Resin composition, pellets, and molded article

Abstract

The invention provides a resin composition, and pellets and a molded article. A resin composition containing 5-50 parts by mass of a flame retardant per 100 parts by mass of the total of a polyalkylene terephthalate resin and a polycarbonate resin, the mass ratio of the polyalkylene terephthalate resin to the polycarbonate resin being 10 / 90-90 / 10 per 100 parts by mass of the total of the polyalkylene terephthalate resin and the polycarbonate resin. The polycarbonate resin contains a polycarbonate resin derived from regeneration, and the amount of branches of the polycarbonate resin derived from regeneration is 50-3500 ppm by mass.

Description

Technical Field

[0001] This invention relates to resin compositions, granules, and molded articles. Background Technology

[0002] Resin compositions comprising polyalkylene terephthalate resins such as polybutylene terephthalate resin and polycarbonate resin have been studied (e.g., Patent Document 1).

[0003] Such resin compositions are widely used in electrical and electronic equipment components, automotive interior and exterior parts, and other electrical components and mechanical parts.

[0004] Existing technical documents

[0005] Patent documents

[0006] Patent Document 1: International Publication No. 2021 / 186025 Summary of the Invention

[0007] The problem that the invention aims to solve

[0008] In recent years, from the perspective of environmental impact, the use of recycled thermoplastic resins has been studied. However, when using recycled thermoplastic resins, there is a tendency for the resulting molded articles to have poor physical properties.

[0009] Based on the above-mentioned situation, the present invention attempts to use recycled polycarbonate resin. Specifically, the object of the present invention is to provide a resin composition, granules, and molded articles, wherein the resin composition comprises polyalkylene terephthalate resin, recycled polycarbonate resin, and a flame retardant, and is capable of achieving physical properties comparable to, or better than, those achieved when using virgin polycarbonate resin alone.

[0010] Solution for solving the problem

[0011] Based on the above-mentioned technical problems, the inventors conducted research and found that the above-mentioned technical problems can be solved by using a specified polycarbonate resin as a recycled polycarbonate resin and incorporating a flame retardant.

[0012] Specifically, the above-mentioned technical problems were solved by the following means.

[0013] <1> A resin composition comprising 5 to 50 parts by weight of a flame retardant relative to 100 parts by weight of a total of alkylene terephthalate resin and polycarbonate resin, wherein the mass ratio of alkylene terephthalate resin to polycarbonate resin in the total 100 parts by weight of the alkylene terephthalate resin and polycarbonate resin is 10 / 90 to 90 / 10, wherein the polycarbonate resin comprises recycled polycarbonate resin having a branching content of 50 to 3500 ppm by weight.

[0014] <2> According to the above <1> The resin composition, wherein, relative to 100 parts by weight of the total alkylene terephthalate resin and polycarbonate resin, comprises 1 to 30 parts by weight of elastomer, wherein the mass ratio of alkylene terephthalate resin to polycarbonate resin in the total 100 parts by weight of the alkylene terephthalate resin and polycarbonate resin is 80 / 20 to 20 / 80, and the recycled polycarbonate resin has a melt volumetric flow rate (MVR) of 2 to 11 cm⁻¹ as determined according to ISO 1133 at 300°C and a load of 1.20 kgf. 3 / 10 minutes.

[0015] <3> according to <1> or <2> The resin composition wherein the recycled polycarbonate resin contains 10 to 80 ppm by weight of bisphenol A.

[0016] <4> according to <1> The resin composition wherein the recycled polycarbonate resin has a melt volumetric flow rate (MVR) of 4–30 cm⁻¹ as determined by ISO 1133 at 300°C and a load of 1.20 kgf. 3 / 10 minutes.

[0017] <5> according to <1> ~ <4> The resin composition of any one of the following, wherein, relative to a total of 100 parts by weight of the polyethylene terephthalate resin and the polycarbonate resin, further comprises 0.01 to 2 parts by weight of an ester exchange inhibitor.

[0018] <6> according to <1> ~ <5> The resin composition according to any one of the following methods, wherein the polyalkylene terephthalate resin comprises 50% or more of polybutylene terephthalate resin.

[0019] <7> according to <1> ~ <6> The resin composition according to any one of the following methods, wherein the flame retardant comprises a brominated flame retardant.

[0020] <8> according to <1> ~ <7> The resin composition according to any one of the following methods further comprises 3 to 30 parts by weight of elastomer relative to a total of 100 parts by weight of the polyethylene terephthalate resin and the polycarbonate resin.

[0021] <9> according to <1> ~ <8> The resin composition according to any one of the following, wherein the polycarbonate resin derived from recycled contains aluminum in a ratio of 0.2 to 1000 ppm by mass and iron in a ratio of 0.2 to 100 ppm by mass.

[0022] <10> according to <1> ~ <9> The resin composition according to any one of the following methods, wherein the resin composition is molded into a test piece for UL-94 testing with a thickness of 0.74 mm or 1.0 mm, and the flame retardancy meets V-0 according to UL-94 testing.

[0023] <11> according to <1> ~ <10> The resin composition of any one of the following, wherein the polycarbonate resin derived from recycled materials comprises at least one of polycarbonate resin derived from bottles, polycarbonate resin derived from discs, polycarbonate resin derived from sheets, polycarbonate resin derived from instrument panels, and polycarbonate resin derived from headlight lenses.

[0024] <12> according to <1> ~ <11> The resin composition described in any one of the following statements, wherein the melt volumetric flow rate (MVR) of the recycled polycarbonate resin, as determined according to ISO 1133 at 300°C and a load of 1.20 kgf, is 4–30 cm⁻¹. 3 / 10 minutes, the resin composition further comprises 0.01 to 2 parts by weight of an exchange inhibitor relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the polyalkylene terephthalate resin comprising polybutylene terephthalate resin, the flame retardant comprising a brominated flame retardant, the resin composition further comprising 1 to 30 parts by weight of an elastomer relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the recycled polycarbonate resin comprising aluminum in a ratio of 0.2 to 1000 ppm by weight and iron in a ratio of 0.2 to 100 ppm by weight, and the resin composition further comprising 0.1 to 3 parts by weight of carbon black relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin.

[0025] <13> according to <1> ~ <12> The resin composition according to any one of the following methods, wherein the mass ratio of the alkylene terephthalate resin to the polycarbonate resin in a total of 100 parts by mass of the alkylene terephthalate resin and the polycarbonate resin is 30 / 70 to 55 / 45.

[0026] <14> according to <1> ~ <13> The resin composition of any one of the following, wherein the polycarbonate resin derived from recycled materials comprises polycarbonate resin derived from bottles and / or sheets.

[0027] <15> according to <1> ~ <14> The resin composition according to any one of the following, wherein the mass ratio of the alkylene terephthalate resin to the polycarbonate resin in a total of 100 parts by mass of the alkylene terephthalate resin and the polycarbonate resin is 30 / 70 to 55 / 45, the polycarbonate resin derived from recycled materials comprises polycarbonate resin derived from bottles and / or sheets, and the resin composition further comprises 0.01 to 2 parts by mass of an exchange inhibitor relative to the total of 100 parts by mass of the alkylene terephthalate resin and the polycarbonate resin, wherein the alkylene terephthalate resin comprises polybutylene terephthalate resin.

[0028] <16> A type of particle, which is based on <1> ~ <15> The resin composition particles described in any one of the above statements.

[0029] <17> A molded article, which is based on <1> ~ <15> The resin composition described in any one of the above statements is formed.

[0030] <18> A molded article, which is based on <16> The aforementioned particle formation.

[0031] In addition, the above-mentioned technical problems were also solved by the following means.

[0032] <2-1> A resin composition comprising, relative to 100 parts by weight of a total of alkylene terephthalate resin and polycarbonate resin, 3 to 30 parts by weight of an elastomer and 5 to 50 parts by weight of a flame retardant, wherein the mass ratio of alkylene terephthalate resin to polycarbonate resin in the total 100 parts by weight of the alkylene terephthalate resin and polycarbonate resin is 80 / 20 to 20 / 80, and the polycarbonate resin comprises recycled polycarbonate resin, wherein the recycled polycarbonate resin has a melt volumetric flow rate (MVR) of 2 to 11 cm⁻¹ as determined according to ISO 1133 under conditions of 300°C and a load of 1.20 kgf. 3 / 10 minutes, and the branched content is 50 to 3500 ppm by mass.

[0033] <2-2> According to the resin composition of <2-1>, wherein the mass ratio of the alkylene terephthalate resin to the polycarbonate resin in a total of 100 parts by mass of the alkylene terephthalate resin and the polycarbonate resin is 30 / 70 to 55 / 45.

[0034] <2-3> The resin composition according to <2-1> or <2-2>, wherein the polycarbonate resin derived from recycled materials comprises polycarbonate resin derived from bottles and / or sheets.

[0035] <2-4> The resin composition according to any one of <2-1> to <2-3> further comprises 0.01 to 2 parts by weight of an ester exchange inhibitor relative to a total of 100 parts by weight of the polyethylene terephthalate resin and the polycarbonate resin.

[0036] <2-5> The resin composition according to any one of <2-1> to <2-4>, wherein the polyalkylene terephthalate resin comprises polybutylene terephthalate resin.

[0037] <2-6> The resin composition according to any one of <2-1> to <2-5>, wherein the mass ratio of the alkylene terephthalate resin to the polycarbonate resin in a total of 100 parts by mass of the alkylene terephthalate resin and the polycarbonate resin is 30 / 70 to 55 / 45, the polycarbonate resin derived from recycled materials comprises 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 relative to a total of 100 parts by mass of the alkylene terephthalate resin and the polycarbonate resin, wherein the alkylene terephthalate resin comprises polybutylene terephthalate resin.

[0038] <2-7> A particle, which is a particle of the resin composition according to any one of <2-1> to <2-6>.

[0039] <2-8> A molded article formed from a resin composition according to any one of <2-1> to <2-6>.

[0040] <2-9> A molded article formed from particles according to <2-7>.

[0041] In addition, the above-mentioned technical problems were also solved by the following means.

[0042] <3-1> A resin composition comprising, relative to 100 parts by weight of a total of alkylene terephthalate resin and polycarbonate resin, 5 to 50 parts by weight of a flame retardant, wherein the mass ratio of alkylene terephthalate resin to polycarbonate resin in the total 100 parts by weight of the alkylene terephthalate resin and polycarbonate resin is 10 / 90 to 90 / 10, wherein the polycarbonate resin comprises recycled polycarbonate resin, wherein the recycled polycarbonate resin comprises 10 to 80 ppm by weight of bisphenol A and has a branching amount of 50 to 3500 ppm by weight.

[0043] <3-2> According to the resin composition described in <3-1>, the melt volumetric flow rate (MVR) of the recycled polycarbonate resin, as determined according to ISO 1133, is 4–30 cm⁻¹ under conditions of 300°C and a load of 1.20 kgf. 3 / 10 minutes.

[0044] <3-3> The resin composition according to <3-1> or <3-2> further comprises 0.01 to 2 parts by weight of an exchange inhibitor relative to 100 parts by weight of the total of the polyethylene terephthalate resin and the polycarbonate resin.

[0045] <3-4> The resin composition according to any one of <3-1> to <3-3>, wherein the polyalkylene terephthalate resin comprises polybutylene terephthalate resin.

[0046] <3-5> The resin composition according to any one of <3-1> to <3-4>, wherein the flame retardant comprises a brominated flame retardant.

[0047] <3-6> The resin composition according to any one of <3-1> to <3-5> further comprises 1 to 30 parts by weight of elastomer relative to a total of 100 parts by weight of the polyethylene terephthalate resin and the polycarbonate resin.

[0048] <3-7> The resin composition according to any one of <3-1> to <3-6>, wherein the polycarbonate resin derived from recycled contains aluminum in a ratio of 0.2 to 1000 ppm by mass and iron in a ratio of 0.2 to 100 ppm by mass.

[0049] <3-8> The resin composition according to any one of <3-1> to <3-7> further comprises 0.1 to 3 parts by weight of carbon black relative to 100 parts by weight of the total of the polyalkylene terephthalate resin and the polycarbonate resin.

[0050] <3-9> The resin composition according to any one of <3-1> to <3-8>, wherein the resin composition is molded into a test piece with a thickness of 0.74 mm for UL-94 testing, and the flame retardancy meets V-0 according to UL-94 testing.

[0051] <3-10> The resin composition according to any one of <3-1> to <3-9>, wherein the polycarbonate resin derived from recycled materials comprises at least one of polycarbonate resin derived from bottles, polycarbonate resin derived from instrument panels, and polycarbonate resin derived from headlight lenses.

[0052] <3-11> The resin composition according to any one of <3-1> to <3-10>, wherein the melt volumetric flow rate (MVR) of the recycled polycarbonate resin, as determined according to ISO 1133, is 4 to 30 cm³ / h at 300°C and a load of 1.20 kgf. 3 / 10 minutes, the resin composition further comprises 0.01 to 2 parts by weight of an exchange inhibitor relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the polyalkylene terephthalate resin comprising polybutylene terephthalate resin, the flame retardant comprising a brominated flame retardant, the resin composition further comprising 1 to 30 parts by weight of an elastomer relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the recycled polycarbonate resin comprising aluminum in a ratio of 0.2 to 1000 ppm by weight and iron in a ratio of 0.2 to 100 ppm by weight, and the resin composition further comprising 0.1 to 3 parts by weight of carbon black relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin.

[0053] <3-12> A particle, which is a particle of the resin composition according to any one of <3-1> to <3-11>.

[0054] <3-13> A molded article formed from a resin composition according to any one of <3-1> to <3-11>.

[0055] <3-14> A molded article formed from particles according to <3-12>.

[0056] Invention Effects

[0057] According to the present invention, a resin composition, granules, and molded articles can be provided, said resin composition comprising polyalkylene terephthalate resin, recycled polycarbonate resin, and flame retardant, which can achieve physical properties comparable to or better than those achieved when using virgin polycarbonate resin alone. Detailed Implementation

[0058] The following describes in detail the methods for implementing the present invention (hereinafter referred to only as "this embodiment"). It should be noted that the following embodiment is an example for illustrating the present invention, and the present invention is not limited to this embodiment.

[0059] It should be noted that in this specification, "~" is used to include the values ​​recorded before and after it as the lower limit and upper limit values.

[0060] Unless otherwise specified, all physical property values ​​and characteristic values ​​in this specification refer to those at 23°C.

[0061] Unless otherwise specified, the measurement methods described in the standards shown in this instruction manual may vary depending on the year, and are based on the standards at the time of January 1, 2023.

[0062] The resin composition of this embodiment is characterized in that it contains 5 to 50 parts by weight of flame retardant relative to a total of 100 parts by weight of alkylene terephthalate resin and polycarbonate resin, wherein the mass ratio of alkylene terephthalate resin to polycarbonate resin in the total of 100 parts by weight of alkylene terephthalate resin and polycarbonate resin is 10 / 90 to 90 / 10, and the polycarbonate resin comprises recycled polycarbonate resin, wherein the branching content of the recycled polycarbonate resin is 50 to 3500 ppm by weight.

[0063] By configuring it in this way, a resin composition comprising a polyalkylene terephthalate resin, a recycled polycarbonate resin (sometimes referred to as "recycled polycarbonate resin" in this specification), and a flame retardant can be obtained, which can achieve physical properties comparable to or better than those achieved when using virgin polycarbonate resin alone.

[0064] For example, if a flame retardant is added to the resin composition, there is usually a tendency for poor impact resistance. However, in this embodiment, by using a specified recycled polycarbonate resin, there is a tendency to achieve high impact resistance. Furthermore, the resin composition of this embodiment also tends to maintain high flame retardancy, with flame retardancy properties equal to or even better than those of virgin polycarbonate resin, and since recycled materials can be used, the environmental impact can be reduced.

[0065] Furthermore, if recycled polycarbonate resin is used, there is a tendency for a difference in nominal strain at break. In this embodiment, by using a specified recycled polycarbonate resin, there is a tendency to increase the nominal strain at break. In addition, the resin composition of this embodiment tends to increase the crystallization temperature (Tc).

[0066] Furthermore, it is known that polycarbonate resins with a high degree of branching generally exhibit excellent flame retardancy. This is believed to be because the numerous branched structures cause polycarbonate molecules to become entangled with each other, making it less likely to cause shape changes in the molded product during combustion and effectively suppressing dripping. Additionally, it is believed that charring occurs on the surface of the molded product, and the charred surface is less likely to collapse, thus shortening the burning time.

