JP2005325154A - Composition for adhesive - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a composition for an adhesive, having a high adhesive power and also a small temperature dependence of the adhesive power. <P>SOLUTION: This composition for the adhesive containing 97-99.9 wt. % following amorphous olefin-based polymer (component (A)) and 0.1-3 wt. % following block copolymer (component (B)) (provided that the total weight of the composition for the adhesive is set as 100 wt. %). The component (A) is the amorphous olefin-based polymer obtained by copolymerizing ethylene and at least 2 kinds of olefins selected from a group consisting of 3-20C α-olefins, and having ≤3 molecular wright distribution, and the component (B) is at least 1 kind of a resin selected from a group consisting of a vinyl aromatic-conjugated diene-based block copolymer and hydrogenated vinyl aromatic-conjugated diene-based block copolymer. <P>COPYRIGHT: (C)2006,JPO&NCIPI

Description

  The present invention relates to an adhesive composition. Specifically, it is to provide a composition for pressure-sensitive adhesives having high adhesive strength and low temperature dependency of adhesive strength.

Conventionally, low-crystallinity polymers such as low-density polyethylene, ethylene-vinyl acetate copolymer resin, and styrene-based rubber and amorphous polymers have been used as self-adhesive adhesives.
However, an adhesive using the above-mentioned low crystalline polymer or amorphous polymer is an adhesive that changes with time at a high temperature. It may be difficult to peel off the adherend or the adhesive may remain on the surface of the adherend after peeling.

  For example, JP-A-2002-302659 discloses that an adhesive film having an adhesive strength that is capable of controlling the adhesive strength without excessively changing over time even at low or high temperatures, A pressure-sensitive adhesive film having a pressure-sensitive adhesive layer made of an olefin copolymer containing at least two kinds of olefin polymerization units selected from the group consisting of α-olefins having 3 to 20 carbon atoms and satisfying specific requirements is described. .

JP 2002-302659 A

Even in the adhesive film described in JP-A-2002-302659, when higher adhesive force is required over a wider temperature range, particularly when higher adhesive force is required even in a high temperature region. However, in order to satisfy market demands, further improvements in adhesive strength were required.
Under such circumstances, an object of the present invention is to provide a pressure-sensitive adhesive composition having high adhesive strength and low temperature dependency of adhesive strength.

As a result of intensive studies, the present inventors have found that the present invention can solve the above problems, and have completed the present invention.
That is, the present invention
For pressure-sensitive adhesive containing 97 to 99.9% by weight of the following amorphous olefin polymer (component (A)) and 0.1 to 3% by weight of the following block copolymer (component (B)) It relates to a composition (however, the total weight of the pressure-sensitive adhesive composition is 100% by weight).
Component (A) is an amorphous olefin system obtained by copolymerizing at least two olefins selected from the group consisting of ethylene and α-olefins having 3 to 20 carbon atoms, and having a molecular weight distribution of 3 or less. It is a polymer.
Component (B) is at least one resin selected from the group consisting of vinyl aromatic-conjugated diene block copolymers and hydrogenated products of vinyl aromatic-conjugated diene block copolymers.

  ADVANTAGE OF THE INVENTION According to this invention, the composition for adhesives with high adhesive force and the small temperature dependence of adhesive force can be obtained.

The amorphous olefin polymer (component (A)) is an amorphous olefin obtained by copolymerizing at least two olefins selected from the group consisting of ethylene and an α-olefin having 3 to 20 carbon atoms. Based polymer.
As a C3-C20 alpha-olefin used for a component (A), a C3-C20 linear olefin and a branched olefin are mentioned, for example.
Examples of the linear olefin include propylene, 1-butene, 1-pentene, 1-hexene, 1-heptene, 1-octene, 1-nonene, 1-decene, 1-undecene, 1-dodecene, 1- Examples include tridecene, 1-tetradecene, 1-pentadecene, 1-hexadecene, 1-heptadecene, 1-octadecene, 1-nonadecene, 1-eicocene and the like.
Examples of the branched olefin include 3-methyl-1-butene, 3-methyl-1-pentene, 4-methyl-1-pentene, 2-ethyl-1-hexene, 2,2,4-trimethyl-1- Examples include pentene.

  Specific combinations of at least two olefins selected from the group consisting of ethylene and an α-olefin having 3 to 20 carbon atoms used for component (A) include ethylene / propylene, ethylene / 1-butene, ethylene / 1-hexene, ethylene / 1-octene, ethylene / 4-methyl-1-pentene, ethylene / propylene / 1-butene, ethylene / propylene / 1-hexene, ethylene / 1-butene / 1-hexene, propylene / 1 -Butene, propylene / 1-hexene, propylene / 1-octene, propylene / 4-methyl-1-pentene, propylene / 1-butene / 1-hexene and the like.

  The component (A) is preferably obtained by copolymerizing olefins in which the total number of carbon atoms of at least two selected olefins is 6 or more from the viewpoint of enhancing the adhesive strength of the pressure-sensitive adhesive composition. It is an amorphous olefin polymer.

  From the viewpoint of further increasing the adhesive strength of the pressure-sensitive adhesive composition, the component (A) is preferably at least two olefins selected from the group consisting of propylene and α-olefins having 4 to 20 carbon atoms. It is an amorphous olefin polymer obtained by copolymerization. More preferably, it is an amorphous propylene polymer obtained by copolymerizing propylene and at least one α-olefin having 4 to 20 carbon atoms, such as propylene / 1-butene copolymer, Examples include propylene / 1-hexene copolymer, propylene / 1-octene copolymer, propylene / 4-methyl-1-pentene copolymer, propylene / 1-butene / 1-hexene copolymer.

  The amorphous olefin polymer (component (A)) is composed of at least two olefins selected from the group consisting of ethylene and an α-olefin having 3 to 20 carbon atoms, and other than the at least two olefins. An amorphous olefin polymer obtained by copolymerizing with a monomer may also be used. Examples of the monomer other than the at least two olefins include cyclic olefins, vinyl aromatic compounds, and polyene compounds.

