JPH1161071A - Hardenable pressure-sensitive adhesive composition - Google Patents

Abstract

PROBLEM TO BE SOLVED: To obtain a hardenable pressure-sensitive adhesive compsn. excellent in heat stability by incorporating a linear block copolymer compsn. contg. a specified amt. of a coupling component and a tackifying resin, each in a specified amt., into the same. SOLUTION: This compsn. contains 100 pts.wt. linear block copolymer compsn. contg. 10-99 wt.% coupling component and 20-400 pts.wt. tackifying resin (e.g. a coumarone resin). The linear block copolymer compsn. is prepd. by the coupling reaction of a living polymer with a silicon compd. represented by the formula: R<1> R<2> SiX2 (R<1> is an arom. hydrocarbon group; R<2> is alkyl, H or the like; and X is halogen) such as diphenyldichlorosilane. The living polymer is obtd. by polymerizing a block copolymer comprising polymer blocks contg. arom. vinyl compd. (e.g. styrene) units and blocks contg. conjugated diene (e.g. butadiene) units and has a peak mol.wt. (by gel permeation chromatography, in terms of standard polystyrene) of 1×40<4> -50×10<4> and a content of total arom. vinyl compd. units of 10-50 wt.%.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

[0001] The present invention relates to a color tone, transparency, and the like based on a block copolymer composition having a specific structure which is coupled with a specific bifunctional coupling agent.
The present invention relates to a pressure-sensitive adhesive composition having excellent heat stability and excellent balance between holding power, tackiness and melt viscosity.

[0002]

2. Description of the Related Art In recent years, hot-melt adhesives have been widely used from the viewpoint of environmental pollution and working environment. An aromatic vinyl-conjugated diene-based block copolymer (SBS) is widely used as a base polymer of a hot-melt adhesive. However, SB
S is generally inferior in thermal stability and insufficient in balance between holding power, tackiness, and melt viscosity, and improvement of these has been desired. Japanese Patent Application Laid-Open No. Sho 64-8 discloses these improved methods.
No. 1877 and “Adhesion” (Vol. 32, No. 1, page 27 ('
88)) discloses an adhesive composition comprising a triblock copolymer and a diblock copolymer. Further, JP-A-61-42582 discloses an adhesive composition comprising a block copolymer obtained by coupling with a specific bifunctional coupling agent (a specific dihalogen compound). I have.

[0003]

However, any of the methods disclosed above have not been sufficiently effective. Against this background, the present invention aims to provide a pressure-sensitive adhesive composition having excellent color tone, transparency, and thermal stability, as well as excellent balance between holding power, tackiness, and melt viscosity. is there.

[0004]

Means for Solving the Problems The inventors of the present invention have conducted intensive studies to develop the above-mentioned preferred adhesive composition, and as a result, they have been coupled with a specific bifunctional silane compound. The present inventors have found that an adhesive composition comprising an aromatic vinyl-conjugated diene-based block copolymer composition having a specific structure is suitable for the purpose, and based on this finding, have completed the present invention. Reached.

That is, the present invention provides (a) a polymer obtained by polymerizing a block copolymer composed of at least one polymer block mainly composed of an aromatic vinyl compound and at least one block mainly composed of a conjugated diene. The peak molecular weight in gel permeation chromatography (GPC) is 1 × 10 ⁴ to 50 in terms of standard polystyrene.
× 10 ⁴ , and the total amount of the wholly aromatic vinyl compound is 10 to 50% by weight. A line obtained by performing a coupling reaction between a living polymer and a silicon compound represented by the following general formula (I): A linear block copolymer composition, wherein the coupled component in the linear block copolymer composition is 10% by weight or more and 99% by weight or less, 100 parts by weight of a linear block copolymer composition; (B) An adhesive composition comprising 20 to 400 parts by weight of a tackifying resin. R ¹ R ² SiX ₂ (I) wherein R ¹ represents an aromatic hydrocarbon group, R ² represents an alkyl group or an aromatic hydrocarbon group or hydrogen, and X represents a halogen. ]

Hereinafter, the present invention will be described in detail. The component (a) constituting the present invention is a gel obtained by polymerizing a block copolymer composed of at least one polymer block mainly composed of an aromatic vinyl compound and at least one block mainly composed of a conjugated diene. The peak molecular weight in permeation chromatography (GPC) is 1 × 10 ⁴ to 50 × 10 ⁴ in terms of standard polystyrene;
The total amount of the aromatic vinyl compound is 10 to 50% by weight, and the living polymer is obtained by coupling reaction with a silicon compound represented by the following general formula (I). R ¹ R ² SiX ₂ (I) wherein R ¹ represents an aromatic hydrocarbon group, R ² represents an alkyl group or an aromatic hydrocarbon group or hydrogen, and X represents a halogen. ]