[0067] However, the inventors conducted research and found that when used in combination with polyalkylene terephthalate resin, the flame retardancy is excellent when the polycarbonate resin has a low branching content. The reason for this is speculated to be that if there are many branches, the terminal hydroxyl groups of the polycarbonate are more likely to undergo transesterification with the polyalkylene terephthalate resin, resulting in an increase in low molecular weight components or a decrease in thermal stability.

[0068] In particular, since recycled polycarbonate resins are often made from a mixture of various raw materials, they mostly contain branched polycarbonate resins. However, the inventors have conducted research and found that by setting the branch content of the recycled polycarbonate resin to 50–3500 ppm by mass, flame retardancy comparable to, or even better than, that achieved when using virgin polycarbonate resin alone can be achieved. As a result, the environmental impact can be reduced because recycled materials can be used.

[0069] <Polyalkyl terephthalate resin>

[0070] The resin composition of this embodiment comprises a polyalkylene terephthalate resin.

[0071] Polyalkylene terephthalate resin is a polyester obtained by polycondensation of terephthalic acid (a dicarboxylic acid compound) and diol, and can be either homopolymer or copolyester.

[0072] As the dicarboxylic acid compound constituting the polyalkylene terephthalate resin, a terephthalic acid compound or its ester-forming derivative is preferably used.

[0073] Aromatic dicarboxylic acids other than terephthalic acid can also be used in combination, such as isophthalic acid, phthalic 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, diphenyl ether-4,4'-dicarboxylic acid, diphenylmethane-4,4'-dicarboxylic acid, diphenyl sulfone-4,4'-dicarboxylic acid, diphenyl isopropylidene-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-butylphenylene-4,4'-dicarboxylic acid, pyridine-2,5-dicarboxylic acid, etc. In addition to being free acids, they can also be used as ester-forming derivatives such as dimethyl esters in polycondensation reactions.

[0074] Of the above, isophthalic acid or its ester-forming derivatives are particularly preferred.

[0075] It should be noted that, if the quantity is small, it can be used in combination with terephthalic acid, the above-mentioned aromatic dicarboxylic acids, adipic acid, azelaic acid, dodecanoic acid, sebacic acid and other aliphatic dicarboxylic acids, 1,2-cyclohexanedicarboxylic acid, 1,3-cyclohexanedicarboxylic acid and 1,4-cyclohexanedicarboxylic acid and other alicyclic dicarboxylic acids.

[0076] Examples of dihydroxy compounds constituting polyalkylene terephthalate resins include: ethylene glycol, propylene glycol, butanediol, hexanediol, neopentyl glycol, aliphatic diols such as 2-methylpropane-1,3-diol, diethylene glycol, and triethylene glycol, alicyclic diols such as cyclohexane-1,4-diethanol, and mixtures thereof. Among these, butanediol and ethylene glycol are particularly preferred.

[0077] It should be noted that one or more long-chain diols with a molecular weight of 400 to 6000, such as polyethylene glycol, poly1,3-propanediol, and polytetramethylene glycol, can also be copolymerized. In addition, aromatic diols such as hydroquinone, resorcinol, naphthalene glycol, dihydroxydiphenyl ether, and 2,2-bis(4-hydroxyphenyl)propane can also be used.

[0078] In addition to the difunctional monomers mentioned above, trifunctional monomers such as trimellitic acid, pyromellitic acid, pyromellitic acid, pentaerythritol, and trimethylolpropane can be used in small amounts to introduce branched structures. In order to adjust the molecular weight, monofunctional compounds such as fatty acids can also be used in small amounts.

[0079] As the polyalkylene terephthalate resin, a resin mainly formed by the condensation polymerization of terephthalic acid and a glycol is preferred. Specifically, the resin is preferably formed from the condensation polymer in an amount exceeding 50% by mass of the total resin, more preferably 70% by mass or more, more preferably 80% by mass or more, further preferably 90% by mass or more, more preferably 95% by mass or more, and even more preferably 99% by mass or more. As the glycol, an aliphatic glycol is preferred, particularly 1,4-butanediol and / or ethylene glycol, more preferably 1,4-butanediol.

[0080] The amount of terminal carboxyl groups in the polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) can be appropriately selected and determined, typically 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, there is a tendency to more effectively suppress gas generation during melt molding of the resin composition. The lower limit of the amount of terminal carboxyl groups is not particularly limited, typically 3 eq / ton or more, preferably 5 eq / ton or more, and more preferably typically 10 eq / ton or more.

[0081] It should be noted that the amount of terminal carboxyl groups in the polyalkylene terephthalate resin is determined by titration using a 0.01 mol / L sodium hydroxide solution in 25 mL of benzyl alcohol after dissolving 0.5 g of the resin. Adjusting the amount of terminal carboxyl groups can be achieved through any conventionally known method, such as adjusting the polymerization conditions (e.g., feed ratio, polymerization temperature, reduced pressure method) or reacting the end-capping agent.

[0082] The intrinsic viscosity of the polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) is preferably 0.40 dL / g or higher, more preferably 0.50 dL / g or higher, even more preferably 0.55 dL / g or higher, further preferably 0.60 dL / g or higher, even more preferably 0.65 dL / g or higher, and even more preferably 0.80 dL / g or higher, 1.00 dL / g or higher, 1.20 dL / g or higher, and 1.23 dL / g or higher. By setting the intrinsic viscosity to the aforementioned lower limit or higher, there is a tendency to effectively suppress the reduction of physical properties such as strength, and consequently, there is a tendency to improve impact resistance and increase the nominal strain at fracture. Furthermore, 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, further 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, and 0.78 dL / g or less. By setting it below the aforementioned upper limit value, there is a tendency to suppress the decrease in resin flowability during injection molding, and there is a tendency to suppress the peak pressure during injection molding.

[0083] Intrinsic viscosity was determined by the following method.

[0084] Particles of polyalkylene terephthalate were dissolved in a mixed solvent of phenol and 1,1,2,2-tetrachloroethane (mass ratio 1 / 1) at 110°C for 1 hour by stirring. The solution was then cooled to 30°C. Using an automated solution viscometer, the drop times of the sample solution and the drop times of the solvent alone were measured at 30°C, and the intrinsic viscosity was calculated using a formula.

[0085] Intrinsic viscosity = ((1+4K)) H η sp ) 0.5 -1) / (2K) H C)

[0086] Here, η sp =η / η0-1, where η is the number of seconds the sample solution falls, η0 is the number of seconds the solvent alone falls, C is the concentration of the sample solution (g / dL), and KH K is the Huggins constant. H Use 0.33.

[0087] The fully automated solution viscometer uses a viscometer manufactured by Shibayama Scientific Corporation.

[0088] In the case where the resin composition of this embodiment contains two or more polyalkylene terephthalate resins, the intrinsic viscosity of the mixture is set.

[0089] As for polyalkylene terephthalate resins, 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 are preferred. Representative examples are polybutylene terephthalate resins and polyethylene terephthalate resins. They are preferably close to homopolymer polyesters, that is, preferably, the resin as a whole is composed of 95 mol% or more of terephthalic acid and 1,4-butanediol or ethylene glycol.

[0090] The preferred polyalkylene terephthalate resin is polybutylene terephthalate resin and / or polyethylene terephthalate resin.

[0091] Preferably, the polyalkylene terephthalate resin contains polybutylene terephthalate resin as a main component; more preferably, more than 50% by mass of the polyalkylene terephthalate resin is polybutylene terephthalate resin; even more preferably, more than 50% by mass of the polyalkylene terephthalate resin is polybutylene terephthalate resin. In this case, it is also preferable that the polyethylene terephthalate resin is present in a range of less than 50% by mass.

[0092] Polybutylene terephthalate (PET) resin can be manufactured by batch or continuous melt polymerization of a dicarboxylic acid component, primarily composed of terephthalic acid, or its ester derivatives, and a diol component, primarily composed of 1,4-butanediol. Furthermore, after manufacturing low molecular weight PET resin via melt polymerization, solid-state polymerization can be carried out under nitrogen flow or reduced pressure, thereby increasing the degree of polymerization (or molecular weight) to the desired value.

[0093] The preferred manufacturing method for polybutylene terephthalate resin is a continuous melt polycondensation process involving a dicarboxylic acid component, with terephthalic acid as the main component, and a diol component, with 1,4-butanediol as the main component.

[0094] The catalyst used in the esterification reaction can be any known catalyst, such as titanium compounds, tin compounds, magnesium compounds, calcium compounds, etc. Among these, titanium compounds are particularly preferred. Specific examples of titanium compounds as esterification catalysts include titanium alkoxides such as tetramethyl titanate, tetraisopropyl titanate, and tetrabutyl titanate, and titanium phenolates such as tetraphenyl titanate.

[0095] Polybutylene terephthalate resin can be a polybutylene terephthalate resin modified by copolymerization (hereinafter, sometimes also referred to as "modified polybutylene terephthalate resin"). As specific preferred copolymers, examples include polyester ether resins copolymerized from polyalkylene glycols (especially polytetramethylene glycol), dimer acid copolymerized polybutylene terephthalate resins, and isophthalic acid copolymerized polybutylene terephthalate resins.

[0096] When using a polyester ether resin copolymerized from polytetramethylene glycol as a modified polybutylene terephthalate resin, the proportion of tetramethylene glycol 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.

[0097] When using dimer acid copolymerized polybutylene terephthalate resin as modified polybutylene terephthalate resin, the proportion of dimer acid component in the total carboxylic acid component, calculated by carboxylic acid groups, is preferably 0.5 to 30 mol%, more preferably 1 to 20 mol%, and even more preferably 3 to 15 mol%.

[0098] When using isophthalic acid copolymer polybutylene terephthalate resin as the modified polybutylene terephthalate resin, the proportion of isophthalic acid in the total carboxylic acid components, calculated by carboxylic acid groups, is preferably 1 to 30 mol%, more preferably 1 to 20 mol%, and even more preferably 3 to 15 mol%.

[0099] Among the modified polybutylene terephthalate resins, polyester ether resins copolymerized from polytetramethylene glycol and isophthalic acid copolymerized polybutylene terephthalate resins are preferred.

[0100] In this embodiment, the content of polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) in the resin composition is preferably 10% by mass or more, more preferably 20% by mass or more, even more preferably 30% by mass or more, and preferably 60% by mass or less, more preferably 50% by mass or less.

[0101] The resin composition of this embodiment may contain only one type of polyalkylene terephthalate resin (preferably polybutylene terephthalate resin), or it may contain two or more types. When two or more types are contained, the total amount is preferably within the range described above.

[0102] Furthermore, the polyalkylene terephthalate resin in the resin composition of this embodiment preferably contains 40% or more of polybutylene terephthalate resin, more preferably 50% or more, 55% or more, 60% or more, 70% or more, 80% or more, 90% or more, and particularly preferably 100% or more.

[0103] <Polycarbonate resin>

[0104] The resin composition of this embodiment comprises polycarbonate resin.

[0105] Polycarbonate resin is a homopolymer or copolymer obtained by reacting a dihydroxy compound or a compound with a small amount of a polyhydroxy compound with phosgene or diester carbonate. There are no particular limitations on the manufacturing method of polycarbonate resin; polycarbonate resins manufactured using conventionally known methods such as the phosgene method (interfacial polymerization) and the melt method (transesterification) can be used. Polycarbonate resins obtained using the melt method tend to have a more branched structure. Furthermore, in interfacial polymerization, polycarbonate resins with branched structures can also be obtained by using a branching agent during polymerization.

[0106] The dihydroxy compound used as a raw material is preferably an aromatic dihydroxy compound, more preferably bisphenol, and even more preferably bisphenol A. Alternatively, a compound having one or more tetraalkylphosphonium sulfonate bondsed to the aforementioned aromatic dihydroxy compound may also be used.

[0107] In this embodiment, it is preferable that 90% or more by mass of the dihydroxy compound used as a raw material monomer is a polycarbonate resin derived from bisphenol A, and more preferably 95% or more by mass is a polycarbonate resin derived from bisphenol A. It should be noted that the structural units represented by formulas (C1) to (C4) described later are also derived from bisphenol A. For example, they are generated by a rearrangement reaction (Fries rearrangement) occurring simultaneously in the polymerization reaction system during polycarbonate polymerization via transesterification of bisphenol A and diphenyl carbonate (melt method). Furthermore, the structural units represented by formulas (C1) to (C4) described later are also generated by a Fris rearrangement occurring in the polycarbonate resin derived from bisphenol A due to photodeterioration caused by ultraviolet light or the like.

[0108] Two or more polycarbonate resins can be used in combination.

[0109] To adjust the molecular weight of polycarbonate resin, monoary aromatic hydroxyl compounds can be used, such as m-methylphenol and p-methylphenol, m-propylphenol and p-propylphenol, p-tert-butylphenol, p-long-chain alkyl-substituted phenols, etc.

[0110] The polycarbonate resin used in this embodiment comprises polycarbonate resin derived from recycled polycarbonate resin (recycled polycarbonate resin).

[0111] Recycled polycarbonate resins often contain bisphenol A due to the thermal history of previous processes. However, by reducing the bisphenol A content to 10–80 ppm by mass of recycled polycarbonate resins, flame retardancy can be obtained that is comparable to or better than that obtained when using virgin polycarbonate resins alone.

[0112] Examples of recycled polycarbonate resins include substances obtained by regenerating recycled used polycarbonate resin molded bodies by crushing, cleaning and reusing the material, substances obtained by chemical regeneration (chemical decomposition method), and preferably substances obtained by material regeneration.

[0113] Chemical recycling involves the chemical decomposition of recycled used polycarbonate resin molds and their return to the raw material level for the resynthesis of polycarbonate. On the other hand, material recycling includes processes such as removing foreign matter from recycled used polycarbonate resin molds, pulverizing, alkali washing, drying, further pulverizing, flake formation, or granulation using an extruder.

[0114] It should be noted that polycarbonate resins that are not recycled polycarbonate resins are referred to as virgin polycarbonate resins.

[0115] Examples of recycled polycarbonate resin include polycarbonate resin derived from bottles, polycarbonate resin derived from discs, polycarbonate resin derived from sheets (derived from polycarbonate resin containing a film), polycarbonate resin derived from instrument covers (e.g., meter covers), and polycarbonate resin derived from headlight lenses. Preferably, at least one of polycarbonate resin derived from bottles, polycarbonate resin derived from instrument covers, and polycarbonate resin derived from headlight lenses is preferred. More preferably, polycarbonate resin derived from bottles and / or sheets is preferred.

[0116] Recycled polycarbonate resins can be categorized as follows: post-consumer recycled (PCR) products obtained by recycling and reusing products used in the market, and post-industrial recycled (PIR) products obtained by recycling materials generated in the product manufacturing process before they enter the market. Any type is acceptable, but from the perspective of reducing environmental impact, post-consumer recycled products are preferred.

[0117] The recycled polycarbonate resin used in this embodiment preferably contains 10 to 80 ppm by weight of bisphenol A. The bisphenol A content in the recycled polycarbonate resin is preferably 15 ppm by weight or more, more preferably 20 ppm by weight or more, even more preferably 25 ppm by weight or more, and preferably 70 ppm by weight or less, more preferably 60 ppm by weight or less, even more preferably 55 ppm by weight or less, even more preferably 50 ppm by weight or less, even more preferably 49 ppm by weight or less, even more preferably 45 ppm by weight or less, particularly more preferably 40 ppm by weight or less, and even more preferably 35 ppm by weight or less and 30 ppm by weight or less. Setting the content above or below the lower limit tends to improve fluidity and increase the availability of recycled polycarbonate resin. Furthermore, setting the content below the upper limit tends to further improve flame retardancy and reduce the amount of gas generated. Moreover, from the viewpoint of balancing the availability, ease of production, and quality stability of recycled polycarbonate resin, it is also preferable to set the content within the upper and lower limits.

[0118] The bisphenol A content in the recycled polycarbonate resin was determined according to the description in the examples described later.

[0119] In this embodiment, the branching amount of the recycled polycarbonate resin used is 50 to 3500 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 1000 ppm by mass or more, even more preferably 1500 ppm by mass or more, even more preferably 2000 ppm by mass or more, and preferably 3000 ppm by mass or less, more preferably 2500 ppm by mass or less. By setting it to the lower limit or above, there is a tendency to further improve the effect of preventing dripping during combustion. Furthermore, by setting it to the upper limit or below, there is a tendency to suppress the decomposition of the resin caused by transesterification between the polyalkylene terephthalate resin and the polycarbonate resin, a tendency to increase the crystallization temperature, a tendency to decrease the combustion time, and a tendency to decrease the amount of gas produced.

[0120] The branching content of the recycled polycarbonate resin was determined according to the description of the examples described later.

