Organic silicon optical adhesive composition, integrated black organic silicon optical transparent adhesive film, and preparation method and application of integrated black organic silicon optical transparent adhesive film

Abstract

The invention relates to an organic silicon optical adhesive composition, an integrated black organic silicon optical transparent adhesive film and a preparation method and application of the integrated black organic silicon optical transparent adhesive film, and the organic silicon optical adhesive composition is prepared from, by weight, 20-70 parts of vinyl silicone oil, 1-25 parts of vinyl silicone resin, 0.1-5 parts of modified graphene oxide slurry and 15-60 parts of hydrogen-containing silicone oil. 0.1 to 10 parts of hydrogen-containing silicon resin; preparation raw materials of the modified graphene oxide slurry comprise a modifier and graphene oxide, the modifier comprises silane and / or polysiloxane, and modification groups contained in the modifier comprise epoxy groups and / or carboxyl groups. The organic silicon optical adhesive composition provided by the invention has good compatibility, dispersibility and storage stability, effectively solves the problems that the existing optical adhesive composition is poor in light transmission and easy to generate stripes and patterns, has a good integrated black display effect, and is widely applied to the field of optical display lamination.

Description

Technical Field

[0001] The present invention relates to the technical field of adhesives, and in particular to an organic silicon optical adhesive composition, an integrated black organic silicon optical transparent adhesive film, and a preparation method and application thereof. Background Art

[0002] Optical Clear Adhesive (OCA) is an important special adhesive with silicone compounds as the main ingredient, which can be used to bond transparent optical components. It has good bonding properties, excellent high temperature resistance, chemical corrosion resistance, high transparency, anti-yellowing performance and strong hot and cold stability. It is currently widely used in the field of optical display bonding, especially in the automotive display industry with good market prospects.

[0003] At present, most of the in-vehicle display screens on the market have a certain color difference after being turned off due to the lighter color of the border, which cannot be consistent with the overall color of the display screen, affecting the visual effect. The integrated black display technology aims to achieve that when the display screen is off, the color difference between the display area and the edge ink area is difficult to distinguish with the naked eye, so that the in-vehicle display or smart terminal can be visually integrated with the environment, thereby enhancing the beauty and high-end feel of the product. Generally, this can be achieved by selecting the components of the display screen or controlling the process, such as the selection of TFT display screen, polarizer, bonding glue and frame ink, or the control of bonding method, coating method and other processes.

[0004] In existing research, in order to achieve the integrated black effect of the display screen, the method of adding carbon black or carbon black slurry to the optical adhesive composition is often used. For example, CN112708396A discloses the preparation of an integrated black silicone OCA, including vinyl silicone oil, tackifier, cross-linking agent, solvent, carbon black pigment, catalyst and inhibitor. However, since carbon black is easy to agglomerate and has high surface energy, it will cause problems such as carbon black agglomeration, uneven dispersion and even sedimentation in the optical adhesive liquid within a short period of time after the preparation is completed, resulting in the overall appearance of the optical adhesive layer produced by the later coating showing regional color difference, color, cross-sectional lines and other undesirable phenomena. In addition, during the coating and curing process of the OCA optical adhesive, carbon black is easy to settle to the surface of the colloid, resulting in the deterioration of the bonding performance and aging reliability of the OCA optical adhesive. Not only that, carbon black has a high light-shielding property, and adding it to the optical adhesive will cause the light transmittance of the colloid to decrease, thereby resulting in a loss of the display effect of the display screen.

[0005] Therefore, how to provide a silicone optical adhesive composition and adhesive film with good light transmittance, low haze, easy dispersion, storage stability, good adhesion and strong aging reliability is a technical problem that needs to be solved in the current field. Summary of the invention

[0006] In view of the above problems, the purpose of the present invention is to provide a silicone optical adhesive composition, an integrated black silicone optical transparent adhesive film and a preparation method and application thereof. Compared with the prior art, the silicone optical adhesive composition provided by the present invention has good compatibility, dispersibility, storage stability and coating uniformity, effectively solving the problems of poor light transmittance and easy appearance of stripes and patterns in the existing optical adhesive compositions, having a good integrated black display effect, and is widely applicable to the field of optical display bonding.

[0007] In order to achieve the purpose of the invention, the present invention adopts the following technical solutions:

[0008] In a first aspect, the present invention provides an organic silicone optical adhesive composition, wherein the raw materials for preparing the organic silicone optical adhesive composition include the following components in parts by weight:

[0009]

[0010]

[0011] The raw materials for preparing the modified graphene oxide slurry include a modifier and graphene oxide;

[0012] The modifier includes silane and / or polysiloxane;

[0013] The modifying group contained in the modifying agent includes an epoxy group and / or a carboxyl group.

[0014] The organic silicone optical adhesive composition provided by the present invention is compounded with components such as vinyl silicone oil, vinyl silicone resin, modified graphene oxide slurry, hydrogen-containing silicone oil and hydrogen-containing silicone resin. The obtained organic silicone optical adhesive composition has good compatibility, dispersibility, storage stability and coating uniformity, and also has excellent bonding properties, optical properties, mechanical properties and aging reliability.

[0015] It is worth noting that the modified graphene oxide slurry used in the present invention is made of graphene oxide and silane or polysiloxane, and the graphene oxide surface has more active functional groups (such as hydroxyl, carboxyl, carbonyl, etc.), which can react with the epoxy / carboxyl group in silane or polysiloxane to obtain modified graphene oxide slurry. In the first aspect, the modified graphene oxide provided by the present invention has strong light transmittance compared with carbon black, so it has significant advantages in optical properties, and can make the organic silicon optical adhesive composition have excellent optical transmittance, with high transmittance and low haze characteristics, and is used in the field of vehicle-mounted display screens to improve its visual effect; in the second aspect, the present invention can achieve better compatibility and dispersibility with components such as vinyl silicone oil, vinyl silicone resin, hydrogen-containing silicone oil and hydrogen-containing silicone resin by grafting siloxane segments on the surface of graphene oxide compared with other organic functional groups, thereby improving the problems of agglomeration, uneven dispersion and even sedimentation caused by directly adding graphene oxide or carbon powder.

