Resin composition, pellet, and molded body

A resin composition combining polyphenylene ether, polyimide, and polycarbonate resins with specific structural units and additives addresses poor film processability and thermal degradation issues, resulting in improved tracking resistance and moldability.

WO2025225252A1PCT designated stage Publication Date: 2025-10-30GLOBAL POLYACETAL CO LTD
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Patent Information

Application Number
PCT/JP2025/011791
Authority / Receiving Office
WO · WO
Patent Type
Applications
Current Assignee / Owner
Priority Date
2024-04-25
Filing Date
2025-03-25
Publication Date
2025-10-30

AI Technical Summary

Technical Problem

Resin compositions containing polyphenylene ether and polyimide resins suffer from poor film processability and eye sludge formation during extrusion due to high melt-kneading temperatures, which can lead to thermal degradation products.

Method used

A resin composition comprising polyphenylene ether, polyimide, and polycarbonate resins, with specific structural units and ratios, along with the inclusion of a lubricant and ceramic particles, to improve film processability by lowering extrusion temperatures and preventing thermal degradation.

Benefits of technology

The composition achieves excellent film processability with reduced eye sludge formation, enhancing the tracking resistance and moldability of the resin.

✦ Generated by Eureka AI based on patent content.

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Abstract

The present invention provides a resin composition having excellent film processability, a pellet, and a molded body (in particular, a film). The present invention includes: a polyphenylene ether resin composed of a resin represented by formula (1) and / or an acid-modified product thereof; a polyimide resin; and a polycarbonate resin. The polyimide resin includes a repeating structural unit represented by formula (2) and a repeating structural unit represented by formula (3). The content ratio of the repeating structural unit represented by formula (2) to a total of 100 mol% of the repeating structural unit represented by formula (2) and the repeating structural unit represented by formula (3) is 20-70 mol% inclusive.
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Description

Resin composition, pellets, and molded body

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

[0002] Polyphenylene ether resin (PPE) is a resin that has excellent properties such as heat resistance, flame retardancy, electrical properties, and dimensional stability, as well as low specific gravity and hydrolysis resistance.

[0003] Resin compositions containing such polyphenylene ether resins (polyphenylene ether resin compositions) have been widely used as materials for various applications, such as electrical components, electronic device components, and vehicle components. Various properties are required of polyphenylene ether resin compositions depending on their applications. For example, when a polyphenylene ether resin composition is used as a spacer between batteries or a bus bar cover material in a battery unit including a battery pack or the like, the polyphenylene ether resin composition is required to have high tracking resistance in addition to the flame retardancy and thin-wall moldability required for the battery spacer or bus bar cover.

[0004] For example, Patent Document 1 discloses a composition that contains 45 to 65% by weight of PPE, 10 to 30% by weight of a polyalkenyl aromatic resin (styrene resin), 1 to 8% by weight of tricalcium phosphate, 3 to 15% by weight of an organic phosphate ester flame retardant, 5 to 10% by weight of titanium oxide, and 3 to 15% by weight of a reinforcing filler, and that exhibits a CTI of 350V or more according to the IEC 60112 standard.

[0005] International Publication No. 2009 / 040751

[0006] The present inventors have investigated blending a polyimide resin into a polyphenylene ether resin composition to improve the tracking resistance of the polyphenylene ether resin composition. However, they have found that when attempting to process a resin composition obtained by blending a polyphenylene ether resin with a polyimide resin into a film, the film processability may be poor. In particular, they have found that eye sludge may occur. The present invention aims to solve these problems and to provide a resin composition, pellets, and molded products (particularly films) that are excellent in film processability.

[0007] In light of the above-mentioned problems, the present inventors have conducted research and found that a resin composition with excellent film processability can be obtained by blending a polycarbonate resin with a resin composition containing a specified polyphenylene ether resin and a specified polyimide resin. Specifically, the above-mentioned problems have been solved by the following means. <1> A resin composition comprising a polyphenylene ether resin made of a resin represented by formula (1) and / or an acid-modified product thereof, a polyimide resin, and a polycarbonate resin, wherein the polyimide resin contains a repeating structural unit represented by formula (2) and a repeating structural unit represented by formula (3), and the content ratio of the repeating structural unit represented by formula (2) is 20 to 70 mol % relative to 100 mol % of the total of the repeating structural units represented by formula (2) and the repeating structural units represented by formula (3). (In formula (1), R 51 ~R 55 , and R 61 ~R 64 are each independently a hydrogen atom, a hydroxy group, or an alkyl group having 1 to 4 carbon atoms, and R 65 is a hydrogen atom or an alkyl group having 1 to 4 carbon atoms. n is the number of repeating structural units and is a number of 10 or more. (In formulas (2) and (3), R 1 is a divalent group having 6 to 22 carbon atoms and containing at least one alicyclic hydrocarbon structure. 2 is a divalent chain aliphatic group having 5 to 16 carbon atoms. 1 and X 2are each independently a tetravalent group having 6 to 22 carbon atoms and containing at least one aromatic ring.) <2> The resin composition according to <1>, further comprising a lubricant. <3> The resin composition according to <1> or <2>, further comprising a lubricant in an amount of 0.1 to 3 parts by mass per 100 parts by mass of the polyphenylene ether resin, polyimide resin, and polycarbonate resin. <4> The resin composition according to any one of <1> to <3>, wherein the mass ratio of the polyphenylene ether resin per 100 parts by mass of the polyphenylene ether resin and polyimide resin is 50 to 99 parts by mass. <5> The resin composition according to any one of <1> to <4>, further comprising 5 to 20 parts by mass of a flame retardant and 0.1 to 10 parts by mass of ceramic particles per 100 parts by mass of the polyphenylene ether resin, polyimide resin, and polycarbonate resin. <6> The resin composition according to <5>, wherein the flame retardant includes a phosphorus-based flame retardant. <7> The resin composition according to <5>, wherein the ceramic particles comprise titanium oxide particles. <8> The resin composition according to any one of <1> to <7>, further comprising a lubricant in an amount of 0.1 to 3 parts by mass per 100 parts by mass of the polyphenylene ether resin, polyimide resin, and polycarbonate resin together, wherein the mass ratio of the polyphenylene ether resin to the total 100 parts by mass of the polyphenylene ether resin and polyimide resin is 50 to 99 parts by mass, and further comprising 5 to 20 parts by mass of a flame retardant and 0.1 to 10 parts by mass of ceramic particles per 100 parts by mass of the polyphenylene ether resin, polyimide resin, and polycarbonate resin together, wherein the flame retardant comprises a phosphorus-based flame retardant, and the ceramic particles comprise titanium oxide particles. <9> Pellets of the resin composition according to any one of <1> to <8>. <10> A molded article formed from the resin composition according to any one of <1> to <8>. <11> A flat plate-like molded product formed from the resin composition according to any one of <1> to <8>.

[0008] The present invention makes it possible to provide a resin composition, pellets, and molded articles (particularly films) that are excellent in film processability.

[0009] 1 is a photograph showing the state of the film of Example 1 during extrusion. 2 is a photograph showing the state of the film of Comparative Example 1 during extrusion.

[0010] Hereinafter, an embodiment of the present invention (hereinafter simply referred to as "the present embodiment") will be described in detail. Note that the following present embodiment is an example for explaining the present invention, and the present invention is not limited to only this embodiment. In this specification, various physical property values ​​and characteristic values ​​are those at 23°C unless otherwise specified.

[0011] The flat-plate-shaped molded body in this specification is intended to include those in the shape of a film or sheet. The terms "film" and "sheet" refer to a generally flat molded body that is thin relative to its length and width, and are not particularly distinguished in this specification. Furthermore, the "film" and "sheet" in this specification may be single-layer or multi-layer, but single-layer is preferred. 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 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 at the time of abolition.

[0012] The resin composition of the present embodiment comprises a polyphenylene ether resin composed of a resin represented by formula (1) and / or an acid-modified product thereof, a polyimide resin, and a polycarbonate resin, wherein the polyimide resin comprises a repeating structural unit represented by formula (2) and a repeating structural unit represented by formula (3), and the content ratio of the repeating structural unit represented by formula (2) is 20 to 70 mol % relative to 100 mol % in total of the repeating structural unit represented by formula (2) and the repeating structural unit represented by formula (3). (In formula (1), R 51 ~R 55 , and R 61 ~R 64 are each independently a hydrogen atom, a hydroxy group, or an alkyl group having 1 to 4 carbon atoms, and R 65 is a hydrogen atom or an alkyl group having 1 to 4 carbon atoms. n is the number of repeating structural units and is a number of 10 or more. (In formulas (2) and (3), R 1 is a divalent group having 6 to 22 carbon atoms and containing at least one alicyclic hydrocarbon structure. 2 is a divalent chain aliphatic group having 5 to 16 carbon atoms. 1 and X 2 are each independently a tetravalent group containing at least one aromatic ring and having 6 to 22 carbon atoms.

[0013] By adopting such a configuration, a resin composition with excellent film processability can be obtained. That is, by blending a predetermined polyimide resin with a predetermined polyphenylene ether resin, the tracking resistance of the resin composition can be improved. However, when a resin composition blending a predetermined polyimide resin with a predetermined polyphenylene ether resin is extruded into a flat-plate molded body (film), eye gunk may occur. In this embodiment, to solve this problem, a polycarbonate resin is blended. It is presumed that blending a polycarbonate resin can lower the extrusion temperature of the resin composition, thereby suppressing the occurrence of eye gunk. That is, eye gunk is generated by volatile matter, moisture, degradation products, or poor dispersion of fillers and additives in the molten resin, and the higher the melt-kneading temperature (extrusion temperature), the more likely thermal degradation products are to occur. Polyphenylene ether, in particular, tends to generate eye gunk composed of thermal degradation products. In this embodiment, since a polyimide resin is used, the melt-kneading temperature (extrusion temperature) tends to be high. Therefore, it is presumed that when the polyimide resin is heated to a temperature at which it melts, the resin becomes more likely to produce a sticky residue derived from thermal degradation. In this embodiment, it is presumed that by blending a polycarbonate resin, which is easily mixed with the polyimide resin and has no melting point, the polyimide resin becomes compatible with the polycarbonate resin, making it possible to process the polyimide resin at a temperature lower than its melting point.

