JPH0571631B2 - - Google Patents

Description

[Detailed description of the invention]

[Industrial Application Fields] The present invention has improved moldability, dimensional stability, mechanical properties,
The present invention relates to a magnetic composite material composition that has excellent heat resistance, flame retardancy, and magnetic properties. [Prior art and problems] At present, magnetic composite materials made of resin and magnetic substances have better mechanical properties, workability, and dimensional accuracy than general sintered magnets, and have stable magnetic properties. Because of this, they are used in a variety of applications such as transformers, motors, and switches. The resins used include epoxy and phenolic resins for thermosetting types, and polypropylene, ethylene-vinyl acetate copolymer, nylon, PBT, and PPS for thermoplastic types.
etc. In general, the maximum energy product increases in proportion to the amount of magnetic material added, and
The thermosetting type allows a larger amount of magnetic material to be added than the thermoplastic type, and the maximum energy product obtained is larger. However, in the case of such thermosetting resin,
There are difficulties in mass production as a composite magnetic material. On the other hand, thermoplastic resins have the advantage of being mass-producible, but have the disadvantage of poor moldability and heat resistance. [Means for Solving the Problems] In view of the above points, the present inventors conducted extensive research and found that if a polymer composition that forms an anisotropic melt phase that can be melt-processed is mixed with magnetic powder as a binder resin, The polymer compositions exhibiting the above-mentioned melt anisotropy have a high melt viscosity because the polymer chains are highly oriented even when no external stress such as stretching is applied during melting, that is, even in a static state. becomes abnormally low,
The magnetic composite material contains a large amount of magnetic material and can be easily processed by injection molding, extrusion molding, compression molding, etc., and the resulting magnetic composite material has excellent properties such as dimensional stability, mechanical properties, heat resistance, and flame retardancy. found that it is excellent. A composite material composition based on this knowledge was previously filed as Japanese Patent Application No. 191368-1982. However, subsequent research has shown that the fluidity of the above composition during melting is still insufficient.
Therefore, there were some difficulties in the magnetic properties of the obtained molded product. Furthermore, there was room for improvement in the mechanical properties of the molded product, especially the impact resistance. As a result of further research, the present inventors found that by adding a specific surface treatment agent to the above composition, the composition had even greater heat resistance.
The inventors have discovered that it is possible to obtain a composition that has improved mechanical strength, improved fluidity during melting, and improved magnetic properties and mechanical strength, leading to the present invention. (A) magnetic powder, (B) binder resin consisting of a melt-processable polymer composition that forms an anisotropic melt phase, (C) low-viscosity, liquid silicone oil with a decomposition temperature of 270°C or higher. The present invention relates to a composite material composition formed by melt-mixing one or more additives selected from the group consisting of a substance and an organic titanate-based or organic silane-based coupling agent, and the binder resin of the present invention is used as a composite material composition. When used, a magnetic composite material composition containing a large amount of magnetic powder with a binder resin content of 80 to 95% by weight based on the total amount of