Coating, coating layer, and light emitting device

Abstract

The present invention relates to a coating, a coating layer, and a light emitting device, wherein the coating includes: modified particles including: a core; and a silane coupling agent having an epoxy group or a silane coupling agent having a double bond grafted to a surface of the core; and a reactive compound, the reactive compound including a non-silicon-containing polyepoxy compound when the silane coupling agent having an epoxy group is grafted to the surface of the core and a silicon-containing polyepoxy compound when the silane coupling agent having a double bond is grafted to the surface of the core.

Description

Technical Field

[0001] This disclosure relates to coatings, and more particularly to the coatings formed by coatings and their applications. Background Technology

[0002] Pure organic polymers struggle to achieve high refractive indices. Inorganic coatings can achieve high refractive indices, but their low flexibility and high density (>2.5cm³) hinder their development. 3 This presents challenges in subsequent applications due to manufacturing difficulties. In summary, there is an urgent need to design new film compositions that combine the advantages of both organic and inorganic materials, enabling their application in high-refractive-index films. Summary of the Invention

[0003] The coating provided in one embodiment of the present invention comprises: modified particles, including: a core; and an epoxy-based silane coupling agent or a double-bonded silane coupling agent grafted onto the surface of the core, wherein the core comprises (1) an oxide of zinc and titanium, wherein the weight ratio of zinc to titanium is 1:0.4 to 1:0.9, (2) an oxide of zirconium and titanium, wherein the weight ratio of zirconium to titanium is 1:0.1 to 1:2, or (3) an oxide of zinc and zirconium, wherein the weight ratio of zinc to zirconium is 1:0.8 to 1:2; and a reactive compound, wherein when the epoxy-based silane coupling agent is grafted onto the surface of the core, the reactive compound comprises a silicon-free polyepoxide compound and a silicon-containing polyepoxide compound, and when the double-bonded silane coupling agent is grafted onto the surface of the core, the reactive compound comprises a compound with multiple double bonds.

[0004] The coating provided in one embodiment of the present invention is formed by the reaction of the above-mentioned coating material.

[0005] A light-emitting device provided in one embodiment of the present invention includes: a substrate; a light-emitting unit located on the substrate; and the aforementioned coating covering the substrate and the light-emitting unit. Detailed Implementation

[0006] The coating provided in one embodiment of this disclosure includes modified particles and reactive compounds. The modified particles include a core; and a silane coupling agent having an epoxy group or a silane coupling agent having a double bond, grafted onto the surface of the core. The core includes (1) an oxide of zinc and titanium, (2) an oxide of zirconium and titanium, or (3) an oxide of zinc and zirconium. When the core includes (1) an oxide of zinc and titanium, the weight ratio of zinc to titanium is 1:0.4 to 1:0.9. If the proportion of zinc is too high, precipitation is likely to occur, and the core is not easy to maintain a stable crystalline state. If the proportion of titanium is too high, the core is likely to gel rapidly during the reaction and become unusable. When the core includes (2) an oxide of zirconium and titanium, the weight ratio of zirconium to titanium is 1:0.1 to 1:2. If the proportion of titanium is too high, the color is too dark yellow and it is difficult to maintain high transmittance and low b* value in the visible light band. When the core includes (3) an oxide of zinc and zirconium, the weight ratio of zinc to zirconium is 1:0.8 to 1:2. In one embodiment, the weight ratio of zinc to zirconium is from 1:0.8 to 1:1.8. If the proportion of zinc is too high, precipitation will occur. If the proportion of zirconium is too high, excessive bonding and gelation will occur.

[0007] When an epoxy-based silane coupling agent is grafted onto the core surface, the reactive compounds include both silicon-free and silicon-containing polyepoxides. When a double-bonded silane coupling agent is grafted onto the core surface, the reactive compounds include compounds with multiple double bonds.

[0008] In one embodiment, the core is formed by the hydrolysis of a zinc source to form zinc oxide, followed by a condensation reaction with a titanium source. The core primarily contains titanium, zinc, and oxygen, such as titanium and zinc oxides, and its surface has multiple hydroxyl and alkoxy groups. It is noteworthy that the core is a titanium and zinc oxide, not a mixture of titanium oxide and zinc oxide (e.g., there is no bond between the titanium in titanium oxide and the oxygen in zinc oxide, nor between the oxygen in titanium oxide and the zinc in zinc oxide). Compared to cores composed of titanium and zinc oxide oxides, cores composed of titanium oxide and zinc oxide precipitate as solids. Then, a silane coupling agent with epoxy groups or a silane coupling agent with double bonds is reacted with the core, causing the Si-O-alkyl group of the silane to react with the -OR (R = H or alkyl) groups on the core surface to form Zn / Ti-O-Si bonds, i.e., the silane coupling agent is grafted onto the surface of the core. It is important to note that the above reaction is only one method, not the only method, for forming modified particles. Those skilled in the art can use appropriate reagents to form the above-mentioned modified particles.

