TW201627161A - Pressure-sensitive adhesive sheet laminate and constituent member laminate of image display device - Google Patents

Abstract

Provided is a novel pressure-sensitive adhesive sheet laminate capable of minimizing contamination by foreign matter in the interface between an adhesive layer and a mold release layer and/or migrative transfer of a mold release agent to the adhesive layer in affixing a constituent member of an image display device, and that has excellent durability after affixing. A pressure-sensitive sheet laminate in which a substrate layer (layer III) is provided via a mold release layer (layer II) to one side or both sides of a photocurable adhesive resin layer (layer I) containing a photocurable adhesive resin, wherein the photocurable adhesive resin layer (layer I) in its uncured stated is formed from a resin composition containing a (meth)acrylic acid ester copolymer (A), a crosslinking agent (B), and a photoinitiator (C), the mold release layer (layer II) is formed from a resin composition containing an olefin polymer (D), and the photocurable adhesive resin layer (layer I) and the mold release layer (layer II) are formed by coextrusion.

Description

Adhesive laminate and image display device

The present invention relates to an adhesive sheet laminate having an adhesive resin layer and a release layer, and an image display device comprising the pressure-sensitive adhesive layer laminate, and a method for manufacturing the same.

From the viewpoint of ensuring handleability or preventing foreign matter from adhering to the adhesive surface as an adhesive sheet, a peelable protective film (also referred to as a "release film") is usually deposited as an adhesive sheet laminate on the adhesive surface.

The transparent double-sided adhesive sheet for constituting a member such as a touch panel, a liquid crystal panel, or a surface protection panel to which the touch display is attached is preferably an optical property or a softness. Since the transparent adhesive sheet itself is made thin and soft, it is often used as an adhesive sheet laminated body formed by laminating a release film on a transparent adhesive sheet.

For example, the ABA type triblock copolymer containing acrylate and methacrylate and having a hydroxyl group are disclosed in Patent Document 1 (Japanese Patent Laid-Open Publication No. 2009-102467). An adhesive sheet in which an acrylic transparent adhesive composition obtained by blending a resin is sandwiched between release sheets and thermally melt-molded.

An adhesive sheet characterized in that an adhesive layer is provided on at least one side of a release film to crosslink the adhesive layer, and the cross-linking is disclosed in Patent Document 2 (Japanese Laid-Open Patent Publication No. 2010-185037). When the adhesive layer is subjected to a temperature dispersion behavior of a tensile storage modulus at a frequency of 1 Hz, it is 50,000 at any temperature within a temperature range of 25 ° C to 120 ° C. Above Pa, 1 million Pa or less.

Further, a transparent double-sided adhesive sheet is disclosed in Patent Document 3 (Japanese Patent Laid-Open Publication No. 2013-181088), which is characterized in that it is used to attach a constituent member for two image display devices. The first feature is that it is used by being cured by heat or ultraviolet rays in a state of being attached to the constituent members of the two image display devices, and the second feature is that the front surface of the adhesive sheet to be adhered to the transparent surface is When the back surface layer has a release film, the average roughness Ra obtained by analyzing the interference fringe image obtained by the laser interferometer is set to (X), and the release film is peeled off and attached to the two images. When the average roughness Ra obtained by analyzing the interference fringe image obtained by the laser interferometer in the state in which the display device is formed on the constituent member is (Y), the surface shape satisfying the specific condition is satisfied.

The release film used in such an adhesive sheet laminate is used for the surface of a film substrate such as a PET (polyethylene terephthalate) film in terms of ease of adjustment of peelability and the like. The release treatment is carried out by applying a polyfluorene-based release agent or the like.

However, the release film obtained by demolding the surface of the film substrate by a polyoxo-type release agent or the like tends to have a high production cost, and the release agent is transferred to the surface of the adhesive layer to impair adhesion. The possibility of quality stability of the film. Further, when the adhesive sheet laminate is produced, there is a possibility that foreign matter or the like is mixed between the film substrate and the adhesive resin layer.

For example, in Patent Document 4 (Japanese Patent Laid-Open Publication No. 2011-256319) and Patent Document 5 (WO2014/007137), it is disclosed that [the release layer containing a polyolefin resin] / [including an acrylic system] An adhesive sheet laminate in which the resin adhesive layer]/[the base layer containing the acrylic resin layer] is formed by co-extrusion molding.

[Previous Technical Literature] [Patent Literature]

[Patent Document 1] Japanese Patent Laid-Open Publication No. 2009-102467

[Patent Document 2] Japanese Patent Laid-Open Publication No. 2010-185037

[Patent Document 3] Japanese Patent Laid-Open Publication No. 2013-181088

[Patent Document 4] Japanese Patent Laid-Open Publication No. 2011-256319

[Patent Document 5] International Publication No. 2014/007137

In the case of bonding the image display device to constitute a member, durability after bonding is particularly required. However, the previously proposed adhesive sheet laminate body does not have sufficient durability when it is used to laminate the image display device constituent members.

Therefore, the present invention provides a foreign matter in which the interface between the adhesive layer and the release layer can be inhibited or the release agent is transferred to the adhesive layer, and the durability after bonding is also excellent, and can be preferably used for the image display device. A novel adhesive sheet laminate that fits the component.

The present invention provides an adhesive sheet laminate comprising a release layer (layer II) on one side or both sides of a photocurable adhesive resin layer (layer I) containing a photocurable adhesive resin. In the material layer (layer III), the photocurable adhesive resin layer (layer I) is composed of a (meth) acrylate copolymer (A), a crosslinking agent (B), and a photopolymerization initiator (C). The layer formed in the state before photohardening of the resin composition, the release layer (layer II) is a layer formed of a resin composition containing an olefin polymer (D), and the photocurable adhesive resin layer ( The layer I) and the above-mentioned release layer (layer II) are formed by co-extrusion.

In the adhesive sheet laminate according to the present invention, a layer (I layer) based on a (meth) acrylate copolymer and a layer (II layer) based on an olefin polymer are used in a state before photohardening. , the interlayer strength is weak and it is easy to cause interlayer peeling, so one layer can be layered (II The layer) is used as a release layer. In contrast, the photocurable adhesive resin layer (I layer) is a photocurable resin combination containing a (meth) acrylate copolymer (A), a crosslinking agent (B), and a photopolymerization initiator (C). Since the layer formed of the material is laminated on the adherend, the photocurable adhesive resin layer (I layer) is photocured, whereby the durability of the photocurable adhesive resin layer (I layer) after bonding can be changed. Excellent. Therefore, for example, it can be preferably used for bonding of constituent members of an image display device.

Further, in the adhesive sheet laminate according to the present invention, the photocurable adhesive resin layer (I layer) and the release layer (II layer) are formed by co-extrusion, so that the photocurable adhesive resin layer (I layer) can be lowered. The possibility of mixing foreign matter with the interface of the release layer (layer II). Further, the release layer (layer II) is not a layer formed of a polyoxymethylene resin, but is a layer formed of a resin composition containing a polyolefin resin, so that the release agent can be prevented from being transferred to photohardening. Adhesively sticking to the resin layer (I layer) and contaminating the adhesive body. Further, since it is not necessary to perform the release treatment on the surface of the base material layer as before, the adhesive sheet laminate can be provided more economically.

Hereinafter, an example of an embodiment of the present invention will be described in detail. However, the invention of the present invention is not limited to the following embodiments.

[Adhesive laminated body]

The adhesive sheet laminate (referred to as "the present adhesive sheet laminate") according to an embodiment of the present invention is provided on one side or both sides of the photocurable adhesive resin layer (I layer) containing a photocurable adhesive resin. The layer (layer II) is provided with an adhesive sheet laminate of a base material layer (III layer).

[Photocurable adhesive resin layer (I layer)]

The photocurable adhesive resin layer (I layer) is a layer formed of a resin composition containing a (meth) acrylate copolymer (A), a crosslinking agent (B), and a photopolymerization initiator (C). Good is the state that is not hardened before light hardening.

In the present invention, the photocurable adhesive resin layer (I layer) is "in a state before photocuring", and the light is not irradiated for the purpose of curing the photocurable adhesive resin layer (I layer). The state of hardening. For example, the state of natural light hardening due to the influence of indoor light or sunlight is "the state before light hardening".

The photocurable adhesive resin layer (I layer) can be formed, for example, from the adhesive composition α or the adhesive composition β described below to form a photocurable adhesive resin layer (I layer). In the resin composition for forming the photocurable adhesive resin layer (I layer), the adhesive compositions α and β are preferably not limited thereto.

When the photocurable adhesive resin layer (I layer) is formed from the adhesive composition α or β, it can be kept in a sheet shape even in the uncrosslinked state before photohardening. In addition, when it is heated in the uncrosslinked state, it can be melted or flowed (hot-melt), and the adhesive can be filled in accordance with the uneven portion such as the printing step, and can be filled without generating bubbles or the like. Further, in the uncrosslinked state, in the normal state, that is, at room temperature, it is possible to have an appropriate adhesion, for example, a peelable degree of adhesion (referred to as "stickiness"), so that positioning at the time of adhesion can be achieved. It becomes simple.

Further, as described below, by adjusting the melt viscosity of the adhesive composition α or β at 130 ° C, the photocurable adhesive resin layer (I layer) and the release layer (layer II) can be co-extruded, and on the other hand, coextrusion In the state where the film is not photo-cured, it is difficult to mutually release the release layer (II layer) based on the olefin-based polymer. Therefore, the co-extruded release layer (layer II) can be used as the release layer.

Further, when the photocurable adhesive resin layer (I layer) is formed from the adhesive composition α or β, the adhesion can be sufficiently improved by the final photocrosslinking.

<adhesive composition α>

The adhesive composition α includes a (meth) acrylate copolymer (A1), a crosslinking agent (B1), and a photopolymerization initiator (C1) containing a graft copolymer having a macromonomer as a branch component. a resin composition.

((Meth)acrylate copolymer (A1))

The above (meth) acrylate copolymer as a base polymer in the adhesive composition α (A1) is a graft copolymer having a macromonomer as a branch component.

In the present invention, the term "base polymer" means a resin which is a main component of the adhesive composition α. No specific content is specified. The standard is 50% by mass or more, more preferably 80% by mass or more, and more preferably 90% by mass or more (including 100% by mass) of the resin contained in the adhesive composition α (again, When the base polymer is two or more, the total amount is equivalent to the above content).

The main component of the (meth) acrylate copolymer (A1) preferably contains a copolymer component containing a repeating unit derived from (meth) acrylate.

The glass transition temperature of the copolymer constituting the main component of the (meth) acrylate copolymer (A1) is preferably -70 to 0 °C.

In this case, the glass transition temperature of the copolymer component constituting the trunk component means a glass transition temperature of a polymer obtained by copolymerizing only the monomer component constituting the trunk component of the (meth) acrylate copolymer (A1). Specifically, it means the value calculated from the calculation formula of Fox from the glass transition temperature and the composition ratio of the polymer obtained from the homopolymer of each component of the copolymer.

Further, the calculation formula of Fox refers to a calculated value obtained by the following formula, and can be obtained by using the values described in the Polymer Handbook [Polymer Handbook, J. Brandrup, Interscience, 1989].

1/(273+Tg)=Σ(Wi/(273+Tgi))

[wherein, Wi represents the weight fraction of monomer i, and Tgi represents the Tg (°C) of the homopolymer of monomer i]

The glass transition temperature of the copolymer component constituting the main component of the above (meth) acrylate copolymer (A1), the softness of the adhesive composition α at room temperature or the wetting of the adhesive composition α to the adherend The effect of the adhesiveness, that is, the adhesiveness, is such that the adhesive composition α obtains moderate adhesion (viscosity) at room temperature, and the glass transition temperature is preferably -70 ° C to 0 ° C, more preferably -65. Above °C or below -5 °C, especially preferably above -60 °C or -10 Below °C.

Here, even if the glass transition temperature of the copolymer component is the same temperature, the viscoelasticity can be adjusted by adjusting the molecular weight. For example, by reducing the molecular weight of the copolymer component, it can be made softer.

Examples of the (meth) acrylate monomer contained in the main component of the (meth) acrylate copolymer (A1) include 2-ethylhexyl (meth) acrylate and (meth) acrylate. Octyl ester, isooctyl (meth)acrylate, n-butyl (meth)acrylate, ethyl (meth)acrylate, methyl (meth)acrylate, and the like. It can also be used for hydroxyethyl (meth)acrylate, hydroxypropyl (meth)acrylate, acrylic acid, methacrylic acid, glycidyl (meth)acrylate, or the like having a hydrophilic group or an organic functional group or the like. Methyl) acrylamide, N,N-dimethyl(meth)acrylamide, (meth)acrylonitrile, and the like.

Further, various vinyl monomers such as vinyl acetate, alkyl vinyl ether or hydroxyalkyl vinyl ether copolymerizable with the above acrylic monomer or methacrylic monomer can be suitably used.