[0014] 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.

[0015] <Polyphenylene ether resin> The resin composition of the present embodiment contains a polyphenylene ether resin (sometimes simply referred to as a "polyphenylene ether resin" in this specification) composed of a resin represented by formula (1) and / or an acid-modified product thereof, and the polyphenylene ether resin is preferably a resin represented by formula (1). (In formula (1), R 51 ~R 55 , and R 61 ~R 64 are each independently a hydrogen atom, a hydroxy group, or an alkyl group having 1 to 4 carbon atoms, and R 65 is a hydrogen atom or an alkyl group having 1 to 4 carbon atoms. n is the number of repeating structural units and is a number of 10 or more.

[0016] In formula (1), R 51 ~R 55 , and R 61 ~R 65 The alkyl group having 1 to 4 carbon atoms in the formula (I) may be either linear or branched, and examples thereof include a methyl group, an ethyl group, an n-propyl group, an isopropyl group, an n-butyl group, an isobutyl group, a sec-butyl group, and a tert-butyl group. Among these, a methyl group, an ethyl group, an n-propyl group, or an isopropyl group is preferred, and a methyl group is more preferred.

[0017] In formula (1), R 51 , R 53 , R 61 , and R 63 is preferably a hydrogen atom or an alkyl group having 1 to 4 carbon atoms, more preferably a hydrogen atom or a methyl group, and even more preferably a hydrogen atom. 52 , R 54 , R 62 , and R 64 is preferably a hydrogen atom or an alkyl group having 1 to 4 carbon atoms, more preferably a hydrogen atom or a methyl group, and even more preferably a methyl group. 65 is preferably a hydrogen atom.

[0018] In formula (1), n ​​is a number of 10 or more, more preferably 20 or more, and although there is no particular upper limit, it is 300 or less.

[0019] As the polyphenylene ether resin, poly(2,6-dimethyl-1,4-phenylene ether) and 2,6-dimethylphenol / 2,3,6-trimethylphenol random copolymer are particularly preferred. Poly(2,6-dimethyl-1,4-phenylene ether) represented by formula (1-1) is particularly preferred. Polyphenylene ether resins having a specified number of terminal groups and copper content, as described in JP-A-2005-344065, can also be suitably used. (wherein n is the same as defined above.)

[0020] The intrinsic viscosity of the polyphenylene ether resin measured in chloroform at 30° C. is preferably 0.20 to 0.60 dL / g, more preferably 0.30 to 0.50 dL / g, and even more preferably 0.30 to 0.45 dL / g, from the viewpoints of exhibiting high flame retardancy and improving moldability. Two or more types of (a) polyphenylene ether resins having different intrinsic viscosities may be used in combination to achieve an intrinsic viscosity within this range.

[0021] The method for producing the polyphenylene ether resin used in the present embodiment is not particularly limited, and may be any known method, for example, a method of oxidatively polymerizing a monomer such as 2,6-dimethylphenol in the presence of an amine copper catalyst, in which the intrinsic viscosity can be controlled within a desired range by selecting the reaction conditions. The control of the intrinsic viscosity can be achieved by selecting conditions such as the polymerization temperature, polymerization time, and catalyst amount.

[0022] Examples of acid-modified resins represented by formula (1) include resins obtained by modifying the resin represented by formula (1) with a carboxylic acid or a carboxylic acid derivative. As the carboxylic acid or carboxylic acid derivative, unsaturated carboxylic acids and their derivatives are preferred from the viewpoint of reactivity with the resin represented by formula (1). Examples of unsaturated carboxylic acids include acrylic acid, methacrylic acid, maleic acid, fumaric acid, itaconic acid, crotonic acid, citraconic acid, sorbic acid, mesaconic acid, angelic acid, and the like. Examples of derivatives of unsaturated carboxylic acids include acid anhydrides, esters, amides, imides, and metal salts, among which acid anhydrides are preferred. Among the above, the acid-modified resin represented by formula (1) is preferably a resin obtained by modifying the resin represented by formula (1) with maleic acid or a maleic acid derivative (a maleic acid-modified resin represented by formula (1)) from the viewpoint of exhibiting high flame retardancy and availability.

[0023] Examples of the maleic acid modified resin represented by formula (1) include resins having a structure represented by formula (1-2) and / or formula (1-3). (In formula (1-2), R 51 ~R 55 , R 61 , R 63 , R 64 , R 65 and n each independently have the same meaning as in formula (1).

[0024] Formula (1-3) (In formula (1-3), R 51 ~R 55 , R 61 , R 63 , R 64 , R 65 and n each independently have the same meaning as in formula (1).

[0025] The polyphenylene ether resin used in this embodiment may be a recycled product (including recovered products, material recycled products, chemical recycled products, etc.), a rejected product, or a scrap material from molding a polyphenylene ether resin.

[0026] <Polycarbonate Resin> The resin composition of this embodiment contains a polycarbonate resin. The inclusion of a polycarbonate resin makes the resin compatible with the polyimide resin, thereby enabling the melting temperature of the resin composition to be lowered. The polycarbonate resin is not particularly limited as long as it contains an -[O-R-OC(═O)]- unit containing a carbonate bond in the molecular main chain (wherein R is an organic group, preferably a hydrocarbon group, more preferably an aliphatic group, an aromatic group, or one containing both an aliphatic group and an aromatic group, and further one having a linear or branched structure). In this embodiment, the polycarbonate resin is preferably an aromatic polycarbonate resin, and more preferably a polycarbonate resin having a bisphenol skeleton. By using such a polycarbonate resin, superior heat resistance and toughness can be achieved in the resulting molded article. In the present embodiment, the polycarbonate resin having a bisphenol skeleton preferably has 90 mol % or more of all structural units that have a bisphenol skeleton, more preferably 90 mol % or more of all structural units that have at least one skeleton of bisphenol A, bisphenol C, and bisphenol AP, and even more preferably 90 mol % or more of all structural units that have a bisphenol A skeleton.

[0027] The viscosity average molecular weight (Mv) of the polycarbonate resin is preferably 10,000 or more, more preferably 12,000 or more, and even more preferably 15,000 or more. The upper limit of the viscosity average molecular weight (Mv) of the polycarbonate resin is preferably 50,000 or less, more preferably 40,000 or less, even more preferably 30,000 or less, still more preferably 25,000 or less, and even more preferably 20,000 or less. By keeping it below the upper limit, the molding processability of the molded product tends to be further improved. The viscosity average molecular weight (Mv) is determined by using methylene chloride as a solvent and an Ubbelohde viscometer to determine the intrinsic viscosity [η] (unit: dL / g) at a temperature of 25°C, and then calculating the viscosity average molecular weight (Mv) using Schnell's viscosity formula, i.e., η = 1.23 × 10 -4 ×Mv 0.83When two or more types of polycarbonate resins are used, the viscosity average molecular weight is the viscosity average molecular weight of the mixture.

[0028] The method for producing the polycarbonate resin is not particularly limited, and polycarbonate resins produced by the conventionally known phosgene method (interfacial polymerization method) or melt method (ester interchange method) can be used. When the melt method is used, a polycarbonate resin in which the amount of OH groups in the terminal groups has been adjusted can be used.

[0029] The polycarbonate resin used in this embodiment may include recycled products. The recycled product refers to a polycarbonate resin derived from a molded product formed from polycarbonate resin, and refers to a product that has undergone some type of molding process on virgin polycarbonate resin. This includes polycarbonate resin molded products, rejected polycarbonate resin molded products, and scraps from the manufacture of polycarbonate resin molded products. Molded products include injection molded products, extrusion molded products, and molded products formed by other manufacturing methods. Examples of recycled polycarbonate resin include those obtained by material recycling, in which recovered used polycarbonate resin molded products are crushed and alkaline-cleaned to be reused as fibers, etc., those obtained by chemical recycling (chemical decomposition method), and those obtained by mechanical recycling. Chemical recycling involves chemically decomposing recovered used polycarbonate resin molded products to return them to their raw material level and resynthesize polycarbonate resin. On the other hand, mechanical recycling is a method that enables more reliable removal of dirt from polycarbonate resin molded products than material recycling by performing alkaline cleaning more rigorously than in the material recycling described above, or by vacuum drying at high temperatures. For example, recycled polycarbonate resin is obtained by removing foreign matter from used polycarbonate resin molded products, crushing and cleaning them, and then pelletizing them in an extruder. Examples of used polycarbonate resin molded products include disks, sheets (including films), meter covers, headlamp lenses, water bottles, and face plates for game and pachinko machines. Virgin products refer to products other than recycled products.

[0030] In addition to the above, for details of the polycarbonate resin, the descriptions in paragraphs 0013 to 0041 of JP-A-2021-084942, the descriptions in paragraphs 0030 to 0035 of JP-A-2021-119211, and the descriptions in paragraphs 0008 to 0064 of JP-A-2023-012167 can be referred to, and the contents thereof are incorporated herein by reference.

[0031] The content of the polycarbonate resin in the resin composition of this embodiment is preferably 1% by mass or more of the resin composition, more preferably 3% by mass or more, even more preferably 5% by mass or more, and even more preferably 8% by mass or more, and is preferably 15% by mass or less, and more preferably 10% by mass or less. 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 is in the above range.

[0032] <Polyimide Resin> The resin composition of the present embodiment includes a polyimide resin (sometimes simply referred to as a "polyimide resin" in this specification) that contains a repeating structural unit represented by formula (2) and a repeating structural unit represented by formula (3), and in which the content of the repeating structural unit represented by formula (2) is 20 to 70 mol % relative to 100 mol % in total of the repeating structural unit represented by formula (2) and the repeating structural unit represented by formula (3). (In formulas (2) and (3), R 1 is a divalent group having 6 to 22 carbon atoms and containing at least one alicyclic hydrocarbon structure. 2 is a divalent chain aliphatic group having 5 to 16 carbon atoms. 1 and X 2 are each independently a tetravalent group containing at least one aromatic ring and having 6 to 22 carbon atoms.

