TW201736121A - Polybutylene terephthalate resin composition and metal composite component - Google Patents

Abstract

A polybutylene terephthalate resin composition which contains (A) a polybutylene terephthalate resin, (B) a polyethylene terephthalate resin and (C) an epoxy group-containing olefin copolymer that contains (c-1) a constituent unit derived from an [alpha]-olefin and (c-2) a constituent unit derived from a glycidyl ester of an [alpha], [beta]-unsaturated acid. A molded article of this polybutylene terephthalate resin composition, which is molded at a molding temperature of 260 DEG C under a holding pressure of 80 MPa with a mold temperature of 80 DEG C in accordance with ISO 3167 (Type A test piece), has a surface roughness of 0.50 [mu]m or less. The content of the epoxy groups in the epoxy group-containing olefin copolymer (C) is from 0.01% by mass to 0.35% by mass (inclusive) relative to the total mass of the polybutylene terephthalate resin composition; and the content of (meth)acrylate ester structures is 1.5% by mass or less relative to the total mass of the polybutylene terephthalate resin composition.

Description

Polybutylene terephthalate resin composition and metal composite member

Embodiments of the present invention relate to a polybutylene terephthalate resin composition. Further, in the embodiment of the present invention, there is also a metal composite member using the polybutylene terephthalate resin composition.

The metal composite member produced by laminating a thermoplastic resin and a metal member by a molding method such as insert molding, insert molding, or hoop molding can be widely used in home electric appliances, information communication equipment, automobile components, and the like. In the case of the thermoplastic resin used in such a metal composite member, it has been reviewed that it can be melt-molded by injection molding or the like, and mechanical properties, heat resistance, electrical properties, weather resistance, water resistance, chemical resistance, solvent resistance, and the like. A polybutylene terephthalate resin composition excellent in various characteristics.

When the polybutylene terephthalate resin composition is insert-molded by a metal member such as a metal terminal, the adhesion between the resin portion formed of the resin composition and the metal member is insufficient, and the airtightness of the interface is insufficient. And the problem of peeling and destruction from the bad part of the connection. Therefore, it is necessary to improve the adhesion between the resin portion and the metal member. Further, in many applications, such as the frame of the mobile terminal device which is required to be broken when it is dropped, impact resistance is required in addition to the adhesion to the metal. At the same time, as the material used in the communication machine components such as the frame of the mobile terminal device, it is necessary to prevent the communication characteristics from being obstructed. It can suppress low transmission loss and low dielectric loss tangent.

In terms of improving the adhesion between the metal member and the resin portion, it is possible to review the mechanical/chemical surface treatment on the metal member so that the metal surface has an anchor such as unevenness, a functional group, and an adhesive layer. the way. For example, JP-A-2006-027018 discloses a method of forming a fine concavo-convex layer on a metal-shaped object, and immersing the solution in a water-soluble alcohol after ejecting the metal-shaped object and the resin composition by injection molding. .

On the other hand, in the case of the polybutylene terephthalate resin composition, a review has been made to improve the adhesion to metals. For example, in the publication of Patent International Publication No. 2011/155289, a polybutylene terephthalate resin composition which can also have excellent adhesion to a metal member at a mold temperature of 100 ° C or less is disclosed. A resin composition of a polybutylene terephthalate resin and a specific amount of a modified polyethylene terephthalate resin. Further, in the publication of Patent International Publication No. 2009/081549, a resin composition which can also be formed at a mold temperature of 100 ° C or lower, which is a polytetraphthalic acid containing a fibrous reinforcing agent and a thermoplastic elastomer, has also been disclosed. A butyl diester resin composition or a modified polybutylene terephthalate resin composition containing a specific modified polybutylene terephthalate resin and a fibrous reinforcing agent.

[Previous Technical Literature]

[Patent Literature]

Patent Document 1 Patent Publication No. 2006-027018

[Patent Document 2] Patent International Publication No. 2011/155289

[Patent Document 3] Patent International Publication No. 2009/081549

Therefore, although various reviews as described above have been carried out, it is necessary to further develop a polybutylene terephthalate resin composition which is excellent in adhesion to metal and which has good impact resistance and low dielectric loss tangent.

Therefore, in the embodiment of the present invention, a polybutylene terephthalate resin composition excellent in balance of metal adhesion, impact resistance, and dielectric loss tangent is provided.

That is, the embodiment of the present invention relates to the following items.

[1] A polybutylene terephthalate resin composition comprising: (A) a polybutylene terephthalate resin, (B) a polyethylene terephthalate resin, and containing: C-1) (C) an epoxy group-containing olefin copolymer derived from a constituent unit of an α-olefin and (c-2) a constituent unit derived from a glycidyl ester of an α,β-unsaturated acid; With a molding temperature of 260 ° C, a mold temperature of 80 ° C, and a holding pressure of 80 MPa, the surface roughness of the molded article according to ISO 3167 (Type A test sheet) has an arithmetic mean roughness of 0.50 μm or less; The content of the epoxy group in the (C) epoxy group-containing olefin copolymer is 0.01% by mass or more and 0.35% by mass or less based on the entire polybutylene terephthalate resin composition, and is also relative to the polyterephthalic acid. The content of the (meth) acrylate structure is 1.5% by mass or less based on the entire butyl diester resin composition.

[2] The polybutylene terephthalate resin composition according to the above [1], wherein a dielectric loss tangent at 2 GHz measured by a cavity resonator perturbation method is 0.01 or less.

[3] The polybutylene terephthalate resin composition according to the above [1] or [2], which further comprises (D) a glass fiber.

[4] The polybutylene terephthalate resin composition according to any one of the above [1], wherein the molded article is subjected to a shock ratio measured according to the method of ISO 179/1eA. The strength is 7 kJ/m ² or more.

The polybutylene terephthalate resin composition according to any one of the above aspects, wherein the (C) epoxy group-containing olefin copolymer does not contain The constituent unit derived from (meth) acrylate.

[6] The polybutylene terephthalate resin composition according to any one of the above [1], wherein the molding temperature is 260 ° C, the mold temperature is 80 ° C, and the holding pressure is maintained. The molding condition of 80 MPa, the shrinkage of the molded article according to ISO 3167 (Type A test sheet) was 0.20 or less.

[7] The polybutylene terephthalate resin composition according to any one of the above [1] to [6], which is used for a metal composite member.

[8] A metal composite member comprising the resin portion composed of the polybutylene terephthalate resin composition according to any one of the above items [1] to [7], and a metal member. .

[9] The metal composite member according to the above [8], wherein the metal member contains a fine uneven surface.

[10] The metal composite member according to the above [8], wherein the bonding strength between the resin portion composed of the polybutylene terephthalate resin composition and the metal member is 30 MPa or more.

