WO2024117245A1

WO2024117245A1 - Polyaryl ether ketone resin composition, molded article of same and method for producing polyaryl ether ketone resin composition

Info

Publication number: WO2024117245A1
Application number: PCT/JP2023/043031
Authority: WO
Inventors: 健太萩原; 佑磨芝崎
Original assignee: 本州化学工業株式会社
Priority date: 2022-12-01
Filing date: 2023-12-01
Publication date: 2024-06-06

Abstract

The present invention addresses the problem of providing a resin material for a polyaryl ether ketone that has improved load-carrying capacity at high temperatures without adding a strengthening agent or a filler to the resin material. The present invention provides, as a means for solving the problem, a polyaryl ether ketone resin composition that contains a first resin component and a second resin component. (First resin component) A polyaryl ether ketone which has a glass transition temperature of 200°C or more and a weight average molecular weight within the range of 2,000 to 1,000,000 (inclusive). (Second resin component) A polyaryl ether ketone which has a glass transition temperature of 100°C or more but less than 220°C and a weight average molecular weight within the range of 2,000 to 1,000,000 (inclusive).

Description

Polyaryletherketone resin composition and molded article thereof, and method for producing polyaryletherketone resin composition

The present invention relates to a polyaryl ether ketone (PAEK) resin composition and its use, and more specifically, to a PAEK resin composition obtained using bisphenol as a raw material and its use.

Polyaryletherketone (PAEK) resins, such as polyarylketone, polyetherketone (PEK), and polyetheretherketone (PEEK), offer highly desirable properties such as solvent resistance, flame retardancy, low wear rate, abrasion resistance, and high strength.
In particular, PEEK is known as a crystalline PAEK and is used in a variety of fields.
However, the relatively low glass transition temperature (Tg) of PEEK limits its use under high temperature loads. This drawback can be improved by the addition of glass fibers (US Pat. No. 5,399,433), carbon fibers (US Pat. No. 5,399,433), other reinforcing agents, and inorganic fillers (US Pat. No. 5,399,433). However, while these improvements improve one property, they adversely affect others. For example, adding fibers increases weight, reduces flowability, and creates anisotropy in the molded article, affecting dimensional change. In some cases, fiber additives can interfere with the surface smoothness of the molded part, resulting in surface non-uniformity.

Chinese Patent Publication No. 108164923 Chinese Patent Publication No. 111057346 JP 2012-97193 A

In consideration of the above problems, the objective of the present invention is to provide a polyaryletherketone resin material that has improved load-bearing capacity at high temperatures without the addition of reinforcing agents or fillers.

As a result of extensive research into solving the above problems, the inventors discovered that a polyaryletherketone resin composition containing a specific polyaryletherketone and a different specific polyaryletherketone has improved load-bearing capacity at high temperatures without the addition of a reinforcing agent or filler, and thus completed the present invention.

The present invention is as follows.
1. A polyaryletherketone resin composition comprising a first resin component and a second resin component.
[First resin component]
A polyaryl ether ketone having a glass transition temperature of 200° C. or higher and a weight average molecular weight in the range of 2,000 to 1,000,000.
[Second resin component]
A polyaryl ether ketone having a glass transition temperature of 100° C. or higher and lower than 220° C. and a weight average molecular weight of 2,000 or higher and 1,000,000 or lower.
2. The polyaryl ether ketone resin composition according to 1., wherein the first resin component and the second resin component are polyaryl ether ketones that are incompatible with each other.
3. The polyaryl ether ketone resin composition according to 1., wherein at least one of the first resin component and the second resin component is a crystalline polyaryl ether ketone.
4. The polyaryl ether ketone resin composition according to 1., wherein a weight ratio of the first resin component to the second resin component, the first resin component:the second resin component, is in the range of 1:99 to 99:1.
5. The polyaryl ether ketone resin composition according to 1., wherein the polyaryl ether ketone of the first resin component has a repeating unit represented by general formula (1A), (1B) or (1C).
(In the formula, each R ₁ independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
(In the formula, each R ₁ independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
(In the formula, each R ₁ independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
6. The polyaryl ether ketone resin composition according to 1., wherein the polyaryl ether ketone of the second resin component is a polyaryl ether ketone containing any one or more of the repeating units represented by chemical formulas (4a) to (4e).
7. The polyaryl ether ketone resin composition according to 1., having a storage modulus at a temperature of 200° C. of 400 MPa or more.
8. A molded article of the polyaryl ether ketone resin composition according to any one of 1. to 7.
9. A method for producing a polyaryl ether ketone resin composition, comprising mixing a first resin component and a second resin component in a molten state.
[First resin component]
A polyaryl ether ketone having a glass transition temperature of 200° C. or higher and a weight average molecular weight in the range of 2,000 to 1,000,000.
[Second resin component]
A polyaryl ether ketone having a glass transition temperature of 100° C. or higher and lower than 220° C. and a weight average molecular weight of 2,000 or higher and 1,000,000 or lower.
10. The method for producing a polyaryl ether ketone resin composition according to 9., wherein the first resin component and the second resin component are polyaryl ether ketones that are incompatible with each other.
11. The method for producing a polyaryl ether ketone resin composition according to 9., wherein at least one of the first resin component and the second resin component is a crystalline polyaryl ether ketone.
12. The method for producing a polyaryl ether ketone resin composition according to 9., wherein a weight ratio of the first resin component to the second resin component (first resin component:second resin component) is in the range of 1:99 to 99:1.
13. The method for producing a polyaryl ether ketone resin composition according to 9., wherein the polyaryl ether ketone of the first resin component has a repeating unit represented by general formula (1A), (1B) or (1C).
(In the formula, each R ₁ independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
(In the formula, each R ₁ independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
(In the formula, each R ₁ independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
14. The method for producing a polyaryl ether ketone resin composition according to 9., wherein the polyaryl ether ketone of the second resin component is a polyaryl ether ketone containing any one or more of the repeating units represented by chemical formulas (4a) to (4e).
15. The method for producing a polyaryl ether ketone resin composition according to 9., wherein the storage modulus of the obtained polyaryl ether ketone resin composition at a temperature of 200° C. is 400 MPa or more.