[0009] In one embodiment, the core is formed by a condensation reaction of a zirconium source and a titanium source. The core mainly contains titanium, zirconium, and oxygen, such as titanium and zirconium oxides, and its surface has multiple hydroxyl and alkoxy groups. It is noteworthy that the core is a titanium and zirconium oxide, rather than a mixture of titanium oxide and zirconium oxide (e.g., there is no bond between the titanium in titanium oxide and the oxygen in zirconium oxide, and no bond between the oxygen in titanium oxide and the zirconium in zirconium oxide). Compared to titanium and zirconium oxide cores, the mixture of titanium oxide and zirconium oxide cores precipitates as a solid precipitate. Then, a silane coupling agent with epoxy groups or a silane coupling agent with double bonds is reacted with the core, causing the Si-O-alkyl group of the silane to react with the -OR (R=H or alkyl) groups on the core surface to form Zr / Ti-O-Si bonds, i.e., the silane coupling agent is grafted onto the surface of the core. It is important to note that the above reaction is only one method for forming modified particles, not the only method.

[0010] In one embodiment, the core is formed by the hydrolysis of a zinc source to form zinc oxide, followed by a condensation reaction with a zirconium source. The core primarily contains zinc, zirconium, and oxygen, such as zinc and zirconium oxides, and its surface has multiple hydroxyl and alkoxy groups. It is noteworthy that the core is a zinc and zirconium oxide, not a mixture of zinc oxide and zirconium oxide (e.g., there is no bond between the zinc in zinc oxide and the oxygen in zirconium oxide, nor between the oxygen in zinc oxide and the zirconium in zirconium oxide). Compared to cores composed of zinc and zirconium oxides, cores composed of zinc oxide and zirconium oxide precipitate as solids. Then, a silane coupling agent with epoxy groups or a silane coupling agent with double bonds is reacted with the core, causing the Si-O-alkyl group of the silane to react with the -OR (R = H or alkyl) groups on the core surface to form Zn / Zr-O-Si bonds, i.e., the silane coupling agent is grafted onto the surface of the core. It is important to note that the above reaction is only one method, not the only method, for forming modified particles. Those skilled in the art can use appropriate reagents to form the above-mentioned modified particles.

[0011] In some embodiments, the zinc source may be zinc acetate, zinc perchlorate, or zinc bromide. In some embodiments, the titanium source may be titanium isopropoxide, titanium tetrachloride, or titanium butoxide. In some embodiments, the zirconium source may be zirconium n-propoxide, zirconium isopropoxide, or zirconium tetrachloride.

[0012] In some embodiments, the weight ratio of the total weight of zinc and titanium in the core to the weight of the epoxy-based silane coupling agent or the silane coupling agent with double bonds is 1:0.1 to 1:3, or 1:0.1 to 1:1.5. In some embodiments, the weight ratio of the total weight of zirconium and titanium in the core to the weight of the epoxy-based silane coupling agent or the silane coupling agent with double bonds is 1:0.1 to 1:3, or 1:0.1 to 1:1.5. In some embodiments, the weight ratio of the total weight of zinc and zirconium in the core to the weight of the epoxy-based silane coupling agent or the silane coupling agent with double bonds is 1:0.1 to 1:3, or 1:0.1 to 1:1.5. If the proportion of silane coupling agent is too low, film formation is impossible. If the proportion of silane coupling agent is too high, the refractive index of the formed coating is insufficient (e.g., less than 1.7).

[0013] In some implementations, the average particle size of the core is 10 nm to 120 nm, or 15 nm to 55 nm. If the average particle size of the core is too small, the coating will not be able to produce a high refractive index effect. If the average particle size of the core is too large, the coating transmittance will be less than 90%, which will not improve the light extraction effect.

[0014] In some embodiments, the epoxy-based silane coupling agent includes 3-glycidyl etheroxypropyltrimethoxysilane, 3-glycidyl etheroxypropyltriethoxysilane, 3-glycidyl etheroxypropylmethyldimethoxysilane, 3-glycidyl etheroxypropylmethyldiethoxysilane, 2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane, or 2-(3,4-epoxycyclohexyl)ethyltriethoxysilane.

[0015] In some embodiments, the silane coupling agent having a double bond includes propyl 3-trimethoxysilane acrylate, 3-(triethoxysilyl)propyl isocyanate, or... Where R is methyl or ethyl, and n = 1-3.

[0016] In some implementations, the weight ratio of the core to the reactive compound is 1:0.2 to 1:0.8. If the proportion of the reactive compound is too low, the resulting coating will split. If the proportion of the reactive compound is too high, the coating will have an insufficient refractive index.

[0017] In some implementations, the weight ratio of the silicone-free epoxy compound to the silicone-containing epoxy compound is from 1:0.4 to 1:1. If the proportion of the silicone-free epoxy compound is too low, the resulting coating will split. If the proportion of the silicone-free epoxy compound is too high, the coating will have insufficient penetration.

[0018] In some embodiments, the silicon-free polyepoxide includes long carbon chains, benzene rings, or cyclic structures, and has a viscosity of <1000 cP at 25°C. For example, silicon-free polyepoxides include...

[0019] k = 1 to 6, or a combination thereof.

[0020] In some embodiments, the silicon-containing polyepoxide includes long carbon chains, benzene rings, or cyclic structures, and has a viscosity of <1000 cP at 25°C. For example, the silicon-containing polyepoxide includes...

[0021] Where m = 1 to 6, n = 1 to 6,

[0022]

[0023] Where n = 1 to 6, or a combination thereof.

[0024] In some embodiments, the multi-double-bond compound comprises a long carbon chain, a benzene ring, or a cyclic structure, and has a viscosity of <1000 cP at 25°C. For example, the multi-double-bond compound includes... Where a = 2 to 6 and b = 2 to 6, or a combination thereof.

