JPH078944B2 - Polyester resin composition for sealing - Google Patents

Description

DETAILED DESCRIPTION OF THE INVENTION (Field of Industrial Application) The present invention relates to a flame-retardant polyester resin composition which gives a molded article having good fluidity and excellent water resistance and heat resistance. More specifically, it can be molded at low injection pressure during injection molding, and the resulting molded product has improved water resistance and high heat distortion temperature, and is useful as a sealing resin for electrical and electronic parts. The present invention relates to a polyester resin composition.

(Prior Art) Currently, electrical and electronic parts such as motor coils, resistors, capacitors, transistors, and ICs are widely sealed with resin for the purpose of protecting them from the environment such as water, heat, and various gases. ing. In sealing and molding, if a high pressure is applied during molding, the electric and electronic parts to be sealed may be deformed or damaged, so it is necessary to mold at a low pressure. Further, after sealing, excellent water resistance, heat resistance and flame retardancy are required to protect electric and electronic parts from the environment such as water and heat.

From this point of view, epoxy resin is now widely used as the encapsulating resin, the transfer molding method is mainly used as the molding method, and the molding pressure (transfer pressure, injection pressure) is 150 kg / cm. ² or less, further 70kg / cm
It is molded at an extremely low pressure of ² or less. However, since the epoxy resin is a thermosetting resin, it is known that there are various problems particularly in the molding process. That is, the storage stability of the resin is poor, and the curing reaction proceeds at high temperatures, so it is necessary to store the resin at a low temperature of 20 ° C or lower, for example. In order to obtain a molded product with a long molding cycle and stable performance because it is thermosetting, post-curing of the molded product, for example, at 170 to 180 ° C
Heat treatment for 10 hours is required. Since burrs are generated during molding, it is necessary to remove burrs after molding. Since continuous molding with an epoxy resin contaminates the mold surface, it is necessary to clean the mold regularly. Usually, after several hundred shots are continuously molded, a melamine resin is molded and cleaned. Since it is a thermosetting resin, it is impossible to reuse the sprue and runner parts other than the molded product body. Since it is a thermosetting resin, it is difficult to automate processes such as loading parts into a mold, sealing molding, and taking out molded products. There are various problems such as. Since the length of the molding cycle is directly reflected in the price of the molded product, various studies have been made. As an example, as a method of covering the length of the molding cycle of thermosetting resin, a large number of molds are taken, for example, several The method of increasing the number of molded products per unit molding number by increasing the number to 100 is adopted, but this not only complicates loading and unloading of the parts into the mold, but also increases the size of the mold. There is a problem in work due to the increase in weight, and it is strongly desired to solve it.

(Problems to be Improved by the Invention) The present inventors investigated the possibility of converting a thermosetting resin of a sealing resin into a thermoplastic resin in order to solve the problems of the epoxy resin. Thermoplastic resin has excellent storage stability before molding, and it is possible to obtain a molded product that does not generate burrs in a short molding cycle by injection molding and does not require post cure. Almost no mold cleaning is required, and the molding process can be automated. It has many advantages such as easier than thermosetting resin and reusable sprue and runner. As the thermoplastic resin, the present inventors have
We selected polyethylene terephthalate resin (hereinafter abbreviated as PET resin), which has excellent mechanical and thermal properties and is relatively inexpensive, and studied to give it performance as a sealing resin.

Since PET resin is excellent in mechanical properties, electrical properties, heat resistance, chemical resistance, etc., it is not only used in many industrial products as fibers and films. The compounded so-called reinforced PET resin has attracted attention as a resin for injection molding and has established itself as an engineering plastic. Generally, reinforced PET resin has excellent mechanical properties and excellent heat resistance such as high heat distortion temperature, but in injection molding, the injection pressure is usually 300-100.
Since it requires a high pressure of 0 kg / cm ^2, it cannot be used as a sealing resin for electrical and electronic parts that is easily damaged. Further, even if it is molded, there is a problem that it cannot be put into practical use because the molded product obtained has extremely poor water resistance. In addition, it is often required to make the resin flame-retardant when encapsulating electric and electronic parts, and there is a strong demand for a flame-retardant resin having excellent heat resistance.