Further, the main component of the (meth) acrylate copolymer (A1) preferably contains a hydrophobic (meth) acrylate monomer and a hydrophilic (meth) acrylate monomer as constituent units.

The hydrophobic (meth) acrylate monomer is preferred because it can suppress the water absorption of the acrylic copolymer (A) or adjust the relative dielectric constant of the acrylic copolymer (A).

On the other hand, when the main component of the (meth) acrylate copolymer (A1) is composed only of a hydrophobic monomer, there is a tendency for wet heat to whiten. Therefore, it is preferred to introduce a hydrophilic monomer into the main component to prevent it. Damp heat whitening.

Specifically, examples of the main component of the (meth) acrylate copolymer (A1) include a hydrophobic (meth) acrylate monomer and a hydrophilic (meth) acrylate monomer and a giant A copolymer component obtained by randomly copolymerizing a polymerizable functional group at the terminal of a monomer.

Here, examples of the hydrophobic (meth) acrylate include methyl (meth)acrylate, ethyl (meth)acrylate, n-butyl (meth)acrylate, and (meth)acryl. Isobutyl acrylate, second butyl (meth) acrylate, tert-butyl (meth) acrylate, isopropyl (meth) acrylate, propyl (meth) acrylate, amyl (meth) acrylate, Isoamyl (meth)acrylate, neopentyl (meth)acrylate, hexyl (meth)acrylate, heptyl (meth)acrylate, octyl (meth)acrylate, isooctyl (meth)acrylate , 2-ethylhexyl (meth)acrylate, decyl (meth)acrylate, isodecyl (meth)acrylate, decyl (meth)acrylate, isodecyl (meth)acrylate, (methyl) , undecyl acrylate, dodecyl (meth) acrylate, stearyl (meth) acrylate, cetyl (meth) acrylate, behenyl (meth) acrylate, and the like.

In addition, it can also be mentioned that (meth)acrylic acid Ester, cyclohexyl (meth)acrylate, 3,5,5-trimethylcyclohexyl (meth)acrylate, dicyclopentanyl (meth)acrylate, dicyclopentenyl (meth)acrylate, (meth) acrylate or styrene having an aliphatic cyclic structure such as dicyclopentenyloxyethyl (meth) acrylate, decene acrylate or a derivative thereof, hydrogenated rosin acrylate or a derivative thereof .

Among them, a monomer having a long-chain alkyl structure or a monomer having a cyclic structure such as 2-ethylhexyl (meth)acrylate or dodecyl (meth)acrylate or stearyl (meth)acrylate The body can be effectively used to adjust the relative dielectric constant of the acrylic polymer (A).

Examples of the hydrophilic (meth) acrylate monomer include 2-hydroxyethyl (meth) acrylate, 2-hydroxypropyl (meth) acrylate, and 4-hydroxybutyl (meth) acrylate. a hydroxyl group-containing (meth) acrylate such as glycerin (meth) acrylate, (meth)acrylic acid, 2-(meth)acryloxyethyl hexahydrophthalic acid, 2-(methyl) Propylene methoxypropyl hexahydrophthalic acid, 2-(meth) propylene methoxyethyl phthalate, 2-(methyl) propylene methoxy propyl phthalate, 2-( Methyl) propylene oxiranyl ethyl maleic acid, 2-(methyl) propylene methoxy propyl maleic acid, 2-(methyl) propylene methoxyethyl succinic acid, 2- (Methyl) propylene methoxy propyl succinic acid, crotonic acid, fumaric acid, maleic acid, itaconic acid, maleic acid monomethyl ester, itaconic acid monomethyl ester, etc. a monomer of a carboxyl group, an amino group-containing (meth)acrylate monomer such as dimethylaminoethyl (meth)acrylate or diethylaminoethyl (meth)acrylate, (meth)acrylamide , N-tert-butyl (meth) acrylamide, N-methylol (meth) acrylamide, N-methoxy Methyl (meth) acrylamide, N-butoxymethyl (meth) acrylamide, diacetone acrylamide, maleimide, maleimide, N, N a monomer containing a guanamine group such as dimethyl methacrylate or hydroxyethyl acrylamide, a heterocyclic basic monomer such as vinyl pyrrolidone, vinyl pyridine or vinyl carbazole. Further, there may be mentioned: tetrahydrofurfuryl (meth)acrylate or (meth)acrylic acid a monomer having a cyclic ether structure such as porphyrin, or an alkoxyalkyl (meth)acrylate such as methoxyethyl (meth)acrylate or ethoxyethyl (meth)acrylate, or methyl acrylate Wait.

The (meth) acrylate copolymer (A1) is preferably a branch component in which a macromonomer is introduced as a graft copolymer, and a repeating unit derived from a macromonomer is contained.

The macromonomer system refers to a polymer monomer having a terminal polymerizable functional group and a high molecular weight skeleton component.

The glass transition temperature (Tg) of the macromonomer is preferably higher than the glass transition temperature of the copolymer component constituting the above (meth) acrylate copolymer (A1).

Specifically, the glass transition temperature (Tg) of the macromonomer affects the heating and melting temperature (hot melt temperature) of the adhesive composition α, so the glass transition temperature (Tg) of the macromonomer is preferably from 30 ° C to 120 ° C. More preferably, it is 40 ° C or more or 110 ° C or less, and further preferably 50 ° C or more or 100 ° C or less.

In the case of such a glass transition temperature (Tg), excellent workability or storage stability can be maintained by adjusting the molecular weight, and it can be adjusted to be hot-melted at about 80 °C.

The glass transition temperature of the macromonomer refers to the glass transition temperature of the macromonomer itself, which can be determined by a differential scanning calorimeter (DSC).

Further, in the room temperature state, the branch components are pulled to each other to maintain the physical cross-linking state as the adhesive composition, and the physical cross-linking can be decomposed by heating to a moderate temperature to obtain fluidity. It is also preferred to adjust the content of macromonomers.

In this regard, the macromonomer is preferably in the (meth) acrylate copolymer (A1). It is contained in a ratio of 5 mass% to 30 mass%, more preferably 6% by mass or more or 25% by mass or less, and further preferably 8% by mass or more or 20% by mass or less.

The component constituting the high molecular weight skeleton of the macromonomer is preferably an acrylic monomer or a vinyl monomer, and more preferably a hydrophobic monomer.

Examples of the component of the high molecular weight skeleton constituting the macromonomer include methyl (meth)acrylate, ethyl (meth)acrylate, n-butyl (meth)acrylate, and isobutyl (meth)acrylate. , (butyl) (meth)acrylate, tert-butyl (meth)acrylate, isopropyl (meth)acrylate, propyl (meth)acrylate, amyl (meth)acrylate, (methyl) Isoamyl acrylate, neopentyl (meth)acrylate, hexyl (meth)acrylate, heptyl (meth)acrylate, octyl (meth)acrylate, isooctyl (meth)acrylate, (methyl) ) 2-ethylhexyl acrylate, decyl (meth) acrylate, isodecyl (meth) acrylate, decyl (meth) acrylate, isodecyl (meth) acrylate, (methyl) acrylate Alkyl ester, dodecyl (meth)acrylate, stearyl (meth)acrylate, cetyl (meth)acrylate, behenyl (meth)acrylate, and the like. Further, examples thereof include a (meth)acrylic acid alkoxyalkyl ester such as methoxyethyl (meth)acrylate or ethoxyethyl (meth)acrylate, and 2-hydroxyethyl (meth)acrylate. Hydroxy-containing (meth) acrylate such as ester, 2-hydroxypropyl (meth) acrylate, 4-hydroxybutyl (meth) acrylate, glycerol (meth) acrylate, (meth) acrylate, 2- (methyl) propylene oxiranyl ethyl hexahydrophthalic acid, 2-(methyl) propylene methoxy propyl hexahydrophthalic acid, 2-(methyl) propylene oxiranyl ethyl benzene Dicarboxylic acid, 2-(methyl) propylene methoxy propyl phthalate, 2-(methyl) propylene oxiranyl ethyl maleate, 2-(methyl) propylene methoxy propyl Maleic acid, 2-(methyl) propylene methoxyethyl succinic acid, 2-(methyl) propylene methoxy propyl succinic acid, crotonic acid, fumaric acid, maleic acid a carboxyl group-containing monomer such as acid, itaconic acid, maleic acid monomethyl ester or itaconic acid monomethyl ester, an acid anhydride group-containing monomer such as maleic anhydride or itaconic acid anhydride, or (meth)acrylic acid Glycidyl ester, α-ethyl methacrylate, 3,4-cyclo(meth)acrylate An epoxy group-containing monomer such as oxybutyl ester, an amino group-containing (meth) acrylate monomer such as dimethylaminoethyl (meth)acrylate or diethylaminoethyl (meth)acrylate, (Meth) acrylamide, N-tert-butyl (meth) acrylamide, N-methylol (meth) acrylamide, N-methoxymethyl (meth) acrylamide, a monomer containing a guanamine group such as N-butoxymethyl (meth) acrylamide, diacetone acrylamide, maleimide, maleimide, vinyl pyrrolidone, a heterocyclic basic monomer such as vinyl pyridine or vinyl carbazole, or a vinyl compound such as styrene, vinyl toluene, α-methyl styrene, acrylonitrile, methacrylonitrile, vinyl acetate or vinyl propionate. Monomer, methoxyethylene glycol allyl ether, methoxy polyethylene glycol allyl ether, methoxy polypropylene glycol allyl ether, butoxy polyethylene glycol allyl ether, butoxy polypropylene glycol Terminal alkoxyallyylated polyether monomer such as propyl ether, methoxy polyethylene glycol-polypropylene glycol allyl ether, butoxy polyethylene glycol-polypropylene glycol allyl ether, (meth)acrylic acid ring Hexyl ester, tert-butyl ring (meth)acrylate Ester, (meth) isobutyl acrylate, Ester, 3,5,5-trimethylcyclohexyl (meth)acrylate, EO modified (meth) acrylate of p-cumylphenol, dicyclopentyl (meth)acrylate, (methyl) Dicyclopentenyl acrylate, dicyclopentenyloxyethyl (meth) acrylate, benzyl (meth) acrylate, phenoxyethyl (meth) acrylate, styrene, tert-butyl styrene , α-methyl styrene, vinyl toluene, and the like.

Among the above components, a monomer having a glass transition temperature of 30 ° C to 120 ° C when the above-mentioned components constituting the high molecular weight skeleton of the macromonomer is a homopolymer is more preferable. Specifically, examples of the monomer include methyl methacrylate, 3,5,5-trimethylcyclohexyl acrylate, and acrylic acid. Ester, dicyclopentanyl acrylate, cyclohexyl methacrylate, and the like.

Further, in the case where the above-mentioned component constituting the high molecular weight skeleton of the macromonomer has crystallinity, it is more preferred that the crystal melting temperature of the component is 30 ° C to 120 ° C when the component is a homopolymer. body. Specifically, examples of the monomer include stearyl acrylate, stearyl methacrylate, cetyl acrylate, cetyl methacrylate, behenyl acrylate, and behenyl methacrylate.

Further, when a high molecular weight skeleton of a macromonomer is formed, one of the monomers may be polymerized and used, and the plurality of monomers may be copolymerized and used.

Examples of the terminal polymerizable functional group of the above-mentioned macromonomer include a methyl methacrylate, an acryl fluorenyl group, and a vinyl group.

The (meth) acrylate copolymer (A1) preferably has a viscosity at a temperature of 130 ° C and a frequency of 0.02 Hz of 100 to 800 Pa. s, more preferably 150~700Pa. s, and further preferably 170 to 600 Pa. s.

The re-adhesion of the (meth) acrylate copolymer (A1) at a temperature of 130 ° C affects the fluidity of the adhesive composition α when the transparent double-sided adhesive is used for heat fusion, so if the complex viscosity is 100 ~800Pa. s, can have excellent hot melt suitability.

In order to adjust the viscosity of the (meth) acrylate copolymer (A1) to the above range, for example, the glass transition temperature of the copolymer component constituting the main component of the (meth) acrylate copolymer (A1) can be adjusted. The adjustment is preferably from -70 ° C to 0 ° C, more preferably -65 ° C or more or -5 ° C or less, and still more preferably -60 ° C or more or -10 ° C or less, and adjusting the copolymer component. The method of adjusting the viscoelasticity by molecular weight. However, it is not limited to this method.

The molecular weight of the (meth) acrylate copolymer (A1) is preferably from 100,000 to 1,000,000, more preferably 150,000 or more, from the viewpoint of adjusting the melt viscosity at 130 ° C to a specific range as described below. Less than 800,000, of which more than 200,000 or less is less than 700,000.