[0033] The polyimide resin used in this embodiment is a thermoplastic resin, and is preferably in the form of powder or pellets. Thermoplastic polyimide resins are distinguished from polyimide resins that do not have a glass transition temperature (Tg), or polyimide resins that decompose at a temperature lower than the glass transition temperature, and are formed by molding a polyimide precursor such as polyamic acid and then closing the imide ring.

[0034] The repeating unit of formula (2) is described in detail below. 1is a divalent group having 6 to 22 carbon atoms and containing at least one alicyclic hydrocarbon structure. Here, the alicyclic hydrocarbon structure refers to a ring derived from an alicyclic hydrocarbon compound, and the alicyclic hydrocarbon compound may be saturated or unsaturated, and may be monocyclic or polycyclic. Examples of alicyclic hydrocarbon structures include, but are not limited to, cycloalkane rings such as a cyclohexane ring, cycloalkene rings such as cyclohexene, bicycloalkane rings such as norbornane, and bicycloalkene rings such as norbornene. Among these, a cycloalkane ring is preferred, a cycloalkane ring having 4 to 7 carbon atoms is more preferred, and a cyclohexane ring is even more preferred. R 1 has 6 to 22 carbon atoms, preferably 8 to 17. 1 contains at least one alicyclic hydrocarbon structure, preferably 1 to 3.

[0035] R1 is preferably a divalent group represented by formula (R1-1) or formula (R1-2). (In formula (R1-1) and formula (R1-2), m11 and m12 each independently represent an integer of 0 to 2. m13 to m15 each independently represent an integer of 0 to 2.) In formula (R1-1) and formula (R1-2), m11 and m12 each independently represent preferably 0 or 1. m13 to m15 each independently represent preferably 0 or 1.

[0036] R 1 is particularly preferably a divalent group represented by formula (R1-3). In the divalent group represented by the above formula (R1-3), the positional relationship of the two methylene groups with respect to the cyclohexane ring may be either cis or trans, and the ratio of cis to trans may be any value.

[0037] In formula (2), X 1is a tetravalent group having 6 to 22 carbon atoms and containing at least one aromatic ring. The aromatic ring may be a single ring or a condensed ring, and examples thereof include a benzene ring, a naphthalene ring, an anthracene ring, and a tetracene ring, but are not limited to these. Among these, a benzene ring and a naphthalene ring are preferred, and a benzene ring is more preferred. X 1 has 6 to 22 carbon atoms, preferably 6 to 18. 1 contains at least one aromatic ring, preferably 1 to 3.

[0038] X 1 is preferably a tetravalent group represented by any one of the following formulae (X-1) to (X-4). (In formulas (X-1) to (X-4), R 11 ~R 18 are each independently an alkyl group having 1 to 4 carbon atoms. 11 ~p 13 are each independently an integer of 0 to 2. p14, p15, p16 and p18 are each independently an integer of 0 to 3. p17 is an integer of 0 to 4. L 11 ~L 13 are each independently a single bond, an ether group, a carbonyl group, or an alkylene group having 1 to 4 carbon atoms.

[0039] In formulas (X-1) to (X-4), p11 to p13 are each independently preferably 0. p14, p15, p16, and p18 are each independently preferably 0. p17 is preferably 0. 1 is a tetravalent group having 6 to 22 carbon atoms and containing at least one aromatic ring, and therefore, R 12 , R 13 , p12 and p13 are selected so that the number of carbon atoms in the tetravalent group represented by formula (X-2) is in the range of 10 to 22. Similarly, L in formula (X-3) 11 , R 14 , R 15 , p14 and p15 are selected so that the number of carbon atoms of the tetravalent group represented by formula (X-3) is in the range of 12 to 22, and L in formula (X-4) 12 , L 13 , R 16, R 17 , R 18 , p 16 , p 17 and p 18 is selected so that the number of carbon atoms in the tetravalent group represented by formula (X-4) falls within the range of 18 to 22.

[0040] X 1 is particularly preferably a tetravalent group represented by formula (X-5) or (X-6).

[0041] Next, the repeating structural unit of formula (3) will be described in detail below. 2 is a divalent chain aliphatic group having 5 to 16 carbon atoms, preferably 6 to 14 carbon atoms, more preferably 7 to 12 carbon atoms, and even more preferably 8 to 10 carbon atoms. Here, the chain aliphatic group means a group derived from a chain aliphatic compound, and the chain aliphatic compound may be saturated or unsaturated, linear or branched, and may contain a heteroatom such as an oxygen atom. 2 is preferably an alkylene group having 5 to 16 carbon atoms, more preferably an alkylene group having 6 to 14 carbon atoms, even more preferably an alkylene group having 7 to 12 carbon atoms, and among these, preferably an alkylene group having 8 to 10 carbon atoms. The alkylene group may be a linear alkylene group or a branched alkylene group, but is preferably a linear alkylene group. 2 is preferably at least one selected from the group consisting of an octamethylene group and a decamethylene group, and particularly preferably an octamethylene group.

[0042] Also, R 2 Another preferred embodiment of is a divalent chain aliphatic group containing an ether group and having 5 to 16 carbon atoms. The number of carbon atoms is preferably 6 to 14, more preferably 7 to 12, and even more preferably 8 to 10. Among these, a divalent group represented by formula (R2-1) or formula (R2-2) is preferred. (In formulas (R2-1) and (R2-2), m21 and m22 each independently represent an integer of 1 to 15. m23 to m25 each independently represent an integer of 1 to 14.)

[0043] In formula (R2-1), m21 and m22 each independently represent preferably 1 to 13, more preferably 1 to 11, and even more preferably 1 to 9. m23 to m25 each independently represent preferably 1 to 12, more preferably 1 to 10, and even more preferably 1 to 8.

[0044] In addition, R 2 is a divalent chain aliphatic group having 5 to 16 carbon atoms (preferably 6 to 14 carbon atoms, more preferably 7 to 12 carbon atoms, and even more preferably 8 to 10 carbon atoms), and therefore m21 and m22 in formula (R2-1) are selected so that the number of carbon atoms in the divalent group represented by formula (R2-1) is within the range of 5 to 16 (preferably 6 to 14 carbon atoms, more preferably 7 to 12 carbon atoms, and even more preferably 8 to 10 carbon atoms). In other words, m21 + m22 is 5 to 16 (preferably 6 to 14, more preferably 7 to 12, and even more preferably 8 to 10 carbon atoms). Similarly, m23 to m25 in formula (R2-2) are selected so that the number of carbon atoms in the divalent group represented by formula (R2-2) is within the range of 5 to 16 (preferably 6 to 14 carbon atoms, more preferably 7 to 12 carbon atoms, and even more preferably 8 to 10 carbon atoms). That is, m23+m24+m25 is 5 to 16 (preferably 6 to 14 carbon atoms, more preferably 7 to 12 carbon atoms, and even more preferably 8 to 10 carbon atoms).

[0045] X 2 is X in formula (2) 1 The definitions and preferred embodiments are the same as above.

[0046] The content ratio of the repeating structural unit of formula (2) relative to the total of the repeating structural units of formula (2) and formula (3) is 20 to 70 mol%. When the content ratio of the repeating structural unit of formula (2) is within the above range, the polyimide resin can be sufficiently crystallized even in a typical injection molding cycle. By setting the content ratio to 20 mol% or more, moldability is improved, and by setting it to 70 mol% or less, crystallinity and heat resistance tend to be improved. From the viewpoint of achieving high crystallinity, the content ratio of the repeating structural unit of formula (2) relative to the total of the repeating structural units of formula (2) and formula (3) is preferably 65 mol% or less, more preferably 60 mol% or less, and even more preferably 50 mol% or less. In particular, the content ratio of the repeating structural unit of formula (2) relative to the total of the repeating structural units of formula (2) and formula (3) is preferably 20 mol% or more but less than 40 mol%. Within this range, the crystallinity of the polyimide resin is high, and a resin composition having better heat resistance can be obtained. From the viewpoint of moldability, the content ratio is preferably 25 mol% or more, more preferably 30 mol% or more, and even more preferably 32 mol% or more, and from the viewpoint of achieving high crystallinity, it is even more preferably 35 mol% or less.

[0047] The total content ratio of the repeating structural unit of formula (2) and the repeating structural unit of formula (3) relative to all repeating structural units constituting the polyimide resin is preferably 50 to 100 mol %, more preferably 75 to 100 mol %, even more preferably 80 to 100 mol %, and still more preferably 85 to 100 mol %.

[0048] The polyimide resin may further contain a repeating structural unit of formula (4). In that case, the content ratio of the repeating structural unit of formula (4) with respect to the total of the repeating structural unit of formula (2) and the repeating structural unit of formula (3) is preferably 25 mol% or less. On the other hand, the lower limit is not particularly limited and may exceed 0 mol%. From the viewpoint of improving heat resistance, the content ratio is preferably 5 mol% or more, more preferably 10 mol% or more, and from the viewpoint of maintaining crystallinity, it is preferably 20 mol% or less, more preferably 15 mol% or less. Formula (4) (In formula (4), R 3 is a divalent group having 6 to 22 carbon atoms containing at least one aromatic ring. X 3 is a tetravalent group having 6 to 22 carbon atoms containing at least one aromatic ring.)

