JPH06145435A - Resin composition - Google Patents

Abstract

PURPOSE:To obtain a resin composition, having excellent adhesive properties and heat resistance as an adhesive layer of various multilayered laminated structures, suitably usable especially as the adhesive layer for interior trim materials for automobiles, etc., requiring adhesive properties at low temperatures or heat-resistant creep properties at high temperatures without causing problems in use of organic solvents or complicated operation steps, etc., for use thereof. CONSTITUTION:This resin composition consists essentially of (A) a multielement copolymer composed of ethylene and a radically copolymerizable acid anhydride and a radically polymerizable comonomer other than them and (B) a salt of an organic carboxylic acid and a metal belonging to group IA, IIA or IIB of the periodic table.

Description

Detailed Description of the Invention [Industrial applications]

The present invention relates to a resin composition, and more specifically, as an adhesive layer for automobile interior materials and the like, which are excellent in adhesiveness and heat resistance, and particularly require adhesiveness at low temperatures and heat creep resistance at high temperatures. The present invention relates to a resin composition of an ethylene-based multi-component copolymer that can be preferably used.

[0002]

2. Description of the Related Art As an interior material for automobiles, vehicles, ships, etc., and as an interior material for enhancing the habitability and aesthetics of a building such as a house, A multilayer laminated structure is used in which a skin material and a substrate material for maintaining and enhancing functionality are adhered. This multi-layer laminated structure can be manufactured by adhering the above-mentioned skin material and substrate material with a solvent-type adhesive. However, the solvent-type adhesive requires time and labor in the work steps such as painting, drying and aging. In recent years, as environmental issues are becoming more important,
There is a problem of industrial hygiene and fire due to organic solvents, and it is hard to say that this is an appropriate manufacturing method. Therefore, instead of the solvent type adhesive, ethylene-acrylic acid ester-maleic anhydride terpolymer, ethylene-vinyl acetate copolymer,
Although a heat-sensitive adhesive resin such as ethylene-acrylic acid ester copolymer or low melting point copolymer nylon is used,
I'm still not completely satisfied. That is, the heat-sensitive adhesive resin generally has insufficient adhesive strength as compared with the solvent-type adhesive and often lacks heat-resistant creep resistance, and is exposed to a high temperature (80 ° C.) such as the temperature inside a car in hot weather for a long time. When,
It has a drawback that it easily causes sagging or peeling. Also,
Although the adhesiveness can be enhanced by setting the heating temperature to a relatively high temperature during the adhesion, in this case, there is a drawback that the epidermis is likely to be damaged. On the other hand, there are heat-sensitive adhesive resins that do not have these drawbacks, but they have the drawback that they are expensive and their use is limited in terms of cost. As described above, it can be used as an adhesive layer for interior materials such as automobiles and houses, has no problems in use such as workability and environmental problems, and has good heat-resistant creep for a wide range of skin materials and substrate materials. Adhesive that exhibits good properties, has adhesiveness at low temperatures that can prevent damage to the skin agent, and is also satisfactory in terms of cost,
The reality is that it has not been developed yet.

[0003]

In view of the above situation, the inventors of the present invention have conducted earnest studies to develop an adhesive that eliminates the conventional drawbacks. As a result, a resin composition containing a specific ethylene-based multi-component copolymer and a salt of an organic carboxylic acid and a specific metal as a main component is used for a wide variety of base materials (skin materials, skin materials,
It has been found that it has good adhesiveness and heat resistance to the substrate material). The present invention has been completed based on such findings. That is, the present invention relates to (A) a multi-component copolymer comprising ethylene, a radical-polymerizable acid anhydride and a radical-polymerizable comonomer other than the above, wherein the radical-polymerizable acid anhydride in the ethylene-based multi-component copolymer is The ethylene-based multi-component copolymer and the organic carboxylic acid (B) in which the proportion of the units derived from is 0.1 to 5% by weight and the proportion of the units derived from other radically polymerizable comonomers is 3 to 50% by weight. And a salt of a metal belonging to Group IA, IIA or IIB of the periodic table.