magnetic powder and binder resin can be easily melted and molded to have excellent properties. It is possible to obtain the desired object. The preferred binder resin content is 5 to 50% by weight, especially 7 to 20% by weight. The binder resin of the present invention is a thermoplastic melt processable polymer composition that exhibits optical anisotropy when melted, and is generally classified as a thermotropic liquid crystal polymer. Polymers that form such an anisotropic melt phase have a property in which polymer molecular chains are regularly arranged in parallel in a molten state. The state in which the molecules are arranged in this way is often called the liquid crystal state or the nematic phase of liquid crystalline substances. Such polymers are generally elongated, oblate, and are made from monomers that are fairly rigid along the long axis of the molecule and have multiple chain length bonds, usually in either coaxial or parallel relationships. Manufactured. The nature of the anisotropic melt phase can be confirmed by conventional polarization testing using crossed polarizers.
More specifically, the confirmation of the anisotropic melt phase is based on the Leitz
This can be done by observing a sample placed on a Leitz hot stage under a nitrogen atmosphere at 40x magnification using a polarizing microscope. The polymer is optically anisotropic. That is, it transmits light when examined between orthogonal polarizers. If the sample is optically anisotropic, polarized light will pass through it even if it is at rest. The constituent components of the polymer forming the anisotropic melt phase as described above include one or more of aromatic dicarboxylic acids and alicyclic dicarboxylic acids, one of aromatic diols, alicyclic diols, and aliphatic diols. Consists of one or more aromatic hydroxycarboxylic acids Consists of one or more aromatic thiol carboxylic acids Consists of one or more of aromatic dithiols, aromatic thiol phenols Polyesters consisting of one or more of aromatic hydroxyamines and aromatic diamines, etc., and polymers that form an anisotropic melt phase are polyesters consisting only of () and (). It is composed of combinations such as polyester ester (2) consisting of polyester (2); Additionally, although not included in the above component combinations, polymers that form anisotropic melt phases include aromatic polyazomethyl; specific examples of such polymers include poly(nitrilo-2-methyl-
1,4-phenylenenitroethyridine-1,4-
phenylene ethyridine); poly(nitrilo-2-
methyl-1,4-phenylenenitriloethyridine-1,4-phenylenemethylidine); and poly(nitrilo-2-chloro-1,4-phenylenenitriloethyridine-1,4-phenylenemethylidine) can be mentioned. Although not included in the above-mentioned combination of components, polyester carbonate is also included as a polymer that forms an anisotropic melt phase. It may consist essentially of 4-oxybenzoyl units, dioxyphenyl units, dioxycarbonyl units and terephthaloyl units. The compounds constituting the above () to () are listed below. Examples of aromatic dicarboxylic acids include terephthalic acid,
4,4'-diphenyldicarboxylic acid, 4,4'-triphenyldicarboxylic acid, 2,4-naphthalene dicarboxylic acid, diphenyl ether-4,4'-dicarboxylic acid, diphenoxyethane-4,4'- dicarboxylic acid, diphenoxybutane-4,4'-dicarboxylic acid, diphenylethane-4,4'-dicarboxylic acid,
Aromatics such as isophthalic acid, diphenyl ether-3,3'-dicarboxylic acid, diphenoxyethane-3,3'-dicarboxylic acid, diphenylethane-3,3'-dicarboxylic acid, naphthalene-1,6-dicarboxylic acid Dicarboxylic acids or alkyl, alkoxy or halogen substitution of the above aromatic dicarboxylic acids such as chloroterephthalic acid, dichloroterephthalic acid, bromoterephthalic acid, methylterephthalic acid, dimethylterephthalic acid, ethylterephthalic acid, methoxyterephthalic acid, ethoxyterephthalic acid The body etc. can be mentioned. As the alicyclic dicarboxylic acid, trans-1,
4-Cyclohexanedicarboxylic acid, cis-1,4
