GB2210623A

GB2210623A - Resin moulding composition

Info

Publication number: GB2210623A
Application number: GB8821909A
Authority: GB
Inventors: Takashi Nakajima; Kiyotaka Misoo; Seiji Morimoto
Original assignee: Mitsubishi Kasei Corp
Current assignee: Mitsubishi Kasei Corp
Priority date: 1987-10-08
Filing date: 1988-09-19
Publication date: 1989-06-14
Anticipated expiration: 2008-09-19
Also published as: KR890006751A; DE3833286A1; GB8821909D0; GB2210623B

Description

2210623 RESIN COMPOSITION The present invention relates to a resin

composition having good moldability and excellent mechanical properties, chemical resistance and heat resistance, which is useful in a wide range of fields including fields of electrical and electronical parts, automobile parts, household utensils, housings for machines and equipments and mechanical parts produced by injection molding, sheets or films produced by extrusion molding and blow molding products.

Polyamide resins or thermoplastic polyester resins have excellent physical and chemical properties. Nevertheless, when such resins are used alone, they have_ some deficiencies or drawbacks. For example, polyamide resins have a drawback that upon absorption of moisture or water, the deterioration in the rigidity and the dimensional change of molded products are substantial. On the other hand, thermoplastic polyester resins have a 2 drawbac that they are inferior in the impact resistance or in the hydrothermal resistance. In order to obtain a resin having such deficiencies comple'mented, a study has been conducted for blending a thermoplastic polyester resin to a polyamide resin. For example, Japanese Unexamined Patent Publications No. 103191/1976, No. 105355/1976 and No. 213256/1986 disclose such blend compositions.

However, a polyamide resin and a thermoplastic polyester resin have poor compatibility with each other, whereby the mechanical properties, particularly the tensile properties or impact properties, tend to deteriorate, or phase separation is likely to result to deteriorate the outer appearance. Therefore, it is practically difficult to obtain a practically useful blend composition by a commercially peasible method such as a melt kneading.

It is an object of the present invention to provide, by an industrially inexpensive and simple method, a composition having the water-absorbing property reduced while maintaining the excellent properties of a polyamide resin and having provided also with the properties of a thermoplastic polyester resin, which is excellent in the impact resistance and mechanical propetties. 25 The present invention provides a resin composition comprising: (1) 100 parts by weight of resin composition comprising (i) from 5 to 95% by weight of a polyamide resin and (ii) from 5 to 95% by weight of a thermoplastic polyester resin; (A) from 0.01 to 30 parts by weight of a bisphenol type high molecular weight epoxy compound which is a condensation product of a bisphenol with epichlorohydrin and which has a polymeriz.ation degree of substantially at least 11; and/or (B) from 1 to 50 parts by weight of a metal ion-containing ethylene copolymer.

Now. the present invention will be described in detail with reference to the preferred embodiments.

The polyamide to be used in the present invention may be a polyamide obtained by the polymerization of an at least 3-membered lactam or a polymerizable w-amino acid, or a polyamide obtained by the polycondensation of a dibasic acid with a diamine. Specifically, it includes polymers of c-caprolactam, aminocaproic acid, enantholactam, 7-aminoheptanoic acid, 11-aminoundecanoic acid, 9-aminononanoic acid, a-pyrrolidone and a-piperidone, polymers obtained by the polycondensation of a diamine such as hexamethylenediamine, nonamethylenediamine, undecamethylenediamine, dodecamethylenediamine or m-xylylenediamine with a dicarboxylic acid such as terephthalic acid, isophthalic acid adipic acid, sebacic acid, dodecanedioic acid or glutaric acid. and copolymers thereof, such as nylon 4, 6, 4 7r 8, 11, 12, 6.6, 6-9, 6.10, 6.11, 6.12, 6T, 6/6.6, 6/12, 6/6T and 61/6T.

The thermoplastic polyester resin to be used in the present invention may be a polyalkylene terephthalate obtained by the polycondensation reaction of terephthalic acid or its dialkyl ester with an aliphatic glycol, or a copolymer thereof. Typical examples include polyethylene terephthalate and polybutylene terephthalate. As the above-mentioned aliphatic glycol, ethylene glycol.

propylene glycol. tetramethylene glycol or hexamethylene glycol may be mentioned. These aliphatic glycols may contain not more than 30% by weight of other diols or polyhydric alcohols, such as cyclohexane diol, cyclohexane dimethanol, xylylene glycol, 2,2-bis(4-hydroxyphenyl)propane. 2,2bis(4-hydroxy-3,5- dibromophenyl)propane, 2,2-bis(4-hydroxyethoxyphenyl)propane. 2..2-bis(4hydroxyethoxy-3,5-dibromophenyl)propane, glycerol and pentaerythritol.