The aromatic vinyl compound used in the component (a) includes, for example, styrene, P-methylstyrene,
Tertiary butylstyrene, α-methylstyrene, 1,1-
Examples include monomers such as diphenylethylene, and among them, styrene is preferred. These monomers may be used alone or in combination of two or more. On the other hand, examples of the conjugated diene include 1,3-butadiene, isoprene, 2,3-dimethyl-1,3-butadiene, piperylene, and 3-butyl-
Monomers such as 1,3-octadiene, phenyl-1,3-butadiene and the like are exemplified, and among them, 1,3-butadiene and isoprene are preferred. These monomers may be used alone or in combination of two or more.

The embodiment of the living polymer in the component (a) is, for example, represented by the following general formula alone or in combination. (AB) m-Li (BAB) m-Li (ABA) m-Li (where A is a polymer block mainly composed of aromatic vinyl, and B is conjugated A polymer block mainly composed of a diene, and m is an integer of 1 to 5.) A polymer block mainly composed of an aromatic vinyl compound is an aromatic block containing 50 to 100% by weight of an aromatic vinyl compound. A vinyl compound alone or a copolymer block with butadiene.

The polymer block mainly composed of a conjugated diene is a butadiene compound alone containing 50 to 100% by weight of a conjugated diene or a copolymer block with an aromatic vinyl compound. The aromatic vinyl hydrocarbons in the copolymer block may be distributed uniformly or non-uniformly (for example, in a tapered shape).

In addition to the coupling reaction of the living polymer represented by the above general formula, living polymers having different composition ratios (structures) are separately adjusted according to the purpose, and the coupling reaction is carried out. Composition (structure) by additional polymerization of monomer and organolithium compound
May be prepared and subjected to a coupling reaction. Further, the living polymer represented by the above general formula may be subjected to a coupling reaction with a (co) polymer living polymer mainly composed of an aromatic vinyl compound or a (co) polymer living polymer mainly composed of a conjugated diene.

In the present invention, the peak molecular weight by GPC of the block copolymer immediately before coupling is 1 × 10 ⁴ to 50 × 10 ⁴ , preferably 3 × 10 ⁴ to 30 × 10 ⁴ in terms of standard polystyrene. . If the peak molecular weight is less than 1 × 10 ⁴ , the holding power of the adhesive composition is significantly impaired, and if it exceeds 50 × 10 ⁴ , the melt viscosity of the adhesive composition becomes extremely high, impairing processability. . In the component (a), the total amount of the block copolymer just before the coupling and the total aromatic vinyl compound in the linear block copolymer composition after the coupling reaction is 10 to 50% by weight, preferably 15 to 40% by weight. It is selected in the range of weight%. If the total amount is less than 10%, the holding power of the pressure-sensitive adhesive composition is significantly impaired, and if it exceeds 50%, the tackiness of the adhesive composition is impaired.

The silane compound used in the component (a) is a silane compound having a structure represented by the following general formula (I). R ¹ R ² SiX ₂ (I) wherein R ¹ represents an aromatic hydrocarbon group, R ² represents an alkyl group or an aromatic hydrocarbon group or hydrogen, and X represents a halogen. The present inventors have made intensive studies on the color tone, especially the heat discoloration property of the adhesive composition, and as a result, the aromatic-based substituents were subjected to thermal degradation when the adhesive was prepared. Having found that the composition has extremely excellent thermal stability, and further studying the same, a block copolymer composition coupled with a silane compound having a specific structure of the present invention and an adhesive comprising the block copolymer composition The inventors have invented the composition.

In this silane compound, it is essential that R ¹ is an aromatic hydrocarbon group. When a silane compound having one or more aromatic hydrocarbon groups as in the present invention is used as compared with the case where both R ¹ and R ² use a silane compound having an aliphatic hydrocarbon group, In addition, heat resistance is greatly improved, and very good performance can be exhibited when obtaining a hot melt type adhesive composition. That is, the hot-melt type adhesive is heated and melted at the time of production and use, so that there is a problem in that the adhesive undergoes heat history and performance degradation such as discoloration occurs. However, since the composition of the present invention uses the above-mentioned specific coupling agent, performance deterioration such as discoloration is greatly reduced.

