JP3489901B2 - Resin composition and laminate - Google Patents

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a resin composition and a laminate having excellent flexibility such as gas barrier property, bending resistance and drop impact resistance.

[0002]

2. Description of the Related Art Saponified ethylene-vinyl acetate copolymer (hereinafter referred to as EVOH) is a thermoplastic resin excellent in transparency, gas barrier property, oil resistance and aroma retention compared with other resins. It is used in various gas barrier films and gas barrier layers of gas barrier containers.
However, a multilayer film that uses EVOH as a gas barrier layer,
Multilayer containers can often have problems due to the high rigidity of EVOH. For example, a multilayer film or container filled with contents may be easily broken or broken when dropped, and a problem that pinholes may occur in the multilayer film filled with contents due to bending or vibration during transportation.
Therefore, there has been proposed a method of blending EVOH with another thermoplastic resin to improve these drawbacks. For example EV
OH ethylene-carboxylic acid vinyl ester copolymer,
Blending an ethylene-acrylic acid ester copolymer improves flex resistance (JP-A-61-282083).
9) or EVOH is blended with α, β-unsaturated carboxylic acid anhydride-modified ethylene-carboxylic acid vinyl ester copolymer or ethylene-acrylic acid ester copolymer to give E.
Improving the impact resistance of VOH (JP-A-61-83)
035) is known. However, with these methods E
The flex resistance and impact resistance of VOH are not sufficient, and they have not been put to practical use.

Regarding the blending of EVOH with a partially saponified ethylene-vinyl acetate copolymer, the provision of interlayer adhesion with polyolefin, and the provision of low-temperature heat-sealing properties, JP-B-51- 485
1 and JP-A-60-161477.
When molded products such as films are produced by these conventional techniques, there are problems such as lack of flexibility, poor thermal stability, severe moldability due to severe neck-in, and patterns such as stripes and satin. There are drawbacks such as generation on the film surface.
Also, blending EVOH with an epoxy-modified olefin polymer is described in JP-A-3-88837. In this blend system, the gas barrier property is good, but the flex resistance is insufficient.

[0004]

The present invention was devised to solve the above-mentioned drawbacks of the prior art, and has excellent gas barrier properties, excellent bending resistance, drop impact resistance, etc. It is an object of the present invention to provide a resin composition and a laminate having the above flexibility.

[0005]

[Means for Solving the Problems] The above objects are as follows: ethylene content is 20 to 65 mol%, and saponification degree of vinyl acetate component is 9%.
Resin composition consisting of 5 mol% or more of saponified ethylene-vinyl acetate copolymer (A), an olefin polymer (B) having an epoxy equivalent of 500 to 10,000 and an olefin polymer (C). And a laminate having a resin composition layer.

The EVOH (A) used in the present invention has an ethylene content of 20 to 65 mol%, preferably 25 to 55 mol%, a saponification degree of the vinyl acetate component of 95 mol% or more, and preferably 98 mol% or more. Resin. When the ethylene content is less than 20 mol%, not only a beautiful molded product such as a film cannot be obtained because it easily gels during melt molding, but also the gas barrier property under high humidity deteriorates. On the other hand, when the ethylene content is higher than 65 mol%, the gas barrier property is greatly deteriorated, which is not preferable. When the degree of saponification is less than 95 mol%, like the case where the ethylene content is less than 20 mol%, gelation is likely to occur during melt molding, and stable operation cannot be performed for a long time.
In addition, EVOH melt index {temperature 190 ℃,
Value measured under a load of 2160 g: However, the melting point is 1
2160g at around 90 ℃ or over 190 ℃
A value obtained by plotting the reciprocal of absolute temperature as the horizontal axis and the melt index logarithm as the vertical axis in a semilogarithmic graph measured at a plurality of temperatures under a load and extrapolated to 190 ° C; hereinafter, M
It is 0.5 to 15 g / 10 minutes. Furthermore, the EVOH referred to in the present invention may be modified with a copolymerization monomer in the range of 5 mol% or less, and as the modifying monomer, propylene, 1-butene, 1-hexene, 4-methyl-1-pentene, Acrylic ester,
Methacrylic acid ester, maleic acid, fumaric acid, itaconic acid, higher fatty acid vinyl ester, alkyl vinyl ether, N-vinylpyrrolidone, N-normal butoxymethylacrylamide, vinyltrimethoxysilane, vinylmethyldimethoxysilane, vinyldimethylmethoxysilane, N- Examples thereof include (2-dimethylaminoethyl) methacrylamides or quaternary products thereof, N-vinylimidazole or quaternary products thereof, and the like.