Further. terephthalic acid or its dialkyl ester may be used in combination with other dibasic acid, a poly basic acid or an alkyl ester thereof, for example, in combination with not more than 30% by weight, relative to terephthalic acid or itS dialkyl ester, of phthalic acid, isophthalic acid, naphthalene dicarboxylic acid, diphenyldicarboxylic acid, adipic acid, sebacic acid, trimesic acid, trimellitic acid, or an alkyl ester thereof.

Here, the blend ratio of the polyamide resin and the thermoplastic polyester resin is from 5 to 95% by weight one of them and from 5 to 95 by weight of the other to make up a total of 100% by weight. outside this range, the characteristics of both polymers can not be maintained. Preferably, the resin composition (I) comprises from 2 to 90% by.weight, more preferably from 40 to 90% by weight, of the polyamide resin and from 10 to 80% by weight, more preferably from 10 to 60% by weight, of the thermoplastic polyester resin.

The bisphenol type high molecular weight epoxy compound in the present invention is a cbndensation of product of a bisphenol such ad bisphenol A with epichloro- hydrin. For example, in the case of bisphenol A, it is a high molecular weight bisphenol type epoxy compound of the formula I wherein the polymerization degree n is substantially at least 11, preferably at least 15.

0 CH 3 OH CH 3 0 CH-C 0 7-'\5 CH CH-CH 1 rl k"I-O-CH -CH-CH 2 2 2 2 2 CH il H 3 3 n Specific examples of the bisphenol include bisphenol A, bisphenol F, bisphenol C, tetramethyl-bisphenol A, tetramethyl-bisphenol F, di-isopropyl-bisphenol A, di-sec-butyl-bisphenol A, tetra-t-butyl-bisphenol A, tetra-t-butyl-bisphenol F, tetra-t-butylbisphenol, 6 1,1-ethylidene-bisphenol, 1,1-isobutylidene-bisphenol, methyl-ethyl-methylene bisphenol, methyl-isobutyl-methylene..bisphenol, methyl-hexyl-methylene- bisphenol, methyl-phenyl-methylene-bisphenol, bisphenol Z, p,pl-bisphenol, methylene- bis(2,4-DTB-3CR), o,pl-bisphenol A, methylpropionate-diphenol, ethylpropionate-diphenol, and tetramethyl-bisphenol S.

The specific bisphenol type high molecular weight epoxy compounds in the present invention may be used in combination of two or more different types.

The epoxy compound is added in an amount of from 0.01 to 30 parts by weight relative to 100 parts by weight of the mixture of the polyamide resin and the thermoplastic polyester resin. If the amount is less than 0.01 part by weight, no adequate effect for compatibility will be obtained. On the other hand, if the amount exceeds 30 parts by weight, the mechanical properties tend to deteriorate. Preferably, the amount is within a range of from 0.05 to 20 parts by weight.

The metal ion-containing ethylene copolymer in the present invention is an ionic polymer composed of an ethylene component, an unsaturated carboxylic acid component and a component of a metal salt of an unsaturated carboxylic acid, and it is commonly called an ionomer. As the unsaturated carboxylic acid component, the one having from 3 to 8 carbon atoms is preferred.

Particularly, preferred is the one derived from acrylic acid, methacrylic acid or ethacrylic acid. The component of a metal salt of an unsaturated catboxylic acid may be a metal salt of the above-mentioned unsaturated carboxylic acid such as a Na, K, M9, Ca, Ba or Zn salt. Preferably, a Na, Mg or Zn salt may be mentioned. The proportions of the above-mentioned components are preferably from 80 to 99 mol of the ethylene component and from 0.1 to 20 mol% of each of the unsaturated carboxylic acid component and its metal salt component. The component of the metal salt of an unsaturated carboxylic is prefrably at least 10 moA relative to the unsaturated carboxylic acid component. Further, the metal ion-containing ethylene copolymer may contain in addition to the above three components, an unsaturated carboxylic acid alkyl ester component such as methyl acrylate or methyl methacrylate, or a vinyl ester component such as vinyl acetate. For the preparation of the metal ion-containing ethylene compolymer, it is possible to utilize the method disclosed in e.g. Japanese Examined Patent Publication No. 31556/1974 and U.S. Patent 3,789,035. The most preferred is, for example, an ionomer resin (Sirline, tradename) manufactured by Dupont Company.