[11] The metal complex according to any one of the above [8] to [10] The composite member, wherein the metal composite member is a communication machine member.

According to the embodiment of the present invention, a polybutylene terephthalate resin composition excellent in balance of metal adhesion, impact resistance and dielectric loss tangent can be provided.

[Fig. 1A] is a schematic cross-sectional view showing an example of a glass fiber having a non-circular cross section.

[Fig. 1B] is a schematic cross-sectional view showing an example of a glass fiber having a non-circular cross section.

[Fig. 1C] is a schematic cross-sectional view showing an example of a glass fiber having a non-circular cross section.

[Fig. 2] is a top surface pattern diagram of a test sheet for evaluating surface roughness and shrinkage. The figure also shows the dimensions of the various parts of the mold. The symbol "h" in the figure indicates the thickness of the test sheet.

Hereinafter, the preferred embodiments of the present invention will be described, but the present invention is not limited to the embodiments described below.

<Polybutylene terephthalate resin composition>

The present inventors have found that: (A) a polybutylene terephthalate resin, (B) a polyethylene terephthalate resin, and a component comprising: (c-1) derived from an α-olefin And (c-2) an epoxy group-containing olefin copolymer derived from a constituent unit of a glycidyl ester of an α,β-unsaturated acid, and having a rough surface of the molded article (Ra), the content (% by mass) of the epoxy group in the epoxy group-containing olefin copolymer of the entire polybutylene terephthalate resin composition, and the amount of the polybutylene terephthalate When the content (% by mass) of the (meth) acrylate structure of the entire ester resin composition is within a specific range, polybutylene terephthalate having excellent balance of metal adhesion, impact resistance, and dielectric loss tangent can be obtained. Resin composition.

That is, the polybutylene terephthalate resin composition according to an embodiment of the present invention is characterized by comprising: (A) polybutylene terephthalate resin, and (B) polyethylene terephthalate a diester resin and a (C) epoxy group containing: (c-1) a constituent unit derived from an α-olefin and (c-2) a constituent unit derived from a glycidyl ester of an α,β-unsaturated acid The olefin-based copolymer; the surface roughness (Ra) of the molded article is 0.50 μm or less; and the (C) epoxy group-containing olefin system is derived from the entire polybutylene terephthalate resin composition. The content of the epoxy group in the copolymer is 0.01% by mass or more and 0.35% by mass or less; and the content of the (meth) acrylate structure in the entire composition of the polybutylene terephthalate resin composition is 1.5% by mass or less.

<surface roughness (Ra)>

In the present specification, the "surface roughness (Ra)" is an index of the surface characteristics of a molded article formed by using the polybutylene terephthalate resin composition of the embodiment of the present invention, specifically, The arithmetic mean roughness Ra of the molded article formed of the butylene terephthalate resin composition. The surface roughness Ra can be obtained by (1) producing a test sheet according to ISO 3167 (Type A test sheet), and (2) measuring the surface roughness of a predetermined portion on the test sheet by a surface roughness measuring machine. Determination. Examples of the measurement conditions will be described in detail in the examples. The example shown in Fig. 2 is a test sheet. The test sheet can be implemented as In the example, the polybutylene terephthalate resin composition was molded at a molding temperature of 260 ° C, a mold temperature of 80 ° C, and a holding pressure of 80 MPa.

In the polybutylene terephthalate resin composition of the present embodiment, the surface roughness (Ra) of the molded article is preferably 0.50 μm or less, more preferably 0.48 μm or less, and still more preferably 0.46 μm or less. When a polybutylene terephthalate resin composition having a surface roughness (Ra) of 0.50 μm or less is used, the airtightness of the interface between the resin portion and the metal member of the metal composite member can be improved.

<shrinkage rate>

In the present specification, the "shrinkage ratio" is an index of the dimensional stability of the polybutylene terephthalate resin composition in the embodiment of the present invention, and may be (1) in accordance with ISO 3167 (Type A test sheet). Making test sheets, (2) measuring the size of the predetermined portion of the test sheet, and (3) following

(formula) shrinkage ratio (%) = {1 - (I _a / I _b )} × 100 (%)

(wherein, I _a represents the size (mm) of the predetermined portion of the test sheet, and I _b is the mold size (mm) of the portion)

Calculation. Examples of the measurement conditions will be described in detail in the examples.

The example shown in Fig. 2 is a test sheet. The test sheet, as set forth in the examples, was formed by forming a polybutylene terephthalate resin composition at a molding temperature of 260 ° C, a mold temperature of 80 ° C, and a holding pressure of 80 MPa.

In the polybutylene terephthalate resin composition of the present embodiment, the shrinkage ratio at the time of molding is preferably 0.20% or less, more preferably 0.19% or less, and still more preferably 0.18% or less. When the polybutylene terephthalate resin composition having a shrinkage ratio at the time of molding of 0.20% or less is used, it is possible to easily suppress peeling of the interface between the resin portion and the metal member by cooling during molding.

<Shaby impact strength>

Further, in a preferred embodiment of the present invention, the polybutylene terephthalate resin composition preferably has a Sabbi impact strength of 7 kJ/m ² or more as measured by the method of ISO 179/1eA, 10 kJ. More preferably /m ² or more, and 12kJ/m ² or more is even better.

Next, each component will be exemplified.

(A) Polybutylene terephthalate resin

(A) a polybutylene terephthalate resin containing at least a dicarboxylic acid component containing at least terephthalic acid or an ester-forming derivative thereof (such as a C _1-6 alkyl ester or an acid halide) A polybutylene terephthalate resin obtained by polycondensation of a diol component of an alkyl diol (1,4-butanediol) having 4 carbon atoms or an ester-forming derivative thereof (such as an acetamidine compound). (A) The polybutylene terephthalate resin is not limited to a homopolybutylene terephthalate resin, and contains not more than 60 mol% of a butylene terephthalate unit (particularly 75 mol% or more and 95%). Copolymers having a molar ratio of less than or equal to % are also acceptable.

The amount of the carboxyl group at the end of the (A) polybutylene terephthalate resin is not particularly limited as long as it can be used for the purpose of the present invention. (A) The amount of the carboxyl group at the end of the polybutylene terephthalate resin is preferably 30 meq/kg or less, more preferably 25 meq/kg or less. When the amount of the carboxyl group at the terminal is used in the range of the polybutylene terephthalate resin, the obtained metal composite member can be prevented from being hydrolyzed by the moist heat environment to lower the strength.

