TW201816047A - Adhesive composition, sealing sheet, and sealed body - Google Patents

Abstract

An adhesive composition containing a modified polyolefin resin (A) and a polyfunctional epoxy compound (B) and whereby a sheet-shaped object formed from said adhesive composition fulfills requirements (I) and (II). Requirement (I): The storage elastic modulus G' of the sheet-shaped object at 80 DEG C is no more than 0.3 MPa. Requirement (II): The amount of outgas generated per 1 cm3 of the sheet-shaped object when the sheet-shaped object is left for 20 minutes in an environment of 120 DEG C is no more than 20 mg/cm3.

Description

Adhesive composition, sealing sheet and sealing body

[0001] The present invention relates to an adhesive composition, a sealing sheet having an adhesive layer formed by the adhesive composition, and a sealing body in which the object to be sealed is sealed with the aforementioned sealing sheet.

[0002] In recent years, organic EL elements have attracted attention as light-emitting elements capable of emitting light with high luminance by being driven at a low voltage DC. However, organic EL elements have a problem that the light-emitting characteristics such as light-emitting luminance, light-emitting efficiency, and light-emitting uniformity tend to decrease over time. As a cause of the decrease in light emission characteristics, it is thought that oxygen or moisture etc. penetrates into the organic EL element and deteriorates the electrode or the organic layer. Therefore, a sealing material is used to seal the organic EL element to prevent the penetration of oxygen or moisture.时 When using a sealing material to seal an organic EL element, if exhaust gas is generated from the sealing material, the organic EL element will be deteriorated. Therefore, a sealing material with low outgassing has been developed. [0003] For example, Patent Document 1 describes a composition for sealing an organic EL element, which contains a specific cation-curable compound, a photocationic polymerization initiator, and an azole-based compound. Patent Document 1 discloses that a hardened product having low outgassing property and moisture resistance can be formed by using a sealing composition of an azole-based compound used as a hardening rolling agent. [Prior Art Literature] [Patent Literature] [0004] [Patent Literature 1] WO2015 / 111525

[Problems to be Solved by the Invention] [0005] Here, when the organic EL element is sealed with a sealing material, the organic EL element has a concave-convex shape, and a minute gap is easily generated with the sealing material. Oxygen or moisture may infiltrate from the minute gaps, which may cause degradation of the light emitting characteristics of the organic EL element. Therefore, the sealing material for an organic EL element is also required to be conformable. Patent Document 1 does not discuss the unevenness compliance of the disclosed sealing composition. [0006] Furthermore, the inventors have investigated that the amount of exhaust gas in the sealing material varies not only due to the hardening and rolling agent, but also due to the type or content of each component included in the composition. Therefore, there is a need for a sealing material that has low outgassing properties and a high effect of suppressing deterioration of the sealed object. [0007] In general, when a resin barrier-containing resin layer is directly laminated on a gas barrier layer included in a gas barrier film, the gas barrier layer and the resin have a low affinity, so the gas barrier may be Adhesion between the layers and the resin layer causes problems. In particular, when a gas barrier layer containing a polymer compound and subjected to modification treatment is used, the adhesion between the gas barrier layer and the resin layer is often deteriorated. Therefore, the adhesive composition is also required to have characteristics as a material for forming a layer having excellent interlayer adhesion with the gas barrier layer. [0008] The present invention has been made in view of the foregoing circumstances, and an object thereof is to provide an adhesive composition which has excellent low outgassing property and irregularity compliance, and can obtain a sealing material having a high suppression effect for deterioration of a sealed object, It is also suitable as a material for forming an adhesive layer having excellent interlayer adhesion with the gas barrier layer, a sealing sheet having the adhesive layer formed of the adhesive composition, and a sealing body in which the object to be sealed is sealed with the sealing sheet. . [Means for Solving the Problem] [0009] The present inventors have found that an adhesive composition containing a modified polyolefin-based resin and a polyfunctional epoxy compound can solve the above problems, and completed the present invention. [0010] That is, the present invention relates to the following [1] to [16]. [1] An adhesive composition, which is an adhesive composition containing a modified polyolefin-based resin (A) and a polyfunctional epoxy compound (B), and the flakes formed by the adhesive composition satisfy the following Requirements (I) and (II), ･ Requirement (I): The storage elastic modulus G 'of the sheet at 80 ° C is 0.3 MPa or less, ･ Requirement (II): The aforementioned sheet is placed in an environment of 120 ° C The amount of exhaust gas generated per 1 cm ³ of the flakes when left standing for 20 minutes was 20 mg / cm ³ or less. [2] The adhesive composition according to the above [1], wherein the component (A) is an acid-modified polyolefin resin. [3] The adhesive agent composition according to the above [1] or [2], wherein the content of the component (A) is 15 to 70% by mass based on the total amount of the active ingredients of the adhesive agent composition. [4] The adhesive composition according to any one of the above [1] to [3], wherein the component (B) is one selected from the group consisting of a polyfunctional alicyclic epoxy compound and a polyfunctional aliphatic epoxy compound. More than that. [5] The content of the component (B) is 25 to 200 parts by mass based on 100 parts by mass of the component (A), and the adhesive composition according to any one of the above [1] to [4]. [6] The adhesive composition according to any one of the above [1] to [5], further comprising an adhesion-imparting agent (C). [7] The adhesive composition according to the above [6], wherein the content of the component (C) is 1 to 200 parts by mass based on 100 parts by mass of the component (A). [8] The adhesive composition according to any one of the above [1] to [7], further comprising an imidazole-based hardening catalyst (D). [9] The adhesive composition according to the above [8], wherein the content of the component (D) is 0.1 to 10 parts by mass based on 100 parts by mass of the component (A). [10] The adhesive composition according to any one of the above [1] to [9], further comprising a silane coupling agent (E). [11] The adhesive composition according to the above [10], wherein the content of the component (E) is 0.01 to 10 parts by mass based on 100 parts by mass of the component (A). [12] A sealing sheet having an adhesive layer formed from the adhesive composition according to any one of the above [1] to [11]. [13] The sealing sheet according to the above [12], further comprising a gas barrier film including a base material layer and a gas barrier layer. [14] The sealing sheet according to the above [13], which is formed by directly stacking the gas barrier layer of the gas barrier film and the adhesive layer. [15] The sealing sheet according to the above [13] or [14], wherein the gas barrier layer is a polymer layer containing a polymer compound and subjected to a modification treatment. [16] A sealing body formed by sealing an organic EL element, an organic EL display element, a liquid crystal display element, or a solar cell element with a sealing sheet according to any one of [12] to [15] above. [Effects of Invention] [0011] Since the composition for bonding of the present invention has excellent low outgassing properties and compliance with unevenness, it is possible to obtain a sealing material with a high effect of suppressing deterioration of the sealed object. In addition, the adhesion between the adhesive layer and the gas barrier layer formed by the adhesive composition is also excellent.