[0049] R 3 is a divalent group having 6 to 22 carbon atoms containing at least one aromatic ring. The aromatic ring may be a monocyclic ring or a condensed ring, and examples include a benzene ring, a naphthalene ring, an anthracene ring, and a tetracene ring, but are not limited thereto. Among these, a benzene ring and a naphthalene ring are preferable, and a benzene ring is more preferable. The carbon number of R 3 is 6 to 22, preferably 6 to 18. R 3 contains at least one aromatic ring, preferably 1 to 3. Further, a monovalent or divalent electron-withdrawing group may be bonded to the aromatic ring. Examples of the monovalent electron-withdrawing group include a nitro group, a cyano group, a p-toluenesulfonyl group, a halogen, a halogenated alkyl group, a phenyl group, an acyl group, etc. Examples of the divalent electron-withdrawing group include an alkylene fluoride group (for example, -C(CF 3 ), -(CF 2 ), -(where p is an integer of 1 to 10)), and in addition to such a halogenated alkylene group, -CO-, -SO 2 ), -SO-, -CONH-, -COO-, etc. p are included. 2

[0050] R 3is preferably a divalent group represented by formula (R4-1) or formula (R4-2). (In formula (R4-1) and formula (R4-2), m31 and m32 are each independently an integer of 0 to 2. m33 and m34 are each independently an integer of 0 to 2. R 21 , R 22 , and R 23 are each independently an alkyl group having 1 to 4 carbon atoms, an alkenyl group having 2 to 4 carbon atoms, or an alkynyl group having 2 to 4 carbon atoms. p21, p22, and p23 are integers of 0 to 4. L 21 is a single bond, an ether group, a carbonyl group, or an alkylene group having 1 to 4 carbon atoms.)

[0051] In formula (R4-1) and formula (R4-2), m31 and m32 are each independently preferably 0 or 1. m33 and m34 are each independently preferably 0 or 1. Since R 3 is a divalent group having 6 to 22 carbon atoms containing at least one aromatic ring, m31, m32, R 21 [[ID=1十七]]and p21 in formula (R4-1) are selected so that the number of carbon atoms of the divalent group represented by formula (R4-1) falls within the range of 6 to 22. Similarly, L 21 , m33, m34, R 22 , R 23 , p22, and p23 in formula (R3-2) are selected so that the number of carbon atoms of the divalent group represented by formula (R3-2) falls within the range of 12 to 22.

[0052] X 3 is defined in the same manner as X 1 in formula (2), and the preferred embodiments are also the same.

[0053] The polyimide resin may further contain a repeating structural unit represented by the following formula (5). Formula (5) (In formula (5), R 4 is a divalent group containing -SO 2 - or Si(Rx)(Ry)O-, and Rx and Ry each independently represent a linear aliphatic group having 1 to 3 carbon atoms or a phenyl group. X 4is a tetravalent group having 6 to 22 carbon atoms and containing at least one aromatic ring. 4 is X in formula (2) 1 The definitions and preferred embodiments are the same as above.

[0054] Although there are no particular limitations on the terminal structure of the polyimide resin, it is preferable that the polyimide resin has a chain aliphatic group having 5 to 14 carbon atoms at the terminal. The chain aliphatic group may be saturated or unsaturated, and may be linear or branched. When the polyimide resin has the above-mentioned specific group at the terminal, a resin composition with excellent heat aging resistance can be obtained. Examples of saturated chain aliphatic groups having 5 to 14 carbon atoms include an n-pentyl group, an n-hexyl group, an n-heptyl group, an n-octyl group, an n-nonyl group, an n-decyl group, an n-undecyl group, a lauryl group, an n-tridecyl group, an n-tetradecyl group, an isopentyl group, a neopentyl group, a 2-methylpentyl group, a 2-methylhexyl group, a 2-ethylpentyl group, a 3-ethylpentyl group, an isooctyl group, a 2-ethylhexyl group, a 3-ethylhexyl group, an isononyl group, a 2-ethyloctyl group, an isodecyl group, an isododecyl group, an isotridecyl group, and an isotetradecyl group. Examples of unsaturated chain aliphatic groups having 5 to 14 carbon atoms include 1-pentenyl, 2-pentenyl, 1-hexenyl, 2-hexenyl, 1-heptenyl, 2-heptenyl, 1-octenyl, 2-octenyl, nonenyl, decenyl, dodecenyl, tridecenyl, and tetradecenyl groups. Among these, the chain aliphatic groups are preferably saturated chain aliphatic groups, and more preferably saturated linear chain aliphatic groups. Furthermore, from the viewpoint of obtaining heat aging resistance, the chain aliphatic groups preferably have 6 or more carbon atoms, more preferably 7 or more carbon atoms, and even more preferably 8 or more carbon atoms, and preferably have 12 or less carbon atoms, more preferably 10 or less carbon atoms, and even more preferably have 9 or less carbon atoms. The chain aliphatic groups may be of one type, or two or more types. The chain aliphatic group is particularly preferably at least one selected from the group consisting of an n-octyl group, an isooctyl group, a 2-ethylhexyl group, an n-nonyl group, an isononyl group, an n-decyl group, and an isodecyl group, further preferably at least one selected from the group consisting of an n-octyl group, an isooctyl group, a 2-ethylhexyl group, an n-nonyl group, and an isononyl group, and most preferably at least one selected from the group consisting of an n-octyl group, an isooctyl group, and a 2-ethylhexyl group.From the viewpoint of heat aging resistance, the polyimide resin preferably has, at its terminals, only chain aliphatic groups having 5 to 14 carbon atoms in addition to terminal amino groups and terminal carboxy groups. When a group other than the above is present at its terminals, the content thereof is preferably 10 mol % or less, more preferably 5 mol % or less, relative to the chain aliphatic groups having 5 to 14 carbon atoms.

[0055] From the viewpoint of exhibiting excellent heat aging resistance, the content of the chain aliphatic groups having 5 to 14 carbon atoms in the polyimide resin is preferably 0.01 mol% or more, more preferably 0.1 mol% or more, and even more preferably 0.2 mol% or more, based on 100 mol% of the total of all repeating structural units constituting the polyimide resin. Furthermore, in order to ensure a sufficient molecular weight and obtain good mechanical properties, the content of the chain aliphatic groups having 5 to 14 carbon atoms in the polyimide resin is preferably 10 mol% or less, more preferably 6 mol% or less, and even more preferably 3.5 mol% or less, based on 100 mol% of the total of all repeating structural units constituting the polyimide resin. The content of the chain aliphatic groups having 5 to 14 carbon atoms in the polyimide resin can be determined by depolymerizing the polyimide resin.

[0056] The polyimide resin preferably has a melting point of 360°C or lower and a glass transition temperature of 150°C or higher. From the viewpoint of heat resistance, the melting point of the polyimide resin is more preferably 280°C or higher, and from the viewpoint of achieving high moldability, it is preferably 345°C or lower, more preferably 340°C or lower, and even more preferably 335°C or lower. From the viewpoint of heat resistance, the glass transition temperature of the polyimide resin is more preferably 160°C or higher, more preferably 170°C or higher, and from the viewpoint of achieving high moldability, it is preferably 250°C or lower, more preferably 230°C or lower, and even more preferably 200°C or lower. The melting point and glass transition temperature of the polyimide resin can both be measured by a differential scanning calorimeter. Furthermore, from the viewpoint of improving crystallinity, heat resistance, mechanical strength, and chemical resistance, the polyimide resin preferably has a heat value of 5.0 mJ / mg or more, more preferably 10.0 mJ / mg or more, and even more preferably 17.0 mJ / mg or more, of the heat value of the exothermic crystallization peak observed when the polyimide resin is melted and then cooled at a temperature decreasing rate of 20°C / min, as measured by a differential scanning calorimeter. The upper limit of the heat value of crystallization is not particularly limited, but is usually 45.0 mJ / mg or less. The melting point, glass transition temperature, and heat value of crystallization of the polyimide resin can be specifically measured by the methods described in the Examples.

[0057] The logarithmic viscosity of a 0.5% by mass solution of polyimide resin in concentrated sulfuric acid at 30°C is preferably in the range of 0.2 to 2.0 dL / g, more preferably 0.3 to 1.8 dL / g. If the logarithmic viscosity is 0.2 dL / g or higher, sufficient mechanical strength can be obtained when the resulting resin composition is molded into a molded article, while if it is 2.0 dL / g or lower, moldability and handleability are improved. The logarithmic viscosity μ is calculated by measuring the flow times of concentrated sulfuric acid and the polyimide resin solution at 30°C using a Cannon-Fenske viscometer and using the following formula: μ = ln(ts / t0) / C, where t0 is the flow time of concentrated sulfuric acid, ts is the flow time of polyimide resin solution, and C is 0.5 (g / dL).

[0058] The weight-average molecular weight Mw of the polyimide resin is preferably in the range of 10,000 to 150,000, more preferably 15,000 to 100,000, even more preferably 20,000 to 80,000, still more preferably 30,000 to 70,000, and even more preferably 35,000 to 65,000. If the weight-average molecular weight Mw of the polyimide resin is 10,000 or more, the mechanical strength of the resulting molded article will be good; if it is 40,000 or more, the stability of the mechanical strength will be good; and if it is 150,000 or less, the moldability will be good. The weight-average molecular weight Mw of the polyimide resin can be measured by gel permeation chromatography (GPC) using polymethyl methacrylate (PMMA) as a standard sample.

[0059] (Method for Producing Polyimide Resin) Polyimide resin can be produced by reacting a tetracarboxylic acid component with a diamine component, wherein the tetracarboxylic acid component contains a tetracarboxylic acid and / or a derivative thereof having at least one aromatic ring, and the diamine component contains a diamine having at least one alicyclic hydrocarbon structure and a chain aliphatic diamine.

[0060] The tetracarboxylic acid containing at least one aromatic ring is preferably a compound in which four carboxy groups are directly bonded to the aromatic ring, and may contain an alkyl group in the structure. The tetracarboxylic acid preferably has 6 to 26 carbon atoms. Examples of the tetracarboxylic acid include pyromellitic acid, 2,3,5,6-toluenetetracarboxylic acid, 3,3',4,4'-benzophenonetetracarboxylic acid, 3,3',4,4'-biphenyltetracarboxylic acid, and 1,4,5,8-naphthalenetetracarboxylic acid. Among these, pyromellitic acid is more preferred.