  Examples of the cyclic olefin include norbornene, 5-methylnorbornene, 5-ethylnorbornene, 5-propylnorbornene, 5,6-dimethylnorbornene, 1-methylnorbornene, 7-methylnorbornene, 5,5,6-trimethyl. Norbornene, 5-phenylnorbornene, 5-benzylnorbornene, 5-ethylidenenorbornene, 5-vinylnorbornene,

1,4,5,8-dimethano-1,2,3,4,4a, 5,8,8a-octahydronaphthalene, 2-methyl-1,4,5,8-dimethano-1,2,3 4,4a, 5,8,8a-octahydronaphthalene, 2-ethyl-1,4,5,8-dimethano-1,2,3,4,4a, 5,8,8a-octahydronaphthalene, 2, 3-dimethyl-1,4,5,8-dimethano-1,2,3,4,4a, 5,8,8a-octahydronaphthalene, 2-hexyl-1,4,5,8-dimethano-1, 2,3,4,4a, 5,8,8a-octahydronaphthalene, 2-ethylidene-1,4,5,8-dimethano-1,2,3,4,4a, 5,8,8a-octahydro Naphthalene,

2-Fluoro-1,4,5,8-dimethano-1,2,3,4,4a, 5,8,8a-octahydronaphthalene, 1,5-dimethyl-1,4,5,8-dimethano- 1,2,3,4,4a, 5,8,8a-octahydronaphthalene, 2-cyclohexyl-1,4,5,8-dimethano-1,2,3,4,4a, 5,8, 8a-octahydronaphthalene, 2,3-dichloro-1,4,5,8-dimethano-1,2,3,4,4a, 5,8,8a-octahydronaphthalene, 2-isobutyl-1,4 5,8-dimethano-1,2,3,4,4a, 5,8,8a-octahydronaphthalene,

1,2-dihydrodicyclopentadiene, 5-chloronorbornene, 5,5-dichloronorbornene, 5-fluoronorbornene, 5,5,6-trifluoro-6-trifluoromethylnorbornene, 5-chloromethylnorbornene, 5- Methoxynorbornene, 5,6-dicarboxylnorbornene anhydrate, 5-dimethylaminonorbornene, 5-cyanonorbornene, cyclopentene, 3-methylcyclopentene, 4-methylcyclopentene, 3,4-dimethylcyclopentene, 3,5-dimethylcyclopentene , 3-chlorocyclopentene, cyclohexene, 3-methylcyclohexene, 4-methylcyclohexene, 3,4-dimethylcyclohexene, 3-chlorocyclohexene, cycloheptene and the like.

  Examples of the vinyl aromatic compound include styrene, α-methylstyrene, p-methylstyrene, vinylxylene, monochlorostyrene, dichlorostyrene, monobromostyrene, dibromostyrene, fluorostyrene, and p-tert-butylstyrene. , Ethyl styrene, vinyl naphthalene and the like.

Examples of the polyene compound include conjugated polyene compounds and non-conjugated polyene compounds. These conjugated polyene compounds and non-conjugated polyene compounds may have an alkoxy group, an aryl group, an aryloxy group, an aralkyl group, an aralkyloxy group, and the like.
Examples of the conjugated polyene compound include aliphatic conjugated polyene compounds such as linear aliphatic conjugated polyene compounds and branched aliphatic conjugated polyene compounds, and alicyclic conjugated polyene compounds. Non-conjugated polyene compounds include aliphatic conjugated polyene compounds. Non-conjugated polyene compounds, alicyclic non-conjugated polyene compounds, aromatic non-conjugated polyene compounds and the like can be mentioned.

Examples of the aliphatic conjugated polyene compound include 1,3-butadiene, isoprene, 2-ethyl-1,3-butadiene, 2-propyl-1,3-butadiene, 2-isopropyl-1,3-butadiene, 2-hexyl-1,3-butadiene, 2,3-dimethyl-1,3-butadiene, 2,3-diethyl-1,3-butadiene, 2-methyl-1,3-pentadiene, 2-methyl-1, 3-hexadiene, 2-methyl-1,3-octadiene, 2-methyl-1,3-decadiene, 2,3-dimethyl-1,3-pentadiene, 2,3-dimethyl-1,3-hexadiene, 2, Examples include 3-dimethyl-1,3-octadiene and 2,3-dimethyl-1,3-decadiene.
Examples of the alicyclic conjugated polyene compound include 2-methyl-1,3-cyclopentadiene, 2-methyl-1,3-cyclohexadiene, 2,3-dimethyl-1,3-cyclopentadiene, 2, 3-dimethyl-1,3-cyclohexadiene, 2-chloro-1,3-butadiene, 2,3-dichloro-1,3-butadiene, 1-fluoro-1,3-butadiene, 2-chloro-1,3 -Pentadiene, 2-chloro-1,3-cyclopentadiene, 2-chloro-1,3-cyclohexadiene and the like are exemplified.

  Examples of the aliphatic non-conjugated polyene compound include 1,4-hexadiene, 1,5-hexadiene, 1,6-heptadiene, 1,6-octadiene, 1,7-octadiene, 1,8-nonadiene, , 9-decadiene, 1,13-tetradecadiene, 1,5,9-decatriene, 3-methyl-1,4-hexadiene, 4-methyl-1,4-hexadiene, 5-methyl-1,4-hexadiene 4-ethyl-1,4-hexadiene, 3-methyl-1,5-hexadiene, 3.3-dimethyl-1,4-hexadiene, 3,4-dimethyl-1,5-hexadiene,

5-methyl-1,4-heptadiene, 5-ethyl-1,4-heptadiene, 5-methyl-1,5-heptadiene, 6-methyl-1,5-heptadiene, 5-ethyl-1,5-heptadiene, 3-methyl-1,6-heptadiene, 4-methyl-1,6-heptadiene, 4,4-dimethyl-1,6-heptadiene, 4-ethyl-1,6-heptadiene,
4-methyl-1,4-octadiene, 5-methyl-1,4-octadiene, 4-ethyl-1,4-octadiene, 5-ethyl-1,4-octadiene, 5-methyl-1,5-octadiene, 6-methyl-1,5-octadiene, 5-ethyl-1,5-octadiene, 6-ethyl-1,5-octadiene, 6-methyl-1,6-octadiene, 7-methyl-1,6-octadiene, 6-ethyl-1,6-octadiene, 6-propyl-1,6-octadiene, 6-butyl-1.6-octadiene,

4-methyl-1,4-nonadiene, 5-methyl-1,4-nonadiene, 4-ethyl-1,4-nonadiene, 5-ethyl-1,4-nonadiene, 5-methyl-1,5-nonadiene, 6-methyl-1,5-nonadiene, 5-ethyl-1,5-nonadiene, 6-ethyl-1,5-nonadiene, 6-methyl-1,6-nonadiene, 7-methyl-1,6-nonadiene, 6-ethyl-1,6-nonadiene, 7-ethyl-1,6-nonadiene, 7-methyl-1,7-nonadiene, 8-methyl-1,7-nonadiene, 7-ethyl-1,7-nonadiene,