(crosslinking agent (B1))

As the crosslinking agent (B1), for example, an epoxy crosslinking agent or an isocyanate crosslinking agent can be suitably selected, and a crosslinking agent such as an oxetane compound, a decane compound or an acrylic compound can be used. Among them, a polyfunctional (meth) acrylate monomer having two or more (meth) acrylonitrile groups is preferred in terms of reactivity or strength of the obtained cured product.

For example, after the photocurable adhesive resin layer (I layer) is bonded to the image display device constituent member and integrated, the crosslinking agent (B1) contained in the photocurable adhesive resin layer (I layer) is dispensed. By the reaction, the photocurable adhesive resin layer (layer I) loses its hot melt property, and instead, it exhibits high cohesive force in a high temperature environment, and excellent foaming reliability is obtained.

Examples of such a polyfunctional (meth) acrylate monomer include 1,4-butanediol di(meth)acrylate, glycerol di(meth)acrylate, and neopentyl glycol di(methyl). Acrylate, glycerol glycidyl ether di(meth)acrylate, 1,6-hexanediol di(meth)acrylate, 1,9-nonanediol di(meth)acrylate, tricyclodecane Dimethanol di(meth)acrylate, bisphenol A polyethoxy di(meth)acrylate, bisphenol A polypropoxy di(meth)acrylate, bisphenol F polyethoxy di(methyl) Acrylate, ethylene glycol di(meth) acrylate, neopentyl glycol di(meth) acrylate, trimethylolpropane trioxyethyl (meth) acrylate, ε-caprolactone Tris(2-hydroxyethyl)isocyanurate tri(meth)acrylate, pentaerythritol tri(meth)acrylate, pentaerythritol tri(meth)acrylate, pentoxide tetraol tris(methyl) Acrylate, pentaerythritol tetra(meth)acrylate, pentaerythritol tetra(meth)acrylate, pentaerythritol tetra(meth)acrylate, dipentaerythritol hexa(meth)acrylate, poly Glycol di(meth)acrylate, tris(propyleneoxyethyl)isocyanurate, pentaerythritol tetra(meth)acrylate, dipentaerythritol hexa(meth)acrylate, dipentaerythritol penta (methyl) Acrylate, tripentaerythritol hexa(meth) acrylate, tripentaerythritol penta (meth) acrylate, hydroxypivalic acid neopentyl glycol di(meth) acrylate, hydroxypivalic acid neopentyl glycol ε - caprolactone adducts of di(meth)acrylate, trimethylolpropane tri(meth)acrylate, trimethylolpropane polyethoxy tri(meth)acrylate, di-trishydroxyl An ultraviolet-curable polyfunctional monomer such as methyl propane tetra(meth)acrylate, and examples thereof include polyester (meth) acrylate, epoxy (meth) acrylate, and (meth) acrylate A multifunctional acrylate oligomer such as a carbamic acid ester or a polyether (meth) acrylate.

In the above-described examples, the polyfunctional (meth) acrylate monomer is preferably a polyfunctional monomer containing a polar functional group such as a hydroxyl group, from the viewpoint of improving the adhesion to the adherend or the effect of suppressing the wet heat whitening. Oligomer. Among them, a polyfunctional (meth) acrylate having a hydroxyl group is preferably used.

Therefore, as a result of preventing wet heat whitening, as the above (meth) acrylate The polymer (A1), that is, the main component of the graft copolymer, preferably contains a hydrophobic acrylate monomer and a hydrophilic acrylate monomer, and further, as a crosslinking agent (B1), preferably has a A polyfunctional (meth) acrylate of a hydroxyl group.

Further, in order to adjust the effects of adhesion, moist heat resistance, heat resistance and the like, a monofunctional (meth) acrylate which reacts with the crosslinking agent (B1) may be added.

The content of the crosslinking agent (B1) is not particularly limited. The standard is preferably 0.5 to 20 parts by mass, more preferably 1 part by mass or more or 15 parts by mass or less, and further preferably 2 parts by mass based on 100 parts by mass of the (meth) acrylate copolymer (A1). A ratio of more than 10 parts by weight.

The photocurable adhesive resin layer (I layer) having an uncrosslinked state and the photocurable adhesive resin layer (I layer) after crosslinking can be obtained by containing the crosslinking agent (B1) in the above range. Resistant to foaming reliability. Among them, considering the balance with other elements, it is also possible to exceed this range.

(Photopolymerization initiator (C1))

The photopolymerization initiator (C1) functions as a reaction initiation aid for the crosslinking reaction of the above crosslinking agent (B1). The photopolymerization initiator can be suitably used in the art. Among them, from the viewpoint of controlling the easiness of the crosslinking reaction, a photopolymerization initiator which induces ultraviolet rays having a wavelength of 380 nm or less is preferable.

On the other hand, when a photopolymerization initiator which induces light having a wavelength longer than a wavelength of 380 nm is used, the crosslinking reaction proceeds easily, for example, even when light is irradiated through a member which lacks ultraviolet ray permeability. The resin layer (I layer) is preferred in terms of hardening.

The photopolymerization initiator is roughly classified into two types according to a radical generation mechanism, and can be roughly classified into a cleavage type photopolymerization initiator which can decompose a single bond of a photopolymerization initiator itself to generate a radical, and The photoexcited initiator and the hydrogen donor in the system form a hydrogen-extracting photopolymerization initiator which promotes the complex and transfers hydrogen to the hydrogen donor.

In the above-mentioned cleavage type photopolymerization initiator, when a radical is generated by light irradiation, it is decomposed into other compounds, and if it is temporarily excited, it does not have a function as a reaction initiator. Therefore, it is preferable that the adhesive material does not remain as an active material in the adhesive material after completion of the crosslinking reaction, and there is no possibility of causing undesired photodegradation or the like to the adhesive material.

On the other hand, when a hydrogen-extracting photopolymerization initiator is reacted by a radical irradiated with an active energy ray such as ultraviolet rays, a decomposition product such as a cleavage type photopolymerization initiator does not occur, so that it is difficult to become a reaction after completion of the reaction. Volatile ingredients are useful in reducing damage to the adherend.

As the above-mentioned cleavable photopolymerization initiator, for example, 2,2-dimethoxy-1,2-diphenylethane-1-one, 1-hydroxycyclohexyl phenyl ketone, 2-hydroxy- 2-methyl-1-phenyl-propan-1-one, 1-(4-(2-hydroxyethoxy)phenyl)-2-hydroxy-2-methyl-1-propan-1-one, 2-hydroxy-1-[4-{4-(2-hydroxy-2-methyl-propenyl)benzyl 1phenyl]-2-methyl-propan-1-one, oligomeric (2-hydroxyl) -2-methyl-1-(4-(1-methylvinyl)phenyl)propanone), methyl phenylglyoxylate, 2-benzyl-2-dimethylamino-1-(4- Polinylphenyl)butan-1-one, 2-methyl-1-[4-(methylthio)phenyl]-2- Lolinylpropan-1-one, 2-(dimethylamino)-2-[(4-methylphenyl)methyl]-1-[4-(4- Phenyl)phenyl]-1-butanone, bis(2,4,6-trimethylbenzylidene)-phenylphosphine oxide, 2,4,6-trimethylbenzimidyl diphenyl Phosphine oxide or such derivatives and the like.

Examples of the hydrogen extraction-type photopolymerization initiator include benzophenone, 4-methyl-benzophenone, 2,4,6-trimethylbenzophenone, and 4-phenyldiphenyl. Methyl ketone, 3,3'-dimethyl-4-methoxybenzophenone, methyl 2-benzimidylbenzoate, methyl benzylidenecarboxylate, bis(2-phenyl-2- Glyoxylate)oxydiethylene, 4-(1,3-propenylmercapto-1,4,7,10,13-pentaoxytridecyl)benzophenone, 9-oxosulfur 2-chloro-9-oxosulfur 3-methyl-9-oxosulfur 2,4-dimethyl 9-oxosulfur , 2-methyl hydrazine, 2-ethyl hydrazine, 2-tert-butyl fluorene, 2-amino hydrazine or a derivative thereof.

However, the photopolymerization initiator is not limited to the above-exemplified substances. Any one of a rupture type photopolymerization initiator and a hydrogen extraction type photopolymerization initiator may be used, or may be combined Use both.

The content of the photopolymerization initiator (C1) is not particularly limited. The standard is preferably 0.1 to 10 parts by mass, more preferably 0.5 part by mass or more or 5 parts by mass or less, and still more preferably 1 part by mass based on 100 parts by mass of the (meth)acrylate copolymer (A1). It is contained in the ratio of the mass part or more or 3 parts by mass or less.

By setting the content of the photopolymerization initiator (C1) to the above range, a moderate reaction sensitivity to the active energy ray can be obtained.

(other ingredients)

The adhesive composition α may also contain a known component formulated in a usual adhesive composition as a component other than the above. For example, various additives such as an adhesion-imparting resin, an antioxidant, a photostabilizer, a metal inerting agent, a rust preventive, an anti-aging agent, a moisture absorbent, a rust preventive, and an anti-hydrolysis agent may be contained.

Moreover, a reaction catalyst (a tertiary amine compound, a quaternary ammonium compound, a lauric acid compound, etc.) may be contained as needed.

<Adhesive composition β>

Examples of the adhesive composition β include a monomer a1 having a glass transition temperature (Tg) of less than 0 ° C and a monomer a 2 and a glass transition temperature (Tg) having a glass transition temperature (Tg) of 0 ° C or more and less than 80 ° C. A (meth) acrylate having a weight average molecular weight of 50,000 to 400,000 obtained by copolymerizing a monomer a3 at 80 ° C or higher at a molar ratio of a1:a2:a3=10 to 40:90 to 35:0 to 25 A resin composition of a copolymer (A2), a crosslinking agent (B2), and a photopolymerization initiator (C2).

((Meth)acrylate copolymer (A2))

In the viewpoint of the shape retention property and the hot-melt property in the room temperature state, the adhesion composition β is based on the viewpoint of adjusting the melt viscosity of 130 ° C to a specific range as described below. The weight average molecular weight of the (meth) acrylate copolymer (A2) of the polymer is preferably from 50,000 to 400,000, more preferably more than 60,000 or less than 350,000. Further, it is preferably 70,000 or more or 300,000 or less.

The (meth) acrylate copolymer (A2) can be suitably adjusted to adjust the glass transition temperature by appropriately selecting the type, composition ratio, polymerization conditions, and the like of the acrylic monomer or methacrylic monomer. Tg) or physical properties such as molecular weight.

In this case, examples of the acrylic monomer constituting the acrylate copolymer include 2-ethylhexyl (meth)acrylate, n-octyl (meth)acrylate, and isooctyl (meth)acrylate. As the main raw material, n-butyl methacrylate, ethyl (meth) acrylate or the like.

In addition to these, it is also possible to copolymerize a (meth)acrylic monomer having various functional groups with the above acrylic monomer for the purpose of imparting aggregating power or imparting polarity.

Examples of the (meth)acrylic monomer having a functional group include methyl methacrylate, methyl acrylate, hydroxyethyl acrylate, acrylic acid, glycidyl (meth)acrylate, and N-substituted (A). Base) acrylamide, acrylonitrile, methacrylonitrile, fluoroalkyl (meth) acrylate, (meth) acrylate containing a decyloxy group, and the like.

As the (meth) acrylate copolymer (A2), a monomer a1 having a glass transition temperature (Tg) of less than 0 ° C and a monomer a2 having a glass transition temperature (Tg) of 0 ° C or more and less than 80 ° C are preferable. (Meth) acrylate copolymerization with a monomer a3 having a glass transition temperature (Tg) of 80 ° C or higher and a molar ratio of a1: a2: a3 = 10 to 40: 90 to 35: 0 to 25 Things.

At this time, the respective glass transition temperatures (Tg) of the monomers a1, a2, and a3 refer to the respective glass transition temperatures (Tg) when the polymer is produced from the monomer (homopolymerization).

The monomer a1 is preferably a (meth) acrylate monomer having an alkyl structure having a side chain having 4 or more carbon atoms.

In this case, the side chain having 4 or more carbon atoms may be a linear chain or a carbon chain containing a branch.

More specifically, the monomer a1 is preferably a (meth) acrylate monomer having a linear alkyl structure of 4 to 10 carbon atoms or a branched alkyl structure having a carbon number of 6 to 18 (A) Base) acrylate monomer.

Here, examples of the (meth) acrylate monomer having a linear alkyl structure having 4 to 10 carbon atoms include n-butyl acrylate, n-hexyl acrylate, and n-octyl (meth) acrylate. N-decyl methacrylate, n-decyl (meth) acrylate, and the like.

On the other hand, as the (meth) acrylate monomer having a branched alkyl structure having 6 to 18 carbon atoms, 2-ethylhexyl (meth)acrylate and (meth)acrylic acid 2 are exemplified. -methylhexyl ester, isooctyl (meth)acrylate, isodecyl (meth)acrylate, isodecyl (meth)acrylate, and the like.