Examples of the aromatic hydrocarbon group include a phenyl group, a tolyl group, a xylyl group, a mesityl group, a cumenyl group,
Benzyl groups, phenethyl groups and derivatives thereof are preferred,
Further, a phenyl group is preferred. R ² must be an alkyl group, an aromatic hydrocarbon group or hydrogen. As the aromatic hydrocarbon group, those similar to the aforementioned R ¹ are suitably used. More preferably likewise a phenyl group and R ^1. R ¹ and R ² may be the same group,
Also, a different group may be used.

The alkyl group must have 1 to 20 carbon atoms. If the number of carbon atoms is larger than this, the reactivity of the silane compound becomes low, and a sufficient coupling reaction does not occur. As the alkyl group having 1 to 20 carbon atoms, all alkyl groups including isomers such as methyl group, ethyl group, n-propyl group and iso-propyl group can be used. Among them, an alkyl group having 1 to 6 carbon atoms is desirable, and a methyl group is particularly desirable. Furthermore, X must be a halogen. Halogen is preferably chlorine, bromine or iodine, and chlorine is particularly preferred because of its high reactivity.

Specifically, diphenyldichlorosilane,
Phenylmethyldichlorosilane, phenyldichlorosilane, phenylethyldichlorosilane, phenylpropyldichlorosilane, tolylmethyldichlorosilane, ditolyldichlorosilane, diphenyldibromosilane, phenylmethyldibromosilane, phenyldibromosilane, phenylethyldibromosilane, phenylpropyldibromosilane, Tolmethyldibromosilane, ditolyldibromosilane and the like can be mentioned.

In the present invention, the ratio of the coupled component of the component (a) must be 10% by weight or more and 99% by weight or less. If the content is less than 10% by weight, the holding power of the adhesive composition cannot be sufficiently obtained because the coupled components are insufficient. It is preferably at least 15% by weight, more preferably at least 20% by weight. On the other hand, when the content exceeds 99% by weight, the tackiness of the adhesive composition cannot be sufficiently obtained because the uncoupled component is insufficient. Preferably, 9
It is 8% by weight, more preferably 95% by weight or less. In addition, the block copolymer obtained by the coupling reaction of the component (a) includes a hydrogenated block copolymer,
Also included are linear block copolymers modified with a modifying agent such as maleic anhydride.

The type of component (b) constituting the present invention is not particularly limited, and may be (hydrogenated) rosin-based terpene-based resin, cumarone-based resin, phenol-based resin, terpene-phenol-based resin, or aromatic. Known tackifying resins such as an aliphatic hydrocarbon resin and an aliphatic hydrocarbon resin may be mentioned, and two or more kinds of these tackifying resins may be used in combination. As the amount of the component (b) used,
(A) It is used in an amount of 20 to 400 parts by weight, preferably 50 to 350 parts by weight, per 100 parts by weight of the component. If the amount used is less than 20 parts by weight, it is difficult to impart a tacky feeling to the adhesive composition, and if it exceeds 400 parts by weight, the holding power of the adhesive composition is reduced, and in any case, This tends to impair the adhesive properties.

The composition of the present invention can use a known naphthene-based or paraffin-based process oil or a mixed oil thereof as a softener. By adding a softener, the viscosity of the composition is reduced, so that the processability is improved and the tackiness is improved. An aroma system is not preferred because it impairs the color tone and heat stability of the adhesive composition. The amount used is from 0 to 200 with respect to the component (a).
When used in an amount of 200 parts by weight, the holding power of the adhesive composition tends to be significantly impaired. Furthermore, stabilizers such as antioxidants and light stabilizers can be added to the adhesive composition of the present invention, if necessary.

Examples of the antioxidant include 2,6-di-t-butyl-4-methylphenol, n-octadecyl-3- (4'-hydroxy-3 ', 5'-di-t-butylphenyl ) Propionate, 2,2′-methylenebis (4-methyl-6-t-butylphenol),
2'-methylenebis (4-ethyl-6-t-butylphenol), 2,4-bis [(octylthio) methyl]-
0-cresol, 2-tert-butyl-6- (3-tert-butyl-2-hydroxy-5-methylbenzyl) -4-methylphenylacrylate, 2,4-di-tert-amyl-6
-[1- (3,5-di-t-amyl-2-hydroxyphenyl) ethyl] phenyl acrylate, 2- [1-
(2-hydroxy-3,5-di-tert-pentylphenyl)] hindered phenolic antioxidants such as acrylate; dilauryl thiodipropionate, lauryl stearyl thiodipropionate pentaerythritol-tetrakis (β-laurylthio) And sulfur-based antioxidants such as tris (nonylphenyl) phosphite and tris (2,4-di-t-butylphenyl) phosphite.

