JPS61181882A - Adhesive composition - Google Patents

Abstract

PURPOSE:To provide the titled composition capable of providing an excellent adhesion between smooth or porous base materials made of PP, PS, PVC, etc., which comprises a modified copolymer prepared by subjecting a specific ethylene-alpha-olefin copolymer etc. to graft modification using an unsaturated carboxylic acid (or its derivatives). CONSTITUTION:25-75wt% of an ethylene-alpha-olefin copolymer (A) having a high or low crystallinity (MI: 0.1-1,000) of which the ethylene content is 20-50mol% and the alpha-olefin content is 80-50mol%, 75-25wt% of an ethylene- vinyl ester copolymer and/or ethylene-unsaturated carboxylate copolymer (B) and an unsaturated carboxylic acid (or its derivatives) (C) [e.g. maleic acid (anhydride)] are simultaneously melted and kneaded in the presence of a radical forming agent such as an organic peroxide to react them with each other, thereby to obtain a modified copolymer of which the graft rate with respect to the component (C) is 0.01-5wt% 100pts.wt. of the modified copolymer is optionally mixed with 25wt% or less of terpene (-phenol) resin as a tackifier, a modifier and various additives.

Description

DETAILED DESCRIPTION OF THE INVENTION [Industrial Field of Application] The present invention relates to adhesive compositions. More specifically, the present invention relates to an adhesive composition that exhibits excellent adhesion between smooth substrates and porous substrates of the same or different types.

[Prior Art] Recently, synthetic resin bases such as polyethylene, ionomer resin, polypropylene, ethylene-vinyl alcohol copolymer, polyester, and polyamide have been used in the fields of automobiles, electrical parts, building materials, sports and other leisure goods, and packaging materials. laminates of metal base materials such as wood, aluminum plates, and steel plates, smooth base materials such as natural and synthetic leather, or laminates of these smooth base materials and porous base materials such as paper, cloth, wood, and synthetic resin foam. A large amount of laminates are used.

Among these laminates, heat-sensitive adhesives are still used when bonding base materials that are relatively easy to adhere to.
When using the above-mentioned smooth substrates, it is difficult to find heat-sensitive adhesives that have sufficient adhesive strength to bond them, so it is necessary to surface-treat the substrate and use a solvent-based adhesive. Currently, they are glued together.

Regarding the performance of heat-sensitive adhesives, various other properties are required in addition to adhesive properties. Mild bonding conditions such as temperature, pressure, and time are required for purposes such as preventing odor generation. On top of that,
The performance requirements for adhesives, such as heat resistance and durability, are diversifying due to their application in various industrial fields.

The heat-sensitive adhesives currently used industrially include α,
Examples include polyolefins graft-modified with β-unsaturated carboxylic acids or their acid anhydrides, but these are not effective adhesives for smooth substrates, especially synthetic resin films.

On the other hand, since the development of adhesives with excellent adhesion to smooth substrates is industrially important, adhesive compositions are disclosed in published patents9. discloses a resin composition comprising a low-crystalline ethylene-α-olefin copolymer and an ethylene-vinyl acetate copolymer, at least one of which is graft-modified with an unsaturated carboxylic acid or its acid anhydride. Furthermore, in JP-A-57-153064, one or two selected from epoxy groups, carboxylic acid groups, and carboxylic acid anhydride groups are disclosed.
Ethylene copolymer (A) containing more than one type of functional group and (
An adhesive resin composition comprising a meth)glycolate copolymer (B) or an ethylene polymer (C) other than the above-mentioned ethylene copolymer (A) is described.

However, as shown in the comparative examples below, when these compositions were evaluated with reference to their specifications, especially the detailed description section of 1 invention and the examples, it was found that these compositions do not necessarily have the adhesive strength currently required in the market. I couldn't be more satisfied.

[Problems to be Solved by the Invention] In view of the current situation, the present inventors have developed a method that has excellent processability in coating work to the base material, good adhesion to the base material even under mild bonding conditions, and a material that can be laminated. As a result of intensive research in search of an adhesive that improves the heat resistance of objects, the inventors have discovered that an adhesive composition consisting of the following components can solve this problem.

[Means for Solving the Problems] and [Operation] That is, the present invention provides a low crystalline or amorphous ethylene-α-olefin copolymer with an ethylene content of 20 to 50 mol% and an α-olefin content of 50 to 80 mol%. The present invention relates to an adhesive composition containing a modified copolymer obtained by graft-modifying a polymer with an unsaturated carboxylic acid or a derivative thereof. This composition can of course contain various olefin polymers and tackifier resins described below.

