A sheet for forming a sealing layer, and a member in which multiple light-emitting elements are sealed.

Abstract

The objective is to provide a sheet for forming a sealing layer that is excellent not only in embedding properties but also in water vapor barrier properties, and that makes the existence of boundaries between components less noticeable, thereby providing a sealed component with excellent migration resistance and boundary invisibility. [Solution] A sealing layer forming sheet for filling the gaps between light-emitting elements in a display using multiple light-emitting elements as a light source, and covering the light-emitting side of the multiple light-emitting elements, The sealing layer forming sheet is arranged in the order of first film 2, sealing layer precursor α, and second film 5, and the sealing layer precursor α has a water vapor permeability of 100 [g / (m²] 2 ·twenty four A sheet for forming a sealing layer, wherein the sealing layer precursor α has a moisture absorption rate of 1.5% by mass or less (less than 1.5 hours), and the sealing layer precursor α comprises a colorless resin composition layer 3 for embedding with a refractive index of 1.51±0.03, and a water vapor barrier layer 4 with a refractive index of 1.53±0.03.

Description

Technical Field

[0001] The present disclosure relates to a sheet for forming a sealing layer and a member in which a plurality of light-emitting elements are sealed. Specifically, it relates to a sheet for forming a sealing layer that can be suitably used for sealing a plurality of micro LED elements, and a member in which a plurality of micro LED elements are sealed.

Background Art

[0002] In recent years, displays have been actively developed using various light-emitting elements for further performance improvement. Specifically, various display specifications such as backlight-type displays using liquid crystals, quantum dots, etc., displays using self-emitting elements such as mini / micro LEDs and organic ELs, plasma displays, electrophoretic displays, etc. are being studied, and are being widely considered for use in large display applications such as signage and TVs over 40 inches and 50 inches, as well as small sizes such as tablets, personal computers, smartphones, wearable devices, etc. In particular, the development of LED-based displays is progressing day by day, and Patent Documents 1 to 4 describe sealing sheets for sealing a plurality of LED elements.

Prior Art Documents

Patent Documents

[0003]

Patent Document 1

Patent Document 2

Patent Document 3

Patent Document 4

Summary of the Invention

Problems to be Solved by the Invention

[0004] In recent years, with the progress of miniaturization, especially in micro-sized LED elements, when the distance between LED elements becomes narrower, there is a problem that finer and denser circuits are more likely to corrode due to water vapor and ion precipitation (hereinafter also referred to as migration). In addition, a display is formed by arranging a large number of members in which a plurality of light-emitting elements are sealed, and there is a problem that the boundary between the members becomes visible and the display performance as a display deteriorates.

[0005] The present disclosure has been made in view of the above problems, and provides a sheet for forming a sealing layer for sealing a micro-LED element, which is excellent not only in embedding property but also in water vapor barrier property, and makes the existence of the boundary between members difficult to see. It is an object to provide a sealed member excellent in migration resistance and invisibility of the boundary.

Means for Solving the Problems

[0006] As a result of intensive studies by the present inventors, it has been found that a micro-LED member capable of solving the above problems can be manufactured with high quality and efficiency by the following sealing layer forming sheet, and the present invention of [1] to [7] below has been completed.

[0007] [1] A sheet for forming a sealing layer for filling between light-emitting elements for a display using a plurality of light-emitting elements as light sources and covering the surfaces on the side where the light of the plurality of light-emitting elements is emitted, The sealing layer forming sheet has a first film 2, a sealing layer precursor α, and a second film 5 arranged in this order, The sealing layer precursor α has a water vapor permeability of less than 100 [g / (m ·24 hours)], and a moisture absorption rate of 1.5 mass% or less, The sealing layer precursor α has a refractive index of 1.51 ± 0.03 and a water vapor permeability of 100 [g / (m 2 ·24 hours)] or more, a colorless resin composition layer 3 for embedding, and a refractive index of 1. 53 ± 0.03 and a water vapor transmission rate of less than 100 [g / (m 2 ·24 h)] of the water vapor barrier layer 4, a sealing layer forming sheet.

[0008] [2] The sealing layer forming sheet according to [1], wherein the water vapor barrier layer 4 is a thermoplastic olefin film.

[0009] [3] At 100°C, the tensile storage modulus E’3 of the colorless resin composition layer 3 for embedding, (100) the tensile storage modulus E’4 of the water vapor barrier layer 4, <00000​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​​[6] A member in which a plurality of light-emitting elements are sealed, wherein at least a portion of the depth of the individual gaps between the light-emitting elements and / or at least a portion of the bottom surface of the individual gaps are filled with a cured product 9' of a colored resin composition 9 for embedding, and the remaining portion of the individual gaps between the light-emitting elements is filled with a cured product 3' of a colorless resin composition 3 for embedding.

[0013] [7] A member in which a plurality of light-emitting elements according to "5" or [6] are sealed, wherein the water vapor barrier layer 4 is a thermoplastic olefin film. [Brief explanation of the drawing]

[0014] [Figure 1] A schematic cross-sectional view of the sealing layer forming sheet of the present invention. [Figure 2] A schematic cross-sectional view illustrating the state of the gaps between light-emitting elements in a component of the present invention in which multiple light-emitting elements are sealed. [Figure 3] A schematic cross-sectional view illustrating the thickness of each layer in a component of the present invention in which multiple light-emitting elements are sealed. [Figure 4] A schematic cross-sectional view illustrating the process of manufacturing a component of the present invention in which multiple light-emitting elements are sealed using a sealing layer forming sheet of the present invention. [Figure 5] A schematic cross-sectional view illustrating the process of manufacturing a component of the present invention in which multiple light-emitting elements are sealed using a sealing layer forming sheet of the present invention. [Figure 6] A schematic cross-sectional view illustrating the process of manufacturing a component of the present invention in which multiple light-emitting elements are sealed using a sealing layer forming sheet of the present invention. [Figure 7] A schematic cross-sectional view illustrating the process of manufacturing a component of the present invention in which multiple light-emitting elements are sealed using a sealing layer forming sheet of the present invention. [Figure 8]A schematic cross-sectional view illustrating the process of manufacturing a component of the present invention in which multiple light-emitting elements are sealed using a sealing layer forming sheet of the present invention. [Figure 9] A schematic cross-sectional view illustrating the process of manufacturing a component of the present invention in which multiple light-emitting elements are sealed using a sealing layer forming sheet of the present invention. [Figure 10] A schematic cross-sectional diagram illustrating the process of preparing the encapsulation targets β2 and β3. [Figure 11] A schematic diagram illustrating the evaluation of the invisibility of the boundaries and other parts of the LED encapsulating member model in the embodiment. [Modes for carrying out the invention]

[0015] The present disclosure will be described in detail below. The embodiments described below are examples of the present disclosure. The present disclosure is not limited to the embodiments described below and includes modifications that do not alter the essence of the present disclosure. In this specification, numerical ranges specified using "~" include the values ​​before and after "~" as the lower and upper limits. (Meth)acrylic acid refers to acrylic acid and methacrylic acid. Unless otherwise noted, each component mentioned in this specification may be used individually or in combination of two or more. When two or more are used in combination, the total content shall be used.

[0016] [Sheet for forming sealing layer] The sealing layer forming sheet 1 of this disclosure is a sheet for forming a sealing member used in the formation of a display. The sealing member is a member in which light-emitting elements (e.g., micro-LED elements) are sealed on a substrate, and the sealing layer forming sheet 1 of this disclosure is a sheet for sealing a plurality of light-emitting elements on a substrate. As shown in Figure 1(1), the sealing layer forming sheet 1 has a first film 2, a sealing layer precursor α, and a second film 5 arranged in that order. The sealing layer precursor α has a colorless resin composition layer 3 for embedding and a water vapor barrier layer 4.

[0017] <Sealing layer precursor α> The sealing layer precursor α has a water vapor permeability of 100 [g / (m³]. 2 (less than 24 hours), moisture absorption rate It is important that the amount is 1.5% by mass or less. The water vapor transmission rate is 70 [g / (m³]. 2 ·24 hours It is preferable that the value is 50[g / (m²) or less, and 50[g / (m²) 2 (24 hours) or less Preferably, 30 [g / (m 2 It is even more preferable that it be less than or equal to 24 hours, and especially 1 0 [g / (m 2 Preferably, the moisture absorption rate is 1% by mass or less (24 hours). It is preferable that the water vapor permeability is 0.8% by mass or less, and more preferably 0.8% by mass or less. Water vapor permeability refers to the speed of water vapor movement, and the moisture absorption rate refers to the water vapor storage capacity. By making the water vapor permeability and moisture absorption rate as low as possible, it becomes more difficult for water vapor to pass through and absorb, improving the migration resistance of the sealed component. This improved migration resistance expands the possibilities for using displays in higher temperature and higher humidity environments. Water vapor transmission was measured using a Labthink C390H (ISO) water vapor transmission meter. Using 15106-2 (compliant with ASTM F1249), transmission area: 5 cm² 2 The values ​​measured over approximately 24 hours under the measurement conditions of 40℃ × 90%RH were [g / (m³]. 2 This refers to (24 hours). Note that although the measured value will not change, the surface that comes into contact with water vapor during measurement should be the side with the colorless resin composition layer. The moisture absorption rate is 10cm 2 After measuring the mass of a film of the specified area in an environment of 23°C and 50%RH, the film is left to stand for 24 hours in an environment of 40°C and 90%RH to allow it to absorb moisture. Then, it is returned to an environment of 23°C and 50%RH, and the mass of the sample after standing is measured within 1 hour. The rate of change in mass calculated based on the following formula is defined as the moisture absorption rate. Moisture absorption rate (%) = [(Value after moisture absorption ÷ Value before moisture absorption) - 1] × 100)

[0018] The thickness of the sealing layer precursor α is preferably 10 to 100 μm, preferably 12 to 50 μm, and particularly preferably 15 to 30 μm. A thickness of 10 μm or more improves water vapor barrier properties, while a thickness of 100 μm or less maintains a high level of transparency. By setting the thickness within this particularly preferred range, it is possible to obtain a display that exhibits high water vapor barrier properties while maintaining high transparency, as well as excellent color development and display performance.

[0019] <Colorless resin composition layer 3 for embedding> The colorless resin composition layer 3 for embedding (hereinafter sometimes abbreviated as colorless resin composition layer 3, colorless resin composition layer, or resin composition layer 3) is for sealing the light-emitting element placed on the substrate. It is important that its refractive index is 1.51 ± 0.03, and it is preferable that the difference between this refractive index and that of the substrate on which the light-emitting element is placed is as small as possible. The substrate will be described later. Furthermore, from the standpoint of display performance as a display, it is important that the embedded resin composition layer 3 is colorless, or more precisely, colorless and transparent. Specifically, in terms of colorlessness, it is important that the b value in the Lab value is 1.5 or less, and preferably 1.0 or less. Also, in terms of transparency, it is important that the haze is 3.0 or less, and preferably 1.0 or less.

[0020] Furthermore, it is desirable that the colorless resin composition layer 3 also has excellent water vapor barrier properties. However, it is difficult to achieve both embedding properties and water vapor barrier properties, and the water vapor transmission rate is 100 [g / (m³] in the sense that it has a higher water vapor transmission rate compared to the water vapor barrier layer 4 described later. 2 ·24 hours)] That's all.

[0021] Furthermore, it is important that the colorless resin composition layer is hydrophobic, and the moisture absorption rate measured by the same method as the sealing layer precursor α is preferably 1.5% or less, and more preferably 1.0% or less. If it exceeds 1.5%, for example, even if the water vapor permeability is low and it is difficult for water vapor to pass through, if it easily absorbs water vapor, the cured product of the colorless resin composition layer after sealing will also easily absorb water vapor. The cured product of the colorless resin composition layer will be sandwiched between the substrate and the water vapor barrier layer as described later, but it is important that it does not absorb water vapor as much as possible until it is sandwiched. Also, after it is sandwiched, it is important to suppress and prevent the absorption of water vapor from the edge. Absorbed moisture can cause the cured product of the colorless resin composition layer to whiten at the interface with the substrate or LED elements, or migration (ion deposition or circuit corrosion) to occur via water. Even a very slight whitening of the cured product significantly impairs display performance and is a fatal defect, especially for transparent displays. The colorless resin composition layer has a hygroscopicity of 1.0% or less, which expands the possibilities for using displays in higher temperature and humidity environments.

[0022] The thickness of the colorless resin composition layer is 5 to 50 μm, preferably 10 to 40 μm, and more preferably 15 to 30 μm, from the viewpoint of embedding ability. By setting the thickness of the colorless resin composition layer within the above range, the pressure applied to the resin composition layer 3 during the pressing process is appropriately distributed and sufficiently uniform, thereby improving embedding performance. By setting the range as described above, the pressure transmission applied to the colorless resin composition layer in the pressing process described later is controlled, and the colorless resin composition layer flows uniformly, resulting in good embedding properties.

[0023] The colorless resin composition layer comprises at least a resin (A) and a polymerization initiator (C). Resin (A) is a substance that functions as a binder, adhering and fixing objects together. The colorless resin composition layer 3 comes into contact with the top surface of the micro-LED element in steps (IV) to (V) of Figure 3, is embedded along the shape of the encapsulation target β1, and in step (VI) of Figure 3, the colorless resin composition layer hardens, thereby fixing the encapsulation layer to the encapsulation target β1. (Figures 4 to 7) The same applies to the case shown in Figure 8, except that there is no step of embedding a colorless resin composition layer along the shape of the encapsulation target β3.

