JP2001116904A - Multilayered antireflection film - Google Patents

Abstract

PROBLEM TO BE SOLVED: To obtain a multilayered antireflection film having a low reflectance of <=1% and excellent in film hardness, durability, adhesion and heat resistance by a low-cost method capable of processing in large quantities and over a large area. SOLUTION: The multilayered antireflection film has an optical interference layer laminated on a transparent substrate and includes at least one layer formed by applying and drying a solution prepared by dissolving benzoyl substituted poly(p-phenylene) and/or benzoyl substituted poly(p/m-phenylene) in a solvent containing at least one solvent selected from the group comprising N-methylpyrrolidone, dimethylformamide and halogenated hydrocarbons as a high refractive index layer.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

The present invention relates to an LCD, a CRT,
The present invention relates to an antireflection film effective for reducing the reflectance of the surface of various displays such as PDPs and various lenses such as spectacle lenses. In particular, the present invention relates to a multilayer antireflection film that achieves mass productivity and high film hardness.

[0002]

2. Description of the Related Art In recent years, as LCDs have become widespread, large-sized, and used outdoors, it has been required to ensure visibility and to improve antifouling properties and heat resistance. Improving visibility is an important issue for displays, and studies are actively being made to improve visibility. In general, the factor that lowers visibility is reflection of scenery due to surface reflection of external light, and a method of providing an anti-reflection film on the outermost surface has been used as a countermeasure against them. Since this antireflection film is provided on the outermost surface in order to exhibit its function, it is inevitably required to improve the performance of the antireflection film in many ways. For example, reduction of reflectance, prevention of adhesion of fingerprints and fats and oils, easy removability, maintenance of various performances in a high temperature environment, and the like. Conventionally, as an antireflection film capable of covering a visible light region, a multilayer film in which transparent thin films such as metal oxides are stacked has been used. A single-layer film is effective only for monochromatic light, whereas a multilayer film has more effective antireflection in a wider wavelength range as the number of layers increases.
However, heretofore, such a multilayer film has been used in which three or more metal oxides or the like are laminated by a physical or chemical vapor deposition method or the like. According to the relationship between the refractive index and the film thickness of each layer, which has been optimally designed in advance, it is necessary to perform the deposition in which the film thickness is controlled with high precision many times. High cost and difficult to process on a large area. On the other hand, in addition to the above-mentioned multilayer film forming method, in order to obtain high productivity, a method in which a solution in which inorganic or organic ultrafine particles are dispersed is applied using spin coating, dip coating, roll coating, or the like, and a method for firing is proposed. ing. However, although this method is advantageous for mass production, it basically requires a high-temperature sintering process. It was inferior in mechanical strength, adhesion, and durability.

[0003] Further, attempts have been made to use a film obtained by applying an organic resin, irradiating ultraviolet rays or electron beams, or heat-curing, as a high refractive index layer, but generally has poor heat resistance.
The durability under high temperature and high humidity was poor.

[0004]

SUMMARY OF THE INVENTION The present invention has been made in view of the above problems, and has a low reflectance of 1% or less, and at the same time, a film hardness, durability, adhesion, and heat resistance. It is an object of the present invention to provide a multilayer antireflection film excellent in quality by a method capable of processing a large amount and a large area at low cost.

[0005]

According to a first aspect of the present invention, there is provided a multilayer antireflection film comprising an optical interference layer laminated on a transparent substrate, wherein the multilayer antireflection film has the following general formula (1):

[0006]

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A benzoyl-substituted poly (p-phenylene) represented by the following general formula (2):

[0008]

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The benzoyl-substituted poly (p / m-
Phenylene) is dissolved in a solvent containing at least one solvent selected from N-methylpyrrolidone, dimethylformamide and halogenated hydrocarbons, and a solution obtained by coating and drying is used as a high refractive index layer. A multilayer antireflection film characterized by containing at least one layer.

