Resin composition, pellets, and molded article

WO2025033541A1PCT designated stage expired Publication Date: 2025-02-13MITSUBISHI CHEM CORP
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Patent Information

Application Number
PCT/JP2024/028658
Authority / Receiving Office
WO · WO
Patent Type
Applications
Current Assignee / Owner
Priority Date
2023-08-09
Filing Date
2024-08-09
Publication Date
2025-02-13

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Abstract

Provided are a resin composition, pellets, and a molded article. The resin composition contains 5-50 mass parts of a flame retardant per 100 total mass parts of a polyalkylene terephthalate resin and a polycarbonate resin. The mass ratio of the polyalkylene terephthalate resin and the polycarbonate resin in 100 total mass parts of the polyalkylene terephthalate resin and polycarbonate resin is 10 / 90-90 / 10, the polycarbonate resin contains recycled polycarbonate resin, and the amount of branching of the recycled polycarbonate resin is 50-3500 mass ppm.
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Description

Resin composition, pellets, and molded products

[0001] The present invention relates to a resin composition, a pellet, and a molded article.

[0002] Resin compositions containing a polyalkylene terephthalate resin, such as a polybutylene terephthalate resin, and a polycarbonate resin have been studied (see, for example, Patent Document 1). Such resin compositions are widely used in electrical and electronic equipment components, automotive interior and exterior components, other electrical components, machine components, and the like.

[0003] International Publication No. 2021 / 186025

[0004] In recent years, from the perspective of environmental impact, the use of recycled materials as thermoplastic resins has been considered. However, when recycled thermoplastic resins are used, the physical properties of the resulting molded articles tend to be inferior. Under these circumstances, the present invention attempts to use recycled polycarbonate resin. Specifically, the present invention aims to provide a resin composition containing a polyalkylene terephthalate resin, a recycled polycarbonate resin, and a flame retardant, which can achieve physical properties comparable to those of virgin polycarbonate resin or better than those of virgin polycarbonate resin alone, as well as pellets and molded articles.

[0005] In light of the above-mentioned problems, the present inventors have conducted research and found that the above-mentioned problems can be solved by using a specific polycarbonate resin as the recycled polycarbonate resin and blending a flame retardant into it. Specifically, the above-mentioned problems have been solved by the following means. <1> A resin composition comprising 5 to 50 parts by mass of a flame retardant per 100 parts by mass of a polyalkylene terephthalate resin and a polycarbonate resin, wherein the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin in the 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin is 10 / 90 to 90 / 10, the polycarbonate resin contains recycled polycarbonate resin, and the amount of branching of the recycled polycarbonate resin is 50 to 3,500 ppm by mass. <2> The composition contains 1 to 30 parts by mass of an elastomer relative to 100 parts by mass of a total of a polyalkylene terephthalate resin and a polycarbonate resin, and the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin in the total of 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin is 80 / 20 to 20 / 80, and the melt volume rate (MVR) of the recycled polycarbonate resin measured in accordance with ISO 1133 under conditions of 300 ° C. and a load of 1.20 kgf is 2 to 11 cm 3 <3> The resin composition according to <1> or <2>, wherein the recycled polycarbonate resin contains 10 to 80 mass ppm of bisphenol A. <4> The recycled polycarbonate resin has a melt volume rate (MVR) of 4 to 30 cm3 measured in accordance with ISO 1133 at 300°C under a load of 1.20 kgf. 3<1> The resin composition according to <1>, wherein the flame retardant is 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin. <5> The resin composition according to any one of <1> to <4>, further comprising an ester exchange inhibitor in an amount of 0.01 to 2 parts by mass per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. <6> The resin composition according to any one of <1> to <5>, wherein the polybutylene terephthalate resin accounts for 50% by mass or more of the polyalkylene terephthalate resin. <7> The resin composition according to any one of <1> to <6>, wherein the flame retardant comprises a brominated flame retardant. <8> The resin composition according to any one of <1> to <7>, further comprising an elastomer in an amount of 3 to 30 parts by mass per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. <9> The resin composition according to any one of <1> to <8>, wherein the recycled polycarbonate resin contains aluminum element at a rate of 0.2 to 1000 ppm by mass and iron element at a rate of 0.2 to 100 ppm by mass. <10> The resin composition according to any one of <1> to <9>, wherein the resin composition is molded into a UL-94 test piece having a thickness of 0.74 mm or 1.0 mm, and the flame retardancy according to the UL-94 test satisfies V-0. <11> The resin composition according to any one of <1> to <10>, wherein the recycled polycarbonate resin includes at least one of polycarbonate resin derived from bottles, polycarbonate resin derived from discs, polycarbonate resin derived from sheets, polycarbonate resin derived from meter covers, and polycarbonate resin derived from headlamp lenses. <12> The melt volume rate (MVR) of the recycled polycarbonate resin measured in accordance with ISO 1133 under conditions of 300 ° C. and a load of 1.20 kgf is 4 to 30 cm 3The resin composition according to any one of <1> to <11>, wherein the polyalkylene terephthalate resin has a viscosity of 100 to 1000 saturations, and the polyalkylene terephthalate resin and the polycarbonate resin have ... <13> The resin composition according to any one of <1> to <12>, wherein the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin is 30 / 70 to 55 / 45, based on a total of 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin. <14> The resin composition according to any one of <1> to <13>, wherein the recycled polycarbonate resin contains a polycarbonate resin derived from bottles and / or sheets. <15> The resin composition according to any one of <1> to <14>, wherein the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin in a total of 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin is 30 / 70 to 55 / 45, the recycled polycarbonate resin contains polycarbonate resin derived from bottles and / or sheets, and further contains 0.01 to 2 parts by mass of an ester exchange inhibitor relative to 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin, and the polyalkylene terephthalate resin contains polybutylene terephthalate resin. <16> Pellets of the resin composition according to any one of <1> to <15>. <17> A molded article formed from the resin composition according to any one of <1> to <15>. <18> A molded article formed from the pellets according to <16>.

[0006] The above problem was also solved by the following means: <2-1> A resin composition comprising 3 to 30 parts by mass of an elastomer and 5 to 50 parts by mass of a flame retardant relative to 100 parts by mass of a polyalkylene terephthalate resin and a polycarbonate resin, wherein the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin in the 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin is 80 / 20 to 20 / 80, the polycarbonate resin contains recycled polycarbonate resin, and the melt volume rate (MVR) of the recycled polycarbonate resin measured in accordance with ISO 1133 at 300°C under a load of 1.20 kgf is 2 to 11 cm 3 / 10 minutes and a branching amount of 50 to 3,500 ppm by mass. <2-2> The resin composition according to <2-1>, wherein the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin, per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin, is 30 / 70 to 55 / 45. <2-3> The resin composition according to <2-1> or <2-2>, wherein the recycled polycarbonate resin includes a polycarbonate resin derived from bottles and / or sheets. <2-4> The resin composition according to any one of <2-1> to <2-3>, further comprising 0.01 to 2 parts by mass of a transesterification inhibitor, per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin. <2-5> The resin composition according to any one of <2-1> to <2-4>, wherein the polyalkylene terephthalate resin comprises a polybutylene terephthalate resin. <2-6> The resin composition according to any one of <2-1> to <2-5>, wherein the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin is 30 / 70 to 55 / 45, per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin, the recycled polycarbonate resin comprises a polycarbonate resin derived from bottles and / or sheets, and the resin composition further comprises 0.01 to 2 parts by mass of an ester exchange inhibitor, per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin, and the polyalkylene terephthalate resin comprises a polybutylene terephthalate resin. <2-7> Pellets of the resin composition according to any one of <2-1> to <2-6>. <2-8> A molded article formed from the resin composition according to any one of <2-1> to <2-6>. <2-9> A molded article formed from the pellets according to <2-7>.

[0007] The above problem was also solved by the following means. <3-1> A resin composition comprising 5 to 50 parts by mass of a flame retardant per 100 parts by mass of a polyalkylene terephthalate resin and a polycarbonate resin, wherein the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin in the 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin is 10 / 90 to 90 / 10, and the polycarbonate resin comprises a recycled polycarbonate resin, which contains 10 to 80 ppm by mass of bisphenol A and has a branching amount of 50 to 3,500 ppm by mass. <3-2> The recycled polycarbonate resin has a melt volume rate (MVR) of 4 to 30 cm as measured in accordance with ISO 1133 at 300°C under a load of 1.20 kgf. 3 / 10 minutes. <3-3> The resin composition according to <3-1> or <3-2>, further comprising an ester exchange inhibitor in an amount of 0.01 to 2 parts by mass per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. <3-4> The resin composition according to any one of <3-1> to <3-3>, wherein the polyalkylene terephthalate resin comprises a polybutylene terephthalate resin. <3-5> The resin composition according to any one of <3-1> to <3-4>, wherein the flame retardant comprises a brominated flame retardant. <3-6> The resin composition according to any one of <3-1> to <3-5>, further comprising an elastomer in an amount of 1 to 30 parts by mass per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. <3-7> The resin composition according to any one of <3-1> to <3-6>, wherein the recycled polycarbonate resin contains aluminum element at a ratio of 0.2 to 1000 ppm by mass and iron element at a ratio of 0.2 to 100 ppm by mass. <3-8> The resin composition according to any one of <3-1> to <3-7>, further containing carbon black in an amount of 0.1 to 3 parts by mass per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. <3-9> The resin composition according to any one of <3-1> to <3-8>, wherein the resin composition is molded into a 0.74 mm thick UL-94 test piece, and the flame retardancy according to the UL-94 test satisfies V-0. <3-10> The resin composition according to any one of <3-1> to <3-9>, wherein the recycled polycarbonate resin comprises at least one of a polycarbonate resin derived from a bottle, a polycarbonate resin derived from a meter cover, and a polycarbonate resin derived from a headlamp lens. <3-11> The recycled polycarbonate resin has a melt volume rate (MVR) of 4 to 30 cm3 measured in accordance with ISO 1133 under conditions of 300°C and a load of 1.20 kgf. 3the polyalkylene terephthalate resin comprises a polybutylene terephthalate resin; the flame retardant comprises a bromine-based flame retardant; and the resin composition according to any one of <3-1> to <3-10>, wherein the polyalkylene terephthalate resin has a viscosity of 1000 saturations, and the viscosity of the polyalkylene terephthalate resin is 100 saturations. <3-12> Pellets of the resin composition according to any one of <3-1> to <3-11>. <3-13> A molded article formed from the resin composition according to any one of <3-1> to <3-11>. <3-14> A molded article formed from the pellets according to <3-12>.

[0008] The present invention makes it possible to provide a resin composition containing a polyalkylene terephthalate resin, a recycled polycarbonate resin, and a flame retardant, which is capable of achieving physical properties comparable to those achieved when virgin polycarbonate resin is used or better than those achieved when virgin polycarbonate resin is used alone, as well as pellets and molded articles.

[0009] Hereinafter, a mode for carrying out the present invention (hereinafter simply referred to as "the present embodiment") will be described in detail. Note that the following present embodiment is an example for explaining the present invention, and the present invention is not limited to only this embodiment. Note that in this specification, the word "to" is used to mean that the numerical values ​​written before and after it are included as lower and upper limits. In this specification, various physical property values ​​and characteristic values ​​are those at 23°C unless otherwise specified. When the measurement methods etc. described in the standards shown in this specification vary depending on the fiscal year, they are based on the standards as of January 1, 2023, unless otherwise specified.

[0010] The resin composition of this embodiment contains 5 to 50 parts by mass of a flame retardant per 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin, and the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin in the total 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin is 10 / 90 to 90 / 10, and the polycarbonate resin contains a recycled polycarbonate resin, and the branching amount of the recycled polycarbonate resin is 50 to 3500 ppm by mass. By adopting such a configuration, a resin composition containing a polyalkylene terephthalate resin, a recycled polycarbonate resin (sometimes referred to in this specification as "recycled polycarbonate resin") and a flame retardant can be obtained, and the resin composition can achieve physical properties comparable to those of virgin polycarbonate resin, or better than those of virgin polycarbonate resin alone. For example, when a flame retardant is blended into a resin composition, impact resistance usually tends to be poor. However, in this embodiment, by using a specific recycled polycarbonate resin, high impact resistance tends to be achieved. Furthermore, the resin composition of this embodiment tends to maintain high flame retardancy, with flame retardancy equivalent to or better than that of virgin polycarbonate resin, and recycled products can be used, thereby reducing the environmental impact. Furthermore, the use of recycled polycarbonate resin tends to result in poor nominal strain at break. In this embodiment, by using a specific recycled polycarbonate resin, the nominal strain at break tends to be improved. Furthermore, the resin composition of this embodiment tends to be able to increase the crystallization temperature (Tc).

[0011] In addition, it is generally known that polycarbonate resins with a higher branching content have better flame retardancy. This is thought to be because the higher branching structure allows polycarbonate molecules to entangle with each other, making it less likely for molded articles to change shape during combustion and effectively suppressing dripping and other issues. It is also thought that the burnt surface of a molded article is less likely to crumble, thereby shortening the burning time. However, the present inventors have conducted research and found that when used in combination with a polyalkylene terephthalate resin, polycarbonate resins with a lower branching content have better flame retardancy. The reason for this is believed to be that higher branching facilitates transesterification between the terminal hydroxyl groups of the polycarbonate and the polyalkylene terephthalate resin, resulting in an increase in low-molecular-weight components and a decrease in thermal stability. In particular, recycled polycarbonate resins often contain polycarbonate resins with branched structures because they are made from a mixture of multiple raw materials, but the inventors have conducted research and found that by adjusting the branching content of recycled polycarbonate resins to 50 to 3,500 ppm by mass, it is possible to achieve flame retardancy comparable to that of virgin polycarbonate resins or better than that of virgin polycarbonate resins alone.As a result, recycled products can be used, thereby reducing the environmental impact.

[0012] <Polyalkylene terephthalate resin> The resin composition of the present embodiment contains a polyalkylene terephthalate resin. 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-tert-phenylene-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. Of 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 and / 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 usually 60 eq / ton or less, preferably 50 eq / ton or less, and more preferably 30 eq / ton or less. By setting it to 60 eq / ton or less, gas generation during melt molding of the resin composition tends to be more effectively suppressed. The lower limit of the amount of terminal carboxyl groups is not particularly specified, but is usually 3 eq / ton or more, preferably 5 eq / ton or more, and more preferably 10 eq / ton or more.

