JPS619477A - Bondable composition - Google Patents

Abstract

PURPOSE:To provide a hot-melt adhesive having excellent adhesion and heat resistance, by melt-mixing a mixture of a peroxide-decomposable non-crystalline olefin copolymer and a peroxide-decomposable crystalline olefin polymer, an unsaturated carboxylic acid and an org. peroxide. CONSTITUTION:90-50wt% peroxide-decomposable non- or low-crystalline olefin copolymer (e.g. propylene/ethylene copolymer or butene-1/ethylene copolymer) is mixed with 10-50wt% peroxide-decomposable crystalline olefin polymer (e.g. isotactic polyproplene or polybutene-1). 100pts.wt. said polymer mixture, 0.01- 5pts.wt. unsaturated carboxylic acid (anhydride) (e.g. acrylic acid or maleic anhydride) and 0.01-3pts.wt. org. peroxide (e.g. dicumyl peroxide) are melt- mixed together to obtain the desired bondable compsn.

Description

DETAILED DESCRIPTION OF THE INVENTION [Field of Industrial Application] The present invention relates to adhesive compositions. More specifically, the present invention relates to an adhesive composition that can be effectively used as a hot melt adhesive for various substrates.

[Conventional technology]

Generally, polyolefin, polyester, polyamide,
Substrates made of aluminum, steel, leather, etc., especially smooth substrates, can be used to create packaging materials, industrial materials, and automobile parts by laminating these substrates with each other or with porous materials such as paper, wood, and synthetic resin foam. It is used in i< fields such as construction parts, household goods, medical supplies, and sporting goods.

Adhesives are used when laminating these various products, but the physical properties required of these adhesives are diverse.
Although they differ depending on the field of application, two of these physical properties that are commonly required are adhesive strength and heat resistance. Of the many adhesives currently in use, only solvent-based adhesives simultaneously and fully satisfy these requirements, such as tetraloprene, nitrile, etc.
Solvent-based adhesives such as epoxy-based adhesives have been applied to substrates whose surfaces have been previously treated with chemicals, plasma, etc. However, when such solvent-based adhesives are used, they not only require drying and solvent recovery steps, but also always pose problems such as environmental deterioration due to solvent vapor and the risk of fire.

Therefore, with hot melt adhesives that do not have such problems,
It is desired to develop a material with excellent adhesive strength and heat resistance.

As hot-melt adhesives, adhesives consisting of components such as ethylene-vinyl acetate copolymer, tackifier, and wax have been widely used. Adhesives are unsatisfactory both in terms of adhesive strength and heat resistance, especially when applied to smooth substrates.

The adhesive composition, which can be applied to smooth substrates, is composed of a low-crystalline ethylene-α-olefin copolymer and an ethylene-vinyl acetate copolymer, and at least one of them is substituted with an unsaturated carboxylic acid or an unsaturated carboxylic acid. A composition graft-modified with an acid anhydride has been proposed (Japanese Unexamined Patent Publication No. 137-1989).
Publication No. 18). Although this adhesive composition does show improved adhesion to smooth substrates compared to the hot-melt adhesive based on the ethylene-vinyl acetate copolymer described above, the improvement effect is still not sufficient. Furthermore, no improvement effect on heat resistance was observed.

In addition, a hot-melt adhesive has been proposed in which a mixture of ethylene-propylene copolymer rubber and crystalline or non-crystalline polypropylene is melt-mixed and reacted in the presence of an organic peroxide to reduce its viscosity. I'm here (Unexamined Japanese Patent Publication No. 5)
5-48236), and although this adhesive may have improved heat resistance, it was confirmed that it had poor adhesive strength to smooth substrates.

[Problem that the invention seeks to solve]

In view of the current situation, the present inventors conducted various studies in search of a hot-melt adhesive that could be sufficiently applied to smooth substrates and also impart sufficient adhesive strength and heat resistance to the adhesive, and as a result, developed the following. It has been found that an adhesive composition comprising a co-melted mixture of components solves this problem.