Next, a second invention provides the high refractive index layer according to the first invention and an adjacent low refractive index layer having a refractive index of 1.6 or less, wherein N-methylpyrrolidone, dimethylformamide and halogenated 5 at least one hydrocarbon solvent
It is characterized by being formed by applying and drying a solution containing at least weight%.

[0011] In a third aspect, the layer formed on the outermost surface of the low refractive index layer used as the optical interference layer according to the second aspect is represented by the following general formula (3):

[0012]

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Wherein R represents an alkyl group having 1 to 5 carbon atoms, and a silicon compound (A) represented by the following formula:
The following general formula (4)

[0014]

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(Wherein R ¹ represents an alkyl group having 1 to 5 carbon atoms, and n represents an integer of 0 to 12), and the following general formula: (5)

[0016]

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Wherein R ² represents a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 12 carbon atoms, and oxalic acid (D) In a ratio of 0.05 to 0.43 mol of the silicon compound (B) to 1 mol of the silicon compound (A), and 1 mol of the total alkoxy groups contained in the silicon compound (A) and the silicon compound (B). Oxalic acid (D) was added to the alcohol (C) in a ratio of 0.5 to 100 moles and to 1 mole of all alkoxy groups contained in the silicon compound (A) and the silicon compound (B).
A reaction mixture containing between 2 and 2 moles is formed and the reaction mixture is maintained at a SiO2 concentration of 0.5 to 10% by weight, calculated from the silicon atoms therein, while maintaining the absence of water. While the total remaining amount of the silicon compound (A) and the silicon compound (B) in the reaction mixture is 5 mol%
By heating at 50 to 180 ° C. until the following, a solution of the resulting polysiloxane is formed, and then a solution of the polysiloxane and at least one of N-methylpyrrolidone, dimethylformamide and a halogenated hydrocarbon Is formed by applying a coating solution containing 5% by weight or more of the solvent to the surface of the layer to be coated, and thermally curing the coating film obtained at this temperature at 80 to 450 ° C. A refractive index of .38 and 90-
A multilayer antireflection film, which is a coating layer having a water contact angle of 115 degrees.

According to a fourth aspect of the present invention, in the third aspect of the present invention, in the formation of the reaction mixture, in addition to the silicon compound (A), the silicon compound (B), the alcohol (C) and the oxalic acid (D), Methyltrimethoxysilane, methyltriethoxysilane, ethyltrimethoxysilane, ethyltriethoxysilane, propyltrimethoxysilane, propyltriethoxysilane, butyltrimethoxysilane,
Butyltriethoxysilane, pentyltrimethoxysilane, pentyltriethoxysilane, heptyltrimethoxysilane, heptyltriethoxysilane, octyltrimethoxysilane, octyltriethoxysilane, dodecyltrimethoxysilane, dodecyltriethoxysilane,
Hexadecyltrimethoxysilane, hexadecyltriethoxysilane, octadecyltrimethoxysilane, octadecyltriethoxysilane, phenyltrimethoxysilane, phenyltriethoxysilane, vinyltrimethoxysilane, vinyltriethoxysilane, γ-aminopropyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-glycidoxypropyltrimethoxysilane, γ-glycidoxypropyltriethoxysilane,
γ-methacryloxypropyltrimethoxysilane, γ-
At least one alkylalkoxysilane selected from the group consisting of methacryloxypropyltriethoxysilane, dimethyldimethoxysilane and dimethyldiethoxysilane is used in an amount of from 0.02 to 1 mol per mol of the silicon compound (A).
It is a multilayer antireflection film used together with a ratio of 0.2 mol.

According to a fifth aspect, in the third and fourth aspects, at least one selected from the group consisting of silica sol, alumina sol, titania sol, zirconia sol, magnesium fluoride sol, and ceria sol is used as an additive of the coating solution. A multilayer antireflection film characterized by being used in combination.

[0020]

BEST MODE FOR CARRYING OUT THE INVENTION Next, the present invention will be described in more detail with reference to embodiments.