The monomer a2 is preferably a (meth) acrylate monomer having a carbon number of 4 or less, a (meth) acrylate monomer having a cyclic skeleton in a side chain, a vinyl monomer having a carbon number of 4 or less, or a side chain. A vinyl monomer having a cyclic skeleton.

Among them, the monomer a2 is particularly preferably a vinyl monomer having a carbon number of 4 or less in the side chain.

Here, examples of the "(meth) acrylate monomer having 4 or less carbon atoms include methyl acrylate, ethyl methacrylate, n-propyl acrylate, n-propyl methacrylate, and isopropyl acrylate. Isopropyl methacrylate, n-butyl methacrylate, tributyl acrylate, isobutyl acrylate, isobutyl methacrylate, and the like.

Examples of the (meth) acrylate monomer having a cyclic chain in the side chain include acrylic acid Ester, cyclohexyl acrylate, cyclohexyl methacrylate, 1,4-cyclohexane dimethanol monoacrylate, tetrahydrofurfuryl methacrylate, benzyl acrylate, benzyl methacrylate, phenoxy acrylate Ester, phenoxyethyl methacrylate, 2-hydroxy-3-phenoxypropyl acrylate, 3,3,5-trimethylcyclohexanol acrylate, cyclic trimethylolpropane methyl acetal Ester, 4-ethoxylated cumylphenol acrylate, dicyclopentenyloxyethyl acrylate, dicyclopentenyloxyethyl methacrylate, dicyclopentenyl acrylate, and the like.

Examples of the "vinyl monomer having 4 or less carbon atoms" include vinyl acetate, propylene vinyl ester, vinyl butyrate, n-propyl vinyl ether, isopropyl vinyl ether, n-butyl vinyl ether, and isobutylene. Vinyl ether and the like.

Examples of the "vinyl monomer having a cyclic skeleton in the side chain" include styrene, cyclohexyl vinyl ether, and lowering. Vinyl ether Alkenyl vinyl ether and the like. Among them, an acrylate monomer having a carbon number of 4 or less in the side chain or a carbon number of 4 or less in the side chain is particularly preferable.

The monomer a3 is preferably a (meth) acrylate monomer having a carbon number of 1 or less in a side chain or a (meth) acrylate monomer having a cyclic skeleton in a side chain.

Here, examples of the "(meth) acrylate monomer having a carbon number of 1 or less in the side chain include methyl methacrylate, acrylic acid, methacrylic acid, and the like.

Examples of the (meth) acrylate monomer having a cyclic chain in the side chain include methacrylic acid Ester, 3,3,5-trimethylcyclohexyl methacrylate, dicyclopentanyl acrylate, dicyclopentanyl methacrylate, dicyclopentenyl methacrylate, and the like.

If the (meth) acrylate copolymer (A2) contains monomer a1 and monomer a2 and monomer a3 is copolymerized at a molar ratio of a1:a2:a3=10~40:90~35:0-25 The (meth) acrylate copolymer can adjust the peak of Tan δ to 0 to 20 ° C, and can maintain a sheet shape in a normal state, that is, at room temperature, and can exhibit a peelable degree. The continuum (called "stickiness"). Further, when the temperature is heated to a heat-fusible temperature, fluidity can be exhibited, and the step portion of the bonding surface can be followed to fill the respective corners.

Therefore, from this point of view, the molar ratio of the monomer a1 and the monomer a2 to the monomer a3 in the (meth) acrylate copolymer constituting the (meth) acrylate copolymer (A2) is preferably a1. :a2:a3=10~40:90~35:0~25, preferably 13~40:87~35:0~23, and more preferably 15~40:85~38:2~20.

Further, in the same viewpoint as described above, the monomer a1 and the monomer a2 and the monomer a3 in the (meth) acrylate copolymer or the vinyl copolymer constituting the (meth) acrylate copolymer (A2) The molar ratio is preferably a2>a1>a3.

(crosslinking agent (B2))

By crosslinking the crosslinking agent (B2), the adhesive composition β can exhibit a high cohesive force in a high-temperature environment, and excellent foaming reliability can be obtained.

As such a crosslinking agent (B2), for example, an epoxy crosslinking agent or an isocyanate crosslinking can be suitably selected. The crosslinking agent includes a crosslinking agent such as an oxetane compound, a decane compound, or an acrylic compound. Among them, in terms of reactivity or strength of the obtained cured product, it is preferred to have two or more (meth) acrylonitrile groups, and among them, it is preferred to have three or more (meth) acryl fluorenyl groups. Functional (meth) acrylate monomer.

Examples of such a polyfunctional (meth) acrylate monomer include 1,4-butanediol di(meth)acrylate, glycerol di(meth)acrylate, and 1,6-hexanediol. (Meth) acrylate, 1,9-nonanediol di(meth) acrylate, tricyclodecane dimethanol di(meth) acrylate, bisphenol A polyethoxy di(meth) acrylate , bisphenol A polypropoxy di(meth) acrylate, bisphenol F polyethoxy di(meth) acrylate, neopentyl glycol di (meth) acrylate, ethylene glycol di(methyl) Acrylate, trimethylolpropane trioxyethyl (meth) acrylate, ε-caprolactone modified tris(2-hydroxyethyl)isocyanurate tri(meth) acrylate, pentaerythritol III (meth) acrylate, pentaerythritol tri(meth) acrylate, pentaerythritol tri(meth) acrylate, pentaerythritol tetra (meth) acrylate, pentaerythritol tetra(meth) acrylate, B Pentaerythritol tetra(meth)acrylate, dipentaerythritol hexa(meth) acrylate, polyethylene glycol di(meth) acrylate, tris(propylene decyloxyethyl)isocyanurate, penta Alcohol tetra (meth) acrylate, dipentaerythritol hexa (meth) acrylate, dipentaerythritol penta (meth) acrylate, tripentaerythritol hexa (meth) acrylate, tripentaerythritol penta (meth) acrylate, hydroxyl Di(meth)acrylate of pivalic acid neopentyl glycol di(meth)acrylate, ε-caprolactone adduct of hydroxypivalic acid neopentyl glycol, trimethylolpropane tris(methyl) UV-curable polyfunctional monomers such as acrylate, trimethylolpropane polyethoxy tris(meth)acrylate, di-trimethylolpropane tetra(meth)acrylate, etc. Polyfunctional acrylate oligomers such as polyester (meth) acrylate, epoxy (meth) acrylate, (meth) acrylate, and polyether (meth) acrylate.

In the above-described examples, from the viewpoint of improving the adhesion to the adherend, the heat resistance, and the effect of suppressing the wet heat whitening, a polyfunctional monomer or oligomer having a polar functional group is preferred. Things. Among them, a polyfunctional (meth) acrylate monomer having a hetero-cyanuric acid ring skeleton is preferably used.

The content of the crosslinking agent (B2) is not particularly limited. The standard is preferably 0.5 to 20 parts by mass, more preferably 1 part by mass or more or 15 parts by mass or less, more preferably 2 parts by mass, per 100 parts by mass of the (meth) acrylate copolymer (A2). A ratio of more than 10 parts by weight.

By the crosslinking agent (B2) in the above range, the shape-stable stability of the photocurable adhesive resin layer (I layer) in an uncrosslinked state and the photocurable adhesive resin layer (I layer) after crosslinking Resistant to foaming reliability. Among them, considering the balance with other elements, it is also possible to exceed this range.

(Photopolymerization initiator (C2))

The photopolymerization initiator (C2) functions as a reaction initiation aid for the crosslinking reaction of the above crosslinking agent (B2). An organic peroxide or a photopolymerization initiator which generates a radical by activating the active energy ray may be suitably used. Among them, from the viewpoint of controlling the easiness of the crosslinking reaction, a photopolymerization initiator, in particular, a photopolymerization initiator which induces ultraviolet rays having a wavelength of 380 nm or less is preferable.

On the other hand, when a photopolymerization initiator which induces light having a wavelength longer than a wavelength of 380 nm is used, the crosslinking reaction proceeds easily, for example, even when light is irradiated through a member which lacks ultraviolet ray permeability. The resin layer (I layer) is preferred in terms of hardening.

The photopolymerization initiator is roughly classified into two types according to a radical generation mechanism, and can be roughly classified into a cleavage type photopolymerization initiator which can decompose a single bond of a photopolymerization initiator itself to generate a radical, and The photoexcited initiator and the hydrogen donor in the system form a hydrogen-extracting photopolymerization initiator which promotes the complex and transfers hydrogen to the hydrogen donor.

In the above-mentioned cleavage type photopolymerization initiator, it is decomposed into other compounds by generating a radical by light irradiation, and if it is temporarily excited, it cannot have the work as a reaction initiator. can. Therefore, it is preferable that the adhesive sheet does not remain as an active material in the adhesive sheet after completion of the crosslinking reaction, and there is no possibility of causing undesired photodegradation or the like to the adhesive sheet.

On the other hand, when a hydrogen-extracting photopolymerization initiator is reacted by a radical irradiated with an active energy ray such as ultraviolet rays, a decomposition product such as a cleavage type photopolymerization initiator does not occur, so that it is difficult to become a reaction after completion of the reaction. Volatile ingredients are useful in reducing damage to the adherend.

Examples of the above-mentioned cleavage type photopolymerization initiator include benzoin butyl ether, benzoin dimethyl ketal, 2-hydroxyacetophenone, and diphenyl-2,4,6-trimethylbenzhydrazide. Phosphine oxide or such derivatives and the like.

Examples of the hydrogen extraction-type photopolymerization initiator include benzophenone, mischoketone, 2-ethylhydrazine, thioxanthone or a derivative thereof.

However, it is not limited to the above-mentioned thing as a photopolymerization initiator. As the adhesive composition β, either a cleavage type photopolymerization initiator or a hydrogen extraction type photopolymerization initiator may be used, or both may be used in combination.

The content of the photopolymerization initiator (C2) is not particularly limited. The standard is preferably 0.1 to 10 parts by mass, more preferably 0.5 part by mass or more or 5 parts by mass or less, and still more preferably 1 part by mass based on 100 parts by mass of the (meth)acrylate copolymer (A2). It is contained in the ratio of the mass part or more or 3 parts by mass or less.

By setting the content of the photopolymerization initiator (C2) to the above range, a moderate reaction sensitivity to the active energy ray can be obtained.

(other ingredients)

The adhesive composition β may also contain a known component formulated in a usual adhesive composition as a component other than the above. For example, various additives such as an adhesion-imparting resin or an antioxidant, a photostabilizer, a metal inerting agent, a rust preventive, an anti-aging agent, and a moisture absorbent may be contained as needed.

Further, a reaction catalyst (a tertiary amine compound or a quaternary ammonium system) may be suitably contained as needed. Compound, tin laurate compound, etc.).

[release layer (layer II)]

The release layer (layer II) is preferably a layer formed of a resin composition containing an olefin-based polymer (D) as a base polymer.

<Olefin polymer (D)>

Examples of the olefin-based polymer (D) include an ethylene-α-olefin copolymer, a styrene-based elastomer, a polyisobutylene resin, a polybutene resin, a polybutadiene resin, a polyisoprene resin, and ethylene. The cyclic olefin copolymer or the like is preferably used alone or in combination of two or more.

Among them, an ethylene-α-olefin copolymer, a styrene-based elastomer, and the like are preferably used from the viewpoint of imparting electrical properties, water vapor barrier properties, transparency, flexibility, sheet processability, and weather resistance reliability. Any one or a combination of two or more kinds of polyisobutylene resins may be used.

In this case, two or more kinds of olefin polymers having different compositions or molecular weights may also be used.

The "ethylene-α-olefin copolymer" may be a copolymer of ethylene and an α-olefin.

The type of the α-olefin copolymerized with ethylene is not particularly limited. Generally, an α-olefin having a carbon number of 3 to 20 can be preferably used. For example, propylene, 1-butene, 1-pentene, 1-hexene, 1-heptene, 1-octene, 1-decene, 1-decene, 3-methyl-1-butene , 4-methyl-1-pentene, and the like. Among them, the α-olefin is preferably a copolymer of 1-butene, 1-hexene or 1-octene as a copolymerization component from the viewpoints of ease of industrial availability, economy, and the like. In this case, the α-olefin copolymerized with ethylene may be used alone or in combination of two or more kinds in any ratio.

Further, the content of the α-olefin copolymerized with ethylene is not particularly limited. For example, it is preferably 2% by mole to 40% by mole based on the total amount of the monomers used in the copolymerization, and more preferably 3 mol% or more or 30 mol% or less, and further preferably 5 mol% or more or 25 mol% or less. When the content of the α-olefin copolymerized with ethylene is within the above range, the crystallinity is lowered by the copolymerization component, and transparency (for example, total light transmittance, haze, etc.) is improved, which is preferable. In addition, when the content of the α-olefin copolymerized with ethylene is within the above range, it is preferable to suppress the occurrence of adhesion or the like in the case of producing the raw material particles.

