Optical member resin sheet, optical member including optical member resin sheet, layered body, or light emitting device, and method for manufacturing optical member resin sheet

Abstract

Provided are: a resin sheet having excellent characteristics as an optical member and exhibiting excellent performance even for a light-emitting device or the like; and a method for producing the resin sheet. Provided is an optical member resin sheet characterized in that: in a width direction of the sheet, a difference between a thickness of an end portion of the sheet and a thickness of a center portion of the sheet is within 5.0% of a total film thickness of the sheet; the thickness of the center portion of the sheet is 10-1000 μm; an area of the sheet is 225 mm 2 or more; and contains at least one phosphor or a reflective material.

Description

Technical Field

[0001] This invention relates to resin sheets for optical components, optical components, layers, or light-emitting devices equipped thereon, and methods for producing resin sheets for optical components. Specifically, this invention relates to resin sheets for optical components exhibiting excellent flatness, which can be used in lighting, display devices, etc., optical components, layers, or light-emitting devices equipped thereon, and methods for producing resin sheets for optical components. Background Technology

[0002] Resin sheets for optical components, exhibiting excellent efficiency, physical properties, and durability, are used in light-emitting devices, including LEDs. Since these resin sheets are used after lamination onto, for example, LED chips, they require excellent flatness. Conventionally, continuous processes such as roll-to-roll processes have been used to manufacture these resin sheets; however, while continuous processes are suitable for high-volume production of sheets with large surface areas, they are not suitable for manufacturing a wide variety of products, such as LEDs, in small batches.

[0003] Patent document 1 discloses a sheet coating machine for use in an inspection system. However, the substrate used in the sheet coating machine described in Patent document 1 is made of glass, and the document does not provide any disclosure regarding coating of flexible substrates such as polymer films. Furthermore, Patent document 2 discloses a method in which a film is formed after adjusting the conditions of a processing liquid when producing a processing liquid film. However, Patent document 2 also does not provide any disclosure regarding substrates corresponding to flexible substrates such as polymer films.

[0004] While patent document 3 discloses a basic sheet coating machine, it does not provide any disclosure regarding how to control product quality or whether sheets exhibiting excellent flatness can be obtained. Although patent documents 4 and 5 also disclose sheet coating machines, in both cases they are used for continuous processes, and the documents do not disclose their use in the production of resin sheets for optical components.

[0005] Existing technical documents

[0006] Patent documents

[0007] Patent Document 1: US Patent No. 2010 / 0189880 - Specification

[0008] Patent document 2: Japanese Unexamined Patent Publication No. 10-76205

[0009] Patent document 3: US Patent No. 4938994

[0010] Patent document 4: International Patent Publication No. 97 / 26999

[0011] Patent document 5: Japanese translation of PCT international application publication number 2016-500382 Summary of the Invention

[0012] The problem this invention seeks to solve

[0013] Therefore, there is a need for resin sheets exhibiting excellent flatness as optical components used in optical devices such as LEDs, and methods for producing them. Specifically, optical component resin sheets and methods for producing them are conventionally unknown, and the optical component resin sheets exhibit a flatness level suitable for products produced by batch processes suitable for small-batch production.

[0014] In addition, there is a need for resin sheets and light-emitting devices including the resin sheets, which, when used in optical components including optical components, provide good efficiency in light-emitting devices such as LEDs and also have excellent durability.

[0015] The present invention was developed to address the aforementioned problems found in the prior art and seeks to provide a resin sheet and a method for producing the resin sheet, which exhibits excellent properties as an optical component and also shows excellent performance when used in light-emitting devices, etc.

[0016] Problem-solving methods

[0017] After conducting in-depth research on the aforementioned problems, the inventors of this invention arrived at the present invention. That is, the object of this invention is achieved through an optical component resin sheet, wherein, with respect to the sheet width direction, the difference between the sheet edge thickness and the sheet center thickness is no more than 5.0% relative to the total sheet thickness, the thickness at the sheet center ranges from 10 to 1,000 μm, and the sheet area is at least 225 mm². 2 It is characterized by containing at least one type of fluorescent or reflective material.

[0018] The width and length of the sheet are preferably 15 mm or greater, and the sheet area is preferably 400 mm². 2 Or larger.

[0019] The center thickness of the aforementioned sheet is preferably in the range of 30 to 900 μm, and the difference between the edge thickness and the center thickness of the sheet is preferably no more than 2.5% relative to the total sheet thickness in the width direction.

[0020] The fluorescent or reflective material is preferably included in an amount ranging from 10% to 90% by mass relative to the total weight of the sheet.

[0021] Fluorescent or reflective materials preferably have a structure in which they are dispersed in an adhesive resin containing at least silicone resin.

[0022] The resin sheet of the optical component made by the present invention is preferably heat-fusible.

[0023] The optical component resin sheet constructed according to the present invention preferably comprises: (A) One or more fluorescent substances selected from oxide phosphors, oxynitride phosphors, nitride phosphors, sulfide phosphors, fluoride phosphors, and oxysulfide phosphors, and (B) Organopolysiloxanes, which have the following molecular structure within their molecular structure: R A SiO 3 / 2 (where R) A It is an arylsiloxane unit represented by an aryl group having 6 to 14 carbon atoms and a arylsiloxane unit represented by the formula (R2SiO2). 2 / 2 ) n The polydiorganosiloxane structure represented by (where R is an aryl group having 6 to 14 carbon atoms or an alkyl group having 1 to 20 carbon atoms, which may be halogenated, and n is a number ranging from 3 to 1,000).

[0024] Component (A) is preferably included in an amount ranging from 10% to 90% by mass relative to the total weight of the sheet.

[0025] Component (B) is preferably an adhesive resin comprising at least a solid particulate component of component (A), and further comprises the formula {(R2SiO2)}. 2 / 2 )} a {R A SiO 3 / 2} 1-a (where R and R) A It is an organopolysiloxane represented by the same group as described above, and a is a number ranging from 0.8 to 0.2.

[0026] At least a portion of the aforementioned fluorescent or reflective material is preferably surface-treated with an organosilicon compound.

[0027] The reflective material is preferably selected from one or more of titanium oxide, barium oxide, chromium oxide, iron oxide, boron nitride, and titanium nitride.

[0028] The optical component resin sheet made according to the present invention may further include (C) silica particles.