The olefin-based polymer (B) having an epoxy group used in the present invention is an olefin-based polymer obtained by randomly copolymerizing an olefin monomer and an epoxy group-containing ethylenically unsaturated monomer. And a modified olefin polymer obtained by graft-polymerizing an epoxy group-containing ethylenically unsaturated monomer with an initiator such as peroxide, heat, light or ionizing radiation. Examples of the epoxy group-containing ethylenically unsaturated monomer include glycidyl methacrylate, glycidyl acrylate, allyl glycidyl ether, vinyl glycidyl ether, hydroxyalkyl acrylate or hydroxyl methacrylate glycidyl ether.

The epoxy group content is 5 in terms of epoxy equivalent.
00 to 10,000, more preferably 1,000 to 6,000. Here, the epoxy equivalent is the number of g of a resin containing 1 g of an epoxy group. If the epoxy equivalent is less than 500, the thickening will be severe, resulting in defects such as gelation and deterioration of moldability, while if it exceeds 10,000,
Poor compatibility with EVOH may result in poor mechanical properties, which is not preferable.

Examples of the olefin polymer include polyolefins such as polyethylene, polypropylene and polybutylene, and olefin copolymers. Specific examples of the olefin-based copolymer include ethylene-propylene copolymer, ethylene-α-olefin copolymer such as ethylene-butylene copolymer, ethylene-acrylic acid ester copolymer, ethylene-vinyl acetate copolymer. Copolymers, butyl rubber and the like can be mentioned, but particularly preferably, ethylene copolymers, particularly ethylene-propylene copolymers, ethylene-vinyl acetate copolymers, ethylene-acrylic acid ester copolymers are used. The MI of the olefin-based copolymer having an epoxy group introduced therein is not particularly limited, but is preferably 0.1 to 50 g / 10 minutes, and more preferably 0.5 to 15 g / 10 minutes. .

The olefin polymer (C) used in the present invention maintains compatibility with EVOH by blending with the olefin polymer having an epoxy group,
It also has the effect of improving flexibility.

Examples of the olefin polymer (C) used in the present invention include polyolefins such as polyethylene, polypropylene and polybutylene, and olefin copolymers. Specific examples of the olefin-based copolymer include ethylene-propylene copolymer, ethylene-α-olefin copolymer such as ethylene-butylene copolymer, ethylene-acrylic acid ester copolymer, ethylene-vinyl acetate copolymer. Examples include coalesce, butyl rubber, etc.
Particularly preferably, ethylene copolymers, particularly ethylene-propylene copolymers, ethylene-vinyl acetate copolymers, ethylene-acrylic acid ester copolymers are used.

The MI of the olefin polymer (C) is not particularly limited, but is preferably 0.1 to 50 g / 10 minutes, and more preferably 0.5 to 15 g / 10 minutes. The olefin polymer (C) is distinguished from (B),
A polyolefin having no epoxy group and having a tensile elastic modulus at room temperature of 1.5 kgf / mm ² or less is preferable. More preferably 1.5 to 0.3 kgf /
mm ² . The tensile elastic modulus was calculated from the slope of the rising straight line when the film was pulled at a speed of 5 mm / min with a film tensile tester (Autograph: Shimadzu AG-500A) using a film having a thickness of 25 μm. It is a value (ASTM D822), and a smaller value means a softer (lower tensile elastic modulus) film.

The resin composition of the present invention is EVOH (A)
And an olefin polymer (B) having an epoxy group,
Mixture with olefin polymer (C), but EVOH
The blending ratio of (A) to the total olefin polymer (B + C) is (A) / {(B) + (C)} = 60/40 to 9
5/5 (weight ratio), more preferably (A) /
{(B) + (C)} = 70/30 to 90/10 (weight ratio). When (A) / {(B) + (C)} exceeds 95/5, drop impact resistance and flex resistance are poor. On the other hand, 60 /
When it is less than 40, not only the transparency is poor, but also the gas barrier property is poor. Further, the blending ratio of the olefin polymer (B) having an epoxy group introduced therein and the olefin polymer (C) is (B) / (C) = 95/5 to 5/95 (weight ratio), Suitably (B) / (C) = 30 / 70-
70/30 (weight ratio). (B) / (C) is 5/9
When it is less than 5, the flexing resistance and the drop impact resistance are poor due to poor compatibility with EVOH. On the other hand, if it exceeds 95/5, the flexibility is poor, and thus the bending resistance and the drop impact resistance are also poor. For this reason, it is preferable that there is not much difference in the blending amount of both.