[0025] The coating provided in one embodiment of the present invention is formed by reacting the aforementioned coating material. For example, if the core surface of the modified particles in the coating is grafted with a silane coupling agent having epoxy groups, and the corresponding reactive compounds include silicon-free polyepoxides and silicon-containing polyepoxides, the coating may further include a catalytic amount of a crosslinking agent. The crosslinking agent can open the epoxy groups to achieve a crosslinking effect. In some embodiments, the weight ratio of coating to crosslinking agent is between 1:0.09 and 1:0.13. If the amount of crosslinking agent is too low, the coating cannot crosslink to form a film during the reaction. If the amount of crosslinking agent is too high, the refractive index will be significantly reduced. In some embodiments, the crosslinking agent is a C2-C6 amine compound, a C2-C6 alcohol compound, or a C2-C6 acid compound. In some embodiments, the crosslinking agent is HO-(CH2). n -NH2, and n is 2 to 4. For example, if the core surface of the modified particles in the coating is grafted with a silane coupling agent having double bonds, and the corresponding reactive compound includes a compound with multiple double bonds, then the coating may further include a catalytic amount of a free radical initiator. For example, the weight ratio of the coating to the free radical initiator may be 1:0.09 to 1:0.13. The free radical initiator may be a thermal initiator or a photoinitiator, which, upon exposure to light or heating, generates free radicals that crosslink the double bonds of the silane coupling agent with the compound with multiple double bonds.

[0026] In some embodiments, the coating can be applied to a substrate by methods such as blade coating or spin coating, and any active or passive cells can be present on or within the substrate. The coating is then cured to form a coating layer. In some embodiments, the coating thickness is 20 to 40 micrometers, the refractive index is 1.70 to 2.4, and the transmittance is 90% to 99.5%. If the coating thickness is too small, it cannot effectively protect the active or passive cells it covers. If the refractive index is too low, light loss due to the difference in refractive index cannot be avoided when covering high-refractive-index cells such as micro-LEDs. If the transmittance of the coating is too low, it is unsuitable as a protective layer for light transmission (such as a protective layer covering light-emitting cells).

[0027] The light-emitting device provided in one embodiment of this disclosure includes: a substrate; a light-emitting unit located on the substrate; and the aforementioned coating covering the light-emitting unit and the substrate. Because the coating in this embodiment has sufficient thickness, refractive index, and light transmittance, it can effectively protect the light-emitting unit. In some embodiments, the light-emitting unit may be a light-emitting diode, such as an organic light-emitting diode, an inorganic light-emitting diode, or other suitable light-emitting diode. Since the refractive index of the material of the light-emitting unit is generally greater than 2, if the refractive index of the film covering the light-emitting unit is too small (e.g., less than 1.7), the difference in refractive index will cause light loss. It is worth noting that although the coating of this disclosure is mainly used to protect the light-emitting unit in the light-emitting device, it should be understood that the film material can also be used to protect other units besides the light-emitting unit, and is not limited to the light-emitting device.

[0028] In summary, the organic-inorganic composite coating of this disclosure simultaneously combines the advantages of organic molecules, such as lightweight, flexibility, high impact resistance, and ease of manufacturing, with the high refractive index, high chemical resistance, and high heat resistance of inorganic materials. Through composite material design, the refractive index can be controlled and high transmittance maintained, and the coating thickness can be further increased. In short, the coating provided by this disclosure can provide a high-transmittance, high-refractive-index, and high-film-thickness coating to achieve the effect of protecting components (such as high-refractive-index light-emitting diodes).

[0029] To make the foregoing contents and other objects, features and advantages of this disclosure more apparent and understandable, preferred embodiments are described in detail below:

[0030] Example

[0031] In the following embodiments, the transmittance of the coating was measured using an ultraviolet / visible spectrometer, with the wavelength defined as 450 nm as the reference point. The refractive index was measured using a thin film analyzer (N&K analyzer). The core particle size was measured using a multi-sample nanoparticle size measurement system (Otsuka nanoSAQLA), with a measurement range of 0.6 nm to 10 μm and an accuracy of ±2%. In the following embodiments, the viscosity was measured according to ASTM D1084, using a Brookfield Viscometer DV-III Ultra instrument.

[0032] Synthesis example 1

[0033] 5g of zinc acetate, 20g of isopropanol, and 1.9g of ethanolamine were dissolved by heating to 80℃ and reacted for 5 minutes. Then, 10g of titanium isopropoxide and 0.25g of isopentanedione were added, and the mixture was reacted at 80℃ for 8 hours to form a core containing zinc and titanium oxides in a weight ratio of 1:0.6. Next, 2.2g of 3-glycidyl etheroxypropyltrimethoxysilane was added for surface modification. The total weight ratio of zinc and titanium in the core to the weight ratio of 3-glycidyl etheroxypropyltrimethoxysilane was 1:0.15, allowing the Si-O-CH3 of the silane to react with the -OR (R=H or CH(CH3)2) on the core surface to form Zn / Ti-O-Si bonds. This silane grafting onto the core surface forms a dispersion of modified particles with an average core particle size of 80nm.

