Integrated sealing sheet, light-emitting electronic component and method for manufacturing the same
The integrated encapsulating sheet with a black and transparent resin layer structure addresses bubble formation issues in mini-LEDs or micro-LEDs, ensuring uniform appearance and improved sealing by controlling weight loss and thickness, thus enhancing manufacturing efficiency.
Patent Information
- Application Number
- JP2024101183
- Authority / Receiving Office
- JP · JP
- Patent Type
- Applications
- Current Assignee / Owner
- Filing Date
- 2024-06-24
- Publication Date
- 2026-01-13
AI Technical Summary
Conventional encapsulating sheets for mini-LEDs or micro-LEDs suffer from bubble generation during thermocompression bonding, leading to manufacturing defects and increased costs due to time-consuming etching processes and incomplete light shielding.
An integrated encapsulating sheet with a laminated structure of a black curable resin layer and a transparent curable resin layer, supported by a substrate, where the total thickness exceeds the height of the light-emitting elements, with a weight loss rate of 0.3 to 10% during curing, and optionally including a light diffusion layer, to suppress bubble formation.
The solution effectively reduces bubble generation, ensuring a uniform appearance and improved sealing of the light-emitting electronic components by controlling the weight loss rate and resin layer thickness, thereby enhancing manufacturing efficiency and reducing defects.
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Figure 2026003301000001_ABST
Abstract
Description
[Technical Field]
[0001] The present invention relates to an integrated encapsulating sheet, a light-emitting electronic component using the sheet, and a method for producing the same. [Background technology]
[0002] In recent years, displays using extremely small light-emitting diodes known as mini-LEDs or micro-LEDs have been attracting attention. There are two main methods known for using such extremely small light-emitting diodes in displays. One is to arrange a large number of light-emitting diodes on a substrate to form a backlight for an LCD and locally control the brightness of the backlight. The other is to have light-emitting diodes of each color (red, green, and blue) emit light and send that color light to the viewer's eyes on a pixel-by-pixel basis.
[0003] Light-emitting diodes such as mini LEDs or micro LEDs are generally arranged on a substrate. When multiple light-emitting diodes (referred to as light-emitting elements) are arranged on a substrate, it is necessary to provide light shielding between adjacent light-emitting elements. As a method for providing light shielding between multiple light-emitting elements using a resin with a light-shielding function, for example, a method using a dry film is known (see Prior Art 1 and Patent Document 1). A dry film is a film obtained, for example, by applying a light-shielding resin composition to a protective film and drying it.
[0004] When a dry film is pressed onto a substrate from above multiple light-emitting elements, a light-shielding resin layer is formed not only in the gaps between the light-emitting elements but also on the upper surfaces (light-emitting surfaces) of the light-emitting elements. Under such circumstances, the resin layer may block light from reaching the viewer of the display. To prevent this, the above-mentioned prior art 1 employs a method in which the light-emitting surface of the light-emitting element is etched using a plasma treatment or other etching method to remove the resin layer on the light-emitting surface, and the removed surface is then re-covered with a light-transmitting sealant.
[0005] However, the etching process in the above-mentioned prior art 1 requires a long time, which increases manufacturing costs. Furthermore, it is difficult to completely remove the light-shielding resin layer (hereinafter also referred to as "light-shielding layer") on the light-emitting surface of the light-emitting element, making it difficult to completely prevent the diffusion of light that should reach the viewer's side of the display. In addition, a step of laminating a highly transparent sealing film after the etching process is required, which increases the number of manufacturing processes.
[0006] In order to solve the problems of the above-mentioned Prior Art 1, the present inventors previously developed a novel integrated encapsulating sheet having a laminated structure of a black curable resin layer for light blocking and a transparent curable resin layer having higher light transmittance than the black curable resin layer, in which the storage elastic modulus of the transparent curable resin layer is greater than that of the black curable resin layer (see Prior Art 2 and Patent Document 2). When such a novel integrated encapsulating sheet is pressed toward the substrate with the black curable resin layer in contact with the top surfaces of multiple light-emitting elements, the black curable resin layer, pressed by the transparent curable resin layer, easily moves between the multiple light-emitting elements due to its relatively small storage elastic modulus. After the integrated encapsulating sheet is attached to the substrate, the black curable resin layer and the transparent curable resin layer are cured, resulting in a light-emitting electronic component in which the black layer fills the spaces between the multiple light-emitting elements and a transparent layer is disposed on the top surfaces of the multiple light-emitting elements. This solves the problems of the above-mentioned Prior Art 1. [Prior art documents] [Patent documents]
[0007] [Patent Document 1] Japanese Patent Publication No. 2022-22562 [Patent Document 2] Japanese Patent Application Publication No. 2024-19873 Summary of the Invention [Problem to be solved by the invention]
[0008] However, there is still room for further improvement in the above-mentioned conventional technique 2. That is, to further suppress the generation of bubbles when the integrated encapsulating sheet is thermocompression bonded to the element-mounted substrate and heat cured. The market is demanding an encapsulating sheet that is less likely to cause defects in appearance due to the generation of bubbles.
[0009] Therefore, an object of the present invention is to provide an integrated encapsulating sheet capable of further suppressing the generation of bubbles, a light-emitting electronic component using the sheet, and a method for producing the same. [Means for solving the problem]
[0010] (1) An integrated encapsulating sheet according to one embodiment for achieving the above object comprises: An integrated encapsulating sheet to be pressure-bonded to a surface of an element-mounted substrate on which a plurality of light-emitting elements are arranged, the surface comprising: a black cured resin layer that blocks light between the plurality of light-emitting elements, a transparent cured resin layer that has higher light transmittance than the black cured resin layer, and a support that supports the transparent cured resin layer, stacked in this order; a total thickness of the black cured resin layer and the transparent cured resin layer is greater than a height of the plurality of light-emitting elements; The total weight loss rate due to curing of the black curable resin layer and the transparent curable resin layer is 0.3 to 10%. (2) In the integrated encapsulating sheet according to another embodiment, preferably, the black curable resin layer and the transparent curable resin layer may contain at least an epoxy resin. (3) In the integrated encapsulating sheet according to another embodiment, preferably, the black curable resin layer may contain a curing catalyst, and the content of the curing catalyst may be 0.3 to 4 parts by mass relative to 100 parts by mass of a total resin solid content of the black curable resin layer. (4) In the all-in-one encapsulating sheet according to another embodiment, the support may preferably include a light diffusion layer for diffusing incident light from the light emitting element. (5) In the all-in-one encapsulating sheet according to another embodiment, preferably, at least one of the surfaces of the support in the thickness direction may be subjected to a release treatment. (6) To achieve the above object, a light-emitting electronic component according to one embodiment comprises: an element-mounted substrate having a plurality of light-emitting elements arranged on the substrate; an integrated encapsulating cured sheet that is pressure-bonded to a surface of the element-mounted substrate on which the plurality of light-emitting elements are arranged, the integrated encapsulating cured sheet includes, from the side in contact with the element-mounted substrate, at least a black resin layer that shields light between the plurality of light-emitting elements and a transparent resin layer that has higher light transmittance than the black resin layer, laminated in this order; a total thickness of the black cured resin layer, which is an uncured state of the black resin layer, and the transparent cured resin layer, which is an uncured state of the transparent resin layer, is greater than a height of the plurality of light-emitting elements; The total weight loss rate due to curing of the black curable resin layer and the transparent curable resin layer is 0.3 to 10%. (7) In the light-emitting electronic component according to another embodiment, the thickness of the black resin layer may preferably be 0.1 to 0.9 times the height of the plurality of light-emitting elements. (8) In the light-emitting electronic component according to another embodiment, the thickness of the transparent resin layer may preferably be 0.1 to 5.0 times the height of the plurality of light-emitting elements. (9) In order to achieve the above object, a method for manufacturing a light-emitting electronic component according to one embodiment includes the steps of: A step of placing the black curing resin layer of any one of the above integrated encapsulating sheets in contact with a surface of an element-mounted substrate on which a plurality of light-emitting elements are arranged, the surface having the plurality of light-emitting elements arranged on the substrate; Filling the integrated encapsulating sheet from the plurality of light-emitting elements toward the substrate; and curing the black curable resin layer and the transparent curable resin layer. [Effects of the Invention]
[0011] According to the present invention, it is possible to provide an integrated encapsulating sheet capable of further suppressing the generation of bubbles, a light-emitting electronic component using the sheet, and a method for manufacturing the same. [Brief explanation of the drawings]
[0012] [Figure 1] FIG. 1 shows a cross-sectional view of the integrated encapsulating sheet according to the first embodiment when cut in the thickness direction. [Figure 2] FIG. 2 shows a cross-sectional view seen in the same manner as FIG. 1 when the integrated encapsulating sheet of FIG. 1 is arranged so that the black curable resin layer thereof is in contact with the top surface of the light emitting element of the element-mounted substrate. [Figure 3] FIG. 3 shows a cross-sectional view, seen from the same perspective as FIG. 1, of a state in which the integrated encapsulating sheet has been pressure-bonded to the element-mounted substrate, proceeding from the stage shown in FIG. 2 up to the state in which the black curable resin layer and the transparent curable resin layer shown in FIG. 1 are embedded between the light-emitting elements. [Figure 4] FIG. 4 shows a cross-sectional view similar to FIG. 1, showing a state after the protective sheet on the hard coat layer has been peeled off and a curing treatment has been carried out, following the stage shown in FIG. [Figure 5] FIG. 5 shows a cross-sectional view of the integrated encapsulating sheet and the light-emitting electronic component according to the second embodiment, taken in the same view as FIG. [Figure 6] FIG. 6 shows a cross-sectional view, taken in the same direction as FIG. 1, of the light-emitting electronic component in a state in which the integrated encapsulating sheet according to the third embodiment and the release-treated support have been peeled off. DETAILED DESCRIPTION OF THE INVENTION
[0013] Next, embodiments of the present invention will be described with reference to the drawings. Note that the embodiments described below do not limit the invention according to the claims, and not all of the elements and combinations thereof described in the embodiments are necessarily essential to the solution of the present invention. In this application, "main component" means a component that accounts for 50% by mass or more of the total solid content of the entire composition. In this application, "total resin solid content" means the total solid mass of the resin and elastomer, and if a curing agent is blended in addition to the elastomer, it also includes the solid mass of the curing agent. A numerical range expressed by "to" means a numerical range with the numbers before and after "to" as the lower and upper limits.
[0014] (First embodiment) FIG. 1 shows a cross-sectional view of the integrated encapsulating sheet according to the first embodiment when cut in the thickness direction. FIG. 2 shows a cross-sectional view, as seen from FIG. 1, of the integrated encapsulating sheet of FIG. 1 when the black curable resin layer is placed in contact with the top surface of the light-emitting element of the element-mounted substrate. FIG. 3 shows a cross-sectional view, as seen from FIG. 1, of a state in which the integrated encapsulating sheet has been pressure-bonded to the element-mounted substrate up to a state in which the black curable resin layer and the transparent curable resin layer of FIG. 1 are embedded between the light-emitting elements, proceeding from the stage of FIG. 2. FIG. 4 shows a cross-sectional view, as seen from FIG. 1, of a state in which the protective sheet on the hard coat layer has been peeled off and a curing treatment has been performed, proceeding further from the stage of FIG. 3.
[0015] 1. Integrated encapsulating sheet The integrated encapsulating sheet 1 is an integrated encapsulating sheet 1 to be pressure-bonded to a surface of an element-mounted substrate 2 on which a plurality of light-emitting elements 21, 22, 23 are arranged, the surface having the light-emitting elements 21, 22, 23 arranged on a substrate 20, and is a laminate in which at least a black curable resin layer 10, a transparent curable resin layer 11, and a support 15 are laminated in this order.
[0016] The black curable resin layer 10 and the transparent curable resin layer 11 are resin layers that have the property of being cured by heat or the like in a curing step described later. That is, the black curable resin layer 10 and the transparent curable resin layer 11 are uncured layers until they undergo the curing step. The support 15 is a laminate of one or more layers including at least a substrate layer 12 described later. As shown in FIG. 1 , the integrated encapsulating sheet 1 according to this embodiment is a laminate in which the substrate layer 12 and the hard coat layer 16 serve as the support 15, and the black curable resin layer 10, the transparent curable resin layer 11, the substrate layer 12, and the hard coat layer 16 are laminated in this order. Although the support 15 according to this embodiment is shown as two layers, the present invention is not limited thereto. For ease of handling, the integrated encapsulating sheet 1 may further include protective sheets 17, 18 on the outer surfaces of either or both of the black curable resin layer 10 and the support 15 (the hard coat layer 16 in this embodiment).
[0017] (L* value of integrated encapsulant sheet) The L* value of the one-piece encapsulating sheet 1 is measured from the support 15 side in accordance with JIS Z 8781-4:2013, using a light source D65, a field of view of 2°, a reflection method, and an SCE method. The L* value is preferably less than 30, and more preferably less than 26. The L* value is measured on a standard white calibration plate. Since the light transmittance of the black curable resin layer 10 in the one-piece encapsulating sheet 1 is low, there is almost no influence of the standard white calibration plate. When the L* value is less than the upper limit, the blackness when the display is turned off can be increased. The L* value is preferably measured in a state where the sheet is not pressed onto or filled into the element-mounted substrate 2.
[0018] (Weight reduction rate) In the integrated encapsulating sheet 1 according to the present embodiment, the total thickness of the black cured resin layer 10 and the transparent cured resin layer 11 is greater than the height of the plurality of light emitting elements 21, 22, and 23, and the total weight loss rate due to curing of the black cured resin layer 10 and the transparent cured resin layer 11 is 0.3 to 10%. The weight loss rate is preferably 1 to 9%, more preferably 2 to 8%, and even more preferably 2.5 to 7%.
[0019] The weight loss rate is an index for evaluating the remaining amount of organic solvent contained in each curable resin layer coating liquid after thermal drying (or the amount volatilized during thermal drying) and the amount volatilized during thermocompression bonding and thermal curing in the black curable resin layer 10 and the transparent curable resin layer 11. When the weight loss rate is within this range, the generation of bubbles in the black resin layer 30 and the transparent resin layer 31 after thermocompression bonding and thermal curing can be suppressed, thereby further suppressing poor appearance and poor sealing of the light-emitting electronic component 5. A weight loss rate equal to or greater than the lower limit indicates that the amount of volatilization of the organic solvent in each curable resin layer coating liquid during thermal drying in producing the integrated encapsulating sheet 1 is not too small. This prevents a large amount of organic solvent from remaining in the integrated encapsulating sheet 1, making it less likely that bubbles will form after thermocompression bonding and thermal curing of the sheet 1. A weight loss rate equal to or less than the upper limit indicates that the amount of volatilization of the organic solvent in each curable resin layer coating liquid during thermal drying in producing the integrated encapsulating sheet 1 is not too large. This prevents air from remaining inside the layers due to early drying of the surface of each curable resin layer, making it more difficult for air bubbles to form after thermocompression bonding and thermal curing of the sheet 1. The weight loss rate will be described in detail below.