The polyaryl ether ketone resin composition of the present invention has improved load-bearing capacity at high temperatures.

1 is a graph showing the dynamic viscoelasticity measurement results of the polyaryl ether ketone resin compositions obtained in Examples 1 and 2, the PEEK used in Comparative Example 1, and the PAEK having a repeating unit represented by the chemical formula (1A-1) used in Comparative Example 2. 1 is a graph showing the dynamic viscoelasticity measurement results of the polyaryl ether ketone resin composition obtained in Example 3, the PEEK used in Comparative Example 1, and the PAEK having a repeating unit represented by the chemical formula (1B-1) used in Comparative Example 3. 1 is a graph showing the dynamic viscoelasticity measurement results of the polyaryl ether ketone resin composition obtained in Example 4, the PEEK used in Comparative Example 1, and the PAEK having a repeating unit represented by chemical formula (1C-1) used in Comparative Example 4. 1 is a graph showing the results of dynamic viscoelasticity measurement of the polyaryl ether ketone resin compositions obtained in Examples 5 and 6 and the PEEK used in Comparative Example 1.

<Polyaryletherketone (PAEK) resin composition of the present invention>
The polyaryletherketone (PAEK) resin composition of the present invention comprises a first resin component and a second resin component.
[First resin component] A polyaryl ether ketone having a glass transition temperature of 200° C. or higher and a weight average molecular weight in the range of 2,000 to 1,000,000.
[Second resin component] A polyaryl ether ketone having a glass transition temperature of 100° C. or higher and lower than 220° C. and a weight average molecular weight in the range of 2,000 or higher and 1,000,000 or lower.
The inventors presume that when the polyaryletherketone of the first resin component and the polyaryletherketone of the second resin component are incompatible with each other, in particular, the resin components in the resin composition obtained by mixing these undergo phase separation, which causes the resin composition of the present invention to exhibit improved load-bearing capacity at high temperatures.
The fact that the polyaryletherketone of the first resin component and the polyaryletherketone of the second resin component are incompatible with each other can be confirmed by the fact that two glass transition points are observed when differential scanning calorimetry (DSC) is performed on the resin composition.
When at least one of the first resin component and the second resin component is a crystalline polyaryletherketone, phase separation of the resin components occurs in the resulting resin composition. It is preferable that the first resin component is a non-crystalline polyaryletherketone and the second resin component is a crystalline polyaryletherketone.

The weight ratio of the first resin component to the second resin component contained in the polyaryletherketone resin composition of the present invention is preferably in the range of 99:1 to 1:99 (first resin component:second resin component). This weight ratio is more preferably in the range of 70:30 to 5:95, even more preferably in the range of 50:50 to 5:95, particularly preferably in the range of 30:70 to 5:95, and most preferably in the range of 20:80 to 5:95.

The storage modulus of the polyaryl ether ketone resin composition of the present invention at a temperature of 200° C. is preferably 400 MPa or more. Since it is in this range, it has sufficient load-bearing capacity at high temperatures. The storage modulus at a temperature of 200° C. is more preferably 500 MPa or more, even more preferably 700 MPa or more, particularly preferably 800 MPa or more, and most preferably 1000 MPa or more.
The larger the storage modulus at 200° C., the better the load-bearing capacity at high temperatures. Therefore, there is no upper limit, but the storage modulus may be 2000 MPa or less.

(First Resin Component)
The first resin component according to the present invention is a polyaryl ether ketone (PAEK) having a glass transition temperature (Tg) of 200° C. or higher and a weight average molecular weight in the range of 2,000 to 1,000,000. Such a PAEK is a PAEK obtained by subjecting a dihalogen compound represented by general formula (2) and an aromatic dihydroxy compound to a desalting polycondensation reaction in the presence of an alkali metal compound. The structure of the PAEK preferably has a repeating unit represented by general formula (1A), (1B), or (1C). The repeating unit as the structure of the PAEK may have a repeating unit other than the repeating unit represented by general formula (1A), (1B), or (1C), but preferably has only the repeating unit represented by general formula (1A), (1B), or (1C).
(In the formula, X represents a halogen atom.)
(In the formula, each R ₁ independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
(In the formula, each R ₁ independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
(In the formula, each R ₁ independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
Each R ₁ independently represents an alkyl group having 1 to 4 carbon atoms, preferably a t-butyl group or a methyl group, and particularly preferably a methyl group.
The bonding position of R ₁ is preferably the ortho position relative to the bonding position of the oxygen atom on the benzene ring.
Each n independently represents 0, 1 or 2, and is preferably 0 or 2.

(Glass-transition temperature)
The glass transition temperature (Tg) of the PAEK of the first resin component according to the present invention is 200° C. or higher. The glass transition temperature (Tg) is preferably 220° C. or higher, more preferably 240° C. or higher, even more preferably 270° C. or higher, and particularly preferably 280° C. or higher.

(Molecular Weight)
The first resin component according to the present invention has a weight average molecular weight (Mw) in the range of 2,000 or more and 1,000,000 or less, preferably in the range of 10,000 or more and 500,000 or less, more preferably in the range of 20,000 or more and 200,000 or less, and particularly preferably in the range of 30,000 or more and 150,000 or less.
The ratio of weight average molecular weight (Mw) to number average molecular weight (Mn), Mw/Mn, is preferably in the range of 1.5 or more and 20 or less, more preferably in the range of 2 or more and 15 or less, even more preferably in the range of 2 or more and 10 or less, and particularly preferably in the range of 2 or more and 8 or less.

(Reduced Viscosity)
The reduced viscosity of the PAEK of the first resin component according to the present invention is preferably 0.1 dL/g or more, more preferably 0.3 dL/g or more, and even more preferably 0.5 dL/g or more, which is a measured value of the viscosity of a 1.0 g/dL solution of the PAEK of the present invention in p-chlorophenol as a solvent at 40°C.

(Method of producing PAEK of the present invention)
The method for producing the PAEK of the first resin component according to the present invention having a glass transition temperature (Tg) of 200° C. or higher is not particularly limited, and the PAEK can be produced, for example, by subjecting a dihalogen compound represented by general formula (2) and an aromatic dihydroxy compound to a desalting polycondensation reaction in the presence of an alkali metal compound.