The present invention also provides (A) an ethylene content of 20 to 50%, α-
Low crystalline or non-crystalline ethylene-α-olefin copolymer with olefin content of 50 to 80 mol%, 25 to 75 g%, and (B) ethylene-vinyl ester copolymer and/or ethylene-unsaturated carboxylic acid ester In an adhesive composition consisting of 75 to 25% by weight of copolymer, 1
The present invention is an adhesive composition in which at least one type of polymeric acid component is modified with unsaturated carboxylic acid or a derivative thereof.

The ethylene-α-olefin copolymer used in the present invention has an ethylene content of 20 to 50 mol % and a melt index of 0.1 to 100 θ, preferably 30 to 45 mol %. As the α-olefin, propylene is used.

Border 7-1. Pentene-1, Hexene-1, Octene-1
Among them, propylene, butene-1, and especially propylene are preferable.
- The olefin content is between 50 and 80 mol%, preferably between 55 and 70 mol%. Ethylene with an α-olefin content of less than 50 mol% or more than 80 mol%
In adhesive compositions containing an α-olefin copolymer as one of the polymer components, polyolefins, particularly polypropylene,
It does not exhibit high adhesion to smooth materials such as ionomer resins, making it unsuitable as a base polymer for adhesive compositions.

In the present invention, as the pace polymer, the above-mentioned ethylene-α-olefin copolymer alone may be used, or other olefin polymers may be used.

For example, polyethylene, polypropylene, polybutene
A suitable combination from the viewpoint of compatibility etc., which may be used in combination with 1 etc., is an ethylene-a-olefin copolymer and an ethylene vinyl ester copolymer and/or an ethylene-unsaturated carboxylic acid ester copolymer. It is a combination with merging.

Examples of the ethylene-vinyl ester copolymer used in the present invention include ethylene-vinyl acetate copolymer, ethylene-vinyl acetate copolymer, and ethylene-vinyl acetate copolymer.
Examples include vinyl propionate copolymer.

Among these, ethylene-vinyl acetate copolymers are preferred, and particularly preferred are ethylene-vinyl acetate copolymers having a vinyl acetate content of 2 to 15 mol % and a melt index of 1 to 1,000.

In addition, the ethylene-unsaturated carboxylic acid ester copolymer used in the present invention includes ethylene-methyl (meth)acrylate copolymer, ethylene-ethyl (meth)acrylate copolymer, and ethylene-(meth)acrylic acid copolymer. Examples include butyl copolymer, ethylene-(meth)acrylic@2-ethylhexyl copolymer, and the like. Among these, ethylene-methyl (meth)acrylate or ethylene copolymer is preferred, especially methyl (meth)acrylate or ethyl (meth)acrylate content of 2 to 15 mol%, melt index of 1 to 1
ooo ethylene-methyl (meth)acrylate or ethyl copolymer is preferred I/-0 Next, in the second embodiment of the present invention, an ethylene-α-olefin copolymer, an ethylene-vinyl ester copolymer and The ratio of the ethylene-unsaturated carboxylic acid ester copolymer is 25% in the adhesive composition consisting of both.
75% by weight.

In particular, a range of 30 to 70% by weight is preferred. If the blending ratio of the ethylene-α-olefin copolymer is less than 25% by weight, the adhesive force to the substrate will decrease, and if it is more than 75% by weight, the tackiness will increase, the cohesive force will decrease, and the workability will deteriorate. This is not preferable, so the blending ratio of the ethylene-α-olefin copolymer needs to be in the range of 25 to 75% by weight.

In the present invention, at least one of a polymer component consisting of an ethylene-α-olefin copolymer alone or the copolymer and an ethylene-vinyl ester copolymer and/or an ethylene-furyurethane carboxylic acid ester copolymer is used. , it is necessary to graft modification with carboxylic acid or its acid anhydride.

Examples of the graft monomer in this case include acrylic acid, methacrylic acid, fumaric acid, crotonic acid, itaconic acid, citraconic acid, maleic anhydride, itaconic anhydride, citraconic anhydride, and maleic acid monoethyl ester. can. Among these, it is most preferred to use maleic acid or maleic anhydride.

In the graft modification, at least one of the unsaturated carboxylic acids or derivatives thereof is added to (A) the copolymer alone in the presence of a radical generator such as an organic peroxide.