[Means for Solving the Problem] and [Operation] Accordingly, the present invention relates to an adhesive composition, which comprises:
(a) Approximately 90-50% by weight of a peroxide-decomposed amorphous to low-crystalline olefin copolymer; and (b) approximately 10-50% by weight of a peroxide-decomposed crystalline olefin-based copolymer.
a co-melted mixture of (C) an unsaturated, carboxylic acid or its acid anhydride, and (d) an organic peroxide; or (a) a peroxide-decomposed amorphous to low-crystalline olefin system. About 90-50% by weight of copolymer and (b
) peroxide decomposition type crystalline olefin polymer about 10~
50% by weight, at least one of these components (a) and (b) is graft-modified with CO) an unsaturated carboxylic acid or an acid anhydride thereof, and (d) an organic peroxide. Consisting of a simultaneous melting mixture of substances.

Examples of the peroxide decomposition type amorphous to low crystalline olefin copolymer used as component (a) include propylene-ethylene copolymer, butene-1-ethylene copolymer, and propylene-butene-1 copolymer. In the case of copolymers, the proportion of comonomers that determines the degree of crystallinity is -chip copolymers, the α-olefin content is approximately 5.
The amount used is 0 mol% or more, preferably about 55 mol% or more.

Among these olefin copolymers, the most preferable one from the viewpoint of flexibility is propylene-ethylene copolymer, and considering rubber properties and viscosity reduction, the propylene content is about 55 to 80 mol%. It is particularly preferable that That is, if the propylene content exceeds this range, the crystallinity will increase and flexibility will be lost, while if the propylene content is below this range, the viscosity will become too high. And these copolymers are
By kneading with an organic peroxide under heating, the decomposition reaction takes precedence over the crosslinking reaction, significantly increasing fluidity.

Examples of the peroxide-decomposed crystalline olefin resin of component (b) include isotactic polypropylene, copolymerized propylene with other olefins, polybutene-1, and the like. These crystalline olefin resins have a melting point of about 100 to 200°C, preferably about 110°C.
~170°C, and those having a crystallinity of about 25% or more are preferably used. Those with a melting point lower than this or those with a crystallinity lower than this are not suitable for improving the heat resistance, which is the objective of the present invention, while those with a melting point higher than this are used at the temperature at which they are used as hot melt adhesives. It becomes unsuitable for the purpose of improving fluidity in the range. By kneading these crystalline olefin resins with organic peroxides under heating, they are thermally decomposed to increase fluidity, and
It also plays a role in improving heat resistance.

In the polymer component consisting of the above components (a) and (b), component (a) is about 90 to 50% by weight, preferably about 80% by weight.
-60% by weight, and component (b) is about 10-50% by weight,
It is used in a proportion of about 20 to 40% by weight.

If the proportion of component (b) exceeds this range, the flexibility and adhesiveness of the composition will be impaired, while if the proportion is below this range, the heat resistance and fluidity of the composition will be impaired.

Examples of the unsaturated carboxylic acid or its acid anhydride as component (c) include maleic acid, fumaric acid, itaconic acid, acrylic acid, methacrylic acid, crotonic acid, maleic anhydride,
Itaconic anhydride, sorbic acid, cinnamic acid, vinyl acetic acid, etc. are used, and among these, maleic anhydride, which is difficult to undergo radical polymerization alone, is preferably used. These unsaturated carvone 11! Alternatively, the acid anhydride is graft-copolymerized with the above-mentioned (a) component and (b) component by heating and kneading with these polymer components in the presence of an organic peroxide. Unsaturated carboxylic acid or its acid anhydride is resin component 1
About 0.01 to 5 parts per 00 parts by weight, preferably about 0
．． It is used in an amount of 5 to 31 parts by weight, more preferably about 1 to 2 parts by weight. If it is used in a proportion greater than this, the coloring will become intense, while if it is used in a proportion less than this, the adhesive strength will be insufficient.

