KR102645231B1 - In-plane encapsulant for organic EL display elements and encapsulant set for organic EL display elements - Google Patents

Abstract

The purpose of the present invention is to provide an in-plane encapsulant for organic EL display elements that is excellent in applicability, wet spreadability, and curability. Additionally, the present invention aims to provide a set of encapsulants for organic EL display elements comprising a peripheral encapsulant and an in-plane encapsulant for organic EL display elements. The present invention is an in-plane encapsulant for organic EL display elements used by applying it to the inside of a peripheral encapsulant for organic EL display elements containing a moisture absorbent, comprising a curable resin and a cationic polymerization initiator, the curable resin comprising: The viscosity of the entire in-plane sealant for organic EL display elements, which contains a cycloalkene oxide type alicyclic epoxy compound having a silicone skeleton, measured using an E-type viscometer under conditions of 25°C and 20 rpm is 50 mPa. It is an in-plane sealing agent for organic EL display elements with a temperature of 150 mPa·s or more and 150 mPa·s or less.

Description

In-plane encapsulant for organic EL display elements and encapsulant set for organic EL display elements

The present invention relates to an in-plane encapsulant for organic EL display elements that is excellent in applicability, wet spreadability, and curability. Additionally, the present invention relates to a set of sealants for organic EL display elements comprising a peripheral sealant and the in-plane sealant for organic EL display elements.

An organic electroluminescent display element (organic EL display element) has a thin film structure in which an organic luminescent material layer is sandwiched between a pair of electrodes that face each other. When electrons are injected into this organic light emitting material layer from one electrode and holes are injected from the other electrode, electrons and holes combine within the organic light emitting material layer to produce self-luminescence. Compared to liquid crystal display elements that require a backlight, it has the advantages of good visibility, thinner design, and direct current low voltage driving.

However, such an organic EL display device has a problem in that its luminescent properties deteriorate rapidly when the organic luminescent material layer or electrode is exposed to the outside air, thereby shortening its lifespan. Therefore, for the purpose of increasing the stability and durability of organic EL display elements, encapsulation technology that blocks the organic light-emitting material layer or electrode from moisture and oxygen in the atmosphere has become indispensable.

Patent Document 1 discloses an organic filled layer made of an in-plane encapsulant that covers and seals a laminate having an organic light-emitting material layer, and a moisture-absorbing seal layer made of a peripheral encapsulant containing a moisture absorbent and covering the side surfaces of the organic filled layer. A method of encapsulating an organic EL display element is disclosed by a structure having the same structure. However, when an organic EL display element is sealed using such a configuration using an in-plane encapsulant and a peripheral encapsulant, even if an in-plane encapsulant with excellent applicability and wett spreadability is used, sufficient curing properties cannot be obtained, or the organic EL There was a problem that display defects sometimes occurred in the display element.

Japanese Patent Publication No. 2014-67598

The purpose of the present invention is to provide an in-plane encapsulant for organic EL display elements that is excellent in applicability, wet spreadability, and curability. Additionally, the present invention aims to provide a set of encapsulants for organic EL display elements comprising a peripheral encapsulant and an in-plane encapsulant for organic EL display elements.

The present invention is an in-plane encapsulant for organic EL display elements used by applying it to the inside of a peripheral encapsulant for organic EL display elements containing a moisture absorbent, comprising a curable resin and a cationic polymerization initiator, the curable resin comprising: The viscosity of the entire in-plane sealant for organic EL display elements, which contains a cycloalkene oxide type alicyclic epoxy compound having a silicone skeleton, measured using an E-type viscometer under conditions of 25°C and 20 rpm is 50 mPa. It is an in-plane sealing agent for organic EL display elements with a temperature of 150 mPa·s or more and 150 mPa·s or less.

The present invention is described in detail below.

The present inventor believes that when an organic EL display element is sealed by a configuration using an in-plane encapsulant and a peripheral encapsulant, the reason why the curing property of the in-plane encapsulant is not sufficiently obtained is the moisture absorbent contained in the peripheral encapsulant, It was thought that the moisture absorbent was inhibiting the curing of the in-plane encapsulant. Therefore, as a result of careful study, the present inventor has found that by using a compound having a specific structure as a curable resin used in the in-plane sealant, applicability, wet spreadability, and curability (especially in combination with a peripheral sealant containing a moisture absorbent) can be improved. It was discovered that an in-plane encapsulant for organic EL display elements having excellent curability when used could be obtained, and the present invention was completed. In addition, by using the in-plane encapsulant for organic EL display elements of the present invention, the occurrence of display defects due to the in-plane encapsulant penetrating into the laminate having the organic luminescent material layer can be suppressed, and a display element with excellent display performance can be obtained. You can.

The in-plane sealing agent for organic EL display elements of the present invention contains a curable resin.

The curable resin contains a cycloalkene oxide type alicyclic epoxy compound having a silicone skeleton. By containing the cycloalkene oxide type alicyclic epoxy compound having the silicon skeleton, the in-plane encapsulant for organic EL display elements of the present invention has excellent curability, and further reduces the appearance of dark spots and the like in the resulting organic EL display elements. It becomes possible to suppress defects.

As the cycloalkene oxide type alicyclic epoxy compound having the silicon skeleton, a compound represented by the following formula (1) is preferable because it has superior wett spreadability and curing properties, and is also used in the low-outgassing and organic light-emitting material layer. The compound represented by the following formula (2) is more preferable because it is excellent in the effect of suppressing penetration into the laminate having.

[Formula 1]

In formula (1), n represents an integer of 0 or more and 10 or less.

[Formula 2]

The preferable lower limit of the content of the cycloalkene oxide type alicyclic epoxy compound having the silicone skeleton in 100 parts by weight of the curable resin is 20 parts by weight, and the preferable upper limit is 70 parts by weight. When the content of the cycloalkene oxide type alicyclic epoxy compound having the silicon skeleton is 20 parts by weight or more, the in-plane sealing agent for organic EL display elements obtained has curability and has a greater effect of suppressing display defects in the organic EL display elements obtained. It becomes excellent. When the content of the cycloalkene oxide type alicyclic epoxy compound having the silicon skeleton is 70 parts by weight or less, the resulting in-plane sealing agent for organic EL display elements has better applicability. The more preferable lower limit of the content of the cycloalkene oxide type alicyclic epoxy compound having the silicone skeleton is 40 parts by weight, and the more preferable upper limit is 60 parts by weight.

