WO2015178474A1

WO2015178474A1 - Resin composition

Info

Publication number: WO2015178474A1
Application number: PCT/JP2015/064709
Authority: WO
Inventors: 高橋　知宏; 研二芥; 照士高橋; 康弘穂積; 吉浩箱根
Original assignee: 日本化薬株式会社
Priority date: 2014-05-23
Filing date: 2015-05-22
Publication date: 2015-11-26
Also published as: TW201609917A

Abstract

Provided are: a resin composition having favorable transparency, moisture permeation resistance, heat resistance, and moist heat resistance; and a resin composition sheet obtained by means of same. The resin composition contains a polyisobutylene resin, a modified polyolefin resin, a tackifying resin, and a polystyrene-polyolefin block copolymer. The resin composition sheet results from forming a resin composition layer from the resin composition on a support body.

Description

Resin composition

The present invention relates to a resin composition that can be suitably used for sealing an organic EL element.

An organic EL (Electroluminescence) element is a light-emitting element using an organic substance as a light-emitting material, and is a material that has been attracting attention in recent years and can obtain high-luminance light emission at a low voltage. However, organic EL elements are extremely sensitive to moisture, and the organic material itself is altered by moisture, resulting in a decrease in brightness, no light emission, the interface between the electrode and the organic EL layer being peeled off due to moisture, metal There is a problem that the metal oxide is oxidized to increase the resistance.

When the thermosetting resin composition is used as a whole surface sealing material, it is mentioned that the lamination work is easy because the material viscosity before curing is low, and the moisture permeability of the cured product after thermosetting is low. . However, on the other hand, there is a problem that the organic EL element deteriorates due to the heating temperature during thermosetting.

Patent Document 1 discloses an encapsulating film containing a polyisobutylene resin and a hydrogenated cyclic olefin-based polymer. However, the film is usually laminated with a protective film, but because of the large tackiness of the film, it is difficult to peel off the protective film, and the film is greatly deformed when the protective film is peeled off. It is known that handling is extremely difficult.

On the other hand, Patent Document 2 discloses a composition for a sealing material containing an isobutylene polymer, an epoxy group-containing compound, and a curing agent for an epoxy resin. However, since this composition performs hot melt coating, It is not possible to produce a sheet as easily as work. In addition, there is no mention of adhesion and handling properties, and no sufficient study has been made.
In addition, as a method for avoiding thermal degradation of the organic EL element, Patent Document 3 discloses a polyisobutylene resin, a polyisoprene resin having a functional group capable of reacting with an epoxy group and / or a polyisobutylene resin, a tackifying resin, and an epoxy resin. There is disclosed a resin composition containing Patent Document 4 discloses a resin composition comprising a styrene-isobutylene-modified resin and (B) a tackifying resin. However, in any case, a process of heating and curing at a high temperature such as 130 ° C. for a long time after coating and drying is required, and there is a problem in flatness such as curling of the film and productivity.

JP 2009-524705 A JP 2008-248055 A WO2011 / 062167 WO2013 / 108731

The object of the present invention is that varnish coating is possible, it can be easily made into a sheet, does not require a heat curing step, can not only greatly reduce the thermal deterioration of the organic EL device, but also greatly improve productivity. It is an object of the present invention to provide a resin composition that can realize a sheet having good transparency, moisture resistance, adhesive strength, and high heat resistance.

Moreover, when processing and using a resin composition in a sheet form, the surface protection film or the peeling film is bonded on the surface so that a damage | wound and dirt may not be attached to the surface of an optical film in a manufacturing process. The surface protective film or the release film may be peeled off before being attached to the organic EL substrate, or the same or another surface protective film may be attached again after being peeled once. And when peeling off this surface protection film or a peeling film, static electricity generate | occur | produced and there existed a problem that a production yield rate fell because circuits, such as an organic electroluminescent panel, are destroyed by this static electricity. Solving this problem is one of the objects of the present invention.

As a result of intensive studies, the present inventor has found that the resin composition contains a polyisobutylene resin (A), a modified polyolefin resin (B), a tackifier resin (C), and a polystyrene-polyolefin block copolymer (D). The present inventors have found that the above-mentioned problems can be solved by using a product, and have reached the present invention.

That is, the present invention
“(1) A resin composition comprising a polyisobutylene resin (A), a modified polyolefin resin (B), a tackifier resin (C), and a polystyrene-polyolefin block copolymer (D),
(2) The resin composition according to the above (1), wherein the content of the polyisobutylene resin (A) is 35 to 95% by mass when the nonvolatile content in the resin composition is 100% by mass. object,
(3) The resin composition as described in (1) or (2) above, wherein the modified polyolefin resin (B) is an olefin-styrene copolymer,
(4) The resin as described in (3) above, wherein the olefin in the olefin-styrene copolymer is ethylene and / or 1-butene, and the olefin-styrene copolymer has a functional group. Composition,
(5) The resin composition as described in any one of (1) to (4) above, wherein the modified polyolefin resin (B) has a functional group, and the functional group is an acid anhydride group. ,
(6) Any of (1) to (5) above, wherein the content of the modified polyolefin resin (B) is 1 to 30% by mass when the nonvolatile content in the resin composition is 100% by mass The resin composition according to claim 1,
(7) The resin composition according to any one of (1) to (6) above, wherein the tackifying resin (C) is a terpene resin,
(8) The resin composition according to any one of (1) to (7) above, wherein the tackifying resin (C) is an aromatic-modified terpene resin,
(9) Any of (1) to (8) above, wherein the content of the tackifying resin (C) is 1 to 30% by mass when the nonvolatile content in the resin composition is 100% by mass The resin composition according to claim 1,
(10) Any one of (1) to (9) above, wherein the styrene content in all the monomers constituting the polystyrene-polyolefin block copolymer (D) is 10 to 50% by mass. The resin composition according to item,
(11) The above-mentioned (1) to (1), wherein the content of the polystyrene-polyolefin block copolymer (D) is 1 to 30% by mass when the nonvolatile content in the resin composition is 100% by mass. The resin composition according to any one of (10),
(12) The resin composition as described in any one of (1) to (11) above, which further contains an ionic surfactant (E),
(13) The resin composition as described in any one of (1) to (12) above, wherein the ionic surfactant (E) has a sulfo group,
(14) The content of the ionic surfactant (E) is from 0.1 to 5% by mass when the nonvolatile content in the resin composition is 100% by mass. The resin composition according to any one of (13),
(15) The resin composition as described in any one of (1) to (14) above, wherein the resin composition has a visible light transmittance of 80 to 100% from 380 to 780 nm,
(16) A resin composition sheet comprising the resin composition according to any one of (1) to (15) above,
(17) The resin composition sheet according to the above (15), wherein the moisture permeability is 0.1 to 40 g / m ² · day,
(18) The resin composition sheet according to (17), which is used for sealing an organic EL device,
(19) The resin composition according to any one of (1) to (15) above or the resin composition sheet according to any one of (16) to (18) above is used. An organic EL device,
(20) The resin composition or the resin composition sheet described in any one of (1) to (19) above, further comprising an inorganic filler (H),
(21) The resin composition or resin composition sheet described in any one of (1) to (20) above, which further contains a hygroscopic metal oxide (I).