[0061] Examples of derivatives of tetracarboxylic acids containing at least one aromatic ring include anhydrides or alkyl esters of tetracarboxylic acids containing at least one aromatic ring. The tetracarboxylic acid derivatives preferably have 6 to 38 carbon atoms. Examples of anhydrides of tetracarboxylic acids include pyromellitic monoanhydride, pyromellitic dianhydride, 2,3,5,6-toluenetetracarboxylic dianhydride, 3,3',4,4'-diphenylsulfonetetracarboxylic dianhydride, 3,3',4,4'-benzophenonetetracarboxylic dianhydride, 3,3',4,4'-biphenyltetracarboxylic dianhydride, and 1,4,5,8-naphthalenetetracarboxylic dianhydride. Examples of alkyl esters of tetracarboxylic acids include dimethyl pyromellitic acid, diethyl pyromellitic acid, dipropyl pyromellitic acid, diisopropyl pyromellitic acid, dimethyl 2,3,5,6-toluenetetracarboxylate, dimethyl 3,3',4,4'-diphenylsulfonetetracarboxylate, dimethyl 3,3',4,4'-benzophenonetetracarboxylate, dimethyl 3,3',4,4'-biphenyltetracarboxylate, dimethyl 1,4,5,8-naphthalenetetracarboxylate, etc. In the alkyl esters of tetracarboxylic acids, the alkyl group preferably has 1 to 3 carbon atoms.

[0062] As the tetracarboxylic acid and / or derivative thereof containing at least one aromatic ring, at least one compound selected from the above may be used alone, or two or more compounds may be used in combination.

[0063] The diamine containing at least one alicyclic hydrocarbon structure preferably has 6 to 22 carbon atoms, and examples thereof include 1,2-bis(aminomethyl)cyclohexane, 1,3-bis(aminomethyl)cyclohexane, 1,4-bis(aminomethyl)cyclohexane, 1,2-cyclohexanediamine, 1,3-cyclohexanediamine, 1,4-cyclohexanediamine, 4,4'-diaminodicyclohexylmethane, 4,4'-methylenebis(2-methylcyclohexylamine), carvonediamine, limonenediamine, isophoronediamine, norbornanediamine, bis(aminomethyl)tricyclo[5.2.1.02,6]decane, 3,3'-dimethyl-4,4'-diaminodicyclohexylmethane, and 4,4'-diaminodicyclohexylpropane. These compounds may be used alone, or two or more compounds selected from these may be used in combination. Of these, 1,3-bis(aminomethyl)cyclohexane is preferred. Diamines containing an alicyclic hydrocarbon structure generally have structural isomers, but the ratio of cis / trans isomers is not limited.

[0064] The chain aliphatic diamine may be linear or branched, and preferably has 5 to 16 carbon atoms, more preferably 6 to 14, and even more preferably 7 to 12. Furthermore, as long as the chain portion has 5 to 16 carbon atoms, it may contain an ether bond therebetween. Preferred examples of the chain aliphatic diamine include 1,5-pentamethylenediamine, 2-methylpentane-1,5-diamine, 3-methylpentane-1,5-diamine, 1,6-hexamethylenediamine, 1,7-heptamethylenediamine, 1,8-octamethylenediamine, 1,9-nonamethylenediamine, 1,10-decamethylenediamine, 1,11-undecamethylenediamine, 1,12-dodecamethylenediamine, 1,13-tridecamethylenediamine, 1,14-tetradecamethylenediamine, 1,16-hexadecamethylenediamine, and 2,2'-(ethylenedioxy)bis(ethyleneamine). The chain aliphatic diamine may be used alone or in combination of two or more. Among these, chain aliphatic diamines having 8 to 10 carbon atoms are preferably used, and in particular, at least one selected from the group consisting of 1,8-octamethylenediamine and 1,10-decamethylenediamine is preferably used.

[0065] In producing a polyimide resin, the molar ratio of the amount of the diamine containing at least one alicyclic hydrocarbon structure charged to the total amount of the diamine containing at least one alicyclic hydrocarbon structure and the chain aliphatic diamine is preferably 20 to 70 mol %. This molar ratio is preferably 25 mol % or more, more preferably 30 mol % or more, and even more preferably 32 mol % or more. From the viewpoint of achieving high crystallinity, it is preferably 60 mol % or less, more preferably 50 mol % or less, even more preferably less than 40 mol %, and even more preferably 35 mol % or less.

[0066] The diamine component may also contain a diamine containing at least one aromatic ring. The diamine containing at least one aromatic ring preferably has 6 to 22 carbon atoms, and examples thereof include ortho-xylylenediamine, meta-xylylenediamine, para-xylylenediamine, 1,2-diethynylbenzenediamine, 1,3-diethynylbenzenediamine, 1,4-diethynylbenzenediamine, 1,2-diaminobenzene, 1,3-diaminobenzene, 1,4-diaminobenzene, 4,4'-diaminodiphenyl ether, 3,4'-diaminodiphenyl ether, 4,4'-diaminodiphenylmethane, α,α'-bis(4-aminophenyl)1,4-diisopropylbenzene, α,α'-bis(3-aminophenyl)-1,4-diisopropylbenzene, 2,2-bis[4-(4-aminophenoxy)phenyl]propane, 2,6-diaminonaphthalene, and 1,5-diaminonaphthalene.

[0067] In the above, the molar ratio of the amount of the diamine containing at least one aromatic ring to the total amount of the diamine containing at least one alicyclic hydrocarbon structure and the chain aliphatic diamine is preferably 25 mol% or less. On the other hand, the lower limit is not particularly limited, as long as it is greater than 0 mol%. From the viewpoint of improving heat resistance, the molar ratio is preferably 5 mol% or more, more preferably 10 mol% or more. On the other hand, from the viewpoint of maintaining crystallinity, the molar ratio is preferably 20 mol% or less, more preferably 15 mol% or less. Furthermore, from the viewpoint of reducing coloration of the polyimide resin, the molar ratio is preferably 12 mol% or less, more preferably 10 mol% or less, even more preferably 5 mol% or less, and even more preferably 0 mol%.

[0068] When producing the polyimide resin, the ratio of the amount of the tetracarboxylic acid component to the amount of the diamine component charged is preferably 0.9 to 1.1 moles of the diamine component per mole of the tetracarboxylic acid component.

[0069] Furthermore, when producing a polyimide resin, a terminal-capping agent may be mixed in addition to the tetracarboxylic acid component and the diamine component. The terminal-capping agent is preferably at least one selected from the group consisting of monoamines and dicarboxylic acids. The amount of terminal-capping agent used may be any amount sufficient to introduce the desired amount of terminal groups into the polyimide resin, and is preferably 0.0001 to 0.1 mol, more preferably 0.001 to 0.06 mol, and even more preferably 0.002 to 0.035 mol per mol of the tetracarboxylic acid and / or its derivative. Among these, monoamine terminal-capping agents are preferred. From the viewpoint of introducing the aforementioned linear aliphatic group having 5 to 14 carbon atoms to the terminal of the polyimide resin to improve heat aging resistance, monoamines having a linear aliphatic group having 5 to 14 carbon atoms are more preferred, and monoamines having a saturated linear aliphatic group having 5 to 14 carbon atoms are even more preferred. The end-capping agent is particularly preferably at least one selected from the group consisting of n-octylamine, isooctylamine, 2-ethylhexylamine, n-nonylamine, isononylamine, n-decylamine, and isodecylamine, more preferably at least one selected from the group consisting of n-octylamine, isooctylamine, 2-ethylhexylamine, n-nonylamine, and isononylamine, and most preferably at least one selected from the group consisting of n-octylamine, isooctylamine, and 2-ethylhexylamine.

[0070] As a polymerization method for producing a polyimide resin, a known polymerization method can be applied, and the method described in WO 2016 / 147996 can be referred to, the contents of which are incorporated herein by reference.

[0071] The polyimide resin used in this embodiment may be a recycled product (including recovered products, material recycled products, chemical recycled products, etc.), a rejected product, or a waste material from polyimide resin molding.

[0072] <Blend of Polyphenylene Ether Resin, Polyimide Resin, and Polycarbonate Resin> Next, the blend ratio of polyphenylene ether resin, polyimide resin, and polycarbonate resin in the resin composition of this embodiment will be described. In the resin composition of this embodiment, the mass ratio of the polyphenylene ether resin relative to 100 parts by mass of the polyphenylene ether resin and the polyimide resin is preferably 50 to 99 parts by mass. Furthermore, relative to 100 parts by mass of the polyphenylene ether resin and the polyimide resin, the mass ratio of the polyphenylene ether resin is preferably 55 parts by mass or more, more preferably 60 parts by mass or more, even more preferably 70 parts by mass or more, even more preferably 80 parts by mass or more, and even more preferably 85 parts by mass or more, and is preferably 95 parts by mass or less, and may be 90 parts by mass or less. By setting the mass ratio at or above the lower limit, flame retardancy tends to be further improved. Furthermore, by setting the mass ratio at or below the upper limit, tracking resistance tends to be further improved. The resin composition of this embodiment may contain only one type of polyphenylene ether resin and one type of polyimide resin, or two or more types of either one or both. When two or more types are contained, it is preferable that the total amount is within the above range. In the resin composition of this embodiment, the polycarbonate resin is preferably contained in an amount of 1 part by mass or more, more preferably 5 parts by mass or more, and even more preferably 7 parts by mass or more, per 100 parts by mass of the total of the polyphenylene ether resin, the polyimide resin, and the polycarbonate resin. Furthermore, it is preferable that the amount is 20 parts by mass or less, and more preferably 15 parts by mass or less. By setting the amount to be equal to or greater than the above lower limit, the generation of sludge during film molding tends to be more effectively suppressed. By setting the amount to be equal to or less than the above upper limit, the tracking resistance of the obtained molded body is significantly improved, and a resin composition with excellent flame retardancy is obtained.

