JPH05239363A - Production of reinforced crystalline engineering plastic composition - Google Patents

Abstract

PURPOSE:To provide a reinforced crystalline engineering plastic composition excellent in the impact resistance, heat resistance processability, etc. CONSTITUTION:This producing method of a reinforced crystalline engineering plastic composition is characterized by melt-kneading (A) 60-97 pts.wt. of a crystalline engineering plastic with (B) 5-100 pts.wt. of glass fibers and subsequently melt-kneading the produced composition with (C) an ethylene copolymer having epoxy groups or acid anhydride groups.

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION The present invention has a good surface smoothness which can be used as a molded product or a sheet by injection molding or extrusion molding, and has excellent mechanical properties such as impact resistance and rigidity. Further, the present invention relates to a method for producing a reinforced crystalline engineering plastics composition having excellent heat resistance and molding processability.

[0002] Crystalline engineering plastics are used in a wide range of fields such as electric and electronic equipment parts and automobile parts due to their excellent properties. Above all, molding materials obtained by blending these engineering plastics with glass fiber as a reinforcing agent are used. In particular, it is drawing attention in applications where high rigidity and high heat distortion temperature are required. However, molded products obtained from engineering plastics containing glass fibers have significantly improved mechanical properties such as impact resistance and heat resistance, but on the other hand, the appearance of molded products such as surface smoothness deteriorates. However, in applications in which the appearance is particularly important, such as electricity and automobile parts, improvement is required.

[0003]

In order to improve the impact resistance of engineering plastics, it is known to add ethylene copolymers containing epoxy groups or acid anhydride groups.
Polyester resins are described in JP-B-58-47419 and JP-B-59-28223. Special fair 2 for polyphenylene sulfide resin
-382 publication. Polycarbonate resins are described in Japanese Patent Publication No. 61-44897. For polyarylate resin, polyester carbonate resin, and polysulfone resin, JP-A-57 / 57
-123251 gazette. The polyamide resin is described in Japanese Patent Publication No. 55-44108.

It is also known that mechanical properties such as tensile strength, compressive strength and bending rigidity and heat resistance are remarkably improved by further adding glass fibers to the crystalline resin. For example, Japanese Patent Publication No. 64-5068 proposes a composition in which an epoxy group-containing ethylene copolymer and glass fiber having a specific shape are blended with a polyester resin to improve the appearance of a molded article. JP-B-64-6665 discloses a molded article obtained by melt-molding a composition containing a polyester resin, an epoxy compound and glass fiber.
A method of heat treatment at a temperature of 280 ° C. for 20 minutes or more has been proposed. Further, JP-A-59-152953 proposes a composition comprising a polyphenylene sulfide resin, an epoxy group-containing ethylene copolymer and glass fiber. However, according to the results of studies by the present inventors, the above-mentioned conventional technique can provide a relatively improved molded product, but it is still insufficient. In particular, it is necessary to improve the appearance of molded products.

[0005]

In order to improve the appearance of molded articles, which is a drawback of such glass fiber reinforced crystalline engineering plastics, the present invention is to melt-knead a specific ethylene copolymer by a special compounding method. The aim is to solve the above problems without compromising the mechanical properties such as heat resistance and impact resistance. The purpose is to make the appearance of molded products whose main component is engineering plastics. The object is to provide a method for producing a glass-reinforced crystalline engineering plastics composition, which has excellent mechanical properties such as rigidity and impact resistance, and excellent heat resistance and moldability.

[0006]

Means for Solving the Problems From the above viewpoints, the present inventors extensively and densely searched for a method for producing a resin composition effective for modifying engineering plastics, and found that glass fiber and a specific structure By melt-kneading the ethylene copolymer with a special blending method, the appearance of the molded product is good, the mechanical properties such as rigidity and impact resistance are good, the heat resistance is good, and the molding processability is also excellent. The present invention has been accomplished by finding a manufacturing method capable of obtaining such a composition.

That is, the present invention comprises (A) 60 to 97 parts by weight of crystalline engineering plastic, and (B)
A glass fiber is melt-kneaded in an amount of 5 to 100 parts by weight with respect to 100 parts by weight of (A) and the following (C). An ethylene copolymer containing 40 to 3 parts by weight (however, the total amount of (A) and (C) is 100 parts by weight),
The present invention relates to a method for producing a reinforced crystalline engineering plastics composition characterized by being melt-kneaded.