[0024] The glass transition temperature of the colorless resin composition layer is the peak top temperature (tanδ peak temperature) of the loss tangent obtained by dynamic viscoelasticity measurement, which is the temperature at which the tanδ curve is maximized. If there are two or more peaks, it refers to the lowest temperature peak. The tanδ peak temperature is preferably 25 to 100°C, more preferably 40 to 80°C, and even more preferably 50 to 70°C. Because the tanδ peak temperature is within the above range, in step (IV) of Figure 3, the resin does not stick firmly to the encapsulation target β1 even while in contact, making it easy to remove misalignment and trapped air. Furthermore, the more preferable range is higher than the LED operating temperature (40°C), so the resin is less likely to degrade and therefore less prone to yellowing. The tanδ peak temperature of the colorless resin composition layer can be adjusted depending on the type and composition of resin (A). If resin (A) is a (meth)acrylic resin, the tanδ peak temperature can be increased by increasing the content of acrylic monomers that form a homopolymer with a high glass transition temperature (Tg), and conversely, if the tanδ peak temperature is to be lowered, the opposite adjustment can be made. The glass transition temperature (Tg) of the homopolymer in this disclosure can be the value described in POLYMER HANDBOOK, 1999, FOURTH EDITION.

[0025] The loss tangent (tanδ) mentioned above is the ratio of the loss modulus to the storage modulus obtained by dynamic viscoelastic measurements in the tensile mode at a frequency of 10 Hz and a temperature of -50 to 150°C. The dynamic viscoelasticity and loss tangent (tanδ) in this disclosure are measured by the method described in the examples below. Note that if the resin composition layer 3 contains either a polymerization initiator (C) or a crosslinking agent, the polymerization / crosslinking reaction is incomplete at the time of measurement. Furthermore, it is preferable to measure a sheet with a thickness of 50 μm or more. If a sheet with a thickness less than this is to be measured, two sets of sealing sheets without a first film are prepared, the colorless resin composition layers 3 are laminated together with a laminator to create a laminate of second film / colorless resin composition layer 3 / second film, and then the second film on one side of the aforementioned laminate is peeled off and the colorless resin composition layers 3 of the sealing sheets are repeatedly laminated until a thickness of 50 μm or more is achieved, after which the dynamic viscoelasticity may be measured.

[0026] The resin (A) needs to have excellent embedding properties and transparency for sealing, and various resins can be selected. Examples include (meth)acrylic resins, polyurethane resins and polyurethane urea resins, epoxy resins, maleic acid resins, styrene-maleic acid copolymers, polystyrene resins, polybutadiene resins, polyester resins, condensation-type polyester resins, addition-type polyester resins, melamine resins, polycarbonate resins, oxetane resins, phenoxy resins, polyimide resins, polyamide-imide resins, alkyd resins, amino resins, polyamide resins, polylactic acid resins, oxazoline resins, benzoxazine resins, silicone resins, fluororesins, butyral resins, chlorinated polyethylene, chlorinated polypropylene, polyvinyl chloride, vinyl chloride-vinyl acetate copolymers, polyvinyl acetate, vinyl resins, rubber resins, cyclic rubber resins, celluloses, polyethylene (HDPE, LDPE), etc. Embedding properties (Meth)acrylic resin, urethane resin, and epoxy resin, which have excellent transparency, are preferred, and (meth)acrylic resin, which is particularly resistant to yellowing due to heat and light, is more preferred. Resin (A) can be used alone or in combination of two or more types.

[0027] The weight-average molecular weight (Mw) of resin (A) is preferably between 10,000 and 1,000,000. More preferably between 30,000 and 300,000, and even more preferably between 50,000 and 150,000. By setting the weight-average molecular weight (Mw) of resin (A) to 1,000,000 or less, it is less likely to gel and less likely to impair transparency, and if it is 10,000 or more... The coating strength is improved while offering excellent embedding properties. Being within a more desirable range means it is less prone to deterioration and yellowing due to heat and light, has a lower moisture absorption rate, and the quality of the finished display is improved. The weight-average molecular weight (Mw) is a polystyrene-based value measured by gel permeation chromatography (GPC). In this disclosure, the weight-average molecular weight (Mw) was measured using the method described in the examples below.

[0028] Resin (A) preferably has one or more radical polymerizable functional groups that can be used in polymerization / crosslinking reactions by utilizing ions or radicals generated by heat or light. Examples of radical polymerizable functional groups include (meth)acryloyl groups, N-vinyl groups, vinyl ether groups, allyl groups, and unsaturated carboxylic acid groups. The functional groups may be appropriately selected based on their reactivity with other resins (A) and with the polymerization initiator (C) and crosslinking agent described later, and may also be self-crosslinkable functional groups.

[0029] [(meth)acrylic resin] (Meth)acrylic resin is an acrylic copolymer obtained by copolymerizing (meth)acrylic acid ester monomers, and is a polymer having 2 to 20,000 monomer-based structural units. A preferred example of the (meth)acrylic acid ester monomer is alkyl (meth)acrylic acid ester monomer. When introducing functional groups that can be used in polymerization / crosslinking reactions, a (meth)acrylic copolymer obtained by copolymerizing a functional group-containing monomer with a (meth)acrylic acid ester monomer is preferred.

[0030] Alkyl (meth)acrylate monomers are compounds obtained by esterifying (meth)acrylic acid and introducing an alkyl group or cycloalkyl group. The alkyl group or cycloalkyl group may be a linear, branched, or cyclic saturated aliphatic hydrocarbon group, and linear alkyl groups with four or more carbon atoms are preferred due to their excellent hydrophobicity. Specific examples include methyl (meth)acrylate, ethyl (meth)acrylate, propyl (meth)acrylate, isopropyl (meth)acrylate, n-butyl (meth)acrylate, isobutyl (meth)acrylate, s-butyl (meth)acrylate, t-butyl (meth)acrylate, pentyl (meth)acrylate, hexyl (meth)acrylate, heptyl (meth)acrylate, octyl (meth)acrylate, 2-ethylhexyl (meth)acrylate, isooctyl (meth)acrylate, nonyl (meth)acrylate, isononyl (meth)acrylate, and (meth)acrylic acid. Examples include decyl, isodecyl (meth)acrylate, undecyl (meth)acrylate, dodecyl (meth)acrylate, tridecyl (meth)acrylate, tetradecyl (meth)acrylate, pentadecyl (meth)acrylate, hexadecyl (meth)acrylate, heptadecyl (meth)acrylate, octadecyl (meth)acrylate, nonadecyl (meth)acrylate, eicosyl (meth)acrylate, lauryl (meth)acrylate, cyclohexyl (meth)acrylate, 4-n-butylcyclohexyl (meth)acrylate, and isobornyl (meth)acrylate. In particular, it is preferable to use n-butyl (meth)acrylate, which has excellent hydrophobicity, a good balance of flexibility and rigidity, and excellent embedding properties and transparency.

[0031] The (meth)acrylic resin preferably contains 1 to 100% by mass of structural units derived from the (meth)acrylate alkyl ester monomer as described above, more preferably 20 to 99.5% by mass, and even more preferably 80 to 99% by mass, from the viewpoint of adhesion.

[0032] (Meth)acrylic resins preferably have structural units derived from functional group-containing monomers and / or unsaturated bonds. Examples of functional group-containing monomers include carboxyl group-containing monomers, hydroxyl group-containing monomers, epoxy group-containing monomers, and amino group-containing monomers. The inclusion of functional group-containing monomers improves the cohesive strength of resin (A) and its adhesion to substrates and circuits. It is also possible to introduce radically polymerizable unsaturated bonds by utilizing the functional groups of the group-containing monomers. Hydroxyl group-containing monomers and amino group-containing monomers are highly hydrophilic and therefore tend to impair hydrophobicity. Epoxy group-containing monomers and carboxy group-containing monomers, which do not significantly affect the hydrophobicity of the colorless resin composition layer, are preferred.

[0033] Examples of carboxyl group-containing monomers include (meth)acrylic acid, β-carboxyethyl (meth)acrylate, p-carboxybenzyl (meth)acrylate, carboxypentyl (meth)acrylate, itaconic acid, maleic acid, fumaric acid, crotonic acid, citraconic acid, and isocrotonic acid. Among these, (meth)acrylic acid is preferred from the viewpoint of adhesion. By reacting the carboxyl groups in the (meth)acrylic copolymer with glycidyl (meth)acrylate or the like, a radically polymerizable unsaturated bond can also be introduced.

[0034] Examples of hydroxyl group-containing monomers include 2-hydroxyethyl (meth)acrylate, 2-hydroxypropyl (meth)acrylate, 2-hydroxybutyl (meth)acrylate, 3-hydroxypropyl (meth)acrylate, 4-hydroxybutyl (meth)acrylate, 6-hydroxyhexyl (meth)acrylate, 8-hydroxyoctyl (meth)acrylate, 10-hydroxydecyl (meth)acrylate, 12-hydroxylauryl (meth)acrylate, and (4-hydroxymethylcyclohexyl)methyl (meth)acrylate. Among these, 4-hydroxybutyl (meth)acrylate and 2-hydroxyethyl (meth)acrylate are more preferred from the viewpoint of adhesion. Radically polymerizable unsaturated bonds can also be introduced by reacting a compound having an isocyanate group and a (meth)acryloyl group with the hydroxyl groups in a (meth)acrylic copolymer.

[0035] Examples of amino group-containing monomers include monoalkylamino esters of (meth)acrylates such as monomethylaminoethyl (meth)acrylate, monoethylaminoethyl (meth)acrylate, monomethylaminopropyl (meth)acrylate, and monoethylaminopropyl (meth)acrylate.

[0036] For the purpose of introducing unsaturated bonds into (meth)acrylic resin, epoxy group-containing monomers can also be used. Examples of epoxy group-containing monomers include glycidyl (meth)acrylate, methylglycidyl (meth)acrylate, 3,4-epoxycyclohexylmethyl (meth)acrylate, and 6-methyl-3,4-epoxycyclohexylmethyl (meth)acrylate. Among these, glycidyl (meth)acrylate is preferred from the viewpoint of reactivity. After obtaining a (meth)acrylic copolymer, it is preferable to react the epoxy group derived from the epoxy group-containing monomer with the carboxyl group of a carboxyl group-containing monomer such as (meth)acrylic acid to introduce an unsaturated bond such as a (meth)acryloyl group into the (meth)acrylic resin. At this time, it is preferable that there is one or fewer epoxy groups per molecule and that no epoxy groups remain.

[0037] The structural units of (meth)acrylic resin are determined by the proportion of each monomer blended during the manufacturing of the (meth)acrylic resin. Specifically, when the total amount of constituent monomers is 100% by mass, the structural units derived from functional group-containing monomers are preferably 0.1 to 20% by mass. A concentration of 0.1% by mass allows for cohesive force to be exerted, while a concentration of 20% by mass or less suppresses the gelation of the resin.

[0038] Examples of functional group-containing monomers include carboxyl group-containing monomers and hydroxyl group-containing monomers. When the functional group-containing monomer is a carboxyl group-containing monomer, it is preferable that the amount is 0.1 to 10% by mass. When the functional group-containing monomer is a constituent unit derived from a hydroxyl group-containing monomer, it is preferable that the amount is 0.1 to 20% by mass. Being within the above range suppresses gelation of the resin while increasing cohesive force. It is preferable that both carboxyl group-containing monomers and hydroxyl group-containing monomers are present, within a range where the total structural units derived from functional group-containing monomers do not deviate from 0.1 to 20% by mass.

[0039] The (meth)acrylic resin may contain structural units derived from alkyl (meth)acrylate esters and other monomers copolymerizable with functional group-containing monomers. Examples include monomers having alkylene oxy groups and other vinyl monomers. For example, methoxyethyl acrylate, methoxydiethylene glycol acrylate, vinyl acetate, vinyl crotate, and styrene can be cited. The structural units derived from the other monomers are preferably present in an amount of 0.1 to 20% by mass of 100% by mass of the (meth)acrylic copolymer.

[0040] (Meth)acrylic resin is obtained by polymerizing an acrylic monomer mixture. A polymerization initiator may be used during polymerization as needed. The content of the polymerization initiator is, for example, 0.01 to 10% by mass per 100% by mass of the monomer mixture. The polymerization method is not limited. For example, polymerization can be carried out by solution polymerization, bulk polymerization, emulsion polymerization, or suspension polymerization, and solution polymerization is the most preferred due to the ease of polymerization control. Examples of solvents used in solution polymerization include acetone, methyl ethyl ketone, methyl isobutyl ketone, methyl acetate, ethyl acetate, butyl acetate, toluene, xylene, anisole, cyclohexanone, and isopropyl alcohol. The polymerization temperature can be, for example, 60 to 120°C, and the polymerization time can be about 2 to 12 hours.

[0041] When polymerizing (meth)acrylic resins, radical polymerization initiators are preferred. Peroxides and azo compounds are suitable radical polymerization initiators.

[0042] [Polymerization initiator (C)] The initiator (C) can be either a thermal polymerization initiator or a photopolymerization initiator. For substrates with complex shapes, it is preferable to use a thermal polymerization initiator, which is less likely to cause problems due to insufficient irradiation. Furthermore, in step (VI) of Figure 3, curing while applying pressure and heat makes it possible to minimize warping and lifting due to curing shrinkage. Although it is also possible to cleave the photopolymerization initiator with heat, it tends to yellow, so a thermal polymerization initiator is preferred because the cleavage residue is less likely to yellow.

