, and more preferably 1,4-butanediol.

[0019] The amount of terminal carboxyl groups in the polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) may be appropriately selected and determined, but is typically 80 eq / ton or less, preferably 50 eq / ton or less, more preferably 30 eq / ton or less, even more preferably 20 eq / ton or less, and even more preferably 15 eq / ton or less. By setting the amount below the upper limit, the hydrolysis resistance of the resin composition tends to be improved. There is no particular lower limit for the amount of terminal carboxyl groups, but it is preferably 1 eq / ton or more, more preferably 5 eq / ton or more, and even more preferably typically 10 eq / ton or more.

[0020] The amount of terminal carboxyl groups in a polyalkylene terephthalate resin is determined by dissolving 0.5 g of the resin in 25 mL of benzyl alcohol and titrating the solution with a 0.01 mol / L benzyl alcohol solution of sodium hydroxide. The amount of terminal carboxyl groups can be adjusted by any conventional method, such as adjusting the polymerization conditions, such as the raw material charge ratio, polymerization temperature, and pressure reduction, or by reacting a terminal blocking agent.

[0021] The intrinsic viscosity of the polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) is preferably 0.50 dL / g or more, more preferably 0.60 dL / g or more, even more preferably 0.70 dL / g or more, even more preferably 0.80 dL / g or more, even more preferably 0.85 dL / g or more, and even more preferably 0.90 dL / g or more. By setting the intrinsic viscosity at or above the lower limit, deterioration of physical properties such as strength tends to be effectively suppressed. Furthermore, the intrinsic viscosity of the polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) is preferably 1.30 dL / g or less, more preferably 1.15 dL / g or less. By setting the intrinsic viscosity at or below the upper limit, deterioration of the fluidity of the resin composition tends to be effectively suppressed.

[0022] The intrinsic viscosity is measured by the following method. Polyalkylene terephthalate resin pellets are dissolved in a phenol / 1,1,2,2-tetrachloroethane (1 / 1 mass ratio) mixed solvent by stirring at 110°C for 1 hour to a concentration of 1.00 g / dL. The solution is then cooled to 30°C. Using a fully automatic solution viscometer, the time it takes for the sample solution and the solvent alone to fall at 30°C is measured, and the intrinsic viscosity is calculated using the formula: Intrinsic viscosity=((1+4K H η sp ) 0.5 -1) / (2K H C) where η sp=η / η0-1, where η is the time it takes for the sample solution to fall, η0 is the time it takes for the solvent alone to fall, C is the concentration of the sample solution (g / dL), and K H is Huggins' constant. K H was set to 0.33. The fully automatic solution viscometer used is manufactured by Shibayama Scientific Co., Ltd. When the resin composition of the present embodiment contains two or more polyalkylene terephthalate resins, the intrinsic viscosity is the intrinsic viscosity of the mixture.

[0023] Preferred polyalkylene terephthalate resins are those in which 95 mol % or more of the acid component is terephthalic acid and 95 mol % or more of the alcohol component is an aliphatic diol, and representative examples thereof are polybutylene terephthalate resin and polyethylene terephthalate resin. These are preferably similar to homopolyesters, i.e., 95 mol % or more of the resin as a whole is composed of terephthalic acid and 1,4-butanediol or ethylene glycol components. The polyalkylene terephthalate resin is preferably a polybutylene terephthalate resin and / or a polyethylene terephthalate resin. Among these, the polyalkylene terephthalate resin preferably contains polybutylene terephthalate resin as a main component, and more than 50% by mass of the polyalkylene terephthalate resin is preferably polybutylene terephthalate resin. In this case, it is also preferable that the polyalkylene terephthalate resin contains less than 50% by mass of polyethylene terephthalate resin.

[0024] Polybutylene terephthalate resin can be produced by batch or continuous melt polymerization of a dicarboxylic acid component containing terephthalic acid as the main component or an ester derivative thereof with a diol component containing 1,4-butanediol as the main component. After producing a low-molecular-weight polybutylene terephthalate resin by melt polymerization, the degree of polymerization (or molecular weight) can be increased to a desired value by further solid-state polymerization under a nitrogen gas flow or reduced pressure.

[0025] The polybutylene terephthalate resin is preferably produced by a continuous melt polycondensation method of a dicarboxylic acid component mainly composed of terephthalic acid and a diol component mainly composed of 1,4-butanediol.

[0026] The catalyst used in carrying out the esterification reaction may be a conventionally known catalyst, such as a titanium compound, a tin compound, a magnesium compound, or a calcium compound. Among these, titanium compounds are particularly preferred. Specific examples of titanium compounds used as esterification catalysts include titanium alcoholates such as tetramethyl titanate, tetraisopropyl titanate, and tetrabutyl titanate, and titanium phenolates such as tetraphenyl titanate.

[0027] The polybutylene terephthalate resin may be a polybutylene terephthalate resin modified by copolymerization (hereinafter, also referred to as a "modified polybutylene terephthalate resin"), and specific preferred copolymers thereof include polyester ether resins copolymerized with polyalkylene glycols (particularly polytetramethylene glycol), dimer acid copolymerized polybutylene terephthalate resins, and isophthalic acid copolymerized polybutylene terephthalate resins.

[0028] When a polyester ether resin copolymerized with polytetramethylene glycol is used as the modified polybutylene terephthalate resin, the proportion of the tetramethylene glycol component in the copolymer is preferably 3 to 40 mass%, more preferably 5 to 30 mass%, and even more preferably 10 to 25 mass%. When a dimer acid copolymerized polybutylene terephthalate resin is used as the modified polybutylene terephthalate resin, the proportion of the dimer acid component in all carboxylic acid components is preferably 0.5 to 30 mol %, more preferably 1 to 20 mol %, and even more preferably 3 to 15 mol %, in terms of carboxylic acid groups. When using an isophthalic acid copolymerized polybutylene terephthalate resin as the modified polybutylene terephthalate resin, the proportion of the isophthalic acid component in all carboxylic acid components is preferably 1 to 30 mol% as carboxylic acid groups, more preferably 1 to 20 mol%, and even more preferably 3 to 15 mol%. Among the modified polybutylene terephthalate resins, polyester ether resins copolymerized with polytetramethylene glycol and isophthalic acid copolymerized polybutylene terephthalate resins are preferred.

[0029] The content of the polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) in the resin composition of the present embodiment is 50 parts by mass or more, preferably 55 parts by mass or more, based on 100 parts by mass of the total of the components excluding glass fibers, and also 95 parts by mass or less, preferably 90 parts by mass or less, more preferably 85 parts by mass or less, even more preferably 79 parts by mass or less, still more preferably 75 parts by mass or less, and even more preferably 70 parts by mass or less. By setting it to be not less than the lower limit value, the mechanical properties of the obtained molded product can be further improved, and by setting it to be not more than the upper limit value, the appearance of the obtained molded product is excellent. The resin composition of the present embodiment may contain only one kind of polyalkylene terephthalate resin (preferably polybutylene terephthalate resin), or may contain two or more kinds. When containing two or more kinds, the total amount is preferably within the above range.

[0030] <C glass fiber and / or A glass fiber> The resin composition of the present embodiment contains C glass fiber and / or A glass fiber, and the C glass fiber and / or A glass fiber contains recycled glass fiber. C-glass fiber and / or A-glass fiber are glass fibers that contain more alkali metal components (usually sodium oxide and / or potassium oxide) than E-glass fiber, and preferably contain 1 part by mass or more (preferably 2 parts by mass or more, more preferably 5 parts by mass or more, and preferably 20 parts by mass or less) of sodium oxide and / or potassium oxide per 100 parts by mass of the C-glass fiber and / or A-glass fiber. In this embodiment, even when such glass fibers are used, the appearance of the molded product obtained can be made good.

[0031] The recycled C-glass fiber and / or A-glass fiber may be recycled glass fiber, preferably mechanically recycled glass fiber. A-glass is the most widely used glass and is an excellent recycled resource. Recycled glass fiber is contrasted with virgin glass fiber, and includes glass fiber that has been put on the market, as well as defective products and scraps that are produced during the manufacturing of glass fiber. In the resin composition of this embodiment, the recycled glass fiber is preferably contained in an amount of 1% by mass or more, alternatively 10% by mass or more, 30% by mass or more, 50% by mass or more, 70% by mass or more, or 90% by mass or more, relative to 100% by mass of the total amount of C glass fiber and A glass fiber contained in the resin composition.

[0032] The C glass fiber and / or A glass fiber preferably has a number-average fiber length of 0.5 to 10 mm, more preferably 1 to 5 mm. The use of glass fibers with such a number-average fiber length can further improve mechanical strength. The number-average fiber length is calculated from the measured values ​​obtained by randomly selecting glass fibers to be measured for fiber length from an image obtained by observation with an optical microscope and measuring the long sides of the fibers. The observation is performed at a magnification of 20x, and the number of fibers measured is 1,000 or more. This roughly corresponds to the cut length. The cross section of the C glass fiber and / or A glass fiber may be any shape, such as a circle, an ellipse, an oval, a rectangle, a rectangle with semicircles on both short sides, or a cocoon shape, but a circle is preferred. Here, the circle includes not only a circle in the geometric sense but also what is generally called a circle in the technical field of this embodiment. The number-average fiber diameter of the C-glass fiber and / or A-glass fiber is preferably 4.0 μm or more, more preferably 4.5 μm or more, and even more preferably 5.0 μm or more. The upper limit of the number-average fiber diameter of the glass fiber is preferably 15.0 μm or less, more preferably 14.0 μm or less. The use of glass fibers having a number-average fiber diameter within this range tends to produce molded products with superior mechanical strength. The number-average fiber diameter of the glass fiber is calculated from the measured values ​​obtained by randomly selecting glass fibers to be measured for fiber diameter from an image obtained by observation with an electron microscope, measuring the fiber diameter near the center, and then measuring the measured fiber diameter. The observation is performed at a magnification of 1,000x, and the number of fibers measured is 1,000 or more. The number-average fiber diameter of glass fibers having a cross section other than a circle is the number-average fiber diameter when converted into a circle with the same area as the cross section. The glass fibers used in this embodiment may be treated with a surface treatment agent or a sizing agent. When the glass fibers are treated with a surface treatment agent or a sizing agent, the content of the surface treatment agent and the sizing agent is preferably 0.01 to 1% by mass of the glass fibers.