Benzoyl-substituted poly (p-phenylene)
(Polymer) and / or benzoyl-substituted poly (p / m-
Phenylene) (copolymer) is N-methylpyrrolidone,
It is a powder that can be dissolved in solvents such as dimethylformamide and halogenated hydrocarbons, and can be used as a solution dissolved in these solvents. Specific examples of the halogenated hydrocarbon include methylene chloride, chloroform,
Carbon tetrachloride, bromoform, 1,2-dichloroethane,
Examples thereof include 1,1-dichloroethane, trichloroethane, and tetrachloroethane. These solvents can be used alone or in combination of two or more.

It is also possible to mix another solvent for the purpose of improving the film forming property. The solid concentration in the solution is not particularly limited, and varies depending on conditions such as the average molecular weight of the polymer, the coating method, and the required film thickness, but is adjusted in the range of 0.5 to 20% by weight in terms of the solid concentration. Is preferred. If it is less than 0.5% by weight, it is difficult to obtain a desired film thickness, and if it is more than 20% by weight, the varnish has a high viscosity and is difficult to handle.

The benzoyl-substituted poly (p-phenylene) and the benzoyl-substituted poly (p / m-phenylene) used have a number average molecular weight in terms of polystyrene, as measured by gel permeation chromatography, of 15,000 to 120,000 is preferred. The number-average molecular weight (in terms of polystyrene) of benzoyl-substituted poly (p-phenylene) and benzoyl-substituted poly (p / m-phenylene) is determined by gel permeation chromatography (solvent: dimethyl) using a solution obtained by dissolving these in N-methylpyrrolidone. Formamide / tetrahydrofuran = 9
9: 1, LiBr 30 mM, H ₃ PO ₄ 30 mM).

The prepared solution is applied to a transparent substrate by a commonly used coating method and dried to obtain 1.68.
A high refractive index layer having a refractive index of ~ 1.70 can be easily obtained. Hot air, a hot plate, an oven, or the like is used for drying, and a desired high refractive index layer is formed by heating at a temperature of 80 ° C. to 500 ° C. for about 5 minutes to 30 minutes.

The drying temperature is limited by the substrate used,
It must be performed below the heat resistant temperature of the substrate. The transparent substrate is not particularly limited, and PET, polycarbonate, triacetyl cellulose, glass, or the like can be used. As for the plastic substrate, it is also effective to use a hard-coated one for the purpose of improving the scratch resistance of the antireflection layer.

As the coating method, a generally known method, for example, a spin coating method, a dip coating method, a roll coating method, a gravure coating method, or the like can be used. The high refractive index layer obtained as described above has a high hardness,
In addition, it has a heat resistance of about 500 ° C. This makes it possible to obtain an antireflection film having excellent heat resistance and durability.

In the high refractive index layer, additives for the purpose of imparting antistatic performance and adjusting the refractive index can be mixed. Examples of the additive include a composite metal oxide containing titania, alumina, antimony, and the like as components.
These are desirably mixed to such an extent that the transparency and the film hardness of the high refractive index layer are not impaired.

Further, the multilayer antireflection film of the present invention includes a low refractive index layer laminated on the high refractive index layer as an optical interference layer. As the low refractive index layer, a conventionally known layer having a refractive index of 1.6 or less can be used. For example, inorganic oxides such as silicon dioxide and aluminum oxide can be used.

The present invention is selected from the group consisting of N-methylpyrrolidone, dimethylformamide and halogenated hydrocarbon, which dissolves the lower high refractive index layer in the coating liquid for forming the low refractive index layer. It is characterized in that at least one solvent is contained in an amount of 5% by weight or more. Conventionally, in the configuration of the resin layer and the inorganic layer, the adhesion between the layers is weak,
There was a defect that the film was peeled off. However, as in the present invention, when a solvent capable of dissolving the lower layer is contained in the upper layer coating solution, the components of the upper layer film enter the lower layer surface, and the interlayer adhesion becomes stronger by subsequent drying. In order to exhibit this effect, the above solvent is required to be 5% by weight or more. The upper limit of the content is determined by the film forming property and the stability of the coating solution.