[0073] In the resin composition of the present embodiment, the total amount of the polyphenylene ether resin, polyimide resin, and polycarbonate resin is preferably 70% by mass or more, more preferably 75% by mass or more, even more preferably 80% by mass or more, and even more preferably 85% by mass or more, based on 100% by mass of the resin composition. It may be 90% by mass or more, and preferably 99% by mass or less, and may be 95% by mass or less, or may be 90% by mass or less.

[0074] <Lubricant> The resin composition of this embodiment may contain a lubricant. The incorporation of a lubricant tends to further improve the tracking resistance and flame retardancy of the resulting molded article. This is presumably because the lubricant is less likely to cause carbonized residue on the material surface and also less likely for the resin to remain or adhere to the die outlet during extrusion (suppressing scum), thereby reducing the risk of contamination with components deteriorated by heat or oxidation. Examples of lubricants include aliphatic carboxylic acids, salts of aliphatic carboxylic acids, esters of aliphatic carboxylic acids and alcohols, aliphatic hydrocarbon compounds with a number-average molecular weight of 200 to 15,000, polysiloxane-based silicone oils, ketone waxes, and light amides. Aliphatic carboxylic acids, salts of aliphatic carboxylic acids, and esters of aliphatic carboxylic acids and alcohols are preferred, with salts of aliphatic carboxylic acids being more preferred, metal stearates being even more preferred, calcium stearate and zinc stearate being even more preferred, and zinc stearate being even more preferred. For details of the lubricant, please refer to paragraphs 0055 to 0061 of JP 2018-095706 A, the contents of which are incorporated herein by reference. When the resin composition of this embodiment contains a lubricant, the content thereof is preferably 0.1 parts by mass or more, more preferably 0.5 parts by mass or more, and even more preferably 0.8 parts by mass or more, relative to 100 parts by mass of the total of the polyphenylene ether resin, polyimide resin, and polycarbonate resin. It is also preferably 3 parts by mass or less, more preferably 2.5 parts by mass or less, even more preferably 2 parts by mass or less, and even more preferably 1.5 parts by mass or less. By setting the content at or above the lower limit, the effect of suppressing the buildup and tracking resistance tend to be further improved. Furthermore, by setting the content at or below the upper limit, it is possible to effectively suppress the lubricant from bleeding out, and it tends to be possible to effectively suppress poor appearance and the lubricant itself from becoming a cause of buildup. Furthermore, by setting the content at or below the upper limit, it tends to be possible to suppress the amount of gas generated during heat processing. The resin composition of the present embodiment may contain only one type of lubricant or may contain two or more types. When two or more types are contained, the total amount is preferably in the above range.

[0075] <Ceramic Particles> It is preferable to include ceramic particles. By including ceramic particles, the tracking resistance of a molded article obtained from the resin composition can be improved. Ceramic particles are usually insulating, and the dispersion of such insulating components tends to effectively suppress the formation of conductive circuits that cause tracking breakdown. In addition, the formation of holes when the resin composition of this embodiment is extruded into a flat-plate molded article (particularly, a film) can be effectively suppressed. This is presumably because the incorporation of ceramic particles allows the polyimide resin to be more effectively dispersed in the molded article. In particular, it is presumed that the resin composition of this embodiment, by including ceramic particles, can disperse the polyphenylene ether resin, polyimide resin, and polycarbonate resin well even without the inclusion of a compatibilizer, and thus a good flat-plate molded article (particularly, a film) can be molded.

[0076] The median diameter (D50) of the ceramic particles used in this embodiment is preferably 0.01 μm or more, more preferably 0.05 μm or more, even more preferably 0.1 μm or more, even more preferably 0.15 μm or more, even more preferably 0.2 μm or more, and preferably 30 μm or less, more preferably 25 μm or less, even more preferably 20 μm or less, even more preferably 15 μm or less, and even more preferably 10 μm or less. By setting the diameter to be equal to or greater than the lower limit, tracking resistance tends to be further improved. Furthermore, by setting the diameter to be equal to or less than the upper limit, the impact resistance and toughness of the resulting molded body tend to be improved. The median diameter (D50) is measured according to a laser diffraction / scattering method. When the resin composition of this embodiment contains two or more types of ceramic particles, the median diameter of the ceramic particles is the median diameter of the mixture.

[0077] The type of ceramic particles is not particularly limited, but is preferably at least one selected from alumina particles, titanium oxide, yttrium oxide particles, silicon nitride particles, silicon carbide particles, magnesium oxide particles, calcium oxide particles, iron oxide particles, copper oxide particles, chromium oxide particles, boron oxide particles, silicon dioxide particles, and nickel oxide particles, and titanium oxide particles are preferred.

[0078] The ceramic particles may be surface-treated with at least one compound selected from polyorganohydrogensiloxanes and organopolysiloxanes. In this case, the amount of the siloxane compound attached to the ceramic particles is preferably 0.1 to 5 mass % of the ceramic particles.

[0079] The content of the ceramic particles in the resin composition of this embodiment is preferably 0.1 parts by mass or more, more preferably 0.5 parts by mass or more, and even more preferably 1 part by mass or more, per 100 parts by mass of the total of the polyphenylene ether resin, polyimide resin, and polycarbonate resin. It is also preferably 10 parts by mass or less, more preferably 8 parts by mass or less, even more preferably 6 parts by mass or less, even more preferably 4 parts by mass or less, and even more preferably 3 parts by mass or less. By setting the content at or above the lower limit, the tracking resistance of the resin composition or molded article tends to be further improved. Furthermore, by setting the content at or below the upper limit, the decrease in impact resistance and toughness of the resulting molded article tends to be more effectively suppressed. The resin composition of this embodiment may contain only one type of ceramic particles, or may contain two or more types. When two or more types are contained, the total amount is preferably within the above range.

[0080] <Flame Retardant> The resin composition of this embodiment preferably contains a flame retardant. By including a flame retardant, the flame retardancy of the resulting molded article can be improved. The type of flame retardant is not particularly limited, and known flame retardants can be used. Examples include phosphorus-based flame retardants, halogen-based flame retardants, and organometallic salt-based flame retardants. Phosphorus-based flame retardants and halogen-based flame retardants are preferred, and phosphorus-based flame retardants are more preferred. By using a phosphorus-based flame retardant, the flame retardancy of the resin composition can be more effectively improved and the viscosity during heat processing tends to be reduced.

[0081] Examples of phosphorus-based flame retardants include metal ethylphosphinate, metal diethylphosphinate, melamine polyphosphate, condensed phosphate esters, and phosphazene compounds. Among these, condensed phosphate esters or phosphazene compounds are preferred, and condensed phosphate esters are more preferred. As the flame retardant, one type of flame retardant may be used alone, or two or more types of flame retardants with different compositions may be used in combination.

[0082] In particular, when a phosphorus-based flame retardant is used as the flame retardant, the phosphorus-based flame retardant is preferably, for example, a phosphoric acid ester represented by formula (3P).

[0083] Formula (3P)

[0084] In formula (3P), R 1 , R 2 , R 3 , R 4 each independently represents an aryl group. The aryl group may be substituted or unsubstituted. X represents a divalent aromatic group. The divalent aromatic group may or may not have another substituent. n represents an integer of 0 to 5.

[0085] R 1 , R 2 , R 3 , R 4Examples of the aryl group represented by each of the above include a phenyl group and a naphthyl group, with a phenyl group being preferred. Examples of the divalent aromatic group represented by X include a phenylene group, a naphthylene group, or a group derived from a bisphenol, with a group derived from a bisphenol being preferred. When X is a group derived from a bisphenol, it is more preferred that it is any of the following groups:

[0086] The R 1 , R 2 , R 3 , R 4 The substituents for each of and X are preferably, for example, an alkyl group, an alkoxy group, or a hydroxy group. When the integer n is 0, the phosphate ester flame retardant represented by formula (3P) is a phosphate ester. When the integer n is any one of 1 to 5, the phosphate ester flame retardant represented by formula (3P) is a condensed phosphate ester. The condensed phosphate ester may be a mixture. In this embodiment, a condensed phosphate ester is preferred.

[0087] Examples of such phosphate ester-based flame retardants include triphenyl phosphate, bisphenol A bisphosphate, hydroquinone bisphosphate, resorcinol bisphosphate, and substitution products, condensates, etc. Commercially available phosphate ester-based flame retardants include, for example, "TPP" (triphenyl phosphate), "CR733S" (resorcinol bis(diphenyl phosphate)), "CR741" (bisphenol A bis(diphenyl phosphate)), "PX-200" (resorcinol bis(dixylenyl phosphate)), and "SR-3000" (non-halogen condensed phosphate ester), all manufactured by Daihachi Chemical Industry Co., Ltd., and "FP-900L" (biphenyl-4,4'-diol bis(diphenyl phosphate)), all manufactured by ADEKA Corporation, and are readily available.

[0088] The content of the flame retardant (preferably a phosphorus-based flame retardant) in the resin composition of this embodiment is preferably 5 parts by mass or more, more preferably 8 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 polyphenylene ether resin, polyimide resin, and polycarbonate resin. It is also preferably 20 parts by mass or less, more preferably 15 parts by mass or less, and even more preferably 13 parts by mass or less. By setting the content at or above the lower limit, the combustion time of the resulting molded article can be shortened and the fluidity of the resin composition tends to be improved. Furthermore, by setting the content at or below the upper limit, the deterioration of the heat resistance and impact resistance of the resulting molded article tends to be more effectively suppressed. The resin composition of this embodiment may contain only one flame retardant (preferably a 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.

[0089] <Stabilizer> The resin composition of the present embodiment may contain a stabilizer. Examples of the stabilizer include a thermal stabilizer and an antioxidant. Examples of the stabilizer include a phenol-based stabilizer, an amine-based stabilizer, a phosphorus-based stabilizer, and a thioether-based stabilizer. Among these, in the present embodiment, it is preferable to contain a phenol-based stabilizer, a phosphorus-based stabilizer, and a thioether-based stabilizer.