[0033] In this embodiment, the total content of C glass fiber and / or A glass fiber in the resin composition is preferably 1% by mass or more, more preferably 3% by mass or more, even more preferably 5% by mass or more, even more preferably 7% by mass or more, still more preferably 10% by mass or more, and is preferably 40% by mass or less, more preferably 35% by mass or less, even more preferably 30% by mass or less, still more preferably 25% by mass or less, and still more preferably 20% by mass or less. By setting the content at or above the lower limit, mechanical properties tend to be further improved. Meanwhile, by setting the content at or below the upper limit, the effect of suppressing poor appearance after moist heat resistance tends to be further improved. The resin composition of the present embodiment may contain only one type of C glass fiber and / or A glass fiber, or may contain two or more types. When two or more types are contained, the total amount is preferably in the above range.

[0034] The resin composition of the present embodiment may or may not contain glass fibers other than the C glass fibers and the A glass fibers. The resin composition of this embodiment may be configured to be substantially free of glass fibers other than C-glass fiber and A-glass fiber. "Substantially free of glass fibers other than C-glass fiber and A-glass fiber" means that the content of glass fibers other than C-glass fiber and A-glass fiber in the resin composition of this embodiment is less than 10% by mass of the resin composition, preferably less than 5% by mass, and more preferably less than 1% by mass. The resin composition of the present embodiment may or may not contain virgin glass fibers. The resin composition of this embodiment may be configured to be substantially free of virgin glass fibers. "Substantially free of virgin glass fibers" means that the content of virgin glass fibers in the resin composition of this embodiment is less than 5% by mass, preferably less than 3% by mass, and more preferably less than 1% by mass.

[0035] In particular, the resin composition of this embodiment may or may not contain E-glass fibers. The E-glass fiber may be virgin glass fiber or recycled glass fiber. Furthermore, when the resin composition of the present embodiment contains E glass fiber, the amount is preferably 1 to 50 parts by mass, and more preferably 1 to 30 parts by mass, per 100 parts by mass of the total amount of glass fiber and / or A glass fiber contained in the resin composition. The resin composition of this embodiment may be configured to be substantially free of E-glass fibers. "Substantially free of E-glass fibers" means that the content of E-glass fibers in the resin composition of this embodiment is less than 10% by mass, preferably less than 5% by mass, and more preferably less than 1% by mass.

[0036] <Resins other than polyester resins> The resin composition of the present embodiment preferably contains a resin other than a polyester resin. By including a resin other than a polyester resin, it tends to be possible to relatively suppress the reaction of terephthalic acid at the terminal of the polyalkylene terephthalate resin with an alkali, resulting in the precipitation of powdery matter. The resin other than the polyester resin may be either a thermoplastic resin or a thermosetting resin, but a thermoplastic resin is preferred. Furthermore, it is also preferable that the resin other than the polyester resin contains both a thermoplastic resin and a thermosetting resin (for example, an epoxy compound).

[0037] The thermoplastic resin preferably contains at least one selected from the group consisting of polyolefin resin, polyamide resin, styrene-based resin, polycarbonate resin, silicone resin, and polyarylene sulfide resin, more preferably contains a styrene-based resin and / or a polycarbonate resin, even more preferably contains a styrene-based resin, and still more preferably contains an acrylonitrile styrene resin. Examples of thermosetting resins include epoxy compounds, oxetane compounds, phenol compounds, polyurethane compounds and melamine compounds, with epoxy compounds being preferred.

[0038] <<Polyolefin resin>> The polyolefin used in this embodiment is not particularly limited, and any known polyolefin can be used. The polyolefin resin is preferably a linear or branched polyolefin resin such as a homopolymer and / or copolymer of ethylene, propylene, butene, norbornene, etc., and examples thereof include polyethylene, polypropylene, ethylene-propylene-butene copolymer, ethylene-propylene copolymer, ethylene-butene copolymer, and propylene-butene copolymer. The polyolefin resin may also be a cyclopolyolefin such as a cycloolefin polymer (COP) or a cycloolefin copolymer (COC).

[0039] <<Polyamide resin>> The polyamide resin used in this embodiment is not particularly limited, and any known polyamide resin can be used. The polyamide resin may be an aliphatic polyamide resin or a semi-aromatic polyamide resin, and an aliphatic polyamide resin is preferred. Examples of aliphatic polyamide resins include polyamide 4, polyamide 46, polyamide 6, polyamide 66, polyamide 666, polyamide 610, polyamide 11, polyamide 12, and the like. Examples of semi-aromatic polyamide resins include terephthalic acid-based polyamide resins (polyamide 6T, polyamide 9T), xylylenediamine-based polyamide resins (MXD6, etc.), and the like.

[0040] <<Styrene-based resin>> The styrene-based resin used in this embodiment is not particularly limited, and any known styrene-based resin can be used. The styrene-based resin may be a polymer of a styrene-based monomer, or may be a resin obtained by polymerizing a styrene-based monomer and, if necessary, one or more other vinyl monomers copolymerizable therewith.

[0041] Examples of the styrene-based monomer include styrene, α-methylstyrene, o-methylstyrene, p-methylstyrene, vinylxylene, ethylstyrene, dimethylstyrene, p-tert-butylstyrene, vinylnaphthalene, and other styrene derivatives, with styrene being particularly preferred. These may be used alone or in combination of two or more.

[0042] Other vinyl monomers copolymerizable with styrene-based monomers include α,β-unsaturated carboxylic acids and their anhydrides, such as acrylic acid, methacrylic acid, maleic acid, maleic anhydride, phthalic acid, and itaconic acid; methacrylic acid alkyl esters, such as methyl methacrylate, ethyl methacrylate, propyl methacrylate, butyl methacrylate, amyl methacrylate, hexyl methacrylate, 2-ethylhexyl methacrylate, octyl methacrylate, cyclohexyl methacrylate, and dodecyl methacrylate; methyl acrylate, ethyl acrylate, and the like. Examples of the acrylic acid ester include alkyl esters of acrylic acid such as butyl acrylate, propyl acrylate, butyl acrylate, amyl acrylate, hexyl acrylate, 2-ethylhexyl acrylate, octyl acrylate, cyclohexyl acrylate, and dodecyl acrylate; aryl esters of acrylic acid such as phenyl acrylate and benzyl acrylate; aryl methacrylate esters such as phenyl methacrylate and benzyl methacrylate; maleimide-based monomers such as maleimide, N-methylmaleimide, and N-phenylmaleimide; and acrylonitrile.

[0043] As the styrene-based resin, a copolymer of a styrene-based monomer and an acrylonitrile monomer (acrylonitrile-styrene resin) is preferred. In the acrylonitrile-styrene resin, the proportion of styrene-based monomers in the total of 100% by mass of the monomers constituting the resin is preferably 20% by mass or more, more preferably 30% by mass or more, and is preferably 90% by mass or less, more preferably 80% by mass or less, and even more preferably 70% by mass or less. The acrylonitrile-styrene resin may be a copolymer of a styrene-based monomer, acrylonitrile, and another monomer copolymerizable with either of them. The proportion of the other monomer is preferably 30% by mass or less, more preferably 20% by mass or less, even more preferably 10% by mass or less, particularly preferably 5% by mass or less, 3% by mass or less, 2% by mass or less, and particularly preferably 1% by mass or less, based on 100% by mass of the total monomers constituting the acrylonitrile-styrene resin. There are no limitations on the method for producing the acrylonitrile-styrene resin, and known methods can be used, such as bulk polymerization, emulsion polymerization, solution polymerization, and suspension polymerization.

[0044] <<Polycarbonate resin>> The polycarbonate resin used in this embodiment may be a known polycarbonate resin. Polycarbonate resins are thermoplastic polymers or copolymers which may be branched and are obtained by reacting a dihydroxy compound or a small amount of a polyhydroxy compound with phosgene or a carbonate diester. The method for producing the polycarbonate resin is not particularly limited, and polycarbonate resins produced by the conventionally known phosgene method (interfacial polymerization method) or melt method (ester interchange method) can be used.

[0045] The dihydroxy compound used as the raw material is preferably an aromatic dihydroxy compound, such as 2,2-bis(4-hydroxyphenyl)propane (i.e., bisphenol A), 2,2-bis(3-methyl-4-hydroxyphenyl)propane (i.e., bisphenol C), tetramethylbisphenol A, bis(4-hydroxyphenyl)-p-diisopropylbenzene, hydroquinone, resorcinol, or 4,4-dihydroxydiphenyl, with bisphenol A and / or bisphenol C being preferred. It is also possible to use compounds in which one or more tetraalkylphosphonium sulfonates are bonded to the above aromatic dihydroxy compounds.

[0046] Among the polycarbonate resins mentioned above, aromatic polycarbonate resins derived from bisphenol A and / or bisphenol C, or aromatic polycarbonate copolymers derived from bisphenol A and / or bisphenol C and other aromatic dihydroxy compounds are preferred. The polycarbonate resin may also be a copolymer, such as a copolymer with a polymer or oligomer having a siloxane structure. Furthermore, two or more of the above polycarbonate resins may be mixed and used.

[0047] <<Silicone resin>> The silicone resin used in this embodiment is not particularly limited, and any known silicone resin can be used. The silicone resin is preferably a resin having a repeating unit of -Si(R)2-O- (wherein R is a hydrogen atom, a hydrocarbon group, an -O-hydrocarbon group, or -OH). R is preferably a hydrogen atom or a hydrocarbon group, more preferably a hydrogen atom, a methyl group, or a phenyl group.