The curable resin preferably contains another curable resin for the purpose of adjusting the viscosity of the resulting in-plane sealant for organic EL display elements.

Examples of the other curable resins include other epoxy compounds, oxetane compounds, and vinyl ether compounds.

Examples of the other epoxy compounds include compounds represented by the following formula (3), dicyclopentadienedimethanol diglycidyl ether, bisphenol A diglycidyl ether, bisphenol F diglycidyl ether, and hydrogenated Bisphenol A diglycidyl ether, hydrogenated bisphenol F diglycidyl ether, etc. are mentioned.

Examples of the oxetane compound include bis((3-ethyloxetan-3-yl)methyl)ether, phenoxymethyloxetane, 3-ethyl-3-hydroxymethyloxetane, and 3-ethyl- 3-(phenoxymethyl)oxetane, 3-ethyl-3-((2-ethylhexyloxy)methyl)oxetane, 3-ethyl-3-((3-(triethoxysilyl)propoxy)methyl ) oxetane, oxetanyl silsesquioxane, phenol novolak oxetane, 1,4-bis (((3-ethyl-3-oxetanyl) methoxy) methyl) benzene, etc.

Examples of the vinyl ether compounds include benzyl vinyl ether, cyclohexanedimethanol monovinyl ether, dicyclopentadiene vinyl ether, 1,4-butanediol divinyl ether, cyclohexanedimethanol divinyl ether, and diethylene glycol. Divinyl ether, triethylene glycol divinyl ether, dipropylene glycol divinyl ether, tripropylene glycol divinyl ether, etc. are mentioned.

Among them, from the viewpoint of curability and low outgassing properties, the compound represented by the following formula (3) is preferable, and the compound represented by the following formula (4-1) and the compound represented by the following formula (4-2) are more preferable.

[Formula 3]

In formula (3), R ¹ to R ¹⁸ are hydrocarbon groups that may contain a hydrogen atom, a halogen atom, an oxygen atom, or a halogen atom, and may be the same or different. X is a bond, an oxygen atom, an alkylene group having 1 to 5 carbon atoms, an oxycarbonyl group, an alkyleneoxycarbonyl group having 2 to 5 carbon atoms, or a secondary amino group.

[Formula 4]

The in-plane sealing agent for organic EL display elements of the present invention contains a cationic polymerization initiator.

Examples of the cationic polymerization initiator include a thermal cationic polymerization initiator that generates a protonic acid or Lewis acid by heating, a photocationic polymerization initiator that generates a protonic acid or Lewis acid by light irradiation, and an ionic polymerization initiator. The acid-generating type may be sufficient, or the nonionic acid-generating type may be used.

Examples of the thermal cationic polymerization initiator include BF ₄ ^- , PF ₆ ^- , SbF ₆ ^- , or (BX ₄ ) ^- (provided that X represents a phenyl group substituted with at least two fluorine or trifluoromethyl groups) ) A sulfonium salt, phosphonium salt, quaternary ammonium salt, diazonium salt, or iodonium salt using as a counter anion is preferable. Among them, sulfonium salts having the above counter anion are more preferable.

Examples of the sulfonium salt include triphenylsulfonium boron tetrafluoride, triphenylsulfonium antimony hexafluoride, triphenylsulfonium arsenic hexafluoride, tri(4-methoxyphenyl)sulfonium arsenic hexafluoride, and diphenyl(4-phenylthiophenyl)sulfonyl. Arsenic hexafluoride, etc. can be mentioned.

Examples of the phosphonium salt include ethyltriphenylphosphonium antimony hexafluoride, tetrabutylphosphonium antimony hexafluoride, and the like.

Examples of the quaternary ammonium salt include dimethylphenyl (4-methoxybenzyl) ammonium hexafluorophosphate, dimethylphenyl (4-methoxybenzyl) ammonium hexafluoroantimonate, and dimethylphenyl (4-meth Toxybenzyl)ammonium tetrakis(pentafluorophenyl)borate, dimethylphenyl(4-methylbenzyl)ammonium hexafluorophosphate, dimethylphenyl(4-methylbenzyl)ammonium hexafluoroantimonate, dimethylphenyl(4-methyl) Benzyl)ammonium hexafluorotetrakis(pentafluorophenyl)borate, methylphenyldibenzylammonium, methylphenyldibenzylammonium hexafluoroantimonate hexafluorophosphate, methylphenyldibenzylammonium tetrakis(pentafluorophenyl)borate, Phenyltribenzylammonium tetrakis(pentafluorophenyl)borate, dimethylphenyl(3,4-dimethylbenzyl)ammonium tetrakis(pentafluorophenyl)borate, N,N-dimethyl-N-benzylanilinium antimony hexafluoride, N,N-diethyl-N-benzylanilinium boron tetrafluoride, N,N-dimethyl-N-benzylpyridinium antimony hexafluoride, N,N-diethyl-N-benzylpyridinium trifluoromethanesulfonic acid, etc. I can hear it.

Examples of commercially available thermal cationic polymerization initiators include a thermal cationic polymerization initiator manufactured by Sanshin Chemical Industries, Ltd., and a thermal cationic polymerization initiator manufactured by King Industries.

Examples of the thermal cationic polymerization initiator manufactured by Sanshin Chemical Industries, Ltd. include San-Aid SI-60, San-Aid SI-80, San-Aid SI-B3, San-Aid SI-B3A, San-Aid SI-B4, etc. You can.

Examples of the thermal cation polymerization initiator manufactured by King Industries include CXC-1612, CXC-1738, and CXC-1821.

Examples of the anionic moiety of the ionic acid-generating photocationic polymerization initiator include BF ₄ ^- , PF ₆ ^- , SbF ₆ ^- , or (BX ₄ ) ^- (where X is at least 2) and a phenyl group substituted with one or more fluorine or trifluoromethyl groups).

Examples of the ionic acid-generating photocationic polymerization initiator include an aromatic sulfonium salt, an aromatic iodonium salt, an aromatic diazonium salt, an aromatic ammonium salt, or (2,4-cyclo and pentadien-1-yl)((1-methylethyl)benzene)-Fe salt.