[0029] The present invention also relates to an optical component equipped with an optical component resin sheet constituted by the present invention.

[0030] In addition, the present invention also relates to a layered body equipped with an optical component resin sheet constituted by the present invention.

[0031] The layered body constructed by the present invention may further be equipped with a peeling layer.

[0032] Furthermore, the present invention also relates to a light-emitting device having a structure sealed with a resin sheet of an optical component constituted by the present invention.

[0033] In addition, the present invention relates to a method for producing an optical component resin sheet made of the present invention, characterized in that the starting material of the optical component resin sheet is applied to a substrate at a viscosity of 10 to 10,000 mPa·s at 25°C and a wet film thickness of 10 to 1,000 μm using a sheet coating machine.

[0034] In the production method constituted by the present invention, a slot coater is used as a sheet coater, and production is preferably carried out with the hydraulic build-up time set to 1.0 / w seconds or less and the coating speed being w (cm / second).

[0035] Invention Effects

[0036] This invention produces resin sheet flatness that is advantageous when used as an optical component. Specifically, when used as a component for light-emitting devices such as LEDs, it provides a component exhibiting excellent wavelength conversion characteristics, light extraction efficiency, and sealing performance.

[0037] Furthermore, the method for producing the optical component resin sheet constituted by the present invention can be carried out using a batch process and is suitable for producing various different products in small batches. In addition, since optical component resin sheets exhibiting excellent flatness can be produced, resin sheets ideally suited for use as components of light-emitting devices can be manufactured. Attached Figure Description

[0038] [ Figure 1 This figure shows a schematic diagram of the coating head of a sheet coating machine according to an embodiment of the present invention.

[0039] [ Figure 2 This figure shows a schematic diagram of a sheet coating machine according to an embodiment of the present invention. Detailed Implementation

[0040] The following describes in detail the resin sheet for optical components made according to the present invention.

[0041] The optical component resin sheet constructed according to the present invention is characterized in that, with respect to the sheet width direction, the difference between the sheet edge thickness and the sheet center thickness is no more than 5.0% relative to the total sheet thickness, and the sheet center thickness ranges from 10 to 1,000 μm. The sheet width direction corresponds to a direction perpendicular to the sheet length direction, and generally refers to a direction on the surface perpendicular to the direction in which the starting material composition is coated or simply film-formed on the substrate. Note that when the sheet is wound, the winding direction corresponds to the length direction, while the sheet width direction corresponds to a direction perpendicular to the length direction. For quadrilateral or approximately quadrilateral films, the film width direction is perpendicular to the length direction, and for square or approximately square films, any direction parallel to or perpendicular to each edge of the square or approximately square film can be considered the width direction.

[0042] The optical component resin sheet constructed according to the present invention is characterized in that, with respect to the width direction of the sheet, the absolute value of the difference between the sheet edge thickness (μm) and the sheet center thickness (μm) is no greater than 5.0% relative to the total sheet thickness, wherein preferably the difference between the sheet edge thickness and the sheet center thickness is no greater than 4.0% relative to the total sheet thickness, and particularly preferably no greater than 2.5%. Note that the sheet preferably has a flat and uniform structure, the structure being substantially free of irregularities on the surface, including protrusions at both ends, and the maximum displacement (difference) of the sheet thickness in the width direction preferably does not exceed 5.0%. Furthermore, it is particularly preferred that the sheet is a flat sheet having a maximum thickness displacement (difference) of 5.0% or less over the entire sheet and without significant non-uniformity.

[0043] The optical component resin sheet constructed according to the present invention is characterized by being a sheet material with a certain thickness, such that the thickness at the center of the sheet exceeds 10 μm, and having a substantially flat structure, wherein the thickness within the sheet is almost uniform. Specifically, the thickness at the center of the sheet in the width direction ranges from 10 to 1,000 μm, preferably from 20 to 950 μm, and particularly preferably from 30 to 900 μm. When the thickness at the center of the sheet is below the aforementioned lower limit, the film thickness is too thin, thus potentially limiting its application as an optical component resin sheet. Furthermore, if the thickness exceeds the aforementioned upper limit, the film thickness is too high when treated as a single layer, thus potentially unsuitable for applications requiring lower thickness, such as light-emitting devices.

[0044] Note that since the optical component resin sheet constructed by this invention is a flat resin sheet without significant non-uniformity, it offers the advantage of being less prone to bubble entrapment, deformation, and defects caused by non-uniformity between resin sheets when forming a resin sheet layer of uniform thickness by overlapping multiple resin sheets, and when using a single layer. That is, although the optical component resin sheet constructed by this invention has a thickness of 10 to 1000 μm, it can also be used to form resin sheet layers exceeding 1000 μm by overlapping multiple film layers to form optical components for various optical devices.

[0045] The optical component resin sheet constructed according to the present invention is characterized by having a certain size (area), and the sheet area is 225 mm². 2 Or larger. The resin sheets of the optical components constructed according to the present invention preferably have a sheet width and length of at least 15 mm, particularly preferably at least 30 mm. Furthermore, the sheet area is preferably 400 mm². 2 Or larger, with 900 mm being particularly preferred. 2 Or larger. The optical component resin sheet constituted by the present invention is a flat film without exhibiting significant non-uniformity, and can have a structure in which the curable component used as a starting material is uniformly applied and cured, potentially on top of the release layer, so any length that allows it to be wound onto a roller in the longitudinal direction can be used without particular limitation. Furthermore, the optical component resin sheet can be cut to the desired size or shape before use.

[0046] The optical component resin sheet made according to the present invention is characterized in that it contains at least one type of fluorescent material or reflective material.

[0047] There are no particular limitations on the fluorescent material contained in the resin sheet of the optical component constituted by the present invention, as long as it can be used as a wavelength conversion material. Examples include yellow, red, green, and blue fluorescent materials made of oxide phosphors, oxynitride phosphors, nitride phosphors, sulfide phosphors, fluoride phosphors, oxysulfide phosphors, etc., which are widely used in light-emitting diodes (LEDs) and organic light-emitting devices (OLEDs). Examples of oxide phosphors include YAG green to yellow luminescent phosphors based on yttrium, aluminum, and garnet containing cerium ions; TAG yellow luminescent phosphors based on terbium, aluminum, and garnet containing cerium ions; and silicate-based green to yellow luminescent phosphors containing cerium and europium ions. Additionally, examples of oxynitride phosphors include silane red to green luminescent phosphors based on silicon, aluminum, oxygen, and nitrogen containing europium ions. Examples of nitride-based phosphors include CASN red luminescent phosphors based on calcium, strontium, aluminum, silicon, and nitrogen containing europium ions. Examples of sulfide-based phosphors include ZnS-based green-colored phosphors containing copper and aluminum ions. Examples of fluoride-based phosphors include KSF phosphors (K2SiF6:Mn). 4+ Examples of oxysulfide phosphors include red luminescent phosphors based on Y₂O₂S containing europium ions. A single fluorescent substance can be used, or two or more fluorescent substances can be used in combination.