As a specific example, a reaction formula of a method for producing PAEK is shown below, in which 4,4'-difluorobenzophenone (2a) is used as the halogen compound represented by the general formula (2), 4,4'-(9-fluorenylidene)bis(2,6-dimethylphenol) (3A-1) is used as the aromatic dihydroxy compound represented by the general formula (3A), and potassium carbonate is used as the alkali metal compound.

(Dihalogen compound represented by general formula (2))
Specific examples of the dihalogen compound represented by the general formula (2) include 3,3'-difluorobenzophenone, 3,3'-dichlorobenzophenone, 3,3'-dibromobenzophenone, 3,3'-diiodobenzophenone, 4,4'-difluorobenzophenone, 4,4'-dichlorobenzophenone, 4,4'-dibromobenzophenone, and 4,4'-diiodobenzophenone.
Of these, 4,4'-difluorobenzophenone and 4,4'-dichlorobenzophenone are preferred, with 4,4'-difluorobenzophenone being particularly preferred.

(Aromatic dihydroxy compounds)
The aromatic dihydroxy compound is not limited as long as it is an aromatic dihydroxy compound that can undergo a polycondensation reaction with the dihalogen compound represented by general formula (2) to form the first resin component, but is preferably an aromatic dihydroxy compound represented by general formula (3A), (3B) or (3C).
(In the formula, _R1 and n are defined as in general formula (1A).)
(In the formula, _R1 and n are the same as defined in general formula (1B).)
(In the formula, R ₁ and n are the same as defined in general formula (1C).)

(Aromatic dihydroxy compound represented by general formula (3A))
In the aromatic dihydroxy compound represented by the general formula (3A), R ₁ and n are defined as in the general formula (1A), and the preferred embodiments are also the same.
Specific examples of the aromatic dihydroxy compound represented by the general formula (3A) include 4,4'-(9-fluorenylidene)bis(2,6-dimethylphenol), 4,4'-(9-fluorenylidene)bis(2,5-dimethylphenol), 4,4'-(9-fluorenylidene)bis(3,5-dimethylphenol), 4,4'-(9-fluorenylidene)bis(2-methylphenol), and 4,4'-(9-fluorenylidene)bis(3-methylphenol).
Among these, 4,4'-(9-fluorenylidene)bis(2,6-dimethylphenol), 4,4'-(9-fluorenylidene)bis(2,5-dimethylphenol) and 4,4'-(9-fluorenylidene)bis(2-methylphenol) are preferred, with 4,4'-(9-fluorenylidene)bis(2,6-dimethylphenol) being particularly preferred.

(Aromatic dihydroxy compound represented by general formula (3B))
In the aromatic dihydroxy compound represented by formula (3B), R ₁ and n are the same as those in formula (1B), and the preferred embodiments are also the same.
Specific examples of the aromatic dihydroxy compound represented by the general formula (3B) include 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2,6-dimethylphenol), 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2,5-dimethylphenol), 4,4'-(3,3,5-trimethylcyclohexylidene)bis(3,5-dimethylphenol), 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2-methylphenol), 4,4'-(3,3,5-trimethylcyclohexylidene)bis(3-methylphenol), and 4,4'-(3,3,5-trimethylcyclohexylidene)bisphenol.
Among these, 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2,6-dimethylphenol), 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2,5-dimethylphenol), 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2-methylphenol), and 4,4'-(3,3,5-trimethylcyclohexylidene)bisphenol are preferred, and 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2,6-dimethylphenol), 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2-methylphenol) and 4,4'-(3,3,5-trimethylcyclohexylidene)bisphenol are more preferred, 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2,6-dimethylphenol) and 4,4'-(3,3,5-trimethylcyclohexylidene)bisphenol are even more preferred, and 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2,6-dimethylphenol) is particularly preferred.

(Aromatic dihydroxy compound represented by general formula (3C))
In the aromatic dihydroxy compound represented by formula (3C), R ₁ and n are the same as those in formula (1C), and the preferred embodiments are also the same.
Specific examples of the aromatic dihydroxy compound represented by the general formula (3C) include 1,3-dihydro-3,3-bis(4-hydroxy-2,6-dimethylphenyl)-1-phenyl-2H-indol-2-one, 1,3-dihydro-3,3-bis(4-hydroxy-2,5-dimethylphenyl)-1-phenyl-2H-indol-2-one, 1,3-dihydro-3,3-bis(4-hydroxy-3,5-dimethylphenyl)-1-phenyl-2H-indol-2-one, 1,3-dihydro-3,3-bis(4-hydroxy-3,5-dimethylphenyl)-1-phenyl-2H-indol-2-one, Examples of the compound include 1,3-dihydro-3,3-bis(4-hydroxy-2,5-dimethylphenyl)-1-phenyl-2H-indol-2-one, 1,3-dihydro-3,3-bis(4-hydroxy-2-methylphenyl)-1-phenyl-2H-indol-2-one, 1,3-dihydro-3,3-bis(4-hydroxy-3-methylphenyl)-1-phenyl-2H-indol-2-one, and 1,3-dihydro-3,3-bis(4-hydroxyphenyl)-1-phenyl-2H-indol-2-one.
Among these, 1,3-dihydro-3,3-bis(4-hydroxy-3,5-dimethylphenyl)-1-phenyl-2H-indol-2-one, 1,3-dihydro-3,3-bis(4-hydroxy-2,5-dimethylphenyl)-1-phenyl-2H-indol-2-one, 1,3-dihydro-3,3-bis(4-hydroxy-3-methylphenyl)-1-phenyl-2H-indol-2-one, and 1,3-dihydro-3,3-bis(4-hydroxyphenyl)-1-phenyl-2H-indol-2-one are preferred, and 1 , 3-dihydro-3,3-bis(4-hydroxy-3,5-dimethylphenyl)-1-phenyl-2H-indol-2-one, 1,3-dihydro-3,3-bis(4-hydroxy-3-methylphenyl)-1-phenyl-2H-indol-2-one, 1,3-dihydro-3,3-bis(4-hydroxyphenyl)-1-phenyl-2H-indol-2-one are more preferred, and 1,3-dihydro-3,3-bis(4-hydroxy-3,5-dimethylphenyl)-1-phenyl-2H-indol-2-one is particularly preferred.
In the PAEK of the present invention, in order to obtain a PAEK having repeating units represented by the general formulae (1A), (1B) and (1C) and other repeating units, other aromatic dihydroxy compounds can be used in combination with the biphenol compounds represented by the general formulae (3A), (3B) and (3C). The other repeating units have a structure derived from these aromatic dihydroxy compounds and a repeating unit having a structure derived from the dihalogen compound represented by the general formula (2). Specific examples of aromatic dihydroxy compounds that can be used in combination include hydroquinone, resorcinol, 2-phenylhydroquinone, 4,4'-biphenol, 2,6-dihydroxynaphthalene, 2,7-dihydroxynaphthalene, 1,1'-bi-2-naphthol, 2,2'-bi-1-naphthol, 1,3-bis[1-methyl-1-(4-hydroxyphenyl)ethyl]benzene, 1,4-bis[1-methyl-1-(4-hydroxyphenyl)ethyl]benzene, 1,3-bis(4-hydroxybenzoyl)benzene, 1,4-bis(4-hydroxybenzoyl)benzene, 1,3-bis(4-hydroxyphenoxy)benzene, 1,4-bis(4-hydroxyphenoxy)benzene, 1,4-bis(4-hydroxyphenyl)benzene, 1,3-bis(4-hydro Examples of the compounds include 4,4'-dimethylphenyl)benzene, 4,4'-methylenebis(phenol), 4,4'-methylenebis(2,6-dimethylphenol), 4,4'-isopropylidenebiphenol (Bis-A), 2,2-bis(4-hydroxyphenyl)-1,1,1,3,3,3-hexafluoropropane, 4,4'-dihydroxybenzophenone, 4,4'-bis(hydroxyphenyl)sulfone, 4,4'-dihydroxydiphenyl ether, bis(4-hydroxyphenyl)methane, 2,2-bis(4-hydroxy-3-phenylphenyl)propane, bisphenol Z (1,1-bis(4-hydroxyphenyl)cyclohexane), 1,1-bis(4-hydroxyphenyl)cyclododecane, and 1,1-bis(4-hydroxyphenyl)-1-phenylethane. These compounds may be used alone or in combination of two or more.