[0020] The amount of terminal carboxyl groups in the 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 during polymerization, or by reacting a terminal blocking agent.

[0021] The intrinsic viscosity of the polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) is preferably 0.40 dL / g or more, more preferably 0.50 dL / g or more, even more preferably 0.55 dL / g or more, even more preferably 0.60 dL / g or more, still more preferably 0.65 dL / g or more, and even more preferably 0.80 dL / g or more, 1.00 dL / g or more, 1.20 dL / g or more, or 1.23 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, and further, impact resistance tends to be improved, and nominal strain at break tends to be improved. The intrinsic viscosity of the polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) is preferably 1.50 dL / g or less, more preferably 1.40 dL / g or less, even more preferably 1.35 dL / g or less, even more preferably 1.30 dL / g or less, and even more preferably 1.2 dL / g or less, 0.86 dL / g or less, 0.80 dL / g or less, or 0.78 L / g or less. By setting the intrinsic viscosity at or below the upper limit, a decrease in the fluidity of the resin during injection molding tends to be suppressed, and the peak pressure during injection molding tends to be suppressed.

[0022] Intrinsic viscosity is measured by the following method. Polyalkylene terephthalate resin pellets are dissolved in a mixed solvent of phenol / 1,1,2,2-tetrachloroethane (1 / 1 by mass ratio) 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 number of seconds it takes for the sample solution and the solvent alone to fall at 30°C are 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 / η 0 -1, η is the number of seconds the sample solution falls, η 0 is the number of seconds for the solvent to fall, C is the concentration of the sample solution (g / dL), K H is Huggins' constant. H The intrinsic viscosity of the mixture is used. The fully automatic solution viscometer used is a product of 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, representative examples of which are polybutylene terephthalate resin and polyethylene terephthalate resin. These are similar to homopolyesters, i.e., preferably, 95 mol % or more of the entire resin is composed of terephthalic acid and 1,4-butanediol or ethylene glycol. The polyalkylene terephthalate resin is preferably polybutylene terephthalate resin and / or polyethylene terephthalate resin. Among these, the polyalkylene terephthalate resin preferably contains polybutylene terephthalate resin as the main component, more preferably 50% by mass or more of the polyalkylene terephthalate resin is polybutylene terephthalate resin, and even more preferably, more than 50% by mass of the polyalkylene terephthalate resin is polybutylene terephthalate resin. In this case, it is also preferable to contain polyethylene terephthalate resin in an amount of less than 50% by mass.

[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. Furthermore, 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 continuous melt polycondensation of a dicarboxylic acid component containing terephthalic acid as the main component and a diol component containing 1,4-butanediol as the main component.

[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% by mass, more preferably 5 to 30% by mass, and even more preferably 10 to 25% by 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 an isophthalic acid copolymerized polybutylene terephthalate resin is used as the modified polybutylene terephthalate resin, the proportion of the isophthalic acid component in all carboxylic acid components is preferably 1 to 30 mol%, more preferably 1 to 20 mol%, and even more preferably 3 to 15 mol%, in terms of carboxylic acid groups. 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 this embodiment is preferably 10% by mass or more, more preferably 20% by mass or more, and even more preferably 30% by mass or more, and preferably 60% by mass or less, and more preferably 50% by mass or less, based on 100% by mass of the resin composition. The resin composition of this embodiment may contain only one polyalkylene terephthalate resin (preferably polybutylene terephthalate resin), or may contain two or more types. When two or more types are contained, it is preferable that the total amount is within the above range. Furthermore, the polyalkylene terephthalate resin in the resin composition of this embodiment preferably contains 40% by mass or more of polybutylene terephthalate resin, more preferably 50% by mass or more, 55% by mass or more, 60% by mass or more, 70% by mass or more, 80% by mass or more, or 90% by mass or more, and particularly preferably 100% by mass.

[0030] <Polycarbonate Resin> The resin composition of this embodiment contains a polycarbonate resin. The polycarbonate resin is a homopolymer or copolymer 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 exchange method) can be used. By using a polycarbonate resin obtained by the melt method, the polycarbonate resin tends to have a branched structure more easily. Furthermore, even in the interfacial polymerization method, a polycarbonate resin having a branched structure can be obtained by using a branching agent during polymerization of the polycarbonate resin.

[0031] The dihydroxy compound used as the raw material is preferably an aromatic dihydroxy compound, more preferably bisphenol, and even more preferably bisphenol A. It is also possible to use a compound in which one or more tetraalkylphosphonium sulfonates are bonded to the above-mentioned aromatic dihydroxy compound.

[0032] In this embodiment, the polycarbonate resin preferably contains 90% by mass or more of the dihydroxy compound raw material monomer derived from bisphenol A, and more preferably 95% by mass or more of the dihydroxy compound derived from bisphenol A. The structural units represented by formulas (C1) to (C4) described below are also derived from bisphenol A. For example, they are produced by a transition reaction (Fries transition) occurring in the polymerization reaction system when polycarbonate is polymerized by a transesterification reaction of bisphenol A and diphenyl carbonate (melt method). The structural units represented by formulas (C1) to (C4) described below are also produced by the Fries transition of the polycarbonate resin derived from bisphenol A due to photodegradation caused by ultraviolet rays or the like. Two or more polycarbonate resins may be used in combination.

[0033] To adjust the molecular weight of the polycarbonate resin, a monovalent aromatic hydroxy compound may be used, such as m- and p-methylphenol, m- and p-propylphenol, p-tert-butylphenol, and p-long-chain alkyl-substituted phenol.

[0034] The polycarbonate resin used in this embodiment includes a recycled polycarbonate resin (recycled polycarbonate resin). Recycled polycarbonate resins often contain bisphenol A due to the thermal history of previous processes. However, by adjusting the bisphenol A content to 10 to 80 mass ppm of recycled polycarbonate resin, flame retardancy comparable to that of virgin polycarbonate resin or better than that of virgin polycarbonate resin alone can be obtained. Examples of recycled polycarbonate resins include those obtained by material recycling, in which recovered used polycarbonate resin molded bodies are crushed, washed, and reused, and those obtained by chemical recycling (chemical decomposition method). Those obtained by material recycling are preferred. Chemical recycling involves chemically decomposing recovered used polycarbonate resin molded bodies, returning them to their raw material level, and resynthesizing the polycarbonate resin. On the other hand, in material recycling, for example, foreign matter is removed from recovered used polycarbonate resin molded bodies, crushed, washed with an alkali, dried, and crushed into flakes or pelletized in an extruder. Note that polycarbonate resin that is not recycled polycarbonate resin is called virgin polycarbonate resin.

[0035] Examples of recycled polycarbonate resins include polycarbonate resins derived from bottles, polycarbonate resins derived from discs, polycarbonate resins derived from sheets (including polycarbonate resins derived from films), polycarbonate resins derived from meter covers (for example, electricity meter covers), and polycarbonate resins derived from headlamp lenses. At least one of polycarbonate resins derived from bottles, polycarbonate resins derived from meter covers, and polycarbonate resins derived from headlamp lenses is preferred, and polycarbonate resins derived from bottles and / or sheets are more preferred.

[0036] Examples of recycled polycarbonate resins include post-consumer recycled (PCR) products, which are made by collecting and recycling used products on the market, and post-industrial recycled (PIR) products, which are made by recycling materials generated in the manufacturing process of products before they are released on the market. Either type is acceptable, but from the viewpoint of reducing the environmental load, post-consumer recycled products are preferred.

[0037] The recycled polycarbonate resin used in this embodiment preferably contains 10 to 80 ppm by mass of bisphenol A. The content of bisphenol A in the recycled polycarbonate resin is preferably 15 ppm by mass or more, more preferably 20 ppm by mass or more, and even more preferably 25 ppm by mass or more. It is also preferably 70 ppm by mass or less, more preferably 60 ppm by mass or less, even more preferably 55 ppm by mass or less, even more preferably 50 ppm by mass or less, even more preferably 49 ppm by mass or less, even more preferably 45 ppm by mass or less, and even more preferably 40 ppm by mass or less, and even more preferably 35 ppm by mass or less, 30 ppm by mass or less. By setting the content at or above the lower limit, the flowability tends to be improved, and the availability of recycled polycarbonate resin tends to be improved. By setting the content at or below the upper limit, the flame retardancy tends to be further improved, and the amount of gas generated tends to be reduced. In addition, from the viewpoint of a balance between the availability, ease of production, and quality stability of the recycled polycarbonate resin, it is preferable to set the content within the above upper and lower limits. The content of bisphenol A in the recycled polycarbonate resin is measured according to the description in the Examples described later.

[0038] The branching amount of the recycled polycarbonate resin used in this embodiment is 50 to 3,500 ppm by mass. The branching amount of the recycled polycarbonate resin is preferably 100 ppm by mass or more, more preferably 200 ppm by mass or more, even more preferably 500 ppm by mass or more, even more preferably 1,000 ppm by mass or more, even more preferably 1,500 ppm by mass or more, even more preferably 2,000 ppm by mass or more, and preferably 3,000 ppm by mass or less, more preferably 2,500 ppm by mass or less. Setting the branching amount to above the lower limit tends to further improve the drip prevention effect during combustion. Setting the branching amount to below the upper limit tends to suppress resin decomposition due to transesterification between the polyalkylene terephthalate resin and the polycarbonate resin, tend to increase the crystallization temperature, tend to shorten the combustion time, and tend to reduce the amount of gas generated. The branching amount of the recycled polycarbonate resin is measured as described in the Examples below.

[0039] The recycled polycarbonate resin used in this embodiment may contain one or more structural units represented by any one of formulas (C1) to (C4).

[0040] The branching amount of the recycled polycarbonate resin used in this embodiment is 50 to 3,500 ppm by mass. The branching amount of the recycled polycarbonate resin is preferably 100 ppm by mass or more, more preferably 200 ppm by mass or more, even more preferably 500 ppm by mass or more, even more preferably 1,000 ppm by mass or more, even more preferably 1,500 ppm by mass or more, even more preferably 2,000 ppm by mass or more, and preferably 3,000 ppm by mass or less, more preferably 2,500 ppm by mass or less. Setting the branching amount to above the lower limit tends to further improve the drip prevention effect during combustion. Setting the branching amount to below the upper limit tends to suppress resin decomposition due to transesterification between the polyalkylene terephthalate resin and the polycarbonate resin, tend to increase the crystallization temperature, tend to shorten the combustion time, and tend to reduce the amount of gas generated. The branching amount of the recycled polycarbonate resin is measured as described in the Examples below.

[0041] The recycled polycarbonate resin used in this embodiment preferably has a PSA content of 5 ppm by mass or more, more preferably 30 ppm by mass or more, even more preferably 50 ppm by mass or more, even more preferably 100 ppm by mass or more, even more preferably 200 ppm by mass or more, and preferably 700 ppm by mass or less, more preferably 600 ppm by mass or less, even more preferably 500 ppm by mass or less, even more preferably 380 ppm by mass or less, and even more preferably 350 ppm by mass or less, when hydrolyzed, relative to 100 parts by mass of the recycled polycarbonate. By setting the PSA content at or above the lower limit, the drip prevention effect during a combustion test tends to be improved. By setting the PSA content at or below the upper limit, decomposition of the resin due to transesterification between the polyalkylene terephthalate resin and the polycarbonate resin tends to be suppressed, resulting in excellent thermal stability, a shorter combustion time, and a reduced amount of gas generated.

[0042] The recycled polycarbonate resin used in this embodiment, when hydrolyzed, preferably has a PSA-Me content of 10 ppm by mass or more, more preferably 50 ppm by mass or more, even more preferably 150 ppm by mass or more, even more preferably 300 ppm by mass or more, even more preferably 500 ppm by mass or more, and preferably 2000 ppm by mass or less, more preferably 1500 ppm by mass or less, even more preferably 1000 ppm by mass or less, even more preferably 900 ppm by mass or less, and even more preferably 800 ppm by mass or less. By setting the PSA-Me content at or above the lower limit, the drip prevention effect during combustion tests tends to be further improved. Furthermore, by setting the PSA-Me content at or below the upper limit, decomposition of the resin due to transesterification between the polyalkylene terephthalate resin and the polycarbonate resin tends to be suppressed, leading to excellent thermal stability, a tendency for combustion time to be shortened, and a tendency for the amount of gas generated to be reduced.

[0043] The recycled polycarbonate resin used in this embodiment may have a PBA content of 0 parts by mass or more, preferably 0.01 ppm by mass or more, more preferably 10 ppm by mass or more, even more preferably 30 ppm by mass or more, still more preferably 100 ppm by mass or more, even more preferably 400 ppm by mass or more, and preferably 2000 ppm by mass or less, more preferably 1500 ppm by mass or less, even more preferably 1000 ppm by mass or less, still more preferably 900 ppm by mass or less, and even more preferably 800 ppm by mass or less, when the PBA content is equal to or more than the lower limit, the effect of preventing dripping during a combustion test tends to be further improved. Furthermore, by setting the content to be equal to or less than the upper limit, decomposition of the resin due to transesterification between the polyalkylene terephthalate resin and the polycarbonate resin tends to be suppressed, the thermal stability tends to be excellent, the combustion time tends to be shortened, and the amount of gas generated tends to be reduced.

[0044] The recycled polycarbonate resin used in this embodiment, when hydrolyzed, preferably has a dicarboxylic acid content (two types of dicarboxylic acids DA1 and DA2 described below) of 1 ppm by mass or more, more preferably 10 ppm by mass or more, even more preferably 100 ppm by mass or more, even more preferably 200 ppm by mass or more, even more preferably 300 ppm by mass or more, relative to 100 parts by mass of recycled polycarbonate, and preferably 1500 ppm by mass or less, more preferably 1000 ppm by mass or less, even more preferably 900 ppm by mass or less, even more preferably 800 ppm by mass or less, and even more preferably 700 ppm by mass or less. By making the content above the lower limit, the effect of preventing dripping during a combustion test tends to be further improved. Furthermore, by setting the content to be equal to or less than the upper limit, decomposition of the resin due to transesterification between the polyalkylene terephthalate resin and the polycarbonate resin tends to be suppressed, the thermal stability tends to be excellent, the combustion time tends to be shortened, and the amount of gas generated tends to be reduced.

[0045]

[0046] The contents of PSA, PSA-Me, PBA, and dicarboxylic acids (DA1, DA2) produced by hydrolysis of recycled polycarbonate resin are measured according to the description in the examples below.