As the light stabilizer, for example, 2-
(2′-hydroxy-5′-methylphenyl) benzotriazole, 2- (2′-hydroxy-3 ′, 5′-t
-Butylphenyl) benzotriazole, 2- (2'-
Hydroxy-3 ′, 5′-di-tert-butylphenyl)-
Benzotriazole ultraviolet absorbers such as 5-chlorobenzotriazole; benzophenone ultraviolet absorbers such as 2-hydroxy-4-methoxybenzophenone; and hindered amine light stabilizers.

In addition to the above stabilizers, the adhesive composition of the present invention may optionally contain pigments such as red iron oxide and titanium dioxide; waxes such as paraffin wax, microcrystalline wax and low molecular weight polyethylene wax; Polyolefin or low molecular weight vinyl aromatic thermoplastic resin such as polyolefin or ethylene-ethyl acrylate copolymer; natural rubber; polyisoprene rubber, polybutadiene rubber, styrene butadiene rubber, ethylene-propylene rubber, chloroprene rubber, acrylic rubber Synthetic rubbers such as isoprene-isobutylene rubber, polypentenamer rubber, and styrene-isoprene-based block copolymers other than the present invention may be added. The adhesive composition of the present invention is prepared by a method of uniformly mixing under heating using a known mixer, kneader or the like.

[0023]

EXAMPLES The present invention will be described below with reference to examples and the like, but these examples and the like do not limit the present invention in any way. In addition, various measurements followed the following method. 1. Measurement of physical properties of linear block copolymer composition 1) Total styrene content: UV spectrophotometer (UV manufactured by Hitachi, Ltd.)
200) and was calculated from the absorption intensity at 262 nm. 2) Peak molecular weight and composition ratio: GPC [The apparatus is manufactured by Waters, and the column is ZORBA manufactured by DuPont.
X Two PSMIOOO-S and one PSM60-S
This is a total of three books. Tetrahydrofuran was used as the solvent, and the measurement conditions were a temperature of 35 ° C. and a flow rate of 0.7 ml /
, A sample concentration of 0.1% by weight, and an injection amount of 50 μl], the peak molecular weight and the composition ratio were determined. The peak molecular weight is a value converted from the following standard polystyrene (manufactured by Waters) calibration curve. 1.75 × 10 ⁶ , 4.1 × 10 ⁵ , 1.12 × 10 ⁵ , 3.5 × 10 ⁴ , 8.5 × 10 ³

2. Measurement of physical properties of the adhesive composition Take it out in a molten state, coat it on a polyester film to a thickness of 50 micrometers with an applicator, make an adhesive tape sample, and measure the color tone, tackiness, holding power, etc. by the following method Was measured. 1) Color Tone The color tone of the adhesive composition was examined and ranked into four grades of 段 階, Δ, ×, XX (○ is the least change in color tone and is excellent). 2) Tack feeling Three ranks of ○, Δ, and X (（is the most sticky and excellent) were given by the touch finger.

3) Holding force The holding force is determined according to JIS Z-1524 by applying an adhesive tape to a stainless steel plate so that an area of 25 mm × 25 mm is in contact with the stainless steel plate and applying a load of 1 kg at 80 ° C. to shift the adhesive tape. The time to fall was measured. 4) Melt Viscosity The melt viscosity of the adhesive composition was measured at 180 ° C. using a Brookfield viscometer. 5) Thermal stability The thermal stability of the adhesive composition was measured by placing it in a gear oven at 190 ° C. and aging for 24 hours.
△, ×, XX (○ has the least change in color tone and is excellent)
4 ranks.