-Alicyclic dicarboxylic acids such as cyclohexanedicarboxylic acid, 1,3-cyclohexanedicarboxylic acid, or trans-1,4-(1-methyl)cyclohexanedicarboxylic acid, trans-1,4-(1-
Examples include alkyl, alkoxy, or halogen-substituted alicyclic dicarboxylic acids such as (chloro)cyclohexanedicarboxylic acid. Aromatic diols include hydroquinone, resorcinol, 4,4'-hydroxydiphenyl, 4,
4'-dihydroxyphenyl, 2,6-naphthalenediol, 4,4'-dihydroxydiphenyl ether, bis(4-hydroxyphenoxy)ethane, 3,3'-dihydroxydiphenyl, 3,3'-
Aromatic diols such as dihydroxydiphenyl ether, 1,6-naphthalenediol, 2,2-bis(4-hydroxyphenyl)propane, 2,2-bis(4-hydroxyphenyl)methane, or chlorohydroquinone, methyl Examples include hydroquinone, 1-butylhydroquinone, phenylhydroquinone, methoxyhydroquinone, phenoxyhydroquinone: alkyl, alkoxy or halogen substituted products of the above aromatic diols such as 4-chlorresorcin and 4-methylresorcin. As the alicyclic diol, trans-1,4-
Cyclohexanediol, cis-1,4-cyclohexanediol, trans-1,4-cyclohexanedimethanol, cis-1,4-cyclohexanedimethanol, trans-1,3-cyclohexanediol, cis-1,2-cyclohexanediol, Alicyclic diols such as trans-1,3-cyclohexanedimethanol or the above alicyclic diols such as trans-1,4-(1-methyl)cyclohexanediol and trans-1,4-(1-chloro)cyclohexanediol Examples include alkyl, alkoxy or halogen substituted diols. Examples of aliphatic diols include linear or branched aliphatic diols such as ethylene glycol, 1,3-propanediol, 1,4-butadiol, and neopentyl glycol. Aromatic hydroxycarboxylic acids include 4-hydroxybenzoic acid, 3-hydroxybenzoic acid, 6-hydroxybenzoic acid,
- Aromatic hydroxycarboxylic acids such as hydroxy-2-naphthoic acid and 6-hydroxy-1-naphthoic acid, or 3-methyl-4-hydroxybenzoic acid, 3,5-dimethyl-4-hydroxybenzoic acid, 2,6 -dimethyl-4-hydroxybenzoic acid, 3-methoxy-4-hydroxybenzoic acid,
3,5-dimethoxy-4-hydroxybenzoic acid,
6-hydroxy-5-methyl-2-naphthoic acid,
6-hydroxy-5-methoxy-2-naphthoic acid, 3-chloro-4-hydroxybenzoic acid, 2-
Chloro-4-hydroxybenzoic acid, 2,3-dichloro-4-hydroxybenzoic acid, 3,5-dichloro-4-hydroxybenzoic acid, 2,5-dichloro-4-hydroxybenzoic acid, 3-bromo-4- Aromatic hydroxycarbons such as hydroxybenzoic acid, 6-hydroxy-5-chloro-2-naphthoic acid, 6-hydroxy-7-chloro-2-naphthoic acid, 6-hydroxy-5,7-dichloro-2-naphthoic acid, etc. Examples include alkyl, alkoxy or halogen substituted acids. Examples of aromatic mercaptocarboxylic acids include 4-mercaptobenzoic acid, 3-mercaptobenzoic acid, and 6-mercaptobenzoic acid.
Mercapto-2-naphthoic acid, 7-mercapto-
Examples include 2-naphthoic acid. As the aromatic dithiol, benzene-1,4
-dithiol, benzene-1,3-dithiol,
Examples include 2,6-naphthalene-dithiol and 2,7-naphthalene-dithiol. Examples of aromatic mercaptophenols include 4-mercaptophenol, 3-mercaptophenol, 6-mercaptophenol, and 7-mercaptophenol. Aromatic hydroxyamine, aromatic diamines include 4-aminophenol, N-methyl-4-aminophenol, 1,4-phenylenediamine,
N-methyl-1,4-phenylenediamine, N,
N'-dimethyl-1,4-phenylenediamine,
3-aminophenol, 3-methyl-4-aminophenol, 2-chloro-4-aminophenol, 4-amino-1-naphthol, 4-amino-
4'-hydroxydiphenyl, 4-amino-4'-hydroxydiphenyl ether, 4-amino-4'-
Hydroxydiphenylmethane, 4-amino-4'-
Hydroxydiphenyl sulfide, 4,4'-diaminophenyl sulfide (thiodianiline), 4,
4'-diaminodiphenyl sulfone, 2,5-diaminotoluene, 4,4'-ethylene dianiline,
4,4'-diaminodiphenoxyethane, 4,4'-
Examples include diaminodiphenylmethane (methylene dianiline) and 4,4'-diaminodiphenyl ether (oxydianiline). The above polymer () consisting of each of the above components
Among the above-mentioned polymers, () may or may not form an anisotropic melt phase depending on the constituent components, the composition ratio in the polymer, and the sequence distribution. Limited to those that form an anisotropic melt phase. The above (), (), () polyester and () polyester amide which are polymers forming an anisotropic melt phase suitable for use in the present invention are:
They can be produced by a variety of ester-forming methods that allow the reaction of organic monomer compounds having functional groups that form the required repeating units by condensation. For example, the functional groups of these organic monomer compounds may be carboxylic acid groups, hydroxyl groups, ester groups, acyloxy groups, acid halides, amino groups, and the like. The above organic monomer compounds can be reacted without the presence of a heat exchange fluid by a melt acidolysis method. In this method, the monomers are first heated together to form a molten solution of the reactants. As the reaction continues, solid polymer particles become suspended in the liquid. Vacuum may be applied to facilitate removal of by-product volatiles (eg acetic acid or water) during the final stage of condensation. Slurry polymerization techniques can also be employed to form fully aromatic polyesters suitable for use in the present invention. In this process, a solid product is obtained suspended in a heat exchange medium. Regardless of whether the above-mentioned melt acidolysis method or slurry polymerization method is employed, the organic monomer reactant for inducing the fully aromatic polyester is in a modified form (i.e., lower (as an acyl ester). The lower acyl group preferably has about 2 to 4 carbon atoms. Preferably, an acetate ester of such an organic monomer reactant is subjected to the reaction. Furthermore, representative examples of catalysts that can be optionally used in either the melt acidolysis method or the slurry method include:
dialkyltin oxides (e.g. dibutyltin oxide), diaryltin oxides, titanium dioxide,
gaseous acid catalysts such as antimony trioxide, alkoxytitanium silicates, titanium alkoxides, alkali and alkaline earth metal salts of carboxylic acids (e.g. zinc acetate) Lewis (e.g. BF ₃ ), hydrogen halides (e.g. HCI), etc. can be mentioned. The amount of catalyst used is generally based on the total weight of monomers in approximately
0.001 to 1% by weight, especially about 0.01 to 0.2% by weight. Fully aromatic polymers suitable for use in the present invention tend to be substantially insoluble in common solvents and are therefore unsuitable for solution processing. However, as previously mentioned, these polymers can be readily processed using conventional melt processing methods. Particularly preferred fully aromatic polymers are somewhat soluble in pentafluorophenol. Fully aromatic polyesters suitable for use in the present invention generally have a weight average molecular weight of about 2,000 to 200,000;
Preferably about 10,000 to 50,000, particularly preferably about
20000-25000. On the other hand, suitable fully aromatic polyesteramides generally have a molecular weight of about 5000 to
50000, preferably about 10000-30000, for example 15000
~17000. Such molecular weight measurements can be carried out by gel permeation chromatography as well as other standard methods of measuring polymers that do not involve solution formation, such as quantification of end groups by infrared spectroscopy on compression molded films. Alternatively, the molecular weight can be measured using a light scattering method using a pentafluorophenol solution. The safe aromatic polyesters and polyesteramides described above or having an logarithmic viscosity (IV) of at least about 2.0 dl/g, e.g. Generally shown. Particularly preferred anisotropic melt phase forming polyesters for use in the present invention include repeating units containing naphthalene moieties such as 6-hydroxy-2-naphthoyl, 2,6-dihydroxynaphthalene and 2,6-dicarboxynaphthalene. It is contained in an amount of about 10 mol% or more. Preferred polyesteramides are those containing repeating units of the naphthalene moiety described above and a moiety consisting of 4-aminophenol or 1,4-phenylenediamine. Specifically, the details are as follows. (1) A polyester consisting essentially of the following repeating units and:

【formula】

[Formula] The polyester contains about 10 to 90 mole percent units and about 10 to 90 mole percent units. In one embodiment, the units are present in an amount of about 65-85 mole%, preferably about 70-80 mole% (eg, about 75 mole%). In another embodiment, the units are about 15-35
It is present in amounts as low as mole %, preferably about 20-30 mole %. In addition, at least some of the hydrogen atoms bonded to the ring may optionally be
It may be substituted with a substituent selected from the group consisting of an alkyl group having 1 to 4 carbon atoms, an alkoxy group having 1 to 4 carbon atoms, halogen, phenyl, substituted phenyl, and a combination thereof. (2) A polyester consisting essentially of the following repeating units, and:

【formula】

【formula】

[Formula] This polyester contains approximately 30-70 mole percent units. The polyester preferably contains about 40-60 mole% units, about 20-30 mole% units, and about 20-30 mole% units. In addition, at least a portion of the hydrogen atoms bonded to the ring may optionally be a group consisting of an alkyl group having 1 to 4 carbon atoms, an alkoxy group having 1 to 4 carbon atoms, halogen, phenyl, substituted phenyl, or a combination thereof. may be substituted with a substituent selected from. (3) A polyester consisting essentially of the following repeating units, and:

【formula】

[ka]

【formula】

[Formula] (wherein R means methyl, chloro, bromo, or a combination thereof, and is a substituent for a hydrogen atom on an aromatic ring), and contains about 20 to 60 mol% of units; about 5 to 18 mole percent, about 5 to 35 mole percent units, and about 20 to 40 mole percent units. The polyester preferably has about 35-45 mole% units, about 10-15 mole% units, about 15-25 mole% units.
units, and about 25 to 35 mole % units. However, the total molar concentration with the unit is substantially equal to the molar concentration of the unit. In addition, at least some of the hydrogen atoms bonded to the ring are
Optionally, it may be substituted with a substituent selected from the group consisting of an alkyl group having 1 to 4 carbon atoms, an alkoxy group having 1 to 4 carbon atoms, halogen, phenyl, substituted phenyl, and a combination thereof. This fully aromatic polyester is
0.3w/v for pentafluorophenol at 60℃
At least 2.0 dl/g when dissolved in % concentration
For example, it generally exhibits an interactive viscosity of 2.0 to 10.0 dl/g. (4) A polyester consisting essentially of the following repeating units, and:

[ka]

[Chemical formula] Dioxyaryl unit represented by the general formula - [O-Ar-O-] (wherein Ar means a divalent group containing at least one aromatic ring), the general formula

It consists of a dicarboxyaryl unit represented by the formula: (wherein Ar' means a divalent group containing at least one aromatic ring), and the unit is about 20 to 40 mol%, and the unit is 10 mol % but not more than about 50 mole %, more than 5 mole % and not more than about 30 mole % units, and more than 5 mole % and not more than about 30 mole % units. This polyester is preferably
about 20 to 30 mol% (e.g., about 25 mol%) units,
Approximately 25 to 40 mol% (e.g., 35 mol%) units, approx.
15 to 25 mole percent (eg, about 20 mole percent) units; and about 15 to 25 mole percent (eg, about 20 mole percent) units. In addition, at least some of the hydrogen atoms bonded to the ring may have a carbon number of 1
It may be substituted with a substituent selected from the group consisting of ~4 alkyl groups, C1-4 alkoxy groups, halogens, phenyls, substituted phenyls, and combinations thereof. units are those in which the divalent bonds connecting these units to other units on either side within the polymer backbone are arranged symmetrically on one or more aromatic rings (e.g., on a naphthalene ring). It is preferable that they be symmetrical in the sense that they are arranged at para positions with respect to each other or on a diagonal ring. However, asymmetric units such as those derived from resorcinol and isophthalic acid can also be used. Preferred dioxyaryl units are

and the preferred dicarboxyaryl unit is

It is [ ]. (5) A polyester consisting essentially of the following repeating units, and:

[Chemical formula] Dioxyaryl unit represented by the general formula - [O-Ar-O-] (wherein Ar means a divalent group containing at least one aromatic ring), the general formula