The crystalline engineering plastic (A) in the present invention is, for example, "Encyclop".
edia of polymer science a
ndenering, Volume 6 "
94 of John Wiley & Sons (1986)
~ 131 pages. That is, it is an acetal resin, a polyamide resin such as polyamide 66, polyamide 6, polyamide 12 or the like, a polyester resin such as polybutylene terephthalate or polyethylene terephthalate, a polyphenylene sulfide resin or a polyether ketone resin.

The glass fiber (B) used in the present invention is
SiO ₂ , B ₂ O ₃ , Al ₂ O ₃ , Cao, Na ₂ O,
Obtained from an inorganic glass containing an oxide such as K ₂ O,
Depending on the purpose, non-alkali glass (E glass), alkali-containing glass (C glass, A glass) and the like are used, but E glass, which is generally used for resin strengthening, is preferable because it has a large strengthening effect. A chopped strand having a length of about 3 mm or 6 mm which is usually used for resin filling is used. The glass fiber can be used without any treatment, but in order to have an affinity with engineering plastics, a silane coupling agent such as aminosilane or epoxysilane, a titanium coupling agent, a chromium coupling agent, and A sizing agent such as a plastic sizing agent for the purpose of sizing the fibers or the like, which has been treated according to other purposes, is used.

The epoxy group-containing ethylene copolymer (C) which is a constituent of the composition according to the present invention is a copolymer composed of an unsaturated epoxy compound unit and an ethylene unit. The composition of the epoxy group-containing ethylene copolymer is not particularly limited, but (a) the ethylene unit is 50 to 99% by weight,
A copolymer having (b) an unsaturated epoxy compound unit of 0.1 to 50% by weight, preferably 1 to 20% by weight, and (c) an ethylenically unsaturated ester compound unit of 0 to 50% by weight is desirable. As the unsaturated epoxy compound (b), an unsaturated compound containing an epoxy group is used. Examples thereof include unsaturated glycidyl esters such as glycidyl acrylate and glycidyl methacrylate. Further, as the (C) ethylenically unsaturated compound, α, β-
Unsaturated carboxylic acid alkyl ester, carboxylic acid vinyl ester, olefins such as propylene and butene-1,
Examples thereof include styrenes.

The (C) epoxy group-containing ethylene copolymer of the present invention is produced by high pressure radical copolymerization, graft copolymerization or the like.

Preferred copolymers produced by high-pressure radical copolymerization are copolymers consisting of ethylene units and glycidyl methacrylate units, copolymers consisting of ethylene units, glycidyl methacrylate units and methyl acrylate units, ethylene units and glycidyl methacrylate units. And a copolymer composed of ethyl acrylate units, a copolymer composed of ethylene units, glycidyl methacrylate units, and vinyl acetate units.

Preferred copolymers produced by graft copolymerization include ethylene-propylene copolymers graft-copolymerized with glycidyl methacrylate, ethylene-propylene-diene copolymers graft-copolymerized with glycidyl methacrylate, and glycidyl. Examples thereof include an ethylene-butene-1 copolymer graft-copolymerized with methacrylate.

The (C) acid anhydride group-containing ethylene copolymer, which is a constituent of the composition of the present invention, is a copolymer comprising (a) ethylene units and (d) maleic anhydride units.
The composition of the acid anhydride group-containing ethylene copolymer is not particularly limited, but (a) the ethylene unit is 40 to 99% by weight, (d)
It is desirable that 0.1 to 10% by weight, preferably 0.3 to 10% by weight, and more preferably 0.5 to 5% by weight of a maleic anhydride unit is copolymerized.

Further, the (C) acid anhydride group-containing ethylene copolymer of the present invention includes a ternary or more multi-component copolymer of (a) ethylene and (d) maleic anhydride and an ethylenically unsaturated compound. It can also be used. Examples of the ethylenically unsaturated compound include α, β-unsaturated carboxylic acid alkyl ester, carboxylic acid vinyl ester, olefins such as propylene and butene-1, styrenes and the like.
Preferably (a) the ethylene unit is 40 to 90% by weight,
(D) 0.3 to 10% by weight of maleic anhydride unit,
(E) An acid anhydride group-containing ethylene copolymer having an α, β-unsaturated carboxylic acid alkyl ester unit of 5 to 60% by weight.