Any alkali metal compound can be used as long as it can convert the aromatic dihydroxy compound used into an alkali metal salt, but usually, carbonates, hydrogen carbonates, hydroxides, etc. of alkali metals are preferably used, with carbonates being particularly preferred. Examples of the alkali metal include lithium, sodium, potassium, rubidium, and cesium, with sodium and potassium being particularly preferred, and potassium being particularly preferred.

　A solvent can be used in the polycondensation reaction to obtain PAEK, and it is preferable to use one. Neutral polar solvents such as N,N-dimethylformamide (DMF), N,N-dimethylacetamide (DMAc), N-methylpyrrolidone (NMP), dimethylimidazolidinone (DMI), dimethylsulfoxide (DMSO), sulfolane, and diphenylsulfone are preferred, but any solvent can be used without any problems as long as it dissolves the monomer and PAEK. The solvent may be used alone, or two or more types may be used in combination as a mixed solvent.

(Polycondensation reaction conditions)
The amount of the dihalogen compound represented by the general formula (2) used is usually in the range of 0.9 to 1.1 times by mole, preferably in the range of 0.95 to 1.06 times by mole, more preferably in the range of 1.0 to 1.04 times by mole, based on the amount of the aromatic dihydroxy compound.
The amount of the alkali metal compound used is usually in the range of 1.0 to 3.0 moles, preferably 1.01 to 1.3 moles, per mole of the aromatic dihydroxy compound.
The reaction temperature is usually in the range of 150 to 350° C., preferably 180 to 250° C., and the reaction time is usually in the range of 1 to 60 hours, preferably 2 to 50 hours.
These reactions are preferably carried out in an atmosphere of an inert gas such as nitrogen, argon, etc. There is no limitation on the reaction pressure, and the reaction may be carried out at reduced pressure, atmospheric pressure, or elevated pressure, but the reaction is usually carried out at atmospheric pressure.

<Post-reaction treatment>
The PAEK produced by the polycondensation reaction can be recovered by a commonly used method such as coagulation, solidification, washing, granulation, extraction, or solvent distillation.
The method for treating the PAEK produced by the polycondensation reaction will be described in more detail below. The liquid containing the PAEK produced by the polycondensation reaction can be diluted with a solvent as necessary, and mixed with the solvent to precipitate the PAEK, thereby obtaining a powdered PAEK. As the solvent used to precipitate the precipitate, for example, methanol, ethanol, acetone, methyl ethyl ketone, xylene, toluene, etc. are preferable, and acetone and methanol are particularly preferable in terms of operability and ease of distillation recovery of the reaction solvent after washing.
The powdered PAEK obtained by precipitating the precipitate is preferably subjected to a washing step in order to remove alkali metal salts such as potassium chloride produced in the desalting polycondensation reaction, the solvent used in the reaction, and the solvent used to precipitate the precipitate.
For washing away alkali metal salts such as potassium chloride produced in the desalting polycondensation reaction, water is preferred, but acidic water containing low concentrations of hydrochloric acid, formic acid, oxalic acid, etc. may also be used.
The conditions for this washing step may be appropriately selected according to the amounts of residual reaction solvent and residual alkali metal salts to be removed, such as the amount of washing solvent used, the number of washings, and the washing temperature.
After washing with water, the powder may be washed with, for example, methanol, ethanol, acetone, methyl ethyl ketone, xylene, or toluene, particularly acetone or methanol.
The washing apparatus may be a combination of a washing tank and a pressure filter or a centrifuge, or a multi-function filter capable of washing, filtering and drying in one apparatus.

A drying step can be carried out to dry the powdered PAEK containing moisture and solvent obtained after the completion of the washing step.
The conditions for this drying step may be any conditions that allow removal of moisture at a temperature equal to or lower than the melting point of the polycondensation reaction product. It is preferable to perform the drying step under an inert gas (nitrogen, argon, etc.) atmosphere, under an inert gas stream, or under reduced pressure so as to minimize contact with air.
The dryer may be a known device such as an evaporator, a tray oven, or a tumbler.