(Means for Solving Problems) Therefore, the inventors of the present invention have excellent low-pressure injection moldability without impairing the excellent mechanical properties, thermal properties, and electrical properties of the PET resin, that is, excellent in a mold. Imparts liquidity, and
As a result of diligent research to obtain a polyethylene terephthalate-based resin composition which is improved in water resistance, which is a drawback of PET resin, and which is also excellent in heat resistance and stability and useful as a sealing resin, polyethylene terephthalate or at least 80 mol % Of ethylene terephthalate repeating unit in a specified amount of crystal nucleating agent, carboxyl group end capping agent, ester plasticizer, flame retardant and flame retardant auxiliary agent, and if necessary, fibrous reinforcement or inorganic The inventors have found that the above objects can be achieved by compounding the compound, and have reached the present invention.

That is, the present invention is based on 100 parts by weight of polyethylene terephthalate or a copolymerized polyester having at least 80 mol% or more of ethylene terephthalate repeating units, (a) an inorganic crystal nucleating agent having an average particle size of 50 μm or less, and a metal salt of a carboxyl group. 0.05 to 10 parts by weight of at least one of an organic compound having a carboxyl group and a polymer compound having a metal salt of a carboxyl group, 0.3 to 10 parts by weight of a (b) ester plasticizer, and (c) a reaction with a terminal carboxyl group of a polyester 1 to 2 functional groups (hereinafter referred to as terminal blocking agent)
Of at least one of the compounds having an amount of the functional group of the terminal blocking agent / the concentration of the terminal carboxyl group of the polyester = 0.5 to 5 times, (d) a halogenated bisphenol epoxy system represented by the following general formula (I) 5 to 30 parts by weight of compound, X: Bromine or chlorine atom Y: Group selected from hydrogen, glycidyl group, alkyl group, phenyl group, benzyl group and its derivatives R: Direct bond, alkylene group, carbonyl group, ether group, thioether group, sulfone group Group n: Epoxy equivalent necessary integer of 2,500 or more p: Integer of 1 to 4 (e) Composition containing 1 to 15 parts by weight of organic or inorganic antimony compound, and fibrous reinforcing material or inorganic compound The present invention relates to a polyester resin composition for encapsulation which is blended in an amount of 0 to 70% by weight based on the total composition.

(Function) The present invention increases the crystallization rate of PET by shortening the molding cycle by blending the components (a) and (b) into polyester composed of PET or copolymerized PET, and as a component (b) By using a specific ester plasticizer, the fluidity of the PET resin in the mold was improved, enabling molding even under low injection pressure. Then, by improving the water resistance of the PET resin by adding the end capping agent of the component (c), the specific flame retardant of the component (d) and the component (e)
By blending the flame retardant auxiliary agent, even when the molded product is heated at high temperature, it imparts excellent flame resistance with heat resistance without bleeding out of the flame retardant to the surface of the molded product. Further, the present invention provides a composition useful as a molding material for encapsulation, which has improved heat resistance, dimensional stability, and thermal conductivity by adding a fibrous reinforcing material or an inorganic compound, if necessary.

The polyethylene terephthalate used in the present invention is one obtained by a usual melt polymerization method from terephthalic acid or an ester of terephthalic acid and ethylene glycol, or one obtained by subjecting it to a solid phase polymerization treatment. And a polyester having at least 80 mol% or more ethylene terephthalate repeating units means 80 mol% or more ethylene terephthalate repeating units and other repeating units,
In other words, it means a copolymer composed of other copolymer components,
Various acid components and glycol components can be used as the above-mentioned other copolymerization component.

Examples of acid components include isophthalic acid, naphthalene dicarboxylic acid, diphenyl ether dicarboxylic acid, diphenylmethane dicarboxylic acid, diphenyl sulfone dicarboxylic acid, p- (2-hydroxyethoxy) benzoic acid, 5-sodium sulfoisophthalic acid, adipic acid, azelaic acid, sebacine. Acid, dodecane-1,12-dicarboxylic acid, tetradecane-1,14-dicarboxylic acid, hexadecane-1,16-dicarboxylic acid, octadecane-1,18-dicarboxylic acid, 6-ethyl-
Hexadecane-1,16-dicarboxylic acid and the like can be mentioned. Examples of the glycol component include propylene glycol, diethylene glycol, butylene glycol, pentyl glycol, neopentyl glycol, hexamethylene glycol, polyethylene glycol, polytetramethylene glycol, and other polyalkylene glycols.