The EVOH, the olefin-based polymer having an epoxy group, and the olefin-based polymer are mixed by a Banbury mixer, a single-screw or twin-screw extruder,
Although there is a method of using a Brabender plastomill or the like, each resin may be directly supplied to various molding machines and kneaded by the molding machine to perform molding processing. Further, when kneading these, a plasticizer, a lubricant, an antioxidant, a colorant, various resins and the like may be added within a range that does not impair the effects of the present invention. The resin composition of the present invention is preferably used as a laminate. At this time, the resin composition of the present invention can be used in any of the intermediate layer, the outermost layer and the innermost layer. The resin to be laminated with the resin composition of the present invention is not particularly limited, but a resin having good transparency is generally preferable, and examples thereof include low density polyethylene, linear low density polyethylene, polypropylene, and ethylene-propylene copolymer. Coalescing,
Polyolefin such as polybutene, ethylene-vinyl acetate copolymer, ethylene-acrylic acid ester copolymer, copolymer mainly composed of olefin such as ionomer, polystyrene, polyamide, polyethylene terephthalate,
Examples include polycarbonate, polyvinyl chloride, and the like, or a mixture thereof. Of these, particularly preferably used are low density polyethylene, linear low density polyethylene, polypropylene, ethylene-propylene copolymer,
The ethylene-vinyl acetate copolymer is a homopolymer or a mixture thereof.

If the interlayer adhesion between these resins and the resin composition of the present invention is not sufficient, it is preferable to provide an adhesive resin layer. The adhesive resin is not particularly limited as long as it does not cause delamination at a practical stage, and is not particularly limited, but an unsaturated carboxylic acid or an anhydride thereof is used as an olefin polymer {for example, low density polyethylene,
Polyolefins such as linear low-density polyethylene, polypropylene, and polybutylene, and copolymers of olefins and unsaturated monomers (vinyl esters, unsaturated carboxylic acid esters, etc.) copolymerizable therewith, such as ethylene-vinyl acetate copolymers. A modified olefin-based copolymer having a carboxyl group, which is obtained by chemically (for example, by an addition reaction or a graft reaction) chemically bonded to a polymer or an ethylene-acrylic acid ethyl ester copolymer. Specifically, one or more selected from maleic anhydride graft-modified polypropylene, maleic anhydride graft-modified ethylene-ethyl acrylate copolymer, anhydride maleic acid graft-modified ethylene-vinyl acetate copolymer and the like. Mixtures are mentioned as suitable. Further, EVOH or the resin composition of the present invention can be mixed with these adhesive resins within a range that does not impair the effects of the present invention. The resin composition of the present invention can be formed into a film, sheet, tube, bottle or the like as a laminate.

The thickness composition of each layer is not particularly limited, but from the viewpoint of transparency, the resin composition layer is preferably used in an amount of 300 μm or less, and more preferably 200 μm or less. On the other hand, from the viewpoint of barrier, it is desirable to use at 20 μm or more, more preferably 30 μm or more.

The method for laminating the resin composition of the present invention is not particularly limited, and examples thereof include a coextrusion method, an extrusion lamination method and a dry lamination method. Particularly, according to the coextrusion method, the resin composition of the present invention can be obtained. It is preferable because the characteristics can be exhibited.

The laminate thus obtained can be used in a bag-in-box having excellent flex resistance, a floor heating pipe, a container having excellent drop impact resistance and the like.

[0019]

The present invention will be described in more detail with reference to the following examples, but the present invention is not limited thereto. "%" In the examples is based on weight unless otherwise specified.

