Resin composition, pellet, and molded article

Abstract

Provided are a novel polybutylene terephthalate resin composition, a pellet, and a molded article. A resin composition according to the present disclosure comprises: a polybutylene terephthalate resin; and at least one among an amorphous thermoplastic resin having a carbonate bond and / or an ester bond and a polystyrene-based resin, wherein the active titanium parameter X of the polybutylene terephthalate resin is 25 or less.

Description

Resin composition, pellets, and molded products

[0001] The present invention relates to a resin composition, a pellet, and a molded article, and more particularly to a resin composition containing a polybutylene terephthalate resin as a main component.

[0002] Polybutylene terephthalate resin, a representative engineering plastic among thermoplastic polyester resins, is widely used in injection-molded products such as automotive parts, electrical and electronic parts, and precision instrument parts due to its ease of molding and processing, mechanical properties, heat resistance, chemical resistance, aroma retention, and other excellent physical and chemical properties.

[0003] When a resin composition containing polybutylene terephthalate resin is injection molded, it is desirable that the crystallization temperature (Tc) during cooling is high. This is because a high crystallization temperature (Tc) during cooling improves the molding cycle. To solve this problem, polybutylene terephthalate resin compositions having a high crystallization temperature (Tc) during cooling have been studied (Patent Document 1, Patent Document 2).

[0004] On the other hand, polybutylene terephthalate resin is a crystalline resin, and therefore has a large molding shrinkage rate. In particular, when inorganic fillers such as glass fiber are blended, anisotropy tends to increase, which can lead to warping of molded products. Therefore, methods of blending various amorphous resins have been proposed to reduce warping (Patent Documents 3 to 5).

[0005] Additionally, polybutylene terephthalate resins are characterized by excellent mechanical properties, electrical properties, processing properties, etc., and are widely used in various applications (Patent Documents 6 to 8).

[0006] JP 2024-42437 A JP 2011-084640 A JP 2006-16559 A JP 2007-314619 A JP 2020-84037 A International Publication No. 2019 / 217680 JP 2018-203932 A International Publication No. 2020 / 246335

[0007] As described above, polybutylene terephthalate resins are widely used, and new materials are still needed. The present invention aims to solve this problem by providing a novel polybutylene terephthalate resin composition, as well as pellets and molded articles.

[0008] The above-mentioned problems have been solved by the following means: [1] A resin composition comprising a polybutylene terephthalate resin, an amorphous thermoplastic resin having a carbonate bond and / or an ester bond, and at least one polystyrene-based resin, wherein the polybutylene terephthalate resin has an active titanium parameter X shown below of 25 or less. [2] A resin composition comprising a polybutylene terephthalate resin and at least one selected from the group consisting of an inorganic filler, a release agent, and a stabilizer, wherein the polybutylene terephthalate resin has a total nitrogen element content of 0.1 to 3,000 ppm by mass and an active titanium parameter X shown below of 25 or less. [3] A resin composition comprising a polybutylene terephthalate resin and an amorphous thermoplastic resin having a carbonate bond and / or an ester bond, wherein the polybutylene terephthalate resin has an active titanium parameter X of 25 or less. [4] The resin composition according to any one of the above, wherein the amorphous thermoplastic resin having a carbonate bond and / or an ester bond comprises a polycarbonate resin. [5] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin comprises a polybutylene terephthalate resin derived from recycled materials. [6] The resin composition according to any one of the above, further comprising a reactive compound. [7] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin contains 0.1 to 100 ppm by mass of sodium element, the polybutylene terephthalate resin contains 0.1 to 3000 ppm by mass of calcium element, the proportion α of active titanium in the polybutylene terephthalate resin, which is represented by the following formula (3), is 0.50 or less, the amorphous thermoplastic resin having a carbonate bond and / or an ester bond contains a polycarbonate resin, the polybutylene terephthalate resin contains a polybutylene terephthalate resin derived from recycled materials, and further contains a reactive compound, and the resin composition is for injection molding. α=X / M...Equation (3) (In equation (3), X is an active titanium parameter, and [M] is the titanium element concentration (ppm by mass) in the polybutylene terephthalate resin.) [8] The polybutylene terephthalate resin contains 0.1 to 100 ppm by mass of sodium element, The polybutylene terephthalate resin contains 0.1 to 3000 ppm by mass of calcium element, The proportion α of active titanium in the polybutylene terephthalate resin, which is represented by the following equation (3), is 0.50 or less, The amorphous thermoplastic resin having a carbonate bond and / or an ester bond contains a polycarbonate resin, The polybutylene terephthalate resin contains a polybutylene terephthalate resin derived from material recycling, Further, it contains a reactive compound, The resin is for injection molding, The terminal carboxyl group concentration of the polybutylene terephthalate resin is 25 μmol / g (μeq / g) or more, The resin composition according to any one of the above, wherein the active titanium parameter X is 12 or less, and the polybutylene terephthalate resin has an Mw / Mn of 2.1 or more.α=X / M (3) (In the formula (3), X is the active titanium parameter, and [M] is the titanium element concentration (ppm by mass) in the polybutylene terephthalate resin.)

[0009] [9] A resin composition comprising a polybutylene terephthalate resin and a polystyrene-based resin, wherein the polybutylene terephthalate resin has an active titanium parameter X of 25 or less.

[10] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin contains 30 to 500 ppm by mass of titanium element.

[11] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin contains 0.1 to 100 ppm by mass of sodium element.

[12] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin contains 0.1 to 3,000 ppm by mass of calcium element.

[13] The resin composition according to any one of the above, wherein the proportion α of active titanium in the polybutylene terephthalate resin, as represented by the following formula (3), is 0.50 or less: α=X / M Formula (3) (In formula (3), X is the active titanium parameter, and [M] is the titanium element concentration (ppm by mass) in the polybutylene terephthalate resin.) (14) The resin composition according to any one of the above, wherein the polybutylene terephthalate resin contains polybutylene terephthalate resin derived from material recycling.

[15] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin comprises two or more polybutylene terephthalate resins having different intrinsic viscosities.

[16] The resin composition according to any one of the above, wherein the resin composition is for injection molding.

[17] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin contains 0.1 to 100 ppm by mass of sodium element, the polybutylene terephthalate resin contains 0.1 to 3000 ppm by mass of calcium element, the proportion α of active titanium in the polybutylene terephthalate resin, represented by the following formula (3), is 0.50 or less, the polybutylene terephthalate resin comprises polybutylene terephthalate resin derived from recycled materials, and the polybutylene terephthalate resin comprises two or more polybutylene terephthalate resins having different intrinsic viscosities. α=X / M (3) (In formula (3), X is the active titanium parameter, and [M] is the titanium element concentration (ppm by mass) in the polybutylene terephthalate resin.)

[18] The polybutylene terephthalate resin contains 0.1 to 100 ppm by mass of sodium element, The polybutylene terephthalate resin contains 0.1 to 3000 ppm by mass of calcium element, The proportion α of active titanium in the polybutylene terephthalate resin, which is represented by the following formula (3), is 0.50 or less, The polybutylene terephthalate resin contains polybutylene terephthalate resin derived from material recycling, The polybutylene terephthalate resin contains two or more polybutylene terephthalate resins having different intrinsic viscosities, The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has a terminal carboxyl group concentration of 25 μmol / g (μeq / g) or more, The active titanium parameter X is 12 or less, The polybutylene terephthalate resin has an Mw / Mn of 2.1 or more. α=X / M (3) (In the formula (3), X is the active titanium parameter, and [M] is the titanium element concentration (ppm by mass) in the polybutylene terephthalate resin.)

[0010]

[19] A resin composition comprising a polybutylene terephthalate resin and at least one selected from the group consisting of an inorganic filler, a release agent, and a stabilizer, wherein the polybutylene terephthalate resin has a total nitrogen element content of 0.1 to 3000 mass ppm and an active titanium parameter X shown below of 25 or less.

[20] The resin composition according to any one of the above, comprising 10 to 150 parts by mass of an inorganic filler per 100 parts by mass of the polybutylene terephthalate resin, wherein the inorganic filler is a fibrous reinforcing material.

[21] The resin composition according to any one of the above, comprising a mold release agent and / or a stabilizer.

[22] The resin composition according to any one of the above, wherein the active titanium parameter X is 12 or less.

[23] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin contains 30 to 500 ppm by mass of titanium element.

[24] The resin composition according to any one of the above, further comprising a recycled polyethylene terephthalate resin.

[25] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has a total sulfur element content of 0.1 to 100 ppm by mass.

[26] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has a terminal vinyl group concentration of 1 to 15 μmol / g.

[27] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has dicarboxylic acid units and diol units, wherein 80 mol % or more of all dicarboxylic acid units are terephthalic acid units derived from fossil resources, and 80 mol % or more of all diol units are 1,4-butanediol units derived from fossil resources.

[28] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has an Mw / Mn ratio of 2.1 or more.

[29] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin contains a recycled product.

[30] The resin composition according to any one of the above, further containing an epoxy compound.

[31] The polybutylene terephthalate resin contains 10 to 150 parts by mass of an inorganic filler relative to 100 parts by mass of the polybutylene terephthalate resin, the inorganic filler being a fibrous reinforcing material, and the polybutylene terephthalate resin contains a release agent and / or a stabilizer, the active titanium parameter X is 12 or less, the polybutylene terephthalate resin contains 30 to 500 ppm by mass of titanium element, the polybutylene terephthalate resin has a terminal carboxyl group concentration of 25 μmol / g or more, and further contains recycled polyethylene terephthalate resin, the polybutylene terephthalate resin has a total sulfur element content of 0.1 to 100 ppm by mass, and the polybutylene terephthalate resin has a terminal vinyl group concentration of 1 to 15 μmol / g, The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has dicarboxylic acid units and diol units, wherein 80 mol % or more of all dicarboxylic acid units are terephthalic acid units and 80 mol % or more of all diol units are 1,4-butanediol units; the polybutylene terephthalate resin has an Mw / Mn of 2.1 or more; and the polybutylene terephthalate resin includes a recycled product.

[32] The resin composition according to any one of the above, further including an epoxy compound.

[33] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has dicarboxylic acid units and diol units, wherein 80 mol % or more of all dicarboxylic acid units are terephthalic acid units derived from fossil resources and 80 mol % or more of all diol units are 1,4-butanediol units derived from fossil resources.

[34] The resin composition according to any one of the above, wherein the resin composition is for use in bonding with an epoxy adhesive.

[0011]

[35] A resin composition comprising 10 to 150 parts by mass of a fibrous reinforcing material per 100 parts by mass of polybutylene terephthalate resin, wherein the polybutylene terephthalate resin has a total nitrogen element content of 1 to 3,000 ppm by mass.

[36] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has a total sulfur element content of 1 to 100 ppm by mass.

[37] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has a terminal vinyl group concentration of 1 to 15 μmol / g.

[38] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has dicarboxylic acid units and diol units, wherein 80 mol % or more of the total dicarboxylic acid units are terephthalic acid units derived from fossil resources and 80 mol % or more of the total diol units are 1,4-butanediol units derived from fossil resources.

[39] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has an Mw / Mn ratio of 2.1 or more.

[40] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin comprises a recycled product.

[41] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has a total sulfur element content of 1 to 100 ppm by mass, wherein the polybutylene terephthalate resin has a terminal vinyl group concentration of 1 to 15 μmol / g, wherein the polybutylene terephthalate resin has dicarboxylic acid units and diol units, wherein 80 mol % or more of the total dicarboxylic acid units are terephthalic acid units and 80 mol % or more of the total diol units are 1,4-butanediol units, wherein the polybutylene terephthalate resin has an Mw / Mn ratio of 2.1 or more, and wherein the polybutylene terephthalate resin comprises a recycled product.

[42] The resin composition according to any one of the above, wherein the polybutylene terephthalate resin has dicarboxylic acid units and diol units, wherein 80 mol % or more of all dicarboxylic acid units are terephthalic acid units derived from fossil resources, and 80 mol % or more of all diol units are 1,4-butanediol units derived from fossil resources.

[43] The resin composition according to any one of the above, which is for use in epoxy adhesive bonding.

[44] Pellets of the resin composition according to any one of the above.

[45] A molded product molded from the resin composition according to any one of the above.

[46] A molded article molded from the above pellets.

[47] A composite comprising any of the molded articles described above and an adhesive layer, the adhesive layer comprising an epoxy-based adhesive.

[0012] According to the present invention, it is possible to provide a novel polybutylene terephthalate resin composition, as well as pellets and molded articles.

[0013] Hereinafter, a mode for carrying out the present invention (hereinafter simply referred to as "the present embodiment") will be described in detail. Note that the following present embodiment is an example for explaining the present invention, and the present invention is not limited to this embodiment. Note that in this specification, "to" is used to mean that the numerical values ​​written before and after it are included as the lower limit and upper limit. "A to B" means A or more and B or less. Furthermore, with regard to the upper and lower limit values ​​of numerical values ​​in this specification, any combination of the upper and lower limit values ​​can be cited as an example of this embodiment.

[0014] In this specification, various physical property values ​​and characteristic values ​​are those at 23°C unless otherwise specified. In this specification, ppm means mass ppm. If the measurement methods, etc. described in the standards shown in this specification vary from year to year, they shall be based on the standards in effect as of January 1, 2024, unless otherwise specified. If the measurement methods, etc. described in the standards shown in this specification are abolished as of January 1, 2024, they shall be based on the standards in effect at the time of abolition.

[0015] The first resin composition of the present embodiment contains a polybutylene terephthalate resin, an amorphous thermoplastic resin having a carbonate bond and / or an ester bond, and at least one polystyrene-based resin, and the polybutylene terephthalate resin has an active titanium parameter X shown below of 25 or less. By adopting such a constitution, it is possible to obtain a resin composition having a high crystallization temperature Tc during cooling, or a resin composition capable of providing a molded product with high weld strength.

[0016] In particular, blending an amorphous thermoplastic resin having a carbonate bond and / or an ester bond results in a resin composition with a high crystallization temperature (Tc) during cooling. The reason for this is that blending a thermoplastic resin having a carbonate bond and / or an ester bond with a polybutylene terephthalate resin tends to increase the crystallization temperature (Tc) during cooling. However, a titanium catalyst is commonly used to produce polybutylene terephthalate resin. Blending a titanium-catalyzed polybutylene terephthalate resin with a thermoplastic resin having a carbonate bond and / or an ester bond results in a transesterification reaction between the polybutylene terephthalate resin and the thermoplastic resin having a carbonate bond and / or an ester bond. The transesterification reaction is more likely to occur when the activity of the titanium catalyst is high. In this embodiment, it is presumed that by setting the active titanium parameter to 25 or less, the transesterification reaction between the polybutylene terephthalate resin and the thermoplastic resin having a carbonate bond and / or an ester bond is suppressed, resulting in a resin composition with a high crystallization temperature (Tc) during cooling.

[0017] Furthermore, the resin composition of this embodiment can reduce mold release resistance during molding. Furthermore, the resin composition of this embodiment can further improve transparency. Furthermore, since the resin composition of this embodiment has a high crystallization temperature Tc during cooling, the molding cycle can be shortened and moldability can be improved.

[0018] On the other hand, by blending a polystyrene-based resin, a resin composition can be obtained that can provide molded articles with high weld strength. Blending a polystyrene-based resin is considered to achieve low warpage in molded articles formed from polybutylene terephthalate resin. However, blending a polystyrene-based resin with a polybutylene terephthalate resin tends to reduce weld strength. Under these circumstances, the present inventors discovered the use of a polybutylene terephthalate resin with low titanium activity. Specifically, when producing polybutylene terephthalate resin, a method is generally used in which butylene glycol and terephthalic acid are reacted in the presence of a titanium catalyst. Here, even in the produced polybutylene terephthalate resin, if titanium activity is high, tetrahydrofuran gas derived from the butanediol terminals is likely to be generated. It is presumed that molding a resin composition containing a large amount of such tetrahydrofuran gas would easily clog voids at the flow end of the mold, resulting in reduced weld strength. In this embodiment, it is presumed that the combined use of polybutylene terephthalate resin with low titanium activity and polystyrene resin effectively suppresses the generation of tetrahydrofuran gas derived from butanediol, thereby improving the weld strength. In particular, as will be shown in the examples described later, a surprising increase in weld strength of about 20% was observed in the present invention.

[0019] The second resin composition of the present embodiment includes a polybutylene terephthalate resin and at least one selected from the group consisting of an inorganic filler, a release agent, and a stabilizer, wherein the polybutylene terephthalate resin has a total nitrogen element content of 0.1 to 3000 ppm by mass and an active titanium parameter X shown below of 25 or less.

[0020] By adopting this configuration, a resin composition can be obtained that has a low gas content in the pellets after production, and can provide molded products that have excellent adhesive strength to other components using an epoxy adhesive while maintaining mechanical strength. That is, it has been found that, depending on the type of polybutylene terephthalate resin, a large amount of gas may be contained in the pellets after production. In this embodiment, by using a specific polybutylene terephthalate resin, gas generation can be effectively suppressed.

[0021] Hereinafter, the embodiments of the present invention will be described in detail. However, the explanation of the constituent elements described below is an example of an embodiment of the present invention, and the present invention is not limited to these contents.

[0022] <Polybutylene terephthalate resin> The resin composition of the present embodiment preferably contains a polybutylene terephthalate resin having an active titanium parameter X shown below of 25 or less. The resin composition also preferably contains 30 to 500 ppm by mass of titanium element.

[0023] Titanium catalysts are commonly added to the polymerization of polybutylene terephthalate resins. However, it has been found that if the titanium catalyst activity is high in the polymerized polybutylene terephthalate resin, transesterification tends to occur more easily with amorphous thermoplastic resins having carbonate bonds and / or ester bonds. In particular, in industrial mass production, extrusion is carried out continuously for long periods of time using a large extruder, and in such cases, transesterification tends to be more accelerated. In this embodiment, it is presumed that the use of a polybutylene terephthalate resin with low titanium activity effectively suppresses the transesterification with amorphous thermoplastic resins having polycarbonate bonds and / or ester bonds.

[0024] On the other hand, it has been found that when the titanium catalyst activity is high in the polybutylene terephthalate resin after polymerization, tetrahydrofuran derived from butanediol tends to be generated easily. In particular, in the case of industrial mass production, extrusion is carried out continuously for a long time using a large extruder, and in such a case, tetrahydrofuran tends to be generated more easily. In this embodiment, it is presumed that by using a polybutylene terephthalate resin with low titanium activity, the generation of tetrahydrofuran gas in the molded product can be effectively suppressed and the weld strength can be improved.