And to give high fluidity, octadecane-1,
It is preferable to use a higher dibasic acid such as 18-dicarboxylic acid or PET in which polyethylene glycol, polytetomethylene glycol or the like is copolymerized, in all or part of the polyester component. Regarding the molecular weight of PET or copolymerized PET, the intrinsic viscosity (phenol / tetrachloroethane = 6 /
It is desirable to use a polyester having a low intrinsic viscosity within a range that maintains the mechanical strength of the composition at 0.8 or less, preferably 0.7 or less at a concentration of 0.5% and a temperature of 20 ° C.).

The inorganic compound used as the component (a) of the present invention has different effects as a crystal nucleating agent depending on its particle size, and its effect decreases when the average particle size exceeds about 50μ. Inorganic compounds are useful.

Specific examples of the inorganic compound having an average particle size of 50 μm or less used in the present invention include carbon black, silica, calcium carbonate, synthetic silicic acid and silicate, zinc white, halosite clay, kaolin, basic carbonic acid. Magnesium, mica, talc, quartz powder, diatomaceous earth, dolomite powder, titanium oxide, zinc oxide, antimony oxide,
Examples thereof include barium sulfate, calcium sulfate, alumina, calcium silicate and the like, and one or more of these inorganic compounds can be used. Among them, mica, kaolin, talc and silica are useful in the present invention. is there.

As the organic compound having a metal salt of a carboxyl group used in the present invention, any compound having a metal salt of a carboxyl group can be used, but it is usually 7 to 30 carbon atoms. Higher fatty acids and metal salts of aromatic acids are used, such as heptanoic acid, pelargonic acid, lauric acid, myristic acid, palmitic acid,
Stearic acid, behenic acid, cerotic acid, montanic acid,
Specific examples include metal salts of higher fatty acids such as melissic acid, and metal salts of aromatic acids such as benzoic acid, terephthalic acid, terephthalic acid monomethyl ester, isophthalic acid and isophthalic acid monomethyl ester.

The polymer compound having a metal salt of a carboxyl group is not particularly limited as long as it is a polymer having a metal salt of a carboxyl group at the terminal or side chain of the polymer. For example, a carboxyl compound obtained by oxidation of polyethylene is used. Group-containing polyethylene, polypropylene obtained by oxidation of polypropylene, copolymers of olefins such as ethylene, propylene and butene-1 with (meth) acrylic acid, copolymers of olefins with maleic anhydride, styrene Specific examples thereof include metal salts such as copolymers of (meth) acrylic acid and copolymers of styrene and maleic anhydride. Usually, olefins and (meth) acrylic acid or styrene and (meth)
A metal salt of a copolymer of acrylic acid is used. As a metal forming a salt with a carboxyl group, an alkaline earth metal, an alkali metal or the like is usually used, but an alkali metal is excellent in the effect as a crystal nucleating agent, and sodium and potassium are particularly useful.

As the ester plasticizer used as the component (b) of the present invention, various compounds can be used,
Among them, ester compounds represented by the following general formulas (II), (III) and (IV) are useful as crystallization accelerators and fluidity improvers for PET.

R ₁ : alkylene group R ₂ , R ₃ : a group selected from an alkyl group, a benzyl group, and an aromatic-substituted benzyl group, and R ₂ and R ₃ are the same or different groups.

m, n: integer greater than or equal to 1 X: direct bond, alkylene group, -SO _2- , -S-, -O- or R ₄ , R ₅ : a group selected from an alkyl group, a benzyl group, a phenyl group or a derivative thereof, and R ₄ and R ₅ are the same or different groups.

R ₆ and R _{7 are} hydrogen, an alkyl group, or halogen, and R ₆ and R ₇ are the same or different groups.

m, n: integer greater than or equal to 1 R ₈ and R _{9 are} hydrogen, an alkyl group, a phenyl group, a benzyl group or a group selected from these derivatives, and R ₈ and R ₉ are the same or different groups.

R ₁₀ : a group selected from a phenyl group, a benzyl group or a derivative thereof.

R ₁₁ is a group consisting of hydrogen, an alkyl group or a group defined by R ₁₀ .

n: An integer of 4 or more.