[0048] While there are no particular limitations on the reflective material contained in the resin sheet of the optical component constituted by the present invention, it may correspond to one or more variants selected from titanium oxide, barium oxide, chromium oxide, iron oxide, boron nitride, and titanium nitride. Specifically, titanium oxide is preferred.

[0049] The fluorescent or reflective material contained in the resin sheet of the optical component constructed according to the present invention preferably has a structure in which it is dispersed in an adhesive resin containing at least silicone resin. Furthermore, to improve the dispersibility in the silicone resin, at least a portion of the fluorescent or reflective material can be surface-treated with an organosilicon compound. Specifically, at least a portion of the fluorescent or reflective material can be surface-treated with alkoxysilanes, organohalosilanes, organozanes, siloxane oligomers, etc.

[0050] The fluorescent or reflective material contained in the resin sheet of the optical component made of the present invention is preferably contained in an amount ranging from 10% to 90% by mass relative to the total weight of the sheet, and particularly preferably in an amount ranging from 15% to 85% by mass.

[0051] The optical component resin sheet constructed according to the present invention preferably comprises: (A) One or more fluorescent substances selected from the group consisting of: oxide phosphors, oxynitride phosphors, nitride phosphors, sulfide phosphors, fluoride phosphors, and oxysulfide phosphors, and (B) Organopolysiloxanes, which have the following molecular structure within their molecular structure: R A SiO 3 / 2 (where R) A Arylsiloxane units represented by aryl groups having 6 to 14 carbon atoms, and those derived from the formula (R₂SiO₃) 2 / 2 ) n The polydiorganosiloxane structure represented by (where R is an aryl group having 6 to 14 carbon atoms or an alkyl group having 1 to 20 carbon atoms, which may be halogenated, and n is a number ranging from 3 to 1,000).

[0052] Component (A) is preferably included in an amount corresponding to 10% to 90% by mass relative to the total weight of the sheet, and particularly preferably in an amount corresponding to 15% to 85% by mass.

[0053] Component (B) is a solid particulate component adhesive resin containing at least component (A), and corresponds to a linear polymer type organopolysiloxane containing T units with aryl groups. Because component (B) exhibits high refractive index and thermal fusibility, it can easily form a uniform thin film-like solid layer.

[0054] The component (B) corresponds to an organopolysiloxane, which has a molecular structure containing the formula R. A SiO 3 / 2 (where R) A Arylsiloxane units represented by aryl groups having 6 to 14 carbon atoms, and those derived from the formula (R₂SiO₃) 2 / 2 ) n The polydiorganosiloxane structure represented by (where R is an aryl group having 6 to 14 carbon atoms or an alkyl group having 1 to 20 carbon atoms, which may be halogenated, and n is a number ranging from 3 to 1,000).

[0055] Here, the aryl group having 6 to 14 carbon atoms is phenyl, tolyl, xylyl, naphthyl, or anthracene, and from an industrial production perspective, phenyl is preferred. Furthermore, R is an alkyl group, such as methyl, ethyl, propyl, butyl, pentyl, hexyl, heptyl, octyl, nonyl, decyl, undecyl, or dodecyl; an aryl group, such as phenyl, tolyl, xylyl, naphthyl, or anthracene; or a group in which some or all of the hydrogen atoms bonded to the above groups are replaced by halogen atoms such as fluorine, chlorine, or bromine atoms, and from a production perspective, methyl or phenyl is preferred.

[0056] More specifically, component (B) has a structure in which the resin structural block containing a siloxane unit is represented as a T unit: R 1 SiO 3 / 2 (where R) 1 It is a monovalent organic group, hydroxyl or alkoxy group having 1 to 6 carbon atoms, and R in each molecule 1 At least one instance is an aryl group having 6 to 14 carbon atoms or an optional Q unit: SiO 4 / 2 And represented as (R2SiO) 2 / 2 ) n The linear structural blocks (where n is a number as defined above, and R is a functional group as defined above) are connected by silane-alkyl groups or Si-O-Si groups, and are further characterized by R A SiO 3 / 2 The unit is a linear organopolysiloxane block copolymer of resin; and in the silane-alkylene bonds or Si-O-Si bonds connecting the resin structural blocks and the linear structural blocks in the polymer, the Si atoms bonded to the resin structure preferably constitute R 1 SiO 3 / 2 unit.

[0057] The resin structural blocks in component (B) are the partial structures that impart overall thermofusibility to component (B) and exhibit a resin-like organopolysiloxane structure. This structure forms a partial structure composed of resin-organopolysiloxane, incorporating a large number of T or Q units, and requires R... A SiO 3 / 2 The term represents an arylsiloxane unit. Specifically, when the molecular structure contains a large number of aryl groups, such as phenyl groups, the refractive index of component (B) can be increased. Preferably, component (B) contains R... A SiO 3 / 2 (where R) A It is an organopolysiloxane containing arylsiloxane units (represented by the functional groups described above), in an amount equal to 20% to 80% by mass of the total organopolysiloxane, and from the perspective of the hot melt properties and refractive index described above, the resin structure is particularly preferably substantially entirely composed of arylsiloxane units through R A SiO 3 / 2 The arylsiloxane unit is formed.