Examples of the aromatic sulfonium salt include bis(4-(diphenylsulfonio)phenyl)sulfide bishexafluorophosphate and bis(4-(diphenylsulfonio)phenyl)sulfide bishexafluorophosphate. Roantimonate, bis(4-(diphenylsulfonio)phenyl)sulfide bistetrafluoroborate, bis(4-(diphenylsulfonio)phenyl)sulfide tetrakis(pentafluorophenyl)borate , diphenyl-4-(phenylthio)phenylsulfonium hexafluorophosphate, diphenyl-4-(phenylthio)phenylsulfonium hexafluoroantimonate, diphenyl-4-(phenylthio)phenylsulfonium tetra Fluoroborate, diphenyl-4-(phenylthio)phenylsulfonium tetrakis(pentafluorophenyl)borate, triphenylsulfonium hexafluorophosphate, triphenylsulfonium hexafluoroantimonate, triphenylsulfonium Tetrafluoroborate, triphenylsulfonium tetrakis(pentafluorophenyl)borate, bis(4-(di(4-(2-hydroxyethoxy))phenylsulfonio)phenyl)sulfide bishexafluoro Phosphate, bis(4-(di(4-(2-hydroxyethoxy))phenylsulfonio)phenyl)sulfidebishexafluoroantimonate, bis(4-(di(4-(2-hyde) Roxyethoxy))phenylsulfonio)phenyl)sulfide bistetrafluoroborate, bis(4-(di(4-(2-hydroxyethoxy))phenylsulfonio)phenyl)sulfide tetrakis( Pentafluorophenyl)borate, etc. can be mentioned.

Examples of the aromatic iodonium salt include diphenyl iodonium hexafluorophosphate, diphenyl iodonium hexafluoroantimonate, diphenyl iodonium tetrafluoroborate, and diphenyl iodonium tetrakis (pentafluorocarbonate). Phenyl)borate, bis(dodecylphenyl)iodonium hexafluorophosphate, bis(dodecylphenyl)iodonium hexafluoroantimonate, bis(dodecylphenyl)iodonium tetrafluoroborate, bis(dodecylphenyl)iodonium hexafluoroantimonate )Iodium tetrakis(pentafluorophenyl)borate, 4-methylphenyl-4-(1-methylethyl)phenyliodonium hexafluorophosphate, 4-methylphenyl-4-(1-methylethyl)phenyliodonium hexafluorophosphate Roantimonate, 4-methylphenyl-4-(1-methylethyl)phenyliodonium tetrafluoroborate, 4-methylphenyl-4-(1-methylethyl)phenyliodonium tetrakis(pentafluorophenyl)borate, etc. can be mentioned.

Examples of the aromatic diazonium salt include phenyldiazonium hexafluorophosphate, phenyldiazonium hexafluoroantimonate, phenyldiazonium tetrafluoroborate, and phenyldiazonium tetrakis(pentafluorophenyl)borate. etc. can be mentioned.

Examples of the aromatic ammonium salt include 1-benzyl-2-cyanopyridinium hexafluorophosphate, 1-benzyl-2-cyanopyridinium hexafluoroantimonate, and 1-benzyl-2-cyano. Pyridinium tetrafluoroborate, 1-benzyl-2-cyanopyridinium tetrakis(pentafluorophenyl)borate, 1-(naphthylmethyl)-2-cyanopyridinium hexafluorophosphate, 1-(naph Tylmethyl)-2-cyanopyridinium hexafluoroantimonate, 1-(naphthylmethyl)-2-cyanopyridinium tetrafluoroborate, 1-(naphthylmethyl)-2-cyanopyridinium Tetrakis(pentafluorophenyl)borate, etc. can be mentioned.

The (2,4-cyclopentadien-1-yl)((1-methylethyl)benzene)-Fe salt includes, for example, (2,4-cyclopentadien-1-yl)((1- Methylethyl)benzene)-Fe (II) hexafluorophosphate, (2,4-cyclopentadien-1-yl)((1-methylethyl)benzene)-Fe (II) hexafluoroantimonate, ( 2,4-cyclopentadien-1-yl)((1-methylethyl)benzene)-Fe (II) tetrafluoroborate, (2,4-cyclopentadien-1-yl)((1-methylethyl )Benzene)-Fe (II) tetrakis(pentafluorophenyl)borate, etc.

Among the photocationic polymerization initiators, nonionic acid-generating types include, for example, nitrobenzyl esters, sulfonic acid derivatives, phosphoric acid esters, phenol sulfonic acid esters, diazo naphthoquinone, and N-hydroxyimide sulfonate. there is.

Among the photocationic polymerization initiators, commercially available ones include, for example, a photocationic polymerization initiator manufactured by Midori Chemical Co., Ltd., a photocationic polymerization initiator manufactured by Union Carbide, a photocationic polymerization initiator manufactured by ADEKA, and a photocationic polymerization initiator manufactured by 3M. A photocationic polymerization initiator manufactured by BASF, a photocationic polymerization initiator manufactured by Rhodia, etc. may be mentioned.

Examples of the photocationic polymerization initiator manufactured by Midori Chemical Co., Ltd. include DTS-200.

Examples of the photocationic polymerization initiator manufactured by Union Carbide include UVI6990 and UVI6974.

Examples of the photocationic polymerization initiator manufactured by ADEKA include SP-150 and SP-170.

Examples of the photocationic polymerization initiator manufactured by 3M include FC-508 and FC-512.

Examples of the photocationic polymerization initiator manufactured by BASF include IRGACURE290.

Examples of the photocationic polymerization initiator manufactured by Rhodia include PI2074 and the like.

Regarding the materials described in both the thermal cation polymerization initiator and the photo cation polymerization initiator, they may be used as the thermal cation polymerization initiator or as the photo cation polymerization initiator.

Among the above-mentioned cationic polymerization initiators, quaternary ammonium salts whose counter anions are borate-based (hereinafter also referred to as “borate-based quaternary ammonium salts”) are preferably used. The counter anion of the borate-based quaternary ammonium salt is preferably BF ₄ ^- or (BX ₄ ) ^- (where X represents a phenyl group substituted with at least two fluorine or trifluoromethyl groups).

The content of the cationic polymerization initiator has a preferable lower limit of 0.05 parts by weight and a preferable upper limit of 10 parts by weight with respect to 100 parts by weight of the cationically polymerizable compound. When the content of the cationic polymerization initiator is within this range, the obtained in-plane sealing agent for organic EL display elements has better curability and storage stability. The more preferable lower limit of the content of the cationic polymerization initiator is 0.1 parts by weight, and the more preferable upper limit is 5 parts by weight.

The in-plane sealing agent for organic EL display elements of the present invention may contain a sensitizer. The sensitizer has a role in further improving the polymerization initiation efficiency of the photocationic polymerization initiator and further promoting the curing reaction of the in-plane encapsulant for organic EL display elements of the present invention.