Examples of the carboxyl group end-blocking agent used in the present invention include compounds having an epoxy group and an isocyanate group, oxazolines, oxazolones, carbodiimides, carbonate compounds and diazo compounds. Specific examples of epoxy compounds include N-glycidyl phthalimide, N-glycidyl tetrahydrophthalimide,
Monofunctional epoxy such as phenylglycidyl ether, p-tert-butylphenylglycidyl ether, dibromophenylglycidyl ether, neohexene oxide, 1-decene oxide, 1-tetradecene oxide, 1-hexadecene oxide, 1-octadecene oxide Examples of the difunctional epoxy compound include ethylene glycol diglycidyl ether, polyethylene glycol diglycidyl ether, propylene glycol diglycidyl ether, polypropylene glycol diglycidyl ether, neopentyl glycol diglycidyl ether, and 1,4-butane. Diol diglycidyl ether, 1,6
-Glycidyl ether compounds such as hexanediol diglycidyl ether, dibromoneopentyl glycol diglycidyl ether, and bisphenol A diglycidyl ether, as well as adipic acid, azelaic acid, sebacic acid, dodecane-1,12-dicarboxylic acid, tetradecane- Diglycidyl ester compounds such as 1,14-dicarboxylic acid, octadecane-1,18-dicarboxylic acid, 6-ethylhexadecane-1,16-dicarboxylic acid, phthalic acid, diphenyletherdicarboxylic acid and others N, N ' -Diglycidylpyromellitic imide, N, N'-diglycidylaniline, N,
Specific examples include N'-diglycidyl barbital. Examples of the compound having an isocyanate group include toluene diisocyanate and diphenylmethane diisocyanate, and examples of the oxazoline compound include bisoxazoline, p- and m-phenylene oxazoline, other ethylene carbonate, diphenylcarbodiimide and di (2,6-isopropyl). Various carbodiimide compounds such as phenyl) carbodiimide can be enumerated. Then, various catalysts may be added in order to accelerate the reaction between these compounds and the end-capping agent.

Among these end-capping agents, polypropylene glycol diglycidyl ether, particularly those having a propylene glycol repeating unit of about 1 to 10 can be used to obtain a composition having improved water resistance and heat resistance without impairing fluidity. Furthermore, octadecane-1,18-dicarboxylic acid diglycidyl ether is also a useful end-capping agent.

The flame retardant used as the component (d) of the present invention is a halogenated bisphenol type epoxy oligomer type or polymer type flame retardant represented by the general formula (I), which has a melting point or a softening point and melts during molding. It has a characteristic that it is well compatible with resins and does not easily bleed out even at high temperatures, for example above 80 ° C. X in the general formula (I) is a group consisting of bromine or chlorine, but bromine is preferable to chlorine from the viewpoint of imparting flame retardancy.

In the general formula (I), when the epoxy equivalent is less than about 2,500, that is, when the amount of epoxy groups in the molecule is large, gel or the like is generated during the production of the resin composition of the present invention, and the fluidity during molding is The epoxy equivalent is preferably about 2,500 or more, and if the epoxy equivalent becomes too large, n will become too large and the compatibility with PET resin will decrease. Epoxy equivalent of 2,500-40,000 is preferable,
It is desirable to have an epoxy equivalent weight of 3,500 to 30,000.

The component (e) used as a flame retardant aid in the present invention
Is an organic or inorganic antimony-containing compound, and examples thereof include antimony trioxide, sodium antimonate, antimony phosphate, and triphenylantimony, with antimony trioxide being particularly preferable.

As the fibrous reinforcing material used in the present invention, for example, glass fiber, carbon fiber, aromatic polyamide fiber, silicon carbide fiber, titanic acid fiber and the like can be mentioned as specific examples, but usually glass fiber is often used. It The diameter and length of various fibers are not particularly limited, but if the fibers are too long, they can be uniformly mixed and dispersed with polyester and other compounding agents, that is, (a) component or (b) component. If the fiber length is too short, on the other hand, the effect as a reinforcing material will be insufficient.
A fiber having a fiber length of up to 10 mm is used. Especially when the fibrous reinforcing material is glass fiber, the fiber length is preferably 0.1 to 7 mm, more preferably 0.3 to 4 mm. The fibrous reinforcing material may be treated with various compounds as necessary for the purpose of improving the interfacial adhesion with polyester and enhancing the reinforcing effect. When used, various surface treatment agents such as vinyltriethoxysilane, γ-methacryloxypropylmethoxysilane, β- (3,4-epoxycyclohexyl) -ethyltrimethoxysilane, γ-glycidoxypropyltrimethoxysilane. Silane, γ-aminopropyltriethoxysilane, γ-chloropropylmethoxysilane,
Those treated with a silane-based treatment agent such as γ-mercaptopropyltrimethoxysilane or a chromium-based treatment agent such as methacrylate chromic chloride are used.