[0016] In the present invention, the raw materials for preparing the organic silicone optical adhesive composition include, by weight, 20-70 parts of vinyl silicone oil, for example, 20 parts, 25 parts, 30 parts, 35 parts, 40 parts, 45 parts, 50 parts, 55 parts, 60 parts, 65 parts or 70 parts, but not limited to the listed values, and other values ​​not listed in the numerical range are also applicable; 1-25 parts of vinyl silicone resin, for example, 1 part, 2 parts, 4 parts, 6 parts, 8 parts, 10 parts, 12 parts, 14 parts, 16 parts, 18 parts, 20 parts, 22 parts or 25 parts, but not limited to the listed values, and other values ​​not listed in the numerical range are also applicable; 0.1 parts of modified graphene oxide slurry -5 parts, for example, it can be 0.1 parts, 1 parts, 2 parts, 3 parts, 4 parts or 5 parts, but not limited to the listed values, and other values ​​not listed in the numerical range are equally applicable; 15-60 parts of hydrogen-containing silicone oil, for example, it can be 15 parts, 20 parts, 25 parts, 30 parts, 35 parts, 40 parts, 45 parts, 50 parts, 55 parts or 60 parts, but not limited to the listed values, and other values ​​not listed in the numerical range are equally applicable; 0.1-10 parts of hydrogen-containing silicone resin, for example, it can be 0.1 parts, 1 parts, 2 parts, 3 parts, 4 parts, 5 parts, 6 parts, 7 parts, 8 parts, 9 parts or 10 parts, but not limited to the listed values, and other values ​​not listed in the numerical range are equally applicable.

[0017] Preferably, the thickness of the graphene oxide is 0.5-10 nm, for example, 0.5 nm, 1 nm, 2 nm, 3 nm, 4 nm, 5 nm, 6 nm, 7 nm, 8 nm, 9 nm or 10 nm, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0018] Preferably, the silane comprises epoxy silane and / or carboxylic acid silane.

[0019] Preferably, the epoxy silane includes any one of γ-glycidyloxypropyltrimethoxysilane, γ-glycidyloxypropyltriethoxysilane or γ-glycidyloxypropyldimethoxyethoxysilane or a combination of at least two thereof.

[0020] Preferably, the polysiloxane includes any one of terminal carboxyl polysiloxane, terminal epoxy polysiloxane, pendant carboxyl polysiloxane or pendant epoxy polysiloxane, or a combination of at least two thereof.

[0021] Preferably, the weight average molecular weight of the polysiloxane is 1000-100000, for example, it can be 1000, 10000 or 100000, but it is not limited to the listed values, and other values ​​not listed in the numerical range are also applicable; the viscosity at 25°C is 100-5000mPa·s, for example, it can be 100mPa·s, 1000mPa·s or 5000mPa·s, but it is not limited to the listed values, and other values ​​not listed in the numerical range are also applicable; the content of epoxy or carboxyl is 0.1-0.5mmol / g, for example, it can be 0.1mmol / g, 0.2mmol / g, 0.4mmol / g or 0.5mmol / g, but it is not limited to the listed values, and other values ​​not listed in the numerical range are also applicable.

[0022] Preferably, the solid content of the modified graphene oxide slurry is 50-80%, for example, it can be 50%, 52%, 54%, 56%, 58%, 60%, 62%, 64%, 66%, 68%, 70%, 72%, 74%, 76%, 78% or 80%, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0023] Preferably, the modifier comprises carboxylic acid silane and / or carboxyl-containing polysiloxane, preferably carboxyl-containing polysiloxane.

[0024] In the present invention, compared with epoxy silane, carboxylic acid silane has low toxicity and better biocompatibility, which improves the safety of the reaction. In addition, the currently commonly used isocyanate silane and amino silane will introduce secondary amine groups after modification, and the secondary amine groups will poison the platinum catalyst in the silicone optical adhesive composition and make it difficult to cure. However, the present invention uses carboxylic acid silane modification and does not have the above problems.

[0025] Furthermore, graphene modified by small molecule silane and polysiloxane can achieve an integrated black effect when added to optical adhesive, but the long flexible siloxane segments on the surface of graphene oxide and the macromolecules of optical adhesive are intertwined with each other, which can further reduce the sedimentation of graphene oxide and enhance the flexibility of the colloid. However, graphene oxide modified by small molecule carboxyl silane has a large amount of alkoxy groups remaining, which will absorb water vapor in the air and increase the haze of the optical adhesive. Therefore, the use of carboxyl polysiloxane to modify graphene oxide is the preferred solution of the present invention.

[0026] Preferably, in the raw material for preparing the modified graphene oxide slurry, the molar ratio of hydroxyl groups contained in graphene oxide to modifying groups contained in the modifier is 1:(1.1-3), for example, it can be 1:1.1, 1:1.2, 1:1.5, 1:1.8, 1:2, 1:2.2, 1:2.5, 1:2.8 or 1:3, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0027] In the present invention, by preferably controlling the molar ratio of the hydroxyl group contained in the graphene oxide to the modified group (i.e., carboxyl or epoxy group) contained in the modifier, a modified graphene oxide slurry having good compatibility with the silicone optical adhesive composition and good viscosity-increasing effect can be obtained. It should be noted that, on the one hand, if the molar ratio of the hydroxyl group to the carboxyl group or epoxy group is too high, the content of siloxane grafted onto the graphene oxide is low, and it is difficult to improve the compatibility, and agglomeration is easy to occur. On the other hand, if the molar ratio of the hydroxyl group to the carboxyl group or epoxy group is too low, there are too many small molecule carboxyl silanes that do not participate in the modification reaction, which will precipitate from the system, and the bonding performance will decrease. The carboxyl polysiloxane that does not participate in the modification reaction acts like a plasticizer in the optical adhesive, affecting the colloidal cohesive strength of the optical adhesive, thereby reducing the bonding performance.

[0028] Preferably, the raw materials for preparing the modified graphene oxide slurry also include a diluent.

[0029] Preferably, the diluent comprises toluene.

[0030] Preferably, the method for preparing the modified graphene oxide slurry comprises the following steps:

[0031] (1) performing a first mixing of graphene oxide and a diluent, then adding a modifier, adjusting the pH value to 4-6, performing a second mixing, and then reacting to obtain a modified graphene oxide mixed solution;

[0032] (2) Grinding the modified graphene oxide mixed solution obtained in step (1) to obtain the modified graphene oxide slurry.

[0033] Preferably, the first mixing time in step (1) is 1-10 min, for example, 1 min, 2 min, 3 min, 4 min, 5 min, 6 min, 7 min, 8 min, 9 min or 10 min, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0034] Preferably, the second mixing time is 1-30 min, for example, it can be 1 min, 2 min, 4 min, 6 min, 8 min, 10 min, 12 min, 14 min, 16 min, 18 min, 20 min, 22 min, 24 min, 26 min, 28 min or 30 min, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0035] Preferably, the temperature of the first mixing and the second mixing is independently 40-45°C, for example, 40°C, 41°C, 42°C, 43°C, 44°C or 45°C, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0036] Preferably, the reaction temperature is 60-90°C, for example, it can be 60°C, 62°C, 64°C, 66°C, 68°C, 70°C, 72°C, 74°C, 76°C, 78°C, 80°C, 82°C, 84°C, 86°C, 88°C or 90°C, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0037] Preferably, the reaction time is 3-6 h, for example, 3 h, 3.5 h, 4 h, 4.5 h, 5 h, 5.5 h or 6 h, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0038] Preferably, the grinding media used in the grinding in step (2) includes zirconium oxide beads.