[0058] The linear structure is composed of (R2SiO) 2 / 2 ) n The non-reactive block is represented and is composed of R2SiO 2 / 2The represented diorganosiloxy unit is a structure in which at least three, but preferably at least five, units are linked together in a chain. The linear block is a partial structure that imparts a moderate level of flexibility to the solid layer formed by the copolymer. In the above formula, n is the degree of polymerization of the diorganosiloxy unit constituting the partial structure, and should preferably range from 3 to 250, more preferably from 5 to 250, 50 to 250, and 100 to 250. When n of the partial structure exceeds the above upper limit, the linear molecular properties derived from the linear structure are strongly expressed, and the film formability may be insufficient. On the other hand, if n is less than the above lower limit, the linear molecular properties may be insufficient, and the characteristic physical properties of component (B) may not be realized; therefore, especially when the film is made thin, shrinks, etc., it is easy for it to not be applied uniformly.

[0059] The functional group R contained in the diorganosiloxy unit constituting the linear structure is alkyl or aryl. These groups are non-reactive to the resin structure and its functional groups within the same molecule, and it is necessary to maintain the linear structure without inducing intramolecular polymerization reactions, such as condensation reactions. The alkyl and aryl groups correspond to the groups described above, and from an industrial production perspective, methyl or phenyl groups are preferred.

[0060] The resin structure and linear structure blocks contained in component (B) are preferably linked by silaneyl bonds arising from the hydrosilylation reaction between hydrogen atoms bonded to alkenyl groups and silicon atoms, or by Si-O-Si bonds arising from condensable reactive groups at the ends of the resin structure or linear structure. Specifically, in the context of this invention, the Si atoms bonded to the resin structure preferably constitute R 1 SiO 3 / 2 Units, and particularly preferably they have the following partial structure (T-Dn). From an industrial production perspective, R 1 Preferably, it is phenyl, and R is preferably methyl or phenyl.

[0061] [Chemical Formula 1] (T-Dn) Preferably, in the aforementioned partial structure, the end of the Si-O- bond on the left side of each T unit is bonded to a hydrogen atom or another siloxane unit constituting the resin structure, preferably another T unit. On the other hand, the end of the Si-O- bond on the right side is bonded to another siloxane unit, a triorganosiloxy unit (M unit), or a hydrogen atom forming a linear structure or resin structure. Note that when a hydrogen atom is bonded to the end of the Si-O- bond, a silanol group (Si-OH) is formed.

[0062] From the perspectives of the thermal fusibility of component (B), the refractive index required to improve light extraction efficiency, and the uniformity of coating, especially when the film is made thin, component (B) is preferably a non-reactive organopolysiloxane containing only R. A SiO 3 / 2 arylsiloxane units and represented as R2SiO 2 / 2 The two organosiloxane units. More specifically, component (B) is preferably an organopolysiloxane represented by the following formula: {(R2SiO2)} 2 / 2 )} a {R A SiO 3 / 2} 1-a

[0063] Among them, R and R A Corresponding to the aforementioned functional group, and a preferably corresponds to a number in the range of 0.8 to 0.2, more preferably in the range of 0.8 to 0.4.

[0064] Component (B) preferably exhibits hot melt properties; specifically, it is preferably non-flowable at 25°C and displays a melt viscosity of 200,000 Pa·s or less at 100°C. Here, non-flowable means that the material does not flow in the unloaded state, for example, below the softening point of a hot melt adhesive as specified by the ring and ball method in JIS K 6863-1994 "Method for testing the softening point of hot melt adhesives". That is, in order for the material to be non-flowable at 25°C, the softening point must be higher than 25°C. Preferably, component (B) exhibits a melt viscosity of 200,000 Pa·s or less, 100,000 Pa·s or less, 50,000 Pa·s or less, 20,000 Pa·s or less, or in the range of 10 to 20,000 Pa·s at 100°C. When the melt viscosity at 100°C falls within the above-mentioned range, the adhesion of the film formed after the hot melt process and cooling to 25°C is advantageous. In addition, using component (B) with a melt viscosity range of 100 to 15,000 Pa·s can effectively suppress deformation or peeling of the film formed after molding in some cases.

[0065] Component (B) is preferably included in an amount corresponding to 10% to 90% by mass relative to the total weight of the sheet, particularly preferably in an amount corresponding to 15% to 85% by mass.

[0066] The optical component resin sheet constructed according to the present invention may contain (C) silica particles. The silica particles can serve as reinforcing fillers, and the shape of the particles is not limited in any particular way. Both solid silica and hollow silica can be used, and particularly when hollow silica is used, high light diffusion can be achieved due to the difference in refractive index.

[0067] Relative to the total weight of the sheet, component (C) is preferably included in an amount corresponding to 0% by mass to 70% by mass, particularly preferably in an amount corresponding to 0% by mass to 50% by mass.

[0068] For the resin sheet of the optical component made according to the present invention, it preferably contains an organohydrogen polysiloxane as a crosslinking agent for the above-mentioned component (A), and further preferably contains a curing catalyst (hydrogenation silylation reaction catalyst, etc.) and a curing delay agent (inhibitor). In addition, it is preferred to contain the aforementioned organohydrogen polysiloxane or organopolysiloxane, and preferably a polydiorganosiloxane with a degree of polymerization of 2 to 150 as a plasticizer.

[0069] For organohydrogen polysiloxanes, organohydrogen polysiloxanes having two or more silicon-bonded hydrogen atoms in their molecular structure can be used without any specific limitations, and when component (A) includes an alkenyl group, the amount of silicon-bonded hydrogen atoms in the organohydrogen polysiloxane should preferably range from 0.2 to 5 moles per 1 mole of alkenyl group. Furthermore, although the molecular structure of the organohydrogen polysiloxane is not subject to any specific limitations, one or more types of organohydrogen polysiloxanes selected from linear, branched, resinous, or cyclic forms with a degree of polymerization of 1000 or lower can be used without any specific limitations.

[0070] For the curing catalyst, hydrosilylation reaction catalysts, condensation catalysts, photoactive catalysts, peroxide catalysts, and other known curing agents can be used without any specific limitations, and the use of hydrosilylation reaction catalysts is preferred from the perspective of reaction control. Furthermore, when using hydrosilylation reaction catalysts, well-known curing delay agents can be added from the perspective of operability, processability, and curability control.