(Second Resin Component)
The second resin component is a polyaryl ether ketone having a glass transition temperature (Tg) in the range of 100°C or higher and lower than 220°C.
Examples of such polyaryl ether ketones (PAEKs) having a glass transition temperature (Tg) in the range of 100° C. or higher and lower than 220° C. include PAEKs containing one or more of the repeating units represented by chemical formulas (4a) to (4e).
The PAEKs containing repeating units represented by chemical formulas (4a) to (4e) are polyether ketone (PEK), polyether ether ketone (PEEK), polyether ketone ether ketone ketone (PEKEKK), polyether ether ether ketone (PEEEK), and polyether ketone ketone (PEKK), respectively.
Specific examples of polyetherketone (PEK) products include Victrex's product names: HT G22 and HT G45. Specific examples of polyetheretherketone (PEEK) products include Victrex's product names: Victrex Powder series and Victrex Granules series, Daicel-Evonik's product names: VestaKeep series, and Solvay Specialty Polymers' product name: KetaSpire PEEK series. Specific examples of polyetherketoneetherketoneketone (PEKEKK) products include Victrex's product name: STG45. Specific examples of polyetheretheretherketone (PEEEK) products include Arkema's product. Specific examples of polyetherketoneketone (PEKK) products include Arkema's product: KEPSTAN6002.

<Method for producing the polyaryl ether ketone (PAEK) resin composition of the present invention>
The polyaryletherketone (PAEK) resin composition of the present invention can be produced by using the first resin component and the second resin component in the above weight ratio and mixing them in a molten state.
The temperature during mixing can be appropriately adjusted depending on the melting points of the first and second resin components used, but can be within the range of 350 to 450° C., for example.
The mixing may be performed in an air atmosphere or in an oxygen-free nitrogen atmosphere, but is preferably performed in a nitrogen atmosphere in order to suppress oxidative deterioration due to oxygen.

The polyaryletherketone resin composition of the present invention can be molded into various articles by known molding and processing methods for thermoplastic resins. Preferred molding and processing methods include, for example, injection molding, blow molding, compression molding, profile extrusion, sheet or film extrusion, sintering, and gas assist.
Examples of such molded articles include molding materials in the form of pellets, chips, etc., membranes, tubing, fibers, composites, semiconductor process tools, wire coatings and jackets, fluid handling components, cookware, food service items, medical devices, trays, plates, handles, helmets, animal cages, electrical connectors, electrical equipment housings, engine parts, automotive parts, aerospace equipment parts, bearings, light sockets and reflectors, electric motor parts, power distribution equipment, communication equipment, computers, devices molded with snap fit connectors, and materials for building 3D printers.
Additionally, the polyaryletherketone resin composition can be used as a material for coatings, such as powder coatings. The polyaryletherketone resin composition can also be extruded into rods or slabs that can be used to form articles by machining.

The polyaryl ether ketone resin composition of the present invention may be blended with various additives, such as colorants such as titanium dioxide, zinc sulfide, and carbon black; stabilizers such as hindered phenols, phosphites, phosphonites, thioesters, and mixtures thereof; mold release agents; lubricants; metal deactivators; plasticizers; nucleating agents such as talc; wear-resistant additives such as fluoropolymers and metal sulfides; flame retardants; smoke suppressants; drip-proofing agents; hue improvers such as phosphonate or phosphite compounds or mixtures thereof; and ultraviolet stabilizers.
The effective amounts and methods of compounding the above-mentioned additives are well known in the art and can be compounded by conventional methods. The effective amount of the additives varies widely, but is typically in the range of 0.01 to 30% by weight based on the weight of the first and second resin components used.

The present invention will be explained in detail below with reference to examples, but the present invention is not limited to these examples.

The analytical method in the present invention is as follows.
<Analysis method>
1. Measurement of Glass Transition Temperature (Tg) and Melting Point The glass transition temperature and melting point of the PAEK obtained in the Synthesis Examples described below, the PAEK resin compositions obtained in the Examples, and the PEEK used in the Comparative Examples were measured using the following apparatus and under the following conditions.
Measurement device: DSC7020 (Hitachi)
Pan: Aluminum Atmosphere: _N2
Heating rate: 10° C./min.
Analysis method:
[Glass-transition temperature]
Glass transition temperature of the ^second heating (intersection of the baseline and the tangent line)
[Melting point]
The intersection of the baseline and the tangent to the endothermic peak appearing near 350° C. during the ^second heating was taken as the melting point.
2. Molecular weight measurement <Molecular weight measurement method 1>
The molecular weights of the PAEK resin compositions obtained in the Examples and the PAEKs obtained in the Synthesis Examples were measured by gel permeation chromatography (GPC) using the following apparatus and conditions.
Equipment: 515 HPLC pump, 717plus automatic insertion device, 2487 UV-Vis detector (Waters)
Column/temperature: 2×PLgel 5μMIXED-D, 7.5×300 mm (Agilent Technologies)/40° C.
Mobile phase: chloroform for HPLC Flow rate: 1.0 mL/min.
Injection volume: 2.5uL
Detection: UV-Vis detector 254 nm
Column calibration: monodisperse PS; EasiCal Type PS-1 polystyrene (Agilent Technologies)
Molecular weight calibration: PS conversion <Molecular weight measurement method 2>
The molecular weight of the PAEK obtained in Synthesis Example 4 was measured by gel permeation chromatography (GPC) using the following apparatus and conditions.
Apparatus: Tosoh Corporation HLC-8320GPC
Column/temperature: Guard Column HXL-L + G4000HXL + G3000HXL + G2000HXL x 2 (7.8 mm ID x 30 cm, Tosoh Corporation) / 40°C
Mobile phase: tetrahydrofuran Flow rate: 1.0 mL/min.
Injection volume: 10 uL
Detection: UV-Vis detector 254 nm
Molecular weight calibration: PS conversion 3. Measurement of reduced viscosity The PAEK resin composition obtained in the examples and the PAEK powder obtained in the synthesis examples were dissolved in p-chlorophenol to prepare a solution having a concentration of 1.0 g/dL, and the viscosity at 40° C. was measured.
4. Dynamic Mechanical Analysis (DMA)
<Preparation of test pieces for dynamic mechanical analysis (DMA)>
Test pieces were prepared using the polyaryletherketone resin compositions obtained in Examples 1 to 4 and the PAEK used in the Comparative Examples as material resins, using a Mini Test Press MP-2FH (manufactured by Toyo Seiki Co., Ltd.). Molding was performed by degassing several times at a temperature of 360°C and a pressure of 1 to 5 MPa, and then pressure bonding at a temperature of 360°C and a pressure of 12 MPa for 5 minutes.
<Measurement equipment and conditions>
Apparatus: DMA0850-00600 (Hitachi)
Heating rate: 3° C./min.
Vibration frequency: 1Hz
Test piece size: length 10 mm x width 2.0±0.5 mm x thickness 0.5-0.9 mm
5. Compatibility Evaluation When the number of glass transition points observed in the above glass transition temperature measurement was two, the first resin component and the second resin component used in the resin composition were evaluated to be incompatible with each other, and when the number of glass transition points observed was one, they were evaluated to be compatible with each other.