The resin composition of the present invention can be applied to a varnish, can be easily formed into a sheet, does not require a heat curing step, can greatly reduce the thermal deterioration of an organic EL device, and greatly increases productivity. A sheet having good transparency, moisture permeability resistance, adhesive strength, high heat resistance, and antistatic properties can be obtained.

The resin composition of the present invention is mainly characterized in that it contains a polyisobutylene resin (A), a modified polyolefin resin (B), a tackifier resin (C), and a polystyrene-polyolefin block copolymer (D).

The polyisobutylene resin (A) (hereinafter also abbreviated as “component (A)”) used in the present invention has an effect of stably maintaining other physical properties while improving the moisture permeability of the resin composition. Have The polyisobutylene resin (A) is preferably in a solid state at room temperature (25 ° C.).

If the component (A) is a polymer mainly composed of a polyisobutylene skeleton, an isobutylene homopolymer (homopolymer) or an appropriate amount of an olefinic compound such as 1-butene or 2-butene is copolymerized with isobutylene. The copolymer skeleton (hereinafter collectively referred to as "isobutylene polymer") is not limited to a segment skeleton composed of monomer components other than isobutylene as long as desired moisture permeation resistance is obtained. It may be a copolymerized copolymer (block copolymer or graft copolymer). Examples of monomer components other than isobutylene in the copolymer include isoprene, styrene, butadiene, ethylene, propylene, acrylonitrile, vinyl chloride, vinyl bromide, hydrogenated styrene, pentadiene, cyclopentadiene, and dicyclopentadiene. These can use 1 type (s) or 2 or more types. Of these, styrene is preferable from the viewpoints of improvement of heat resistance and moisture permeability. In the copolymer, the proportion of the polyisobutylene skeleton is preferably 50% by mass or more, more preferably 60% by mass or more of the whole polymer. The preferred copolymer composition (polyisobutylene skeleton / segment skeleton composed of monomer components other than isobutylene) is 60 to 90% by mass / 10 to 40% by mass, more preferably 65 to 80% by mass / 20 to 35% by mass. It is. The copolymer may be used in combination with an isobutylene polymer.

Specific examples of the component (A) include commercially available products such as Opanol B12, B15, B50, B80, B100, B120, B150, B200 (manufactured by BASF), JSR butyl 065, 268, 365 (manufactured by JSR), Vista NEX LM-MS, MH, H, MML-80, 100, 120, 140 (manufactured by Exxon Chemical), HYCAR (manufactured by Goodrich), SIBSTARＳＴT102 (manufactured by Kaneka) and the like. These may be used alone or in combination of two or more.

The average molecular weight of the component (A) is not particularly limited, but the viscosity average molecular weight is preferably 4000,000 or less, and more preferably 3000,000 or less, from the viewpoint of providing good coatability and compatibility. On the other hand, the viscosity average molecular weight is preferably 200,000 or more from the viewpoint of preventing repelling during coating of the resin composition, expressing moisture resistance of the resin composition sheet, and improving mechanical strength. 000 or more is more preferable. In addition, the viscosity average molecular weight in this invention is calculated | required using a viscosity formula from the value of intrinsic viscosity obtained by measuring the viscosity of the polymer dilute solution at predetermined temperature according to a conventional method. Alternatively, it can be obtained from the melt viscosity of the resin according to the Flory melt viscosity formula.

(A) A component can use 1 type (s) or 2 or more types. Although there is no restriction | limiting in particular in content of (A) component in a resin composition, it is resin composition from a viewpoint of bringing about favorable coating property and compatibility, and ensuring favorable heat resistance and handleability (tack suppression). 95 mass% or less is preferable with respect to 100 mass% of non volatile matters in a thing, and 80 mass% or less is more preferable. On the other hand, from the viewpoint of obtaining necessary moisture permeation resistance, 35% by mass or more is preferable and 50% by mass or more is more preferable with respect to 100% by mass of the nonvolatile content in the resin composition.

The modified polyolefin resin (B) used in the present invention (hereinafter also abbreviated as “component (B)”) has a cohesive strength while maintaining good adhesion to the substrate of the resin composition sheet obtained. (Holding power) is improved, heat resistance is improved, and handleability in the sheet processing step is also improved. Here, the improvement of the holding power means that the shear deviation amount after 1 hour at 80 ° C. and 1 kg load is preferably 0.5 mm or less.

The component (B) can be further subjected to a crosslinking reaction after forming the sheet to further improve the cohesive force (holding force) and improve the heat resistance.

The component (B) is a polymer mainly composed of an olefin skeleton, and is not particularly limited as long as it is a homopolymer (homopolymer) or a copolymer containing an olefin skeleton. The form of the copolymer is not particularly limited, and examples thereof include a random copolymer, a block copolymer, and a graft copolymer.
The component (B) preferably has a functional group.

Examples of the monomer component of the olefin include ethylene, propylene, 1-butene, 2-butene and the like, and these can be used alone or in combination of two or more. Of these, ethylene and 1-butene are preferable from the viewpoint of compatibility with the component (A). Examples of the monomer component other than the olefin include styrene, butadiene, acrylonitrile, vinyl chloride, vinyl bromide, hydrogenated styrene, pentadiene, cyclopentadiene, dicyclopentadiene, and the like. The above can be used. Of these, styrene is preferable from the viewpoints of improvement of heat resistance and moisture permeability.

A preferred embodiment of the component (B) includes a copolymer having ethylene and / or 1-butene and styrene as monomers and having a functional group.

In the above copolymer, the proportion of each component of ethylene, 1-butene and styrene as a monomer is not particularly limited, but the total proportion of ethylene and / or 1-butene component is 20% by mass of the total monomers. % Or more is preferable, and 40 mass% or more is more preferable. The proportion of the styrene component is preferably 10% by mass or more, more preferably 20% by mass or more based on the total monomers.

The functional group possessed by the component (B) may have any structure as long as it does not adversely affect the desired moisture resistance and adhesiveness. For example, a carboxyl group, an acid anhydride group [—C (O) —O —C (O) —], epoxy group, amino group, hydroxyl group, oxazoline group, oxetane group, cyanate group, phenol group [—Ph—OH], hydrazide group, amide group and the like, and acid anhydride groups are preferred. . These may be any one kind or two or more kinds.

Preferable specific examples of the component (B) include a copolymer containing ethylene and / or 1-butene and styrene having an acid anhydride group.

In the copolymer containing ethylene and / or 1-butene and styrene having an acid anhydride group, the acid value is preferably 1 to 50 mgKOH / g, and more preferably 5 to 30 mgKOH / g. The acid value referred to here is based on JIS K 2501-2003 petroleum product and lubricating oil-neutralization number test method.

Although the number average molecular weight of (B) component is not specifically limited, From a viewpoint of improving the compatibility of a resin composition, 300000 or less are preferable and 150,000 or less are more preferable. Moreover, 5000 or more are preferable and 10,000 or more are more preferable from a viewpoint of exhibiting the moisture permeability resistance of a resin composition. The component (B) is preferably a solid at room temperature (25 ° C.).

In addition, the number average molecular weight in this invention is measured by the gel permeation chromatography (GPC) method (polystyrene conversion). Specifically, the number average molecular weight by the GPC method is LC-9A / RID-6A manufactured by Shimadzu Corporation as a measuring device, and Shodex K-800P / K-804L / K-804L manufactured by Showa Denko KK as a column. Measured at a column temperature of 40 ° C. using tetrahydrofuran or the like as the mobile phase, and can be calculated using a standard polystyrene calibration curve.