(B) Copolymer alone, or (A) and (B)
This is carried out by reacting a mixture of copolymers by a known method such as a solution method or a melt method.

What should be noted here is (A) component ethylene-α-olefin copolymer, (B) component ethylene-vinyl ester copolymer and/or ethylene-unsaturated carboxylic acid ester copolymer and unsaturated carboxylic acid ester copolymer. When a polymer and an unsaturated carboxylic acid or its derivative are simultaneously melt-kneaded and reacted in the presence of an organic peroxide, an adhesive composition with extremely high adhesive performance can be obtained, although the mechanism of action is unclear. That's true. Therefore, in order to produce the adhesive composition of the present invention, a method may be adopted in which component (A), component (B), and an unsaturated carboxylic acid or a derivative thereof are simultaneously melt-kneaded in the presence of an organic peroxide. preferable.

The amount of the unsaturated carboxylic acid or its derivative is about 0.01 to 5% by weight in the resulting graft modified product (composition).

The graft reaction is carried out in such a proportion that it accounts for If the amount of grafting is less than this, the desired adhesive strength cannot be obtained, whereas if it exceeds about 5% by weight, the tendency for the adhesive strength to increase will reach almost saturation, so generally, the amount of grafting less than this is sufficient. In addition, it is preferable that it has a melt flow rate of about 0.1 to 1.000 g/10 minutes. If the melt flow rate is less than this value, the fluidity is low and it is not suitable for bonding at low temperature and low pressure. On the other hand, if it exceeds this value, the cohesive force will decrease and the adhesive force will also decrease.

The adhesive composition of the present invention generally has good adhesive properties on its own, but it can further improve adhesive performance when bonding under milder bonding conditions or when bonding to difficult-to-adhesive substrates. It is also possible to add less than 25 parts by weight of a tackifying resin to 100 parts by weight of the adhesive composition for the purpose of increasing the adhesive composition. Examples of tackifier resins that can be used in this case include rosin and its derivatives, terpene resins, terpene-phenol resins, aromatic, aliphatic, alicyclic or copolymer petroleum resins, coumaron-indene resins, and styrene resins. Terpene resins, terpene-phenol resins, aliphatic petroleum resins, and alicyclic and copolymer petroleum resins thereof are particularly preferred from the viewpoint of compatibility with monopolymer plants and adhesive properties.

In addition to the above-mentioned tackifier resin, the adhesive composition of the present invention may contain various modifiers and additives, as necessary, within a range that does not impair its performance. For example, paraffin wax, buiclocrystalline wax, etc. Petroleum waxes such as, synthetic waxes such as polyethylene wax and polypropylene wax, liquid polybutene, dioctyl phthalate,
Examples include plasticizers such as dibutyl phthalate, phenolic or bisphenol antioxidants, ultraviolet absorbers, fillers such as calcium carbonate, talc, and glass fibers, known lubricants, roll release agents, and antiblocking agents. can.

The adhesive composition of the present invention is prepared by triblending the components simultaneously or sequentially. Tri-blend is made using a Henschel mixer or tumbler.
Mixing may be carried out using various blenders such as mixers and Ripon blenders, and in the case of melt blending, mixing may be carried out using a single screw extruder, twin screw extruder, Banbury mixer, etc., and there is no particular restriction on the mixing order.

Substrates to which the adhesive composition of the present invention can be effectively applied include, for example, polyethylene, polypropylene, polystyrene, vinyl chloride resin, ethylene-vinyl alcohol copolymer, polyester, polyamide, polyvinylidene chloride, polyacrylonitrile, and polycarbonate. , ethylene-vinyl acetate copolymer, ethylene-(meth)acrylic acid ester copolymer, ethylene-(meth)acrylic acid copolymer, ionomer resin and other synthetic resin films, sheets and other molded products, aluminum foil, copper metals such as foil,
Examples include natural and synthetic leathers, paper, woven and non-woven fabrics, wood, synthetic resin foams, etc., and are effective for laminating one or more base materials selected from these base materials.

Lamination of these base materials with adhesive compositions is performed, for example, by the following method.

(1) Heat fusion method A method in which an adhesive composition film formed by an inflatable polymerization method, T-Guy method, etc. is sandwiched between base materials and bonded under heat, or at least one of the base materials is coated with a coextrusion method or extrusion coating. A method in which an adhesive composition is laminated in advance by a method such as a method, and then bonded to the other base material by thermocompression bonding.