[0034] Synthesis example 2

[0035] 5g of zinc acetate, 20g of isopropanol, and 1.9g of ethanolamine were dissolved by heating to 80℃ and reacted for 5 minutes. Then, 10g of titanium isopropoxide and 0.25g of isopentene were added, and the mixture was reacted at 80℃ for 8 hours to form a core containing zinc and titanium oxides in a weight ratio of 1:0.6. Next, 2.2g of 3-glycidyl etheroxypropyltrimethoxysilane was added for surface modification. The total weight ratio of zinc and titanium in the core to 3-glycidyl etheroxypropyltrimethoxysilane was 1:0.15, allowing the Si-O-CH3 of the silane to react with the -OR (R=H or CH(CH3)2) on the core surface to form Zn / Ti-O-Si bonds. This silane grafting onto the core surface forms a dispersion of modified particles with an average core particle size of 80nm. Finally, isopropanol was replaced with toluene.

[0036] Synthesis example 3

[0037] 15g of zirconium n-propoxide, 15g of titanium isopropoxide, 20g of isopropanol, and 0.25g of isopentanedione were reacted at 80℃ for 8 hours to form a core containing zirconium and titanium oxides in a weight ratio of 1:0.9. Then, 3g of 3-glycidyl etheroxypropyltrimethoxysilane was added for surface modification. The total weight ratio of zirconium and titanium in the core to 3-glycidyl etheroxypropyltrimethoxysilane was 1:0.1, allowing the Si-O-CH3 of the silane to react with the -OR (R=H or CH(CH3)2) on the core surface to form Zr / Ti-O-Si bonds. This silane grafting onto the core surface forms a dispersion of modified particles with an average core particle size of 40nm.

[0038] Synthesis example 4

[0039] 5g of zinc acetate, 20g of isopropanol, and 1.9g of ethanolamine were dissolved by heating to 80℃ and reacted for 5 minutes. Then, 10g of titanium isopropoxide and 0.25g of isopentene were added, and the mixture was reacted at 80℃ for 8 hours to form a core containing zinc and titanium oxides in a weight ratio of 1:0.6. Subsequently, 2.2g of propyl 3-trimethoxysilane acrylate was added for surface modification. The total weight ratio of zinc and titanium in the core to propyl 3-trimethoxysilane acrylate was 1:0.15, allowing the Si-O-CH3 of silane to react with the -OR (R=H or CH(CH3)2) on the core surface to form Zn / Ti-O-Si bonds. This silane grafting onto the core surface forms a dispersion of modified particles with an average core particle size of 75nm.

[0040] Synthesis example 5

[0041] Take 5g of zinc acetate, 20g of isopropanol, and 3mL of KOH (0.48M), heat to 80℃ to dissolve, and react for 5 minutes. Then add 10g of zirconium n-propoxide and react at 80℃ for 8 hours to form a core containing zinc and zirconium oxides in a weight ratio of 1:1.8. Next, add 2.2g of propyl 3-trimethoxysilane acrylate for surface modification. The total weight ratio of zinc and zirconium in the core to propyl 3-trimethoxysilane acrylate is 1:0.15, allowing the Si-O-CH3 of silane to react with the -OR (R=H or CH(CH3)2) on the core surface to form Zn / Zr-O-Si bonds. This silane grafting onto the core surface forms a dispersion of modified particles with an average core particle size of 79nm.

[0042] Verification Example

[0043] Take 0.25g of silicon-containing polyepoxide compound GT1250 (purchased from Guangke Industrial, its structure is as follows) Where m = 1–6 and n = 1–6, the mixture, after being mixed with a dispersion containing 1 g of the modified particles from Synthesis Example 1, remained in a phase-free liquid state without precipitation. As can be seen from the above, the silicon-containing epoxy compound GT1250 is compatible with the modified particles. The above solution can be coated and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, GT1250 can be considered as one of the options for reactive compounds.

[0044] Take 0.25g of the silicon-containing polyepoxide compound ESP-EDTP0204 (self-synthesized, its structure is as follows) When ESP-EDTP0204 was mixed with a dispersion containing 1g of the modified particles from Synthesis Example 1, phase separation or precipitation occurred. Similarly, when 0.25g of the silicon-containing polyepoxide compound ESP-EDTP0204 was mixed with 1g of the modified particles from Synthesis Example 2, phase separation or precipitation also occurred. Therefore, it is clear that the silicon-containing epoxy compound ESP-EDTP0204 is incompatible with the modified particles. In conclusion, ESP-EDTP0204 cannot be used as a reactive compound.

[0045] Take 0.25g of the silicon-containing polyepoxide compound SIT8715.6 (purchased from Gelest, its structure is as follows). The solution, when mixed with a dispersion containing 1 g of the modified particles from Synthesis Example 1, remained a liquid without phase separation and showed no precipitation. Therefore, the silicon-containing epoxy compound SIT8715.6 is compatible with the modified particles. The solution can be coated and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, SIT8715.6 can be considered as one of the options for reactive compounds.

[0046] Take 0.25g of the silicon-containing polyepoxide compound SIT7281.5 (purchased from Gelest, its structure is as follows). The modified particles from Synthetic Example 1, when mixed with a dispersion containing 1g of the modified particles, remained in a liquid state without phase separation or precipitation. Similarly, 0.25g of the silicon-containing polyepoxide compound SIT7281.5, when mixed with a dispersion containing 1g of the modified particles from Synthetic Example 2, also remained in a liquid state without phase separation or precipitation. This indicates that the silicon-containing epoxy compound SIT7281.5 is compatible with the modified particles. However, neither solution can be coated and baked (80°C for 10 minutes and 120°C for 10 minutes) to form a 5-micrometer-thick dry film. Therefore, SIT7281.5 should not be considered as a reactive compound.