<Synthesis Example 1: PAEK-1A-1>
A powder of PAEK (PAEK-1A-1) having a repeating unit represented by chemical formula (1A-1) was synthesized by the reaction shown in the following reaction formula.
Into a 500 mL four-necked reaction vessel equipped with a Dean-Stark tube filled with toluene, a stirrer, and a nitrogen inlet tube, 27 g of 4,4'-difluorobenzophenone represented by chemical formula (2a), 50 g of 4,4'-(9-fluorenylidene)bis(2,6-dimethylphenol) represented by chemical formula (3A-1), 20 g of potassium carbonate, and 200 g of N-methylpyrrolidone (NMP) were added and dissolved at room temperature while passing nitrogen through. The reaction vessel was then heated to 200°C over 1 hour, after which a small amount of toluene was added and refluxed, followed by polymerization at 200°C for 10 hours.
After the reaction was completed, the reaction solution was cooled to room temperature, and the solution diluted with 156 g of NMP was added to 2850 g of methanol to precipitate. The precipitate was filtered off, and the resulting powder was suspended and washed in 1000 g of a 1.4% aqueous oxalic acid solution, and then repeatedly washed with hot water until the water after washing became neutral, and then washed with methanol. The washed powder was dried under reduced pressure at 150° C. for 12 hours to obtain 65 g of a powder of PAEK having a repeating unit represented by the chemical formula (1A-1) (Mw: 76,856, Mw/Mn: 5.5) (PAEK-1A-1) in a yield of 87%.
The resulting PAEK had a reduced viscosity of 0.63 dL/g.
Differential scanning calorimetry of the resulting PAEK showed that it had a glass transition temperature (Tg) of 286° C. and no melting point was observed.

<Synthesis Example 2: PAEK-1B-1(1)>
A powder of PAEK (PAEK-1B-1(1)) having a repeating unit represented by chemical formula (1B-1) was synthesized by the reaction shown in the following reaction formula.
Into a 500 mL four-necked reaction vessel equipped with a Dean-Stark tube filled with toluene, a stirrer, and a nitrogen inlet tube, 31 g of 4,4'-difluorobenzophenone represented by chemical formula (2a), 50 g of 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2,6-dimethylphenol) represented by chemical formula (3B-1), 17 g of sodium carbonate, and 240 g of NMP were added and dissolved at room temperature while passing nitrogen through. The reaction vessel was then heated to 200°C over 1 hour, after which a small amount of toluene was added and refluxed, followed by polymerization at 200°C for 50 hours.
After the reaction was completed, the reaction solution was cooled to room temperature, and the solution diluted with 180 g of NMP was added to 3200 g of methanol to precipitate. The precipitate was filtered off, and the resulting powder was suspended and washed in 1000 g of a 1.4% aqueous oxalic acid solution, and then repeatedly washed with hot water until the water after washing became neutral, and then washed with methanol. The washed powder was dried under reduced pressure at 150° C. for 12 hours to obtain 65 g of a powder of PAEK having a repeating unit represented by the chemical formula (1B-1) (Mw: 51,200, Mw/Mn: 3.0) (PAEK-1B-1(1)) in a yield of 85%.
The resulting PAEK had a reduced viscosity of 0.45 dL/g.
Differential scanning calorimetry of the resulting PAEK revealed that it had a glass transition temperature (Tg) of 243° C. and no melting point was observed.

<Synthesis Example 3: PAEK-1C-1>
A powder of PAEK (PAEK-1C-1) having a repeating unit represented by chemical formula (1C-1) was synthesized by the reaction shown in the following reaction formula.
Into a 500 mL four-necked reaction vessel equipped with a Dean-Stark tube filled with toluene, a stirrer, and a nitrogen inlet tube, 34 g of 4,4'-difluorobenzophenone represented by chemical formula (2a), 19 g of 1,3-dihydro-3,3-bis(4-hydroxyphenyl)-1-phenyl-2H-indol-2-one represented by chemical formula (3C-1), 11 g of sodium carbonate, and 161 g of NMP were added and dissolved at room temperature while passing nitrogen through. The reaction vessel was then heated to 200°C over 1 hour, after which a small amount of toluene was added and refluxed, followed by polymerization at 200°C for 7 hours.
After the reaction was completed, the reaction solution was cooled to room temperature, and the solution was diluted with 107 g of NMP, and precipitates were precipitated in 2150 g of methanol. The precipitate was separated by filtration, suspended and washed in 800 g of a 1.4% aqueous oxalic acid solution, further washed with hot water until neutral, and then washed with methanol. It was dried under reduced pressure at 150° C. for 12 hours, and 44 g of a powder of PAEK having a repeating unit represented by chemical formula (1C-1) (Mw: 49,500, Mw/Mn: 3.1) (PAEK-1C-1) was obtained in a yield of 87%.
The resulting PAEK had a reduced viscosity of 0.56 dL/g.
Differential scanning calorimetry of the resulting PAEK revealed that it had a glass transition point (Tg) of 240° C. and no melting point was observed.