[0121] The recycled polycarbonate resin used in this embodiment may contain any one or more structural units of formulas (C1) to (C4).

[0122] [Chemical Formula 1]

[0123]

[0124] In this embodiment, the branching content of the recycled polycarbonate resin is 50 to 3500 ppm by mass. Preferably, the branching content of the recycled polycarbonate resin is 100 ppm by mass or more, more preferably 200 ppm by mass or more, further preferably 500 ppm by mass or more, even more preferably 1000 ppm by mass or more, even more preferably 1500 ppm by mass or more, even more preferably 2000 ppm by mass or more, and preferably 3000 ppm by mass or less, more preferably 2500 ppm by mass or less. By setting the value to the lower limit or above, there is a tendency to further improve the effect of preventing dripping during combustion. Furthermore, by setting the value to the upper limit or below, there is a tendency to suppress the decomposition of the resin caused by transesterification between the polyalkylene terephthalate resin and the polycarbonate resin, a tendency to increase the crystallization temperature, a tendency to decrease the combustion time, and a tendency to decrease the amount of gas produced.

[0125] The branching content of the recycled polycarbonate resin was determined according to the description of the examples described later.

[0126] In this embodiment, the recycled polycarbonate resin, during hydrolysis, preferably contains PSA at 5 ppm or more, more preferably 30 ppm or more, further preferably 50 ppm or more, more preferably 100 ppm or more, and even more preferably 200 ppm or more. It is also preferably 700 ppm or less, more preferably 600 ppm or less, more preferably 500 ppm or less, even more preferably 380 ppm or less, and even more preferably 350 ppm or less. By setting the value above the lower limit, there is a tendency to further improve the anti-dripping effect during combustion tests. Furthermore, by setting the value below the upper limit, there is a tendency to suppress resin decomposition caused by transesterification between the polyalkylene terephthalate resin and the polycarbonate resin, resulting in excellent thermal stability, reduced combustion time, and reduced gas production.

[0127] In this embodiment, the content of PSA-Me relative to 100 parts by weight of recycled polycarbonate resin during hydrolysis is preferably 10 ppm or more, more preferably 50 ppm or more, further preferably 150 ppm or more, even more preferably 300 ppm or more, and still more preferably 500 ppm or more. It is also preferably 2000 ppm or less, more preferably 1500 ppm or less, even more preferably 1000 ppm or less, still more preferably 900 ppm or less, and still more preferably 800 ppm or less. By setting the content to the lower limit or above, there is a tendency to further improve the anti-dripping effect during combustion tests. Furthermore, by setting the content to the upper limit or below, there is a tendency to suppress resin decomposition caused by transesterification between polyalkylene terephthalate resin and polycarbonate resin, a tendency to have excellent thermal stability, a tendency to reduce combustion time, and a tendency to reduce the amount of gas produced.

[0128] In this embodiment, the recycled polycarbonate resin, during hydrolysis, has a PBA content of 0 parts by mass or more relative to 100 parts by mass of recycled polycarbonate, preferably 0.01 ppm or more, more preferably 10 ppm or more, further preferably 30 ppm or more, even more preferably 100 ppm or more, even more preferably 400 ppm or more, and preferably 2000 ppm or less, more preferably 1500 ppm or less, even more preferably 1000 ppm or less, even more preferably 900 ppm or less, and even more preferably 800 ppm or less. By setting the value to the lower limit or above, there is a tendency to further improve the effect of preventing dripping during combustion tests. Furthermore, by setting the value to the upper limit or below, there is a tendency to suppress the decomposition of the resin caused by transesterification between the polyalkylene terephthalate resin and the polycarbonate resin, a tendency to have excellent thermal stability, a tendency to reduce combustion time, and a tendency to reduce the amount of gas produced.

[0129] In this embodiment, the content of dicarboxylic acids (DA1 and DA2, described later) in the recycled polycarbonate resin during hydrolysis is preferably 1 ppm or more, more preferably 10 ppm or more, further preferably 100 ppm or more, even more preferably 200 ppm or more, and still more preferably 300 ppm or more. Furthermore, it is preferably 1500 ppm or less, more preferably 1000 ppm or less, even more preferably 900 ppm or less, still more preferably 800 ppm or less, and still more preferably 700 ppm or less. By setting the content to the lower limit or above, there is a tendency to further improve the anti-dripping effect during combustion tests. Furthermore, by setting the content to the upper limit or below, there is a tendency to suppress resin decomposition caused by transesterification between the alkylene terephthalate resin and the polycarbonate resin, a tendency to have excellent thermal stability, a tendency to reduce combustion time, and a tendency to reduce the amount of gas produced.

[0130] [Chemical Formula 2]

[0131]

[0132] The contents of PSA, PSA-Me, PBA, and dicarboxylic acids (DA1, DA2) generated from the hydrolysis of recycled polycarbonate resin were determined according to the description of the examples described later.

[0133] In the resin composition of this embodiment, the melt volumetric flow rate (MVR) of the recycled polycarbonate resin, measured according to ISO 1133 at 300°C and a load of 1.20 kgf, is preferably 2 to 30 cm. 3 / 10 minutes.

[0134] The MVR of the recycled polycarbonate resin is more preferably 3cm. 3 / 10 minutes or more, further preferably 4cm 3 / 10 minutes or more, then the next step is to optimize to 5cm 3 / 10 minutes or more, with 6cm being a further preferred size 3 / 10 minutes or more, and preferably 20cm 3 / less than 10 minutes, preferably 15cm 3 / less than 10 minutes, further preferably 11cm 3 / less than 10 minutes, the next step is to select 10cm 3 / less than 10 minutes, with 9cm being a further preferred option 3 / less than 10 minutes, with 8cm being a further preferred size 3 / less than 10 minutes, especially preferably 7cm 3 / less than 10 minutes. Setting it above the lower limit tends to increase fluidity. Furthermore, setting it below the upper limit tends to increase mechanical properties and impact resistance.

[0135] The resin composition of this embodiment may contain only one type of recycled polycarbonate resin, or it may contain two or more types. When two or more types are contained, the MVR of the mixture is preferably within the range described above.

[0136] The dispersion (Mw / Mn) of the recycled polycarbonate resin is preferably 2.6 or higher, and more preferably 3.5 or lower, and even more preferably 3.3 or lower. The dispersion of the recycled polycarbonate resin is measured according to the description in the examples described later.

[0137] Recycled polycarbonate resin typically has a higher metal content than virgin polycarbonate resin due to the resin consumption / regeneration process. However, even recycled polycarbonate resin can sometimes have a low metal content.

[0138] From the viewpoint of ease of obtaining, ease of production, and quality stability of recycled polycarbonate resin, the aluminum content in the recycled polycarbonate resin used in this embodiment is preferably 0.2 to 1000 ppm by weight relative to 100 parts by weight of the recycled polycarbonate resin. Furthermore, the aluminum content is preferably 0.3 ppm by weight or more, more preferably 0.5 ppm by weight or more, even more preferably 1 ppm by weight or more, further preferably 2 ppm by weight or more, even more preferably 5 ppm by weight or more, even more preferably 7 ppm by weight or more, particularly more preferably 8 ppm by weight or more, further preferably 500 ppm by weight or less, even more preferably 300 ppm by weight or less, even more preferably 100 ppm by weight or less, even more preferably 50 ppm by weight or less, even more preferably 30 ppm by weight or less, even more preferably 15 ppm by weight or less, and particularly more preferably 10 ppm by weight or less. By setting the content to the lower limit or above, there is a tendency to improve the laser marking properties. Furthermore, by setting the value below the aforementioned upper limit, there is a tendency for insulation properties such as dielectric breakdown strength to be further improved, for resistance to tracking to be improved, and for the amount of gas generated to be reduced.

[0139] From the viewpoint of ease of obtaining recycled polycarbonate resin, ease of production, and quality stability, in this embodiment, the recycled polycarbonate resin preferably contains iron in a ratio of 0.2 to 100 ppm by mass relative to the polycarbonate resin. The iron content relative to the recycled polycarbonate resin is more preferably 0.8 ppm by mass or more, further 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, further 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 value above or below the lower limit, there is a tendency for improved laser marking properties. Furthermore, by setting the value below the upper limit, there is a tendency for further improved insulation properties such as dielectric breakdown strength, improved resistance to tracking, and reduced gas generation.

[0140] From the viewpoint of ease of obtaining recycled polycarbonate resin, ease of production, and quality stability, in this embodiment, the recycled polycarbonate resin preferably contains phosphorus in a ratio of 1 to 200 ppm by mass relative to the polycarbonate resin. The phosphorus content relative to the recycled polycarbonate resin is more preferably 2 ppm by mass or more, further preferably 3 ppm by mass or more, even more preferably 4 ppm by mass or more, and still more preferably 5 ppm by mass or more. Furthermore, it is more preferably 150 ppm by mass or less, even more preferably 100 ppm by mass or less, still more preferably 50 ppm by mass or less, and still more preferably 10 ppm by mass or less. By setting the content to the lower limit or above, there is a tendency to suppress transesterification of the mixture of polyalkylene terephthalate resin and recycled polycarbonate resin and to improve the heat resistance of the resin. Furthermore, by setting the content to the upper limit or below, there is a tendency to further improve insulation properties such as dielectric breakdown strength, a tendency to reduce the amount of gas generated, and a tendency to improve hydrolysis resistance.

[0141] In the resin composition of this embodiment, the polycarbonate resin may contain only recycled polycarbonate resin, or it may further contain virgin polycarbonate resin in addition to recycled polycarbonate resin.

[0142] The content of recycled polycarbonate resin in the resin composition of this embodiment is preferably 50 parts by weight or more, more preferably 60 parts by weight or more, even more preferably 70 parts by weight or more, further preferably 80 parts by weight or more, even more preferably 90 parts by weight or more, and further preferably 100 parts by weight or less. By setting it to the lower limit or above, recyclability is improved. By setting it to the upper limit or below, there is a tendency to further improve generation stability and quality stability.

[0143] <Blend ratio of alkylene terephthalate resin to polycarbonate resin>

[0144] In the resin composition of this embodiment, the mass ratio of alkyl terephthalate resin to polycarbonate resin in a total of 100 parts by mass of alkyl terephthalate resin (preferably polybutylene terephthalate resin) and polycarbonate resin is 10 / 90 to 90 / 10, preferably 80 / 20 to 20 / 80, and more preferably 30 / 70 to 55 / 45. By setting such a blending ratio, various molded articles with excellent physical properties can be obtained, and there is a tendency to further improve the balance between chemical resistance and dimensional stability.

[0145] Furthermore, regarding the blending ratio, in a total of 100 parts by weight of polyalkylene terephthalate resin and polycarbonate resin, the proportion of polyalkylene terephthalate resin is preferably 20 parts by weight or more, more preferably 30 parts by weight or more, even more preferably 35 parts by weight or more, further preferably 40 parts by weight or more, even more preferably 45 parts by weight or more, depending on the application, even more preferably 50 parts by weight or more, particularly more preferably 60 parts by weight or more, 70 parts by weight or more, 75 parts by weight or more, and preferably 85 parts by weight or less. Depending on the application, it can be 50 parts by weight or less, or 49 parts by weight or less.

[0146] The resin composition of this embodiment may contain only one type of polyalkylene terephthalate resin and one type of polycarbonate resin, or it may contain two or more types. When two or more types are contained, the total amount is preferably within the range described above.

[0147] In this embodiment, the total amount of polyalkylene terephthalate resin (preferably polybutylene terephthalate resin) and polycarbonate resin (preferably recycled polycarbonate resin) in the resin composition is preferably 10% by mass or more, more preferably 20% by mass or more, further preferably 30% by mass or more, even more preferably 40% by mass or more, and still more preferably 45% by mass or more. Furthermore, it is preferably 90% by mass or less, more preferably 80% by mass or less, even more preferably 70% by mass or less, still more preferably 60% by mass or less, and still more preferably 55% by mass or less. By setting the value above the lower limit, there is a tendency for improved moldability, increased nominal strain at break, and improved impact resistance. Furthermore, by setting the value below the upper limit, there is a tendency for improved appearance of the molded article and improved flame retardancy.

[0148] Flame retardants

[0149] The resin composition of this embodiment contains a flame retardant. By including a flame retardant, flame retardancy can be achieved.

[0150] Flame retardants include halogenated flame retardants, phosphorus-based flame retardants (such as metal salts of phosphonates and melamine polyphosphate), nitrogen-based flame retardants (such as melamine cyanurate), and metal hydroxides (such as magnesium hydroxide). Phosphorus-based and halogenated flame retardants are preferred, with halogenated flame retardants being more preferred. Among phosphorus-based flame retardants, metal salts of phosphonates are more preferred. Among halogenated flame retardants, bromine-based flame retardants are more preferred.

[0151] In the resin composition of this embodiment, the proportion of brominated flame retardant in the flame retardant 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 in addition, 100% by mass or less.

[0152] When using brominated flame retardants as flame retardants, there is no particular limitation on the type of flame retardant. 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.

[0153] As a brominated phthalimide, the substance represented by formula (1) is preferred.

[0154] [Chemical Formula 3]

[0155]

[0156] (In formula (1), D represents a group consisting of two or more combinations of alkylene, arylene, -S(=O)2-, -C(=O)-, and -O-. i is an integer from 1 to 4.)

[0157] In formula (1), D represents a group consisting of two or more combinations of alkylene, arylene, -S(=O)2-, -C(=O)- and -O-, preferably a group consisting of a combination of alkylene or arylene with at least one of -S(=O)2-, -C(=O)- and -O-, more preferably a group consisting of a combination of alkylene or arylene with one of -S(=O)2-, -C(=O)- and -O-, and even more preferably alkylene.

[0158] As a group consisting of a combination of alkylene and -O-, for example, it is intended to also include combinations of two alkylene and one -O- (the same applies to other combinations).

[0159] The alkylene group of D is preferably an alkylene group having 1 to 6 carbon atoms, and more preferably methylene, ethylene, propylene, or butylene. The aryl group is preferably phenylene.

[0160] i is an integer from 1 to 4, preferably 4.

[0161] Examples of brominated phthalimides 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) diphenyl sulfone, N,N'-(bistetrabromophthalimide) diphenyl ketone, and N,N'-(bistetrabromophthalimide) diphenyl ether.

[0162] As a bromophthalimide, formula (1) is preferably a bromophthalimide represented by formula (2).

[0163] [Chemical Formula 4]

[0164]

[0165] (In equation (2), i is an integer from 1 to 4.)

[0166] i is an integer from 1 to 4, preferably 4.

[0167] As a brominated poly(meth)acrylate, the preferred polymer is obtained by homopolymerization of benzyl (meth)acrylate containing bromine atoms, copolymerization of two or more monomers, or copolymerization with other vinyl monomers, wherein the bromine atoms are added to the benzene rings and the number of additions is preferably 1 to 5 per benzene ring, and more preferably 4 to 5.

[0168] Examples of benzyl acrylates containing bromine atoms include pentabromobenzyl acrylate, tetrabromobenzyl acrylate, tribromobenzyl acrylate, or mixtures thereof. Furthermore, examples of benzyl methacrylates containing bromine atoms include methacrylates corresponding to the aforementioned acrylates.

[0169] Other vinyl monomers used for copolymerization with benzyl methacrylate containing bromine atoms include, specifically: acrylates such as acrylic acid, methyl acrylate, ethyl acrylate, butyl acrylate, and benzyl acrylate; methacrylates such as methacrylic acid, methyl methacrylate, ethyl methacrylate, butyl methacrylate, and benzyl methacrylate; unsaturated carboxylic acids or their anhydrides such as styrene, acrylonitrile, fumaric acid, and maleic acid; vinyl acetate, vinyl chloride, etc.

[0170] They are generally preferred to be used in amounts of equimolar or less, and especially preferred to be used in amounts of 0.5 times or less, relative to benzyl methacrylate containing bromine atoms.

[0171] In addition, as vinyl monomers, xylene diacrylate, xylene dimethacrylate, tetrabromoxylene diacrylate, tetrabromoxylene dimethacrylate, butadiene, isoprene, divinylbenzene, etc. can also be used, and they can usually be used in amounts of less than 0.5 times the molar amount of benzyl acrylate or benzyl methacrylate containing bromine atoms.

[0172] As a brominated poly(meth)acrylate, the preferred polymer is one obtained by homopolymerization of bromine-containing (meth)acrylate monomers, particularly benzyl (meth)acrylate, or copolymerization of two or more monomers, or copolymerization with other vinyl monomers. Furthermore, the bromine atom is added to the benzene ring, preferably 1 to 5 bromine atoms per benzene ring, and particularly preferably 4 to 5 bromine atoms per benzene ring.