[0071] For the resin sheet of the optical component constructed according to the present invention, optional additives may be included, such as adhesion modifiers, for example, organofunctional alkoxysilane compounds, such as vinyltriethoxysilane, allyltrimethoxysilane, allyltriethoxysilane, 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane, or 3-methacryloyloxypropyltrimethoxysilane, provided that the purpose of the present invention is not hindered. Additionally, other optional components may be added, including antioxidants, such as those based on phenol, quinone, amine, phosphorus, phosphite, sulfur, thioether, etc.; light stabilizers, such as those based on triazole, benzophenone, etc.; flame retardants, such as those based on phosphate esters, halogens, phosphorus, antimony, etc.; one or more antistatic agents selected from cationic surfactants, anionic surfactants, and nonionic surfactants; and dyes, pigments, etc., provided that they do not impair the technical effects provided by the present invention. Note that when manufacturing the film, any particulate components with an average primary particle size exceeding 100 nm should preferably not be added.

[0072] The starting material for the resin sheet used in the optical components constructed according to the present invention can be dispersed in an organic solvent before coating to form a film or thin coating as described below. The type of organic solvent used is not limited in any particular way, as long as it is a compound capable of dissolving all or some of the constituent components of the composition, and preferably a solvent with a boiling point range of 80°C to 200°C. Examples include non-halogen solvents such as isopropanol, tert-butanol, cyclohexanol, cyclohexanone, methyl ethyl ketone, methyl isobutyl ketone, toluene, xylene, mesitylene, 1,4-dioxane, dibutyl ether, anisole, 4-methylanisole, ethylbenzene, ethoxybenzene, ethylene glycol, ethylene glycol dimethyl ether, ethylene glycol ethyl ether, 2-methoxyethanol (ethylene glycol monomethyl ether), diethylene glycol dimethyl ether, diethylene glycol monomethyl ether, ethyl acetate, butyl acetate, propyl propionate, 1-methoxy-2-propyl acetate, 1-ethoxy-2-propyl acetate, octamethylcyclotetrasiloxane, and hexamethyldisiloxane, as well as halogen-based solvents such as trifluoromethylbenzene, 1,2-bis(trifluoromethyl)benzene, 1,3-bis(trifluoromethyl)benzene, 1,4-bis(trifluoromethyl)benzene, trifluoromethylchlorobenzene, trifluoromethylfluorobenzene, and hydrofluoroethers. These organic solvents can be used alone or in combination of two or more. From the perspectives of operability and processability, uniformity of solid layer and improved heat resistance, isopropanol, methyl isobutyl alcohol, etc. are preferred.

[0073] The hardness of the resin sheet for the optical components made by the present invention will depend on the substrate and is therefore not limited in any particular way, but in practice, in terms of pencil hardness, it should preferably correspond to 2B or higher.

[0074] The optical component resin sheet made by the present invention is particularly suitable as a solid layer constituting a layered structure, and specifically, it is preferably placed at the interface with the surrounding air as a solid layer constituting a light-emitting device or a layered structure for a light-emitting device.

[0075] In one embodiment, the optical component resin sheet constituted by the present invention can be used as a component of a laminate equipped with a release layer. When the optical component resin sheet constituted by the present invention is formed on top of the release layer, the optical component resin sheet of the present invention or the laminate equipped with said optical component resin sheet can be used after separation from the release layer. Examples of laminates constituted by the present invention include laminates having the following structure. Note that in the following examples, " / " indicates that the layers are opposite each other in the lamination direction of the laminate (generally perpendicular to the thickness direction of the substrate). In addition, the substrate and the release layer can be integral or part of the same layer (a substrate that can be peeled off by establishing material or physical inhomogeneity), and each layer can be composed of multiple layers.

[0076] Example 1: Substrate / Release Layer / Resin Sheet for Optical Components Constructed by the Invention / Other Optional Layers

[0077] Example 2: Substrate / Release Layer / Resin Sheet for Optical Components Constructed by the Invention / Other Optional Layers / Release Layer / Substrate

[0078] Specifically, when the structure allows the optical component resin sheet made of the present invention, or an optical component equipped with the optical component resin sheet, to be sandwiched between two release layers as in Example 2, components equipped with the optical component resin sheet made of the present invention can be transported while the components are protected by a substrate. The substrate equipped with the release layers can be separated from both sides of the laminate at a desired time and place, and the optical component resin sheet made of the present invention, or only the optical component, can be positioned and laminated onto a target structure (such as a light source for a light-emitting device). Therefore, it is useful in terms of improving operability and processability.

[0079] The substrate used in the layered structure is not particularly limited in any way, and examples include paperboard, paperboard, clay-coated paper, polyolefin laminated paper, especially polyethylene laminated paper, synthetic resin film, natural fiber cloth, synthetic fiber cloth, artificial leather cloth, and metal foil. Specifically, synthetic resin film is preferred, and examples of synthetic resins include polyimide, polyethylene, polypropylene, polystyrene, polyvinyl chloride, polyvinylidene chloride, polycarbonate, polyethylene terephthalate, cyclic polyolefins, nylon, etc. The substrate is preferably in the form of a film or sheet. The corresponding thickness is not limited in any particular way, and the substrate can be designed to have a desired thickness based on the application. It should be noted that, as described below, the base material itself can be the material used as the release layer and can have a structure that imparts a degree of peelability by physically forming fine irregularities on the surface of the substrate.

[0080] The release layer is sometimes referred to as a release liner, release layer, or release coating, and may preferably be a release layer with release coating function, such as a siloxane release agent, a fluorinated release agent, an alkyd resin release agent, or a fluorosiloxane release agent, or a substrate that does not easily adhere to the resin sheet of the optical component made of the present invention due to the physical formation of minute irregularities on the substrate surface.

[0081] Other layers included in the laminations may correspond to one or more layers, or to two or more layers equipped with different functions. Furthermore, the total thickness of the laminations laminated onto the resin sheet of the optical component constituted by the present invention is not specifically limited in any way, but is preferably 10 μm or greater from the perspective of operability and processability, more preferably in the range of 50 to 10,000 μm, and particularly preferably in the range of 100 to 5,000 μm.

[0082] The optical component resin sheet constituted by the present invention, and the layered body equipped with the optical component resin sheet, can be used as a sealing sheet and can have a structure in which they are positioned on top of a light source such as an organic light-emitting diode, thereby sealing it. Here, when the optical component resin sheet constituted by the present invention contains a fluorescent material, the light emitted from the light source undergoes wavelength conversion.

[0083] In one embodiment, the optical component resin sheet constituted by the present invention is produced by applying an optical component resin sheet starting material to a substrate at a viscosity of 10 to 10,000 mPa·s at 25°C and a wet film thickness of 10 to 1,000 μm using a sheet coating machine.