In addition, in the present invention, an inorganic compound is blended as necessary for the purpose of improving the thermal conductivity, reducing the thermal expansion coefficient, preventing the sink of the molded article, and the like. Other than the specific examples of the inorganic crystal nucleating agent, silicon carbide, silicon nitride, beryllium oxide, boron nitride, magnesium oxide and the like can be mentioned.

Regarding the blending amount of each component in the polyester resin composition of the present invention, the component (a), that is, an inorganic compound having an average particle size of 50 μm or less, an organic compound having a metal salt of a carboxyl group, and a high metal salt having a metal salt of a carboxyl group are used. If the compounding amount of at least one of the molecular compounds is less than 0.05 parts by weight per 100 parts by weight of the polyester component, the effect as a crystal nucleating agent is insufficient. The effect as a nucleating agent is not proportional to the compounding amount, and an excessively compounded compound only acts as a filler.

Therefore, the blending amount of component (a) is 100 polyester components.
0.05 to 10 parts by weight, preferably 0.1
-5 parts by weight, more preferably 0.1-3 parts by weight.
Further, regarding the blending amount of the component (b), that is, the ester plasticizer, the blending amount of the component (b) is 100% of the polyester component.
If the amount is less than 0.3 part by weight, the effect as a crystallization accelerator and the effect of improving fluidity are insufficient, and a molded product having excellent surface properties cannot be obtained. Since other performances such as thermal properties are reduced,
The blending amount of the component (b) is 0.3 to 10 parts by weight, preferably 2 to 10 parts by weight, and more preferably 3 to 7 parts by weight with respect to 100 parts by weight of the polyester component. Furthermore, regarding the amount of the component (c), that is, the terminal carboxyl group blocking agent of the polyester, it depends on the type of the terminal blocking agent used, but the ratio of the functional group concentration of the terminal blocking agent / the terminal carboxyl group concentration of the polyester is less than 0.5. If it is too small, the effect of blocking the terminal carboxyl groups is insufficient, and the water resistance of polyester is not improved. On the other hand, if it is greater than 5, the water resistance is improved, but the operation stability in the kneading step and molding step of the composition is improved. It is not desirable because it may decrease or other deterioration in performance may be observed.

Therefore, the above ratio is preferably in the range of 0.5 to 5, and more preferably in the range of 1 to 3. When the amount of the component (d), that is, the flame retardant represented by the general formula (I) is less than 5 parts by weight, the effect of imparting flame retardancy is insufficient.
Since the mechanical properties and the fluidity will be significantly deteriorated when the amount is more than the weight part, the compounding amount of the component (d) is 5 to 30 parts by weight, preferably 10 to 25 parts by weight with respect to 100 parts by weight of the PET resin. The amount of the antimony-containing compound as the component (e) blended as the flame retardant aid is 1 to 15 parts by weight, preferably 2 to 10 parts by weight.

Further, in the present invention, the amount of the fibrous reinforcing material or the inorganic compound to be blended, if necessary, varies depending on the required performance of the end use. Is not preferable because it is difficult to uniformly mix and disperse it in the composition, and the fluidity of the composition is also reduced. Usually, it is desirable to control the content to 70% by weight or less.

The composition of the present invention further comprises an antioxidant, if necessary.
Various inorganic or organic compounds such as an ultraviolet absorber, a colorant, a release agent and a filler can be blended. The polyester composition of the present invention can be produced by mixing it by various methods, and the production method is not particularly limited, but it is usually an extruder in which each component or additive is added to polyester pellets. It is manufactured by a method of mixing using a kneader.