Examples of the sensitizer include anthracene-based compounds, thioxanthone-based compounds, 2,2-dimethoxy-1,2-diphenylethan-1-one, benzophenone, 2,4-dichlorobenzophenone, o -Methyl benzoylbenzoate, 4,4'-bis(dimethylamino)benzophenone, 4-benzoyl-4'-methyldiphenyl sulfide, etc. are mentioned.

Examples of the anthracene-based compound include 9,10-dibutoxyanthracene.

Examples of the thioxanthone-based compound include 2,4-diethylthioxanthone.

The content of the sensitizer has a preferable lower limit of 0.05 parts by weight and a preferable upper limit of 3 parts by weight with respect to 100 parts by weight of the curable resin. When the content of the sensitizer is 0.05 parts by weight or more, the sensitizing effect is more exhibited. When the content of the sensitizer is 3 parts by weight or less, light can be transmitted to the deep part without excessive absorption. The more preferable lower limit of the content of the sensitizer is 0.1 part by weight, and the more preferable upper limit is 1 part by weight.

The in-plane sealing agent for organic EL display elements of the present invention may contain a thermosetting agent.

Examples of the thermal curing agent include hydrazide compounds, imidazole derivatives, acid anhydrides, dicyandiamide, guanidine derivatives, modified aliphatic polyamines, and addition products of various amines and epoxy resins.

Examples of the hydrazide compounds include 1,3-bis(hydrazinocarboethyl)-5-isopropylhydantoin, sebacic acid dihydrazide, isophthalic acid dihydrazide, adipic acid dihydrazide, and malone. Sandihydrazide, etc. can be mentioned.

Examples of the imidazole derivative include 1-cyanoethyl-2-phenylimidazole, N-(2-(2-methyl-1-imidazolyl)ethyl)urea, and 2,4-diamino. -6-(2'-Methylimidazolyl-(1'))-ethyl-s-triazine, N,N'-bis(2-methyl-1-imidazolylethyl)urea, N,N'- (2-methyl-1-imidazolylethyl)-adipamide, 2-phenyl-4-methyl-5-hydroxymethylimidazole, 2-phenyl-4, 5-dihydroxymethylimidazole, etc. can be mentioned.

Examples of the acid anhydride include tetrahydrophthalic anhydride, ethylene glycol bis(anhydrotrimellitate), and the like.

These thermosetting agents may be used individually, or two or more types may be used together.

Examples of commercially available thermal curing agents include a thermal curing agent manufactured by Nippon Fine-Chem, a thermal curing agent manufactured by Otsuka Chemical Company, and a thermal curing agent manufactured by Ajinomoto Fine Techno.

Examples of the thermal curing agent manufactured by Nippon Finechem Co., Ltd. include SDH and the like.

Examples of the thermal curing agent manufactured by Otsuka Chemical Co., Ltd. include ADH.

Examples of the heat curing agent manufactured by Ajinomoto Fine Techno Co., Ltd. include Amicure VDH, Amicure VDH-J, and Amicure UDH.

The content of the thermosetting agent has a preferable lower limit of 0.5 parts by weight and a preferable upper limit of 30 parts by weight based on 100 parts by weight of the cationically polymerizable compound. When the content of the thermosetting agent is 0.5 parts by weight or more, the obtained in-plane sealing agent for organic EL display elements becomes more excellent in thermosetting properties. When the content of the thermosetting agent is 30 parts by weight or less, the obtained in-plane sealing agent for organic EL display elements has better storage stability. The more preferable lower limit of the content of the heat curing agent is 1 part by weight, and the more preferable upper limit is 15 parts by weight.

It is preferable that the in-plane sealing agent for organic EL display elements of the present invention contains a stabilizer. By containing the above stabilizer, the in-plane sealing agent for organic EL display elements of the present invention has more excellent storage stability.

Examples of the stabilizer include amine-based compounds such as benzylamine and aminophenol-type epoxy resins.

The content of the stabilizer has a preferable lower limit of 0.001 parts by weight and a preferable upper limit of 2 parts by weight based on 100 parts by weight of the cationically polymerizable compound. When the content of the stabilizer is within this range, the obtained in-plane sealing agent for organic EL display elements has better storage stability while maintaining excellent curability. The more preferable lower limit of the content of the stabilizer is 0.005 parts by weight, and the more preferable upper limit is 1 part by weight.

The in-plane sealing agent for organic EL display elements of the present invention may contain a silane coupling agent. The silane coupling agent has a role in improving the adhesion between the in-plane encapsulant for organic EL display elements of the present invention and the substrate.

Examples of the silane coupling agent include 3-aminopropyltrimethoxysilane, 3-mercaptopropyltrimethoxysilane, 3-glycidoxypropyltrimethoxysilane, 3-isocyanatepropyltrimethoxysilane, etc. can be mentioned. These silane coupling agents may be used individually, or two or more types may be used together.

The content of the silane coupling agent has a preferable lower limit of 0.1 parts by weight and a preferable upper limit of 10 parts by weight based on 100 parts by weight of the cationically polymerizable compound. When the content of the silane coupling agent is within this range, the effect of improving the adhesion of the resulting in-plane sealing agent for organic EL display elements is more excellent while preventing bleed-out of the excess silane coupling agent. The more preferable lower limit of the content of the silane coupling agent is 0.5 parts by weight, and the more preferable upper limit is 5 parts by weight.

The in-plane sealing agent for organic EL display elements of the present invention may contain a surface modifier within a range that does not impair the purpose of the present invention. By containing the surface modifier, the flatness of the coating film of the in-plane sealant for organic EL display elements of the present invention can be improved.

Examples of the surface modifier include surfactants and leveling agents.

Examples of the surface modifier include silicone-based, acrylic-based, and fluorine-based ones.

Examples of commercially available surface modifiers include a surface modifier manufactured by Big Chemie Japan, a surface modifier manufactured by Kusumoto Chemical Company, and a surface modifier manufactured by AGC Semi Chemicals.

Examples of the surface modifiers manufactured by Big Chemie Japan include BYK-300, BYK-302, and BYK-331.

Examples of the surface modifier manufactured by Kusumoto Chemical Company include UVX-272.

Examples of the surface modifier manufactured by AGC Semichemical Company include Surfron S-611.

The in-plane encapsulant for organic EL display elements of the present invention is a compound or ion that reacts with the acid generated in the in-plane encapsulant for organic EL display elements in order to improve the durability of the device electrode within a range that does not impair the purpose of the present invention. An exchange resin may be contained.