[0039] Preferably, the particle size of the grinding medium is 0.1-2 mm, for example, it can be 0.1 mm, 0.2 mm, 0.4 mm, 0.6 mm, 0.8 mm, 1 mm, 1.2 mm, 1.4 mm, 1.6 mm, 1.8 mm or 2 mm, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0040] Preferably, the grinding time is 1-3 h, for example, 1 h, 1.5 h, 2 h, 2.5 h or 3 h, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0041] Preferably, the grinding rotation speed is 100-200rpm, for example, it can be 100rpm, 110rpm, 120rpm, 130rpm, 140rpm, 150rpm, 160rpm, 170rpm, 180rpm, 190rpm or 200rpm, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0042] Preferably, the method for preparing the modified graphene oxide slurry specifically comprises the following steps:

[0043] (1) mixing graphene oxide and a diluent for a first time for 1-10 minutes, then adding a modifier, adjusting the pH value to 4-6, performing a second mixing for 1-30 minutes, and then reacting at a temperature of 60-90° C. for 3-6 hours to obtain a modified graphene oxide mixed solution;

[0044] (2) Grinding the modified graphene oxide mixed solution obtained in step (1) with zirconium oxide beads having a particle size of 0.1-2 mm at a rotation speed of 100-200 rpm for 1-3 h to obtain the modified graphene oxide slurry.

[0045] Preferably, the vinyl silicone oil includes any one or a combination of at least two of silicone oil containing vinyl groups at the terminal, silicone oil containing vinyl groups at the side groups, or silicone oil containing vinyl groups at both the terminal and the side groups.

[0046] Preferably, the viscosity of the vinyl silicone oil at 25°C is 100-25000 mPa·s, for example, it may be 100 mPa·s, 500 mPa·s, 1000 mPa·s, 2000 mPa·s, 4000 mPa·s, 6000 mPa·s, 8000 mPa·s, 10000 mPa·s, 12000 mPa·s, 14000 mPa·s, 16000 mPa·s, 18000 mPa·s, 20000 mPa·s, 22000 mPa·s or 25000 mPa·s, but is not limited to the listed values, and other unlisted values ​​within the numerical range are equally applicable.

[0047] Preferably, the vinyl content in the vinyl silicone oil is 0.1-0.75 mmol / g, for example, it can be 0.1 mmol / g, 0.2 mmol / g, 0.3 mmol / g, 0.4 mmol / g, 0.5 mmol / g, 0.6 mmol / g, 0.7 mmol / g or 0.75 mmol / g, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0048] Preferably, the viscosity of the vinyl silicone resin at 25°C is 5000-50000 mPa·s, for example, it may be 5000 mPa·s, 8000 mPa·s, 10000 mPa·s, 15000 mPa·s, 20000 mPa·s, 25000 mPa·s, 30000 mPa·s, 35000 mPa·s, 40000 mPa·s, 45000 mPa·s or 50000 mPa·s, but is not limited to the listed values, and other unlisted values ​​within the numerical range are equally applicable.

[0049] Preferably, the vinyl content in the vinyl silicone resin is 0.2-1.0 mmol / g, for example, it can be 0.2 mmol / g, 0.3 mmol / g, 0.4 mmol / g, 0.5 mmol / g, 0.6 mmol / g, 0.7 mmol / g, 0.8 mmol / g or 1 mmol / g, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0050] Preferably, the weight average molecular weight of the hydrogen-containing silicone oil is 1000-200000, for example, it can be 1000, 5000, 8000, 10000, 20000, 40000, 60000, 80000, 100000, 120000, 140000, 160000, 180000 or 200000, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0051] Preferably, the silicon-hydrogen bond content of the hydrogen-containing silicone oil is 0.4-0.8 mmol / g, for example, 0.4 mmol / g, 0.5 mmol / g, 0.6 mmol / g, 0.7 mmol / g or 0.8 mmol / g, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0052] Preferably, the viscosity of the hydrogenated silicone resin at 25° C. is 30,000-40,000 mPa·s, for example, 30,000 mPa·s, 32,000 mPa·s, 34,000 mPa·s, 36,000 mPa·s, 38,000 mPa·s or 40,000 mPa·s, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0053] Preferably, the silicon-hydrogen bond content of the hydrogen-containing silicone resin is 0.4-0.8 mmol / g, for example, 0.4 mmol / g, 0.5 mmol / g, 0.6 mmol / g, 0.7 mmol / g or 0.8 mmol / g, but is not limited to the listed values, and other values ​​not listed within the numerical range are also applicable.

[0054] Preferably, the raw materials for preparing the organic silicone optical adhesive composition also include a catalyst.

[0055] Preferably, the raw materials for preparing the silicone optical adhesive composition include 0.0001-0.1 parts of catalyst by weight, for example, it can be 0.0001 parts, 0.0002 parts, 0.0005 parts, 0.0008 parts, 0.001 parts, 0.002 parts, 0.005 parts, 0.008 parts, 0.01 parts, 0.02 parts, 0.05 parts, 0.08 parts or 0.1 parts, but is not limited to the listed values, and other values ​​not listed within the numerical range are also applicable.

[0056] Preferably, in the raw materials for preparing the organic silicone optical adhesive composition, the catalyst includes any one of chloroplatinic acid isopropanol solution, Karstedt platinum catalyst, Willing platinum catalyst, (trimethyl) methylcyclopentadiene platinum or acetylacetonate platinum, or a combination of at least two thereof.

[0057] Preferably, the raw materials for preparing the organic silicone optical adhesive composition further include an inhibitor.

[0058] Preferably, the raw materials for preparing the organic silicone optical adhesive composition include 0.0001-1 parts of inhibitors by weight, for example, it can be 0.0001 parts, 0.0005 parts, 0.0008 parts, 0.001 parts, 0.005 parts, 0.008 parts, 0.01 parts, 0.02 parts, 0.05 parts, 0.08 parts, 0.1 parts, 0.2 parts, 0.5 parts, 0.8 parts or 1 parts, but is not limited to the listed values, and other values ​​not listed within the numerical range are equally applicable.

[0059] Preferably, the inhibitor comprises any one of alkynol substances, vinyl ring bodies or maleate substances, or a combination of at least two of them.