[0020] The weight loss rate is calculated by the following formula 1 and calculation methods (i) to (vii).
[0021]
number
[0022] (i) For the integrated encapsulating sheet 1 manufactured by the manufacturing method described later, the thicknesses of the entire integrated encapsulating sheet 1, the black curable resin layer 10, and the transparent curable resin layer 11 are measured and designated as Ttotal, T1, and T2, respectively. When the black curable resin layer 10 and the transparent curable resin layer 11 are applied using an applicator or the like that can specify the film thickness, this step may be skipped. (ii) The integrated encapsulating sheet 1 is left to stand for 3 hours in a constant temperature and humidity chamber at 23±2°C and 50±10 RH%. (iii) The integrated encapsulating sheet 1 after being left standing is cut into a measurement sample having a size of 100 mm square. (iv) The weight of the cut measurement sample is measured using a precision balance, and this weight is defined as the weight before drying (W1). Note that if a protective sheet 17 is provided on the black curable resin layer 10, the sheet 17 is peeled off before the weight measurement. (v) Place the measurement sample in an oven set to 120°C and heat for 30 minutes. (vi) After heating, remove the sample from the oven and measure its weight using a precision balance. This weight is the post-dry weight (W2). (vii) Each measured value is substituted into Equation 1 to calculate the weight loss rate.
[0023] When the protective sheets 17 and 18 are provided on the integrated encapsulating sheet 1, the above-mentioned value of Ttotal is measured excluding the thickness of the protective sheets 17 and 18. That is, the value of Ttotal is the total value of the black curable resin layer 10, the transparent curable resin layer 11, and the support 15 (in the present embodiment, the base layer 12 and the hard coat layer 16). When other functional layers, such as the light diffusion layer 13 and the second base layer 14 in another embodiment described later, are provided, the value of Ttotal also includes the thickness of the functional layers.
[0024] Hereinafter, each layer of the integrated encapsulating sheet 1 according to this embodiment will be described in detail.
[0025] (1) Black curable resin layer The black curable resin layer 10 is a layer for blocking light between the light-emitting elements 21, 22, and 23. It also serves to improve the contrast of the display. Furthermore, the black curable resin layer 10 sufficiently fills the spaces between the light-emitting elements 21, 22, and 23 arranged on the element-mounted substrate 2 during a compression bonding process, such as thermocompression bonding, and serves to prevent poor appearance due to expansion of unfilled voids during a curing process, such as thermosetting, and damage to the light-emitting elements 21, 22, and 23 due to external factors in subsequent processes. In this embodiment, the black curable resin layer 10 has a transparent curable resin layer 11 laminated on one side and a protective sheet 17 on the other side. The black curable resin layer 10 is cured through a curing process to become the black resin layer 30 described below. In other words, the black curable resin layer 10 is an uncured layer.
[0026] [L*a*b* value] The L*a*b* values of the black curable resin layer 10 in a cured state, as measured in accordance with JIS Z 8781-4:2013 using a D65 light source, a 2° field of view, a reflection method, and the SCE method, are preferably L*: 3 to 40, a*: -10 to 10, and b*: -20 to 20, and more preferably L*: 3 to 30, a*: -5 to 5, and b*: -15 to 15. The L*a*b* values are measured using a standard white calibration plate. Because the light transmittance of the black curable resin layer 10 is low, the influence of the standard white calibration plate is minimal. By ensuring that the L*a*b* values in the cured state are within the preferred range, the black curable resin layer 10, after curing, can shield light from the light-emitting elements 21, 22, and 23, thereby further improving the contrast of the display. The same indices apply to the uncured black curable resin layer 10.
[0027] [Total light transmittance] The total light transmittance of the black curable resin layer 10 in a cured state is lower than the total light transmittance of the transparent curable resin layer 11 in a cured state. Specifically, the black curable resin layer 10 is prepared so that the total light transmittance of the black curable resin layer 10 in a cured state is 0 to 50%. The total light transmittance of the black curable resin layer 10 in a cured state is preferably prepared so that the total light transmittance is 0 to 40%, more preferably 0 to 30%. When the total light transmittance is equal to or less than an upper limit value such as 50%, 40%, or 30%, the black curable resin layer 10 can achieve light shielding between the light-emitting elements 21, 22, and 23 after curing. The total light transmittance in this specification can be measured using a haze meter in accordance with JIS K 7361-1. The total light transmittance in a cured state can be changed mainly by the presence or absence of carbon black or the amount of carbon black added. The total light transmittance in a cured state can also be changed by the thickness of the black curable resin layer 10 and the type of resin composition.
[0028] [Storage modulus] The storage modulus of the black curable resin layer 10 in an uncured state is preferably smaller than the storage modulus of the transparent curable resin layer 11 in an uncured state. The storage modulus of the black curable resin layer 10 in an uncured state at 100° C. is preferably 1.0×10 5 Pa or less, and more preferably 1.0×10 1 ~1.0×10 5 Pa, and even more preferably 1.0×10 2 ~5.0×10 4 Pa. When the storage modulus of the black curable resin layer 10 at 100°C in an uncured state is equal to or less than the preferred upper limit, the black curable resin layer 10 exhibits sufficient fluidity when pressure-bonded to the plurality of light-emitting elements 21, 22, and 23, and can sufficiently fill the spaces between the plurality of light-emitting elements 21, 22, and 23. When the storage modulus of the black curable resin layer 10 at 100°C in an uncured state is equal to or greater than the preferred lower limit, it is possible to prevent uneven pressure during thermocompression bonding of the black curable resin layer 10 and the transparent curable resin layer 11, and to maintain a uniform appearance. It is also possible to prevent the resin from leaking outside a predetermined range, ensuring a film thickness after pressure bonding.
[0029] The storage modulus of the black curable resin layer 10 in an uncured state at 150° C. is preferably 5.0×10 5 Pa or less, and more preferably 5.0 × 10 2 ~5.0×10 5 Pa, and even more preferably 1.0×10 3 ~1.0×10 5 Pa. When the storage modulus of the black curable resin layer 10 at 150°C in an uncured state is equal to or less than the preferred upper limit, cracks due to cure shrinkage are less likely to occur during thermal curing. When the storage modulus of the black curable resin layer 10 at 150°C is equal to or greater than the preferred lower limit, flow during thermal curing can be suppressed, and poor appearance after curing, such as repellency, can be suppressed.
[0030] [Curable resin composition] The black curable resin layer 10 includes a curable resin composition. Examples of the curable resin composition include a curable resin composition containing at least one resin selected from epoxy resin, acrylic resin, polyester resin, polyurethane resin, and silicone resin, and a curing agent. Among the curable resin compositions, epoxy resin compositions, which have excellent heat resistance and reliability, are preferred. In this specification, an epoxy resin composition refers to a composition containing an epoxy resin as a main component, or a composition containing an epoxy resin and a curing agent as main components. Using an epoxy resin composition, which is a thermosetting resin, facilitates the calculation of the weight loss rate using the above method and also contributes to the suppression of air bubble formation in the light-emitting electronic component 5.
[0031] When the black curable resin layer 10 is composed of an epoxy resin composition, it may contain a curing agent for epoxy resins other than the modified elastomer having a functional group reactive with an epoxy group. Examples of other curing agents include known curing agents such as phenol-based curing agents, acid anhydride-based curing agents, and amine-based curing agents. Two or more of the other curing agents may be used in combination.
[0032] (epoxy resin) In this application, an epoxy resin is a compound having an epoxy group in the molecule. The epoxy resin used in the present invention is preferably one having two or more epoxy groups in one molecule. This is because a crosslinked structure is formed by reaction with a modified resin having a functional group reactive with the epoxy group, and the cured product can exhibit high heat resistance. Furthermore, when an epoxy resin having two or more epoxy groups is used, the degree of crosslinking with a curing agent having a functional group reactive with the epoxy group is sufficient, and sufficient heat resistance can be obtained in the cured product.
[0033] Examples of epoxy resins include bifunctional epoxy resins having two epoxy groups per molecule, multifunctional epoxy resins having three or more epoxy groups per molecule, and high-molecular-weight epoxy resins having a weight-average molecular weight of 10,000 or more. These may also be hydrogenated epoxy resins. In this application, epoxy resins having a weight-average molecular weight of 10,000 or more are not classified as bifunctional or multifunctional epoxy resins, but as high-molecular-weight epoxy resins, regardless of the number of epoxy groups per molecule. The weight-average molecular weight of an epoxy resin is the molecular weight in terms of polystyrene measured by gel permeation chromatography.
[0034] Examples of epoxy resins include bisphenol-based epoxy resins such as bisphenol A type epoxy resin, bisphenol F type epoxy resin, or phenoxy resins obtained by polymerizing these resins, and hydrogenated versions of these resins; novolac type epoxy resins such as phenol novolac epoxy resin, o-cresol novolac epoxy resin, bisphenol A novolac epoxy resin, xylene structure-containing novolac epoxy resin, and naphthol novolac type epoxy resin; glycidyl ester-based epoxy resins such as phthalic acid diglycidyl ester, isophthalic acid diglycidyl ester, terephthalic acid diglycidyl ester, p-hydroxybenzoic acid glycidyl ester, tetrahydrophthalic acid diglycidyl ester, succinic acid diglycidyl ester, adipic acid diglycidyl ester, sebacic acid diglycidyl ester, and trimellitic acid triglycidyl ester; ethylene glycol diglycidyl ether, propylene glycol diglycidyl ether, 1,4-butanediol diglycidyl ether, 1,6-hexanediol diglycidyl ether, glycidyl ether-based epoxy resins such as glycidyl ether, trimethylolpropane triglycidyl ether, pentaerythritol tetraglycidyl ether, tetraphenylglycidyl ether ethane, triphenylglycidyl ether ethane, polyglycidyl ether of sorbitol, and polyglycidyl ether of polyglycerol; glycidylamine-based epoxy resins such as triglycidyl isocyanurate and tetraglycidyldiaminodiphenylmethane; linear aliphatic epoxy resins such as epoxidized polybutadiene and epoxidized soybean oil; and special skeleton epoxy resins such as brominated bisphenol A-type epoxy resins, phosphorus-containing epoxy resins, fluorine-containing epoxy resins, dicyclopentadiene skeleton-containing epoxy resins, naphthalene skeleton-containing epoxy resins, anthracene-type epoxy resins, tertiary butylcatechol-type epoxy resins, triphenylmethane-type epoxy resins, tetraphenylethane-type epoxy resins, biphenyl-type epoxy resins, and bisphenol S-type epoxy resins, but are not limited to these.
[0035] Examples of high molecular weight epoxy resins that can be used include phenoxy resin, epoxy-modified polybutadiene, copolymers of glycidyl methacrylate and methyl methacrylate, modified polymers obtained by epoxy-modifying other resins, etc. These epoxy resins may be used alone or in combination of two or more.
[0036] Among the above epoxy resins, polyfunctional epoxy resins are preferred as the epoxy resin used in the black curable resin layer 10 from the viewpoint of increasing the crosslink density after curing. Among polyfunctional epoxy resins, novolac-type epoxy resins are particularly preferred for the following reasons. Novolac-type epoxy resins are epoxy resins that can be appropriately introduced with a flexible skeleton, allowing for adjustment of flexibility and softening point. This makes the cured product less susceptible to brittle fracture, improving the performance stability of the cured product of the epoxy resin composition over long-term use and increasing the crosslink density. Additionally, the heat resistance of the cured product is also improved.
[0037] Specific examples of novolac-type epoxy resins include "YX7700" manufactured by Mitsubishi Chemical Corporation, "NC7000L", "XD1000", and "EOCN-1020" manufactured by Nippon Kayaku Co., Ltd., "ESN485" manufactured by Nippon Steel Chemical & Material Co., Ltd., and "N-660", "N-690", "N-695", and "HP-7200H" manufactured by DIC Corporation.
[0038] The amount of polyfunctional epoxy resin in the black curing resin layer 10 is preferably 10 to 99 parts by mass, more preferably 40 to 95 parts by mass, and even more preferably 60 to 90 parts by mass, relative to 100 parts by mass of the total resin solids content of the black curing resin layer 10. When the amount is equal to or greater than the lower limit, the crosslinking density can be increased, thereby imparting chemical resistance and heat resistance. When the amount is equal to or less than the upper limit, the storage modulus during thermocompression bonding can be adjusted, thereby ensuring the fluidity of the black curing resin layer 10.
[0039] The black curable resin layer 10 preferably does not contain a high-molecular-weight epoxy resin. This makes it easier to ensure sufficient fluidity of the black curable resin layer 10 during thermocompression bonding. When the black curable resin layer 10 contains a high-molecular-weight epoxy resin, the amount of the high-molecular-weight epoxy resin blended is preferably less than 50 parts by mass, more preferably less than 30 parts by mass, and even more preferably less than 10 parts by mass, relative to 100 parts by mass of the total resin solid content of the black curable resin layer 10.
[0040] From the viewpoint of ensuring sufficient fluidity during thermocompression bonding, the black curable resin layer 10 preferably contains an epoxy resin having a softening point or melting point of 100° C. or less. From the viewpoint of handleability and heat resistance of the cured product, the black curable resin layer 10 more preferably contains an epoxy resin having a softening point or melting point of 40 to 95° C. By containing an epoxy resin having a softening point or melting point within the above range, it becomes easier to control the storage modulus of the black curable resin layer 10.
[0041] The total amount of epoxy resin in the black curing resin layer 10 is preferably 10 to 100 parts by mass, more preferably 20 to 99 parts by mass, and even more preferably 35 to 95 parts by mass, relative to 100 parts by mass of the total resin solids content of the black curing resin layer 10. Within this range, it is easy to control the storage modulus of the black curing resin layer 10, and appropriate fluidity during thermocompression bonding can be ensured. Furthermore, when the amount is equal to or greater than the above lower limit, the heat resistance of the black curing resin layer 10 after curing can be improved.
[0042] (Elastomer) The black curable resin layer 10 preferably contains an elastomer in addition to a resin such as an epoxy resin. By containing an elastomer, it becomes easier to control the storage modulus of the black curable resin layer 10, i.e., to control the fluidity.
[0043] As the elastomer, a thermosetting elastomer, commonly called "rubber," is preferred because it provides excellent heat resistance. Examples of thermosetting elastomers include acrylonitrile butadiene rubber (NBR), which is a random copolymer of butadiene and acrylonitrile, acrylic rubber, styrene butadiene rubber, vinyl acetate resin, and silicone resin. Among these, NBR is preferred. NBR has good compatibility with epoxy resins, making it easy to control the fluidity of the black curable resin layer 10 at around 100°C, resulting in good adhesion between the black curable resin layer 10 and the transparent curable resin layer 11 and the element-mounted substrate 2.