[0047] The resin composition of this embodiment is a recycled polycarbonate resin having a melt volume rate (MVR) of 2 to 30 cm3 measured in accordance with ISO 1133 under conditions of 300°C and a load of 1.20 kgf. 3 The MVR of the recycled polycarbonate resin is preferably 3 cm / 10 min. 3 / 10 minutes or more is more preferable, and 4 cm 3 / 10 minutes or more is more preferable, 3 / 10 minutes or more is more preferable, and 6 cm 3 / 10 minutes or more is more preferable, and 3 / 10 minutes or less is preferable, and 15 cm 3 / 10 minutes or less is more preferable, and 11 cm 3 / 10 minutes or less is more preferable, and 10 cm 3 / 10 minutes or less is more preferable, 3 / 10 minutes or less is even more preferable, 3 / 10 minutes or less, and even more preferably 7 cm 3 It is particularly preferable that the MVR is 10 minutes or less. By making the MVR equal to or greater than the lower limit, the flowability tends to be improved. Furthermore, by making the MVR equal to or less than the upper limit, the mechanical properties tend to be improved, and the impact resistance tends to be improved. The resin composition of the present embodiment may contain only one type of recycled polycarbonate resin, or may contain two or more types. When two or more types are contained, it is preferable that the MVR of the mixture is in the above range.

[0048] The polydispersity (Mw / Mn) of the recycled polycarbonate resin is preferably 2.6 or more, and is preferably 3.5 or less, and more preferably 3.3 or less. The polydispersity of the recycled polycarbonate resin is measured according to the description in the examples described later.

[0049] Recycled polycarbonate resins typically have a higher metal element content than virgin products due to the resin consumption and recycling process. However, some recycled polycarbonate resins do not have a high metal element content. From the viewpoints of availability, ease of production, and quality stability of recycled polycarbonate resins, the recycled polycarbonate resin used in this embodiment preferably has an aluminum element content of 0.2 to 1,000 ppm by mass per 100 parts by mass of the recycled polycarbonate resin. Furthermore, the content of the aluminum element is preferably 0.3 mass ppm or more, more preferably 0.5 mass ppm or more, even more preferably 1 mass ppm or more, even more preferably 2 mass ppm or more, even more preferably 5 mass ppm or more, even more preferably 7 mass ppm or more, particularly more preferably 8 mass ppm or more, and more preferably 500 mass ppm or less, even more preferably 300 mass ppm or less, even more preferably 100 mass ppm or less, even more preferably 50 mass ppm or less, even more preferably 30 mass ppm or less, even more preferably 15 mass ppm or less, and particularly more preferably 10 mass ppm or less, relative to 100 mass parts of the recycled polycarbonate resin. By setting the content at or above the lower limit, laser marking properties tend to be improved. On the other hand, by setting the content at or below the upper limit, insulating properties such as dielectric breakdown strength tend to be further improved, tracking resistance tends to be improved, and the amount of gas generated tends to be reduced.

[0050] From the viewpoints of the availability, ease of production, and quality stability of recycled polycarbonate resins, in this embodiment, it is preferable that the recycled polycarbonate resin contains iron element in a proportion of 0.2 to 100 ppm by mass relative to the polycarbonate resin. The iron element content is more preferably 0.8 ppm by mass or more, even more preferably 1 ppm by mass or more, even more preferably 2 ppm by mass or more, even more preferably 3 ppm by mass or more, even more preferably 4 ppm by mass or more, and more preferably 50 ppm by mass or less, even more preferably 35 ppm by mass or less, even more preferably 20 ppm by mass or less, even more preferably 15 ppm by mass or less, even more preferably 10 ppm by mass or less, and particularly preferably 8 ppm by mass or less. By setting the iron element content at or above the lower limit, laser marking properties tend to be improved. Furthermore, by making the thickness equal to or less than the upper limit, the insulating properties such as the dielectric breakdown strength tend to be further improved, the tracking resistance tends to be improved, and the amount of gas generated tends to be reduced.

[0051] From the viewpoints of the availability, ease of production, and quality stability of the recycled polycarbonate resin, in this embodiment, it is preferable that the recycled polycarbonate resin contains phosphorus in a proportion of 1 to 200 ppm by mass relative to the polycarbonate resin. The phosphorus content is more preferably 2 ppm by mass or more, even more preferably 3 ppm by mass or more, even more preferably 4 ppm by mass or more, and even more preferably 5 ppm by mass or more, and more preferably 150 ppm by mass or less, even more preferably 100 ppm by mass or less, even more preferably 50 ppm by mass or less, and even more preferably 10 ppm by mass or less. By setting the content at or above the lower limit, transesterification of the mixture of polyalkylene terephthalate resin and recycled polycarbonate resin is suppressed, and the heat resistance of the resin tends to be improved. Furthermore, by setting the content at or below the upper limit, insulating properties such as dielectric breakdown strength tend to be further improved, the amount of gas generated tends to be reduced, and hydrolysis resistance tends to be improved.

[0052] The resin composition of this embodiment may contain only recycled polycarbonate resin as the polycarbonate resin, or may contain virgin polycarbonate resin in addition to the recycled polycarbonate resin. The content of recycled polycarbonate resin in the resin composition of this embodiment is preferably 50 parts by mass or more, more preferably 60 parts by mass or more, even more preferably 70 parts by mass or more, even more preferably 80 parts by mass or more, and even more preferably 90 parts by mass or more, and is 100 parts by mass or less, per 100 parts by mass of the polycarbonate resin. By setting the content at or above the lower limit, recyclability is improved. By setting the content at or below the upper limit, production stability and quality stability tend to be further improved.

[0053] <Blend Ratio of Polyalkylene Terephthalate Resin and Polycarbonate Resin> In the resin composition of this embodiment, the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin per 100 parts by mass of the polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) and the polycarbonate resin is 10 / 90 to 90 / 10, preferably 80 / 20 to 20 / 80, and more preferably 30 / 70 to 55 / 45. By using such a blend ratio, molded articles having excellent physical properties can be obtained, and the balance between chemical resistance and dimensional stability tends to be further improved. The blend ratio is preferably 20 parts by mass or more, more preferably 30 parts by mass or more, even more preferably 35 parts by mass or more, even more preferably 40 parts by mass or more, even more preferably 45 parts by mass or more, and even more preferably 50 parts by mass or more, depending on the application, etc., and even more preferably 60 parts by mass or more, 70 parts by mass or more, 75 parts by mass or more, particularly more preferably 85 parts by mass or less, and depending on the application, etc., it may be 50 parts by mass or less, or 49 parts by mass or less. The resin composition of this embodiment may contain only one type of polyalkylene terephthalate resin and one type of polycarbonate resin, or may contain two or more types. When two or more types are contained, it is preferable that the total amount is within the above range.

[0054] The total amount of polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) and polycarbonate resin (preferably recycled polycarbonate resin) in the resin composition of this embodiment is preferably 10% by mass or more, more preferably 20% by mass or more, even more preferably 30% by mass or more, even more preferably 40% by mass or more, even more preferably 45% by mass or more, and preferably 90% by mass or less, more preferably 80% by mass or less, even more preferably 70% by mass or less, even more preferably 60% by mass or less, and even more preferably 55% by mass or less. By setting it to the lower limit or more, moldability tends to be improved, the nominal fracture strain tends to be improved, and impact resistance tends to be improved. Furthermore, by setting it to the upper limit or less, the appearance of the molded article tends to be improved, and flame retardancy tends to be improved.

[0055] <Flame Retardant> The resin composition of this embodiment contains a flame retardant. By including a flame retardant, flame retardancy can be achieved. Examples of flame retardants include halogen-based flame retardants, phosphorus-based flame retardants (metal phosphinate, melamine polyphosphate, etc.), nitrogen-based flame retardants (melamine cyanurate, etc.), and metal hydroxides (magnesium hydroxide, etc.). Phosphorus-based flame retardants and halogen-based flame retardants are preferred, and halogen-based flame retardants are more preferred. As phosphorus-based flame retardants, metal phosphinate is more preferred. As halogen-based flame retardants, bromine-based flame retardants are more preferred. Of the flame retardants contained in the resin composition of this embodiment, the proportion of bromine-based flame retardants is preferably 50% by mass or more, more preferably 60% by mass or more, even more preferably 70% by mass or more, even more preferably 80% by mass or more, even more preferably 90% by mass or more, and 100% by mass or less.

[0056] When a brominated flame retardant is used as the flame retardant, the type thereof is not particularly limited, but brominated phthalimide, brominated poly(meth)acrylate, brominated polycarbonate, brominated epoxy, and brominated polystyrene are preferred, brominated polycarbonate, brominated poly(meth)acrylate, and brominated epoxy are more preferred, and brominated polycarbonate is even more preferred.

[0057] The brominated phthalimide is preferably one represented by formula (1). (In formula (1), D represents an alkylene group, an arylene group, or —S(═O) 2 represents a group consisting of a combination of two or more of -, -C(=O)-, and -O-, and i is an integer of 1 to 4.

[0058] In formula (1), D is an alkylene group, an arylene group, or —S(═O) 2 represents a group consisting of a combination of two or more of -, -C(=O)-, and -O-, and is an alkylene group or an arylene group and -S(=O) 2 A group consisting of a combination of at least one of -, -C(=O)-, and -O- is preferred, and an alkylene group or an arylene group and -S(=O) 2 A group formed by combining one of -, -C(=O)-, and -O- is more preferred, and an alkylene group is even more preferred. The group formed by combining 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, and more preferably a methylene group, ethylene group, propylene group, or butylene group. The arylene group is preferably a phenylene group. i is an integer of 1 to 4, and preferably 4.

[0059] 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.

[0060] The brominated phthalimide represented by formula (1) is preferably a brominated phthalimide represented by formula (2). (In formula (2), i is an integer of 1 to 4.) i is an integer of 1 to 4, and is preferably 4.

[0061] 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-containing benzyl (meth)acrylate with another vinyl monomer, and the bromine atoms are attached to a benzene ring, with 1 to 5 bromine atoms, preferably 4 to 5 bromine atoms, attached to each benzene ring.

[0062] 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.

[0063] 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.

[0064] These are usually used in an equimolar amount or less, preferably 0.5 times or less, of the amount of benzyl (meth)acrylate containing a bromine atom.

[0065] Furthermore, examples of vinyl monomers that can be used include xylene diacrylate, xylene dimethacrylate, tetrabromxylene diacrylate, tetrabromxylene dimethacrylate, butadiene, isoprene, and divinylbenzene. 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.

[0066] 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 benzene rings, with 1 to 5 bromine atoms, preferably 4 to 5 bromine atoms attached per benzene ring.

[0067] As the brominated poly(meth)acrylate, pentabromobenzyl poly(meth)acrylate is preferred because of its high bromine content.

[0068] 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 it to the lower limit or higher, 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 it to the upper limit or lower, the flowability of the resin composition tends to be further improved.

[0069] 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. Specific examples of brominated polycarbonates include brominated bisphenol A, particularly brominated polycarbonates obtained from tetrabromobisphenol A. Examples of terminal structures include phenyl groups, 4-t-butylphenyl groups, and 2,4,6-tribromophenyl groups. Those having a 2,4,6-tribromophenyl group as a terminal group structure are particularly preferred.

[0070] The average number of carbonate structural units in the brominated polycarbonate may be appropriately selected and determined, but is preferably 2 to 30, more preferably 3 to 15, and even more preferably 3 to 10.

[0071] 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.

[0072] 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.

[0073] 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.

[0074] 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 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 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. By setting the weight average molecular weight at or below the upper limit, the flowability of the resin composition tends to be further improved. 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.

[0075] A brominated epoxy oligomer can also be used as the brominated epoxy. In this case, for example, by using an oligomer having a Mw of 5,000 or less in a proportion of about 50% by mass or less, the flame retardancy, mold releasability, and flowability can be appropriately adjusted. The bromine atom content in the brominated epoxy compound is optional, but in order to impart 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, with the upper limit being 60% by mass, and preferably 55% by mass or less.

[0076] The brominated polystyrene preferably includes a brominated polystyrene containing a constituent unit represented by formula (3). (In formula (3), t is an integer of 1 to 5, and n is the number of constitutional units.)

[0077] Brominated polystyrene may be produced by either brominating polystyrene or polymerizing brominated styrene monomers, but polymerizing brominated styrene is preferred because it has a low amount of free bromine (atoms). In formula (3), the CH group bonded to the brominated benzene 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 types with different structures, and may contain units derived from styrene monomers with different bromine numbers in a single molecular chain.

[0078] 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 bromine groups include poly(2,4,6-tribromostyrene), poly(2,4,5-tribromostyrene), poly(2,4,6-tribromostyrene), poly(2,4,5-tribromostyrene), and poly(2,4,6-tribromostyrene). Of these, 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.

[0079] 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 brominated polystyrene described above, the weight average molecular weight (Mw) is preferably 50,000 to 70,000, and in the case of brominated polystyrene obtained by polymerization, the weight average molecular weight (Mw) is preferably about 10,000 to 30,000.

[0080] 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 it to the lower limit or more, 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.

[0081] 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 moiety represented by formula (4) or formula (5) and a metal ion of the cation moiety is any one of calcium, magnesium, aluminum, and zinc.

[0082] (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, 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 the aryl group has a substituent, it is preferably an alkyl group having 1 to 3 carbon atoms. It is also preferable that the aryl group is 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 (5) is preferred. In this embodiment, aluminum phosphinate is preferred.

[0083] 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 metal phosphinates include magnesium methanedi(methylphosphinate), aluminum methanebis(methylphosphinate), zinc methanebis(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 of the metal phosphinates, please refer to paragraphs 0052 to 0058 of WO 2010 / 010669, the contents of which are incorporated herein by reference.

[0084] The content of the flame retardant (preferably a brominated flame retardant) in the resin composition of this embodiment is, relative to 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin, the lower limit is 5 parts by mass or more, preferably 7 parts by mass or more, more preferably 8 parts by mass or more, even more preferably 10 parts by mass or more, even more preferably 11 parts by mass or more, even more preferably 13 parts by mass or more, even more preferably 14 parts by mass or more, and particularly more preferably 15 parts by mass or more. By setting the content at or above the lower limit, the flame retardancy of the resulting molded article tends to be further improved. The upper limit of the content of the flame retardant is, relative to 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin, 50 parts by mass or less, preferably 45 parts by mass or less, more preferably 40 parts by mass or less, even more preferably 35 parts by mass or less, even more preferably 30 parts by mass or less, even more preferably 25 parts by mass or less, even more preferably 20 parts by mass or less, and particularly more preferably 15 parts by mass or less. By setting the content to the upper limit or less, it is possible to more effectively prevent a decrease in the mechanical strength of the obtained molded article. The resin composition of this embodiment may contain only one flame retardant, or may contain two or more flame retardants. When two or more flame retardants are contained, it is preferable that the total amount is in the above range.