[0173] As a brominated poly(meth)acrylate, pentabromobenzyl poly(meth)acrylate is preferred from the perspective of high bromine content.

[0174] The molecular weight of the brominated poly(meth)acrylate is arbitrary and can be appropriately selected. Preferred by weight-average molecular weight (Mw), it is 3000 or more, more preferably 10000 or more, further preferably 15000 or more, even more preferably 20000 or more, and still more preferably 25000 or more. By setting it to the lower limit or above, there is a tendency to obtain molded articles with higher mechanical strength. Furthermore, the upper limit of the weight-average molecular weight (Mw) is preferably 100000 or less, more preferably 80000 or less, even more preferably 60000 or less, still more preferably 50000 or less, and still more preferably 35000 or less. By setting it to the upper limit or below, there is a tendency to further improve the flowability of the resin composition.

[0175] The free bromine content of the brominated polycarbonate is preferably 0.05% by mass or more, and more preferably 0.20% by mass or less. By setting it within this range, there is a tendency to further improve the heat resistance stability of the resin composition. Furthermore, the chlorine atom content of the brominated polycarbonate is preferably 0.001% by mass or more, and more preferably 0.20% by mass or less. By setting it within this range, there is a tendency to further improve the resistance to mold corrosion during molding.

[0176] As a brominated polycarbonate, brominated polycarbonates obtained from bromobisphenol A, particularly tetrabromobisphenol A, are preferred. Examples of its terminal structures include phenyl, 4-tert-butylphenyl, and 2,4,6-tribromophenyl, with a 2,4,6-tribromophenyl terminal structure being particularly preferred.

[0177] The average number of carbonate structural units in the brominated polycarbonate can be appropriately selected and determined, preferably 2 to 30, more preferably 3 to 15, and even more preferably 3 to 10.

[0178] The molecular weight of brominated polycarbonate is arbitrary and can be determined by appropriate selection. Preferably, the viscosity-average molecular weight is 1,000 to 20,000, and more preferably 2,000 to 10,000.

[0179] The brominated polycarbonate obtained from the above-mentioned bromobisphenol A can be obtained, for example, by a conventional method of reacting bromobisphenol with phosgene. Aromatic monohydroxy compounds, which can be substituted with halogen or organic groups, can be listed as end-capping agents.

[0180] Specifically, bisphenol A-type brominated epoxy compounds, such as tetrabromobisphenol A epoxy compounds and glycidyl brominated bisphenol A epoxy compounds, are preferred examples of brominated epoxy compounds.

[0181] The molecular weight of the brominated epoxy compound is arbitrary and can be appropriately selected. Preferred by weight-average molecular weight (Mw), it is 3000 or more, more preferably 10000 or more, further preferably 13000 or more, even more preferably 15000 or more, and still more preferably 18000 or more. By setting it to the lower limit or above, there is a tendency to obtain molded articles with higher mechanical strength. Furthermore, the upper limit of the weight-average molecular weight (Mw) is preferably 100000 or less, more preferably 80000 or less, even more preferably 78000 or less, still more preferably 75000 or less, even more preferably 70000 or less, and further preferably 50000 or less, 30000 or less, or 25000 or less. By setting it to the upper limit or below, there is a tendency to further improve the flowability of the resin composition.

[0182] The epoxy equivalent of the brominated epoxy compound is preferably 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.

[0183] Furthermore, brominated epoxy oligomers can also be used in conjunction with the brominated epoxy compound. In this case, for example, by using an oligomer with a Mw of 5000 or less at a proportion of about 50% by mass or less, the flame retardancy, mold release properties, and flowability can be appropriately adjusted. The bromine atom content in the brominated epoxy compound is arbitrary, but from the perspective of imparting sufficient flame retardancy, it is typically 10% by mass or more, preferably 20% by mass or more, particularly preferably 30% by mass or more, and preferably up to 60% by mass, with a preferred maximum of 55% by mass or less.

[0184] As brominated polystyrene, brominated polystyrene containing the structural unit represented by formula (3) is preferably listed.

[0185] [Chemical Formula 5]

[0186]

[0187] (In equation (3), t is an integer from 1 to 5, and n is the number of structural units.)

[0188] As brominated polystyrene, it can be any product manufactured by brominating polystyrene or by polymerizing brominated polystyrene monomers. Substances obtained by polymerizing brominated polystyrene are preferred because they contain less free bromine (atoms). It should be noted that in formula (3), the CH group bonded to bromobenzene can be replaced by a methyl group. Furthermore, brominated polystyrene can be a copolymer formed by copolymerizing other vinyl monomers. Examples of vinyl monomers in this case include styrene, α-methylstyrene, (meth)acrylonitrile, (meth)acrylate, butadiene, and vinyl acetate. In addition, brominated polystyrene can be used as a single substance or as a mixture of two or more substances with different structures, and it can also contain units derived from styrene monomers with different numbers of bromine atoms in a single molecular chain.

[0189] 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), poly(4-bromo-α-methylstyrene), poly(2,4-dibromo-α-methylstyrene), poly(2,5-dibromo-α-methylstyrene), poly(2,4,6-tribromo-α-methylstyrene), and poly(2,4,5-tribromo-α-methylstyrene), etc. Poly(2,4,6-tribromostyrene), poly(2,4,5-tribromostyrene), and poly(2,4,6-tribromo-α-methylstyrene) containing an average of 2 to 3 bromine groups in the benzene ring are particularly preferred.

[0190] In brominated polystyrene, the number of structural units n (average degree of polymerization) in formula (3) is preferably 30 to 1500, more preferably 150 to 1000, and particularly preferably 300 to 800. When the average degree of polymerization is less than 30, blooming is likely to occur. On the other hand, when the average degree of polymerization exceeds 1500, poor dispersion is likely to occur, and mechanical properties are likely to decrease. Furthermore, the weight-average molecular weight (Mw) of brominated polystyrene is preferably 5000 to 500000, more preferably 10000 to 500000, further preferably 10000 to 300000, even more preferably 10000 to 100000, and even more preferably 10000 to 70000. In particular, in the case of the brominated polystyrene described above, the weight-average molecular weight (Mw) is preferably 50000 to 70000, and in the case of brominated polystyrene based on polymerization, the weight-average molecular weight (Mw) is preferably around 10000 to 30000.

[0191] The bromine concentration (Br content in the examples described later) 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 above, there is a tendency to effectively improve the flame retardancy of the molded article. 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 also be 65% by mass or less.

[0192] When using phosphonic acid metal salts as flame retardants, there is no particular limitation on the type of phosphonic acid metal salt. Preferably, the anionic portion of the phosphonic acid metal salt is represented by formula (4) or formula (5), and the metal ion of the cationic portion is any one of calcium, magnesium, aluminum or zinc.

[0193] [Chemical Formula 6]

[0194]

[0195] (where R) 1 and R 2 Each independently represents an alkyl group having 1 to 6 carbon atoms or an aryl group optionally having substituents, R 1 They can be the same or different, R 3 R represents an alkylene group having 2 to 10 carbon atoms, an arylene group optionally having substituents, or a combination thereof. 3 They can be the same or different, where n represents an integer from 0 to 2.

[0196] The aryl group optionally having a substituent is preferably a phenyl group optionally having a substituent. When substituents are present, alkyl groups having 1 to 3 carbon atoms are preferred. Furthermore, unsubstituted groups are preferred.

[0197] The optionally substituted arylene is preferably an optionally substituted phenylene. The optionally substituted arylene is preferably unsubstituted or an alkyl group (preferably methyl) having 1 to 3 carbon atoms as a substituent.

[0198] In this embodiment, a metal salt of hypophosphonic acid represented by formula (5) is preferred. Furthermore, in this embodiment, aluminum hypophosphonate is preferred.

[0199] Specific examples of metal salts of phosphinic acid include: calcium dimethylphosphinic acid, magnesium dimethylphosphinic acid, aluminum dimethylphosphinic acid, zinc dimethylphosphinic acid, calcium ethylmethylphosphinic acid, magnesium ethylmethylphosphinic acid, aluminum ethylmethylphosphinic acid, zinc ethylmethylphosphinic acid, calcium diethylphosphinic acid, magnesium diethylphosphinic acid, aluminum diethylphosphinic acid, zinc diethylphosphinic acid, calcium methyl-n-propylphosphinic acid, magnesium methyl-n-propylphosphinic acid, aluminum methyl-n-propylphosphinic acid, zinc methyl-n-propylphosphinic acid, and methanedi(methylphosphinic acid). Calcium, magnesium methane bis(methylphosphine), aluminum methane bis(methylphosphine), zinc methane bis(methylphosphine), calcium benzene-1,4-bis(methylphosphine), magnesium benzene-1,4-bis(methylphosphine), aluminum benzene-1,4-bis(methylphosphine), zinc benzene-1,4-bis(methylphosphine), calcium methylphenylphosphine, magnesium methylphenylphosphine, aluminum methylphenylphosphine, zinc methylphenylphosphine, calcium diphenylphosphine, magnesium diphenylphosphine, aluminum diphenylphosphine, zinc diphenylphosphine.

[0200] For details on phosphonates, please refer to paragraphs 0052 to 0058 of International Publication No. 2010 / 010669, which are incorporated herein by reference.

[0201] Regarding the content of the flame retardant (preferably a brominated flame retardant) in the resin composition of this embodiment, relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the lower limit is 5 parts by weight or more, preferably 7 parts by weight or more, more preferably 8 parts by weight or more, further preferably 10 parts by weight or more, even more preferably 11 parts by weight or more, even more preferably 13 parts by weight or more, even more preferably 14 parts by weight or more, and particularly more preferably 15 parts by weight or more. By setting it to the lower limit or above, there is a tendency to further improve the flame retardancy of the obtained molded article. Relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the upper limit of the content of the flame retardant is 50 parts by weight or less, preferably 45 parts by weight or less, more preferably 40 parts by weight or less, even more preferably 35 parts by weight or less, even more preferably 30 parts by weight or less, even more preferably 25 parts by weight or less, even more preferably 20 parts by weight or less, and particularly more preferably 15 parts by weight or less. By setting it below the aforementioned upper limit value, the reduction in the mechanical strength of the resulting molded article can be more effectively suppressed.

[0202] 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, the total amount is preferably within the range described above.

[0203] <Elastomers>

[0204] The resin composition of this embodiment preferably includes an elastomer. By including an elastomer, there is a tendency for the impact resistance of the resulting molded article to be further improved.

[0205] There are no particular restrictions on the type of elastomer, and any known elastomer can be used.

[0206] An example of an elastomer is an elastomer containing epoxy groups. By including elastomers containing epoxy groups, there is a tendency for increased affinity with polybutylene terephthalate resins, and a tendency to obtain molded articles with high impact resistance.

[0207] In a first embodiment of an epoxy-containing elastomer, a copolymer is obtained by copolymerizing an α-olefin, a glycidyl ester of an α,β-unsaturated acid, and an unsaturated monomer capable of copolymerizing with them, as needed. Preferably, 60% by mass or more of the α-olefin and the glycidyl ester of the α,β-unsaturated acid are used in the total copolymer components of the copolymer.

[0208] Examples of α-olefins include ethylene, propylene, 1-butene, and 1-pentene. Two or more of these may be used. Examples of glycidyl esters of α,β-unsaturated acids include glycidyl acrylate, glycidyl methacrylate, glycidyl ethyl acrylate, and glycidyl itaconic acid. Two or more of these may be used. Examples of vinyl monomers capable of copolymerizing with the above components include vinyl ethers, vinyl acetate, vinyl propionate, methyl, ethyl, propyl, butyl, acrylic acid, and methacrylates, acrylonitrile, and styrene. Two or more of these may be used.

[0209] Preferred examples of epoxy-containing elastomers according to the first embodiment include ethylene / glycidyl methacrylate copolymers, ethylene / glycidyl methacrylate / vinyl acetate copolymers, ethylene / glycidyl methacrylate / alkyl acrylate copolymers, and ethylene / alkyl acrylate / vinyl acetate copolymers. Particularly from the viewpoint of excellent toughness and further improved resistance to damp heat and impact of molded articles, ethylene / glycidyl methacrylate / alkyl acrylate (preferably butyl acrylate) copolymers are preferred. Specific examples of epoxy-containing elastomers according to the first embodiment are available under trade names such as "Lotader" (registered trademark) AX8900 and AX8700 manufactured by Arkema.

[0210] A second embodiment of the epoxy-containing elastomer is a core-shell elastomer. By using a core-shell elastomer, the molecular particle size is small, making it easy to disperse in polybutylene terephthalate resin, and there is a tendency for improved weld strength through the reaction of reactive groups. Examples of core-shell elastomers include substances formed by grafting comonomer components onto the polymer core.

[0211] The core is preferably a rubber-based polymer, and examples include acrylonitrile / acrylic rubber-based polymer / styrene graft copolymer (ASA resin), methyl methacrylate / acrylic rubber-based polymer / styrene graft copolymer (MSA resin), methyl methacrylate / acrylonitrile / acrylic rubber-based polymer / styrene graft copolymer (MASA resin), rubber-based polymers containing polyorganosiloxanes, etc., with rubber-based polymers containing polyorganosiloxanes being more preferred.

[0212] The glass transition temperature of rubber polymers containing polyorganosiloxanes is typically below 0°C, preferably below -20°C, and more preferably below -30°C. As specific examples of rubber components, there are no particular limitations as long as the rubber contains polyorganosiloxanes; examples include polyorganosiloxane rubbers, and (IPN type) composite rubbers of polyorganosiloxane rubbers and polyalkyl acrylate rubbers.

[0213] Specific examples of monomeric components capable of nucleograft copolymerization include aromatic vinyl compounds, cyanide vinyl compounds, (meth)acrylate compounds, (meth)acrylic acid compounds, glycidyl (meth)acrylate and other epoxy-containing (meth)acrylate compounds, maleimide compounds such as maleimide, N-methylmaleimide, N-phenylmaleimide, etc.; α,β-unsaturated carboxylic acid compounds such as maleic acid, phthalic acid, itaconic acid, etc., and their anhydrides (e.g. maleic anhydride, etc.).

[0214] Specific examples of rubbery polymers, aromatic vinyl compounds, cyanide vinyl compounds, and (meth)acrylate compounds can be found in paragraphs 0042 to 0046 of Japanese Patent Application Publication No. 2019-059813, which are incorporated herein by reference.

[0215] The epoxy-containing elastomer of the second embodiment is preferably a compound formed by grafting an epoxy-containing (meth)acrylate compound onto a rubbery polymer containing a polyorganosiloxane (preferably a composite rubber of polyorganosiloxane rubber and polyalkyl acrylate rubber).

[0216] Specific examples of epoxy-containing elastomers in the second embodiment include, for example, “METABLEN (registered trademark, hereinafter the same) S-2002” and “METABLEN S-2200” manufactured by Mitsubishi Rayon.

[0217] Other examples of elastomers include graft copolymers, which are formed by graft copolymerizing a rubber component with a monomer component that can copolymerize with it. Graft copolymers can be manufactured using any method, such as bulk polymerization, solution polymerization, suspension polymerization, or emulsion polymerization, and the copolymerization process can be single-stage or multi-stage grafting.

[0218] The glass transition temperature of rubber components is typically below 0°C, preferably below -20°C, and more preferably below -30°C. Specific examples of rubber components include: polybutadiene rubber, polyisoprene rubber, polybutyl acrylate, poly(2-ethylhexyl acrylate), butyl acrylate / 2-ethylhexyl acrylate copolymers, polyalkyl acrylate rubbers, silicone rubbers such as polysiloxane rubbers, butadiene-acrylic acid composite rubbers, IPN (Interpenetrating Polymer Network) type composite rubbers formed from polysiloxane rubbers and polyalkyl acrylate rubbers, styrene-butadiene rubber, ethylene-propylene rubber, ethylene-butene rubber, ethylene-octene rubber, ethylene-α-olefin rubbers, ethylene-acrylic acid rubber, fluororubber, etc. These can be used alone or in mixtures of two or more. Among them, considering mechanical properties and surface appearance, polybutadiene rubber, polyalkyl acrylate rubber, polyorganosiloxane rubber, IPN type composite rubber formed by polyorganosiloxane rubber and polyalkyl acrylate rubber, and styrene-butadiene rubber are preferred.

[0219] As a specific example of a monomer component capable of graft copolymerization with a rubber component, the above-mentioned specific examples of monomer components capable of graft copolymerization with a rubber component are the same as those of an epoxy-containing elastomer.