Commercially available products that can be used as the component (B) include Surflene P-1000 (a 20% solution of a special polyolefin-based resin acid-modified product (number average molecular weight 70000), acid value 13 to 16 mg KOH / g, manufactured by Mitsubishi Chemical Corporation). Can be mentioned.

(B) 1 type (s) or 2 or more types can be used for a component. The content of the component (B) in the resin composition is not particularly limited, but is 100% by mass based on the nonvolatile content in the resin composition from the viewpoint of ensuring good moisture permeability and transparency of the resin composition. 30 mass% or less is preferable, and 20 mass% or less is more preferable. Moreover, from a viewpoint of expressing the favorable cohesion force of the sheet | seat obtained from a resin composition, 1 mass% or more is preferable with respect to 100 mass% of non volatile matters in a resin composition, and 5 mass% or more is more preferable.

The tackifier resin (C) used in the present invention (hereinafter also abbreviated as “component (C)”) can stably maintain other physical properties while improving the adhesiveness of the resin composition. . The component (C) is not particularly limited, and is a terpene resin, modified terpene resin (hydrogenated terpene resin, terpene phenol copolymer resin, aromatic modified terpene resin, etc.), coumarone resin, indene resin, petroleum resin. (Aliphatic petroleum resins, hydrogenated alicyclic petroleum resins, aromatic petroleum resins, aliphatic aromatic copolymer petroleum resins, alicyclic petroleum resins, dicyclopentadiene petroleum resins and their hydrides) Are preferably used. Among them, terpene resin, aromatic modified terpene resin, terpene phenol copolymer resin, hydrogenated alicyclic petroleum resin, aromatic petroleum resin, aliphatic aromatic copolymer in terms of compatibility, adhesion, and moisture permeability resistance -Based petroleum resins and alicyclic petroleum resins are more preferable, terpene resins and aromatic-modified terpene resins are more preferable, and aromatic-modified terpene resins are particularly preferable. The component (C) may be used alone or in combination of two or more.

Examples of commercially available products that can be used as component (C) include terpene resins such as YS resin PX and YS resin PXN (both manufactured by Yasuhara Chemical Co., Ltd.), and aromatic-modified terpene resins such as YS resin TO and TR series (any Are Yasuhara Chemical Co., Ltd.), and hydrogenated terpene resins include Clearon P, Clearon M, Clearon K series (all manufactured by Yasuhara Chemical Co., Ltd.), and terpene phenol copolymer resins are YS Polystar 2000, Polystar U. , Polystar T, Polystar S, Mighty Ace G (all manufactured by Yashara Chemical Co., Ltd.) and the like, Escorez 5300 series, 5600 series (all manufactured by ExxonMobil), aromatic petroleum resin as hydrogenated alicyclic petroleum resin As END X155 (manufactured by Eastman Chemical Company), (manufactured by Nippon Zeon Co.) QuintoneD100 as aliphatic aromatic copolymer petroleum resin, (manufactured by Nippon Zeon Co.) Quintone1345 as alicyclic petroleum resins and the like.

Although there is no restriction | limiting in particular in content of (C) component in a resin composition, From a viewpoint of maintaining favorable moisture permeability resistance, 30 mass% or less is with respect to 100 mass% of non volatile matters in a resin composition. Preferably, 20 mass% or less is more preferable. Moreover, from a viewpoint of giving sufficient adhesiveness, 1 mass% or more is preferable with respect to 100 mass% of non volatile matters in a resin composition, and 5 mass% or more is more preferable.

The softening point of the component (C) is preferably 50 to 200 ° C., more preferably 90 to 160 ° C., from the viewpoint that the sheet softens in the step of laminating the resin composition sheet and has the desired heat resistance. The softening point is measured by the ring and ball method according to JIS K2207.

The polystyrene-polyolefin block copolymer (D) (hereinafter also abbreviated as “component (D)”) used in the present invention exhibits good tensile properties (tensile elasticity, breaking strength, breaking elongation, etc.) The resulting resin composition sheet has the effect of improving the cohesive strength (holding power) and improving heat resistance. Here, the improvement in holding force means that the shear deviation amount after 1 hour at 105 ° C. and 1 kg load is preferably 0.5 mm or less. The component (D) is composed of a polystyrene block which becomes a crosslinking point below the glass transition point of polystyrene and an elastomer block having a flexible polyolefin structure. Coalescence is preferably used. In the block copolymer, examples of the elastomer block having a polyolefin structure include ethylene, propylene, butylene, ethylene / propylene, ethylene / butylene, and ethylene-ethylene / propylene. These are used alone or in combination of two or more. be able to. Among these, from the viewpoint of tensile properties, polystyrene-poly (ethylene / propylene) block, polystyrene-poly (ethylene / propylene) block-polystyrene, polystyrene-poly (ethylene / butylene) block-polystyrene, polystyrene-poly (ethylene-ethylene / ethylene / polyethylene). A structure such as propylene) block-polystyrene is preferable, and polystyrene-poly (ethylene-ethylene / propylene) block-polystyrene is more preferable. In the block copolymer, the proportion of the polystyrene skeleton is preferably from 5 to 65% by mass, more preferably from 10 to 40% by mass, based on the whole polymer, from the viewpoint of giving sufficient hardness.

Examples of commercially available products that can be used as component (D) include the Septon series and Septon V-series (manufactured by Kuraray Co., Ltd.).
In the case of using Septon V-series, in order to adjust the cohesive strength of the sheet obtained from the resin composition, an organic peroxide, as long as it does not adversely affect transparency, moisture resistance, and adhesiveness, Crosslinking may be introduced by electron beam, ultraviolet ray, or the like. Examples of the organic peroxide include Perbutyl P-40 (α, α'-di (tert-butylperoxy) diisopropylbenzene 40% inert filler-carrying) manufactured by NOF Corporation. TAIC WH-60 (trial isocyanurate 60% white carbon supported) manufactured by Nippon Kasei Co., Ltd. may be used in combination.

The content of the component (D) in the resin composition is not particularly limited, but is 30% by mass with respect to 100% by mass of the nonvolatile content in the resin composition from the viewpoint of maintaining good moisture resistance and transparency. The following is preferable, and 20% by mass or less is more preferable. Moreover, from a viewpoint of giving sufficient tensile characteristics and hardness, 1 mass% or more is preferable with respect to 100 mass% of non volatile matters in a resin composition, and 5 mass% or more is more preferable.

The resin composition of the present invention further contains an ionic surfactant (E) (hereinafter also abbreviated as “component (E)”) to such an extent that the effects of the present invention are not hindered. Static electricity generated at the time of peeling can be reduced. The component (E) is not particularly limited as long as it is an ionic surfactant, but has excellent solubility or dispersibility in toluene in order to improve dispersibility in the components (A) to (D). Are preferred, and those having a sulfo group are more preferred.