It consists of a dicarboxyaryl unit represented by the formula: (wherein Ar' means a divalent group containing at least one aromatic ring); 45 mol%, and contains units in an amount of 5 to 45 mol%. The polyester preferably contains about 20-80 mole% units, about 10-40 mole%
units, and about 10 to 40 mol% units. More preferably, the polyester contains about 60 to 80 mole percent units, about 10 to 20 mole percent units, and about 10 to 20 mole percent units. In addition, at least a portion of the hydrogen atoms bonded to the ring may optionally be a group consisting of an alkyl group having 1 to 4 carbon atoms, an alkoxy group having 1 to 4 carbon atoms, halogen, phenyl, substituted phenyl, or a combination thereof. may be substituted with a substituent selected from. Preferred dioxyaryl units are

and the preferred dicarboxyaryl unit is

It is [ ]. (6) A polysteramide consisting essentially of the following repeating units, and:

[ka] general formula

[Formula] (wherein A means a divalent group containing at least one aromatic ring or a divalent trans-cyclohexane group), General formula - [Y-Ar-Z-] (wherein Ar is at least A divalent group containing one aromatic ring, Y is O,
NH or NR, Z means NH or NR respectively, R means an alkyl group having 1 to 6 carbon atoms or an aryl group), general formula - [O-Ar'-O-] (in the formula, Ar′ means a divalent group containing at least one aromatic ring), and consists of about 10 to 90 mol% of units, about 5 to 45 mol% of units, about 5 to 45 mol% of units, and contains the unit in an amount of about 0 to 40 mol%. In addition, at least a portion of the hydrogen atoms bonded to the ring may optionally be a group consisting of an alkyl group having 1 to 4 carbon atoms, an alkoxy group having 1 to 4 carbon atoms, halogen, phenyl, substituted phenyl, or a combination thereof. may be substituted with a substituent selected from. Preferred dicarboxyaryl units are

[ka] and the preferred unit is

[expression] or

【formula】 and the preferred dioxyaryl unit is

〔Example〕

Examples of the magnetic composite material composition of the present invention are shown below, but the present invention is not limited to these examples. In the examples, all parts represent parts by weight. Examples 1 to 7 Strontium ferrite powder with an average particle size of 1.2 μm, rare earth cobalt with an average particle size of 4 μm, a binder resin consisting of a polymer that forms an anisotropic melt phase described later, various surface treatment agents, and oily substances After blending in the proportions shown in Table 1,
Chips were manufactured by melt extrusion at 300°C. This chip is heated at a cylinder temperature of 300℃ and a mold temperature of 70℃.
Injection molding was performed in a magnetic field at an injection pressure of 800 Kg/cm ² and an applied magnetic field of 12,000 Oe to prepare a disc-shaped test piece with a diameter of 20 mm and a thickness of 5 mm, and the fluidity and magnetic properties during melting were measured. In addition, under the applied molding conditions and without applying a magnetic field, test pieces with a length of 63.6 mm x 6.35 mm x 12.80 mm and a test piece with a length of 130 mm x width 13 mm x 6.4 mm were created. Impact strength and heat distortion temperature were measured. The results are shown in Table 2. Comparative Examples 1 to 4 Experiments were conducted in the same manner as in the examples except that no surface treatment agent or oily substance was used. Second result
Shown in the table. The polymers A, B, C, and D used as the binder resin and forming the anisotropic melt phase have the following structural units.