[0043] In this embodiment, a thermal cationic polymerization initiator and a thermal radical polymerization initiator can be used as thermal polymerization initiators. A thermal radical polymerization initiator is preferred because of its storage stability of the colorless resin composition layer and its fast curing rate after cleavage, which increases the production rate. Thermal cationic polymerization initiators have the function of generating ions when heated. Examples of thermal cationic polymerization initiators include sulfonium cations, quaternary ammonium cations, and iodonium cations as cationic components, and antimony hexafluoride anions, phosphorus hexafluoride anions, tetrakis(pentafluorophenyl) borate anions, and trifluoromethanesulfonic acid as anionic components. Thermal radical polymerization initiators have the function of generating radicals by heat. Examples of thermal radical polymerization initiators include organic peroxide polymerization initiators and azo thermal polymerization initiators, with organic peroxide polymerization initiators being preferred from the viewpoint of preventing yellowing.

[0044] Examples of organic peroxide polymerization initiators include diacetyl peroxide, di-t-butyl peroxide, di-t-hexyl peroxide, dicumyl peroxide, t-butylcumyl peroxide, and α,α'-bis(t-butylperoxy-m-isopropyl). Benzene, 2,5-dimethyl-2,5-bis(t-butylperoxy)hexyn-3, 2,5-dimethyl-2,5-bis(t-butylperoxy)hexane, 1,3-bis(t-butylperoxyisopropyl)hexane, (2-ethylhexanoyl)(t-butyl) Dialkyl peroxides such as peroxides; Dipropionyl peroxide, t-butyl peroxyacetate, t-butyl peroxybenzoate, 2,5-dimethyl-2,5-di(benzoylperoxy)hexane, bis(3,5,5-trimethylhexanoyl)peroxide, 1,1,3,3-tetramethylbutyl peroxyneodecanoate, α-cumyl peroxyneodecanoate, t-butyl peroxyneodecanoate, t-hexyl peroxyneodecanoate, t-butyl peroxyneoheptanoate, t-hexyl peroxypivalate, t-butyl peroxypivalate, 1,1,3,3-tetramethylbutyl peroxy-2-ethylhexanoate, t-amyl peroxy-2-ethylhexanoate, t-butyl peroxy-2-ethylhexanoate, Peroxyesters such as t-butyl peroxyisobutyrate, di-t-butyl peroxyhexahydroterephthalate, 1,1,3,3-tetramethylbutyl peroxy-3,5,5-trimethylhexanate, t-amyl peroxy-3,5,5-trimethylhexanoate, t-butyl peroxy-3,5,5-trimethylhexanoate, dibutyl peroxytrimethyl adipate, 2,5-dimethyl-2,5-di-2-ethylhexanoyl peroxyhexane, t-hexyl peroxy-2-ethylhexanoate, t-hexyl peroxyisopropyl monocarbonate, t-butyl peroxylaurate, t-butyl peroxyisopropyl monocarbonate, and t-butyl peroxy-2-ethylhexyl monocarbonate; Ketone peroxides such as methyl ethyl ketone peroxide, methyl isobutyl ketone peroxide, acetylacetone peroxide, cyclohexanone peroxide, 3,3,5-trimethylcyclohexanone peroxide, methylcyclohexanone peroxide, t-butyl benzoate, and pivaloyl t-butyl peroxide; Peroxyketals such as 2,2-bis(t-butylperoxy)butane, 2,2-bis(4,4-di-t-butylperoxycyclohexyl)propane, 1,1-bis(t-butylperoxy)3,3,5-trimethylcyclohexane, 1,1-bis(t-hexylperoxy)-3,3,5-trimethylcyclohexane, 1,1-bis(t-butylperoxy)cyclohexane, 1,1-bis(t-hexylperoxy)cyclohexane, and 4,4-bis(t-butylperoxy)butyl pentanoate; Hydroperoxides such as t-butyl hydroperoxide, cumene hydroperoxide, diisopropylbenzene hydroperoxide, 2,5-dimethylcyclohexane-2,5-dihydroperoxide, 1,1,3,3-tetramethylbutyl hydroperoxide, and p-menthane hydroperoxide; Diacyl peroxides such as dibenzoyl peroxide, didecanoyl peroxide, dilauroyl peroxide, diisobutyryl peroxide, bis-3,5,5-trimethylhexanol peroxide, m-toluylbenzoyl peroxide, succinate peroxide, and 2,4-dichlorobenzoyl peroxide; Examples of peroxydicarbonates include, but are not limited to, bis(t-butylcyclohexyl)peroxydicarbonate, diisopropyl peroxydicarbonate, di-n-propyl peroxydicarbonate, di(2-ethoxyethyl)peroxydicarbonate, t-butylperoxyisopropyl carbonate, di-2-ethylhexyl peroxycarbonate, di-sec-butylperoxycarbonate, di-3-methoxybutyl peroxydicarbonate, di-2-ethylhexyl peroxydicarbonate, t-amylperoxyisopropyl carbonate, t-butylperoxy-2-ethylhexyl carbonate, and 6-bis(t-butylperoxycarboxyloxy)hexane. From the viewpoint of storage stability, dialkyl peroxides are preferred, and di-t-butyl peroxide is more preferred.

[0045] As an azo thermal polymerization initiator, 2,2'-azobispropionamides are preferred from the viewpoint of storage stability, and 2,2'-azobis(N-butyl-2-methylpropionamide) is more preferred.

[0046] The 10-hour half-life temperature of the thermal radical polymerization initiator is preferably 60 to 180°C, more preferably 70 to 140°C, and even more preferably 80 to 120°C. Setting it above 60°C improves the storage stability of the colorless resin composition layer, while setting it below 180°C reduces warping due to differences in shrinkage rates of the substrate and encapsulation layer precursor in step (IV) of Figure 3, etc.

[0047] The 10-hour half-life temperature is the temperature at which the thermal polymerization initiator is reduced to half of its initial value after 10 hours due to thermal decomposition. Specifically, a thermal polymerization initiator solution is prepared using a solvent inert to the radicals of the thermal polymerization initiator, and sealed in a glass tube purged with nitrogen. This is then immersed in a constant temperature chamber set to a predetermined temperature for 10 hours to allow thermal decomposition, and the amount of remaining thermal polymerization initiator is measured. By performing this series of operations at several temperatures and plotting the results, the half-life can be determined from the resulting straight line.

[0048] The amount of thermal radical polymerization initiator is preferably 0.01 to 20 parts by mass, more preferably 0.05 to 10 parts by mass, and even more preferably 0.1 to 5 parts by mass, per 100 parts by mass of resin (A). By using the above content, the adhesion can be suitably adjusted.

[0049] Examples of photopolymerization initiators include triazine-based photopolymerization initiators, borate-based photopolymerization initiators, carbazole-based photopolymerization initiators, acetophenone-based photopolymerization initiators, and oxime ester-based photopolymerization initiators. Acetophenone-based photopolymerization initiators and oxime ester-based photopolymerization initiators are preferred because they cause less yellowing during the heating and aging process. From the viewpoint of preventing yellowing, the photopolymerization initiator content is preferably 0.5 to 10 parts by mass, and more preferably 0.5 to 5 parts by mass, per 100 parts by mass of resin (A).

[0050] [Other ingredients] The colorless resin composition layer may contain other components, to the extent that they do not impair the purpose of this disclosure. For example, refractive index modifiers, crosslinking agents, monomers, surface conditioning additives, curing accelerators, curing retarders, softeners, antistatic agents, lubricants, antiblocking agents, adhesion improvers, etc. Examples of refractive index modifiers include urethane (meth)acrylates and inorganic fillers.

[0051] Compared to (meth)acrylic resins, urethane (meth)acrylate has a higher refractive index and is more compatible, making it easier to adjust the refractive index of the colorless resin composition layer used for embedding while maintaining transparency.

[0052] Urethane (meth)acrylate is a reaction product of a compound having an isocyanate group and a (meth)acrylate having a hydroxyl group, and has a (meth)acryloyl group at the end of the molecule. It is preferable to use a polyfunctional compound having an isocyanate group and reacting it with a (meth)acrylate having one hydroxyl group, or to use a monofunctional compound having an isocyanate group and reacting it with a (meth)acrylate having multiple hydroxyl groups to use a urethane (meth)acrylate having multiple (meth)acryloyl groups. High Mw urethane (meth)acrylates are obtained by reacting a prepolymer having isocyanate groups, which is formed by reacting various diols and diamines with relatively low molecular weight compounds having isocyanate groups, with a (meth)acrylate having hydroxyl groups. It is possible.

[0053] Examples of diols include diols having a linear aliphatic structure and diols having a branched aliphatic structure. Examples of diamines include diamines having a linear aliphatic structure and diamines having a branched aliphatic structure, as well as diamines having an alicyclic structure.

[0054] Urethane (meth)acrylates containing multiple (meth)acryloyl groups rapidly harden upon exposure to peroxides or ultraviolet light due to unsaturated carbon bonds derived from the (meth)acrylate. The resulting cured product has a high crosslink density and excellent chemical resistance and transparency. It is preferable that the urethane (meth)acrylate has three or more double-bond functional groups in one molecule.

[0055] The weight-average molecular weight (Mw) of the urethane (meth)acrylate is preferably 300 to 4000. An Mw of 4000 or less facilitates compatibility with the (meth)acrylate resin, allowing for the production of a colorless resin composition layer with excellent transparency. An Mw of 300 or more prevents bleed-out from the colorless resin composition layer.

[0056] The amount of urethane (meth)acrylate added to the (meth)acrylic resin is preferably (meth)acrylic resin / urethane (meth)acrylate = 95% / 5%~60% / 40% when the total is 100% by mass, and more preferably 90% / 10%~80% / 20%. The urethane (meth)acrylate content tends to increase when it is 5% by mass or more, and suppresses bleed-out of urethane (meth)acrylate when it is 40% by mass or less.

[0057] Examples of inorganic fillers with a refractive index of 1.55 or higher include inorganic compounds such as borosilicate glass, alumina, magnesium hydroxide, barium sulfate, calcium carbonate, titanium dioxide, zinc oxide, antimony trioxide, magnesium oxide, zirconium oxide, talc, kaolinite, mica, magnesium carbonate base, sericite, montmorrolinite, bentonite, boron nitride, aluminum nitride, and titanium nitride. Among these, titanium dioxide, aluminum oxide, and zirconium oxide are preferred from the viewpoint of easily adjusting the refractive index while maintaining transparency. Furthermore, if the refractive index of resin (A) is high, the refractive index of the colorless resin composition layer for embedding can be adjusted by incorporating a component with a lower refractive index.

[0058] The crosslinking agent enhances the cohesive force of the resin composition layer and improves adhesion by crosslinking with the reactive functional groups of resin (A) during the hot pressing and heat aging processes in the pressing process. The crosslinking agent has multiple functional groups that can react with the functional groups of resin (A). Examples of known crosslinking agents include silane coupling agents, acid anhydride group-containing compounds, imidazole compounds, isocyanate compounds, aziridine compounds, and amine compounds. Isocyanate compounds, aziridine compounds, and imidazole compounds are preferred to improve adhesion to circuits and substrates. Silane coupling agents are particularly preferred to improve adhesion to glass, such as glass substrates.

[0059] Examples of aziridine compounds include trimethylolpropane tris[3-(aziridin-1-yl)propionate], tetramethylolmethane-tri-β-aziridinylpropionate, N,N'-diphenylmethane-4,4'-bis(1-aziridincarboxyamide), N,N'-hexamethylene-1,6-bis(1-aziridincarboxyamide), tris-2,4,6-(1-aziridinyl)-1,3,5-triazine, and 4,4'-bis(ethyleneiminocarbonylamino)diphenylmethane.

[0060] The isocyanate compound is an isocyanate having two or more isocyanate groups. The isocyanate compound is preferably an isocyanate monomer such as aromatic polyisocyanates, aliphatic polyisocyanates, aromatic aliphatic polyisocyanates, or alicyclic polyisocyanates, as well as their burette, nurate, and adduct forms. From the viewpoint of forming a sufficient cross-linked structure, trifunctional isocyanate compounds are preferred.