(Example) Next, the present invention will be specifically described with reference to Examples and Comparative Examples. The "parts" shown in Examples and Comparative Examples are "parts by weight".
Indicates.

Examples 1 to 6, Comparative Examples 1 to 4 Polyethylene terephthalate (abbreviated as PET) and copolymerized polyethylene terephthalate (abbreviated as copolymerized PET) shown in Table 1 were produced according to a conventional method. However, the intrinsic viscosity is the value measured in a phenol / tetrachloroethane = 6/4 solvent, concentration 0.5%, temperature 20 ° C.
Also, the terminal carboxyl group concentration of polyester [-COOH]
Is a value measured by an ordinary method.

Next, various crystal nucleating agents, ester plasticizers, end-capping agents, flame retardants, antimony oxide, glass fibers (3 mm long chopped strands, product number NO.429 made by Asahi Fiber Glass Co., Ltd.) and inorganic materials are used for PET or copolymer PET. Compounds are mixed and kneaded with a twin-screw extruder to produce the various pellets shown in Table 2, dried, and then the temperature of the cylinder is 250-260-270 ℃ and the mold temperature is 100 using a mold for spiral flow measurement. The fluidity was compared by measuring the spiral flow length (cm) of the resin under constant conditions of ℃, injection pressure of 150 kg / cm ² and cooling time of 15 seconds. Similarly, cylinder temperature 250-260-270 ℃, mold temperature 100 ℃, injection pressure 400-600kg / cm ² , injection holding time 10 seconds, cooling time 20
1/4 inch × 1/2 inch × 5 inch tanzaque test piece is molded in seconds, bending strength, heat distortion temperature HDT (load 18.56 kg / c
m ² ) was measured. Also, under the same conditions, 1/16 inch × 1/2 inch × 5 inch test pieces were molded, flame retardancy was evaluated according to the UL94 measurement method, and the test pieces were heat treated at 120 ° C for 24 hours. The presence or absence of bleed-out of the flame retardant was investigated. Furthermore, a 1/8 inch thick × 1/4 inch diameter disk was molded under the same molding conditions and the volume resistivity was measured. Or changes in flexural strength and volume resistivity after immersing a test piece in 80 ° C warm water to evaluate water resistance, after pressure cooker test (PCT, left in 121 ° C-2 atmosphere steam) 24 hours later The bending strength and the volume resistivity of the above were measured. The results are summarized in Table 3.

From this, the following was found. When PET is blended with a specific ester plasticizer, the fluidity is improved. Improves fluidity when blended with copolymerized PET. When a specific end-capping agent is added, the strength retention after the water resistance test will increase. Improve the heat distortion temperature by adding an ester plasticizer. That is, the heat distortion temperature of PET depends on the crystallinity of PET, but the normal PET temperature of 100 ℃
If a specific ester plasticizer was added even under conditions where crystallization was difficult, the crystallization rate under a low temperature mold increased, and as a result, crystallization proceeded even at a mold temperature of 100 ° C and the heat distortion temperature improved. Is. When the flame retardant represented by the general formula (I) is used as the flame retardant, the fluidity is not deteriorated, excellent flame retardancy is imparted, and the flame retardant does not bleed out even when the molded product is heat-treated. As can be seen, the composition of the present invention has excellent performance.

Example 7, Comparative Example 5 The pellets shown in Example 2 and Comparative Example 2 were mixed at 130 ° C. for 5 hours.
After drying with hot air for a period of time, set the mold for condenser molding in the low pressure injection molding machine JT03-25V (made by Japan Steel Works), cylinder temperature 250-260-270 ℃, mold temperature 100 ℃, injection time 20
Molding test was performed with a cooling time of 30 seconds. In the pellet of Example 2, the primary injection pressure (before the gate portion) 180 kg / cm ² ,
The resin was filled in the mold at the secondary injection pressure (after the gate part) of 70 kg / cm ² , but in the pellet of Comparative Example 2, the primary injection pressure was
The filling was insufficient even at 200 kg / cm ² and the secondary injection pressure of 110 kg / cm ² .

(Effect of the invention) Since the composition of the present invention has excellent fluidity as compared with a normal polyester resin composition, low-pressure injection molding is possible,
Moreover, since it has improved water resistance, flame retardancy and heat resistance, it is useful as a resin for sealing electric and electronic parts that are easily deformed or damaged.