The metal ion-containing ethylene copolymer is incorporated in an amount of from 1 to 50 parts by weight, preferably from 3 to 30 parts by weight, relative to 100 parts by weight of the mixture of the polyamide resin and the thermoplastic polyester resin. If the amount is less 8 than 1 part by weight, no adequate effect for improving the compatibility of the polyamide resin and the thermoplastic polyester resin will be obtained. On the other hand, if the amount exceeds 50 parts by weight, the deterioration of the heat resistance tends to be substantial.

The blending of the composition of the present invention can be conducted by a melt-kneading method well-known to those skilled in the art. There is no particular restriction as to the temperature or time for kneading. However, a temperature of from 150 to 350 oc is usually recommended. Specifically, an extruder,.Bunbury mixer, a super mixer, a roll mill or a kneader may be mentioned as a means for carrying out the blending.

is It is preferred to simultaneously melt-kneading all the components. In some cases, however, two components out of the three may be melt-kneaded first, and then the remaining component is blended, followed by further melt-kneading. The epoxy compound and the metal ion-containing ethylene copolymer of the present invention may be incorporated alone, or may be used together in. combination. Further, they may contain small amounts of impurities.

In the present invention, other resins may be incorporated so long as the properties of the resin composition of the present invention are not impaired.

In order to further improve the compatibility between the polyamide resin and the saturated polyester resin, a conventional additive such as a modified polyolefin resin or an olefin elastomer may be incorporated.

Especially when an ethylene/acrylic acid ester copolymer, an"elastomer or the like is incorporated in an amount of from 0.1 to 10 parts by weight relative to 100 parts by weight of the mixture of the polyamide resin and the unsaturated polyester resin, the impact properties can further be imProved. Here, as the elastomer, a rubber-like polymer or a rubber-modified styrene resin may be mentioned. Specific examples of the rubber-like polymer include a polybutadiene, a butadiene-styrene copolymer, an ethylene-propylene copolymer, an ethylenepropylene-diene copolymer, polyisoprene, an ethylene-n-olefin copolymer, a polyisobutylene, a polyacrylate, a polyester, a polyurethane and various modified polymers thereof. Specific examples of the rubber-modified styrene resin includes, for example, a butadiene rubber-modified polystyrene, a butadiene rubber-modified styrene-acrylonitrile copolymet, an acryl rubber-modified polystyrene, an acryl rubber-modified styrene acrylonitrile copolymer, an ethylene-propylene copolymer-modified polystyrene and an ethylene methylmethacrylate copolymer-modified polystyrene.

The composition of the present invention may contain various other well-known additives including reinforcing materials such-as glass fibers, carbon fibers and metal whiskers, fillers, such as silica, alumina, silica-alumina clay minerals, silica magnecium clay minerals, calcium silicate, calcium carbonate, asbestos and carbon black, lubricants, nucleating agents, antioxidants, flame retardants, antistatic agents, weather resistance-imparting agents, etc.

Now. the present invention will be described in further detail with reference to Examples. However, it should be understood that the present invention is by no means restricted to such specific Examples. In the following Examples, the physical properties were measured as follows.

(1) Tensile strength, elongation In accordance with ASTM D-638 is (2) Tensile impact value In accordance with ASTM D-1822 (3) Izod impact value In accordance with ASTM D-256 by using a test piece having a thickness of 1/8 inch.

EXAMPLES 1 and 2 Nylon 6 having a relative viscosity of 2.5 as measured by Ostwald's viscometer in accordance with JIS K 6810 as the polyamide, polybutylene terephthalate having an intrinsic viscosity of 1.2 (Novadur 5010, trademark, manufactured by Mitsubishi Kasei Corporation) and a high molecular weight bisphenol-type epoxy compound were blended to have a composition as identified in Table 1, and the,,blend was melt-mixed by an extruder at a tempera. ture of from 250 to 3200C. The obtained composition was injection-molded under the conditions as identified in Table 2.