Examples of the organic peroxide of component (d) used for the decomposition reaction and grafting reaction of the polymer component include dicumyl peroxide, ditert-butyl peroxide,
．． 5-dimethyl-2,5-di(tert-butylperoxy)
Hexane, 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne-3,1,3-bis(tert-butylperoxyisoglobil)benzene, 1,1-bis(tert-butylperoxy) -3,3,5-)limethylcyclohexane, n-butyl-4,4-bis(tert-butylperoxy)valerate, benzoyl peroxide, p-chlorobenzoyl peroxide, 2,4-dichlorobenzoyl peroxide, tert-butyl Examples include peroxybenzoate, tert-butylperoxyisopropyl carbonate, diacetyl peroxide, lauroyl peroxide, and tert-butyl cumyl peroxide. These organic peroxides are used in an amount of about 0.01 to 3 mfit parts, preferably about 0.05 to 1 mfit parts, per 100 parts by weight of the resin component.
It is used in a proportion of about 0.1 to 1 part by weight, more preferably about 0.1 to 1 part by weight.

In addition, the adhesive composition of the present invention may contain ethylene-vinyl, ester copolymer, An ethylene-unsaturated carboxylic acid (ester) copolymer or the like can also be used in combination.

The adhesive composition is prepared by mixing the above-mentioned components using a Banbury mixer, a kneader 1 melt stirrer, an extruder, etc. (a)
and (b) after melting and kneading at a temperature higher than the decomposition temperature of the same component, it is once formed into granules, flakes, pellets, rods, etc., and used in various bonding methods. Here, (a) to (
c) When melting and kneading each component in an extruder, there is insufficient crosstalk due to insufficient residence time in the extruder or poor crosstalk performance of the extruder, resulting in insufficient increase in the melt index of the product and insufficient improvement in heat resistance. In this case, the desired adhesive composition can be obtained by further adding an organic peroxide or by melting and kneading it again using an extruder without adding an organic peroxide. In addition, considering the capacity and performance of the extruder, after kneading each component (a), (b), and (d) in the first extruder, (c) (b1) A method of adding the same components can also be adopted.

When preparing the adhesive composition of the present invention! The important thing is (a)
~(c) components are allowed to coexist, and this is melted and kneaded in the presence of the organic peroxide of component (i) to simultaneously perform the cleavage and decomposition reaction of the polymer component and the melt work,
Only in this way can the object of the invention be achieved. On the other hand, after melting, kneading, and decomposing and modifying components (a), (c), and (d), this decomposition and modification product and (b)
An adhesive composition with excellent heat resistance as in the present invention cannot be obtained by simply melting and kneading the components.

The adhesive composition of the present invention is thus prepared as a simultaneous melt mixture of each of the components (a) to (d), but at least one of the same components (a) and (b) is pregrafted in an amount. Target: 0.01-5% unsaturated carbon ill! In addition, the unsaturated carboxylic acid of the peroxide-decomposed amorphous to low-crystalline olefin copolymer obtained by graft-modifying the mineral with an acid anhydride or its acid anhydride graft-modified product. (b) unsaturated carboxylic acid of a peroxide-decomposed crystalline olefin resin, or both of the unsaturated carboxylic acid and an acid anhydride graft modification thereof, or a graft modification of one of these (a)
') or (b') and the other unmodified form (b) or (a
) in the presence of about 0.01 to 3 parts by weight of (d) organic peroxide per 100 cuttings of these polymer components. In addition, the preparation is performed according to the case where each component (a) to (d) is used.

The organic peroxide of component (d) is simply (a) and (b))
Each component does not act solely as a graft modification catalyst. Adhesive compositions prepared without the (Ll) component in each of these adhesive compositions showed better adhesion than those prepared without the (Ll) component, especially when prepared into hot melt adhesives from them. This is evidenced by its remarkable superiority, especially in terms of shear failure temperature.

The adhesive composition of the present invention containing each of the above components (a) to (d) as basic essential components may optionally include a tackifier resin,
Contains wax, plasticizer, filler, antioxidant, etc.
Hot melt adhesives can be prepared.