Further, the kind and content of the α-olefin copolymerized with ethylene can be analyzed by a well-known method such as a nuclear magnetic resonance (NMR: Nuclear Magnetic Resonance) measuring device or another machine analyzing device.

The above ethylene-α-olefin copolymer may also contain a monomer unit based on a monomer other than the α-olefin.

Examples of the monomer unit include a cyclic olefin, a vinyl aromatic compound (such as styrene), and a polyene compound.

When the content of the monomer unit is 100 mol% of all the monomer units in the ethylene-α-olefin copolymer, it is preferably 20 mol% or less, more preferably 15 mol% or less. .

Further, the stereostructure, branching, branching distribution, molecular weight distribution or copolymerization form (random, block, etc.) of the ethylene-α-olefin copolymer is not particularly limited, and for example, a copolymer having a long-chain branch, that is, a main The copolymer having a branched chain itself is generally excellent in mechanical properties, and has an advantage that the melt tension at the time of film formation is increased, and the formability is improved.

The above ethylene-α-olefin copolymer may have a crystal melting peak or no crystal melting peak. The upper limit of the crystal melting peak temperature is not particularly limited. In consideration of transparency or low-temperature flexibility, it is preferably 100 ° C or lower, more preferably 80 ° C or lower, and still more preferably 65 ° C or lower. Further, in consideration of the anti-blocking property of the raw material particles or the shape retention property at room temperature, the lower limit of the crystal melting peak temperature is preferably 20 ° C or more, more preferably 30 ° C or more, and further preferably It is 40 ° C or more. Also, the crystal melting peak temperature can be plural One.

The heat of crystal fusion of the ethylene-α-olefin copolymer is not particularly limited. It is preferably 0 to 100 J/g, more preferably 5 J/g or more or 80 J/g or less, and more preferably 10 J/g or more or 65 J/g or less. When it is in the above range, flexibility, transparency, and the like can be secured, which is preferable.

Further, the crystal melting peak temperature and the crystal melting heat amount can be measured by a differential scanning calorimeter (DSC) at a heating rate of 10 ° C/min in accordance with JIS K-7121.

The MFR (melt mass-flow rate) of the above-mentioned ethylene-α-olefin copolymer JIS K-7210 is preferably from 1 to 80 g/10 min, more preferably from 5 g/10 min to 60 g/10 min. More preferably, it is 8 g/10 min or more or 50 g/10 min or less.

The ethylene-α-olefin copolymer is preferably an ethylene-α-olefin copolymer having a density of 0.850 to 0.900 g/cm ³ , more preferably a density of 0.860 to 0.885 g, in order to impart excellent transparency or low-temperature characteristics. /cm ³ ethylene-α-olefin copolymer (linear low density polyethylene).

Among the ethylene-α-olefin copolymers, an ethylene-α-olefin random copolymer is more preferable from the viewpoint of low crystallinity and excellent light transmittance and flexibility. These may be used alone or in combination of two or more.

The method for producing the ethylene-α-olefin copolymer is not particularly limited, and a known polymerization method using a known catalyst for ethylene polymerization can be employed. As a known polymerization method, for example, a single catalyst represented by a Ziegler-Natta type catalyst or a single catalyst represented by a metallocene catalyst or a metallocene catalyst may be used. A slurry polymerization method, a solution polymerization method, a gas phase polymerization method, and the like, and a bulk polymerization method using a radical initiator.

From the viewpoints of easiness of pelletization after polymerization or anti-blocking of raw material particles, etc., it is preferred to use a single-touch which can be polymerized using a material having a low molecular weight component and a narrow molecular weight distribution. Manufactured by a polymerization method of a medium.

Examples of the "styrene-based elastomer" include SBR (styrene-butadiene). Ethylene rubber), SIB (styrene-isobutylene rubber), SBS (styrene-butylene-styrene block copolymer), SIS (styrene-isobutylene-styrene block copolymer), SEBS (styrene-ethylene) -butylene-styrene block copolymer), SEBC (styrene-ethylene-butylene-ethylene block copolymer), SIB (styrene-isobutylene block copolymer), HSBR (hydrogenated styrene butadiene rubber) )Wait.

The styrene content in the styrene-based elastomer is not particularly limited. For example, from the viewpoint of weather resistance, it is preferably 20 mol% or less based on the total monomer components constituting the elastomer.

The MFR of the above styrene-based elastomer (JIS K7210: temperature: 190 ° C, load: 21.18 N) is not particularly limited. It is preferably 5 g/10 min to 100 g/10 min, more preferably 8 g/10 min or more or 80 g/10 min or less, and further preferably 10 g/10 min or more or 50 g/10 min or less.

The "polyisobutylene resin" may be a resin having a polyisobutylene skeleton in a main chain or a side chain. For example, a homopolymer of an isobutylene monomer, a copolymer of isobutylene and a small amount of isoprene, a copolymer of isobutylene and n-butane or butadiene, and the like.

The viscosity average molecular weight (Mv) of the above polyisobutylene resin is not particularly limited. It is preferably 50,000 to 400,000, more preferably 70,000 or more, or 300,000 or less, and further preferably 100,000 or more and 200,000 or less. When the viscosity average molecular weight (Mv) is within the above range, workability, shape stability after processing, and practical heat resistance can be easily improved.

The olefin-based polymer (D) may have a functional group. By using an olefin-based polymer having a functional group, compatibility with an additive such as the following antioxidant can be improved, and the adhesion strength to the photocurable resin layer (I layer) or the substrate layer (III layer) can be adjusted. . Further, these may be used singly or in combination with an olefin-based polymer having no functional group, and in view of moldability, economy, and the like at the time of sheet formation, it is preferred to use an olefin polymerization having no functional group in combination. Things.

The olefin-based polymer having a functional group is preferably selected from a decane-modified olefin-based polymer or an acid-modified olefin-based polymer, an ethylene-vinyl acetate copolymer (EVA), and B. Ethylene-vinyl alcohol copolymer (EVOH), ethylene-methyl methacrylate copolymer (E-MMA), ethylene-ethyl acrylate copolymer (E-EAA), ethylene-glycidyl methacrylate copolymer (E -GMA) at least one resin of the group consisting of.

The molecular weight of the olefin polymer (D) is preferably from 50,000 to 400,000, more preferably from 60,000 to 300,000, and more preferably from 60,000 to 300,000, from the viewpoint of adjusting the melt viscosity at 130 ° C to a specific range as described below. It is especially good for more than 70,000 or less than 200,000.

<Other resins>

In the mold release layer (layer II), various additives may be added as needed in addition to the above olefin polymer (D).

Examples of the additive include a decane coupling agent, an antioxidant, a weathering stabilizer, a processing aid, a nucleating agent, an ultraviolet absorber, a flame retardant, and an anti-tarnishing agent. These additives may be used singly or in combination of two or more.

[Substrate layer (III layer)]

The base material layer (III layer) may function as a base material for easily releasing the release layer (layer II). Therefore, it is preferred to have a certain degree of hardness or viscosity, at least as compared with the bonding strength of the photocurable adhesive resin layer (I layer) based on the (meth) acrylate copolymer (A)-based resin, and The olefin-based polymer (D) is a release layer (layer II) of the base resin having a higher bonding strength.

In this regard, the base material layer (III layer) preferably contains one or two or more thermoplastic resins selected from the group consisting of polyester, polyolefin, polycarbonate, and acrylic resin as a base resin. Floor.

Among them, in order to improve the adhesion strength to the release layer (layer II), a polyolefin resin is preferably used.

Further, in addition to the above base resin, the base material layer (III layer) may be added with various additives as needed.

Examples of the additive include a decane coupling agent, an antioxidant, and weathering stability. A fixative, a processing aid, a nucleating agent, a UV absorber, a flame retardant, an anti-tarnishing agent, and the like. These additives may be used singly or in combination of two or more.

[layered structure]

The adhesive sheet laminate may have a base layer (III layer) on one side of the photocurable adhesive resin layer (I layer), and a photocurable adhesive resin layer on the other hand. The other side of the (I layer) has a structure of a release layer (IV layer) and a base material layer (V layer). In this case, it is preferred that the photocurable adhesive resin layer (I layer) and the release layer (II layer) on both sides are coextruded in two layers.

In this case, the release layer (IV layer) and the base material layer (V layer) which are laminated on the other side of the photocurable adhesive resin layer (I layer) can be, for example, a known method in which the surface of the film is subjected to release treatment. Mold film.

In addition, a structure in which a base layer (III layer) is provided on both sides of the photocurable adhesive resin layer (I layer) with a release layer (II layer) may be provided. In this case, the photocurable adhesive resin layer (I layer) may be coextruded with two types of three layers of the release layer (layer II).

Further, by making the composition of the release layer (layer II) located on both sides of the photocurable adhesive resin layer (I layer) different, three types of three layers can be co-extruded.

Further, other layers may be contained, and specific examples thereof include a transparent inorganic oxide film layer such as SiO ₂ or Al ₂ O ₃ , a barrier film layer, a retardation film layer for display, and an antistatic layer.

[thickness]

The thickness of the adhesive sheet laminate body can be reduced in thickness by reducing the thickness of the sheet. However, if the thickness becomes too thin, for example, when there is a concavo-convex portion on the surface of the bonding member, it is considered that there is a step around the generation. The possibility of bubbles.

From this point of view, the thickness of the adhesive sheet laminate is preferably from 80 to 2000 μm, more preferably from 100 μm to 1500 μm, and particularly preferably from 150 μm to 1000 μm.

The thickness of the photocurable adhesive resin layer (I layer) is preferably 50 μm to 1000 μm, more preferably 70 μm or more or 500 μm or less, further preferably 100 μm or more or 350 μm or less, and the release layer (layer II). The thickness is preferably from 5 μm to 500 μm, of which Preferably, it is 10 μm or more or 350 μm or less, and further preferably 18 μm or more or 250 μm or less, and the thickness of the base material layer (III layer) is preferably 25 μm to 500 μm, more preferably 38 μm or more or 350 μm or less. Preferably, it is 50 μm or more or 250 μm or less.

[This adhesive sheet laminate]

The adhesive sheet laminate can obtain the following physical properties.

<Fused viscosity>

In the adhesive sheet laminate, the I layer melt viscosity η _I at 130 ° C of the resin composition constituting the photocurable adhesive resin layer (I layer) and the resin composition constituting the release layer (layer II) are 130 The melt viscosity η _II of the layer II of °C is 1×10 ¹ ~5×10 ³ Pa. Within the range of s, the ratio η _II /η _{I of the} melt viscosity η _I of the layer _I to the melt viscosity η _II of the layer _II is preferably 0.05 to 30.

The first layer melt viscosity η _I of the resin composition constituting the photocurable adhesive resin layer (I layer) based on the (meth) acrylate copolymer (A) and the olefin-containing polymer (D) The second layer melt viscosity η _II of the resin composition as the release layer (II layer) of the base resin is adjusted to a specific range, and can exhibit the same degree of viscosity characteristics at the same temperature, so that it can be co-extruded by a total of Extrusion can improve the adhesion between the layers when integrated, so the interfacial adhesion between the two layers can be improved.

From this point of view, the layer I melt viscosity η _I of the resin composition constituting the photocurable adhesive resin layer (I layer) and the II layer melt viscosity η _II of the resin composition constituting the release layer (layer II) are preferably Both are 1 × 10 ¹ ~ 5 × 10 ³ Pa. s. If both are 1 × 10 ¹ Pa. Above s, it is easy to heat one side of the sheet, if it is 5 × 10 ³ Pa. Below s, it is preferable to maintain the adhesion between the layers and to facilitate integration of the layers. Wherein, the 130 ° C melt viscosity η is preferably 2 × 10 ¹ Pa. s above or 3 × 10 ³ Pa. Below s, especially preferably 3 × 10 ¹ Pa. s above or 1 × 10 ³ Pa. s below.

Further, from the above viewpoints, the η _II /η _{I of the} melt viscous η _{I of the I} layer and the melt viscosity η _II of the II layer are preferably 0.05 to 30, preferably 0.1 or more, or 25 or less, and further preferably 0.2 or more or 20 or less, and further preferably 0.3 or more or 15 or less.

One of the methods for adjusting the melt viscosity η _{I of the first} layer and the melt viscosity η _II of the layer _II is a resin which is a main component of each resin composition, that is, a (meth) acrylate copolymer (A) and an olefin polymerization. A method of molecular weight of the substance (D).

From this point of view, the weight average molecular weight (Mw) of the (meth) acrylate copolymer (A) is preferably from 100,000 to 800,000, more preferably more than 150,000 or less than 550,000, of which 20 is particularly preferred. More than 10,000 or less than 500,000.