[0025] The active titanium parameter X of the polybutylene terephthalate resin used in this embodiment is 25 or less, preferably 20 or less, more preferably 15 or less, even more preferably 12 or less, and still more preferably 10 or less. The lower limit of the active titanium parameter X of the polybutylene terephthalate resin is preferably 0, but even if it is 1 or more, the required performance is sufficiently satisfied. When two or more polybutylene terephthalate resins are used, it is preferable that the polybutylene terephthalate resin with the greatest content satisfies the above active titanium parameter, and it is more preferable that all of the polybutylene terephthalate resins satisfy the above active titanium parameter.

[0026] Polybutylene terephthalate resin synthesized using a titanium catalyst and having a low titanium activity parameter X can be obtained, for example, by the following method: (1) Increasing the concentration of metal elements, such as sodium and calcium, in the polybutylene terephthalate resin. These metal elements tend to reduce the activity of the titanium catalyst. (2) Increasing the alkaline components in the polybutylene terephthalate resin. Because titanium catalysts are acid catalysts, the presence of alkaline components tends to reduce their activity. (3) Increasing the terminal carboxylic acid concentration of the polybutylene terephthalate resin. (4) Using recycled polybutylene terephthalate resin. Material-recycled polybutylene terephthalate resins, in particular, tend to have low titanium activity. α=X / M...Equation (3) (In Equation (3), X is the titanium activity parameter, and [M] is the titanium element concentration (ppm by mass) in the polybutylene terephthalate resin.)

[0027] The evaluation of the change in terminal carboxyl group concentration over time is carried out in a nitrogen atmosphere to prevent the influence of oxygen. Furthermore, if the water concentration in the polybutylene terephthalate resin being evaluated is high, hydrolysis reactions occur frequently, making it difficult to accurately grasp the decomposition behavior associated with catalytic activity other than hydrolysis. Therefore, a low water concentration is preferable, and the evaluation is carried out at 300 mass ppm or less. The evaluation is carried out at a temperature of 245°C. Under these heat treatment conditions, the decrease in number average molecular weight due to reactions other than hydrolysis caused by the water contained in the polybutylene terephthalate resin can be ignored, and the increase in terminal carboxyl group concentration due to the hydrolysis reaction can be considered to be equal to the increase in terminal hydroxyl group concentration before and after the heat treatment. Therefore, the change in terminal carboxyl group concentration due to thermal decomposition reactions other than hydrolysis reactions can be calculated using the following formula (4):

[0028] Formula (4)

[0029] The titanium element concentration in the polybutylene terephthalate resin used in the present embodiment is preferably 30 ppm by mass or more, and may be 35 ppm by mass or more, 40 ppm by mass or more, 45 ppm by mass or more, 50 ppm by mass or more, 55 ppm by mass or more, 60 ppm by mass or more, 65 ppm by mass or more, 70 ppm by mass or more, or 75 ppm by mass or more, and is preferably 500 ppm by mass or less, and may be 400 ppm by mass or less, 300 ppm by mass or less, 150 ppm by mass or less, 120 ppm by mass or less, 110 ppm by mass or less, 100 ppm by mass or less, 90 ppm by mass or less, or 80 ppm by mass or less.

[0030] The sodium element concentration in the polybutylene terephthalate resin used in this embodiment is preferably 0.1 ppm by mass or more, more preferably 0.5 ppm by mass or more, even more preferably 0.7 ppm by mass or more, even more preferably 0.9 ppm by mass or more, still more preferably 1 ppm by mass or more, and preferably 100 ppm by mass or less, more preferably 50 ppm by mass or less, even more preferably 30 ppm by mass or less, still more preferably 20 ppm by mass or less, and still more preferably 10 ppm by mass or less. By setting the sodium element concentration at or above the lower limit, the transesterification reaction tends to be more effectively suppressed. Furthermore, by setting the sodium element concentration at or above the lower limit, the generation of tetrahydrofuran gas tends to be more effectively suppressed. Furthermore, by setting the sodium element concentration at or below the upper limit, the alkali decomposition resistance tends to be further improved. The sodium element in the polybutylene terephthalate resin is derived, for example, from the detergent used in the resin washing process.

[0031] The calcium element concentration of the polybutylene terephthalate resin used in this embodiment is preferably 0.1 mass ppm or more, more preferably 1 mass ppm or more, more preferably 3 mass ppm or more, even more preferably 5 mass ppm or more, and even more preferably 7 mass ppm or more. It is also preferably 3000 mass ppm or less, more preferably 2500 mass ppm or less, more preferably 2000 mass ppm or less, preferably 1000 mass ppm or less, more preferably 500 mass ppm or less, more preferably 300 mass ppm or less, even more preferably 200 mass ppm or less, and may be 100 mass ppm or less, 50 mass ppm or less, 30 mass ppm or less, or 10 mass ppm or less. By setting it to the lower limit or higher, transesterification tends to be more effectively suppressed. Furthermore, by setting it to the lower limit or higher, generation of tetrahydrofuran gas tends to be more effectively suppressed. Furthermore, by making the content not more than the upper limit, resistance to alkaline decomposition tends to be further improved. The calcium element in the polybutylene terephthalate resin is derived from, for example, the inorganic filler of the inorganic filler.

[0032] The titanium element concentration, sodium element concentration, and calcium element concentration are measured according to the description in the Examples section below.

[0033] The polybutylene terephthalate resin used in this embodiment preferably has an active titanium ratio α, represented by formula (3), of 0.50 or less. By setting the active titanium ratio α to 0.50 or less, transesterification tends to be more effectively suppressed. α = X / M (3) (In formula (3), X is the active titanium parameter, and [M] is the titanium element concentration (ppm by mass) in the polybutylene terephthalate resin.) The active titanium ratio α is preferably 0.45 or less, more preferably 0.40 or less, even more preferably 0.35 or less, even more preferably 0.30 or less, even more preferably 0.25 or less, even more preferably 0.20 or less, and even more preferably 0.15 or less. The lower limit of the active titanium ratio α is preferably 0, but even if it is 0.01 or more, the required performance is sufficiently met.

[0034] The resin composition of the present embodiment preferably contains a polybutylene terephthalate resin having a total nitrogen content of 0.1 to 3,000 ppm by mass. Use of such a polybutylene terephthalate resin can increase the adhesive strength with an epoxy adhesive.

[0035] In the polybutylene phthalate resin used in this embodiment, the total nitrogen element content is 0.1 mass ppm or more, preferably 1 mass ppm or more, more preferably 2 mass ppm or more, even more preferably 3 mass ppm or more, and even more preferably 4 mass ppm or more, and is 3000 mass ppm or less, preferably 2500 mass ppm or less, more preferably 2000 mass ppm or less, even more preferably 1000 mass ppm or less, even more preferably 100 mass ppm or less, even more preferably 50 mass ppm or less, even more preferably 20 mass ppm or less, and particularly preferably 10 mass ppm or less. By setting the content at or above the lower limit, the adhesive strength of the adhesive tends to be further improved. Furthermore, by setting the content at or below the upper limit, color change tends to be reduced. The total nitrogen element content is measured according to the description in the Examples below.

[0036] In the polybutylene phthalate resin used in this embodiment, the total sulfur element content is preferably 0.1 mass ppm or more, more preferably 1 mass ppm or more, even more preferably 2 mass ppm or more, even more preferably 4 mass ppm or more, and even more preferably 7 mass ppm or more, and is preferably 100 mass ppm or less, more preferably 80 mass ppm or less, even more preferably 60 mass ppm or less, even more preferably 40 mass ppm or less, even more preferably 25 mass ppm or less, even more preferably 20 mass ppm or less, and particularly preferably 15 mass ppm or less. By setting the content at or above the lower limit, the adhesive strength of the adhesive tends to be further improved. Furthermore, by setting the content at or below the upper limit, decomposition gas tends to be reduced. The total sulfur element content is measured according to the description in the examples below.

[0037] In the polybutylene phthalate resin used in this embodiment, the total amount of nitrogen element and sulfur element is, for example, 0.2 mass ppm or more, preferably 0.5 mass ppm or more, preferably 1 mass ppm or more, preferably 2 mass ppm or more, more preferably 5 mass ppm or more, even more preferably 10 mass ppm or more, and even more preferably 12 mass ppm or more. It is also preferably 120 mass ppm or less, more preferably 100 mass ppm or less, even more preferably 60 mass ppm or less, even more preferably 40 mass ppm or less, even more preferably 30 mass ppm or less, even more preferably 25 mass ppm or less, and particularly preferably 20 mass ppm or less. By setting it to the lower limit or more, the adhesive strength of the adhesive tends to be further improved. Furthermore, by setting it to the upper limit or less, decomposition gas or color change tends to be reduced.

[0038] To obtain such polybutylene terephthalate resins with high total nitrogen and sulfur content, a nitrogen source or a sulfur source (such as nitrogen or sulfur themselves, or a resin additive containing nitrogen or sulfur) may be blended into virgin polybutylene terephthalate resin, or recycled polybutylene terephthalate resin may be used. Recycled polybutylene terephthalate resins contain residual resin additives such as lubricants, release agents, and antioxidants, and the nitrogen and sulfur sources derived from these can be effectively utilized. In particular, in this embodiment, polybutylene terephthalate resins obtained from recycled connector parts, etc., are preferred because they often have a total nitrogen content within the desired range.

[0039] The intrinsic viscosity of the polybutylene terephthalate resin is preferably 0.60 dL / g or more, more preferably 0.70 dL / g or more, even more preferably 0.75 dL / g or more, even more preferably 0.80 dL / g or more, and even more preferably 0.85 dL / g or more. By setting the intrinsic viscosity at or above the lower limit, deterioration of physical properties such as strength tends to be effectively suppressed. Furthermore, the intrinsic viscosity of the polybutylene terephthalate resin is preferably 1.30 dL / g or less, more preferably 1.10 dL / g or less, even more preferably 1.00 dL / g or less, and even more preferably 0.90 dL / g or less. By setting the intrinsic viscosity at or below the upper limit, deterioration of fluidity tends to be effectively suppressed. In this embodiment, two or more polybutylene terephthalate resins having different intrinsic viscosities may be used. For example, a polybutylene terephthalate resin having an intrinsic viscosity of 0.60 to 0.75 dL / g and a polybutylene terephthalate resin having an intrinsic viscosity of more than 0.75 dL / g but not more than 0.95 dL / g may be blended in a mass ratio of 1 to 10:99 to 90. This composition tends to result in a higher deflection temperature under load of the resulting molded article. The intrinsic viscosity is measured as described in the Examples section below.

[0040] In the resin composition of this embodiment, the terminal carboxyl group concentration (acid value) of the polybutylene terephthalate resin is preferably 100 μmol / g or less (μeq / g), more preferably 80 μmol / g or less, more preferably 70 μmol / g or less, even more preferably 60 μmol / g or less, even more preferably 40 μmol / g or less, even more preferably 30 μmol / g or less, and preferably 10 μmol / g or more, more preferably 20 μmol / g or more, even more preferably 25 μmol / g or more, and even more preferably 27 μmol / g or more. By setting the acid value to be equal to or less than the upper limit, excellent hydrolysis resistance tends to be achieved. Furthermore, by setting the acid value to be equal to or greater than the lower limit, adhesive strength to adhesives tends to be further improved. When the resin composition of this embodiment contains two or more polybutylene terephthalate resins, the terminal carboxyl group concentration of the mixture is preferably within the above range. The terminal carboxyl group concentration of the polybutylene terephthalate resin is measured as described in the Examples below. A polybutylene terephthalate resin having such a terminal carboxyl group concentration can be obtained by, for example, subjecting the resin to a thermal history of a temperature equal to or higher than the melting point, such as by melt-kneading.

[0041] In the resin composition of this embodiment, the terminal hydroxy group concentration of the polybutylene terephthalate resin is preferably 110 μmol / g or less, more preferably 100 μmol / g or less, and even more preferably 95 μmol / g or less, and is preferably 30 μmol / g or more, more preferably 35 μmol / g or more, even more preferably 40 μmol / g or more, and even more preferably 50 μmol / g or more. By setting the concentration below the upper limit, transesterification reactions are suppressed during melt-kneading with other resins such as polycarbonate, and the molding cycle is shortened. Furthermore, by setting the concentration above the lower limit, adhesive strength to adhesives tends to be further improved.

[0042] When the resin composition of this embodiment contains two or more polybutylene terephthalate resins, the terminal hydroxyl group concentration of the mixture is preferably within the above range. The terminal hydroxyl group concentration of the polybutylene terephthalate resin is measured according to the description in the Examples below. Polybutylene terephthalate resins having such a terminal hydroxyl group concentration can be obtained by, for example, applying a thermal history above the melting point, such as melt-kneading.

[0043] The terminal vinyl group concentration of the polybutylene terephthalate resin is preferably 50 μmol / g or less, more preferably 15 μmol / g or less, even more preferably 12 μmol / g or less, even more preferably 10 μmol / g or less, even more preferably 8 μmol / g or less, and preferably 1 μmol / g or more, more preferably 2 μmol / g or more, and even more preferably 3 μmol / g or more. By setting the terminal vinyl group concentration at or below the upper limit, the terminal hydroxyl group concentration and terminal carboxyl group concentration become relatively high, which tends to further improve adhesion to epoxy adhesives. On the other hand, by setting the terminal vinyl group concentration at or above the lower limit, the terminal hydroxyl group concentration and terminal carboxyl group concentration become relatively low, which tends to suppress reactivity with other resins such as polycarbonate and epoxy resin, reduce the thickening effect, and improve fluidity. When the resin composition of this embodiment contains two or more polybutylene terephthalate resins, it is preferable that the terminal vinyl group concentration of the mixture be within the above range. The terminal vinyl group concentration of the polybutylene terephthalate resin is measured as described in the Examples below. A polybutylene terephthalate resin having such a terminal vinyl group concentration can be obtained by increasing the number of times the polybutylene terephthalate resin is subjected to heat history, for example, by increasing the number of times it is melt-kneaded.

[0044] The polybutylene terephthalate resin used in the resin composition of the present embodiment is a polyester resin having a structure in which terephthalic acid units and 1,4-butanediol units are ester-bonded, and includes, in addition to polybutylene terephthalate resin (homopolymer), polybutylene terephthalate copolymers containing other copolymerization components other than terephthalic acid units and 1,4-butanediol units, and mixtures of homopolymers and polybutylene terephthalate copolymers.

[0045] The polybutylene terephthalate resin may contain one or more dicarboxylic acid units other than terephthalic acid. Specific examples of the other dicarboxylic acids include aromatic dicarboxylic acids such as isophthalic acid, orthophthalic acid, 1,5-naphthalenedicarboxylic acid, 2,5-naphthalenedicarboxylic acid, 2,6-naphthalenedicarboxylic acid, biphenyl-2,2'-dicarboxylic acid, biphenyl-3,3'-dicarboxylic acid, biphenyl-4,4'-dicarboxylic acid, bis(4,4'-carboxyphenyl)methane, anthracenedicarboxylic acid, and 4,4'-diphenyletherdicarboxylic acid, alicyclic dicarboxylic acids such as 1,4-cyclohexanedicarboxylic acid and 4,4'-dicyclohexyldicarboxylic acid, and aliphatic dicarboxylic acids such as adipic acid, sebacic acid, azelaic acid, and dimer acid. In the polybutylene terephthalate resin used in the present embodiment, terephthalic acid units preferably account for 80 mol % or more of all dicarboxylic acid units, more preferably 90 mol % or more, even more preferably 95 mol % or more, and may even account for 99 mol % or more.

[0046] The diol unit may contain one or more other diol units in addition to 1,4-butanediol. Specific examples of other diol units include aliphatic or alicyclic diols having 2 to 20 carbon atoms, bisphenol derivatives, and the like. Specific examples include ethylene glycol, propylene glycol, 1,5-pentanediol, 1,6-hexanediol, neopentyl glycol, decamethylene glycol, cyclohexanedimethanol, 4,4'-dicyclohexylhydroxymethane, 4,4'-dicyclohexylhydroxypropane, and ethylene oxide addition diol of bisphenol A. In addition to the above-mentioned bifunctional monomers, small amounts of trifunctional monomers such as trimellitic acid, trimesic acid, pyromellitic acid, pentaerythritol, and trimethylolpropane can also be used in combination to introduce a branched structure, or monofunctional compounds such as fatty acids can be used in combination to adjust the molecular weight. In the polybutylene terephthalate resin used in the present embodiment, 1,4-butanediol units preferably account for 80 mol % or more of all diol units, more preferably 90 mol % or more, even more preferably 95 mol % or more, and may even account for 99 mol % or more.

[0047] As described above, the polybutylene terephthalate resin is preferably a polybutylene terephthalate homopolymer obtained by polycondensation of terephthalic acid and 1,4-butanediol. Alternatively, the polybutylene terephthalate copolymer may contain, as the carboxylic acid unit, one or more dicarboxylic acids other than the terephthalic acid and / or, as the diol unit, one or more diols other than the 1,4-butanediol. When the polybutylene terephthalate resin is a polybutylene terephthalate resin modified by copolymerization, specific preferred copolymers include polyester ether resins copolymerized with polyalkylene glycols, particularly polytetramethylene glycol, dimer acid-copolymerized polybutylene terephthalate resins, and isophthalic acid-copolymerized polybutylene terephthalate resins. Of these, polyester ether resins copolymerized with polytetramethylene glycol are preferred. When the polybutylene terephthalate resin is a copolymer, the copolymerization amount is 1 mol% or more but less than 50 mol% of the total units of the polybutylene terephthalate resin. In particular, the copolymerization amount is preferably 2 mol % or more but less than 50 mol %, more preferably 3 to 40 mol %, and even more preferably 5 to 20 mol %. By setting the copolymerization ratio in this range, molded articles having a small mold shrinkage rate and high impact resistance can be obtained, which is preferable.

[0048] The polybutylene terephthalate resin used in this embodiment preferably has a high degree of dispersion. A high degree of dispersion increases the amount of terminal groups (particularly the amount of terminal hydroxyl groups and / or the amount of terminal carboxyl groups) in the polybutylene terephthalate resin, thereby further improving adhesion to an epoxy adhesive.

[0049] The polybutylene terephthalate resin preferably has an Mw / Mn of 2.1 or more, more preferably 2.2 or more, and even more preferably 2.3 or more, and preferably 3.5 or less, more preferably 3.0 or less, even more preferably 2.7 or less, even more preferably 2.6 or less, and even more preferably 2.5 or less. By setting the Mw / Mn at or above the lower limit, the adhesive strength to epoxy adhesives tends to be further improved. By setting the Mw / Mn at or below the upper limit, the transesterification suppression effect and mechanical strength tend to be further improved. Such a polybutylene terephthalate resin with a high degree of dispersion can be obtained by increasing the number of times the polybutylene terephthalate resin is subjected to heat history, for example, by increasing the number of times it is melt-kneaded, or by blending two or more polybutylene terephthalate resins with different average molecular weights.