Compounds that react with the generated acid include substances that neutralize the acid, for example, carbonate or hydrogen carbonate of an alkali metal, or carbonate or hydrogen carbonate of an alkaline earth metal. Specifically, for example, calcium carbonate, calcium bicarbonate, sodium carbonate, sodium bicarbonate, etc. are used.

As the ion exchange resin, cation exchange type, anion exchange type, and both ion exchange type can be used, but cation exchange type or both ion exchange type that can adsorb chloride ions are particularly preferred.

In addition, the in-plane encapsulant for organic EL display elements of the present invention may contain a curing retardant, reinforcing agent, softener, plasticizer, viscosity modifier, ultraviolet absorber, antioxidant, etc., as necessary, within the range that does not impair the purpose of the present invention. It may contain various known additives.

It is preferable that the in-plane sealing agent for organic EL display elements of the present invention does not contain a solvent from the viewpoint of further suppressing the generation of outgassing. The in-plane sealing agent for organic EL display elements of the present invention can be excellent in applicability even if it does not contain the solvent.

The method for producing the in-plane encapsulant for organic EL display elements of the present invention includes, for example, using a mixer such as a homodisper, homomixer, universal mixer, planetary mixer, kneader, or three roll, to achieve curing properties. A method of mixing a resin, a cationic polymerization initiator, and additives such as a stabilizer or a silane coupling agent added as needed can be mentioned.

The in-plane sealing agent for organic EL display elements of the present invention has a lower limit of total viscosity of 50 mPa·s and an upper limit of 150 mPa·s as measured under conditions of 25°C and 20 rpm using an E-type viscometer. When the viscosity is within this range, the obtained in-plane sealing agent for organic EL display elements has excellent applicability and is particularly suitable as an in-plane sealing agent for organic EL display elements. The preferable lower limit of the viscosity is 60 mPa·s, the preferable upper limit is 140 mPa·s, the more preferable lower limit is 80 mPa·s, and the more preferable upper limit is 120 mPa·s.

In addition, as the E-type viscometer, for example, VISCOMETER TV-22 (manufactured by Toki Sangyo Co., Ltd.) can be used, and measurement can be performed with a CP1 cone plate.

The surface tension of the in-plane encapsulant for organic EL display elements of the present invention has a preferable lower limit of 15 mN/m and a preferable upper limit of 45 mN/m. When the surface tension is within this range, the resulting in-plane sealing agent for organic EL display elements has excellent applicability and is particularly suitable as an in-plane sealing agent for organic EL display elements. A more preferable lower limit of the surface tension is 20 mN/m, and a more preferable upper limit is 35 mN/m.

In addition, in this specification, the surface tension can be measured by a dynamic wettability tester at 25°C.

The in-plane encapsulant for organic EL display elements of the present invention is used by applying it to the inside of a peripheral encapsulant for organic EL display elements containing a moisture absorbent.

A set of encapsulants for organic EL display elements used to encapsulate organic EL display elements, comprising a peripheral encapsulant for sealing the peripheral portion of an organic EL display element and a laminate having an organic light-emitting material layer inside the peripheral encapsulant. It consists of an in-plane encapsulant that is coated and sealed, and the peripheral encapsulant contains a curable resin, a polymerization initiator, and a moisture absorbent, and the in-plane encapsulant is an in-plane encapsulant for an organic EL display device of the present invention. A sealant set is also one of the present inventions.

The peripheral encapsulant contains a curable resin.

The curable resin used in the peripheral encapsulant includes a cationically polymerizable compound having a cationic polymerizable group such as an epoxy group, oxetanyl group, or vinyl ether group, or a radical having a radical polymerizable group such as a (meth)acryloyl group. Polymerizable compounds can be mentioned.

Cationically polymerizable compounds used in the peripheral encapsulant include epoxy resins having a bisphenol skeleton, epoxy resins having a novolac skeleton, epoxy resins having a naphthalene skeleton, and dicyclopolymers, from the viewpoint of easy viscosity adjustment. At least one type of epoxy resin selected from the group consisting of epoxy resins having a pentadiene skeleton is preferable. Among them, an epoxy resin having a bisphenol skeleton is more preferable, and a bisphenol F-type epoxy resin is more preferable.

Moreover, from the viewpoint of suppressing the generation of outgas, the peripheral sealing agent preferably contains a compound represented by the formula (3) as the cationically polymerizable compound, and is represented by the formula (4-1) It is preferable to contain a compound and/or a compound represented by the above formula (4-2).

As the radically polymerizable compound, a (meth)acrylic compound is preferably used.

Examples of the (meth)acrylic compound include epoxy (meth)acrylate, (meth)acrylic acid ester compound, and urethane (meth)acrylate. Among them, epoxy (meth)acrylate is preferable.

In addition, in this specification, the above-mentioned “(meth)acrylic” refers to acrylic or methacrylic, the above-mentioned “(meth)acrylate” refers to acrylate or methacrylate, and the above-mentioned “epoxy (meth)acrylate”. 」 indicates that it is a compound obtained by reacting all the epoxy groups in the epoxy resin with (meth)acrylic acid.

Among the above-mentioned epoxy (meth)acrylates, commercially available ones include, for example, epoxy (meth)acrylate manufactured by Daicel Allnex, epoxy (meth)acrylate manufactured by Shinnakamura Chemical Industries, Ltd., and Kyoeisha Chemical Company. Epoxy (meth)acrylate manufactured by Nagase Chemtex Co., Ltd., and epoxy (meth)acrylate manufactured by Nagase Chemtex Corporation.

Examples of the epoxy (meth)acrylate manufactured by Daicel Allnex include EBECRYL860, EBECRYL3200, EBECRYL3201, EBECRYL3412, EBECRYL3600, EBECRYL3700, EBECRYL3701, EBECRYL3702, EBECRYL3703, and EBECRYL37. 08, EBECRYL3800, EBECRYL6040, EBECRYL RDX63182, etc. I can hear it.

Examples of the epoxy (meth)acrylate manufactured by Shinnakamura Chemical Co., Ltd. include EA-1010, EA-1020, EA-5323, EA-5520, EA-CHD, and EMA-1020.

The epoxy (meth)acrylate manufactured by Kyoeisha Chemical Co., Ltd. includes, for example, epoxy ester M-600A, epoxy ester 40EM, epoxy ester 70PA, epoxy ester 200PA, epoxy ester 80MFA, epoxy ester 3002M, epoxy ester 3002A, Examples include epoxy ester 1600A, epoxy ester 3000M, epoxy ester 3000A, epoxy ester 200EA, and epoxy ester 400EA.