[0060] In the present invention, the acetylene alcohol substance, vinyl ring body or maleate substance in the inhibitor can adopt any corresponding substance used for inhibitors in the art. For example, the acetylene alcohol substance can be any one of 1,4-butynediol, ethynyl cyclohexanol or 2-methyl-3-butyn-2-ol or a combination of at least two thereof; the vinyl ring body includes tetramethyltetravinylcyclotetrasiloxane.

[0061] Preferably, the raw materials for preparing the organic silicone optical adhesive composition include the following components in parts by weight:

[0062]

[0063] In the present invention, the preparation method of the organic silicone optical adhesive composition comprises the following steps:

[0064] Vinyl silicone resin, vinyl silicone oil, hydrogen-containing silicone oil, hydrogen-containing silicone resin, modified graphene oxide slurry, catalyst and inhibitor are mixed according to the formula, and stirred and vacuum degassed in sequence to obtain an organic silicone optical adhesive composition.

[0065] In a second aspect, the present invention provides an integrated black organosilicon optically transparent adhesive film, wherein the integrated black organosilicon optically transparent adhesive film comprises a first release film, an optical adhesive layer, and a second release film which are sequentially stacked;

[0066] The optical adhesive layer is obtained by curing the organic silicon optical adhesive composition described in the first aspect of the present invention.

[0067] In the integrated black organic silicone optical transparent adhesive film provided by the present invention, a laminated structure of a first release film, an optical adhesive layer and a second release film is set, and the optical adhesive layer obtained by curing the organic silicone optical adhesive composition described in the first aspect of the present invention has good bonding properties, optical properties, mechanical properties and aging reliability, and has good optical transmittance.

[0068] Preferably, the thickness of the optical adhesive layer is 25-2000μm, for example, it can be 25μm, 50μm, 80μm, 100μm, 200μm, 400μm, 600μm, 800μm, 1000μm, 1200μm, 1400μm, 1600μm, 1800μm or 2000μm, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0069] Preferably, the first release film and the second release film are independently selected from any one of a non-silicone release film and a fluorosilicone release film.

[0070] Preferably, the thickness of the first release film is 25-100 μm, for example, it can be 25 μm, 30 μm, 35 μm, 40 μm, 45 μm, 50 μm, 55 μm, 60 μm, 65 μm, 70 μm, 75 μm, 80 μm, 85 μm, 90 μm, 95 μm or 100 μm, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0071] Preferably, the thickness of the second release film is 50-200 μm, for example, 50 μm, 80 μm, 100 μm, 120 μm, 140 μm, 160 μm, 180 μm or 200 μm, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0072] Preferably, the absolute value of the difference in release force between the first release film and the second release film is 5-30 gf / inch, for example, it can be 5 gf / inch, 8 gf / inch, 10 gf / inch, 12 gf / inch, 15 gf / inch, 18 gf / inch, 20 gf / inch, 22 gf / inch, 25 gf / inch, 28 gf / inch or 30 gf / inch, but is not limited to the listed values, and other values ​​not listed within the numerical range are also applicable.

[0073] In a third aspect, the present invention provides a method for preparing the integrated black organic silicone optically transparent adhesive film as described in the second aspect of the present invention, the preparation method comprising the following steps:

[0074] (a) coating one side of a first release film with the organosilicon optical adhesive composition according to the first aspect of the present invention, and then curing the same to obtain an optical adhesive layer;

[0075] (b) Laying a second release film on the side of the optical adhesive layer in step (a) away from the first release film to obtain the integrated black organic silicone optical transparent adhesive film.

[0076] In the preparation method provided by the present invention, by adopting coating, curing, lamination and other processes, an integrated black organic silicone optical transparent adhesive film with good bonding properties, optical properties, mechanical properties and aging reliability can be prepared, wherein after laminating the second release film, the subsequent processing technology can be designed and selected according to needs, such as subsequent striping, winding and other steps to obtain an integrated black organic silicone optical transparent adhesive film.

[0077] Preferably, the coating method in step (a) includes any one of slit coating, double-roller coating, comma blade coating, anilox coating or micro-concave coating, or a combination of at least two thereof.

[0078] Preferably, the curing temperature in step (a) is 60-100°C, for example, 60°C, 65°C, 70°C, 75°C, 80°C, 85°C, 90°C, 95°C or 100°C, but is not limited to the listed values, and other unlisted values ​​within the numerical range are also applicable.

[0079] In a fourth aspect, the present invention provides an application of the organic silicone optical adhesive composition as described in the first aspect of the present invention or the integrated black organic silicone optical transparent adhesive film as described in the second aspect of the present invention, wherein the organic silicone optical adhesive composition or the integrated black organic silicone optical transparent adhesive film is used in a display bonding process.

[0080] The one-piece black organic silicon optically transparent adhesive film provided by the present invention has an excellent one-piece black display effect and is widely applicable to the field of optical display bonding.

[0081] Compared with the prior art, the present invention has the following beneficial effects:

[0082] (1) In the organic silicone optical adhesive composition provided by the present invention, by using modified graphene oxide slurry as the black pigment slurry, that is, using silane / polysiloxane to graft and modify graphene oxide, the compatibility and dispersibility of graphene oxide with the organic silicone system can be improved, the storage stability of the composition can be improved, and the coating uniformity of the optical adhesive layer of the subsequent integrated black organic silicone optical transparent adhesive film can be better.

[0083] (2) Compared with carbon black, graphene flakes have excellent optical transmittance and water vapor barrier properties. The modified graphene oxide slurry adopted in the present invention can be better dispersed in the optical adhesive and can be stored for a long time without sedimentation, which can effectively avoid the problem of inorganic materials enriched on the surface of the optical adhesive and resulting in a decrease in the interfacial bonding performance. In addition, graphene flakes are more conducive to the barrier of water vapor, reducing the absorption of water vapor by the optical adhesive, achieving the integrated black optical adhesive while maintaining high transmittance and low haze, and can be used in the field of vehicle-mounted display screens to enhance its visual effect.

[0084] (3) The organic silicone optical adhesive composition provided by the present invention is compounded with components such as vinyl silicone oil, vinyl silicone resin, modified graphene oxide slurry, hydrogen-containing silicone oil and hydrogen-containing silicone resin. The obtained organic silicone optical adhesive composition has good compatibility, dispersibility, storage stability and coating uniformity, and also has excellent bonding performance, optical performance, mechanical performance and aging reliability, has good integrated black display effect, and is widely applicable to the field of optical display bonding. DETAILED DESCRIPTION

[0085] The technical solution of the present invention is further described below by specific implementation methods. It should be understood by those skilled in the art that the embodiments are only to help understand the present invention and should not be regarded as specific limitations of the present invention.