[0050] The number average molecular weight (Mn) of the polybutylene terephthalate resin used in this embodiment is preferably 2500 or more, more preferably 3000 or more, even more preferably 3500 or more, even more preferably 3700 or more, even more preferably 4000 or more, and preferably 20000 or less, more preferably 18000 or less, even more preferably 14000 or less, even more preferably 10000 or less, and even more preferably 6000 or less. By setting it to be equal to or greater than the lower limit, the mechanical strength tends to be excellent. On the other hand, by setting it to be equal to or less than the upper limit, the fluidity of the resin tends to be improved.

[0051] The weight average molecular weight (Mw) of the polybutylene terephthalate resin used in this embodiment is preferably 5,000 or more, more preferably 6,000 or more, even more preferably 7,000 or more, even more preferably 8,000 or more, and even more preferably 9,500 or more, and is preferably 40,000 or less, more preferably 35,000 or less, even more preferably 30,000 or less, even more preferably 25,000 or less, and even more preferably 20,000 or less. By making it equal to or greater than the lower limit, the mechanical strength tends to be further improved. On the other hand, by making it equal to or less than the upper limit, the fluidity of the resin tends to be improved.

[0052] The number average molecular weight and weight average molecular weight of the polybutylene terephthalate resin are measured according to the description in the Examples section below.

[0053] The melting point (Tm) of the polybutylene terephthalate resin used in this embodiment, measured according to DSC, is preferably 200°C or higher, more preferably 205°C or higher, even more preferably 210°C or higher, even more preferably 215°C or higher, and even more preferably 220°C or higher, and is preferably 280°C or lower, more preferably 270°C or lower, even more preferably 260°C or lower, even more preferably 255°C or lower, and even more preferably 240°C or lower. By setting the melting point at or above the lower limit, heat resistance tends to be further improved. Furthermore, by setting the melting point at or below the upper limit, molding cycle tends to be further improved. When the resin composition of this embodiment contains two or more polyalkylene terephthalate resins, the melting point is the melting point of the mixture. When multiple melting point peaks are detected, it is sufficient that at least one of the multiple melting points falls within the range of not less than the lower limit and not more than the upper limit. However, it is preferable that the component with the highest content among the multiple melting points falls within the range of not less than the lower limit and not more than the upper limit, and it is more preferable that all of the multiple melting points fall within the range of not less than the lower limit and not more than the upper limit.

[0054] The crystallization temperature (Tc) of the polybutylene terephthalate resin used in this embodiment, measured according to DSC, is preferably 130°C or higher, more preferably 145°C or higher, even more preferably 160°C or higher, even more preferably 175°C or higher, even more preferably 190°C or higher, and preferably 240°C or lower, more preferably 230°C or lower, even more preferably 220°C or lower, even more preferably 210°C or lower, and even more preferably 200°C or lower. By setting the crystallization temperature at or above the lower limit, the solidification rate tends to be improved and the molding cycle tends to be further improved. Furthermore, by setting the crystallization temperature at or below the upper limit, the appearance of the molded article tends to be improved. When the resin composition of this embodiment contains two or more polyalkylene terephthalate resins, the crystallization temperature is the crystallization temperature of the mixture. When multiple crystallization temperature peaks are detected, it is sufficient that at least one of the multiple crystallization temperatures is within the range of not less than the lower limit and not more than the upper limit, but it is preferable that the component with the highest content among the multiple crystallization temperatures is within the range of not less than the lower limit and not more than the upper limit, and it is more preferable that all of the multiple crystallization temperatures are within the range of not less than the lower limit and not more than the upper limit. The Tm and Tc of the polyalkylene terephthalate resin are measured according to the description in the Examples below.

[0055] In particular, the polybutylene terephthalate resin used in this embodiment has dicarboxylic acid units and diol units, and preferably 80 mol% or more (preferably 90 mol% or more, more preferably 95 mol% or more, and even more preferably 99 mol% or more) of all dicarboxylic acid units are terephthalic acid units derived from fossil resources, and 80 mol% or more (preferably 90 mol% or more, more preferably 95 mol% or more, and even more preferably 99 mol% or more) of all diol units are 1,4-butanediol units derived from fossil resources. Furthermore, the polybutylene terephthalate resin used in this embodiment is preferably not a bio-based polybutylene terephthalate resin. An example of a bio-based polybutylene terephthalate resin is a polybutylene terephthalate resin in which 10% by mass or more, or even 30% by mass or more, or 90% by mass or less, or even 60% by mass or less of the total amount of dicarboxylic acids and diols used as raw materials for the polybutylene terephthalate resin are bio-based raw materials.

[0056] The polybutylene terephthalate resin used in this embodiment may be a recycled product. Examples of recycled polybutylene terephthalate resin include those obtained by material recycling, in which molded products of recovered used polybutylene terephthalate resin are crushed, cleaned, and reused, and those obtained by chemical recycling (chemical decomposition). In this embodiment, it is preferable to include polybutylene terephthalate resin derived from material recycling. Polybutylene terephthalate resin derived from material recycling may be contaminated with alkaline components during use as a product or during the cleaning process during recycling. It is presumed that the inclusion of such alkaline components in the polybutylene terephthalate resin reduces the titanium catalytic activity of the polybutylene terephthalate resin. In this embodiment, recycled polybutylene terephthalate resin that has undergone a large number of thermal cycles can be used. Examples of thermal cycles include melt-kneading and thermoforming, such as injection molding and extrusion molding. In this embodiment, a polybutylene terephthalate resin with a thermal cycle of 3 to 10 cycles is exemplified. Examples of such recycled products include connectors, home appliances, toothbrushes, fibers, miscellaneous goods, automobile parts, films, tubes, and other extruded parts.

[0057] Polybutylene terephthalate resin, especially recycled polybutylene terephthalate resin, may contain metal elements as impurities, which may come from the reactor or cutters used during pulverization or pelletization.

[0058] The amount of iron element in the polybutylene terephthalate resin used in this embodiment is preferably 0.1 μg / g or more, and is preferably 100 μg / g or less, more preferably 70 μg / g or less, even more preferably 50 μg / g or less, still more preferably 10 μg / g or less, and even more preferably 5 μg / g or less.

[0059] The amount of aluminum element in the polybutylene terephthalate resin used in this embodiment is preferably 0.1 μg / g or more, and preferably 100 μg / g or less, more preferably 70 μg / g or less, even more preferably 50 μg / g or less, still more preferably 10 μg / g or less, and even more preferably 5 μg / g or less. The amounts of iron element and aluminum element in the polybutylene terephthalate resin are measured according to the method described in the Examples below.

[0060] The content of the polybutylene terephthalate resin in the resin composition of this embodiment is preferably 30% by mass or more, more preferably 35% by mass or more, even more preferably 40% by mass or more, and even more preferably 45% by mass or more, based on 100% by mass of the resin composition. It is also preferably 85% by mass or less, more preferably 80% by mass or less, and even more preferably 75% by mass or less. Depending on the application, it is preferably 60% by mass or less, more preferably 55% by mass or less, and even more preferably 50% by mass or less. By setting it to the lower limit or more, the heat resistance of the obtained molded article tends to be further improved. Furthermore, by setting it to the upper limit or less, the shrinkage rate of the obtained molded article tends to be small. The resin composition of this embodiment may contain only one type of polybutylene terephthalate resin, or may contain two or more types. When two or more types are contained, it is preferable that the total amount is within the above range.

[0061] <Amorphous Thermoplastic Resin Having a Carbonate Bond and / or an Ester Bond> The resin composition of this embodiment contains an amorphous thermoplastic resin having a carbonate bond and / or an ester bond. By incorporating the amorphous resin, the crystallization temperature (Tc) of the resulting resin composition during cooling can be increased. In particular, in the resin composition of this embodiment, even when an amorphous thermoplastic resin having a carbonate bond and / or an ester bond is incorporated into a polybutylene terephthalate resin, transesterification can be effectively suppressed. Examples of amorphous thermoplastic resins having a carbonate bond and / or an ester bond include polycarbonate resin, polyarylate resin, isophthalic acid copolymerized polyethylene terephthalate resin, and cyclohexanedimethanol copolymerized polyethylene terephthalate resin, with polycarbonate resin being preferred.

[0062] Polycarbonate resins are thermoplastic polymers or copolymers which may be branched and are obtained by reacting a dihydroxy compound or a small amount of a polyhydroxy compound with phosgene or a carbonic acid diester.

[0063] The dihydroxy compound used as the raw material is preferably an aromatic dihydroxy compound. Specific examples include 2,2-bis(4-hydroxyphenyl)propane (i.e., bisphenol A), 4,4'-isopropylidenebis(2-methylphenol) (i.e., bisphenol C), tetramethylbisphenol A, bis(4-hydroxyphenyl)-p-diisopropylbenzene, hydroquinone, resorcinol, and 4,4-dihydroxydiphenyl, with bisphenol A being preferred. Compounds in which one or more tetraalkylphosphonium sulfonates are bonded to the above aromatic dihydroxy compounds can also be used. The polycarbonate resin used in this embodiment preferably contains 90% by mass or more (preferably 95% by mass or more) of its structural units derived from an aromatic hydroxy compound, more preferably structural units derived from bisphenol A and / or bisphenol C, and even more preferably structural units derived from bisphenol A.

[0064] To adjust the molecular weight of the polycarbonate resin, a monovalent aromatic hydroxy compound may be used, such as m- and p-methylphenol, m- and p-propylphenol, p-tert-butylphenol, and p-long-chain alkyl-substituted phenol.

[0065] The viscosity average molecular weight (Mv) of the polycarbonate resin is preferably 10,000 or more, more preferably 12,000 or more, even more preferably 13,000 or more, and particularly preferably more than 14,000. If a viscosity average molecular weight lower than 10,000 is used, the resulting resin composition tends to have low mechanical strength such as impact resistance. Furthermore, Mv is preferably 60,000 or less, more preferably 40,000 or less, even more preferably 35,000 or less, even more preferably 30,000 or less, and may be 25,000 or less, or 20,000 or less. If it is higher than 60,000, the fluidity of the resin composition may be poor and moldability may be impaired.

[0066] In the present invention, the viscosity average molecular weight (Mv) of the polycarbonate resin is a value calculated from the intrinsic viscosity ([η]) obtained by measuring the viscosity of a methylene chloride solution of the polycarbonate resin at 25°C using an Ubbelohde viscometer, and then using the following Schnell viscosity formula: [η] = 1.23 × 10 －４ Mv ０．８３

[0067] The melt mass flow rate (MFR) of the polycarbonate resin, measured in accordance with JIS K7210 (temperature 300°C, load 1.20 kgf), is preferably 3 g / 10 min or more, more preferably 6 g / 10 min or more, and is preferably 100 g / 10 min or less, more preferably 70 g / 10 min or less. When the MFR is in the above range, the effects of the present invention tend to be more effectively exhibited.

[0068] The melt volume rate (MVR) of polycarbonate resin measured in accordance with JIS K7210 (temperature 300°C, load 1.20 kgf) is 0.5 to 20 cm ３g / 10 min, and 1 to 10 cm ３ When the MVR is in the above range, the effects of the present invention tend to be more effectively exhibited.

[0069] The method for producing the polycarbonate resin is not particularly limited, and polycarbonate resins produced by either the phosgene method (interfacial polymerization method) or the melt method (ester interchange method) can be used. Also preferred is a polycarbonate resin produced by the melt method and then subjected to post-treatment to adjust the amount of terminal OH groups.

[0070] The polycarbonate resin may be a recycled polycarbonate resin. Examples of recycled polycarbonate resin include those obtained by material recycling, in which recovered used polycarbonate resin molded articles are crushed, washed, and reused; those obtained by chemical recycling (chemical decomposition method); and those obtained by mechanical recycling. Chemical recycling involves chemically decomposing recovered used polycarbonate resin molded articles to return them to their raw material level and resynthesize the polycarbonate resin. On the other hand, mechanical recycling is a method that enables more reliable removal of dirt from polycarbonate resin molded articles than material recycling by performing alkaline washing more rigorously than in the above-mentioned material recycling or by vacuum drying at high temperatures. For example, recycled polycarbonate resin is obtained by removing foreign matter from used polycarbonate resin molded articles, crushing and washing them, and then pelletizing them using an extruder.

[0071] The content of the amorphous thermoplastic resin having a carbonate bond and / or an ester bond in the resin composition of this embodiment is preferably 5 parts by mass or more, more preferably 10 parts by mass or more, even more preferably 15 parts by mass or more, even more preferably 20 parts by mass or more, even more preferably 25 parts by mass or more, relative to 100 parts by mass of the total of the polybutylene terephthalate resin and the amorphous thermoplastic resin having a carbonate bond and / or an ester bond. It is also preferably 55 parts by mass or less, more preferably 50 parts by mass or less, even more preferably 45 parts by mass or less, even more preferably 40 parts by mass or less, and even more preferably 35 parts by mass or less. By setting the content at or above the lower limit, the shrinkage rate of the resulting molded article tends to be reduced. Furthermore, by setting the content at or below the upper limit, the heat resistance of the resulting molded article tends to be further improved. The resin composition of this embodiment may contain only one type of amorphous thermoplastic resin having a carbonate bond and / or an ester bond, or may contain two or more types. When two or more types are contained, the total amount is preferably within the above range.

[0072] The content of the polycarbonate resin in the resin composition of this embodiment is preferably 5 parts by mass or more, more preferably 7 parts by mass or more, and even more preferably 10 parts by mass or more, per 100 parts by mass of the total of the polybutylene terephthalate resin and the polystyrene-based resin, and is preferably 25 parts by mass or less, and more preferably 20 parts by mass or less. By making the content equal to or greater than the lower limit, the mechanical properties such as tensile strength of the molded article tend to be further improved. Furthermore, by making the content equal to or less than the upper limit, the heat resistance of the molded article tends to be further improved. The resin composition of this embodiment may contain only one type of polycarbonate resin, or may contain two or more types. When two or more types are contained, it is preferable that the total amount be within the above range.

[0073] <Polystyrene-based Resin> The resin composition of this embodiment contains a polystyrene-based resin. By including a polystyrene-based resin, it is possible to effectively suppress warpage of the resulting molded article. The polystyrene-based resin may be a crystalline resin or an amorphous resin. Examples of the polystyrene-based resin in this embodiment include a homopolymer of a styrene-based monomer, a copolymer of a styrene-based monomer and a monomer copolymerizable with the styrene-based monomer, and the like. In the copolymer of a styrene-based monomer and a copolymerizable monomer, the styrene-based monomer preferably accounts for 50% by mass or more of the total monomers, more preferably 60% by mass or more, and preferably 100% by mass or less.

[0074] The styrene-based monomer refers to styrene and styrene having a substituent, and examples thereof include styrene, α-methylstyrene, p-methylstyrene, vinylxylene, ethylstyrene, dimethylstyrene, p-tert-butylstyrene, vinylnaphthalene, methoxystyrene, monobromostyrene, dibromostyrene, fluorostyrene, tribromostyrene, etc., with styrene and α-methylstyrene being more preferred, and styrene being particularly preferred. Furthermore, among the monomers constituting the polystyrene-based resin, examples of monomers other than styrene-based monomers include (meth)acrylic acid ester-based monomers, maleimide-based monomers such as maleimide, N-methylmaleimide, and N-phenylmaleimide, α,β-unsaturated carboxylic acids and anhydrides thereof such as acrylic acid, methacrylic acid, maleic acid, maleic anhydride, phthalic acid, and itaconic acid, and rubbers such as butadiene.

[0075] The polystyrene resin used in this embodiment may contain a rubber-reinforced polystyrene resin. Specific examples of the rubber-reinforced polystyrene resin include acrylonitrile-styrene copolymer (AS resin), high impact polystyrene resin (HIPS), acrylonitrile-butadiene-styrene copolymer (ABS resin), acrylonitrile-acrylic rubber-styrene copolymer (AAS resin), acrylonitrile-styrene-acrylic rubber copolymer (ASA resin), acrylonitrile-ethylene propylene rubber-styrene copolymer (AES resin), and styrene-IPN type rubber copolymer.

[0076] The polystyrene resin used in this embodiment preferably contains a styrene-maleic acid polymer (preferably a styrene-maleic anhydride polymer). The styrene-maleic acid polymer acts as a compatibilizer between the polybutylene terephthalate resin and the polystyrene resin and / or rubber-reinforced polystyrene resin. As a result, the strength of the resulting molded article can be increased.

[0077] In this embodiment, the polystyrene resin preferably includes at least one selected from polystyrene resin (GPPS), acrylonitrile-styrene copolymer (AS resin), high-impact polystyrene resin (HIPS), acrylonitrile-butadiene-styrene copolymer (ABS resin), acrylonitrile-acrylic rubber-styrene copolymer (AAS resin), acrylonitrile-styrene-acrylic rubber copolymer (ASA resin), and acrylonitrile-ethylene propylene rubber-styrene copolymer (AES resin), and more preferably includes high-impact polystyrene resin (HIPS). Furthermore, from the viewpoint of heat resistance, polystyrene resin (GPPS) and acrylonitrile-styrene copolymer (AS resin) are more preferable, and polystyrene resin (GPPS) is even more preferable.

[0078] The polystyrene resin used in this embodiment may include recycled products. Examples of recycled polystyrene resins include those obtained by material recycling in which scraps or rejected products of molded products, or recovered used polystyrene resin molded products are crushed, washed, and reused, and those obtained by chemical recycling (chemical decomposition method).

[0079] The content of the polystyrene-based resin in the resin composition of this embodiment is preferably 30 parts by mass or more, more preferably 35 parts by mass or more, even more preferably 40 parts by mass or more, even more preferably 45 parts by mass or more, and even more preferably more than 50 parts by mass, relative to 100 parts by mass of the total of the polybutylene terephthalate resin and the polystyrene-based resin. It is also preferably 70 parts by mass or less, more preferably 65 parts by mass or less, and even more preferably 60 parts by mass or less. By setting the content at or above the lower limit, the shrinkage rate of the molded article tends to be reduced. Furthermore, by setting the content at or below the upper limit, the heat resistance of the molded article tends to be further improved. The resin composition of this embodiment may contain only one type of polystyrene-based resin, or may contain two or more types. When two or more types are contained, the total amount is preferably within the above range.