5-methyl-1,4-decadiene, 5-ethyl-1,4-decadiene, 5-methyl-1,5-decadiene, 6-methyl-1,5-decadiene, 5-ethyl-1,5-decadiene, 6-ethyl-1,5-decadiene, 6-methyl-1,6-decadiene, 6-ethyl-1,6-decadiene, 7-methyl-1,6-decadiene, 7-ethyl-1,6-decadiene, 7-methyl-1,7-decadiene, 8-methyl-1,7-decadiene, 7-ethyl-1,7-decadiene, 8-ethyl-1,7-decadiene, 8-methyl-1,8-decadiene, 9-methyl-1,8-decadiene, 8-ethyl-1,8-decadiene,

6-methyl-1,6-undecadiene, 9-methyl-1,8-undecadiene, 6,10-dimethyl 1,5,9-undecatriene, 5,9-dimethyl-1,4,8-decatriene, 4 -Ethylidene 8-methyl-1,7-nonadiene, 13-ethyl-9-methyl-1,9,12-pentadecatriene, 5,9,13-trimethyl-1,4,8,12-tetradecadiene, Examples include 8,14,16-trimethyl-1,7,14-hexadecatriene, 4-ethylidene-12-methyl-1,11-pentadecadien, and the like.

  Examples of the alicyclic non-conjugated polyene compound include vinylcyclohexene, 5-vinyl 2-norbornene, 5-ethylidene-2-norbornene, 5-methylene-2-norbornene, 5-isopropenyl-2-norbornene, cyclo Hexadiene, dicyclopentadiene, cyclooctadiene, 2,5-norbornadiene, 2-methyl-2,5-norbornadiene, 2-ethyl-2,5-norbornadiene, 2,3-diisopropylidene-5-norbornene, 2- Ethylidene-3-isopropylidene-5-norbornene, 6-chloromethyl-5-isopropenyl-2-norbornene, 1,4-divinylcyclohexane, 1,3-divinylcyclohexane, 1,3-divinylcyclopentane, 1,5 -Divinylcyclooctane, 1-allyl- -Vinylcyclohexane, 1,4-diallylcyclohexane, 1-allyl-5-vinylcyclooctane, 1,5-diallylcyclooctane, 1-allyl-4-isopropenylcyclohexane, 1-isopropenyl-4-vinylcyclohexane, 1 -Isopropenyl-3-vinylcyclopentane, methyltetrahydroindene and the like are exemplified.

  Examples of the aromatic non-conjugated polyene compound include divinylbenzene and vinylisopropenylbenzene.

  The content of the structural unit derived from ethylene contained in the amorphous olefin polymer (component (A)) is usually 70 mol% or less from the viewpoint of increasing the adhesive strength of the adhesive composition, Preferably it is 50 mol% or less, More preferably, it is 20 mol% or less, More preferably, it is 0 mol%.

The content of the structural unit derived from propylene contained in the amorphous olefin polymer (component (A)) is usually 50 mol% or more from the viewpoint of increasing the adhesive strength of the pressure-sensitive adhesive composition, More preferably, it is 60 mol% or more, More preferably, it is 70 mol% or more, Especially preferably, it is 80 mol% or more, Most preferably, it is 90 mol% or more.
In addition, the content of the structural unit derived from propylene contained in the amorphous olefin polymer (component (A)) is usually 99.99 from the viewpoint of increasing the adhesive strength at low temperatures of the pressure-sensitive adhesive composition. It is 9 mol% or less, preferably 99 mol% or less, more preferably 98.5 mol% or less, and still more preferably 98 mol% or less.

  The amorphous nature of the amorphous olefin polymer (component (A)) is a crystal whose heat of crystal melting observed in the temperature range of −100 to 200 ° C. by differential scanning calorimetry (DSC) is 1 J / g or more. This is determined by whether a melting peak or a crystallization peak with a crystallization heat amount of 1 J / g or more is observed.

  As the amorphous olefin polymer (component (A)), preferably, the amount of heat of crystal melting is 1 J in the temperature range of −100 to 200 ° C. by differential scanning calorimetry (DSC) from the viewpoint of increasing the adhesive strength. It is an amorphous olefin polymer in which neither a crystal melting peak of not less than / g or a crystallization peak having a heat of crystallization of 1 J / g or more is observed.

As the amorphous olefin polymer (component (A)), preferably, from the viewpoint of enhancing the adhesive strength of the pressure-sensitive adhesive composition of the present invention, the amorphous olefin system satisfying the relationship of the following formula (1) It is a polymer.
[Y / (x + y)] ≧ 0.3 Formula (1)
(In Formula (1), x represents content (mol%) of the structural unit derived from ethylene contained in a component (A), and y is C4-C20 contained in a component (A). This represents the content (mol%) of structural units derived from α-olefin, provided that the total content of structural units derived from olefins contained in component (A) is 100 mol%.

As a more preferable relationship that the amorphous olefin polymer (component (A)) satisfies, the relationship of the following formula (2),
[Y / (x + y)] ≧ 0.5 Formula (2)
A more preferable relationship is the relationship of the following formula (3):
[Y / (x + y)] ≧ 0.8 Formula (3)
And a more preferable relationship is the relationship of the following formula (4):
[Y / (x + y)] = 1 Formula (4)
It is.

The intrinsic viscosity [η] of the amorphous olefin polymer (component (A)) is the intrinsic viscosity [η] measured using an Ubbelohde viscometer in 135 ° C. tetralin and used for the pressure-sensitive adhesive of the present invention. From the viewpoint of preventing the glue from remaining when peeling after the composition is adhered, it is preferably 0.1 dl / g or more, more preferably 0.3 dl / g or more, and even more preferably 0.5 dl. / G or more, more preferably 0.7 dl / g or more.
In addition, from the viewpoint of enhancing processability in the molding process of the pressure-sensitive adhesive composition of the present invention, the above intrinsic viscosity [η] is preferably 10 dl / g or less, more preferably 7 dl / g or less, More preferably, it is 5 dl / g or less, More preferably, it is 4 dl / g or less.

The molecular weight distribution (Mw / Mn) of the amorphous olefin polymer (component (A)) is from the viewpoint of inhibiting the adhesive from remaining after peeling after the adhesive composition of the present invention is adhered. 3 or less.
Said molecular weight distribution (Mw / Mn) is measured by gel permeation chromatography (GPC), Mw represents a weight average weight molecular weight, and Mn represents a number average molecular weight.

  Examples of the method for producing the amorphous olefin polymer (component (A)) include a method using a known Ziegler-Natta type catalyst or a known single site catalyst. From the viewpoint of further improving scratch resistance and heat resistance, the production method is preferably a method using a known single site catalyst.