[0047] Take 0.25g of silicon-free polyepoxide compound YX7400 (Mitsubishi Chemical, its structure is...). When mixed with a dispersion containing 1 g of the modified particles from Synthesis Example 1 (k = 1-6), the mixture remained a liquid without phase separation and showed no precipitation. As can be seen from the above, the silicon-free epoxy compound YX7400 is compatible with the modified particles. The solution from Synthesis Example 1 can be coated and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, YX7400 can be considered as one of the options for reactive compounds.

[0048] Take 0.25g of silicon-free polyepoxide compound 412P (purchased from Double Bond Chemical, its structure is as follows) The mixture, when mixed with a dispersion containing 1 g of the modified particles from Synthesis Example 1, remained in a phase-free liquid state without precipitation. As can be seen from the above, the silicon-free epoxy compound 412P is compatible with the modified particles. The above solution can be coated and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, 412P can be considered as one of the options for reactive compounds.

[0049] Take 0.25g of the silicon-containing polyepoxide compound DMS-EC13 (purchased from Gelest, its structure is as follows) When n = 1 to 6) is mixed with a dispersion containing 1 g of the modified particles from Synthetic Example 1, it remains a liquid without phase separation and precipitation. Similarly, when 0.25 g of the silicon-containing polyepoxide compound DMS-EC13 is mixed with a dispersion containing 1 g of the modified particles from Synthetic Example 2, it also remains a liquid without phase separation and precipitation. Therefore, the silicon-containing epoxy compound DMS-EC13 is compatible with the modified particles. The above solution can be coated and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, DMS-EC13 can be considered as one of the reactive compounds.

[0050] Take 0.25g of the silicon-containing polyepoxide compound ECMS-924 (purchased from Gelest, its structure is as follows) When the mixture (where m = 1–6, n = 1–6) is mixed with a dispersion containing 1 g of the modified particles from Synthesis Example 1, phase separation or precipitation occurs. As can be seen from the above, the silicon-containing epoxy compound ECMS-924 is incompatible with the modified particles. Therefore, ECMS-924 cannot be considered as a reactive compound.

[0051] Take 0.25g of the silicon-containing polyepoxide compound SIB-1110 (purchased from Gelest, its structure is as follows) The mixture, after being mixed with a dispersion containing 1 g of the modified particles from Synthesis Example 1, remained in a liquid state without phase separation and without precipitation. As can be seen from the above, the silicon-containing epoxy compound SIB-1110 is compatible with the modified particles. The above solution can be coated and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, SIB-1110 can be considered as one of the options for reactive compounds.

[0052] Take 0.25 g of the silicon-free polyepoxide compound HDGE (1,6-hexanediol diglycidyl ether) (purchased from Aldrich, its structure is as follows). The solution, when mixed with a dispersion containing 1 g of the modified particles from Synthetic Example 1, remained a liquid without phase separation and showed no precipitation. As can be seen from the above, the silicon-free epoxy compound HDGE is compatible with the modified particles. The above solution can be coated and baked (at 80°C for 10 minutes and at 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, HDGE can be considered as one of the options for reactive compounds.

[0053] Take 0.25g of silicon-free polyepoxide compound YL983U (purchased from Mitsubishi Chemical, its structure is as follows) The solution, when mixed with a dispersion containing 1 g of the modified particles from Synthesis Example 1, remained a liquid without phase separation and showed no precipitation. Therefore, the silicon-free epoxy compound YL983U is compatible with the modified particles. The solution can be coated and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, YL983U can be considered as one of the reactive compounds.

[0054] Take 0.25g of silicon-free polyepoxide compound YL 980 (purchased from Mitsubishi Chemical, its structure is as follows) The solution, when mixed with a dispersion containing 1 g of the modified particles from Synthesis Example 1, remained a liquid without phase separation and showed no precipitation. Therefore, the silicon-free epoxy compound YL980 is compatible with the modified particles. The solution can be coated and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, YL 980 can be considered as one of the options for reactive compounds.

[0055] Take 0.25 g of the compound SR238 (purchased from Sartomer AMERICAS, its structure is as follows) The compound SR238, when mixed with a dispersion containing 1 g of the modified particles from Synthesis Example 1, remained in a liquid state without phase separation or precipitation. This indicates that the aforementioned compound with multiple double bonds, SR238, is compatible with the modified particles. The solution can be coated and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, SR238 can be considered as one of the options for reactive compounds.

[0056] Take 0.25 g of the compound SR601 (purchased from Sartomer AMERICAS, its structure is as follows) Where a = 2–6 and b = 2–6, the mixture, after being mixed with a dispersion containing 1 g of the modified particles from Synthesis Example 1, remained in a phase-free liquid state without precipitation. As can be seen from the above, the aforementioned multi-double-bond compound SR601 is compatible with the modified particles. The above solution can be coated and cured by heat (baking at 80°C for 10 minutes and at 120°C for 10 minutes) to form a 5-micrometer-thick dry film. In conclusion, SR601 can be considered as one of the options for reactive compounds.