The ultimate viscosity of the (A) polybutylene terephthalate resin is not particularly limited as long as it is within the scope of the object of the present invention. The ultimate viscosity (IV) of the (A) polybutylene terephthalate resin is preferably 0.60 dL/g or more and 1.2 dL/g or less. More preferably, it is 0.65 dL/g or more and 0.9 dL/g or less. In use When the polybutylene terephthalate resin having a viscosity in this range is limited, the obtained polybutylene terephthalate resin composition can be particularly excellent in formability. Furthermore, the ultimate viscosity can be adjusted by mixing polybutylene terephthalate resins having different ultimate viscosities. For example, when a polybutylene terephthalate resin having an ultimate viscosity of 1.0 dL/g is mixed with a polybutylene terephthalate resin having an ultimate viscosity of 0.7 dL/g, the final viscosity can be adjusted to 0.9 dL/g. Polybutylene terephthalate resin. (A) The ultimate viscosity (IV) of the polybutylene terephthalate resin can be determined as in the case of o-chlorophenol at a temperature of 35 °C.

(A) In the polybutylene terephthalate resin, examples of the dicarboxylic acid component (co-monomer component) other than terephthalic acid and an ester-forming derivative thereof include isophthalic acid, C _8-14 aromatic dicarboxylic acid such as phthalic acid, 2,6-naphthalenedicarboxylic acid or 4,4'-dicarboxydiphenyl ether; succinic acid, adipic acid, sebacic acid, sebacic acid An alkyl dicarboxylic acid such as C _4-16 ; a C _5-10 cycloalkanedicarboxylic acid such as cyclohexane dicarboxylic acid; an ester-forming derivative of such a dicarboxylic acid component (alkyl ester of C _1-6 ) Derivatives and acid halides, etc.). These dicarboxylic acid components may be used singly or in combination of two or more kinds.

Among such dicarboxylic acid components, a C _2-12 aromatic dicarboxylic acid such as isophthalic acid, and a C _6-12 alkanedicarboxylic acid such as adipic acid, sebacic acid or sebacic acid are preferred.

(A) In the polybutylene terephthalate resin, a diol component (co-monomer component) other than 1,4-butanediol may, for example, be ethylene glycol, propylene glycol or trimethylene. C _2-10 alkanediol such as alcohol, 1,3-butanediol, hexamethylene glycol, neopentyl glycol, 1,3-octanediol; diethylene glycol, triethylene glycol Polyoxyalkylene glycol such as dipropylene glycol; cyclohexane diol such as cyclohexane dimethanol or hydrogenated bisphenol A; aromatic diol such as bisphenol A or 4,4'-dihydroxybiphenyl; oxygen of bisphenol A Ethylene 2 molar addition, bisphenol A oxypropylene 3 molar addition, etc., bisphenol A C _2-4 oxy olefin adduct; or ester forming derivative of such diol (B Telluride, etc.). These diol components may be used singly or in combination of two or more kinds.

Among such diol components, a C _2-6 alkanediol such as ethylene glycol or trimethylene glycol, a polyoxyalkylene glycol such as diethylene glycol, or an alicyclic diol such as cyclohexane dimethanol And so on.

Examples of the comonomer component which can be used in addition to the dicarboxylic acid component and the diol component include 4-hydroxybenzoic acid, 3-hydroxybenzoic acid, 6-hydroxy-2-naphthoic acid, and 4-carboxy-4. An aromatic hydroxycarboxylic acid such as '-hydroxybiphenyl; an aliphatic hydroxycarboxylic acid such as glycolic acid or hydroxycaproic acid; propyl lactone, butyrolactone, valerolactone, caprolactone (ε-caprolactone, etc.) _3-12 lactone; an ester-forming derivative of such a comonomer component (alkyl ester derivative of _C1-6 , acid halide, acetylide, etc.).

All of the polybutylene terephthalate copolymers copolymerized with the comonomer components described above are suitably used as the (A) polybutylene terephthalate resin. Further, in the case of the (A) polybutylene terephthalate resin, a homopolybutylene terephthalate polymer and a polybutylene terephthalate polymer may be used in combination.

(B) Polyethylene terephthalate resin

(B) Polyethylene terephthalate resin, which is a terephthalic acid or an ester-forming derivative thereof (alkyl ester of _C1-6 , acid halide, etc.), and ethylene glycol or an ester thereof A forming derivative (acetate, etc.), a polyester resin obtained by polycondensation in a generally known manner.

(B) Polyethylene terephthalate resin, in the range of the object of the present invention, may be a small amount of a modified component which can provide a repeating unit other than a p-xylylene unit and a dioxyethylene unit. The person who has been upgraded. Polyparaphenylene The amount of the repeating unit other than the terephthalic acid unit and the dioxyethylene unit contained in the acid ethylene glycol resin is less than 4 m in all the repeating units of the polyethylene terephthalate resin. % is better, 3 mol% or less is better, and 2 mol% is better.

Further, the (B) polyethylene terephthalate resin may be a repeating unit derived from the above-mentioned modified component, and contains 4 moles in all repeating units of the (B) polyethylene terephthalate resin. More than %. In the present specification, such a polyethylene terephthalate resin may be referred to as "modified polyethylene terephthalate resin".

The modified polyethylene terephthalate resin may also contain a dicarboxylic acid other than terephthalic acid or an ester-forming derivative thereof (C _1-6 alkyl group) within the scope of the object of the present invention. Dicarbonyl units of ester derivatives and acid halides, etc.). The amount of the dicarbonyl unit other than the p-xylylene group unit contained in the modified polyethylene terephthalate resin is preferably 5 mol% or more and 50 mol% or less of the total dicarbonyl unit. 7 mol% or more and 30 mol% or less is more preferable, and particularly preferably 10 mol% or more and 25 mol% or less.

Preferred examples of the dicarboxylic acid or an ester-forming derivative thereof contained in the modifying component include, for example, isophthalic acid, phthalic acid, 2,6-naphthalenedicarboxylic acid, 4,4'. - C _8-14 aromatic dicarboxylic acid such as dicarboxydiphenyl ether; C _4-16 alkanedicarboxylic acid such as succinic acid, adipic acid, sebacic acid or sebacic acid; cyclohexanedicarboxylic acid And a C _5-10 cycloalkanedicarboxylic acid; an ester-forming derivative of such a dicarboxylic acid component (alkyl ester derivative of C _1-6 and acid halide, etc.). Such dicarboxylic acids may be used singly or in combination of two or more kinds.

Among such dicarboxylic acids or ester-forming derivatives thereof, a C _2-12 aromatic dicarboxylic acid such as isophthalic acid or an ester-forming derivative thereof, and adipic acid, sebacic acid, and anthracene A C _6-12 alkanedicarboxylic acid such as a diacid or an ester-forming derivative thereof is preferred. Moreover, since the obtained polybutylene terephthalate resin composition can have excellent metal adhesion and mechanical properties, the dicarboxylic acid or its ester-forming derivative in the modified component, particularly isophthalic acid An ester-forming derivative of diformic acid or isophthalic acid (dimethyl phthalate, diethyl isophthalate, dichloroisophthalic acid, etc.) is preferred.