The outermost layer of the multilayer antireflection film of the present invention is preferably a fluorine-based material from the viewpoint of preventing contamination. Examples of such a material include a vinylidene fluoride copolymer, a fluoroolefin / hydrocarbon olefin copolymer, a fluorine-containing epoxy resin, a fluorine-containing epoxy acrylate, a fluorine-containing silicone, and a fluorine-containing silane dissolved in an organic solvent. Can be Particularly preferably, the fluorinated silane described in the claims is desirable. As a result, an antireflection film having excellent antireflection characteristics, film hardness, adhesion, antifouling performance, and the like can be obtained.

Although the thickness of the low refractive index layer as the outermost surface varies depending on the optical design, the minimum value of the reflectance is 400 to 700 n.
m, more preferably 500 to 600 nm.

The low refractive index layer can be formed in the same manner as in the formation of the above high refractive index layer.

In the multilayer antireflection film of the present invention, as the optical interference layer that can be used, in addition to the above-mentioned optical interference layer in which the high refractive index layer and the low refractive index layer are laminated one by one, a medium refractive index layer and An optical interference layer in which a high refractive index layer and a low refractive index layer are sequentially stacked can be used. In this case, a layer having a refractive index located between the substrate or the hard coat layer and the high refractive index layer described in the claims is used as the middle refractive index layer.

The multilayer antireflection film of the present invention can be used for various displays (LCD, PDP, CRT) and various lenses. In a display or a lens having such an antireflection film, reflection of incident light is prevented and visibility is remarkably improved.

[0035]

EXAMPLES The present invention will be described in more detail with reference to the following Examples, but it should not be construed that the present invention is limited thereto.

Example 1 A high-refractive-index layer and a low-refractive-index layer were sequentially laminated on a 100-μm-thick hard-coated PET film to form a multilayer antireflection film. The coating liquid for forming the high refractive index layer was adjusted as follows.

In a 100 ml flask, benzoyl-substituted poly (p-phenylene) (number average molecular weight: 117,32)
0) [Product name: Parmax-1000 (trademark) ma
0.5 g of Xdem] was further weighed, 49.5 g of N-methylpyrrolidone was further added, and the mixture was stirred and dissolved while heating at 70 ° C.

Next, this coating solution was applied on a substrate using a spin coater and dried at 120 ° C. for 30 minutes to form a high refractive index layer. The refractive index of the formed high refractive index layer was 1.67, and the film thickness was 80 nm.

Next, the coating liquid for forming the low refractive index layer was adjusted as follows.

70.6 g of ethanol was weighed into a four-necked flask equipped with a reflux tube, and oxalic anhydride 1 was stirred under stirring.
2.0 g was added little by little to dissolve oxalic acid. Next, this solution was heated to reflux temperature, and under reflux 9.4 g of tetraethoxysilane, 6.2 g of tridecafluorooctyltrimethoxysilane, 1.2 g of γ-glycidoxypropyltrimethoxysilane and 1.2 g of γ-aminopropyltrimethoxysilane. A mixture of 0.6 g of methoxysilane was added dropwise. After the completion of the dropwise addition, heating was continued under reflux for 5 hours and then cooled to obtain a polysiloxane solution. When this solution was analyzed by gas chromatography, no alkoxide monomer was detected.

Further, 51.0 g of a methanol-dispersed silica sol containing 15.7% by weight of colloidal silica having a particle diameter of 8 nm as SiO ₂ , 134 g of ethanol and 15.0 g of N-methylpyrrolidone were mixed to form a low refractive index layer. A coating liquid for use was obtained.

This coating solution was applied on a substrate on which a high refractive index layer was formed using a spin coater, and was cured by heating at 120 ° C. for 30 minutes. The refractive index of the obtained low refractive index layer was 1.
At 36, the film thickness was about 90 nm. The contact angle of water was 104 degrees.