[0084] The substrate used in the method for producing the resin sheet of the optical component constituted by the present invention is preferably a flexible substrate. Specifically, substrates listed in the aforementioned substrates used in the layered body can be used.

[0085] Examples of well-known methods for coating flexible substrates with coating solutions include curtain coating and bar coating, among which curtain coating is suitable for large-scale production but not for small-batch processing. Additionally, bar coating has the disadvantage of not maintaining a uniform surface on the sheet when used to apply coating solutions with particularly high viscosity or containing particles.

[0086] In contrast, the use of a coater or slit coater is suitable as a method for producing resin sheets for optical components made of the present invention because it allows for relatively easy implementation of batch processes in small quantities. Specifically, the use of a slit coater is preferred.

[0087] A slot coater that can be used in a method for producing resin sheets of optical components made according to the present invention is described herein with reference to the accompanying drawings. Figure 1 A schematic diagram of the coating head of a sheet coating machine according to an embodiment of the present invention is shown.

[0088] like Figure 1 As shown, the coating head 1 is equipped with a chamber 2 and a slot 3. A coating composition is supplied to the chamber 2 using a pump or the like. The coating composition is supplied from one side of the coating head 1 or from the side opposite to the slot 3.

[0089] The coating composition is preferably supplied to chamber 2 at a coating speed of w (cm / s), wherein the hydraulic build-up time is set to 1.0 / w s or less. During the initial coating process, it is necessary to rapidly form stable beads between the coating head and the substrate, and if the hydraulic build-up time is less than the time specified above, it is possible to reduce sheet loss caused by uneven film thickness at the beginning of the coating process.

[0090] The shape of chamber 2 is not subject to any particular restriction, and the chamber can be circular or semi-circular. Furthermore, a plug can be disposed on at least one side surface to prevent leakage of the composition during coating.

[0091] The slot 3 is the flow path used when the coating composition is discharged from the chamber 2 onto the substrate. Like the chamber 2, a plug may be provided on at least one side surface to prevent leakage of the composition during coating. Furthermore, an adjustment mechanism may be provided to adjust the width and length of the slot 3.

[0092] When the coating composition is applied to a substrate, the coating head 1 is positioned close to the substrate, and the coating composition is supplied to the substrate through the chamber 2 and the slot 3. Then, either the coating head 1 or the substrate moves in one direction. When this occurs, the distance between the coating head and the substrate preferably remains constant. Alternatively, both can move simultaneously to apply the coating, such that their relative speed remains constant.

[0093] Furthermore, the tip of the coating head 1 can be parallel or not parallel to the substrate. Additionally, the angle between the slot and the substrate is not limited in any particular way and can be, for example, perpendicular or not perpendicular to the substrate.

[0094] Figure 2 A schematic diagram of a sheet coating machine according to an embodiment of the present invention is shown. In addition to the coating head 1, the sheet coating machine is also equipped with a worktable 4, a coating head mounting base 5, a movable element 6 for moving the coating head up and down, and a movable element 7 for moving the worktable laterally.

[0095] The worktable 4 is a supporting base on which the substrate is placed, and is preferably equipped with a fixing device to ensure that the substrate does not move during the coating process. The fixing device can be drawn in from a suction port provided on the surface of the worktable 4, or it can be a physical fixation using metal fittings or the like.

[0096] The coating head 1 is positioned on top of the worktable 4 and is secured in place by a mounting base 5 and a movable element 6. The mounting base 5 is independent of the worktable 4 and, during coating, either the mounting base 5 or the worktable 4 moves horizontally. When the worktable 4 moves, it moves horizontally via the movable element 7. When the mounting base 5 moves, it can be moved via tracks extending along both sides of the worktable 4.

[0097] The coating head 1 can be moved vertically relative to the worktable 4 via the movable element 6. Therefore, the distance between the coating head 1 and the worktable 4 can be changed according to the physical properties of the coating composition used in coating, the target film thickness, the displacement speed of the worktable 4 or the mounting base 5 during the coating process, etc.

[0098] The resin sheet for optical components constructed according to the present invention can be processed in the form of a layer, and once peeled off, the resin sheet placed on top of the peeling layer can be used. When used as an optical component, the peeled resin sheet can be used to seal the light-emitting device.

[0099] If necessary, the resin sheet formed on the substrate or release layer can be appropriately cut before use. Specifically, the ends of the film with uneven thickness can be cut off to further improve the flatness of the film.

[0100] Example

[0101] The present invention is described in detail through the following examples, but is not limited to these examples. Note that in all the following examples, parts are given in the form of parts by mass.

[0102] (Synthesis of organopolysiloxanes)

[0103] Synthesis Example 1

[0104] The hydrolysis product of phenylsilsesquioxane (324 g, 2.37 mol Si) and propyl propionate (275 g) were added to a 2 L four-necked round-bottom flask and mixed together. Under a nitrogen atmosphere, the mixture was heated and reacted under reflux for 30 min. The reaction mixture was cooled to 100°C, and then a solution of propyl propionate (66%, 610.8 g) of diacetoxy-terminated polyphenylmethylsiloxane (degree of polymerization: 170) was added. The mixture was heated and refluxed for two hours, and then allowed to stand overnight. Vinylmethyldiacetoxysilane (21 g, 0.11 mol Si) was then added, and the mixture was refluxed for one hour. Water (57 mL) was then added, and azeotropic dehydration was performed to reduce the acetic acid concentration. The resulting reaction mixture was cooled to 100°C, and then a 1:1 mixture of methyltriacetoxysilane and ethyltriacetoxysilane (38.7 g, 0.17 mol Si) was added, and the mixture was refluxed for one hour. Then water (57 mL) was added, and the acetic acid concentration was reduced by azeotropic dehydration. The above procedure was repeated twice, followed by partial distillation of propyl propionate to obtain a transparent propyl propionate solution of organopolysiloxane with a linear polymer structure of resin (weight average molecular weight: 83,000, solids concentration: 74.2%).

[0105] The platinum content is 1 ppm and the average unit formula is (HMe2SiO). 1 / 2 ) 0.60 (PhSiO 3 / 2 ) 0.4 A platinum-divinyldisiloxane complex was prepared such that the SiH / Vi ratio was 1, and then propyl propionate was added to prepare a propyl propionate solution containing a total of 75.5% siloxane.