[0080] <Other Thermoplastic Resins> The resin composition of this embodiment may contain a thermoplastic resin other than those described above. Such a thermoplastic resin may be a crystalline thermoplastic resin or an amorphous thermoplastic resin, and is preferably an amorphous thermoplastic resin. Examples of crystalline thermoplastic resins include polyethylene terephthalate resin, polyethylene resin, polypropylene resin, polyamide resin, polyacetal resin, etc., and polyethylene terephthalate resin is preferred.

[0081] A first example of a preferred blend form of thermoplastic resins in this embodiment is a resin composition in which polybutylene terephthalate resin and polycarbonate resin account for 90% by mass or more (preferably 95% by mass or more, and preferably 100% by mass or less) of the thermoplastic resins contained in the resin composition. A second example of a preferred blend form of thermoplastic resins in this embodiment is a resin composition in which polybutylene terephthalate resin, polycarbonate resin, and polystyrene resin account for 90% by mass or more (preferably 95% by mass or more, and preferably 100% by mass or less) of the thermoplastic resins contained in the resin composition.

[0082] A third example of a preferred blend form of thermoplastic resins in this embodiment is a resin composition in which polybutylene terephthalate resin and polystyrene resin account for 90% by mass or more (preferably 95% by mass or more, and preferably 100% by mass or less) of the thermoplastic resins contained in the resin composition. A fourth example of a preferred blend form of thermoplastic resins in this embodiment is a resin composition in which polybutylene terephthalate resin, polycarbonate resin, and polystyrene resin account for 90% by mass or more (preferably 95% by mass or more, and preferably 100% by mass or less) of the thermoplastic resins contained in the resin composition.

[0083] <Reactive Compound> The resin composition of this embodiment may contain a reactive compound. By including a reactive compound, the mechanical strength of the molded article is improved, and a resin composition with excellent hydrolysis resistance is obtained. Furthermore, in the resin composition of this embodiment, even when a reactive compound is blended into the resin composition, thickening of the resin composition tends to be effectively suppressed. As a result, the transparency of the obtained molded article also tends to be maintained at a high level. The reactive compound used in this embodiment preferably contains at least one selected from the group consisting of a compound having an epoxy group, a carbodiimide compound, a compound having an oxazoline group, and a compound having an oxazine group, and more preferably contains a compound having an epoxy group. In particular, the resin composition of this embodiment may contain an epoxy compound. By including an epoxy compound, the hydrolysis resistance of the obtained molded article tends to be improved, and adhesion to an epoxy-based adhesive tends to be improved, which is preferable.

[0084] <<Compound Having Epoxy Group (Epoxy Resin)>> The compound having an epoxy group is a compound having one or more epoxy groups in one molecule, and examples thereof include a glycidyl compound, an aromatic ring-containing compound having an epoxy group, and an alicyclic compound having an epoxy group, and it is preferable that the compound contains at least an aromatic ring-containing compound having an epoxy group.

[0085] The epoxy compound may be a monofunctional epoxy compound or a polyfunctional epoxy compound, but a polyfunctional epoxy compound is preferred. Specific examples of the compound having an epoxy group include bisphenol A type epoxy compounds (including bisphenol A diglycidyl ether), bisphenol F type epoxy compounds (including bisphenol F diglycidyl ether), biphenyl type epoxy compounds (including bis(glycidyloxy)biphenyl), resorcinol type epoxy compounds (including resorcinol diglycidyl ether), novolac type epoxy compounds, epoxy compounds having an aromatic ring such as benzoic acid glycidyl ester, terephthalic acid diglycidyl ester, orthophthalic acid diglycidyl ester, methyl glycidyl ether, butyl glycidyl ether, 2-ethylhexyl glycidyl ether, and decyl glycidyl ether. Examples of suitable epoxy compounds include (di)glycidyl ethers such as stearyl glycidyl ether, phenyl glycidyl ether, butylphenyl glycidyl ether, allyl glycidyl ether, neopentyl glycol diglycidyl ether, ethylene glycol diglycidyl ether, glycerin diglycidyl ether, and propylene glycol diglycidyl ether; paraffinic (e.g., saturated fatty acid) or olefinic (e.g., unsaturated fatty acid) (di)glycidyl esters such as sorbic acid glycidyl ester, adipic acid diglycidyl ester, epoxidized linseed oil, and epoxidized soybean oil; and alicyclic epoxy compounds such as vinylcyclohexene dioxide and dicyclopentadiene oxide. Among these, styrene-acrylic copolymers containing glycidyl groups in their side chains, bisphenol A-type epoxy compounds, novolac-type epoxy compounds, bisphenol F-type epoxy compounds, and biphenyl-type epoxy compounds are preferred, with bisphenol A-type epoxy compounds being more preferred. Furthermore, the epoxy compound may be a copolymer containing a glycidyl group-containing compound as a constituent component. For example, a copolymer of a glycidyl ester of an α,β-unsaturated acid and one or more monomers selected from the group consisting of α-olefin, acrylic acid, acrylic acid ester, methacrylic acid, methacrylic acid ester, and styrene can be mentioned.Furthermore, the epoxy compound is preferably a copolymer of an epoxy group-containing monomer and a styrene-based monomer, and may also be a copolymer with other copolymerizable monomers. Examples of the styrene-based monomer constituting the copolymer of an epoxy group-containing monomer and a styrene-based monomer include glycidyl (meth)acrylate and glycidyl itaconate, with glycidyl methacrylate and glycidyl acrylate being preferred, and glycidyl methacrylate being particularly preferred. Examples of the styrene-based monomer include styrene, α-methylstyrene, p-methylstyrene, vinylxylene, ethylstyrene, dimethylstyrene, p-tert-butylstyrene, vinylnaphthalene, methoxystyrene, monobromostyrene, dibromostyrene, fluorostyrene, and tribromostyrene, with styrene and α-methylstyrene being more preferred, and styrene being particularly preferred. Specific examples of copolymers of epoxy group-containing monomers and styrene-based monomers include glycidyl (meth)acrylate-styrene copolymers and glycidyl (meth)acrylate-styrene-methyl (meth)acrylate, which tend to improve adhesion to epoxy-based adhesives and are therefore particularly preferred.

[0086] The epoxy equivalent of the epoxy compound used in this embodiment is preferably 100 g / eq or more, more preferably 150 g / eq or more, and is preferably 1000 g / eq or less, more preferably 300 g / eq or less, and even more preferably 250 g / eq or less. When the resin composition of this embodiment contains two or more epoxy compounds, the epoxy equivalent is the value (weighted average value) obtained by multiplying the epoxy equivalent of each epoxy compound by the mass fraction of each epoxy compound.

[0087] In addition to the above, the epoxy compounds can be found in paragraphs 0038 to 0050 of JP-A-2020-199755 and paragraph 0043 of JP-A-2020-125468, the contents of which are incorporated herein by reference.

[0088] The content of the reactive compound (preferably a compound having an epoxy group (epoxy resin)) in the resin composition of this embodiment is preferably 0.01 mass% or more, more preferably 0.05 mass% or more, and even more preferably 0.1 mass% or more, based on 100 mass% of the resin composition. By making the content equal to or greater than the lower limit, hydrolysis resistance tends to be further improved. Furthermore, the content of the reactive compound (preferably a compound having an epoxy group (epoxy resin)) in the resin composition is preferably 10.0 mass% or less, more preferably 5.0 mass% or less, even more preferably 3.0 mass% or less, and even more preferably 2.0 mass% or less. By making the content equal to or less than the upper limit, melt viscosity tends to be more stable and moldability tends to be improved. Furthermore, when the resin composition of this embodiment contains an epoxy compound, the content thereof is preferably 0.01 parts by mass or more, more preferably 0.05 parts by mass or more, based on 100 parts by mass of the polybutylene terephthalate resin. The upper limit of the content of the epoxy compound is preferably 15 parts by mass or less, more preferably 10 parts by mass or less, even more preferably 7.0 parts by mass or less, and even more preferably 2.0 parts by mass or less, relative to 100 parts by mass of the polybutylene terephthalate resin. The resin composition of this embodiment may contain only one type of reactive compound, or may contain two or more types. When two or more types are contained, it is preferable that the total amount is within the above range.

[0089] <Stabilizer> The resin composition of this embodiment may contain a stabilizer. By containing a stabilizer, a resin composition or a molded article having excellent thermal stability can be obtained. The stabilizer preferably contains one or more compounds selected from the group consisting of thioether compounds, hindered phenol compounds, and phosphite compounds, and more preferably contains one or more compounds selected from the group consisting of hindered phenol compounds and phosphite compounds.

[0090] As the thioether-based compound, any conventionally known sulfur-containing compound can be used, and among them, thioethers are preferred. By including the thioether-based compound in the resin composition of the present embodiment, the appearance of the molded article tends to be improved and color change tends to be suppressed. Specific examples include didodecylthiodipropionate, ditetradecylthiodipropionate, dioctadecylthiodipropionate, pentaerythritol tetrakis(3-dodecylthiopropionate), 2,2-bis{[3-(dodecylthio)-1-oxopropoxy]methyl}propane-1,3-diylbis[3-(dodecylthio)propionate], thiobis(N-phenyl-β-naphthylamine), 2-mercaptobenzothiazole, 2-mercaptobenzimidazole, tetramethylthiuram monosulfide, tetramethylthiuram disulfide, nickel dibutyldithiocarbamate, nickel isopropyl xanthate, and trilauryl trithiophosphite. Among these, 2,2-bis{[3-(dodecylthio)-1-oxopropoxy]methyl}propane-1,3-diylbis[3-(dodecylthio)propionate] is preferred. Commercially available products include "Seenox 412S" manufactured by Shipro Chemical Co., Ltd. and "ADK STAB AO-412S" manufactured by ADEKA Corporation.

[0091] Examples of hindered phenol compounds include pentaerythritol tetrakis(3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate), octadecyl-3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate, thiodiethylenebis(3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate), pentaerythritol tetrakis(3-(3,5-di-neopentyl-4-hydroxyphenyl)propionate), and 1,3,5-trimethyl-2,4,6-tris(3,5-di-tert-butyl-4-hydroxybenzyl)benzene. Of these, pentaerythritol tetrakis(3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate) and octadecyl-3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate are preferred. Commercially available products include those manufactured by ADEKA Corporation under the trade names "ADK STAB AO-60" and "ADK STAB AO-330," those manufactured by EVERSPRING CHEMICAL under the trade name "EVERNOX-10," and those manufactured by BASF under the trade name "IRGANOX 1010."

[0092] The phosphite compound is preferably a compound represented by the formula: ２ O-P (OR ３ ) (OR ４ ) (wherein, R ２ , R ３ and R ４ are each a hydrogen atom, an alkyl group having 1 to 30 carbon atoms, or an aryl group having 6 to 30 carbon atoms, and R ２ , R ３ and R ４At least one of the groups is an aryl group having 6 to 30 carbon atoms. Examples of the phosphite compound include triphenyl phosphite, tris(nonylphenyl) phosphite, dilauryl hydrogen phosphite, triethyl phosphite, tridecyl phosphite, tris(2-ethylhexyl) phosphite, tris(tridecyl) phosphite, tristearyl phosphite, diphenyl monodecyl phosphite, monophenyl didecyl phosphite, diphenyl mono(tridecyl) phosphite, tetraphenyl dipropylene glycol diphosphite, tetraphenyl tetra(tridecyl)pentaerythritol tetraphosphite, hydrogenated bisphenol A phenol phosphite polymer, diphenyl hydrogen phosphite, 4,4'-butylidene-bis(3-methyl-6-tert-butylphenyl di(tridecyl) phosphite), tetra(tridecyl) 4,4'-isopropyl phosphate, tetra(tridecyl) ... propylidenediphenyl diphosphite, bis(tridecyl)pentaerythritol diphosphite, bis(nonylphenyl)pentaerythritol diphosphite, dilauryl pentaerythritol diphosphite, distearyl pentaerythritol diphosphite, tris(4-tert-butylphenyl)phosphite, tris(2,4-di-tert-butylphenyl)phosphite, hydrogenated bisphenol A pentaerythritol phosphite polymer, bis(2,4-di-tert-butylphenyl)pentaerythritol diphosphite, bis(2,6-di-tert-butyl-4-methylphenyl)pentaerythritol diphosphite, 2,2'-methylenebis(4,6-di-tert-butylphenyl)octyl phosphite, bis(2,4-dicumylphenyl)pentaerythritol diphosphite, and the like. Among these, bis(2,6-di-tert-butyl-4-methylphenyl)pentaerythritol diphosphite is preferred. Commercially available products include those manufactured by ADEKA Corporation under the trade names "ADEKA STAB PEP-36" and "AX-71."

[0093] Other examples of stabilizers include the following: the descriptions in paragraphs 0067 to 0075 of JP-A-2021-063196, the descriptions in paragraphs 0046 to 0057 of JP-A-2018-070722, the descriptions in paragraphs 0030 to 0037 of JP-A-2019-056035, and the descriptions in paragraphs 0066 to 0078 of WO 2017 / 038949. The contents of these descriptions are incorporated herein by reference.

[0094] The content of the stabilizer in the resin composition of this embodiment is, for example, 0.01 parts by mass or more, preferably 0.05 parts by mass or more, more preferably 0.1 parts by mass or more, and even more preferably 0.3 parts by mass or more, relative to 100 parts by mass of the thermoplastic resin contained in the resin composition. By setting the content at or above the lower limit, the effect of suppressing thermal degradation and oxidative degradation of the resin during melt-kneading, molding, and use as a molded product tends to be more improved, and discoloration of the resin tends to be more effectively suppressed. Furthermore, the upper limit of the stabilizer content is preferably 3.0 parts by mass or less, more preferably 2.0 parts by mass or less, and even more preferably 1.0 parts by mass or less, relative to 100 parts by mass of the polybutylene terephthalate resin and polyethylene terephthalate resin combined. Depending on the application, it may be 0.8 parts by mass or less, 0.6 parts by mass or less, 0.5 parts by mass or less, or 0.4 parts by mass or less. By setting the content at or below the upper limit, adverse effects on appearance and physical properties due to aggregation of additives such as stabilizers can be effectively suppressed.

[0095] An example of 100 parts by mass of the thermoplastic resin contained in the resin composition is a total of 100 parts by mass of polybutylene terephthalate resin and an amorphous thermoplastic resin having a carbonate bond and / or an ester bond. Another example of 100 parts by mass of the thermoplastic resin contained in the resin composition is a total of 100 parts by mass of polybutylene terephthalate resin and a polystyrene-based resin. Another example of 100 parts by mass of the thermoplastic resin contained in the resin composition is 100 parts by mass of polybutylene terephthalate resin. The resin composition of this embodiment may contain only one type of stabilizer, or may contain two or more types. When two or more types are contained, it is preferable that the total amount be in the above range.

[0096] <Inorganic Filler> The resin composition of this embodiment preferably further contains an inorganic filler. The inorganic filler is preferably a fibrous or scaly inorganic filler, more preferably glass fiber and / or glass flake. By including such an inorganic filler, the mechanical strength of the resulting molded article tends to be improved.

[0097] The inorganic filler that can be contained in the resin composition of this embodiment has the effect of improving the mechanical properties of the resulting resin composition when blended with the resin, and commonly used inorganic fillers for plastics can be used. Fibrous inorganic fillers such as glass fiber, carbon fiber, basalt fiber, wollastonite, and potassium titanate fiber are preferred. Granular or amorphous fillers such as calcium carbonate, titanium oxide, feldspar minerals, clay, organoclay, and glass beads; plate-like fillers such as talc; and scaly inorganic fillers such as glass flakes, mica, and graphite can also be used. Among these, glass fiber and / or glass flakes are preferred from the viewpoints of mechanical strength, rigidity, and heat resistance, and glass fiber is particularly preferred. Glass fiber with either a round or irregular cross-sectional shape can be used. It is more preferred to use inorganic fillers that have been surface-treated with a surface treatment agent such as a coupling agent. Glass fiber with a surface treatment agent attached is preferred because it has excellent durability, moist heat resistance, hydrolysis resistance, and heat shock resistance.

[0098] Any conventionally known surface treatment agent can be used, and specific preferred examples include silane coupling agents such as aminosilane-based, epoxysilane-based, allylsilane-based, and vinylsilane-based silane coupling agents. Of these, aminosilane-based surface treatment agents are preferred, and specific preferred examples include γ-aminopropyltriethoxysilane, γ-aminopropyltrimethoxysilane, and γ-(2-aminoethyl)aminopropyltrimethoxysilane.

[0099] Other preferred surface treatment agents include epoxy resin-based surface treatment agents such as novolac-type and bisphenol A-type epoxy resin-based surface treatment agents, with novolac-type epoxy resin-based surface treatment agents being particularly preferred. Silane-based surface treatment agents and epoxy resin-based surface treatment agents may be used alone or in combination, and a combination of both is also preferred. In this embodiment, glass fiber refers to a fibrous glass material. More specifically, a chopped shape is preferred, in which 1,000 to 10,000 glass fibers are bundled and cut to a predetermined length. In this embodiment, glass fibers preferably have a number-average fiber length of 0.5 to 10 mm, more preferably 1 to 5 mm. Using glass fibers with such a number-average fiber length can further improve mechanical strength. The number-average fiber length is calculated by randomly selecting glass fibers to be measured from an image obtained by optical microscope observation and measuring their long sides. The observation magnification is 20x, and the number of fibers measured is 1,000 or more. This roughly corresponds to the cut length. The cross section of the glass fiber may be any shape, such as a circle, an ellipse, an oval, a rectangle, a shape with semicircles on both short sides of a rectangle, or a cocoon shape, but a circle is preferred. Here, the term "circle" refers not only to a geometric circle but also to what is commonly referred to as a circle in the technical field of this embodiment. The lower limit of the number average fiber diameter of the glass fiber is preferably 4.0 μm or more, more preferably 4.5 μm or more, and even more preferably 5.0 μm or more. The upper limit of the number average fiber diameter of the glass fiber is preferably 15.0 μm or less, more preferably 14.0 μm or less. Using glass fibers having a number average fiber diameter within this range tends to produce molded products with superior mechanical strength. The number average fiber diameter of the glass fiber is calculated from the measured values ​​obtained by randomly selecting glass fibers to be measured for fiber diameter from an image obtained by electron microscope observation, measuring the fiber diameter near the center, and then calculating the measured value. The observation magnification is 1,000x, and the number of measurements is 1,000 or more. The number average fiber diameter of glass fibers having a cross section other than a circle is the number average fiber diameter when converted into a circle having the same area as the cross section.

[0100] The glass fiber may be a fiber obtained by melt spinning a commonly supplied glass such as E-glass (Electrical glass), C-glass (Chemical glass), A-glass (Alkali glass), S-glass (High strength glass), D-glass, R-glass, or alkali-resistant glass, but any glass fiber may be used without any particular limitation. In the present embodiment, it is preferable to include E-glass.