Example 2 As in Example 1, a high refractive index layer and a low refractive index layer were sequentially laminated on a 100 μm-thick hard-coated PET film to produce an antireflection-treated film.

The coating liquid for forming the high refractive index layer was adjusted as follows.

In a 100 ml flask, benzoyl-substituted poly (p / m-phenylene) (number average molecular weight: 46.0
00) [trade name Parmax-1200 (trademark) ma
0.5 g of Xdem] was further weighed, 49.5 g of N-methylpyrrolidone was further added, and the mixture was stirred and dissolved while heating at 70 ° C.

Next, this coating solution was applied on a substrate using a spin coater, and dried at 120 ° C. for 30 minutes to form a high refractive index layer. The refractive index of the formed high refractive index layer was 1.68, and the film thickness was 75 nm.

Next, a low refractive index layer was formed in the same manner as in Example 1 to obtain an antireflection-treated film.

Example 3 Benzoyl-substituted poly (p-phenylene) [trade name: Pa
rmax-1000 (manufactured by maxdem)], an antireflection-treated film was produced in the same manner as in Example 1 except that the number average molecular weight was 32,000. At this time, the refractive index of the obtained high refractive index layer was 1.67 and the film thickness was 70 n.
m.

Example 4 Benzoyl-substituted poly (p / m-phenylene) [trade name P
armmax-1200 (manufactured by maxdem)], and an antireflection-treated film was produced in the same manner as in Example 2 except that the number average molecular weight was 22,800. The high refractive index layer thus obtained has a refractive index of 1.70 and a thickness of 60.
nm.

Example 5 Benzoyl-substituted poly (p / m-phenylene) [trade name P
armmax-1200 (trademark) manufactured by maxdem]
Example 2 except that the number average molecular weight was 17,200.
In the same manner as in the above, an antireflection-treated film was produced. The high refractive index layer obtained at this time had a refractive index of 1.70 and a thickness of 6
It was 5 nm.

Example 6 Example 1 was repeated except that the thickness of the high refractive index layer was 165 nm.
An anti-reflection film was produced in the same manner as in 1.

Example 7 Example 2 was repeated except that the thickness of the high refractive index layer was changed to 162 nm.
An anti-reflection film was produced in the same manner as in 1.

Example 8 A high-refractive-index layer and a low-refractive-index layer were sequentially laminated on a hard-coated triacetylcellulose film to prepare an antireflection-treated film.

The same procedure as in Example 1 was carried out except that each layer was dried at 100 ° C.

Example 9 A high-refractive-index layer and a low-refractive-index layer were sequentially laminated on soda lime glass to prepare an antireflection-treated film. 4 for each layer
Except for drying at 00 ° C., the procedure was the same as in Example 1.

At this time, the high refractive layer had a refractive index of 1.70 and a thickness of 80 nm. The low refractive index layer had a refractive index of 1.36 and a thickness of 80 nm.

Comparative Example 1 A high-refractive index layer and a low-refractive index layer were sequentially laminated on a hard-coated PET film to produce an antireflection film.

The coating liquid for forming the high refractive index layer was adjusted as follows. 81.0 g of ethanol was weighed into a 200 ml eggplant flask, and tetraethoxysilane was added to the flask.
2 g and 14.0 g of tetraethoxytitanium were mixed and stirred. Then, 0.4 g of 60% nitric acid and 1.4 g of water were added,
The mixture was stirred at room temperature for 30 minutes to prepare a coating solution.

This coating solution was applied on a substrate using a spin coater, and dried at 120 ° C. for 30 minutes to form a high refractive index layer. The refractive index of the formed high refractive index layer is 1.7.
In No. 4, the film thickness was 72 nm.

The subsequent formation of a low refractive index layer was performed in the same manner as in Example 1 to obtain an antireflection-treated film.

Comparative Example 2 A high-refractive-index layer and a low-refractive-index layer were sequentially laminated on a hard-coated PET film to prepare an antireflection film. The coating liquid for forming a high refractive index layer was formed in the same manner as in Comparative Example 1 so that the dry film thickness was 160 nm. Subsequent formation of the low refractive index layer was performed in the same manner as in Example 1 to obtain an antireflection-treated film.