[0012] In the present specification, regarding a preferred numerical range (such as a range of content, etc.), the lower limit value and the upper limit value may be described in stages, which can be combined independently. For example, the description of "preferably 10 ~ 90, and more preferably 30 ~ 60" can be a combination of "better lower limit value (10)" and "more preferred upper limit value (60)", or it can be set to " 10 ~ 60 ". [Adhesive Composition] The adhesive composition of the present invention contains a modified polyolefin-based resin (A) and a polyfunctional epoxy compound (B), and the flakes formed by the adhesive composition satisfy the following conditions: The requirements (I) and (II) are described. ･ Requirement (I): The storage elastic modulus G 'of the sheet at 80 ° C is 0.3 MPa or less. ･ Requirement (II): Each 1 cm of the sheet when the sheet is left to stand at 120 ° C for 20 minutes ³ The exhaust volume generated in the process is 20mg / cm ³ the following. [0014] As required by the requirement (1), since the storage elastic modulus G ′ of the sheet at 80 ° C. is 0.3 MPa or less, the adhesive composition of the present invention can obtain a sealing material having excellent unevenness compliance. In addition, as specified in the requirement (II), every 1 cm of the thin sheet ³ The amount of exhaust gas that can be generated is 20mg / cm ³ Hereinafter, the adhesive composition of the present invention may also be referred to as a sealing material having low outgassing properties. That is, the adhesive composition of the present invention is prepared so as to satisfy the above requirements (I) and (II), and therefore has excellent low outgassing property and irregularity compliance, and can have a high suppression effect for deterioration of the sealed object. Of sealing material. [0015] In the adhesive composition of the present invention, the storage elasticity G ′ at 80 ° C. of the aforementioned sheet-like material specified in the requirement (I) is relatively high from the viewpoint of a sealing material having excellent unevenness compliance. It is preferably 0.2 MPa or less, still more preferably 0.1 MPa or less, more preferably 0.09 MPa or less, and from the viewpoint of operability, usually 0.001 MPa or more, preferably 0.005 MPa or more, and still more preferably 0.01. Above MPa. In addition, in this specification, the storage elasticity G 'of the said sheet-like object prescribed | regulated by the requirement (I) means the value measured by the method as described in an Example. [0016] In the adhesive composition of the present invention, each of the sheet-like objects when the sheet-like objects are allowed to stand for 20 minutes under an environment of 120 ° C. as specified in the requirement (II). ³ The amount of exhaust gas generated in the medium is preferably 18 mg / cm from the viewpoint of a sealing material having excellent low exhaust gas properties and a high suppressing effect on the deterioration of the sealed object. ³ Hereinafter, it is more preferably 15 mg / cm ³ Below, more preferably 10 mg / cm ³ Hereinafter, it is more preferably 8 mg / cm ³ Below, and usually 0.1mg / cm ³ the above. In addition, in this specification, the exhaust gas amount of the said thin object prescribed | regulated by the requirement (II) means the value measured by the method as described in an Example. [0017] In the adhesive composition of the present invention, it is preferable that the flakes formed by the adhesive composition simultaneously satisfy the following requirements (III) and the requirements (I) and (II). ･ Requirement (III): The haze of the sheet is 2.0% or less. [0018] A sealing material for sealing an optical element such as an organic EL element is required to have high transparency. As required by requirement (III), if the haze of the flakes is 2.0% or less, the adhesive composition can be suitably used as a sealing material for sealing an optical element such as an organic EL element. [0019] From the above point of view, the haze of the aforementioned sheet-like article specified in the requirement (III) in the adhesive composition of the present invention is preferably 2.0% or less, and still more preferably 1.5% or less. It is preferably 1.0% or less. In addition, in the present specification, the haze of the flakes specified in the requirement (III) means a value measured by the method described in the examples. [0020] The adhesive composition of the present invention is contained by combining a modified polyolefin resin (A) and a polyfunctional epoxy compound (B), and is prepared so as to satisfy the requirements (I) and (II) described above. A more specific method of the adhesive composition for satisfying the above requirements (I) to (III) is as described in the description of each component described in detail below. [0021] The adhesive composition of the present invention satisfies the above-mentioned requirements (I) and (II), and may contain components other than the components (A) and (B) as long as the effects of the present invention are not impaired. As such a component, the adhesive composition of the present invention further contains one or more selected from the group consisting of an adhesion-imparting agent (C), an imidazole-based hardening catalyst (D), and a silane coupling agent (E), and further contains a component (C ), (D) and (E) are even better. [0022] The total content of the components (A) and (B) in the adhesive composition of the present invention is preferably 30% by mass or more relative to the total amount (100% by mass) of the active ingredients of the adhesive composition. , More preferably 50% by mass or more, more preferably 60% by mass or more, even more preferably 65% by mass or more, particularly preferably 70% by mass or more, and usually 100% by mass or less, preferably 99.9% by mass %the following. [0023] In the adhesive composition of the present invention, the total content of the components (A), (B), (C), (D), and (E) is relative to the total amount of the active ingredients of the adhesive composition ( 100% by mass), preferably 60 to 100% by mass, even more preferably 70 to 100% by mass, more preferably 80 to 100% by mass, and even more preferably 90 to 100% by mass. In addition, in this specification, the active ingredient of an adhesive composition means the component which remove | eliminates the dilution solvent contained in an adhesive composition which is not related to a physical property. [Component (A): Modified Polyolefin Resin> The adhesive composition of the present invention contains a modified polyolefin resin (A). By containing the modified polyolefin resin (A), the adhesive composition of the present invention can be used as a composition having excellent adhesion strength, and can also form a thin film (adhesive layer) having a thin film thickness. good. The modified polyolefin resin (A) may be used alone or in combination of two or more kinds. [0025] In the present invention, the modified polyolefin-based resin means a polyolefin resin having a functional group obtained by subjecting the polyolefin resin as a precursor to a modification treatment using a modifier having a functional group. And, the polyolefin resin means a polymer having a repeating unit derived from an olefin-based monomer. In addition, in the present invention, the polyolefin resin may be a polymer composed of only repeating units derived from an olefin-based monomer, or may have a repeating unit derived from an olefin-based monomer and also have a source derived from other than an olefin-based monomer. Copolymer of repeating units of monomers. [0026] As the olefin-based monomer, an α-olefin having 2 to 8 carbon atoms is preferred, ethylene, propylene, 1-butene, isobutylene, or 1-hexane is even more preferred, and ethylene or propylene is more preferred. . Examples of the monomer other than the olefin-based monomer include vinyl acetate, (meth) acrylate, and styrene. [0027] Examples of the polyolefin resin include ultra-low density polyethylene (VLDPE), low density polyethylene (LDPE), medium density polyethylene (MDPE), high density polyethylene (HDPE), and linear low density polymer. Ethylene, polypropylene (PP), ethylene-propylene copolymers, olefin-based elastomers (TPO), ethylene-vinyl acetate copolymers (EVA), ethylene- (meth) acrylic copolymers, ethylene- (formaldehyde) Group) acrylate copolymers and the like. [0028] As long as the modifier used for the modification treatment of the polyolefin resin is a compound having a functional group in a molecule, that is, a compound having a group capable of contributing to a crosslinking reaction described later. Examples of the functional group include a carboxyl group, a carboxylic acid anhydride-derived group, a carboxylic acid ester group, a hydroxyl group, an epoxy group, a fluorenylamino group, an ammonium group, a nitrile group, an amine group, a fluorenimine group, an isocyanate group, and an acetamidine group , Thiol group, ether group, thiol ether group, fluorenyl group, phosphorus group, nitro group, urethane group, halogen atom, and the like. Among these, a carboxyl group, a carboxylic acid anhydride-derived group, a carboxylic acid ester group, a hydroxyl group, an ammonium group, an amine group, an iminoamino group, or an isocyanate group are preferable, and a carboxylic acid anhydride-based group or an alkoxysilyl group is further preferable. Preferably, a group derived from a carboxylic anhydride is more preferable. The modifier used may be a compound having two or more functional groups in the molecule. [0029] As the modified polyolefin-based resin (A), from the viewpoint of an adhesive composition satisfying the above requirements (I) and (II), it is an acid-modified