The modified component used in the production of the polyethylene terephthalate resin may contain a second amount of a dicarboxylic acid or an ester-forming derivative thereof in addition to the object of the present invention. A diol component other than an alcohol and an ester-forming derivative thereof, a hydroxycarboxylic acid component, a lactone component, and the like. In the modified polyethylene terephthalate resin composition, the amount of repeating units derived from the modified components of such a diol component, a hydroxycarboxylic acid component, and a lactone component is all modified polyterephthalic acid. Among all the repeating units in the ethylene glycol resin, 30 mol% or less is preferable, and 25 mol% or less is more preferable, and particularly preferably 20 mol% or less.

Examples of the diol component contained in the modified component include butanediol, trimethylene glycol, 1,4-butanediol, 1,3-butylene glycol, and hexamethylene glycol. a C _2-10 alkyl diol such as neopentyl glycol or 1,3-octanediol; a polyoxyalkylene glycol such as diethylene glycol, triethylene glycol or dipropylene glycol; cyclohexane dimethanol; Hydrogenated diol such as bisphenol A; aromatic diol such as bisphenol A or 4,4'-dihydroxybiphenyl; oxyethylene 2 molar addition of bisphenol A; oxypropylene 3 of bisphenol A An argon adduct or the like, an oxyalkylene adduct of C _2-4 of bisphenol A; or an ester-forming derivative of such a diol (acetamidine or the like). These diol components may be used singly or in combination of two or more kinds.

Examples of the hydroxycarboxylic acid component contained in the modified component include 4-hydroxybenzoic acid, 3-hydroxybenzoic acid, 6-hydroxy-2-naphthoic acid, 4-carboxy-4'-hydroxybiphenyl, and the like. An aromatic hydroxycarboxylic acid; an aliphatic hydroxycarboxylic acid such as glycolic acid or hydroxycaproic acid; or an ester-forming derivative of such a hydroxycarboxylic acid (C _1-6 alkyl ester derivative, acid halide, acetylated product) Wait). These hydroxycarboxylic acid components can be used singly or in combination of two or more kinds.

The lactone component contained in the modified component may, for example, be a C _3-12 lactone such as propiolactone, butyrolactone, valerolactone or caprolactone (ε-caprolactone). Such lactone components may be used singly or in combination of two or more kinds.

(B) The polyethylene terephthalate resin may be used alone or in combination of two or more. From the viewpoint of improving the bonding strength, the polyethylene terephthalate resin (sometimes also referred to as "non-modified polyethylene terephthalate resin") is derived from the above-mentioned modified component. It is preferred that the repeating unit is less than 4 mol% (including 0 mol%) in all the repeating units.

The polyethylene terephthalate resin as described above is presumed to have improved fluidity of the polybutylene terephthalate resin composition in the polybutylene terephthalate resin composition of the present embodiment. Further, the resin composition is allowed to easily enter the fine concavo-convex portion of the surface of the metal member. In addition, it is presumed that the crystallization rate of the polybutylene terephthalate resin composition is lowered to reduce the shrinkage ratio. Therefore, it is possible to exhibit an effect of suppressing the resin which is solidified in the concave portion after cooling from being easily detached from the concave portion. Due to such effects, it is presumed to be related to the improvement of the adhesion of the polybutylene terephthalate resin composition to the metal.

In the present embodiment, the content of the (B) polyethylene terephthalate resin is improved from the viewpoint of improving the adhesion to the metal, and is relative to the (A) polybutylene terephthalate resin. And (B) polyethylene terephthalate The total mass of the ester resin is preferably 1% by mass or more, more preferably 5% by mass or more, and more preferably 50% by mass or less from the viewpoint of further suppressing reduction in mechanical properties and chemical resistance. The content of the polyethylene terephthalate resin is preferably 40% by mass or less, and more preferably 35% by mass or less based on the total mass of the polybutylene terephthalate resin and the polyethylene terephthalate resin. More preferably, it is more preferably 30% by mass or less. Further, it is more preferably 10% by mass or more and 25% by mass or less.

(C) an epoxy group-containing olefin copolymer

The polybutylene terephthalate resin composition of the present embodiment also contains (c-1) a constituent unit derived from an α-olefin, and (c-2) a ring derived from an α,β-unsaturated acid. (C) an epoxy group-containing olefin-based copolymer as a constituent unit of oxypropyl ester. In particular, since the dielectric loss tangent of the obtained polybutylene terephthalate resin composition can be lowered, the epoxy group-containing olefin-based copolymer added to the material for the communication machine component is not derived from The olefin-based copolymer of the constituent unit of (meth) acrylate is preferred. Further, in the following, an ester of (meth)acrylic acid is also referred to as a (meth) acrylate. For example, glycidyl (meth)acrylate is also known as glycidyl (meth)acrylate. In the present specification, "(meth)acrylic acid" means both of acrylic acid and methacrylic acid, and "(meth)acrylate" means both acrylate and methacrylate.

(c-1) The α-olefin derived from the constituent unit of the α-olefin is not particularly limited, and examples thereof include ethylene, propylene, butylene, and the like, and ethylene is particularly preferable. The α-olefin may be used alone or in combination of two or more. When the (C) epoxy group-containing olefin-based copolymer contains (c-1) a constituent unit derived from an α-olefin, it is easy to impart polybutylene terephthalate in the present embodiment. The flexibility of the resin portion formed by the diester resin composition. The imparting flexibility imparts a softness to the resin portion and is associated with an improvement in the bonding strength between the metal member and the resin portion. At the same time, when such an olefin-based copolymer containing an epoxy group is contained, the effect of improving impact resistance is also easily obtained.

(c-2) The glycidyl ester of an α,β-unsaturated acid having a constituent unit of a glycidyl ester of an α,β-unsaturated acid is not particularly limited, and examples thereof include: Glycidyl acrylate, glycidyl methacrylate, glycidyl ethacrylate, etc., and especially glycidyl methacrylate is preferred. (c-2) The glycidyl ester derived from the α,β-unsaturated acid may be used alone or in combination of two or more. When the (C) epoxy group-containing olefin-based copolymer contains a glycidyl ester of an α,β-unsaturated acid, the effect of improving the bonding strength between the metal member and the resin portion can be easily obtained.