[0220] From the perspectives of impact resistance and surface appearance, the graft copolymer formed by copolymerizing rubber components is preferably a core / shell type graft copolymer. Particularly preferred are core / shell type graft copolymers consisting of a core layer and a shell layer formed by copolymerizing (meth)acrylate around it. The core layer is at least one rubber component selected from rubbers containing polybutadiene, rubbers containing polybutyl acrylate, polysiloxane rubbers, and IPN-type composite rubbers formed from polysiloxane rubbers and polyalkyl acrylate rubbers. In the above-mentioned core / shell type graft copolymers, it is preferable to contain 40% by mass or more of rubber component, and more preferably 60% by mass or more of rubber component. Furthermore, (meth)acrylate is preferably contained at 10% by mass or more. It should be noted that the core / shell type in this embodiment does not necessarily mean that the core and shell layers can be clearly distinguished; its meaning broadly includes compounds obtained by grafting and polymerizing rubber components around the portion that forms the core.

[0221] Preferred examples of these core / shell 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, and methyl methacrylate-(acrylic / silicone IPN rubber) copolymer. Such rubbery polymers can be used alone or in combination with two or more.

[0222] Examples of such elastomers include: "PARALOID EXL2602", "PARALOID EXL2603", "PARALOID EXL2655", "PARALOID XL2311", "PARALOID EXL2313", "PARALOID EXL2315", "PARALOID KM330", "PARALOID KM336P", and "PARALOID KCZ201" manufactured by Rohm and Haas Japan; "METABLEN C-223A", "METABLEN E-901", "METABLEN S-2001", and "METABLEN SRK-200" manufactured by Mitsubishi Rayon; and "KANE ACE M-511", "KANE ACE M-600", "KANE ACE M-400", "KANE ACE M-580", and "KANE ACE" manufactured by Kaneka. "M-711", "KANE ACE MR-01", "UBESTA XPA" manufactured by Ube Industries, etc.

[0223] Other examples of elastomers include acrylic block copolymers.

[0224] Examples of acrylic block copolymers include block copolymers comprising hard segments composed of methyl methacrylate blocks and soft segments composed of alkyl acrylate blocks.

[0225] The acrylic block copolymer is preferably a triblock copolymer having two hard-chain segments on either side of one soft-chain segment, or a diblock copolymer having one soft-chain segment and one hard-chain segment. That is, the acrylic block copolymer in this embodiment preferably has a triblock structure composed of methyl methacrylate blocks, alkyl acrylate blocks, and methyl methacrylate blocks, or a diblock structure composed of methyl methacrylate blocks and alkyl acrylate blocks.

[0226] Examples of alkyl acrylates constituting the soft segments 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, toluene acrylate, benzyl acrylate, isobornyl acrylate, 2-methoxyethyl acrylate, 3-methoxybutyl acrylate, 2-hydroxyethyl acrylate, 2-hydroxypropyl acrylate, stearyl acrylate, glycidyl acrylate, 2-aminoethyl acrylate, γ-(acryloyl) The following are one or more combinations of the following: (oxypropyl)trimethoxysilane, γ-(acryloyloxypropyl)dimethoxymethylsilane, ethylene oxide adduct of acrylic acid, trifluoromethyl methacrylate, 2-trifluoromethyl ethyl acrylate, 2-perfluoroethyl acrylate, 2-perfluoroethyl-2-perfluorobutyl acrylate, 2-perfluoroethyl acrylate, perfluoromethyl acrylate, diperfluoromethyl acrylate, 2-perfluoromethyl-2-perfluoroethyl acrylate, 2-perfluorohexyl acrylate, 2-perfluorodecyl ethyl acrylate, and 2-perfluorohexadecyl ethyl acrylate, wherein butyl acrylate or butyl acrylate / 2-ethylhexyl acrylate are preferred.

[0227] There are no particular limitations on the acrylic block copolymers as long as they can achieve the effects of the present invention. Among the above, it is preferred to have a diblock structure composed of methyl methacrylate block-butyl acrylate block or methyl methacrylate block-butyl acrylate / 2-ethylhexyl acrylate block, or a triblock structure composed of methyl methacrylate block-butyl acrylate block-methyl methacrylate block or methyl methacrylate block-butyl acrylate / 2-ethylhexyl acrylate block-methyl methacrylate block.

[0228] In acrylic block copolymers, the ratio of hard segments to soft segments is preferably in the range of 3:97 to 40:60 by weight, more preferably 5:95 to 35:65. A higher proportion of soft segments improves the softening of vinyl chloride-based resins; however, a lower proportion of hard segments, as mentioned above, reduces compatibility with vinyl chloride-based resins, thus deteriorating moldability. Conversely, a lower proportion of soft segments reduces the efficiency of softening vinyl chloride-based resins.

[0229] Examples of commercially available acrylic block copolymers include LA1892, LA4285, LA2270, LA2250, LA2140, LA2330, and LA3320 from the Clarity (registered trademark) LA series manufactured by Kuraray, and M51, M52, and M22 from the Nanostrength (registered trademark) series manufactured by Arkema. Furthermore, acrylic copolymers that use butyl acrylate / 2-ethylhexyl acrylate in the soft segment are commercially available as LK9243 and KL-LK9333 from the Clarity (registered trademark) LK series manufactured by Kuraray, which are examples of acrylic block copolymers that use butyl acrylate / 2-ethylhexyl acrylate in the soft segment.

[0230] The melt mass flow rate (MFR) of the elastomer used in this embodiment, as measured according to ISO 1133 at 190°C and a load of 2.16 kgf, is preferably 1 g / 10 min or more, more preferably 2 g / 10 min or more, and even more preferably 15 g / 10 min or less, and more preferably 10 g / 10 min or less.

[0231] In the case where the resin composition of this embodiment contains two or more elastomers, the MFR of the elastomers is a weighted average.

[0232] In addition to the above, other elastic materials may also be used, such as those described in paragraphs 0075 to 0088 of Japanese Patent Application Publication No. 2012-251061, paragraphs 0101 to 0107 of Japanese Patent Application Publication No. 2012-177047, paragraphs 0076 to 0087 of Japanese Patent Application Publication No. 2016-98242, and paragraphs 0080 to 0087 of Japanese Patent Application Publication No. 2019-11514. These contents are incorporated in this specification.

[0233] In this embodiment, it is preferable to use an epoxy-containing elastomer (preferably the epoxy-containing elastomer of the first embodiment described above) in combination with an acrylic block copolymer. By using them in combination, there is a tendency to achieve a good balance between improved flowability and impact resistance.

[0234] When the resin composition of this embodiment includes an elastomer, its content is preferably 1 part by mass or more, more preferably 3 parts by mass or more, further 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, even more preferably 9 parts by mass or more, and 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 also be 12 parts by mass or less, or 10 parts by mass or less. By setting it to the lower limit or above, there is a tendency for further improvement in impact resistance. By setting it to the upper limit or below, there is a tendency for improved flowability, and there is a tendency for it to easily exhibit high flame retardancy.

[0235] The resin composition of this embodiment may contain only one elastomer or may contain two or more elastomers. When two or more elastomers are contained, it is preferable that the total amount is within the range described above.

[0236] Flame retardant additives

[0237] The resin composition of this embodiment may contain a flame retardant additive. By including a flame retardant additive, the flame retardancy of the molded article can be further improved. Flame retardant additives are particularly preferred when halogen-based flame retardants are included. Examples of flame retardant additives used in this embodiment include antimony compounds, such as antimony trioxide (Sb₂O₃), antimony tetroxide (Sb₂O₄), antimony pentoxide (Sb₂O₅), and sodium antimonate. Especially from the perspective of impact resistance, antimony oxide is preferred, and antimony trioxide is particularly preferred.

[0238] When combined with flame retardant additives, it can be formulated in the form of masterbatch. The content of antimony compound in the masterbatch is preferably 30-90% by mass, more preferably 40-85% by mass, even more preferably 50-85% by mass, even more preferably 60-85% by mass, and even more preferably 70-85% by mass. The resin used in the masterbatch is preferably polyester resin, more preferably polybutylene terephthalate resin.

[0239] When the resin composition of this embodiment contains a flame retardant additive (e.g., an antimony compound), its content is preferably 0.1 parts by mass or more, more preferably 1 part by mass or more, further 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 total polyalkylene terephthalate resin and polycarbonate resin. By setting it to the lower limit or above, there is a tendency to more effectively exert flame retardancy. Furthermore, the upper limit of the antimony compound content relative to 100 parts by mass of the total polyalkylene terephthalate resin and polycarbonate resin 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. By setting it to the upper limit or below, there is a tendency to improve the moldability and impact resistance of the resulting molded article.

[0240] The resin composition of this embodiment may contain only one flame retardant additive, or it may contain two or more. When two or more are contained, the total amount is preferably within the range described above.

[0241] Anti-dripping agent

[0242] The resin composition of this embodiment may also contain an anti-dripping agent. Polytetrafluoroethylene (PTFE) is preferred as the anti-dripping agent, and substances that have fibrillation-forming ability, are easily dispersed in the resin composition, and tend to form a fibrous network structure in the resin are also preferred. Suspension polymers can be cited as examples of PTFEs in the resin composition of this embodiment that have fibrillation-forming ability. Furthermore, from the viewpoint of reducing environmental impact, perfluorooctanoic acid (PFOA) reduced products or PFOA-free products are preferred as PTFEs.

[0243] Preferably, the anti-dripping agent content is 0.1 to 20 parts by weight, more preferably 0.2 parts by weight or more, further preferably 0.3 parts by weight or more, even more preferably 0.4 parts by weight or more, more preferably 10 parts by weight or less, further preferably 5 parts by weight or less, and even more preferably 1 part by weight or less. By setting the content to the lower limit or above, there is a tendency to suppress dripping during combustion, a tendency to improve impact resistance, and a tendency to achieve a more complete flame retardant effect. Furthermore, by setting the content to the upper limit or below, there is a tendency to improve the appearance of the molded article and a tendency to improve flowability. More preferably, the anti-dripping agent content is 0.5 to 10 parts by weight, relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin.

[0244] The resin composition of this embodiment may contain only one anti-dripping agent, or it may contain two or more. When two or more are contained, the total amount is preferably within the range described above.

[0245] <Transesterification Inhibitor>

[0246] The resin composition of this embodiment may contain an exchange inhibitor. By including an exchange inhibitor, a resin composition and even a molded article with excellent thermal stability can be obtained.

[0247] As an example of an transesterification inhibitor, phosphates and / or phosphoric acid are preferred. Examples of phosphates include zinc phosphate, phosphates of Group 1 or Group 2 metals, and metal salts of organophosphates. Examples of phosphoric acid include organophosphates, which are preferred because they tend to reduce the amount of gas generated, improve the appearance of the molded article, increase the crystallization temperature, and improve mold release properties.

[0248] In this embodiment, the phosphate preferably comprises at least one of the compounds represented by formula (P1) and the compounds represented by formula (P2).

[0249]

[0250] (In equations (P1) and (P2), R) x Each can independently represent a straight-chain or branched alkyl group having 3 to 30 carbon atoms.

[0251] R x The number of carbon atoms is preferably 8 or more, more preferably 13 or more, even more preferably 15 or more, and preferably 25 or less, more preferably 20 or less, even more preferably 18 or less, and most preferably 18.

[0252] R x It is a straight-chain or branched alkyl group, preferably a straight-chain alkyl group.

[0253] In this embodiment, the phosphate further preferably comprises at least one of the compounds represented by formula (P1-1) and the compounds represented by formula (P2-1). In this embodiment, a mixture of the compounds represented by formula (P1-1) and the compounds represented by formula (P2-1) is more preferred.

[0254]

[0255] Phosphoric acid preferably contains at least one of the compounds represented by formula (P3).

[0256]

[0257] (In formula (P3), R represents a straight-chain or branched alkyl group with 2 to 18 carbon atoms. nx represents 1 or 2.)

[0258] The number of carbon atoms in R is preferably 8 or more, more preferably 13 or more, even more preferably 15 or more, and preferably 25 or less, more preferably 20 or less, even more preferably 18 or less, and most preferably 18.

[0259] R is a straight-chain or branched alkyl group, preferably a straight-chain alkyl group.

[0260] nx is 1 or 2, preferably a mixture of 1 and 2.

[0261] Transesterification inhibitors can be commercially available products, such as those manufactured by ADEKA, AX-71, Jōhoku Chemical Co., Ltd., and JP-518Zn.

[0262] Relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the content of the transesterification inhibitor in the resin composition of this embodiment is preferably 0.01 parts by weight or more, more preferably 0.05 parts by weight or more, even more preferably 0.1 parts by weight or more, and preferably 2 parts by weight or less, more preferably 1.5 parts by weight or less, even more preferably 1 part by weight or less, and even more preferably 0.8 parts by weight or less, or possibly 0.5 parts by weight or less. By setting the content to the lower limit or above, there is a tendency to further improve the inhibition effect of the resin's thermal deterioration and oxidative deterioration during melt mixing, molding, and use in the form of a molded article; there is a tendency to more effectively suppress the discoloration of the resin; there is a tendency to improve flame retardancy; there is a tendency to increase the crystallization temperature; and there is a tendency to improve the appearance of the molded article. By setting the content to the upper limit or below, there is a tendency to effectively suppress the adverse effects on appearance and physical properties caused by the agglomeration of additives such as stabilizers.

[0263] The resin composition of this embodiment may contain only one transesterification inhibitor, or it may contain two or more. When two or more are contained, the total amount is preferably within the range described above.

[0264] <Non-fibrous inorganic fillers>

[0265] The resin composition of this embodiment preferably contains a non-fibrous inorganic filler. By including a non-fibrous inorganic filler, the physical properties, heat resistance, and anisotropy of shrinkage during molding are improved.

[0266] As a non-fibrous inorganic filler, it refers to a filler in a shape other than fiber, preferably a plate-shaped filler or a particle-shaped filler.

[0267] 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 dioxide, zinc oxide, magnesium oxide, calcium titanate, magnesium titanate, barium titanate, etc. Preferred fillers include calcium carbonate, talc, mica, silica, kaolin, barium sulfate, zirconium silicate, and titanium dioxide. More preferred fillers are calcium carbonate, talc, and titanium dioxide. Titanium dioxide tends to improve impact resistance, flame retardancy, and resistance to electrical tracking, and is therefore further preferred.

[0268] Furthermore, the non-fibrous inorganic filler used in this embodiment preferably has undergone surface treatment with acid, siloxane-based compounds, or inorganic compounds. In particular, in the case of titanium oxide, from the viewpoint of thermal stability, it is preferable that the surface has undergone treatment with organosiloxane-based compounds or with inorganic compounds such as alumina or silica.

[0269] Examples of acids used in acid treatment include fatty acids, rosin acids, and lignin acids, with saturated or unsaturated fatty acids having 6 to 20 carbon atoms being 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.

[0270] In this embodiment, the average particle size of the non-fibrous inorganic filler is preferably 5 μm or less, more preferably 3 μm or less, further 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. In this embodiment, the average particle size is obtained by averaging the particle sizes observable in magnified images from a scanning electron microscope. It should be noted that in the case of surface-treated titanium oxide, the primary particle size of the surface-treated titanium oxide is set as the average particle size.

[0271] Relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the content of the non-fibrous inorganic filler is preferably 1 part by weight or more, more preferably 2 parts by weight or more, further preferably 3 parts by weight or more, and particularly preferably 3.5 parts by weight or more. Setting this content above the lower limit tends to improve impact resistance, flame retardancy, and resistance to electrical tracking. Furthermore, relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the upper limit of the content of the non-fibrous inorganic filler is preferably 12 parts by weight or less, more preferably 10 parts by weight or less, further preferably 8 parts by weight or less, even more preferably 6 parts by weight or less, and still more preferably 5 parts by weight or less. Setting this content below the upper limit tends to improve the surface appearance of the molded article.

[0272] The content of the non-fibrous inorganic filler in the resin composition of this embodiment is preferably 0.5% by mass or more, more preferably 1.0% by mass or more, even more preferably 2.0% by mass or more, and still more preferably 2.5% by mass or more. By setting this lower limit or above, there is a tendency for improved impact resistance, improved flame retardancy, and improved resistance to electrical tracking. Furthermore, the content of the non-fibrous inorganic filler in the resin composition of this embodiment is preferably 50% by mass or less, more preferably 40% by mass or less, even more preferably 30% by mass or less, still more preferably 20% by mass or less, even more preferably 10% by mass or less, still more preferably 7% by mass or less, and particularly preferably 5% by mass or less. By setting this upper limit or below, there is a tendency for the surface appearance of the molded article to become better and the flowability to improve.

[0273] The resin composition of this embodiment may contain only one non-fibrous inorganic filler, or it may contain two or more. When two or more fillers are contained, the total amount is preferably within the range described above.