polyolefin-based resin or a silane-modified polyolefin-based resin. The resin is preferred, and an acid-modified polyolefin resin is even more preferred. [0030] In the present invention, an acid-modified polyolefin-based resin means a polyolefin resin grafted and modified with an acid having a functional group of a modifier. For example, after reacting a polyolefin resin with an unsaturated carboxylic acid and / or an unsaturated carboxylic acid anhydride, a carboxyl group and / or a group derived from a carboxylic acid anhydride (graft modification) is introduced. [0031] Examples of unsaturated carboxylic acids and anhydrides of unsaturated carboxylic acids that react with polyolefin resins include maleic acid, butenedioic acid, itaconic acid, pyrocitric acid, pentenedioic acid, and tetrahydrophthalic acid. Acid, aconitic acid, maleic anhydride, itaconic anhydride, glutaric anhydride, pyrocitric anhydride, aconitic anhydride, norbornene dicarboxylic anhydride, tetrahydrophthalic anhydride, and the like. These may be used alone or in combination of two or more. Among these, from the viewpoint of further improving the adhesive strength and satisfying the adhesive composition of the above-mentioned requirements (I) and (II), maleic anhydride is preferred. [0032] The amount of the unsaturated carboxylic acid and / or the unsaturated carboxylic acid anhydride compounded with the polyolefin resin is used to further improve the bonding strength, and at the same time meet the requirements of the adhesive composition of the above requirements (I) and (II) From a viewpoint, it is preferably 0.1 to 5 parts by mass, more preferably 0.2 to 3 parts by mass, and still more preferably 0.2 to 1.0 part by mass with respect to 100 parts by mass of the polyolefin resin before the modification. [0033] In the present invention, a commercially available product can be used as the acid-modified polyolefin resin. Commercially available acid-modified polyolefin resins include, for example, Admar (registered trademark) (Mitsui Chemical Co., Ltd.), Unistall (registered trademark) (Mitsui Chemical Co., Ltd.), BondyRam (Polyram), ororevac (Registered trademark) (made by ARKEMA), Modic (registered trademark) (made by Mitsubishi Chemical Corporation), and the like. [0034] In the present invention, the silane-modified polyolefin resin refers to a polyolefin resin grafted and modified with an unsaturated silane compound containing a modifier. That is, the silane-modified polyolefin resin has a structure in which an unsaturated silane compound having a side chain on the polyolefin resin of the main chain is graft-copolymerized. [0035] As the unsaturated silane compound that reacts with the polyolefin resin, a vinyl silane compound is preferred, and examples thereof include vinyltrimethoxysilane, vinyltriethoxysilane, vinyltripropoxysilane, and ethylene. Triisopropoxysilane, vinyltributoxysilane, vinyltripentyloxysilane, vinyltriphenoxysilane, vinyltribenzyloxysilane, vinyltrimethylenedioxysilane , Vinyltrivinyldioxysilane, vinylpropanyloxysilane, vinyltriethoxysilane, vinyltricarboxysilane, etc. These unsaturated silane compounds may be used alone or in combination of two or more. In addition, the conditions for graft polymerization of an unsaturated silane compound and a polyolefin resin in the main chain may be a general method known for graft polymerization. [0036] The compounding amount of the unsaturated silane compound to be reacted with the polyolefin resin is used to further improve the adhesive strength, and the viewpoint of the adhesive composition that satisfies the requirements (I) and (II) described above is relative to that before the modification. The polyolefin resin is 100 parts by mass, preferably 0.1 to 10 parts by mass, still more preferably 0.3 to 7 parts by mass, and more preferably 0.5 to 5 parts by mass. [0037] Specific silane-modified polyolefin resins include, for example, silane-modified polyethylene resins and silane-modified ethylene-vinyl acetate copolymers, which are silane-modified low-density polyethylene and silane-modified Silane-modified polyethylene resins such as low-density polyethylene and silane-modified linear low-density polyethylene are preferred. [0038] In the present invention, commercially available products can be used as the silane-modified polyolefin resin. Commercially available silane-modified polyolefin resins include, for example, Linklon (registered trademark) (manufactured by Mitsubishi Chemical Corporation), but they are low-density polyethylene-based Linklons and linear low-density polyethylene-based resins. Linklon, ultra-low density polyethylene based linklon and vinyl-vinyl acetate copolymer based linklon are preferred. [0039] As a weight average molecular weight (Mw) of the modified polyolefin resin (A), from the viewpoint of improving the adhesive strength and satisfying the adhesive composition of the above requirements (I) and (II), From the viewpoint of improving the shape maintenance property when the adhesive composition is formed into a sheet shape, it is preferably 10,000 to 2,000,000, more preferably 20,000 to 1,500,000, more preferably 25,000 to 250,000, and even more preferably It is 30,000 ~ 150,000. When the weight average molecular weight of the modified polyolefin-based resin (A) is within the above range, even when the content of the modified polyolefin-based resin (A) in the adhesive composition is large, it is formed from the adhesive composition as In the shape of a sheet, the shape maintainability is also good. [0040] In this specification, the weight average molecular weight (Mw) is a standard polystyrene conversion value measured by a gel permeation chromatography (GPC) method using tetrahydrofuran as a solvent, and specifically, it is based on Values measured by the methods described in the examples. The following are the same. [0041] The modified polyolefin-based resin (A) is preferably solid at room temperature (25 ° C) from the viewpoint of improving the shape maintenance property when the adhesive composition is formed into a sheet. [0042] The content of the component (A) in the adhesive composition of the present invention is preferably 15 to 70% by mass, more preferably 23 to the total amount (100% by mass) of the active ingredients of the adhesive composition. ~ 60 mass%, more preferably 30 to 50 mass%. [Component (B): Polyfunctional Epoxy Compound> The adhesive composition of the present invention contains a polyfunctional epoxy compound (B). By including the polyfunctional epoxy compound (B) in the adhesive composition of the present invention, a sealing material having excellent water vapor barrier properties can be obtained. The polyfunctional epoxy compound (B) may be used alone or in combination of two or more kinds. [0044] In the present invention, a polyfunctional epoxy compound means a compound having at least two epoxy groups in the molecule. As the component (B), a bifunctional epoxy compound having two epoxy groups is preferred from the viewpoint of an adhesive composition that satisfies the requirements (I) and (II) described above. [0045] Examples of the bifunctional epoxy compound include bisphenol A diglycidyl ether, bisphenol F diglycidyl ether, bisphenol S diglycidyl ether, brominated bisphenol A diglycidyl ether, and brominated bis Phenol F diglycidyl ether, brominated bisphenol S diglycidyl ether, phenolic resin epoxy resins (e.g., phenolic novolac resin epoxy resin, cresol novolac resin epoxy resin, brominated phenolic novolac resin Resin type epoxy resin) and other aromatic epoxy compounds; hydrogenated bisphenol A diglycidyl ether, hydrogenated bisphenol F diglycidyl ether, alicyclic epoxy compounds such as hydrogenated bisphenol S diglycidyl ether; pentaerythritol Polyglycidyl ether, 1,6-hexanediol diglycidyl ether, diglycidyl hexahydrophthalate, neopentyl glycol diglycidyl ether, trimethylolpropane polyglycidyl ether, 2, 2 -Aliphatic epoxy compounds such as bis (3-glycidyl-4-glycidyloxyphenyl) propane, dimethylol tricyclodecane diglycidyl ether, and the like. [0046] Among them, the polyfunctional epoxy compound (B) is selected from a polyfunctional alicyclic epoxy compound and a polyfunctional aliphatic epoxy compound from the viewpoint of an adhesive composition satisfying the requirement (III). More than one is preferred. [0047] In addition, a sealing material formed of an adhesive composition containing an aromatic epoxy compound tends to have a higher haze. Therefore, from the viewpoint of an adhesive composition that satisfies the requirement (III), the content of the aromatic epoxy compound is extremely small. From the above viewpoint, the content of the aromatic epoxy compound relative to the total amount (100% by mass) of the component (B) is preferably 0 to 50% by mass, still more preferably 0 to 20% by mass, and more preferably 0 to 10% by mass, and even more preferably 0 to 2% by mass. [0048] In the adhesive composition of the present invention, it is preferred that the component (B) contains a polyfunctional epoxy compound (B1) which is liquid at 25 ° C. (B1) When the adhesive composition is at a high temperature, the component has an effect of reducing the storage elastic modulus of the adhesive composition (hereinafter sometimes referred to as "storage elasticity reduction effect"). Therefore, by including the component (B1) in the adhesive composition of the present invention, an adhesive layer having excellent unevenness compliance can be efficiently formed. [0049] The weight average molecular weight (Mw) of the polyfunctional epoxy compound (B1) that is liquid at 25 ° C is preferably 1,000 or more from the viewpoint of an adhesive composition satisfying the requirement (II), and It is preferably 1,200 or more, more preferably 