In the present embodiment, when the dielectric polybutylene terephthalate resin composition has a lower dielectric loss tangent, (C) the epoxy group-containing olefin copolymer does not contain (meth) The constituent unit of the acrylate is preferable, but may be contained in the range which does not impair the effects of the present invention. The (meth) acrylate is not particularly limited, and examples thereof include methyl acrylate, ethyl acrylate, n-propyl acrylate, isopropyl acrylate, n-butyl acrylate, n-hexyl acrylate, and n-octyl acrylate. Acrylate; methyl methacrylate, ethyl methacrylate, n-propyl methacrylate, isopropyl methacrylate, n-butyl methacrylate, isobutyl methacrylate, n-amyl methacrylate And methacrylate such as n-octyl methacrylate.

The (meth) acrylate may be used alone or in combination of two or more. Dielectric of the resulting polybutylene terephthalate resin composition In view of the reduction in loss tangent, it is preferable that the constituent unit derived from (meth) acrylate is contained. Further, since the constituent unit of the glycidyl ester derived from the α,β-unsaturated acid also contains a (meth) acrylate structure, the propylene oxide derived from the α,β-unsaturated acid is contained therein. When the constituent units of the ester are excessive, the dielectric loss tangent is also increased. Therefore, the content of the entire (meth) acrylate structure of the polybutylene terephthalate resin composition in the present embodiment is not limited to the presence of the constituent unit derived from (meth) acrylate, and includes The amount present in the constituent unit of the glycidyl ester derived from the α,β-unsaturated acid. Further, the content of the entire (meth) acrylate structure of the polybutylene terephthalate resin composition is not limited to (C) (meth)acrylic acid contained in the epoxy group-containing olefin-based copolymer. The content of the ester structure includes a total value of the content when the other component also contains a (meth) acrylate structure. However, from the viewpoint of suppressing the dielectric loss tangent, it is preferable to contain a (meth) acrylate structure without adding other components. The content of the entire (meth) acrylate structure of the polybutylene terephthalate resin composition is preferably 1.5% by mass or less, more preferably 1.0% by mass or less, and even more preferably 0.7% by mass or less, particularly 0.5. More preferably, the mass is below.

An olefin-based copolymer containing a constituent unit derived from an α-olefin and a constituent unit derived from a glycidyl ester of an α,β-unsaturated acid, and other olefins containing a constituent unit derived from a (meth) acrylate The copolymer can be produced by copolymerization in a manner generally known in the art. For example, the above copolymer can be obtained by copolymerization by a generally known radical polymerization reaction. The kind of the copolymer is not particularly relevant, and may be, for example, a random copolymer or a block copolymer. Further, the above olefin-based copolymers such as polymethyl methacrylate, polyethyl methacrylate, polymethyl acrylate, polyethyl acrylate, polybutyl acrylate, polyacrylic acid-2- Ethylhexyl ester, polystyrene, polyacrylonitrile, acrylonitrile/styrene copolymer, butyl acrylate/styrene copolymer, etc., may also be a branched or crosslinked structure and then chemically bonded olefin-based graft copolymer .

In the present embodiment, the (C) epoxy group-containing olefin-based copolymer may contain a constituent unit derived from another copolymerization component in the range of the effects of the present invention.

More specifically, (C) the epoxy group-containing olefin-based copolymer may, for example, be a glycidyl methacrylate-modified ethylene copolymer or a glycidyl ether-modified ethylene copolymer. Among them, a glycidyl methacrylate-modified ethylene-based copolymer is preferred.

Examples of the propylene glycol methacrylate-modified ethylene-based copolymer include a glycidyl methacrylate graft-modified ethylene polymer, an ethylene-glycidyl methacrylate copolymer, and ethylene. Glycidyl methacrylate-methyl acrylate copolymer. Among them, in particular, a metal-resin composite molded body excellent in dielectric loss tangent is preferable, and an ethylene-glycidyl methacrylate copolymer is preferred. Specific examples of the ethylene-glycidyl methacrylate copolymer include "Bond First" (manufactured by Sumitomo Chemical Co., Ltd.).

Examples of the epoxy propylene ether-modified ethylene copolymer include a glycidyl ether graft copolymerized ethylene copolymer and a glycidyl ether-ethylene copolymer.

(C) an epoxy group-containing olefin copolymer, wherein the content of the epoxy group in the (C) epoxy group-containing olefin copolymer is 0.1 to (C) the epoxy group-containing olefin copolymer; 10.0% by mass is preferred, 0.5 to 4.0% by mass is more preferred, and 1.0 to 3.0% by mass is more preferably.

(C) the content of the epoxy group-containing olefin-based copolymer is based on The content of the epoxy group is preferably more than 0% by mass and more preferably 9% by mass or less, more preferably 1.5% by mass or more and 7% by mass or less, based on the total amount of the polybutylene terephthalate resin composition. More than 6% by mass or less is more preferable.

The content of the epoxy group in the (C) epoxy group-containing olefin-based copolymer is preferably 0.01% by mass or more and less than 0.35% by mass, and preferably 0.02% by mass based on the total of the polybutylene terephthalate resin composition. The above is preferably 0.30% by mass or less, more preferably 0.03% by mass or more and 0.20% by mass or less, and more preferably 0.05% by mass or more and 0.25% by mass or less.

The content of the (C) epoxy group-containing olefin-based copolymer, the content of the epoxy group derived from the (C) epoxy group-containing olefin copolymer in the polybutylene terephthalate resin composition, Or when the content of the epoxy group in the (C) epoxy group-containing olefin-based copolymer is in the above range, good impact resistance can be easily maintained, and good bonding between the resin portion and the metal member can be easily obtained. strength.

(D) Glass fiber

The polybutylene terephthalate resin composition of the present embodiment may contain glass fibers at the same time.

(D) Regarding the glass fiber, any generally known glass fiber is suitable for use. There is no particular limitation on the diameter of the glass fiber, the cross-sectional shape of the glass fiber (cylinder, 茧 shape, long circular cross section, etc.), the length at which the fine fiber or the thick fiber is cut, the length at which the short glass ray is produced, and the method of cutting the glass fiber. . In the present embodiment, the type of the glass which is a raw material of the glass fiber is not particularly limited, and it is preferable to use E glass and a corrosion-resistant glass containing a zirconium element in the composition.

According to an embodiment of the present invention, (D) the glass fiber is preferably a non-circular cross section having a longitudinal axis in cross section. Using glass fiber with a non-circular cross section In the case of the dimension, the molding shrinkage ratio and the coefficient of linear expansion of the molded article can be lowered, the dimensional stability can be improved, and the impact resistance can be further improved. For the glass fiber having such a non-circular cross section, a cross section such as a dome shape (Fig. 1A), an oblong shape (Fig. 1B), and an elliptical shape (Fig. 1C) as shown in Figs. 1A to C can be used. By. The cross-sectional odds ratio of such a cross section (a:b of Fig. 1) is preferably 1.5:1 to 6:1, more preferably 2:1 to 5:1, and even more preferably 2.5:1 to 4:1. When the cross-sectional profile ratio is within the above range, the effect of making the cross-section flat is higher, and at the same time, it is possible to further suppress the fiber from being excessively flattened and broken, thereby lowering the strength.