Example 1 A 10-liter stainless steel reactor equipped with a jacket and a stirrer was sufficiently purged with nitrogen, 7000 cc of cyclohexane and 1.4 of tetrahydrofuran.
g of styrene and 350 g of styrene, and warm water was passed through the jacket to set the contents at about 70 ° C. Thereafter, an n-butyllithium cyclohexane solution (1.6 g in pure content) was added to initiate polymerization of styrene. After the styrene has completely polymerized, butadiene (1,3-butadiene) 65
0 g was added to continue the polymerization, and after butadiene was almost completely polymerized, phenylmethyldichlorosilane was added as a coupling agent to effect coupling. After addition of the coupling agent, 0.5 g of water was added. Immediately after charging the styrene, the system was continuously stirred with a stirrer during this period. Thereafter, the solution of the block copolymer composition was withdrawn, and 1.9 g of 2,6-di-t-butyl-4-methylphenol and 1.1 g of tris (nonylphenyl) phosphite were obtained.
2 g was added, and the obtained solution was subjected to steam stripping to remove the solvent, followed by dehydration and drying with a hot roll (120 ° C.) to obtain a block copolymer. The styrene content of the block copolymer composition thus obtained was 35% by weight, and the peak molecular weight (hereinafter, simply referred to as peak molecular weight) of the coupled block copolymer was 142,000. The ratio of the coupled components in the total block copolymer (hereinafter, simply referred to as the coupling ratio) was 30% by weight. 150 g of the obtained block copolymer was used as the block copolymer 1
300 parts by weight of Clearon M105 (manufactured by Yasuhara Yushi) as a tackifying resin, 50 parts by weight of Diana Process Oil PW-90 (manufactured by Idemitsu Kosan: trade name) as a softener, based on 00 parts by weight. Further, as an antioxidant, Irganox 1010 (manufactured by Ciba Geigy: trade name)
At a mixing ratio of 1 part by weight, 180 ° C. × 2 hours, 1
The mixture was melted and kneaded in a 1-liter container equipped with a stirrer to obtain a hot-melt adhesive composition. As a result of measuring the physical properties of these adhesive compositions, the holding power was 14 minutes, and the melt viscosity was 1450.
cps. The color tone of the adhesive was 粘, the tackiness was ○, and the thermal stability was ○. Table 1 shows the polymerization conditions.
Table 2 shows the results of analysis of the obtained copolymer, and Table 3 shows the results of measurement of physical properties of the adhesive.

Examples 2 to 4 Polymerization was carried out under the same conditions as in Example 1 except for the conditions shown in Table 1, and each block copolymer was obtained by the same operation. Table 2 shows the analysis results of the obtained block copolymer. Further, a hot melt type adhesive composition was obtained in the same manner as in Example 1. Table 3 shows the measurement results of the physical properties of the adhesive composition.

(Example 5) A 10-liter stainless steel reactor equipped with a jacket and a stirrer was sufficiently purged with nitrogen, 7000 cc of cyclohexane and 1.4 of tetrahydrofuran.
g, tetramethylene diamine (TMEDA) 0.7 g,
270 g of styrene was charged, and warm water was passed through the jacket to set the content at about 70 ° C. Thereafter, an n-butyllithium cyclohexane solution (1.5 g in pure content) was added, and polymerization of styrene was started. After the styrene has completely polymerized, butadiene (1,3-butadiene) 700
g and 30 g of styrene (referred to as second styrene) were added to continue the polymerization, and after butadiene and the second styrene were almost completely polymerized, phenylmethyldichlorosilane was added as a coupling agent and coupled. . After addition of the coupling agent, 0.5 g of water was added. Immediately after charging the styrene, the system was continuously stirred with a stirrer during this period. Thereafter, a solution of the block copolymer composition was withdrawn, and 1.9 g of 2,6-di-t-butyl-4-methylphenol and 1.2 g of tris (nonylphenyl) phosphite were added. Was subjected to steam stripping to remove the solvent, followed by dehydration and drying with a hot roll (120 ° C.) to obtain a block copolymer. The styrene content of the block copolymer composition thus obtained was 30% by weight, and the peak molecular weight was 176.
000. The coupling ratio was 70% by weight. The same operation as in Example 1 was performed using 150 g of the obtained block copolymer to obtain a hot-melt adhesive composition. As a result of measuring the physical properties of these adhesive compositions, the holding power was 19 minutes, and the melt viscosity was 3200 cps.
Met. The color tone of the adhesive is ○, the tackiness is 、,
The thermal stability was also good. Table 1 shows the polymerization conditions, Table 2 shows the analysis results of the obtained copolymer, and Table 3 shows the measurement results of the physical properties of the adhesive.

(Example 6) Polymerization was carried out under the same conditions as in Example 1 except that diphenyldichlorosilane was used as a coupling agent to obtain a block copolymer. Table 2 shows the analysis results of the obtained block copolymer. The same operation as in Example 1 was performed using 150 g of the obtained block copolymer to obtain a hot-melt adhesive composition. As a result of measuring the physical properties of these adhesive compositions, the holding power was 15 minutes, and the melt viscosity was 1550 cps. The color tone of the adhesive was 粘, the tackiness was ○, and the thermal stability was ○.

