JPH04236266A - Resin composition and its production - Google Patents

Abstract

PURPOSE:To obtain a resin composition having the characteristic features of organic materials as well as those of inorganic materials and useful as a molding material, sealing material, paint, adhesive, etc., by precipitating silica particles by a sol-gel process in the presence of an OH-containing resin. CONSTITUTION:The objective resin composition called as an organic-inorganic composite material or a silica-composite resin contains (A) an OH-containing resin (e.g. polyvinyl acetal or vinyl acetate/vinyl alcohol copolymer) and (B) silica particles produced by a sol-get process at a weight ratio (A/B) of 99/1 to 20/80, preferably 95/5 to 40/60. It can be produced by adding 0.5-20mol (preferably 0.75-10mol) of water (based on 1mol of alkoxy group) to an alkoxysilane (e.g. tetramethoxy-silane or methyl tri-t-butoxysilane) in the presence of a basic catalyst (preferably low-boiling amine or ammonia) and preferably in the copresence of the component A and hydrolyzing the alkoxysilane at 0-200 deg.C (preferably 20-150 deg.C) to precipitate silica particles.

Description

[Detailed description of the invention]

0001

[Field of Industrial Application] The present invention relates to a resin composition containing silica particles and a method for producing the same, and the composition of the present invention can also be referred to as an organic-inorganic composite or a silica composite resin. The composition is characterized by consisting of a resin having a hydroxyl group and silica particles precipitated by a sol-gel method, particularly by hydrolyzing alkoxysilane, and can be used as a molding material, a sealant, a paint, an adhesive, etc. It is a material that can be used for various purposes, and is widely used in various industries that use them.

0002

[Prior art] Silicone-modified resin has been proposed and put into practical use as a material that combines the flexibility and moldability of resins with the hardness, heat resistance, weather resistance, and nonflammability of inorganic materials. has been done. However, the degree of bonding between silicone and resin is low, and there are restrictions on the types of resins that can be used, so the results are not always satisfactory and the applications for which they can be used are also limited.

On the other hand, in recent years, organic/inorganic composites in which fine silica particles and resin are combined have been proposed and put into practical use. A silica composite resin is produced by heat treatment, and has properties such as hardness and nonflammability that cannot be obtained with resin alone.

0004

[Problems to be Solved by the Invention] However, such a silica composite resin cannot be produced without first synthesizing fine silica particles, mixing and dispersing them in a resin, and causing a reaction between the silica particles and the resin by heat treatment or the like. However, the process is complicated, and a binder such as an alkoxysilane compound is required to composite the silica particles and the resin.

An object of the present invention is to solve the above-mentioned problems and to obtain a resin composition which can be called an excellent silica composite resin.

[0006]

[Means for Solving the Problems] As a result of intensive studies by the present inventors to solve the above-mentioned problems, the present inventors have developed a method that consists of silica particles precipitated by hydrolysis of an alkoxysilane compound and a resin having a hydroxyl group using a sol-gel method. The resin composition is
The present invention was completed by solving these problems and discovering that the silica composite resin is an excellent silica composite resin.

That is, the present invention relates to a resin composition characterized in that it consists of a resin having a hydroxyl group and silica particles produced by a sol-gel method, and a resin composition that is characterized in that it consists of a resin having a hydroxyl group and silica particles produced by a sol-gel method. The present invention relates to a method for producing the resin composition described above, which comprises hydrolyzing silane.

○Resin The resin in the present invention is a resin having one or more hydroxyl groups in one molecule, and such a resin does not have any particular restrictions for producing the composition of the present invention. , This point is a major feature of the present invention.

Specific resins include widely known ones, such as polyvinyl acetal, polyester resin, alkyd resin, acrylic resin, urethane resin, polyalkylene glycol, polyvinyl alcohol, vinyl acetate/vinyl alcohol, etc. In the present invention, one selected from such resins is used.
A species or more than one species of resin can be used.

[0010] In the present invention, the resin can be used regardless of whether it is liquid or solid, but since the silica particles produced by the sol-gel method used in the present invention are precipitated in a solvent, it is difficult to dissolve the resin uniformly in the solvent. , is preferred for the present invention.

[0011] As the resin having a hydroxyl group, it is also possible to use the resin and a curing agent for the resin in combination. Such curing agents are also known, and for example, melamine resins, urea resins, guanidine resins, polyisocyanate resins, epoxy resins, phenol resins, etc. are selected depending on the use and purpose.