EXAMPLES 3 to 8 By using a polyethylene terephthalate having an intrinsic biscosity of 0. 6 and a melting point of 2 0 0 C instead of the polybutylene terephthalate used in Examples 1 and 2, a blend composition was prepared in the same manner as in Examples 1 and 2 to have the composition as identified in Table 1, and the composition was injection-molded under the conditions as identified in Table 2. COMPARATIVE EXAMPLES 1 and 2 A blend composition was prepared by melt-mixing in an extruder in the same manner as the compositions of the Examples 1 to 8 except that no high molecular weight bisphenol epoxy compound was added, and the composition was in-ection-molded under the conditions as identified in Table 2. COMPARATIVE EXAMPLES 3 to 6 By using a bisphenol type epoxy compound having a relatively low molecular weight of the formula I wherein n is less than 10, a blend composition was prepared to have the composition as identified in Table 1 and melt-mixed by an extruder in the same manner as in Examples 1 to 8 to obtain a composition, which was injection-molded under the 12 - conditions as identified in Table 2. COMPARATIVE EXAMPLES 7 to 9 By using an epoxy compound otherthan the bisphenol type epoxy compound, a blend composition was prepared to have the composition as identified in Table 1 and melt-mixed by an extruder in the same manner as in Examples 1 to 8 to obtain a composition, which was injection-molded under the conditions as identified in Table 2.

With respect to the injection-molded products of the resin compositions of Examples 1 to 8 and Comparative Examples 1 to 9 thus obtained, the tensile strength, the tensile elongation, the tensile impact value and the Izod impact value were measured. The results are shown in Table 2.

t Table 1

Resin (1) Epoxy compound Nylon 6 Polybutylene Polyethylene Compound used Polymeri- Epoxy Amount terephthalate terephthalate zation equiva- relative (WM (Wt%) (wt%) degree lent to 100 parts by (n) (g/eq) weight of the resin (I) (parts by weiqht) Example 1 80 20 Bisphenol A type 25 3f700 5 epoxy compound Example 2 80 20 - Bisphenol F type is 2,000 5 epoxy compound Example 3 90 - 10 Bisphenol A type 25 3,700 5 epoxy compound Example 4 80 - 20 Bisphenol A type 25 30700 5 epoxy compound Example 5 80 Bisphenol A type 25 30,700 2 epoxy compound Example 6 80 - 20 Bisphenol A type is 20300 5 epoxy compound 8 W 1 1-, Table 1 (continued) Resin (I) Epoxy compound Nylon 6 Polybutylene Polyethylene Compound used' PolymeriEpoxy Amount terephthalate terephthalate zation equiva- relative (WM (wt%) (wt%) degree lent to 100 parts by (n) (g/eq) weight of the resin (I) (parts by weight) Example 7 80 20 Bisphenol F type is 2,000 5 epoxy compound Example 8 60 - 40 Bisphenol A type 30 4,400 8 epoxy compound Comparative 80 20 - - - - Example 1

Comparative 80 - 20 - - - Example 2

Comparative 80 20 - Bisphenol A t5pe 2 450 1 Example 3 epoxy compound Comparative 80 20 Bisphenol A type 2 450 1 Example 4 epoxy compound 1 A 1 A 11 Table 1 (continued Resin (1) Epoxy compound Nylon 6 Polybutylene Polyethylene Compound used Polymeri- Epoxy Amount terephthalate terephthalate zation equiva- relative (wt%) (Wt%) (wt%) degree lent to 100 parts by (n) (g/eq) weight of the resin (I) (parts by weight) Comparative 80 20 Bisphenol A type 8 1,300 0.5 Example 5 epoxy compound Comparative 80 20 Bisphenol A type 5 880 5 Example 6 epoxy compound Comparative 80 20 0-cresol novolak 2 210 5 Example 7 type epoxy compound Comparative 80 20 Phenol novolak 2 180 5 Example 8 type epoxy compound Comparative 80 20 Glycidylamine 120 5 Example 9 type epoxy compound 9 cn a 1 1 J Table 2