[0057] Example 1

[0058] A dispersion containing 8 parts by weight of the modified particles from Synthesis Example 1, 1 part by weight of the silicon-free polyepoxide compound HDGE, and 1 part by weight of the silicon-containing polyepoxide compound SIB-1110 were mixed. 3 parts by weight of the solvent were then removed to form a solution with a viscosity of 30.3 cP at 25°C. This solution was then applied as a coating material to a 50-micrometer-thick wet film on a glass substrate using a doctor blade. The film was then heat-cured (80°C for 10 minutes and 120°C for 10 minutes) to form a 20-micrometer-thick coating. The coating exhibited a transmittance of 96.1%, a haze of 1.91 (haze-light scattering value), and a refractive index of 2.01 for light with a wavelength of 550 nm.

[0059] Example 2

[0060] A dispersion containing 7 parts by weight of the modified particles from Synthesis Example 1, 1.8 parts by weight of the silicon-free polyepoxide compound HDGE, and 1.2 parts by weight of the silicon-containing polyepoxide compound SIB-1110 were mixed. 3 parts by weight of the solvent were removed to form a solution with a viscosity of 35.6 cP at 25°C, which was then used as a coating. This solution was applied as a 50-micrometer-thick wet film onto a glass substrate using a doctor blade and cured by baking (at 80°C for 10 minutes and then at 120°C for 10 minutes) to form a 22-micrometer-thick coating. The coating had a transmittance of 97.0%, a haze of 1.03 (haze-light scattering value), and a refractive index of 1.85 for light with a wavelength of 550 nm. Subsequent transmittance testing at 110°C for 500 hours showed a change rate ≤1.61%.

[0061] Example 3

[0062] A dispersion containing 7 parts by weight of the modified particles from Synthesis Example 1, 1.5 parts by weight of the silicon-free polyepoxide compound HDGE, and 1.5 parts by weight of the silicon-containing polyepoxide compound SIB-1110 were mixed. 3 parts by weight of the solvent were removed to form a solution with a viscosity of 32.3 cP at 25°C. This solution was then used as a coating material and applied as a 50-micrometer-thick wet film onto a glass substrate using a doctor blade. The film was then heat-cured (80°C for 10 minutes and 120°C for 10 minutes) to form a 21-micrometer-thick coating. The coating had a transmittance of 96.7%, a haze of 1.33 (haze-light scattering value), and a refractive index of 1.88 for light with a wavelength of 550 nm.

[0063] Example 4

[0064] A dispersion containing 6 parts by weight of the modified particles from Synthesis Example 1, 2 parts by weight of the silicon-free polyepoxide compound HDGE, and 2 parts by weight of the silicon-containing polyepoxide compound SIB-1110 were mixed. 3 parts by weight of the solvent were then removed to form a solution with a viscosity of 41.0 cP at 25°C. This solution was used as a coating material and applied as a 50-micrometer-thick wet film onto a glass substrate using a doctor blade. The film was then heat-cured (80°C for 10 minutes and 120°C for 10 minutes) to form a 30-micrometer-thick coating. The coating had a transmittance of 95.6%, a haze of 1.10 (haze-light scattering value), and a refractive index of 1.80 for light with a wavelength of 550 nm.

[0065] Example 5

[0066] A dispersion containing 7 parts by weight of the modified particles from Synthesis Example 3, 1.5 parts by weight of the silicon-free polyepoxide compound HDGE, and 1.5 parts by weight of the silicon-containing polyepoxide compound SIB-1110 were mixed. 3 parts by weight of the solvent were removed to form a solution with a viscosity of 5.1 cP at 25°C. This solution was then applied as a coating material to a 50-micrometer-thick wet film on a glass substrate using a doctor blade. The film was then heat-cured (80°C for 10 minutes and 120°C for 10 minutes) to form a 23-micrometer-thick coating. The coating exhibited a transmittance of 96.3%, a haze of 0.71 (haze-light scattering value), and a refractive index of 1.87 for light with a wavelength of 550 nm.

[0067] Example 6

[0068] A dispersion containing 5 parts by weight of the modified particles from Synthesis Example 1, 2.5 parts by weight of the silicon-free polyepoxide compound HDGE, and 2.5 parts by weight of the silicon-containing polyepoxide compound SIB-1110 were mixed. 3 parts by weight of the solvent were then removed to form a solution with a viscosity of 48 cP at 25°C. This solution was then applied as a coating to a 50-micrometer-thick wet film on a glass substrate using a doctor blade. The film was then heat-cured (80°C for 10 minutes and 120°C for 10 minutes) to form a 36-micrometer-thick coating. The coating exhibited a transmittance of 98.9%, a haze of 1.54 (haze-light scattering value), and a refractive index of 1.77 for light with a wavelength of 550 nm.

[0069] Comparative Example 1

[0070] A dispersion containing 9 parts by weight of the modified particles of Synthesis Example 1, 0.5 parts by weight of the non-silicone polyepoxide HDGE, and 0.5 parts by weight of the silicon-containing polyepoxide SIB-1110 were mixed. 3 parts by weight of the solvent were removed to form a coating. The coating was then applied as a 50-micron-thick wet film onto a glass substrate using a doctor blade. During heat curing (baking at 80°C for 10 minutes and at 120°C for 10 minutes), the coating cracked.