[0085] <Elastomer> The resin composition of this embodiment preferably contains an elastomer. By containing an elastomer, the impact resistance of the resulting molded article tends to be further improved. The type of elastomer is not particularly limited, and known elastomers can be used.

[0086] An example of an elastomer is an elastomer containing an epoxy group, which tends to have a higher affinity with polybutylene terephthalate resin, and thus tends to produce molded products with high impact resistance.

[0087] A first embodiment of the epoxy group-containing elastomer is a copolymer obtained by copolymerizing an α-olefin, a glycidyl ester of an α,β-unsaturated acid, and, if necessary, an unsaturated monomer copolymerizable therewith. Of all the copolymerization components in the copolymer, it is preferable to use 60 mass % or more of the α-olefin and the glycidyl ester of an α,β-unsaturated acid.

[0088] Examples of α-olefins include ethylene, propylene, butene-1, and pentene-1. Two or more of these may be used. Examples of glycidyl esters of α,β-unsaturated acids include glycidyl acrylate, glycidyl methacrylate, glycidyl ethacrylate, and glycidyl itaconate. Two or more of these may be used. Examples of vinyl monomers copolymerizable with the above components include vinyl ethers, vinyl esters such as vinyl acetate and vinyl propionate, acrylic and methacrylic acid esters such as methyl, ethyl, propyl, and butyl, acrylonitrile, and styrene. Two or more of these may be used.

[0089] Preferred examples of the epoxy group-containing elastomer of the first embodiment include ethylene / glycidyl methacrylate copolymer, ethylene / glycidyl methacrylate / vinyl acetate copolymer, ethylene / glycidyl methacrylate / alkyl acrylate copolymer, and ethylene / alkyl acrylate / vinyl acetate copolymer. In particular, from the viewpoint of excellent toughness and further improving the moist heat resistance and impact resistance of molded articles, ethylene / glycidyl methacrylate / alkyl acrylate (preferably butyl acrylate) copolymer is preferred. Specific examples of the epoxy group-containing elastomer of the first embodiment are available from Arkema under the trade names "Rotader" (registered trademark) AX8900 and AX8700.

[0090] A second embodiment of the epoxy group-containing elastomer is a core-shell elastomer. The use of a core-shell elastomer facilitates dispersion in polybutylene terephthalate resin due to its small molecular particle size, and the reaction of the reactive groups tends to increase welding strength. Examples of core-shell elastomers include those in which a monomer component is graft-copolymerized onto a core polymer. The core is preferably a rubbery polymer, such as an acrylonitrile-acrylic rubbery polymer-styrene graft copolymer (ASA resin), a methyl methacrylate-acrylic rubbery polymer-styrene graft copolymer (MSA resin), a methyl methacrylate-acrylonitrile-acrylic rubbery polymer-styrene graft copolymer (MASA resin), or a polyorganosiloxane-containing rubbery polymer. A polyorganosiloxane-containing rubbery polymer is preferred. The polyorganosiloxane-containing rubbery polymer typically has a glass transition temperature of 0°C or below, preferably −20°C or below, and more preferably −30°C or below. Specific examples of the rubber component are not particularly limited as long as it contains polyorganosiloxane rubber, and include polyorganosiloxane rubber, and composite rubber (IPN type) of polyorganosiloxane rubber and polyalkyl acrylate rubber.

[0091] Specific examples of the monomer component graft copolymerizable with the core include aromatic vinyl compounds, vinyl cyanide compounds, (meth)acrylic acid ester compounds, (meth)acrylic acid compounds, epoxy group-containing (meth)acrylic acid ester compounds such as glycidyl (meth)acrylate, maleimide compounds such as maleimide, N-methylmaleimide, and N-phenylmaleimide; α,β-unsaturated carboxylic acid compounds such as maleic acid, phthalic acid, and itaconic acid, and anhydrides thereof (for example, maleic anhydride, etc.).

[0092] Specific examples of rubber polymers, aromatic vinyl compounds, vinyl cyanide compounds, and (meth)acrylic acid ester compounds are described in paragraphs 0042 to 0046 of JP 2019-059813 A, the contents of which are incorporated herein by reference.

[0093] The epoxy group-containing elastomer of the second embodiment is preferably a compound obtained by graft polymerizing an epoxy group-containing (meth)acrylic acid ester compound onto a polyorganosiloxane-containing rubbery polymer (preferably a composite rubber of polyorganosiloxane rubber and polyalkyl acrylate rubber).

[0094] Specific examples of the elastomer containing an epoxy group according to the second embodiment include "Metablen (registered trademark, the same applies hereinafter) S-2002" and "Metablen S-2200" manufactured by Mitsubishi Rayon Co., Ltd.

[0095] Another example of the elastomer is a graft copolymer obtained by graft copolymerizing a rubber component with a monomer component copolymerizable therewith. The graft copolymer may be produced by any of bulk polymerization, solution polymerization, suspension polymerization, emulsion polymerization, etc., and the copolymerization method may be either single-stage grafting or multi-stage grafting.

[0096] The rubber component usually has a glass transition temperature of 0°C or lower, preferably -20°C or lower, and more preferably -30°C or lower. Specific examples of the rubber component include polybutadiene rubber, polyisoprene rubber, polybutyl acrylate, poly(2-ethylhexyl acrylate), polyalkyl acrylate rubbers such as butyl acrylate-2-ethylhexyl acrylate copolymers, silicone rubbers such as polyorganosiloxane rubber, butadiene-acrylic composite rubber, IPN (Interpenetrating Polymer Network) composite rubbers consisting of polyorganosiloxane rubber and polyalkyl acrylate rubber, styrene-butadiene rubber, ethylene-α-olefin rubbers such as ethylene-propylene rubber, ethylene-butene rubber, and ethylene-octene rubber, ethylene-acrylic rubber, and fluororubber. These may be used alone or in combination of two or more. Among these, polybutadiene rubber, polyalkyl acrylate rubber, polyorganosiloxane rubber, IPN type composite rubber consisting of polyorganosiloxane rubber and polyalkyl acrylate rubber, and styrene-butadiene rubber are preferred in terms of mechanical properties and surface appearance.

[0097] Specific examples of the monomer component capable of graft copolymerization with the rubber component include the epoxy group-containing elastomer, and are the same as the specific examples of the monomer component capable of graft copolymerization with the rubber component described above.

[0098] The graft copolymer copolymerized with a rubber component is preferably a core / shell graft copolymer in terms of impact resistance and surface appearance. Among these, a core / shell graft copolymer is particularly preferred, which comprises a core layer made of at least one rubber component selected from polybutadiene-containing rubber, polybutyl acrylate-containing rubber, polyorganosiloxane rubber, and an IPN-type composite rubber composed of polyorganosiloxane rubber and polyalkyl acrylate rubber, and a shell layer formed by copolymerizing a (meth)acrylic acid ester around the core layer. The core / shell graft copolymer preferably contains 40% by mass or more of the rubber component, more preferably 60% by mass or more. Furthermore, it is preferable that the (meth)acrylic acid content be 10% by mass or more. Note that the core / shell type in this embodiment does not necessarily have to be one in which the core layer and the shell layer are clearly distinguishable; it is intended to broadly include compounds obtained by graft polymerizing a rubber component around the core portion.

[0099] Preferred specific examples of these core / shell type graft copolymers include methyl methacrylate-butadiene-styrene copolymer (MBS), methyl methacrylate-acrylonitrile-butadiene-styrene copolymer (MABS), methyl methacrylate-butadiene copolymer (MB), methyl methacrylate-acrylic rubber copolymer (MA), methyl methacrylate-acrylic rubber-styrene copolymer (MAS), methyl methacrylate-acrylic-butadiene rubber copolymer, methyl methacrylate-acrylic-butadiene rubber-styrene copolymer, methyl methacrylate-(acrylic-silicone IPN rubber) copolymer, etc. One of these rubbery polymers may be used alone, or two or more of them may be used in combination.

[0100] Examples of such elastomers include "Paraloid (registered trademark, the same applies hereinafter) EXL2602," "Paraloid (registered trademark, the same applies hereinafter) EXL2603," "Paraloid (registered trademark, the same applies hereinafter) EXL2655," "Paraloid (registered trademark, the same applies hereinafter) EXL2311," "Paraloid (registered trademark, the same applies hereinafter) EXL2313," "Paraloid (registered trademark, the same applies hereinafter) EXL2315," "Paraloid (registered trademark, the same applies hereinafter) EXL230," "Paraloid (registered trademark, the same applies hereinafter) EXL2315 ... XPA" and others.

[0101] Another example of the elastomer is an acrylic block copolymer, which includes a hard segment made of a methyl methacrylate block and a soft segment made of an alkyl acrylate block.

[0102] The acrylic block copolymer is preferably a triblock copolymer having two hard segment blocks on either side of a soft segment block, or a diblock copolymer having one soft segment block and one hard segment block. That is, the acrylic block copolymer in this embodiment preferably has a triblock structure consisting of a methyl methacrylate block-alkyl acrylate block-methyl methacrylate block, or a diblock structure consisting of a methyl methacrylate block-alkyl acrylate block.

[0103] Examples of alkyl acrylates constituting the soft segment include n-propyl acrylate, isopropyl acrylate, n-butyl acrylate, isobutyl acrylate, tert-butyl acrylate, n-pentyl acrylate, n-hexyl acrylate, cyclohexyl acrylate, n-heptyl acrylate, n-octyl acrylate, 2-ethylhexyl acrylate, nonyl acrylate, decyl acrylate, dodecyl acrylate, phenyl acrylate, toluyl acrylate, benzyl acrylate, isobornyl acrylate, 2-methoxyethyl acrylate, 3-methoxybutyl acrylate, 2-hydroxyethyl acrylate, 2-hydroxypropyl acrylate, stearyl acrylate, glycidyl acrylate, 2-aminoethyl acrylate, and γ-(acryloyloxypropyl)trimethicone. Examples of suitable acrylates include xysilane, γ-(acryloyloxypropyl)dimethoxymethylsilane, ethylene oxide adduct of acrylic acid, trifluoromethylmethyl acrylate, 2-trifluoromethylethyl acrylate, 2-perfluoroethylethyl acrylate, 2-perfluoroethyl-2-perfluorobutylethyl acrylate, 2-perfluoroethyl acrylate, perfluoromethyl acrylate, diperfluoromethylmethyl acrylate, 2-perfluoromethyl-2-perfluoroethylmethyl acrylate, 2-perfluorohexylethyl acrylate, 2-perfluorodecylethyl acrylate, and 2-perfluorohexadecylethyl acrylate, and among these, butyl acrylate or butyl acrylate / 2-ethylhexyl acrylate is preferred.

[0104] The acrylic block copolymer is not particularly limited as long as it can exhibit the effects of the present invention. Among the above, it is preferable that the acrylic block copolymer has a diblock structure consisting of a methyl methacrylate block-butyl acrylate block or a methyl methacrylate block-butyl acrylate / 2-ethylhexyl acrylate block, or a triblock structure consisting of a methyl methacrylate block-butyl acrylate block-methyl methacrylate block or a methyl methacrylate block-butyl acrylate / 2-ethylhexyl acrylate block-methyl methacrylate block.

[0105] In the acrylic block copolymer, the ratio of hard segments to soft segments is preferably in the range of 3:97 to 40:60 by mass, more preferably 5:95 to 35:65. The greater the proportion of soft segments, the more the vinyl chloride resin can be softened. However, if the proportion of hard segments is too low, the compatibility with the vinyl chloride resin decreases as described above, resulting in poor moldability. On the other hand, the smaller the proportion of soft segments, the less efficient the vinyl chloride resin softening becomes.

[0106] Examples of commercially available acrylic block copolymers include LA1892, LA4285, LA2270, LA2250, LA2140, LA2330, and LA3320, which are part of the LA series of Kuraray Co., Ltd.'s Kuraryt (registered trademark), and M51, M52, and M22, which are part of the Nanostrength (registered trademark) series of Arkema Co., Ltd. In addition, acrylic copolymers using butyl acrylate / 2-ethylhexyl acrylate as the soft segment are commercially available as LK9243 and KL-LK9333, which are part of the LK series of Kuraray Co., Ltd.'s Kuraryt (registered trademark).

[0107] The elastomer used in this embodiment preferably has a melt mass flow rate (MFR) of 1 g / 10 min or more, more preferably 2 g / 10 min or more, and preferably 15 g / 10 min or less, and even more preferably 10 g / 10 min or less, as measured in accordance with ISO 1133 at 190°C and a load of 2.16 kgf. When the resin composition of this embodiment contains two or more elastomers, the MFR of the elastomers is a weighted average value.

[0108] In addition to the above, the elastomer may be any of the elastomers described in paragraphs

[0075] to

[0088] of JP-A-2012-251061, the elastomers described in paragraphs

[0101] to

[0107] of JP-A-2012-177047, the elastomers described in paragraphs

[0076] to

[0087] of JP-A-2016-98242, and the elastomers described in paragraphs

[0080] to

[0087] of JP-A-2019-11514, the contents of which are incorporated herein by reference.

[0109] In this embodiment, it is preferable to use an epoxy group-containing elastomer (preferably the epoxy group-containing elastomer of the first embodiment) in combination with an acrylic block copolymer, which tends to improve fluidity and impact resistance in a well-balanced manner.

[0110] When the resin composition of this embodiment contains an elastomer, the content thereof is preferably 1 part by mass or more, more preferably 3 parts by mass or more, even more preferably 5 parts by mass or more, even more preferably 7 parts by mass or more, even more preferably 8 parts by mass or more, and even more preferably 9 parts by mass or more, per 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin. The content is preferably 30 parts by mass or less, more preferably 25 parts by mass or less, even more preferably 20 parts by mass or less, even more preferably 20 parts by mass or less, even more preferably 15 parts by mass or less, and may be 12 parts by mass or less, or even 10 parts by mass or less. By setting the content at or above the lower limit, impact resistance tends to be further improved. By setting the content at or below the upper limit, fluidity tends to be improved, and high flame retardancy tends to be easily achieved. The resin composition of this embodiment may contain only one type of elastomer, or may contain two or more types. When two or more types are contained, the total amount is preferably within the above range.