[0061] Silane coupling agents are compounds in which hydrolyzable groups such as methoxy groups and ethoxy groups, and functional groups such as epoxy groups, are bonded to Si atoms via alkylene groups. Silane coupling agents include alkoxysilane compounds having a (meth)acryloxy group, such as 3-(meth)acryloxypropyltrimethoxysilane, 3-(meth)acryloxypropyltriethoxysilane, 3-(meth)acryloxypropyltripropoxysilane, 3-(meth)acryloxypropyltributoxysilane, 3-(meth)acryloxypropylmethyldimethoxysilane, and 3-(meth)acryloxypropylmethyldiethoxysilane; Alkoxysilane compounds having a vinyl group, such as vinyltrimethoxysilane, vinyltriethoxysilane, vinyltriisopropoxysilane, vinyltributoxysilane, vinylmethyldimethoxysilane, and vinylmethyldiethoxysilane; Alkoxysilane compounds having an amino group, such as 3-aminopropyltrimethoxysilane, 3-aminopropyltriethoxysilane, 3-aminopropyltripropoxysilane, 3-aminopropylmethyldimethoxysilane, 3-aminopropylmethyldiethoxysilane, N-(2-aminoethyl)-3-aminopropyltrimethoxysilane, N-(2-aminoethyl)-3-aminopropyltriethoxysilane, N-(2-aminoethyl)-3-aminopropylmethyldimethoxysilane, N-(2-aminoethyl)-3-aminopropylmethyldiethoxysilane, and N-phenyl-3-aminopropyltrimethoxysilane; Alkoxysilane compounds having a mercapto group, such as 3-mercaptopropyltrimethoxysilane, 3-mercaptopropyltriethoxysilane, 3-mercaptopropyltripropoxysilane, 3-mercaptopropylmethyldimethoxysilane, and 3-mercaptopropylmethyldiethoxysilane; Alkoxysilane compounds having one epoxy group, such as 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropyltriethoxysilane, 3-glycidoxypropyltripropoxysilane, 3-glycidoxypropyltributoxysilane, 3-glycidoxypropylmethyldimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane, and 2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane; Tetraalkoxysilane compounds such as tetramethoxysilane, tetraethoxysilane, tetrapropoxysilane, and tetrabutoxysilane; Examples include 3-chloropropyltrimethoxysilane, n-hexyltrimethoxysilane, n-hexyltriethoxysilane, n-decyltrimethoxysilane, n-decyltriethoxysilane, styryltrimethoxysilane, phenyltrimethoxysilane, diphenyldimethoxysilane, 3-triethoxysilyl-N-(1,3-dimethylbutylidene)propylamine, 1,3,5-tris(3-trimethoxysilylpropyl)isocyanurate, 3-isocyanatetopropyltrimethoxysilane, 3-isocyanatetopropyltriethoxysilane, hexamethyldisilazane, and silicone resins having alkoxysilyl groups in the molecule. When the same functional group as resin (A) is used, 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropyltriethoxysilane, vinyltrimethoxysilane, and vinyltriethoxysilane are preferred because the cross-linking structure improves cohesive force and adhesion.

[0062] The crosslinking agent content is preferably 0.01 to 10 parts by mass per 100 parts by mass of resin (A). This content increases the cohesive force and improves adhesion to various sealing targets. To rise.

[0063] <Water vapor barrier layer 4> Next, we will describe the water vapor barrier layer 4 that constitutes the sealing layer precursor α together with the colorless resin composition layer 3 for embedding. The water vapor barrier layer is positioned to suppress ion deposition and circuit corrosion caused by water vapor. It is important that it has low water vapor permeability and low moisture absorption. In other words, the water vapor transmission rate is 100 [g / (m³] 2 It is important that it is less than 24 hours. , 70[g / (m 2 It is preferable that the amount is 50 [g / (m³) or less (24 hours) 2 It is more preferable that it be less than or equal to 24 hours, and 30 [g / (m³)2 (24 hours) or less It is even more preferable, and especially 10 [g / (m 2 It is preferable that it be less than or equal to 24 hours. Furthermore, it is important that the moisture absorption rate is 1.5% by mass or less, preferably 1% by mass or less, and more preferably 0.8% by mass or less.

[0064] It is important that the water vapor barrier layer 4 has a refractive index of 1.53 ± 0.03, and it is preferable that the difference between this and the refractive index of the substrate on which the light-emitting element is mounted is as small as possible. The substrate will be described later. Furthermore, from the standpoint of display performance, it is important that the water vapor barrier layer, like the colorless resin composition layer 3, is colorless, or more precisely, colorless and transparent. Specifically, in terms of colorlessness, it is important that the b value in the Lab value is 1.5 or less, and preferably 1.0 or less. Also, in terms of transparency, it is important that the haze is 3.0 or less, and preferably 1.0 or less.

[0065] Incidentally, as shown in Figures 4 to 9, when manufacturing a sealing member by sealing a light-emitting element placed on a substrate, a molding process is carried out. Therefore, the water vapor barrier layer is required to suppress uneven pressure distribution during embedding and to prevent the colorless resin composition layer from overflowing to areas other than the target area during embedding. Furthermore, the manufacturing process of the sealing member may involve a cleaning process with organic solvents, etc. Therefore, the water vapor barrier layer is also required to have low shrinkage and chemical resistance from the viewpoint of protecting the colorless resin composition layer for embedding and its cured product from damage during these processes. To satisfy a certain level of rigidity, flexibility, and chemical resistance, the film is preferably made of a thermoplastic resin. Examples of thermoplastic resin films include polyester film, polyolefin film, polyvinyl chloride film, polyurethane film, nylon film, acrylic film, and triacetylcellulose film, and also include plastic films having a metal oxide film such as aluminum oxide. Polyester films include polyethylene terephthalate film, polybutylene terephthalate film, and polyethylene naphthalate film. Polyolefin films include polypropylene film, polyethylene film, and cycloolefin films. Cycloolefin films include not only cycloolefin (COP) film, but also films made from cycloolefin copolymer (COC) and cycloolefin block copolymer (CBC). Due to their high transparency and low thermal shrinkage rate, transparent polyimide, polyethylene terephthalate, and polyethylene naphthalate are preferred, and from the viewpoint of water vapor barrier properties, polyethylene terephthalate film with a metal oxide film is preferred, but cycloolefin-based films with a small refractive index difference with alkali-free glass, which is important as a substrate on which the light-emitting element is mounted, are particularly preferred.

[0066] The thickness of the water vapor barrier layer is preferably 5 to 50 μm, more preferably 8 to 40 μm, and even more preferably 10 to 20 μm. A thickness of 5 μm or more improves water vapor barrier properties and stabilizes embedding. A thickness of 50 μm or less improves transparency. Displays are thinner. Since this is preferable, the above objective can be satisfied at a high level if the thickness of the water vapor barrier layer is within a more preferable range. Furthermore, if it is within a more preferable range, when a colorless resin composition layer is embedded in the gap between light-emitting elements, irregularities are less likely to occur on the surface of the water vapor barrier layer, and the water vapor barrier performance after sealing is further improved.

[0067] <First Film 2>, <Second Film 5> As shown in Figure 1, the sealing layer precursor α is sandwiched between the first film 2 and the second film 5. The first film 2 and the second film 5 are peeled off during the process of sealing multiple light-emitting elements 7 placed on the substrate using a sealing layer forming sheet, as shown in Figures 3 to 7.

[0068] <First Film 2> The first film 2 is not particularly limited, but examples include polyester film, polyolefin film, polyvinyl chloride film, polyurethane film, nylon film, acrylic film, triacetylcellulose film, etc. Examples of polyester films include polyethylene terephthalate film, polybutylene terephthalate film, and polyethylene naphthalate film. Examples of polyolefin films include polypropylene film, polyethylene film, and cycloolefin film. From a handling standpoint, polyester film and polyolefin film are preferred.

[0069] The first film 2 has a release layer on the surface facing the resin composition layer 3. The release layer is preferably formed by applying a release agent such as silicone resin, alkyd resin, fluororesin, or melamine resin to the film, and a release layer using silicone resin is more preferable from the viewpoint of handling (prevention of separation). The peeling force of the first film 2 is preferably 0.1 to 3 gf / 20 mm, more preferably 0.3 to 2 gf / 20 mm, and even more preferably 0.5 to 1 gf / 20 mm. The peeling force of the first film 2 can be adjusted by the release treatment of the release layer. For example, it can be adjusted by the type of release agent, the amount of release agent applied, and the surface roughness of the release layer. To decrease the peeling force, it is effective to increase the surface roughness or increase the amount of release agent applied, and to increase the peeling force, the opposite adjustments should be made. The peeling force of the first film 2 can be measured, for example, by attaching the second film 5 of the sealing layer forming sheet to a SUS plate, and peeling the first film 2 from the resin composition layer 3 at a peeling angle of 180° and a peeling speed of 300 mm / min in an environment of 23°C and 50% relative humidity. The first film 2 may have a functional layer in addition to the release layer. Specific examples of functional layers include an antistatic layer and an anti-blocking layer.

[0070] The thickness of the first film 2 is preferably 2 to 250 μm, more preferably 10 to 100 μm, and even more preferably 20 to 60 μm. If a release layer or a functional layer is provided on the first film 2, the thickness includes the release layer. By setting the thickness within the above range, it is possible to control the transfer of the waviness of the first film 2 to the colorless resin composition layer and form a uniform colorless resin composition layer. The first film 2 is preferably directly laminated with a colorless resin composition layer as shown in Figure 1(1). When the first film 2 is directly laminated with a colorless resin composition layer, the surface roughness Ra of the surface of the first film 2 in contact with the colorless resin composition layer is preferably 0.02 μm or more. The surface roughness of the surface of the first film 2 in contact with the colorless resin composition layer will be transferred in reverse to the surface of the colorless resin composition layer. Therefore, by using the first film 2 with the above-mentioned surface roughness, the colorless resin composition layer is less likely to adhere excessively to the surface of the light-emitting element during the process shown in Figure 3(IV), etc., and the placement position of the sealing layer forming sheet can be easily corrected. Furthermore, by using a colorless resin composition layer with a surface roughness Ra of 0.02 μm or more, during the process shown in Figure 3(V), Figure 4(V-2), etc., the substrate, light-emitting element, and Air is less likely to remain at the interface between the colored resin composition layer and the colorless resin composition layer, resulting in a better appearance. Specifically, from the viewpoint of blocking suppression and prevention, and air entrapment suppression and prevention, the surface roughness Ra of the first film 2 and the colorless resin composition layer in contact with the first film 2 is preferably 0.02 μm or more, more preferably 0.1 μm or more, and even more preferably 0.5 μm or more. From the viewpoint that the size of the irregularities does not easily affect the water vapor barrier layer, the upper limit of the surface roughness is preferably 20% or less of the thickness of the colorless resin composition layer.

[0071] Furthermore, the difference in cutting levels Rδc of the contour curve at the surface in contact with the colorless resin composition layer of the first film 2 is preferably 0.05 μm or more, and preferably 0.1 μm or more. It is preferable that the cross-section level difference Rδc of the contour curve be 20 μm or less, and more preferably 10 μm or less. Furthermore, it is even more preferable that the thickness be 6 μm or less. By transferring the irregularities of the first film 2 to the colorless resin composition layer, when the colorless resin composition layer comes into contact with the LED element or substrate, it does not immediately adhere, making it easier to correct for misalignment, and it also makes it easier to remove voids when embedding in a vacuum environment. Being within the preferred range allows for excellent correction of misalignment while sliding on the surface of the object to be sealed, and is excellent in removing voids.

[0072] <Second Film 5> The second film 5 supports the water vapor barrier layer during pressing and curing (heating and UV irradiation) in the processes shown in Figures 3(V) to (VI), 4(V-2) to (VI), etc., and functions as a cushion to suppress pressure unevenness and mold marks. To more reliably support the water vapor barrier layer, it is preferable to have a slightly adhesive layer on the surface in contact with the water vapor barrier layer.

[0073] The substrate of the second film 5 is not particularly limited, but for example, There are no particular restrictions, but examples include polyester film, polyolefin film, polyvinyl chloride film, polyurethane film, nylon film, acrylic film, triacetylcellulose film, etc. Examples of polyester films include polyethylene terephthalate film, polybutylene terephthalate film, and polyethylene naphthalate film. Examples of polyolefin films include polypropylene film, polyethylene film, and cycloolefin film. From the viewpoint of handling, polyimide film, polyester film, and polyolefin film are preferred, and considering heat resistance, polyimide film, polyethylene naphthalate film, and polyethylene terephthalate film are more preferred.

[0074] The adhesive layer provided on the surface of the second film 5 can be formed using various adhesives. Examples of adhesives include acrylic, urethane, silicone, elastomer, and ester types. From the viewpoint of heat resistance, acrylic, urethane, and silicone types are preferred, and furthermore, due to the low amount of impurities, acrylic and urethane adhesives are preferred. The thickness of the adhesive layer of the second film 5 is preferably 1 to 50 μm, more preferably 2 to 20 μm, and particularly preferably 3 to 10 μm. A thickness of 1 μm or more provides adhesion, and a thickness of 50 μm or less prevents the adhesive layer from protruding from the edges of the second film 5 during embedding. The adhesion strength to the water vapor barrier layer is preferably 1 to 300 gf / 25 mm, more preferably 2 to 200 gf / 25 mm, and even more preferably 3 to 100 gf / 25 mm relative to the water vapor barrier layer. The adhesion of the second film 5 to the water vapor barrier layer 4 can be adjusted by the type of adhesive, the amount applied, and the surface roughness. To reduce the adhesion, the surface roughness can be increased, while to increase the adhesion, the amount applied can be increased. The force can be measured, for example, by fixing the surface of the colorless resin composition layer 3 of the sealing sheet to a SUS plate and peeling off the second film 5 at a peeling angle of 180° and peeling speed of 300 mm / min in an environment of 23°C and 50% relative humidity.

[0075] The thickness of the second film 5 is preferably 12 to 188 μm, more preferably 12 to 100 μm, and even more preferably 20 to 60 μm. By setting the thickness within this range, the pressure transmission applied to the colorless resin composition layer during the pressing process is controlled, and the colorless resin composition layer flows uniformly, resulting in good embedding properties.

[0076] The aforementioned colorless resin composition layer 3 for embedding, the water vapor barrier layer 4, and the second film 5 each have a tensile storage modulus E' at 100°C. (100) It is preferable that the following relationship is satisfied. E'4 (100) / E'3 (100) is 100-1000 and, E'5 (100) / E'4 (100) 0.5~3 E'3 (100) The tensile storage modulus of the colorless resin composition layer 3 for embedding at 100°C is E'4 (100) The tensile storage modulus of the water vapor barrier layer 4 at 100°C is, E'5 (100) These represent the tensile storage modulus of the second film 5 at 100°C.