[0274] In particular, by including rutile titanium dioxide with an average particle size of 0.15 to 0.4 μm in 0.5 to 10 parts by weight relative to a total of 100 parts by weight of polyethylene terephthalate resin and polycarbonate resin, it tends to readily and effectively exert high flame retardancy, resistance to electrical tracking, and impact resistance, and is therefore preferred.

[0275] The resin composition of this embodiment may further include a fibrous filler, or it may not include a fibrous filler. Preferably, the resin composition of this embodiment does not substantially contain a fibrous filler. "Substantially does not contain" means that the content of the fibrous filler 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.

[0276] Antioxidants

[0277] The resin composition of this embodiment may contain an antioxidant. By including an antioxidant, a resin composition or molded article with excellent thermal stability can be obtained.

[0278] The antioxidant preferably comprises one or more compounds selected from the group consisting of thioether compounds, hindered phenolic compounds, and phosphite compounds, and more preferably comprises hindered phenolic compounds.

[0279] In this embodiment, it is also preferable to use two or more of the following compounds: thioether compounds, hindered phenolic compounds, and phosphite compounds. By using two or more antioxidants in this way, there is a tendency to further improve thermal stability and thus maintain thermal stability over a long period of time.

[0280] As a thioether compound, any sulfur-containing compound known in the art can be used, with thioethers being preferred. The resin composition of this embodiment, by containing a thioether compound, tends to improve the appearance of the molded article and suppress color variations. Specifically, examples include: didodecyl thiodipropionate, ditetradecyl thiodipropionate, dioctadecyl thiodipropionate, pentaerythritol tetra(3-dodecyl thiopropionate), 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 them, 2,2-bis{[3-(dodecylthio)-1-oxopropoxy]methyl}propane-1,3-dimethylbis[3-(dodecylthio)propionate] is preferred. Commercially available examples include Shipro Kasei Co., Ltd., under the trade name "Cinox412S", and ADEKA Co., Ltd., under the trade name "ADK STAB AO-412S".

[0281] Examples of hindered phenolic compounds include pentaerythritol tetra(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 tetra(3-(3,5-dineopentyl-4-hydroxyphenyl)propionate), and 1,3,5-trimethyl-2,4,6-tris(3,5-di-tert-butyl-4-hydroxybenzyl)benzene. Among these, pentaerythritol tetra(3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate and octadecyl-3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate are preferred. Commercially available examples include those manufactured by ADEKA under the trade names "ADK STAB AO-60" and "ADK STAB AO-330".

[0282] As phosphite compounds, compounds represented by the following formula are preferred:

[0283] R 2 OP (OR) 3 (OR) 4 )

[0284] (where R) 2 R 3 and R 4 They are, respectively, an alkyl group with 1 to 30 carbon atoms or an aryl group with 6 to 30 carbon atoms, R 2 R 3以及 R 4 At least one of them is an aryl group having 6 to 30 carbon atoms.

[0285] Examples of phosphite compounds include: triphenyl phosphite, tris(nonylphenyl) phosphite, dilauryl hydrogen phosphite, triethyl phosphite, tridecyl phosphite, tri(2-ethylhexyl) phosphite, tri(tridecyl) phosphite, tristearate phosphite, diphenylmonodecane phosphite, monophenyldidecyl phosphite, diphenylmonodecane phosphite, tetraphenyldipropylene glycol diphosphite, tetraphenyltetra(tridecyl)pentaerythritol tetraphosphite, hydrogenated bisphenol A phenyl phosphite polymer, diphenyl hydrogen phosphite, 4,4'-butylene-bis(3-methyl-6-tert-butylphenyl di(tridecyl)phosphite, tetra(tridecyl)4, 4'-Isopropylidene diphenyl diphosphite, bis(tetranyl)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'-methylene bis(4,6-di-tert-butylphenyl)octyl phosphite, bis(2,4-dicumylphenyl)pentaerythritol diphosphite, etc. Among these, bis(2,6-di-tert-butyl-4-methylphenyl)pentaerythritol diphosphite is preferred. As a commercially available product, one example is the product manufactured by ADEKA under the brand name "ADK STABPEP-36".

[0286] Furthermore, as an antioxidant, specifically, reference can be made to paragraphs 0067 to 0075 of Japanese Patent Application Publication No. 2021-063196, paragraphs 0046 to 0057 of Japanese Patent Application Publication No. 2018-070722, paragraphs 0030 to 0037 of Japanese Patent Application Publication No. 2019-056035, and paragraphs 0066 to 0078 of International Publication No. 2017 / 038949, all of which are incorporated herein by reference.

[0287] Relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the antioxidant content in the resin composition of this embodiment is 0.01 parts by weight or more, preferably 0.05 parts by weight or more, more preferably 0.1 parts by weight or more, and even more preferably 0.3 parts by weight or more. By setting this lower limit or above, there is a tendency to further improve the inhibition effect on the thermal deterioration and oxidative deterioration of the resin during melt mixing, molding, and use in the form of a molded article, and there is a tendency to more effectively suppress the discoloration of the resin. Furthermore, relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the upper limit of the antioxidant content is preferably 2.0 parts by weight or less, more preferably 1.5 parts by weight or less, and even more preferably 1.0 parts by weight or less. By setting this upper limit or below, the adverse effects on appearance and physical properties such as the aggregation of antioxidants and other additives can be effectively suppressed.

[0288] The resin composition of this embodiment may contain only one antioxidant or two or more. When two or more antioxidants are contained, the total amount is preferably within the range described above.

[0289] <Reinforced Packing>

[0290] The resin composition of this embodiment may include reinforcing fillers. By including reinforcing fillers, the mechanical strength of the resulting molded object can be improved.

[0291] Examples of the shape of the reinforcing filler include flake-shaped, spherical, needle-shaped, and fibrous shapes, with fibrous reinforcing fillers (reinforcing fibers) being preferred. Examples of the composition of the reinforcing filler include glass, metal oxides, metal hydroxides, carbonates, sulfates, etc., with glass being preferred.

[0292] Carbon fiber and glass fiber are preferred as reinforcing fibers, and glass fiber is more preferred.

[0293] Next, the glass fiber preferably used in this embodiment will be described.

[0294] The glass fiber is obtained by melt spinning commonly supplied E glass, C glass, D glass, R glass, A glass, S glass, and alkali-resistant glass. Any glass that can be made into glass fiber can be used; there are no particular limitations. In this embodiment, E glass is preferably included.

[0295] In this embodiment, the glass fiber is preferably surface-treated using known silane coupling agents such as epoxy silane, amino silane, and vinyl silane, or phosphoric acid. The amount of surface treatment agent adhering is preferably 0.01 to 1% by mass of the glass fiber. Furthermore, depending on the requirements, substances surface-treated using fatty acid amide compounds, lubricants such as silicone oil, antistatic agents such as quaternary ammonium salts, resins with film-forming ability such as epoxy resin and polyurethane resin, or mixtures of resins with film-forming ability and heat-resistant oxidation agents may also be used.

[0296] Fiberglass is available in commercially available products. 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 Co., Ltd.; HP3540 manufactured by PPG Industries Co., Ltd.; and CSG3PA820 manufactured by Nittobo Co., Ltd.

[0297] When reinforcing filler (preferably glass fiber) is included, the content of reinforcing filler in the resin composition of this embodiment is preferably 20 parts by mass or more, more preferably 30 parts by mass or more, further preferably 40 parts by mass or more, even more preferably 50 parts by mass or more, and 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 also be 75 parts by mass or less, relative to a total of 100 parts by mass of alkylene terephthalate resin and polycarbonate resin.

[0298] In this embodiment, when the resin composition contains reinforcing filler, the reinforcing filler (preferably glass fiber) preferably accounts for 10 to 45% by mass, more preferably 15 to 40% by mass, and may also be 20 to 35% by mass.

[0299] The resin composition of this embodiment may contain only one reinforcing filler, or it may contain two or more. When two or more fillers are contained, the total amount is preferably within the range described above.

[0300] <Coloring agent>

[0301] The resin composition of this embodiment may contain a colorant. The colorant may be a pigment or a dye; from the viewpoint of flame retardancy, a pigment is preferred, and carbon black is more preferred.

[0302] For details regarding carbon black, please refer to paragraph 0021 of Japanese Patent Application Publication No. 2011-57977, which is incorporated herein by reference.

[0303] Furthermore, when a colorant such as carbon black is incorporated into the resin composition of this embodiment, it is preferable to compound it with a polyalkylene terephthalate resin or the like after the masterbatch is formed. A polyester resin is preferably used in the masterbatch, more preferably a polyalkylene terephthalate resin, even more preferably a polyethylene terephthalate resin and / or a polybutylene terephthalate resin, and even more preferably a polybutylene terephthalate resin. By using polybutylene terephthalate resin, the crystallization of the resin composition is promoted. In particular, when polybutylene terephthalate resin is present in the vicinity of a colorant such as carbon black, the crystallization-promoting effect is more effectively exerted.

[0304] The proportion of colorant in the masterbatch is preferably 5% by mass or more, more preferably 10% by mass or more, and preferably 50% by mass or less, more preferably 40% by mass or less.

[0305] When the resin composition of this embodiment contains a colorant (preferably carbon black), its content is preferably 0.1 parts by mass or more, more preferably 0.2 parts by mass or more, further preferably 0.4 parts by mass or more, even more preferably 0.6 parts by mass or more, and preferably 3 parts by mass or less, more preferably 2 parts by mass or less, and even more preferably 1 part by mass.

[0306] The resin composition of this embodiment may contain only one colorant (preferably carbon black), or it may contain two or more. When two or more colorants are contained, the total amount is preferably within the range described above.

[0307] <UV absorber>

[0308] The resin composition of this embodiment may contain an ultraviolet absorber.

[0309] As ultraviolet absorbers, benzotriazole-based ultraviolet absorbers, benzoxazine-based ultraviolet absorbers, triazine-based ultraviolet absorbers, and malonate-based ultraviolet absorbers are preferred, with benzotriazole-based ultraviolet absorbers being the most preferred. By selecting an organic ultraviolet absorber, the resin composition of this embodiment exhibits good transparency and mechanical properties.

[0310] Examples of 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-pentyl-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)octane, 1,1-bis(3-(2H-5-chlorobenzotriazol-2-yl)-2-hydroxy-5-methylphenyl)octane, 1,2-ethanediylbis(3-(2H-benzotriazol-2-yl)-2-hydroxy-5-methylphenyl)octane, 1,12-dodecadiylbis(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-methylphenylacetate), 3,6-dioxa-1,8-octanediylbis(3-(5-methoxy-2H-benzotriazol-2-yl)-4-hydroxyphenylacetate), 1,6-Hexanediyl bis(3-(3-(2H-benzotriazol-2-yl)-4-hydroxy-5-tert-butylphenyl)propionate, p-xyldiyl bis(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)octyl ester, 2-(2H-benzotriazol-2-yl)-4-hydroxy-5-propyltoluyl)octyl ester, The following are examples of phenolic compounds: 2-(2H-benzotriazol-2-yl)-6-phthalimide methyl-4-methylphenol, 2-(2H-benzotriazol-2-yl)-6-phthalimide ethyl-4-methylphenol, 2-(2H-benzotriazol-2-yl)-6-phthalimide octyl-4-methylphenol, 2-(2H-benzotriazol-2-yl)-6-phthalimide methyl-4-tert-butylphenol, 2-(2H-benzotriazol-2-yl)-6-phthalimide methyl-4-cumylphenol, and 2-(2H-benzotriazol-2-yl)-4,6-bis(phthalimide methyl)phenol. Among these, 2-(2-hydroxy-5-tert-octylphenyl)-2H-benzotriazol is preferred.

[0311] As an ultraviolet absorber, reference can be made to paragraphs 0059 to 0062 of Japanese Patent Application Publication No. 2016-216534 and paragraphs 0069 to 0082 of Japanese Patent Application Publication No. 2018-178019, the contents of which are incorporated herein by reference.

[0312] In the resin composition of this embodiment, the content of the ultraviolet absorber is preferably 0.01 to 1 part by weight relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin. More preferably, the content of the ultraviolet absorber is 0.03 to 0.7 parts by weight, and even more preferably 0.05 to 0.5 parts by weight, relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin. By adding it within this range, the resin composition of this embodiment can be endowed with good weather resistance.

[0313] The ultraviolet absorber may contain only one type or two or more types. When two or more types are included, the total amount is preferably within the range described above.

[0314] <Mold Release Agent>

[0315] The resin composition of this embodiment preferably contains a release agent.

[0316] Release agents can be widely used and are well-known, such as aliphatic carboxylic acid amides, aliphatic carboxylic acids, esters of aliphatic carboxylic acids and alcohols, aliphatic hydrocarbon compounds with a number average molecular weight of 200 to 15,000, and polysiloxane-based silicone oils.

[0317] As aliphatic carboxylic acid amide systems, examples include compounds obtained by the dehydration reaction of higher aliphatic monocarboxylic acids and / or polycarboxylic acids with diamines.

[0318] As higher aliphatic monocarboxylic acids, saturated aliphatic monocarboxylic acids and hydroxycarboxylic acids with 16 or more carbon atoms are preferred, such as palmitic acid, stearic acid, behenic acid, linalic acid, 12-hydroxystearic acid, etc.

[0319] Examples of polycarboxylic 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.

[0320] Examples of diamines include ethylenediamine, 1,3-diaminopropane, 1,4-diaminobutane, hexamethylenediamine, m-phenylenediamine, toluenediamine, p-phenylenediamine, phenylenediamine, isophoronediamine, etc.

[0321] As a carboxylic acid amide compound, a compound obtained by condensation polymerization of stearic acid, sebacic acid, and ethylenediamine is preferred, and a compound obtained by condensation polymerization of 2 moles of stearic acid, 1 mole of sebacic acid, and 2 moles of ethylenediamine is more preferred. In addition to diamide compounds obtained by reacting diamines with aliphatic carboxylic acids, such as N,N'-methylenebis-stearamide and N,N'-ethylenebis-stearamide, dicarboxylic acid amide compounds such as N,N'-bisoctadecylterephthalamide may also be used appropriately.

[0322] Examples of aliphatic carboxylic acids include, for example, 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 with 6 to 36 carbon atoms, and more preferably, saturated aliphatic mono-carboxylic acids with 6 to 36 carbon atoms. Specific examples of such aliphatic carboxylic acids include: palmitic acid, stearic acid, hexanoic acid, decanoic acid, lauric acid, arachidic acid, benzanoic acid, tetracosanoic acid, ceric acid, beeswax acid, tritetracosanoic acid, linaloic acid, adipic acid, azelaic acid, etc.

[0323] The aliphatic carboxylic acid in the ester of an aliphatic carboxylic acid and an alcohol can be, for example, the same aliphatic carboxylic acid as the aliphatic carboxylic acid. On the other hand, the alcohol can be, for example, a saturated or unsaturated monohydric or polyhydric alcohol. These alcohols may have substituents such as fluorine atoms or aryl groups. Among these, monohydric or polyhydric saturated alcohols with 30 or fewer carbon atoms are preferred, and aliphatic or alicyclic saturated monohydric alcohols or aliphatic saturated polyhydric alcohols with 30 or fewer carbon atoms are more preferred.

[0324] Specific examples of this alcohol include: octanol, decanol, dodecylol, stearyl alcohol, behenol, ethylene glycol, diethylene glycol, glycerol, pentaerythritol, 2,2-dihydroxyperfluoropropanol, neopentyl glycol, bis(trimethylolpropane), dipentaerythritol, etc.

[0325] Specific examples of esters of aliphatic carboxylic acids and alcohols include: beeswax (a mixture with myristyl palmitate as the main component), stearate, behenate, stearate, glyceryl monopalmitate, glyceryl monostearate, glyceryl distearate, glyceryl tristearate, pentaerythritol monopalmitate, pentaerythritol monostearate, pentaerythritol distearate, pentaerythritol tristearate, pentaerythritol tetrastearate, esters of lignite acid and polyfunctional alcohols, etc.

[0326] Examples of aliphatic hydrocarbons with 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 with 3 to 12 carbon atoms. It should be noted that aliphatic hydrocarbons here also include alicyclic hydrocarbons. Furthermore, the number average molecular weight of aliphatic hydrocarbons is preferably 5,000 or less.

[0327] Examples of polyolefin waxes include polyethylene wax, polypropylene wax, and polyethylene propylene wax, with polyethylene wax being preferred.