[0048] <<Polyarylene sulfide resin>> The polyarylene sulfide (PAS) resin used in this embodiment is not particularly limited, and any known polyarylene sulfide (PAS) resin can be used. Polyarylene sulfide (PAS) resin is a polymer compound whose main structural unit is an arylene sulfide group (-Ar-S-). PAS resins may be homopolymers consisting of only one type of structural unit, or copolymers containing multiple types of structural units. "Ar" represents an arylene group.

[0049] Examples of the arylene group include an o-phenylene group, an m-phenylene group, a p-phenylene group, a substituted phenylene group, an m-phenylene sulfide group, a p-phenylene sulfide group, a p,p'-diphenylene sulfone group, a p,p'-biphenylene group, a p,p'-diphenylene ether group, a p,p'-diphenylene carbonyl group, and a naphthalene group.

[0050] The constituent unit of the homopolymer is not particularly limited, but it is preferable that the arylene group has a p-phenylene sulfide group as a constituent unit.

[0051] The copolymer is preferably composed of monomers having different arylene groups. In particular, the copolymer is preferably a combination of a monomer having an m-phenylene sulfide group and a monomer having a p-phenylene sulfide group. The copolymer preferably contains p-phenylene sulfide groups at a ratio of 70 mol % or more, and more preferably contains p-phenylene sulfide groups at a ratio of 80 mol % or more. By containing p-phenylene sulfide groups at a ratio of 70 mol % or more, the heat resistance, moldability, mechanical properties, etc. of the copolymer can be improved. The polyarylene sulfide resin is preferably a polyphenylene sulfide resin.

[0052] The mass ratio of the polyalkylene terephthalate resin to the thermoplastic resin other than the polyester resin in the resin composition of this embodiment is preferably 10:90 to 90:10. Furthermore, the proportion of the polyalkylene terephthalate resin relative to 100 parts by mass of the total of the polyalkylene terephthalate resin and the thermoplastic resin is preferably 10 parts by mass or more, preferably 20 parts by mass or more, more preferably 30 parts by mass or more, more preferably 40 parts by mass or more, even more preferably 50 parts by mass or more, still more preferably 60 parts by mass or more, and preferably 90 parts by mass or less, more preferably 80 parts by mass or less, and still more preferably 70 parts by mass or less. The resin composition of the present embodiment may contain only one thermoplastic resin other than polyester resin, or may contain two or more thermoplastic resins. When two or more thermoplastic resins are contained, the total amount is preferably in the above range.

[0053] <<Epoxy compounds>> The resin composition of the present embodiment may contain an epoxy compound. By containing an epoxy compound, the hydrolysis resistance of the resulting molded article tends to be improved. The epoxy compound may be a monofunctional epoxy compound or a polyfunctional epoxy compound, but a polyfunctional epoxy compound is preferred. Examples of polyfunctional epoxy compounds include bisphenol A epoxy compounds, bisphenol F epoxy compounds, resorcinol epoxy compounds, novolac epoxy compounds, alicyclic compound diepoxy compounds, glycidyl ethers, and epoxidized polybutadienes. More specifically, alicyclic compound epoxy compounds such as bisphenol A epoxy compounds, bisphenol F epoxy compounds, resorcinol epoxy compounds, novolac epoxy compounds, vinylcyclohexene dioxide, and dicyclopentadiene oxide can all be preferably used. Among these, bisphenol A epoxy compounds and novolac epoxy compounds are more preferred. The epoxy compound may also be a copolymer containing a glycidyl group-containing compound as a constituent component, such as a copolymer of a glycidyl ester of an α,β-unsaturated acid with one or more monomers selected from the group consisting of an α-olefin, acrylic acid, an acrylic acid ester, methacrylic acid, a methacrylic acid ester, and styrene. Furthermore, the epoxy compound is preferably a copolymer of an epoxy group-containing monomer and a styrene-based monomer, and may also be a copolymer with other copolymerizable monomers. Examples of the styrene-based monomer constituting the copolymer of an epoxy group-containing monomer and a styrene-based monomer include glycidyl (meth)acrylate and glycidyl itaconate, with glycidyl methacrylate and glycidyl acrylate being preferred, and glycidyl methacrylate being particularly preferred. Examples of the styrene-based monomer include styrene, α-methylstyrene, p-methylstyrene, vinylxylene, ethylstyrene, dimethylstyrene, p-tert-butylstyrene, vinylnaphthalene, methoxystyrene, monobromostyrene, dibromostyrene, fluorostyrene, and tribromostyrene, with styrene and α-methylstyrene being more preferred, and styrene being particularly preferred. Specific examples of copolymers of epoxy group-containing monomers and styrene-based monomers include glycidyl (meth)acrylate-styrene copolymers and glycidyl (meth)acrylate-styrene-methyl (meth)acrylate, which tend to improve adhesion to epoxy-based adhesives and are therefore particularly preferred.

[0054] The epoxy equivalent of the epoxy compound used in this embodiment is preferably 100 g / eq or more, more preferably 150 g / eq or more, and is preferably 1000 g / eq or less, more preferably 300 g / eq or less, and even more preferably 250 g / eq or less. When the resin composition of the present embodiment contains two or more epoxy compounds, the epoxy equivalent is the value (weighted average value) obtained by multiplying the epoxy equivalent of each epoxy compound by the mass fraction of each epoxy compound.

[0055] In addition to the above, the epoxy compounds can be found in paragraphs 0038 to 0050 of JP-A-2020-199755 and paragraph 0043 of JP-A-2020-125468, the contents of which are incorporated herein by reference.

[0056] The epoxy compound used in this embodiment may be an epoxidized fatty acid ester. The use of an epoxidized fatty acid ester effectively suppresses thickening of the resin composition, and furthermore, allows a significantly high strength retention rate to be achieved even after a moist heat treatment test. This is presumably because the epoxy groups in the epoxidized fatty acid ester are unevenly distributed in the side chains, making them less reactive than terminal epoxy groups. Epoxidized fatty acid esters are compounds obtained by epoxidizing fatty acid esters. The fatty acid ester is preferably a fatty acid ester having one or more (preferably 2 to 10) unsaturated bonds in the molecule. The fatty acid ester is preferably an epoxidized natural fat or oil. As the epoxidized natural oil or fat, epoxidized animal oil or epoxidized vegetable oil or fat can be used. Examples of animal fats and oils include beef tallow, lard, chicken fat, milk fat, and fish oil. Examples of vegetable fats and oils include soybean oil, rapeseed oil, linseed oil, corn oil, palm oil, sunflower oil, grape oil, cottonseed oil, sesame oil, rice bran oil, peanut oil, castor oil, tung oil, safflower oil, olive oil, and grapeseed oil. At least one selected from the group consisting of soybean oil, rapeseed oil, linseed oil, corn oil, and palm oil is preferred, soybean oil and / or linseed oil is more preferred, and linseed oil is even more preferred.

[0057] For details of the epoxidized fatty acid ester, in addition to the above, the descriptions in paragraphs 0046 to 0070 of JP-A-2019-026727 and the descriptions in paragraphs 0016 to 0025 of JP-A-2023-136871 can be referred to, the contents of which are incorporated herein by reference. Commercially available epoxidized fatty acid esters can also be used. For example, Chemicizer SE-100 (epoxidized soybean oil, ESBO, general-purpose grade), Chemicizer SE-100ST (epoxidized soybean oil, high-grade), and Chemicizer ELS-100 (epoxidized linseed oil), all manufactured by Sanwa Synthetic Chemical Industry Co., Ltd.; and Sanso Cizer E-2000H (epoxidized soybean oil), Sanso Cizer E-9000H (epoxidized linseed oil), all manufactured by Shin-Nihon Rikagaku Co., Ltd. Examples of such epoxidized fatty acids include SANSO CIZER E-4030 (epoxidized fatty acid isobutyl ester), SANSO CIZER E-6000 (epoxidized fatty acid 2-ethylhexyl ester), manufactured by ADEKA Corporation, ADEKA CIZER O-130P (epoxidized soybean oil), ADEKA CIZER O-180A (epoxidized linseed oil), ADEKA CIZER D-32 (epoxidized fatty acid octyl ester), and ADEKA CIZER D-55 (epoxidized fatty acid alkyl ester).

[0058] When the resin composition of this embodiment contains a thermosetting resin (preferably an epoxy compound), the content thereof is preferably 0.01 parts by mass or more, and more preferably 0.05 parts by mass or more, relative to 100 parts by mass of the polyalkylene terephthalate resin. The upper limit of the content of the epoxy compound is preferably 15 parts by mass or less, more preferably 10 parts by mass or less, even more preferably 7.0 parts by mass or less, and even more preferably 2.0 parts by mass or less, relative to 100 parts by mass of the polyalkylene terephthalate resin. The resin composition of the present embodiment may contain only one type of thermosetting resin (preferably an epoxy compound), or may contain two or more types. When two or more types are contained, the total amount is preferably in the above range.

[0059] <Stabilizer> The resin composition of the present embodiment may contain a stabilizer (a light stabilizer and / or a heat stabilizer). The stabilizer preferably contains one or more compounds selected from the group consisting of thioether compounds, hindered phenol compounds, and phosphite compounds, and more preferably a hindered phenol compound. In this embodiment, it is also preferable to use two or more of the thioether-based compounds, hindered phenol-based compounds, and phosphite-based compounds in combination as needed.