The ethylene-based multi-component copolymer constituting the component (A) of the resin composition of the present invention comprises ethylene, a radical-polymerizable acid anhydride and a radical-polymerizable comonomer other than the above radical-polymerizable acid anhydride. It is a multi-component copolymer.
Here, the radical-polymerizable acid anhydride is a compound having at least one radical-polymerizable unsaturated bond and at least one acid anhydride group in the molecule, and capable of introducing an acid anhydride group into the molecule by polymerization. Means The acid anhydride group is preferably cyclic. Examples of such compounds include maleic anhydride, itaconic anhydride, endic acid anhydride, citraconic anhydride, dodecenyl succinic anhydride, 1-butene-3,4.
-Dicarboxylic acid anhydrides, alkenylsuccinic anhydrides having a double bond at the terminal having at most 18 carbons, alkadienyl succinic anhydride having a double bond at the terminal having at most 18 carbons, and the like. These alone
Alternatively, two or more kinds may be used in combination. Among these, maleic anhydride and itaconic anhydride are particularly preferable. The proportion of the units derived from the radical-polymerizable acid anhydride in the component (A) is in the range of 0.1 to 5% by weight, preferably 0.5 to 4.5% by weight, more preferably 1 It is in the range of 0.0 to 4.0% by weight. Here, if the proportion of the radical-polymerizable acid anhydride is less than 0.1% by weight, the adhesiveness is insufficient and good adhesive strength cannot be obtained. On the other hand, if it exceeds 5% by weight, it becomes difficult to produce an ethylene-based copolymer, which is not practical.

There are various compounds as radical-polymerizable comonomers other than radical-polymerizable acid anhydrides, such as ethylenically unsaturated ester compounds, ethylenically unsaturated amide compounds, ethylenically unsaturated acid compounds, and ethylenically unsaturated compounds. Examples thereof include saturated ether compounds, ethylenically unsaturated hydrocarbon compounds, and other compounds. Specifically describing these, as the ethylenically unsaturated ester compound,
For example, vinyl acetate, methyl (meth) acrylate, ethyl (meth) acrylate, propyl (meth) acrylate,
Butyl (meth) acrylate, hexyl (meth) acrylate, octyl (meth) acrylate, lauryl (meth) acrylate, benzyl (meth) acrylate, methyl fumarate, ethyl fumarate, propyl fumarate, butyl fumarate , Dimethyl fumarate, diethyl fumarate, dipropyl fumarate, dibutyl fumarate, methyl maleate, ethyl maleate, propyl maleate, butyl maleate, dimethyl maleate, diethyl maleate, dipropyl maleate, dibutyl maleate, etc. Can be mentioned.
Examples of the ethylenically unsaturated amide compound include (meth) acrylamide, N-methyl (meth) acrylamide, N-ethyl (meth) acrylamide, N-propyl (meth) acrylamide, N-butyl (meth) acrylamide, N- Hexyl (meth) acrylamide, N-octyl (meth) acrylamide; N, N-dimethyl (meth) acrylamide; N, N-diethyl (meth) acrylamide and the like. Examples of the ethylenically unsaturated acid compound include (meth) acrylic acid, fumaric acid, maleic acid and the like. Examples of the ethylenically unsaturated ether compound include methyl vinyl ether, ethyl vinyl ether, propyl vinyl ether, butyl vinyl ether, octadecyl vinyl ether, phenyl vinyl ether and the like. Examples of the ethylenically unsaturated hydrocarbon compound include styrene, α-methylstyrene, (meth) acrylonitrile, acrolein, crotonaldehyde, trimethoxyvinylsilane, triethoxyvinylsilane, vinyl chloride, vinylidene chloride, norbornene and butadiene. . Among these,
(Meth) acrylic acid esters and (meth) acrylic acid are mentioned as particularly preferable compounds. These comonomers may be used alone or in combination of two or more. The proportion of the units derived from the radical-polymerizable comonomer in the component (A) is in the range of 3 to 50% by weight, preferably 4 to 45% by weight, more preferably 5 to 40% by weight. . Here, if the proportion of the radical-polymerizable comonomer is less than 3% by weight, the crystal melting point of the ethylene-based multi-component copolymer is not sufficiently lowered, and the low-temperature adhesiveness which is a feature of the present invention cannot be sufficiently exhibited. On the other hand, if it exceeds 50% by weight, it becomes difficult to handle the resin and the heat resistance of the product deteriorates.