[0044] The weight-average molecular weight of the elastomer is preferably 100,000 to 1,000,000, more preferably 120,000 to 500,000, and even more preferably 150,000 to 300,000. When the weight-average molecular weight of the elastomer is within the above range, the storage modulus of the black curable resin layer 10 can be easily controlled, and fluidity during thermocompression bonding can be ensured. When the weight-average molecular weight of the elastomer is equal to or less than the above upper limit, compatibility between the elastomer and the epoxy resin is improved, and fluidity during thermal curing of the black curable resin layer 10 can be more effectively controlled.
[0045] In particular, when the black curable resin layer 10 is composed of an epoxy resin composition, it preferably contains a modified elastomer having a functional group reactive with an epoxy group. The modified elastomer having a functional group reactive with an epoxy group also functions as a curing agent for the epoxy resin. Furthermore, because the modified elastomer can react and bond with the epoxy resin, the heat resistance and thermal shock resistance of the cured black curable resin layer 10 are improved. Furthermore, the difference in polarity between the functional group reactive with the epoxy resin and the resin skeleton favorably affects dispersibility, resulting in good dispersibility when carbon black is added to the black curable resin layer 10.
[0046] Examples of functional groups that can react with epoxy groups include acid groups such as carboxy groups, sulfo groups, nitro groups, and phosphate groups, as well as their acid anhydride groups, hydroxyl groups, and amino groups. Among these, acid groups and acid anhydride groups are preferred because they allow curing at low temperatures and ensure a long usable time. For the same reasons, carboxy groups and carboxylic acid anhydride groups are particularly preferred.
[0047] That is, when the black curable resin layer 10 is composed of an epoxy resin composition, it preferably contains an acid-modified elastomer having an acid group or an acid anhydride group, more preferably contains an acid-modified elastomer having a carboxy group, and even more preferably contains modified NBR having a carboxy group.
[0048] The modified NBR having a carboxy group is preferably a carboxylated acrylonitrile rubber into which acrylic acid, methacrylic acid, maleic anhydride, etc. have been introduced. Commercially available carboxylated acrylonitrile rubbers include "NX775" and "1072CGJ" manufactured by Zeon Corporation. Two or more modified elastomers having a functional group reactive with an epoxy group may be used in combination.
[0049] The amount of elastomer in the black curable resin layer 10 is preferably 0.01 to 90 parts by mass, more preferably 1 to 80 parts by mass, and even more preferably 5 to 65 parts by mass, relative to 100 parts by mass of the total resin solids content of the black curable resin layer 10. Within this range, the storage modulus of the black curable resin layer 10 can be easily controlled, ensuring appropriate fluidity of the black curable resin layer 10 during thermocompression bonding. Furthermore, when the amount is equal to or greater than the lower limit, the dispersibility of carbon black in the epoxy resin composition is improved. Furthermore, the film-forming properties of the epoxy resin composition are improved, allowing for a narrower film thickness distribution when the epoxy resin composition is applied to form a film.
[0050] (hardening agent) When the black curable resin layer 10 is composed of an epoxy resin composition, it may contain a curing agent for epoxy resins other than the modified elastomer having a functional group reactive with an epoxy group. Examples of other curing agents include known curing agents such as phenol-based curing agents, acid anhydride-based curing agents, and amine-based curing agents. Two or more of the other curing agents may be used in combination.
[0051] (curing catalyst) When the black curable resin layer 10 is composed of an epoxy resin composition, it may contain a curing catalyst that promotes the curing reaction of the epoxy resin. Examples of curing catalysts include imidazole-based, tertiary amine-based, and phosphorus compound-based catalysts. Among these, imidazole-based catalysts are preferred because they are compatible with epoxy resins and less likely to cause yellowing. Among imidazole-based curing catalysts, those containing a cyanoethyl group are particularly preferred because they are easily soluble in epoxy resins. The blending amount of the curing catalyst is preferably 0.01 to 5 parts by mass, more preferably 0.05 to 4 parts by mass, and even more preferably 0.3 to 4 parts by mass, relative to 100 parts by mass of the total resin solids content of the black curable resin layer 10. Within the above range, the curing of the black curable resin layer 10 can be sufficiently promoted, ensuring the usable life of the integrated encapsulating sheet 1. Furthermore, the curing rate of the integrated encapsulating sheet 1 can be adjusted within an appropriate range, and the generation of bubbles can be further suppressed. Two or more curing catalysts may be used in combination.
[0052] (black pigments such as carbon black) The black curable resin layer 10 is colored black, and for coloring purposes, it may preferably contain carbon black, titanium oxide, iron oxide, etc., more preferably carbon black. By containing carbon black, it is possible to achieve light blocking properties between the multiple light emitting elements 21, 22, 23 of the element-mounted substrate 2.
[0053] The particle size of carbon black is preferably 10 to 500 nm, more preferably 10 to 300 nm, and even more preferably 10 to 100 nm. The particle size refers to the average particle size, and in this specification, the average particle size of carbon black refers to the average particle size measured by a dynamic light scattering method. An example of a measuring device using the dynamic light scattering method is the NanotracWave II UT151 manufactured by Microtrack Bell.
[0054] As the carbon black, one or more types of known carbon black such as gas black, channel black, furnace black, thermal black, and lamp black can be used. Resin-coated carbon black may also be used. Furthermore, carbon nanofibers and carbon nanotubes may also be used.
[0055] Among the above options, gas black is preferred because it has a large amount of surface functional groups, is highly dispersible, and exhibits sufficient light-blocking properties even when added in small amounts. Furthermore, when the black curable resin layer 10 contains a modified elastomer having functional groups reactive with epoxy resins, the interaction between the surface functional groups of the gas black and the functional groups of the modified elastomer having functional groups reactive with epoxy resins further enhances dispersibility, ensuring good light-blocking properties and coating liquid stability.
[0056] The amount of carbon black blended is preferably 0.1 to 15 parts by mass, and more preferably 1.0 to 10 parts by mass, relative to 100 parts by mass of the total resin solids content of the black cured resin layer 10. When the amount of carbon black blended is equal to or greater than the above-mentioned lower limit, sufficient light-blocking properties are obtained. When the amount of carbon black blended is equal to or less than the above-mentioned upper limit, the thixotropy of the black cured resin layer 10 is suppressed, fluidity during thermocompression bonding is improved, and the gaps between the multiple light-emitting elements 21, 22, and 23 of the element-mounted substrate 2 can be sufficiently filled.
[0057] (Other ingredients) The black curable resin layer 10 may contain inorganic fillers to improve flame retardancy and heat resistance and to adjust the refractive index. However, it is preferable that the black curable resin layer 10 does not contain inorganic fillers other than carbon black, since this increases thixotropy and reduces fluidity during thermocompression bonding, making it impossible to sufficiently fill the spaces between the multiple light-emitting elements 21, 22, and 23 of the element-mounted substrate 2.
[0058] The black curable resin layer 10 may further contain, as needed, resins other than epoxy resins and elastomers, thickeners, antifoaming agents and / or leveling agents, adhesion promoters such as coupling agents, and flame retardants.
[0059] (2)Transparent curable resin layer The transparent curable resin layer 11 is a layer for sufficiently pressing the black curable resin layer 10 between the plurality of light-emitting elements 21, 22, and 23 arranged on the element-mounted substrate 2. The transparent curable resin layer 11 has higher light transmittance than the black curable resin layer 10. In this application, "light transmittance" refers to light transmittance measured by various known methods, and may be, for example, total light transmittance measured using a haze meter in accordance with JIS K 7361-1. In this embodiment, the transparent curable resin layer 11 is formed between the black curable resin layer 10 and a substrate layer 12 described below. The transparent curable resin layer 11 is cured through a curing process to become a transparent resin layer 31 described below. In other words, the transparent curable resin layer 11 is an uncured layer.
[0060] [Total light transmittance] The total light transmittance of the transparent curable resin layer 11 in a cured state is higher than the total light transmittance of the black curable resin layer 11 in a cured state. The total light transmittance of the transparent curable resin layer 11 in a cured state is not particularly limited, and is preferably adjusted to be 50 to 99%, more preferably 60 to 99%, and even more preferably 70 to 99%.
[0061] [Storage modulus] The storage modulus of the transparent curable resin layer 11 in an uncured state is preferably greater than that of the black curable resin layer 10. Similarly, at 100°C and 150°C, the storage modulus of the transparent curable resin layer 11 is preferably greater than that of the black curable resin layer 10.
[0062] The storage modulus of the transparent curable resin layer 11 is preferably greater than that of the black curable resin layer 10 at 100 to 150°C. When the storage modulus of the transparent curable resin layer 11 is greater than that of the black curable resin layer 10 at 100°C and 150°C, the storage modulus of the transparent curable resin layer 11 is usually greater than that of the black curable resin layer 10 over the entire range of 100 to 150°C.
[0063] The storage modulus of the transparent curable resin layer 11 at 100° C. is preferably 1.0×10 3 ~1.0×10 7 Pa, and more preferably 5.0×10 3 ~5.0×10 5 It is Pa.
[0064] When the storage modulus of the transparent curable resin layer 11 at 100°C is equal to or less than the preferred upper limit, the black curable resin layer 11 has an appropriate flexibility that does not hinder the flow of the black curable resin layer 11 when it is pressure-bonded to the element-mounted substrate 2. In addition, the spaces between the plurality of light-emitting elements 21, 22, and 23 can be sufficiently filled.
[0065] When the storage modulus of the transparent curable resin layer 11 at 100°C is equal to or greater than the preferred lower limit, the fluidity of the transparent curable resin layer 11 is suppressed, and the surface of the transparent curable resin layer 11 can be made smoother after thermocompression bonding to fit the light emitting elements 21, 22, and 23. As a result, the appearance can be improved, and appearance defects such as repellency, which causes depressions on the layer surface during thermal curing, can be made less likely to occur.
[0066] The storage modulus of the transparent curable resin layer 11 at 150° C. is preferably 1.0×10 4 Pa or more, more preferably 1.0×104 ~5.0×10 7 Pa, and even more preferably 1.0×10 5 ~5.0×10 6 It is Pa.
[0067] When the storage modulus of the transparent curable resin layer 11 at 150°C is equal to or less than the preferred upper limit, cracks due to cure shrinkage during thermal curing are less likely to occur. When the storage modulus of the transparent curable resin layer 11 at 150°C is equal to or greater than the preferred lower limit, flow of the transparent curable resin layer 11 during thermal curing can be suppressed, and poor appearance after curing, such as repellency, can be suppressed.
[0068] The storage elastic modulus of the transparent curable resin layer 11 at 100°C is preferably 10 to 1,000 times, and more preferably 30 to 500 times, the storage elastic modulus of the black curable resin layer 10. The storage elastic modulus of the transparent curable resin layer 11 at 150°C is preferably 5 to 10,000 times, and more preferably 10 to 1,000 times, the storage elastic modulus of the black curable resin layer 10. When the storage elastic modulus of the transparent curable resin layer 11 is higher than that of the black curable resin layer 10 at 100°C and 150°C, the storage elastic modulus of the transparent curable resin layer 11 is usually higher than that of the black curable resin layer 10 over the entire temperature range from 100 to 150°C.
[0069] [Curable resin composition] The transparent curable resin layer 11 is composed of a curable resin composition. As with the black curable resin layer 10, the curable resin composition may be, for example, a curable resin composition containing at least one resin selected from epoxy resin, acrylic resin, polyester resin, polyurethane resin, and silicone resin, and a curing agent. Among these, an epoxy resin composition is preferred because it has excellent heat resistance and reliability, is a thermosetting resin, and enables the calculation of the weight loss rate, thereby contributing to preventing the generation of bubbles.
[0070] (epoxy resin) Examples of epoxy resins used in the transparent curable resin layer 11 include the same types as those used in the black curable resin layer 10. From the viewpoint of being able to impart an appropriate viscosity during compression bonding to the transparent curable resin layer 11, the transparent curable resin layer 11 preferably contains a high-molecular-weight epoxy resin having a weight-average molecular weight of 10,000 to 100,000. Furthermore, from the viewpoint of having good compatibility with other resin components and being able to dissolve without mixing with a high-boiling-point solvent that may remain in the integrated encapsulating sheet 1 even after drying, the transparent curable resin layer 11 more preferably contains a high-molecular-weight epoxy resin having a weight-average molecular weight of 10,000 to 35,000.
[0071] The transparent curable resin layer 11 contains a high-molecular-weight epoxy resin with a weight-average molecular weight of 10,000 to 100,000, and thus has an appropriate viscosity when heated. Therefore, the storage modulus of the transparent curable resin layer 11 at 100 to 150°C can be adjusted to a preferred range. The high-molecular-weight epoxy resin is preferably a phenoxy resin because of its good compatibility with other epoxy resins.
[0072] Phenoxy resin has a relatively large molecular weight among epoxy resins and has an appropriate viscosity when heated. Therefore, the storage modulus of the transparent curable resin layer 11 containing phenoxy resin can be adjusted within a preferred range within a temperature range of 100 to 150°C. Furthermore, unlike other thermoplastic resins such as polyester, phenoxy resin can be cured as an epoxy resin. Therefore, phenoxy resin increases crosslink density and does not impair the heat resistance of the cured product or the reliability of its performance over long periods of use. From the viewpoint of ensuring a storage modulus sufficient to compress the black curable resin layer 10 during thermocompression bonding, the glass transition temperature of the phenoxy resin used in the transparent curable resin layer 11 is preferably 100°C or higher.
[0073] Specific examples of phenoxy resins include "1256," "YX7200," "YX8100," and "YX7180" manufactured by Mitsubishi Chemical Corporation, "YP-50," "YP-50S," and "YP-70" manufactured by Nippon Steel Chemical & Material Co., Ltd., and "N-690," "H-157," and "EXA-192" manufactured by DIC Corporation.
[0074] The blending amount of the high-molecular-weight epoxy resin in the transparent curable resin layer 11 is preferably 30 to 80 parts by mass, more preferably 40 to 70 parts by mass, and even more preferably 45 to 60 parts by mass, relative to 100 parts by mass of the total resin solid content of the transparent curable resin layer 11. The same is true for the preferred blending amount of the phenoxy resin in the transparent curable resin layer 11.
[0075] When the blending amount is within the above range, it becomes easy to control the storage modulus. This ensures a storage modulus sufficient to compress the transparent curable resin layer 11 during thermocompression bonding. Furthermore, flow during thermal curing can be suppressed, and poor appearance after curing, such as repellency, can be suppressed. Furthermore, problems are less likely to occur when etching is performed in a subsequent process. Furthermore, toughness is improved, and crack-like defects are less likely to occur during thermocompression bonding. Furthermore, when the blending amount is equal to or less than the above upper limit, the crosslink density of the transparent curable resin layer 11 in the cured state can be increased, and heat resistance and chemical resistance can be improved.