1,500 or more, even more preferably 1,800 or more, and particularly preferably 2,100 or more. From the viewpoint of satisfying the adhesive composition of the requirement (I), the weight average molecular weight (Mw) of the polyfunctional epoxy compound (B1) which is liquid at 25 ° C is preferably 4,000 or less, and still more preferably 3,700 or less, more preferably 3,400 or less. [0050] The epoxy equivalent of the polyfunctional epoxy compound (B1) which is liquid at 25 ° C is preferably 100 to 500 g / eq, still more preferably 120 to 400 g / eq, and more preferably 150 to 300 g / eq. . [0051] The adhesive composition of the present invention preferably contains, as component (B), a polyfunctional epoxy compound (B2) which is solid at 25 ° C. The polyfunctional epoxy compound of the component (B2) is different from the polyfunctional epoxy compound of the component (B1), and has almost no storage elasticity reduction effect. On the other hand, by including the component (B2) in the adhesive composition, the performance of the adhesive layer in maintaining the sheet shape is improved. As a result, when (B2) component is used in combination with (B1) component, the storage elasticity reduction effect which (B1) component has can be improved more. The presence of the (B2) component can maintain the sheet shape performance of the adhesive layer and increase the content of the (B) component in the adhesive composition at the same time. Therefore, in the adhesive composition, in the phase-separated structure formed by the component (A) and the component (B), the ratio of the region of the continuous phase of the component (B) increases. When the adhesive layer formed by such an adhesive composition is heated, the continuous phase region of the component (B) is softened, so that it can exhibit a high storage elasticity reduction effect. Therefore, it is more preferable that the adhesive composition of the present invention contains both the (B1) component and the (B2) component. [0052] The weight average molecular weight (Mw) of the functional epoxy compound (B2) which is solid at 25 ° C is preferably 3,800 or more, and still more preferably 4,000 or more. By using an adhesive composition having a weight average molecular weight (Mw) of 3,800 or more of the polyfunctional epoxy compound (B2), it is easier to maintain the sheet shape of the adhesive layer. The weight-average molecular weight (Mw) of the polyfunctional epoxy compound (B2) which is solid at 25 ° C is preferably 8,000 or less, and more preferably 7,000 or less. [0053] The epoxy equivalent of the polyfunctional epoxy compound (B2) which is solid at 25 ° C is preferably 600 to 6,000 g / eq, and more preferably 700 to 5,500 g / eq. By using an adhesive composition having an epoxy equivalent of 600 to 6,000 g / eq of the polyfunctional epoxy compound (B2), it is easier to maintain the sheet shape of the adhesive layer. [0054] The content of the component (B) in the adhesive composition of the present invention is more than 100 parts by mass of the component (A) from the viewpoint of the adhesive composition satisfying the requirements (I) and (II). It is preferably 25 to 200 parts by mass, still more preferably 30 to 180 parts by mass, more preferably 50 to 150 parts by mass, and even more preferably 65 to 120 parts by mass. [0055] When the adhesive composition of the present invention contains both (B1) component and (B2) component, the content ratio (mass ratio) of (B1) component and (B2) component is [(B1) component: (B2) Ingredient] = 100: 1 ~ 1: 1 is more preferable, and 10: 1 ~ 2: 1 is more preferable. As the amount of the component (B2) relative to the component (B1) increases, when the adhesive composition is formed into a sheet shape, it tends to be easily maintained in a certain shape. [0056] <Component (C): Adhesion imparting agent> The adhesive composition of the present invention preferably further contains an adhesion imparting agent (C) from the viewpoint of further improving the shape maintaining property of the formed sealing material. [0057] Examples of the adhesion-imparting agent (C) include rosin-based resins such as polymerized rosin, polymerized rosin esters, and rosin derivatives; polyterpene resins, aromatic modified terpene resins, and their hydrides, terpene-based resins, and the like. Terpene-based resins; benzofuran / indene resins; aliphatic petroleum-based resins, aromatic petroleum resins and their hydrides, aliphatic / aromatic copolymer petroleum resins, and other petroleum resins; styrene or substituted styrene polymerization Products; α-methylstyrene single polymer resin, copolymer of α-methylstyrene and styrene, copolymer of styrene monomer and aliphatic monomer, styrene monomer and α -Copolymers of methylstyrene and aliphatic monomers, individual polymers made of styrene monomers, copolymers of styrene monomers and aromatic monomers, and other styrene resins ;Wait. These adhesion-imparting agents (C) may be used alone or in combination of two or more. Among these, as the component (C), a styrene-based resin is preferable, and a copolymer of a styrene-based monomer and an aliphatic monomer is more preferable. [0058] The softening point of the adhesion-imparting agent (C) is further improved from the viewpoint of an adhesive composition capable of further improving the shape maintainability of the formed sealing material and capable of exhibiting excellent adhesiveness even in a high-temperature environment. It is preferably 80 ° C or higher, more preferably 85 to 170 ° C, and still more preferably 90 to 150 ° C. In this specification, the softening point means a value measured in accordance with JIS K 5902. When two or more types of adhesion-imparting agents are used, it is preferable that the increase in the softening point of these plural adhesion-imparting agents belongs to the above range on average. [0059] In the adhesive composition of the present invention, the content of the component (C) is from the viewpoint of an adhesive composition that further maintains the shape retention of the formed sealing material, with respect to 100 mass of the component (A). 1 to 200 parts by mass, more preferably 10 to 150 parts by mass, still more preferably 15 to 100 parts by mass, and still more preferably 20 to 80 parts by mass. [Component (D): Imidazole-based hardening catalyst> The adhesive composition of the present invention further contains an imidazole-based hardening catalyst from the viewpoint of an adhesive composition that can exhibit excellent adhesion even in a high-temperature environment. Medium (D) is preferred. [0061] Examples of the imidazole-based curing catalyst (D) include 2-methylimidazole, 2-phenylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, and 2-ethyl-4-methyl Imidazole, 2-phenyl-4-methylimidazole, 2-phenyl-4-methyl-5-hydroxymethylimidazole, 2-phenyl-4,5-dihydroxymethylimidazole, and the like. These imidazole-based hardening catalysts (D) may be used alone or in combination of two or more. Among these, as the component (D), 2-ethyl-4-methylimidazole is preferable. [0062] The content of the component (D) in the adhesive composition of the present invention is 100 mass% of the component (A) component from the viewpoint of an adhesive composition that can exhibit excellent adhesiveness even in a high-temperature environment. It is preferably 0.1 to 10 parts by mass, more preferably 0.2 to 5 parts by mass, and still more preferably 0.3 to 2.5 parts by mass. [Component (E): Silane Coupling Agent> The adhesive composition of the present invention is an adhesive composition capable of forming a sealant having excellent adhesive strength even at normal temperature and high temperature environments. It is preferable to further contain a silane coupling agent (E). [0064] As the silane coupling agent (E), an organic silicon compound having at least one alkoxysilyl group in the molecule is preferred from the above viewpoint. Specific examples of the silane coupling agent (E) include polymerizable unsaturated group-containing silicon such as vinyltrimethoxysilane, vinyltriethoxysilane, and methacryloxypropyltrimethoxysilane. Compound; 3-glycidyloxypropyltrimethoxysilane, glycidyloxyoctyltrimethoxysilane, 2- (3,4-epoxycyclohexyl) ethyltrimethoxysilane, etc. have epoxy structure Silicon compounds; 3-aminopropyltrimethoxysilane, N- (2-aminoethyl) -3-aminopropyltrimethoxysilane, N- (2-aminoethyl) -3- Amine-containing silicon compounds such as aminopropylmethyldimethoxysilane; 3-chloropropyltrimethoxysilane; 3-isocyanatepropyltriethoxysilane; etc. These silane coupling agents (E) may be used alone or in combination of two or more kinds. [0065] In the adhesive composition of the present invention, the content of the component (E) is relatively high in terms of an adhesive composition capable of forming a sealant having excellent adhesive strength even at normal temperature and high temperature environments. 