On the other hand, the weight average molecular weight (Mw) of the olefin-based polymer (D) is preferably 50,000 to 400,000, more preferably 60,000 or more, or 200,000 or less, and particularly preferably 70,000 or more and 150,000 or less. .

Further, the melt viscosity can be adjusted by increasing or decreasing the amount of the component added such as the crosslinking agent or the photocrosslinking initiator.

<Si existence ratio of surface of layer I>

The Si of the surface of the photocurable adhesive resin layer (I layer) is preferably less than 2.0 atom%.

When the ratio of the Si of the surface of the photocurable adhesive resin layer (I layer) is less than 2.0 atom%, there is no possibility that the adhesion of the photocurable adhesive resin layer is lowered or the adherend is contaminated by the migration of Si. Preferably.

From this point of view, the Si of the surface of the photocurable adhesive resin layer (I layer) is preferably less than 2.0 atom%, more preferably less than 1.5 atom%, and particularly preferably less than 1.0 atom%.

If the ratio of Si on the surface of the photocurable adhesive resin layer (I layer) is less than 2.0 atom%, the transition component related to the release layer (layer II) may not be mixed. Among them, this method is not limited.

<II layer peeling force>

The release layer (layer II) is removed from the photocurable adhesive resin layer (I layer) at a peeling speed of 300 The peeling force at the time of 180° peeling of mm/min is preferably 0.3 N/cm or less.

When the peeling force is 0.3 N/cm or less, the peeling resistance is small and the workability is excellent, which is preferable. However, if the peeling force is too small, there is a possibility that bulging or peeling occurs in an unintended scene during work or when it is stored as a wound body.

Therefore, from this point of view, the peeling force is preferably 0.3 N/cm or less, more preferably 0.01 N/cm or more or 0.25 N/cm or less, and particularly preferably 0.02 N/cm or more or 0.2 N/cm. the following.

Moreover, it is preferable that the peeling force of the base material layer (III layer) and the mold release layer (II layer) is larger than the peeling force between the photocurable adhesive resin layer (I layer) and the release layer (II layer).

Self-photohardening by the peeling force between the base layer (III layer) and the release layer (II layer) is greater than the peeling force between the photocurable adhesive resin layer (I layer) and the release layer (II layer) The adhesive layer (layer I) was peeled off from the substrate layer (layer III) and the release layer (layer II).

Further, in the present adhesive layer system, a release layer (layer II) is provided on one side of the photocurable adhesive resin layer (I layer) to provide a base layer (III layer), and photocurable adhesive is provided on the other hand. When the other side of the resin layer (I layer) is provided with a release layer (IV layer) and a base layer (V layer), the photocurable adhesive resin layer (I layer) and the release layer (II) can be used. The peeling force of the layer) is different from the peeling force of the photocurable adhesive resin layer (I layer) and the release layer (IV layer).

Thus, if the peeling force of the photocurable adhesive resin layer (I layer) and the release layer (II layer) is different from the peeling force of the photocurable adhesive resin layer (I layer) and the release layer (IV layer), for example, When the peeling force is small, in other words, the release layer on the side which is easy to peel off is peeled off, the release layer on the other side can be prevented from being peeled off at the same time, and workability can be improved.

<I layer adhesion>

The adhesion of the photocurable adhesive resin layer (I layer) is preferably from 3 N/cm to 30 N/cm.

When the adhesion of the photocurable adhesive resin layer (I layer) is from 3 N/cm to 30 N/cm, it is easy to obtain the foaming reliability of the laminated body.

Therefore, from the viewpoint of the above, the adhesion of the photocurable adhesive resin layer (I layer) is preferably from 3 N/cm to 30 N/cm, more preferably from 4 N/cm to 25 N/cm, and particularly preferably It is 5 N/cm or more or 20 N/cm or less.

Further, in order to adjust the adhesion of the photocurable adhesive resin layer (I layer) to 3 N/cm to 30 N/cm, it is preferred to adjust the composition (I layer) of the (meth) acrylate copolymer (A). In addition to the composition or molecular weight or the adjustment of the crosslinking agent (B), it is also suitable to add an additive such as a decane coupling agent which contributes to the improvement of the adhesion. However, it is not limited to this method.

[Method of manufacturing the adhesive sheet laminate]

Next, an example of a method of manufacturing the present adhesive sheet laminate will be described. However, this is only an example, and the manufacturing method of the adhesive sheet laminate is not limited to the following manufacturing method.

The adhesive sheet laminate can be produced, for example, by a resin composition for forming a photocurable adhesive resin layer (I layer), that is, a (meth) acrylate copolymer (A), a crosslinking agent. The resin composition of (B) and the photopolymerization initiator (C) is co-extruded with the resin composition forming the release layer (layer II), that is, the resin composition containing the olefin polymer (D). After the release layer (layer II) is laminated on one side or both sides of the photocurable adhesive resin layer (I layer), it is not photohardened, and a base material layer (III layer) is laminated on the release layer (layer II). The adhesive sheet layer provided with the base material layer (III layer) on one side or both sides of the photocurable adhesive resin layer (I layer) containing the photocurable adhesive resin is formed by interposing the release layer (II layer). body.

In this case, the resin composition for forming the photocurable adhesive resin layer (I layer) and the resin composition for forming the release layer (II layer) and the resin composition for further forming the base material layer (III layer) may be used. The present adhesive sheet laminate was produced by co-extrusion.

[Method of Manufacturing Image Display Device Building Member Laminate]

Next, a method of manufacturing an image-displaying device constituent member laminated body using the present adhesive sheet laminate to form an image-displaying device constituent member laminated body (referred to as "the present image display device constituting member laminated body") will be described.

The image display device constituting member laminate can be manufactured, for example, by the method described above. The adhesive sheet laminate is obtained by separating the release layer (II layer) and the base material layer (III layer) from the photocurable adhesive resin layer (I layer) of the adhesive sheet laminate, and then separating the light hardening layer. Adhesive adhesive layer (I layer) is formed by two image display device constituent members, and one or two of the image display device constituent members are irradiated with light to cure the photocurable adhesive resin layer (I layer), thereby manufacturing The image display device constitutes a component laminate.

<Shaping processing>

Alternatively, the present adhesive sheet laminate may be formed in the same shape as the uneven shape of the bonding surface of the image display device constituent member, and the present image forming apparatus constituent member laminate may be produced by using the adhesive sheet laminate as described above.

Further, as the shaping method, for example, the adhesive sheet laminate can be formed by a shape of a pressurizing mold, shaping using a mold, forming by a roll, forming by lamination, and the like. .

Among them, from the viewpoints of productivity, precision of forming processing, and the like, it is preferably a forming method by a press frame or a roll. In other words, as a method of forming a surface shape having the same shape as the uneven shape of the bonding surface of the image forming device constituent member, a mold for molding the uneven shape of the bonding surface of the image forming device constituent member can be preferably exemplified. Pressing at least one side surface of the photocurable adhesive resin layer (I layer) via the release layer (layer II) and the substrate layer (layer III), that is, with the release layer (layer II) and the substrate layer (III) Layer) A method of forming together.

In the case where the release film is formed as described above, in other words, when the release film is formed together, it is preferable to use an unstretched film as the release film of the release layer (layer II). When the forming treatment is performed by a press treatment or the like by using the unstretched film, it is possible to have an effect of easily forming a surface shape substantially the same as that of the original mold.

In the above unstretched film, it is more preferable to use any of an unstretched polypropylene film, an unstretched polyethylene film, and an unstretched polyester film from the viewpoint of mechanical strength, flexibility, and chemical resistance of the film itself. .

The shape of the pressurizing mold frame can be exemplified by the release layer (layer II) and the substrate layer (layer III). A method of pressurizing at least one side surface of the photocurable adhesive resin layer (I layer).

Further, the mold release layer (II layer) and the base material layer (III layer) may be press-formed by a press mold, and the mold release layer (II layer) and the base material layer (III layer) may be formed thereon. The adhesive composition layer is coated or inflowed to produce a shaped adhesive sheet. At this time, the shaping of the mold can also be carried out by forming the adhesive composition into the mold frame and solidifying it to produce a shaped double-sided adhesive sheet.

By forming the roll, the adhesive sheet layer having the photocurable adhesive resin layer (I layer), the release layer (II layer), and the base material layer (III layer) can be formed by passing between the rolls. .

By forming the laminate, the two-sided adhesive sheet 1 can be formed by forming two planar adhesive sheets of different sizes and overlapping them.

When the surface of the adhesive sheet laminate is formed in the same shape as the uneven surface of the bonding surface of the image display device constituent member, even if the bonding surface of the image display device constituent member has a step portion due to printing or the like, A constituent member for each image display device such as a surface protection panel or a touch panel can be bonded without a gap.

The specific shaping method will be described below. However, it is not limited to these methods.

(Formation method using a pressurizing frame)

a) a method of pressurizing through a release layer (layer II) and a substrate layer

It is suitable to cut an adhesive sheet layer having a photocurable adhesive resin layer (I layer), a release layer (II layer), and a base material layer (III layer), and roll the cut adhesive sheet laminate body while using it along the side. The surface of the adherend, which is a concave-convex shape of the surface of the adherend, that is, the surface of the surface to be coated, is heat-pressed through the release layer (layer II) and the base layer (layer III) to form a surface.

Next, the release layer (layer II) is peeled off, and the exposed adhesive sheet is cut along the shape of the shaped shape, and the unnecessary adhesive layer of the outer periphery of the outer shape is discarded, and the new release film larger than the outer cut size is reattached.

Again, the monolithic cut is made into an operable shape, and the adhesive sheet laminate is produced.

b) method of directly pressing the adhesive sheet

It is suitable to cut an adhesive sheet layer having a photocurable adhesive resin layer (I layer), a release layer (II layer), and a base material layer (III layer), and roll off the cut adhesive sheet laminate body while peeling off the release sheet In the layer (layer II), the photocurable adhesive resin layer (I layer) is directly subjected to thermal pressurization using a pressure mold frame along the surface uneven shape of the adherend, that is, the surface shape of the surface 2a to be faced. Forming.

Next, the photocurable adhesive resin layer (I layer) exposed on one side is cut along the shape of the shape, and the unnecessary release adhesive material on the outer periphery of the outer shape is discarded, and the new release film larger than the outer cut size is reattached. .

Again, the monolithic cut is made into an operable shape, and the adhesive sheet laminate is produced.

The material of the pressurizing mold frame is not particularly limited, and a polyphthalocyanine resin or a fluorine-based resin excellent in mold release property can also be used. Further, even if it is a material having no mold release property such as stainless steel or aluminum, it can be preferably used by applying various release agents.

The temperature of the hot press is, for example, room temperature or higher, preferably 80 ° C or higher, more preferably 100 ° C or higher. Further, the pressurizing pressure, the pressurizing depth, and the pressurizing time can be appropriately adjusted depending on the size, shape, and shaping state.

Further, as the cutting method, for example, a cutting method using a Tomson knife or a rotary knife can be cited.

Further, there is a method in which the surface forming and the outer shape cutting are performed in different processes as described above. For example, if a mold for integrating the forming mold and the cutting mold is used, the surface forming can be performed in one step. Shape cutting.

(Formation method using the release film of the shaped processing)

The release film which is previously formed into a surface shape which is substantially the same as the surface unevenness of the adherend, that is, the surface shape of the surface to be coated, is disposed at least on one side, and an adhesive is applied to form a surface-forming adhesive. The sheet is the original sheet of the photocurable adhesive resin layer (I layer).

Next, after appropriately cutting according to the width of the surface irregular shape of the original sheet, the cut adhesive sheet is peeled off from the one side of the release sheet in the next step, and is cut along the outer shape. After sticking to the one side, discard the unwanted adhesive material on the outer circumference of the outer shape, and then reattach the new release film larger than the outer cut size.

Again, the monolithic cut is made into an operable shape, and the adhesive sheet laminate is produced.

(using the shaping method of the mold)

A surface-formed adhesive sheet, that is, a photocurable adhesive resin layer (I layer), is formed by applying or injecting an adhesive to a surface of the surface of the adherend which is molded into a concave-convex shape, that is, a surface to be coated.

When the mold is only one side, after applying or injecting the adhesive, the release film is bonded to the opposite side, and the rubber sheet or the like is adhered thereto.

After the adhesive is cured, the adhesive sheet laminate is pulled away from the mold by pulling off the release film.

The material of the mold is not particularly limited, and a polyoxymethylene resin or a fluorine-based resin excellent in mold release property can also be used. Further, even a mold having a material such as stainless steel or aluminum which is not released from the mold can be preferably used by applying various release agents.

(Using the shape of the roller)

After applying a photocurable adhesive resin layer (I layer) between the two flat release films, the surface irregularities of the molded adherend are disposed on at least one side, that is, the surface shape of the surface to be coated. The roll is formed by sandwiching and passing between the roll and the roll on the other side, and the film is formed into an original sheet of an adhesive sheet, that is, a photocurable adhesive resin layer (I layer).