In producing the ethylene-based multi-component copolymer which is the above-mentioned component (A), it is possible to basically utilize ordinary production equipment for high-pressure low-density polyethylene and its technology. Generally, by the bulk polymerization method, 70
Polymerization pressure of 0 to 3,000 atm, preferably 1,000 to 2,500 atm, and 100 to 300 ° C., preferably 15
It is produced by radical polymerization at a polymerization temperature of 0 to 270 ° C. When the polymerization pressure is less than 700 atm, the molecular weight of the polymer becomes low, and the moldability and the resin physical properties of the resin composition deteriorate.
On the other hand, when the pressure exceeds 3,000 atm, the manufacturing cost is increased and it is practically meaningless. Also, the polymerization temperature is 10
If the temperature is lower than 0 ° C, the polymerization reaction is not stable and the conversion rate to the copolymer is lowered, which is economically problematic. On the other hand, when the temperature exceeds 300 ° C, the molecular weight of the copolymer decreases, and at the same time, there is a risk of a runaway reaction. As the polymerization apparatus, it is preferable to use a vessel type reactor. Particularly, since radical-polymerizable acid anhydrides have poor polymerization stability, a high degree of homogenization within the reactor is required. If necessary, a plurality of reactors may be connected in series or in parallel to carry out multistage polymerization.
Further, by partitioning the inside of the reactor into a plurality of zones, more precise temperature control can be performed.

The ethylene-based multi-component copolymer is produced in the presence of at least one free radical initiator under the above reaction conditions. Here, as the free radical initiator, specifically, for example, oxygen; dialkyl peroxides such as di-t-butyl peroxide, t-butyl cumyl peroxide, dicumyl peroxide; acetyl peroxide, i-butane Diacyl peroxides such as noyl peroxide and octanoyl peroxide; peroxy-dicarbonates such as di-i-propyl peroxy-dicarbonate and di-2-ethylhexyl peroxy-dicarbonate; t-butyl peroxypivalate, Peroxyesters such as t-butylperoxylaurate; ketone peroxides such as methylethylketone peroxide and cyclohexanone peroxide; 1,1-bis-t-butylperoxycyclohexane, 2,2-bis-t-butylperoxy Peroki such as octane Ketal; t-
Examples thereof include hydroperoxides such as butyl hydroperoxide and cumene hydroperoxide; azo compounds such as 2,2-azo-i-butyronitrile. Further, in the polymerization, various chain transfer agents can be used as the molecular weight modifier. As the chain transfer agent, for example,
Olefins such as propylene, butene and hexene; Paraffins such as ethane, propane and butane; Carbonyl compounds such as acetone, methyl ethyl ketone and methyl acetate;
Aromatic hydrocarbons such as toluene, xylene, and ethylbenzene are listed.

The ethylene-based multi-component copolymer produced in this manner melts at a relatively low temperature and is rich in physicochemical interactions and reactivity with various base materials (skin materials, substrate materials). Therefore, the resin composition of the present invention plays a large role in exhibiting high adhesive strength even in low temperature molding.

Next, the organic carboxylic acid which constitutes the component (B) of the resin composition of the present invention and the periodic table IA group, IIA group or II.
The salt with a metal belonging to Group B means a compound in which an organic carboxylic acid is completely or partially neutralized with a metal belonging to Group IA, IIA or IIB of the periodic table. As the above-mentioned organic carboxylic acid, various ones can be used, and examples thereof include lauric acid, myristic acid, stearic acid, palmitic acid, decanoic acid, pentadecanoic acid, eicosanoic acid, docosanoic acid. Saturated fatty acids having 10 or more carbon atoms (usually 10 to 40) such as acid, tricosanoic acid, triacontanoic acid, suberic acid, azelaic acid, sebacic acid, and hexadecanedioic acid; oleic acid, erucic acid, linolein Acids, linolenic acid, arachidonic acid, etc. having 10 or more carbon atoms (usually 10 to 40 unsaturated fatty acids;
Examples thereof include polymeric carboxylic acids such as copolymers of ethylene and (meth) acrylic acid. On the other hand, the metal forming a salt with an organic carboxylic acid is a group IA, IIA or
It is a metal belonging to the IIB group. The component (B) plays a large role in improving the adhesive strength of the resin composition of the present invention, particularly the heat creep resistance, but the adhesive strength cannot be sufficiently improved with metals other than the above. Among the components (B), preferred are sodium stearate, sodium oleate, and metal salts of high molecular weight carboxylic acids generally called ionomers (for example, sodium compounds of ethylene- (meth) acrylic acid copolymers or Partially neutralized products with zinc compounds) and the like. (B)
The components may be used alone or in combination of two or more.