Molding conditions Mechanical properties Resin temp. Injection Tensile Elongation Tensile Izod impact 0 pressure strength impact value C) (kg/cm 2 (kg/cm 2 value (kg.cm/cm) (kg.cm/ cm 2 Example 1 270 400 750 15 3 412 10.0 Example 2 270 450 740 141 410 10.2 Example 3 270 350 810 250 430 12.2 Example 4 270 380 805 183 394 11.7 Example 5 270 380 810 172 405 11.5 Example 6 270 350 800 16'8 402 11.5 Example 7 270 400 810 165 390 10.8 Example 8 270 400 810 190 405 11.5 v k 11 Table 2 (continued) Molding conditions Mechanical properties Resin temp. Injection Tensile Elongation Tensile Izod impact 0 pressure strength impact value C) 2 2 value 2 (kg/cm (kg/cm (kg.cin/cm (kg.cm/cm) Comparative 280 480 390 5 12 2.2 -Example 1

Comparative 280 480 380 4 15 1.7 Example 2

Comparative 280 500 470 9 25 5.6 Example 3

Comparative 280 500 450 7 31 4.8 Example 4

Compartive 280 450 510 12 31 5.5 -Example 5

Comparative 280 440 500 11 40 4.5 Example 6

Comparative 280 460 470 8 25 4.8 Example 7

Comaprative 280 450 510 8 38 5.5 -Example -8

Comaprative 280 450 470 7 35 5.4 Example 9 1 -- 18 EXAMPLES 9 to 17 A blend composition was prepared to have the composition as shown in Table 3 by using nylon 6 or nylon 66 having a relative viscosity of 3.0 as measured by Ostwald's viscometer in accordance with JIS K-6810 as the polyamide resin, polybuteneterephthalate (hereinafter referred to simply as PBT) having an intrinsic viscosity of 1.1 or polyethyleneterephthalate (hereinafter referred to simply as PET) having an intrinsic viscosity of 0.8 as the thermoplastic polyester resin and an ionomer resin of Dupont Company (Sirline, trademark) as the metal ion-containing ethylene copolymer, and the blend composition was me lt-mixed by a 40 mm 6 extruder at a resin temperature within a range of from 240 to 280 0 C.

Then, the obtained composition was injection-molded by an injection molding machine with a mold clamping force of 75 tones (IS 75 S, manufactured by Toshiba Kikai K.K.). EXAMPLES 18 to 22 The operation was conducted in the same manner as in Examples 9 to 17 except that a high molecular weight bisphenol type epoxy compound or an ethylene propylene terpolymer rubber (EPDM) was incorporated in addition to the composition of Example 12 to have the composition as identified in Table 3.

COMPARATIVE EXAMPLES 10 to 12 The operation was conducted in the same manner as in Examples 9 to 17 except that the metal ion-containing 19 ethylene copolymer was omitted.

With respect to the injection-molded products of the resin compositions of Examples 9 to 22 and Comparative Examples 10 to 12 thus obtained, the tensile strength, the elongation, the Izod impact value were measured. The results are shown in Table 4.

( 1 Table 3

Polyamide resin Polyester Metal ion-containing Others resin eth lene copolymer Type Amount Type Amount Type Amount relative to Type Amount relative to (wt%) (wt%) 100 parts by weight 100 parts by weight of polyamide/ of polyamide/ polyester polyester (parts by weight) (parts by weight) Example 9 Nylon 6 80 PET 20 Sirline 5 - 1601 Example 10 60 40 00 5 - Example 11 99 60 40 Sirline 5 - 1650 Example 12 91 60 go 40 Sirline 10 1601 Example 13 99 60 go 40 go 20 - Example 14 40 to 60 or 40 - Example 15 80 PBT 20 10 Example 16 g 60 of 40 10 1 tID C 1 Sirline 1601: Na ion-containing ionomer (manufactured by DuPont,Co.) Sirline 1650: Zn ion-containing ionomer (manufactured by DuPont Co.) YD7020: Bisphenol type epoxy compound (manufactured by Toto Kasei K.K.) VAIG03: EPDM (manufactured by Exxon Co.) Table 3 (continued) Sirline 1601: Na ion-containing ionomer (manufactured by DuPont Co.) Sirline 1650: Zn ion-containing ionomer (manufactured by DuPont Co.) YD7020: Bisphenol type epoxy compound (manufactured by Toto Kasei K.K.) VA1803: EPM (manufactured by Exxon Co.) Polyamide resin Polyester metal ion-containing Others resin ethylene copolymer Type Amount Type Amount Type Amount relative to Type Amount relative to (wt%) (wt%) 100 parts by weight 100 parts by weight of polyamide/ of polyamide/ polyester polyester (parts by weiqht) (parts by weiqht) Example 17 Nylon 66 60 PET 40 Sirline 10 - 1601 Example 18 Nylon 6 60 be 40 10 YD7020 5 Example 19 60 40 10 VA1803 5 Example 20 60 40 10 YD7020 3 Example 21 60 40 20 5 Example 22 Nylon 66 60 40 10 5 Table 3 (continued) Polyamide resin Polyester Metal ion-containing Others resin eth lene copolymer Type Amount Type Amount Type Amount relative to Type Amount relative to (wt%) (wt%) 100 parts by weight 100 parts by weight of polyamide/ of polyamide/ polyester polyester (parts by weight) (parts by weight) Comparative Nylon 6 80 PET 20 Example 10