[0060] The thioether-based compound may be any conventionally known sulfur-containing compound, and among these, thioethers are preferred. By including the thioether-based compound in the resin composition of the present embodiment, the appearance of the molded article tends to be improved and the thermal stability tends to be improved. Specific examples include didodecylthiodipropionate, ditetradecylthiodipropionate, dioctadecylthiodipropionate, pentaerythritol tetrakis(3-dodecylthiopropionate), 2,2-bis{[3-(dodecylthio)-1-oxopropoxy]methyl}propane-1,3-diylbis[3-(dodecylthio)propionate], thiobis(N-phenyl-β-naphthylamine), 2-mercaptobenzothiazole, 2-mercaptobenzimidazole, tetramethylthiuram monosulfide, tetramethylthiuram disulfide, nickel dibutyldithiocarbamate, nickel isopropyl xanthate, and trilauryl trithiophosphite. Among these, 2,2-bis{[3-(dodecylthio)-1-oxopropoxy]methyl}propane-1,3-diylbis[3-(dodecylthio)propionate] is preferred. Commercially available products include Shipro Chemicals' product name "Seenox 412S" and ADEKA's product name "Adekastab AO-412S."

[0061] Examples of hindered phenol compounds include pentaerythritol tetrakis(3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate), octadecyl-3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate, thiodiethylenebis(3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate), pentaerythritol tetrakis(3-(3,5-di-neopentyl-4-hydroxyphenyl)propionate), and 1,3,5-trimethyl-2,4,6-tris(3,5-di-tert-butyl-4-hydroxybenzyl)benzene. Among these, pentaerythritol tetrakis(3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate) and octadecyl-3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate are preferred. Commercially available products include those manufactured by ADEKA under the trade names "ADK STAB AO-60" and "ADK STAB AO-330," and those manufactured by BASF under the trade name "IRGANOX NOX 1010."

[0062] The phosphite compound is preferably a compound represented by the formula: R 2 OP(OR 3 )(OR 4 ) (In the formula, R 2 , R 3 and R 4 are each a hydrogen atom, an alkyl group having 1 to 30 carbon atoms, or an aryl group having 6 to 30 carbon atoms, and R 2 , R 3 and R 4 At least one of the groups is an aryl group having 6 to 30 carbon atoms.) Examples of the compound include compounds represented by the following formula: Examples of the phosphite compound include triphenyl phosphite, tris(nonylphenyl) phosphite, dilauryl hydrogen phosphite, triethyl phosphite, tridecyl phosphite, tris(2-ethylhexyl) phosphite, tris(tridecyl) phosphite, tristearyl phosphite, diphenyl monodecyl phosphite, monophenyl didecyl phosphite, diphenyl mono(tridecyl) phosphite, tetraphenyl dipropylene glycol diphosphite, tetraphenyl tetra(tridecyl) pentaerythritol tetraphosphite, hydrogenated bisphenol A phenol phosphite polymer, diphenyl hydrogen phosphite, 4,4'-butylidene-bis(3-methyl-6-tert-butylphenyl di(tridecyl) phosphite), tetra(tridecyl) 4,4'-isopropyl phosphate, tetra(tridecyl) ... propylidenediphenyl diphosphite, bis(tridecyl)pentaerythritol diphosphite, bis(nonylphenyl)pentaerythritol diphosphite, dilauryl pentaerythritol diphosphite, distearyl pentaerythritol diphosphite, tris(4-tert-butylphenyl)phosphite, tris(2,4-di-tert-butylphenyl)phosphite, hydrogenated bisphenol A pentaerythritol phosphite polymer, bis(2,4-di-tert-butylphenyl)pentaerythritol diphosphite, bis(2,6-di-tert-butyl-4-methylphenyl)pentaerythritol diphosphite, 2,2'-methylenebis(4,6-di-tert-butylphenyl)octyl phosphite, bis(2,4-dicumylphenyl)pentaerythritol diphosphite, and the like. Among these, bis(2,6-di-tert-butyl-4-methylphenyl)pentaerythritol diphosphite is preferred. An example of a commercially available product is "ADEKA STAB PEP-36" manufactured by ADEKA Corporation.

[0063] Other examples of stabilizers include the descriptions in paragraphs 0067 to 0075 of JP 2021-063196 A, paragraphs 0046 to 0057 of JP 2018-070722 A, paragraphs 0030 to 0037 of JP 2019-056035 A, and paragraphs 0066 to 0078 of WO 2017 / 038949 A. The contents of these descriptions are incorporated herein by reference.

[0064] The content of the stabilizer in the resin composition of this embodiment is preferably 0.01 parts by mass or more, more preferably 0.05 parts by mass or more, and even more preferably 0.1 parts by mass or more, relative to 100 parts by mass of the polyalkylene terephthalate resin. By ensuring that the content is above the lower limit, the effect of suppressing thermal and oxidative degradation of the resin during melt-kneading, molding, and use as a molded product tends to be more improved, and heat resistance tends to be improved. Furthermore, the upper limit of the stabilizer content is preferably 1.0 parts by mass or less, more preferably 0.8 parts by mass or less, more preferably 0.6 parts by mass or less, even more preferably 0.5 parts by mass or less, and even more preferably 0.4 parts by mass or less, relative to 100 parts by mass of the polyalkylene terephthalate resin. By ensuring that the content is below the upper limit, adverse effects on appearance and physical properties due to aggregation of additives such as stabilizers tend to be effectively suppressed, and discoloration of the resin composition tends to be suppressed. The resin composition of the present embodiment may contain only one stabilizer, or may contain two or more stabilizers. When two or more stabilizers are contained, the total amount is preferably in the above range.

[0065] <Flame retardant> The resin composition of the present embodiment preferably contains a flame retardant. By blending a flame retardant into the resin composition of the present embodiment, the appearance of the resulting molded article can be improved in addition to the flame retardancy. The type of flame retardant is not particularly limited, and known flame retardants can be used, such as halogen-based flame retardants, phosphorus-based flame retardants (metal phosphinates, melamine polyphosphate, etc.), nitrogen-based flame retardants (melamine cyanurate, etc.), and metal hydroxides (magnesium hydroxide, etc.). The resin composition of the present embodiment preferably contains a halogen-based flame retardant.

[0066] <<Halogen-based flame retardants>> When a halogen-based flame retardant is used as the flame retardant, the type is not particularly limited, but a bromine-based flame retardant is preferred. The brominated flame retardant is preferably brominated phthalimide, brominated poly(meth)acrylate, brominated polycarbonate, brominated epoxy, or brominated polystyrene, more preferably brominated polycarbonate, brominated poly(meth)acrylate, or brominated epoxy, and even more preferably brominated polycarbonate.

[0067] The brominated phthalimide is preferably one represented by formula (1). [ka] (In formula (1), D represents an alkylene group, an arylene group, or a group formed by combining two or more of -S(=O)2-, -C(=O)-, and -O-. i is an integer of 1 to 4.)

[0068] In formula (1), D represents a group consisting of a combination of two or more of an alkylene group, an arylene group, -S(=O)2-, -C(=O)-, and -O-; a group consisting of a combination of an alkylene group or an arylene group with at least one of -S(=O)2-, -C(=O)-, and -O- is preferred; a group consisting of a combination of an alkylene group or an arylene group with one of -S(=O)2-, -C(=O)-, and -O- is more preferred; and an alkylene group is even more preferred. The group consisting of a combination of an alkylene group and -O- is intended to include, for example, a combination of two alkylene groups and one -O- (the same applies to other combinations). The alkylene group represented by D is preferably an alkylene group having 1 to 6 carbon atoms, more preferably a methylene group, an ethylene group, a propylene group or a butylene group. The arylene group is preferably a phenylene group. i is an integer of 1 to 4, and is preferably 4.

[0069] Examples of the brominated phthalimide represented by formula (1) include N,N'-(bistetrabromophthalimide)ethane, N,N'-(bistetrabromophthalimide)propane, N,N'-(bistetrabromophthalimide)butane, N,N'-(bistetrabromophthalimide)diethyl ether, N,N'-(bistetrabromophthalimide)dipropyl ether, N,N'-(bistetrabromophthalimide)dibutyl ether, N,N'-(bistetrabromophthalimide)diphenylsulfone, N,N'-(bistetrabromophthalimide)diphenyl ketone, and N,N'-(bistetrabromophthalimide)diphenyl ether.

[0070] The brominated phthalimide represented by formula (1) is preferably a brominated phthalimide represented by formula (2). [ka] (In formula (2), i is an integer of 1 to 4.) i is an integer of 1 to 4, and is preferably 4.

[0071] The brominated poly(meth)acrylate is preferably a polymer obtained by polymerizing a bromine atom-containing benzyl (meth)acrylate alone, copolymerizing two or more types of bromine atom-containing benzyl (meth)acrylate, or copolymerizing the bromine atom with another vinyl monomer. The bromine atoms are attached to benzene rings, and the number of bromine atoms attached is preferably 1 to 5, and more preferably 4 to 5, per benzene ring.

[0072] Examples of the benzyl acrylate containing a bromine atom include pentabromobenzyl acrylate, tetrabromobenzyl acrylate, tribromobenzyl acrylate, and mixtures thereof. Examples of the benzyl methacrylate containing a bromine atom include methacrylates corresponding to the above-mentioned acrylates.

[0073] Specific examples of other vinyl monomers that can be copolymerized with the bromine atom-containing benzyl (meth)acrylate include acrylic acid esters such as acrylic acid, methyl acrylate, ethyl acrylate, butyl acrylate, and benzyl acrylate; methacrylic acid esters such as methacrylic acid, methyl methacrylate, ethyl methacrylate, butyl methacrylate, and benzyl methacrylate; unsaturated carboxylic acids or anhydrides thereof such as styrene, acrylonitrile, fumaric acid, and maleic acid; vinyl acetate; and vinyl chloride.

[0074] These are usually used in an equimolar amount or less, particularly preferably 0.5 times or less, of the amount of benzyl (meth)acrylate containing a bromine atom.

[0075] Furthermore, vinyl monomers such as xylene diacrylate, xylene dimethacrylate, tetrabromxylene diacrylate, tetrabromxylene dimethacrylate, butadiene, isoprene, and divinylbenzene can also be used, and these can usually be used in an amount of 0.5 times or less by mole relative to the bromine atom-containing benzyl acrylate or benzyl methacrylate.