As the ionic surfactant (E) having a sulfo group, for example, an alkylsulfonic acid metal salt is suitable. When the ionic surfactant (E) having a sulfo group is an alkylsulfonic acid metal salt, the alkyl group preferably has 11 to 15 carbon atoms in view of the antistatic effect. When the ionic surfactant (E) having a sulfo group is an alkylsulfonic acid metal salt, a sodium salt, potassium salt, lithium salt, calcium salt, magnesium salt, or the like can be used as the metal salt. Is preferably a lithium salt. The alkylsulfonic acid metal salts can be used alone or in combination of two or more.

Examples of commercially available products that can be used as component (E) include Elecut S-417 (manufactured by Takemoto Yushi Co., Ltd.).

The content of the component (E) in the resin composition is not particularly limited, but is preferably 5% by mass or less and preferably 3% by mass with respect to 100% by mass of the nonvolatile content in the resin composition from the viewpoint of maintaining adhesion. % Or less is more preferable. Moreover, from a viewpoint of exhibiting sufficient antistatic property, 0.1 mass% or more is preferable with respect to 100 mass% of non volatile matters in a resin composition, and 1 mass% or more is more preferable.

The surface resistance of the pressure-sensitive adhesive sheet obtained from the resin composition, 1 × 10 ¹² Ω / □ or less, more preferably more preferably 1 × ¹⁰ 10 Ω / □ or less, more preferably 1 × 10 ⁹ Ω / □ Below. When the surface resistance exceeds 1 × 10 ¹² Ω / □, the antistatic function is not sufficient, and static electricity is generated and charged when the release film is peeled off, and this static electricity destroys circuits such as organic EL panels. There is a case.

In order to adjust the cohesive strength of the sheet obtained from the resin composition, liquid polybutadiene and / or liquid polysiloxane having a functional group capable of reacting with an isocyanate group within a range that does not adversely affect moisture permeability and adhesiveness. Isoprene (F) (hereinafter also abbreviated as “component (F)”) may be used in combination. Here, “liquid polybutadiene” is a liquid butadiene-based polymer, and “liquid polyisoprene” is a liquid isoprene-based polymer. “Liquid” is a state at room temperature (25 ° C.). Examples of commercially available liquid polybutadiene and liquid polyisoprene having a functional group capable of reacting with an isocyanate group include NIISO-PB G series and GI series (manufactured by Nippon Soda Co., Ltd.) as liquid polybutadiene. Examples of liquid polyisoprene include Epol (made by Idemitsu Kosan Co., Ltd.). You may use these 1 type or in combination of 2 or more types.

The content of the component (F) in the resin composition is not particularly limited, but is preferably 20% by mass or less with respect to 100% by mass of the nonvolatile content in the resin composition from the viewpoint of maintaining desired transparency. 15% by mass or less is more preferable. Moreover, 1 mass% or more is preferable with respect to 100 mass% of non volatile matters in a resin composition from a viewpoint of fully expressing the effect which mix | blends the said component, and 2 mass% or more is more preferable.

The resin composition of the present invention further contains a curing agent (G) (hereinafter also abbreviated as “component (G)”) to such an extent that the effects of the present invention are not impaired. Can be improved. The curing agent (G) in the present invention is a compound that reacts with the functional group of the component (B) or the component (F), and is not particularly limited, but is an epoxy compound, an isocyanate compound, a metal chelate compound, a metal alkoxide, Examples thereof include metal salts, amine compounds, hydrazine compounds, and aldehyde compounds. You may use these 1 type or in combination of 2 or more types. When using an isocyanate compound, a tin compound may be used in combination as a catalyst.

Although there is no restriction | limiting in particular in content of a hardening | curing agent (G), From a viewpoint of preventing a moisture-resistant fall, 5 mass% or less is preferable with respect to 100 mass% of non volatile matters in a resin composition, 1 mass. % Or less is more preferable. On the other hand, from the viewpoint of developing good holding power, 0.01% by mass or more is preferable and 0.05% by mass or more is more preferable with respect to 100% by mass of the nonvolatile content in the resin composition.

By adding an inorganic filler (H) to the resin composition of the present invention to the extent that the effects of the present invention are not impaired, the moisture permeability of the cured product is improved and repelling during film processing is prevented. be able to. The inorganic filler is not particularly limited, but silica, alumina, barium sulfate, talc, clay, mica powder, aluminum hydroxide, magnesium hydroxide, calcium carbonate, magnesium carbonate, boron nitride, aluminum borate, barium titanate Strontium titanate, calcium titanate, magnesium titanate, bismuth titanate, titanium oxide, barium zirconate, calcium zirconate and the like. Among these, talc and mica are preferable and talc is particularly preferable from the viewpoint of improving the moisture permeability of the cured resin. You may use these 1 type or in combination of 2 or more types.

The inorganic filler (H) is preferably one that has been surface treated with a surface treatment agent to improve its moisture resistance. As the surface treatment agent, aminosilane-based cups such as aminopropylmethoxysilane, aminopropyltriethoxysilane, ureidopropyltriethoxysilane, N-phenylaminopropyltrimethoxysilane, N-2 (aminoethyl) aminopropyl trimethoxysilane, etc. Epoxy silanes such as ring agents, glycidoxypropyltrimethoxysilane, glycidoxypropyltriethoxysilane, glycidoxypropylmethyldiethoxysilane, glycidylbutyltrimethoxysilane, (3,4-epoxycyclohexyl) ethyltrimethoxysilane Coupling agents, mercaptosilane coupling agents such as mercaptopropyltrimethoxysilane, mercaptopropyltriethoxysilane, methyltrimethoxysilane, octadecyltrimethoxy Silane coupling agents such as Sisilane, Phenyltrimethoxysilane, Methacryloxypropyltrimethoxysilane, Imidazolesilane, Triazinesilane, Hexamethyldisilazane, Hexaphenyldisilazane, Trisilazane, Cyclotrisilazane, 1,1,3,3 , 5,5-hexametacyclotrisilazane, organosilazane compounds, butyl titanate dimer, titanium octylene glycolate, diisopropoxy titanium bis (triethanolaminate), dihydroxy titanium bis lactate, dihydroxy bis (ammonium lactate) titanium, bis (Dioctyl pyrophosphate) ethylene titanate, bis (dioctyl pyrophosphate) oxyacetate titanate, tri-n-butoxy titanium monostearate Tetra-n-butyl titanate, tetra (2-ethylhexyl) titanate, tetraisopropyl bis (dioctyl phosphite) titanate, tetraoctyl bis (ditridecyl phosphite) titanate, tetra (2,2-diallyloxymethyl-1-butyl ) Bis (ditridecyl) phosphite titanate, isopropyl trioctanoyl titanate, isopropyl tricumyl phenyl titanate, isopropyl triisostearoyl titanate, isopropyl isostearoyl diacryl titanate, isopropyl dimethacryl isostearoyl titanate, isopropyl tri (dioctyl phosphate) titanate, isopropyl Tridodecylbenzenesulfonyl titanate, isopropyltris (dioctylpyrophosphate) G) titanate, isopropyl tri (N- amidoethyl-aminoethyl) titanate coupling agents such as titanates. You may use these 1 type or in combination of 2 or more types.

The average particle size of the inorganic filler (H) is not particularly limited, but is preferably 10 μm or less and more preferably 5 μm or less from the viewpoint of not damaging the organic EL element. On the other hand, from the viewpoint of exhibiting moisture permeability resistance, 0.05 μm or more is preferable, and 0.1 μm or more is more preferable.