[0076] Furthermore, the epoxy resin used in the transparent curable resin layer 11 preferably contains a multifunctional epoxy resin. The multifunctional epoxy resin increases the crosslink density, thereby further improving the stability of the performance of the cured product of the epoxy resin composition over long-term use and improving heat resistance. Furthermore, the viscosity of the multifunctional epoxy resin is lower than that of the phenoxy resin in the range of 100 to 150°C. Therefore, by combining the multifunctional epoxy resin with the phenoxy resin, the storage modulus of the transparent curable resin layer 11 can be adjusted.
[0077] Specific examples of polyfunctional epoxy resins include "YX7700," "157S70," and "1032H60" manufactured by Mitsubishi Chemical Corporation, "NC7000L," "XD1000," and "EOCN-1020" manufactured by Nippon Kayaku Co., Ltd., "ESN485" manufactured by Nippon Steel Chemical & Material Co., Ltd., and "N-660," "N-690," "N-695," and "HP-7200H" manufactured by DIC Corporation.
[0078] The amount of polyfunctional epoxy resin in the transparent curable resin layer 11 is preferably 90 parts by mass or less, more preferably 10 to 80 parts by mass, and even more preferably 25 to 60 parts by mass, relative to 100 parts by mass of the total resin solid content of the transparent curable resin layer 11. Within the above ranges, the storage modulus of the transparent curable resin layer 11 during thermocompression bonding can be controlled, and heat resistance and chemical resistance can be imparted in the cured state.
[0079] From the viewpoint of ensuring sufficient fluidity during thermocompression bonding, the transparent curable resin layer 11 preferably contains an epoxy resin having a softening point or melting point of 120° C. or less, and from the viewpoint of handleability and heat resistance of the cured product, more preferably contains an epoxy resin having a softening point or melting point of 50 to 105° C. By containing an epoxy resin having a softening point or melting point within the above range, it becomes possible to control the storage modulus.
[0080] The total amount of epoxy resin in the transparent curable resin layer 11 is preferably 10 to 100 parts by mass, more preferably 30 to 99 parts by mass, and even more preferably 50 to 95 parts by mass, relative to 100 parts by mass of the total resin solids content of the transparent curable resin layer 11. Within this range, control of the storage modulus is easy. This ensures a storage modulus sufficient to compress the black curable resin layer 10 during thermocompression bonding. Furthermore, within this range, flow during thermal curing can be suppressed, and poor appearance after curing, such as repellency, can be suppressed. Furthermore, problems are less likely to occur when etching is performed in a subsequent process. Furthermore, when the amount is equal to or greater than the lower limit, heat resistance in the cured state is improved.
[0081] (Elastomer) The transparent curable resin layer 11 preferably contains an elastomer in addition to a resin such as an epoxy resin. The inclusion of an elastomer makes it easier to control the storage modulus. Examples of elastomers include the same types as those used for the black curable resin layer 10. Among them, NBR is preferred for the following reasons: NBR has good compatibility with epoxy resins. Furthermore, it can increase the storage modulus of the transparent curable resin layer 11 at around 150°C, thereby improving the adhesion between the transparent curable resin layer 11 and the black curable resin layer 10. The preferred weight-average molecular weight of the elastomer is the same as that of the black curable resin layer 10.
[0082] In particular, when the transparent curable resin layer 11 is composed of an epoxy resin composition, it preferably contains a modified elastomer having a functional group capable of reacting with an epoxy group. The modified elastomer also functions as a curing agent for the epoxy resin. Furthermore, because it reacts with and bonds to the epoxy resin, it improves heat resistance and reliability against thermal shock. Furthermore, the difference in polarity between the functional group and the resin backbone favorably affects dispersibility. This allows for favorable dispersibility when carbon black is incorporated into the transparent curable resin layer 11.
[0083] Examples of functional groups capable of reacting with an epoxy group include the same types as those of the black curable resin layer 10. Among them, an acid group or an acid anhydride group is preferred, and a carboxy group or a carboxylic acid anhydride group is particularly preferred, because they can be cured at low temperatures and ensure a long usable time.
[0084] When the transparent curable resin layer 11 is composed of an epoxy resin composition, it particularly preferably contains modified NBR having a carboxy group. Examples of modified NBR having a carboxy group include the same types as those used for the black curable resin layer 10. Two or more types of modified elastomers having a functional group reactive with an epoxy group may be used in combination.
[0085] The amount of elastomer in the transparent curable resin layer 11 is preferably 0 to 50 parts by mass, more preferably 1 to 50 parts by mass, and even more preferably 5 to 50 parts by mass, relative to 100 parts by mass of the total resin solids content of the transparent curable resin layer 11. Within this range, the storage modulus can be controlled. Furthermore, when the amount is equal to or less than the upper limit, a storage modulus sufficient to compress the black curable resin layer 10 during thermocompression bonding can be ensured. Furthermore, flow during thermal curing can be suppressed, and poor appearance after curing, such as repellency, can be suppressed. Furthermore, problems are less likely to occur when etching is performed in a subsequent process. Furthermore, when the amount is equal to or greater than the lower limit, the dispersibility of carbon black is improved. Furthermore, film-formability is improved, and the film thickness distribution can be narrowed when the epoxy resin composition is applied to form a film.
[0086] (hardening agent) When the transparent curable resin layer 11 is composed of an epoxy resin composition, it may contain, in addition to the modified elastomer having a functional group reactive with an epoxy group, other curing agents for epoxy resins. Examples of other curing agents include the same curing agents as those used in the black curable resin layer 10. Two or more types of other curing agents may be used in combination.
[0087] (curing catalyst) When the transparent curable resin layer 11 is made of an epoxy resin composition, it may contain a curing catalyst that accelerates the curing reaction of the epoxy resin. Examples of the curing catalyst include the same curing catalysts as those used for the black curable resin layer 10, and preferred embodiments are also the same.
[0088] The blending amount of the curing catalyst is preferably 0.01 to 5 parts by mass, more preferably 0.05 to 4 parts by mass, and even more preferably 0.1 to 3 parts by mass, relative to 100 parts by mass of the total resin solid content of the transparent curing resin layer 11. Within the above range, curing can be sufficiently promoted, and the usable life of the one-piece encapsulating sheet 1 can be ensured. Two or more types of curing catalysts may be used in combination.
[0089] (Silane coupling agent) The transparent curable resin layer 11 preferably contains a silane coupling agent. The silane coupling agent is a silane compound represented by the following chemical formula (I) that has at least one hydrolyzable group and one or more organic functional groups. The silane coupling agent chemically bonds the cured transparent curable resin layer 11 (the transparent resin layer 31 described below) and the base layer 12 through a cross-linking reaction caused by heating. The addition of the silane coupling agent can further improve the long-term reliability of the light-emitting electronic component 5 under high-temperature and high-humidity conditions.
[0090] [ka] (R represents an organic functional group. R 2 and R 3 (OR) indicates a methyl group or an ethyl group, respectively. 2 ) n represents a hydrolyzable group. n in chemical formula (I) is 1 to 3. Although not shown, a spacer consisting of a saturated hydrocarbon chain may be present between the silicon atom and the organic reactive group and / or the hydrolyzable group.
[0091] The organic functional group of the silane coupling agent is not particularly limited as long as it is not a vinyl group, but may be, for example, an epoxy group, an amino group, a methacryl group, an isocyanate group, or a mercapto group. The organic functional group is preferably one or more selected from methacryl groups or isocyanate groups, more preferably an isocyanate group. The silane coupling agent may be a multifunctional silane coupling agent containing two or more organic functional groups, as long as it does not contain a vinyl group as the organic functional group. Alternatively, a functional group-protected silane coupling agent in which the organic functional group is protected with a protecting group or the like until the reaction begins may be used. When the organic reactive group is protected with a protecting group, the deprotection method is not particularly limited. However, from the viewpoint of being able to deprotect the organic reactive group in parallel with the curing of the transparent curable resin layer 11, it is preferable that the organic reactive group be deprotected by heating to generate the organic functional group.
[0092] The hydrolyzable group of the silane coupling agent is not particularly limited, but is, for example, an alkoxy group such as an ethoxy group or a methoxy group. The silane coupling agent is preferably a dialkoxy type containing two alkoxy groups or a trialkoxy type containing three alkoxy groups, and more preferably a trialkoxy type having a high density of hydrolyzable groups from the viewpoint of improving adhesion.
[0093] (Silicone filler) The transparent curable resin layer 11 preferably further contains a silicone filler. The silicone filler is a filler of a polymer compound having a main skeleton formed by siloxane bonds. Examples of the silicone filler include a silicone resin or silicone rubber filler. The form of the silicone filler is not particularly limited, but is preferably granular. By containing the silicone filler, the transparent curable resin layer 11 can be provided with adhesion and light diffusion properties at high temperatures. By containing the silicone filler in the transparent curable resin layer 11, a transparent resin layer having appropriate hardness even in a high-temperature environment can be obtained. Furthermore, adhesion between the transparent resin layer and the support 15 can be ensured. Consequently, the long-term reliability of the integrated encapsulating sheet 1 can be improved. Furthermore, by providing the transparent curable resin layer 11 with light diffusion properties, incident light from the light-emitting elements 21, 22, and 23 can be diffused. Even if the light-emitting elements 21, 22, and 23 are light-emitting diodes such as mini LEDs or micro LEDs with high directionality, brightness unevenness due to viewing angles can be suppressed. Furthermore, by using it in combination with the above-mentioned silane coupling agent, the polar functional groups contained in the silicone filler and the cured resin (i.e., the resin contained in the transparent resin layer) are partially bonded to the silane coupling agent, thereby suppressing swelling and changes in refractive index of the resin in the transparent resin layer due to moisture absorption even in a high-humidity environment, and maintaining light diffusion properties.
[0094] The amount of silicone filler blended is preferably 3 to 40 parts by mass, more preferably 5 to 20 parts by mass, and even more preferably 7 to 15 parts by mass, per 100 parts by mass of the total resin solid content. If the amount is equal to or greater than the lower limit, the effect of reducing brightness unevenness is likely to be achieved. By blending the amount of silicone filler blended is equal to or less than the upper limit, an excessive increase in the L* value can be suppressed, and the blackness can be maintained when the display is turned off.
[0095] The average particle size of the silicone filler is not particularly limited, but is preferably 1 to 5.5 μm, and more preferably 1.5 to 5 μm. In this specification, the average particle size of the silicone filler is defined as the cumulative average diameter D in the volume-based particle size distribution determined by a laser diffraction / scattering method. 50 The measurement device used in the laser diffraction / scattering method is the MT3300EXII manufactured by Microtrack Bell.
[0096] (Other ingredients) The transparent curable resin layer 11 may contain a black pigment to suppress uneven light emission and uneven color.
[0097] When the transparent curable resin layer 11 contains carbon black, the amount of carbon black is preferably less than 5 parts by mass, more preferably 1 part by mass or less, and even more preferably 0.1 parts by mass or less, relative to 100 parts by mass of the total resin solids content. The transparent curable resin layer 11 may further contain, as necessary, a resin other than the epoxy resin and elastomer, a thickener, a defoaming agent and / or a leveling agent, an adhesion imparting agent such as a coupling agent, and a flame retardant.
[0098] [Film thickness] The thickness of the transparent curable resin layer 11 is not particularly limited, but is preferably 10 to 250 μm, more preferably 20 to 225 μm, and even more preferably 25 to 150 μm.
[0099] (3) Support The support 15 is a layer or laminate for supporting the transparent curable resin layer 11. In this embodiment, the support 15 is a laminate in which two layers, a substrate layer 12 and a hard coat layer 16, are laminated in this order from the side of the transparent curable resin layer 11 that contacts the side opposite the side that contacts the black curable resin layer 10. However, the support 15 is not limited to this and may be arranged so that the substrate layer 12 contacts the transparent curable resin layer 11. For example, the support 15 may be a single layer consisting of only the substrate layer 12, or may be a laminate in which three or more identical or different functional layers are laminated. Each layer that can constitute the support 15 according to this embodiment will be described below.
[0100] (3-1) Base material layer The substrate layer 12 is a layer for supporting the transparent curable resin layer 11. When the above-mentioned support 15 is a single layer, the substrate layer 12 is the same as the support 15. When the integrated encapsulating sheet 1 includes a light diffusion layer 13 described later, the substrate layer 12 also serves as a layer for separating the light diffusion layer 13 from the light emitting elements 21, 22, and 23. The substrate layer 12 is a curable layer. In the present embodiment, the substrate layer 12 is formed between the transparent curable resin layer 11 and the hard coat layer 16.
[0101] [Film thickness] The thickness of the base layer 12 is not particularly limited, but is preferably 20 to 300 μm, more preferably 25 to 200 μm, and even more preferably 25 to 100 μm. When the thickness of the base layer 12 is within the above range, uneven brightness can be suppressed.
[0102] [Total light transmittance] The total light transmittance of the base layer 12 is preferably adjusted to 30 to 99%, more preferably adjusted to 35 to 95%, and even more preferably adjusted to 40 to 95%. When the total light transmittance of the base layer 12 is equal to or greater than the lower limit, light is not prevented from reaching the viewer's side.
[0103] [Storage modulus] The storage modulus of the base layer 12 at 60°C is preferably 7×10 8 ~2×1010 Pa, more preferably 1×10 9 ~1×10 10 Pa, and even more preferably 2×10 9 ~6×10 9 Pa. When the storage modulus of the base layer 12 at 60° C. is equal to or less than the preferred upper limit, cracking of the base layer 12 can be reduced.
[0104] The storage modulus of the base layer 12 at 100° C. is preferably greater than the storage modulus of the black curable resin layer 10 and the transparent curable resin layer 11 in an uncured state at 100° C. The storage modulus of the base layer 12 is preferably 1×10 9 ~5×10 9 Pa, and more preferably 2×10 9 ~4×10 9 Pa. This makes it difficult for the black curable resin layer 10 to remain on the light emitting elements 21, 22, and 23.
[0105] [resin] The substrate layer 12 may be composed of a thermoplastic resin or a thermosetting resin. Examples of resins that may be used for the substrate layer 12 include polyethylene terephthalate resin, polybutylene terephthalate resin, polyethylene 2,6-naphthalate resin, polyamide resin, polycarbonate resin, polycarbonate copolymer resin, triacetyl cellulose resin, polymethylpentene resin, phenoxy resin, syndiotactic polystyrene resin, and polyimide resin. In terms of heat resistance, weather resistance, availability, cost, and other factors, the substrate layer 12 preferably contains at least one resin selected from polyethylene terephthalate resin, polyethylene 2,6-naphthalate resin, polycarbonate resin, polycarbonate copolymer resin, and polyamide resin. The inclusion of these resins can prevent deformation during pressure bonding. The substrate layer 12 may also contain a black pigment to suppress uneven light emission and color.