[0111] <Flame Retardant Auxiliary Agent> The resin composition of the present embodiment may contain a flame retardant auxiliary agent. By containing a flame retardant auxiliary agent, the flame retardancy of the molded article can be further improved. The flame retardant auxiliary agent is particularly preferably used when a halogen-based flame retardant agent is contained. Examples of the flame retardant auxiliary agent used in the present embodiment include antimony compounds, and antimony trioxide (Sb 2 O 3 ), antimony tetroxide (Sb 2 O 4 ), antimony pentoxide (Sb 2 O 5), sodium antimonate, etc. In particular, from the viewpoint of impact resistance, antimony oxide, especially antimony trioxide, is preferred. 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%, even 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.

[0112] 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 and the polycarbonate resin combined. 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 and the polycarbonate resin combined. 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 this embodiment may contain only one type of flame retardant aid, or may contain two or more types. When two or more types are contained, the total amount is preferably within the above range.

[0113] <Anti-Drip Agent> The resin composition of this embodiment can also contain an anti-dripping agent. Polytetrafluoroethylene (PTFE) is preferred as the anti-dripping agent, and it is preferable that the anti-dripping agent 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 PTFE with reduced perfluorooctanoic acid (PFOA) or PFOA-free content. 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, per 100 parts by mass of the polyalkylene terephthalate resin and polycarbonate resin combined. 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 sufficiently effective. Furthermore, by setting the content at or below the upper limit, the appearance of the molded article tends to be improved, and fluidity tends to be improved. The content of the anti-dripping agent is more preferably 0.5 to 10 parts by mass per 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin. The resin composition of this 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 within the above range.

[0114] <Transesterification inhibitor> The resin composition of this embodiment may contain a transesterification inhibitor. By including a transesterification inhibitor, a resin composition or molded article having excellent thermal stability can be obtained. Preferred examples of the transesterification inhibitor include phosphates and / or phosphoric acid. Examples of phosphates include zinc phosphate, phosphates of Group 1 or Group 2 metals, and metal salts of organic phosphates. Examples of phosphoric acid include organic phosphates, which are preferred because they tend to reduce the amount of gas generated, tend to improve the appearance of molded articles, tend to increase the crystallization temperature, and tend to improve demolding properties.

[0115] In this embodiment, the phosphate preferably contains at least one of a compound represented by formula (P1) and a compound represented by formula (P2). Formula (P1) Formula (P2) (In formula (P1) and formula (P2), R x each independently represents a linear or branched alkyl group having 3 to 30 carbon atoms.

[0116] R x The number of carbon atoms in R is preferably 8 or more, more preferably 13 or more, and even more preferably 15 or more, and is preferably 25 or less, more preferably 20 or less, and even more preferably 18 or less, and most preferably 18. x is a straight-chain or branched alkyl group, but is preferably a straight-chain alkyl group.

[0117] In this embodiment, it is more preferable that the phosphate salt contains at least one of a compound represented by formula (P1-1) and a compound represented by formula (P2-1). In this embodiment, a mixture of a compound represented by formula (P1-1) and a compound represented by formula (P2-1) is more preferable. Formula (P1-1) Formula (P2-1)

[0118] The phosphoric acid preferably contains at least one compound represented by formula (P3): (In formula (P3), R represents a linear or branched alkyl group having 2 to 18 carbon atoms. nx represents 1 or 2.) The number of carbon atoms in R is preferably 8 or more, more preferably 13 or more, and even more preferably 15 or more, and is preferably 25 or less, more preferably 20 or less, even more preferably 18 or less, and most preferably 18. R represents a linear or branched alkyl group, and is preferably a linear alkyl group.

[0119] nx is 1 or 2, and is preferably a mixture of 1 and 2.

[0120] The transesterification inhibitor may be a commercially available product, and examples thereof include AX-71 manufactured by ADEKA Corporation and JP-518Zn manufactured by Johoku Chemical Co., Ltd.

[0121] The content of the transesterification inhibitor 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, per 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin. It is also preferably 2 parts by mass or less, more preferably 1.5 parts by mass or less, even more preferably 1 part by mass or less, and even more preferably 0.8 parts by mass or less, and may be 0.5 parts by mass or less. By setting the content at or above the lower limit, the effect of suppressing thermal degradation and oxidative degradation of the resin during melt-kneading, molding, and use as a molded product tends to be more improved, discoloration of the resin tends to be more effectively suppressed, flame retardancy tends to be improved, the crystallization temperature tends to be higher, and the appearance of the molded product tends to be improved. By setting the content at or below the upper limit, adverse effects on appearance and physical properties due to aggregation of additives such as stabilizers tend to be effectively suppressed. The resin composition of this embodiment may contain only one type of transesterification inhibitor, or may contain two or more types. When two or more types are contained, the total amount is preferably within the above range.

[0122] <Non-fibrous inorganic filler> The resin composition of this embodiment preferably contains a non-fibrous inorganic filler. By containing a non-fibrous inorganic filler, the physical properties and heat resistance are improved, and the effect of reducing the anisotropy of shrinkage during molding is improved. The non-fibrous inorganic filler refers to a filler in a shape other than fiber, and a plate-like filler or a particulate filler is preferred. Examples of non-fibrous inorganic fillers include calcium carbonate, talc, mica, silica, kaolin, wollastonite, barium sulfate, zirconium silicate, clay, bentonite, hydrotalcite, calcium sulfate, barium carbonate, magnesium carbonate, magnesium sulfate, calcium silicate, alumina, glass beads, glass flakes, titanium oxide, zinc oxide, magnesium oxide, calcium titanate, magnesium titanate, and barium titanate. Preferred are calcium carbonate, talc, mica, silica, kaolin, barium sulfate, zirconium silicate, and titanium oxide. More preferred are calcium carbonate, talc, and titanium oxide. Titanium oxide tends to improve impact resistance, flame retardancy, and tracking resistance, making it even more preferred. Furthermore, the non-fibrous inorganic filler used in this embodiment is preferably surface-treated with an acid, a siloxane compound, an inorganic compound, or the like. In particular, in the case of titanium oxide, it is preferred that the surface be treated with an organosiloxane compound or an inorganic compound such as alumina or silica, from the viewpoint of thermal stability. Examples of acids used in the acid treatment include fatty acids, rosin acid, and lignic acid, and saturated or unsaturated fatty acids having 6 to 20 carbon atoms are preferred. Examples of saturated or unsaturated fatty acids having 6 to 20 carbon atoms include stearic acid, palmitic acid, lauric acid, oleic acid, and linoleic acid.

[0123] The non-fibrous inorganic filler used in this embodiment preferably has an average particle size of 5 μm or less, more preferably 3 μm or less, even more preferably 1 μm or less, even more preferably 0.8 μm or less, even more preferably 0.5 μm or less, and particularly preferably 0.3 μm or less. The lower limit of the average particle size is preferably 0.01 μm or more, more preferably 0.08 μm or more, even more preferably 0.10 μm or more, and even more preferably 0.15 μm or more. The average particle size in this embodiment is the average of particle sizes observable from a magnified image taken with a scanning electron microscope. In the case of surface-treated titanium oxide, the primary particle size of the titanium oxide after surface treatment was taken as the average particle size.

[0124] The content of the non-fibrous inorganic filler is preferably 1 part by mass or more, more preferably 2 parts by mass or more, even more preferably 3 parts by mass or more, and particularly preferably 3.5 parts by mass or more, per 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin. By setting it at or above the lower limit, impact resistance tends to be improved, flame retardancy tends to be improved, and tracking resistance tends to be improved. Furthermore, the upper limit of the content of the non-fibrous inorganic filler is preferably 12 parts by mass or less, more preferably 10 parts by mass or less, even more preferably 8 parts by mass or less, even more preferably 6 parts by mass or less, and even more preferably 5 parts by mass or less, per 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin. By setting it at or below the upper limit, the surface appearance of the molded article tends to be improved.

[0125] The content of the non-fibrous inorganic filler in the resin composition of this embodiment is preferably 0.5% by mass or more of the resin composition, more preferably 1.0% by mass or more, even more preferably 2.0% by mass or more, and even more preferably 2.5% by mass or more. By setting it to the above lower limit or more, impact resistance tends to be improved, flame retardancy tends to be improved, and tracking resistance tends to be improved. Furthermore, the content of the non-fibrous inorganic filler in the resin composition of this embodiment is preferably 50% by mass or less of the resin composition, more preferably 40% by mass or less, even more preferably 30% by mass or less, even more preferably 20% by mass or less, even more preferably 10% by mass or less, even more preferably 7% by mass or less, and particularly preferably 5% by mass or less. By setting it to the above upper limit or less, the surface appearance of the molded article tends to be better and the flowability tends to be improved. The resin composition of this embodiment may contain only one type of non-fibrous inorganic filler, or may contain two or more types. When two or more types are included, it is preferable that the total amount is within the above range. In particular, it is preferable to contain 0.5 to 10 parts by mass of rutile-type titanium oxide having an average particle size of 0.15 to 0.4 μm per 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin, as this tends to make it easier to effectively exhibit high levels of flame retardancy, tracking resistance, and impact resistance.

[0126] The resin composition of this embodiment may or may not further contain a fibrous filler. Preferably, the resin composition of this embodiment is substantially free of a fibrous filler. "Substantially free" means that the content of the fibrous filler contained in the resin composition of this embodiment is less than 5% by mass of the resin composition, preferably less than 3% by mass, more preferably less than 1% by mass, and even more preferably less than 0.1% by mass.

[0127] <Antioxidant> The resin composition of this embodiment may contain an antioxidant. By including an antioxidant, a resin composition or molded article having excellent thermal stability can be obtained. The antioxidant preferably contains one or more compounds selected from the group consisting of thioether compounds, hindered phenol compounds, and phosphite compounds, and more preferably contains a hindered phenol compound. In this embodiment, it is also preferable to use two or more thioether compounds, hindered phenol compounds, and phosphite compounds in combination. By using two or more antioxidants in combination in this way, thermal stability is further improved and tends to be maintained for a long period of time.

[0128] 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 color change tends to be suppressed. 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 "Seenox 412S" manufactured by Shipro Chemical Co., Ltd. and "ADK STAB AO-412S" manufactured by ADEKA Corporation.

[0129] 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. Of 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 Corporation under the trade names "ADK STAB AO-60" and "ADK STAB AO-330."

[0130] The phosphite compound is preferably a compound represented by the formula: 2 O-P (OR 3 ) (OR 4 ) (wherein, 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 4At least one of the groups is an aryl group having 6 to 30 carbon atoms. 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.

[0131] Other examples of antioxidants include the descriptions in paragraphs 0067 to 0075 of JP-A-2021-063196, the descriptions in paragraphs 0046 to 0057 of JP-A-2018-070722, the descriptions in paragraphs 0030 to 0037 of JP-A-2019-056035, and the descriptions in paragraphs 0066 to 0078 of WO 2017 / 038949. The contents of these descriptions are incorporated herein by reference.

[0132] The content of the antioxidant in the resin composition of this embodiment is 0.01 parts by mass or more, preferably 0.05 parts by mass or more, more preferably 0.1 parts by mass or more, and even more preferably 0.3 parts by mass or more, per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. 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 discoloration of the resin tends to be more effectively suppressed. Furthermore, the upper limit of the antioxidant content is preferably 2.0 parts by mass or less, more preferably 1.5 parts by mass or less, and even more preferably 1.0 part by mass or less, per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. By ensuring that the content is below the upper limit, adverse effects on appearance and physical properties due to aggregation of additives such as the antioxidant can be effectively suppressed. The resin composition of this embodiment may contain only one antioxidant, or may contain two or more antioxidants. When two or more types are contained, the total amount is preferably within the above range.

[0133] <Reinforcing Filler> The resin composition of this embodiment may contain a reinforcing filler. By containing a reinforcing filler, the mechanical strength of the resulting shaped object can be improved. Examples of the shape of the reinforcing filler include scale-like, spherical, needle-like, and fibrous shapes, with fibrous reinforcing fillers (reinforcing fibers) being preferred. Examples of components of the reinforcing filler include glass, metal oxides, metal hydroxides, carbonates, and sulfates, with glass being preferred. As the reinforcing fiber, carbon fiber and glass fiber are preferred, and it is more preferred that the composition contains glass fiber.

[0134] Next, the glass fiber preferably used in this embodiment will be described. The glass fiber is a fiber obtained by melt spinning a commonly supplied glass such as E-glass, C-glass, D-glass, R-glass, A-glass, S-glass, and alkali-resistant glass, but any glass fiber that can be made into a glass fiber can be used, and there is no particular limitation. In this embodiment, it is preferable to include E-glass.

[0135] The glass fiber used in this embodiment is preferably surface-treated with a known silane coupling agent such as epoxy silane, amino silane, or vinyl silane, or with phosphoric acid. The amount of the surface treatment agent attached is preferably 0.01 to 1 mass% of the glass fiber. Furthermore, if necessary, the glass fiber may be surface-treated with a lubricant such as a fatty acid amide compound or silicone oil, an antistatic agent such as a quaternary ammonium salt, a resin capable of forming a film such as an epoxy resin or urethane resin, or a mixture of a resin capable of forming a film and a thermal oxidation inhibitor.

[0136] Glass fibers are commercially available, and examples of commercially available products include T-187, T-187H, T-127, T-127H, T-286H, T-756H, and T-289H manufactured by Nippon Electric Glass Co., Ltd., DEFT2A manufactured by Owens Corning, HP3540 manufactured by PPG, and CSG3PA820 manufactured by Nitto Boseki Co., Ltd.

[0137] When the resin composition of the present embodiment contains a reinforcing filler (preferably glass fiber), the content of the reinforcing filler is preferably 20 parts by mass or more, more preferably 30 parts by mass or more, even more preferably 40 parts by mass or more, and even more preferably 50 parts by mass or more, relative to 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin, and is preferably 150 parts by mass or less, more preferably 125 parts by mass or less, even more preferably 100 parts by mass or less, and may be 75 parts by mass or less.