[0076] The brominated poly(meth)acrylate is preferably a polymer obtained by polymerizing a bromine atom-containing (meth)acrylate monomer, particularly benzyl (meth)acrylate, alone or by copolymerizing two or more of them, or by copolymerizing them with other vinyl monomers. The bromine atoms are attached to the benzene ring, and the number of bromine atoms attached is preferably 1 to 5, more preferably 4 to 5, per benzene ring.

[0077] As the brominated poly(meth)acrylate, pentabromobenzyl poly(meth)acrylate is preferred because of its high bromine content.

[0078] The molecular weight of the brominated poly(meth)acrylate is optional and may be appropriately selected and determined, but the weight-average molecular weight (Mw) is preferably 3,000 or more, more preferably 10,000 or more, even more preferably 15,000 or more, even more preferably 20,000 or more, and even more preferably 25,000 or more. By setting the weight-average molecular weight at or above the lower limit, molded articles with higher mechanical strength tend to be obtained. Furthermore, the upper limit of the weight-average molecular weight (Mw) is preferably 100,000 or less, more preferably 80,000 or less, even more preferably 60,000 or less, even more preferably 50,000 or less, and even more preferably 35,000 or less. By setting the weight-average molecular weight at or below the upper limit, the flowability of the resin composition tends to be further improved.

[0079] The brominated polycarbonate preferably has a free bromine content of 0.05% by mass or more and preferably 0.20% by mass or less. By setting the content within these ranges, the heat resistance stability of the resin composition tends to be further improved. The brominated polycarbonate also preferably has a chlorine atom content of 0.001% by mass or more and preferably 0.20% by mass or less. By setting the content within these ranges, the mold corrosion resistance during molding tends to be further improved. Specifically, the brominated polycarbonate is preferably a brominated polycarbonate obtained from brominated bisphenol A, particularly tetrabromobisphenol A. Examples of the terminal structure include a phenyl group, a 4-t-butylphenyl group, and a 2,4,6-tribromophenyl group, and particularly, those having a 2,4,6-tribromophenyl group in the terminal group structure are preferred.

[0080] The average number of carbonate structural units in the brominated polycarbonate may be appropriately selected and determined, but is preferably 2-30, more preferably 3-15, and even more preferably 3-10.

[0081] The molecular weight of the brominated polycarbonate is optional and may be appropriately selected and determined, but preferably has a viscosity average molecular weight of 1,000 to 20,000, more preferably 2,000 to 10,000.

[0082] The brominated polycarbonate obtained from the above brominated bisphenol A can be obtained, for example, by a conventional method of reacting brominated bisphenol with phosgene. The end-capping agent includes an aromatic monohydroxy compound, which may be substituted with a halogen or an organic group.

[0083] Specific preferred examples of the brominated epoxy include bisphenol A type brominated epoxy compounds, such as tetrabromobisphenol A epoxy compounds and glycidyl brominated bisphenol A epoxy compounds.

[0084] The molecular weight of the brominated epoxy compound is optional and may be appropriately selected and determined. However, the weight-average molecular weight (Mw) is preferably 3,000 or more, more preferably 10,000 or more, even more preferably 13,000 or more, even more preferably 15,000 or more, and even more preferably 18,000 or more. By setting the Mw at or above the lower limit, molded articles with higher mechanical strength tend to be obtained. The upper limit of the weight-average molecular weight (Mw) is preferably 100,000 or less, more preferably 80,000 or less, even more preferably 78,000 or less, even more preferably 75,000 or less, even more preferably 70,000 or less, and may even be 50,000 or less, 30,000 or less, or 25,000 or less. Setting the Mw at or below the upper limit tends to further improve the flowability of the resin composition. The brominated epoxy compound preferably has an epoxy equivalent of 3,000 to 40,000 g / eq, more preferably 4,000 to 35,000 g / eq, and particularly preferably 10,000 to 30,000 g / eq.

[0085] Brominated epoxy oligomers can also be used in combination with the brominated epoxy. In this case, for example, by using an oligomer with an Mw of 5,000 or less in a proportion of about 50% by mass or less, flame retardancy, mold releasability, and flowability can be appropriately adjusted. The bromine atom content in the brominated epoxy compound is optional, but to provide sufficient flame retardancy, it is usually 10% by mass or more, preferably 20% by mass or more, and particularly preferably 30% by mass or more. The upper limit is 60% by mass, and preferably 55% by mass or less.

[0086] The brominated polystyrene preferably includes a brominated polystyrene containing a constitutional unit represented by formula (3). [ka] (In formula (3), t is an integer of 1 to 5, and n is the number of constitutional units.)

[0087] Brominated polystyrene can be produced by either brominating polystyrene or polymerizing brominated styrene monomers. Polymerization of brominated styrene is preferred because it contains a smaller amount of free bromine atoms. In formula (3), the CH group to which the brominated benzene is bonded may be substituted with a methyl group. Brominated polystyrene may also be a copolymer copolymerized with other vinyl monomers. Examples of vinyl monomers in this case include styrene, α-methylstyrene, (meth)acrylonitrile, methyl (meth)acrylate, butadiene, and vinyl acetate. Brominated polystyrene may be used alone or as a mixture of two or more different structures, and may contain units derived from styrene monomers with different bromine numbers in a single molecular chain.

[0088] Specific examples of brominated polystyrene include poly(4-bromostyrene), poly(2-bromostyrene), poly(3-bromostyrene), poly(2,4-dibromostyrene), poly(2,6-dibromostyrene), poly(2,5-dibromostyrene), poly(3,5-dibromostyrene), poly(2,4,6-tribromostyrene), poly(2,4,5-tribromostyrene), poly(2,3,5-tribromostyrene), and poly(4-bromo-α-methylstyrene). Examples of suitable styrene copolymers include poly(2,4-dibromostyrene), poly(2,4-dibromo-α-methylstyrene), poly(2,5-dibromo-α-methylstyrene), poly(2,4,6-tribromo-α-methylstyrene), and poly(2,4,5-tribromo-α-methylstyrene), and poly(2,4,6-tribromostyrene), poly(2,4,5-tribromostyrene), and polydibromostyrene and polytribromostyrene containing an average of 2 to 3 bromine groups in the benzene ring are particularly preferred.

[0089] The brominated polystyrene preferably has the number n (average degree of polymerization) of structural units in formula (3) of 30 to 1,500, more preferably 150 to 1,000, and particularly preferably 300 to 800. If the average degree of polymerization is less than 30, blooming is likely to occur, while if it exceeds 1,500, poor dispersion is likely to occur and mechanical properties are likely to deteriorate. The weight-average molecular weight (Mw) of the brominated polystyrene is preferably 5,000 to 500,000, more preferably 10,000 to 500,000, even more preferably 10,000 to 300,000, even more preferably 10,000 to 100,000, and even more preferably 10,000 to 70,000. In particular, in the case of the above-mentioned brominated polystyrene, the weight average molecular weight (Mw) is preferably 50,000 to 70,000, and in the case of brominated polystyrene produced by a polymerization method, the weight average molecular weight (Mw) is preferably about 10,000 to 30,000.

[0090] The bromine concentration (Br content in the examples described below) in the brominated flame retardant is preferably 45% by mass or more, more preferably 48% by mass or more, and even more preferably 50% by mass or more. By setting the bromine concentration at or above the lower limit, the flame retardancy of the molded article tends to be effectively improved. The upper limit of the bromine concentration is preferably 75% by mass or less, more preferably 73% by mass or less, even more preferably 71% by mass or less, and may be 65% by mass or less.

[0091] When the resin composition of this embodiment contains a halogen-based flame retardant, the content thereof is preferably 1 part by mass or more, more preferably 5 parts by mass or more, and even more preferably 9 parts by mass or more, and preferably 25 parts by mass or less, and more preferably 60 parts by mass or less, per 100 parts by mass of the polyalkylene terephthalate resin. By setting the content at or above the lower limit, the flame retardancy and appearance of the resulting molded article tend to be further improved. On the other hand, by setting the content at or below the upper limit, the mechanical strength tends to be further improved, gelation during production of the resin composition tends to be suppressed, and a decrease in fluidity due to thickening of the resin composition tends to be suppressed. The resin composition of the present embodiment may contain only one halogen-based flame retardant, or may contain two or more halogen-based flame retardants. When two or more halogen-based flame retardants are contained, the total amount is preferably in the above range.

[0092] <<Phosphorus-based flame retardants>> Examples of phosphorus-based flame retardants include metal phosphinates, melamine polyphosphates, condensed phosphate esters, and phosphazene compounds, with metal phosphinates being preferred.

[0093] When a metal phosphinate is used as a flame retardant, the type thereof is not particularly limited, but it is preferable that the metal phosphinate has an anion portion represented by formula (4) or formula (5) and a metal ion of the cation portion is any of calcium, magnesium, aluminum, and zinc.

[0094] [ka] (In the formula, R 1 and R 2 each independently represents an alkyl group having 1 to 6 carbon atoms or an aryl group which may have a substituent, and R 1 may be the same or different, and R 3 represents an alkylene group having 2 to 10 carbon atoms, an arylene group which may have a substituent, or a group consisting of a combination thereof; R 3 may be the same or different, and n represents an integer of 0 to 2.) The aryl group which may have a substituent is preferably a phenyl group which may have a substituent. When it has a substituent, it is preferably an alkyl group having 1 to 3 carbon atoms. It is also preferably unsubstituted. The arylene group which may have a substituent is preferably a phenylene group which may have a substituent. The arylene group which may have a substituent is preferably unsubstituted or has an alkyl group having 1 to 3 carbon atoms (preferably a methyl group) as a substituent. In this embodiment, a metal phosphinate represented by formula (4) is preferred. Also, in this embodiment, aluminum phosphinate is preferred.