[0101] The glass fiber used in this embodiment is preferably surface-treated with a surface treatment agent such as a silane coupling agent, for example, γ-methacryloxypropyltrimethoxysilane, γ-glycidoxypropyltrimethoxysilane, or γ-aminopropyltriethoxysilane. The amount of the surface treatment agent attached is preferably 0.01 to 1 mass% of the glass fiber. Furthermore, if necessary, the glass fiber may be surface-treated with a lubricant such as a fatty acid amide compound or silicone oil, an antistatic agent such as a quaternary ammonium salt, a resin capable of forming a film, such as an epoxy resin or urethane resin, or a mixture of a resin capable of forming a film and a heat stabilizer.

[0102] Glass fibers are commercially available, and examples of commercially available products include T-286H, T-756H, T-127, and T-289H manufactured by Nippon Electric Glass Co., Ltd., DEFT2A manufactured by Owens Corning, HP3540 manufactured by PPG, and CSG3PA820 manufactured by Nitto Boseki Co., Ltd.

[0103] The content of the inorganic filler (preferably glass fiber) in the resin composition of this embodiment is preferably 10 parts by mass or more, more preferably 15 parts by mass or more, even more preferably 20 parts by mass or more, even more preferably 25 parts by mass or more, and even more preferably 30 parts by mass or more, relative to 100 parts by mass of the thermoplastic resin contained in the resin composition of this embodiment. By setting the content at or above the lower limit, the mechanical strength of the resulting molded product tends to be high. Furthermore, the upper limit of the content of the inorganic filler is preferably 150 parts by mass or less, more preferably 140 parts by mass or less, even more preferably 120 parts by mass or less, even more preferably 100 parts by mass or less, even more preferably 80 parts by mass or less, and depending on the application, preferably 70 parts by mass or less, more preferably 60 parts by mass or less, and even more preferably 50 parts by mass or less. By setting the content at or below the upper limit, the welding strength of the interface tends to be high.

[0104] An example of 100 parts by mass of the thermoplastic resin contained in the resin composition is a total of 100 parts by mass of polybutylene terephthalate resin and an amorphous thermoplastic resin having a carbonate bond and / or an ester bond. Another example of 100 parts by mass of the thermoplastic resin contained in the resin composition is a total of 100 parts by mass of polybutylene terephthalate resin and a polystyrene-based resin. Another example of 100 parts by mass of the thermoplastic resin contained in the resin composition is 100 parts by mass of polybutylene terephthalate resin. The resin composition of the present embodiment may contain only one type of stabilizer, or may contain two or more types. When two or more types are contained, it is preferable that the total amount be in the above range.

[0105] The content of the inorganic filler (preferably glass fiber) in the resin composition of this embodiment is, for example, 10% by mass or more, preferably 15% by mass or more, and depending on the application, etc., preferably 20% by mass or more, more preferably 25% by mass or more. The content of the inorganic filler (preferably glass fiber) is, for example, 60% by mass or less, preferably 55% by mass or less, and depending on the application, etc., preferably 45% by mass or less, more preferably 40% by mass or less, more preferably 38% by mass or less. The resin composition of this embodiment may contain only one type of inorganic filler (preferably glass fiber), or may contain two or more types. When two or more types are contained, it is preferable that the total amount is within the above range.

[0106] <Release Agent> The resin composition of the present embodiment preferably contains a release agent. A wide variety of known release agents can be used as the release agent, and examples thereof include aliphatic carboxylic acid amides, aliphatic carboxylic acids, esters of aliphatic carboxylic acids and alcohols, aliphatic hydrocarbon compounds having a number average molecular weight of 200 to 15,000, and polysiloxane-based silicone oils. Of these, aliphatic hydrocarbons having a number average molecular weight of 200 to 15,000 are preferred.

[0107] Examples of aliphatic carboxylic acid amides include compounds obtained by the dehydration reaction of higher aliphatic monocarboxylic acids and / or polybasic acids with diamines. Preferred higher aliphatic monocarboxylic acids include saturated aliphatic monocarboxylic acids and hydroxycarboxylic acids having 16 or more carbon atoms, such as palmitic acid, stearic acid, behenic acid, montanic acid, and 12-hydroxystearic acid. Examples of polybasic acids include aliphatic dicarboxylic acids such as malonic acid, succinic acid, adipic acid, sebacic acid, pimelic acid, and azelaic acid; aromatic dicarboxylic acids such as phthalic acid and terephthalic acid; and alicyclic dicarboxylic acids such as cyclohexanedicarboxylic acid and cyclohexylsuccinic acid. Examples of diamines include ethylenediamine, 1,3-diaminopropane, 1,4-diaminobutane, hexamethylenediamine, metaxylylenediamine, tolylenediamine, paraxylylenediamine, phenylenediamine, and isophoronediamine. As the carboxylic acid amide compound, a compound obtained by polycondensation of stearic acid, sebacic acid, and ethylenediamine is preferred, and a compound obtained by polycondensation of 2 moles of stearic acid, 1 mole of sebacic acid, and 2 moles of ethylenediamine is more preferred. In addition to bisamide compounds obtained by reacting a diamine with an aliphatic carboxylic acid, such as N,N'-methylenebisstearamide or N,N'-ethylenebisstearamide, dicarboxylic acid amide compounds such as N,N'-dioctadecylterephthalamide can also be suitably used.

[0108] Examples of aliphatic carboxylic acids include saturated or unsaturated aliphatic mono-, di-, or tri-carboxylic acids. Aliphatic carboxylic acids also include alicyclic carboxylic acids. Among these, preferred aliphatic carboxylic acids are mono- or di-carboxylic acids having 6 to 36 carbon atoms, with saturated aliphatic mono-carboxylic acids having 6 to 36 carbon atoms being more preferred. Specific examples of such aliphatic carboxylic acids include palmitic acid, stearic acid, caproic acid, capric acid, lauric acid, arachic acid, behenic acid, lignoceric acid, cerotic acid, melissic acid, tetralinic acid, montanic acid, adipic acid, and azelaic acid.

[0109] In the ester of an aliphatic carboxylic acid and an alcohol, the same aliphatic carboxylic acid as used herein can be used. On the other hand, examples of the alcohol include saturated or unsaturated monohydric or polyhydric alcohols. These alcohols may have a substituent such as a fluorine atom or an aryl group. Among these, monohydric or polyhydric saturated alcohols having 30 or less carbon atoms are preferred, and aliphatic or alicyclic saturated monohydric alcohols or aliphatic saturated polyhydric alcohols having 30 or less carbon atoms are more preferred. Specific examples of such alcohols include octanol, decanol, dodecanol, stearyl alcohol, behenyl alcohol, ethylene glycol, diethylene glycol, glycerin, pentaerythritol, 2,2-dihydroxyperfluoropropanol, neopentylene glycol, ditrimethylolpropane, and dipentaerythritol. Specific examples of esters of aliphatic carboxylic acids and alcohols include beeswax (a mixture containing myricyl palmitate as a main component), stearyl stearate, behenyl behenate, stearyl behenate, glycerin monopalmitate, glycerin monostearate, glycerin distearate, glycerin tristearate, pentaerythritol monopalmitate, pentaerythritol monostearate, pentaerythritol distearate, pentaerythritol tristearate, pentaerythritol tetrastearate, and esters of montanic acid and polyfunctional alcohols.

[0110] Examples of aliphatic hydrocarbons having a number average molecular weight of 200 to 15,000 include liquid paraffin, paraffin wax, microcrystalline wax, polyethylene wax, Fischer-Tropsch wax, and α-olefin oligomers having 3 to 12 carbon atoms. Note that the aliphatic hydrocarbons herein also include alicyclic hydrocarbons. The number average molecular weight of the aliphatic hydrocarbons is preferably 5,000 or less.

[0111] Examples of polyolefin waxes include polyethylene wax, polypropylene wax, and polyethylene propylene wax, with polyethylene wax being preferred. The polyolefin wax may be unmodified or modified. Examples of modified polyolefin waxes include vinyl ester-modified polyolefin wax, acid-modified polyolefin wax, and oxidized polyolefin wax, with oxidized polyolefin wax being preferred. Oxidized polyolefin waxes have excellent compatibility with polyalkylene terephthalate resins and tend to effectively suppress mold deposits in the resulting resin composition.

[0112] Oxidized polyolefin waxes can be obtained by oxidizing the corresponding unmodified polyolefin wax. Examples of oxidized polyethylene waxes include Licowax (registered trademark) PED521, PED522, and PED121 manufactured by Clariant Chemicals; Ceridust (registered trademark) 3715, and the like. In addition to the above, commercially available polyolefin waxes can be found in paragraph 0028 of JP 2022-140470 A, the contents of which are incorporated herein by reference.

[0113] The weight-average molecular weight of the polyolefin wax is preferably 800 or more, more preferably 1,000 or more, even more preferably 1,500 or more, even more preferably 2,000 or more, and even more preferably 2,500 or more. By setting it to the lower limit or more, the glowing time tends to be further shortened. Furthermore, the weight-average molecular weight of the polyolefin wax is preferably 30,000 or less, more preferably 20,000 or less, even more preferably 15,000 or less, and even more preferably 10,000 or less. By setting it to the upper limit or less, the fluidity of the resin composition during molding tends to be further improved. The weight average molecular weight can be measured by GPC (gel permeation chromatography) using a Tosoh HLC-8320GPC EcoSEC, tetrahydrofuran as a solvent, three Shodex KF-G and KF-805L columns, and a KF-800D column at a column temperature of 40°C and a flow rate of 1.2 mL / min, and can be measured as a polystyrene-equivalent value detected with a detector (UV-8320) at a detection wavelength of 254 nm. When the resin composition in this embodiment contains two or more types of polyolefin waxes, the weight average molecular weight is the weight average molecular weight of the mixture.

[0114] The dropping point of the polyolefin wax is preferably 165° C. or less, more preferably 160° C. or less, even more preferably 155° C. or less, even more preferably 150° C. or less, even more preferably 145° C. or less, even more preferably 140° C. or less, even more preferably 135° C. or less, particularly more preferably 130° C. or less, and preferably 80° C. or more, more preferably 85° C. or more, even more preferably 85° C. or more, even more preferably 90° C. or more, and even more preferably 95° C. or more. The dropping point is the temperature at which the first drop of molten material falls from a standard cup with an opening of 2.8 mm when the polyolefin wax is heated to change from a solid to a liquid state.

[0115] As for the release agent, in addition to the above, the descriptions in paragraphs 0063 to 0077 of JP-A-2018-070722 and the descriptions in paragraphs 0090 to 0098 of JP-A-2019-123809 can be referred to, and the contents of these can be incorporated into this specification.

[0116] In the resin composition of this embodiment, the release agent is preferably contained in an amount of 0.01 parts by mass or more, more preferably 0.1 parts by mass or more, even more preferably 0.3 parts by mass or more, and even more preferably 0.5 parts by mass or more, relative to 100 parts by mass of the thermoplastic resin contained in the resin composition. It is also preferably contained in an amount of 5 parts by mass or less, more preferably 4 parts by mass or less, even more preferably 3 parts by mass or less, and even more preferably 2 parts by mass or less. By setting the amount to be equal to or greater than the lower limit, the releasability of the resulting molded article tends to be further improved. Furthermore, by setting the amount to be equal to or less than the upper limit, bleed-out of the resulting molded article can be effectively suppressed. The resin composition may contain only one type of release agent, or two or more types. When two or more types are contained, the total amount is preferably within the above range.

[0117] An example of 100 parts by mass of thermoplastic resin contained in the resin composition is a total of 100 parts by mass of polybutylene terephthalate resin and an amorphous thermoplastic resin having a carbonate bond and / or an ester bond. Another example of 100 parts by mass of thermoplastic resin contained in the resin composition is a total of 100 parts by mass of polybutylene terephthalate resin and polystyrene-based resin. Another example of 100 parts by mass of thermoplastic resin contained in the resin composition is 100 parts by mass of polybutylene terephthalate resin. The resin composition of this embodiment may contain only one type of stabilizer, or may contain two or more types. When two or more types are contained, it is preferable that the total amount is in the above range.

[0118] <Colorant> The resin composition of this embodiment may contain a colorant (dye and / or pigment). By containing a colorant, the design of the resulting molded article can be improved. The colorant may be a dye or a pigment. The dye used in this embodiment is preferably a black dye and / or a black dye composition. The black dye composition refers to a dye composition that exhibits black by combining two or more chromatic dyes such as red, blue, and green. A first embodiment of the black dye composition is a form that contains a green dye and a red dye. A second embodiment of the black dye composition is a form that contains a red dye, a blue dye, and a yellow dye.

[0119] Examples of commercially available light-transmitting dyes include colorants Plast Yellow 8000, Plast Red M 8315, Plast Red 8370, and Oil Green 5602 manufactured by Arimoto Chemical Co., Ltd.; colorants Macrolex Yellow 3G, Macrolex Red EG, and Macrolex Green 5B manufactured by LANXESS Corporation; and colorants KP Plast HK, KP Plast Red HG, KP Plast Red H2G, KP Plast Blue R, KP Plast Blue GR, and KP Plast Green G manufactured by Kiwa Chemical Industry Co., Ltd. Furthermore, dyes described in Japanese Patent No. 4157300 and Japanese Patent No. 4040460 can also be used, the contents of which are incorporated herein by reference.

[0120] Examples of pigments used in this embodiment include inorganic pigments (black pigments such as carbon black (e.g., acetylene black, lamp black, thermal black, furnace black, channel black, ketjen black, etc.), red pigments such as iron oxide red, orange pigments such as molybdate orange, and white pigments such as titanium oxide), and organic pigments (yellow pigments, orange pigments, red pigments, blue pigments, green pigments, etc.), with black pigments being preferred and carbon black being more preferred. When the resin composition of this embodiment contains a pigment, it is preferable to use it as a masterbatch with a thermoplastic resin (preferably a polyester resin, more preferably a polybutylene terephthalate resin). The concentration of the pigment in the masterbatch is preferably 1 to 50% by mass.

[0121] When the resin composition of this embodiment contains a colorant, the content thereof is preferably 0.1 parts by mass or more, more preferably 0.2 parts by mass or more, and even more preferably 0.4 parts by mass or more, relative to 100 parts by mass of the thermoplastic resin contained in the resin composition, and is preferably 5 parts by mass or less, and more preferably 4 parts by mass or less. The resin composition of this embodiment may contain only one type of colorant, or may contain two or more types. When two or more types are contained, it is preferable that the total amount is in the above range.

[0122] An example of 100 parts by mass of the thermoplastic resin contained in the resin composition is a total of 100 parts by mass of polybutylene terephthalate resin and an amorphous thermoplastic resin having a carbonate bond and / or an ester bond. Another example of 100 parts by mass of the thermoplastic resin contained in the resin composition is a total of 100 parts by mass of polybutylene terephthalate resin and a polystyrene-based resin. Another example of 100 parts by mass of the thermoplastic resin contained in the resin composition is 100 parts by mass of polybutylene terephthalate resin. The resin composition of the present embodiment may contain only one type of stabilizer, or may contain two or more types. When two or more types are contained, it is preferable that the total amount be in the above range.

[0123] <Flame Retardant> The resin composition of this embodiment preferably contains a flame retardant. The type of flame retardant is not particularly limited, and known flame retardants can be used, such as halogen-based flame retardants, phosphorus-based flame retardants (metal phosphinate, melamine polyphosphate, etc.), nitrogen-based flame retardants (melamine cyanurate, etc.), and metal hydroxides (magnesium hydroxide, etc.). One example of the flame retardant in this embodiment is a phosphorus-based flame retardant, another example is a nitrogen-based flame retardant, and yet another example is a halogen-based flame retardant.

[0124] <<Halogen-Based Flame Retardant>> As the halogen-based flame retardant, a brominated flame retardant is more preferable. Although the type of brominated flame retardant is not particularly limited, brominated phthalimide, brominated poly(meth)acrylate, brominated polycarbonate, brominated epoxy, and brominated polystyrene are preferable, and brominated epoxy is more preferable.

[0125] The brominated phthalimide is preferably one represented by formula (1). (In formula (1), D represents an alkylene group, an arylene group, or —S(═O) ２ represents a group consisting of a combination of two or more of -, -C(=O)-, and -O-, and i is an integer of 1 to 4.

[0126] In formula (1), D is an alkylene group, an arylene group, or —S(═O) ２ represents a group consisting of a combination of two or more of -, -C(=O)-, and -O-, and is an alkylene group or an arylene group and -S(=O) ２ A group consisting of a combination of at least one of -, -C(=O)-, and -O- is preferred, and an alkylene group or an arylene group and -S(=O) ２A group formed by combining one of -, -C(=O)-, and -O- is more preferred, and an alkylene group is even more preferred. The group formed by combining an alkylene group and -O- is intended to include, for example, a combination of two alkylene groups and one -O- (the same applies to other combinations). The alkylene group represented by D is preferably an alkylene group having 1 to 6 carbon atoms, and more preferably a methylene group, ethylene group, propylene group, or butylene group. The arylene group is preferably a phenylene group. i is an integer of 1 to 4, and preferably 4.

[0127] Examples of the brominated phthalimide represented by formula (1) include N,N'-(bistetrabromophthalimide)ethane, N,N'-(bistetrabromophthalimide)propane, N,N'-(bistetrabromophthalimide)butane, N,N'-(bistetrabromophthalimide)diethyl ether, N,N'-(bistetrabromophthalimide)dipropyl ether, N,N'-(bistetrabromophthalimide)dibutyl ether, N,N'-(bistetrabromophthalimide)diphenylsulfone, N,N'-(bistetrabromophthalimide)diphenyl ketone, and N,N'-(bistetrabromophthalimide)diphenyl ether.

[0128] The brominated phthalimide represented by formula (1) is preferably a brominated phthalimide represented by formula (2). (In formula (2), i is an integer of 1 to 4.) i is an integer of 1 to 4, and is preferably 4.

[0129] The brominated poly(meth)acrylate is preferably a polymer obtained by polymerizing a bromine atom-containing benzyl (meth)acrylate alone, copolymerizing two or more types of bromine atom-containing benzyl (meth)acrylate, or copolymerizing the bromine atom-containing benzyl (meth)acrylate with another vinyl monomer, and the bromine atoms are attached to a benzene ring, with 1 to 5 bromine atoms, preferably 4 to 5 bromine atoms, attached to each benzene ring.

[0130] Examples of benzyl acrylates containing bromine atoms include pentabromobenzyl acrylate, tetrabromobenzyl acrylate, tribromobenzyl acrylate, and mixtures thereof. Examples of benzyl methacrylates containing bromine atoms include methacrylates corresponding to the above-mentioned acrylates.