(2) Sandwich lamination method A method of laminating substrates through a molten film of an adhesive composition using the T-Guy method or the like.

(3) Co-extrusion method A method in which all constituent layers, including the adhesive composition, are adhesively laminated by extrusion molding when the base material can be extruded.

(4) A hot-melt adhesive prepared by adding wax, tackifying resin, etc. to the hot-melt adhesive composition, if necessary, is applied to the base material using a hot-melt gun or the like, and bonded by pressure. Method.

The structure of the present invention has been described in detail above, and the first feature of the present invention is the discovery that an ethylene-α-olefin copolymer with a specific comonomer content has excellent adhesive performance.
The point is that this is used as a component of an adhesive composition. The second characteristic is that it overcomes the disadvantages of the ethylene-α-olefin copolymer: 1) increases cohesive force, 2) prevents adhesion and blocking of adhesive compositions and their coated products, and 2) facilitates extrusion coating work on substrates. Ethylene-vinyl ester copolymer and ethylene/vinyl ester copolymer are used as polymers that improve processing properties, such as the maximum take-up speed, and (1) increase the heat resistance of the laminate without impairing the adhesive performance of the ethylene-α-olefin copolymer. - It was discovered that an unsaturated carboxylic acid ester copolymer was effective, and it was used as the second component of an adhesive composition. As a result, the third characteristic is that (A) component ethylene-
α-olefin copolymer is organic peroxide decomposition type, CB)
Since the copolymers mainly composed of ethylene, such as the component ethylene-vinyl ester copolymer or the ethylene-unsaturated carboxylic acid ester copolymer, are organic peroxide crosslinked type (A
), (B) When both components and an unsaturated carboxylic acid or its derivative are simultaneously melt-kneaded and reacted in the presence of an organic peroxide, there is little decrease in the melt index, which is important for adhesive properties, during the reaction. Although the mechanism is not clear, adhesive compositions with extremely high adhesive performance can now be obtained. The fourth feature is (B)
Since the component ethylene-vinyl ester copolymer and/or ethylene-unsaturated carboxylic acid ester copolymer has excellent compatibility with the tackifying resin, it is easy to add the tackifying resin to the adhesive composition. This means that it has become possible to further improve the adhesive performance of the ethylene-α-olefin copolymer component (A).

[Examples] Next, the present invention will be explained in detail using examples. The compositions prepared in each Example and Comparative Example were evaluated as follows.

(1) Method for evaluating adhesive strength of adhesive composition: (a) Heat-sealing method The adhesive composition was heated and melted at 160° C., and a sheet with a thickness of 200 ILm was prepared using a hot press. This adhesive sheet was sandwiched between the base materials, and a heat sealer was used to seal with a sealing width of 25 mm, a sealing temperature of 150°C (temperature of the top and bottom surfaces of the seal bar), a sealing pressure of 3 kg/cm2 G, and a sealing time of 5 seconds. After heat-sealing under the following conditions, the sample was cut into a width of 251 mm, and the T-peel strength of this sample was measured using an Instron tester at a tensile rate of 300 cm/sin and a temperature of 23°C.

(b) Extrusion coating method Adhesive composition is coated with 65μ/L extrusion coating machine (L/L).
Mouth=24. The adhesive layer was coated to a thickness of 100 gm using a roll surface length of 710 m/layer under conditions of a resin temperature of 170° C. and a line speed of 20 m/inch.

This laminate is bonded to the aluminum plate or synthetic leather using a heat sealer, with a sealing width of 25 layers and a sealing temperature of 150cm.
°C (temperature of the top and bottom surfaces of the seal bar), sealing pressure 3K
After heat-sealing under the conditions of g/cm2 and a sealing time of 5 seconds, the sample was cut into a width of 25 cm, and the sample was tested using an Instron tester at a tensile rate of 300 cm/sin and a temperature of 23 cm.
T-peel strength was measured under conditions of .degree.

The base material for these adhesive strength measurements was a polypropylene film (PP: an inflatable film made from Mitsui Petrochemical's polyfluoroethylene, 200 g thick).
m), soft aluminum plate (Al: thickness 200ILm)
Cotton cloth (Cotton-9A manufactured by Achilles) and synthetic leather (Cordray-32941-1110-KO5 manufactured by Kijinsha) were used.