[0106] (3-2) Hard Coat Layer The hard coat layer 16 has a scratch-resistant effect on the base layer 12 or the second base layer 14 described below, and is a layer for protecting the light-emitting electronic component 5 from scratches, and is an optional component of the support 15. The hard coat layer 16 may be provided with a protective sheet 18 described below on the surface opposite to the surface in contact with the base layer 12 or the second base layer 14. The hard coat layer 16 is a cured layer. In this embodiment, the hard coat layer 16 is laminated on the base layer 12 and covered with the protective sheet 18.
[0107] [Surface hardness] The surface hardness of the hard coat layer 16 is not particularly limited, but is, for example, preferably H or more, more preferably 2H or more, and further more preferably 3H or more in pencil hardness. By providing the hard coat layer 16, the surface hardness of the one-piece encapsulating sheet 1 can be increased.
[0108] [Surface roughness] The surface roughness of the hard coat layer 16 is expressed as the arithmetic mean roughness (Ra). The arithmetic mean roughness (Ra) is preferably 0.1 to 1 μm, more preferably 0.2 to 1 μm, and even more preferably 0.3 to 1 μm. When the Ra of the hard coat layer 16 is equal to or greater than the preferred lower limit, the reflectance of the surface of the hard coat layer 16 can be reduced. When the Ra of the hard coat layer 16 is equal to or less than the preferred upper limit, production can be facilitated.
[0109] [Total light transmittance] The hard coat layer 16 is preferably prepared so that the total light transmittance is 30 to 99%, more preferably 50 to 99%, and even more preferably 60 to 99%. When the total light transmittance of the hard coat layer 16 is equal to or greater than the lower limit, light reaching the viewer side is not hindered.
[0110] [resin] The hard coat layer 16 may be composed of either a thermoplastic resin or a thermosetting resin, and is preferably composed of a thermosetting resin. Examples of the thermosetting resin that constitutes the hard coat layer 16 include acrylic resin, polyurethane resin, silicone resin, melamine resin, etc., and the hard coat layer 16 may contain one or more of these. The hard coat layer 16 may also contain a black pigment.
[0111] [Fine particles] The hard coat layer 16 may contain fine particles. As the fine particles, inorganic fine particles, organic fine particles, or both can be used. Examples of inorganic fine particles include silica fine particles and titanium fine particles. Examples of organic fine particles include polymethyl methacrylate resin (PMMA resin) and polyurethane resin. Among these, silica fine particles are preferred. By including fine particles, the surface roughness of the hard coat layer 16 can be adjusted and the surface hardness can be improved.
[0112] [Film thickness] The thickness of the hard coat layer 16 is preferably 1 to 20 μm, more preferably 2 to 10 μm, and even more preferably 3 to 8 μm. When the thickness of the hard coat layer 16 is equal to or greater than the preferred lower limit, sufficient hardness can be ensured. When the thickness of the hard coat layer 16 is equal to or less than the preferred upper limit, defects such as curling do not occur.
[0113] (4) Protective sheet The protective sheets 17 and 18 have a role of protecting the integrated encapsulating sheet 1. When the integrated encapsulating sheet 1 is formed, the protective sheet 17 can also be used as a sheet onto which a coating liquid of a curable resin composition for the black curable resin layer 10 is applied.
[0114] The protective sheets 17 and 18 may be made of, for example, polyester such as polyethylene terephthalate or polyethylene naphthalate, or a thermoplastic resin such as polyimide, polyamide-imide, polyethylene, polytetrafluoroethylene, polypropylene, or polystyrene, or surface-treated paper.
[0115] Among these, polyester sheets are preferred from the viewpoints of heat resistance, mechanical strength, ease of handling, etc. The thickness of the protective sheets 17, 18 is not particularly limited and may be selected appropriately depending on the application within the range of approximately 10 to 150 μm. The surface of the protective sheet 17 on which the black curable resin layer 10 is to be provided may be subjected to a release treatment.
[0116] 2. Manufacturing method of integrated encapsulating sheet In the present embodiment, to obtain the integrated encapsulating sheet 1, first, a sheet (hereinafter also referred to as a transparent layer laminated sheet) is prepared by applying and drying a coating liquid of a curable resin composition for the transparent curable resin layer 11 to the surface opposite to the surface on which the hard coat layer 16 is formed, of the substrate layer 12 having the hard coat layer 16 formed on one surface in advance. Further, a sheet (hereinafter also referred to as a black layer laminated sheet) is prepared by applying and drying a coating liquid of a curable resin composition for the black curable resin layer 10 to a protective sheet 17.
[0117] Thereafter, the transparent layer laminate sheet and the black layer laminate sheet are laminated together so that the transparent curable resin layer 11 and the black curable resin layer 10 are in contact with each other, thereby obtaining a laminate in which the black curable resin layer 10, the transparent curable resin layer 11, the base layer 12, and the hard coat layer 16 are laminated in this order on the protective sheet 17. A protective sheet 18 may be laminated on the outer surface of the hard coat layer 16, if necessary.
[0118] The coating liquid of the curable resin composition for the black curable resin layer 10 and the transparent curable resin layer 11 preferably contains an organic solvent in an amount that provides a viscosity sufficient for smooth coating. The organic solvent is not particularly limited, but examples thereof include ketones, aromatic hydrocarbons, glycol ethers, glycol ether acetates, esters, alcohols, aliphatic hydrocarbons, and petroleum-based solvents. Specific examples include ketones such as methyl ethyl ketone, cyclohexanone, methyl butyl ketone, and methyl isobutyl ketone; aromatic hydrocarbons such as toluene, xylene, and tetramethylbenzene; glycol ethers such as cellosolve, methyl cellosolve, butyl cellosolve, carbitol, methyl carbitol, butyl carbitol, ethylene glycol monomethyl ether, ethylene glycol monoethyl ether, ethylene glycol monobutyl ether, propylene glycol monomethyl ether, dipropylene glycol monomethyl ether, dipropylene glycol diethyl ether, and triethylene glycol monoethyl ether; ethyl acetate, butyl acetate, isobutyl acetate, and ethylene glycol monoethyl ether. Examples of suitable solvents include esters such as propylene glycol monoethyl ether acetate, dipropylene glycol methyl ether acetate, propylene glycol methyl ether acetate, propylene glycol ethyl ether acetate, and propylene glycol butyl ether acetate; alcohols such as ethanol, propanol, 2-methoxypropanol, n-butanol, isobutyl alcohol, isopentyl alcohol, ethylene glycol, and propylene glycol; aliphatic hydrocarbons such as octane and decane; petroleum solvents such as petroleum ether, petroleum naphtha, hydrogenated petroleum naphtha, and solvent naphtha, as well as N,N-dimethylformamide (DMF), tetrachloroethylene, and turpentine. When incorporating carbon black into the coating liquid, carbon black powder may be added to the coating liquid, or a liquid in which carbon black has been previously dispersed (carbon black dispersion) may be added.
[0119] Examples of methods for applying the curable resin composition include methods using various coaters such as a die coater, gravure coater, roll coater, curtain flow coater, spin coater, bar coater, reverse coater, kiss coater, fountain coater, rod coater, air doctor coater, knife coater, blade coater, cast coater, and screen coater. The drying temperature is preferably 80 to 160°C, more preferably 80 to 130°C, and even more preferably 80 to 120°C, so as not to excessively reduce the amount of volatilization of the organic solvent. Here, the drying process is performed so that the total weight loss due to curing of the black curable resin layer 10 and the transparent curable resin layer 11 is in the range of 0.3 to 10%.
[0120] The temperature during lamination is preferably 20 to 120°C, more preferably 30 to 100°C, and even more preferably 40 to 80°C. By setting the temperature at or above the preferred lower limit, it is possible to ensure adhesion between the black curable resin layer 10 and the transparent curable resin layer 11 that allows handling even in uncured states. Furthermore, by setting the temperature at or below the preferred upper limit, it is possible to prevent air bubbles from being trapped between the black curable resin layer 10 and the transparent curable resin layer 11 and the occurrence of wrinkles in the layers 10 and 11. Lamination can be performed using, for example, a roll laminator, a press, a vacuum press, or the like.
[0121] 3. Substrate with elements As shown in Fig. 2, the element-mounted substrate 2 has a plurality of light-emitting elements 21, 22, and 23 arranged on a substrate 20. Fig. 2 and other figures schematically show a portion where three light-emitting elements (light-emitting element 21, light-emitting element 22, and light-emitting element 23) are arranged.
[0122] There is no limitation on the material of the substrate 20, but known printed circuit boards can be suitably used, such as epoxy glass substrates, fluororesin substrates, ceramic substrates, and glass substrates.
[0123] The light-emitting elements 21, 22, and 23 are typically light-emitting diodes. This embodiment is particularly suitable for cases where the light-emitting elements 21, 22, and 23 are extremely small. For example, light-emitting diodes with a height of 1000 nm to 200 μm and a side length of 0.001 to 0.5 mm can be used. The element-mounted substrate 20 for obtaining mini LEDs or micro LEDs can use light-emitting diodes of three colors (R, G, and B) or blue light-emitting diodes as the light-emitting elements 21, 22, and 23. Furthermore, the heights of the multiple light-emitting elements 21, 22, and 23 on the substrate 20 do not all need to be the same, and may be different from each other, preferably at least at one point.
[0124] 4. Light-emitting electronic components and manufacturing methods thereof The light-emitting electronic component 5 comprises an element-mounted substrate 2 having a plurality of light-emitting elements 21, 22, 23 arranged on a substrate 20, and an integrated encapsulating cured sheet 3 pressed against the surface of the element-mounted substrate 2 on which the plurality of light-emitting elements 21, 22, 23 are arranged.
[0125] The integrated encapsulating cured sheet 3 is formed by laminating, in this order from at least the side in contact with the element-mounted substrate 2, a black resin layer 30 capable of blocking light between the light emitting elements 21, 22, and 23, and a transparent resin layer 31 having higher light transmittance than the black resin layer 30. Furthermore, in this embodiment, a support 15 supporting the transparent resin layer 31 is laminated on the surface of the transparent resin layer 31 opposite to the surface in contact with the black resin layer 30. The black resin layer 30 and the transparent resin layer 31 are layers formed after the black curable resin layer 10 and the transparent curable resin layer 11 are cured. That is, the integrated encapsulating cured sheet 3 is a sheet formed from the above-mentioned integrated encapsulating sheet 1 after the black curable resin layer 10 and the transparent curable resin layer 11 are cured. As described above, the total thickness of the black curable resin layer 10, which is the black resin layer 30 before curing, and the transparent curable resin layer 11, which is the transparent resin layer 31 before curing, is greater than the height of the plurality of light emitting elements 21, 22, 23, and the total weight loss rate due to curing of the black curable resin layer 10 and the transparent curable resin layer 11 is 0.3 to 10%. The weight loss rate is preferably 1 to 9%, more preferably 2 to 8%, and even more preferably 2.5 to 7%. When the weight loss rate is within this range, the generation of bubbles in the black resin layer 30 and the transparent resin layer 31 can be suppressed, thereby further suppressing poor appearance and poor sealing of the light-emitting electronic component 5.
[0126] In this embodiment, the integrated encapsulating cured sheet 3 has the black resin layer 30, the transparent resin layer 31, the base material layer 12, and the hard coat layer 16 laminated in this order from the side that contacts the element-mounted substrate 2. In the integrated encapsulating cured sheet 3 of this embodiment, preferably at least the black resin layer 30 is filled between the light emitting elements 21, 22, and 23.
[0127] The thickness of the transparent resin layer 31 is not particularly limited, but is preferably 0.1 to 5.0 times the height of the plurality of light-emitting elements 21, 22, and 23. The thickness of the black resin layer 30 is not particularly limited, but is preferably 0.1 to 0.9 times the height of the plurality of light-emitting elements 21, 22, and 23.
[0128] The method for manufacturing a light-emitting electronic component includes the steps of: placing the black curable resin layer 10 side of the integrated encapsulating sheet 1 on the surface of the element-mounted substrate 2, on which the plurality of light-emitting elements 21, 22, 23 are arranged, and starting pressure bonding (hereinafter referred to as the placing step); continuing pressure bonding to fill the spaces between the plurality of light-emitting elements 21, 22, 23 with at least a portion of the black curable resin layer 10 and the transparent curable resin layer 11 (hereinafter referred to as the filling step); and curing the filled black curable resin layer 10 and the transparent curable resin layer 11 (hereinafter referred to as the curing step). Hereinafter, a method for manufacturing a light-emitting electronic component according to one embodiment will be described with reference to FIGS. 2 to 4.
[0129] (i) Placement process In the arrangement step, first, the protective sheet 17 is peeled off to expose the black curable resin layer 10. Thereafter, as shown in FIG. 2 , the black curable resin layer 10 is brought into contact with the surface of the element-mounted substrate 2 on which the light emitting elements 21, 22, and 23 are arranged, and pressure bonding of the integrated encapsulating sheet 1 is started.
[0130] Before compression bonding, the thickness of the black curable resin layer 10 is preferably 10 to 95% of the height of the light emitting elements 21, 22, 23. The lower limit is more preferably 15% or more, and even more preferably 30% or more. The upper limit is more preferably 85% or less, and even more preferably 75% or less.
[0131] When the thickness of the black curable resin layer 10 is 10% or more of the height of the light-emitting elements 21, 22, and 23, the black curable resin layer 10 has a sufficient light-shielding function between the light-emitting elements 21, 22, and 23. Furthermore, when the black curable resin layer 10 has a relatively low storage modulus and high fluidity, the resin can be sufficiently filled between the light-emitting elements 21, 22, and 23. When the thickness of the black curable resin layer 10 is 15% or more of the height of the light-emitting elements 21, 22, and 23, crack-like defects are less likely to occur on the surface even when the fluidity of the transparent curable resin layer 11 is relatively low. When the thickness of the black curable resin layer 10 is 30% or more of the height of the light-emitting elements 21, 22, and 23, the black curable resin layer 10 having a light-shielding function can be appropriately filled between the light-emitting elements 21, 22, and 23.
[0132] If the thickness of the black curable resin layer 10 is 95% or less of the height of the light emitting elements 21, 22, and 23, leakage of the black curable resin layer 10 to the outside during thermocompression bonding can be prevented, and light from the light emitting elements 21, 22, and 23 is less likely to be hindered from reaching the viewer. If the thickness of the black curable resin layer 10 is 85% or less of the height of the light emitting elements 21, 22, and 23, fluctuations in the film thickness of the black curable resin layer 10 that flows after pressing are less likely to occur, and variations in black shading are less likely to occur. If the thickness of the black curable resin layer 10 is 75% or less of the height of the light emitting elements 21, 22, and 23, the black curable resin layer 10, which has a light-blocking function, can be appropriately filled between the light emitting elements 21, 22, and 23.