The compounding ratio of the components (A) and (B) is not particularly limited, and the performance required for the resin composition of the present invention,
For example, it can be set to an arbitrary ratio depending on the type of the base material to be adhered, the step of the adhesion work, the use of the obtained multilayer laminated structure, and the like. Generally, the ratio of the number of moles of metal atoms in the component (B) to the number of moles of units derived from the radical-polymerizable acid anhydride in the component (A) is in the range of 1/10 to 10/1,
The range is preferably 2/10 to 10/2, and more preferably 3/10 to 10/3. The resin composition of the present invention prepared with this blending ratio shows good adhesiveness, and particularly in the production of a multilayer laminated structure used as an interior material for automobiles, etc., the skin material and the substrate material are strongly bonded at low temperature. Can be bonded and has excellent heat-resistant creep resistance. Also, in the case of a special application, for example, when adhesion at a very low temperature (about 90 ° C) is required,
The compounding ratio may be outside the above range.

In addition to the components (A) and (B) described above, the resin composition of the present invention contains various additives, compounding agents, and fillers within a range that does not impair the characteristics of the resin composition of the present invention. Agents and the like can be added. Specifically, for example, inorganic materials such as antioxidants (heat resistance stabilizers), ultraviolet absorbers (light stabilizers), antistatic agents, antifogging agents, flame retardants, lubricants (slip agents, antiblocking agents), glass fillers, etc. Examples include fillers, organic fillers, reinforcing agents, colorants (dyes and pigments), foaming agents, cross-linking agents, and fragrances. These additives and the like may be added at the time of producing the resin composition of the present invention, (A)
It may be added to the component or the component (B) from the beginning.

The resin composition of the present invention is prepared by mixing the components (A) and (B) and, if necessary, other components. When mixing each component,
Various commonly known methods can be used. Specifically, for example, a method of dissolving and reprecipitating each component in a solvent such as high temperature toluene, a method of mixing each component in a molten state, that is, a commonly used pressure kneader, roll, Banbury Examples thereof include a method using a mixer, a static mixer, a screw type extruder and the like. In some cases, the components may be dry blended to form a composition during molding. That is, the respective components can be mixed in the form of pellets or powder, and melt-mixed by utilizing the manufacturing stage of a film or the like.

The resin composition of the present invention can be applied to various uses and molding methods as an adhesive layer of a multilayer laminated structure. As the molding method, various conventionally known methods,
For example, a method of sandwiching and thermally adhering the above resin composition formed into a film by inflation molding or T-die molding between substrates, coating the above resin composition on a substrate by extrusion laminating, and then applying another substrate. Examples include a method of thermally adhering to a material, a method of sprinkling the above resin composition as a powder adhesive on a base material, and the like, but the resin composition of the present invention is suitable for a wide range of base materials. It exhibits adhesiveness, which is one of the features of the present invention.
Examples of such an adherable substrate include high-quality paper,
Various kinds of paper such as kraft paper, glassine paper, Japanese paper, cardboard base paper, synthetic paper, art paper, coated paper, etc .; various woven or non-woven fabrics made of cotton, linen, polyester, nylon, etc .; wood board; iron, aluminum, copper, tin plate Various metal plates or foils; plates, molded products, films or foams made of various plastics such as polypropylene, polystyrene, polyethylene, polyester, nylon, polycarbonate, acrylic resin, phenol resin, polyurethane and the like;
Examples include various inorganic substances such as glass fiber and ceramics. Further, these base materials may be subjected to surface treatment, coating, printing or the like, if necessary.

The resin composition of the present invention can be suitably used particularly as an adhesive layer for interior materials for automobiles and the like, which are required to have adhesiveness at low temperature and heat creep resistance at high temperature. Here, the skin material and the substrate material that can be bonded are not particularly limited, and the present invention can be applied to various materials that are currently generally used as interior materials for automobiles, vehicles, ships and the like. For example, as the skin material, polyester non-woven fabric, brushed knit, fabric, suede-like synthetic leather, vinyl chloride (polyvinyl chloride) leather, polyurethane leather, polypropylene thermoplastic elastomer, or urethane foam, foamed to these materials to provide cushioning properties. Examples include those obtained by adhering polypropylene, foamed polyethylene, foamed polyvinylidene, and the like. On the other hand, examples of the substrate material include resin felt, glass fiber-containing phenol resin plate, corrugated board, polypropylene honeycomb, polystyrene foam, or a material obtained by laminating a non-woven fabric to these materials.