[0131] Specific examples of other vinyl monomers that can be copolymerized with the bromine atom-containing benzyl (meth)acrylate include acrylic acid esters such as acrylic acid, methyl acrylate, ethyl acrylate, butyl acrylate, and benzyl acrylate; methacrylic acid esters such as methacrylic acid, methyl methacrylate, ethyl methacrylate, butyl methacrylate, and benzyl methacrylate; unsaturated carboxylic acids or anhydrides thereof such as styrene, acrylonitrile, fumaric acid, and maleic acid; vinyl acetate; and vinyl chloride.

[0132] These are usually used in an amount of not more than equimolar, particularly preferably not more than 0.5 times the molar amount of the bromine atom-containing benzyl (meth)acrylate.

[0133] Furthermore, examples of vinyl monomers that can be used include xylene diacrylate, xylene dimethacrylate, tetrabromxylene diacrylate, tetrabromxylene dimethacrylate, butadiene, isoprene, and divinylbenzene. These can usually be used in an amount of 0.5 times or less by mole relative to the bromine atom-containing benzyl acrylate or benzyl methacrylate.

[0134] The brominated poly(meth)acrylate is preferably a polymer obtained by polymerizing a bromine atom-containing (meth)acrylate monomer, particularly benzyl (meth)acrylate, alone or by copolymerizing two or more of them, or by copolymerizing them with other vinyl monomers. The bromine atoms are attached to the benzene ring, and the number of bromine atoms attached is preferably 1 to 5, more preferably 4 to 5, per benzene ring.

[0135] As the brominated poly(meth)acrylate, pentabromobenzyl poly(meth)acrylate is preferred because of its high bromine content.

[0136] The molecular weight of the brominated poly(meth)acrylate is optional and may be appropriately selected and determined, but the weight average molecular weight (Mw) is preferably 3,000 or more, more preferably 10,000 or more, and even more preferably 15,000 or more. By setting it to the lower limit or higher, molded articles with higher mechanical strength tend to be obtained. Furthermore, the upper limit of the weight average molecular weight (Mw) is preferably 100,000 or less, more preferably 80,000 or less, even more preferably 60,000 or less, even more preferably 50,000 or less, and even more preferably 35,000 or less. By setting it to the upper limit or lower, the flowability of the resin composition tends to be further improved.

[0137] The brominated polycarbonate preferably has a free bromine content of 0.05% by mass or more, and preferably 0.20% by mass or less. By setting the content within these ranges, the heat resistance stability of the resin composition tends to be further improved. The brominated polycarbonate also preferably has a chlorine atom content of 0.001% by mass or more, and preferably 0.20% by mass or less. By setting the content within these ranges, the mold corrosion resistance during molding tends to be further improved. Specific examples of brominated polycarbonates include brominated bisphenol A, particularly brominated polycarbonates obtained from tetrabromobisphenol A. Examples of terminal structures include phenyl groups, 4-t-butylphenyl groups, and 2,4,6-tribromophenyl groups. Those having a 2,4,6-tribromophenyl group as a terminal group structure are particularly preferred.

[0138] The average number of carbonate structural units in the brominated polycarbonate may be appropriately selected and determined, but is preferably 2 to 30, more preferably 3 to 15, and even more preferably 3 to 10.

[0139] The molecular weight of the brominated polycarbonate is optional and may be appropriately selected and determined, but preferably has a viscosity average molecular weight of 1,000 to 20,000, more preferably 2,000 to 10,000.

[0140] The brominated polycarbonate obtained from the above brominated bisphenol A can be obtained, for example, by a conventional method of reacting brominated bisphenol with phosgene. The end-capping agent includes an aromatic monohydroxy compound, which may be substituted with a halogen or an organic group.

[0141] Specific preferred examples of the brominated epoxy include bisphenol A type brominated epoxy compounds, such as tetrabromobisphenol A epoxy compounds and glycidyl brominated bisphenol A epoxy compounds.

[0142] The molecular weight of the brominated epoxy compound is optional and may be appropriately selected and determined, but the weight average molecular weight (Mw) is preferably 3,000 or more, more preferably 10,000 or more, even more preferably 13,000 or more, even more preferably 15,000 or more, and even more preferably 18,000 or more. By setting the weight average molecular weight at or above the lower limit, molded articles having higher mechanical strength tend to be obtained. Furthermore, the upper limit of the weight average molecular weight (Mw) is preferably 100,000 or less, more preferably 80,000 or less, even more preferably 78,000 or less, even more preferably 75,000 or less, and even more preferably 70,000 or less. By setting the weight average molecular weight at or below the upper limit, the flowability of the resin composition tends to be further improved. The brominated epoxy compound preferably has an epoxy equivalent of 3,000 to 40,000 g / eq, more preferably 4,000 to 35,000 g / eq, and particularly preferably 10,000 to 30,000 g / eq.

[0143] A brominated epoxy oligomer can also be used as the brominated epoxy. In this case, for example, by using an oligomer having a Mw of 5,000 or less in a proportion of about 50% by mass or less, the flame retardancy, mold releasability, and flowability can be appropriately adjusted. The bromine atom content in the brominated epoxy compound is optional, but in order to impart sufficient flame retardancy, it is usually 10% by mass or more, preferably 20% by mass or more, and particularly preferably 30% by mass or more, with the upper limit being 60% by mass, and preferably 55% by mass or less.

[0144] The brominated polystyrene preferably includes a brominated polystyrene containing a constituent unit represented by formula (3). (In formula (3), t is an integer of 1 to 5, and n is the number of constitutional units.)

[0145] Brominated polystyrene may be produced by brominating polystyrene or by polymerizing brominated styrene monomers, but polymerized brominated styrene is preferred because it has a low amount of free bromine (atoms). In formula (3), the CH group to which the brominated benzene is bonded may be substituted with a methyl group. Brominated polystyrene may also be a copolymer in which other vinyl monomers are copolymerized. Examples of vinyl monomers in this case include styrene, α-methylstyrene, (meth)acrylonitrile, methyl (meth)acrylate, butadiene, and vinyl acetate. Brominated polystyrene may be used alone or as a mixture of two or more types with different structures, and may contain units derived from styrene monomers with different bromine numbers in a single molecular chain.

[0146] Specific examples of brominated polystyrene include poly(4-bromostyrene), poly(2-bromostyrene), poly(3-bromostyrene), poly(2,4-dibromostyrene), poly(2,6-dibromostyrene), poly(2,5-dibromostyrene), poly(3,5-dibromostyrene), poly(2,4,6-tribromostyrene), poly(2,4,5-tribromostyrene), poly(2,3,5-tribromostyrene), and poly(4-bromo-α-methylstyrene). Examples of suitable bromine groups include poly(2,4,6-tribromostyrene), poly(2,4,5-tribromostyrene), poly(2,4,6-tribromostyrene), poly(2,4,5-tribromostyrene), and poly(2,4,6-tribromostyrene). Of these, poly(2,4,6-tribromostyrene), poly(2,4,5-tribromostyrene), and polydibromostyrene and polytribromostyrene containing an average of 2 to 3 bromine groups in the benzene ring are particularly preferred.

[0147] The brominated polystyrene preferably has the number n (average degree of polymerization) of structural units in formula (3) of 30 to 1,500, more preferably 150 to 1,000, and particularly preferably 300 to 800. If the average degree of polymerization is less than 30, blooming is likely to occur, while if it exceeds 1,500, poor dispersion is likely to occur and mechanical properties are likely to deteriorate. The weight-average molecular weight (Mw) of the brominated polystyrene is preferably 5,000 to 500,000, more preferably 10,000 to 500,000, even more preferably 10,000 to 300,000, even more preferably 10,000 to 100,000, and even more preferably 10,000 to 70,000. In particular, in the case of the brominated polystyrene described above, the weight average molecular weight (Mw) is preferably 50,000 to 70,000, and in the case of brominated polystyrene obtained by polymerization, the weight average molecular weight (Mw) is preferably about 10,000 to 30,000. The weight average molecular weight (Mw) can be determined as a value converted into standard polystyrene by GPC measurement.

[0148] The content of the halogen-based flame retardant in the resin composition of this embodiment is preferably 1 part by mass or more, more preferably 3 parts by mass or more, even more preferably 5 parts by mass or more, even more preferably 7 parts by mass or more, even more preferably 9 parts by mass or more, relative to 100 parts by mass of the thermoplastic resin contained in the resin composition, and is preferably 40 parts by mass or less, preferably 30 parts by mass or less, and even more preferably 20 parts by mass or less. By setting the content at or above the lower limit, the flame retardancy of the obtained molded article tends to be further improved. Furthermore, by setting the content at or below the upper limit, the mechanical strength of the obtained molded article tends to be further improved. The resin composition of this embodiment may contain only one type of halogen-based flame retardant, or may contain two or more types. When two or more types are contained, the total amount is preferably within the above range.

[0149] <<Phosphorus-Based Flame Retardant>> Examples of phosphorus-based flame retardants include metal phosphinates, melamine polyphosphates, condensed phosphate esters, and phosphazene compounds, with metal phosphinates being preferred.

[0150] When a metal phosphinate is used as a flame retardant, the type thereof is not particularly limited, but it is preferable that the metal phosphinate has an anion moiety represented by formula (4) or formula (5) and a metal ion of the cation moiety is any one of calcium, magnesium, aluminum, and zinc.

[0151] (In the formula, R １ and R ２ each independently represents an alkyl group having 1 to 6 carbon atoms or an aryl group which may have a substituent, R １ may be the same or different, and R ３ represents an alkylene group having 2 to 10 carbon atoms, an arylene group which may have a substituent, or a group consisting of a combination thereof; R ３may be the same or different, and n represents an integer of 0 to 2.) The aryl group which may have a substituent is preferably a phenyl group which may have a substituent. If it has a substituent, it is preferably an alkyl group having 1 to 3 carbon atoms. It is also preferably unsubstituted. The arylene group which may have a substituent is preferably a phenylene group which may have a substituent. The arylene group which may have a substituent is preferably unsubstituted or has an alkyl group having 1 to 3 carbon atoms (preferably a methyl group) as a substituent. In this embodiment, a metal phosphinate represented by formula (4) is preferred. In this embodiment, aluminum phosphinate is preferred.

[0152] Specific examples of the metal phosphinate include calcium dimethylphosphinate, magnesium dimethylphosphinate, aluminum dimethylphosphinate, zinc dimethylphosphinate, calcium ethylmethylphosphinate, magnesium ethylmethylphosphinate, aluminum ethylmethylphosphinate, zinc ethylmethylphosphinate, calcium diethylphosphinate, magnesium diethylphosphinate, aluminum diethylphosphinate, zinc diethylphosphinate, calcium methyl-n-propylphosphinate, magnesium methyl-n-propylphosphinate, aluminum methyl-n-propylphosphinate, zinc methyl-n-propylphosphinate, and calcium methanedi(methylphosphinate). Examples of suitable metal phosphinates include magnesium methanedi(methylphosphinate), aluminum methanebis(methylphosphinate), zinc methanebis(methylphosphinate), calcium benzene-1,4-bis(methylphosphinate), magnesium benzene-1,4-bis(methylphosphinate), aluminum benzene-1,4-bis(methylphosphinate), zinc benzene-1,4-bis(methylphosphinate), calcium methylphenylphosphinate, magnesium methylphenylphosphinate, aluminum methylphenylphosphinate, zinc methylphenylphosphinate, calcium diphenylphosphinate, magnesium diphenylphosphinate, aluminum diphenylphosphinate, and zinc diphenylphosphinate. For details of the metal phosphinates, please refer to paragraphs 0052 to 0058 of WO 2010 / 010669, the contents of which are incorporated herein by reference. For details of the phosphorus-based flame retardant, please refer to paragraphs 0064 to 0084 of WO 2021 / 241471, the contents of which are incorporated herein by reference.

[0153] The content of the phosphorus-based flame retardant in the resin composition of this embodiment is preferably 1 part by mass or more, more preferably 5 parts by mass or more, even more preferably 10 parts by mass or more, even more preferably 15 parts by mass or more, even more preferably 20 parts by mass or more, even more preferably 25 parts by mass or more, and preferably 40 parts by mass or less, more preferably 35 parts by mass or less, and even more preferably 30 parts by mass or less, per 100 parts by mass of the thermoplastic resin contained in the resin composition. By setting the content at or above the lower limit, the flame retardancy of the obtained molded article tends to be further improved. Furthermore, by setting the content at or below the upper limit, the mechanical strength of the obtained molded article tends to be further improved. The resin composition of this embodiment may contain only one type of phosphorus-based flame retardant, or may contain two or more types. When two or more types are contained, the total amount is preferably within the above range.

[0154] <<Nitrogen-Based Flame Retardants>> Examples of nitrogen-based flame retardants include aliphatic amine compounds, aromatic amine compounds, nitrogen-containing heterocyclic compounds, cyan compounds, aliphatic amides, aromatic amides, urea, and thiourea. Examples of aliphatic amines include ethylamine, butylamine, diethylamine, ethylenediamine, butylenediamine, triethylenetetramine, 1,2-diaminocyclohexane, and 1,2-diaminocyclooctane. Examples of aromatic amines include aniline and phenylenediamine. Examples of nitrogen-containing heterocyclic compounds include uric acid, adenine, guanine, 2,6-diaminopurine, 2,4,6-triaminopyridine, and triazine compounds. Examples of cyan compounds include dicyandiamide, examples of aliphatic amides include N,N-dimethylacetamide, and examples of aromatic amides include N,N-diphenylacetamide.

[0155] The triazine compounds exemplified above are nitrogen-containing heterocyclic compounds having a triazine skeleton, and examples thereof include triazine, melamine, benzoguanamine, methylguanamine, cyanuric acid, melamine cyanurate, melamine isocyanurate, trimethyltriazine, triphenyltriazine, ameline, amelide, thiocyanuric acid, diaminomercaptotriazine, diaminomethyltriazine, diaminophenyltriazine, diaminoisopropoxytriazine, etc. As the melamine cyanurate or melamine isocyanurate, an adduct of cyanuric acid or isocyanuric acid with a triazine compound is preferred, and examples thereof include adducts having a molar ratio of usually 1:1, and in some cases 1:2.

[0156] Among the nitrogen-based flame retardants, nitrogen-containing heterocyclic compounds are preferred, among which triazine compounds are more preferred, and melamine cyanurate is even more preferred.

[0157] The resin composition of this embodiment may or may not contain a nitrogen-based flame retardant. When the resin composition of this embodiment contains a nitrogen-based flame retardant, the content thereof is preferably 1 part by mass or more, more preferably 5 parts by mass or more, and even more preferably 10 parts by mass or more, relative to 100 parts by mass of the thermoplastic resin contained in the resin composition. It is also preferably 19 parts by mass or less, more preferably 18 parts by mass or less, more preferably 16 parts by mass or less, even more preferably 14 parts by mass or less, even more preferably 13 parts by mass or less, and even more preferably 10 parts by mass or less. Depending on the application, it may be 8 parts by mass or less, 5 parts by mass or less, 3 parts by mass or less, 1 part by mass or less, or 0.1 parts by mass or less. By setting the content at or above the lower limit, the flame retardancy and tracking resistance of the obtained molded article tend to be further improved. Furthermore, by setting the content at or below the upper limit, the mechanical strength tends to be further improved, gelation during the production of the resin composition tends to be suppressed, and a decrease in fluidity due to thickening of the resin composition tends to be suppressed. The resin composition of the present embodiment may contain only one nitrogen-based flame retardant, or may contain two or more nitrogen-based flame retardants. When two or more nitrogen-based flame retardants are contained, the total amount is preferably in the above range.

[0158] The content (total amount) of the flame retardant in the resin composition of this embodiment is preferably 1 part by mass or more, more preferably 5 parts by mass or more, more preferably 10 parts by mass or more, even more preferably 15 parts by mass or more, even more preferably 20 parts by mass or more, and even more preferably 25 parts by mass or more, relative to 100 parts by mass of the thermoplastic resin contained in the resin composition. It is also preferably 40 parts by mass or less, more preferably 35 parts by mass or less, even more preferably 30 parts by mass or less, even more preferably 25 parts by mass or less, and even more preferably 20 parts by mass or less. By setting the content at or above the lower limit, flame retardancy tends to be further improved. Furthermore, by setting the content at or below the upper limit, mechanical strength tends to be further improved. The resin composition of this embodiment may contain only one type of flame retardant, or may contain two or more types. When two or more types are contained, it is preferable that the total amount is within the above range.

[0159] <Flame Retardant Auxiliary> The resin composition of the present embodiment may contain a flame retardant auxiliary. When a flame retardant auxiliary is contained, it is preferable to contain an antimony compound. The flame retardant auxiliary (preferably an antimony compound) improves the flame retardancy of the resulting molded article. Examples of the antimony compound include antimony trioxide (Sb ２ O ３ ), antimony pentoxide (Sb ２ O ５ ) and sodium antimonate, and among these, antimony trioxide is particularly preferred.

[0160] In the resin composition of this embodiment, the antimony compound may be blended as a masterbatch with the thermoplastic resin. This makes it easier for the antimony compound to be present in the thermoplastic resin phase, improving thermal stability during melt-kneading and molding, suppressing a decrease in impact resistance, and tending to reduce variations in flame retardancy and impact resistance. The content of the antimony compound in the masterbatch is preferably 20 to 90% by mass. The content of the antimony compound in the masterbatch is more preferably 30% by mass or more, even more preferably 40% by mass or more, even more preferably 50% by mass or more, even more preferably 60% by mass or more, and particularly preferably 70% by mass or more.

[0161] The content of the antimony compound in the resin composition of this embodiment is preferably 0.1 parts by mass or more, more preferably 1 part by mass or more, and even more preferably 2 parts by mass or more, per 100 parts by mass of the thermoplastic resin contained in the resin composition of this embodiment. By setting the content at or above the lower limit, the flame retardancy of the resulting molded article is further improved. Furthermore, the upper limit of the content of the antimony compound is preferably 40 parts by mass or less, more preferably 30 parts by mass or less, even more preferably 20 parts by mass or less, even more preferably 10 parts by mass or less, and even more preferably 5 parts by mass or less, per 100 parts by mass of the thermoplastic resin. By setting the content at or below the upper limit, the mold releasability and impact resistance of the resulting molded article tend to be improved.