[0133] The thickness of the transparent curable resin layer 11 before compression bonding is preferably 10 to 500% of the height of the light emitting elements 21, 22, 23. The lower limit is more preferably 20% or more, and even more preferably 30% or more. The upper limit is more preferably 200% or less, and even more preferably 150% or less.
[0134] When the thickness of the transparent curable resin layer 11 is 10% or more of the height of the light-emitting elements 21, 22, and 23, the transparent curable resin layer 11 easily functions as a sealing layer covering the light-emitting elements 21, 22, and 23. Furthermore, when the storage modulus of the transparent curable resin layer 11 is relatively high and the fluidity of the transparent curable resin layer 11 is suppressed, the transparent curable resin layer 11 can be prevented from flowing together with the black curable resin layer 10 during thermal curing, making it less likely for poor appearance to occur on the surface. When the thickness of the transparent curable resin layer 11 is 20% or more of the height of the light-emitting elements 21, 22, and 23, the range in which the transparent curable resin layer 11 can flow is sufficient, making it less likely for crack-like defects to occur on the surface. When the thickness of the transparent curable resin layer 11 is 30% or more of the height of the light-emitting elements 21, 22, and 23, the transparent curable resin layer 11 easily functions as a sealing layer covering the light-emitting elements 21, 22, and 23. Furthermore, when the storage modulus of the transparent curable resin layer 11 is relatively high and the fluidity of the layer 11 is suppressed, the transparent curable resin layer 11 can sufficiently press into the black curable resin layer 10.
[0135] The total thickness of the black curable resin layer 10 and the transparent curable resin layer 11 before compression bonding is preferably 110 to 550% of the height of the light emitting elements 21, 22, and 23. When the total thickness is equal to or greater than the above-mentioned lower limit value with respect to the height of the light emitting elements 21, 22, and 23, a part of the integrated encapsulating sheet 1 can be sufficiently embedded between the light emitting elements 21, 22, and 23. When the total thickness is equal to or less than the above-mentioned upper limit value with respect to the height of the light emitting elements 21, 22, and 23, thickness unevenness is unlikely to occur during compression bonding, and poor appearance is unlikely to occur on the surface.
[0136] The ratio of the thickness of the black curable resin layer 10 before compression bonding to the total thickness of the transparent curable resin layer 11 and the black curable resin layer 10 before compression bonding is preferably 10 to 90%, more preferably 15 to 70%. If this thickness ratio is equal to or greater than the above-mentioned lower limit, the degree of blackness can be increased and the contrast of the display can be sufficiently improved. If this thickness ratio is equal to or less than the above-mentioned upper limit, the black curable resin layer 10 is less likely to remain on the light-emitting elements 21, 22, and 23 during compression bonding, and brightness can be sufficiently improved.
[0137] (ii) Filling process Next, pressure bonding is continued to embed at least a part of the black curable resin layer 10 and the transparent curable resin layer 11 of the integrated encapsulating sheet 1 between the light emitting elements 21, 22, and 23 as shown in FIG. 3. At this time, the black curable resin layer 10 and the transparent curable resin layer 11 are filled between the plurality of light emitting elements 21, 22, and 23. At this time, if the storage modulus of the black curable resin layer 10 is relatively low and the fluidity of the layer 10 is ensured, the black curable resin layer 10 will easily follow the unevenness of the light emitting elements 21, 22, and 23 and fill between the light emitting elements 21, 22, and 23.
[0138] The temperature in the thermocompression bonding is preferably 80 to 120°C, more preferably 90 to 110°C. By setting the temperature to 80°C or higher, the fluidity of the black curing resin layer 10 of the integrated encapsulating sheet 1 is easily ensured. Furthermore, by setting the temperature to 120°C or lower, the light emitting elements 21, 22, and 23 are less likely to be damaged. By setting the temperature to 90 to 110°C, the fluidity of the black curing resin layer 10 can be controlled more precisely, and the occurrence of unevenness and crack-like defects can be suppressed.
[0139] The pressure in the thermocompression bonding is 0.05 to 5.0 MPa, preferably 0.05 to 1.0 MPa, and more preferably 0.1 to 0.5 MPa. By setting the pressure to a preferred lower limit or higher, the black curable resin layer 10 can be sufficiently filled between the light emitting elements 21, 22, and 23. By setting the pressure to a preferred upper limit or lower, damage to the light emitting elements 21, 22, and 23 is reduced. The thermocompression bonding is preferably performed using a vacuum press capable of molding in a vacuum state. This makes it easier to avoid defects caused by air being mixed into the resulting light-emitting electronic component 5.
[0140] (iii) Curing process After the pressure-bonding, as shown in FIG. 4, the protective sheet 18 is peeled off and then thermally cured, so that the black curable resin layer 10 and the transparent curable resin layer 11 of the integrated encapsulating sheet 1 become a black resin layer 30 (a cured layer of the black curable resin layer 10) and a transparent resin layer 31 (a cured layer of the transparent curable resin layer 11), thereby obtaining a light-emitting electronic component 5.
[0141] The curing temperature is preferably 100 to 160°C, and more preferably 110 to 150°C. By setting the curing temperature to 100°C or higher, the black curable resin layer 10 and the transparent curable resin layer 11 of the integrated encapsulating sheet 1 can be reliably cured. By setting the curing temperature to 110°C or higher, the curing time of the black curable resin layer 10 and the transparent curable resin layer 11 can be shortened. Furthermore, by setting the curing temperature to the above upper limit temperature or lower, the light emitting elements 21, 22, and 23 are less likely to be damaged.
[0142] The curing time varies depending on the curing temperature, but is preferably 30 to 360 minutes, more preferably 45 to 180 minutes. If the storage modulus of the transparent curable resin layer 11 is relatively high and the fluidity of the layer 11 is suppressed at the curing temperature, poor appearance of the black curable resin layer 10 and the transparent curable resin layer 11 after curing can be suppressed.
[0143] The curing step is preferably carried out stepwise at two or more temperature and / or time stages. By carrying out the curing stepwise, the generation of bubbles in the light-emitting electronic component 5 can be more reliably suppressed as long as the weight loss rate of the integrated encapsulating sheet 1 is within the above-mentioned numerical range.
[0144] 2 to 4 , a light-emitting electronic component 5 is obtained in which the element-mounted substrate 2 has a plurality of light-emitting elements 21, 22, and 23 arranged on a substrate 20, and the integrated encapsulating cured sheet 3 is pressure-bonded to the surface on which the light-emitting elements 21, 22, and 23 are arranged. In the obtained light-emitting electronic component 5 according to this embodiment, the black curable resin layer 10 and the transparent curable resin layer 11 are cured to form the black resin layer 30 and the transparent resin layer 31. Furthermore, at least the black resin layer 30 is filled between the plurality of light-emitting elements 21, 22, and 23.
[0145] (Second embodiment) FIG. 5 shows a cross-sectional view of an integrated encapsulant sheet and a light-emitting electronic component according to a second embodiment, taken in the same direction as FIG. 1. The integrated encapsulant sheet 1a according to this embodiment includes a black curable resin layer 10, a transparent curable resin layer 11, and a support 15a. The support 15a differs from the support 15 in that it includes a light diffusion layer 13. The support 15a in this embodiment is a laminate in which four layers, namely, a substrate layer 12, a light diffusion layer 13, a second substrate layer 14, and a hard coat layer 16, are laminated in this order from the side contacting the surface of the transparent curable resin layer 11 opposite to the side contacting the black curable resin layer 10. That is, the integrated encapsulant sheet 1a according to this embodiment is a laminate in which the black curable resin layer 10, the transparent curable resin layer 11, the substrate layer 12, the light diffusion layer 13, the second substrate layer 14, and the hard coat layer 16 are laminated in this order. However, the configuration of the support 15a is not limited to four layers, and may be two to three layers, or five or more layers, as long as it includes the base layer 12 and the light diffusion layer 13. Furthermore, the components of the support 15a excluding the base layer 12 and the light diffusion layer 13 are not limited to the second base layer 14 and the hard coat layer 16, and various known functional layers may be laminated. In Figure 5, protective sheets 17 and 18 are further provided so as to be in contact with the black curable resin layer 10 and the hard coat layer 16.
[0146] The value of Ttotal in the integrated encapsulating sheet 1a according to the present embodiment is the total thickness of the black curable resin layer 10, the transparent curable resin layer 11, and the support 15a (in the present embodiment, including four layers: the substrate layer 12, the light diffusion layer 13, the second substrate layer 14, and the hard coat layer 16).
[0147] Hereinafter, each layer that can constitute the support 15a according to this embodiment will be described, but the contents that overlap with those of the support 15 will be omitted.
[0148] (3-3) Light diffusion layer The light diffusion layer 13 contains a filler and is a layer for diffusing incident light from the light emitting elements 21, 22, and 23. The light diffusion layer 13 may be a cured layer or an uncured layer, but is preferably a cured layer. In this embodiment, the light diffusion layer 13 is formed between the base layer 12 and the second base layer 14, but is not limited thereto and may not be in contact with the base layer 12.
[0149] By providing the light diffusion layer 13 separately from the curable resin layer containing a black colorant (in this embodiment, the black curable resin layer 10), it is possible to suppress uneven brightness without the need for the curable resin layer containing a black colorant to cover the entire light emitting elements 21, 22, 23. Furthermore, since the curable resin layer containing a black colorant does not need to cover the upper surfaces (light emitting surfaces) of the light emitting elements 21, 22, 23, light reaching the viewer side from the light emitting elements 21, 22, 23 is not hindered when the display emits light.
[0150] [Photocurable resin composition] The light diffusion layer 13 is a layer containing a curable resin composition, preferably a photocurable resin composition. In this specification, the "photocurable resin composition" is preferably a photocurable resin composition containing at least one resin selected from an epoxy resin, an acrylic resin, and / or a polyurethane resin, and a photopolymerization initiator. The light diffusion layer 13 also contains a filler, which will be described later, in the curable resin composition.
[0151] The light diffusion layer 13 is not particularly limited, but is preferably a cured layer containing at least one of an epoxy resin, an acrylic resin, and / or a polyurethane resin. By using these resins, the heat resistance of the light diffusion layer 13 can be improved.
[0152] When an epoxy resin is used for the light diffusion layer 13, any of the above-mentioned epoxy resins may be used as appropriate, but it is preferable to use an alicyclic epoxy resin, which has high curing properties when exposed to ultraviolet light and is less likely to yellow when exposed to sunlight. An example of such an alicyclic epoxy resin is "8EC-001" manufactured by Taisei Fine Chemical Co., Ltd.
[0153] In the present application, "acrylic resin" refers to a resin having an acrylic skeleton and / or a methacrylic skeleton. When an acrylic resin is used for the light diffusion layer 13, various known acrylic resins can be used, including polymers of acrylic monomers such as acrylic acid esters or methacrylic acid esters, and copolymers of acrylic monomers with other monomers. A specific example of such acrylic resins is "8KX-212" manufactured by Taisei Fine Chemical Co., Ltd. A combination of two or more of these acrylic resins may also be used.
[0154] In this application, "polyurethane resin" refers to a resin having a urethane bond in the molecule. When a polyurethane resin is used for the light diffusion layer 13, examples of the polyurethane resin include polyether-type polyurethane resins containing ether bonds in the main chain in addition to urethane bonds, polyester-type polyurethane resins containing ester bonds in the main chain, and polycarbonate-type polyurethane resins containing carbonate bonds in the main chain. Among these, polycarbonate-type polyurethane resins are preferred, and a specific example is "UF-A7-52" manufactured by Kyoeisha Chemical Co., Ltd. Two or more of these polyurethane resins may be used in combination.
[0155] (Photopolymerization initiator) The photopolymerization initiator contained in the photocurable resin composition is not particularly limited, but when curing an epoxy resin, a photocationic polymerization initiator is preferred. Furthermore, when curing an acrylic resin or a polyurethane resin, a photoradical polymerization initiator is preferred. The photocationic polymerization initiator is preferably an iodonium salt-based photopolymerization initiator. Specific examples of iodonium salt-based photopolymerization initiators include "WPI-113," "WPI-116," "WPI-124," and "WPI-170" manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. The photoradical polymerization initiator is preferably an acylphosphine oxide-based photopolymerization initiator. Specific examples of acylphosphine oxide-based photopolymerization initiators include "Omnirad TPO H" manufactured by IGM Resins BV.
[0156] (sensitizer) The photocurable resin composition may contain a sensitizer, such as Omnirad 127 D manufactured by IGM Resins BV.
[0157] The photocurable resin composition may be cured by light of various wavelengths, such as visible light, electron beams, and / or ultraviolet light, but is preferably cured by ultraviolet light from the viewpoint of handling and cost. That is, the light diffusion layer 13 is preferably an ultraviolet-curable resin.
[0158] [Film thickness] The thickness of the light diffusion layer 13 is not particularly limited, but is preferably 20 to 150 μm, more preferably 30 to 120 μm, even more preferably 50 to 100 μm, and particularly preferably 50 to 80 μm. When the thickness of the light diffusion layer 13 is within the above range, the light reaching the viewer side is not hindered, and the incident light from the light emitting elements 21, 22, and 23 can be efficiently diffused.
[0159] [Filler] In the present application, the term "filler" is not particularly limited as long as it does not prevent light from reaching the viewer side, and any suitable known inorganic filler and / or organic filler can be used as appropriate, with silicone resin being preferred. If the filler is made of such a material, it will not excessively impair the transparency of the light diffusion layer 13 and will not prevent light from reaching the viewer side.
[0160] The addition of filler can diffuse the incident light from the light emitting elements 21, 22, and 23. As a result, even if the light emitting elements 21, 22, and 23 are highly directional elements such as LEDs, the light emitted from the light emitting elements 21, 22, and 23 can be diffused and the light can be output more uniformly. As a result, when used in the light emitting electronic component 5, uneven color and brightness can be improved.
[0161] The form of the filler is not particularly limited, and any form of filler can be used. For example, it may be in the form of irregular particles or granules, and granules are preferred.
[0162] When a silicone resin is used as the filler, any known silicone material having a siloxane bond in the main chain, excluding silicone oil, can be used. Examples of silicone resin fillers include "KMP-706," "X52-1621," and "X52-854" manufactured by Shin-Etsu Chemical Co., Ltd., and "Tospearl 2000B" manufactured by Momentive Corporation.
[0163] The average particle size of the filler is not particularly limited as long as it does not prevent light from reaching the viewer side, but is preferably 0.5 to 10 μm, more preferably 1.0 to 5.5 μm, and even more preferably 1.5 to 5.5 μm. When the average particle size of the filler is within the above numerical range, it is possible to suppress uneven brightness while increasing the blackness when the display is turned off. The average particle size of the filler can be measured in the same manner as for the silicone filler contained in the transparent curable resin layer 11 described above.