The refractive index and the film thickness were measured by the following methods.

Refractive index: The refractive index at 633 nm was measured using an ellipsometer DVA-36L manufactured by Mizojiri Optical Co., Ltd.

Thickness: The dried film is scratched with a cutter, and after curing, using a Talystep manufactured by Rank Taylor Hobson,
The film thickness was determined by measuring the step. The measurement of the refractive index and the film thickness used a film formed on a silicon substrate under the same conditions.

The pencil hardness, scratch resistance and reflectivity of the prepared antireflection-treated substrate were measured by the following methods. Table 1 shows the results.

Pencil hardness: Measured according to JIS K5400.

Reflectance: Spectrophotometer U manufactured by Shimadzu Corporation
Using V3100PC, 5 ° absolute reflectance was measured. At this time, the surface that had not been subjected to the anti-reflection treatment was treated with black ink and measured in a light-shielded state.

Scratch Resistance: Using # 0000 steel wool, the degree of scratching after 10 reciprocations under a load of 200 g was evaluated.

Durability: The sample was left for 1000 hours under conditions of a temperature of 65 ° C. and a humidity of 95%, and evaluated for changes in reflection spectrum, generation of cracks, and adhesion.

Adhesion: The adhesion was measured by a cellophane tape peeling test using a cross cut with a base.

Fingerprint removal property: A fingerprint was attached to the film surface, rubbed several times with a tissue, and the degree of fingerprint removal was visually judged.

[0072]

[Table 1] Table 1 Evaluation results Reflectivity Pencil hardness Abrasion resistance Adhesion durability Durability Fingerprint removal Example 1 0.2 3H ○ ○ ○ ○ Example 2 0.2 3H ○ ○ ○ ○ Example 3 0.2 3H ○ ○ ○ ○ Example 4 0.23H ○ ○ ○ ○ Example 5 0.13H ○ ○ ○ ○ Example 6 0.23H ○ ○ ○ ○ Example 7 0.23H ○ ○ ○ ○ Example 8 0.3 3H ○ ○ ○ ○ Example 9 0.18H ○ ○ ○ ○ Comparative Example 1 0.2 H △ △ △ ○ Comparative Example 2 0.2 H × △ × ○ (Note) [Scratch resistance [Evaluation]: (○) No damage; (△) Several scratches; (×) Countless scratches [Durability evaluation]: (○) No change; (△) Spectrum change; (×) Spectrum change , Crack generation, change in adhesion [Evaluation of adhesion]: (○) No peeling; (△) Partial peeling; There removal assessment] :( ○) without fingerprints (×) fingerprints

[0073]

According to the present invention, antireflection performance, film hardness,
An antireflection film having excellent durability can be provided by a method having excellent productivity. These are useful for improving the visibility of various displays and lenses.

Continued on the front page F term (reference) 2K009 AA05 BB24 CC09 CC21 CC42 DD02 DD06 4F100 AA06C AA06H AA19C AA19H AA20C AA20H AA21C AA21H AA27C AA27H AH06C AH06K AK42 AK80B03 BA08BA03 BA00 BA03 BA00 JN01A JN06 JN18B JN18C JN30B 5G435 AA01 AA14 FF02 HH03 KK07

Claims (5)