The average particle diameter of the inorganic filler (H) can be measured by a laser diffraction / scattering method based on Mie scattering theory. Specifically, the particle size distribution of the inorganic filler (H) can be created on a volume basis with a laser diffraction particle size distribution measuring device, and the median diameter can be measured as the average particle diameter. Measurement sample is inorganic filler (
What H) was disperse | distributed in water with the ultrasonic wave can be used preferably. As a laser diffraction particle size distribution measuring device, LA-500 manufactured by Horiba, Ltd. can be used.

Although content of an inorganic filler (H) is not specifically limited, From a viewpoint of preventing that the viscosity of a resin composition raises and preventing the intensity | strength of hardened | cured material falling and becoming brittle. The non-volatile content in the resin composition is preferably 50% by mass or less, more preferably 40% by mass or less, and still more preferably 30% by mass or less. On the other hand, from the viewpoint of sufficiently obtaining the effect of blending the inorganic filler (H), it is preferably 1% by mass or more, more preferably 5% by mass or more, with respect to 100% by mass of the nonvolatile content in the resin composition. More preferably, it is more than mass%.

The resin composition of the present invention can further contain a hygroscopic metal oxide (I) in order to further improve the moisture permeability resistance of the cured product. Here, the “hygroscopic metal oxide” means a metal oxide that has a capability of absorbing moisture and chemically reacts with moisture that has been absorbed to become a hydroxide. Specifically, it is one kind selected from calcium oxide, magnesium oxide, strontium oxide, aluminum oxide, barium oxide, or the like, or a mixture or solid solution of two or more kinds. Among these, calcium oxide and magnesium oxide are preferable from the viewpoint of high hygroscopicity, cost, and stability of raw materials. Specific examples of the mixture or solid solution of two or more types include calcined dolomite (a mixture containing calcium oxide and magnesium oxide), calcined hydrotalcite (a solid solution of calcium oxide and aluminum oxide), and the like. It is done. Such a hygroscopic metal oxide (I) is known as a hygroscopic material in various technical fields, and a commercially available product can be used. Specifically, calcium oxide (“Moystop # 10” manufactured by Sankyo Flour Milling Co., Ltd.), magnesium oxide (“Kyowa Mag MF-150”, “Kyowa Mag MF-30” manufactured by Kyowa Chemical Industry Co., Ltd., “Pure Mag” manufactured by Tateho Chemical Industry Co., Ltd. FNMG ”, etc.), lightly burned magnesium oxide (“ # 500 ”,“ # 1000 ”,“ # 5000 ”, etc., manufactured by Tateho Chemical Industries, Ltd.), calcined dolomite (“ KT ”, etc., produced by Yoshizawa Lime), calcined hydrotalcite (“Hydrotalcite” manufactured by Toda Kogyo Co., Ltd.) and the like. These may use 1 type (s) or 2 or more types.

The average particle diameter of the hygroscopic metal oxide (I) is not particularly limited, but from the viewpoint of preventing coarse particles from damaging the organic EL element in the sealing step and increasing the interfacial bond strength with the resin component. 10 μm or less is preferable, 5 μm or less is more preferable, and 1 μm or less is even more preferable. On the other hand, 0.001 μm or more is preferable from the viewpoint of preventing the particles from being easily aggregated and preventing it from being difficult to impart sufficiently high moisture resistance to the cured product due to poor dispersion in the composition. 0.01 μm or more is more preferable, and 0.1 μm or more is more preferable.

If the average particle size of the hygroscopic metal oxide (I) is 10 μm or less, it can be used as it is, but if the average particle size of the commercial product exceeds 10 μm, the average particle size is obtained by pulverization, classification, etc. It is preferable to use after preparing into a granular material having a diameter of 10 μm or less.

Further, the hygroscopic metal oxide (I) preferably has an average particle diameter in the above preferred range and does not contain coarse particles having a particle diameter of 20 μm or more. More preferably, it does not contain coarse particles of 5 μm or more. By not including such coarse particles, it is advantageous in that the EL element is hardly damaged in the sealing process.

The average particle diameter of the hygroscopic metal oxide (I) can be measured by a laser diffraction / scattering method based on the Mie scattering theory. Specifically, the particle size distribution of the hygroscopic metal oxide (I) can be created on a volume basis by a laser diffraction particle size distribution measuring device, and the median diameter can be measured as the average particle diameter. As the measurement sample, a hygroscopic metal oxide (I) dispersed in water by ultrasonic waves can be preferably used. As a laser diffraction particle size distribution measuring apparatus, LA-500 manufactured by Horiba Ltd. can be used.

As the hygroscopic metal oxide (I), a surface treated with a surface treatment agent can be used. By using such a surface-treated hygroscopic metal oxide (I), the adhesion stability of the cured product can be further increased. In the stage before curing, moisture in the resin and the hygroscopic metal oxide ( I) can be prevented from reacting.

The content of the hygroscopic metal oxide (I) is not particularly limited, but it prevents the viscosity of the resin composition from increasing and prevents the strength of the cured product from decreasing and becoming brittle. From the viewpoint, the content is preferably 50% by mass or less, more preferably 40% by mass or less, and still more preferably 30% by mass or less with respect to 100% by mass of the nonvolatile content in the resin composition. On the other hand, from the viewpoint of sufficiently obtaining the effect of blending the inorganic filler (H), it is preferably 1% by mass or more, more preferably 5% by mass or more, with respect to 100% by mass of the nonvolatile content in the resin composition. More preferably, it is more than mass%.

As the surface treatment agent used for the surface treatment, for example, higher fatty acids, alkylsilanes, silane coupling agents and the like can be used, and among these, higher fatty acids or alkylsilanes are preferable. You may use these 1 type or in combination of 2 or more types.

The higher fatty acid is preferably a higher fatty acid having 18 or more carbon atoms such as stearic acid, montanic acid, myristic acid and palmitic acid. Of these, stearic acid is preferred. You may use these 1 type or in combination of 2 or more types.

Examples of the alkylsilane include methyltrimethoxysilane, ethyltrimethoxysilane, hexyltrimethoxysilane, octyltrimethoxysilane, decyltrimethoxysilane, octadecyltrimethoxysilane, dimethyldimethoxysilane, octyltriethoxysilane, n-octadecyldimethyl (3 -(Trimethoxysilyl) propyl) ammonium chloride and the like. You may use these 1 type or in combination of 2 or more types.