Examples of the epoxy (meth)acrylate manufactured by Nagase Chemtex Co., Ltd. include Denachol Acrylate DA-141, Denacol Acrylate DA-314, and Denacol Acrylate DA-911.

The peripheral encapsulant preferably contains a resin having a polyisobutylene skeleton from the viewpoints of transparency, moisture resistance, and adhesiveness, and the resin having a polyisobutylene skeleton and the radically polymerizable compound are combined. It is more preferable to use them in combination.

The resin having the polyisobutylene skeleton includes, for example, a homopolymer of isobutene, an isobutylene/isoprene copolymer obtained by copolymerizing isobutene and about several weight percent of isoprene relative to the isobutene, Examples include so-called butyl rubber, which is formed by crosslinking the double bond site derived from isoprene in the isobutylene/isoprene copolymer.

The peripheral encapsulant contains a polymerization initiator.

As the polymerization initiator used in the peripheral sealing agent, a cationic polymerization initiator or a radical polymerization initiator can be used.

Examples of the cationic polymerization initiator used in the peripheral sealing agent include those similar to the cationic polymerization initiator described above in the in-plane sealing agent for organic EL display elements of the present invention.

As the radical polymerization initiator, a photo radical polymerization initiator or a thermal radical polymerization initiator can be used.

Examples of the photo radical polymerization initiator include benzophenone-based compounds, acetophenone-based compounds, acylphosphine oxide-based compounds, titanocene-based compounds, oxime ester-based compounds, benzoin ether-based compounds, benzyl, thioxanthone, etc. can be mentioned.

The photo radical polymerization initiator specifically includes, for example, 1-hydroxycyclohexylphenyl ketone, 2-benzyl-2-dimethylamino-1-(4-morpholinophenyl)butanone, 1,2- (dimethylamino)-2-((4-methylphenyl)methyl)-1-(4-(4-morpholinyl)phenyl)-1-butanone, 2,2-dimethoxy-1,2-diphenylethane -1-one, bis(2,4,6-trimethylbenzoyl)phenylphosphine oxide, 2-methyl-1-(4-methylthiophenyl)-2-morpholinopropan-1-one, 1-(4 -(2-hydroxyethoxy)-phenyl)-2-hydroxy-2-methyl-1-propan-1-one, 1-(4-(phenylthio)phenyl)-1,2-octanedione 2- (O-benzoyloxime), 2,4,6-trimethylbenzoyldiphenylphosphine oxide, benzoin methyl ether, benzoin ethyl ether, benzoin isopropyl ether, etc.

Examples of the thermal radical polymerization initiator include peroxides and azo compounds.

Examples of commercially available thermal radical polymerization initiators include a thermal radical polymerization initiator manufactured by Nichiyu Corporation, a thermal radical polymerization initiator manufactured by Fujifilm Wako Pure Chemical Industries, Ltd., and the like.

Examples of the thermal radical polymerization initiator manufactured by Nichiyu Corporation include perbutyl O, perhexyl O, and perbutyl PV.

Examples of the thermal radical polymerization initiator manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. include V-30, V-65, V-501, V-601, and VPE-0201.

The content of the polymerization initiator used in the peripheral sealing agent has a preferable lower limit of 0.1 parts by weight and a preferable upper limit of 10 parts by weight with respect to 100 parts by weight of the curable resin. When the content of the polymerization initiator used in the peripheral sealing agent is within this range, the resulting peripheral sealing agent becomes more excellent in curability, storage stability, and barrier properties. The more preferable lower limit of the content of the polymerization initiator used in the peripheral encapsulant is 0.5 parts by weight, and the more preferable upper limit is 5 parts by weight.

The said peripheral sealing agent may contain a thermosetting agent. Examples of the thermal curing agent used in the peripheral sealing agent include those similar to the thermal curing agent described above in the in-plane sealing agent for organic EL display elements of the present invention.

The peripheral encapsulant contains a moisture absorbent. By containing the moisture absorbent, the peripheral encapsulant has excellent barrier properties.

The encapsulant set for organic EL display elements of the present invention uses the encapsulant containing the moisture absorbent as the peripheral encapsulant, but uses the encapsulant for organic EL display elements of the present invention as the inner encapsulant, so these can be combined. Even if used, the in-plane sealant can be sufficiently cured, and occurrence of display defects in the resulting organic EL display element can be suppressed.

The preferred lower limit of the water absorption rate of the moisture absorbent is 10% by weight. When the water absorption rate of the moisture absorbent is 10% by weight or more, the resulting peripheral encapsulant has more excellent barrier properties. A more preferable lower limit of the water absorption rate of the moisture absorbent is 20% by weight.

Additionally, there is no particular upper limit to the preferable water absorption rate of the moisture absorbent, but the practical upper limit is 50% by weight.

In addition, the above “water absorption rate” means the rate of change in weight when a high-temperature, high-humidity test is conducted in which the material is left for 24 hours in an atmosphere of 85°C and 85% humidity. Specifically, when the weight before the high-temperature, high-humidity test (85°C - 85%, 24 hours) is set to W ₁ and the weight after the high-temperature, high-humidity test is set to W ₂ , the weight is calculated using the following formula (I).

Absorption rate (% by weight) = ((W ₂ - W ₁ )/W ₁ ) × 100 (I)

Examples of materials constituting the moisture absorbent include oxides of alkaline earth metals such as calcium oxide, strontium oxide, and barium oxide, magnesium oxide, and molecular sieve. Among them, from the viewpoint of water absorption, oxides of alkaline earth metals are preferable, and calcium oxide is more preferable.

The content of the moisture absorbent in the peripheral encapsulant has a preferable lower limit of 5 parts by weight and a preferable upper limit of 60 parts by weight with respect to 100 parts by weight of the curable resin. When the content of the moisture absorbent in the peripheral sealant is within this range, the resulting peripheral sealant has excellent barrier properties and is excellent in the effect of suppressing panel peeling. The more preferable lower limit of the content of the moisture absorbent in the peripheral encapsulant is 10 parts by weight, and the more preferable upper limit is 40 parts by weight.

The peripheral encapsulant may contain other fillers in addition to the moisture absorbent within a range that does not impair the purpose of the present invention for the purpose of improving adhesiveness, etc.