[0138] When the resin composition of this embodiment contains a reinforcing filler, the reinforcing filler (preferably glass fiber) preferably accounts for 10 to 45 mass %, more preferably 15 to 40 mass %, and may even be 20 to 35 mass % of the resin composition. The resin composition of this embodiment may contain only one type of reinforcing filler, or may contain two or more types. When two or more types are contained, the total amount is preferably in the above range.

[0139] <Colorant> The resin composition of this embodiment may contain a colorant. The colorant may be a pigment or a dye. However, from the viewpoint of flame retardancy, a pigment is preferred, and carbon black is more preferred. For details about carbon black, see paragraph 0021 of JP 2011-57977 A, the contents of which are incorporated herein by reference. Furthermore, when a colorant such as carbon black is blended into the resin composition of this embodiment, it is preferable to form a masterbatch and then knead it with a polyalkylene terephthalate resin or the like. For the masterbatch, a polyester resin is preferably used, a polyalkylene terephthalate resin is more preferably used, a polyethylene terephthalate resin and / or a polybutylene terephthalate resin is even more preferably used, and a polybutylene terephthalate resin is even more preferably used. The use of a polybutylene terephthalate resin promotes crystallization of the resin composition. In particular, the presence of a polybutylene terephthalate resin in the vicinity of a colorant such as carbon black more effectively promotes crystallization. The proportion of the colorant in the masterbatch is preferably 5% by mass or more, more preferably 10% by mass or more, and is preferably 50% by mass or less, more preferably 40% by mass or less.

[0140] When the resin composition of this embodiment contains a colorant (preferably carbon black), the content thereof is preferably 0.1 parts by mass or more, more preferably 0.2 parts by mass or more, even more preferably 0.4 parts by mass or more, and even more preferably 0.6 parts by mass or more, relative to 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin, and is preferably 3 parts by mass or less, more preferably 2 parts by mass or less, and even more preferably 1 part by mass. The resin composition of this embodiment may contain only one type of colorant (preferably carbon black), or may contain two or more types. When two or more types are contained, it is preferable that the total amount is in the above range.

[0141] <Ultraviolet Absorber> The resin composition of this embodiment may contain an ultraviolet absorber. Preferred examples of the ultraviolet absorber include benzotriazole-based ultraviolet absorbers, benzoxazine-based ultraviolet absorbers, triazine-based ultraviolet absorbers, and malonic acid ester-based ultraviolet absorbers, with benzotriazole-based ultraviolet absorbers being preferred. By selecting an organic ultraviolet absorber, the transparency and mechanical properties of the resin composition of this embodiment can be improved.

[0142] Examples of the benzotriazole-based ultraviolet absorbers include 2-(2-hydroxy-5-methylphenyl)-2H-benzotriazole, 2-(2-hydroxy-3,5-di-tert-butylphenyl)-2H-benzotriazole, 2-(2-hydroxy-3-tert-butyl-5-methylphenyl)-2H-benzotriazole, 2-(2-hydroxy-5-tert-octylphenyl)-2H-benzotriazole, 2-(3,5-di-tert-octyl-2-hydroxyphenyl)-2H-benzotriazole, 2- (3,5-di-tert-amyl-2-hydroxyphenyl)-2H-benzotriazole, 2-(3-lauryl-5-methyl-2-hydroxyphenyl)-2H-benzotriazole, 2-(3,5-di-tert-butyl-2-hydroxyphenyl)-5-chloro-2H-benzotriazole, 2-(3-tert-butyl-5-methyl-2-hydroxyphenyl)-5-chloro-2H-benzotriazole, 2-(3,5-bis(1-methyl-1-phenylethyl)-2-hydroxyphenyl)-2H-benzotriazole, Bis(3-(2H-benzotriazol-2-yl)-2-hydroxy-5-methylphenyl)methane, bis(3-(2H-benzotriazol-2-yl)-2-hydroxy-5-(1,1,3,3-tetramethylbutyl)phenyl)methane, bis(3-(2H-benzotriazol-2-yl)-2-hydroxy-5-cumylphenyl)methane, bis(3-(2H-benzotriazol-2-yl)-2-hydroxy-5-octylphenyl)methane, 1,1-bis(3-(2H-benzotriazol-2-yl)-2-hydroxy-5-methylphenyl)methane 1,1-bis(3-(2H-5-chlorobenzotriazol-2-yl)-2-hydroxy-5-methylphenyl)octane, 1,2-ethanediylbis(3-(2H-benzotriazol-2-yl)-2-hydroxybenzoate), 1,12-dodecanediylbis(3-(2H-benzotriazol-2-yl)-4-hydroxybenzoate), 1,3-cyclohexanediylbis(3-(5-chloro-2H-benzotriazol-2-yl)-2-hydroxybenzoate), 1,4-butanediylbis(3-(2H-benzotriazol-2-yl)-4-hydroxy-5-methylphenylethanoate), 3,6-dioxa-1,8-octanediylbis(3-(5-methoxy-2H-benzotriazol-2-yl)-4-hydroxyphenylethanoate), 1,6-hexanediylbis(3-(3-(2H-benzotriazol-2-yl)-4-hydroxy-5-tert-butylphenyl)propionate), p-xylenediylbis(3-(3-(2H-benzotriazol-2-yl)-4-hydroxyphenyl)propionate), bis(3-(2H-benzotriazol-2-yl)-4-hydroxytoluyl)malonate, bis(2-(3-(2H-benzotriazol-2-yl)-4-hydroxy-5-octylphenyl) ethyl) terephthalate, bis(3-(2H-benzotriazol-2-yl)-4-hydroxy-5-propyltoluyl)octadioate, 2-(2H-benzotriazol-2-yl)-6-phthalimidomethyl-4-methylphenol, 2-(2H-benzotriazol-2-yl)-6-phthalimidoethyl-4-methylphenol, 2-(2H-benzotriazol-2-yl)-6-phthalimidooctyl-4-methylphenol, 2-(2H-benzotriazol-2-yl)-6-phthalimidomethyl-4-tert-butylphenol, 2-(2H-benzotriazol-2-yl)-6-phthalimidomethyl-4-cumylphenol, 2-(2H-benzotriazol-2-yl)-4,6-bis(phthalimidomethyl)phenol, and the like. Among these, 2-(2-hydroxy-5-tert-octylphenyl)-2H-benzotriazole is preferred.

[0143] For ultraviolet absorbers, the descriptions in paragraphs 0059 to 0062 of JP-A-2016-216534 and paragraphs 0069 to 0082 of JP-A-2018-178019 can be referred to, the contents of which are incorporated herein by reference.

[0144] In the resin composition of this embodiment, the content of the ultraviolet absorber is preferably 0.01 to 1 part by mass per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. The content of the ultraviolet absorber is more preferably 0.03 to 0.7 parts by mass, and even more preferably 0.05 to 0.5 parts by mass per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. Addition within such a range can impart good weather resistance to the resin composition of this embodiment. Only one type of ultraviolet absorber may be contained, or two or more types may be contained. When two or more types are contained, it is preferable that the total amount be within the above range.

[0145] <Release Agent> The resin composition of the present embodiment preferably contains a release agent. A wide variety of known release agents can be used as the release agent, and examples thereof include aliphatic carboxylic acid amides, aliphatic carboxylic acids, esters of aliphatic carboxylic acids and alcohols, aliphatic hydrocarbon compounds having a number average molecular weight of 200 to 15,000, and polysiloxane-based silicone oils.

[0146] Examples of aliphatic carboxylic acid amides include compounds obtained by the dehydration reaction of higher aliphatic monocarboxylic acids and / or polybasic acids with diamines. Preferred higher aliphatic monocarboxylic acids include saturated aliphatic monocarboxylic acids and hydroxycarboxylic acids having 16 or more carbon atoms, such as palmitic acid, stearic acid, behenic acid, montanic acid, and 12-hydroxystearic acid. Examples of polybasic acids include aliphatic dicarboxylic acids such as malonic acid, succinic acid, adipic acid, sebacic acid, pimelic acid, and azelaic acid; aromatic dicarboxylic acids such as phthalic acid and terephthalic acid; and alicyclic dicarboxylic acids such as cyclohexanedicarboxylic acid and cyclohexylsuccinic acid. Examples of diamines include ethylenediamine, 1,3-diaminopropane, 1,4-diaminobutane, hexamethylenediamine, metaxylylenediamine, tolylenediamine, paraxylylenediamine, phenylenediamine, and isophoronediamine. As the carboxylic acid amide compound, a compound obtained by polycondensation of stearic acid, sebacic acid, and ethylenediamine is preferred, and a compound obtained by polycondensation of 2 moles of stearic acid, 1 mole of sebacic acid, and 2 moles of ethylenediamine is more preferred. In addition to bisamide compounds obtained by reacting a diamine with an aliphatic carboxylic acid, such as N,N'-methylenebisstearamide or N,N'-ethylenebisstearamide, dicarboxylic acid amide compounds such as N,N'-dioctadecylterephthalamide can also be suitably used.

[0147] Examples of aliphatic carboxylic acids include saturated or unsaturated aliphatic mono-, di-, or tri-carboxylic acids. Aliphatic carboxylic acids also include alicyclic carboxylic acids. Among these, preferred aliphatic carboxylic acids are mono- or di-carboxylic acids having 6 to 36 carbon atoms, with saturated aliphatic mono-carboxylic acids having 6 to 36 carbon atoms being more preferred. Specific examples of such aliphatic carboxylic acids include palmitic acid, stearic acid, caproic acid, capric acid, lauric acid, arachic acid, behenic acid, lignoceric acid, cerotic acid, melissic acid, tetralinic acid, montanic acid, adipic acid, and azelaic acid.

[0148] In the ester of an aliphatic carboxylic acid and an alcohol, the same aliphatic carboxylic acid as used herein can be used. On the other hand, examples of the alcohol include saturated or unsaturated monohydric or polyhydric alcohols. These alcohols may have a substituent such as a fluorine atom or an aryl group. Among these, monohydric or polyhydric saturated alcohols having 30 or less carbon atoms are preferred, and aliphatic or alicyclic saturated monohydric alcohols or aliphatic saturated polyhydric alcohols having 30 or less carbon atoms are more preferred. Specific examples of such alcohols include octanol, decanol, dodecanol, stearyl alcohol, behenyl alcohol, ethylene glycol, diethylene glycol, glycerin, pentaerythritol, 2,2-dihydroxyperfluoropropanol, neopentylene glycol, ditrimethylolpropane, and dipentaerythritol. Specific examples of esters of aliphatic carboxylic acids and alcohols include beeswax (a mixture containing myricyl palmitate as a main component), stearyl stearate, behenyl behenate, stearyl behenate, glycerin monopalmitate, glycerin monostearate, glycerin distearate, glycerin tristearate, pentaerythritol monopalmitate, pentaerythritol monostearate, pentaerythritol distearate, pentaerythritol tristearate, pentaerythritol tetrastearate, and esters of montanic acid and polyfunctional alcohols.

[0149] Examples of aliphatic hydrocarbons having a number average molecular weight of 200 to 15,000 include liquid paraffin, paraffin wax, microcrystalline wax, polyethylene wax, Fischer-Tropsch wax, and α-olefin oligomers having 3 to 12 carbon atoms. Note that the aliphatic hydrocarbons herein also include alicyclic hydrocarbons. The number average molecular weight of the aliphatic hydrocarbons is preferably 5,000 or less.

[0150] Examples of polyolefin waxes include polyethylene wax, polypropylene wax, and polyethylene propylene wax, with polyethylene wax being preferred. The polyolefin wax may be unmodified or modified. Examples of modified polyolefin waxes include vinyl ester-modified polyolefin wax, acid-modified polyolefin wax, and oxidized polyolefin wax, with oxidized polyolefin wax being preferred. Oxidized polyolefin waxes have excellent compatibility with polyalkylene terephthalate resins and tend to effectively suppress mold deposits in the resulting resin composition.

[0151] Oxidized polyolefin waxes can be obtained by oxidizing the corresponding unmodified polyolefin wax. Examples of oxidized polyethylene waxes include Licowax (registered trademark) PED521, PED522, and PED121 manufactured by Clariant Chemicals; Ceridust (registered trademark) 3715, and the like. In addition to the above, commercially available polyolefin waxes can be found in paragraph 0028 of JP 2022-140470 A, the contents of which are incorporated herein by reference.

[0152] The weight-average molecular weight of the polyolefin wax is preferably 800 or more, more preferably 1,000 or more, even more preferably 1,500 or more, even more preferably 2,000 or more, and even more preferably 2,500 or more. By setting it to the lower limit or more, the glowing time tends to be further shortened. Furthermore, the weight-average molecular weight of the polyolefin wax is preferably 30,000 or less, more preferably 20,000 or less, even more preferably 15,000 or less, and even more preferably 10,000 or less. By setting it to the upper limit or less, the fluidity of the resin composition during molding tends to be further improved. The weight average molecular weight can be measured by GPC (gel permeation chromatography) using a Tosoh HLC-8320GPC EcoSEC, tetrahydrofuran as a solvent, three Shodex KF-G and KF-805L columns, and a KF-800D column at a column temperature of 40°C and a flow rate of 1.2 mL / min, and can be measured as a polystyrene-equivalent value detected with a detector (UV-8320) at a detection wavelength of 254 nm. When the resin composition in this embodiment contains two or more types of polyolefin waxes, the weight average molecular weight is the weight average molecular weight of the mixture.

[0153] The dropping point of the polyolefin wax is preferably 165° C. or less, more preferably 160° C. or less, even more preferably 155° C. or less, even more preferably 150° C. or less, even more preferably 145° C. or less, even more preferably 140° C. or less, even more preferably 135° C. or less, particularly more preferably 130° C. or less, and preferably 80° C. or more, more preferably 85° C. or more, even more preferably 85° C. or more, even more preferably 90° C. or more, and even more preferably 95° C. or more. The dropping point is the temperature at which the first drop of molten material falls from a standard cup with an opening of 2.8 mm when the polyolefin wax is heated to change from a solid to a liquid state.

[0154] As for the release agent, in addition to the above, the descriptions in paragraphs 0063 to 0077 of JP-A-2018-070722 and the descriptions in paragraphs 0090 to 0098 of JP-A-2019-123809 can be referred to, and the contents of these can be incorporated into this specification.