Next, after appropriately cutting according to the width of the surface irregular shape of the original sheet, the cut adhesive sheet is peeled off from the release film on one side in the next step, and the exposed adhesive sheet is cut along the shape of the shaped shape, and discarded. After the outer edge of the outer shape is not required to be adhered to the edge material, the new release film is larger than the outer cut size.

Again, the monolithic cut is made into an operable shape, and the adhesive sheet laminate is produced.

Regarding the roll temperature, the shaping roll is disposed, and the temperature at the time of surface forming between the roll and the roll on the other side is preferably room temperature or more, more preferably 80 ° C or more. More preferably, it is 100 ° C or more.

(by layering)

It is suitable for cutting a flat sheet of a light-curable adhesive resin layer (I layer) which is a flat adhesive sheet having a release film of two areas, and respectively forming a flat first adhesive sheet which is cut into a shape of the open surface, and is cut into steps. A second adhesive sheet having a flat shape having a different surface shape.

Thereafter, the release film on one side is peeled off, and the exposed adhesive faces are superposed on each other to form a desired adhesive sheet laminate having a desired surface shape.

<Description of statement>

In the case of the present invention, the expression "X~Y" (where X and Y are arbitrary numbers), unless otherwise specified, includes "more preferably greater than the meaning of "X or more and Y or less". X" or "preferably less than Y" means.

In the case of "X or above" (X is an arbitrary number) or "Y below" (Y is an arbitrary number), it is intended to include the meaning of "better than X" or "preferably not up to Y". .

In addition, the term "slice" in the definition of JIS generally means a product which is relatively thin and generally has a thickness smaller than the length and width. Generally, the term "film" means that the thickness is extremely small and the maximum thickness is arbitrary. A thin, flat product is usually supplied in the form of a reel (Japanese Industrial Standard JIS K6900). For example, in terms of thickness, a person who is 100 μm or more in a narrow sense is sometimes referred to as a sheet, and a person who is less than 100 μm is referred to as a film. However, the boundary between the sheet and the film is not certain, and it is not necessary to distinguish the two in writing in the present invention. Therefore, in the present invention, the case of "film" also includes "slice", which is called "slice". It also includes "film".

[Examples]

Hereinafter, the details will be described in further detail by way of examples. However, the invention is not limited by these.

[Resin Composition 1 for Layer I]

The number average molecular weight of the (meth) acrylate copolymer (A) is 2,400. 15 parts by weight of a polymethyl methacrylate macromonomer, and an acrylate copolymer (A-1) (weight average molecular weight: 230,000) obtained by randomly copolymerizing 81 parts by weight of butyl acrylate and 4 parts by weight of acrylic acid, Glycerol dimethacrylate (manufactured by Kyoeisha Chemical Co., Ltd., product name: G101P) (B-1) 100 g as a crosslinking agent (B), 2, 4, 6- as a photopolymerization initiator (C) A mixture of trimethylbenzophenone and 4-methylbenzophenone (manufactured by Lanberti Co., Ltd., product name: Esacure TZT) (C-1) 15 g was uniformly mixed to prepare a resin composition for layer I (I-1) ).

The 130 ° C melt viscosity η _I of the resin composition for layer I (I-1) is 4.7 × 10 ¹ Pa. s.

[Resin Composition 2 for Layer I]

A vinyl copolymer obtained by randomly copolymerizing 55 parts by mass of 2-ethylhexyl acrylate as a (meth) acrylate copolymer (A) with 40 parts by mass of vinyl acetate and 5 parts by mass of acrylic acid (A) -2) (weight average molecular weight: 170,000) 1 kg, uniformly mixed as a crosslinking agent (B) of triacrylic acid (2,4,6-trioxo-1,3,5-three -1,3,5-triyl)trisole (B-2) (manufactured by Toagosei Co., Ltd., product name: ARONIX M315) 75 g and Esacure KTO46 (C-2) as photopolymerization initiator (C) 15 g of (manufactured by Lanberti Co., Ltd.) was used to prepare a resin composition (I-2) for layer I.

The 130 ° C melt viscosity η _I of the resin composition for layer I (I-2) is 4.0 × 10 ² Pa. s.

[Resin Composition 3 for Layer I]

As the resin composition for layer I 3, a block copolymer of methyl methacrylate and butyl acrylate was prepared (manufactured by Kuraray Co., Ltd., product name: KURARITY LA2140e, density: 1080 kg/m ³ , melting point: 55 ° C, weight average Molecular weight (Mw): 100,000, MFR (190 ° C, 21.18 N): 35 g/10 min) was used as the resin composition (I-3) for the I layer.

The 130 ° C melt viscosity η _I of the resin composition for layer I (I-3) is 1.7 × 10 ⁵ Pa. s.

[Resin Composition for Layer II 1]

As the olefin-based polymer (D), an ethylene-butene random copolymer (d-1) (density: 870 kg/m ³ , melting point: 55 ° C, weight average molecular weight (Mw): 100,000, MFR (190 ° C) 21.18N): 35 g/10 min) as a resin composition (II-1) for a layer II.

The melt viscosity η _II at 130 ° C of the resin composition for layer II (II-1) is 7.3 × 10 ² Pa. s.

[Resin Composition 2 for Layer II]

As the olefin-based polymer (D), for the ethylene-butene random copolymer (d-1) 1 kg, a mixed decane-modified ethylene-octene random copolymer (d-2) (density: 870 kg/m ³ , Melting point: 50 ° C, MFR (190 ° C, 21.18 N): 36 g/10 min, weight average molecular weight (Mw): 250,000) 100 g, and used as the resin composition (II-2) for the second layer.

The 130 ° C melt viscosity η _II of the resin composition for layer II (II-2) is 7.5 × 10 ² Pa. s.

[Resin Composition 3 for Layer II]

As the olefin-based polymer (D), as the ethylene-butene random copolymer (d-1) (density: 870 kg/m ³ , melting point: 55 ° C, weight average molecular weight (Mw): 100,000, MFR ( 190 ° C, 21.18 N): 35 g/10 min) 1 kg, mixed ethylene-methacrylate copolymer (d-3) (density: 946 kg / m ³ , melting point: 93 ° C, weight average molecular weight (Mw): 160,000, MFR (190 ° C, 21.18 N): 5.0 g/10 min) 110 g, and a resin composition (II-3) for a layer II was produced.

The 130 ° C melt viscosity η _II of the resin composition for layer II (II-3) is 9.9×10 ² Pa. s.

[Example 1]

For the polyethylene terephthalate film (III-1: manufactured by Mitsubishi Plastics Co., Ltd., product name: DIAFOIL T-100, thickness 50 μm) as a base material layer (III layer), the layer was sequentially laminated as a release layer. The resin composition (II-1) (thickness: 38 μm) of the (II layer) and the resin composition (I-1) (thickness: 150 μm) as the photocurable adhesive resin layer (I layer) were extruded. After being co-extruded at 130 ° C and formed into a sheet shape, the release-treated polyethylene terephthalate film (manufactured by Mitsubishi Plastics Co., Ltd., product name: DIAFOIL MRA, thickness: 100 μm, marked as " The release sheet ") is overlaid on the photocurable adhesive resin layer (I layer) to form an adhesive sheet laminate 1.

[Embodiment 2]

In addition to the use of the resin composition (I-2) in place of the resin composition (I-1), The adhesive sheet laminate 2 is produced in the same manner.

[Example 3]

The adhesive sheet laminate 3 was produced in the same manner as in Example 1 except that the resin composition (II-2) was used instead of the resin composition (II-1).

[Example 4]

The adhesive sheet laminate 4 was produced in the same manner as in Example 1 except that the resin composition (II-3) was used instead of the resin composition (II-1).

[Example 5]

A resin composition (II-2) as a release layer (II layer) was sequentially laminated on a biaxially oriented polypropylene film (III-2: thickness: 38 μm) as a substrate layer (III layer) (thickness: 50 μm), a resin composition (I-1) (thickness: 100 μm) as a photocurable adhesive resin layer (I layer), which is co-extruded at a pressing temperature of 130 ° C to form a sheet, and then A release-treated polyethylene terephthalate film (manufactured by Mitsubishi Plastics Co., Ltd., product name: DIAFOIL MRF, thickness: 75 μm) was overlaid on the photocurable adhesive resin layer (I layer) to form an adhesive sheet laminate. 5.

[Comparative Example 1]

The release treatment surface of the polyethylene terephthalate film (manufactured by Mitsubishi Plastics Co., Ltd., product name: DIAFOIL MRF, thickness: 75 μm) which has been subjected to mold release treatment by a polyoxyl resin in advance is used only as a release surface. After the resin composition (I-1) (thickness: 150 μm) of the layer I of the photocurable adhesive resin layer (I layer) is formed into a sheet shape, the release-treated polyethylene terephthalate film (Mitsubishi) The resin company, product name: DIAFOIL MRA, thickness: 100 μm) was coated with a photocurable adhesive resin layer (I layer) to form an adhesive sheet laminate 6.

[Comparative Example 2]

The same procedure as in Example 1 except that the resin composition (I-3) for the first layer was replaced by the resin composition (I-1) for the first layer, and co-extruded at a pressing temperature of 160 ° C to form a sheet. In the manner, the adhesive sheet laminate 7 is produced.

[Comparative Example 3]

The release layer of the polyethylene terephthalate film (manufactured by Mitsubishi Plastics Co., Ltd., product name: DIAFOIL MRA, thickness: 100 μm) which has been subjected to release treatment is sequentially laminated as a photocurable adhesive resin layer ( The resin composition (I-1) (thickness: 150 μm) of the layer I, and the resin composition (II-3) (thickness: 100 μm) as the release layer (layer II) were extruded at 180 ° C. The adhesive sheet laminate 8 was produced by co-extrusion and forming into a sheet shape.

[Evaluation]

(Peel force)

A soda lime glass having a width of 75 mm, a length of 200 mm, and a thickness of 3 mm was used as a support substrate for measuring the peeling force of the release layer (layer II).

The adhesive sheet laminate produced in the examples and the comparative examples was cut into a width of 50 mm and a length of 200 mm, and the opposite side of the base material layer (III layer) was hand-pressed using a double-sided tape (manufactured by Nitto Denko Corporation, product name: No. 5000). That is, the laminate of the release-treated polyethylene terephthalate film is pressure-bonded to the support substrate.

The base material layer (III layer)/release layer (II layer) of the above sample was peeled off from the photocurable adhesive resin layer (I layer) at a peeling angle of 180° and a peeling angle of 300 mm/min, and the release layer (layer II) was measured. The peeling force (N/cm) of the photocurable adhesive resin layer (I layer) is shown as "II layer peeling force" in the table.

In addition, since the base material layer (III layer) was not laminated in the adhesive sheet laminate 8 of Comparative Example 3, only the release layer (II layer) was peeled off from the photocurable adhesive resin layer (I layer).

Further, in the adhesive sheet laminate 6 of Comparative Example 1, a polyethylene terephthalate film (manufactured by Mitsubishi Plastics, Inc., product name: DIAFOIL MRA, thickness: 100 μm) was attached to the support substrate, and the peeling was removed. The value of the mold-treated polyethylene terephthalate film (manufactured by Mitsubishi Plastics Co., Ltd., product name: DIAFOIL MRF, thickness: 75 μm) is shown in the table.

(adhesion)

In the adhesive sheet laminate produced in the examples and the comparative examples, the release layer (layer II) was peeled off from the photocurable adhesive resin layer (I layer), and the exposed adhesive surface was bonded to a substrate film of 100 μm. A PET film (manufactured by Toyobo Co., Ltd., product name: COSMOSHINE A4300, thickness: 100 μm) was used to produce a laminate. After the laminated product was cut into a width of 10 mm and a length of 150 mm, the remaining release film was peeled off, and the exposed adhesive surface roll was pressure-bonded to the soda lime glass using a hand roller. After the final bonding was carried out by autoclaving (80 ° C, gauge pressure: 0.2 MPa, 30 minutes) of the thus obtained laminate, a high-pressure mercury pump was used from the side of the substrate PET film to have a cumulative light amount of 2000 mJ/cm ² . The 365 nm ultraviolet light is irradiated to harden the adhesive sheet. The mixture was cured at 23 ° C and 50% RH for 15 hours to prepare a sample for adhesion measurement.

The peeling force measurement sample was peeled off at a peeling angle of 180° in an environment of 23° C. and 40% RH at a peeling speed of 60 mm/min, and the adhesion of the layer I to the glass (N/cm) was measured. "I layer adhesion".

(by elemental analysis of ESCA)

The release layer (layer II) of the adhesive sheet laminate produced in the examples and the comparative examples was peeled off, and an adhesive photoelectron spectroscopy device (manufactured by ULVAC-PHI Co., Ltd.) was used for the exposed photocurable adhesive resin layer (I layer). Product name: ESCA-5100) The surface composition ratio (atom%) of Si was determined, and the table shows "the ratio of Si on the surface of the layer I".