100 parts by mass of the component (A) is preferably 0.01 to 10 parts by mass, still more preferably 0.02 to 5 parts by mass, and still more preferably 0.05 to 2 parts by mass. [0066] <Other additives> The adhesive composition of the present invention may contain other additives other than the aforementioned components (A) to (E), as long as the effect of the present invention is not impaired. Other additives can be appropriately selected depending on the application, but examples include additives such as ultraviolet absorbers, antistatic agents, light stabilizers, antioxidants, resin stabilizers, fillers, pigments, extenders, and softeners. These additives may be used alone or in combination of two or more. [0067] From the viewpoint of an adhesive composition that satisfies the requirement (III), the content of the filler and the pigment is extremely small. From the above viewpoints, the total content of the filler and pigment is preferably 0 to 10% by mass, and more preferably 0 to 5% by mass relative to the total amount (100% by mass) of the active ingredients of the aforementioned adhesive composition. %, More preferably 0 to 1% by mass, and even more preferably 0 to 0.001% by mass. [0068] In addition, the adhesive composition of the present invention may further contain a diluent solvent from the viewpoint of improving moldability. The diluent solvent can be appropriately selected from organic solvents. Specific examples include aromatic hydrocarbon solvents such as benzene and toluene; ester solvents such as ethyl acetate and butyl acetate; and acetone and methyl ethyl. Ketone solvents such as methyl ketone, methyl isobutyl ketone, etc .; aliphatic hydrocarbon solvents such as n-pentane, n-hexane, n-heptane; cyclopentane, cyclohexane, methylcyclohexane Etc. alicyclic hydrocarbon solvents; etc. These solvents may be used alone or in combination of two or more. The content of the solvent can be appropriately set in consideration of coating properties and the like. [Sealing Sheet] The sealing sheet of the present invention has an adhesive layer formed of the above-mentioned adhesive composition. The thickness of the adhesive layer is appropriately set depending on the application, but is preferably 2 to 50 μm, more preferably 5 to 25 μm, and still more preferably 10 to 20 μm. [0070] Moreover, the haze of the adhesive layer of the sealing sheet of the present invention is preferably 2.0% or less, still more preferably 1.5% or less, and even more preferably 1.0% or less. [0071] In addition, the adhesive layer included in the sealing sheet of the present invention is the same as the aforementioned sheet-like object specified in the above requirements (I) to (II). Therefore, the appropriate ranges of the storage elastic modulus G 'and the exhaust gas volume of the adhesive layer of the sealing sheet of the present invention at 80 ° C. are the same as the prescribed ranges of the requirements (I) and (II), respectively. [0072] The adhesive layer of the sealing sheet of the present invention has better thermosetting properties. In this way, after the adhesive layer is cured, the adhesive strength is extremely excellent. The conditions for thermally curing the adhesive layer are not particularly limited, but the heating temperature is usually 80 to 200 ° C (preferably 90 to 150 ° C), and the heating time is usually 30 minutes to 12 hours (preferably 1 to 6 hours). ). [0073] Specific examples of the sealing sheet of the present invention include the following sealing sheet (α) and sealing sheet (β). ･ Sealing sheet (α): A sealing sheet having a structure in which an adhesive layer formed by the adhesive composition of the present invention is sandwiched between two release films. ･ Sealing sheet (β): a sealing sheet having a gas barrier film and an adhesive layer formed by the adhesive composition of the present invention, the gas barrier film having a substrate layer and a gas barrier layer. Further, in the sealing sheet (β), a release film may be further laminated on the adhesive layer. In addition, these sealing sheets show the state before use, and when using the sealing sheet of the present invention, the release film is usually peeled off and removed. [0074] The release film constituting the sealing sheet (α) has a function as a support in the manufacturing step of the sealing sheet (α), and simultaneously has a protective sheet as an adhesive layer between the use of the sealing sheet (α). Function. [0075] As the release film, a conventionally known one can be used. For example, the release film substrate has a release layer that has been subjected to a release treatment with a release agent. Examples of the substrate for the release film include paper substrates such as cellophane, coated paper, and high-quality paper; laminating papers on which a thermoplastic resin such as polyethylene is bonded to the paper substrate; and polyethylene-based Plastic films formed from terephthalate resin, polybutylene terephthalate resin, polyvinyl naphthalate resin, polypropylene resin, polyethylene resin, etc .; etc. Examples of the release agent include rubber-based elastomers such as silicone resins, olefin-based resins, isoprene-based resins, and butadiene-based resins; . [0076] The two peeling films of the sealing sheet (α) may be the same or different from each other, but those having peeling forces different from each other are preferred. [0077] The manufacturing method of the sealing sheet (α) is not particularly limited, and for example, the adhesive composition of the present invention is coated on the release-treated surface of a release film to form a coating film, and the coating film is dried to form an adhesive layer. method. A sealing sheet (α) can be obtained by further laminating one release film on the formed adhesive layer. [0078] Examples of the coating method of the adhesive composition include a spin coating method, a spray coating method, a bar coating method, a knife coating method, a roll coating method, a blade coating method, a die coating method, and a gravure coating method. In addition, from the viewpoint of improving the coating property, the adhesive composition is preferably in the form of a solution in addition to the above-mentioned dilution solvent. As a drying condition when the coating film is dried, for example, a drying treatment usually performed at 80 to 150 ° C. for 30 seconds to 5 minutes is preferred. [0079] The gas barrier film included in the sealing sheet (β) is one having a base material layer and a gas barrier layer. The gas barrier film can also be formed by directly stacking the substrate layer and the gas barrier layer, or a primer layer can be provided between the substrate layer and the gas barrier layer to improve the adhesion with the two layers. Of the composition. [0080] In the sealing sheet (β), a gas barrier layer and an adhesive layer that are directly laminated with a gas barrier film are preferred. In particular, when a gas barrier layer contains a polymer compound as described later, and a polymer layer subjected to a modification treatment, the interlayer adhesion between a general adhesive layer and the gas barrier layer may deteriorate. However, the adhesive layer formed by the adhesive composition of the present invention is closely adhered to the gas barrier layer of such a polymer layer by containing a modified polyolefin resin (A) and a polyfunctional epoxy resin (B). Better performance. [0081] The sealing sheet (β) preferably has a water vapor transmission rate of 0.1 g / m under an environment of a temperature of 40 ° C and 90% RH (relative humidity). ² / day or less, more preferably 0.05g / m ² / day or less, more preferably 0.005g / m ² / day or less. If the water vapor transmission rate of the sealing sheet (β) is 0.1g / m ² / day or less, it is possible to suppress oxygen or moisture from penetrating into the inside of an element such as an organic EL element formed on a transparent substrate, and effectively suppress deterioration of an electrode or an organic layer. In this specification, the water vapor transmission rate can be measured using a general gas transmission rate measurement device. Examples of the gas transmission rate measuring device include a product name "PERMATRAN" manufactured by Mocon Corporation. The water vapor transmission rate of the sealing sheet (β) is a value measured when the sealing sheet (β) is supplied for use, that is, when the sealing sheet (β) includes a release film, the release film is removed. Measured value. [0082] Here, the peeling film and the adhesive layer included in the sealing sheet (β) include the same as the peeling film and the adhesive layer included in the sealing sheet (α). [0083] As the base material layer included in the gas barrier film, a resin film containing a resin component is preferred. Examples of the resin component include polyimide, polyimide, polyamidoimide, polyphenylene ether, polyetherketone, polyetheretherketone, polyolefin, polyester, polycarbonate, Polyfluorene, polyetherfluorene, polyphenylene sulfide, polyaromatic esters, acrylic resins, cycloolefin polymers, aromatic polymers, polyurethane polymers, and the like. These resin components may be used alone or in combination of two or more. The thickness of the substrate layer of the gas barrier film is not particularly limited. From the viewpoint of ease of operation, it is preferably 0.5 to 500 μm, more preferably 1 to 200 μm, and still more preferably 5 to 100 μm. [0084] The gas barrier layer included in the gas barrier film includes an inorganic film or a polymer compound from the viewpoint of being capable of reducing the thickness of the gas barrier film and having excellent gas barrier properties. The modified polymer layer is preferred, and the polymer layer is even more preferred. Since a polymer layer containing a polymer compound and subjected to a modification treatment is excellent in flexibility, the gas barrier layer can be used as the polymer layer, which can be used as a gas barrier laminate having excellent resistance to bending. [0085] Examples of the polymer compound contained in the polymer layer include silicon-containing polymer compounds such as polyorganosiloxane and polysilazane-based compounds, polyimide, polyimide, and polyimide Polyimide, polyphenylene ether, polyether ketone, polyether ether ketone, polyolefin, polyester, polycarbonate, polyfluorene, polyetherfluorene, polyphenylene sulfide, polyaromatic ester, acrylic resin, Cycloolefin-based polymers, aromatic polymers, and the like. These polymer compounds may be