[0077] E'4 (100) / E'3 (100) It is preferably 100 to 1000, more preferably 200 to 800, and even more preferably 400 to 700. E'4 (100) and E'3 (100) This relationship ensures excellent embedding properties in the encapsulation target, while preventing irregularities originating from the light-emitting elements in the encapsulation target from affecting the surface of the water vapor barrier layer. A value of 100 or higher allows the water vapor barrier layer 4, which is sufficiently harder than the colorless resin composition layer 3, to uniformly and sufficiently press the colorless resin composition layer 3 into the recesses of the encapsulation target. A value of 1000 or lower prevents the water vapor barrier layer 4 from becoming too hard, thus preventing pressure imbalances due to irregularities in the encapsulation target from affecting the water vapor barrier layer 4 and creating an uneven surface. Also, E'5 (100) / E'4 (100) It is preferably 0.5 to 3, and more preferably 1.1 to 2.0. E'5 (100) and E'4 (100) This relationship prevents the formation of an uneven pattern on the surface of the water vapor barrier layer 4 that corresponds to the irregularities of the object being sealed. In a more preferable range, since the second film 5 is as hard as or slightly harder than the water vapor barrier layer 4, the second film 5 can further assist in embedding the resin composition 3. The respective tensile storage moduli were measured using a dynamic viscoelasticity measuring device DVA-200 / L2 (manufactured by IT Measurement Control Co., Ltd.) at a frequency of 10 Hz, a measurement temperature range of -50 to 150°C, a heating rate of 5°C / min, and in tensile mode. The storage moduli at 100°C were then read.

[0078] The sealing layer sheet 1 can be obtained, for example, as follows. A coating liquid for forming a colorless resin composition layer for embedding is applied to one side of the first film 2 and dried to form a colorless resin composition layer 3 for embedding. Separately, a water vapor barrier layer 4 is laminated to one side of the second film 5. Then, the colorless resin composition layer 3 for embedding and the water vapor barrier layer 4 are laminated together. Alternatively, a coating liquid for forming a colorless resin composition layer for embedding is applied to one side of the first film 2 and dried to form a colorless resin composition layer 3 for embedding. Next, a water vapor barrier layer 4 is laminated onto the colorless resin composition layer 3 for embedding. Then, the second film 5 is laminated onto the water vapor barrier layer 4. Alternatively, a water vapor barrier layer 4 is laminated on one side of the second film 5. Next, a coating liquid for forming a colorless resin composition layer for embedding is applied to the water vapor barrier layer 4 and dried to form a colorless resin composition layer 3 for embedding. Then, the colorless resin composition layer 3 for embedding is Stack two films. For coating the colorless resin composition layer for embedding, known methods such as the roll coater method, comma coater method, lip coater method, die coater method, reverse coater method, silkscreen method, and gravure coater method can be used. After coating, it can be dried using a hot air oven, infrared heater, or the like.

[0079] A roll-shaped sealing layer forming sheet can be obtained by winding the sealing layer forming sheet 1 onto a core in a roll shape after manufacturing it, or while manufacturing the sealing layer forming sheet. The winding length can be designed according to the application. From the viewpoint of increasing productivity, it is preferable to have a winding length of 30 m or more, and more preferably 100 m or more. From the viewpoint of manufacturing yield, it is preferable to have a winding length of 10,000 m or less. The thickness of the sealing layer forming sheet is preferably 60 to 200 μm from the viewpoint of ease of winding when winding it into a roll shape.

[0080] As for how to wind the roll-shaped sealing layer forming sheet 1, the sheet shown in Figure 1(1) can be wound with the first film 2 on the core side, or, as shown in Figure 1(2), the first film 2 can be superimposed on the side of the second film 5 that is not in contact with the water vapor barrier layer 4, and the colorless resin composition layer 3 for embedding can be wound with the core side. In the latter case, from the second pass onward, the first film 2 comes into contact with the colorless resin composition layer 3 for embedding. When using the roll-shaped sealing layer forming sheet 1, the first film can be peeled off immediately when the roll is unrolled, exposing the colorless resin composition layer 3 for embedding. This is preferable because it improves the productivity of the component 8 in which the light-emitting element 7 is sealed. The latter roll-shaped sealing layer-forming sheet 1 can also be obtained by laminating the first film 2 and the second film 5, laminating a water vapor barrier layer 4 on the other side of the second film 5, applying a coating liquid for forming a colorless resin composition layer for embedding to the other side of the water vapor barrier layer 4, drying it to form a colorless resin composition layer for embedding, and then rolling it up with the colorless resin composition layer 3 for embedding on the inside.

[0081] [Component 8 containing multiple light-emitting elements] Next, we will describe the component 8 (hereinafter also referred to as the sealed component) in which the multiple light-emitting elements are sealed. As described above, the sealed member 8 of the present invention has a substrate 6 and a plurality of light-emitting elements 7 placed on the substrate 6 at intervals, and at least a portion of the depth direction of the individual gaps between the light-emitting elements 7 has a refractive index of 1.51 ± 0.03 and a water vapor transmission rate of 100 [g / (m³] 2 The side of the multiple light-emitting elements that is embedded with a cured product 3' of a colorless resin composition 3 for embedding (24 hours or longer) is the cured product 3', and the refractive index is 1.53 ± 0.03 and 100 [g / (m 2 It is covered in a water vapor barrier layer 4 with a duration of less than 24 hours. Furthermore, the sealed member 8 may have at least a portion of the depth direction of the individual gaps between the light-emitting elements 7, and / or at least a portion of the bottom surface of the individual gaps, filled with a cured colored resin composition 9' for filling, while the remaining portion of the individual gaps between the light-emitting elements 7 may be filled with a cured colorless resin composition 9' for filling.

[0082] Figure 2 shows various forms of the gaps between the light-emitting elements 7 in the sealed member 8. Figure 2(1) shows a component in which there is no colored resin composition cured product 9' in the gap between the light-emitting elements 7, and the gap is filled with a colorless resin composition layer cured product 3', and the cured product 3' is further covered with a water vapor barrier layer 4. Figures 2(2) to 2(5) show a configuration in which a cured product 9' of a colored resin composition, i.e., a color-enhancing layer such as a reflective layer or a color-mixing prevention layer, is present in at least a portion of the gap between the light-emitting elements 7. The color-enhancing layer is placed on the sides of the light-emitting elements 7 other than the display side (light-emitting surface, the top side in the figure) or on the bottom of the gap, and there are no restrictions on the method of placement. For example, as in Figure 2(2), the cured product 9' of the colored resin composition may not completely cover the sides of the light-emitting elements 7, or as in Figure 2(3), the light-emitting elements may not completely cover the sides of the light-emitting elements. The cured colored resin composition 9' filling the gap can cover the sides of the light-emitting element 7, while the surface of the cured material 9' in the gap may have irregularities created by etching or other processes. Alternatively, as shown in Figure 2(4), the cured colored resin composition 9' can thinly cover the substrate on the sides of the light-emitting element 7 and the bottom of the gap, while having a deep space in the depth direction in the middle of the gap. Or, as shown in Figure 2(5), the cured colored resin composition 9' can be placed in the gap without contacting the light-emitting element 7. The shape of the object to be embedded by the colorless resin composition layer 3 may change depending on the presence or absence of the cured product 9' of the colored resin composition and the shape of the cured product 9' of the colored resin composition. However, the interface between the cured product 3' of the colorless resin composition layer and the water vapor barrier layer 4 laminated on the cured product 3' of the colorless resin composition layer, and the surface of the water vapor barrier layer 4, are preferably as parallel as possible to the surface of the substrate 6 on which the light-emitting element 7 is placed, regardless of the shape of the gap that is to be sealed, and the surface of the water vapor barrier layer 4 is preferably as smooth as possible.

[0083] <Board 6> The material of the substrate 6 on which the light-emitting element 7 is mounted is not particularly limited, but examples include acrylic, urethane, polycarbonate, epoxy, polyimide, glass, glass epoxy, paper, cloth, aluminum, ceramic, or polyethylene terephthalate. It can also be used for transparent display applications, and from the viewpoint of cost, durability, and transparency, glass is preferred, and it is preferable that it has electrode portions. To prevent corrosion of the light-emitting element by ionic components, alkali-free glass is preferred as the glass material. Furthermore, the refractive index of the glass substrate is preferably 1.49 to 1.59, and more preferably 1.50 to 1.55. The refractive index can be adjusted, for example, by adjusting the ratio of silicon oxide, aluminum oxide, and boron oxide, and generally, the refractive index can be increased by increasing the ratio of boron oxide. In addition to boron oxide, the refractive index can also be increased by incorporating alkaline earth oxides.

[0084] <Light-emitting element 7> Examples of light-emitting elements 7 placed on the substrate 6 include LED elements, and microLED elements are preferred. The micro-LED element has a thickness of 100 μm or less and a planar area of ​​40,000 μm². 2 The following are preferred: a thickness of 50 μm or less and a planar area of ​​10,000 μm². 2 The following are more preferable: a thickness of 20 μm or less and a planar area of ​​2,500 μm². 2 below Even better is the material. By mounting multiple of these LED elements on a substrate with wiring and circuits, a display is formed that uses multiple optical semiconductor elements as light sources. The spacing between micro-LED elements mounted on the substrate is, for example, 10 to 5,000 μm. When red, green, and blue micro-LED elements are mounted on the substrate as a set of 1 pixel, the spacing between pixels is, for example, 10 to 2,000 μm, preferably 20 to 1,800 μm, and more preferably 500 to 1,500 μm. The spacing between micro-LED elements within a single pixel is, for example, 10 to 200 μm, preferably 10 to 100 μm, and more preferably 20 to 60 μm. The number of microLED elements is not particularly limited. In display applications, the number of microLED elements used is determined by the display size and the number of pixels. Furthermore, the emitted color of the microLED elements is not particularly limited, and examples of colors include red, green, blue, white, and yellow. MicroLEDs are formed from LED elements such as GaAs, GaP, AlGaInP, and InGaN, as well as a sealing resin, package substrate, electrodes, etc., and their operating temperature is 25 to 60°C.

[0085] <Cured product 3' of the colorless resin composition layer 3 for embedding> The cured product 3' of the colorless resin composition layer 3 for embedding completely encloses the LED element and the substrate, and the LED element, the substrate, and the brightness-enhancing layer without any gaps, and high transparency and water vapor barrier properties are required. It can be done. As mentioned above, it is important that the refractive index of the cured colorless resin composition layer is 1.51 ± 0.03, and it is preferable that the difference between this refractive index and that of the substrate on which the light-emitting element is mounted is as small as possible.

[0086] As explained in Figure 3-1, the thickness T1 of the cured product 3' of the colorless resin composition layer between the top surface of the LED element 7 and the bottom surface of the water vapor barrier layer 4 is preferably 5 to 30 μm, and 7 to 25 It is more preferably μm, and particularly preferably 10-20 μm. T1 is 30 μm or less. This improves transparency. Since T1 is 5μ or more, the top surface of the LED element 7 and L The uneven shape created by the bottom surface of the gap between the ED elements 7 is less likely to affect the surface of the water vapor barrier layer 4, thereby improving the water vapor barrier properties. Being within a more preferable range allows the above objective to be satisfied at a high level. Similarly, in the case where a portion of the gap between the LED elements 7 is filled by the cured product 9' of the colored resin composition layer, as shown in Figure 3-2, it is preferable that the thickness T1 of the cured product 3' of the colorless resin composition layer between the top surface of the LED element 7 and the bottom surface of the water vapor barrier layer 4 be within the range described above. Oh, the same applies to the cases shown in Figures 2(3) to (5).

[0087] <Water vapor barrier layer 4> As shown in Figures 3-1 and 3-2, the thickness T2 of the water vapor barrier layer 4 in the LED encapsulation member 8 is as described above. Furthermore, the combined thickness T1 of the cured colorless resin composition layer 3' and the thickness T2 of the water vapor barrier layer 4 is preferably 5 to 50 μm, more preferably 7 to 30 μm, and even more preferably 10 to 15 μm. Being within this more preferable range allows for sealing the LED elements and substrate within the component while maintaining a high level of water vapor barrier properties and transparency, and satisfying the thinness required for displays.

[0088] <Cured product 9' of colored resin composition 9 for embedding> As the colored resin composition 9 for embedding, a coating solution containing at least resin (A) and polymerization initiator (C), and further containing a black pigment or a white pigment, can be applied and dried to form a sheet, similar to the case of the colorless resin composition layer 3 described above. Typical black pigments include carbon black, and typical color pigments include titanium dioxide and zinc oxide. Based on Figure 10, various methods for forming a cured product 9' of a colored resin composition between the light-emitting elements 7 will be described. For example, as shown in Figures 10(1-a) and (1-b), a sheet of colored resin composition 9, which is sufficiently thick compared to the height of the light-emitting elements 7, is embedded in the gaps between the light-emitting elements 7 in the encapsulation target β1 by pressing or the like, and then cured as shown in Figure 10(1-c). Next, the hardened material 9' is removed to approximately the same height as the light-emitting element 7 by laser etching, chemical etching, polishing, etc., to obtain the encapsulation target β3 (see Figure 9) as shown in Figure 10(1-d). Furthermore, by thinning or excavating the hardened material 9' in the gap between the light-emitting elements 7, a encapsulation target β2 (see Figures 5-6) can be obtained as shown in Figures 10(1-e) and 10(1-f). Laser etching offers superior processing accuracy, while chemical etching offers superior productivity. For micro-LED elements requiring fine processing, laser etching is preferable.