<Synthesis Example 4: PAEK-1B-1(2)>
A powder of PAEK (PAEK-1B-1(2)) having a repeating unit represented by chemical formula (1B-1) was synthesized by the reaction shown in the following reaction formula.
Into a 2 L four-necked reaction vessel equipped with a Dean-Stark tube filled with toluene, a stirrer, and a nitrogen inlet tube, 79 g of 4,4'-difluorobenzophenone represented by chemical formula (2a), 150 g of 4,4'-(3,3,5-trimethylcyclohexylidene)bis(2,6-dimethylphenol) represented by chemical formula (3B-1), 50 g of potassium carbonate, 720 g of NMP, and 29 g of toluene were added and dissolved at room temperature while passing nitrogen through. The reaction vessel was then heated to 196°C over one and a half hours, and polymerization was carried out for 10 hours.
After the reaction was completed, the reaction solution was cooled to room temperature, and the cooled reaction solution was added to 3000 g of methanol to precipitate. The precipitate was filtered off, and the resulting powder was suspended and washed in 4000 g of a 1.1% aqueous oxalic acid solution, and repeatedly washed until the water became neutral, and then washed with methanol. The washed powder was dried under reduced pressure at 55° C. for 8 hours to obtain 196 g of a powder of PAEK having a repeating unit represented by chemical formula (1B-1) (Mw: 9,000, Mw/Mn: 1.9) (PAEK-1B-1(2)) in a yield of 96%.
Differential scanning calorimetry of the resulting PAEK showed that it had a glass transition temperature (Tg) of 216° C. and no melting point was observed.

<Examples 1 to 6>
A PAEK resin composition was produced by polymer blending the PAEK obtained in Synthesis Examples 1 to 4 as the first resin component and polyether ether ketone (hereinafter referred to as PEEK) sold by Victrex as VICTREX 450G as the second resin component in the parts by mass shown in Table 1. The polymer blending was carried out using the following apparatus and conditions.
(Polymer Blending Equipment and Conditions)
Equipment: Circulation mixer [Xplore MC15HT] (manufactured by Xplore Instrument)
Temperature/time: 370°C/5min.
Rotation speed: 100 rpm
Screw shape: Conical type twin screw Kneading environment: Under _N2 flow Compatibility evaluation and differential scanning calorimetry of the PAEK resin composition obtained by polymer blending were performed by the above-mentioned method. The results, that is, the number of glass transition points expressed, the glass transition temperature, and the melting point, are shown in Table 1. In addition, the obtained PAEK resin composition was used to prepare a test piece for dynamic viscoelasticity measurement, and dynamic viscoelasticity measurement was performed by the above-mentioned method. The results are shown in Table 2.

<Comparative Example 1>
Using commercially available PEEK450G (manufactured by Victrex) (PEEK), test pieces for compatibility evaluation, differential scanning calorimetry, and dynamic viscoelasticity measurement were prepared and dynamic viscoelasticity measurement was performed in the same manner as in Examples 1 to 4. The results are shown in Tables 1 and 2.

<Comparative Examples 2 to 4>
Using the PAEKs obtained in Synthesis Examples 1 to 4, test pieces for compatibility evaluation, differential scanning calorimetry, and dynamic viscoelasticity measurement were prepared and dynamic viscoelasticity measurement was performed in the same manner as in Examples 1 to 6. The results are shown in Tables 1 and 2.

From the results in Table 1, it became clear that the PAEK resin compositions obtained in Examples 1 to 6 exhibited two glass transition points, and therefore the PAEK of the first resin component and the PAEK of the second resin component were incompatible with each other.
In addition, the PAEK resin compositions obtained in Examples 1 to 6 have melting points, unlike the PAEKs not blended with polymers in Comparative Examples 2 to 4. This is believed to be a result suggesting that these are resin materials that retain the crystallinity of PEEK.

The dynamic viscoelasticity measurement results of the PAEK resin compositions obtained in Examples 1 and 2, the PEEK used in Comparative Example 1, and the PAEK having a repeating unit represented by the chemical formula (1A-1) used in Comparative Example 2 are summarized in FIG. 1.
The storage modulus of the PEEK used in Comparative Example 1 significantly decreased from 1646 MPa to 223 MPa as the temperature increased from 150°C to 200°C.
The storage modulus of the PAEK used in Comparative Example 2 did not decrease significantly until around 280° C. in FIG. 1, but as shown in Table 2, it rapidly decreased from 1510 MPa to 101 MPa from 275° C. to 296° C.
In contrast, it was revealed that the storage modulus of the PAEK resin composition obtained in Example 1 was higher than that of the PEEK used in Comparative Example 1 up to 296°C, which is the upper limit of the measurement temperature range. It was also revealed that the storage modulus of the PAEK resin composition obtained in Example 1 did not decrease abruptly like the PAEK used in Comparative Example 2, but decreased gradually. It was also revealed that at 296°C, which is the upper limit of the measurement temperature range, the storage modulus of the PAEK resin composition obtained in Example 1 was 133 MPa, which was higher than the 101 MPa of the PAEK used in Comparative Example 2.
In addition, the storage modulus of the PAEK used in Comparative Example 2 does not decrease significantly up to 280 ° C. in FIG. 1, but begins to decrease rapidly at temperatures higher than 280 ° C. The decrease rate of the storage modulus per 1 ° C. in the range of 275 ° C. to 296 ° C. is large at 67 MPa / ° C. In contrast, it was revealed that the storage modulus of the PAEK resin composition obtained in Example 2 has a higher storage modulus up to 280 ° C. than the PEEK used in Comparative Example 1. In addition, the storage modulus of the PAEK resin composition obtained in Example 2 maintains a high value up to 275 ° C. in FIG. 1. Although it decreases rapidly at temperatures higher than 275 ° C., unlike the PAEK used in Comparative Example 2, the decrease becomes gentle at temperatures higher than 275 ° C., and it was revealed that the decrease rate of the storage modulus per 1 ° C. in the range of 275 ° C. to 296 ° C. is small at 11 MPa / ° C.