Example 1 Melt index (MI) measured according to ASTM D1238 65T under conditions of ethylene content of 32 mol%, saponification degree of vinyl acetate component of 99.4 mol%, 190 ° C. and 2160 g load. 1.2g / 10min EVO
Obtained by adding 4 parts of glycidyl methacrylate and 0.6 part of dicumyl peroxide to 100 parts of ethylene-propylene copolymer having 70% of H and 90% by weight of ethylene content and kneading at 170 ° C. for 10 minutes in a Brabender plastomill. Epoxy equivalent is 1050, MI is 1.5 g / 10 min glycidylmethacrylate grafted ethylene-propylene copolymer 15%, and room temperature tensile modulus 0.5 kgf /
mm ² and an ethylene-propylene copolymer 15% having an ethylene content of 86% by weight and having an MI of 1.2 g / 10 min, 30
The pellets were blended and pelletized at a temperature of 220 ° C. using a φ-direction twin-screw extruder. Then, using this pellet, 40φ
The film was formed by the film forming machine consisting of the extruder and the T-die at the extruder temperature of 180 to 220 ° C. and the T-die temperature of 215 ° C. to obtain a film having a thickness of 25 μm. About the film, film surface, moldability, haze, flex resistance, oxygen gas permeation amount (O
TR) was evaluated.

The film surface was evaluated by visually scoring streaks, satin and spots in five grades A to E shown in Table 1.

[0022]

[Table 1]

The haze was measured using a Poic integrating sphere type light transmittance meter manufactured by Nippon Seimitsu Optical Co., Ltd. The flex resistance was evaluated using a gelbo flex tester manufactured by Rigaku Kogyo Co., Ltd., a 12-inch x 8-inch film was made into a cylindrical shape with a diameter of 3.5 inches, both ends were gripped, and the initial gripping interval was 7 inches. , Gripping interval at maximum bending is 1 inch, twist of 440 degree is added at the first 3.5 inch of stroke, and then 2.5 inch is linear horizontal movement 40 times / min. It was performed by determining the number of pinholes of the film after repeating 300 times and 400 times under the conditions of 20 ° C. and 65% RH at the speed of.
The tensile elastic modulus (Young's modulus) is ASTMD-882-
According to 67, the measurement was performed under the conditions of 20 ° C. and 65% RH.
The oxygen gas transmission rate (OTR) is measured by Modern C
OX-TRAN 10-50A manufactured by Ontrol Co. was used, and the measurement was performed under the conditions of 20 ° C. and 65% RH. The evaluation results of each are shown in Tables 2 and 3, and this resin composition is
It has good permeability and excellent bending resistance and gas barrier properties.

Examples 2 to 5 Various EVOHs, various epoxy group-containing olefin polymers and various olefin polymers were used to prepare 25 μm-thick films in the same manner as in Example 1 and various evaluations were performed. The results are shown in Table 2. Here, the combinations of the epoxy group-containing olefin-based polymer and the olefin-based polymer used in each example are shown below. In Example 2, an ethylene-propylene copolymer 10 having an ethylene content of 88% by weight was used.
Epoxy equivalent 2500 obtained by adding 3 parts of glycidyl acrylate and 0.6 part of dicumyl peroxide to 0 part and kneading at 170 ° C. for 10 minutes in Brabender Plastomill.
And a glycidyl acrylate grafted ethylene-propylene copolymer having an MI of 5.0 g / 10 min and a tensile elastic modulus of 0.6 kgf / mm ² at room temperature, an MI of 5.2 g / 1.
An ethylene-propylene copolymer having an ethylene content of 0 minutes at 89% by weight was used. In Example 3, the epoxy equivalent is 30.
00, MI is 1.5 g / 10 min, glycidyl acrylate random copolymer modified low density polyethylene and room temperature tensile elastic modulus 1.0 kgf / mm ² , MI 1.3 g /
10 minutes of low density polyethylene was used. In Example 4,
Glycidyl methacrylate random copolymer modified low-density polyethylene with epoxy equivalent of 4500 and MI of 5.2 g / 10 min and tensile elastic modulus at room temperature of 0.6 kgf / mm ²
Then, an ethylene-propylene copolymer having an MI of 5.2 g / 10 minutes and an ethylene content of 89% by weight was used. In Example 5,
Glycidyl methacrylate random copolymer modified low density polyethylene with an epoxy equivalent of 800 and MI of 17 g / 10 min, and a tensile elastic modulus at room temperature of 0.7 kgf / mm ² with MI of 14 g / 10 min and ethylene content of 91% by weight. A polymer was used. In each of Examples 2 to 5, the bending resistance and the gas barrier property were good, and the film surface and the transparency were also excellent.