[0095] Specific examples of the metal phosphinate include calcium dimethylphosphinate, magnesium dimethylphosphinate, aluminum dimethylphosphinate, zinc dimethylphosphinate, calcium ethylmethylphosphinate, magnesium ethylmethylphosphinate, aluminum ethylmethylphosphinate, zinc ethylmethylphosphinate, calcium diethylphosphinate, magnesium diethylphosphinate, aluminum diethylphosphinate, zinc diethylphosphinate, calcium methyl-n-propylphosphinate, magnesium methyl-n-propylphosphinate, aluminum methyl-n-propylphosphinate, zinc methyl-n-propylphosphinate, and calcium methanedi(methylphosphinate). Examples of suitable methyl phenyl phosphates include magnesium methane di(methylphosphinate), aluminum methane bis(methylphosphinate), zinc methane bis(methylphosphinate), calcium benzene-1,4-bis(methylphosphinate), magnesium benzene-1,4-bis(methylphosphinate), aluminum benzene-1,4-bis(methylphosphinate), zinc benzene-1,4-bis(methylphosphinate), calcium methylphenylphosphinate, magnesium methylphenylphosphinate, aluminum methylphenylphosphinate, zinc methylphenylphosphinate, calcium diphenylphosphinate, magnesium diphenylphosphinate, aluminum diphenylphosphinate, and zinc diphenylphosphinate. For details about the metal phosphinate, please refer to paragraphs 0052 to 0058 of WO 2010 / 010669, the contents of which are incorporated herein by reference. For further details of the phosphorus-based flame retardant, please refer to paragraphs 0064 to 0084 of International Publication No. 2021 / 241471, the contents of which are incorporated herein by reference.

[0096] The content of the phosphorus-based flame retardant in the resin composition of this embodiment is preferably 1 part by mass or more, more preferably 5 parts by mass or more, even more preferably 10 parts by mass or more, even more preferably 15 parts by mass or more, even more preferably 20 parts by mass or more, even more preferably 25 parts by mass or more, and preferably 40 parts by mass or less, more preferably 35 parts by mass or less, and even more preferably 30 parts by mass or less, per 100 parts by mass of the polyalkylene terephthalate resin. By setting the content at or above the lower limit, the flame retardancy and tracking resistance of the resulting molded article tend to be further improved. Meanwhile, by setting the content at or below the upper limit, the mechanical strength of the resulting molded article tends to be further improved. The resin composition of the present embodiment may contain only one phosphorus-based flame retardant, or may contain two or more phosphorus-based flame retardants. When two or more phosphorus-based flame retardants are contained, the total amount is preferably in the above range.

[0097] <<Nitrogen-based flame retardants>> Examples of the nitrogen-based flame retardant include aliphatic amine compounds, aromatic amine compounds, nitrogen-containing heterocyclic compounds, cyanide compounds, aliphatic amides, aromatic amides, urea, and thiourea. Examples of the aliphatic amine include ethylamine, butylamine, diethylamine, ethylenediamine, butylenediamine, triethylenetetramine, 1,2-diaminocyclohexane, and 1,2-diaminocyclooctane. Examples of aromatic amines include aniline and phenylenediamine, and examples of nitrogen-containing heterocyclic compounds include uric acid, adenine, guanine, 2,6-diaminopurine, 2,4,6-triaminopyridine, and triazine compounds. Examples of the cyanide compound include dicyandiamide, examples of the aliphatic amide include N,N-dimethylacetamide, and examples of the aromatic amide include N,N-diphenylacetamide.

[0098] The triazine compounds exemplified above are nitrogen-containing heterocyclic compounds having a triazine skeleton, and examples thereof include triazine, melamine, benzoguanamine, methylguanamine, cyanuric acid, melamine cyanurate, melamine isocyanurate, trimethyltriazine, triphenyltriazine, ameline, amelide, thiocyanuric acid, diaminomercaptotriazine, diaminomethyltriazine, diaminophenyltriazine, and diaminoisopropoxytriazine. The melamine cyanurate or melamine isocyanurate is preferably an adduct of cyanuric acid or isocyanuric acid with a triazine compound, and examples thereof include adducts having a composition usually of 1:1 (molar ratio), and in some cases of 1:2 (molar ratio).

[0099] Among the nitrogen-based flame retardants, nitrogen-containing heterocyclic compounds are preferred, among which triazine compounds are more preferred, and melamine cyanurate is even more preferred.

[0100] The resin composition of this embodiment may or may not contain a nitrogen-based flame retardant. When the resin composition of this embodiment contains a nitrogen-based flame retardant, the content thereof is preferably 1 part by mass or more, more preferably 5 parts by mass or more, and even more preferably 10 parts by mass or more, relative to 100 parts by mass of the polyalkylene terephthalate resin. It is also preferably 19 parts by mass or less, more preferably 18 parts by mass or less, more preferably 16 parts by mass or less, even more preferably 14 parts by mass or less, even more preferably 13 parts by mass or less, and even more preferably 10 parts by mass or less. Depending on the application, it may be 8 parts by mass or less, 5 parts by mass or less, 3 parts by mass or less, 1 part by mass or less, or 0.1 parts by mass or less. By setting the content at or above the lower limit, the flame retardancy and tracking resistance of the resulting molded article tend to be further improved. By setting the content at or below the upper limit, the mechanical strength tends to be further improved, gelation during production of the resin composition tends to be suppressed, and a decrease in fluidity due to thickening of the resin composition tends to be suppressed. The resin composition of the present embodiment may contain only one nitrogen-based flame retardant, or may contain two or more nitrogen-based flame retardants. When two or more nitrogen-based flame retardants are contained, the total amount is preferably in the above range.

[0101] The content (total amount) of the flame retardant in the resin composition of this embodiment is preferably 5 parts by mass or more, more preferably 10 parts by mass or more, and even more preferably 15 parts by mass or more, relative to 100 parts by mass of the polyalkylene terephthalate resin, and is preferably 50 parts by mass or less, more preferably 40 parts by mass or less, and even more preferably 35 parts by mass or less. By setting the content at or above the lower limit, flame retardancy tends to be further improved. Meanwhile, by setting the content at or below the upper limit, mechanical strength tends to be further improved. The resin composition of the present embodiment may contain only one type of flame retardant, or may contain two or more types. When two or more types are contained, the total amount is preferably in the above range.

[0102] <Flame retardant synergist> The resin composition of this embodiment may contain a flame retardant aid. By including a flame retardant aid, the flame retardancy of the molded article can be further improved. The flame retardant aid is particularly preferably used when a halogen-based flame retardant is included. Examples of the flame retardant aid used in this embodiment include antimony compounds, such as antimony trioxide (Sb2O3), antimony tetroxide (Sb2O4), antimony pentoxide (Sb2O5), and sodium antimonate. In particular, antimony oxide, and especially antimony trioxide, is preferred from the viewpoint of impact resistance. When a flame retardant aid is blended, it may be blended as a masterbatch. The content of the antimony compound in the masterbatch is preferably 30 to 90 mass%, more preferably 40 to 85 mass%, even more preferably 50 to 85 mass%, still more preferably 60 to 85 mass%, and even more preferably 70 to 85 mass%. The resin used in the masterbatch is preferably a polyester resin, more preferably a polybutylene terephthalate resin.

[0103] When the resin composition of this embodiment contains a flame retardant aid (e.g., an antimony compound), the content thereof is preferably 0.1 parts by mass or more, more preferably 1 part by mass or more, even more preferably 2 parts by mass or more, even more preferably 3 parts by mass or more, and even more preferably 5 parts by mass or more, relative to 100 parts by mass of the polyalkylene terephthalate resin. By setting the content at or above the lower limit, flame retardancy tends to be more effectively exhibited. Furthermore, the upper limit of the content of the antimony compound is preferably 20 parts by mass or less, more preferably 15 parts by mass or less, even more preferably 10 parts by mass or less, even more preferably 8 parts by mass or less, and even more preferably 5 parts by mass or less, relative to 100 parts by mass of the polyalkylene terephthalate resin. By setting the content at or below the upper limit, the mold releasability and impact resistance of the resulting molded article tend to be improved. The resin composition of the present embodiment may contain only one type of flame retardant auxiliary, or may contain two or more types. When two or more types are contained, the total amount is preferably in the above range.

[0104] <Anti-drip agent> The resin composition of this embodiment may also contain an anti-dripping agent. The anti-dripping agent is preferably polytetrafluoroethylene (PTFE), which has fibril-forming ability, disperses easily in the resin composition, and tends to form a fibrous network structure in the resin. Examples of PTFE that tends to have fibril-forming ability in the resin composition of this embodiment include suspension polymerization products. Furthermore, from the perspective of reducing environmental impact, it is preferable to use a PTFE that contains reduced perfluorooctanoic acid (PFOA) or that does not contain PFOA. The content of the anti-dripping agent is preferably 0.1 to 20 parts by mass, more preferably 0.2 parts by mass or more, even more preferably 0.3 parts by mass or more, even more preferably 0.4 parts by mass or more, more preferably 10 parts by mass or less, even more preferably 5 parts by mass or less, and even more preferably 1 part by mass or less, relative to 100 parts by mass of the polyalkylene terephthalate resin. By setting the content at or above the lower limit, dripping during combustion tends to be suppressed, impact resistance tends to be improved, and flame retardancy tends to be more effectively achieved. Furthermore, by setting the content at or below the upper limit, the appearance of the molded article tends to be improved, and flowability tends to be improved. The resin composition of the present embodiment may contain only one type of anti-dripping agent, or may contain two or more types. When two or more types are contained, the total amount is preferably in the above range.

[0105] <Coloring agent> The resin composition of the present embodiment may contain a colorant. By containing a colorant, the resulting molded article can be given a design feature. The colorant may be a pigment or a dye, with a pigment being preferred. The colorant may be a chromatic colorant or an achromatic colorant, and is preferably an achromatic colorant.