[0106] Synthesis Example 2

[0107] The hydrolysis product of phenylsilsesquioxane (324 g, 2.37 mol Si) and toluene (268 g) were added to a 2 L four-necked round-bottom flask and mixed together. Under a nitrogen atmosphere, the mixture was heated and reacted under reflux for 30 min. The reaction mixture was cooled to 100°C, and then a toluene solution (65%, 608 g) of diacetoxy-terminated polyphenylmethylsiloxane (degree of polymerization: 100) was added. After heating the reaction mixture under reflux for 2 hours, methyltriacetoxysilane (38 g, 0.17 mol Si) was added, and the mixture was refluxed for 2.5 hours. Then, vinylmethyldiacetoxysilane (21 g, 0.11 mol Si) was added, and the mixture was refluxed for 2 hours. Water (76 mL) was then added, and azeotropic dehydration was performed for 30 min until the organic layer separated and the aqueous layer removed from below. Next, the water was replaced with saturated brine, and the same procedure was repeated twice to reduce the acetic acid concentration, followed by two more repetitions with water. Toluene was partially distilled off to obtain a toluene solution of an organopolysiloxane with a transparent resin linear polymer structure (weight average molecular weight: 60,000, solids concentration: 75.8%). Propyl propionate was added to the toluene solution using a rotary evaporator, and the toluene was removed three times to obtain a transparent propyl propionate solution of an organopolysiloxane with a resin linear polymer structure (solids concentration: 78%).

[0108] The platinum content is 1 ppm and the average unit formula is (HMe2SiO). 1 / 2 ) 0.60 (PhSiO 3 / 2 ) 0.4 A platinum-divinyldisiloxane complex was prepared such that the SiH / Vi ratio was 1, and then propyl propionate was added to prepare a propyl propionate solution containing a total of 75.5% siloxane.

[0109] (Preparation of resin sheet composition)

[0110] Example 1

[0111] More than 8.0 g of the solution obtained in Synthesis Example 1, 5.93 g of fluorescent material (manufactured by Intematix, NYAG 4454-L), 9.59 g of silica particles (manufactured by Denka, FB-5SDC, average particle size: 5 μm), and 3.25 g of propyl propionate were mixed together and stirred until homogeneous using an automatic stirrer (Thinky, ARV-310LED) equipped with a vacuum degassing mechanism to obtain resin sheet composition 1. The viscosity of the thixotropic solution was 2,173 mPa·s (10 1 / s) and 5,105 mPa·s (1 1 / s). Using a coating machine (PI-1210 FILM COATER), a T788 PET film manufactured by Daicel Value Coating Co., Ltd. was coated with a frame coater (IMC-3501 type) manufactured by Imoto Seisakusho, with a gap of 260 μm. The coated sheet was then dried in an oven at 70°C for 30 minutes. The resulting sheet was a rectangular sheet with a width of 150 mm and a length of 310 mm.

[0112] The film thickness of the obtained sheet in the width direction was measured using a film thickness gauge (DIGIMICRO MFC-101A manufactured by Nikon), and the film has a uniform thickness of 103 ± 1 μm.

[0113] Example 2

[0114] 8.0 g or more of the solution obtained in Synthesis Example 1, 15.53 g of fluorescent material (manufactured by Intermay, NYAG 4454-L), and 1.75 g of propyl propionate were mixed together and stirred until homogeneous using an automatic stirrer (Thinky, ARV-310LED) equipped with a vacuum degassing mechanism to obtain resin sheet composition 2. The viscosity was 3,269 mPa·s (10 1 / s). Using a coater (PI-1210 FILM COATER), a T788 PET film manufactured by Celebratory Value Coatings Co., Ltd. was coated with a frame coater (IMC-3501 type) manufactured by Imoto Seisakusho, with a gap of 253 μm. The coated sheet was then dried in an oven at 70°C for 30 minutes. The resulting sheet was a rectangular sheet with a width of 150 mm and a length of 310 mm.

[0115] The film thickness of the obtained sheet in the width direction was measured using a film thickness gauge (DIGIMICRO MFC-101A manufactured by Nikon), and the film has a uniform thickness of 103 ± 1 μm.

[0116] Example 3

[0117] More than 40.0 g of the solution obtained in Synthesis Example 1 and 7.56 g of fluorescent material (manufactured by Intermay, NYAG 4454-S) were mixed together and stirred until homogeneous using an automatic stirrer (Thinky, ARV-310LED) equipped with a vacuum degassing mechanism to obtain resin sheet composition 3. The viscosity was 10,573 mPa·s (10 1 / s). Using a coater (PI-1210 FILM COATER), a T788 PET film manufactured by Celebratory Value Coatings Co., Ltd. was coated with a frame coater (IMC-3501 type) manufactured by Imoto Seisakusho, with a gap of 236 μm. The coated sheet was then dried in an oven at 70°C for 30 minutes. The resulting sheet was a rectangular sheet with a width of 150 mm and a length of 310 mm.

[0118] The film thickness of the obtained sheet in the width direction was measured using a film thickness gauge (DIGIMICRO MFC-101A manufactured by Nikon), and the film has a uniform thickness of 93 ± 1 μm.

[0119] Example 4

[0120] 40.0 g or more of the solution obtained in Synthesis Example 1, 7.33 g of fluorescent material (manufactured by Intermay, NYAG 4454-S), and 0.25 g of REOROSEAL (DM-30) were mixed together and stirred until homogeneous using an automatic stirrer (Thinky, ARV-310LED) equipped with a vacuum degassing mechanism to obtain resin sheet composition 4. The viscosity was 11,988 mPa·s (10 1 / s). Using a coater (PI-1210 FILM COATER), a T788 PET film manufactured by Celebratory Value Coatings Co., Ltd. was coated with a frame coater (IMC-3501 type) manufactured by Imoto Seisakusho, with a gap of 236 μm. The coated sheet was then dried in an oven at 70°C for 30 minutes. The resulting sheet was a rectangular sheet with a width of 160 mm and a length of 310 mm.

[0121] The film thickness of the obtained sheet in the width direction was measured using a film thickness gauge (DIGIMICRO MFC-101A manufactured by Nikon), and the film has a uniform thickness of 93 ± 1 μm.