Examples of the other fillers include inorganic fillers such as silica, talc, and alumina, and organic fillers such as polyester fine particles, polyurethane fine particles, vinyl polymer fine particles, and acrylic polymer fine particles. Among them, talc is preferable.

The peripheral encapsulant may contain additives such as sensitizers, stabilizers, silane coupling agents, surface modifiers, ion exchange resins, curing retarders, reinforcing agents, softeners, plasticizers, viscosity modifiers, ultraviolet absorbers, and antioxidants. These additives include the same additives as those described above in the in-plane sealing agent for organic EL display elements of the present invention.

It is preferable that the peripheral sealing agent does not contain a solvent from the viewpoint of further suppressing the generation of outgassing. The peripheral sealant can be made to have excellent applicability even if it does not contain the solvent.

A method of manufacturing the peripheral encapsulant includes, for example, using a mixer such as a homodisper, homomixer, universal mixer, planetary mixer, kneader, or three roll, a curable resin, a polymerization initiator, Examples include a method of mixing a moisture absorbent and additives such as a silane coupling agent added as needed.

It is preferable that the said peripheral sealing agent is a paste whose viscosity measured under 25 degreeC conditions using an E-type viscometer is 150 Pa·s or more and 500 Pa·s or less. When the viscosity of the peripheral encapsulant is within this range, both the applicability and the dispersibility of the moisture absorbent become more excellent. The more preferable lower limit of the viscosity of the peripheral encapsulant is 200 Pa·s, and the more preferable upper limit is 400 Pa·s. Additionally, when a solvent is used to adjust the viscosity of the peripheral encapsulant, it becomes difficult to suppress the generation of outgassing.

In addition, the viscosity of the peripheral encapsulant is appropriately determined from the optimal torque number in each viscosity region by using a VISCOMETER TV-22 (manufactured by Toki Sangyo Co., Ltd.) as an E-type viscometer and using a cone plate of CP1, for example. It can be measured by selecting a rotation speed of ~ 100 rpm.

According to the present invention, it is possible to provide an in-plane sealant for organic EL display elements that is excellent in applicability, wet spreadability, and curability. Moreover, according to the present invention, it is possible to provide a set of sealants for organic EL display elements consisting of a peripheral sealant and the in-plane sealant for organic EL display elements.

The present invention will be described in more detail below with reference to examples, but the present invention is not limited to these examples.

(Examples 1 to 8, Comparative Examples 1 to 5)

According to the mixing ratios shown in Tables 1 to 3, each material was stirred and mixed uniformly at a stirring speed of 3000 rpm using a stirring mixer (“AR-250” manufactured by Thinky), and Examples 1 to 8 and Comparative Examples were obtained. In-plane encapsulants for organic EL display elements 1 to 5 were produced.

In addition, “X22-163” in the table is a compound represented by the following formula (5).

[Formula 5]

＜Evaluation＞

The following evaluation was performed on each in-plane encapsulant for organic EL display elements obtained in Examples and Comparative Examples. The results are shown in Tables 1 to 3.

(1) Viscosity

For each of the in-plane encapsulants for organic EL display elements obtained in the examples and comparative examples, the viscosity was measured at 25°C and 20 rpm using an E-type viscometer (“VISCOMETER TV-22”, manufactured by Toki Sangyo Co., Ltd.). Measured.

(2) Wet spreadability

Using a pipette, 0.1 ml of each in-plane sealant for organic EL display elements obtained in Examples and Comparative Examples was applied onto a glass substrate, and the diffused diameter was measured 1 minute later. Wet spreadability was evaluated by assigning “○” when the diameter was 15 mm or more, “△” when it was 10 mm or more and less than 15 mm, and “×” when it was less than 10 mm.

(3) Prevention of seepage

Each of the in-plane encapsulants for organic EL display elements obtained in Examples and Comparative Examples was applied onto glass substrates having holes of different sizes. As a result, the case in which the encapsulant did not penetrate into the 2 ㎛ hole was marked as “○”; the case in which penetration was not confirmed in the 0.5 ㎛ hole, but penetration was confirmed in the 2 ㎛ hole as “△”; the 0.5 ㎛ hole was marked as “△.” Cases where seepage was confirmed even through the holes were set as “×”, and the seepage prevention property was evaluated.

(4) Low out gasiness

300 mg of each in-plane sealant for organic EL display elements obtained in the examples and comparative examples was weighed and sealed in a vial, and then cured by heating at 100°C for 30 minutes. Additionally, this vial was heated in a constant temperature oven at 85°C for 100 hours, and the vaporized components in the vial were measured using a gas chromatograph mass spectrometer (JMS-Q1050, manufactured by JEOL Co., Ltd.).

Low-out gas properties were evaluated by setting the case where the amount of vaporized component was less than 50 ppm as “○”, the case where it was 50 ppm to less than 100 ppm as “△”, and the case where it was 100 ppm or more as “×”.

(5) Curability of in-plane encapsulant and display performance of organic EL display element

(Production of a substrate on which a laminate having an organic light-emitting material layer is disposed)

An ITO electrode was formed to a thickness of 1000 Å on a glass substrate (length 45 mm, width 45 mm, thickness 0.7 mm), which was used as a substrate. The substrate was ultrasonically cleaned with acetone, aqueous alkaline solution, ion-exchanged water, and isopropyl alcohol for 15 minutes each, then cleaned with boiled isopropyl alcohol for 10 minutes, and further washed with UV-ozone cleaner (manufactured by Nippon Laser Electronics). The previous treatment was performed with “NL-UV253”).

Next, this substrate was fixed to the substrate folder of the vacuum evaporation device, and 200 mg of N,N'-di(1-naphthyl)-N,N'-diphenylbenzidine (α-NPD) was added to the unglazed crucible. 200 mg of tris(8-quinolinolatto)aluminum (Alq ₃ ) was placed in another different unglazed crucible, and the pressure inside the vacuum chamber was reduced to 1×10 ^-4 Pa. Afterwards, the crucible containing α-NPD was heated, α-NPD was deposited on the substrate at a deposition rate of 15 Å/s, and a hole transport layer with a film thickness of 600 Å was formed. Next, the crucible containing Alq ₃ was heated, and an organic light-emitting material layer with a film thickness of 600 Å was formed at a deposition rate of 15 Å/s. After that, the substrate on which the hole transport layer and the organic light-emitting material layer were formed was transferred to another vacuum evaporation apparatus, and 200 mg of lithium fluoride was placed in a tungsten resistance heating boat in this vacuum evaporation apparatus, and 1.0 g of aluminum wire was placed in another tungsten boat. Afterwards, the pressure inside the evaporator of the vacuum evaporation device was reduced to 2 × 10 ^-4 Pa to form a 5 Å film of lithium fluoride at a deposition rate of 0.2 Å/s, and then a 1000 Å film of aluminum was formed at a rate of 20 Å/s. The inside of the evaporator was returned to normal pressure with nitrogen, and the substrate on which the laminate having a 10 mm × 10 mm organic light-emitting material layer was disposed was taken out.