used alone or in combination of two or more kinds. Among these, from the viewpoint of being able to form a gas barrier layer having excellent gas barrier properties, the polymer compound contained in the polymer layer is preferably a silicon-containing polymer compound, and is a polysilazane system. Compounds are even more preferred. The number average molecular weight of the polysilazane-based compound is preferably 100 to 50,000. [0086] The polysilazane-based compound is a polymer having a repeating unit including -Si-N-bond (silazane bond) in the molecule, and specifically, is a compound having the following general formula (1) Polymers expressed in repeating units are preferred. [0087] [0088] In the general formula (1), n represents the number of repeating units, and represents an integer of 1 or more. Rx, Ry, and Rz each independently represent a hydrogen atom, an unsubstituted if or substituted alkyl group, an unsubstituted or substituted cycloalkyl group, an unsubstituted or substituted alkenyl group, an unsubstituted or substituted group Aryl or alkylsilyl. Among these, Rx, Ry, and Rz are preferably a hydrogen atom, an alkyl group having 1 to 6 carbon atoms or a phenyl group, and even more preferably a hydrogen atom. In addition, as the polymer compound contained in the gas barrier layer, it may be an inorganic polysilazane in which all of Rx, Ry, and Rz in the foregoing general formula (1) are hydrogen atoms, or at least Rx, Ry, and Rz. An organopolysilazane having a base other than a hydrogen atom. [0089] The polysilazane-based compound may be used alone or in combination of two or more. In addition, as the polysilazane-based compound, a polysilazane modified product can be used, and a commercially available product can also be used. [0090] In addition to the above-mentioned polymer compound, the polymer layer may further contain other components as long as the effect of the present invention is not impaired. Examples of other components include hardeners, other polymers, anti-aging agents, light stabilizers, and flame retardants. The content of the polymer compound in the polymer layer is preferably from 50 to 100% of the total amount of the components in the polymer layer from the viewpoint of a gas barrier layer having more excellent gas barrier properties. 100% by mass, more preferably 70 to 100% by mass, and even more preferably 80 to 100% by mass. [0091] In addition, the thickness of the polymer layer of the gas barrier film is preferably 50 to 300 nm, and more preferably 50 to 200 nm. In the present invention, even if the thickness of the polymer layer is in the order of nanometers, a sealing sheet having sufficient gas barrier properties can be obtained. [0092] As a method of forming a polymer layer, for example, a spin coater, a knife coater, or a gravure coater is used to form a polymer layer forming solution containing at least one polymer compound, other desired components, and a solvent. A method of applying a known device to form a coating film and drying the coating film. [0093] Examples of the modification treatment of the polymer layer include ion implantation treatment, plasma treatment, radiation irradiation treatment, and heat treatment. The treatment for changing the bond structure of the polymer layer is preferable. These processes may be performed alone or in combination of two or more. The ion implantation process, as described later, is a method of implanting ions into the polymer layer to modify the polymer layer. Plasma treatment is a method of exposing a polymer layer to a plasma to modify the polymer layer. For example, plasma processing can be performed according to the method described in Japanese Patent Application Laid-Open No. 2012-106421. The radiation irradiation treatment is a method of irradiating a polymer layer with radiation to modify the polymer layer. Short-wavelengths with high effects of changing the bond structure of the polymer layer are preferable. Ultraviolet rays, especially vacuum ultraviolet rays, are preferred. For example, vacuum ultraviolet light modification treatment can be performed according to the method described in Japanese Patent Application Laid-Open No. 2013-226757. Among these, from the viewpoint of effectively reforming the surface of the polymer layer to the inside and forming a gas barrier layer having better gas barrier properties, as a modification treatment of the polymer layer, Ion implantation is preferred. [0094] During the ion implantation process, as the ions implanted into the polymer layer, there are ions of rare gases such as argon, helium, neon, krypton, and xenon; fluorocarbon, hydrogen, nitrogen, oxygen, carbon dioxide, chlorine, fluorine, Sulfur and other ions; Methane, ethane and other alkane-based gas ions; Ethylene, propylene and other olefin-based gas ions; pentadiene and butadiene-based diene-based gas ions; acetylene and other ions Ions of alkyne gas; Ions of aromatic hydrocarbon gas such as benzene and toluene; Ions of cycloalkane gas such as cyclopropane; Ions of cycloolefin gas such as cyclopentene; metal ions; Ions of organosilicon compounds; etc. These ions may be used alone or in combination of two or more. Among these, in view of being able to implant ions more easily, and in particular to obtain a gas barrier layer having excellent gas barrier properties, ions of a rare gas such as argon, helium, neon, krypton, xenon, etc. are preferred, Argon ions are more preferred. [0095] The method of implanting ions is not particularly limited. For example, a method of irradiating ions (ion beams) accelerated by an electric field, a method of implanting ions (plasma-generating gas ions) in a plasma, and the like are simply obtained by looking at a gas barrier layer. An ion method (hereinafter sometimes referred to as "plasma ion implantation method") is preferred. Plasma ion implantation, for example, generates plasma in an environment containing plasma-generating gas. By applying a negative high-voltage pulse to the ion-implanted layer, ions (cations) in the plasma can be implanted with implanted ions. The surface portion of the layer is carried out. [0096] The manufacturing method of the sealing sheet (β) is not particularly limited. For example, in the manufacturing method of the sealing sheet (α) described above, the sealing sheet (β) can be manufactured by replacing one release film with a gas barrier film. In addition, after the sealing sheet (α) is manufactured, one of the two peeling films included in the sealing sheet (α) is peeled off, and a gas barrier layer of the exposed adhesive layer and the gas barrier film can be bonded to produce a seal. Flakes (β). In this case, when the sealing sheet (α) has two peeling films having different peeling forces, a peeling film having a small peeling and peeling force is preferred from the viewpoint of operability. [0097] Further, as another type of the sealing sheet of the present invention, it may be a sealing sheet having the following structure, replacing the base material layer of the sealing sheet (β) with a release film, and having two layers of peeling The film sandwiches the gas barrier layer and the adhesive layer. The sealing sheet preferably has a structure in which a gas barrier layer and an adhesive layer are directly laminated. [Sealing Body] The sealing body of the present invention is a sealed object that is sealed with the sealing sheet of the present invention. The sealing body of the present invention includes, for example, a transparent substrate, an element (an object to be sealed) formed on the transparent substrate, and a sealing material for sealing the element. The sealing material is the sealing sheet of the present invention. Then the agent layer. [0099] The transparent substrate is not particularly limited, and various substrate materials can be used. In particular, it is preferable to use a substrate material having a high visible light transmittance. In addition, a material having a high barrier property to prevent moisture or gas to be immersed from the outside of the element and having excellent solvent resistance or weather resistance is preferred. Specific examples include transparent inorganic materials such as quartz and glass; polyvinyl terephthalate, polyvinyl naphthalate, polycarbonate, polystyrene, polyethylene, polypropylene, and poly Phenyl sulfide, polyvinyl fluoride, cellulose acetate, brominated phenoxy, aromatic polyamines, polyimides, polystyrenes, polyaromatic esters, polyfluorenes, polyolefins, etc. Transparent plastic, the aforementioned gas barrier film. The thickness of the transparent substrate is not particularly limited, and it can be appropriately selected in consideration of the light transmittance or the performance inside and outside the shielding element. [0100] Examples of the object to be sealed include an organic EL element, an organic EL display element, a liquid crystal display element, and a solar cell element. That is, the sealing body of the present invention is preferably one in which an organic EL element, an organic EL display element, a liquid crystal display element, or a solar cell element is sealed with the sealing sheet of the present invention. [0101] The method for producing the sealing body of the present invention is not particularly limited. For example, after the adhesive layer of the sealing sheet of the present invention is superposed on the object to be sealed, the adhesive layer of the sealing sheet and the object to be sealed are adhered by heating. Then, by hardening this adhesive layer, the sealing body of this invention can be manufactured. [0102] The bonding conditions for bonding the adhesive layer of the sealing sheet to the sealed object are not particularly limited. The next temperature