[0089] Alternatively, as shown in Figure 10(2-a), a sheet of colored resin composition 3 that is relatively thin compared to the height of the light-emitting element 7 can be placed on the top surface of the light-emitting element 7, and by using a vacuum forming method such as TOM molding, the colored resin composition 3 can be arranged along the surfaces of the light-emitting element 7 and the substrate 6 as shown in Figure 10(2-b). After curing the resin composition as shown in Figure 10(2-c) Furthermore, a encapsulation target β2 (see Figure 7) can be prepared as shown in Figure 10(2-d) or Figure 10(2-d') by laser etching, chemical etching, polishing, etc.

[0090] Furthermore, a encapsulation target β2 in which the cured product 9' of the colored resin composition, as shown in Figure 8, is located in the gap between the light-emitting elements 7 but hardly touches the sides of the light-emitting elements 7, can be obtained, for example, by using the laser lift-off method. Specifically, as shown in Figure 10(3-a), a colored resin composition 9 of a desired size is placed on the release film at a position corresponding to the gap between the light-emitting elements 7. Next, as shown in Figure 10(3-b), the colored resin composition 9 is brought into contact with the substrate 6 in the gap between the light-emitting elements 7, and then a laser is irradiated from behind the release film to detach the colored resin composition 9 from the release film, as shown in Figure 10(3-c). By curing the colored resin composition, a encapsulation target β2 as shown in Figure 10(3-d) can be prepared.

[0091] The member 8, in which multiple light-emitting elements 7 are sealed, can be formed in various ways. For example, as shown in Figure 4(I-1), a encapsulation target β1 is prepared in which a plurality of light-emitting elements 7 (e.g., micro-LED elements) are provided on a substrate 6 at predetermined intervals. Separately, prepare the sealing layer-forming sheet 1 as shown in Figure 4(II). Figure 4(III) As shown, the first film 2 is peeled off from the sealing layer forming sheet 1, exposing the colorless resin composition layer 3 for embedding. The peeling method for removing the first film 2 from the sealing layer forming sheet 1 is not particularly limited. For example, the sealing layer forming sheet 1 can be prepared in a roll shape, and the sealing layer forming sheet 1 can be unwound and the first film 2 can be peeled off simultaneously using a roll-to-roll method.

[0092] Next, as shown in Figure 4(IV), the exposed colorless resin composition layer 3 is placed so as to directly cover the upper surface of the micro-LED element 7 in the encapsulation target β1. Step (IV) is preferably performed under vacuum or reduced pressure in order to prevent gaps from forming at the contact surface between the upper surface of the micro-LED element 7 and the colorless resin composition layer 3, and to embed the colorless resin composition layer 3 so that no gaps will form between the micro-LED elements 7 in the next step. Furthermore, it is preferable to preheat the colorless resin composition layer in step (IV) in order to increase its fluidity in the next step. The heating temperature is preferably 10°C or more higher than the Tg of the resin composition, and more preferably 30°C or more higher. That is, from the Tg of the resin composition described later, 30 to 200°C is preferred, 40 to 150°C is more preferred, 50 to 130°C is even more preferred, and 60 to 110°C is most preferred. Then, as shown in Figure 4(V-1), the colorless resin composition layer 3 is made to flow by pressing and filled between the micro-LED elements 7. It can also be filled around the micro-LED elements 7. When pressing, it is preferable to heat the colorless resin composition layer 3 to increase its fluidity, but if the temperature is too high, the colorless resin composition layer 3 will harden and hinder filling, so it is preferable that the temperature be lower than the next step (VI), i.e., about the same as the temperature of step (IV). From the viewpoint of the fillability of the colorless resin composition layer 3, 30 to 200°C is preferred, 40 to 150°C is more preferred, 50 to 130°C is even more preferred, and 60 to 110°C is most preferred.

[0093] As shown in Figure 4(VI), active energy rays such as ultraviolet light or electron beams, or heat can be used to cure the filled colorless resin composition layer 3. Curing by heating is particularly preferred because it is less likely to result in uneven or insufficient irradiation. The heating temperature is preferably such that it allows for rapid curing and also suppresses the shrinkage of the water vapor barrier layer 4, i.e., 60 to 250°C is preferred, 70 to 200°C is more preferred, 80 to 150°C is even more preferred, and 90 to 120°C is most preferred. When curing the colorless resin composition layer 3, it can be cured under pressure as in step (VI), or it can be cured without any particular pressure. A colorless resin composition filled between and around the micro-LED elements 7. By curing the layers, the cured product 3' of the colorless resin composition layer and the barrier layer 4 seal the target β1, and a member 8 containing multiple light-emitting elements can be obtained.

[0094] Alternatively, a member 8 can be obtained in which multiple light-emitting elements are sealed by filling at least a portion of the depth of the individual gaps between the micro-LED elements 7 in the encapsulation target β1, and / or at least a portion of the bottom surface of the individual gaps, with the cured product 9' of the colored resin composition 9 for embedding in the manner described above (see Figure 10), and using a separately prepared encapsulation layer forming sheet 1 as in the case of Figure 4, the cured product 3' of the resin composition layer and the barrier layer 4 seal the encapsulation target β2, as shown in Figures 5 to 8. Furthermore, the individual gaps between the micro-LED elements 7 in the encapsulation target β1 are filled up to the height of the micro-LED elements 7 with a cured colored resin composition 9' for embedding in the manner described above, to prepare the encapsulation target β3 (see Figure 10). Then, using a separately prepared encapsulation layer forming sheet 1, as in the case of Figure 4, the cured resin composition layer 3' and barrier layer 4 encapsulate the encapsulation target β3, as shown in Figure 9, to obtain a member 8 in which multiple light-emitting elements 7 are encapsulated.

[0095] [Examples] The present disclosure will be described in detail below with reference to examples and comparative examples, but the present disclosure is not particularly limited to the examples. In the following description, "parts" and "%" refer to "parts by mass" and "% by mass," respectively, unless otherwise specified.

[0096] Manufacturing of resin (A) solution Manufacturing Example 1 [(Meth)acrylic resin (A-1) solution manufacturing example] A reaction vessel (hereinafter simply referred to as "reaction vessel") equipped with a stirrer, thermometer, reflux condenser, dropping device, and nitrogen inlet tube contains 80 parts ethyl acetate, 25 parts methyl methacrylate, 73 parts n-butyl methacrylate, 2 parts acrylic acid, and 2,2'-azobisisobutyropropyl alcohol as an initiator. 0.1 parts of nitrile were added, and the atmosphere in the reaction vessel was replaced with nitrogen gas. Then, under a nitrogen atmosphere, the mixture was heated to 65°C with stirring, and polymerization was carried out at the same temperature for 4 hours. After that, an amount of glycidyl methacrylate equivalent to half the amount of carboxyl groups of acrylic acid was added, and the mixture was stirred at 60°C for 24 hours. After the reaction was complete, the mixture was cooled and diluted with ethyl acetate to obtain a solution of (meth)acrylic resin (A-1) with a weight-average molecular weight (Mw): 100,000, a glass transition temperature (Tg): 50°C, and a solids content of 50%. Furthermore, the weight-average molecular weight (Mw), Tg, refractive index, water vapor transmission rate, moisture absorption rate, and elastic modulus at 100°C were determined according to the methods described later.

[0097] Manufacturing Example 2 [Example of manufacturing a solution of (meth)acrylic resin (A-2)] This is the same as Production Example 1, except that the amount of 2,2'-azobisisobutyronitrile was changed to 0.3 parts. Polymerization was carried out in the manner described above, and after polymerization, half the amount of glycidyl methacrylate was reacted with the carboxyl groups of the acrylic acid in the same manner as in Production Example 1 to produce a solution of (meth)acrylic resin (A-2) with a weight-average molecular weight (Mw): 50,000, Tg: 46°C, and solids content: 50%.

[0098] Manufacturing Example 3 [Manufacturing Example of (Meth)acrylic Resin (A-3) Solution] The preparation method is the same as in Production Example 1, except that 0.05 parts of 2,2'-azobisisobutyronitrile were used instead. Polymerization was carried out, and after polymerization, half the amount of glycidyl methacrylate was reacted with the carboxyl groups of the acrylic acid in the same manner as in Production Example 1 to produce a solution of (meth)acrylic resin (A-3) with a weight-average molecular weight (Mw): 220,000, Tg: 52°C, and solids content: 50%.

[0099] Manufacturing Example 4 [Example of manufacturing a solution of (meth)acrylic resin (A-4)] The monomer composition is 30 parts methyl methacrylate, 64 parts n-butyl methacrylate, and acrylic acid. The amount of lylic acid was changed to 6 parts, and the initiator was changed to 0.05 parts of 2,2'-azobisisobutyronitrile. Polymerization was carried out in the same manner as in Production Example 1, except for the components mentioned above. After polymerization, half the amount of glycidyl methacrylate was reacted with the carboxyl groups of the acrylic acid in the same manner as in Production Example 1 to produce a solution of (meth)acrylic resin (A-4) with a weight-average molecular weight (Mw): 220,000, Tg: 55°C, and solids content: 50%.

[0100] Manufacturing Example 5 [Manufacturing Example of (Meth)acrylic Resin (A-5) Solution] The monomer composition is 25 parts methyl methacrylate, 68 parts n-butyl methacrylate, 2 parts acrylic acid, and 5 parts 2-(dimethylamino)ethyl acrylate, with the initiator being 2,2'-A Polymerization was carried out in the same manner as in Production Example 1, except that 0.15 parts of zobisisobutyronitrile were used. After polymerization, half the amount of glycidyl methacrylate was reacted with the carboxyl group of the acrylic acid in the same manner as in Production Example 1 to produce a solution of (meth)acrylic resin (A-5) with a weight-average molecular weight (Mw): 110,000, Tg: 47°C, and solids content: 50%.

[0101] Manufacturing Example 6 [Manufacturing Example of (Meth)acrylic Resin (A-6) Solution] Polymerization was carried out in the same manner as in Production Example 1, except that the carboxyl groups were not reacted with glycidyl methacrylate after polymerization, to obtain a solution of (meth)acrylic resin (A-6) with a weight-average molecular weight (Mw): 100,000, Tg: 48°C, and solids content: 50%.

[0102] Manufacturing Example 7 [Manufacturing Example of (Meth)acrylic Resin (A-7) Solution] Except for changing the monomer content to 98 parts n-butyl acrylate and 2 parts acrylic acid, and changing the initiator to 0.1 parts 2,2'-azobisisobutyronitrile, the process was carried out in the same manner as in Production Example 1. After polymerization, half the amount of glycidyl methacrylate was reacted with the carboxyl groups of the acrylic acid in the same manner as in Production Example 1 to obtain a solution of (meth)acrylic resin (A-7) with a weight-average molecular weight (Mw): 200,000, Tg: -17°C, and solids content: 50%.

[0103] Manufacturing Example 8 [Manufacturing Example of (Meth)acrylic Resin (A-8) Solution] A reaction vessel (hereinafter simply referred to as "reaction vessel") equipped with a stirrer, thermometer, reflux condenser, dropping device, and nitrogen inlet tube contains 80 parts ethyl acetate, 22 parts n-butyl acrylate, 76 parts n-butyl methacrylate, 2 parts acrylic acid, and 2,2'-azobisisobutyl as an initiator. 0.1 parts of ronitrile were added, and the atmosphere in the reaction vessel was replaced with nitrogen gas. Then, the reaction was started by heating to 65°C while stirring under a nitrogen atmosphere. Subsequently, half the equivalent amount of glycidyl methacrylate was added to the carboxyl group of the acrylic acid in the same manner as in the production of (meth)acrylic resin (A-1), and the reaction was carried out at 65°C for 4 hours. After the reaction was complete, it was cooled and diluted with ethyl acetate to obtain a solution of (meth)acrylic resin (A-8) with a weight-average molecular weight (Mw): 200,000, Tg: 10°C, and solids content: 50%.

[0104] Manufacturing Example 9 [Manufacturing Example of (Meth)acrylic Resin (A-9) Solution] The monomer composition was 25 parts methyl methacrylate, 58 parts n-butyl methacrylate, 15 parts N-vinyl-2-pyrrolidone (hereinafter also referred to as NVP), and 2 parts acrylic acid, and the initiator was 0.1 parts 2,2'-azobisisobutyronitrile. Otherwise, the process was carried out in the same manner as in Production Example 1, except that nitrogen was used. The reaction was initiated by heating to 65°C while stirring under atmospheric conditions. The reaction solution was then reacted at 65°C for 4 hours to complete the reaction, cooled, and diluted with ethyl acetate to obtain a solution of (meth)acrylic resin (A-9) with a weight-average molecular weight (Mw): 100,000, Tg: 46°C, and solids content: 50%.

[0105] [Weight average molecular weight (Mw)] The weight-average molecular weight (Mw) was determined by using the Shimadzu LC-GPC system, which uses polystyrene with a known molecular weight as a standard substance for calculation. Equipment name: Shimadzu Corporation, LC-GPC system "Prominence" Columns: Four Tosoh GMHXL columns and one Tosoh HXL-H column were connected together. Mobile phase solvent: tetrahydrofuran Flow rate: 1.0mL / min Column temperature: 40℃

[0106] [Glass transition temperature (Tg: temperature of maximum tanδ)] The resin solutions obtained in each manufacturing example were applied to the release surface of a release film, dried at 100°C for 2 minutes to create a resin sheet with a thickness of 50 μm, cut to a size of 0.5 cm × 2 cm, and the release film was peeled off to prepare the sample for measurement. Dynamic viscoelasticity was measured using a dynamic viscoelasticity measuring instrument DVA-200 / L2 (manufactured by IT Measurement Control Co., Ltd.) at a frequency of 10 Hz, a measurement temperature range of -50 to 150°C, a heating rate of 5°C / min, and in tensile mode. The storage modulus, loss modulus, and loss tangent (tanδ) were plotted. The peak top temperature (maximum value of tanδ) of the loss tangent (tanδ) was read from the obtained graph.