[0122] Example 5

[0123] More than 40.0 g of the solution obtained in Synthesis Example 2 was mixed with 20.12 g of titanium dioxide (SX-3103, average 0.2 μmD) and stirred until homogeneous using an automatic stirrer (Thinky Corporation, ARV-310LED) equipped with a vacuum degassing mechanism to obtain resin sheet composition 5. The viscosity was 9,554 mPa·s (10 1 / s). Using a coating machine (PI-1210FILM COATER), a frame coater (IMC-3501 type) manufactured by Imoto Seisakusho was used to coat a T788 PET film manufactured by Celebratory Value Coatings Co., Ltd. with a gap of 254 μm. The coated sheet was then dried in an oven at 70°C for 30 minutes. The resulting sheet was a rectangular sheet with a width of 160 mm and a length of 310 mm.

[0124] The film thickness of the obtained sheet in the width direction was measured using a film thickness gauge (DIGIMICRO MFC-101A manufactured by Nikon), and the film has a uniform thickness of 106 ± 2 μm.

[0125] Comparison Example 1

[0126] The resin sheet composition 3 prepared in Example 3 was applied to a release sheet (Daicel, T788) using a rod (manufactured by RD Specialties, No. 10). The coated sheet was then dried in an oven at 70°C for 30 minutes. The resulting sheet was a rectangular sheet with a width of 150 mm and a length of 300 mm.

[0127] The film thickness of the obtained sheet in the width direction was measured using a film thickness gauge (DIGIMICRO MFC-101A manufactured by Nikon), and the film had a non-uniform thickness ranging from 42 to 54 μm (the difference between the thickness at the edge of the sheet and the thickness at the center of the sheet was 12 μm).

[0128] As shown above, although substantially flat optical component resin sheets were obtained in Examples 1 to 5, it was not possible to obtain flat optical component resin sheets in Comparative Example 1, which used a different manufacturing process.

[0129] Industrial applicability

[0130] The optical component resin sheet constituted by the present invention, and the layered body equipped with the optical component resin sheet, can be suitably used as an optical component in optical devices such as LEDs. Furthermore, the method for producing the optical component resin sheet constituted by the present invention is applicable to the purpose of producing various different optical component resin sheets in small batches.

[0131] Explanation of reference numerals in the attached figures

[0132] 1 Coating head

[0133] 2 chambers

[0134] 3. Slot

[0135] 4 workbench

[0136] 5. Mounting base

[0137] 6 movable components

[0138] 7. Movable components

Claims

1. A resin sheet for an optical component, wherein, with respect to the width direction of the sheet, the difference between the thickness at the edge of the sheet and the thickness at the center of the sheet is not greater than 5.0% relative to the total sheet thickness, the thickness at the center of the sheet ranges from 10 to 1,000 μm, and the sheet area is at least 225 mm². 2 And characterized in that It contains at least one type of fluorescent or reflective material. The optical component resin sheet comprises: (A) One or more fluorescent substances selected from oxide phosphors, oxynitride phosphors, nitride phosphors, sulfide phosphors, fluoride phosphors, and oxysulfide phosphors, and (B) A linear organopolysiloxane block copolymer of resin, which has alkenyl and siloxane units in its molecular structure, and is derived from formula R. A SiO 3 / 2 It means that R A It is an aryl group having 6 to 14 carbon atoms, and is composed of the formula (R2SiO) 2 / 2 ) n The polydiorganosiloxane structure is represented, wherein R is an aryl group having 6 to 14 carbon atoms or an alkyl group having 1 to 20 carbon atoms, which may be halogen-substituted, and n is a number ranging from 3 to 1,000, wherein component (B) is non-flowing at 25°C. Organohydropolysiloxanes, which have the formula (HR) B SiO 1 / 2 ) x (R A SiO 3 / 2 ) y , where R B Independently, it is an alkyl group having 1 to 20 carbon atoms, R A An aryl group having 6 to 14 carbon atoms, x>0, y>0 and x+y=1, and having at least two silicon-bonded hydrogen atoms; and Catalyst for hydrogenation silylation reaction.

2. The optical component resin sheet as claimed in claim 1, further comprising (C) silica particles.

3. A layered body equipped with the optical component resin sheet as described in claim 1.

4. The layered body as claimed in claim 3, further provided with a peeling layer.

5. A light-emitting device having a structure sealed with an optical component resin sheet as described in claim 1.

6. A method for producing resin sheets for optical components, wherein, with respect to the width direction of the sheet, the difference between the thickness at the edge of the sheet and the thickness at the center of the sheet is not greater than 5.0% relative to the total sheet thickness, the thickness at the center of the sheet ranges from 10 to 1,000 μm, and the sheet area is at least 225 mm². 2 Its characteristics are, Using a coater or slot coater as a sheet coater, the starting material for the optical component resin sheet is applied to the substrate at a viscosity of 10 to 10,000 mPa·s at 25°C and a wet film thickness of 10 to 1,000 μm.

7. The method for producing resin sheets for optical components as described in claim 6, characterized in that, Production was carried out using a slot coater as a sheet coater, with the hydraulic build-up time set to 1.0 / w seconds or less and the coating speed at w (cm / s).

8. The method for producing an optical component resin sheet as claimed in claim 6, wherein the starting material of the optical component resin sheet comprises: (A) One or more fluorescent substances selected from oxide phosphors, oxynitride phosphors, nitride phosphors, sulfide phosphors, fluoride phosphors, and oxysulfide phosphors, and (B) Organopolysiloxanes, which have the following molecular structure within their molecular structure: R A SiO 3 / 2 The arylsiloxane unit is represented by R. A It is an aryl group having 6 to 14 carbon atoms, and is composed of the formula (R2SiO) 2 / 2 ) n The polydiorganosiloxane structure is represented, wherein R is an aryl group having 6 to 14 carbon atoms or an alkyl group having 1 to 20 carbon atoms, which may be halogen-substituted, and n is a number ranging from 3 to 1,000.

9. The method for producing resin sheets for optical components as described in claim 6, wherein, The organopolysiloxane (B) also contains an alkenyl group within its molecular structure.

10. The method for producing resin sheets for optical components as described in claim 9, wherein, The starting material for the optical component resin sheet also includes an organohydrogen polysiloxane having at least two hydrogen atoms bonded to silicon atoms, and a hydrogenation silylation reaction catalyst.

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