Examples of the silane coupling agent include 3-glycidyloxypropyltrimethoxysilane, 3-glycidyloxypropyltriethoxysilane, 3-glycidyloxypropyl (dimethoxy) methylsilane, and 2- (3,4-epoxycyclohexyl) ethyltrimethoxy. Epoxy silane coupling agents such as silane; mercapto silane coupling agents such as 3-mercaptopropyltrimethoxysilane, 3-mercaptopropyltriethoxysilane, 3-mercaptopropylmethyldimethoxysilane and 11-mercaptoundecyltrimethoxysilane ; 3-aminopropyltrimethoxysilane, 3-aminopropyltriethoxysilane, 3-aminopropyldimethoxymethylsilane, N-phenyl-3-aminopropyltrime Amino silane cups such as xylsilane, N-methylaminopropyltrimethoxysilane, N- (2-aminoethyl) -3-aminopropyltrimethoxysilane and N- (2-aminoethyl) -3-aminopropyldimethoxymethylsilane Ringing agents; Ureido silane coupling agents such as 3-ureidopropyltriethoxysilane, vinyl silane coupling agents such as vinyltrimethoxysilane, vinyltriethoxysilane and vinylmethyldiethoxysilane; p-styryltrimethoxysilane Styryl-based silane coupling agents; acrylate-based silane coupling agents such as 3-acryloxypropyltrimethoxysilane and 3-methacryloxypropyltrimethoxysilane; 3-isocyanatopropyltrimethoxy Isocyanate-based silane coupling agents such as silane, sulfide-based silane coupling agents such as bis (triethoxysilylpropyl) disulfide and bis (triethoxysilylpropyl) tetrasulfide; phenyltrimethoxysilane, methacryloxypropyltrimethoxysilane, imidazole Examples thereof include silane and triazine silane. You may use these 1 type or in combination of 2 or more types.

The surface treatment can be performed, for example, by adding and spraying a surface treatment agent and stirring for 5 to 60 minutes while stirring and dispersing untreated hygroscopic metal oxide (I) at room temperature with a mixer. As a mixer, a well-known mixer can be used, For example, blenders, such as V blender, a ribbon blender, and a bubble cone blender, mixers, such as a Henschel mixer and a concrete mixer, a ball mill, a cutter mill, etc. are mentioned. Further, when the hygroscopic material is pulverized with a ball mill or the like, a method of surface treatment by mixing the above-mentioned higher fatty acid, alkylsilane or silane coupling agent is also possible. The treatment amount of the surface treatment agent varies depending on the type of the hygroscopic metal oxide (I) or the type of the surface treatment agent, but is preferably 1 to 10% by weight with respect to the hygroscopic metal oxide (I).

The resin composition of the present invention may optionally contain various resin additives other than the above-described components to the extent that the effects of the present invention are not impaired. Examples of such resin additives include organic fillers such as rubber particles, silicon powder, nylon powder, and fluorine powder, thickeners such as olben and benton, silicone-based, fluorine-based, and polymer-based antifoaming agents. Alternatively, adhesion promoters such as leveling agents, triazole compounds, thiazole compounds, triazine compounds, porphyrin compounds, and the like can be given.

The method for preparing the resin composition of the present invention is not particularly limited, and examples thereof include a method in which a compounding component is added with a solvent or the like as necessary and mixed using a rotary mixer or the like.

The transparency of the cured product of the resin composition of the present invention can be measured with a spectrophotometer, and examples of the cured product of the resin composition include a resin composition sheet. The higher the transparency, the better the luminous efficiency of the EL element. Specifically, the transmittance at 380 to 780 nm calculated based on JIS Z8722 is preferably 80% or more, more preferably 82% or more, still more preferably 84% or more, still more preferably 86% or more, and 88% The above is particularly preferable, and 90% or more is particularly preferable.

The moisture permeability resistance of the resin composition sheet of the present invention can be measured by the differential pressure method of JIS K-7129A. (Measuring conditions: temperature 40 ° C., relative humidity 90%) The lower the moisture permeability, the more delayed the penetration of moisture from the outside into the EL device, so that a 50 μm-thick resin composition layer is 40 ° C. 90% RH. The value when measured under the conditions is preferably 40 g / m ² · day or less, more preferably 20 g / m ² · day or less, and still more preferably 10 g / m ² or less. On the other hand, the lower the moisture permeability, the better, but practically 0.1 g / m ² · day or more is preferable.

Although the use of the resin composition of the present invention is not particularly limited, it can be used as a sealing material for various devices such as semiconductors, solar cells, high-brightness LEDs, LCDs, and organic ELs, and is particularly suitable for organic EL devices. Can be used.

The resin composition sheet of the present invention includes both those obtained by forming the resin composition of the present invention into a sheet and those obtained by forming a layer of the resin composition of the present invention on a support. For application to various devices, a resin composition sheet in which a layer of the resin composition of the present invention is formed on a support is laminated on a necessary portion of the application object, and the resin composition layer is applied to the application object. You may make it transfer to.

When the resin composition sheet in which the resin composition layer of the present invention is formed on a support is applied to an organic EL device, the organic EL element is sealed by pre-curing the organic EL element before the sealing step. Thereafter, it is possible to obtain a sheet that does not require heat curing and greatly reduces thermal deterioration of the organic EL element. Industrially, a method using such a resin composition sheet is preferable.

The resin composition sheet having a support can be implemented using methods known to those skilled in the art, such as die coating, spin coating, doctor blade coating, calendering, and extrusion molding. For example, it can be produced by preparing a varnish in which a resin composition is dissolved in an organic solvent, applying the varnish on a support, and further drying the organic solvent by heating or blowing hot air.

Examples of the organic solvent include aliphatic hydrocarbons such as hexane, heptane, and octane, alicyclic hydrocarbons such as cyclohexane and methylcyclohexane, and aromatic hydrocarbons such as toluene and xylene. From the viewpoint of the shelf life (usable period) of the resin composition sheet, those having a low boiling point are preferred, and one or a combination of two or more may be used.

The drying conditions for the resin composition sheet of the present invention are not particularly limited, but are preferably 50 to 140 ° C. and 3 to 20 minutes. When the temperature is lower than 50 ° C., the amount of the solvent remaining in the resin composition layer tends to increase. When the temperature is higher than 140 ° C., the support tends to be deformed by heat when the layer of the resin composition of the present invention is formed on the support.

The resin composition sheet of the present invention can be cured by heating in advance to react the component (B), the component (F) and the component (G) before the sealing step. By such curing, it can be used as a resin composition sheet having better cohesive strength, adhesiveness and handleability. The curing conditions are not particularly limited, but the curing temperature is preferably 20 to 50 ° C, more preferably 30 to 40 ° C. The curing time is preferably 1 to 10 days, and more preferably 3 to 7 days.

The thickness of the cured resin composition sheet is preferably 3 to 200 μm, more preferably 10 to 100 μm, and still more preferably 20 to 80 μm.

The cured resin composition sheet preferably has a resin composition weight reduction amount (residual solvent amount) of 0.1% or less when it is dried at 130 ° C. for 15 minutes. By being 0.1% or less, the effect of reducing damage to the element after the sealing step to the organic EL device is improved.

As the support used for the resin composition sheet, it is preferable to use a moisture-proof support (sealing substrate). Examples of the sealing substrate include a moisture-proof plastic film or a metal foil such as a copper foil and an aluminum foil. Examples of the plastic film having moisture resistance include a plastic film in which an inorganic substance such as silicon oxide (silica), silicon nitride, SiON, SiCN, or amorphous silicon is deposited on the surface. Examples of the plastic film include polyolefins such as polyethylene, polypropylene, and polyvinyl chloride, polyethylene terephthalate (hereinafter sometimes referred to as “PET”), polyesters such as polyethylene naphthalate, polycarbonate, polyimide, and cycloolefin polymers (hereinafter “ A plastic film such as “COP” may be used. As the plastic film, COP is particularly preferable. Examples of commercially available plastic films with moisture resistance include Tech Barrier HX, AX, LX, L series (Mitsubishi Resin Co., Ltd.) and X-BARRIER (Mitsubishi Resin Co., Ltd.) with further improved moisture resistance. It is done. A sealing substrate having a multilayer structure of two or more layers may be used. Also, a support of the type in which the plastic film and the metal foil are bonded to each other with an adhesive in order to improve handling properties is inexpensive and industrially convenient. A plastic film or the like that does not have moisture resistance can also be used as a support, and the surface of the resin composition may be protected by means such as a release liner. In that case, after forming the resin composition sheet on the substrate on which the organic EL element is formed, it is preferable to peel the support, and then separately laminate a sealing substrate on the resin composition sheet.