[0328] Polyolefin waxes can be unmodified or modified. Examples of modified polyolefin waxes include vinyl ester modified polyolefin waxes, acid-modified polyolefin waxes, and oxidized polyolefin waxes, with oxidized polyolefin waxes being preferred. Oxidized polyolefin waxes exhibit excellent compatibility with polyalkylene terephthalate resins and tend to effectively suppress mold fouling in the resulting resin compositions.

[0329] Oxidized polyolefin waxes can be obtained by oxidizing the corresponding unmodified polyolefin wax. Examples of oxidized polyethylene waxes include Clariant Chemicals' Licowax (registered trademark) PED521, Licowax PED522, and Licowax PED121; and Ceridust (registered trademark) 3715.

[0330] In addition to the above, the description of Japanese Patent Application Publication No. 2022-140470, paragraph 0028, which is incorporated herein by reference, can also be used for commercially available polyolefin waxes.

[0331] The weight-average molecular weight of the polyolefin wax is preferably 800 or more, more preferably 1000 or more, further preferably 1500 or more, even more preferably 2000 or more, and still more preferably 2500 or more. Setting it to the lower limit or above tends to further shorten the ignition time. 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 still more preferably 10,000 or less. Setting it to the upper limit or below tends to further improve the fluidity of the resin composition during molding.

[0332] The weight-average molecular weight was determined using a Tosoh HLC-8320 GPC EcoSEC with tetrahydrofuran as solvent and Shodex KF-G, three KF-805L, and KF-800D columns at a column temperature of 40°C and a flow rate of 1.2 mL / min via GPC (gel permeation chromatography). The result was presented as a polystyrene equivalent value detected at a detector (UV-8320) and a detection wavelength of 254 nm.

[0333] In this embodiment, when the resin composition contains two or more polyolefin waxes, the weight-average molecular weight of the mixture is taken as the weight-average molecular weight.

[0334] The dropping point of the polyolefin wax is preferably below 165°C, more preferably below 160°C, further preferably below 155°C, even more preferably below 150°C, even more preferably below 145°C, even more preferably below 140°C, even more preferably below 135°C, particularly preferably below 130°C, and preferably above 80°C, more preferably above 85°C, even more preferably above 85°C, even more preferably above 90°C, and even more preferably above 95°C.

[0335] Dropping point is the temperature at which the first drop of molten polyolefin wax, heated from a solid to a liquid, falls from a standard cup with a 2.8 mm opening.

[0336] In addition to the above, as a release agent, reference may also be made to paragraphs 0063 to 0077 of Japanese Patent Application Publication No. 2018-070722 and paragraphs 0090 to 0098 of Japanese Patent Application Publication No. 2019-123809, the contents of which are incorporated herein by reference.

[0337] In the resin composition of this embodiment, relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, it is preferable to contain 0.01 parts by weight or more of a release agent, more preferably 0.1 parts by weight or more of a release agent, even more preferably 0.3 parts by weight or more of a release agent, and even more preferably 0.5 parts by weight or more of a release agent. Depending on the application, it may contain 0.8 parts by weight or more of a release agent, or 1.0 parts by weight or more of a release agent. Furthermore, it is preferably 5 parts by weight or less, more preferably 4 parts by weight or less, even more preferably 3 parts by weight or less, and even more preferably 2 parts by weight or less. Depending on the application, it may also contain 1 part by weight or less. By setting the value to the lower limit or above, there is a tendency to further improve the release properties of the obtained molded article. Furthermore, by setting the value to the upper limit or below, exudation of the obtained molded article can be effectively suppressed.

[0338] The resin composition may contain only one type of release agent, or it may contain two or more types. When two or more types are contained, the total amount is preferably within the range described above.

[0339] <Nucleating Agent>

[0340] The resin composition of this embodiment may contain a nucleating agent. By containing a nucleating agent, the crystallization of the resin composition is promoted.

[0341] The type of nucleating agent is not particularly limited; it can be an inorganic nucleating agent or an organic nucleating agent, with organic nucleating agents being more preferred. By using organic nucleating agents, the amount of compounding can be reduced, and the mechanical strength and shrinkage rate of the obtained molded product can be further improved.

[0342] 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. Furthermore, talc tends to improve the rigidity of the resin composition and improve its moldability, and is therefore more preferred.

[0343] As an organic nucleating agent, an organoalkali metal salt is preferred, an organocarboxylic acid alkali metal salt is more preferred, and an alkali metal salt (preferably a sodium or potassium salt, more preferably a sodium salt) of a fatty acid (preferably a fatty acid with 5 to 50 carbon atoms) is even more preferred. Specific examples of organic nucleating agents include ionomers, sodium benzoate, sodium palmitate, sodium stearate, sodium behenate, and sodium lignite, among which sodium stearate, sodium behenate, and sodium lignite are more preferred, and sodium lignite is even more preferred. By using an organoalkali metal salt, the effect as a crystallization nucleating agent is improved, the crystallinity of the resin composition is increased, and therefore the molded article formed from the resin composition tends to have a balanced improvement in the various properties shown in the following examples, and is therefore further preferred.

[0344] Relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the content of the nucleating agent (preferably talc) in the resin composition of this embodiment is preferably 0.1 parts by weight or more, more preferably 0.2 parts by weight or more, even more preferably 0.5 parts by weight or more, even more preferably 1.0 parts by weight or more, and even more preferably 1.5 parts by weight or more. By setting the content of the nucleating agent to the aforementioned lower limit or above, there is a tendency to improve the moldability and mechanical strength of the molded article. In particular, by including preferably 1.6 parts by weight or more, more preferably 1.8 parts by weight or more, of the nucleating agent (preferably talc) relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the flame retardancy of the resin composition can be further improved. Furthermore, relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, the upper limit of the content of the nucleating agent is 10 parts by weight or less, preferably 8 parts by weight or less, more preferably 5 parts by weight or less, and even more preferably 3 parts by weight or less. By setting the value below the upper limit, resin decomposition is suppressed, thereby tending to improve the mechanical strength, especially the impact resistance, of the molded article.

[0345] The resin composition of this embodiment may contain only one nucleating agent or two or more. When two or more nucleating agents are contained, the total amount is preferably within the range described above.

[0346] <Other Ingredients>

[0347] The resin composition of this embodiment may contain other components besides those described above, provided that it does not significantly impair the desired physical properties. Examples of other components include thermoplastic resins other than polyarylene terephthalate resins and polycarbonate resins, and various resin additives. It should be noted that other components may be one or more in any combination and ratio.

[0348] Specifically, examples include reactive compounds (such as epoxy compounds), antistatic agents, antifogging agents, antiblocking agents, flow improvers, plasticizers, dispersants, and antibacterial agents.

[0349] Furthermore, without departing from the spirit of the invention, additives described in paragraphs 0047 to 0103 of International Publication No. 2021 / 241471 may be incorporated into the resin composition of this embodiment, the contents of which are incorporated herein by reference.

[0350] In the resin composition of this embodiment, the total amount of polyalkylene terephthalate resin, polycarbonate resin, elastomer, flame retardant, and other components to be added as needed is 100 by mass.

[0351] In one embodiment of the present invention, the total amount of the polyalkylene terephthalate resin, polycarbonate resin, elastomer, and flame retardant in the resin composition preferably accounts for 85% or more by mass, more preferably 90% or more by mass, further preferably 93% or more by mass, and even more preferably 95% or more by mass.

[0352] In another embodiment of the present invention, in the resin composition of this embodiment, the total amount of polyalkylene terephthalate resin, polycarbonate resin, elastomer, flame retardant, and glass fiber as required preferably accounts for 85% or more by mass of the resin composition, more preferably 90% or more by mass, further preferably 93% or more by mass, and even more preferably 95% or more by mass.

[0353] Furthermore, in one embodiment of the present invention, the total amount of the polyalkylene terephthalate resin, polycarbonate resin, elastomer, flame retardant, flame retardant additive, anti-dripping agent, transesterification inhibitor, non-fibrous inorganic filler, antioxidant, ultraviolet absorber, and release agent, and glass fiber as required, in the resin composition preferably accounts for 90% or more by mass, more preferably 95% or more by mass, further preferably 97% or more by mass, and even more preferably 99% or more by mass.

[0354] <Physical Properties of Resin Compositions>

[0355] The resin composition of this embodiment preferably has a high content of recycled material (recycling ratio (mass%)).

[0356] Specifically, the content of recycled material in the resin composition is preferably 10% by mass or more, more preferably 20% by mass or more, further preferably 30% by mass or more, and even more preferably 35% by mass or more. The upper limit of recycled material can be 100% by mass, but in practice it is 50% by mass or less.

[0357] Furthermore, in this embodiment, 40-60% by mass of the resin component may be recycled.

[0358] The recycled product contained in the resin composition of this embodiment is preferably a post-consumer recycled (PCR) product.

[0359] The resin composition of this embodiment preferably has a high nominal strain at break.

[0360] Specifically, the resin composition is injection molded into a multi-purpose test piece A1 according to JIS K7139. The nominal strain at break, measured according to JIS K7161-1, is preferably 50% or more, more preferably 74% or more, further preferably 80% or more, and even more preferably 90% or more. There is no particular upper limit to the nominal strain at break; for example, even 130% or less is sufficient to meet the required performance.

[0361] The high nominal fracture strain can be achieved, for example, by using recycled polycarbonate resin derived from bottles or sheets with a relatively low tendency for foreign matter, using polycarbonate resin with low MVR, using polyalkylene terephthalate resin with high intrinsic viscosity, and coordinating elastomers.

[0362] The resin composition of this embodiment preferably has a high Tc (crystallization temperature). A high Tc tends to result in molded articles with excellent mold release properties. Furthermore, a resin composition with excellent moldability can be obtained.

[0363] When the Tc of the resin composition of this embodiment is measured according to JIS K7121, the value of the first cycle is preferably 180°C or higher, more preferably 182°C or higher, even more preferably 184°C or higher, and even more preferably 185°C or higher. Furthermore, as an upper limit, it is preferably 200°C or lower.

[0364] When the Tc of the resin composition of this embodiment is measured according to JIS K7121, the value in the second cycle is preferably 143°C or higher, more preferably 150°C or higher, even more preferably 154°C or higher, and even more preferably 157°C or higher. Furthermore, as an upper limit, it is preferably 190°C or lower.

[0365] The high crystallization temperature can be achieved, for example, by including an ester exchange inhibitor in the resin composition, setting the amount of branched chain in the recycled polycarbonate below the upper limit, and avoiding excessive high temperature and retention during the manufacture of the resin composition.

[0366] The resin composition of this embodiment preferably has excellent impact resistance.

[0367] Specifically, the resin composition of this embodiment is injection molded into a multi-purpose test piece A1 according to JIS K7139, and the unnotched Charpy impact strength (unit: kJ / m) is measured at 23°C according to JIS K7111-1. 2 The preferred value is 21 kJ / m 2 The above, more preferably 25 kJ / m 2 The above is further optimized to 30 kJ / m 2 The above is further optimized to 35 kJ / m 2 The above is further optimized to 40 kJ / m2 The above is further optimized to 45 kJ / m 2 The above, and particularly preferred, is 50 kJ / m 2 The above, and even more specifically preferred, is 55 kJ / m 2 The above. The upper limit of the unnotched Charpy impact strength is, for example, 80 kJ / m. 2 the following.

[0368] The impact resistance can be achieved, for example, by increasing the proportion of polycarbonate resin in the resin composition, using recycled polycarbonate resin with low MVR, incorporating elastomers, or incorporating titanium dioxide. In particular, the resin composition of this embodiment, despite containing a flame retardant, is highly valuable in achieving excellent impact resistance.

[0369] The resin composition of this embodiment preferably has excellent flame retardancy.

[0370] Specifically, the resin composition is preferably molded into a test piece with a thickness of 0.74 mm or 1.0 mm for UL-94 testing, and the flame retardancy meets V-0 requirements according to the UL-94 test.

[0371] Furthermore, the resin composition is molded into test pieces with a thickness of 0.74 mm or 1.0 mm for UL-94 testing. The total burning time according to the UL-94 test is preferably less than 50 seconds, more preferably less than 45 seconds, further preferably less than 40 seconds, even more preferably less than 35 seconds, even more preferably less than 30 seconds, even more preferably less than 25 seconds, even more preferably less than 20 seconds, and particularly preferably less than 18 seconds. Ideally, the lower limit of the total burning time is 0 seconds, but in practice it is more than 1 second.

[0372] The flame retardancy can be achieved, for example, by combining it with flame retardants, flame retardant additives, anti-dripping agents, etc., or by combining it with titanium dioxide.

[0373] The resin composition of this embodiment preferably has excellent heat resistance.

[0374] Specifically, when the resin composition is molded into an ISO tensile test piece (4 mm thick), the load flexural temperature (DTUL) under 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 still more preferably 188°C or higher. There is no particular limitation on the upper limit of the load flexural temperature, but even 220°C or lower is sufficient to meet the required performance.

[0375] The resin composition of this embodiment preferably has excellent flowability.

[0376] Specifically, the melt volumetric flow rate (MVR) of the resin composition in this embodiment, according to ISO 1133, at 250°C and a load of 5 kgf, is preferably 3 cm. 3 / 10 minutes or more, can reach 10cm 3 / 10 minutes or more, or 15cm 3 / 10 minutes or more. Furthermore, the upper limit of the MVR is, for example, actually 50cm. 3 / Less than 10 minutes.

[0377] The resin composition of this embodiment preferably exhibits excellent resistance to electrical tracking.

[0378] Specifically, the resin composition is injection molded to a thickness of 100mm × 100mm × 3mm, and the CTI value measured according to UL746A is preferably 600V or higher. There is no particular upper limit to the CTI value; for example, even a value below 1000V is sufficient to meet the required performance.

[0379] The resistance to electrical tracking can be achieved, for example, by using the optimal type and amount of elastomer, optimizing the ratio of polycarbonate resin to polyethylene terephthalate resin, using titanium dioxide, and using the optimal type and amount of flame retardant.

[0380] The resin composition of this embodiment can reduce peak pressure during molding.

[0381] Specifically, the peak molding pressure when molding the resin composition of this embodiment into a multipurpose test piece A1 according to JIS K7139 can be set to 102 MPa or less, 96 MPa or less, or 95 MPa or less. The lower limit of the peak molding pressure is, for example, 40 MPa or more.

[0382] The low peak pressure during molding can be achieved, for example, by using polycarbonate resin with a low MVR value or by optimizing the type and amount of elastomer.

[0383] The recyclability described above was calculated according to the embodiments described later. The nominal fracture strain, Tc (crystallization temperature), impact resistance, flame retardancy, load flexural temperature, MVR, tracking resistance, and peak pressure during molding were measured according to the embodiments described later.

[0384] <Method for manufacturing resin composition>

[0385] The resin composition of this embodiment can be manufactured using conventional methods for resin compositions containing thermoplastic resins. For example, the resin composition of this embodiment can be manufactured by a method comprising feeding polyalkylene terephthalate resin, polycarbonate resin, flame retardant, and other components to an extruder and performing melt compounding. Reinforcing fillers can also be side-fed into the extruder. Furthermore, if the resin composition contains a colorant, it can be formulated and melt-compounded in the form of a masterbatch pre-mixed with the thermoplastic resin.

[0386] The heating temperature during melt mixing can usually be appropriately selected from the range of 220 to 350°C, preferably from the range of 220°C to 320°C, and more preferably from the range of 220°C to 280°C.

[0387] <Manufacturing Methods for Molded Articles>

[0388] The resin composition of this embodiment is molded according to a known method.

[0389] There are no particular limitations on the manufacturing method of the molded article; any molding method commonly used for resin compositions can be adopted. Examples include injection molding, high-speed injection molding, injection compression molding, two-color molding, gas-assisted hollow molding, molding using insulated molds, molding using rapidly heated molds, foam molding (including supercritical fluid), insert molding, IMC (in-mold coating) molding, extrusion molding, sheet molding, thermoforming, rotational molding, lamination molding, compression molding, and blow molding, among which injection molding is preferred.

[0390] For details of the injection molding method, please refer to paragraphs 0113 to 0116 of Japanese Patent No. 6183822, which are incorporated herein by reference.

[0391] In addition, the mold temperature during injection molding and other mold forming processes is preferably 40 to 150°C.

[0392] <Application>

[0393] One example of the resin composition in this embodiment is granules.

[0394] The molded article of this embodiment is formed from the resin composition of this embodiment or the particles of this embodiment.

[0395] The molded articles of this embodiment can be applied to a variety of uses, such as various storage containers, electrical / electronic equipment components, office automation (OA) equipment components, home appliance components, mechanical mechanism components, vehicle components (vehicle mechanism components, vehicle housing components), etc.