  Examples of the single site catalyst include metallocene catalysts and nonmetallocene complex catalysts. Examples of the metallocene catalyst include, for example, JP-A-58-19309, JP-A-60-35005, JP-A-60-35006, JP-A-60-35007, and JP-A-60-35008. JP, JP 61-130314, JP 3-163088, JP 4-268307, JP 9-12790, JP 9-87313, JP 11-80233. And metallocene catalysts described in JP-A-10-508055 and the like.

  Examples of the nonmetallocene complex catalyst include, for example, JP-A-10-316710, JP-A-11-1000039, JP-A-11-80228, JP-A-11-80227, and JP-T-10-513289. Non-metallocene complex catalysts described in JP-A-10-338706, JP-A-11-71420 and the like can be mentioned.

The single site catalyst is preferably a metallocene catalyst from the viewpoint of easy availability, and more preferably has at least one cyclopentadiene-type anion skeleton, and has a C ₁ enantiomorphic structure. Group 12 transition metal complex.
Moreover, as an example of the manufacturing method using a metallocene catalyst, the method of European Patent Application Publication No. 12111287 is exemplified.

  The block copolymer (component (B)) is at least one selected from the group consisting of vinyl aromatic-conjugated diene block copolymers and hydrogenated vinyl aromatic-conjugated diene block copolymers. Resin.

  A vinyl aromatic-conjugated diene block copolymer used as a block copolymer (component (B)) is composed of a polymer block mainly composed of a vinyl aromatic compound and a polymer block mainly composed of a conjugated diene compound. Is a block copolymer.

The polymer block mainly containing a vinyl aromatic compound is a polymer block containing a vinyl aromatic compound as a main component and a conjugated diene compound as another constituent component.
Examples of the vinyl aromatic compound include styrene, α-methylstyrene, p-methylstyrene, vinylxylene, monochlorostyrene, dichlorostyrene, monobromostyrene, dibromostyrene, fluorostyrene, p-tert-butylstyrene, ethylstyrene, Examples include vinyl naphthalene. These vinyl aromatic compounds may be used alone or in combination of at least two kinds. As the vinyl aromatic compound, styrene is preferable.

  The content of the vinyl aromatic compound contained in the polymer block mainly composed of the vinyl aromatic compound is preferably 60 to 100% by weight from the viewpoint of reducing the temperature dependency of the adhesive force.

The polymer block mainly containing a conjugated diene compound is a polymer block containing a conjugated diene compound as a main component and a vinyl aromatic compound as another constituent component.
As the conjugated diene compound, 1,3-butadiene, isoprene, 2,3-dimethyl-1,3-butadiene, 2-neopentyl-1,3-butadiene, 2-chloro-1,3-butadiene, 2-cyano- Examples thereof include 1,3-butadiene, substituted linear conjugated pentadienes, linear and side chain conjugated hexadienes, and the like. These conjugated diene compounds may be used alone or in combination of at least two kinds. As the conjugated diene compound, 1,3-butadiene and isoprene are preferable.

  The content of the conjugated diene compound contained in the polymer block mainly composed of the conjugated diene compound is preferably 60 to 100% by weight from the viewpoint of enhancing the adhesive strength.

Specifically, the vinyl aromatic-conjugated diene block copolymer is represented by the following formula (I), formula (II), or formula (III).
(AB) n Formula (I)
(AB) n-A Formula (II)
(AB) n-X Formula (III)
(In the formula, A represents a polymer block mainly composed of an aromatic vinyl group compound (referred to as block A), B represents a polymer block composed mainly of a conjugated diene compound (referred to as block B), and X represents a cup. Represents a ring agent residue, and n represents an integer of 1 or more.)

  The ratio of the content of the polymer block mainly composed of vinyl aromatic compound / polymer block mainly composed of conjugated diene compound in the vinyl aromatic-conjugated diene block copolymer is preferably used for the pressure-sensitive adhesive of the present invention. From the viewpoint of reducing the temperature dependency of the adhesive strength of the composition and from the viewpoint of increasing the adhesive strength, it is 2/98 to 50/50.

  As a method for producing a vinyl aromatic-conjugated diene block copolymer, for example, generally, block A is polymerized first using a polymerization initiator such as an organic lithium compound in an organic solvent, and then block B is polymerized. Or a method of first polymerizing block B and then polymerizing block A.

  Moreover, as a manufacturing method of the block copolymer (n represents an integer greater than or equal to 1) represented by (A-B) n, generally in an organic solvent, using polymerization initiators, such as an organic lithium compound, First, the method of producing by repeating the polymerization of block A and then the polymerization of block B, or the method of producing by repeating the polymerization of block B and then the polymerization of block A can be mentioned. .

  Moreover, as a manufacturing method of the block copolymer represented by ABA, block A is polymerized using a polymerization initiator such as an organic lithium compound in an organic solvent, and then the block is B polymerized. In addition, a method of polymerizing the block A is exemplified, and (AB) as a method for producing the block copolymer represented by nA (n represents an integer of 1 or more), in an organic solvent Then, after repeating the polymerization of the block A using a polymerization initiator such as an organic lithium compound and the subsequent B polymerization of the block, a method of further polymerizing the block A can be mentioned.

  Moreover, as a manufacturing method of the block copolymer (A-B) n-X (X represents a coupling agent residue and n represents an integer greater than or equal to 1), it is manufactured by said method. (AB) The method of manufacturing by adding a coupling agent to the block copolymer represented by n is mentioned.

  As coupling agents, diethyl adipate, divinylbenzene, tetrachlorosilane, butyltrichlorosilane, tetrachlorotin, butyltrichlorotin, dimethyldichlorosilane, tetrachlorogermanium, 1,2-dibromoethane, 1,4-chloromethylbenzene Bis (trichlorosilyl) ethane, epoxidized linseed oil, tolylene diisocyanate, 1,2,4-benzene triisocyanate and the like.

As a method for producing a hydrogenated vinyl aromatic-conjugated diene block copolymer, for example, the above vinyl aromatic-conjugated diene block copolymer is dissolved in an inert solvent, 20 to 150 ° C., A method of performing hydrogenation in the presence of a hydrogenation catalyst under pressurized hydrogen of 0.1 to 10 MPaG can be mentioned.
The hydrogenation rate of the conjugated diene compound contained in the vinyl aromatic-conjugated diene block copolymer varies depending on the hydrogenation catalyst, the amount of hydrogen added, or the hydrogen pressure and reaction time during the hydrogen addition reaction. Adjusted by.

  The intrinsic viscosity [η] of the block copolymer (component (B)) is the intrinsic viscosity [η] measured using an Ubbelohde viscometer in toluene at 30 ° C., and the pressure-sensitive adhesive composition of the present invention From the viewpoint of preventing the glue from being left after peeling, it is preferably 0.1 dl / g or more, more preferably 0.3 dl / g or more, and further preferably 0.5 dl / g or more. And more preferably 0.7 dl / g or more.