(Preparation of peripheral encapsulant)

The curable resin, photocationic polymerization initiator, moisture absorbent, and silane coupling agent were uniformly mixed at a stirring speed of 3000 rpm using a Homo Disper type stirring mixer (“Homo Disper L type” manufactured by Primix). By stirring and mixing, a peripheral encapsulant was prepared.

The curable resin includes 65 parts by weight of novolak-type epoxy resin (“D.E.N.431” manufactured by Dow Chemical Company), 20 parts by weight of bisphenol F-type epoxy resin (“EPICLON EXA-830LVP” manufactured by DIC Corporation), and 15 parts by weight of dicyclopentadiene type epoxy resin (“EPICLON HP-7200” manufactured by DIC) was used.

As the photocationic polymerization initiator, 1 part by weight of an aromatic sulfonium salt (“DTS-200” manufactured by Midori Chemical Co., Ltd.) was used.

As the moisture absorbent, 20 parts by weight of calcium oxide (“Quicklime J1P” manufactured by Yoshizawa Lime Industry Co., Ltd.) was used.

As the silane coupling agent, 1.5 parts by weight of 3-glycidoxypropyltrimethoxysilane (KBM-403, manufactured by Shin-Etsu Chemical Co., Ltd.) was used.

With respect to the obtained peripheral sealant, the viscosity measured at 25°C using an E-type viscometer ("VISCOMETER TV-22", manufactured by Toki Sangyo Co., Ltd.) was 250 Pa·s.

(Production of organic EL display elements)

The prepared peripheral encapsulant was applied to the outer periphery of the substrate on which the laminate was placed so that the line width was 6 mm, and the in-plane encapsulant for each organic EL display element obtained in the examples and comparative examples was applied to the inside so as to cover the entire laminate. After that, another glass substrate (length 45 mm, width 45 mm, thickness 0.7 mm) was overlapped. Afterwards, using a high-pressure mercury lamp, ultraviolet rays with a wavelength of 365 nm are irradiated at an irradiation dose of 3000 mJ/cm2, and further heated at 100°C for 30 minutes to cure the in-plane encapsulant and the surrounding encapsulant to produce an organic EL display element. did. In addition, regarding the in-plane sealing agent for organic EL display elements obtained in Example 4, the in-plane sealing agent and the peripheral sealing agent were cured without heating. In addition, the organic EL display element used for the evaluation of "(curability of in-plane encapsulant)" below was produced in the same manner.

(Curability of in-plane encapsulant)

For the obtained organic EL display element, the curing rate of the in-plane encapsulant was measured at the interface between the peripheral encapsulant and the in-plane encapsulant. As a result, the curing property of the in-plane sealant was evaluated by setting the case where the cure rate was 80% or more as “○”, the case where the cure rate was 50% or more but less than 80% as “△”, and the case where the cure rate was less than 50% as “×”.

(Display performance of organic EL display element)

After the obtained organic EL display element was exposed to an environment of 85°C and 85%RH for 1000 hours, a voltage of 10 V was applied to visually inspect the luminescence state of the organic EL display element (presence or absence of dark spots and extinction around the pixel). observed. The organic EL display element is designated as “○” when there is no dark spot or ambient light and emits light evenly, “△” when a slightly dark spot or ambient light is confirmed, and “×” when the non-light emitting area is significantly enlarged. The display performance was evaluated.

According to the present invention, it is possible to provide an in-plane sealant for organic EL display elements that is excellent in applicability, wet spreadability, and curability. Moreover, according to the present invention, it is possible to provide a set of sealants for organic EL display elements consisting of a peripheral sealant and the in-plane sealant for organic EL display elements.

Claims (6)

An in-plane encapsulant for organic EL display elements used by applying it to the inside of a peripheral encapsulant for organic EL display elements containing a moisture absorbent,
Contains a curable resin and a cationic polymerization initiator,
The curable resin contains a cycloalkene oxide type alicyclic epoxy compound having a silicone skeleton,
An organic EL display element characterized in that the viscosity of the entire in-plane encapsulant for an organic EL display element, measured using an E-type viscometer under conditions of 25°C and 20 rpm, is 50 mPa·s or more and 150 mPa·s or less. In-plane encapsulant. According to claim 1,
The cycloalkene oxide type alicyclic epoxy compound having the silicon skeleton is an in-plane sealing agent for organic EL display elements, which is a compound represented by the following formula (1).

In formula (1), n represents an integer of 0 to 10. According to claim 2,
The cycloalkene oxide type alicyclic epoxy compound having the silicon skeleton is an in-plane sealing agent for organic EL display elements, which is a compound represented by the following formula (2).

The method of claim 1, 2 or 3,
An in-plane sealant for organic EL display elements, wherein the content of the cycloalkene oxide type alicyclic epoxy compound having the silicone skeleton in 100 parts by weight of the curable resin is 20 parts by weight or more and 70 parts by weight or less. The method of claim 1, 2 or 3,
The curable resin is an in-plane sealant for organic EL display elements containing a compound represented by the following formula (3).

In formula (3), R ¹ to R ¹⁸ are hydrocarbon groups that may contain a hydrogen atom, a halogen atom, an oxygen atom, or a halogen atom, and may be the same or different. X is a bond, an oxygen atom, an alkylene group having 1 to 5 carbon atoms, an oxycarbonyl group, an alkyleneoxycarbonyl group having 2 to 5 carbon atoms, or a secondary amino group. A set of encapsulants for organic EL display elements used to encapsulate organic EL display elements,
It consists of a peripheral encapsulant that seals the peripheral portion of the organic EL display element, and an in-plane encapsulant that covers and seals the laminate having the organic luminescent material layer inside the peripheral encapsulant,
The peripheral encapsulant contains a curable resin, a polymerization initiator, and a moisture absorbent,
The said in-plane sealing agent is a sealing agent set for organic EL display elements which is the in-plane sealing agent for organic EL display elements of Claim 1, 2, or 3.