[ka]

[ka]

【formula】

[Chemical formula] The specific manufacturing methods of the resins A, B, C, and D are described below. <Resin A> 1081 parts by weight of 4-acetoxybenzoic acid, 460 parts by weight of 6-acetoxy-2-naphthoic acid, 166 parts by weight of isophthalic acid, 194 parts by weight of 1,4-diacetoxybenzene
The weight part was charged into a reactor equipped with a stirrer, a nitrogen inlet tube and a distillation tube, and the mixture was heated under a nitrogen stream.
Heated to 260°C. The mixture was vigorously stirred at 260°C for 2.5 hours and then at 280°C for 3 hours while distilling acetic acid from the reactor. Furthermore, the temperature was raised to 320° C., and after stopping the introduction of nitrogen, the pressure in the reactor was gradually reduced to 0.1 mmHg after 15 minutes, and the mixture was stirred at this temperature and pressure for 1 hour. The resulting polymer had an intrinsic viscosity of 5.0, measured in pentafluorophenol at 60° C. at a concentration of 0.1% by weight. <Resin B> 1081 parts by weight of 4-acetoxybenzoic acid, 2,6-
489 parts by weight of diacetoxynaphthalene and 332 parts by weight of terephthalic acid were charged into a reactor equipped with a stirrer, a nitrogen inlet tube, and a distillation tube, and the mixture was heated to 250° C. under a nitrogen stream. The mixture was vigorously stirred at 250°C for 2 hours and then at 280°C for 2.5 hours while distilling acetic acid from the reactor. Furthermore, the temperature was raised to 320℃,
After stopping the introduction of nitrogen, the pressure in the reactor was gradually reduced to 0.2 mmHg after 30 minutes, and at this temperature,
Stirred at pressure for 1.5 hours. The resulting polymer had an intrinsic viscosity of 2.5, measured in pentalfluorophenol at 60° C. and a concentration of 0.1% by weight. <Resin C> 1261 parts by weight of 4-acetoxybenzoic acid, 691 parts by weight of 6-acetoxy-2-naphthoic acid, a stirrer,
The mixture was charged into a reactor equipped with a nitrogen inlet tube and a distillation tube, and heated to 250° C. under a nitrogen stream.
The mixture was vigorously stirred at 250°C for 3 hours and then at 280°C for 2 hours while distilling acetic acid from the reactor. Furthermore,
After raising the temperature to 320℃ and stopping the introduction of nitrogen, the pressure inside the reactor was gradually reduced and the pressure was increased after 20 minutes.
The temperature was lowered to 0.1 mmHg, and the mixture was stirred for 1 hour at this temperature and pressure. The resulting polymer had an intrinsic viscosity of 5.4, measured in pentalfluorophenol at a concentration of 0.1% by weight at 60°C. <Resin D> 1612 parts by weight of 6-acetoxy-2-naphthoic acid,
290 parts by weight of 4-acetoxyacetanilide, 249 parts by weight of terephthalic acid, and 0.4 parts by weight of sodium acetate were charged into a reactor equipped with a stirrer, a nitrogen introduction pipe, and a distillation pipe, and the mixture was heated to 250°C under a nitrogen stream. did. 250 while distilling acetic acid from the reactor.
Stir vigorously for 1 hour at 300°C and then for 3 hours at 300°C.
Further, the temperature was raised to 340°C, and after stopping the introduction of nitrogen, the pressure inside the reactor was gradually reduced, and after 30 minutes, the pressure was lowered to 0.2 mmHg, and stirring was continued at this temperature and pressure for 30 minutes. The resulting polymer had an intrinsic viscosity of 3.9, measured in pentafluorophenol at a concentration of 0.1% by weight at 60°C.

【table】

【table】

Claims (1)

[Claims] 1. (A) magnetic powder, (B) binder resin consisting of a melt-processable polymer composition forming an anisotropic melt phase, (C) silicone-based having a decomposition temperature of 270°C or higher. A composite material composition prepared by melt-mixing one or more additives selected from the group consisting of a low-viscosity, liquid oily substance and an organic titanate-based or organic silane-based coupling agent. 2. The composite material composition according to claim 1, wherein the organic silane coupling agent is an epoxy or thiol coupling agent. 3. The composite material composition according to claim 1 or 2, wherein the coupling agent has a decomposition temperature of 300°C or higher. 4 The coupling agent is 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethyldimethoxysilane, 2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane,
or 3-mercaptopropyltrimethoxysilane, the composite material composition according to claim 3.