[0086] In the following preparation examples, embodiments and comparative examples, the sources of raw materials and equipment used are as follows:

[0087] (1) Vinyl silicone oil

[0088]

[0089] (2) Vinyl silicone resin

[0090]

[0091] (3) Hydrogenated silicone oil

[0092]

[0093]

[0094] (4) Hydrogenated silicone resin

[0095] The general structural formula is: (HMe2SiO 1 / 2 ) x (HMeSiO 2 / 2 ) y (MeSiO 3 / 2 ) z , wherein Me is methyl.

[0096]

[0097] (5) Catalyst

[0098] Code supplier model E-1 Anhui Iyota Silicone Oil Co., Ltd. IOTAPC16

[0099] (6) Inhibitors

[0100] Code supplier model F-1 Aladdin Reagent B103673

[0101] (7) Graphene oxide

[0102] Code Manufacturer Brand Thickness(nm) G-1 Merck Materials 796034 ＜10 G-2 Hangzhou Gaoxi Technology Co., Ltd. GX-pGO-1 ＜10

[0103] (8) Modifier

[0104]

[0105]

[0106] (9) Carbon black

[0107] Code Manufacturer Brand Particle size (nm) I-1 Cabot BP1000 ＜1000

[0108] (10) Coating equipment

[0109] Code Manufacturer Brand Gluing method Coating Machine Shangwang Printing Machinery Co., Ltd. THVG-1100 Dimple coating

[0110] Preparation Example 1

[0111] This preparation example provides a method for preparing a modified graphene oxide slurry, and the preparation method comprises the following steps:

[0112] (1) 30 g of G-1 and 70 mL of toluene were mixed in a stirred reaction vessel for 5 min, the mixing temperature was maintained at 40° C., and then 75 g of H-1 was added to the stirred reaction vessel while stirring, the pH was adjusted to 5, and a second mixing was performed for 15 min. The temperature was then raised to 80° C. for reaction for 3 h, and the solvent and water were removed by distillation under reduced pressure to obtain a modified graphene oxide mixed solution, wherein the molar ratio of the hydroxyl group contained in the G-1 to the carboxyl group contained in the H-1 was 1:2;

[0113] (2) The modified graphene oxide mixed solution obtained in step (1) was ground with zirconium oxide beads having a particle size of 1 mm at a rotation speed of 200 rpm for 2 h to obtain the modified graphene oxide slurry, which was recorded as K-1.

[0114] Preparation Example 2

[0115] This preparation example provides a method for preparing a modified graphene oxide slurry, and the preparation method comprises the following steps:

[0116] (1) 30 g of G-1 and 70 mL of toluene were mixed in a stirred reaction vessel for 2 min, the reaction temperature was maintained at 40° C., and then 46 g of H-2 was added to the stirred reaction vessel while stirring, the pH was adjusted to 4, and a second mixing was performed for 25 min. The temperature was then raised to 70° C. for reaction for 4.5 h, and the solvent and water were removed by distillation under reduced pressure to obtain a modified graphene oxide mixed solution, wherein the molar ratio of the hydroxyl group contained in the G-1 to the carboxyl group contained in the H-2 was 1:1.1;

[0117] (2) The modified graphene oxide mixed solution obtained in step (1) was ground for 3 h using zirconium oxide beads with a particle size of 2 mm at a rotation speed of 100 rpm to obtain the modified graphene oxide slurry, which was recorded as K-2.

[0118] Preparation Example 3

[0119] This preparation example provides a method for preparing a modified graphene oxide slurry, and the preparation method comprises the following steps:

[0120] (1) 30 g of G-2 and 70 mL of toluene were mixed in a stirred reaction vessel for 8 min, the reaction temperature was maintained at 40° C., and then 112.5 g of H-1 was added to the stirred reaction vessel while stirring, the pH was adjusted to 6, and a second mixing was performed for 10 min. The temperature was then raised to 65° C. for reaction for 6 h, and the solvent and water were removed by distillation under reduced pressure to obtain a modified graphene oxide mixed solution, wherein the molar ratio of the hydroxyl group contained in the G-2 to the carboxyl group contained in the H-1 was 1:3;

[0121] (2) The modified graphene oxide mixed solution obtained in step (1) was ground with zirconium oxide beads having a particle size of 1 mm at a rotation speed of 150 rpm for 1 h to obtain the modified graphene oxide slurry, which was recorded as K-3.

[0122] Preparation Example 4

[0123] This preparation example provides a method for preparing a modified graphene oxide slurry, and the preparation method comprises the following steps:

[0124] (1) 30 g of G-2 and 70 mL of toluene were mixed in a stirred reaction vessel for 5 min, the reaction temperature was maintained at 40° C., and then 75 g of H-2 was added to the stirred reaction vessel while stirring, the pH was adjusted to 5, and a second mixing was performed for 15 min. The temperature was then raised to 80° C. for reaction for 3 h, and the solvent and water were removed by distillation under reduced pressure to obtain a modified graphene oxide mixed solution, wherein the molar ratio of the hydroxyl group contained in the G-2 to the carboxyl group contained in the H-2 was 1:1.3;

[0125] (2) The modified graphene oxide mixed solution obtained in step (1) was ground with zirconium oxide beads having a particle size of 1 mm at a rotation speed of 200 rpm for 2 h to obtain the modified graphene oxide slurry, which was recorded as K-4.

[0126] Preparation Example 5

[0127] This preparation example provides a preparation method for a modified graphene oxide slurry. The difference between the preparation method and Preparation Example 1 is that the amount of H-1 added is adjusted so that the molar ratio of the hydroxyl group contained in G-1 to the carboxyl group contained in H-1 is 1:0.8, and the modified graphene oxide slurry is obtained, which is recorded as K-5.

[0128] Preparation Example 6

[0129] This preparation example provides a preparation method for a modified graphene oxide slurry. The difference between the preparation method and Preparation Example 1 is that the amount of H-1 added is adjusted so that the molar ratio of the hydroxyl group contained in G-1 to the carboxyl group contained in H-1 is 1:3.5, and the modified graphene oxide slurry is obtained, which is recorded as K-6.

[0130] Preparation Example 7

[0131] This preparation example provides a preparation method for a modified graphene oxide slurry. The difference between the preparation method and Preparation Example 1 is that H-1 is replaced with γ-glycidyloxypropyltrimethoxysilane (H-3), and the molar ratio of the hydroxyl group contained in G-1 to the epoxy group contained in H-3 is ensured to be 1:2, thereby obtaining the modified graphene oxide slurry, which is recorded as K-7.