[0107] <Colorless resin composition layer for embedding [CR]> [CR-1]~[CR-5] As shown in Table 1, 200 parts of a solution of resins (A-1) to (A-5) with a solid content of 50%, 0.3 parts of initiator C-1, and methyl ethyl ketone were added to bring the solid content to 40%. This solution was then applied with an applicator to the release-treated surface of the first film FA-1, which had been cut into 15 cm squares. The solvent was removed by drying in a drying oven at 80°C for 5 minutes to obtain a colorless resin composition layer [CR-1] to [CR-5] with a thickness of 10 μm for embedding. The measurement of Tg, refractive index, etc. of the resin composition layer will be described later. Note that the prescriptions in the table represent the solid content.

[0108] [CR-6] As shown in Table 1, a colorless resin composition layer [CR-6] with a thickness of 10 μm was formed on the first film FA-1 in the same manner as for the resin composition layer [CR-1], except that the mixture consisted of 200 parts of a solution of resin (A-6) with a solid content of 50% and 1 part of initiator C-3.

[0109] [CR-7]~[CR-25], [CR-101]~[CR-107] A colorless resin composition layer for embedding was formed according to the formulations shown in Tables 2-4 (indicated by solid content).

[0110] [Other transparent resin solutions] • B-1 A polyester resin (Byron 200, Mw: 20,000, Tg: 67°C) and toluene were mixed in a 1:1 ratio to obtain a polyester resin solution with a solid content of 50%. • B-2 Polyurethane resin (Polysic UP, Mw: 60000, Tg: 20℃, manufactured by Sanyo Chemical Industries, Ltd.) • B-3 Rubber-based resin (styrene-ethylene-propylene polymer: SEPTON20) Toluene was added to 63 (Mw: 120,000, Tg: 65°C, manufactured by Kuraray Co., Ltd.), dissolved in a disperser at 60°C, and returned to room temperature to obtain a rubber-based resin solution with a solid content of 20%. The Mw and Tg values ​​for the above resins were determined in the same manner as for resin (A-1).

[0111] [Initiator / Hardener C] • C-1: Di-t-butyl peroxide (half-life temperature: 123°C) • C-2: 1,1-di(tert-butylperoxy)cyclohexane (half-life temperature: 84°C) • C-3: Polyisocyanate (manufactured by Asahi Kasei, Duranate TPA100, HDI nulate, 100% solids content)

[0112] n [Other Additives U] [Example of dispersion (U-1) production] 95 parts of alumina AKP-G07 manufactured by Sumitomo Chemical (manufactured by Mitsubishi Chemical Corporation), 10 parts of a resin (A-1) solution with a solid content of 50%, and 400 parts of methyl ethyl ketone as a solvent were mixed and pre-dispersed in a disperser. Then, the final dispersion was carried out for 2 hours in a 0.6 L volume Dynomill filled with 1800 g of zirconia beads with a diameter of 0.3 mm, and the zirconia beads were removed to obtain an alumina dispersion (U-1) with a solid content of 20%.

[0113] (U-2) Urethane acrylate oligomer Mw:1500 6-functional (U-3) Urethane acrylate oligomer Mw:3000 Trifunctional • (U-4) Ethyleneimine (P1000, manufactured by Nippon Shokubai Co., Ltd.) • (U-5) N-vinyl-2-pyrrolidone (manufactured by Tokyo Chemical Industry Co., Ltd.)

[0114] [Table 1]

[0115] [Table 2]

[0116] [Table 3]

[0117] [Table 4]

[0118] [Glass transition temperature (Tg: temperature of maximum tanδ)] Each embedding resin composition layer was peeled off from the first film FA-1 and measured in the same manner as for resin (A-1).

[0119] [thickness] The total thickness of the first film FA-1 and each colorless resin composition layer for embedding provided on the first film FA-1 was measured with a thickness gauge (Mitutoyo, probe size: 10 mm, measuring force: 1.0 N), and the value obtained by subtracting the thickness of the first film FA-1 from the measured value was used for each embedding. The thickness of the colorless resin composition layer was determined accordingly.

[0120] [Refractive index] The refractive index was defined as the value measured at a measurement wavelength of 594 nm using a prism coupler (Metricon 2010M) on the surface of each embedded resin composition layer provided on the first film FA-1, under conditions of 25°C and 50% RH.

[0121] [Water vapor transmission rate] <Colorless resin composition layer for embedding> Since the colorless resin composition layer used for embedding is difficult to isolate, the water vapor permeability was determined as follows. Specifically, for the entire structure of the first film FA-1 and each colorless resin composition layer for embedding provided on the first film FA-1, a water vapor transmission rate measuring device C390H manufactured by Labthink was used, with the surface in contact with water vapor during measurement being the side facing the colorless resin composition layer, and the transmission area being 5 cm². 2 Under measurement conditions of 40℃ and 90%RH, the water vapor transmission value P[g / (m³] was obtained 24 hours after measurement. 2 The value of the water vapor transmission rate P2[g / (m³)) was read separately for the first film FA-1 under the same conditions. 2 The following was measured: a colorless resin composition layer. Water vapor transmission value P3[g / (m³] 2 The value of (day) was calculated according to the following formula. P3 = |P × P2| / |P2 - P|

[0122] <Water vapor barrier layer> For the water vapor barrier layer, the water vapor permeability was measured independently under the same conditions. <Sealing layer precursor> For the sealing layer precursor, the surface exposed to water vapor during measurement was the side with the colorless resin composition layer, and the water vapor permeability was measured under the same conditions.

[0123] [Moisture absorption rate] Each resin composition layer for embedding, along with the first film FA-1, was cut into 5cm squares. The first film FA-1 side was placed on a stainless steel plate and left standing at 80°C for 120 minutes. After that, it was removed to an environment of 23°C and 50%RH, and its mass was measured after 15 minutes. Then, it was left standing at 40°C and 90%RH for 24 hours to allow it to absorb moisture, and after that, it was removed to an environment of 23°C and 50%RH, and its mass was measured after 15 minutes. The moisture absorption rate was determined from the change in mass before and after moisture absorption based on the following formula. When measuring the mass, the value was recorded to the third decimal place, rounded to the fourth decimal place. Moisture absorption rate (%) = [(Mass after moisture absorption ÷ Mass before moisture absorption) - 1] × 100

[0124] [Modulus of elasticity at 100°C (Pa)] The value of the storage modulus plotted at 100°C during Tg measurement.

[0125] [b value] Each resin composition layer for embedding was peeled from the first film FA-1, laminated onto a glass plate, and measured in transmission mode using a colorimeter (ZE6000, manufactured by Nippon Denshoku Kogyo Co., Ltd., light source: D60) with the glass plate, and the b value was read.

[0126] [HAZE] Each resin composition layer for embedding was peeled from the first film FA-1, laminated onto a glass plate at room temperature, and measured and evaluated using a haze meter (NDH8000, manufactured by Nippon Denshoku Kogyo Co., Ltd., light source: D60) along with the glass plate. Since the b-value and HAZE of the glass plate itself were both extremely small, the values ​​measured for the glass plate as a whole were used as the values ​​for each resin composition layer used for embedding.

[0127] <Water vapor barrier layer SB> <SB-1~SB-6> A cycloolefin resin was introduced into a Toyo Seiki Plastmill equipped with a 25mm wide fishblow-type T-die at its tip at a cylinder temperature of 230°C. Under the conditions of T-die temperature of 220°C, discharge rate of 10g / min, T-die clearance of 30μm, and winding speed of 2m / min, a cycloolefin film with a thickness of 7μm and a width of 20cm was obtained. Furthermore, by cutting both sides perpendicular to the film's flow direction (MD) (TD), a cycloolefin film SB-1 with a thickness of 7 μm and a square length of 15 cm was obtained. Under similar temperature and discharge conditions, cycloolefin films with thicknesses of 10 μm (SB-2), 13 μm (SB-3), 20 μm (SB-4), 30 μm (SB-5), and 50 μm (SB-6) were obtained by adjusting the winding speed and T-die clearance.

[0128] <sb-7>,<SB-101~SB-103> 100g of urethane acrylate (Mw:2000, 10-functionality) was mixed with 1g of the initiator ESACURE ONE (manufactured by DKSH) and 50g of methyl ethyl ketone using a disperser to prepare the coating solution. The coating solution is applied to the release film using an applicator so that it dries to a thickness of 30 μm, dried at 80°C for 3 minutes, and then heated with a high-pressure mercury lamp at 80 W / cm². 2 The output is cured and placed on the release film. A cured urethane acrylate film with a thickness of 30 μm, SB-7, was obtained. Furthermore, by changing the grit size of the applicator used during coating, cured urethane acrylate films with thicknesses of 20 μm (SB-101), 15 μm (SB-102), and 10 μm (SB-103) were obtained.

[0129] • SB-104 Biaxially oriented polypropylene (OPP) film, 20μm thick (OPP sheet manufactured by Naniwa Paper Co., Ltd.) • SB-105 Polyethylene terephthalate (PET) film, 12μm thick • SB-106 Aluminum oxide vapor-deposited PET film, 12μm thick (Toray Barrierox)

[0130] The refractive index, water vapor transmission rate, moisture absorption rate, b-value, and haze were measured using the same apparatus and conditions as for the resin composition layer used for embedding. For SB-1 to SB-7, the release film was peeled off, the water vapor barrier layer was isolated, and then measured. Table 5 shows the refractive index, water vapor permeability, etc., of each water vapor barrier layer.

[0131] [Table 5]

[0132] [Daiichi Film FA] • FA-1 KOBATECH RF 40TLGN (manufactured by Kobayashi Co., Ltd.), thickness 40 μm, Ra: 0.14 μm, Rδc: 0.21 μm • FA-2 KOBATECH RF 40TLSN (manufactured by Kobayashi Co., Ltd.), thickness 40 μm, Ra: 0.31 μm, Rδc: 0.50 μm • FA-3 KOBATECH RF 40TLMN (manufactured by Kobayashi Co., Ltd.), thickness 40 μm, Ra: 1.10 μm, Rδc: 1.52 μm FA-4 Cosmopeel E7002 (manufactured by Toyobo Co., Ltd.), thickness 50 μm, Ra: 0.01 μm, Rδc: 0.03 μm • FA-5 PG7H (manufactured by Gōdō Jushi Kōgyō Co., Ltd.), thickness 50 μm, Ra: 2.73 μm, Rδc: 4.41 μm

[0133] <Surface roughness Ra, difference in cutting level of contour curve Rδc> The surface roughness Ra in the first film described above is calculated by taking a section of the roughness curve with a measurement length L in the direction of its centerline, and taking the arithmetic mean of the absolute values ​​of the deviations between the centerline of this section and the roughness curve. The cross-section level difference Rδc of the contour curve is the difference in the height direction level that coincides with any two load length ratios within the roughness curve, and the two load length ratios were defined as 25% and 75%. Specifically, measurement data was acquired using a laser microscope (Keyence Corporation, VK-X100), and the acquired measurement data was imported into analysis software (analysis application "VK-H1XA" equipped with the JIS B0601:2013 surface texture measurement module "VK-H1XR", both manufactured by Keyence Corporation), and the JIS B0601:2013 surface texture measurement was performed to calculate the results. To determine the roughness curve from the measured cross-sectional curve obtained by measurement, a λc contour curve filter was used to remove short wavelengths such as noise, and a λs contour curve filter was used to remove long wavelengths such as undulations. Depending on the surface condition being measured, the surface roughness measurement in the analysis application was set to either a 2.5 μm λs contour curve filter and a 0.8 mm λc contour curve filter, an 8 μm λs contour curve filter and a 2.5 mm λc contour curve filter, or a 25 μm λs contour curve filter and an 8 mm λc contour curve filter, and the surface roughness Ra and the difference in cutting levels of the contour curve Rδc were measured.

[0134] [Second Film FB] • FB-1: A slightly tacky film (60 μm thick, manufactured by Toyo Chem, LE951) with an acrylic-based slightly tacky layer on one side of a polyester film. Elastic modulus at 100°C: 1.2 × 10⁻⁶ 9 Pa • FB-2 polyester film (thickness 50 μm, manufactured by Toray, Lumirror #50), modulus of elasticity at 100°C: 9.8 × 10 8 Pa • FB-3 A slightly tacky film (thickness 50 μm, manufactured by San-ei Chemicals, PAC3-50) with an elastomer-based slightly tacky layer on one side of a polyethylene film, modulus of elasticity at 100°C: 1.9 × 10⁻⁶ 7 Pa • FB-4 A slightly adhesive film (thickness 50 μm, manufactured by Nipper, OPP-SD3) with a silicone-based slightly adhesive layer on one side of a polypropylene film, modulus of elasticity at 100°C: 2.1 × 10 8 Pa

[0135] [Example 1] A colorless resin composition layer CR-1 with a thickness of 10 μm was provided on the first film FA-1. Next, the colorless resin composition layer CR-1 and the water vapor barrier layer SB-2 were laminated at 80°C to obtain a sealing layer precursor. Next, the water vapor barrier layer SB-2 and the slightly adhesive side of the second film FB-1 were laminated at room temperature to obtain the sealing layer forming sheet SH-1.