[0071] Comparative Example 2

[0072] A dispersion containing 7 parts by weight of the modified particles from Synthetic Example 1 was mixed with 3 parts by weight of the silicone-free polyepoxide compound HDGE. 3 parts by weight of the solvent were then removed to form a coating. This coating was applied as a 50-micron-thick wet film onto a glass substrate using a doctor blade and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a coating layer. The coating's transmittance was <80%.

[0073] Comparative Example 3

[0074] A dispersion containing 7 parts by weight of the modified particles from Synthesis Example 1, 2.4 parts by weight of the silicone-free polyepoxide compound HDGE, and 0.6 parts by weight of the silicone-containing polyepoxide compound SIB-1110 were mixed. 3 parts by weight of the solvent were then removed to form a coating. This coating was applied as a 50-micron-thick wet film onto a glass substrate using a doctor blade and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a coating layer. The coating's transmittance was <80%.

[0075] Comparative Example 4

[0076] A dispersion containing 7 parts by weight of the modified particles from Synthesis Example 1, 1.2 parts by weight of the silicon-free polyepoxide HDGE, and 1.8 parts by weight of the silicon-containing polyepoxide SIB-1110 were mixed. 3 parts by weight of the solvent were then removed to form a coating. This coating was applied as a 50-micron-thick wet film onto a glass substrate using a doctor blade and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a coating layer. The coating layer exhibited cracking after being left at room temperature for a period of time.

[0077] Comparative Example 5

[0078] A dispersion containing 7 parts by weight of the modified particles from Synthesis Example 1, 0.6 parts by weight of the silicon-free polyepoxide HDGE, and 2.4 parts by weight of the silicon-containing polyepoxide SIB-1110 were mixed. 3 parts by weight of the solvent were then removed to form a coating. This coating was applied as a 50-micron-thick wet film onto a glass substrate using a doctor blade and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a coating layer. The coating layer exhibited cracking after being left at room temperature for a period of time.

[0079] Comparative Example 6

[0080] A dispersion containing 7 parts by weight of the modified particles from Synthesis Example 1 and 3 parts by weight of the silicon-containing polyepoxide compound SIB-1110 were mixed. 3 parts by weight of the solvent were then removed to form a coating. This coating was applied as a 50-micron-thick wet film onto a glass substrate using a doctor blade and cured by heat (80°C for 10 minutes and 120°C for 10 minutes) to form a coating layer. The coating layer exhibited cracking after being left at room temperature for a period of time.

[0081] Comparative Example 7

[0082] A dispersion containing 7 parts by weight of the core (unmodified) of Synthesis Example 1, 1.5 parts by weight of the non-silicone polyepoxide compound HDGE, and 1.5 parts by weight of the silicon-containing polyepoxide compound SIB-1110 were mixed. 3 parts by weight of the solvent were removed to form a coating. The coating was then applied as a 50-micron-thick wet film onto a glass substrate using a doctor blade. During heat curing (baking at 80°C for 10 minutes and at 120°C for 10 minutes), the coating cracked.

[0083] Example 7

[0084] A dispersion containing 8 parts by weight of the modified particles from Synthesis Example 4, 2 parts by weight of the multi-double-bond compound SR238, and 0.01 parts by weight of the initiator azobisisobutyronitrile (AIBN) was mixed. 3 parts by weight of the solvent were then removed to form a solution with a viscosity of 6.8 cP at 25°C. This solution was then applied as a coating to a 50-micron-thick wet film on a glass substrate using a doctor blade. After baking at 80°C for 10 minutes, it was UV cured (1500 J / cm²). 2In 1 minute, a 21-micron-thick coating is formed. The coating has a transmittance of 95.8%, a haze of 1.91 (haze-light scattering value), and a refractive index of 1.88 for light with a wavelength of 550 nm.

[0085] Example 8

[0086] A dispersion containing 7 parts by weight of the modified particles from Synthesis Example 4, 3 parts by weight of the multi-double-bond compound SR238, and 0.01 parts by weight of the initiator azobisisobutyronitrile (AIBN) was mixed. 3 parts by weight of the solvent were then removed to form a solution with a viscosity of 5.9 cP at 25°C. This solution was then applied as a coating to a 50-micron-thick wet film on a glass substrate using a doctor blade. After baking at 80°C for 10 minutes, it was UV cured (1500 J / cm²). 2 In 1 minute, a 22-micrometer-thick coating is formed. The coating has a transmittance of 96.3%, a haze of 1.82 (haze-light scattering value), and a refractive index of 1.82 for light with a wavelength of 550 nm.

[0087] Example 9

[0088] A dispersion containing 6 parts by weight of the modified particles from Synthesis Example 4, 4 parts by weight of the multi-double-bond compound SR238, and 0.01 parts by weight of the initiator azobisisobutyronitrile (AIBN) was prepared by removing 3 parts by weight of solvent to form a solution with a viscosity of 6.5 cP at 25°C. This solution was then coated onto a glass substrate as a 50-micron-thick wet film using a doctor blade. After baking at 80°C for 10 minutes, it was UV cured (1500 J / cm²). 2 In 1 minute, a 23-micrometer-thick coating is formed. The coating has a transmittance of 96.9%, a Hz of 1.72 (haze-light scattering value), and a refractive index of 1.80 for light with a wavelength of 550 nm.