  In addition, the intrinsic viscosity [η] of the component (B) is preferably 10 dl / g or less, more preferably 7 dl / g or less, from the viewpoint of improving processability in the molding process of the pressure-sensitive adhesive composition of the present invention. More preferably, it is 5 dl / g or less, More preferably, it is 4 dl / g or less.

  The molecular weight distribution (Mw / Mn) of the component (B) is preferably 3 or less, more preferably from the viewpoint of preventing the adhesive from remaining when peeling after the pressure-sensitive adhesive composition of the present invention is adhered. Is 2 or less, more preferably 1.5 or less. In addition, the molecular weight distribution of a component (B) is measured by a gel permeation chromatograph (GPC), Mw represents a weight average molecular weight and Mn represents a number average molecular weight.

The pressure-sensitive adhesive composition of the present invention comprises an amorphous olefin polymer (component (A)) 97 to 99.9% by weight, and a block copolymer (component (B)) 0.1 to 3% by weight. (However, the total weight of the pressure-sensitive adhesive composition is 100% by weight).
The content of the component (A) is preferably 97.5% by weight or more, more preferably 98% by weight or more from the viewpoint of enhancing the weather resistance of the pressure-sensitive adhesive composition of the present invention. In addition, the content of the component (A) is preferably 99.7% by weight or less from the viewpoint of preventing the adhesive from remaining when peeling after the pressure-sensitive adhesive composition of the present invention is adhered, More preferably, it is 99.5 weight% or less, More preferably, it is 99 weight% or less.

  The content of the component (B) is preferably 2.5% by weight or less, more preferably from the viewpoint of preventing the adhesive from remaining when peeling after the pressure-sensitive adhesive composition of the present invention is adhered. Is 2% by weight or less. Further, the content of the component (B) is preferably 0.3% by weight or more, more preferably 0.5% by weight or more from the viewpoint of enhancing the weather resistance of the pressure-sensitive adhesive composition of the present invention. More preferably 1% by weight or more.

You may add well-known resin and elastomers other than the component (A) and component (B) used by this invention to the composition for adhesives of this invention as needed.
Examples of the resin other than the component (A) and the component (B) used in the present invention include polyethylene resins such as high density polyethylene, medium density polyethylene, low density polyethylene and linear low density polyethylene (LLDPE), ethylene-acetic acid Vinyl copolymer resin, ethylene-acrylic acid copolymer resin, ethylene-acrylic acid ester copolymer resin, ethylene-methacrylic acid copolymer resin, ethylene-methacrylic acid ester copolymer resin, ethylene-glycidyl methacrylate copolymer Polymer resin, ethylene-acrylic acid ester-glycidyl methacrylate copolymer resin, polypropylene resin, polybutene resin, poly-4-methyl-pentene-1 resin, polystyrene resin, polyester resin, polyamide resin, Polyphenylene ether resin, polyaceta Le resins, polycarbonate resins.

  Examples of elastomers other than component (A) and component (B) used in the present invention include natural rubber, polybutadiene, liquid polybutadiene, styrene-butadiene random copolymer rubber, polyacrylonitrile rubber, acrylonitrile-butadiene copolymer rubber, and part. Examples include hydrogenated acrylonitrile-butadiene copolymer rubber, butyl rubber, chloroprene rubber, fluorine rubber, chlorosulfonated polyethylene, silicon rubber, urethane rubber, isobutylene-isoprene copolymer rubber, and halogenated isobutylene-isoprene copolymer rubber. .

The pressure-sensitive adhesive composition of the present invention may be subjected to cross-linking such as sulfur cross-linking, peroxide cross-linking, metal ion cross-linking, silane cross-linking, resin cross-linking, electron beam cross-linking, etc., if necessary. .
Examples of the crosslinking agent include sulfur, phenol resin, metal oxide, metal hydroxide, metal chloride, p-quinone dioxime, and bismaleimide-based crosslinking agent.
The crosslinking agent may be used in combination with a crosslinking accelerator in order to adjust the crosslinking rate. Examples of the crosslinking accelerator include oxidants such as red lead and dibenzothiazoyl sulfide.
The crosslinking agent may be used in combination with a dispersing agent such as a metal oxide or stearic acid. Examples of the metal oxide include zinc oxide, magnesium oxide, lead oxide, and calcium oxide, and zinc oxide and magnesium oxide are preferable.
Further, the pressure-sensitive adhesive composition of the present invention may be dynamically cross-linked in the presence of a cross-linking agent.

Examples of the method for producing the pressure-sensitive adhesive composition of the present invention include a method in which each component is kneaded by a normal kneading apparatus such as a rubber mill, a Brabender mixer, a Banbury mixer, a pressure kneader, a single screw or a twin screw extruder, or the like. The
The kneading device may be either a closed type device or an open type device. Preferably, it is a sealed device that can be replaced by an inert gas.
The kneading temperature is usually 120 to 250 ° C, preferably 140 to 240 ° C.
The kneading time is appropriately determined depending on the type and amount of components used or the type of kneading apparatus, and is usually about 3 to 10 minutes when a kneading apparatus such as a pressure kneader or a Banbury mixer is used.
Examples of the kneading method include a method of kneading each component at once, and a multistage division kneading method in which a part of each component is kneaded and then the remainder is added to continue kneading.

  In the composition for pressure-sensitive adhesives of the present invention, the rosin resin, polyterpene resin, synthetic petroleum resin, coumarone resin, phenol resin, xylene resin, styrene resin, isoprene resin, etc. Other resins than the component (A) and the component (B) used in the invention may be added.

  Examples of the rosin resin include natural rosin, polymerized rosin, partially hydrogenated rosin, fully hydrogenated rosin, esterified products of these rosins (eg, glycerin ester, pentaerythritol ester, ethylene glycol ester, methyl ester), rosin Derivatives (eg, disproportionated rosin, fumarized rosin, limeified rosin, etc.) are exemplified.

  Examples of the polyterpene resin include homopolymers of cyclic terpenes such as α-pinene, β-pinene, and dipentene, copolymers of the cyclic terpenes, and copolymers of the cyclic terpenes and phenolic compounds such as phenol and bisphenol. Polymers (for example, terpene-phenolic resins such as α-pinene-phenolic resin, dipentene-phenolic resin, terpene-bisphenolic resin, etc.), aromatic modified terpene resins that are copolymers of the above cyclic terpenes and aromatic monomers Illustrated.