At the same time, in order to improve (D) glass fiber and (A) polybutylene terephthalate resin, (B) polyethylene terephthalate resin, and (C) epoxy group-containing olefin copolymer For the purpose of the interface characteristics of the resin substrate to be formed, the glass fiber may be subjected to surface treatment by an organic treating agent such as a decane compound or an epoxy compound. The type of the decane compound and the epoxy compound is not particularly limited, and any one known in general is suitable for use.

When the (D) glass fiber is contained, the content of the (D) glass fiber is 100 parts by mass based on the total of (A) the polybutylene terephthalate resin and the (B) polyethylene terephthalate resin. It is preferably 20 parts by mass or more and 100 parts by mass or less, more preferably 30 parts by mass or more and 90 parts by mass or less, and still more preferably 40 parts by mass or more and 80 parts by mass or less. When the content of the (D) glass fiber is 20 parts by mass or more based on 100 parts by mass of the total of the (A) polybutylene terephthalate resin and the (B) polyethylene terephthalate resin, When the impact resistance is improved and the amount is 80 parts by mass or less, the fluidity of the resin composition can be further suppressed during molding.

(E) Other ingredients

The polybutylene terephthalate resin composition of the present embodiment is regarded as the And (A) polybutylene terephthalate resin, (B) polyethylene terephthalate resin, (C) epoxy group-containing olefin copolymer, and (D) glass fiber Any component other than that. (E) Other components, for example, antioxidants, heat stabilizers, molecular weight regulators, ultraviolet absorbers, antistatic agents, dyes, pigments, lubricants, mold release agents, crystallization accelerators, crystal nucleating agents A near-infrared ray absorbing agent, a flame retardant, a flame-resistant auxiliaries, a filler other than glass fibers, and the like are not limited thereto.

In the polybutylene terephthalate resin composition of the present embodiment, the total content of the components (A) to (D) is preferably 70% by mass or more, and 80% by mass or more based on the total composition. More preferably, 90% by mass or more is even better. The upper limit is not particularly limited and may be 100% by mass. When the total content of the components (A) to (D) is within the above range, the adhesion to the metal and the dielectric loss tangent are better.

The form of the polybutylene terephthalate resin composition in the present embodiment is preferably at least the components (A) to (C) described above, and at least the components (A) to (D) described above are more preferable. There are no special restrictions. The entire composition of the polybutylene terephthalate resin composition may be integrated into a form of pellets, tablets, or powder by melt-mixing or melt-molding.

(Method for producing polybutylene terephthalate resin composition)

The polybutylene terephthalate resin composition can be produced by various methods generally known in the production method of the thermoplastic resin composition. A preferred method is a method in which the components are mixed and then extruded into pellets by a melt mixing device such as a uniaxial or biaxial extruder.

The composition of polybutylene terephthalate resin in this embodiment Preferably, the dielectric loss tangent at 2 GHz measured by the cavity resonator perturbation method is preferably 0.01 or less. The dielectric loss tangent at 2 GHz measured by the cavity resonator perturbation method was a test piece prepared into a predetermined shape (a cross section of 1.8 mm × 1.8 mm and a length of 80 mm) at a molding temperature of 260 ° C and a mold temperature of 80 ° C. The value of the dielectric loss tangent at 2 GHz at 23 ° C as measured by the cavity resonator perturbation method.

<Formed product of polybutylene terephthalate resin composition>

The method of obtaining a molded article of the polybutylene terephthalate resin composition of the present embodiment is not particularly limited, and a generally known method can be employed. For example, pellets of a polybutylene terephthalate resin composition are added to an injection molding machine of a predetermined mold of the apparatus, and then produced by injection molding.

<Metal composite member>

As described above, since the polybutylene terephthalate resin composition of the present embodiment is excellent in adhesion to metal, it is suitably used for a metal composite member. Therefore, the embodiment of the present invention relates to a resin portion comprising a molded article containing the polybutylene terephthalate resin composition of the above embodiment, and a metal composite member of the metal member.

In the metal composite member of the present embodiment, the bonding strength between the resin portion and the metal member is preferably 25 MPa or more, more preferably 30 MPa or more, and still more preferably 32 MPa or more.

In the present specification, the bonding strength between the resin portion and the metal member can be measured as follows. Examples of the measurement conditions will be described in detail in the examples.

(1) First make a metal composite having the shape specified in ISO 19095 a test piece, (2) as specified in ISO 19095, pressurized to peel the resin part in a state in which the metal member is fixed, and (3) measure the load at the time point when the resin part is peeled off by the metal member (N) And calculate the joint strength (MPa).

The material of the metal member constituting the metal composite member in the present embodiment is not particularly limited, and examples thereof include metals such as aluminum, copper, iron, magnesium, nickel, and titanium; and alloys such as aluminum alloy, phosphor bronze, and stainless steel; A metal bond or the like. Further, the material constituting the metal member is not limited to a metal, and may be any member as long as the surface thereof contains a metal layer. The member having a metal layer on the surface may, for example, be a member subjected to metal plating such as nickel, chromium or gold.

The shape of the metal member is not particularly limited as long as it can be combined with the polybutylene terephthalate resin composition, and various shapes of members such as a plate shape, a cylindrical shape, and a rod shape can be used. The metal member may have a hub for the purpose of the screw clamp, a rib for reinforcing the purpose, a socket for providing a member such as a gear, and the like, and various components required for the combination of the final product such as an electric appliance/electronic product. The shape of the portion where the metal member is in contact with the resin portion is not particularly limited, and any shape such as a square, a circle, or an ellipse may be selected. Further, the shape of the surface in which the metal member is in contact with the resin portion is not particularly limited, and may be a flat surface or a curved surface. The surface of the metal member in contact with the resin portion may be a single plane or a curved surface, and the inside of the plane or the curved surface of the metal sheet may also include a convex portion and a concave portion. The area of the portion where the metal member is in contact with the resin portion is also not particularly limited.

It is preferable that the metal member is at least partially subjected to roughening treatment (fine unevenness treatment) in a portion in contact with the resin portion.