The (C) acid anhydride group-containing ethylene copolymer of the present invention is produced by high pressure radical copolymerization, graft copolymerization or the like. Preferred copolymers produced by high-pressure radical copolymerization include copolymers consisting of ethylene units and maleic anhydride units, copolymers consisting of ethylene units and maleic anhydride units and methyl acrylate units, ethylene units and maleic anhydride units. Examples thereof include a copolymer composed of a unit and an ethyl acrylate unit, a copolymer composed of an ethylene unit, a maleic anhydride unit and a butyl acrylate unit, a copolymer composed of an ethylene unit, a maleic anhydride unit and a methyl methacrylate unit.

Preferred copolymers produced by graft copolymerization are ethylene-propylene copolymers graft-copolymerized with maleic anhydride and ethylene-propylene-diene copolymers graft-copolymerized with maleic anhydride. And an ethylene-butene-1 copolymer graft-copolymerized with maleic anhydride.

The melt index (JIS K6760) of the ethylene copolymer (C) containing an epoxy group or an acid anhydride group of the present invention is 0.5 to 100 g / 10.
Minutes. When the melt index exceeds 100 g / 10 minutes, it is not preferable in terms of mechanical properties when formed into a composition, and when it is less than 0.5 g / 10 minutes, compatibility with engineering plastics is lacking.

The ethylene copolymer containing epoxy groups or acid anhydride groups of the present invention can be prepared by various methods. Random copolymerization method in which unsaturated epoxy compound or unsaturated acid anhydride compound is introduced into the main chain of the copolymer, and unsaturated epoxy compound or unsaturated acid anhydride compound is introduced as a side chain of the copolymer Any of the graft copolymerization methods described above can be used. The production method is as follows: in the presence of an unsaturated epoxy compound or unsaturated acid anhydride compound and a radical generator, at 500 to 4000 atm and 100 to 300 ° C. in the presence or absence of a suitable solvent or chain transfer agent. Examples thereof include a method of polymerizing, a method of mixing an ethylene-propylene copolymer with an unsaturated epoxy compound, an unsaturated acid anhydride compound and a radical generator and performing melt graft copolymerization in an extruder.

In the reinforced crystalline engineering plastics composition of the present invention, the component (A) crystalline engineering plastic is contained in an amount of 60 to 97 parts by weight, preferably 70 to 90 parts by weight, and the component (C) epoxy. The ethylene copolymer containing a group or an acid anhydride group is contained in an amount of 40 to 3 parts by weight, preferably 30 to 10 parts by weight. However, the total amount of the constituent component (A) and the constituent component (C) is 100 parts by weight. If the content of the engineering plastics component (A) is less than 60 parts by weight, the rigidity and heat resistance are insufficient, and if it exceeds 97 parts by weight, favorable results cannot be obtained in impact resistance.

The blending amount of the constituent component (B) glass fiber is
5 to 1 per 100 parts by weight of the total amount of (A) and (C)
The amount is 00 parts by weight, preferably 10 to 60 parts by weight. If the amount is less than 5 parts by weight, sufficient mechanical strength cannot be obtained and 1
If it exceeds 100 parts by weight, molding becomes difficult, the appearance becomes poor, and the toughness tends to be insufficient, which is not preferable.

The method for producing the reinforced crystalline engineering plastics composition of the present invention is a method of kneading in a molten state. The method is as follows: (A) a crystalline engineering plastics component and (B) a glass fiber component are melt-kneaded, and (C) an ethylene group containing an epoxy group or an acid anhydride group This is a method of adding a polymer component and melt-kneading. By adopting this special compounding method, a composition was obtained in which the appearance of the molded product was remarkably good, and mechanical properties such as rigidity and impact resistance, heat resistance, and moldability were also good.

For melt kneading, generally used kneading devices such as a single-screw or twin-screw extruder, a Banbury mixer, a roll, and various kneaders can be used. To melt knead by adding the component (C) of the present invention,
For example, the melt-kneaded composition of the component (A) and the component (B) may be once granulated and produced by an extruder, then the component (C) may be added, and the mixture may be melt-kneaded again by the extruder. Preferably, an extruder equipped with a side feed device is used to produce a melt-kneaded composition of component (A) and component (B) in the former stage (feed side), and by a side feed device in the latter stage (discharge side) of the same extruder. It is preferably produced by adding the component (C) in the solid or molten state and melt-kneading. Also,
The melt-kneaded composition of the component (A) and the component (B) is once granulated and produced by an extruder, and then the component (C) is dry-blended by pellet blending and melt-kneaded in a molding machine such as an injection molding machine. However, the method for producing a molded article at once is a method in which one step of melt-kneading is omitted and is an industrially preferable method.