[0162] <Other Components> The resin composition of this embodiment may contain other components in addition to those described above, as necessary, as long as the desired physical properties are not significantly impaired. Examples of other components include various resin additives. One type of other component may be contained, or two or more types may be contained in any combination and ratio. The total amount of these other components is preferably 0 to 5% by mass, more preferably 0 to 3% by mass, and even more preferably 0 to 1% by mass, based on 100% by mass of the resin composition. Specific examples include ultraviolet absorbers, antistatic agents, antifogging agents, antiblocking agents, flow improvers, plasticizers, dispersants, and antibacterial agents. The resin composition of this embodiment may also contain additives described in paragraphs 0047 to 0103 of WO 2021 / 241471 within the spirit and scope of the present invention, the contents of which are incorporated herein by reference.

[0163] The resin composition (1) of this embodiment is a resin composition having a high crystallization temperature Tc during cooling. In the resin composition (1) of this embodiment, the polybutylene terephthalate resin, the amorphous thermoplastic resin (amorphous thermoplastic resin having a carbonate bond and / or an ester bond, and an amorphous thermoplastic resin having no carbonate bond or ester bond, which is blended as needed), and the glass fiber preferably account for 80% by mass or more of the resin composition, more preferably 85% by mass or more, even more preferably 90% by mass or more, and even more preferably 95% by mass or more, and may also be 100% by mass or less. Furthermore, in the resin composition (1) of the present embodiment, the polybutylene terephthalate resin, the amorphous thermoplastic resin having a carbonate bond and / or an ester bond, and the glass fiber, the amorphous thermoplastic resin not having a carbonate bond and an ester bond, the reactive compound, the stabilizer, the release agent, and the colorant, which are blended as necessary, preferably account for 90% by mass or more of the resin composition, more preferably 95% by mass or more, and even more preferably 97% by mass or more, and may account for 99% by mass or more, or may be 100% by mass or less.

[0164] The resin composition (2) of this embodiment is a resin composition in which a polybutylene terephthalate resin is blended with a polystyrene-based resin, and is capable of providing a molded product with high weld strength. In the resin composition (2) of this embodiment, the total of the polybutylene terephthalate resin, the polystyrene-based resin, and the glass fiber preferably accounts for 80% by mass or more of the resin composition, more preferably 85% by mass or more, even more preferably 90% by mass or more, even more preferably 95% by mass or more, and may be 100% by mass or less. Furthermore, in the resin composition (2) of this embodiment, the total of the polybutylene terephthalate resin, the polystyrene-based resin, the polycarbonate resin, and the glass fiber, stabilizer, release agent, and colorant, which are optionally blended, preferably accounts for 90% by mass or more of the resin composition, more preferably 95% by mass or more, even more preferably 97% by mass or more, and may account for 99% by mass or more, or may be 100% by mass or less.

[0165] The resin composition (3) of this embodiment has a low gas content in the pellets after production, and is capable of providing molded articles with excellent adhesive strength to other components using an epoxy adhesive while maintaining mechanical strength. One example of the resin composition (3) of this embodiment is a resin composition in which the polybutylene terephthalate resin, fibrous reinforcing material, and optional components are combined to form a total of 100% by mass. In the resin composition (3) of this embodiment, the total of the polybutylene terephthalate resin, epoxy compound, stabilizer, and fibrous reinforcing material preferably accounts for 90% by mass or more of the resin composition, more preferably 95% by mass or more, and may even be 100% by mass. Another example of the resin composition (3) of this embodiment is a resin composition in which the total of the polybutylene terephthalate resin, a thermoplastic resin other than the polybutylene terephthalate resin (e.g., polyethylene terephthalate resin), epoxy compound, stabilizer, and fibrous reinforcing material preferably accounts for 90% by mass or more of the resin composition, more preferably 95% by mass or more, and may even be 100% by mass.

[0166] <Physical Properties of Resin Composition> The resin composition of the present embodiment (particularly the resin composition (3)) has a melt volume rate (MVR) of 4 cm at 250°C and a load of 5 kgf. ３ / min or more, and ３ / min or more is more preferable, ３ / min or more, and more preferably 15 cm ３ / min or more, and more preferably 25 cm ３ / min or more, and more preferably 100 cm ３ / min or less, and ３ / min or less, and more preferably 80 cm ３ / min or less, and more preferably 65 cm ３ / min or less, more preferably 50 cm ３ / min or less is even more preferable. By setting the melt flow rate at or above the lower limit, the fluidity in the molten state is improved, and moldability tends to be excellent. Furthermore, by setting the melt flow rate at or below the upper limit, mechanical properties such as tensile strength tend to be excellent.

[0167] The resin composition of this embodiment (particularly the resin composition (3)) is molded into an ISO test piece (4 mm thick) and has a tensile modulus measured according to ISO 527-1 and ISO 527-2 of preferably 5000 MPa or more, more preferably 6000 MPa or more, even more preferably 7000 MPa or more, even more preferably 8000 MPa or more, and even more preferably 9000 MPa or more. There is no particular upper limit, but for example, even if it is 100,000 MPa or less, the required performance is sufficiently satisfied. By making it equal to or greater than the lower limit, the rigidity of the molded article is improved, and it tends to be possible to make the molded article thinner and lighter.

[0168] The resin composition of this embodiment (particularly the resin composition (3)) is molded into an ISO test piece (4 mm thick) and the tensile strength measured in accordance with ISO 527-1 and ISO 527-2 is preferably 70 MPa or more, more preferably 80 MPa or more, even more preferably 90 MPa or more, even more preferably 100 MPa or more, and even more preferably 120 MPa or more. There is no particular upper limit, but even if it is 500 MPa or less, the required performance is sufficiently satisfied. By making it equal to or greater than the lower limit, the mechanical strength of the molded article tends to be excellent.

[0169] The resin composition of this embodiment (particularly the resin composition (3)) is molded into an ISO test piece (4 mm thick) and the tensile break strain measured in accordance with ISO 527-1 and ISO 527-2 is preferably 0.5% or more, more preferably 0.8% or more, even more preferably 1.0% or more, even more preferably 1.2% or more, and even more preferably 1.5% or more. There is no particular upper limit, but even if it is 10% or less, the required performance is sufficiently satisfied. By making it equal to or greater than the lower limit, the toughness of the molded article tends to be excellent.

[0170] <Method for Producing Resin Composition> The resin composition of this embodiment can be produced by a conventional method for preparing a resin composition (e.g., pellets). Typically, the components and various optional additives are thoroughly mixed together and then melt-kneaded in a single-screw or twin-screw extruder. Alternatively, the resin composition of this embodiment can be prepared without premixing the components, or by premixing only a portion of the components, feeding the mixture into an extruder using a feeder and melt-kneading the mixture. For example, it is preferable to feed glass fibers into an extruder using a side feeder and melt-knead them. Alternatively, a masterbatch may be prepared by melt-kneading some of the components, such as a colorant, with a thermoplastic resin to prepare a masterbatch, and then blending the remaining components with the masterbatch and melt-kneading the resulting mixture.

[0171] <Method for Manufacturing Molded Articles> The resin composition or pellets of this embodiment are molded according to known methods. The method for manufacturing molded articles is not particularly limited, and any molding method commonly used for resin compositions can be used. Examples include injection molding, ultra-high speed injection molding, injection compression molding, two-color molding, gas-assisted hollow molding, molding using an insulated mold, molding using a rapidly heated mold, foam molding (including supercritical fluid), insert molding, IMC (in-mold coating molding), extrusion molding, sheet molding, thermoforming, rotational molding, laminate molding, press molding, and blow molding. Of these, injection molding is preferred. For details of injection molding, see paragraphs 0113 to 0116 of Japanese Patent No. 6183822, the contents of which are incorporated herein by reference. Furthermore, the mold temperature during mold molding, such as injection molding, is preferably 40 to 150°C.

[0172] <Applications> The resin composition of this embodiment is used as a molded article formed from the resin composition or pellets. The applications of the resin composition and pellets are not particularly limited, and they can be widely used as resin compositions for injection molding. Fields of use include, for example, electrical and electronic equipment materials, vehicle materials, housing materials, and materials for manufacturing parts in other industrial fields, both indoors and outdoors. In this embodiment, food containers, pharmaceutical containers, oil and fat product containers, hollow vehicle parts (various tanks, intake manifold parts, camera housings), vehicle electrical parts (various control units, ignition coil parts, etc.), motor parts, various sensor parts, connector parts, switch parts, breaker parts, relay parts, coil parts, transformer parts, lamp parts, etc. More specific examples of vehicle parts include lamp housings, reflectors, bezels, and extensions, as well as connectors, ECU cases, housings for in-vehicle cameras and millimeter-wave radars, battery cases, and sensor housings. More specific examples of electric and electronic components include display devices such as personal computers, game consoles and televisions, printers, copy machines, scanners, fax machines, electronic organizers and PDAs, electronic desk calculators, electronic dictionaries, cameras, video cameras, mobile phones, battery packs, drives and readers for recording media, mice, numeric keypads, CD players, MD players, portable radios and audio players, housings, covers, keyboards, buttons, switch members, casings for wattmeters, battery cases, battery transport trays, relays, sensors, actuators, terminal switches, and grill cooking appliance parts.

[0173] The present invention will be explained in more detail below with reference to examples. The materials, amounts used, ratios, treatment contents, treatment procedures, etc. shown in the following examples can be changed as appropriate without departing from the spirit of the present invention. Therefore, the scope of the present invention is not limited to the specific examples shown below. If the measuring instruments used in the examples are difficult to obtain due to discontinuation or the like, measurements can be made using other instruments with equivalent performance.

[0174] 1. Raw materials The following raw materials were used:

[0175] Synthesis Example 1 A slurry containing 1.80 moles of 1,4-butanediol (BDO) mixed with 1.00 moles of terephthalic acid was continuously supplied to an esterification reactor equipped with a screw-type agitator and filled with a polybutylene terephthalate (PBT) oligomer having an esterification rate of 99%, and an esterification reaction was carried out. A titanium catalyst solution of tetrabutyl titanate was supplied to the esterification reactor in an amount such that the titanium concentration relative to the PBT was 54 ppm by mass. Additional BDO was supplied to the esterification reactor so that the molar ratio of BDO to terephthalic acid was 2.5. The reactor temperature was 226°C, the pressure was 60 kPa, and the average residence time was 180 minutes. The PBT oligomer with an esterification rate of 96.5% was then continuously transferred to a first polycondensation reactor. A polycondensation reaction was carried out continuously in the first polycondensation reactor. The reaction temperature was 230°C, the pressure was 3.9 kPa, and the average residence time was 120 minutes. The product was then transferred to a second polycondensation reaction tank, where a continuous polycondensation reaction was carried out. The reaction temperature was 240°C, the pressure was 130 Pa, and the average residence time was 60 minutes. The resulting polymer was continuously extracted in the form of strands from the die head via a extraction line using a gear pump and a filter, and then cut with a rotary cutter to obtain PBT pellets (major axis approximately 3 mm, minor axis approximately 2 mm, length approximately 4 mm).

[0176] Synthesis Example 2 A slurry containing 1.80 moles of BDO mixed with 1.00 moles of terephthalic acid was continuously fed to an esterification reactor equipped with a screw agitator and filled with a PBT oligomer having an esterification rate of 99%, whereby an esterification reaction was carried out. A titanium catalyst solution of tetrabutyl titanate was fed to the esterification reactor in an amount such that the titanium concentration relative to the PBT was 43 ppm by mass. Additional BDO was fed to the esterification reactor so that the molar ratio of BDO to terephthalic acid was 2.5. The reactor temperature was 226°C, the pressure was 60 kPa, and the average residence time was 180 minutes. The PBT oligomer with an esterification rate of 96.5% was then continuously transferred to a first polycondensation reactor. A polycondensation reaction was carried out continuously in the first polycondensation reactor. The reaction temperature was 230°C, the pressure was 3.9 kPa, and the average residence time was 120 minutes. The product was then transferred to a second polycondensation reactor, where a continuous polycondensation reaction was carried out. The reaction temperature was 240°C, the pressure was 130 Pa, and the average residence time was 60 minutes. The resulting polymer was continuously withdrawn in the form of strands from the die head via a withdrawal line using a withdrawal gear pump and a filter, and then cut with a rotary cutter to obtain PBT pellets (major axis approximately 3 mm, minor axis approximately 2 mm, length approximately 4 mm).

[0177] Synthesis Example 3: A slurry containing 1.80 moles of BDO mixed with 1.00 moles of terephthalic acid was continuously fed to an esterification reactor equipped with a screw agitator and filled with a PBT oligomer having an esterification rate of 99%, whereby an esterification reaction was carried out. A BDO solution of tetrabutyl titanate was fed to the esterification reactor in an amount such that the titanium concentration relative to the PBT was 40 ppm by mass. Additional BDO was fed to the esterification reactor so that the molar ratio of BDO to terephthalic acid was 3.2. The reactor temperature was 226°C, the pressure was 60 kPa, and the average residence time was 180 minutes. Next, a BDO solution of magnesium acetate tetrahydrate was continuously fed to the PBT oligomer having an esterification rate of 96.5%, in an amount such that the magnesium concentration relative to the PBT was 10 ppm by mass. The oligomer was continuously transferred to a first polycondensation reactor. A polycondensation reaction was carried out continuously in the first polycondensation reactor. The reaction temperature was 230°C, the pressure was 3.9 kPa, and the average residence time was 120 minutes. The product was then transferred to a second polycondensation reaction tank, where a continuous polycondensation reaction was carried out. The reaction temperature was 240°C, the pressure was 130 Pa, and the average residence time was 80 minutes. The resulting polymer was continuously extracted in the form of strands from the die head via a extraction line using a gear pump and a filter, and then cut with a rotary cutter to obtain PBT pellets (major axis approximately 3 mm, minor axis approximately 2 mm, length approximately 4 mm).

[0178] Synthesis Example 4: A slurry containing 1.80 moles of BDO mixed with 1.00 moles of terephthalic acid was continuously supplied to an esterification reactor equipped with a screw agitator and filled with a PBT oligomer having an esterification rate of 99%, and an esterification reaction was carried out. A BDO solution of tetrabutyl titanate was supplied to the esterification reactor in an amount such that the titanium concentration relative to the PBT was 40 ppm by mass. Additional BDO was supplied to the esterification reactor so that the molar ratio of BDO to terephthalic acid was 3.2. The reactor temperature was 226°C, the pressure was 60 kPa, and the average residence time was 180 minutes.

[0179] Next, a BDO solution of magnesium acetate tetrahydrate was continuously supplied to the PBT oligomer with an esterification rate of 96.5%, in an amount equivalent to 10 ppm by mass of magnesium element relative to the PBT. The oligomer was continuously transferred to a first polycondensation reaction tank. A polycondensation reaction was continuously carried out in the first polycondensation reaction tank. The reaction temperature was 230°C, the pressure was 3.9 kPa, and the average residence time was 120 minutes. This product was then transferred to a second polycondensation reaction tank, where a polycondensation reaction was continuously carried out. The reaction temperature was 240°C, the pressure was 130 Pa, and the average residence time was 60 minutes.

[0180] The obtained polymer was passed through a discharge line by a discharge gear pump, passed through a filter, and continuously discharged in the form of strands from a die head. The strands were then cut with a rotary cutter to obtain PBT pellets (major axis approximately 3 mm, minor axis approximately 2 mm, length approximately 4 mm).

[0181] <Measurement of Ti concentration, Na concentration, and Ca concentration> Qualitative / semi-quantitative analysis (μg / g) of Ti, Na, and Ca in polybutylene terephthalate resin was performed by ICP atomic emission spectrometry. In this case, 200 mg of sample was weighed as a pretreatment, subjected to Kjeldahl wet hydrolysis (sulfuric acid / nitric acid, sulfuric acid / hydrogen peroxide), and the volume was adjusted to 50 mL. Subsequently, ICP atomic emission spectrometry was performed using the acid concentration matching single point calibration method. The units are shown in ppm by mass. ICP atomic emission spectrometry was performed using a ThermoThermo Fisher Scientific "iCAP7600duo iCAP76000uo" using axial / radial photometry.

[0182] <Active Titanium Parameter X and Active Titanium Ratio α> Five capillaries with an inner diameter of 5 mm were filled with the polybutylene terephthalate resin (pellets) powder obtained above. Next, after thoroughly replacing the contents with nitrogen, the capillaries were immersed in an oil bath precisely controlled at 245°C (temperature T), removed over time, and rapidly cooled with liquid nitrogen. The contents were then removed, and the terminal carboxyl group concentration and terminal hydroxyl group concentration were determined. Using these values, the active titanium ratio α was calculated from equations (1), (2), and (3). α=X / M (3) (In formula (3), X is the active titanium parameter, and [M] is the titanium element concentration (ppm by mass) in the polybutylene terephthalate resin.)

[0183] The evaluation of the change in terminal carboxyl group concentration over time is carried out in a nitrogen atmosphere to prevent the influence of oxygen. Furthermore, if the water concentration in the polybutylene terephthalate resin being evaluated is high, hydrolysis reactions occur frequently, making it difficult to accurately grasp the decomposition behavior associated with catalytic activity other than hydrolysis. Therefore, a low water concentration is preferable, and the evaluation is carried out at 300 mass ppm or less. The evaluation is carried out at a temperature of 245°C. Under these heat treatment conditions, the decrease in number average molecular weight due to reactions other than hydrolysis caused by the water contained in the polybutylene terephthalate resin can be ignored, and the increase in terminal carboxyl group concentration due to the hydrolysis reaction can be considered to be equal to the increase in terminal hydroxyl group concentration before and after the heat treatment. Therefore, the change in terminal carboxyl group concentration due to thermal decomposition reactions other than hydrolysis reactions can be calculated using the following formula (4):

[0184] Formula (4)

[0185] <Intrinsic Viscosity (IV)> The intrinsic viscosity was measured by the following method. Polybutylene terephthalate resin pellets were dissolved in a mixed solvent of phenol / 1,1,2,2-tetrachloroethane (1 / 1 by mass ratio) by stirring at 110°C for 1 hour to a concentration of 1.00 g / dL. The solution was then cooled to 30°C. Using a fully automatic solution viscometer, the number of seconds it took for the sample solution and the solvent alone to fall at 30°C were measured, and the intrinsic viscosity was calculated using the formula: Intrinsic viscosity = ((1 + 4K Ｈ η ｓｐ ) ０．５ -1) / (2K Ｈ C) where η ｓｐ = η / η ０ -1, η is the number of seconds the sample solution falls, η ０ is the number of seconds for the solvent to fall, C is the concentration of the sample solution (g / dL), K Ｈ is Huggins' constant. Ｈ The viscosity was 0.33. The unit was dL / g. The fully automatic solution viscometer manufactured by Shibayama Scientific Co., Ltd. was used.