[0136] The first film FA-1 and the second film FB-1 were peeled off from the sealing layer formation sheet SH-1, and the HAZE, b-value, water vapor transmission rate, and moisture absorption rate as sealing layer precursors were determined using the aforementioned apparatus and conditions. When determining the moisture absorption rate, the water vapor barrier layer was kept in contact with the stainless steel plate. Total light transmittance was measured and evaluated using a haze meter (NDH8000, manufactured by Nippon Denshoku Kogyo Co., Ltd., light source: D60) in the same manner as HAZE.

[0137] [Examples 2-25], [Comparative Examples 101-107] As shown in Tables 6-8, a sheet for forming a sealing layer was obtained in the same manner as in Example 1, except that the colorless resin composition layer for embedding was one of CR-7-CR-25 or CR-101-107, and the water vapor barrier layer was SB-1 or SB-2.

[0138] [Examples 26-29] In forming the colorless resin composition layer CR-1 for embedding, FA-2 to FA-5 were used instead of the first film FA-1, and SB-1 was used as the water vapor barrier layer. Except for these differences, the sealing layer-forming sheets were obtained in the same manner as in Example 1.

[0139] [Examples 30-32] A sheet for forming a sealing layer was obtained in the same manner as in Example 1, except that a colorless resin composition layer CR-1 for embedding was formed on the first film FA-1, SB-1 was used as the water vapor barrier layer, and FB-2 to FB-4 were used instead of FB-1 as the second film.

[0140] [Examples 33-38], [Comparative Examples 107-112] A sheet for forming a sealing layer was obtained in the same manner as in Example 1, except that a colorless resin composition layer CR-1 for embedding was formed on the first film FA-1, SB-3 to SB-7 and SB-101 to SB-106 were used as the water vapor barrier layer instead of SB-2, and FB-1 was used as the second film.

[0141] [Comparative Examples 113-115] Comparative Example 113 has a laminated structure consisting of a first film FA-1 / a colorless resin composition layer for embedding CR-1 / a second film FB-2, without a water vapor barrier layer. Comparative Example 114 is a laminated structure that does not use a second film, consisting of a first film FA-1 / a colorless resin composition layer for embedding CR-1 / a water vapor barrier layer SB-1. Comparative Example 115 has a laminated structure consisting of a first film FA-1 / water vapor barrier layer SB-1 / second film FB-2, without a colorless resin composition layer for embedding. This is a sheet for forming a sealing layer.

[0142] [Evaluation] For the sheets for forming the sealing layer obtained in each example and each comparative example, various performances were evaluated according to the following methods. [Test Substrate] A plate (see Fig. 11(1)) with 10 substantially parallel grooves having a width of 100 μm, a depth of 5 μm, and a spacing of 100 μm drawn in a substantially central portion of one surface of a glass plate with a size of 25 mm × 25 mm.

[0143] [LED Encapsulation Member Model] The first film was peeled off from the sheet for forming the sealing layer to expose the colorless resin composition layer for embedding, and the colorless resin composition layer for embedding was placed on the surface of the test substrate on which the concavo-convex portions were formed. A 50-μm-thick TPX (Opulran X-44B, manufactured by Mitsui Chemicals Toagosei Co., Ltd.) and a 2.0-mm-thick vinyl chloride film (Celebre T, manufactured by Okamoto Corporation) were sequentially placed on the second film as cushioning materials, and pressed at 5 MPa and 100 °C for 20 minutes. After pressing, the second film and the cushioning materials were peeled off, and then left standing at 150 °C for 2 hours to cure the colorless resin composition layer for embedding, and a 25-mm square LED encapsulation member model was obtained. In Comparative Example 115, since it did not have a resin composition layer for embedding and the water vapor barrier layer did not adhere to the test substrate, an LED encapsulation member model could not be made.

[0144] [Evaluation of Embeddability] The 10 grooves in the substantially central portion of the 25-mm square LED encapsulation member model were observed with a microscope at a magnification of 100 times with a coaxial light source from the side of the water vapor barrier layer, and the embeddability was evaluated based on the presence or absence and number of voids less than 10 μm due to poor embedding. In addition, when the maximum diameter of the voids was 10 μm or more, even if there was only one place, it was regarded as a fatal "lifting". S: There were no voids or "lifting", and all the concave portions were embedded. A: There were 1 to 5 voids and no "lifting". B: There were 6 to  10 voids and no "lifting". C: There were more than 10 voids, but no "lifting". D: There was one or more "floating" spots. In Comparative Example 114, since the second film was not laminated, a network-like pattern of marks appeared on the entire surface of the water vapor barrier layer on the muskmelon skin due to the difference in shrinkage of each layer (embedding resin composition layer, water vapor barrier layer, and cushioning material) during embedding. Therefore, no further evaluations were performed.

[0145] [Evaluation of the smoothness of the top surface] The top surface of the LED encapsulation component model, i.e., the surface of the water vapor barrier layer, was observed using a laser microscope (Keyence VK-X3000) at 100x magnification in an area of ​​5 mm vertically x 7 mm horizontally. The line roughness was measured in an area of ​​approximately 1 mm in length (at any three locations) perpendicular to the grooves of the test substrate in the observed image, and the average height was determined. Note that irregularities caused by foreign matter other than the 100 μm intervals corresponding to the grooves were excluded. S: Average height is 1.0 μm or less A: Average height of 1.1 μm or more, and difference in surface depth of 2.0 μm or less. B: Average height of 2.1 μm or more, and difference in surface depth of 3.0 μm or less. C: Average height of 3.1 μm or more, difference in surface area of ​​4.0 μm or less. D: Average height is 4.1 μm or greater

[0146] [Migration resistance] The sealing layer forming sheet was cut to a size of 2.5 cm vertically x 4 cm horizontally, and the first film was peeled off to expose the colorless resin composition layer for embedding. This sheet was then placed on an evaluation substrate on which a comb-shaped electrode (material: silver-plated copper foil, pattern pitch: 50 μm, L / S = 25 μm / 25 μm, 2.5 cm vertically x 5 cm horizontally) was formed on a polyimide film. A 50 μm thick TPX (Opulan X-44B, manufactured by Mitsui Chemicals Tohcello Co., Ltd.) and a 2.0 mm thick PVC film (Celeb T, manufactured by Okamoto Co., Ltd.) were placed sequentially on the second film as cushioning material, and pressed at 5 MPa and 100°C for 20 minutes. After pressing, the second film and cushioning material were peeled off, and the mixture was left to stand at 150°C for 2 hours to cure the colorless resin composition layer for embedding, which was then used as a test specimen to evaluate migration resistance. After applying a voltage of 30V or 50V to the test specimen for 1,000 hours in an environment of 85°C and 85%RH, the surface resistance was measured at room temperature (23°C) by placing a probe on the water vapor barrier surface of the sealing layer using a resistivity meter (Hi-Resta UX), and the number of leak touches during the 1,000 hours was confirmed. A "leak touch" is defined as dielectric breakdown due to a short circuit, which causes a momentary drop in resistance and allows current to flow. The absence of a leak touch means that the insulation performance does not decrease. S: Resistance value is 1 × 10 8 Omega or higher, and no leaks. A: Resistance value is 1 × 10 8 Less than Ω, 1 × 10 7 Omega or higher, and no leaks. B: Resistance value is 1 × 10 8 Less than Ω, 1 × 10 7 Omega or higher, and one leak touch. C: Resistance value is 1 × 10 7 Less than Ω, 1 × 10 6 Ω or higher, and 3 or fewer leak touches. D: Resistance value is 1 × 10 6 Less than Ω, or 4 or more leak touches.

[0147] The evaluation under a 30V application condition assumes the use of displays in a wide range of regions including temperate, subarctic, polar, and arid zones, while the evaluation under a 50V application pressure condition also assumes the use of displays in tropical regions. In both cases, S is best suited for forming high-power large displays of 50 inches or more, A is suitable for forming large displays, B is suitable for forming general-purpose displays of less than 50 inches, C is limited to forming small displays of less than 10 inches, and D is unsuitable.

[0148] [Yellowing Resistant] Using a CR-300 colorimeter (manufactured by Konica Minolta), the b* value (measured from the water vapor barrier layer side) of the LED encapsulation material model was determined before and after a heating test at 110°C for 500 hours, according to the method described in JIS-Z8722. The difference Δb* value was used to evaluate the resistance to yellowing. Furthermore, if the total light transmittance of the LED encapsulating material model was 70% or higher, the measurement was performed under transmission conditions; if the total light transmittance was less than 70%, the measurement was performed under reflection conditions. Δb* value = b* value after heating test - b* value before heating test S: Δb* value is less than 0.3. A: The Δb* value is 0.3 or greater, and less than 0.5. B: The Δb* value is 0.5 or greater and less than 1.0. C: Δb* value is 1.0 or greater, and less than 1.5. D: Δb* value is 1.5 or greater. S is suitable for use in transparent displays, A is suitable for use in applications other than transparent displays, B is suitable for general use, C is suitable for limited use, and D is unsuitable for use.

[0149] [Invisibility of boundaries, etc.] Four LED encapsulation component models were prepared, and a white X-shaped marker was placed in the center of the bottom surface of a black plastic case (Sekisei Granblock case) measuring 23mm deep x 146mm long x 70mm wide. Inside the case, as shown in Figure 11(1), the models were arranged in pairs vertically and horizontally, so that each side of the models and each side of the case were as parallel as possible. The intersections of the four models were at the positions of the white markers. Figure 11(1) is a schematic top view of the case with the four models arranged inside. Next, silicone oil (Shin-Etsu Silicone X-48-1800, refractive index 1.51) was poured over the top surface of the model until it was more than 3 mm to 5 mm deep, immersing the entire model. Under fluorescent lighting, as shown in Figure 11(2), three arbitrary people peered at the model from the short side of the case, 50 cm away from the white Marcolor, at a 45° angle, near the center of the short side of the case, to check whether the boundaries between the models and the surrounding areas of the models were visible, and evaluated them as follows. The lowest evaluation among the three people was adopted. S: I don't know if four models exist. A: Among the boundary lines of the four models, the boundary lines parallel to the short side of the case are visible, but the existence of the other four models cannot be determined. B: Among the boundary lines of the four models, the boundary lines parallel to the long side and the short side of the case appear in a cross shape. C: Not only the cross-shaped boundary lines but also the outer peripheries of the four models are visible. D: The cross-shaped boundary lines, the outer peripheries of the four models, and the upper surfaces of the four models are visible. S can be preferably used in a transparent display, A can be used limitedly in a transparent display, B can be preferably used in a high-definition colored display, C can be used in a general-purpose colored display, and D is not suitable for use.

[0150]

Table 6

[0151]

Table 7

[0152]

Table 8

[0153]

Table 9

Claims

1. A sealing layer forming sheet for filling the gaps between light-emitting elements in a display using multiple light-emitting elements as a light source, and for covering the light-emitting surfaces of the multiple light-emitting elements, The aforementioned sealing layer forming sheet has the first film 2, sealing layer precursor α, and second film 5 arranged in this order. The sealing layer precursor α has a water vapor permeability of 100 [g / (m²)]. 2 - Less than 24 hours, moisture absorption The ratio is 1.5% by mass or less. The sealing layer precursor α has a refractive index of 1.51 ± 0.03 and a water vapor permeability of 100 [g / (m²)]. 2 - A colorless resin composition layer 3 for embedding (for 24 hours or more), and a refractive index of 1. 53 ± 0.03, and water vapor transmission rate of 100 [g / (m³] 2 - Water vapor less than 24 hours It has a rear layer 4. Sheet for forming a sealing layer.

2. The sealing layer forming sheet according to claim 1, wherein the water vapor barrier layer 4 is a thermoplastic olefin film.

3. The tensile storage modulus E'3 of the colorless resin composition layer 3 for embedding at 100°C. (100) , the tensile storage modulus E'4 of the water vapor barrier layer 4 (100) , the tensile storage modulus E'5 of the second film 5 (100) However, the sealing layer forming sheet according to claim 1 satisfies the following relationship. E'4 (100) / E'3 (100) is 100 to 1000 and, E'5 (100) / E'4 (100) is 0.5 to 3

4. The sealing layer forming sheet according to claim 1, wherein the total light transmittance of the sealing layer precursor α is 85% or more.

5. It has a substrate and a plurality of light-emitting elements placed on the substrate at intervals, At least a portion of the depth direction of the individual gaps between the light-emitting elements has a refractive index of 1.51 ± 0.03 and a water vapor transmission rate of 100 [g / (m²]). 2 - Colorless trees for burying (24 hours or more) The cured product 3' of lipid composition 3 is embedded, The side from which the light of the multiple light-emitting elements is made of the cured material 3', and has a refractive index of 1.53 ± 0.03 and 100 [g / (m²]. 2 - Covered in the order of a water vapor barrier layer 4 less than 24 hours 、 A component in which multiple light-emitting elements are sealed.

6. The member containing a plurality of light-emitting elements according to claim 5, wherein at least a portion of the depth direction of the individual gaps between the light-emitting elements, and / or at least a portion of the bottom surface of the individual gaps, is filled with a cured product 9' of a colored resin composition 9 for embedding, and the remaining portion of the individual gaps between the light-emitting elements is filled with a cured product 3' of a colorless resin composition 3 for embedding.

7. The member in which a plurality of light-emitting elements are sealed, according to claim 5, wherein the water vapor barrier layer 4 is a thermoplastic olefin film.

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