The resin composition of the present invention can be provided in various shapes. For example, when the encapsulating resin composition is used as an encapsulant for an electronic device, the resin composition sheet can be used by being combined with a component of the electronic device.

For example, the resin composition sheet can be used in combination with an optical film such as a color filter, a polarizing plate, or a retardation plate.

EXAMPLES The present invention will be specifically described below with reference to examples, but the present invention is not limited to these examples. In the following description, “parts” means “parts by mass” and “%” means “% by mass” unless otherwise specified.

[Materials used]
The materials used in the experiment will be described.
Polyisobutylene resin (A)
Polyisobutylene (isobutylene-based weight body) (Opanol B100, viscosity average molecular weight 1110000, manufactured by BASF)
Polyisobutylene (isobutylene-based weight body) (Opanol B200, viscosity average molecular weight 4000000, manufactured by BASF)

Modified polyolefin resin (B)
・ Surflen P-1000 (20% solution of special polyolefin-based resin acid-modified product (number average molecular weight 70000), acid value 13-16 mg KOH / g, manufactured by Mitsubishi Chemical Corporation)

Tackifying resin (C)
Aromatic modified terpene resin (YS resin TO125, softening point 125 ° C., manufactured by Yasuhara Chemical Co., Ltd.)

Polystyrene-polyolefin block copolymer (D)
・ Polystyrene-poly (ethylene-ethylene / propylene) block-polystyrene (Septon 4055, manufactured by Kuraray Co., Ltd.)

Others ・ Solvent: Toluene

[Measurement and evaluation methods]
Various measurement methods and evaluation methods will be described.

<Measurement and evaluation of transparency>
Using a resin composition sheet having a thickness of 50 μm, a spectral spectrum from 380 to 780 nm was measured with a spectrophotometer UV-3600 manufactured by Shimadzu Corporation, and a visible light transmittance was calculated in accordance with JIS Z8722.
<Evaluation of haze>
Using a haze meter (TC-HIIIDPK manufactured by Tokyo Denshoku Co., Ltd.), the haze value of the obtained pressure-sensitive adhesive sheet was measured according to JIS K6714.
<Evaluation of holding power against glass>
A glass plate as the adherend and each adhesive sheet was laminated with an adhesion area of 25 mm × 25 mm, 50 ° C., and pressed at 0.5P _a 30 minutes, then the 1000g free end of the adhesive tape by hanging the glass plate A uniform load was applied, and the length of the adhesive tape after shifting for 1 hour at 105 ° C. was measured. ("Retention force deviation" in Table 1)
<Adhesive strength to glass>
Each adhesive tape was cut into a size of 25 mm × 200 mm on a glass plate as an adherend was laminated with an adhesion area of 25 × 80 mm, 50 ° C., and pressed at 0.5P _a 30 min, after 20 min at 23 ° C. Then, the force required for the peeling was measured. (180 degree peeling, tensile speed 300 mm / min, 23 ° C., 65% RH atmosphere) (“Peel” in Table 1)
<Evaluation of moisture permeability>
The resin composition sheet having a thickness of 50 μm was measured by an isobaric method (humidity sensitive sensor method) using a water vapor permeability evaluation apparatus L80-5000 manufactured by Systech Instruments. (Measurement conditions according to JIS K-7129A: temperature 40 ° C., relative humidity 90%) (“moisture permeability” in Table 1)
<Evaluation of antistatic properties>
The pressure-sensitive adhesive was applied onto the release film so that the film thickness after drying was 50 μm, dried, and then bonded to the moisture-proof treatment layer side of the moisture-proof COP to prepare a laminated sheet of the moisture-proof film and the pressure-sensitive adhesive. Immediately after peeling the release film of the laminated sheet, the surface resistance value of the adhesive layer was measured with a high resistivity meter Hiresta (applied voltage 500 V).
<Evaluation of heat resistance and moist heat resistance>
The pressure-sensitive adhesive was applied onto the release film so that the film thickness after drying was 50 μm, dried, and then bonded to the moisture-proof treatment layer side of the moisture-proof COP to prepare a laminated sheet of the moisture-proof film and the pressure-sensitive adhesive. A release film of such a laminated sheet is peeled off and bonded to a glass plate, and a polyvinyl alcohol polarizing plate having a cellulose triacetate film as a protective layer (average polymerization degree 1700 of polyvinyl alcohol polarizing film, average saponification degree 99.5). A polarizing plate having an adhesive layer on the cellulose triacetate film side (mol%, 5-fold stretching) was pressed and bonded to the moisture-proof film surface of the laminated sheet of the moisture-proof film and the pressure-sensitive adhesive with a roller. A durability test (105 ° C. or 85 ° C. 85% for 500 hours) was performed on the bonded product, and the foamed state, the peeled state, and the deteriorated state were observed. The results are shown in Table 1.

Example 1
To a polyisobutylene solution (10.0% toluene solution of Oppanol B100) and 67.5 parts of a polyisobutylene solution (4.0% toluene solution of Oppanol B200), a modified polyolefin resin solution (Surflen P-1000: special polyolefin system) 5.4 parts of a resin acid-modified product (20% solution), 5.4 parts of an aromatic modified terpene resin solution (50% toluene solution of YS resin TO-125), 7 parts of a polystyrene-polyolefin block copolymer solution (Septon 4055) 0.04% toluene solution) was mixed and uniformly dispersed with a mixer to obtain a varnish.
The obtained varnish is uniformly applied on a release treatment surface of a PET film (thickness 38 μm) treated with an alkyd release agent with a comma coater so that the thickness of the resin composition layer after drying becomes 50 μm. The resin composition sheet was obtained by applying and drying at 110 ° C. for 10 minutes.

Example 2
A varnish was obtained in the same manner as in Example 1, except that the amount of the polystyrene-polyolefin block copolymer solution (7.0% toluene solution of Septon 4055) was 30.9 parts, according to the recipe shown in Table 1 below. It was. Using the obtained varnish, a resin composition sheet was obtained in exactly the same manner as in Example 1.

Example 3
A varnish was obtained in the same manner as in Example 1 except that the amount of the polystyrene-polyolefin block copolymer solution (7.0% toluene solution of Septon 4055) was 46.3 parts according to the formulation table in Table 1 below. It was. Using the obtained varnish, a resin composition sheet was obtained in exactly the same manner as in Example 1.

Example 4
Further, a varnish was obtained according to the formulation table of Table 1 below in the same manner as in Example 1 except that 1.8 parts of an ionic surfactant (10% toluene solution of ELECUT S-417) was mixed. Using the obtained varnish, a resin composition sheet was obtained in exactly the same manner as in Example 1.