The method of roughening the fine concavities and convexities on the surface of the metal member is not particularly limited, and the material and shape of the metal, the required characteristics, and the like are appropriately selected from the conventional metal roughening treatment method. In the treatment of forming fine concavities and convexities on the metal surface, physical processing such as chemical etching, aluminum anodizing treatment, liquid calendering, and sand blasting may be performed without electroless plating. Chemical etching is a method of treating a metal surface with a chemical or the like. It is known that various methods have been known depending on the type of metal and the purpose of the treatment, and it can be utilized in various industrial fields. When the chemical etching is performed by the roughening treatment method of the metal member, the chemical etching method is not particularly limited and can be arbitrarily selected by a conventional method. Specific examples of the chemical etching method include the methods described in Japanese Laid-Open Patent Publication No. Hei 10-96088, and the Japanese Patent Publication No. Hei 10-56263.

For example, when the material of the metal member is aluminum or an aluminum alloy, the oxide film is removed by (1) being finely etched with an acidic aqueous solution and/or an alkaline aqueous solution, or (2) after forming an oxide film on the surface of the metal member, and then the oxide film is removed. It is preferred to treat the surface of the metal member with ammonia water, hydrazine, a water-soluble amine compound or the like. Specifically, it can be processed by the method described in JP-A-2006-001216.

Further, the aluminum anodizing treatment of the general surface treatment method for aluminum can be carried out by electrolysis with aluminum as an anode, and a porous layer of several tens of nm to several tens of μm can be formed. Moreover, not only a concave portion can be formed on the surface, but a TRI treatment or the like is also known in the method of forming the convex portion.

Therefore, it is possible to form irregularities of several tens of nm to several tens of μm on the surface of the metal member by chemical, physical, electrical, or the like, or a combination thereof, and to make the metal member and the polyterephthalic acid. The butadiene resin composition has better adhesion.

(Manufacturing method of metal composite member)

The method for producing the metal composite member in the present embodiment is not particularly limited. For example, after the metal member is placed on the mold, the polybutylene terephthalate resin composition is supplied by a molding machine, that is, it can be insert-molded. Manufacturing. The molding machine used for the production of the metal composite member is not particularly limited as long as the metal member and the polybutylene terephthalate resin composition can be formed into a composite molded body, and an injection molding machine can be used and extruded. Various molding machines used for molding conventional metal composite members such as a molding machine and a compression molding machine. Further, it is preferable to use an injection molding machine in the case where the metal member is provided in the easiness of the mold, the simplicity of the device, and the productivity of the metal composite member. In another method, a molded article of a resin composition may be produced by a general molding method such as injection molding, and the metal member may be brought into contact with the resin molded article at a desired joint position, and then the contact may be supplied. The surface heat energy is a method of melting a vicinity of a contact surface of a resin molded article to produce a metal composite member.

The metal composite member in the present embodiment is excellent in adhesion between the metal member and the resin portion. Therefore, the metal composite member of the present embodiment is suitably used for members such as various electric/electronic products. Examples of electrical/electronic products suitable for the metal composite member obtained by the method of the present invention include mobile phones, digital cameras, mobile communication terminals (PDAs), portable electronic game terminals, electronic book displays, and the like. OA machines such as mobile terminals, notebook PCs, desktop PCs, photocopying machines, printers, and fax machines. Since the metal composite member of the present embodiment is excellent in strength, lightness, and design properties such as impact resistance, it is particularly suitable for use in a mobile terminal, a computer, an OA machine, or the like. Further, the metal composite member of the present embodiment, It is also excellent in communication characteristics using low dielectric parameters, and is therefore also suitable for use as a communication machine component.

[Examples]

Hereinafter, the present invention will be specifically described by way of examples, but the invention is not limited to the examples below.

<Manufacture of Polybutylene Terephthalate Resin Composition>

The details of each component are as follows.

PBT: Polybutylene terephthalate resin with an ultimate viscosity of 0.69 (DURANEX (registered trademark) manufactured by WinTech Polymer)

PET: non-modified polyethylene terephthalate resin with an ultimate viscosity of 0.68

Modified PET: 12.5 mol% of isophthalic acid modified polyethylene terephthalate resin with an ultimate viscosity of 0.64

PC: polycarbonate resin with a number average molecular weight of 20,000

EGMA Elastomer-1: Ethylene/methyl acrylate/glycidyl methacrylate copolymer (epoxy group content: 1% by mass, methyl acrylate unit content: 27% by mass, glycidyl methacrylate unit) The content is 3% by mass)

EGMA-based elastomer-2: ethylene/methyl acrylate/glycidyl methacrylate copolymer (epoxy group content: 2% by mass, methyl acrylate unit content: 27% by mass, glycidyl methacrylate unit) The content is 6 mass%)

EGMA Elastomer-3: Ethylene/glycidyl methacrylate copolymer (epoxy group content is 4% by mass, methyl acrylate unit content is 0% by mass, and glycidyl methacrylate unit content is 12% by mass) %)

EGMA Elastomer-4: Ethylene/glycidyl methacrylate copolymer (epoxy group content is 2% by mass, methyl acrylate unit content is 0% by mass, methyl group) The content of glycidyl acrylate is 6% by mass)

Core-shell polymer (without epoxy propyl): alkyl acrylate / alkyl methacrylate copolymer

Ethylene-octene copolymer: ethylene-octene-1 copolymer (Manufactured by Dow Chemical Co., Ltd. ENGAGE 8440)

EEA: Ethylene-ethyl acrylate copolymer (NUC-6570, manufactured by NUC Corporation)

Ethylene-butene copolymer: (NEO-ZEX 20201J, manufactured by Prime Polymer)

Glass fiber 1: Glass fiber with a circular cross section (CSF3PE-941 manufactured by Nitto Bose Co., Ltd., cross-sectional shape: circular (cross-sectional specific ratio 1), cross-sectional diameter 13 μm, length 3.8 mm)

Glass fiber 2: Glass fiber with non-circular cross section (CSH3PA-860 manufactured by Nitto Bose Co., Ltd., cross-sectional shape: 茧 shape (cross-sectional specific ratio 2), cross-section long diameter 20 μm, short-diameter section 10 μm, length 3.0 mm)

Glass fiber 3: Glass fiber with non-circular cross section (CSG3PA-830 manufactured by Nitto Denko Co., Ltd., cross-sectional shape: oblong (section-shaped ratio 4), long-diameter section 28 μm, short-diameter section 7 μm, length 3.0 mm)

The components shown in Table 1 were dry-mixed in the proportions (mass parts) shown in Tables 1 to 4, and then biaxial extruder (TEX-30α manufactured by Nippon Steel Works Co., Ltd.) at a cylinder temperature of 260 ° C. The pellets of the polybutylene terephthalate resin composition were melt-mixed under the conditions of a feed amount of 15 kg/hr and a shaft rotation speed of 130 rpm.

<rating>

The obtained granules were further evaluated as follows. The results are shown in Tables 1 to 5.