[0089] Example 10

[0090] A dispersion containing 5 parts by weight of the modified particles from Synthesis Example 4, 5 parts by weight of the multi-double-bond compound SR238, and 0.01 parts by weight of the initiator azobisisobutyronitrile (AIBN) was mixed. 3 parts by weight of the solvent were removed to form a solution with a viscosity of 6.1 cP at 25°C, which was then used as a coating. This solution was applied as a 50-micron-thick wet film onto a glass substrate using a doctor blade. After baking at 80°C for 10 minutes, it was UV cured (1500 J / cm²). 2 In 1 minute, a 23-micrometer-thick coating is formed. The coating has a transmittance of 98.2%, a Hz of 1.4 (haze-light scattering value), and a refractive index of 1.75 for light with a wavelength of 550 nm.

[0091] Comparative Example 8

[0092] Take a dispersion containing 9 parts by weight of the modified particles from Synthetic Example 4, 1 part by weight of the multi-double-bond compound SR238, and 0.01 parts by weight of the initiator azobisisobutyronitrile (AIBN), remove 3 parts by weight of solvent to form a coating, bake at 80°C for 10 minutes, and then UV cure (1500 J / cm). 2 The coating cracked after 1 minute.

[0093] Example 11

[0094] A dispersion containing 8 parts by weight of the modified particles from Synthesis Example 5, 1.5 parts by weight of the silicon-free polyepoxide compound HDGE, and 1.5 parts by weight of the silicon-containing polyepoxide compound SIB-1110 were mixed. 3 parts by weight of the solvent were removed to form a solution with a viscosity of 46.7 cP at 25°C, which was then used as a coating. This solution was applied as a 50-micrometer-thick wet film onto a glass substrate using a doctor blade and cured by baking (at 80°C for 10 minutes and at 120°C for 10 minutes) to form a 25-micrometer-thick coating. The coating had a transmittance of 97.1%, a haze of 0.47 (haze-light scattering value), and a refractive index of 1.82 for light with a wavelength of 550 nm.

[0095] Although this disclosure has been presented above with reference to several preferred embodiments, it is not intended to limit the scope of this disclosure. Anyone skilled in the art can make any modifications and alterations without departing from the spirit and scope of this disclosure. Therefore, the scope of protection of this disclosure shall be determined by the appended claims.

Claims

1. A coating comprising: Modified particles, including: Core; and Silane coupling agents with epoxy groups or silane coupling agents with double bonds are grafted onto the surface of the core. The core comprises (1) an oxide of zinc and titanium, wherein the weight ratio of zinc to titanium is 1:0.4 to 1:0.9; (2) an oxide of zirconium and titanium, wherein the weight ratio of zirconium to titanium is 1:0.1 to 1:2; or (3) an oxide of zinc and zirconium, wherein the weight ratio of zinc to zirconium is 1:0.8 to 1:2; and Reactive compounds, When the epoxy-based silane coupling agent is grafted onto the surface of the core, the reactive compound includes both silicon-free and silicon-containing polyepoxides. The silicon-free polyepoxide compound includes , , , , k = 1~6, or a combination thereof; The silicon-containing polyepoxide compound includes , Where m = 1~6 and n = 1~6, , Where n = 1~6, or a combination thereof, When the silane coupling agent with double bonds is grafted onto the surface of the core, the reactive compound includes compounds with multiple double bonds. The multi-double-bond compound includes , , where a=2~6 and b=2~6, or a combination thereof.

2. The coating of claim 1, wherein the total weight of zinc and titanium, zirconium and titanium, or zinc and zirconium in the core is in a weight ratio of 1:0.1 to 1:3 to the epoxy-based silane coupling agent or the double-bonded silane coupling agent.

3. The coating of claim 1, wherein the average particle size of the core is 10 nm to 120 nm.

4. The coating of claim 1, wherein the epoxy-containing silane coupling agent comprises 3-glycidyl etheroxypropyltrimethoxysilane, 3-glycidyl etheroxypropyltriethoxysilane, 3-glycidyl etheroxypropylmethyldimethoxysilane, 3-glycidyl etheroxypropylmethyldiethoxysilane, 2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane, or 2-(3,4-epoxycyclohexyl)ethyltriethoxysilane.

5. The coating of claim 1, wherein the silane coupling agent having double bonds comprises propyl 3-trimethoxysilane acrylate, 3-(triethoxysilyl)propyl isocyanate, or , where R is methyl or ethyl, and n = 1-3.

6. The coating of claim 1, wherein the weight ratio of the core to the reactive compound is from 1:0.2 to 1:0.

8.

7. The coating of claim 1, wherein the weight ratio of the silicon-free polyepoxide to the silicon-containing polyepoxide is from 1:0.4 to 1:

1.

8. A coating formed by reacting the coating of claim 1.

9. The coating of claim 8, wherein the coating has a thickness of 20 micrometers to 40 micrometers, a refractive index of 1.7 to 2.4, and a transmittance of 90% to 99.5%.

10. A light-emitting device, comprising: substrate; The light-emitting unit is located on the substrate; as well as The coating as described in claim 8 covers the substrate and the light-emitting unit.

11. The light-emitting device of claim 10, wherein the coating has a thickness of 20 micrometers to 40 micrometers, a refractive index of 1.7 to 2.4, and a transmittance of 90% to 99.5%.

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