Examples of the tackifying resin include rosin or its derivatives, terpene resins, terpene-7 enol resins, aromatic, aliphatic, alicyclic or copolymerized petroleum resins, coumaron-indene resins, styrene resins, etc. mentioned,
From the viewpoint of compatibility and adhesiveness, terpene resins and alicyclic petroleum resins are particularly preferred, and from the viewpoint of heat resistance, terpene resins are particularly preferred. It is preferably used in an amount of about 50 to 150 parts by weight.

Examples of the wax used as a viscosity reducing agent in the composition include paraffin wax, microcrystalline wax, polyethylene wax, polypropylene wax, etc., and these waxes are generally used in an amount of about 50 parts by weight or less per 100 parts by weight of the adhesive composition. used. When this composition is used as an adhesive that can be applied with a hot melt ablation IJ+-ter, its viscosity (b80℃)
The viscosity of the composition is desirably about 100 poise or less, preferably about 50 poise or less, so the viscosity of the composition can be adjusted to a desired level by adjusting the amount of each component.

The adhesive composition thus prepared is preferably in the form of a hot-melt adhesive, such as polyethylene, polypropylene, polystyrene, hard or soft vinyl chloride resin, ethylene-vinyl acetate copolymer or its adhesive. Films, sheets, foams, non-woven fabrics and other molded products made of various resins such as chemical compound, polyester, polyamide, ethylene-acrylic acid (ester) copolymer, ionomer resin, aluminum foil, copper foil, steel plate, paper, wood, etc. It can be used as an effective adhesive for various substrates including smooth substrates.

Application of the adhesive composition to these substrates can be carried out, for example, by the following methods. Sandwich the film or sheet between the base materials,
A method of thermal fusion, or a method of laminating an adhesive composition on at least one base material side by a coextrusion method, an extrusion coating method, etc., and then laminating the other base material (2) Sandwich lamination method T - A method of laminating a substrate through a molten film of an adhesive composition using a die method or the like (3) Coextrusion method If the substrate can be extruded, including the adhesive composition,
A method in which all constituent layers are coextruded and laminated using an extrusion molding method (4) Hot melt method An adhesive composition to which a tackifier resin, wax, etc. are added as necessary is coated using a hot melt gun, roll twoter, extrusion coater, etc. Method of applying to a substrate and bonding by pressing [Effect of the invention] Since the adhesive composition according to the present invention has good adhesive strength and heat resistance, it can be applied to a smooth substrate with at least one substrate. It can also be effectively used as an adhesive, especially a hot melt adhesive. In particular, the adhesive composition of the present invention can provide good adhesion and heat resistance to polypropylene, which has traditionally been difficult to adhere to among smooth substrates, or to other substrates. Well, I have to say that it is worth mentioning.

〔Example〕

Next, the present invention will be described in detail with reference to examples.

The compositions prepared in each Example and Comparative Example were evaluated as follows.

Adhesive crab (a) Heat-sealing method A hot-melt adhesive was melted by heating at 180° C., and a sheet with a thickness of 0.2 sheets was produced using a hot press.

This adhesive sheet was sandwiched between adherends, and using a sheet sealer, the sealing width was 251+ll and the sealing temperature was 16.
0°C (temperature of the top and bottom of the sealer), sealing pressure 3
~G1 After heat sealing under the conditions of sealing time of 5 seconds, the sample was cut into a width of 251 ml and 1 m, and the T-peel strength was measured using an Instron tensile tester at a tensile speed of 300 m/min and a temperature of 23°C. did.

(b) Hot-melt applicator method A hot-melt adhesive was heated and melted at 180°C, and then pressed using a Nordson hot-melt applicator under conditions of an open time of 5 seconds, a press pressure of 3 to G, and a press time of 5 seconds. A sample with a width of 25 WI was prepared, and this sample was tested at a tensile speed of 300 a using an Instron tensile tester.
The T-peel strength was measured under conditions of m/min and a temperature of 23°C.