is, for example, 23 to 100 ° C, and preferably 40 to 80 ° C. This subsequent treatment may be performed while applying pressure. As the curing conditions when the adhesive layer is cured, the conditions described above can be exemplified. [Examples] [0103] Examples of the present invention will be described in more detail below. However, the present invention is not limited to the following examples. The weight average molecular weight (Mw) of the modified polyolefin-based resin and the polyfunctional epoxy compound is a value measured by the following method. <Weight average molecular weight (Mw) of modified polyolefin resin> The weight average molecular weight (Mw) of modified polyolefin resin is a gel permeation chromatography (GPC) device (manufactured by Tosoh Corporation, product name "HLC" -8320 ") and measured under the following conditions, using the value converted to the weight average molecular weight of standard polystyrene. (Measurement conditions) ･ Measurement sample: Tetrahydrofuran solution with a sample concentration of 1% by mass ･ Column: 2 "TSK gel Super HM-H" and 1 "TSK gel Super H2000" (Either are manufactured by Tosoh Corporation) ) Sequentially connected: column temperature: 40 ° C ･ developing solvent: tetrahydrofuran ･ flow rate: 0.60mL / min <weight average molecular weight (Mw) of polyfunctional epoxy compound> weight average molecular weight (Mw) of polyfunctional epoxy compound is Using the above-mentioned gel permeation chromatography (GPC) device and measuring under the above conditions, among the observed peaks, the weight average molecular weight of standard polystyrene corresponding to the retention time of the peak end of the peak with the largest area was converted. [0104] Examples 1 to 3 and Comparative Examples 1 to 2 (1) Preparation of Adhesive Composition Each component shown below was added at the blending amount (effective ingredient ratio) described in Table 1, and was added as Diethyl ethyl ketone was diluted. In Examples 1 to 2 and Comparative Examples 1 to 2, an adhesive composition with an active ingredient concentration of 30% by mass was prepared, and an adhesive with an active ingredient concentration of 25% by mass was prepared in Example 3.组合 物。 Composition. The details of each component used are as follows. ･ Modified polyolefin resin: Made by Mitsui Chemicals Co., Ltd., product name "Unistall H-200", acid modified α-olefin polymer, solid at 25 ° C, weight average molecular weight (Mw) = 52,000. ･ Multifunctional epoxy compound (1): manufactured by Mitsubishi Chemical Corporation, product name "YX8034", hydrogenated bisphenol A diglycidyl ether, epoxy equivalent = 270 g / eq, liquid at 25 ° C, weight average molecular weight (Mw ) = 3,200. ･ Multifunctional epoxy compound (2): manufactured by Mitsubishi Chemical Corporation, product name "YL980", bisphenol A diglycidyl ether is liquid at 25 ° C, epoxy equivalent = 180 ~ 190g / eq, weight average molecular weight ( Mw) = 2,400. ･ Multifunctional epoxy compound (3): manufactured by Kyoeisha Chemical Co., Ltd., product name "Epolight 4000", hydrogenated bisphenol A diglycidyl ether, liquid at 25 ° C, epoxy equivalent = 215 ~ 245g / eq , Weight average molecular weight (Mw) = 800. ･ Polyfunctional epoxy compound (4): manufactured by Mitsubishi Chemical Corporation, product name "YX8000", hydrogenated bisphenol A diglycidyl ether, liquid at 25 ° C, epoxy equivalent = 205 g / eq, weight average molecular weight ( Mw) = 1,400. ･ Multifunctional epoxy compound (5): manufactured by Mitsubishi Chemical Corporation, product name "YX8040", hydrogenated bisphenol A diglycidyl ether, solid at 25 ° C, epoxy equivalent = 1,100 g / eq, weight average molecular weight ( Mw) = 4,200. ･ Adhesion imparting agent: made by Mitsui Chemicals Co., Ltd., product name "FTR6100", copolymer of styrene monomer and aliphatic monomer, softening point = 95 ° C. Imidazole hardening catalyst: manufactured by Shikoku Chemical Industry Co., Ltd., product name "Curezol 2E4MZ", 2-ethyl-4-methylimidazole. ･ Silane coupling agent: manufactured by Shin-Etsu Chemical Industry Co., Ltd., product name "KBM-4803", glycidyloxyoctyltrimethoxysilane. (2) forming a sheet (adhesive layer) on the release-treated surface of a release film (manufactured by Lintec Corporation, product name "SP-PET382150"), applying a prepared adhesive composition to form a coating film, This coating film was dried at 100 ° C. for 2 minutes to form a sheet-like object (adhesive layer) having a thickness of 12 μm, and a laminate including a release film and a sheet-like object (adhesive layer) was obtained. [0106] (3) Production of a sealing sheet with a base material, and a polyethylene layer having a thickness of 25 μm was laminated on the surface of the adhesive layer of the sheet-like object of the laminate produced in the same manner as in the above (2). Based on a terephthalate film (manufactured by Mitsubishi Chemical Corporation, product name "T600E"), a sealing sheet with a substrate was obtained by laminating a release film, an adhesive layer, and a substrate in this order. [0107] Using the above-mentioned laminates and sealing sheets with substrates produced in the examples and comparative examples, the following physical property values were measured and evaluated. The results are shown in Table 1. [Storage elastic modulus G 'of sheet-like article] The sheet-like article (adhesive agent layer) of the release film was removed from the laminate produced in the examples or comparative examples in a plurality of layers, and a heat-applicator was used at 60 ° C. It was compressed by heating to obtain a laminated body having a thickness of 1 mm. Using this laminate as a test sample, a viscoelasticity measuring device (manufactured by Anton Paar, product name "Physica MCR301") was used to measure the laminate before curing at a temperature range of 23 to 150 ° C at a frequency of 1 Hz. The storage elasticity G 'of the body. Table 1 shows the values of the storage elasticity G ′ at 80 ° C. after the measurement. [Exhaust Volume of the Sheet] The surface of the sheet of the laminated body prepared in the example or the comparative example was placed on the flat surface of a glass plate, and then a heat bonding machine was used at 60 ° C. The release film of the laminate is removed. A test sample is obtained. The amount of exhaust gas generated by the sheet when the test sample was left at rest at 120 ° C for 20 minutes was measured using the following apparatus. ･ Equipment: Gas chromatography mass spectrometer (manufactured by Shimadzu Corporation, product name "GCMSQP2010"). ･ Column: 5MS system column (product name: "SH-Rtx (registered trademark)-5MS" manufactured by Shimadzu Corporation, 5% diphenyl / 95% dimethylpolysiloxane). ･ Calibration line: toluene. [Haze of sheet-like article] The aforementioned test sample used for the measurement of the "emission amount of sheet-like article" was allowed to stand at 100 ° C for 2 hours to harden the sheet-like article, The haze of the hardened flakes was measured in accordance with JIS K7136. [0111] [Evaluation of Concavity and Conformity of Sheets] A small piece of polyethylene terephthalate with a thickness of 10 μm was left as a pseudo device on a glass substrate. In addition, the peeling film of the sealing sheet with a base material produced in the examples and comparative examples was removed, and the exposed adhesive layer was laminated on the glass substrate and the pseudo device, so that it was completely covered by the pseudo device on the glass substrate. Then, it was sealed at 80 ° C. using a hot laminator, and then subjected to a pressure treatment at 80 ° C. and 0.5 MPa for 20 minutes. Then, it heated at 100 degreeC for 2 hours, and hardened the adhesive layer. Using an optical microscope, the interface between the pseudo device and the adhesive layer after hardening was observed in a flat view, and the conformity of the unevenness of the sheet-like object was evaluated based on the presence or absence of a gap between the pseudo device and the adhesive layer. A: There is no gap between the pseudo-device and the adhesive layer, so the compliance of unevenness is good. F: A gap was observed between the pseudo-device and the adhesive layer, so the compliance of the unevenness was poor. [Evaluation of Sealability of Sealing Sheet] (i) Fabrication of organic EL element as an anode, a glass substrate formed using an indium tin oxide (ITO) film (thickness: 100 nm, sheet resistance: 50 Ω / □), An organic EL element was produced by the following method. N, N'-bis (naphthalene-1-yl) -N, N'-bis (phenyl) -benzidine) (manufactured by Luminescence Technology) on the ITO film of the aforementioned glass substrate at a speed of 0.1 to 0.2 nm / Evaporate at a rate of one minute to form a positive hole transport layer with a thickness of 50 nm. In addition, on the formed positive-hole transport layer, ginseng (8-hydroxy-hydroquinone ester) aluminum (manufactured by Luminescence Technology) was vaporized at a rate of 0.1 to 0.2 nm / minute to form a light-emitting layer having a thickness of 50 nm. Furthermore, lithium fluoride (LiF) (manufactured by High Purity Chemical Research Institute) was evaporated on the formed light emitting layer at a rate of 0.1 nm / minute to form an electron injection layer having a thickness of 4 nm. Finally, aluminum (Al) (manufactured by High Purity Chemical Research Institute) was evaporated on the formed electron injection layer at a rate of 0.1 nm / minute to form a cathode having a thickness of 100 nm to obtain an organic EL device. In addition, the degree of vacuum when steaming is all 1 × 10 ^-4 Pa or less. [0113] (ii) Production of electronic device The surface of the adhesive layer of the laminates produced