Comparative 60 40 Exam le 11 ve P' 11 r Comparative 60 PBT 40 Exa ple_12 1 1 1 1 1 1 1 1 Sirline 1601; Na ion-containing lonomer (manufactured by DuPont Co.) Sirline 1650: Zn ion-containing ionomer (manufactured by DuPont Co.) YD7020: Bisphenol type epoxy compound (manufactured by Toto Kasel K.K.) VA1803: EPW (manufactured by Uxon Co.) l>, 1 1 Table 4

Tensile Elongation Izod impact strength value (kg/cm 2 (kg.CM/cm) Example 9 620 120 6.7 Example 10 630 110 7.0 Example 11 640 120 6.6 Example 12 640 160 11.3 Example 13 580 180 13.8.

Example 14 490 80 9.8 Example 15 620 90 6.9 Example 16 610 110 7.4 Example 17 630 70 7.1 Example 18 610 210 15.0 Example 19 600 230 16.7 1 24 - Table 4 (continued) Tensile Elongation Izod impact strength (%) value (kg/cm 2 (kg.cm/cm) Example 20 620 190 14.3 Example 21 590 230 16.8 Example 22 620 190 12.4 Comparative 210 1.1.4 Example 10

Comparative 170 1 1.3 Example 11

Comparative 180 1 0.9 Example 12

1.

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Claims

CLAIMS: 1. A resin composition comprising:

(1) 100 parts by weight of resin'composition comprising (i) from 5 to 95 by weight of a polyamide resin and (ii) from 5 to 95 by weight of a thermoplastic polyester resin; (A) from 0.01 to 30 parts by weight of a bisphenol type high molecular weight epoxy compound which is a condensation product of a bisphenol with epichlorohydrin and which has a polymerization degree of substantially at least 11; and/or (B) from 1 to 50 parts by weight of a metal ion-containing ethylene copolyme ^ r.
2. The resin composition according to Claim 1, wherein the bisphenol type high molecular weight epoxy compound (A) is represented by the following formula:

0 CH OH CH 0
3 3 r- CH -C 0-J7-\\- -Q\,O-CH 'k"-O-CH 2-CH,2fC 2_ 2 2-CH-CH2 CH 3 n1H 3 wherein n is an integer of at least 11, and the benzene rings may have substituents. 3. The resin composition according to Claim 1, wherein the bisphenol type high molecular weight epoxy compound (A) has a polymerization degree of substantially at least 15.
4. The resin composition according to Claim 1, wherein 26 the metal ion-containing ethylene copolymer (B) is a copolymer of ethylene with an unsaturated carboxylic acid, having metal ions bonded thereto.
5. The resin composition according to Claim 1, wherein the resin composition (I) comprises (i) from 20 to 90% by weight of the polyamide resin and (ii) from 10 to 80% by weight of the thermoplastic polyester resin.
6. The resin composition according to Claim 1, wherein the resin composition (I) comprises (i) from 40 to 90% by weight of the polyamide resin and (ii) from 10 to 60% by weight of the thermoplastic polyester resin.
7. The resin composition according to Claim 1, wherein the bisphenol type high molecular weight epoxy compound (A) is in an amount of from 0.05 to 20 parts by weight relative to 100 parts by weight of the resin composition (I).
8. The resin composition according to Claim 1, wherein the metal ion-containing ethylene copolymer (B) is in an amount of Crom 3 to 30 parts by weight relative to 100 parts by weight of the resin composition (I).

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