[0396] Examples of vehicle components include housings for lights, rearview mirrors, bezels, extension components, connectors, ECU housings, head-up display housings, in-vehicle camera housings, millimeter-wave radar housings, battery housings, inverters, high-voltage connectors, sensor housings, and housings for charging components for EVs.

[0397] As electrical / electronic components, examples include display devices such as personal computers, game consoles, and televisions; printers, copiers, scanners, fax machines, electronic notebooks, PDAs, desktop calculators, electronic dictionaries, cameras, camcorders, mobile phones, battery packs, drivers and reading devices for recording media, mice, numeric keys, CD players, MD players, portable radios / audio players, housings, covers, keyboards, buttons, switching components, housings for power meters, battery housings, battery transport trays, relays, sensors, actuators, terminal switches, and components for barbecue and cooking equipment.

[0398] Example

[0399] The present invention will be further described in detail below with examples. The materials, amounts, proportions, processing contents, and processing order shown in the following examples can be appropriately modified without departing from the spirit of the invention. Therefore, the scope of the present invention is not limited to the specific examples shown below.

[0400] If the measuring equipment used in the examples is difficult to obtain due to production stoppages or other reasons, other equipment with equivalent performance can be used for the measurement.

[0401] 1. Raw materials

[0402] Use the raw materials shown in Tables 1 and 2 below.

[0403]

[0404]

[0405] <Determination of Bisphenol A (BPA) Content in Polycarbonate Resins (Virgin and Recycled)>

[0406] Polycarbonate resin was dissolved in dichloromethane solution, and methanol was added dropwise to allow the polymer components to precipitate again. The precipitate was then filtered, dried, and solidified. The resulting substance was dissolved in 5 mL of methanol. The bisphenol A content was determined by analyzing the methanol solution using high-performance liquid chromatography (HPLC) (Shimadzu Corporation "LC-20AD Prominence"). It should be noted that a calibration curve prepared using separately adjusted standard substances was used to calculate the content.

[0407] <Determination of branching content in polycarbonate resins (virgin and recycled)>

[0408] In this embodiment, the branching amount of the polycarbonate resin refers to the total content (unit: mass ppm) of PSA, PSA-Me, PBA, and dicarboxylic acids (DA1, DA2) (structures shown below) obtained after hydrolyzing the polycarbonate resin.

[0409] Specifically, 0.5 g of polycarbonate resin was dissolved in 5 mL of dichloromethane, followed by the addition of 45 mL of methanol and 5 mL of 25% sodium hydroxide aqueous solution. The mixture was then stirred at 70°C for 30 minutes to hydrolyze the solution (in dichloromethane). Next, 6 equivalents of hydrochloric acid were added to the dichloromethane solution to adjust the pH to approximately 2, and the solution was then diluted to 100 mL with pure water.

[0410] Next, 20 μL of the adjusted dichloromethane solution was injected into a liquid chromatograph to determine the contents of PSA, PSA-Me, PBA, and dicarboxylic acids (DA1, DBA2) as shown in the following structures. Their total amount was taken as the branching amount of the polycarbonate resin (unit: mass ppm).

[0411] The liquid chromatography method and determination conditions are as follows.

[0412] Liquid chromatography: LC-10AD manufactured by Shimadzu Corporation.

[0413] Column: YMC PACK ODS-AM M-307-3

[0414] 4.6mm ID × 75mm L.

[0415] Detector: UV280nm.

[0416] Eluent: (A) 0.05% trifluoroacetic acid aqueous solution (B) methanol.

[0417] Gradient conditions: 0 minutes (B=40%), 25 minutes (B-95%).

[0418] The contents of PSA, PSA-Me, PBA, and dicarboxylic acids (DA1, DA2) were calculated from their respective peak areas based on a calibration curve prepared with bisphenol A.

[0419] The PSA, PSA-Me, PBA, and dicarboxylic acids (DA1, DA2) mentioned above are described below.

[0420] [Chemical Formula 10]

[0421]

[0422] <Determination of MVR in Polycarbonate Resins (Virgin and Recycled)>

[0423] For polycarbonate resins (virgin and recycled), the melt volumetric flow rate is determined according to ISO 1133 at 300°C and a load of 1.20 kgf. The unit is cm. 3 Expressed in / 10min format.

[0424] <Dispersion (Mw / Mn) of polycarbonate resins (virgin and recycled)>

[0425] The weight-average molecular weight (Mw) and number-average molecular weight (Mn) of polycarbonate resins (virgin and recycled) were determined using an HLC-8320 GPC / EcoSEC (manufactured by TOSOH) and calculated using polystyrene conversion. The determination conditions are as follows.

[0426] Chromatographic column: Shodex KF-G+KF-805L×3+KF-800D.

[0427] Detector: UV detector 254nm.

[0428] Column temperature: 40℃.

[0429] Eluent: Tetrahydrofuran (THF).

[0430] Based on the obtained Mw and Mn, the dispersion (Mw / Mn) is calculated.

[0431] It should be noted that Mw and Mn in this specification are values ​​determined by the above method for each component.

[0432] Furthermore, in cases containing two or more polycarbonate resins, the Mw and Mn of the polycarbonate resins are respectively the Mw and Mn of the mixture. The same applies to other components.

[0433] <Determination of the Amount of Metallic Elements>

[0434] Qualitative / semi-quantitative analysis of metallic elements (Al, Fe, P) in polycarbonate resin was performed using ICP emission spectroscopy. As a pretreatment step, 200 mg of sample was weighed and subjected to Kjeldahl wet decomposition (sulfuric acid / nitric acid, sulfuric acid / hydrogen peroxide), then diluted to 50 mL. ICP emission spectroscopy was then performed using an acid concentration-matched single-point calibration method. Units are expressed in ppm (mass).

[0435] ICP emission spectroscopy was performed using the Thermo-Thrmo Fisher Scientific "iCAP7600duoiCAP76000uo" via axial / radial photometry.

[0436] The details of PC-1 to PC-6 are as follows.

[0437]

[0438] 2. Examples 1-1 to 1-3, Comparative Example 1, Reference Example 1

[0439] <Mix>

[0440] The components shown in Table 1 or Table 2 are uniformly mixed using a drum mixer in the proportions shown in Table 4 (each component in Table 4 is expressed in parts by mass). The resulting mixture is fed into a twin-screw extruder (Nippon Steel Works "TEX30α"). The mixture is melt-blended at a barrel temperature of 260°C and a screw speed of 200 rpm. The resulting resin composition is then rapidly cooled in a water bath and granulated using a granulator to obtain granules of the resin composition.

[0441] <Regeneration Rate (mass%)>

[0442] Calculate the ratio (mass%) of the recycled component to the total amount of the resin composition.

[0443] <Nominal strain of fracture>

[0444] After drying the resin composition particles obtained above at 120°C for 5 hours, they were injection molded into JIS K7139 multipurpose test piece A1 (4mm thick) using a Nippon Steel Corporation injection molding machine "J-85AD-60H" at a barrel temperature of 250°C and a mold temperature of 80°C.

[0445] The nominal strain at tensile fracture is determined based on JIS K7161-1.

[0446] Crystallization temperature (Tc)

[0447] The particle size of the above resin composition was determined using a differential scanning calorimeter (DSC) based on JIS K7121. Under a nitrogen atmosphere, the temperature was increased from 40°C to 300°C at a rate of 20°C / min, held at 300°C for 3 minutes, and then decreased to 40°C at a rate of -20°C / min. This was repeated as one cycle, and two cycles were performed. The maximum peak temperature generated by crystallization during cooling in each cycle was taken as the crystallization temperature.

[0448] The differential scanning calorimeter used is the “DSC7020” manufactured by Hitachi High-Tech Science Co., Ltd.

[0449] Charpy impact strength with notch

[0450] After drying the resin composition particles obtained above at 120°C for 5 hours, they were injection molded into JISK7139 multipurpose test piece A1 (4mm thick) using a "J-85 AD-60H" injection molding machine manufactured by Nippon Steel Works Co., Ltd., under conditions of barrel temperature 250°C and mold temperature 80°C.

[0451] Using the aforementioned multipurpose test piece (4 mm thick), the unnotched Charpy impact strength (unit: KJ / m²) was determined based on the JIS K7111-1 standard. 2 ).

[0452] Flame retardancy

[0453] After drying the resin composition particles obtained above at 120°C for 5 hours, they were injection molded into combustion test pieces (12.7 mm wide × 127 mm long × 1.0 mm thick) using an injection molding machine (J-50AD manufactured by Japan Steel Works Co., Ltd.) at a barrel temperature of 250°C and a mold temperature of 80°C.

[0454] After the obtained combustion test specimens were left to stand at 70°C for one week, their flame retardancy was evaluated according to the Underwriters Laboratories Subject 94 (UL 94) method.

[0455] <Critical Tracking Resistance (CTI)>

[0456] The obtained granules were dried at 120°C for 6 hours until nearly dry. Then, using an injection molding machine (Nissei Resin Kogyo Co., Ltd. "NEX-80"), flat test pieces measuring 100mm × 100mm × 3mm were formed at a barrel temperature of 260°C. The resistance to tracking, as specified in UL746A23, was tested according to ASTM D3638. Electrolyte (0.1% ammonium chloride aqueous solution, resistivity 385 Ω·cm at 23°C) was added dropwise from the nozzle at 30-second intervals. A voltage of less than 600V (in 25V increments) was applied between the two platinum electrodes. The number of electrolyte drops required to reach the point of tracking was measured, and the average of five drops was calculated as the maximum voltage (in V) for 50 drops.

[0457] Peak pressure during molding (MPa)

[0458] After drying the resin composition particles obtained above at 120°C for 5 hours, the peak injection pressure (MPa) of the JISK7139 multipurpose test piece A1 (4mm thick) was read using an injection molding machine "J-85AD-60H" manufactured by Nippon Steel Works Co., Ltd., under the conditions of barrel temperature 250°C and mold temperature 80°C.

[0459]

[0460] As can be seen from the above results, the resin composition of the present invention has a good and excellent balance of various physical properties.

[0461] 3. Examples 2-1 to 2-5, Comparative Example 2, Reference Example 2

[0462] <Mix>

[0463] The components shown in Table 1 or Table 2 are mixed uniformly using a drum mixer in the proportions shown in Table 5 or Table 6 (each component in Table 5 and Table 6 is expressed in parts by mass), excluding glass fiber. The resulting mixture is fed into a twin-screw extruder (TEX30α, manufactured by Nippon Steel Works) through the main feed inlet. The barrel temperature of the first mixing section is set to 260°C, and glass fiber is supplied by a side feeder. The resin composition is melt-mixed at a barrel temperature of 260°C and a screw speed of 200 rpm after the addition of glass fiber. The resulting resin composition is then rapidly cooled in a water bath and granulated using a granulator to obtain granules of the resin composition.

[0464] <MVR of Resin Compositions>

[0465] The melt flow rate of the obtained resin composition was determined according to ISO 1133 at 250°C and a load of 5 kgf. The unit is cm. 3 Expressed in / 10min format.

[0466] <Load Flexural Temperature (DTUL)>

[0467] After drying the obtained resin particles at 120°C for 6 hours, they were injection molded into ISO tensile test pieces (4 mm thick) using an injection molding machine ("J-85AD" manufactured by Nippon Steel Works Co., Ltd.) at a barrel temperature of 250°C and a mold temperature of 80°C.

[0468] According to ISO 75-1 and 2, the load flexural temperature (unit: °C) was determined using the above-mentioned ISO tensile test specimen (thickness 4 mm) under a load of 1.80 MPa.

[0469] Flame retardancy

[0470] After drying the resin composition particles obtained above at 120°C for 5 hours, they were injection molded into combustion test pieces (12.7 mm wide × 127 mm long × 0.74 mm thick) using an injection molding machine (J-50AD manufactured by Japan Steel Works Co., Ltd.) at a barrel temperature of 250°C and a mold temperature of 80°C.

[0471] After the obtained combustion test specimens were left to stand at 70°C for one week, their flame retardancy was evaluated according to the Underwriters Laboratories Subject 94 (UL 94) method.

[0472] For each of the five test pieces, a burner flame was applied to the lower end of the vertically supported test piece and held for 10 seconds, then the burner flame was moved away from the test piece. Immediately after the flame disappeared, the burner flame was applied again for 10 seconds, and then the burner flame was removed.

[0473] The total flaming time (in seconds) of the five test pieces and the results of the UL-94 determination are shown in Tables 5 and 6.

[0474]

[0475]

[0476] The PBT:PC (mass ratio) in the table also includes the PBT resin in the antimony trioxide masterbatch and carbon black masterbatch.

[0477] As can be seen from the above results, the resin composition of the present invention achieves excellent flame retardancy despite using recycled polycarbonate resin (Examples 2-1 to 2-5).

[0478] On the other hand, the flame retardancy is poor when using virgin polycarbonate resin (PC-5) with a high branching content (Comparative Example 2) or recycled polycarbonate resin (PC-4) with a high bisphenol A content (Reference Example 2).

Claims

1. A resin composition comprising 5 to 50 parts by weight of a flame retardant relative to 100 parts by weight of a total of alkylene terephthalate resin and polycarbonate resin. The mass ratio of alkyl terephthalate resin to polycarbonate resin in 100 parts by mass of the total mixture of alkyl terephthalate resin and polycarbonate resin is 10 / 90 to 90 / 10. The polycarbonate resin comprises polycarbonate resin derived from recycled sources. The branching content of the polycarbonate resin derived from recycled polycarbonate is 50 to 3500 ppm by mass.

2. The resin composition according to claim 1, wherein, The elastomer comprises 1 to 30 parts by weight relative to 100 parts by weight of the total mixture of alkylene terephthalate resin and polycarbonate resin. The mass ratio of polyalkylene terephthalate resin to polycarbonate resin in 100 parts by mass of the total mixture of polyalkylene terephthalate resin and polycarbonate resin is 80 / 20 to 20 / 80. The recycled polycarbonate resin, when subjected to a melt volumetric flow rate (MVR) of 2–11 cm⁻¹ under conditions of 300°C and a load of 1.20 kgf, as determined according to ISO 1133. 3 / 10 minutes.

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

4. The resin composition according to claim 1, wherein, The recycled polycarbonate resin, when subjected to a melt volumetric flow rate (MVR) of 4–30 cm⁻¹ under conditions of 300°C and a load of 1.20 kgf, as determined according to ISO 1133. 3 / 10 minutes.

5. The resin composition according to claim 1, 2 or 4, wherein, Relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin, it further comprises 0.01 to 2 parts by weight of an ester exchange inhibitor.

6. The resin composition according to claim 1, 2 or 4, wherein, In the polyalkylene terephthalate resin, polybutylene terephthalate resin accounts for more than 50% by mass.

7. The resin composition according to claim 1, 2 or 4, wherein, The flame retardant includes a brominated flame retardant.

8. The resin composition according to claim 1, 2 or 4, wherein, The mixture further comprises 3 to 30 parts by weight of elastomer, relative to a total of 100 parts by weight of the alkylene terephthalate resin and the polycarbonate resin.

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

10. The resin composition according to claim 1, 2 or 4, wherein, The resin composition is molded into test pieces with a thickness of 0.74 mm or 1.0 mm for UL-94 testing, and the flame retardancy meets V-0 requirements according to the UL-94 test.

11. The resin composition according to claim 1, 2 or 4, wherein, The recycled polycarbonate resin includes at least one of the following: polycarbonate resin derived from bottles, polycarbonate resin derived from discs, polycarbonate resin derived from sheets, polycarbonate resin derived from instrument panels, and polycarbonate resin derived from headlight lenses.

12. The resin composition according to claim 1, wherein, The recycled polycarbonate resin, when subjected to a melt volumetric flow rate (MVR) of 4–30 cm⁻¹ under conditions of 300°C and a load of 1.20 kgf, as determined according to ISO 1133. 3 / 10 minutes, The resin composition further comprises 0.01 to 2 parts by weight of an exchange inhibitor relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin. The polyalkylene terephthalate resin comprises polybutylene terephthalate resin. The flame retardant includes a brominated flame retardant. The resin composition further comprises 1 to 30 parts by weight of elastomer relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin. The recycled polycarbonate resin contains aluminum in a ratio of 0.2 to 1000 ppm by mass and iron in a ratio of 0.2 to 100 ppm by mass. The resin composition further comprises 0.1 to 3 parts by weight of carbon black relative to 100 parts by weight of the total polyalkylene terephthalate resin and polycarbonate resin.

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

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

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

16. A particle, which is a particle of the resin composition according to claim 1, 2, 4, 12 or 15.

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

18. A molded article formed from the particles according to claim 16.

Images