[0132] Comparative Preparation Example 1

[0133] This comparative preparation example provides a method for preparing a black slurry, and the preparation method comprises the following steps:

[0134] (1) 30 g of G-1 and 70 mL of toluene were added to a stirring container and stirred at 500 rpm for 30 min to obtain an unmodified graphene oxide mixed solution;

[0135] (2) The unmodified graphene oxide mixed solution obtained in step (1) was placed in a zirconia ball mill using zirconia beads with a particle size of 1 mm and ground and dispersed at a speed of 200 rpm for 2 h to obtain an unmodified graphene oxide black slurry, which was recorded as K-1'.

[0136] Comparative Preparation Example 2

[0137] This comparative preparation example provides a method for preparing a modified carbon black slurry, and the preparation method comprises the following steps:

[0138] (1) 30 g of I-1 and 70 mL of toluene were mixed in a stirred reaction vessel for 5 min, the mixing temperature was maintained at 40° C., and then 75 g of H-1 was added to the stirred reaction vessel while stirring, the pH was adjusted to 5, and a second mixing was performed for 15 min. The temperature was then raised to 80° C. for reaction for 3 h, and the solvent and water were removed by distillation under reduced pressure to obtain a modified graphene oxide mixed solution, wherein the molar ratio of the hydroxyl group contained in the I-1 to the carboxyl group contained in the H-1 was 1:2;

[0139] (2) The modified graphene oxide mixed solution obtained in step (1) was ground with zirconium oxide beads having a particle size of 1 mm at a rotation speed of 200 rpm for 2 h to obtain the modified graphene oxide slurry, which was recorded as K-2'.

[0140] Comparative Preparation Example 3

[0141] This comparative preparation example provides a commercially available black paste, denoted as K-3', and the black paste is a common silica gel color paste (Guangzhou Tianen Chemical TN-6601) that has not been modified with a carboxyl siloxane polymer.

[0142] Example 1

[0143] The present embodiment provides a silicone optical adhesive composition, wherein the raw materials for preparing the silicone optical adhesive composition include, by weight, 10 parts of vinyl silicone resin, 40 parts of vinyl silicone oil, 0.5 parts of modified graphene oxide slurry, 15 parts of hydrogenated silicone oil, 5 parts of hydrogenated silicone resin, 0.0002 parts of catalyst and 0.5 parts of inhibitor. According to the formula, vinyl silicone resin, vinyl silicone oil, hydrogenated silicone oil, hydrogenated silicone resin, modified graphene oxide slurry, catalyst and inhibitor are mixed, stirred and vacuum degassed in turn to obtain the silicone optical adhesive composition. The modified graphene oxide slurry in the present embodiment is the modified graphene oxide slurry K-1 obtained in Preparation Example 1.

[0144] The present embodiment provides an integrated black organic silicone optically transparent adhesive film, which includes a first release film, an optical adhesive layer, and a second release film stacked in sequence, and the optical adhesive layer is obtained by curing the organic silicone optical adhesive composition provided in the present embodiment; the first release film is a light release film with a thickness of 75 μm and a release force of 10 gf / inch; the second release film is a heavy release film with a thickness of 100 μm and a release force of 20 gf / inch; the thickness of the optical adhesive layer is 200 μm.

[0145] This embodiment provides a method for preparing the above-mentioned integrated black organic silicon optically transparent adhesive film, and the preparation method comprises the following steps:

[0146] (a) coating one side of the first release film with an organic silicone optical adhesive composition, and then curing it at 80° C. for 15 min to obtain an optical adhesive layer;

[0147] (b) Laying a second release film on the side of the optical adhesive layer in step (a) away from the first release film to obtain the integrated black organic silicone optical transparent adhesive film.

[0148] Example 2

[0149] The present embodiment provides a silicone optical adhesive composition, wherein the raw materials for preparing the silicone optical adhesive composition include, by weight, 20 parts of vinyl silicone resin, 25 parts of vinyl silicone oil, 0.1 parts of modified graphene oxide slurry, 15 parts of hydrogenated silicone oil, 10 parts of hydrogenated silicone resin, 0.0001 parts of catalyst and 0.0001 parts of inhibitor. According to the formula, vinyl silicone resin, vinyl silicone oil, hydrogenated silicone oil, hydrogenated silicone resin, modified graphene oxide slurry, catalyst and inhibitor are mixed, stirred and vacuum degassed in turn to obtain the silicone optical adhesive composition. The modified graphene oxide slurry in the present embodiment is the modified graphene oxide slurry K-2 obtained in Preparation Example 2.

[0150] The present embodiment provides an integrated black organic silicone optically transparent adhesive film, which includes a first release film, an optical adhesive layer, and a second release film stacked in sequence, and the optical adhesive layer is obtained by curing the organic silicone optical adhesive composition provided in the present embodiment; the first release film is a light release film with a thickness of 75 μm and a release force of 10 gf / inch; the second release film is a heavy release film with a thickness of 100 μm and a release force of 20 gf / inch; the thickness of the optical adhesive layer is 200 μm.

[0151] This embodiment provides a method for preparing the above-mentioned integrated black organic silicon optically transparent adhesive film, and the preparation method comprises the following steps:

[0152] (a) coating one side of the first release film with an organic silicone optical adhesive composition, and then curing it at 80° C. for 15 min to obtain an optical adhesive layer;

[0153] (b) Laying a second release film on the side of the optical adhesive layer in step (a) away from the first release film to obtain the integrated black organic silicone optical transparent adhesive film.

[0154] Example 3

[0155] The present embodiment provides a silicone optical adhesive composition, wherein the raw materials for preparing the silicone optical adhesive composition include, by weight, 25 parts of vinyl silicone resin, 70 parts of vinyl silicone oil, 5 parts of modified graphene oxide slurry, 50 parts of hydrogenated silicone oil, 0.1 parts of hydrogenated silicone resin, 0.1 parts of catalyst and 0.1 parts of inhibitor. According to the formula, vinyl silicone resin, vinyl silicone oil, hydrogenated silicone oil, hydrogenated silicone resin, modified graphene oxide slurry, catalyst and inhibitor are mixed, stirred and vacuum degassed in turn to obtain the silicone optical adhesive composition. The modified graphene oxide slurry in the present embodiment is the modified graphene oxide slurry K-3 obtained in Preparation Example 3.

[0156] The present embodiment provides an integrated black organic silicone optically transparent adhesive film, which includes a first release film, an optical adhesive layer, and a second release film stacked in sequence, and the optical adhesive layer is obtained by curing the organic silicone optical adhesive composition provided in the present embodiment; the first release film is a light release film with a thickness of 75 μm and a release force of 10 gf / inch; the second release film is a heavy release film with a thickness of 100 μm and a release force of 20 gf / inch; the thickness of the optical adhesive layer is 200 μm.