Examples of the synthetic petroleum resin, C ₅ fraction naphtha cracked oil, C ₆ -C ₁₁ fraction, other olefinic fractions homopolymer or a copolymer, the water of these homopolymers and copolymers Examples thereof include aliphatic petroleum resins, aromatic petroleum resins, alicyclic petroleum resins, and aliphatic-alicyclic copolymer resins that are additives. Examples of the synthetic petroleum resin further include a copolymer of the naphtha cracked oil and the terpene, and a copolymer petroleum resin that is a hydrogenated product of the copolymer.

Preferred C ₅ fractions of the above naphtha cracked oil include isoprene, cyclopentadiene, 1,3-pentadiene, 2-methyl-1-butene, methylbutenes such as 2-methyl-2-butene, and 1-pentene. And pentenes such as 2-pentene and dicyclopentadiene.
Preferred C _{6 to} C ₁₁ fractions include methyl styrenes such as indene, styrene, o-vinyltoluene, m-vinyltoluene, p-vinyltoluene, α-methylstyrene, β-methylstyrene, methylindene, and ethylindene. , Vinyl xylene and propenylbenzene. Preferred other olefinic fractions include butene, hexene, heptene, octene, butadiene, and octadiene.

  Examples of the phenolic resin include alkylphenol resins, alkylphenol-acetylene resins obtained by condensation of alkylphenol and acetylene, and modified products of these resins. Moreover, as said phenol-type resin, any of the novolak-type resin which phenol-ized methylol with the acid catalyst, and the resol-type resin which methylated with the alkali catalyst may be sufficient.

  Examples of the xylene-based resin include a xylene-formaldehyde resin composed of m-xylene and formaldehyde, and a modified resin obtained by adding a third component to react with the xylene-formaldehyde resin.

  Examples of the styrene resin include a low molecular weight product of styrene, a copolymer resin of α-methylstyrene and vinyltoluene, and a copolymer resin of styrene, acrylonitrile, and indene.

Examples of the isoprene-based resins, resins obtained by copolymerizing a C ₁₀ alicyclic compound and C ₁₀ chain compound is a dimer product of isoprene are exemplified.

If necessary, a stabilizer, an additive, a filler, and a mineral oil softener may be added to the pressure-sensitive adhesive composition of the present invention.
Examples of the stabilizer include an antioxidant, an antioxidant, an ozone deterioration inhibitor, an ultraviolet absorber, and a light stabilizer.
Examples of the additive include an antistatic agent, a slip agent, an internal release agent, a colorant, a dispersant, an antiblocking agent, a lubricant, and an antifogging agent.
Examples of the filler include glass fiber, carbon fiber, metal fiber, glass bead, asbestos, mica, calcium carbonate, potassium titanate whisker, talc, aramid fiber, barium sulfate, glass flake, and fluororesin.
Examples of the mineral oil softener include naphthenic oil and paraffinic mineral oil.

  You may add a flame retardant to the composition for adhesives of this invention as needed. Examples of flame retardants include antimony flame retardants, aluminum hydroxide, magnesium hydroxide, zinc borate, guanidine flame retardants, zirconium flame retardants, and other inorganic compounds; ammonium polyphosphate, ethylene bistris (2-cyanoethyl) phosphor Phosphate esters and phosphorus compounds such as nium chloride, tris (tribromophenyl) phosphate, tris (tribromophenyl) phosphate, tris (3-hydroxypropyl) phosphine oxide; chlorinated paraffin, chlorinated polyolefin, perchlorocyclopentadecane, etc. Chlorinated flame retardants of: hexabromobenzene, ethylene bisdibromonorbornane dicarboximide, ethylene bistetrabromophthalimide, tetrabromobisphenol A derivatives, tetrabromobisphenol S, te Raburo modular pentaerythritol brominated flame retardants and the like. These flame retardants may be used alone or in combination of at least two kinds.

  The composition for pressure-sensitive adhesives of the present invention may be foamed by adding a foaming agent as necessary. As foaming agents, inorganic foaming agents such as sodium bicarbonate, ammonium bicarbonate and ammonium carbonate; nitroso compounds such as N, N′-dinitrosopentamethylenetetramine; azo compounds such as azocarbonamide and azoisobutyronitrile; benzenesulfonyl Examples thereof include sulfonyl hydrazides such as hydrazine, p, p′-oxybis (benzenesulfonyl hydrazide), toluenesulfonyl hydrazide, and toluenesulfonyl hydrazide derivatives. You may use together a foaming agent and foaming aids, such as a salicylic acid, urea, and a urea derivative.

  If necessary, a high-frequency processing aid such as a polar polymer may be added to the pressure-sensitive adhesive composition of the present invention. Examples of the high-frequency processing aid include a copolymer of ethylene and at least one comonomer. Comonomers include monocarboxylic acids such as acrylic acid, methacrylic acid, ethacrylic acid, and crotonic acid; dicarboxylic acids such as maleic acid, fumaric acid, itaconic acid, and citraconic acid; monoesters of the above dicarboxylic acids; methacrylic acids such as methyl methacrylate Examples include esters; acrylic acid esters such as methyl acrylate and ethyl acrylate; vinyl esters of saturated carboxylic acids such as vinyl acetate and vinyl propionate; and ionomers of these acids and esters.

  If necessary, a tackifier may be added to the pressure-sensitive adhesive composition of the present invention. Tackifiers include natural rosin resins such as rosin and dammar; modified rosin and its attractant; terpene resin and its modified body; aliphatic hydrocarbon resin, aromatic hydrocarbon resin, alkylphenol resin, chromanindene resin Etc. are exemplified. Among these, terpenes such as terpene phenol and α-polyterpene are preferable. Examples of terpenes include YS Resin TO-105, Clearon (above, trade name manufactured by Yashara Chemical Co., Ltd.), Alcon, Ester Gum and Pencel (above, trade name manufactured by Arakawa Chemical Co., Ltd.).

  The pressure-sensitive adhesive composition of the present invention may be used alone to form a single-layer body, and has at least one pressure-sensitive adhesive layer containing the pressure-sensitive adhesive composition of the present invention as an outermost layer, as a multilayer laminate of at least two layers. Also good. In the above multilayer laminate, the materials constituting the layers other than at least one layer containing the pressure-sensitive adhesive composition of the present invention may be the same or different. Examples of the material constituting the layer other than at least one layer containing the pressure-sensitive adhesive composition of the present invention include other known thermoplastic resins, rubbers and other components other than the pressure-sensitive adhesive composition of the present invention.