[0155] The resin composition of this embodiment preferably contains 0.01 parts by mass or more of the release agent relative to 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin, more preferably 0.1 parts by mass or more, even more preferably 0.3 parts by mass or more, and even more preferably 0.5 parts by mass or more. Depending on the application, etc., it may contain 0.8 parts by mass or more, or even 1.0 part by mass or more. Furthermore, it is preferably 5 parts by mass or less, more preferably 4 parts by mass or less, even more preferably 3 parts by mass or less, and even more preferably 2 parts by mass or less. Depending on the application, etc., it may be 1 part by mass or less. By setting the content at or above the lower limit, the releasability of the resulting molded article tends to be further improved. Furthermore, by setting the content at or below the upper limit, bleed-out of the resulting molded article can be effectively suppressed. The resin composition may contain only one type of release agent, or two or more types. When two or more types are contained, the total amount is preferably within the above range.

[0156] <Nucleating Agent> The resin composition of this embodiment may contain a nucleating agent. The inclusion of a nucleating agent promotes crystallization of the resin composition. The type of nucleating agent is not particularly limited, and may be an inorganic nucleating agent or an organic nucleating agent, with organic nucleating agents being more preferred. The use of an organic nucleating agent allows for a reduced blending amount, thereby further improving the mechanical strength and shrinkage rate of the resulting molded product. 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.

[0157] 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, making it even more preferred.

[0158] 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 parts by mass or more, and even more preferably 1.5 parts by mass or more, per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. By setting the content of the nucleating agent at or above the lower limit, the mold release properties and mechanical strength of the molded product tend to be improved. In particular, by including preferably 1.6 parts by mass or more, more preferably 1.8 parts by mass or more of the nucleating agent (preferably talc) per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined, the flame retardancy of the resin composition can be further 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, per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined. By setting the content to the upper limit or less, decomposition of the resin is suppressed, and the mechanical strength, particularly impact resistance, of the molded product tends to be improved. The resin composition of this embodiment may contain only one type of nucleating agent, or may contain two or more types. When two or more types are contained, it is preferable that the total amount is in the above range.

[0159] <Other Components> The resin composition of this embodiment may contain other components in addition to those described above, as necessary, as long as the desired physical properties are not significantly impaired. Examples of other components include thermoplastic resins other than polyarylene terephthalate resins and polycarbonate resins, and various resin additives. One type of other component may be contained, or two or more types may be contained in any combination and ratio. Specific examples include reactive compounds (such as epoxy compounds), antistatic agents, antifogging agents, antiblocking agents, flow improvers, plasticizers, dispersants, and antibacterial agents. The resin composition of this embodiment may also contain additives described in paragraphs 0047 to 0103 of WO 2021 / 241471 within the scope of the present invention, the contents of which are incorporated herein by reference. In the resin composition of this embodiment, the total of the polyalkylene terephthalate resin, polycarbonate resin, elastomer, flame retardant, and components blended as needed is 100% by mass. In one embodiment of the present invention, the resin composition of this embodiment preferably comprises the polyalkylene terephthalate resin, polycarbonate resin, elastomer, and flame retardant in a total amount of 85% by mass or more, more preferably 90% by mass or more, even more preferably 93% by mass or more, and even more preferably 95% by mass or more. In another embodiment of the present invention, the resin composition of this embodiment preferably comprises the polyalkylene terephthalate resin, polycarbonate resin, elastomer, flame retardant, and optionally blended glass fiber in a total amount of 85% by mass or more, more preferably 90% by mass or more, even more preferably 93% by mass or more, and even more preferably 95% by mass or more.Furthermore, in one embodiment of the present invention, the resin composition of this embodiment preferably comprises the polyalkylene terephthalate resin, polycarbonate resin, elastomer, flame retardant, flame retardant aid, anti-dripping agent, transesterification inhibitor, non-fibrous inorganic filler, antioxidant, ultraviolet absorber, and mold release agent, as well as glass fibers blended as needed, in a total amount that accounts for 90% by mass or more of the resin composition, more preferably 95% by mass or more, even more preferably 97% by mass or more, and even more preferably 99% by mass or more.

[0160] <Physical Properties of Resin Composition> The resin composition of this embodiment preferably has a high recycled content (recycle ratio (mass %)). Specifically, the recycled content in the resin composition is preferably 10 mass % or more, more preferably 20 mass % or more, even more preferably 30 mass % or more, and even more preferably 35 mass % or more. The upper limit of the recycled content may be 100 mass %, but 50 mass % or less is practical. Furthermore, the resin composition of this embodiment may have 40 to 60 mass % of the resin component as recycled content. The recycled content contained in the resin composition of this embodiment is preferably a post-consumer recycled (PCR) product.

[0161] The resin composition of this embodiment preferably has a high nominal breaking strain. Specifically, the resin composition is injection-molded into a multipurpose test piece A1 in accordance with JIS K7139, and the nominal breaking strain measured in accordance with JIS K7161-1 is preferably 50% or more, more preferably 74% or more, even more preferably 80% or more, and even more preferably 90% or more. There is no particular upper limit to the nominal breaking strain, but even if it is 130% or less, the required performance is fully satisfied. The high nominal breaking strain can be achieved, for example, by using recycled polycarbonate resin derived from bottles or sheets, which tend to have a relatively low amount of foreign matter, using a polycarbonate resin with a low MVR, using a polyalkylene terephthalate resin with a high intrinsic viscosity, or by blending an elastomer.

[0162] The resin composition of this embodiment preferably has a high Tc (crystallization temperature). A high Tc tends to result in molded articles with excellent moldability. Furthermore, a resin composition with excellent moldability can be obtained. When measured according to JIS K7121, the Tc of the resin composition of this embodiment is preferably 180°C or higher in the first cycle, more preferably 182°C or higher, even more preferably 184°C or higher, and even more preferably 185°C or higher. The upper limit is preferably 200°C or lower. When measured according to JIS K7121, the Tc of the resin composition of this embodiment is preferably 143°C or higher in the second cycle, more preferably 150°C or higher, even more preferably 154°C or higher, and even more preferably 157°C or higher. The upper limit is preferably 190°C or lower. The high crystallization temperature can be achieved, for example, by including a transesterification inhibitor in the resin composition, by controlling the branching amount in the recycled polycarbonate to an upper limit or lower, or by avoiding excessively high temperatures or stagnation during the production of the resin composition.

[0163] The resin composition of this embodiment preferably has excellent impact resistance. Specifically, the resin composition of this embodiment is injection-molded into a multipurpose test piece A1 in accordance with JIS K7139, and the unnotched Charpy impact strength (unit: kJ / m) measured at a temperature of 23°C in accordance with JIS K7111-1 is 2 ) is 21 kJ / m 2 It is preferable that the concentration is 25 kJ / m or more. 2 More preferably, it is 30 kJ / m or more. 2 More preferably, it is 35 kJ / m or more. 2 More preferably, it is 40 kJ / m or more. 2 More preferably, it is 45 kJ / m or more. 2 It is even more preferable that the value is 50 kJ / m or more. 2 It is particularly preferable that the value is 55 kJ / m or more. 2 The upper limit of the unnotched Charpy impact strength is, for example, 80 kJ / m or more. 2The following are practical. The impact resistance can be achieved, for example, by increasing the proportion of polycarbonate resin in the resin composition, using a recycled polycarbonate resin with a low MVR, blending an elastomer, blending titanium oxide, etc. In particular, the resin composition of this embodiment is highly valuable in that it can achieve excellent impact resistance despite the incorporation of a flame retardant.

[0164] The resin composition of this embodiment preferably has excellent flame retardancy. Specifically, the resin composition is preferably molded into a 0.74 mm or 1.0 mm thick UL-94 test piece, and the flame retardancy according to the UL-94 test satisfies V-0. Furthermore, the resin composition is molded into a 0.74 mm or 1.0 mm thick UL-94 test piece, and the total burning time according to the UL-94 test is preferably 50 seconds or less, more preferably 45 seconds or less, even more preferably 40 seconds or less, even more preferably 35 seconds or less, even more preferably 30 seconds or less, even more preferably 25 seconds or less, even more preferably 20 seconds or less, and particularly preferably 18 seconds or less. The lower limit of the total burning time is ideally 0 seconds, but 1 second or more is practical. The flame retardancy can be achieved by blending a flame retardant, a flame retardant auxiliary, an anti-dripping agent, etc., as well as by blending, for example, titanium oxide.

[0165] The resin composition of this embodiment preferably has excellent heat resistance. Specifically, when the resin composition is molded into an ISO tensile test piece (4 mm thick), the deflection temperature under load (DTUL) at a load of 1.8 MPa is preferably 180°C or higher, more preferably 185°C or higher, even more preferably 186°C or higher, and even more preferably 188°C or higher. The upper limit of the deflection temperature under load is not particularly specified, but even if it is 220°C or lower, the required performance is sufficiently satisfied.

[0166] The resin composition of this embodiment preferably has excellent fluidity. Specifically, the resin composition of this embodiment preferably has a melt volume rate (MVR) of 3 cm or more at 250°C and a load of 5 kgf according to ISO 1133.3 / 10 minutes or more is preferable, and 10 cm 3 / 10 minutes or more, 15 cm 3 The upper limit of the MVR may be, for example, 50 cm / 10 minutes or more. 3 / 10 minutes or less is practical.

[0167] The resin composition of this embodiment preferably has excellent tracking resistance. Specifically, the resin composition is injection molded into a 100 mm x 100 mm x 3 mm thick object, and the CTI value measured according to UL746A is preferably 600 V or higher. The upper limit of the CTI is not particularly specified, but even if it is 1000 V or lower, the required performance is fully satisfied. The tracking resistance can be achieved, for example, by blending an optimal type and amount of elastomer, optimizing the blending ratio of polycarbonate resin and polyalkylene terephthalate resin, blending titanium oxide, blending an optimal type and amount of flame retardant, etc.

[0168] The resin composition of this embodiment can reduce the peak molding pressure. Specifically, when the resin composition of this embodiment is molded into a multipurpose test piece A1 according to JIS K7139, the peak molding pressure can be 102 MPa or less, 96 MPa or less, or even 95 MPa or less. The lower limit of the peak molding pressure is, for example, 40 MPa or more. The low peak molding pressure can be achieved, for example, by using a polycarbonate resin with a low MVR value, optimizing the type and amount of elastomer, etc. The recyclability is calculated according to the description in the Examples below. The nominal strain at break, Tc (crystallization temperature), impact resistance, flame retardancy, deflection temperature under load, MVR, tracking resistance, and peak molding pressure are measured according to the description in the Examples below.

[0169] <Method for Producing Resin Composition> The resin composition of this embodiment can be produced by a conventional method for producing a resin composition containing a thermoplastic resin. For example, the resin composition of this embodiment can be produced by a method including feeding a polyalkylene terephthalate resin, a polycarbonate resin, a flame retardant, and other components, as needed, into an extruder and melt-kneading the components. A reinforcing filler may be side-fed into the extruder. Furthermore, when the resin composition contains a colorant, the colorant may be blended as a masterbatch premixed with the thermoplastic resin and then melt-kneaded. The heating temperature during melt-kneading can generally be selected from the range of 220 to 350°C, preferably from 220 to 320°C, and more preferably from 220 to 280°C.

[0170] <Method for Manufacturing Molded Article> The resin composition of this embodiment is molded according to a known method. The method for manufacturing the molded article is not particularly limited, and any molding method commonly used for resin compositions can be used. Examples include injection molding, ultra-high speed injection molding, injection compression molding, two-color molding, gas-assisted hollow molding, molding using an insulated mold, molding using a rapidly heated mold, foam molding (including supercritical fluid), insert molding, IMC (in-mold coating molding), extrusion molding, sheet molding, thermoforming, rotational molding, laminate molding, press molding, and blow molding. Of these, injection molding is preferred. For details of the injection molding method, please refer to paragraphs 0113 to 0116 of Japanese Patent No. 6183822, the contents of which are incorporated herein by reference. Furthermore, the mold temperature during mold molding, such as injection molding, is preferably 40 to 150°C.

[0171] <Applications> An example of the resin composition of this embodiment is pellets. A molded article of this embodiment is formed from the resin composition of this embodiment or the pellets of this embodiment. The molded article of this embodiment can be used in a variety of applications, such as various storage containers, electrical and electronic equipment parts, office automation (OA) equipment parts, home appliance parts, mechanical mechanism parts, and vehicle parts (vehicle mechanism parts, vehicle housing parts). Examples of vehicle parts include lamp housings, reflectors, bezels, and extensions, as well as connectors, ECU cases, head-up display housings, housings for vehicle-mounted cameras and millimeter-wave radars, battery cases, inverters, high-voltage connectors, sensor housings, and housings for charging components for EVs. Examples of electric and electronic parts include housings, covers, keyboards, buttons, switch members, casings for power meters, battery cases, battery transport trays, relays, sensors, actuators, terminal switches, and grill cooking equipment parts for personal computers, game consoles, display devices such as televisions, printers, copy machines, scanners, fax machines, electronic organizers and PDAs, electronic desk calculators, electronic dictionaries, cameras, video cameras, mobile phones, battery packs, drives and readers for recording media, mice, numeric keypads, CD players, MD players, portable radios and audio players, and the like.

[0172] The present invention will be explained in more detail below with reference to examples. The materials, amounts used, ratios, treatment contents, treatment procedures, etc. shown in the following examples can be changed as appropriate 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.

[0173] 1. Raw Materials The raw materials shown in Tables 1 and 2 below were used.

[0174]

[0175]

[0176] <Measurement of the amount of bisphenol A (BPA amount) in polycarbonate resin (virgin product and recycled product)> Polycarbonate resin was dissolved in a dichloromethane solution, methanol was added dropwise to reprecipitate the polymer component, and the solution was filtered. The filtrate was dried and dissolved in 5 mL of methanol. The methanol solution was analyzed by high-performance liquid chromatography (Shimadzu Corporation, "LC-20AD Prominence") to determine the content of bisphenol A. A calibration curve prepared from a separately prepared standard substance was used to calculate the content.