The dynamic viscoelasticity measurement results of the PAEK resin composition obtained in Example 3, the PEEK used in Comparative Example 1, and the PAEK having a repeating unit represented by the chemical formula (1B-1) used in Comparative Example 3 are summarized in FIG. 2.
The storage modulus of the PAEK used in Comparative Example 3 does not decrease significantly up to 250° C. in FIG. 2, but begins to decrease rapidly at temperatures higher than 250° C. and continues to decrease to less than 10 MPa. In the range from 250° C. to 275° C., the decrease rate of the storage modulus per degree C. is large at 42 MPa/° C.
In contrast, it was revealed that the storage modulus of the PAEK resin composition obtained in Example 3 was higher up to 260° C. than that of the PEEK used in Comparative Example 1. In addition, the storage modulus of the PAEK resin composition obtained in Example 3 maintains a high value up to 250° C. in FIG. 2. Although the storage modulus drops sharply at temperatures higher than 250° C., unlike the PAEK used in Comparative Example 3, the drop once slows down at temperatures higher than 250° C., and it was revealed that the rate of decrease in the storage modulus per degree C. in the range from 250° C. to 275° C. is small at 17 MPa/° C.

The dynamic viscoelasticity measurement results of the PAEK resin composition obtained in Example 4, the PEEK used in Comparative Example 1, and the PAEK having a repeating unit represented by the chemical formula (1C-1) used in Comparative Example 4 are summarized in FIG.
The storage modulus of the PAEK used in Comparative Example 4 does not decrease significantly up to 240° C. in FIG. 3, but decreases rapidly at temperatures higher than 240° C. and continues to decrease to less than 10 MPa.
In contrast, it was revealed that the storage modulus of the PAEK resin composition obtained in Example 4 was higher up to 240° C. than that of the PEEK used in Comparative Example 1. In addition, the storage modulus of the PAEK resin composition obtained in Example 4 maintained a high value up to 240° C. in FIG. 3. Although the storage modulus dropped sharply at temperatures higher than 240° C., it was revealed that, unlike the PAEK used in Comparative Example 4, the drop once became gentler at temperatures higher than 240° C.

The results of dynamic viscoelasticity measurement of the PAEK resin compositions obtained in Examples 5 and 6 and the PEEK used in Comparative Example 1 are shown together in FIG.
The storage modulus of the PEEK used in Comparative Example 1 significantly decreased from 1646 MPa to 223 MPa as the temperature increased from 150°C to 200°C.
In contrast, it was revealed that the storage modulus of the PAEK resin compositions obtained in Examples 5 and 6 was higher than that of the PEEK used in Comparative Example 1 up to 296°C, which is the upper limit of the measurement temperature range.
In addition, it was revealed that at 296°C, which is the upper limit of the measurement temperature range, the storage modulus of the PAEK resin compositions obtained in Examples 5 and 6 was 114 MPa, which was higher than the 91 MPa of the PEEK used in Comparative Example 1.

From the above, it has become clear that the PAEK resin composition of the present invention is a resin material with improved load-bearing capacity at high temperatures without the addition of reinforcing agents or fillers.

Claims

A polyaryletherketone resin composition comprising a first resin component and a second resin component.
[First resin component]
A polyaryl ether ketone having a glass transition temperature of 200° C. or higher and a weight average molecular weight in the range of 2,000 to 1,000,000.
[Second resin component]
A polyaryl ether ketone having a glass transition temperature of 100° C. or higher and lower than 220° C. and a weight average molecular weight of 2,000 or higher and 1,000,000 or lower.
The polyaryletherketone resin composition according to claim 1, wherein the first resin component and the second resin component are mutually incompatible polyaryletherketones.
The polyaryletherketone resin composition according to claim 1, wherein at least one of the first resin component and the second resin component is a crystalline polyaryletherketone.
The polyaryl ether ketone resin composition according to claim 1, wherein the weight ratio of the first resin component to the second resin component is in the range of 1:99 to 99:1 (first resin component:second resin component).
The polyaryl ether ketone resin composition according to claim 1, wherein the polyaryl ether ketone of the first resin component has a repeating unit represented by general formula (1A), (1B) or (1C).
(In the formula, each R 1 independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
(In the formula, each R 1 independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
(In the formula, each R 1 independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
The polyaryl ether ketone of the second resin component is a polyaryl ether ketone containing any one or more of the repeating units represented by chemical formulas (4a) to (4e). The polyaryl ether ketone resin composition according to claim 1.
The polyaryl ether ketone resin composition according to claim 1, having a storage modulus of 400 MPa or more at a temperature of 200°C.
A molded article made from the polyaryl ether ketone resin composition according to any one of claims 1 to 7.
A method for producing a polyaryl ether ketone resin composition, comprising mixing a first resin component and a second resin component in a molten state.
[First resin component]
A polyaryl ether ketone having a glass transition temperature of 200° C. or higher and a weight average molecular weight in the range of 2,000 to 1,000,000.
[Second resin component]
A polyaryl ether ketone having a glass transition temperature of 100° C. or higher and lower than 220° C. and a weight average molecular weight of 2,000 or higher and 1,000,000 or lower.
The method for producing a polyaryl ether ketone resin composition according to claim 9, wherein the first resin component and the second resin component are mutually incompatible polyaryl ether ketones.
The method for producing a polyaryl ether ketone resin composition according to claim 9, wherein at least one of the first resin component and the second resin component is a crystalline polyaryl ether ketone.
The method for producing a polyaryl ether ketone resin composition according to claim 9, wherein the weight ratio of the first resin component to the second resin component is in the range of 1:99 to 99:1.
The method for producing a polyaryl ether ketone resin composition according to claim 9, wherein the polyaryl ether ketone of the first resin component has a repeating unit represented by general formula (1A), (1B) or (1C).
(In the formula, each R 1 independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
(In the formula, each R 1 independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
(In the formula, each R 1 independently represents an alkyl group having 1 to 4 carbon atoms, and each n independently represents 0, 1, or 2.)
The polyaryl ether ketone of the second resin component is a polyaryl ether ketone containing any one or more of the repeating units represented by chemical formulas (4a) to (4e). The method for producing a polyaryl ether ketone resin composition according to claim 9.
The method for producing a polyaryl ether ketone resin composition according to claim 9, wherein the storage modulus of the resulting polyaryl ether ketone resin composition at a temperature of 200°C is 400 MPa or more.