When the resin composition of the present invention is used to manufacture interior materials for automobiles and the like, various molding methods can be adopted. For example, a substrate material is heated to a predetermined temperature, set in a vacuum forming machine, the above resin composition formed into a film by inflation molding, T-die molding or the like is placed thereon, and then the skin is heated to a predetermined temperature in advance. A method of stacking materials and vacuum-pressing; a method of sandwiching the above film between a skin material and a substrate material and hot pressing; a laminate material obtained by coating the skin material with the resin composition of the present invention by extrusion molding and a substrate material. Method of hot pressing with a hot press or hot roll; powdering the resin composition of the present invention, sprinkling it on a substrate material placed on a hot press, and hot pressing a skin material thereon; Examples include a method of previously laminating the above film on the adhesive side with a hot roll, and then thermocompression bonding with a hot press or a hot roll.

[0016]

EXAMPLES Further, the present invention will be specifically described with reference to Examples, Comparative Examples and Application Examples. Example 1 An ethylene-maleic anhydride-methyl methacrylate terpolymer was used as the ethylene-based multi-component copolymer (A). This ternary copolymer utilizes equipment of a high-pressure low-density polyethylene plant, and has a polymerization temperature of 240 ° C and a polymerization pressure of 1,9.
It was manufactured under the conditions of 00 kg / cm ² . The MFR of this terpolymer (JIS-K7210, 190 ° C., hereinafter, MF
R uses this condition for all. ) Was 15 g / 10 minutes, the proportion of units derived from maleic anhydride was 2.2% by weight, and the proportion of units derived from methyl methacrylate was 16% by weight. The composition of the comonomer was determined by infrared absorption spectrum. On the other hand, as the metal salt (B) of the organic carboxylic acid, the ionomer (a) was used. This ionomer (a) was obtained by adding a copolymer of ethylene and methacrylic acid (methacrylic acid content: 20% by weight) to water / methanol = 1/1.
Of the unit derived from methacrylic acid in the copolymer, treated with sodium acetate at 50 ° C for 2 hours in
It is a partially neutralized product obtained by neutralizing mol%. The weight ratio ((A) / (B)) of the above two components is set to 85/15, and this (A)
After dry blending 0.2% by weight of magnesium silicate and 0.2% by weight of erucic acid amide as an additive with respect to the total amount of the components and (B) by a tumbler, using a 37 mmφ co-directional twin-screw extruder at 180 ° C. The mixture was melt-kneaded to obtain resin composition pellets. The contents of this formulation are shown in Table 1.

Comparative Example 1 A resin composition pellet was obtained in the same manner as in Example 1 except that the ionomer was not added. The contents of this formulation are shown in Table 1.

Comparative Example 2 The procedure of Example 1 was repeated except that an ethylene-methyl methacrylate binary copolymer was used as the component (A),
Pellets of the resin composition were obtained. The contents of this formulation are shown in Table 1.

Examples 2 to 7 Various ethylene-based multi-component copolymers (A) were produced according to Example 1, and various kinds of metal salts of organic carboxylic acids (B) were also prepared. Various resin compositions shown as Examples 2 to 7 were prepared. The content of the formulation is shown in Table 1.

[0020]

[Table 1]

[0021]

[Table 2]

Application Example 1 The pellets obtained in Example 1 were formed into a film having a thickness of 75 μm with an inflation film molding machine having an extruder of 45 mmφ, and a cylindrical film was cut to obtain 4
A 0 cm wide film was obtained. Using this film as an adhesive layer, a skin material and a substrate material, which are actually used as interior materials for automobiles, were adhered, and the adhesiveness was tested. The skin material is polyethylene terephthalate (PET) non-woven fabric,
Resin felt (RF) was used as the substrate material. Adhesion was performed by sandwiching a skin material, the above film, and a substrate material in this order from the top in a hot press set at 110 ° C. for the upper plate and 140 ° C. for the lower plate, and pressure-bonding them under conditions of a substantial surface pressure of 2 kg / cm ² for 30 seconds. The press size of the board material is 150m according to JIS-K6829.
It was set to m × 175 mm. After bonding, 23 ℃, relative humidity 50
% For 24 hours, cut into a 25 mm wide test piece, and use a tensile tester at room temperature (23 ° C.) and high temperature (8
A 180 ° peel test at 5 ° C was performed. As a general rule, the adhesive strength (g / 25 mm) at the time of peeling was measured. However, when the skin material or the substrate material was broken before peeling, the strength at break was measured. In addition, the test piece that was partially peeled 10
A peeling distance (mm) was measured when a load of 0 g was suspended and the sample was allowed to stand in an atmosphere of 80 ° C. for 24 hours, and used as a measure of heat-resistant creep resistance. The adhesive strength value is an average value of 5 test pieces (maximum, minimum 2 point cut), and the heat creep resistance is an average value of 3 test pieces. The results are shown in Table 2.