Further, it is preferable to add glass fibers to the molten engineering plastics in order to prevent breakage of the glass fibers during melt-kneading of the components (A) and (B). At that time, it is preferable to use the above-mentioned side feed device. At the time of kneading, it is preferable to uniformly mix each component with a device such as a tumbler or a Henschel mixer, but if necessary, omit the mixing and also use a method of separately supplying a fixed amount to the kneading device. You can

The composition of the present invention contains other components such as a cross-linking agent, a compatibilizer, a compatibilizer, a pigment, a dye, a heat stabilizer, an antioxidant, etc. as long as the moldability and physical properties are not impaired. Additives such as weathering agents, nucleating agents, antistatic agents, flame retardants, plasticizers, and other copolymers may be added. Also, carbon fiber, talc, calcium carbonate,
A reinforcing material such as magnesium hydroxide or a filler can be added and compounded.

The reinforced crystalline engineering plastics composition of the present invention is molded by various molding methods such as injection molding, extrusion molding, blow molding and the like.

[0027]

The present invention will be described below with reference to examples, but the present invention is not limited thereto. In the examples and comparative examples, the following were used as the crystalline engineering plastics (A), the glass fibers (B), and the ethylene copolymer (C) containing an epoxy group or an acid anhydride group. (A) Crystalline engineering plastics Polybutylene terephthalate (abbreviated as PBT) Toughpet (registered trademark) PBT N1000 (manufactured by Mitsubishi Rayon), IV = 1.0 dl / g Polyethylene terephthalate (abbreviated as PET) Polyester resin MA2103 (manufactured by Unitika) , IV
= 0.68 dl / g Polyamide-6 (abbreviated as PA-6) Unitika Nylon 6 resin A1020BRL, η = 2.
1 Polyamide-6,6 (abbreviated as PA-66) UBE nylon 2015B, η = 2.6 (B) Glass fiber (chopped strand) Glass fiber (1) CS-03-MA419, PBT glass fiber (2) CS For -03-MA429, PET Glass fiber (3) For CS-03-MAFT558, PA-6 Glass fiber (4) For CS-03-MA416, PA-66 All of the above are made by Asahi Fiber Glass, strand length It is 3 mm. (C) Ethylene Copolymer Containing Epoxy Group or Acid Anhydride Group Copolymer (1) E / GMA / MA = 65/7/28 wt%, MI = 10
g / 10 minutes Copolymer (2) E / MAH / EA = 67/3/30% by weight, MI = 7 g
/ 10 min Here, E: ethylene, GMA: glycidyl methacrylate, MA: methyl acrylate, EA: ethyl acrylate, MI = melt index (190 ° C., 216
0 g), IV: intrinsic viscosity, η: relative viscosity.

Physical properties in Examples and Comparative Examples are measured as follows.
I went with the method. (1) According to MFR JIS K 6760, PBT and PA-6
230 ° C, 280 ° C for PET and PA-66, both 21
It was carried out at 60 g. (2) Flexural modulus According to JIS K 7203 (thickness 3.2 mm sample)
Was carried out. (3) Tensile properties According to JIS K 7113 (thickness 3.2 mm sample), tensile breaking strength (US)
Was carried out. Tensile elongation at break (UE) According to JIS K 7113 (thickness 3.2 mm sample)
Was carried out. (4) Izod impact strength JIS K 7110 (thickness 3.2 mm sample, measurement
Performed according to temperatures 23 ° C and -30 ° C with V notches)
did. (5) Drop weight impact strength (FWI) JIS K 7211 (-30 ° C, load 5 kg, thickness 3)
mm sample). (6) Heat distortion temperature (HDT) JIS K 7207 (thickness 6.4 mm sample, bending
Stress 4.6kg / cm ²). (7) Surface smoothness It was performed by visual observation.