[0090] Any known phosphorus stabilizer can be used. Specific examples include phosphorus oxoacids such as phosphoric acid, phosphonic acid, phosphorous acid, phosphinic acid, and polyphosphoric acid; metal acid pyrophosphates such as sodium acid pyrophosphate, potassium acid pyrophosphate, and calcium acid pyrophosphate; phosphates of Group 1 or Group 2B metals such as potassium phosphate, sodium phosphate, cesium phosphate, and zinc phosphate; organic phosphate compounds, organic phosphite compounds, and organic phosphonite compounds, with organic phosphite compounds being particularly preferred.

[0091] Examples of the organic phosphite compound include triphenyl phosphite, tris(mononylphenyl)phosphite, tris(mononyl / dinonyl phenyl)phosphite, tris(2,4-di-tert-butylphenyl)phosphite, monooctyldiphenyl phosphite, dioctylmonophenyl phosphite, monodecyldiphenyl phosphite, didecylmonophenyl phosphite, tridecyl phosphite, trilauryl phosphite, tristearyl phosphite, and 2,2-methylenebis(4,6-di-tert-butylphenyl)octyl phosphite. Specific examples of such organic phosphite compounds include "ADK STAB (registered trademark; the same applies hereinafter) 1178," "ADK STAB 2112," "ADK STAB HP-10," and "PEP-36" manufactured by ADEKA Corporation; "JP-351," "JP-360," and "JP-3CP" manufactured by Johoku Chemical Industry Co., Ltd.; and "IRGAFOS (registered trademark; the same applies hereinafter) 168" manufactured by BASF.

[0092] As the phenol-based stabilizer, a hindered phenol-based stabilizer is preferably used. Specific examples of hindered phenol stabilizers 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], N,N'-hexane-1,6-diylbis[3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionamide], 2,4-dimethyl-6-(1-methylpentadecyl)phenol, diethyl[[3,5-bis(1,1-dimethylethyl)-4-hydroxyphenyl]methyl]phosphate, 3,3',3'',5,5',5''-hexa-tert-butyl-a,a',a''-(mesityle) 4,6-bis(octylthiomethyl)-o-cresol, ethylene bis(oxyethylene) bis[3-(5-tert-butyl-4-hydroxy-m-tolyl)propionate], hexamethylene bis[3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate], 1,3,5-tris(3,5-di-tert-butyl 2,6-di-tert-butyl-4-(4,6-bis(octylthio)-1,3,5-triazin-2-ylamino)phenol, 2-[1-(2-hydroxy-3,5-di-tert-pentylphenyl)ethyl]-4,6-di-tert-pentylphenyl acrylate, and the like.

[0093] Among these, pentaerythritol tetrakis[3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate] and octadecyl-3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate are preferred. Specific examples of such hindered phenol stabilizers include "Irganox (registered trademark; the same applies hereinafter) 1010" and "Irganox 1076" manufactured by BASF, and "ADK STAB AO-50" and "ADK STAB AO-60" manufactured by ADEKA Corporation.

[0094] Examples of thioether stabilizers include dilauryl thiodipropionate, distearyl thiodipropionate, dimyristyl thiodipropionate, laurylstearyl thiodipropionate, pentaerythritol tetrakis(3-dodecylthiopropionate), pentaerythritol tetrakis(3-laurylthiopropionate), and the like. For example, commercially available products such as DSTP "Yoshitomi", DLTP "Yoshitomi", DLTOIB, and DMTP "Yoshitomi" (all manufactured by API Corporation), Seenox 412S (manufactured by Shipro Chemical Co., Ltd.), Adekastab AO-412S (manufactured by ADEKA Corporation), Cyanox 1212 (manufactured by Cyanamid Corporation), and Sumilizer TP-D (manufactured by Sumitomo Chemical Co., Ltd.) can be used (all are trade names).

[0095] The content of the stabilizer in the resin composition of this embodiment is usually 0.001 parts by mass or more, preferably 0.005 parts by mass or more, more preferably 0.01 parts by mass or more, and usually 5 parts by mass or less, preferably 3 parts by mass or less, more preferably 1 part by mass or less, per 100 parts by mass of the total amount of the polyphenylene ether resin, polyimide resin, and polycarbonate resin. By setting the content of the stabilizer within the above range, the effect of adding the stabilizer can be more effectively exhibited. 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] <Other Components> The resin composition of the present embodiment may contain other components in addition to those described above. Examples of other components include resin additives and fillers other than ceramic particles.

[0097] Resin additives may include dyes, pigments, weather resistance improvers, nucleating agents, impact modifiers, plasticizers, flow improvers, etc. The total amount of these resin additives is preferably less than 10% by mass, more preferably less than 5% by mass, and even more preferably less than 3% by mass, based on 100% by mass of the resin composition. In addition, the resin composition of this embodiment can be blended with additives described in paragraphs 0047 to 0103 of WO 2021 / 241471 within the scope of the present invention, the contents of which are incorporated herein by reference.

[0098] Examples of fillers other than ceramic particles include glass fiber, carbon fiber, etc. The total amount of fillers other than ceramic particles in the resin composition of this embodiment is preferably less than 10% by mass, more preferably less than 5% by mass, even more preferably less than 3% by mass, and even more preferably less than 1% by mass, based on 100% by mass of the resin composition.

[0099] In the resin composition of the present embodiment, the polyphenylene ether resin, polyimide resin, and polycarbonate resin, as well as the lubricant, flame retardant, ceramic particles, and stabilizer that are blended as needed, preferably account 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 even account for 99% by mass or more.

[0100] <Physical Properties of Resin Composition> The resin composition of this embodiment preferably has excellent tracking resistance. Specifically, the resin composition is molded into a 100 mm × 150 mm × 3.2 mm test piece, and the CTI value measured by a measurement method in accordance with IEC 60112 is preferably 500 V or more, more preferably 550 V or more, even more preferably 600 V or more, and even more preferably 650 V or more. Depending on the application, it may be 700 V or more. The upper limit of the CTI value is preferably the measurement limit value, for example, 1000 V. The CTI value is measured according to the description in the examples below.

[0101] The resin composition of this embodiment preferably has excellent flame retardancy. Specifically, the resin composition is molded into a 0.125 μm thick plate-like molded article, and the result of a flammability test in accordance with UL-94 preferably satisfies VTM-1, and more preferably VTM-0. The flame retardancy is measured according to the description in the Examples below.

[0102] <Method of Manufacturing Resin Composition> The method of manufacturing the resin composition of this embodiment is not limited, and a wide variety of known methods for manufacturing resin compositions can be used. Examples include a method in which the polyphenylene ether resin, polyimide resin, and polycarbonate resin, as well as other components added as needed, are premixed using various mixers such as a tumbler or Henschel mixer, and then melt-kneaded using a mixer such as a Banbury mixer, roll, Brabender, single-screw kneading extruder, twin-screw kneading extruder, or kneader. The melt-kneading temperature is not particularly limited, but is preferably 330°C or lower, more preferably 320°C or lower, even more preferably 310°C or lower, even more preferably 300°C or lower, and even more preferably 290°C or lower. The lower limit of the melt-kneading temperature is preferably 240°C or higher, and may be 250°C or higher, 260°C or higher, or 270°C or higher. An example of a resin composition is pellets.

[0103] <Molded Article> The molded article of this embodiment is formed from the resin composition or pellets of this embodiment. In this embodiment, the molded article may be produced by pelletizing the resin composition and molding the resulting pellets using various molding methods. Alternatively, the molded article may be produced by directly molding a resin composition melt-kneaded in a kneader without going through pelletization. The above-mentioned resin composition (e.g., pellets) is molded into a molded article using various molding methods. The shape of the molded article is not particularly limited and can be appropriately selected depending on the application and purpose of the molded article. Examples of the shape of the molded article include flat, rod-shaped, cylindrical, annular, circular, elliptical, polygonal, irregular, hollow, frame-shaped, box-shaped, panel-shaped, and button-shaped articles. An example of the molded article of this embodiment is a flat-plate molded article (film, sheet). The thickness of the plate-like molded article of this embodiment is, for example, preferably 10 μm or more, more preferably 25 μm or more, even more preferably 50 μm or more, even more preferably 75 μm or more, even more preferably 100 μm or more, and preferably 2000 μm or less, more preferably 1000 μm or less, even more preferably 750 μm or less, even more preferably 500 μm or less, and even more preferably 250 μm or less. The temperature during film molding is not particularly limited, but is preferably 330 ° C or less, more preferably 320 ° C or less, even more preferably 310 ° C or less, even more preferably 300 ° C or less, and even more preferably 290 ° C or less. The lower limit of the temperature during film molding is preferably 240 ° C or more, and may be 250 ° C or more, 260 ° C or more, or 270 ° C or more.

[0104] The method for molding the molded article is not particularly limited, and conventionally known molding methods can be used, such as injection molding, injection compression molding, extrusion molding, profile extrusion, transfer molding, blow molding, gas-assisted blow molding, blow molding, extrusion blow molding, IMC (in-mold coating molding), rotational molding, multilayer molding, two-color molding, insert molding, sandwich molding, foam molding, and pressure molding. In particular, the resin composition of this embodiment is suitable for molded articles (extrusion molded articles, particularly flat extrusion molded articles) obtained by injection molding, injection compression molding, and extrusion molding, and is particularly suitable for molded articles obtained by extrusion molding. However, it goes without saying that the resin composition of this embodiment is not limited to molded articles obtained by these methods.

[0105] <Applications> The resin composition, pellets, and molded article of this embodiment are widely used in applications where polyphenylene ether resins, particularly blends of polyphenylene ether resins and polyimide resins, are commonly used. The resin composition, pellets, and molded article of this embodiment are applicable to applications requiring high flame retardancy and tracking resistance, such as electric vehicle battery modules, battery housings, battery cases, battery cell frames, battery cell spacers, battery cell retainers, bus bar holders, bus bar covers, terminal covers, electrical connectors, automotive electrical connectors, relays, charging couplers, charging adapters, and outlets.