[0186] <Terminal Carboxyl Group Concentration (Acid Value)> The terminal carboxyl group concentration of the polybutylene terephthalate resin was determined by dissolving 0.5 g of the polybutylene terephthalate resin in 25 mL of benzyl alcohol and titrating the solution with a 0.01 mol / L benzyl alcohol solution of sodium hydroxide. The unit is μmol / g (μeq / g).

[0187] <Terminal hydroxyl group concentration> The terminal hydroxyl group concentration of the polyalkylene terephthalate resin was measured by dissolving 25 mg of a sample in a vial in 0.75 mL of a mixed solvent of deuterated chloroform / hexafluoroisopropanol (volume ratio: 7 / 3) containing a trace amount of TMS (tetramethylsilane), adding 25 μL of deuterated pyridine, and transferring the solution to an NMR sample tube with an outer diameter of 5 mm. １ H NMR spectrum was measured at a resonance frequency of 600, 1 MHz, a flip angle of 45°, a data acquisition time of 3 s, a pulse repetition time of 10 s, an accumulation number of 16, and a temperature of 25° C. The unit is μmol / g.

[0188] <Terminal Vinyl Group Concentration> The terminal vinyl group concentration of the polyalkylene terephthalate resin was measured under the same conditions as for the terminal hydroxyl group concentration of the polyalkylene terephthalate resin, and the unit is μmol / g.

[0189] <Weight-average molecular weight (Mw) and number-average molecular weight (Mn)> The weight-average molecular weight and number-average molecular weight of the resin were measured using a Tosoh HLC-8320. The polyalkylene terephthalate resin was weighed, and a predetermined amount of HFIP (hexafluoro-2-propanol) and 10 mM CF3COONa eluent was added and allowed to dissolve overnight at room temperature. Subsequently, the sample was filtered through a 0.45 μm PTFE cartridge filter. The molecular weight (Mw, Mn) of the dissolved sample (filtrate) was measured by GPC. The calibration curve was a cubic approximation curve using standard PMMA, and the molecular weight was expressed as PMMA equivalent. A Tosoh TSKgel GMHhr-M column (Tosoh) was used for the GPC measurements.

[0190] <Melting Point (Tm) and Crystallization Temperature (Tc) During Cooling> The crystallization temperature (Tc) during cooling of the polybutylene terephthalate resin was measured using a differential scanning calorimeter (DSC) in accordance with JIS K7121. The temperature was increased from 40°C to 300°C at a heating rate of 20°C / min under a nitrogen atmosphere, and after holding at 300°C for 3 minutes, the temperature was decreased to 40°C at a heating rate of -20°C / min. This constituted one cycle. The temperature of the maximum peak due to crystallization during cooling was taken as the crystallization temperature during cooling, Tc. The melting point, Tm, was determined from the peak during melting. The units are shown in °C. The units are shown in °C. The differential scanning calorimeter used was a "DSC7020" manufactured by Hitachi High-Tech Science Corporation.

[0191] <Ash content> After incineration for 3 hours in an electric furnace at 500°C to burn only the resin component, the ash content was measured from the ratio of the residue mass. The ratio of the ash content in the polyalkylene terephthalate resin was expressed in units of mass%. The electric furnace used was "Electric Muffle Furnace KM-28" manufactured by Toyo Seisakusho Co., Ltd.

[0192] <Measurement of the amount of metal elements> Qualitative / semi-quantitative analysis of metal elements (Al, Fe) in polybutylene terephthalate resin was performed by ICP optical emission spectrometry. In this case, as a pretreatment, 200 mg of sample was weighed, subjected to Kjeldahl wet hydrolysis (sulfuric acid / nitric acid, sulfuric acid / hydrogen peroxide), and the volume was adjusted to 50 mL. Subsequently, ICP optical emission spectrometry was performed using the acid concentration matching single point calibration method. The unit is expressed in ppm by mass. ICP optical emission spectrometry was performed using a ThermoThermo Fisher Scientific "iCAP7600duo iCAP76000uo" by axial / radial photometry.

[0193] <Total nitrogen content in polybutylene terephthalate resin (TN (total nitrogen content))> The resin was burned under an argon and oxygen atmosphere, and the generated combustion gas was measured with a trace nitrogen analyzer using the reduced pressure chemiluminescence method. Aniline dissolved in toluene was used as the standard sample. (Apparatus) Total nitrogen analyzer: TN-2100H model manufactured by Nitto Seiko Analytech Co., Ltd.

[0194] <Total sulfur content in polybutylene terephthalate resin (S-N (total sulfur content))> The resin and combustion improver were collected in a magnetic boat and heated in a quartz tube furnace. The sulfur component in the combustion gas was removed by H ２ O ２ The absorbent was an aqueous solution. ４ ２－ was measured by ion chromatography. (Apparatus) Quartz tube furnace: AQF2100H model manufactured by Nitto Seiko Analytech Co., Ltd. Ion chromatogram: ICS-1600 model manufactured by Thermo Fisher Scientific Co., Ltd.

[0195] <Measurement of Ti concentration> Qualitative / semi-quantitative analysis (μg / g) of Ti in polybutylene terephthalate resin was performed by ICP atomic emission spectrometry. In this case, as a pretreatment, 200 mg of sample was weighed, subjected to Kjeldahl wet hydrolysis (sulfuric acid / nitric acid, sulfuric acid / hydrogen peroxide), and the volume was adjusted to 50 mL. Subsequently, ICP atomic emission spectrometry was performed using the acid concentration matching single point calibration method. The unit is expressed in ppm by mass. ICP atomic emission spectrometry was performed using a ThermoThermo Fisher Scientific "iCAP7600duo iCAP76000uo" by axial / radial photometry.

[0196]

[0197]

[0198] Examples 1-1 to 1-5, Comparative Examples 1-1 to 1-3 <Compound> The components shown in Tables 1 and 2 were mixed uniformly in a tumbler mixer in the proportions shown in Tables 4 to 6 (each component in Tables 4 to 6 is shown in parts by mass), with the exception of the glass fiber. The resulting mixture was fed to a twin-screw extruder through the main feed port. The cylinder temperature setting for the first kneading section was set to 260°C, and the glass fiber was fed through a side feeder. The resin composition was melt-kneaded under conditions of a cylinder temperature setting of 220°C after the addition of the glass fiber and a screw rotation speed of 200 rpm, and then quenched in a water bath and pelletized using a pelletizer to obtain pellets of the resin composition. The extruder used in Examples 1-1, 1-2, Comparative Examples 1-1, 1-3, and 1-2 was "TEX30α" manufactured by The Japan Steel Works, Ltd., and the extruder used in Examples 1-4, 1-5, and Comparative Example 1-3 was "TEX-53αII" manufactured by The Japan Steel Works, Ltd.

[0199] <Measurement of MVR of Resin Composition> The melt volume rate of the pellets of the resin composition obtained above was measured at 250°C under a load of 5 kgf in accordance with ISO 1133. The unit is cm ３ / 10 min.

[0200] <Transmittance> The pellets obtained above were dried at 120°C for 5 hours, and then a 60 mm square, 1.5 mm thick plate-shaped molded article was injection molded using an injection molding machine ("NEX80" manufactured by Nissei Plastic Industrial Co., Ltd.) under conditions of a cylinder temperature of 260°C and a mold temperature of 60°C. The obtained plate was measured for light transmittance (unit: %) at 1064 nm at a point 45 mm from the gate and at the center of the test plate width using a UV-visible spectrophotometer. The UV-visible spectrophotometer used was a "UV-3300PC" manufactured by Shimadzu Corporation equipped with an integrating sphere. The transmittance was expressed in units of %.

[0201] <Amount of gas generated> The amount of gas (THF) generated in the resin composition was measured by the following method. Pellets of the resin composition were heated at 150°C for 10 minutes, and the resulting gas was analyzed. The gas analysis was performed by headspace gas chromatography. The amount of gas generated (THF) was measured. The gas analysis was performed using a Nexis GC-2030 manufactured by Shimadzu Corporation.

[0202]

[0203]

[0204]

[0205] The resin compositions of the present invention, when compared with the resin compositions of the comparative examples, exhibited a higher crystallization temperature (Tc) during cooling and a higher transmittance when using the same extruder. Furthermore, the amount of gas contained in the pellets could be reduced. The crystallization temperature (Tc) during cooling varied depending on the scale of the extruder. That is, the crystallization temperature (Tc) during cooling was lower in Examples 1-4, 1-5, and Comparative Example 1-3, which were continuously produced using a large-scale extruder.

[0206] Example 2-1, Example 2-2, Comparative Example 2-1 <Compound> Pellets of a resin composition were obtained in the same manner as in Example 1-1, except that the components shown in Table 1 and Table 2 were used in the proportions shown in Table 8 (each component in Table 8 is shown in parts by mass).

[0207] <Tensile Properties> The resin pellets obtained above were dried at 120°C for 5 hours, and then ISO multipurpose test specimens (thickness 4 mm) were injection molded using an injection molding machine ("J85AD" manufactured by The Japan Steel Works, Ltd.) under conditions of a cylinder temperature of 250°C and a mold temperature of 80°C. Using the molded multipurpose ISO multipurpose test specimens, the tensile strength (unit: MPa) and tensile modulus (unit: MPa) were measured in accordance with ISO527-1 and ISO527-2.

[0208] <Weld Strength> Tests were carried out at a test speed of 5 mm / min using 4 mm thick 1A-type test pieces in accordance with ISO 527-1 and 2. A mold (gate distance 170 mm) with two gates on the surface center line in the longitudinal direction of the test piece was used, and the test piece with a weld formed in the center was molded under conditions of a cylinder temperature of 250°C, a mold temperature of 80°C, and a molding cycle of 40 seconds, and the weld strength (unit: MPa) was measured.

[0209] <Deflection Temperature Under Load (DTUL)> Using the above ISO multipurpose test piece (4 mm thick), the deflection temperature under load (unit: ° C.) was measured under a load of 1.80 MPa in accordance with ISO 75-1 and ISO 75-2.

[0210] <Amount of Gas Generated> The amount of gas (THF) generated in the resin composition was measured in the same manner as in Example 1-1.

[0211]

[0212] As is clear from the above results, molded articles formed from the resin composition of the present invention had high weld strength. Furthermore, they also had excellent tensile properties and high deflection temperatures under load (Examples 2-1 and 2-2). Furthermore, the amount of gas contained in the pellets could be reduced. In contrast, when the activated titanium was outside the range of the present invention, the weld strength was significantly lower. Furthermore, the tensile properties were also poor (Comparative Example 2-1).

[0213] Examples 3-1 to 3-4, Comparative Examples 3-1 to 3-3 <Compound> The components shown in Table 1 or Table 2 were uniformly mixed in a tumbler mixer in the proportions shown in Table 9 or Table 10 (each component in Table 9 or Table 10 is shown in parts by mass), with the exception of glass fiber. The resulting mixture was extruded in a twin-screw extruder ("TEX30α" manufactured by The Japan Steel Works, Ltd.) in the same manner as in Example 1-1 to obtain pellets of a resin composition.

[0214] <Measurement of MVR of Resin Composition> The MVR of the resin composition pellets obtained above was measured in the same manner as in Example 1-1.

[0215] <Adhesive Strength> The resin pellets obtained above were dried at 120°C for 5 hours, and then ISO multipurpose test specimens (4 mm thick) were injection molded using an injection molding machine (manufactured by The Japan Steel Works, Ltd., "J-85AD-60H") under conditions of a cylinder temperature of 250°C and a mold temperature of 80°C. Nitto Corporation's NITOFLON adhesive tape (10 mm wide x 0.18 mm thick) was attached to the chuck portion of the obtained ISO multipurpose test specimen to create a 20 mm x 20 mm square adhesive application area. A one-component, heat-curing epoxy adhesive was then applied to this area, and the chuck portion of another ISO multipurpose test specimen made of the same material was attached and secured with a binder clip. The adhesive was then treated under the specified curing conditions and bonded. A tensile test was performed using a Shimadzu Corporation AUTOGRAPH AGS-X 10kN at a tensile speed of 5 mm / min, and the adhesive strength (unit: N) was measured.

[0216] <Tensile Properties> The pellets obtained above were dried at 110°C for 5 hours, and then 4 mm thick ISO test specimens were injection molded using an injection molding machine ("J85AD" manufactured by The Japan Steel Works, Ltd.) under conditions of a cylinder temperature of 250°C and a mold temperature of 80°C. The ISO test specimens (4 mm thick) obtained above were measured for tensile modulus (unit: MPa), tensile strength (unit: MPa), and tensile break strain (unit: %) in accordance with ISO527-1 and ISO527-2.

[0217] <Amount of Gas Generated> The amount of gas (THF) generated in the resin composition was measured in the same manner as in Example 1-1.

[0218]

[0219] As is clear from the above results, molded articles formed from the resin composition of the present invention had high adhesive strength to epoxy adhesives (Examples 3-1 to 3-4). Furthermore, various mechanical properties were also excellent. Furthermore, the amount of gas contained in the pellets could be reduced. In contrast, when polybutylene terephthalate resins with a low total nitrogen element content were used (Comparative Examples 3-1 to 3-3), the adhesive strength to epoxy adhesives was low. Furthermore, the amount of gas generated in the pellets was also high.

[0220] Examples 4-1 to 4-3, Comparative Examples 4-1 to 4-2 <Compound> The components shown in Table 1 or Table 2 were uniformly mixed in a tumbler mixer, except for the glass fiber, in the proportions shown in Table 11 (each component in Table 11 is shown in parts by mass). The resulting mixture was extruded in a twin-screw extruder ("TEX30α" manufactured by The Japan Steel Works, Ltd.) in the same manner as in Example 1-1 to obtain pellets of a resin composition.

[0221] <Tensile Strength> The resin pellets obtained above were dried at 120°C for 5 hours, and then ISO multipurpose test pieces (thickness 4 mm) were injection molded using an injection molding machine ("J85AD" manufactured by The Japan Steel Works, Ltd.) under conditions of a cylinder temperature of 250°C and a mold temperature of 80°C. Using the molded multipurpose ISO multipurpose test pieces, the tensile strength (unit: MPa) was measured in accordance with ISO527-1 and ISO527-2.

[0222] <Amount of gas evolved upon heating (ppm)> The obtained pellets were heated at 280°C for 10 minutes, and the gas evolved with He was allowed to flow, and the gas evolved at -10°C was trapped. The trapped substance was analyzed by GC-MS. The gas amounts of tetrahydrofuran (THF) and 1,4BG (1,4-butanediol) were measured. The gas amounts were expressed in ppm by mass, calculated as decane.

[0223] GC-MS conditions: The gas was held at 50°C for 2 minutes, then heated to 380°C at 10°C / min, and the detected substances were calculated in terms of decane concentration. Apparatus: Shimadzu TD-20 (TD) / GC-2010 Plus (GC) / GC-MS-QP-2010 Ultra (MS) Column: UA5 0.25mm ID x 30m

[0224] <Flame Retardancy> The pellets obtained above were dried at 110°C for 5 hours, and then injection-molded into combustion test specimens (12.7 mm width × 127 mm length × 1.5 mm thickness) using an injection molding machine ("J-50AD" manufactured by The Japan Steel Works, Ltd.) under conditions of a cylinder temperature of 250°C and a mold temperature of 80°C. The obtained combustion test specimens were allowed to stand in an atmosphere of 70°C for 1 week, and then their flame retardancy was evaluated in accordance with the method of Subject 94 (UL94) of Underwriters Laboratories.

[0225] As is clear from the above results, the resin composition of the present invention was able to effectively suppress gas generation by containing a polybutylene terephthalate resin with a low titanium activity parameter.

[0226] Although the present invention has been described in detail with reference to specific embodiments, it will be apparent to those skilled in the art that various modifications can be made without departing from the spirit and scope of the invention.

Claims

1. A resin composition comprising a polybutylene terephthalate resin, an amorphous thermoplastic resin having a carbonate bond and / or an ester bond, and at least one polystyrene-based resin, wherein the polybutylene terephthalate resin has an active titanium parameter X of 25 or less.

2. A resin composition comprising a polybutylene terephthalate resin and at least one selected from the group consisting of an inorganic filler, a release agent and a stabilizer, wherein the polybutylene terephthalate resin has a total nitrogen element content of 0.1 to 3000 mass ppm and an active titanium parameter X shown below of 25 or less.

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

4. The resin composition according to any one of claims 1 to 3, further comprising a flame retardant.

5. The resin composition according to any one of claims 1 to 4, wherein the active titanium parameter X is 12 or less.

6. The resin composition according to any one of claims 1 to 5, wherein the polybutylene terephthalate resin contains 30 to 500 ppm by mass of titanium element.

7. The resin composition according to any one of claims 1 to 6, which contains an inorganic filler, and the inorganic filler is a fibrous reinforcing material.

8. The resin composition according to any one of claims 1 to 7, wherein the polybutylene terephthalate resin has a terminal carboxyl group concentration of 25 µmol / g or more.

9. The resin composition according to any one of claims 1 to 8, wherein the polybutylene terephthalate resin has an Mw / Mn ratio of 2.1 or more.

10. The resin composition according to any one of claims 1 to 9, further comprising recycled polyethylene terephthalate resin.

11. The resin composition according to any one of claims 1 to 10, wherein the polybutylene terephthalate resin has a total sulfur element content of 0.1 to 100 ppm by mass.

12. The resin composition according to any one of claims 1 to 11, wherein the polybutylene terephthalate resin contains 0.1 to 100 ppm by mass of sodium element.

13. The resin composition according to any one of claims 1 to 12, wherein the polybutylene terephthalate resin contains calcium element in an amount of 0.1 to 3,000 ppm by mass.

14. The resin composition according to any one of claims 1 to 13, wherein the polybutylene terephthalate resin has a terminal vinyl group concentration of 1 to 15 μmol / g.

15. The resin composition according to any one of claims 1 to 14, wherein the proportion α of active titanium in the polybutylene terephthalate resin, represented by the following formula (3), is 0.50 or less: α = X / M ... formula (3) (In formula (3), X is the active titanium parameter, and [M] is the titanium element concentration (ppm by mass) in the polybutylene terephthalate resin.) 16. The resin composition according to any one of claims 1 and 3 to 15, wherein the amorphous thermoplastic resin having a carbonate bond and / or an ester bond includes a polycarbonate resin.

17. The resin composition according to any one of claims 1 to 16, wherein the polybutylene terephthalate resin contains a polybutylene terephthalate resin derived from material recycling.

18. The resin composition according to any one of claims 1 to 17, further comprising a reactive compound.

19. The resin composition according to any one of claims 1 to 18, which is for injection molding.

20. Pellets of the resin composition according to any one of claims 1 to 19.

21. A molded article formed from the resin composition according to any one of claims 1 to 19.

22. A molded article formed from the pellets of claim 20.

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