[0164] The filler content is not particularly limited as long as it does not prevent light from reaching the viewer side, but the mass ratio of the filler is preferably 5 to 40 parts by mass, and more preferably 10 to 30 parts by mass, per 100 parts by mass of the resin solid content of the light diffusion layer 13. When the filler content is within the above range, it is possible to suppress uneven brightness and increase the blackness when the display is turned off.
[0165] (Silane coupling agent) The light diffusion layer 13 may contain a silane coupling agent, similar to the transparent curable resin layer 11. The preferred embodiments are the same as those of the transparent curable resin layer 11.
[0166] (3-4) Second base layer The second substrate layer 14 is a layer for supporting the light diffusion layer 13, and is an optional component constituting the support 15a. The second substrate layer 14 may be the outermost layer of the one-piece encapsulant sheet 1, but may preferably have a hard coat layer 16 (described later) on the surface opposite to the surface in contact with the light diffusion layer 13. In the present embodiment, the second substrate layer 14 is formed between the light diffusion layer 13 and the hard coat layer 16.
[0167] [Film thickness] The thickness of the second base layer 14 is preferably 10 to 250 μm, more preferably 20 to 225 μm, and even more preferably 25 to 150 μm. When the thickness of the second base layer 14 is equal to or greater than the preferred lower limit, it is possible to suppress the occurrence of wrinkles when the integrated encapsulating sheet 1 is thermocompression bonded to the plurality of light emitting elements 21, 22, and 23, and also to improve the handleability. When the thickness of the second base layer 14 is equal to or less than the preferred upper limit, it is possible to improve the visibility and reduce the cost.
[0168] The material of the second base material layer 14 may be the same as or different from the material of the base material layer 12. Other preferred aspects are the same as those of the base material layer 12 described above.
[0169] 2. Manufacturing method of integrated encapsulating sheet In this embodiment, to obtain the integrated encapsulating sheet 1a, first, a coating liquid of a photocurable resin composition for the light diffusion layer 13 is applied and dried on the surface opposite to the surface on which the hard coat layer 16 has been formed of the second substrate layer 14 in advance on one surface. Furthermore, the substrate layer 12 is laminated on the surface of the coating liquid opposite to the surface in contact with the second substrate layer 14, and the coating liquid is photocured. Thereafter, a sheet (hereinafter also referred to as a second transparent layer laminated sheet) is prepared by applying and drying a coating liquid of a curable resin composition for the transparent curable resin layer 11 on the surface of the substrate layer 12 opposite to the surface in contact with the light diffusion layer 13. Furthermore, a sheet (hereinafter also referred to as a black layer laminated sheet) is prepared by applying and drying a coating liquid of a curable resin composition for the black curable resin layer 10 on a protective sheet 17.
[0170] Thereafter, the second transparent layer laminate sheet and the black layer laminate sheet are laminated together so that the transparent curable resin layer 11 and the black curable resin layer 10 are in contact with each other, thereby obtaining a laminate in which the black curable resin layer 10, the transparent curable resin layer 11, the substrate layer 12, the light diffusion layer 13, the second substrate layer 14, and the hard coat layer 16 are sequentially laminated on the protective sheet 17. A protective sheet 18 may be laminated on the outer surface of the hard coat layer 16, if necessary.
[0171] 3. Substrate with elements The element-mounted substrate 2 is the same as that in the first embodiment.
[0172] 4. Light-emitting electronic components and manufacturing methods thereof The light-emitting electronic component 5a comprises an element-mounted substrate 2 having a plurality of light-emitting elements 21, 22, 23 arranged on a substrate 20, and an integrated sealing cured sheet 3a pressed against the surface of the element-mounted substrate 2 on which the plurality of light-emitting elements 21, 22, 23 are arranged.
[0173] The integrated encapsulating cured sheet 3a is formed by laminating, in this order from at least the side in contact with the element-mounted substrate 2, a black resin layer 30 capable of blocking light between the light emitting elements 21, 22, and 23, and a transparent resin layer 31 having higher light transmittance than the black resin layer 30. In this embodiment, a support 15a supporting the transparent resin layer 31 is laminated on the surface of the transparent resin layer 31 opposite to the surface in contact with the black resin layer 30. The black resin layer 30 and the transparent resin layer 31 are the same as those in the first embodiment, and therefore description thereof will be omitted.
[0174] In this embodiment, the integrated encapsulating cured sheet 3a is formed by laminating a black resin layer 30, a transparent resin layer 31, a substrate layer 12, a light diffusion layer 13, a second substrate layer 14, and a hard coat layer 16 in this order from the side contacting the element-mounted substrate 2.
[0175] The manufacturing method of the light-emitting electronic component 5a is the same as that of the first embodiment.
[0176] (Third embodiment) FIG. 6 shows a cross-sectional view, as seen in FIG. 1, of an integrated encapsulating sheet according to a third embodiment and a light-emitting electronic component in a state in which the release-treated support has been peeled off. The integrated encapsulating sheet 1b according to this embodiment includes a support 15b having at least one surface in its thickness direction that has been subjected to release treatment. The support 15b differs from the supports 15 and 15a in that the support 15b is release-treated and therefore can be peeled off after the black curable resin layer 10 and the transparent curable resin layer 11 are cured. In this embodiment, the support 15b is laminated on the surface of the transparent curable resin layer 11 opposite to the surface on which the black curable resin layer 10 is laminated. That is, the integrated encapsulating sheet 1b according to this embodiment is a laminate in which the black curable resin layer 10, the transparent curable resin layer 11, and the support 15b are laminated in this order.
[0177] A preferred embodiment of the support 15b is, for example, a sheet made of a thermoplastic resin such as polyester, e.g., polyethylene terephthalate or polyethylene naphthalate, polyimide, polyamideimide, polyethylene, polytetrafluoroethylene, polypropylene, or polystyrene, or surface-treated paper.
[0178] Among these, a polyester sheet can be preferably used from the viewpoints of heat resistance, mechanical strength, ease of handling, etc. The thickness of the support 15b is not particularly limited and is appropriately selected in the range of approximately 10 to 150 μm depending on the application.
[0179] As described above, the support 15b can be peeled from the cured transparent resin layer 31, but unlike the protective sheets 17 and 18, it is not excluded when measuring the value of Ttotal, which is the weight reduction rate in the present invention. That is, the value of Ttotal in the integrated encapsulating sheet 1b is the sum of the thicknesses of the black curable resin layer 10, the transparent curable resin layer 11, and the support 15b.
[0180] 2. Manufacturing method of integrated encapsulating sheet In the present embodiment, to obtain the integrated encapsulating sheet 1b, first, a sheet (hereinafter also referred to as a third transparent layer laminated sheet) is prepared by applying a coating liquid of a curable resin composition for the transparent curable resin layer 11 to one surface of the support 15b and drying the applied liquid. Further, a sheet (hereinafter also referred to as a black layer laminated sheet) is prepared by applying a coating liquid of a curable resin composition for the black curable resin layer 10 to a protective sheet 17 and drying the applied liquid.
[0181] Thereafter, the third transparent layer laminate sheet and the black layer laminate sheet are laminated together so that the transparent curable resin layer 11 and the black curable resin layer 10 are in contact with each other, thereby obtaining a laminate in which the black curable resin layer 10, the transparent curable resin layer 11, and the support 15b are laminated in this order on the protective sheet 17. Although not shown in the drawings, a protective sheet may be further laminated on the outer surface of the support 15b as necessary.
[0182] 3. Substrate with elements The element-mounted substrate 2 is the same as that in the first embodiment.
[0183] 4. Light-emitting electronic components and manufacturing methods thereof The light-emitting electronic component 5b comprises an element-mounted substrate 2 having a plurality of light-emitting elements 21, 22, 23 arranged on a substrate 20, and an integrated sealing cured sheet 3b pressed onto the surface of the element-mounted substrate 2 on which the plurality of light-emitting elements 21, 22, 23 are arranged.
[0184] The integrated encapsulating cured sheet 3b is formed by laminating, in this order from at least the side in contact with the element-mounted substrate 2, a black resin layer 30 capable of blocking light between the light emitting elements 21, 22, and 23, and a transparent resin layer 31 having higher light transmittance than the black resin layer 30. The black resin layer 30 and the transparent resin layer 31 are the same as those in the first embodiment, and therefore their explanation will be omitted. The support 15b supporting the transparent resin layer 31 may be peeled off after curing, or may be laminated directly on the transparent resin layer 31.
[0185] In this embodiment, integrated encapsulating cured sheet 3b has black resin layer 30 and transparent resin layer 31 laminated in this order from the side in contact with element-mounted substrate 2. In Fig. 6, support 15b is in a peeled state.
[0186] The method for manufacturing the light-emitting electronic component 5b is the same as that of the first embodiment, except that a step of peeling the support 15b from the transparent resin layer 31 may be further carried out after the curing step is completed. [Example]
[0187] The present invention will be specifically described below with reference to examples, although the present invention is not limited to these examples.
[0188] <Raw materials> Details of the raw materials used in each example and comparative example are as follows.
[0189] [Epoxy resin for curable resin layer] HP-7200H: DIC Corporation, cyclopentadiene novolac multifunctional epoxy resin (solid), softening point 82°C, epoxy equivalent 227g / eq. jER (registered trademark) YX7200B35: manufactured by Mitsubishi Chemical Corporation, phenoxy resin (MEK solution, solid content 35% by mass), glass transition temperature 150°C, epoxy equivalent 8781 g / eq., weight average molecular weight 30,000. jER(R) 1032H60: Mitsubishi Chemical Corporation, multifunctional epoxy resin (solid), softening point 62°C, epoxy equivalent 168g / eq.
[0190] [Elastomer] NX775: Zeon Corporation, carboxy-modified nitrile rubber, weight average molecular weight 208,000.
[0191] [Curing catalyst] 2PZ-CN: 1-cyanoethyl-2-phenylimidazole, manufactured by Shikoku Chemicals Co., Ltd.
[0192] [Carbon black] Special Black #4: Gas black, manufactured by ORION ENGINEERED CARBONS.
[0193] [solvent] MEK: Methyl ethyl ketone, manufactured by Junsei Chemical Co., Ltd.
[0194] [Resin for light diffusion layer] 8EC-001: Taisei Fine Chemical Co., Ltd., alicyclic epoxy resin, epoxy equivalent 414g / eq.
[0195] [Filler for light diffusion layers and transparent curable resin layers] KMP-706: Silicone resin powder manufactured by Shin-Etsu Chemical Co., Ltd., average particle size 2.0 μm.
[0196] [Silane coupling agents] KBE-9007N: Manufactured by Shin-Etsu Chemical Co., Ltd., contains an isocyanate group as an organic functional group. X-12-1308ES: Manufactured by Shin-Etsu Chemical Co., Ltd., contains an isocyanate group protected by a protecting group as an organic functional group. The protecting group is removed by heating to generate an isocyanate group.
[0197] [Photopolymerization initiator] WPI-170: Photocationic polymerization initiator manufactured by Fujifilm Wako Pure Chemical Industries, Ltd. Omnirad TPO H: Photo-radical polymerization initiator manufactured by IGM Resins BV.
[0198] [Sensitizer] Omnirad 127 D: Sensitizer manufactured by IGM Resins BV.
[0199] [PET film for support] Support film 1: PET film with hard coat layer, manufactured by Shin-Etsu Polymer Co., Ltd., thickness 80 μm (the formation of the hard coat layer will be described later). · Support film 2: Release PET film, Nippa 1-TRE, thickness 50 μm. Support film 3: PET film, manufactured by Shin-Etsu Polymer Co., Ltd., thickness 75 μm (no hard coat layer).
[0200] [Protection sheet] 1-TRE: Release film manufactured by Nippa, thickness 50μm.
[0201] [Resin and fine particles for hard coat layer] 8KX-078: Manufactured by Taisei Fine Chemical Co., Ltd., solids concentration 40% by mass, UV-curable acrylic polymer, weight-average molecular weight 40,000. Chemisnow (registered trademark) MX-500L: manufactured by Soken Chemical & Engineering Co., Ltd., cross-linked acrylic monodisperse particles, average particle diameter 5 μm.
[0202] [Preparation of coating liquid for curable resin layer] The coating liquids for the black curable resin layer and the transparent curable resin layer were prepared with the compositions shown below. Specifically, the compositions shown below were mixed with MEK solvent to prepare a coating liquid for the black curable resin layer with a solid content of 50% by mass and a coating liquid for the transparent curable resin layer with a solid content of 40% by mass. The compositions shown are in parts by mass of the solid content of each material.
[0203] [Coating liquid 1 for black curable resin layer] ·HP7200H (70 parts by mass) ·NX775 (30 parts by mass) ·2PZ-CN (1 part by mass) ·Special Black #4 (1 part by mass)
[0204] [Coating liquid 2 for black curable resin layer] ·HP7200H (70 parts by mass) ·NX775 (30 parts by mass) ·2PZ-CN (3 parts by mass) ·Special Black #4 (1 part by mass)
[0205] [Coating liquid 3 for black curable resin layer] ·HP7200H (70 parts by mass) ·NX775 (30 parts by mass) ·2PZ-CN (5 parts by mass) ·Special Black #4 (1 part by mass)
[0206] [Coating liquid for transparent curable resin layer] ·1032H60 (40 parts by mass) ·YX7200B35 (40 parts by mass) ·NX775 (20 parts by mass) ·2PZ-CN (1 part by mass) ·KMP-706 (15 parts by mass) ·X-12-1308ES (1.5 parts by mass)
[0207] [Preparation of coating liquid for light diffusion layer] A coating liquid for a light diffusion layer was prepared with the composition shown below. Specifically, the composition shown below was mixed with MEK solvent to prepare a coating liquid for a light diffusion layer with a solid content concentration of 60% by mass. The composition shown is in parts by mass of the solid content of each material. [Coating liquid for light diffusion layer] ·8EC-001 (100 parts by mass) ·WPI-170 (2 parts by mass) ·Omnirad 127 D (1 part by mass) ·KMP-706 (15 parts by mass) ·KBE-9007N (1.5 parts by mass)
[0208] [Preparation of Coating Agent for Hard Coat Layer] A coating agent for a hard coat layer was prepared according to the following composition: Specifically, the composition described below was mixed with an MEK solvent to prepare a coating agent for a hard coat layer with a solid content concentration of 30 mass %. [Coating agent for hard coat layer] ·8KX-078 (100 parts by mass) ·MX-500L (15 parts by mass) ·Omnirad TPO H (1 part by mass) ·Omnirad 127 D (1 part by mass)
[0209] [Preparation of Support Film 1] One side of a 75 μm thick PET film was subjected to corona treatment, and a coating agent for a hard coat layer was applied using a bar coater so that the dry film thickness was 5 μm. After drying at 100° C. for 5 minutes, ultraviolet rays with a wavelength of 365 nm were applied at 400 mJ / cm. 2 The coating agent was cured by irradiation to form a hard coat layer, thereby obtaining a film 1 for support (a laminate of a second base material layer and a hard coat layer) having a thickness of 80 μm.