[0106] 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.

[0107] <Raw Materials> The raw materials shown in Table 1 below were used.

[0108]

[0109] Synthesis Example 1: Production of Polyimide Resin 1 Into a 2 L separable flask equipped with a Dean-Stark apparatus, a Liebig condenser, a thermocouple, and a four-paddle blade, 500 g of 2-(2-methoxyethoxy)ethanol (manufactured by Nippon Nyukazai Co., Ltd.) and 218.12 g (1.00 mol) of pyromellitic dianhydride (manufactured by Mitsubishi Gas Chemical Company, Inc.) were introduced, and after flowing nitrogen, the mixture was stirred at 150 rpm to obtain a uniform suspension. Meanwhile, using a 500 mL beaker, 49.79 g (0.35 mol) of 1,3-bis(aminomethyl)cyclohexane (manufactured by Mitsubishi Gas Chemical Company, Inc., cis / trans ratio = 7 / 3) and 93.77 g (0.65 mol) of 1,8-octamethylenediamine (manufactured by Kanto Chemical Co., Inc.) were dissolved in 250 g of 2-(2-methoxyethoxy)ethanol to prepare a mixed diamine solution. This mixed diamine solution was gradually added using a plunger pump. Although heat was generated during the dropwise addition, the internal temperature was adjusted to remain within the range of 40 to 80°C. During the dropwise addition of the mixed diamine solution, nitrogen flow was maintained throughout, and the stirring impeller rotation speed was set to 250 rpm. After the dropwise addition was completed, 130 g of 2-(2-methoxyethoxy)ethanol and 1.284 g (0.010 mol) of n-octylamine (Kanto Chemical Co., Inc.), an end-capping agent, were added and further stirred. At this stage, a pale yellow polyamic acid solution was obtained. Next, the stirring speed was increased to 200 rpm, and the polyamic acid solution in the 2-L separable flask was heated to 190°C. During the temperature increase, precipitation of polyimide resin powder and dehydration associated with imidization were observed between 120 and 140°C. After holding at 190°C for 30 minutes, the solution was allowed to cool to room temperature and then filtered. The obtained polyimide resin powder was washed with 300 g of 2-(2-methoxyethoxy)ethanol and 300 g of methanol, filtered, and then dried in a dryer at 180°C for 10 hours to obtain 317 g of powder of crystalline thermoplastic polyimide resin 1 (hereinafter also simply referred to as "polyimide resin 1"). The IR spectrum of polyimide resin 1 was measured, revealing a ν(C=O) 1768, 1697 (cm -1) characteristic absorption of an imide ring was observed. The inherent viscosity was 1.30 dL / g, Tm was 323°C, Tg was 184°C, Tc was 266°C, the heat of fusion was 26.7 mJ / mg, the heat of crystallization was 30.0 mJ / mg, the crystallization half time was 20 seconds or less, and the Mw was 55,000. The IR spectrum, relative viscosity, Tm, Tg, Tc, heat of fusion, crystallization half time, and weight average molecular weight were measured according to the descriptions in paragraphs 0114 to 0117 of WO 2016 / 084475.

[0110] Synthesis Example 2 A polyimide resin was synthesized according to the description in paragraph 0134 of WO 2016 / 147996. The Tm was 283°C, the Tg was 165°C, the Tc was 237°C, the heat of crystallization was 21.0 mJ / mg, and the crystallization half time was 20 seconds or less.

[0111] <Method for producing resin composition> In each of Example 1 and Comparative Example 1, the components shown in Table 1 were mixed in the ratios (parts by mass) shown in Table 2 below, and the mixture of the components was melt-kneaded using a twin-screw extruder (TEM26SX, manufactured by Shibaura Machine Co., Ltd.) at the cylinder temperature (extrusion temperature) shown in Table 2 and a screw rotation speed of 200 rpm to obtain a resin composition (pellet). The obtained resin composition (pellet) was used to perform the following evaluations. The results are shown in Table 2.

[0112] <Evaluation of Tracking Resistance> The pellets obtained by the above manufacturing method were dried at 120°C for 4 hours and then fed to an injection molding machine ("EC75SX" manufactured by Shibaura Machine Co., Ltd.), and molded articles measuring length x width x thickness = 100 mm x 100 mm x 3 mm were produced in this injection molding machine under conditions of a cylinder temperature shown in Table 2 and a mold temperature of 130°C. Using the produced molded articles, the maximum voltage at which tracking failure of the molded articles did not occur, i.e., the CTI value (unit: V), was measured by a measurement method in accordance with IEC60112 (electrolyte used: solution A, number of drops: 50).

[0113] <Film Processability> The pellets obtained by the above manufacturing method were dried at 120°C for 4 hours and then fed into a T-die extrusion molding machine (a small extruder manufactured by Technovel Co., Ltd.). The cylinder temperature (film processing temperature) was adjusted to the film processing temperature shown in Table 2, and extrusion molding was performed at a screw rotation speed of 25 rpm. The film was taken up at a chill roll setting temperature of 140°C and a take-up speed of 0.8 to 1.5 m / min, yielding a film having a thickness of 150 μm and a width of 140 mm. Photographs of the extrusion of the film from Example 1 and Comparative Example 1 are shown in Figures 1 and 2, respectively. As is clear from Figures 1 and 2, no eye scum was observed in Example 1 (Figure 1), but eye scum was observed near the die opening of the extruder in Comparative Example 1 (Figure 2). Evaluation was performed according to the following criteria. Evaluation was performed visually by five experts and judged by majority vote. A: No eye scum was observed. B: Eye scum was observed.

[0114] <Flame Retardancy> The pellets obtained by the above manufacturing method were dried at 120°C for 4 hours and then fed into a T-die extrusion molding machine (a small extruder manufactured by Technovel Co., Ltd.) and extruded at a cylinder setting temperature of 310°C to 340°C and a screw rotation speed of 25 rpm. The extrusion was performed at a chill roll setting temperature of 140°C and a take-up speed of 0.8 to 1.5 m / min, yielding a film having a thickness of 125 nm and a width of 140 mm. Films (0.125 μm thick) obtained under the same conditions as the film moldability described above were cut into 200 mm x 50 mm pieces and subjected to a vertical flame resistance test (UL-94 VTM test) for sets of five pieces in accordance with the UL-94 standard. The UL-94 standard grades are classified as VTM-0, VTM-1, VTM-2, and non-compliant, in descending order of quality. Each set was graded based on the vertical flame resistance test, and the results are shown in Table 2.

[0115]

[0116] As is clear from the above results, the film formed from the resin composition of the present invention was excellent in film processability. Furthermore, the molded article formed from the resin composition of the present invention was excellent in tracking resistance and flame retardancy (Examples 1 and 2).

[0117] 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 polyphenylene ether resin consisting of a resin represented by formula (1) and / or an acid-modified product thereof, a polyimide resin, and a polycarbonate resin, wherein the polyimide resin comprises a repeating structural unit represented by formula (2) and a repeating structural unit represented by formula (3), and the content of the repeating structural unit represented by formula (2) is 20 to 70 mol % relative to 100 mol % in total of the repeating structural units represented by formula (2) and the repeating structural units represented by formula (3). (In formula (1), R 51 ~R 55 , and R 61 ~R 64 are each independently a hydrogen atom, a hydroxy group, or an alkyl group having 1 to 4 carbon atoms, and R 65 is a hydrogen atom or an alkyl group having 1 to 4 carbon atoms. n is the number of repeating structural units and is a number of 10 or more. (In formulas (2) and (3), R 1 is a divalent group having 6 to 22 carbon atoms and containing at least one alicyclic hydrocarbon structure. 2 is a divalent chain aliphatic group having 5 to 16 carbon atoms. 1 and X 2 are each independently a tetravalent group containing at least one aromatic ring and having 6 to 22 carbon atoms.

2. The resin composition according to claim 1, further comprising a lubricant.

3. The resin composition according to claim 1 or 2, further comprising a lubricant in an amount of 0.1 to 3 parts by mass per 100 parts by mass of the polyphenylene ether resin, polyimide resin, and polycarbonate resin combined.

4. The resin composition according to claim 1 or 2, wherein the mass ratio of the polyphenylene ether resin to the total of 100 parts by mass of the polyphenylene ether resin and the polyimide resin is 50 to 99 parts by mass.

5. The resin composition according to claim 1 or 2, further comprising 5 to 20 parts by mass of a flame retardant and 0.1 to 10 parts by mass of ceramic particles per 100 parts by mass of the polyphenylene ether resin, polyimide resin, and polycarbonate resin combined.

6. The resin composition according to claim 5, wherein the flame retardant comprises a phosphorus-based flame retardant.

7. The resin composition according to claim 5, wherein the ceramic particles include titanium oxide particles.

8. The resin composition according to claim 1, further comprising a lubricant in an amount of 0.1 to 3 parts by mass per 100 parts by mass of the polyphenylene ether resin, polyimide resin, and polycarbonate resin combined, wherein the mass ratio of the polyphenylene ether resin to 100 parts by mass of the polyphenylene ether resin and polyimide resin is 50 to 99 parts by mass, and further comprising 5 to 20 parts by mass of a flame retardant and 0.1 to 10 parts by mass of ceramic particles per 100 parts by mass of the polyphenylene ether resin, polyimide resin, and polycarbonate resin combined, wherein the flame retardant comprises a phosphorus-based flame retardant, and the ceramic particles comprise titanium oxide particles.

9. Pellets of the resin composition according to claim 1, 2 or 8.

10. A molded article formed from the resin composition according to claim 1, 2 or 8.

11. A flat plate-shaped molded product formed from the resin composition according to claim 1, 2 or 8.

Citation Information

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