Comparative Example 1 In Example 1, ethylene content was 32 mol%, saponification degree of vinyl acetate component was 99.4 mol%, and MI was 1.2 g.
/ 10 min EVOH 70% and ethylene content 90% by weight ethylene-propylene copolymer 100 parts glycidyl methacrylate 4 parts and dicumyl peroxide 0.6 parts were added and kneaded at 170 ° C. for 10 minutes in a Brabender Plastomill. The obtained epoxy equivalent was 1050 and MI was 1.
Glycidyl methacrylate grafted ethylene-propylene copolymer 15% at 5 g / 10 minutes, and a tensile elastic modulus of 0.5 kgf / mm ² at room temperature, and an ethylene-propylene copolymer weight at an ethylene content of 86% by weight of MI 1.2 g / 10 minutes. Change to a resin composition consisting of 15%
Tables 2 and 3 show the results of various evaluations of a single film having a thickness of 25 μm. It has good gas barrier properties, film surface and transparency, but poor flex resistance.

Comparative Examples 2 to6 EVOH and various epoxy group-containing olefin polymers
And various olefin polymers as in Example 1
A 25 μ film was prepared and various evaluations were performed. The result
It shows in Table 2. Here, the epoxy group containing used in each comparative example
The olefin polymer and the olefin polymer are as follows.
It is shown. Epoxy group-containing ole used in Comparative Example 2
The fin-based polymer is the same as that described in Example 1.
Epoxy group-containing olefin polymer used in Comparative Example 3
Is the same as described in Example 2. Epoxy group used in Comparative Example 4
The content of the olefin-based polymer is the same as that described in Example 5.ratioComparison
An example5The epoxy group-containing olefin polymer used in
Ethylene-propylene copolymer having a ethylene content of 89% by weight
100 parts of glycidyl acrylate and 1 part of dicumylpa
-Add 0.5 parts of oxide and Brabender Plastomill
Epoxy equivalent 12 obtained by kneading in 150 ° C for 80 minutes
000, MI of 1.3 g / 10 min glycidyl acryl
Using rate-grafted ethylene-propylene copolymer
It was Comparative example6Polymerization of olefins containing epoxy groups used in
The body has an epoxy equivalent of 300 and an MI of 4.8 g / 10
Glycidyl methacrylate random copolymer modified low density
Degree polyethylene was used. Comparative Example 1 is a gas barrier,
Good film surface and transparency, but extremely poor bending resistance
It Comparative Example 2FourIs a gas barrier, film surface, transparency
Comparatively good, but poor in flex resistance. Comparative example5-6
Has poor film surface, transparency, and bending resistance.

Example 6 EVOH7 having an ethylene content of 32 mol%, a saponification degree of a vinyl acetate component of 99.4 mol% and an MI of 1.2 g / 10 min.
Obtained by adding 4 parts of glycidyl methacrylate and 0.6 part of dicumyl peroxide to 100 parts of an ethylene-propylene copolymer having 0% and an ethylene content of 90% by weight, and kneading at 170 ° C. for 10 minutes in a Brabender plastomill. Epoxy equivalent is 1050, MI is 1.5 g / 10 min glycidyl methacrylate grafted ethylene-propylene copolymer 15%, and room temperature tensile modulus 0.5 kgf
Ethylene content of 1.2 g / 10 min at 86 / mm ² 86
A 15 μm-thick intermediate layer consisting of 15% by weight of ethylene-propylene copolymer, and 30 each on each side of the intermediate layer.
μ 4-methyl-1-pentene as a copolymerization component, containing 3.2 mol% of the copolymerization component, MI having a surface layer consisting of linear low-density polyethylene of 1.8 g / 10 min, A laminated film of 85 μm in total, which is arranged between the layers with an adhesive resin layer made of ethylene maleic anhydride-vinyl acetate copolymer having a vinyl acetate content of 5 μm and a maleic anhydride content of 0.5 wt%. Was obtained by a coextrusion method using three extruders and a three-layer, five-layer multi-layer die head. As the resin composition used for the intermediate layer, pellets preliminarily blended by an extruder were used.