[0210] Example 1 [Preparation of Transparent Curable Resin Layer] The coating liquid for the transparent curable resin layer was applied to the support film 1 using a film applicator with a film thickness adjustment function (All Good Co., Ltd.) so that the dry film thickness would be 50 μm. After the coating liquid was applied, the support film 1 was transported to a drying oven at a line speed of 1 m / min and passed through the oven. Drying was carried out in two stages using two continuous drying ovens. The length of both ovens used was 2 m. The drying conditions were as follows: the set temperature of the first drying oven was 80°C, and the set temperature of the subsequent second drying oven was 105°C (hereinafter, the line speed and drying conditions are collectively referred to as coating condition 1). In this way, a transparent layer laminated sheet was obtained in which a hard coat layer, a substrate layer, and a transparent curable resin layer were laminated in this order.
[0211] [Preparation of black curable resin layer] Coating liquid 1 for the black curable resin layer was applied to the release surface of release PET 1-TRE (Nippa Corporation, 50 μm) using a film applicator with film thickness adjustment function (Allgood Co., Ltd.) so that the dry film thickness would be 50 μm. The release PET after coating with the coating liquid was coated and dried at a line speed of 0.5 m / min under the same coating conditions as coating condition 1 (hereinafter referred to as coating condition 2). In this way, a black layer laminate sheet in which the black curable resin layer was supported by the release PET was obtained.
[0212] [Production of integrated encapsulating sheet] The obtained transparent layer laminated sheet and the black layer laminated sheet were stacked so that the transparent curable resin layer and the black curable resin layer were in contact with each other, and laminated with a roll laminator at 60°C to obtain an integrated encapsulating sheet of Example 1 (referred to as integrated encapsulating sheet configuration 1 in Tables 2 and 4). The obtained integrated encapsulating sheet was subjected to measurement of the weight loss rate.
[0213] [Substrate with evaluation element] A substrate with LED light emitting elements for evaluation was prepared by arranging a plurality of LED light emitting elements, each 0.1×0.2 mm in size and 65 μm in height, on an epoxy glass substrate.
[0214] [Manufacturing of light-emitting electronic components] The release PET from each integrated encapsulating sheet was peeled off, and the black curable resin layer was placed in contact with the LED light-emitting element of the evaluation element-mounted substrate. The black curable resin layer and the transparent curable resin layer were then filled between the light-emitting elements in a vacuum press under conditions of 100 hPa, 100°C, 0.36 MPa, and 3 minutes. After filling, the black curable resin layer and the transparent curable resin layer were thermally cured under one of the following curing conditions to obtain a light-emitting electronic component. The light-emitting electronic component was then subjected to the bubble evaluation described below. Curing condition 1: Place in an oven set at 150°C for 1 hour to thermally cure. Curing condition 2: Place in an oven set at 100°C for 1 hour, then place in an oven set at 150°C for 45 minutes for thermal curing.
[0215] <Example 2> The same procedures as in Example 1 were carried out except that the coating conditions for the black curable resin layer coating liquid 1 were changed to coating conditions 1.
[0216] Example 3 The coating conditions for the black curable resin layer coating liquid 1 were the same as those in Example 1, except that the line speed was changed to 0.3 m / min and the drying conditions were the same as those in Coating Condition 1 (hereinafter referred to as Coating Condition 3).
[0217] Example 4 The coating conditions for the coating liquid for the transparent curable resin layer were the same as in Example 1, except that the line speed was the same as in Coating Condition 1, and the drying conditions were changed to a coating condition in which the set temperature of the first drying oven was 80°C and the set temperature of the subsequent second drying oven was 115°C (hereinafter referred to as Coating Condition 4).
[0218] <Example 5> The coating conditions for the black curable resin layer coating liquid 1 were changed to coating conditions 4, and the coating conditions for the transparent curable resin layer coating liquid were changed to coating conditions (hereinafter referred to as coating conditions 5) in which the line speed was the same as in coating conditions 3 and the drying conditions were the same as in coating conditions 4, as in Example 1.
[0219] Example 6 The same procedures as in Example 1 were carried out except that the coating conditions for the black curable resin layer coating liquid 1 were changed to coating conditions 5 and the coating conditions for the transparent curable resin layer coating liquid were changed to coating conditions 3.
[0220] Example 7 The same procedure as in Example 1 was carried out except that the support film coated with the coating liquid for the transparent curable resin layer was changed to support film 2 (referred to as integrated encapsulating sheet configuration 2 in Tables 2 and 4).
[0221] Example 8 The same procedures as in Example 7 were carried out except that the coating conditions for the black curable resin layer coating liquid 1 were changed to coating conditions 3.
[0222] Example 9 In this example, the configuration of the integrated encapsulating sheet was changed to a laminate in which a hard coat layer, a second substrate layer, a light diffusion layer, a substrate layer, a transparent curable resin layer, and a black curable resin layer were laminated in this order. Specifically, the following procedure was performed.
[0223] [Preparation of support] The coating liquid for the light diffusion layer was applied to the support film 1 using a film applicator with a film thickness adjustment function (All Good Co., Ltd.) so that the dry film thickness would be 50 μm. After application, the coating liquid for the light diffusion layer 1 was dried at 100°C for 4 minutes. Thereafter, the support film 3 was laminated at 100°C and 2 m / min using a roll laminator MAII-550 manufactured by Taisei Laminator Co., Ltd., on the surface of the coating liquid for the light diffusion layer opposite to the surface in contact with the support film 1. Ultraviolet light with a wavelength of 365 nm was applied at 300 mJ / cm. 2 The coating liquid for the light diffusion layer was cured by irradiation, and a support having a hard coat layer, a second substrate layer, a light diffusion layer, and a substrate layer laminated in this order was obtained. The support was used to prepare an integrated encapsulating sheet, which will be described later.
[0224] [Preparation of Transparent Curable Resin Layer] On the surface of the support on the substrate layer side, a coating liquid for a transparent curable resin layer was applied and dried under coating condition 1 using a film applicator with a film thickness adjustment function (ALL GOOD Co., Ltd.) so that the dry film thickness would be 50 μm. In this way, a second transparent layer laminated sheet was obtained in which the hard coat layer, second substrate layer, light diffusion layer, substrate layer, and transparent curable resin layer were laminated in this order.
[0225] [Preparation of black curable resin layer] Onto the release surface of release PET 1-TRE (Nippa Corporation, 50 μm), black curable resin layer coating liquid 1 was applied using a film applicator with film thickness adjustment function (Allgood Corporation) under coating condition 2 so that the dry film thickness would be 50 μm, followed by drying. In this way, a black layer laminate sheet in which the black curable resin layer was supported by the release PET was obtained.
[0226] [Production of integrated encapsulating sheet] The obtained second transparent layer laminated sheet and the black layer laminated sheet were stacked so that the transparent curable resin layer and the black curable resin layer were in contact with each other, and laminated with a roll laminator at 60°C to obtain an integrated encapsulating sheet of Example 9 (referred to as integrated encapsulating sheet configuration 3 in Tables 2 and 4). The subsequent steps were the same as those of Example 1.
[0227] Example 10 The same procedures as in Example 9 were carried out except that the coating conditions for the black curable resin layer coating liquid 1 were changed to coating conditions 3.
[0228] Example 11 The same procedure as in Example 1 was carried out except that the coating liquid 1 for black curable resin layer was changed to the coating liquid 2 for black curable resin layer (referred to as integrated encapsulating sheet configuration 4 in Tables 2 and 4).
[0229] Example 12 The same procedure as in Example 1 was carried out except that the coating liquid 1 for black curable resin layer was changed to the coating liquid 3 for black curable resin layer (described as integrated encapsulating sheet configuration 5 in Tables 2 and 4).
[0230] <Comparative Example 1> The same procedures as in Example 1 were carried out except that the coating conditions for both the black curable resin layer coating liquid 1 and the transparent curable resin layer coating liquid were changed to coating conditions 5.
[0231] <Comparative Example 2> The coating conditions for the black curable resin layer coating liquid 1 and the transparent curable resin layer coating liquid were the same as those in Example 1, except that the line speed was the same as in Coating Condition 1, and the drying conditions were changed to a coating condition in which the set temperature of the first drying oven was 70°C and the set temperature of the subsequent second drying oven was 90°C (hereinafter referred to as Coating Condition 6).
[0232] Table 1 shows the composition of each coating liquid for the black curable resin layer, Table 2 shows the configuration of each integrated encapsulating sheet, and Table 3 shows the details of each coating condition.
[0233] [Table 1]
[0234] [Table 2]
[0235] [Table 3]
[0236] <Evaluation method> [Weight loss rate measurement] The integrated encapsulating sheets according to each of the Examples and Comparative Examples prepared as described above were subjected to measurement of the weight loss rate as follows. Each of the prepared integrated encapsulating sheets was left to stand for 3 hours in a constant temperature and humidity chamber at 23±2°C and 50±10 RH%. Each of the left-standing integrated encapsulating sheets was cut into a 100 mm square as a measurement sample. The protective sheet provided on the black curable resin layer side of the cut-out measurement sample was peeled off, and the weight was measured using a precision balance. This weight was designated as the weight before drying (W1). The measurement sample was placed in an oven set to 120°C and heated for 30 minutes. After heating, the measurement sample was removed from the oven, and its weight was similarly measured using a precision balance. The measured weight was designated as the weight after drying (W2). Each measured value was substituted into the following mathematical formula 1 to calculate the weight loss rate. This was performed three times, and the average value was calculated. The results are shown in Table 4 below.
[0237]
number
[0238] [Air bubble evaluation] For the light-emitting electronic components according to each Example and Comparative Example, the surface of the integrated encapsulating cured sheet press-bonded to the substrate was observed at 20x magnification using a microscope (product name: VHX-8000, manufactured by Keyence Corporation) from the side opposite the side press-bonded to the substrate to check for the presence or absence of air bubbles. The observation results were evaluated as follows. The evaluation results are shown in Table 4 below. A: No bubbles were observed. B: Bubbles were observed.
[0239] Furthermore, an overall evaluation was made based on the results of each bubble evaluation for each of the above-mentioned curing conditions 1 and 2, with A and B being considered pass and C being considered fail. The evaluation results are shown in Table 4 below. A: The air bubbles were evaluated as A under both curing condition 1 and curing condition 2. B: The bubble evaluation for either curing condition 1 or curing condition 2 was A. C: The air bubbles were evaluated as B under both curing condition 1 and curing condition 2.
[0240] [Table 4]
[0241] <Evaluation results> The integrated encapsulating sheets according to the examples were less likely to generate bubbles than the sheets according to the comparative examples. This suggests that by maintaining the weight loss rate within a certain numerical range, the amount of solvent volatilized from the curable resin layer can be kept within an appropriate range, thereby suppressing the generation of bubbles. Therefore, it can be said that the integrated encapsulating sheet according to the present invention is a sheet that suppresses the generation of bubbles more than conventional products. [Industrial Applicability]
[0242] The integrated encapsulating sheet according to the present invention can be used, for example, as a sheet for sealing a substrate on which a plurality of light-emitting elements are arranged. [Explanation of symbols]
[0243] DESCRIPTION OF SYMBOLS 1, 1a, 1b... Integrated encapsulating sheet, 2... Substrate with element, 3... Integrated encapsulating cured sheet, 5... Light-emitting electronic component, 10... Black curable resin layer, 11... Transparent curable resin layer, 12... Base material layer, 13... Light-diffusing layer, 14... Second base material layer, 15, 15a, 15b... Support, 16... Hard coat layer, 17, 18... Protective sheet, 20... Substrate, 21, 22, 23... Light-emitting element, 30... Black resin layer, 31... Transparent resin layer
Claims
1. An integrated encapsulating sheet to be pressure-bonded to a surface of an element-mounted substrate on which a plurality of light-emitting elements are arranged, the surface comprising: a black cured resin layer that shields light between the plurality of light-emitting elements, a transparent cured resin layer that has higher light transmittance than the black cured resin layer, and a support that supports the transparent cured resin layer, stacked in this order; a total thickness of the black cured resin layer and the transparent cured resin layer is greater than a height of the plurality of light-emitting elements; and a total weight loss rate due to curing of the black curable resin layer and the transparent curable resin layer is 0.3 to 10%.
2. The integrated encapsulating sheet according to claim 1 , wherein the black curable resin layer and the transparent curable resin layer contain at least an epoxy resin.
3. the black curable resin layer contains a curing catalyst, The integrated sealing sheet according to claim 1, wherein the content of the curing catalyst is 0.3 to 4 parts by mass with respect to 100 parts by mass of the total resin solid content of the black curable resin layer.
4. The integrated encapsulating sheet according to claim 1 , wherein the support includes a light diffusion layer for diffusing incident light from the light emitting element.
5. The integrated encapsulating sheet according to claim 1, wherein the support has at least one surface in the thickness direction thereof subjected to a release treatment.
6. an element-mounted substrate having a plurality of light-emitting elements arranged on the substrate; an integrated encapsulating cured sheet that is pressure-bonded to a surface of the element-mounted substrate on which the plurality of light-emitting elements are arranged, the integrated encapsulating cured sheet includes, from the side in contact with the element-mounted substrate, at least a black resin layer that shields light between the plurality of light-emitting elements and a transparent resin layer that has higher light transmittance than the black resin layer, laminated in this order; a total thickness of the black cured resin layer, which is an uncured state of the black resin layer, and the transparent cured resin layer, which is an uncured state of the transparent resin layer, is greater than a height of the plurality of light-emitting elements; and a total weight loss rate due to curing of the black curable resin layer and the transparent curable resin layer is 0.3 to 10%.
7. 7. The light-emitting electronic component according to claim 6, wherein the thickness of the black resin layer is 0.1 to 0.9 times the height of the plurality of light-emitting elements.
8. 7. The light-emitting electronic component according to claim 6, wherein the thickness of the transparent resin layer is 0.1 to 5.0 times the height of the plurality of light-emitting elements.
9. A step of placing the black curable resin layer of the integrated encapsulating sheet according to any one of claims 1 to 5 in contact with a surface of an element-mounted substrate on which a plurality of light-emitting elements are arranged, the surface having the plurality of light-emitting elements arranged on the substrate; Filling the integrated encapsulating sheet from the plurality of light-emitting elements toward the substrate; and curing the black curable resin layer and the transparent curable resin layer.
Citation Information
Patent Citations
Curable resin composition, dry film, cured product, and electronic component
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Dry film, light-emitting electronic component, and method for manufacturing light-emitting electronic component
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