  Examples of the thermoplastic resin include various polyethylene resins, various polypropylene resins, various polybutene resins, various polymethylpentene resins, polystyrene resins, copolymer resins of ethylene and acrylic monomers, and ethylene-acetic acid. Examples include vinyl copolymer resins, ethylene-methacrylic acid monomer copolymer resins, acrylic resins, polyester resins, polycarbonate resins, nylon resins, polyvinyl alcohol resins, and the like. -Olefin copolymer rubber, ethylene / α-olefin / polyene copolymer rubber, styrene rubber, hydrogenated styrene rubber, diene rubber, known cross-linkable rubber, etc. Examples thereof include woven fabric and non-woven fabric.

  In addition, the above thermoplastic resin, rubber, and other components include various stabilizers, various additives, fillers, mineral oil softeners, flame retardants, high frequency processing aids, rosin resins, polyterpene resins, synthetics Petroleum resin, coumarone-based resin, phenol-based resin, xylene-based resin, isoprene-based resin and the like may be appropriately blended.

As the above multilayer laminate, preferably, a laminate having at least one layer containing the composition for pressure-sensitive adhesives of the present invention on one side of the base material layer, or a composition for pressure-sensitive adhesives of the present invention on both sides of the base material layer. It is a laminated body which has at least 1 layer containing.
The material constituting the base material layer is preferably a polyolefin polymer from the viewpoint of the recyclability of the multilayer laminate.

  The base material layer may be a single layer or a multilayer composed of at least two layers. Moreover, the surface of said base material layer may be processed by well-known surface treatment methods, such as a corona discharge process, a plasma process, a flame process, an electron beam irradiation process, and an ultraviolet irradiation process. The base material layer may be a colorless and transparent layer, or may be a colored layer or a printed layer.

  As a method for producing a multilayer laminate having a pressure-sensitive adhesive layer containing the pressure-sensitive adhesive composition of the present invention, a substrate layer and the pressure-sensitive adhesive of the present invention are prepared using an apparatus such as an inflation film production apparatus or a T-die film production apparatus. Examples thereof include a method of co-extrusion with a pressure-sensitive adhesive layer containing the composition for extrusion and a method of extrusion coating (also referred to as extrusion lamination method).

  Said base material layer may be extended | stretched in the uniaxial direction or the biaxial direction as needed. Examples of the uniaxial stretching method include a normal roll stretching method, and examples of the biaxial stretching method include a sequential stretching method in which biaxial stretching is performed after uniaxial stretching, and a simultaneous biaxial stretching method such as a tubular stretching method. .

As thickness of the multilayer laminated body which has an adhesive layer containing the composition for adhesives of this invention, it is about 0.001-5 mm normally, Preferably it is about 0.005-2 mm.
The thicknesses of the base material layer and the pressure-sensitive adhesive layer may be determined according to the type of adherend and the physical properties required for the pressure-sensitive adhesive film (for example, pressure-sensitive adhesive strength).

In the case of producing a multilayer laminate having an adhesive layer containing the adhesive composition of the present invention as a rolled up roll, from the viewpoint of ease of pulling out an adhesive film from the roll, that is, from the viewpoint of self-peeling, Release paper may be sandwiched between the scrolls, or a release agent may be applied to the back surface of the base material layer.
Examples of the release agent include silicone release agents and non-silicone release agents. Examples of silicone release agents include thermosetting silicone release agents, photocurable silicone release agents, copolymer release agents with other polymers, and blend release agents with other polymers. Examples of the non-silicone release agent include release agents mainly composed of long-chain alkyl polymers, polyolefins, and fluorine compounds.

  If necessary, an additive such as a release agent may be added to the thermoplastic resin used for the base material layer in order to impart a function such as slipperiness to the surface of the base material layer.

  The multilayer laminate having the pressure-sensitive adhesive layer containing the pressure-sensitive adhesive composition of the present invention is used in the electronics field such as semiconductor wafer back grinding tape, dicing tape, electronic component transport protection tape, and printed circuit board protection tape. Applications: Window glass protective film, baking coating film, guard film for protecting automobiles to users, marking film for display, decorative marking film, automobiles such as sponge tape for cushioning / protection / insulation / soundproofing Applications in the field; applications in the field of medical and hygiene materials such as adhesive bandages and transdermal patches; electrical insulation, identification, duct construction, window glass protection, curing, packaging, packaging, office use Examples of applications in the housing and construction fields such as household, fixing, binding, and repair adhesive films and protective films.

  Especially as a use of the multilayer laminated body which has an adhesive layer containing the composition for adhesives of this invention, Preferably, a synthetic resin board, a stainless steel board (for example, for building materials), an aluminum board, a decorative plywood, a steel plate, glass Film used to protect the surface of plates, home appliances, precision machinery, automobile bodies during manufacturing, etc .; Film used to prevent scratches when stacking, storing, or transporting articles A film used to prevent scratching when secondary processing of the article (for example, bending or pressing).

Hereinafter, the present invention will be described in more detail with reference to Examples and Comparative Examples.
The physical properties of the present invention were measured by the following method.
(1) Monomer composition of amorphous olefin polymer (unit: mol%)
It calculated based on the measurement result of a < ¹³ > C-NMR spectrum using the nuclear magnetic resonance apparatus (Bruker brand name AC-250). Specifically, in the ¹³ C-NMR spectrum, the composition ratio of the propylene unit and the 1-butene unit was calculated from the intensity ratio of the methyl carbon spectrum derived from the propylene unit and the methyl carbon spectrum derived from the 1-butene unit.

(2) Intrinsic viscosity ([η], unit: dl / g)
The measurement was performed at 135 ° C. using an Ubbelohde viscometer. A tetralin solution of an amorphous olefin polymer having an amorphous olefin polymer concentration c per unit volume of tetralin of 0.6, 1.0, 1.5 mg / ml was prepared, and the limit at 135 ° C. The viscosity was measured. The measurement was repeated three times at each concentration, the average value of the three values obtained was taken as the specific viscosity (η _sp ) at that concentration, and the value obtained by extrapolating c of η _sp / c to zero was used as the intrinsic viscosity [η ]

(3) Molecular weight distribution It measured by the gel permeation chromatograph (GPC) method on the following conditions.
Apparatus: 150C ALC / GPC manufactured by Waters
Column: Shodex Packed Column A-80M manufactured by Showa Denko KK
Two temperature: 140 ° C
Solvent: o-dichlorobenzene elution solvent flow rate: 1.0 ml / min
Sample concentration: 1 mg / ml
Measurement injection volume: 400 μl
Molecular weight reference material: Standard polystyrene detector: Differential refraction

(4) Crystal melting peak (unit: ° C), crystal melting heat (unit: J / g), crystallization peak (unit: ° C), crystallization heat (unit: J / g)
It measured on condition of the following using the differential scanning calorimeter (Seiko Electronics Co., Ltd. DSC220C: input compensation DSC).
(I) About 5 mg of the sample was heated from room temperature to 200 ° C. at a temperature increase rate of 30 ° C./min, and held for 5 minutes after the temperature increase was completed.
(Ii) Next, the temperature was decreased from 200 ° C. to −100 ° C. at a rate of temperature decrease of 10 ° C./min, and held for 5 minutes after the temperature decrease was completed. The peak observed in (ii) was a crystallization peak, and the presence or absence of a crystallization peak with a peak area of 1 J / g or more was confirmed.
(Iii) Next, the temperature was increased from −100 ° C. to 200 ° C. at a temperature increase rate of 10 ° C./min. The peak observed in (iii) was a melting peak of crystals, and the presence or absence of a melting peak having a peak area of 1 J / g or more was confirmed.