(1) Surface roughness (Ra)

The obtained resin composition pellets were molded into test sheets in accordance with ISO 3167 (Type A test sheet) at a molding temperature of 260 ° C, a mold temperature of 80 ° C, and a holding pressure of 80 MPa. The shape of the test sheet is as shown in Fig. 2. Then, using a surface roughness measuring machine (Surfto Extreme SV-3000 manufactured by Mitsutoyo Co., Ltd.), under the general environmental conditions (usually about 23 ° C), any of the straight lines connecting the point A and the point A' in FIG. 2 can be measured. The arithmetic surface roughness (Ra) of 5 points (measured length of each point: 0.8 mm), and the average value thereof was calculated.

(2) Shrinkage rate (%)

The obtained resin composition pellets were molded into test sheets in accordance with ISO 3167 (Type A test sheet) at a molding temperature of 260 ° C, a mold temperature of 80 ° C, and a holding pressure of 80 MPa. The shape of the test sheet is as shown in Fig. 2. Then, using a digital caliper (CD-45C manufactured by Mitsutoyo Co., Ltd.), the length (mm) of I ₃ in Fig. 2 is measured under normal environmental conditions (usually about 23 ° C), and the size of the mold in which the cylinder is located ( After 180 mm), the shrinkage ratio was calculated according to the following formula.

(Formula) Shrinkage (%) = {1-(I ₃ /180)} × 100 (%)

(3) Sabie impact strength

The obtained resin composition pellets were injection-molded at a molding temperature of 260 ° C and a mold temperature of 80 ° C to prepare a Rabbi impact test sheet, which was then evaluated at 23 ° C according to the evaluation standard specified in ISO 179/1eA. the amount.

(4) Joint strength

(4-1) Production of test sheets

Hereinafter, the method for measuring the adhesion of the resin composition to the metal is to measure the joint strength between the resin portion and the metal member in accordance with ISO 19095. Injection molding machine (manufactured by Sodick Co., Ltd., TR-40VR), the mold temperature was set to 140 ° C, and after the metal member was placed in the mold, the test piece for adhesion evaluation was injection-molded under the following conditions. Further, as the metal member, a surface roughened aluminum (A5052) plate which is generally known as a chemical etching type "NMT treatment by Dacheng Plus" is used.

Injection molding conditions

Barrel (resin) temperature: 260 ° C

Injection speed: 100mm / sec

Holding pressure: 98MPa

(4-2) Assessment

First, the maximum load (N) when the resin portion was peeled off from the aluminum plate was measured in accordance with ISO 19095. The evaluation of the adhesion was carried out under the general environmental conditions (usually about 23 ° C) using Tensilon UTA-50KN manufactured by Orient Tech. In Tables 1 to 4, A to D are as follows.

A: ≧30MPa

B: 25MPa or more and less than 30MPa

C: 20MPa or more and less than 25MPa

D: less than 20MPa

(5) Dielectric loss tangent

The dielectric loss tangent at 2 GHz at 23 ° C was measured by a cavity resonator perturbation method using a Network Analyzer 8757D manufactured by Agilent and a cavity resonator complex dielectric parameter measuring device manufactured by Kanto Electronics Co., Ltd. Further, in the measurement, a test piece having a predetermined shape (a cross section of 1.8 mm × 1.8 mm and a length of 80 mm) was injection-molded at a molding temperature of 260 ° C and a mold temperature of 80 ° C.

As shown in Examples 1 to 8, it is known that: (A) polybutylene terephthalate resin, (B) polyethylene terephthalate resin, and: (c-1) derived from α- The constituent unit of the olefin and (c-2) the molded article of the (C) epoxy group-containing olefin resin derived from the constituent unit of the glycidyl ester of the α,β-unsaturated acid, and having a surface roughness of 0.50 μm or less And the content of the epoxy group derived from the (C) epoxy group-containing olefin-based copolymer is 0.01% by mass or more and 0.35% by mass or less, and the total amount of the polybutylene terephthalate resin composition is used. When the content of the (meth) acrylate structure is 1.5% by mass or less, the bonding strength is 30 MPa or more, and the dielectric loss tangent is 0.010 or less. Therefore, the adhesion between the resin portion and the metal portion and the dielectric loss tangent can be obtained. Excellent metal composite components. Further, it is also known that in such an embodiment, a good sand impact strength can be maintained, so that a resin composition having a good balance between metal adhesion and impact resistance can be obtained.

The entire disclosure of Japanese Patent Application No. 2015-256281 is incorporated herein by reference.

And all documents, patent applications, and technical specifications contained in this specification are to be construed as being For reference in the manual.

Claims (11)

A polybutylene terephthalate resin composition comprising: (A) polybutylene terephthalate resin, (B) polyethylene terephthalate resin, and containing: (c-1 a constituent unit derived from an α-olefin and (c-2) an epoxy group-containing olefin-based copolymer derived from a constituent unit of a glycidyl ester of an α,β-unsaturated acid; The molding conditions of 260 ° C, the mold temperature of 80 ° C, and the holding pressure of 80 MPa, the surface roughness of the molded article according to ISO 3167 Type A is 0.5 μm or less; and the composition is compared with the polybutylene terephthalate resin. (C) The content of the epoxy group in the epoxy group-containing olefin-based copolymer is 0.01% by mass or more and 0.35% by mass or less, and the total composition of the polybutylene terephthalate resin (A) The content of the acrylate structure is 1.5% by mass or less. The polybutylene terephthalate resin composition according to the first aspect of the invention, wherein the dielectric loss tangent at 2 GHz measured by a cavity resonator perturbation method is 0.01 or less. The polybutylene terephthalate resin composition according to claim 1, wherein (D) the glass fiber is further contained. The polybutylene terephthalate resin composition according to the first aspect of the invention, wherein the molded article has a Raby impact strength of 7 kJ/m ² or more as measured according to the method of ISO 179/1eA. The polybutylene terephthalate resin composition according to claim 1, wherein (C) the epoxy group-containing olefin copolymer does not contain a constituent unit derived from (meth) acrylate. . The polybutylene terephthalate resin composition according to the first aspect of the invention, wherein the forming temperature is 260 ° C, the mold temperature is 80 ° C, and the holding pressure is 80 MPa, according to the ISO 3167 Type A test. The shrinkage of the molded article of the sheet was 0.20 or less. The polybutylene terephthalate resin composition according to claim 1, which is used for a metal composite member. A metal composite member comprising a resin portion composed of a polybutylene terephthalate resin composition according to any one of claims 1 to 7 and a metal member. The metal composite member according to claim 8, wherein the metal member contains a fine uneven surface. The metal composite member according to claim 8 or 9, wherein the bonding strength between the resin portion composed of the polybutylene terephthalate resin composition and the metal member is 30 MPa or more. The metal composite member according to claim 8 or 9, wherein the metal composite member is a communication machine member.