[0157] This embodiment provides a method for preparing the above-mentioned integrated black organic silicon optically transparent adhesive film, and the preparation method comprises the following steps:

[0158] (a) coating one side of the first release film with an organic silicone optical adhesive composition, and then curing it at 80° C. for 15 min to obtain an optical adhesive layer;

[0159] (b) Laying a second release film on the side of the optical adhesive layer in step (a) away from the first release film to obtain the integrated black organic silicone optical transparent adhesive film.

[0160] Embodiment 4-7

[0161] The present embodiments 4-7 respectively provide an organosilicon optical adhesive composition, and the difference between the organosilicon optical adhesive composition and the embodiment 1 is only that the modified graphene oxide slurries K-4 to K-7 prepared in the embodiments 4-7 are respectively used.

[0162] Embodiments 4-7 of the present invention also provide an integrated black organosilicon optical transparent adhesive film and a preparation method thereof, which are the same as Embodiment 1 except that the organosilicon optical adhesive composition is replaced by the organosilicon optical adhesive composition provided in Embodiments 4-7 respectively.

[0163] Comparative Examples 1-3

[0164] Comparative Examples 1-3 provide a kind of organic silicone optical adhesive composition respectively, and the difference between the organic silicone optical adhesive composition and Example 1 is that the modified graphene oxide slurry is replaced by the black slurry provided by Comparative Preparation Examples 1-3 respectively.

[0165] The present comparative examples 1-3 also provide an integrated black organosilicon optical transparent adhesive film and a preparation method thereof, respectively. Except that the organosilicon optical adhesive composition is replaced by the organosilicon optical adhesive composition provided in comparative examples 1-3, the rest is the same as that in Example 1.

[0166] Comparative Examples 4-5

[0167] Comparative Examples 4-5 provide a kind of organic silicone optical adhesive composition respectively, and the difference between the organic silicone optical adhesive composition and Example 1 is only that the weight fraction of the modified graphene oxide slurry K-1 is 0.05 parts and 7 parts respectively.

[0168] The present comparative examples 4-5 also provide an integrated black organosilicon optical transparent adhesive film and a preparation method thereof, respectively. Except that the organosilicon optical adhesive composition is replaced by the organosilicon optical adhesive composition provided in comparative examples 4-5, the rest is the same as Example 1.

[0169] Comparative Example 6

[0170] This comparative example provides an organic silicone optical adhesive composition, which is different from Example 1 only in that the modified graphene oxide slurry is not added.

[0171] This comparative example also provides an integrated black organosilicon optical transparent adhesive film and a preparation method thereof, which is the same as Example 1 except that the organosilicon optical adhesive composition is replaced by the organosilicon optical adhesive composition provided in Comparative Example 6.

[0172] The components and amounts of the optical adhesive compositions provided in the above Examples 1-7 are shown in Table 1, and the components and amounts of the optical adhesive compositions provided in Comparative Examples 1-6 are shown in Table 2, and the amounts of the components are all in parts by weight.

[0173] Table 1

[0174]

[0175] Table 2

[0176]

[0177]

[0178] In Table 1 and Table 2, “ / ” means that the component is not contained.

[0179] Performance Test:

[0180] The performance tests were conducted on the organic silicone optically transparent adhesive films provided in the above-mentioned Examples 1-7 and Comparative Examples 1-6, respectively. The test items and standards are shown in Table 3, and the test results are shown in Table 4.

[0181] Table 3

[0182] Test items Test Standards Initial adhesion GB / T 4852-1984 Shear strength / Mpa GB / T7124-2008 Pull-out strength / Mpa GB / T 31541-2015 Peel force N / 25mm GB / T 2792-1998 Holding force / h GB / T 4851 Transmittance % GB / T2410-2008 Haze GB / T2410-2008

[0183] Table 4

[0184]

[0185] From the data in Table 4, we can see the following points:

[0186] (1) From the data of Examples 1-7, it can be seen that the organic silicone optical transparent adhesive film prepared by using the organic silicone optical adhesive composition provided by the present invention has a higher transmittance and lower haze, an initial adhesion of more than 15#, a shear strength of more than 0.28MPa, a pull-out strength of more than 0.29MPa, a peel force of more than 10.8N / 25mm, and a lasting adhesion of more than 457h; under better conditions, the transmittance is more than 84.2%, the haze is less than 8.4, the initial adhesion is more than 20#, the shear strength is more than 0.38MPa, the pull-out strength is more than 0.39MPa, the peel force is more than 14.7N / 25mm, the lasting adhesion is more than 571h, and the color is uniform.

[0187] (2) Comprehensive comparison of the data of Example 1 and Examples 5-6 shows that the present invention, by preferably controlling the molar ratio of the hydroxyl groups contained in the graphene oxide to the carboxyl groups contained in the carboxylsiloxane polymer, can, on the one hand, avoid too little content of the siloxane segments grafted onto the graphene oxide, poor dispersibility, and agglomeration and sedimentation, which lead to granular color difference and poor black effect in the organic silicone optical transparent adhesive film; on the other hand, avoid the problem of decreased initial adhesion of the optical adhesive due to too large a molar ratio of the hydroxyl groups to the carboxyl groups contained in the carboxylsiloxane polymer.

[0188] (3) Comprehensive comparison of the data of Example 1 and Example 7 shows that although the addition of small molecule silane modified graphene slurry to optical adhesive can achieve a uniform one-piece black effect, the alkoxy group can absorb water in the air, causing the optical adhesive to become foggy. The haze is higher than that of the one-piece black optical adhesive prepared by carboxyl polysiloxane modified graphene oxide.

[0189] (4) Comprehensive comparison of the data of Example 1 and Comparative Examples 1-3 shows that the modified graphene oxide slurry provided by the present invention can effectively avoid the occurrence of regional color difference, transverse lines and other undesirable phenomena in the silicone optical transparent adhesive film, improve the transmittance and reduce the haze, and has better bonding performance, compared with the unmodified graphene oxide, the carbon black slurry modified by the carboxylsiloxane polymer and the commercially available black slurry.

[0190] (5) Comprehensive comparison of the data of Example 1 and Comparative Examples 4-6 shows that the organic silicone optical adhesive composition provided by the present invention can ensure the transmittance and haze of the obtained organic silicone optical transparent adhesive film by adding modified graphene oxide slurry and controlling its weight percentage, while achieving good bonding performance.

[0191] In summary, the silicone optical adhesive composition provided by the present invention has good compatibility, dispersibility, storage stability and coating uniformity, effectively solves the problems of poor light transmittance and easy appearance of stripes and patterns in existing optical adhesive compositions, has good integrated black display effect, and is widely applicable to the field of optical display bonding.

[0192] The applicant declares that the above is only a specific implementation mode of the present invention, but the protection scope of the present invention is not limited thereto. Those skilled in the art should understand that any changes or substitutions that can be easily thought of by those skilled in the art within the technical scope disclosed by the present invention shall fall within the protection scope and disclosure scope of the present invention.