Example 1 A side feed device and a vented 30 mmφ twin-screw extruder (TEX30 manufactured by Japan Steel Works, L / D = 40) were used with a preset cylinder temperature of 260 ° C. and (A) PBT7.
32 parts by weight of the glass fiber (1) (B) was melt-kneaded by a side feed device installed in the middle of the extruder barrel while 4 parts by weight of the composition was supplied from the main supply port and melted to obtain a composition. After drying this at 120 ° C. for 3 hours, (C)
26 parts by weight of the copolymer (1) was mixed with pellets, and a physical property test of the composition was performed using a 5 ounce injection molding machine (Toshiba IS-100-EN type) at a cylinder setting temperature of 260 ° C and a mold temperature of 70 ° C. Pieces were made. The physical property measurement results are shown in Table 1.

Comparative Example 1 (A) 74 parts by weight of PBT and (C) copolymer (1) 2
Composition was the same as in Example 1 except that 32 parts by weight of the glass fiber (1) (B) was melt-kneaded by a side feed device installed in the middle of the extruder barrel while 6 parts by weight of the glass was melt-kneaded from the main supply port. I got a thing. 120 this
After drying at 0 ° C. for 3 hours, physical property test pieces were obtained using the same injection molding machine and molding conditions as in Example 1. The physical property measurement results are shown in Table 1.

Comparative Example 2 Same as Example 1 except that 74 parts by weight of (A) PBT, 26 parts by weight of (B) glass fiber (1) and (C) copolymer (1) were melt-kneaded from the main supply port. To obtain a composition. The physical property measurement results are shown in Table 1.

Comparative Example 3 While (A) 74 parts by weight of PBT was supplied from the main supply port and melted, (B) 32 parts by weight of glass fiber (1) was melt-kneaded by a side feed device to obtain (C) copolymer. A composition was obtained in the same manner as in Example 1 except that it was not used. The physical property measurement results are shown in Table 1.

Example 2 The same apparatus and set cylinder temperature as in Example 1 were set to 280.
(A) PET 79 parts by weight is supplied from the main supply port and melted under the same kneading conditions except that the temperature is set to (B).
43 parts by weight of glass fiber (2) was melt-kneaded by a side feed device to obtain a composition, which was dried in the same manner as in Example 1 and 21 parts by weight of (C) copolymer (1) were pelletized. After mixing, an injection molding machine was used to obtain a physical property test piece of the composition. The physical property measurement results are shown in Table 1.

Comparative Example 4 79 parts by weight of (A) PET and (C) copolymer (1) 21
While supplying parts by weight from the main supply port and melting,
A composition was obtained in the same manner as in Example 2 except that 43 parts by weight of the glass fiber (2) (B) was melt-kneaded by a side feed device. In the same manner as in Example 2, the dried product was subjected to an injection molding machine to obtain a physical property test piece. Table 1 shows the physical property measurement results.
Shown in.

Example 3 (A) and (B) with a preset cylinder temperature of 260 ° C.
The same procedure as in Example 2 was repeated except that PA-6 and glass fiber (3) were used respectively. The physical property measurement results are shown in Table 2.

Comparative Example 5 (A) and (B) with a preset cylinder temperature of 260 ° C.
The same method as in Comparative Example 4 was carried out, except that PA-6 and glass fiber (3) were used respectively. The physical property measurement results are shown in Table 2.

Example 4 Example 4 except that the set cylinder temperature was 260 ° C. and PA-6, glass fiber (3) and copolymer (2) were used as (A), (B) and (C), respectively. It carried out by the method similar to 2. The physical property measurement results are shown in Table 2.

Comparative Example 6 Comparative Example 6 except that the set cylinder temperature was 260 ° C. and PA-6, glass fiber (3) and copolymer (2) were used as (A), (B) and (C), respectively. It carried out by the method similar to 4. The physical property measurement results are shown in Table 2.

Example 5 The same procedure as in Example 2 was carried out except that PA-66 and glass fiber (4) were used as (A) and (B), respectively. Table 3 shows the results of measuring physical properties.

Comparative Example 7 The procedure of Comparative Example 4 was repeated except that PA-66 and glass fiber (4) were used as (A) and (B), respectively. Table 3 shows the results of measuring physical properties.

Example 6 PA-6 as (A), (B) and (C) respectively
The same procedure as in Example 2 was performed except that 6, the glass fiber (4) and the copolymer (2) were used. Table 3 shows the results of measuring physical properties.