in the examples and comparative examples was superimposed on a metal foil film, and adhered at 40 ° C. using a thermal laminator. Then, the release film of the laminate was removed and the exposed adhesive layer was laminated to cover the organic EL element formed on the glass substrate, followed by bonding at 40 ° C using a thermal laminator, and then at 100 ° C. It heated at 2 degreeC for 2 hours, hardened the adhesive layer, and obtained the bottom emission type electronic device which sealed the sealing body of an organic EL element. (Iii) Sealability evaluation After the produced electronic device was left to stand in an environment of 85 ° C. and 85% RH (relative humidity) for 240 hours, the electronic device was started, and the dark point (non-light emitting) of the organic EL element was measured. Area) S ₁ . Measure the dark spot area S of the organic EL element before leaving it in the above environment in advance ₀ The enlargement ratio of the dark spot was calculated from the following formula (1), and the sealing property of the sealing sheet was evaluated based on the following criteria. [Enlargement rate of dark spots (%)] = (S ₁ / S ₀ ) × 100 ･ ･ ･ (1) A: The enlargement rate of dark spots is less than 150%. F: The enlargement rate of dark spots is 150% or more. Moreover, the larger the value of the dark spot enlargement ratio, the more the deterioration of the electrode or the organic layer progresses. [0115] [0116] The flakes (adhesive layer) formed from the adhesive composition of Examples 1 to 3 produced less exhaust gas, had excellent unevenness compliance, and had a good evaluation of sealing performance. Therefore, the sealing sheet having the adhesive layer formed by the adhesive composition can be said to be a sealing material with a high inhibitory effect on the deterioration of the object to be sealed. On the other hand, as for the flake (adhesive layer) formed by the adhesive composition of Comparative Example 1, the storage elasticity G ′ at 80 ° C. was high, and the unevenness compliance was poor. Moreover, as for the sheet-like object (adhesive agent layer) formed by the adhesive agent composition of Comparative Example 2, a large amount of exhaust gas was generated, and the sealing property was also poor. Production Example 1 (Production of Gas Barrier Film) Polyethylene terephthalate (PET) film (manufactured by Toyobo Co., Ltd., product name "PET50A4300") with a thickness of 50 μm, which was easily adhered to both sides, was applied. ), An ultraviolet curable acrylate resin composition (manufactured by JSR Corporation, product name "Opstar Z7530") was applied using a wire ingot to form a coating film, and the coating film was dried at 70 ° C for 1 minute. Furthermore, an electrodeless UV lamp system (manufactured by Heraeus Co., Ltd.) was used with an illumination intensity of 250 mW / cm ² Light quantity 170mJ / cm ² The coating film was hardened by irradiating ultraviolet rays to form a primer layer having a thickness of 1000 nm. In addition, a spin coater (manufactured by Mikasa Co., Ltd., product name "MS-A200") was used to coat the formed primer layer with a number of revolutions of 3000 rpm and a rotation time of 30 seconds. A coating agent (manufactured by Merck Performance Materials, product name "Aquamica NL110-20", solvent: xylene) having a solid content concentration of 10% by mass forms a coating film. Then, the coating film was dried at 120 ° C. for 2 minutes to form a polysilazane layer made of polysilazane with a thickness of 150 nm on the primer layer. Next, a plasma ion implantation device was used on the surface of the aforementioned polysilazane layer to form a gas barrier layer having a thickness of 150 nm by using a plasma ion implantation modification process under the following conditions. Thereby, a gas barrier film having a PET film and a gas barrier layer was produced. (Processing conditions for plasma ion implantation) 压 Internal pressure of the chamber: 0.2Pa ･ Plasma generated gas: Argon ･ Gas flow rate: 100 sccm ･ RF output: 1000W ･ RF frequency: 1000Hz ･ RF pulse width: 50μs Second: DC voltage: -6kV; DC frequency: 1000Hz; DC pulse width: 5μs; DC delay: 50μs; Duty ratio: 0.5%; Processing time: 200 seconds. [0118] Example 4 The surface of the adhesive layer with a thickness of 12 μm on the release film of the laminated body and the surface of the gas barrier layer with a thickness of 150 nm of the gas barrier film produced in Production Example 1 were bonded at 60 ° C. using a heat bonding machine to produce Gas barrier laminated body (1). Comparative Example 3 The above-mentioned modified polyolefin-based resin (manufactured by Mitsui Chemicals Co., Ltd., product name "Unistall H-200", acid-modified α-olefin polymer, weight average molecular weight (Mw) = 52,000) was prepared only Adhesive composition having an effective ingredient concentration of 30% by mass diluted with methyl ethyl ketone. In addition, as described above, the prepared adhesive composition was coated on the release-treated surface of the release film to form a coating film, and the coating film was dried at 100 ° C. for 2 minutes to form an adhesive layer having a thickness of 12 μm. Next, the surface of the adhesive layer and the surface of the gas barrier layer having a thickness of 150 nm of the gas barrier film produced in Production Example 1 were bonded together at 60 ° C using a thermal laminator to produce a gas barrier layered body (2 ). [0120] Using the gas barrier barrier laminates obtained in Example 4 and Comparative Example 3, the following interlayer adhesion evaluation was performed. [Interlayer Adhesiveness] The gas barrier laminates produced in Example 4 and Comparative Example 3 were cut to a length of 25 mm × 300 mm in width, the release film was removed, and the surface of the exposed adhesive layer was attached to a glass plate. Using a heat laminator, a test sample was produced by pressing at 60 ° C. In addition, this test sample was heated at 100 ° C for 2 hours to harden the adhesive layer, and then left to stand for 24 hours in an environment of 23 ° C and a relative humidity of 50%. Furthermore, when the gas barrier barrier laminate was peeled from the glass plate at a temperature of 85 ° C and 85% RH (relative humidity) for 168 hours at a peeling angle of 180 °, it was confirmed whether the adhesive layer was transferred to glass plate. [0121] As a result of the above confirmation, in the gas barrier layered product (1) of Example 4, no transfer of the adhesive layer to the glass plate was confirmed, and the adhesion between the adhesive layer and the gas barrier layer was good. On the other hand, in the gas barrier layered laminate (2) of Comparative Example 3, it was confirmed that the adhesive layer was transferred to the glass plate. As a result, the interlayer adhesion between the adhesive layer and the gas barrier layer was problematic.

Claims (16)

An adhesive composition comprising an adhesive composition containing a modified polyolefin resin (A) and a polyfunctional epoxy compound (B), and a sheet-like material formed by the adhesive composition satisfies the following requirements (I) and (II), ･ Requirement (I): The storage elasticity G 'of the sheet at 80 ° C is 0.3 MPa or less, ･ Requirement (II): The sheet is placed in an environment of 120 ° C When left standing for 20 minutes, the amount of exhaust gas generated per 1 cm ³ of the sheet-like object is 20 mg / cm ³ or less. The adhesive composition according to claim 1, wherein the component (A) is an acid-modified polyolefin resin. For example, the adhesive composition of claim 1 or 2, wherein the content of the component (A) is 15 to 70% by mass based on the total amount of the active ingredients of the adhesive composition. The adhesive composition according to claim 1 or 2, wherein the component (B) is one or more selected from the group consisting of a polyfunctional alicyclic epoxy compound and a polyfunctional aliphatic epoxy compound. The adhesive composition according to claim 1 or 2, wherein the content of the component (B) is 25 to 200 parts by mass based on 100 parts by mass of the ingredient (A). The adhesive composition according to claim 1 or 2, further comprising an adhesion-imparting agent (C). The adhesive composition according to claim 6, wherein the content of the component (C) is 1 to 200 parts by mass based on 100 parts by mass of the ingredient (A). The adhesive composition according to claim 1 or 2, further comprising an imidazole curing catalyst (D). The adhesive composition according to claim 8, wherein the content of the component (D) is 0.1 to 10 parts by mass based on 100 parts by mass of the ingredient (A). The adhesive composition according to claim 1 or 2, further comprising a silane coupling agent (E). The adhesive composition according to claim 10, wherein the content of the component (E) is 0.01 to 10 parts by mass based on 100 parts by mass of the component (A). A sealing sheet having an adhesive layer formed from the adhesive composition according to any one of claims 1 to 11. The sealing sheet according to claim 12, further comprising a gas barrier film, the gas barrier film having a base material layer and a gas barrier layer. For example, the sealing sheet of claim 13 has a structure in which the gas barrier layer of the gas barrier film and the adhesive layer are directly laminated. The sealing sheet according to claim 13 or 14, wherein the gas barrier layer is a polymer layer containing a polymer compound and subjected to a modification treatment. A sealing body is formed by sealing an organic EL element, an organic EL display element, a liquid crystal display element, or a solar cell element with a sealing sheet according to any one of claims 12 to 15.