The adherend for these adhesive strength measurements was a polypropylene film (PP: a blown film made from Tamashi Petrochemical Products' polypropylene, with a thickness of 2.
00μ), polyethylene tele7 tallate film (Pl
iiT: Toshi product Lumirror, thickness 200μ) and soft aluminum plate (A1: thickness 200μ) were used, respectively.

Bath melt viscosity: The melt viscosity of hot melt adhesive at 180°C is B.
Measured using a rotary viscometer.

Shear bond failure temperature: In the adhesive strength measurement method, an adhesive sheet was sandwiched between kraft papers and heat-sealed under the same conditions, then a sample with a width of 25 cm was prepared, and a load of 1 Kf was applied to it. 0.30
The falling temperature was measured when the temperature was raised at the same rate as that of the other parts.

Further, the melt flow rate of each component (IL) and (b) used was measured at 190°C.

Example 1 Propylene-ethylene copolymer rubber (propylene content 60
Mol%, melt 70-rate 0.29) 70 parts (amount taken,
), 30 parts of crystalline polypropylene (melt 70-rate 15), 1.5 parts of maleic anhydride and 2.5 parts of maleic anhydride
-Dimethyl-2,5-di(tert-butylperoxy)hexyne-30.2 parts were blended in a Henschel mixer, and this mixture was passed through an extruder with a diameter of 1151 m (h/rt-2).
8, using an intermediate Dalmage screw) at a resin temperature of 300°C to obtain pellets.

Melt 70 of adhesive composition thus prepared
The rate (b90°C, 2160 g), shear bond failure temperature, and adhesive strength by heat sealing method were measured.

Example 2 In Example 1, the amount of polypylene-ethylene copolymer rubber was changed to 90 parts, and the amount of crystalline polypropylene was changed to 10 parts.

Example 3 In Example 1, the same amount of propylene-butene-1 copolymer (propylene content 70 mol%, crystallinity 25% by melt tetra-rate 2k01Xi method) was used instead of crystalline polypropylene. .

Comparative Example 1 In Example 1, maleic anhydride was not used.

Comparative Example 2 In Example 1, the same amount of ethylene-propylene copolymer rubber (ethylene content 60 mol%, melt 70-rate 0.6) was used in place of the propylene-ethylene copolymer rubber.

Comparative Example 3 In Example 1, no crystalline polypropylene was used,
Only 100 parts of propylene-ethylene copolymer rubber was used.

Comparative Example 4 70 parts of the maleic anhydride grafted modified propylene-ethylene copolymer rubber obtained in Comparative Example 3 and 30 parts of the crystalline polypropylene were melt-blended in an extruder.

Example 4 100 parts of the crystalline polypropylene, 1 part of maleic anhydride
．． 5 parts and 30.2 parts of 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne were triblended and subjected to a graft reaction in the same manner as in Example 1.

The maleic anhydride grafted modified product of the obtained crystalline polypropylene (maleic anhydride grafting amount: 1.51ffi%)
) 30 parts, 70 parts of the maleic anhydride grafted modified product of the propylene-ethylene copolymer rubber obtained in Comparative Example 3 (maleic anhydride graft mi, s weight %), and 2.5-dimethyl-2,5-di( Tri-blend of tert-butylperoxy)hexyne-30.2m was extruded at 300° C. using an extruder with a diameter of 65 to form pellets.

Comparative Example 5 In Example 4, 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne-3 was not used.

The adhesive compositions obtained in Examples 2 to 4 and each comparative example above were evaluated in the same manner as in Example 1, and the measurement results are shown in Table 1 below along with the measurement results of Example 1. shown.

Table 1 Example 1 35 139 140
0 2720 Example 2 25 115
1150 1450 Example 3 20
114 4500 5560 Example 4
40 139 1050 1
080 Comparative Example 1 50 136
120 0 Comparative example 2 4 10
8 1120 280 Comparative Example 3 10
70 910 680 Comparative example 4
14 98 1280 1540 Comparative example 5 32 99 1300
1620 Example 5 40 parts of the adhesive composition of Example 1, terpene resin as tackifying resin (cheap crude oil product YSL/'Zin Px 10
0) 40 parts and microcrystalline wax (
20 parts of Hiki Sei Smoked Products Pax 2191) were put into a Neigu and kneaded at 200 to 220°C for 1 hour to prepare a hot melt adhesive.