At this time, when the surface composition ratio (atom%) of Si does not reach the detection limit, the table indicates "undetected".

Further, with respect to the adhesive sheet laminate 6 of Comparative Example 1, the polyethylene terephthalate film (manufactured by Mitsubishi Plastics Co., Ltd., product name: DIAFOIL MRF, thickness: 75 μm) was peeled off to expose the photocurable adhesive resin layer. The surface of (I layer) was measured.

(Processability)

The adhesive sheet laminates 1 to 8 produced in the examples and the comparative examples were cut into 100 pieces using a Tomson punch with a 50 mm × 80 mm to confirm the presence or absence of the release layer (layer II) or the release film. Those who have more than 10 ridges at the end will be judged as "×(poor)", less than 10 It is judged as "○ (good)".

(keeping stability)

50 pieces of the cut pieces of the adhesive sheet laminated body produced in the above-mentioned processing suitability evaluation were allowed to stand for 3 days in an environment of 40 ° C.

The adhesives of the adhesive sheet laminates which were placed in an overlapping manner after curing were judged to be "x (poor)", and those who were not observed were judged as "○ (good)".

(Flame resistance reliability)

A black film having a thickness of 20 μm was applied to a peripheral portion of 5 mm of soda lime glass (82 mm × 53 mm × thickness: 0.5 mm) to prepare a glass substrate for evaluation having a printing step of 20 μm in the peripheral portion.

A single polarizing plate ("HLC2-5618" manufactured by Sanritz Co., Ltd.) was bonded to a glass plate (83 × 52 mm × t 0.5 mm) in advance as a coating adherend for evaluation. Face.

The adhesive sheet laminates 1 to 8 produced in the examples and the comparative examples were cut into 80 mm × 50 mm. The release layer (layer II) was peeled off, and the exposed photocurable adhesive resin layer (I layer) was adhered to the surface having the printing step of the evaluation release substrate by using a hand roller to cover the printing step portion. Then, the remaining release film was peeled off, and the polarizing plate surface of the above-mentioned evaluation adherend was pressure-bonded to the exposed adhesive surface under reduced pressure (absolute pressure: 5 kPa), and autoclave treatment was performed (80 ° C, gauge pressure: 0.2 MPa, 30 minutes) The final bonding was performed, and the laminated body for evaluation was produced.

The laminated body for evaluation was irradiated with ultraviolet rays so that the cumulative light amount at 365 nm became 2000 mJ/cm ^{2 from} the side of the glass substrate for evaluation, and the adhesive sheet was cured at 23 ° C and 50% RH. 15 hours as a sample for evaluation of foaming reliability.

The foaming reliability evaluation sample prepared in this manner was stored in an environment of 85 ° C and 85% RH for 100 hours, and then the appearance was visually observed, and the deformation or foaming of the adhesive material after the environmental test was performed, and the peeling was judged as "×. (Poor), and the unproduced person is judged as "○ (good)".

(Overview)

A comprehensive evaluation of all the above-mentioned evaluation items is shown as "○ (good)", and a comprehensive evaluation of one or more evaluation items that does not show good results is "x (poor)".

[investigation]

The adhesive sheet laminates produced in Examples 1 to 5 are excellent in not only the release layer (II layer) but also the photocurable adhesive resin layer (I layer), and are formed by co-extrusion. There is a rise due to the trimming process, and the workability is excellent. Further, in the surface of the photocurable adhesive resin layer (I layer) which is in contact with the release layer (layer II), a migration component such as a polyfluorene release agent is not confirmed, and the stain resistance of the adherend is also excellent. . Further, the photocurable adhesive resin layer has photocurability, and is excellent in foaming resistance after bonding the adhesive sheet.

On the other hand, the adhesive sheet layer system of Comparative Example 1 was formed by releasing the film on the two surface areas of the photocurable adhesive resin layer (I layer). Therefore, the release agent was adhered to the surface of the first layer, and it was confirmed that The release agent migrates to the adherend when it is attached. Further, if the release property of the release film is to be improved, that is, a release film having a small peeling force is used, a release film is likely to be formed at the time of cutting. The bulging is inferior in workability as compared with the above embodiment.

In the adhesive sheet laminate of Comparative Example 2, a resin having no photocurability was used as the adhesive resin layer, and as a result, the workability was excellent, but it was difficult to affinity with the uneven surface, and foaming occurred under high-temperature and high-humidity environment, and the quality of the adhesive sheet was obtained. Poor.

Since the adhesive sheet laminate of Comparative Example 3 does not have the base material layer (III layer), the exposed release layer (layer II) and the release film which are placed in an overlapping manner are partially gelled (adhesively) with a long period of time, and the storage stability is inferior.

As the adhesive sheet laminates obtained in Examples 1 to 5, it was confirmed that the peeling force of the base material layer (III layer) and the release layer (II layer) was larger than that of the photocurable adhesive resin layer (I layer) and the release layer ( Stripping force between layers II).

It is considered that the 130 ° C melt viscosity of the resin composition constituting the photocurable adhesive resin layer (I layer) and the release layer (II layer) is preferably the result of the test conducted by the above-described examples and the inventors. η _I and η _II are 1 × 10 ¹ ~ 5 × 10 ³ Pa. s, and the melt viscosity of 130 ℃ constituting the light-curing adhesive resin layer (I layer) of the resin composition of the melt viscosity η 130 ℃ _I constituting the parting layer (II layer) of the resin composition of η _II ratio η _II /η _I is in the range of 0.05 to 30.

It is preferable that the thickness of the photocurable adhesive resin layer (I layer) is preferably 50 μm to 1000 μm, and more preferably 70 μm or more or 500 μm or less, from the results of the above-described examples and the results of experiments conducted by the inventors. Further, it is preferably 100 μm or more or 350 μm or less, and the thickness of the release layer (layer II) is preferably 5 μm to 500 μm, more preferably 10 μm or more or 350 μm or less, and further preferably 18 μm or more or 250 μm or less. The thickness of the base material layer (III layer) is preferably 25 μm to 500 μm, more preferably 38 μm or more or 350 μm or less, and further preferably 50 μm or more or 250 μm or less.

Claims (17)

An adhesive sheet laminate characterized in that it is provided on a one side or both sides of a photocurable adhesive resin layer (I layer) containing a photocurable adhesive resin, and a release layer (layer II) is provided to have a substrate layer (Layer 3), and the photocurable adhesive resin layer (I layer) is a resin containing a (meth) acrylate copolymer (A), a crosslinking agent (B), and a photopolymerization initiator (C). The layer formed in the state before photohardening of the composition, the release layer (layer II) is a layer formed of a resin composition containing the olefin polymer (D), and the photocurable adhesive resin layer (I) The layer) and the above-mentioned release layer (layer II) are coextruded bodies. An adhesive sheet laminate characterized in that it is provided on a one side or both sides of a photocurable adhesive resin layer (I layer) containing a photocurable adhesive resin, and a release layer (layer II) is provided to have a substrate layer (Layer 3), and the photocurable adhesive resin layer (I layer) is a resin containing a (meth) acrylate copolymer (A), a crosslinking agent (B), and a photopolymerization initiator (C). The layer formed in the state before photohardening of the composition, the release layer (layer II) is a layer formed of a resin composition containing the olefin polymer (D), and constitutes the photocurable adhesive resin layer ( The 130 ° C melt viscosity η _I and η _II of the resin layer of the layer I and the above release layer (II layer) are both 1×10 ¹ to 5×10 ³ Pa. s. The adhesive sheet laminate according to claim 1 or 2, wherein a peeling force of the base material layer (III layer) and the release layer (II layer) is greater than that of the photocurable adhesive resin layer (I layer) and the release layer (II layer) The peeling force between them. The adhesive sheet laminate according to any one of claims 1 to 3, wherein the photocurable adhesive layer The (meth) acrylate copolymer (A) of the resin layer (I layer) contains an acrylic copolymer having a graft copolymer of a macromonomer as a branch component. The adhesive sheet laminate according to any one of claims 1 to 3, wherein the (meth) acrylate copolymer (A) of the photocurable adhesive resin layer (I layer) has a glass transition temperature (Tg) The monomer a1 at 0 °C and the monomer a2 having a glass transition temperature (Tg) of 0 ° C or higher and less than 80 ° C and the monomer a3 having a glass transition temperature (Tg) of 80 ° C or higher are a1: a2: a3 = 10~ A (meth) acrylate copolymer having a weight average molecular weight of 50,000 to 400,000 obtained by copolymerization of a molar ratio of 40:90 to 35:0 to 25. The adhesive sheet laminate according to any one of claims 1 to 5, wherein a 130 ° C melt viscosity η _I of the resin composition constituting the photocurable adhesive resin layer (I layer) and the release layer (II layer) η _II is 1 × 10 ¹ ~ 5 × 10 ³ Pa. s, deg.] C and a melt viscosity constituting the light 130.-curing adhesive resin layer (I layer) of the resin of deg.] C the composition of the melt viscosity of _I [eta] and 130. constituting the parting layer (II layer) of the resin composition of η _II ratio η _II /η _I is 0.05~30. The adhesive sheet laminate according to any one of claims 1 to 6, wherein the crosslinking agent (B) of the photocurable adhesive resin layer (I layer) is a polyfunctional (meth) acrylate monomer. The adhesive sheet laminate according to any one of claims 1 to 7, wherein the olefin polymer (D) of the release layer (II layer) is an ethylene-α-olefin copolymer, and the MFR of JIS K-7210 It is 1~80g/10min. The adhesive sheet laminate according to any one of claims 1 to 8, wherein the release layer (layer II) is peeled off from the photocurable adhesive resin layer (I layer) at 180° peeling at a peeling speed of 300 mm/min. The force is 0.3 N/cm or less. The adhesive sheet laminate according to any one of claims 1 to 9, wherein the substrate layer (layer III) contains one or two selected from the group consisting of polyester, polyolefin, polycarbonate, and acrylic resin. More than one type of thermoplastic resin. The adhesive sheet laminate according to any one of claims 1 to 10, wherein the thickness of the photocurable adhesive resin layer (I layer) is 50 μm to 1000 μm, and the thickness of the release layer (layer II) is thick. The degree is 5 μm to 500 μm, and the thickness of the base material layer (III layer) is 25 μm to 500 μm. The adhesive sheet laminate according to any one of claims 1 to 11, which is provided on the both sides of the photocurable adhesive resin layer (I layer) with a release layer (II layer) and a base layer (III layer) And the peeling force of the photocurable adhesive resin layer (I layer) and the release layer (II layer) on one side is different from that of the other side of the photocurable adhesive resin layer (I layer) and the release layer (II) Peeling force of the layer). The method for producing an adhesive sheet laminate according to any one of claims 1 to 12, wherein the photocurable adhesive resin layer (I layer) and the release layer (layer II) are laminated by co-extrusion. ). A method for producing an adhesive sheet laminate comprising a release layer (II layer) on one side or both sides of a photocurable adhesive resin layer (I layer) containing a photocurable adhesive resin A method for producing an adhesive layer laminate of a base material layer (III layer), and a resin containing a (meth) acrylate copolymer (A), a crosslinking agent (B), and a photopolymerization initiator (C) The composition is co-extruded with the resin composition containing the olefin polymer (D), and after the release layer (layer II) is laminated on one side or both sides of the photocurable adhesive resin layer (I layer), no light is emitted. After hardening, a base material layer (III layer) is laminated on the release layer (layer II), thereby producing an adhesive sheet laminate. An image display device is a method of manufacturing a laminated body of a member, which is characterized in that the image display device is used to manufacture an image display device constituting a laminated body of an image-forming layer using the adhesive sheet laminate according to any one of claims 1 to 12. In the method for producing the laminated body of the member, the release layer (layer II) and the substrate layer (layer III) are simultaneously peeled off from the photocurable adhesive resin layer (I layer) of the adhesive sheet laminate, and then the spacer layer is separated. The photocurable adhesive resin layer (I layer) is formed by two image display device constituent members, and the photocurable adhesive resin layer (I layer) is irradiated with light to be hardened by one or two of the image display device constituent members. The image display device of claim 14 or 15 is a method of manufacturing a laminated body of a member, wherein the adhesive sheet layer according to any one of claims 1 to 12 is shaped to be attached to a member of the image display device. The shape of the surface of the concave and convex shape of the surface. The image display device of claim 16 is a method of manufacturing a laminated body, wherein the image is formed by a method of forming a surface shape of a concave-convex shape of a bonding surface of the image forming device constituent member. The mold having the uneven shape of the bonding surface of the display device constituent member is formed by pressing against the at least one side surface of the photocurable adhesive resin layer (I layer) via the base material layer (III layer).