[0177] <Measurement of Branching Amount of Polycarbonate Resin (Virgin Product and Recycled Product)> In this embodiment, the branching amount of a polycarbonate resin refers to the total content (unit: ppm by mass) of PSA, PSA-Me, PBA, and dicarboxylic acids (DA1, DA2) (structures shown below) obtained after hydrolysis of the polycarbonate resin. Specifically, 0.5 g of polycarbonate resin was dissolved in 5 mL of methylene chloride, and then 45 mL of methanol and 5 mL of a 25% by mass aqueous sodium hydroxide solution were added. The mixture was stirred at 70°C for 30 minutes to hydrolyze (methylene chloride solution). Subsequently, 6N hydrochloric acid was added to this methylene chloride solution to adjust the pH of the solution to about 2, and the volume was adjusted to 100 mL with pure water. Next, 20 μL of the prepared methylene chloride solution was injected into a liquid chromatograph, and the contents of PSA, PSA-Me, PBA, and dicarboxylic acids (DA1 and DBA2) shown in the structures below were measured, and the total amount was taken as the branching amount of the polycarbonate resin (unit: mass ppm). The liquid chromatograph and measurement conditions were as follows. Liquid chromatograph: LC-10AD manufactured by Shimadzu Corporation Column: YMC PACK ODS-AM M-307-3 4.6 mm ID × 75 mm L Detector: UV 280 nm Eluent: (A) 0.05% aqueous trifluoroacetic acid solution (B) methanol Gradient conditions: 0 min (B = 40%), 25 min (B - 95%) The contents of PSA, PSA-Me, PBA, and dicarboxylic acids (DA1 and DA2) were calculated from the respective peak areas based on a calibration curve prepared using bisphenol A.

[0178] The PSA, PSA-Me, PBA, and dicarboxylic acids (DA1, DA2) are as follows:

[0179] <Measurement of MVR of Polycarbonate Resin (Virgin Product and Recycled Product)> The melt volume rate of polycarbonate resin (virgin product and recycled product) was measured in accordance with ISO 1133 under conditions of 300°C and a load of 1.20 kgf. The unit is cm 3 / 10 min.

[0180] <Dispersity (Mw / Mn) of Polycarbonate Resin (Virgin Product and Recycled Product)> The weight average molecular weight (Mw) and number average molecular weight (Mn) of polycarbonate resin (virgin product and recycled product) were measured using HLC-8320GPC / EcoSEC (manufactured by TOSOH Corporation) and calculated in terms of polystyrene. The measurement conditions were as follows: Column: Shodex KF-G + KF-805L x 3 + KF-800D Detector: UV detector 254 nm Column temperature: 40°C Eluent: tetrahydrofuran (THF) The dispersity (Mw / Mn) was calculated based on the obtained Mw and Mn. Note that Mw and Mn in this specification are values ​​measured by the above method for all components. Furthermore, when two or more polycarbonate resins are contained, the Mw and Mn of the polycarbonate resins are the Mw and Mn of the mixture, respectively. The same applies to the other components.

[0181] <Measurement of the amount of metal elements> Qualitative / semi-quantitative analysis of metal elements (Al, Fe, P) in polycarbonate resin was performed by ICP atomic emission spectrometry. In this case, as a pretreatment, 200 mg of sample was weighed and subjected to Kjeldahl wet hydrolysis (sulfuric acid / nitric acid, sulfuric acid / hydrogen peroxide), and the volume was adjusted to 50 mL. Subsequently, ICP atomic emission spectrometry was performed using the acid concentration matching single point calibration method. The unit is expressed in ppm by mass. ICP atomic emission spectrometry was performed using a ThermoThermo Fisher Scientific "iCAP7600duo iCAP76000uo" by axial / radial photometry.

[0182] Details of PC-1 to PC-6 are as follows.

[0183] *ND: Below detection limit

[0184] 2. Examples 1-1 to 1-3, Comparative Example 1, Reference Example 1 <Compound> The components shown in Table 1 or Table 2 were uniformly mixed using a tumbler mixer in the proportions shown in Table 4 (each component in Table 4 is shown in parts by mass). The resulting mixture was fed to a twin-screw extruder ("TEX30α" manufactured by The Japan Steel Works, Ltd.). The resin composition was melt-kneaded under conditions of a cylinder setting temperature of 260°C and a screw rotation speed of 200 rpm, rapidly cooled in a water tank, and pelletized using a pelletizer to obtain pellets of the resin composition.

[0185] <Recycled Ratio (% by Mass)> The ratio (% by mass) of the recycled component to the total amount of the resin composition was calculated.

[0186] <Nominal strain at break> The resin composition pellets obtained above were dried at 120°C for 5 hours, and then injection-molded into JIS K7139 multipurpose test pieces A1 (4 mm thick) using an injection molding machine "J-85AD-60H" manufactured by The Japan Steel Works, Ltd., under conditions of a cylinder temperature of 250°C and a mold temperature of 80°C. The nominal tensile strain at break was determined based on JIS K7161-1.

[0187] <Crystallization Temperature (Tc)> Pellets of the resin composition were measured using a differential scanning calorimeter (DSC) in accordance with JIS K7121. The temperature was increased from 40°C to 300°C at a rate of 20°C / min under a nitrogen atmosphere, held at 300°C for 3 minutes, and then decreased to 40°C at a rate of -20°C / min. This constituted one cycle, and two cycles were performed. The maximum peak temperature due to crystallization during the temperature decrease in each cycle was taken as the crystallization temperature. The differential scanning calorimeter used was a "DSC7020" manufactured by Hitachi High-Tech Science Corporation.

[0188] <Notched Charpy Impact Strength> The resin composition pellets obtained above were dried at 120°C for 5 hours, and then injection molded into JIS K7139 multipurpose test pieces A1 (4 mm thick) using an injection molding machine "J-85AD-60H" manufactured by The Japan Steel Works, Ltd., under conditions of a cylinder temperature of 250°C and a mold temperature of 80°C. The multipurpose test pieces (4 mm thick) were used to measure the unnotched Charpy impact strength (unit: KJ / m) in accordance with the JIS K7111-1 standard. 2 ) was measured.

[0189] <Flame Retardancy> The resin composition pellets obtained above were dried at 120°C for 5 hours, and then injection-molded into combustion test specimens (12.7 mm width x 127 mm length x 1.0 mm 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 allowed to stand in an atmosphere of 70°C for 1 week, and then their flame retardancy was evaluated in accordance with the method of Subject 94 (UL94) of Underwriters Laboratories.

[0190] <Tracking Resistance (CTI)> The pellets obtained above were dried at 120°C for 6 hours until just beforehand, and then a 100mm x 100mm x 3mm thick plate-shaped test piece was molded using an injection molding machine ("NEX-80" manufactured by Nissei Plastic Industrial Co., Ltd.) at a cylinder temperature of 260°C, and the tracking resistance test specified in the test method UL746A23 was performed and measured in accordance with ASTM D3638. An electrolyte (0.1% aqueous solution of ammonium chloride, resistivity 385Ω cm at 23°C) was dropped from the nozzle of the device at 30 second intervals, and a voltage of 600V or less (25V steps) was applied between both platinum electrodes, and the number of drops of electrolyte until tracking occurred was measured, and the maximum voltage (unit: V) at which the average value of 5 drops was 50 drops was determined.

[0191] <Peak pressure during molding (MPa)> The resin composition pellets obtained above were dried at 120°C for 5 hours, and then the peak injection pressure (MPa) was read when injection molding a JIS K7139 multipurpose test piece A1 (4 mm thick) using an injection molding machine "J-85AD-60H" manufactured by The Japan Steel Works, Ltd. under conditions of a cylinder temperature of 250°C and a mold temperature of 80°C.

[0192]

[0193] As is clear from the above results, the resin composition of the present invention was excellent in terms of various physical properties in a well-balanced manner.

[0194] 3. Examples 2-1 to 2-5, Comparative Example 2, Reference Example 2 <Compound> The components shown in Table 1 or Table 2 were mixed uniformly in a tumbler mixer in the proportions shown in Table 5 or Table 6 (each component in Table 5 and Table 6 is shown in parts by mass), with the exception of glass fiber. The resulting mixture was fed into a twin-screw extruder ("TEX30α" manufactured by The Japan Steel Works, Ltd.) through the main feed port. The cylinder temperature setting of the first kneading section was set to 260°C, and glass fiber was fed through a side feeder. The resin composition was melt-kneaded under conditions of a cylinder temperature setting of 260°C after the addition of glass fiber and a screw rotation speed of 200 rpm, and then quenched in a water bath and pelletized using a pelletizer to obtain pellets of the resin composition.

[0195] <MVR of Resin Composition> The melt volume rate of the resulting resin composition was measured at 250°C under a load of 5 kgf in accordance with ISO 1133. The unit is cm 3 / 10 min.

[0196] <Deflection temperature under load (DTUL)> The obtained resin pellets were dried at 120°C for 6 hours, and then injection molded into ISO tensile test pieces (4 mm thick) using an injection molding machine ("J-85AD" manufactured by The Japan Steel Works, Ltd.) under conditions of a cylinder temperature of 250°C and a mold temperature of 80°C. In accordance with ISO 75-1 and 2, the deflection temperature under load (unit: °C) was measured using the above ISO tensile test pieces (4 mm thick) under a load of 1.80 MPa.

[0197] <Flame Retardancy> The resin composition pellets obtained above were dried at 120°C for 5 hours and then injection-molded into combustion test specimens (12.7 mm wide x 127 mm long x 0.74 mm thick) 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 at 70°C for 1 week, and then their flame retardancy was evaluated in accordance with the Subject 94 (UL94) method of Underwriters Laboratories. For each of the five test specimens, a burner flame was applied to the lower end of the vertically supported test specimen and maintained for 10 seconds, after which the burner flame was removed from the test specimen. Once the flame had extinguished, the burner flame was immediately applied for another 10 seconds and then removed. The total flaming combustion time (unit: seconds) of the five test specimens and the UL-94 evaluation results are shown in Tables 5 and 6.

[0198]

[0199]

[0200] The PBT:PC (mass ratio) in the table was calculated including the PBT resin in the antimony trioxide masterbatch and the carbon black masterbatch.

[0201] As is clear from the above results, the resin compositions of the present invention achieved excellent flame retardancy despite using recycled polycarbonate resins (Examples 2-1 to 2-5). On the other hand, when a virgin polycarbonate resin with a high branching amount (PC-5) was used (Comparative Example 2) or a recycled polycarbonate resin with a high bisphenol A content (PC-4) was used (Reference Example 2), the flame retardancy was poor.

Claims

1. A resin composition comprising 5 to 50 parts by mass of a flame retardant per 100 parts by mass of a total of a polyalkylene terephthalate resin and a polycarbonate resin, wherein the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin in the total 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin is 10 / 90 to 90 / 10, the polycarbonate resin contains a polycarbonate resin derived from recycled materials, and the branching amount of the polycarbonate resin derived from recycled materials is 50 to 3,500 ppm by mass.

2. The elastomer is contained in an amount of 1 to 30 parts by mass per 100 parts by mass of the total of polyalkylene terephthalate resin and polycarbonate resin, and the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin in the total of 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin is 80 / 20 to 20 / 80, and the melt volume rate (MVR) of the recycled polycarbonate resin measured according to ISO1133 under conditions of 300°C and a load of 1.20 kgf is 2 to 11 cm 3 The resin composition according to claim 1, wherein the curing time is 10 minutes.

3. The resin composition according to claim 1 or 2, wherein the recycled polycarbonate resin contains 10 to 80 ppm by mass of bisphenol A.

4. The melt volume rate (MVR) of the recycled polycarbonate resin measured in accordance with ISO 1133 at 300°C and a load of 1.20 kgf is 4 to 30 cm 3 The resin composition according to claim 1, wherein the viscosity is 100 / 10 minutes.

5. The resin composition according to claim 1, 2 or 4, further comprising an ester exchange inhibitor in an amount of 0.01 to 2 parts by mass per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined.

6. A resin composition according to claim 1, 2 or 4, wherein the polyalkylene terephthalate resin contains 50 mass% or more of polybutylene terephthalate resin. 7.00 The resin composition according to claim 1, 2 or 4, wherein the flame retardant comprises a brominated flame retardant.

8. The resin composition according to claim 1, 2 or 4, further comprising 3 to 30 parts by mass of an elastomer per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin combined.

9. The resin composition according to claim 1, 2 or 4, wherein the recycled polycarbonate resin contains 0.2 to 1000 ppm by mass of aluminum element and 0.2 to 100 ppm by mass of iron element.

10. The resin composition according to claim 1, 2 or 4, which, when molded into a UL-94 test piece having a thickness of 0.74 mm or 1.0 mm, has a flame retardancy according to the UL-94 test that satisfies V-0.

11. The resin composition according to claim 1, 2 or 4, wherein the recycled polycarbonate resin comprises at least one of polycarbonate resin derived from bottles, polycarbonate resin derived from discs, polycarbonate resin derived from sheets, polycarbonate resin derived from meter covers, and polycarbonate resin derived from headlamp lenses.

12. The melt volume rate (MVR) of the recycled polycarbonate resin measured in accordance with ISO 1133 at 300°C and a load of 1.20 kgf is 4 to 30 cm 3 2. The resin composition according to claim 1, wherein the polyalkylene terephthalate resin has a viscosity of 100 to 150° C. / 10 minutes, further comprising an ester exchange inhibitor in an amount of 0.01 to 2 parts by mass per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin, the polyalkylene terephthalate resin comprises a polybutylene terephthalate resin, the flame retardant comprises a bromine-based flame retardant, further comprising an elastomer in an amount of 1 to 30 parts by mass per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin, the recycled polycarbonate resin comprising 0.2 to 1000 ppm by mass of aluminum element and 0.2 to 100 ppm by mass of iron element, and further comprising 0.1 to 3 parts by mass of carbon black per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin.

13. The resin composition according to claim 1, 2, 4 or 12, wherein the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin in a total of 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin is 30 / 70 to 55 / 45.

14. The resin composition according to claim 1, 2, 4 or 12, wherein the recycled polycarbonate resin comprises a polycarbonate resin derived from bottles and / or sheets.

15. The resin composition according to claim 1, wherein a mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin in a total of 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin is 30 / 70 to 55 / 45, the recycled polycarbonate resin contains polycarbonate resin derived from bottles and / or sheets, and further contains 0.01 to 2 parts by mass of an ester exchange inhibitor per 100 parts by mass of the polyalkylene terephthalate resin and the polycarbonate resin, and the polyalkylene terephthalate resin contains polybutylene terephthalate resin.

16. Pellets of the resin composition according to claim 1, 2, 4, 12 or 15.

17. A molded article formed from the resin composition according to claim 1, 2, 4, 12 or 15.

18. A molded article formed from the pellets of claim 16.

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