The melt viscosity, shear welding failure temperature, and bonding strength by heat sealing method of the hot melt adhesive produced in this way were measured.

Example 6 In the actual frll J5, the same amount of polyethylene wax (Tamashi Petrochemical Products Hiwax 110 F) was used instead of the microcrystalline wax. Example 7 In Example 5, the adhesive composition of Example 1 was used. 45 copies of things,
The amount of terpene resin was changed to 45 parts, and the amount of microcrystalline wax was changed to 10 parts.

Example 8 In Example 5, the same amount of alicyclic thread oil resin (Esso Chemical Products Esfrets 5300) was used instead of the terpene resin.
) was used.

Example 9 In Example 5, instead of the adhesive composition of Example 1,
The same amount of the adhesive composition of Example 4 was used.

Comparative Example 6 In Example 5, instead of the adhesive composition of Example 1,
The same amount of the composition of Comparative Example 1 was used.

Comparative Example 7 Example 5 K, J5 In place of the adhesive composition of Example 1, the same amount of the composition of Comparative Example 2 was used.

Example 2 of Example 8 In Example 5, instead of the adhesive composition of Example 1,
The same amount of the composition of Comparative Example 3 was used.

Ratio 1ij54 Example 9 Example 5 Odor-C1 Instead of the adhesive composition of Example 1, the same amount of the composition of Comparative Example 4 was used.

Comparative Example 10 In Example 5, instead of the adhesive composition of Example 1,
The same amount of the composition of Comparative Example 5 was used. The hot-melt adhesives obtained in Examples 6 to 9 and Comparative Examples 6 to 10 in 1-1 below were evaluated in the same manner as in Example 5 (however, only in Example 7 was the adhesion (by hot melt applicator method), the measurement results are shown in Table 2 below, together with the measurement results of Example 5.

Table 2 Example 5 7.5 89 5.5
5.4 5.0 Example 6 8.0
99 5.7 5.0 5.6 Example 7 33.0 101 7.0 6
．． 5 9.5 Example 8 9.0 84
5.5 5.5 5.2 Example 9
9.8 110 6.0 6.8
5.2 Comparative Example 6 4.8 85
1.8 2. ．． 9 1.6 Comparative Example 7110
81 3.3 0 0 Comparative example 8 35 58 6.6 5.6
5.2 Comparative Example 9 16.5 65
5.3 7.4 4.2 Comparative example 10 9
．． 8 68 5.2 5.0
5.3 Example 10 210 o parts of the crystalline polyplastic resin, 5 maleic anhydride
and 30.2 parts of 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne,
The graft reaction was carried out in the same manner as in Example 1.

Maleic anhydride of the obtained crystalline polypropylene? Futo modified product (maleic anhydride graph) amount 1.5%) 3
0 parts 1, 70 parts of the propylene-ethylene copolymer rubber used in Example 1 and 2,5-dimethyl-2,5-di(
30.2 parts of tert-butylperoxy)hexyne was triblended, and this was extruded into pellets using an extruder with a diameter of 651 at a resin temperature of 300°C.

Example 11 70 parts of the composition of Comparative Example 3, 30 parts of crystalline polypropylene, and 30.2 parts of 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne were triblended, and this was 65m! ! Using the extrusion pattern of 1, the tree ut [degree 3
The pellets were extruded at 00°C.

Comparative Example 11 In Example 1O, the anhydrous maleic graft modified product of crystalline polypropylene and the propylene-ethylene conjugated rubber were combined into 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne-3 Melt blended in the absence of.

Example 12 In Example 5, instead of the adhesive composition of Example 1,
The same amount of the adhesive composition of Example 1O was used.