(5) Melt flow rate (MFR, unit: g / 10 min)
According to JIS-K-7210, the measurement was performed under the conditions of a load of 21.18 N and a temperature of 230 ° C.

(6) Peel strength of adhesive film (adhesive strength, unit: N / 25 mm width)
According to JIS-Z-0237, 180 degree peeling adhesive strength between the adhesive film and the SUS304 steel plate was measured in an atmosphere of −10 ° C., 23 ° C. and 60 ° C.

Example 1
[1] Production of Amorphous Olefin Polymer In a 100 L SUS polymerizer equipped with a stirrer, propylene and 1-butene were continuously copolymerized by the following method using hydrogen as a molecular weight control. Thus, a propylene-1-butene copolymer corresponding to the amorphous α-olefin polymer of the present invention was obtained.
From the lower part of the polymerization vessel, hexane as a polymerization solvent was continuously fed at a feeding rate of 100 L / hour, propylene was fed at a feeding rate of 24.00 Kg / hour, and 1-butene was fed at a feeding rate of 1.81 Kg / hour. Supplied.
From the top of the polymerization vessel, the reaction mixture was continuously withdrawn so that the reaction mixture in the polymerization vessel maintained an amount of 100 L.
From the lower part of the polymerization vessel, as a component of the polymerization catalyst, dimethylsilyl (tetramethylcyclopentadienyl) (3-tert-butyl-5-methyl-2-phenoxy) titanium dichloride is supplied at a rate of 0.005 g / hour, Triphenylmethyltetrakis (pentafluorophenyl) borate was continuously fed at a feed rate of 0.298 g / hr and triisobutylaluminum was fed at a feed rate of 2.315 g / hr.
The copolymerization reaction was carried out at 45 ° C. by circulating cooling water through a jacket attached to the outside of the polymerization vessel.
Stop the polymerization reaction by adding a small amount of ethanol to the reaction mixture continuously extracted from the top of the polymerization vessel, then de-monomerize and wash with water, and then remove the solvent with steam in a large amount of water. To obtain a propylene-1-butene copolymer, which was dried under reduced pressure at 80 ° C. for 1 day. The production rate of the copolymer was 7.10 kg / hour.
The physical property evaluation results of the resulting propylene-1-butene copolymer are shown in Table 1.
When x is the content (mol%) of the ethylene unit in the copolymer and y is the content (mol%) of the α-olefin unit having 4 to 20 carbon atoms, x = 0 and y = 4. Yes, [y / (x + y)] = 1, which indicates that the requirement of component (A) is satisfied.

[2] Production of composition for pressure-sensitive adhesive 99 parts by weight of amorphous propylene-1-butene copolymer produced by the above method and hydrogenated styrene-butadiene block copolymer (Tuftec H1052, manufactured by Asahi Kasei Chemicals Corporation, containing styrene units) 20 wt%, MFR (230 ° C.) = 13 g / 10 min) and 1 part by weight, and using a kneader having a brand name of Plasticorder PLV151 manufactured by Brabender, 200 at a screw speed of 10 rpm. After kneading for 2 minutes at 0 ° C., the mixture was further kneaded for 5 minutes at 100 rpm to obtain a pressure-sensitive adhesive composition.

[3] Manufacture of pressure-sensitive adhesive film A composition for pressure-sensitive adhesives as a pressure-sensitive adhesive layer, and a polypropylene resin (Excellen EPX EP3725, Sumitomo Chemical Co., Ltd., MFR (230 ° C.) = 2.5 g / 10 minutes, manufactured by Sumitomo Chemical Co., Ltd.) as a base material layer Each was formed into a film having a thickness of 100 μm, and both were bonded together, and then heat-sealed by press molding at 150 ° C. to obtain an adhesive film. Table 2 shows the physical properties of this adhesive film.

Comparative Example 1
The same procedure as in Example 1 was performed except that 100 parts by weight of the amorphous propylene-1-butene copolymer produced by the above method was used as the pressure-sensitive adhesive composition.

In Example 1, it can be seen that the composition satisfying the requirements of the present invention has high adhesive force and low temperature dependency of adhesive force.
On the other hand, Comparative Example 1 is a composition that does not use the component (B) that is a requirement of the present invention.

Claims (3)

For pressure-sensitive adhesive containing 97 to 99.9% by weight of the following amorphous olefin polymer (component (A)) and 0.1 to 3% by weight of the following block copolymer (component (B)) Composition (however, the total weight of the pressure-sensitive adhesive composition is 100% by weight).
Component (A) is an amorphous olefin system obtained by copolymerizing at least two olefins selected from the group consisting of ethylene and α-olefins having 3 to 20 carbon atoms, and having a molecular weight distribution of 3 or less. It is a polymer.
Component (B) is at least one resin selected from the group consisting of vinyl aromatic-conjugated diene block copolymers and hydrogenated products of vinyl aromatic-conjugated diene block copolymers. The amorphous olefin polymer (component (A)) is obtained by copolymerizing olefins having a total of 6 or more carbon atoms in at least two selected olefins, and has the relationship of the following formula (1) The composition for pressure-sensitive adhesives according to claim 1, which is an amorphous olefin polymer satisfying the formula.
[Y / (x + y)] ≧ 0.3 Formula (1)
(In Formula (1), x represents content (mol%) of the structural unit derived from ethylene contained in a component (A), and y is C4-C20 contained in a component (A). This represents the content (mol%) of structural units derived from α-olefin, provided that the total content of structural units derived from olefins contained in component (A) is 100 mol%.   The amorphous olefin polymer (component (A)) is an amorphous propylene polymer obtained by copolymerizing propylene and at least one α-olefin having 4 to 20 carbon atoms. Item 2. The pressure-sensitive adhesive composition according to Item 1.