Example 7 Polymerization was carried out under the same conditions as in Example 1 except that phenyldichlorosilane was used as a coupling agent, to obtain a block copolymer. Table 2 shows the analysis results of the obtained block copolymer. The same operation as in Example 1 was performed using 150 g of the obtained block copolymer to obtain a hot-melt adhesive composition. Table 3 shows the measurement results of the physical properties of these adhesive compositions.

(Comparative Example 1) After sufficiently replacing a 10-liter stainless steel reactor equipped with a jacket and a stirrer with nitrogen, 7000 cc of cyclohexane and 1.4 of tetrahydrofuran were obtained.
g and 150 g of styrene, and warm water was passed through the jacket to set the contents at about 70 ° C. Thereafter, an n-butyllithium cyclohexane solution (1.0 g in pure content) was added to initiate polymerization of styrene. After the styrene has completely polymerized, butadiene (1,3-butadiene) 70
0 g is added to continue the polymerization, and after butadiene is almost completely polymerized, 150 g of styrene (hereinafter referred to as third styrene) is further added to continue the polymerization. After the tertiary styrene had almost completely polymerized, 0.5 g of water was added. Immediately after charging the first styrene, the inside of the system was continuously stirred with a stirrer during this period. Thereafter, the solution of the block copolymer composition was withdrawn and 2,6-di-t-butyl-4-.
1.9 g of methylphenol, tris (nonylphenyl)
1.2 g of phosphite was added, the obtained solution was subjected to steam stripping to remove the solvent, and subsequently dehydrated and dried with a hot roll (120 ° C.) to obtain a block copolymer. The styrene content of the block copolymer composition thus obtained was 30% by weight, and the peak molecular weight was 102,000. In addition, it was confirmed by GPC that no coupling was performed. The same operation as in Example 1 was performed using 150 g of the obtained block copolymer to obtain a hot-melt adhesive composition. Table 3 shows the measurement results of the physical properties of these adhesive compositions.

Comparative Example 2 Polymerization was carried out under the same conditions as in Comparative Example 1 except for the conditions shown in Table 1, and a block copolymer was obtained by the same operation. Table 2 shows the analysis results of the obtained block copolymer. Further, a hot melt type adhesive composition was obtained in the same manner as in Example 1. Table 3 shows the measurement results of the physical properties of the adhesive composition.

Comparative Example 3 Polymerization was carried out under the same conditions as in Example 1 except that dimethyldichlorosilane was used as a coupling agent, and a block copolymer was obtained by the same operation. Table 2 shows the analysis results of the obtained block copolymer. Further, a hot melt type adhesive composition was obtained in the same manner as in Example 1. Table 3 shows the measurement results of the physical properties of the adhesive composition.
Shown in

Comparative Example 4 Polymerization was conducted under the same conditions as in Comparative Example 3 except that ethyl acetate was used as a coupling agent.
A block copolymer was obtained by the same operation. Table 2 shows the analysis results of the obtained block copolymer. Further, a hot melt type adhesive composition was obtained in the same manner as in Example 1. Table 3 shows the measurement results of the physical properties of the adhesive composition. From the above results, it can be seen that the composition of the present invention has very excellent performance as an adhesive.

[0035]

[Table 1]

[0036]

[Table 2]

[0037]

[Table 3]

Claims (1)

[Claims] 1. Gel permeation obtained by polymerizing (a) a block copolymer composed of at least one polymer block mainly composed of an aromatic vinyl compound and at least one block mainly composed of a conjugated diene. The peak molecular weight in chromatography (GPC) is 1 × 10 ⁴ to 50 × 10 ⁴ in terms of standard polystyrene;
And a linear block copolymer obtained by subjecting a living polymer having a total amount of the aromatic vinyl compound of 10 to 50% by weight to a silicon compound represented by the following general formula (I) to a coupling reaction. The composition, wherein the coupled component in the linear block copolymer composition is 10
100 parts by weight of the linear block copolymer composition of not less than 99% by weight and not less than 99% by weight;
A pressure-sensitive adhesive composition comprising 100 parts by weight. R ¹ R ² SiX ₂ (I) wherein R ¹ represents an aromatic hydrocarbon group, R ² represents an alkyl group or an aromatic hydrocarbon group or hydrogen, and X represents a halogen. ]