(2) Heat resistance (shear adhesive failure temperature): Method for measuring adhesive strength (a) In the heat sealing method,
A 200 m sheet of the adhesive composition was sandwiched between kraft papers and heat-sealed under the same conditions, then a 25 m wide sample was prepared, and a load of 1 kg was applied to the sample at 0.3 °C/min. The temperature at which the load fell when the temperature was raised at a certain rate was measured and used as a measure of heat resistance.

(3) Non-adhesiveness: The tackiness of the surface of the 200 parts m sheet of the adhesive composition was evaluated by finger tack at 23°C as follows.

0 If there is no tack Δ If there is some tack Maximum take-up speed (m/■in) that increases and does not break
) was used as a guideline for processability during melting.

Example 1. la and 1c propylene-ethylene copolymer (propylene content 60 mol%, melt flow rate) 1.5. (hereinafter abbreviated as PER-1), 100 parts (weight, same below), maleic anhydride 1
．． 5 parts and 30.2 parts of 2,5-dimethyl-2,5-bis(t-butylperoxy)hexyne were blended in a Henschel mixer, and this mixture was transferred to a 301-inch extruder (L/D-32 , using a Dalmage screw) at a resin temperature of 260°C to obtain a maleic anhydride-modified propylene-ethylene copolymer (hereinafter MAH-PER-1).
A pellet was obtained. The melt flow rate was 25 and the maleic anhydride grafting rate was 1.1% by weight (Example 1).
MAR-PER-1100 was melt-blended with 20 parts of alicyclic petroleum resin (Arayo Kagaku, Alcon P100) to 1100 parts of E-1 to obtain pellets (Example 1b).
and unmodified ethylene-ethyl acrylate copolymer (Evaflex A-704 manufactured by DuPont Mitsui Polychemicals,
EA content 27% by weight, melt flow rate) 210. 100 parts of EEA-1 (hereinafter abbreviated as EEA-1) were melt-blended using the same extruder at a resin temperature of 170°C to obtain pellets with a melt flow rate of 65. The adhesive strength by heat sealing method, shear adhesive failure temperature, and workability of each adhesive composition thus prepared were measured, and the results are shown in the table.

Example 2 In Example 1c, unmodified EEA-2 (manufactured by DuPont Mitsui Polychemicals, Evaflex A-703, EA content 25% by weight, melt flow rate 6) was used instead of unmodified EEA-1. .

The melt flow rate of the obtained pellets was 10.

Example 3 In Example 1c, instead of PER-1, EEA-
A maleic anhydride-modified ethylene ethyl acrylate copolymer (hereinafter referred to as MA) (abbreviated as I-EEA-1) was obtained using Example 1. The melt flow rate was 90, and the maleic anhydride grafting rate was 1.1% by weight. 1100 parts of MAR-EEA thus obtained and unmodified PER
-1100 parts were melt blended in the same manner as in Example 1c to obtain pellets with a melt flow rate of 7.

Example 4 1100 parts of MAR-EEA obtained in Example 1 and 1100 parts of MAR-EEA obtained in Example 3 were added to Example 1.
Melt blending was performed in the same manner as above to obtain pellets with a melt flow rate of 55.

Example 5 In Example 1c, in place of unmodified ethylene-ethyl acrylate, ethylene-vinyl acetate copolymer (manufactured by DuPont Mitsui Polychemicals, Evaflex #210.V) was used.
A28% by weight, melt flow rate) 400; hereinafter EVA
-1) to obtain adhesive composition pellets. This melt flow rate was 85.

Comparative Example 1 In Example 2, only 1MAR-EEA-1 was used.

Comparative Example 2 Pellets were obtained by melt blending 1100 parts of unmodified PER and 1100 parts of unmodified EEA under the same conditions as in Example 1c. The melt flow rate of this pellet was 20.

Comparative Example 3 In Comparative Example 2, melt blending was performed using unmodified EVA-1 instead of unmodified EEA-1. The melt flow rate of this pellet was 50. Comparative Example 4 In Example 1, EPR-1 with a high ethylene content (80 mol% ethylene, melt flow rate 4) was used instead of PER-1. Maleic anhydride-modified ethylene-propylene copolymer (hereinafter abbreviated as MAR-EPR-1) pellets were obtained.

The maleic anhydride grafting rate of this pellet was 1.0% by weight, and the melt flow rate was 2.7. Example 1c 1100 parts of MAR-EPR thus obtained
Melt blend under the same conditions as above, melt flow rate 5
0 pellets were obtained.