No pinholes were observed until the bending resistance test of 10,000 reciprocations was completed.
It was confirmed that one pinhole had occurred at the time when the presence or absence of a pinhole was inspected after the round trip. Further, delamination between the layers was not recognized at all. The haze of the film was 4%, transparency was good, and no stripes or satin was observed. Comparative Example 7 In Example 6, the intermediate layer had an ethylene content of 32 mol%, a saponification degree of the vinyl acetate component of 99.4 mol%, and MI.
Was used in the same manner as in Example 6 except that a single EVOH having a viscosity of 1.2 g / 10 min was used, and various evaluations were performed. The results are shown in Table 4. The film has poor flex resistance.

Example 7 EVOH7 having an ethylene content of 44 mol%, a saponification degree of a vinyl acetate component of 99.5 mol% and an MI of 5.5 g / 10 min.
Epoxy obtained by adding 0%, 100 parts of an ethylene-propylene copolymer having an ethylene content of 88% by weight, 3 parts of glycidyl acrylate and 0.6 part of dicumyl peroxide and kneading at 170 ° C. for 10 minutes in a Brabender plastomill. Equivalent of 2500, MI of 5.0 g / 10 min, glycidyl acrylate grafted ethylene-propylene copolymer 15% and room temperature tensile elastic modulus of 0.6 kgf / mm
² , MI 5.2g / 10min ethylene content 89% by weight
Of a resin composition layer consisting of 15% of ethylene-propylene copolymer as an intermediate layer, and two containers (internal volume 10 L) having inner and outer layers having an average thickness of all layers of 300 μ are used as an extruder and a die head for two kinds of three layers. It was obtained by co-extrusion and direct blow molding. The resin composition used for the intermediate layer here was pellets blended in advance with an extruder.
This container was filled with 10 L of water and dropped three times from a height of 1.2 m, but the bag was not broken and good drop impact resistance was exhibited.

Comparative Example 8 In Example 7, the ethylene content was 44 mol%, the saponification degree of the vinyl acetate component was 99.5 mol%, and the MI was 5.5 g /
EVOH 70% for 10 minutes, 100 parts of ethylene-propylene copolymer having an ethylene content of 88% by weight, 3 parts of glycidyl acrylate and 0.6 part of dicumyl peroxide were added and kneaded at 170 ° C. for 10 minutes in a Brabender Plastomill. The obtained epoxy equivalent is 2500 and MI is 5.0 g /
10 minutes glycidyl acrylate grafted ethylene-
A multilayer direct blow container was molded in the same manner as in Example 7 except that a resin composition containing 30% of a propylene copolymer was used as the resin for the intermediate layer, and the same drop test was performed.
The container broke in the first drop test, and the drop impact resistance was poor.

[0031]

[Table 2]

[0032]

[Table 3]

[0033]

[Table 4]

[0034]

INDUSTRIAL APPLICABILITY The resin composition of the present invention has good gas barrier properties, film surface and transparency, and has significantly better flexibility than EVOH alone and other blend systems, and the resin composition layer The laminate including at least one layer of is excellent in bending resistance and drop impact resistance.

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Claims (5)

(57) [Claims] 1. An ethylene-vinyl acetate copolymer saponification product (A) having an ethylene content of 20 to 65 mol% and a saponification degree of a vinyl acetate component of 95 mol% or more, and an epoxy equivalent of 500 to 10,000. Olefin-based polymer (B) and olefin-based polymer as a base of (B)
Consisting of an olefin polymer (C) different from the polymer,
The weight ratio of (A) / {(B) + (C)} is 60/40 to 9
5/5, and the weight ratio of (B) / (C) is 5 / 95-9.
The resin composition which is 5/5. 2. The olefin polymer (B) having an epoxy group is selected from the group consisting of glycidyl methacrylate, glycidyl acrylate, allyl glycidyl ether, vinyl glycidyl ether, hydroxyalkyl acrylate glycidyl ether and hydroxyalkyl methacrylate glycidyl ether. The resin composition according to claim 1, which is a modified olefin-based polymer modified with at least one epoxy group-containing ethylenically unsaturated monomer. 3. A laminate comprising at least one resin composition layer according to claim 1 or 2. 4. A film comprising the laminate according to claim 3. 5. A container comprising the laminate according to claim 3.