Application Examples 2 to 4 As shown in Table 2, the same operation as in Application Example 1 was performed except that the kinds of the resin composition for the adhesive layer, the skin material and the substrate material were changed. The results are shown in Table 2.

Application Example 5 Using the film obtained in Application Example 1 as a skin material, 0.2
Adhesiveness was tested using 2 mm foamed polypropylene (PP) with mm vinyl chloride leather attached and resin felt (RF) as the substrate material. For the adhesion, first, the outer skin and the film were sandwiched by a Teflon coat roll heated to 130 ° C., and a heat roll laminating process was performed at a speed of 5 m / min to bond them. Next, the substrate material was heated to 80 ° C. for 3 minutes and the skin was heated to 120 ° C. and bonded by a vacuum bonding method. The results are shown in Table 2.

Application Examples 6 to 8 As shown in Table 2, the same operation as in Application Example 5 was carried out except that the kinds of the resin composition for the adhesive layer, the skin material and the substrate material were changed. The results are shown in Table 2.

Reference Examples 1 to 4 Films were produced from the pellets obtained in Comparative Example 1 in the same manner as in Application Example 1. Using this film as an adhesive layer, as shown in Table 2, the types of skin material and substrate material were changed, and the same operation as in Application Example 1 was performed. The results are shown in Table 2.

Reference Examples 5-8 Films were produced from the pellets obtained in Comparative Example 2 in the same manner as in Application Example 1. Using this film as an adhesive layer, as shown in Table 2, the types of skin material and substrate material were changed, and the same operation as in Application Example 1 was performed. The results are shown in Table 2.

The results of the above tests are shown in Table 2. Example 1
In the case of the resin compositions of Nos. 7 to 7 (Application Examples 1 to 8), both the adhesive strength at room temperature and high temperature and the heat-resistant creep resistance were good. Also, the bonding work was very easy and hygienic, and the workability was also good. That is, the resin composition of the present invention can be widely used as an adhesive layer of various multilayer laminated structures, particularly an adhesive layer of a multilayer laminated structure used as an interior material for automobiles and the like. Furthermore, the resin composition of the present invention can be used without sticking a pattern peculiar to vinyl chloride leather even when adhering a skin material on which a vinyl chloride leather (leather of vinyl chloride resin) is adhered (Application Examples 5 to 8). It can be used extensively without damaging the material. On the other hand, in the case of the resin composition of Comparative Example 1 (Reference Examples 1 to 4), the adhesive strength was relatively good, but the heat-resistant creep property was significantly inferior, and it was used as an interior material for automobiles and the like. Is a big problem. Further, in the case of the resin composition of Comparative Example 2 (Reference Examples 5 to 8), before the measurement of the heat creep resistance,
The adhesive strength was completely insufficient, and it was not possible to obtain a multi-layer laminated structure that could withstand practical use.

[0029]

[Table 3]

[0030]

[Table 4]

[0031]

[Table 5]

[0032]

As described above, the resin composition of the present invention is
It has excellent adhesiveness at room temperature and high temperature, and can be suitably used as an adhesive layer for various multilayer laminated structures. In particular, since it can be bonded at a low temperature without damaging the skin material and has excellent heat-resistant creep resistance, it can be suitably used as an interior material for automobiles and the like. Moreover, since it is not necessary to use an organic solvent at the time of adhesion and the working process is simple, there is no problem in use. Further, since it can be manufactured using the same method and equipment as those of the conventional adhesive resin, it can be manufactured relatively inexpensively and easily. Therefore, the resin composition of the present invention is effectively used as an adhesive layer of a multilayer laminated structure.

 ─────────────────────────────────────────────────── ─── Continuation of the front page (72) Inventor Hirotaka Takoshi 2nd Nakanosu, Oita City, Oita Prefecture Showa Denko Oita Laboratory

Claims (1)

[Claims] 1. A multi-component copolymer comprising (A) ethylene, a radical-polymerizable acid anhydride and a radical-polymerizable comonomer other than the above, which is a radical-polymerizable acid anhydride in the ethylene-based multi-component copolymer. The ratio of derived units is 0.1-5
An ethylene-based multi-component copolymer having a weight percentage of 3 to 50% by weight of units derived from other radically polymerizable comonomers, (B) an organic carboxylic acid, and Group IA, II of the periodic table.
A resin composition comprising a salt with a metal belonging to Group A or Group IIB.