Example 5
A varnish was obtained in the same manner as in Example 4 except that the amount of the polystyrene-polyolefin block copolymer solution (7.0% toluene solution of Septon 4055) was 30.9 parts, according to the formulation table of Table 1 below. It was. Using the obtained varnish, a resin composition sheet was obtained in exactly the same manner as in Example 1.

Example 6
A varnish was obtained in the same manner as in Example 4 except that the amount of the polystyrene-polyolefin block copolymer solution (7.0% toluene solution of Septon 4055) was 46.3 parts, according to the formulation table of Table 1 below. It was. Using the obtained varnish, a resin composition sheet was obtained in exactly the same manner as in Example 1.

Comparative Example 1
A varnish was obtained in the same manner as in Example 1 except that a polystyrene-polyolefin block copolymer solution (7.0% toluene solution of Septon 4055) was not used according to the formulation table in Table 1 below. Using the obtained varnish, a resin composition sheet was obtained in exactly the same manner as in Example 1.

Comparative Example 2
A varnish was obtained in the same manner as in Example 2 except that a modified polyolefin resin solution (Surflen P-1000: 20% solution of a special polyolefin-based resin acid modified product) was not used according to the formulation table of Table 1 below. Using the obtained varnish, a resin composition sheet was obtained in exactly the same manner as in Example 1.

Comparative Example 3
In the same manner as in Example 1 except that the amount of the modified polyolefin resin solution (Surflen P-1000: 20% solution of the special polyolefin-based resin acid modified product) was 32.4 parts, Although a varnish was obtained, a resin composition sheet having poor compatibility and good surface properties and transparency of the coating film could not be obtained.

Comparative Example 4
A varnish was obtained in the same manner as in Example 1 except that the amount of the polystyrene-polyolefin block copolymer solution (7.0% toluene solution of Septon 4055) was 92.6 parts according to the formulation table in Table 1 below. However, it was not possible to obtain a resin composition sheet with poor compatibility and good surface properties and transparency of the coating film.

Comparative Example 5
A varnish was obtained in the same manner as in Example 4 except that a polystyrene-polyolefin block copolymer solution (7.0% toluene solution of Septon 4055) was not used according to the formulation table in Table 1 below. Using the obtained varnish, a resin composition sheet was obtained in exactly the same manner as in Example 1.

Comparative Example 6
A varnish was obtained in the same manner as in Example 4 except that the modified polyolefin resin solution (Surflen P-1000: 20% solution of a special polyolefin resin acid-modified product) was not used according to the formulation table of Table 1 below. Using the obtained varnish, a resin composition sheet was obtained in exactly the same manner as in Example 1.

Comparative Example 7
In the same manner as in Example 4 except that the amount of the modified polyolefin resin solution (Surflen P-1000: 20% solution of the special polyolefin-based resin acid-modified product) was 32.4 parts, Although a varnish was obtained, a resin composition sheet having poor compatibility and good surface properties and transparency of the coating film could not be obtained.

Comparative Example 8
A varnish was obtained in the same manner as in Example 4 except that the amount of the polystyrene-polyolefin block copolymer solution (7.0% toluene solution of Septon 4055) was 92.6 parts according to the formulation table in Table 1 below. However, it was not possible to obtain a resin composition sheet with poor compatibility and good surface properties and transparency of the coating film.

Table 1 shows the results of testing the resin composition sheet obtained as described above by the measurement method and the evaluation method described above.

From Examples 1 to 6, the resin composition sheet obtained from the resin composition of the present invention does not require high-temperature heating such as 80 ° C. for curing, and does not require heat-curing during lamination. It can be bonded with a sufficiently high adhesive force by low temperature heating, can maintain a good appearance even after being placed in a high temperature, high humidity environment after lamination with a polarizing plate, and also has good transparency and good Excellent moisture permeability. Therefore, according to the present invention, a resin composition serving as a sealing material capable of forming a highly reliable sealing structure without causing deterioration of the organic EL element with respect to the organic EL element that is likely to be deteriorated by moisture or heat. Products and resin composition sheets can be obtained, and a highly reliable organic EL device can be provided.

On the other hand, in Comparative Examples 1 and 2, the modified polyolefin resin (B) or the polystyrene-polyolefin block copolymer (D) is not used, and the effects of the present invention are not exhibited. That is, it is understood that it is important to mix the component (B) and the component (D) in order to exert the effect of the present invention. Further, in Examples 4 to 6 using the ionic surfactant (E) having a sulfo group, the surface resistance value was greatly reduced as compared with Examples 1 to 3, and the effect of antistatic property was exhibited. In Comparative Example 4, the polystyrene-polyolefin block copolymer (D) is not used, and the antistatic effect is not exhibited. Therefore, it is understood that it is important to contain not only the component (E) but also the component (D) in order to exhibit the antistatic effect.

Claims

A resin composition comprising a polyisobutylene resin (A), a modified polyolefin resin (B), a tackifier resin (C), and a polystyrene-polyolefin block copolymer (D).
The resin composition according to claim 1, wherein the content of the polyisobutylene resin (A) is 35 to 95% by mass when the nonvolatile content in the resin composition is 100% by mass.
3. The resin composition according to claim 1, wherein the modified polyolefin resin (B) is an olefin-styrene copolymer.
4. The resin composition according to claim 1, wherein the olefin is an olefin-styrene copolymer having ethylene and / or 1-butene and having a functional group.
The resin composition according to any one of claims 1 to 4, wherein the functional group of the modified polyolefin resin (B) is an acid anhydride group.
6. The modified polyolefin resin (B) content is 1 to 30% by mass when the nonvolatile content in the resin composition is 100% by mass, according to any one of claims 1 to 5. Resin composition.
The resin composition according to any one of claims 1 to 6, wherein the tackifying resin (C) is a terpene resin.
The resin composition according to any one of claims 1 to 7, wherein the tackifying resin (C) is an aromatic modified terpene resin.
The tackifying resin (C) content is 1 to 30% by mass when the nonvolatile content in the resin composition is 100% by mass, according to any one of claims 1 to 8. Resin composition.
The resin composition according to any one of claims 1 to 9, wherein the polystyrene-polyolefin block copolymer (D) has a styrene content of 20 to 40% by mass.
11. The content of the polystyrene-polyolefin block copolymer (D) is 1 to 30% by mass when the nonvolatile content in the resin composition is 100% by mass. 2. The resin composition according to item 1.
The resin composition according to any one of claims 1 to 11, further comprising an ionic surfactant (E).
The resin composition according to any one of claims 1 to 12, wherein the ionic surfactant (E) has a sulfo group.
14. The content of the ionic surfactant (E) is 0.1 to 5% by mass when the nonvolatile content in the resin composition is 100% by mass. 2. The resin composition according to item 1.
The resin composition according to any one of claims 1 to 14, wherein the resin composition has a visible light transmittance of 80 to 100% from 380 nm to 780 nm.
A resin composition sheet comprising the resin composition according to any one of claims 1 to 15.
The resin composition sheet according to claim 16, wherein the moisture permeability is 0.1 to 40 g / m 2 · day.
The resin composition sheet according to claim 17, which is used for sealing an organic EL element.
An organic EL device comprising the resin composition according to any one of claims 1 to 15.
The resin composition according to any one of claims 1 to 15, further comprising an inorganic filler (H).
The resin composition according to any one of claims 1 to 15, further comprising a hygroscopic metal oxide (I).