Example 13 In Example 5, instead of the adhesive composition of Example 1,
The same amount of the composition of Example 11 was used.

Comparative Example 12 In Example 5, instead of the adhesive composition of Example 1,
The same amount of the composition of Comparative Example 11 was used.

The (adhesive) compositions and hot melt adhesives obtained in Examples 10 to 13 and Comparative Examples 11 to 12 were evaluated in the same manner as in Examples 1 and 5.

The measurement results are shown in Table 3 below.

Table 3 Agent Patent Attorney Yoshi 1) Toshio Procedural Amendment (b) July 30, 1980 Patent Application No. 128910 2 Name of invention Adhesive composition 3 Relationship with the person making the amendment Patent Applicant name: Mitsui Polychemical Co., Ltd. 4 Agent (〒105) Address: 1-2-7 Shiba Daimon, Minato-ku, Tokyo≧＼Kenichi (b) ji!Page 11, line 14f Melting stirrer, Delete.

(2) On page 12, lines 2 and 3, [Add or do not add, correct j to "add."

(3) Page 14, line 11, line 14, and page 24, line 1
Correct "alicyclic" in the three lines to "alicyclic j".

(4) “Poise” on page 15, line 7 (2 places), page 26, table 2, and page 28, table 3 are respectively IrPa-8JI
Correct.

(5) "Sheet seal" in lines 1 and 2 of page 18 is corrected to "heat seal j."

(6) Correct "rm1 minute" in line 7 of page 18 to "Fmm/min."

(7) Ir65 rl15s+s+J on page 20, line 2
Correct to w+nJl.

(8) Ii'1O00J rlooJ on page 15, line 7
Correct to l.

Claims (1)

[Claims] 1. (a) about 90 to 50% by weight of a peroxide-decomposed amorphous to low-crystalline olefin copolymer; and (b) a peroxide-decomposed crystalline olefin copolymer. An adhesive composition comprising a co-melted mixture of a polymer component comprising about 10 to 50% by weight of a combined polymer component, (c) an unsaturated carboxylic acid or anhydride thereof, and (d) an organic peroxide. 2. The adhesive composition according to claim 1, wherein component (a) is a propylene-ethylene copolymer having a propylene content of 50 mol% or more. 3. The adhesive composition according to claim 1, wherein component (b) is a propylene homopolymer or copolymer. 4. The adhesive composition according to claim 1, wherein component (c) is maleic acid or maleic anhydride. 5. Component (c) is about 0.0 per 100 parts by weight of the polymer component.
The adhesive composition according to claim 1 or 4, which is used in a proportion of 1 to 5 parts by weight. 6. Component (d) is about 0.0 per 100 parts by weight of the polymer component.
The adhesive composition according to claim 1, wherein the adhesive composition is used in an amount of 1 to 3 parts by weight. 7. (a) about 90-50% by weight of a peroxide-decomposed amorphous to low-crystalline olefin copolymer and (b) about 10-50% by weight of a peroxide-decomposed crystalline olefin-based copolymer %, at least one of these components (a) and (b) is graft-modified with (c) an unsaturated carboxylic acid or its acid anhydride, and (d) an organic polymer component. An adhesive composition comprising a co-melted mixture of oxides. 8. The adhesive composition according to claim 7, wherein the olefin copolymer used in component (a) is a propylene-ethylene copolymer having a propylene content of 50 mol% or more. 9. The adhesive composition according to claim 7, wherein the olefin polymer used in component (b) is a propylene homopolymer or copolymer. 10. The adhesive composition according to claim 7, wherein the graft modified polymer component is maleic acid or maleic anhydride graft modified product. 11. Claim 7 or 1, wherein the graft modified product component of the polymer is an unsaturated carboxylic acid or its acid anhydride grafted product with a graft amount of about 0.01 to 5% by weight.
Adhesive composition according to item 0. 12. Component (d) is about 0.0% per 100 parts by weight of the polymer component.
Claim 7 used in a proportion of 01 to 3 parts by weight
The adhesive composition described in .