Comparative Example 8 PA-6 as (A), (B) and (C) respectively
The same procedure as in Comparative Example 4 was performed except that 6, the glass fiber (4) and the copolymer (2) were used. Table 3 shows the results of measuring physical properties.

[0043]

EFFECTS OF THE INVENTION The reinforced crystalline engineering plastics composition obtained by the production method of the present invention has a good appearance of a molded article and has a good balance of mechanical properties such as impact resistance and various physical properties such as thermal properties. It is also excellent in flow processability. In particular, there are no known documents such as patents, etc. implemented by the special compounding method as in the present invention. Therefore, the compounding method of the present invention having a remarkable effect is an invention that breaks the common sense of the prior art. Further, the composition provided by the present invention can be easily processed into molded articles, films, sheets, etc. by ordinary molding methods such as injection molding, extrusion molding, etc., to obtain impact resistance, rigidity, heat resistance, etc. The product has an extremely good balance of physical properties, and has excellent appearance uniformity and smoothness.

[0044]

[Table 1]

[0045]

[Table 2]

[0046]

[Table 3]

─────────────────────────────────────────────────── ─── Continuation of the front page (51) Int.Cl. ⁵ Identification code Internal reference number FI Technical indication C08L 67/00 LPA 8933-4J LPB 8933-4J 77/00 LQS 9286-4J 81/02 LRG 7167- 4J // C08L 23:08 67:00 77:00 81:02 (72) Inventor Noboru Yamaguchi No. 1 Izakizaki Coast, Ichihara City, Chiba Prefecture Sumitomo Chemical Co., Ltd. (72) Inventor Kenzo Konari, Chiba City 1-5 Anezaki Kaigan, Hara City Within Sumitomo Chemical Co., Ltd.

Claims (11)

[Claims] 1. A total amount 1 of (A) crystalline engineering plastics 60 to 97 parts by weight, (B) glass fibers, and (A) and the following (C).
5 to 100 parts by weight with respect to 00 parts by weight of the composition obtained by melt-kneading, and (C) 40 to 3 parts by weight of an ethylene copolymer containing an epoxy group or an acid anhydride group (however, (A The total amount of () and (C) is 100 parts by weight), and the mixture is melt-kneaded to produce a reinforced crystalline engineering plastics composition. 2. The method for producing a reinforced crystalline engineering plastics composition according to claim 1, wherein the melt-kneading of the ethylene copolymer (C) is carried out by an injection molding machine. 3. The method for producing a reinforced crystalline engineering plastic composition according to claim 1, wherein the crystalline engineering plastic (A) is a saturated polyester resin. 4. The method for producing a reinforced crystalline engineering plastics composition according to claim 3, wherein the saturated polyester resin is polybutylene terephthalate. 5. The method for producing a reinforced crystalline engineering plastics composition according to claim 3, wherein the saturated polyester resin is polyethylene terephthalate. 6. The method for producing a reinforced crystalline engineering plastic composition according to claim 1, wherein the crystalline engineering plastic (A) is polyphenylene sulfide. 7. The method for producing a reinforced crystalline engineering plastics composition according to claim 1, wherein the crystalline engineering plastics (A) is a polyamide resin. 8. The method for producing a reinforced crystalline engineering plastics composition according to claim 7, wherein the polyamide resin is polyamide 6. 9. The method for producing a reinforced crystalline engineering plastics composition according to claim 7, wherein the polyamide resin is polyamide 66. 10. The ethylene copolymer (C) comprises (a) an ethylene unit of 50 to 99% by weight, (b) an unsaturated carboxylic acid glycidyl ester unit of 0.1 to 50% by weight, and (c).
Ethylenically unsaturated ester compound unit 0 to 50% by weight
The method for producing a reinforced crystalline engineering plastics composition according to claim 1, which is an epoxy group-containing ethylene copolymer comprising 11. The ethylene copolymer (C) comprises (a) an ethylene unit of 40 to 90% by weight, (d) a maleic anhydride unit of 0.3 to 10% by weight, and (e) an α, β-unsaturated compound. The method for producing a reinforced crystalline engineering plastics composition according to claim 1, which is an acid anhydride group-containing ethylene copolymer comprising 5 to 60% by weight of a saturated carboxylic acid alkyl ester unit.