[Claims] 1. A multilayer antireflection film comprising an optical interference layer laminated on a transparent substrate, wherein the multilayer antireflection film has the following general formula (1): And / or a benzoyl-substituted poly (p-phenylene) represented by the following general formula (2): A benzoyl-substituted poly (p / m-phenylene) represented by
Is dissolved in a solvent containing at least one solvent selected from the group consisting of N-methylpyrrolidone, dimethylformamide and halogenated hydrocarbons, and a layer obtained by applying and drying the solution is coated with a high refractive index. A multilayer antireflection film comprising at least one layer as a layer. 2. The high-refractive-index layer and the adjacent low-refractive-index layer having a refractive index of 1.6 or less are at least selected from the group consisting of N-methylpyrrolidone, dimethylformamide and halogenated hydrocarbons. 5% by weight of a solvent
The multilayer antireflection film according to claim 1, wherein the multilayer antireflection film is formed by applying and drying a solution containing the above. 3. A low refractive index layer used as an optical interference layer, a layer formed on the outermost surface is represented by the following general formula (3). (Where R represents an alkyl group having 1 to 5 carbon atoms) and a silicon compound (A) represented by the following general formula (4): (However, R ¹ represents an alkyl group having 1 to 5 carbon atoms, and n represents an integer of 0 to 12.) and a silicon compound (B) represented by the following general formula (5) Embedded image Wherein R ² represents a hydrogen atom or an unsubstituted or substituted alkyl group having 1 to 12 carbon atoms, and an oxalic acid (D) Silicon compound (B) per mole of compound (A)
The alcohol (C) is in a ratio of 0.05 to 0.43 mol, and the alcohol (C) is in a ratio of 0.5 to 100 mol with respect to 1 mol of all alkoxy groups contained in the silicon compound (A) and the silicon compound (B). A reaction mixture containing 0.2 to 2 mol of oxalic acid (D) to 1 mol of all alkoxy groups contained in compound (A) and silicon compound (B) is formed, and the reaction mixture is formed therein. 0.5-converted from the silicon atom of
The silicon compound (A) in the reaction mixture was maintained while maintaining a SiO 2 concentration of 10% by weight and the absence of water.
And heating at 50 to 180 ° C. until the total remaining amount of the silicon compound (B) becomes 5 mol% or less, thereby producing a solution of the polysiloxane produced thereby, and then a solution of the polysiloxane and N 2 A coating solution containing at least one solvent of 5% by weight or more of methylpyrrolidone, dimethylformamide and a halogenated hydrocarbon is applied to the surface of the layer to be coated;
3. The coating layer according to claim 1, wherein the coating layer is formed by thermosetting at 0 to 450 ° C., and has a refractive index of 1.28 to 1.38 and a water contact angle of 90 to 115 degrees. 4. Multilayer anti-reflective coating. 4. In the formation of the reaction mixture, in addition to the silicon compound (A), the silicon compound (B), the alcohol (C) and the oxalic acid (D), methyltrimethoxysilane, methyltriethoxy as a modifying agent (E) Silane, ethyltrimethoxysilane, ethyltriethoxysilane, propyltrimethoxysilane, propyltriethoxysilane, butyltrimethoxysilane, butyltriethoxysilane, pentyltrimethoxysilane, pentyltriethoxysilane,
Heptyltrimethoxysilane, heptyltriethoxysilane, octyltrimethoxysilane, octyltriethoxysilane, dodecyltrimethoxysilane, dodecyltriethoxysilane, hexadecyltrimethoxysilane,
Hexadecyltriethoxysilane, octadecyltrimethoxysilane, octadecyltriethoxysilane, phenyltrimethoxysilane, phenyltriethoxysilane, vinyltrimethoxysilane, vinyltriethoxysilane, γ-aminopropyltrimethoxysilane, γ-aminopropyltriethoxy Consists of silane, γ-glycidoxypropyltrimethoxysilane, γ-glycidoxypropyltriethoxysilane, γ-methacryloxypropyltrimethoxysilane, γ-methacryloxypropyltriethoxysilane, dimethyldimethoxysilane and dimethyldiethoxysilane The multilayer antireflection according to claim 3, wherein at least one alkylalkoxysilane selected from the group is used in a ratio of 0.02 to 0.2 mol per 1 mol of the silicon compound (A). 5. The multilayer antireflection film according to claim 3, wherein at least one sol selected from the group consisting of silica sol, alumina sol, titania sol, zirconia sol, magnesium fluoride sol, and ceria sol is used as an additive of the coating solution.