─────────────────────────────────────────────────── ─── Continuation of the front page (51) Int.Cl. ⁶ Identification code Internal reference number FI Technical display area C08L 67/02 LNZ // (C08L 67/02 63:02)

Claims (9)

[Claims] 1. Polyethylene terephthalate or 100 parts by weight of a copolyester having at least 80 mol% or more of ethylene terephthalate repeating units,
(A) At least one of an inorganic crystal nucleating agent having an average particle size of 50 μm or less, an organic compound having a metal salt of a carboxyl group, and a polymer compound having a metal salt of a carboxyl group is used.
05 to 10 parts by weight, (b) ester plasticizer 0.3 to 10 parts by weight, and (c) a compound having one or two functional groups that react with the terminal carboxyl groups of the polyester (hereinafter referred to as the terminal blocking agent) Of at least one of the functional groups of the end capping agent / the terminal carboxyl group concentration of the polyester = 0.
5 to 5 times amount, (d) 5 to 30 parts by weight of halogenated bisphenol type epoxy compound represented by the following general formula (I) X: Bromine or chlorine atom Y: Group selected from hydrogen, glycidyl group, alkyl group, phenyl group, benzyl group and its derivatives R: Direct bond, alkylene group, carbonyl group, ether group, thioether group, sulfone group Group n: Epoxy equivalent integer required to be 2,500 or more p: Integer of 1 to 4 (e) Organic or inorganic antimony-containing compound 1 to 15
A polyester resin composition for encapsulation, which comprises a composition containing 1 part by weight of a fibrous reinforcing material or an inorganic compound in an amount of 0 to 70% by weight based on the total composition. 2. The polyester resin according to claim 1, wherein one or more inorganic substances selected from the group consisting of talc, mica, kaolin and silica are used as the inorganic compound having an average particle size of 50 μm or less. Composition. 3. The polyester resin composition according to claim 1, wherein the compound having a metal salt of a carboxyl group is a sodium salt or potassium salt of an organic compound or a polymer compound. 4. The polyester resin composition according to claim 1, wherein the compound having a metal salt of a carboxyl group is a compound having 7 to 30 carbon atoms. 5. The polyester resin composition according to claim 1, wherein the polymer compound having a carboxyl group is a copolymer of olefin and (meth) acrylic acid or a copolymer of styrene and (meth) acrylic acid. object. 6. An ester plasticizer is represented by the following general formula (II):
The polyester resin composition according to claim 1, which is an ester compound of at least one of (III) and (IV). R ₁ : alkylene group R ₂ , R ₃ : a group selected from an alkyl group, a benzyl group, and an aromatic-substituted benzyl group, and R ₂ and R ₃ are the same or different groups. m, n: integer greater than or equal to 1 X: direct bond, alkylene group, -SO _2- , -S-, -O- or R ₄ , R ₅ : a group selected from an alkyl group, a benzyl group, a phenyl group or a derivative thereof, and R ₄ and R ₅ are the same or different groups. R ₆ and R _{7 are} hydrogen, an alkyl group, or halogen, and R ₆ and R ₇ are the same or different groups. m, n: integer greater than or equal to 1 R ₈ and R _{9 are} hydrogen, an alkyl group, a phenyl group, a benzyl group or a group selected from these derivatives, and R ₈ and R ₉ are the same or different groups. R ₁₀ : a group selected from a phenyl group, a benzyl group or a derivative thereof. R ₁₁ is a group consisting of hydrogen, an alkyl group or a group defined by R ₁₀ . n: An integer of 4 or more. 7. The end capping agent is polyethylene glycol diglycidyl ether, polypropylene diglycidyl ether, octadecane-1,18-diglycidyl ester, 6-ethyl-hexadecane-1,16-dicarboxylic acid diglycidyl ester, di (2, The polyester resin composition according to claim 1, which is an end-capping agent of at least one of 6-isopropylphenyl) carbodiimide. 8. The polyester resin composition according to claim 1, wherein the fibrous reinforcing material is glass fiber. 9. The inorganic compound is talc, mica, silica, kaolin, alumina magnesium oxide, beryllium oxide,
The polyester resin composition according to claim 1, which is at least one inorganic compound of silicon carbide.