Comparative Example 5 Ethylene-methacrylic acid copolymer (Mitsui DuPont Polychemical Co., Ltd., New Cool 41G, acid content 9% by weight, Melt Flowray) 10 or less (abbreviated as EMMA-1)
50 parts were melt blended using 215 parts of EEA and 135 parts of EVA under conditions similar to Example 1c,
Pellets with a melt flow rate of 35 were obtained.

Example 6 PER-150 parts, maleic anhydride 1.5 parts and 2.
5-bis(t-butylperoxy)hexane-30,2
of the maleic anhydride-modified adhesive composition (
MA)! -CPER/EEA)-1) pellets were obtained. The melt flow rate of this composition was 8, and the maleic anhydride grafting ratio was 1.2.

Example 7 Example 6 except for PER-1100 parts and EEA-140 parts
Pellets of a maleic anhydride-modified polyolefin polymer composition (abbreviated as MAR-CPER/EEA)-2) were obtained in the same manner as above. The melt flow rate of this composition was 1O, and the maleic anhydride grafting ratio was 1.2.

Example 8 The same procedure as in Example 7 was carried out except that EVA-1 was used instead of EEA-1, and a maleic anhydride-modified polyolefin polymer composition (MA) I-CPER/EVA) was prepared.
-1) pellets were obtained. The melt flow rate of this composition was 20, and the maleic anhydride grafting rate was 1.
．． It was 2.

The adhesive strength, shear bond failure temperature, and processability of the adhesive compositions prepared in Examples 2 to 8 and Comparative Examples 1 to 6 were measured by heat sealing, respectively. The results are shown in the table.

Example 9 100 parts of melt blend pellets of MAR-PER-150% and EEA-250 parts obtained in Example 2,
Part of alicyclic petroleum resin (Alcon P100 manufactured by Arayo Kagaku), 0.1 part of erucic acid amide (Neutron S manufactured by Nippon Kumiyaku Co., Ltd.) and polyethylene glycol (PEG-40 manufactured by Wako Tsumugi Pharmaceutical Co., Ltd.)
00) was melt-blended using an extruder to obtain pellets with a melt flow rate of 20.

Example 10 MAI(-(MAR-(PE
R/EE Todoroki) - 1100 parts, alicyclic petroleum resin (Esso Chemical Niscollet 5300) 20 parts, engineered pericamide 0.
1 part and 0.1 part of polyethylene glycol were melt blended using an extruder to obtain a pellet with a melt flow rate of 1O.

Comparative Example 7 In Example 9, melt blending was performed using unmodified PER-1 instead of MAR-PER-1 to obtain pellets with a melt flow rate of 3.5.

As described above, the adhesive strength and processability of the adhesive compositions prepared in Example 9.10 and Comparative Example 7 by extrusion coating method were measured. The results are shown in the table.

Claims (7)

[Claims] (1) By graft-modifying a low crystalline or non-crystalline ethylene-α-olefin copolymer with an ethylene content of 20 to 50 mol% and an α-olefin content of 50 to 80 mol% with an unsaturated carboxylic acid or a derivative thereof. An adhesive composition containing the obtained modified copolymer. (2) The composition according to claim 1, wherein the grafting rate of the unsaturated carboxylic acid or its derivative in the modified copolymer is 0.01 to 5% by weight. (3) The composition according to claim 1, which contains a tackifier resin consisting of at least one of a terpene resin, a terpene-phenol resin, an aliphatic petroleum resin, and a copolymer petroleum resin. (4) (A) Low crystalline or non-crystalline ethylene-α-olefin copolymer with an ethylene content of 20 to 50 mol% and an α-olefin content of 50 to 80 mol%, and (B) ethylene- Vinyl ester copolymer and/or
or ethylene-unsaturated carboxylic acid ester copolymer 7
An adhesive composition comprising 5 to 25% by weight, wherein at least one of the polymer components is modified with an unsaturated carboxylic acid or a derivative thereof. (5) The adhesive composition according to claim 4, wherein the low-crystalline or non-crystalline ethylene-α-olefin copolymer is an ethylene-propylene copolymer. (6) The adhesive composition according to claim 4 or 5, wherein the ethylene-unsaturated carboxylic acid ester copolymer is an acrylic acid or methacrylic acid aliphatic alkyl ester. (7) The adhesive composition according to claim 4, which is produced by simultaneous melt mixing of component (A), component (B), unsaturated carboxylic acid or its derivative, and organic peroxide.