[0106] Examples of inorganic pigments include sulfide pigments such as carbon black, cadmium red, and cadmium yellow; silicate pigments such as ultramarine; oxide pigments such as titanium oxide, zinc white, red iron oxide, chromium oxide, iron black, titanium yellow, zinc-iron brown, titanium-cobalt green, cobalt green, cobalt blue, copper-chromium black, and copper-iron black; chromate pigments such as yellow lead and molybdate orange; and ferrocyanide pigments such as iron blue.

[0107] Examples of organic pigments and / or organic dyes include phthalocyanine dyes and pigments such as copper phthalocyanine blue and copper phthalocyanine green; azo dyes and pigments such as nickel azo yellow; methine dyes and pigments, pyrazolone dyes and pigments, thioindigo dyes and pigments, perinone dyes and pigments, perylene dyes and pigments, quinacridone dyes and pigments, dioxazine dyes and pigments, isoindolinone dyes and pigments, quinophthalone dyes and pigments, and other condensed polycyclic dyes and pigments; anthraquinone dyes and pigments, heterocyclic dyes and pigments, and methyl dyes and pigments.

[0108] In this embodiment, the colorant preferably contains a black pigment, and more preferably contains carbon black. By blending the black pigment into the resin composition of this embodiment, the blackness can be increased. When a pigment is blended, it may be blended as a masterbatch. The content of the pigment in the masterbatch is preferably 10 to 50 mass %, more preferably 15 to 45 mass %. The resin used in the masterbatch is preferably a polyester resin, more preferably a polybutylene terephthalate resin.

[0109] The content of the colorant in the resin composition of this embodiment is usually 0.01 part by mass or more, preferably 0.05 part by mass or more, more preferably 0.1 part by mass or more, and usually 5.0 parts by mass or less, preferably 3.0 parts by mass or less, more preferably 1.0 part by mass or less, relative to 100 parts by mass of the polyalkylene terephthalate resin. By setting the content of the colorant within this range, the effect of adding the colorant can be more effectively exhibited. The resin composition of the present embodiment may contain only one type of colorant, or may contain two or more types. When two or more types are contained, the total amount is preferably in the above range.

[0110] <Nucleating agent> The resin composition of the present embodiment may contain a nucleating agent, which promotes crystallization of the resin composition. The type of nucleating agent is not particularly limited, but may be either an inorganic nucleating agent or an organic nucleating agent, with organic nucleating agents being more preferred. By using an organic nucleating agent, the amount of the nucleating agent can be reduced, and the mechanical strength and shrinkage rate of the resulting molded article can be further improved. Examples of inorganic nucleating agents include talc, boron nitride, mica, kaolin, barium sulfate, sodium phosphate, silicon nitride, and molybdenum disulfide. Among these, talc, barium sulfate, sodium phosphate, and boron nitride are preferred, and talc is more preferred because it tends to increase the rigidity of the resin composition and improve moldability.

[0111] As the organic nucleating agent, an organic alkali metal salt is preferred, an organic carboxylic acid alkali metal salt is more preferred, and an alkali metal salt (preferably a sodium salt or potassium salt, more preferably a sodium salt) of a fatty acid (preferably a fatty acid having 5 to 50 carbon atoms) is even more preferred. Specific examples of the organic nucleating agent include ionomer, sodium benzoate, sodium palmitate, sodium stearate, sodium behenate, and sodium montanate, of which sodium stearate, sodium behenate, and sodium montanate are more preferred, with sodium montanate being even more preferred. The use of an organic alkali metal salt enhances the effect as a crystal nucleating agent and improves the crystallinity of the resin composition, which tends to result in a well-balanced improvement in the various performances of molded articles formed from the resin composition, as will be shown in the examples described below. This is even more preferred.

[0112] The content of the nucleating agent (preferably talc) in the resin composition of this embodiment is preferably 0.1 parts by mass or more, more preferably 0.2 parts by mass or more, even more preferably 0.5 parts by mass or more, even more preferably 1.0 part by mass or more, and even more preferably 1.5 parts by mass or more, relative to 100 parts by mass of the polyalkylene terephthalate resin. By setting the content of the nucleating agent at or above the lower limit, the mold release properties and mechanical strength of the molded article tend to be improved. Furthermore, the upper limit of the content of the nucleating agent is 10 parts by mass or less, preferably 8 parts by mass or less, more preferably 5 parts by mass or less, and even more preferably 3 parts by mass or less, relative to 100 parts by mass of the polyalkylene terephthalate resin. By setting the content at or below the upper limit, decomposition of the resin is suppressed, and the mechanical strength, particularly impact resistance, of the molded article tends to be improved. The resin composition of the present embodiment may contain only one type of nucleating agent, or may contain two or more types. When two or more types are contained, the total amount is preferably in the above range.

[0113] <Other ingredients> The resin composition of the present embodiment may contain other components in addition to those described above, as necessary, as long as the desired physical properties are not significantly impaired. The other components may be contained alone or in any combination and ratio of two or more. Examples of other components include resin additives, fillers other than the above-mentioned glass fibers, and the like. Specific examples of resin additives include transesterification inhibitors, ultraviolet absorbers, mold release agents, nucleating agents, antistatic agents, antifogging agents, antiblocking agents, flow improvers, plasticizers, and dispersants. The total amount of these other components is preferably 0% by mass or more and less than 10% by mass, more preferably 0% by mass or more and less than 5% by mass, and even more preferably 0% by mass or more and less than 3% by mass, based on 100% by mass of the resin composition. In the resin composition of this embodiment, the polyalkylene terephthalate resin, C-glass fiber and / or A-glass fiber, and optionally blended thermoplastic resin (preferably a styrene-based resin and / or a polycarbonate resin), thermosetting resin (preferably an epoxy compound), stabilizer, mold release agent, flame retardant (preferably a halogen-based flame retardant), colorant, nucleating agent, flame retardant aid, and anti-dripping agent preferably account for 90% by mass or more of the resin composition, more preferably 95% by mass or more, and may even be 100% by mass.

[0114] <Physical properties of resin composition> The resin composition of the present embodiment preferably has excellent mechanical properties. Specifically, the resin composition of this embodiment is molded into an ISO test piece (4 mm thick) and the tensile strength measured in accordance with ISO 527-1 and ISO 527-2 is preferably 70 MPa or more, more preferably 80 MPa or more, even more preferably 90 MPa or more, even more preferably 100 MPa or more, and even more preferably 110 MPa or more. There is no particular upper limit, but even if it is 500 MPa or less, the requirements are fully met. By making it equal to or greater than the lower limit, the mechanical strength of the molded product tends to be excellent. The tensile strength is measured as described in the Examples below.

[0115] The resin composition of this embodiment is molded into an ISO test piece (4 mm thick) and the tensile strain at break measured in accordance with ISO 527-1 and ISO 527-2 is preferably 0.5% or more, more preferably 0.8% or more, even more preferably 1.0% or more, even more preferably 1.2% or more, and even more preferably 1.5% or more. There is no particular upper limit, but even if it is 10% or less, the required performance is sufficiently met. By making it equal to or greater than the lower limit, the toughness of the molded product tends to be excellent.

[0116] The resin composition of this embodiment is molded into an ISO test piece (4 mm thick) and has a flexural modulus of preferably 2000 MPa or more, more preferably 3000 MPa or more, even more preferably 4000 MPa or more, even more preferably 4500 MPa or more, and even more preferably 5000 MPa or more, as measured in accordance with ISO 178. There is no particular upper limit, but even if it is 30000 MPa or less, the required performance is fully satisfied. By adjusting the modulus to be equal to or greater than the lower limit, the rigidity of the molded article tends to be excellent. The flexural modulus is measured as described in the Examples section below.

[0117] The resin composition of this embodiment was molded into an ISO test piece (4 mm thick) and had a Charpy impact strength (unnotched) of 1 kJ / m2 measured in accordance with ISO179-1. 2 It is preferable that the concentration is 2 kJ / m or more. 2 More preferably, it is 3 kJ / m or more. 2 More preferably, it is 4 kJ / m or more. 2 More preferably, it is 5 kJ / m or more. 2 It is more preferable that the upper limit is 100 kJ / m or more. There is no particular upper limit. 2 By making the content equal to or greater than the lower limit, the toughness of the molded article tends to be excellent. The Charpy impact strength (unnotched) is measured as described in the Examples below.

[0118] <Method of manufacturing resin composition> The resin composition of this embodiment can be produced by a conventional method for preparing a resin composition (e.g., pellets). Typically, the components and various optional additives are thoroughly mixed together and then melt-kneaded in a single-screw or twin-screw extruder. Alternatively, the resin composition of this embodiment can be prepared without premixing the components, or by premixing only a portion of the components, feeding the mixture into an extruder using a feeder and melt-kneading the mixture. For example, glass fibers are preferably fed into an extruder using a side feeder and melt-kneaded. Alternatively, a masterbatch may be prepared by melt-kneading some of the components with a thermoplastic resin, followed by blending the remaining components with the masterbatch and melt-kneading the resulting mixture. The thermoplastic resin to be used for the masterbatch is preferably a polyalkylene terephthalate resin, more preferably a polybutylene terephthalate resin and / or a polyethylene terephthalate resin, and even more preferably a polybutylene terephthalate resin.

[0119] <Method of manufacturing molded products> The resin composition or pellets of this embodiment are molded according to a known method. The method for producing the molded article is not particularly limited, and any molding method generally used for resin compositions can be used. Examples thereof include injection molding, ultra-high speed injection molding, injection compression molding, two-color molding, gas-assisted or other hollow molding, molding using a heat-insulating mold, molding using a rapid heating mold, foam molding (including supercritical fluid), insert molding, IMC (in-mold coating molding), extrusion molding, sheet molding, thermoforming, rotational molding, lamination molding, press molding, blow molding, etc., among which injection molding is preferred. For details of the injection molding method, please refer to the description in paragraphs 0113 to 0116 of Japanese Patent No. 6183822, the contents of which are incorporated herein by reference. Furthermore, the mold temperature during molding such as injection molding is preferably 40 to 150°C.