Claims

1. A silicone optical adhesive composition, characterized in that: The raw materials for preparing the organic silicone optical adhesive composition include the following components in parts by weight: The raw materials for preparing the modified graphene oxide slurry include a modifier and graphene oxide; The modifier includes silane and / or polysiloxane; The modifying group contained in the modifying agent includes an epoxy group and / or a carboxyl group.

2. The organic silicone optical adhesive composition according to claim 1, characterized in that: The thickness of the graphene oxide is 0.5-10 nm; Preferably, the silane comprises epoxy silane and / or carboxylic acid silane; Preferably, the epoxy silane includes any one of γ-glycidyloxypropyltrimethoxysilane, γ-glycidyloxypropyltriethoxysilane or γ-glycidyloxypropyldimethoxyethoxysilane or a combination of at least two thereof; Preferably, the polysiloxane comprises any one or a combination of at least two of terminal carboxyl polysiloxane, terminal epoxy polysiloxane, pendant carboxyl polysiloxane or pendant epoxy polysiloxane; Preferably, the weight average molecular weight of the polysiloxane is 1000-100000, the viscosity at 25° C. is 100-5000 mPa·s, and the content of epoxy or carboxyl groups is 0.1-0.5 mmol / g; Preferably, the solid content of the modified graphene oxide slurry is 50-80%; Preferably, the modifier comprises carboxylic acid silane and / or carboxyl-containing polysiloxane, preferably carboxyl-containing polysiloxane; Preferably, in the raw material for preparing the modified graphene oxide slurry, the molar ratio of the hydroxyl group contained in the graphene oxide to the modified group contained in the modifier is 1:(1.1-3); Preferably, the raw materials for preparing the modified graphene oxide slurry further include a diluent; Preferably, the diluent comprises toluene; Preferably, the method for preparing the modified graphene oxide slurry comprises the following steps: (1) performing a first mixing of graphene oxide and a diluent, then adding a modifier, adjusting the pH value to 4-6, performing a second mixing, and then reacting to obtain a modified graphene oxide mixed solution; (2) grinding the modified graphene oxide mixed solution obtained in step (1) to obtain the modified graphene oxide slurry; Preferably, the first mixing time in step (1) is 1-10 min; Preferably, the second mixing time is 1-30min; Preferably, the reaction temperature is 60-90°C; Preferably, the reaction time is 3-6h; Preferably, the grinding medium used in the grinding in step (2) comprises zirconium oxide beads; Preferably, the particle size of the grinding medium is 0.1-2 mm; Preferably, the grinding time is 1-3h; Preferably, the grinding speed is 100-200 rpm.

3. The organic silicon optical adhesive composition according to claim 1 or 2, characterized in that: The vinyl silicone oil includes any one or a combination of at least two of a silicone oil containing vinyl at the terminal, a silicone oil containing vinyl at the side group, or a silicone oil containing vinyl at both the terminal and the side group; Preferably, the viscosity of the vinyl silicone oil at 25° C. is 100-25000 mPa·s; Preferably, the vinyl content in the vinyl silicone oil is 0.1-0.75 mmol / g; Preferably, the viscosity of the vinyl silicone resin at 25° C. is 5000-50000 mPa·s; Preferably, the vinyl content in the vinyl silicone resin is 0.2-1.0 mmol / g; Preferably, the weight average molecular weight of the hydrogen-containing silicone oil is 1000-200000; Preferably, the silicon-hydrogen bond content of the hydrogen-containing silicone oil is 0.4-0.8 mmol / g; Preferably, the viscosity of the hydrogenated silicone resin at 25° C. is 30,000-40,000 mPa·s; Preferably, the silicon-hydrogen bond content of the hydrogen-containing silicone resin is 0.4-0.8 mmol / g; Preferably, the raw materials for preparing the organic silicon optical adhesive composition further include a catalyst; Preferably, the raw materials for preparing the organic silicone optical adhesive composition include 0.0001-0.1 parts by weight of a catalyst; Preferably, in the raw materials for preparing the organic silicone optical adhesive composition, the catalyst includes any one or a combination of at least two of chloroplatinic acid isopropanol solution, Karstedt platinum catalyst, Willing platinum catalyst, (trimethyl) methylcyclopentadiene platinum or acetylacetonate platinum; Preferably, the raw materials for preparing the organic silicon optical adhesive composition further include an inhibitor; Preferably, the raw materials for preparing the organic silicone optical adhesive composition include 0.0001-1 part of inhibitor by weight; Preferably, the inhibitor comprises any one or a combination of at least two of alkynol substances, vinyl ring bodies or maleate substances; Preferably, the raw materials for preparing the organic silicone optical adhesive composition include the following components in parts by weight:

4. An integrated black organic silicon optically transparent adhesive film, characterized in that: The integrated black organic silicon optical transparent adhesive film comprises a first release film, an optical adhesive layer and a second release film which are stacked in sequence; The optical adhesive layer is obtained by curing the organic silicon optical adhesive composition according to any one of claims 1 to 3.

5. The integrated black organic silicon optically transparent adhesive film according to claim 4, characterized in that: The thickness of the optical adhesive layer is 25-2000 μm.

6. The integrated black organic silicon optically transparent adhesive film according to claim 4 or 5, characterized in that: The first release film and the second release film are independently selected from any one of a non-silicone release film and a fluorosilicone release film; Preferably, the thickness of the first release film is 25-100 μm; Preferably, the thickness of the second release film is 50-200 μm; Preferably, the absolute value of the difference between the release forces of the first release film and the second release film is 5-30 gf / inch.

7. A method for preparing the integrated black organosilicon optically transparent adhesive film according to any one of claims 4 to 6, characterized in that: The preparation method comprises the following steps: (a) coating one side of a first release film with the organosilicon optical adhesive composition according to any one of claims 1 to 3, and then curing the same to obtain an optical adhesive layer; (b) Laying a second release film on the side of the optical adhesive layer in step (a) away from the first release film to obtain the integrated black organic silicone optical transparent adhesive film.

8. The preparation method according to claim 7, characterized in that: The coating method in step (a) includes any one of slit coating, double-roller coating, comma blade coating, screen coating or micro-concave coating, or a combination of at least two thereof.

9. The preparation method according to claim 7 or 8, characterized in that: The curing temperature in step (a) is 60-100°C.

10. An application of the organic silicon optical adhesive composition according to any one of claims 1 to 3 or the integrated black organic silicon optical transparent adhesive film according to any one of claims 4 to 6, characterized in that: The organic silicon optical adhesive composition or the integrated black organic silicon optical transparent adhesive film is used in a display bonding process.

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