[0120] <Application> The resin composition of the present embodiment is used as a molded article formed from the resin composition or pellets. The resin composition and pellets can be used for a wide range of known applications. For example, they can be used indoors or outdoors as materials for electrical and electronic devices, automobiles, housing, and parts manufacturing in other industrial fields. More specifically, examples of the material include breakers, electromagnetic switches, various relay parts, transformer parts, sensor parts, switch parts, connector parts, terminal parts, actuator parts, outlet parts, socket parts, plug parts, capacitor parts, resistor parts, charging parts, battery parts, housing parts, structural parts, insulating parts, etc. In particular, the material can be suitably used as a material for parts located near electrical contacts. Automotive materials include lamp housings, reflectors, bezels, extensions, connectors, ECU cases, housings for in-vehicle cameras and millimeter-wave radars, battery cases, and sensor housings. Electrical and electronic components include various housings, display devices for personal computers, game consoles, televisions, etc., printers, copiers, scanners, fax machines, electronic organizers and PDAs, electronic desk calculators, electronic dictionaries, cameras, video cameras, mobile phones, battery packs, recording medium drives and readers, mice, numeric keypads, CD players, MD players, portable radios and audio players, housings, covers, keyboards, buttons, switch components, power meter casings, battery cases, battery transport trays, relays, sensors, actuators, terminal switches, and grill cooking equipment parts. [Example]

[0121] The present invention will be explained in more detail below with reference to examples. The materials, amounts used, ratios, processing details, processing procedures, etc. shown in the following examples can be appropriately changed without departing from the spirit of the present invention. Therefore, the scope of the present invention is not limited to the specific examples shown below. If the measuring instruments used in the examples are difficult to obtain due to discontinuation or the like, measurements can be made using other instruments with equivalent performance.

[0122] 1. Raw materials The following raw materials were used.

Table 1

[0123]

Table 2

[0124] 2. Examples 1 - 6, Comparative Examples 1 - 2, and Reference Examples 1 - 2 <Compound> The components shown in Table 1 or Table 2 were uniformly mixed using a tumbler mixer at the ratios shown in Table 3 or Table 4 (each component in Table 3 or Table 4 is expressed in mass%). The obtained mixture was fed into a twin - screw extruder (TEX30α manufactured by Japan Steel Works, Ltd.) through the main feed port. The cylinder set temperature of the first kneading section was set at 260°C, and the glass fiber was fed through a side feeder. The resin composition was melt - kneaded under the conditions of a cylinder set temperature of 220°C and a screw rotation speed of 200 rpm after the addition of the glass fiber, quenched in a water tank, and pelletized using a pelletizer to obtain pellets of the resin composition.

[0125] <Molding of test specimens> The resin composition pellets obtained above were dried at 120°C for 5 hours and then, using an injection molding machine (J - 85AD - 60H), a JIS K7139 multi - purpose test specimen (4 mm thick) was injection - molded under the conditions of a cylinder temperature of 265°C and a mold temperature of 80°C. The obtained multi - purpose test specimen (4 mm thick) was treated for 25 hours using a pressure cooker tester under the conditions of a temperature of 121°C, a relative humidity of 100%, and a pressure of 2 atm. The ESPEC EH8 - 221M pressure cooker tester was used.

[0126] <PCT 25hr Appearance> Regarding the test specimens after the 25 - hour treatment, the appearance was visually observed and evaluated as follows. A: The test piece maintained a good appearance. B: A small amount of powder was observed on the surface of the test piece, but it was at a practical level. C: Powdery matter was found on the surface of the test piece.

[0127] <Mechanical properties> The pellets obtained above were dried at 110°C for 5 hours, and then injection-molded into 4 mm thick ISO test specimens using an injection molding machine ("J85AD" manufactured by The Japan Steel Works, Ltd.) at a cylinder temperature of 250°C and a mold temperature of 80°C. The ISO test specimens (4 mm thick) obtained above were measured for tensile modulus (unit: MPa), tensile strength (unit: MPa), and tensile breaking strain (unit: %) according to ISO527-1 and ISO527-2. The ISO test specimens (4 mm thick) obtained above were measured for flexural strength (unit: MPa) and flexural modulus (unit: MPa) in accordance with ISO178. The ISO test specimens (4 mm thick) obtained above were subjected to the Charpy impact strength (unnotched) test (unit: kJ / m 2 ) was measured.

[0128] <Flame retardancy> The pellets obtained above were dried at 110°C for 5 hours, and then injection-molded into combustion test specimens (12.7mm width x 127mm length x 1.6mm thickness, 12.7mm width x 127mm length x 1.6mm thickness 0.8mm thickness) using an injection molding machine ("J-50AD" manufactured by The Japan Steel Works, Ltd.) under conditions of a cylinder temperature of 250°C and a mold temperature of 80°C. The obtained combustion test specimens were left to stand in an atmosphere of 70°C for one week, and then the flame retardancy was evaluated in accordance with the method of Subject 94 (UL94) of Underwriters Laboratories.

[0129] [Table 3]

[0130] [Table 4]

[0131] As is clear from the above results, the resin compositions of the present embodiment did not precipitate powdery matter and exhibited excellent appearance (Examples 1 to 6). In contrast, when no resin other than polyester resin and no flame retardant was blended and the proportion of polyalkylene terephthalate resin was high, powdery matter precipitated on the surface after the moist heat treatment test (Comparative Examples 1 and 2). Furthermore, when E glass fiber was used, no powdery matter was deposited and an excellent appearance was exhibited (Reference Examples 1 and 2).

[0132] Although the present invention has been described in detail with reference to specific embodiments, it will be apparent to those skilled in the art that various modifications can be made without departing from the spirit and scope of the invention.

Claims

1. a polyalkylene terephthalate resin; The composite material comprises at least one of C glass fiber and / or A glass fiber, wherein the C glass fiber and / or A glass fiber comprises recycled glass fiber; A resin composition comprising: A resin composition, wherein the content of the polyalkylene terephthalate resin in the resin composition is 50 to 95 parts by mass per 100 parts by mass of the total of all components excluding the glass fiber.

2. The resin composition according to claim 1 , wherein the polyalkylene terephthalate resin comprises a polybutylene terephthalate resin.

3. The resin composition according to claim 1 or 2, wherein the polyalkylene terephthalate resin has a terminal carboxyl group concentration of 1 eq / ton or more.

4. The resin composition according to claim 1 , wherein the resin composition contains a thermoplastic resin other than a polyester resin.

5. The resin composition according to claim 4, wherein the mass ratio of the polyalkylene terephthalate resin to the thermoplastic resin other than the polyester resin is 10:90 to 90:

10.

6. 6. The resin composition according to claim 4 or 5, wherein the thermoplastic resin other than the polyester resin comprises at least one selected from the group consisting of a polyolefin resin, a polyamide resin, a styrene-based resin, a polycarbonate resin, a silicone resin, and a polyarylene sulfide resin.

7. The resin composition according to claim 4 or 5, wherein the thermoplastic resin other than the polyester resin comprises a styrene-based resin and / or a polycarbonate resin.

8. The resin composition according to claim 1 , wherein the resin composition comprises a flame retardant.

9. The resin composition according to claim 8, wherein the flame retardant comprises at least one selected from the group consisting of brominated phthalimide, brominated poly(meth)acrylate, brominated polycarbonate, brominated epoxy, and brominated polystyrene.

10. 10. The resin composition according to claim 1, wherein the C glass fiber and / or the A glass fiber contains 1 mass % or more of recycled glass fiber.

11. 10. The resin composition according to claim 1, wherein the C glass fiber and / or the A glass fiber contains sodium oxide and / or potassium oxide in a total amount of 1 part by mass or more per 100 parts by mass of the C glass fiber and / or the A glass fiber.

12. the polyalkylene terephthalate resin comprises a polybutylene terephthalate resin, the polyalkylene terephthalate resin has a terminal carboxyl group concentration of 1 eq / ton or more; the resin composition contains a thermoplastic resin other than a polyester resin and / or a flame retardant, the thermoplastic resin other than the polyester resin includes a styrene-based resin and / or a polycarbonate resin; the flame retardant comprises at least one selected from brominated phthalimide, brominated poly(meth)acrylate, brominated polycarbonate, brominated epoxy, and brominated polystyrene; The C glass fiber and / or A glass fiber contains 1 mass % or more of recycled glass fiber, 2. The resin composition according to claim 1, wherein the C glass fiber and / or the A glass fiber contains sodium oxide and / or potassium oxide in a total amount of 1 part by mass or more per 100 parts by mass of the C glass fiber and / or the A glass fiber.

13. Pellets of the resin composition according to claim 1, 2, 4, 5, 8, 9 or 12.

14. A molded article molded from the resin composition according to claim 1, 2, 4, 5, 8, 9 or 12.

15. A molded article formed from the pellets according to claim 13.

16. A method for improving the appearance of a resin composition containing a polyalkylene terephthalate resin and at least one of C-glass fiber and / or A-glass fiber, wherein the C-glass fiber and / or A-glass fiber contains recycled glass fiber, the method comprising blending a resin other than polyester resin and / or a flame retardant.

17. An appearance improver for a resin composition comprising a polyalkylene terephthalate resin and at least one of C-glass fiber and / or A-glass fiber, wherein the C-glass fiber and / or the A-glass fiber contains recycled glass fiber, and the appearance improver contains a resin other than a polyester resin and / or a flame retardant.

Citation Information

Patent Citations

  • Thermally conductive polyalkylene terephthalate-based resin composition

    JP2012087234A

  • Resin composition, molded product, electromagnetic wave absorber and method for measuring absorptivity of resin composition

    JP2022008175A