Silica particles The silica particles used in the present invention are characterized by being produced by a sol-gel method, particularly by the hydrolysis reaction of an alkoxysilane compound. be.

[0013] The alkoxysilane compound used in the sol-gel method is a compound represented by the following general formula (1) and/or
or a partial condensate thereof. (R2)nSi(OR1)4-n (1) (In the formula, R1 represents an alkyl group, aryl group, alkenyl group, or hydrogen atom, R2 represents an alkyl group, aryl group, or alkenyl group, and n is 0 to (It is an integer of 1.)

0014
] The alkyl group, aryl group and alkenyl group which are substituents R1 in the above general formula (1) are specifically methyl group, ethyl group, n-propyl group, i-propyl group, n
- lower alkyl groups such as butyl, i-butyl, s-butyl, t-butyl; phenyl, tolyl, mesityl, etc.; vinyl, allyl, i-propenyl, etc., and higher alkyl It is preferable to avoid groups since they have poor reactivity during hydrolysis.

Specific examples of alkoxysilane compounds include tetramethoxysilane, tetraethoxysilane, tetra-n-propoxysilane, tetra-i-propoxysilane, tetra-n-butoxysilane, tetra-i-butoxysilane, and tetra- Examples include t-butoxysilane, methyltrimethoxysilane, methyltriethoxysilane, methyltri-n-propoxysilane, methyltri-i-propoxysilane, methyltri-n-butoxysilane, and methyltri-t-butoxysilane.

[0016] The alkoxysilane compound, if necessary,
Metal alkoxides other than Si 2 such as Zr, Ti 2 , Al 2 , B, etc. and/or coordination compounds can also be used as the alkoxysilane compound. Specific examples thereof include, for example, tetra-i-propoxytitanium, tetra-n-butoxytitanium, tetra-i-butoxytitanium, diacetylacetate titanium propylate, titanium tetrakis (acetylacetonate),
Examples include tetraethoxyzirconium, tetra-n-butoxyzirconium, zirconium bis(acetylacetonate), tri-i-propoxyaluminum, aluminum tris(ethylacetoacetate), and triethyl borate.

[0017] Silica particles are produced by dissolving an alkoxysilane compound in a solvent, if necessary, and carrying out a hydrolysis reaction using a sol-gel method. The shape of the obtained silica particles can be appropriately adjusted depending on conditions such as the solvent used, the alkoxysilane concentration, the amount of water, the catalyst, the liquid temperature, and the reaction time.

The solvent used in the sol-gel method is preferably one that is easily compatible with the alkoxysilane compound and water, or one that dissolves and disperses the resin; water; alcohols such as methanol, ethanol, propanol, butanol; acetone; , ketones such as methyl ethyl ketone; glycol monoethers such as ethylene glycol methyl ether, ethylene glycol ethyl ether, ethylene glycol butyl ether, propylene glycol ethyl ether, and mixed solvents of two or more selected from these solvents. . In addition, aromatics such as toluene, xylene, ethylbenzene, and mesitylene; esters such as ethyl acetate, butyl acetate, and ethylene glycol methyl ether acetate may also be mixed and used as appropriate.

The catalyst is preferably a basic catalyst, such as ammonia, amines such as ethylamine, diethylamine, and triethylamine, inorganic bases such as sodium hydroxide and potassium hydroxide, anion exchange resins, lead hydroxyapatite, and hydrotal. Although solid bases such as bismuth trioxide, bismuth trioxide, and hydrous bismuth (V) oxide can be used, low-boiling amines and ammonia are particularly preferred.

The amount of water during hydrolysis is preferably 0.5 to 20 moles, more preferably 0.75 to 10 moles, per mole of alkoxy groups in the alkoxysilane compound. Such water can be added before or after addition of the alkoxysilane.

The reaction temperature for hydrolysis is preferably 0 to 200°C, more preferably 20 to 150°C. If the reaction temperature is below 0°C, the reaction progresses very slowly and is impractical, and if it is above 200°C, the reaction cannot be controlled, resulting in gelation or particles having a size and shape inappropriate for the present invention. There is a risk.

Silica particles are produced by precipitation in a liquid under the conditions described above. In the present invention, the silica particles precipitated in the liquid can be blended as they are with the resin, which is the other component of the present invention, which is a major feature of the present invention.

[0023] Alternatively, the solvent of the dispersion of silica particles produced by the above method may be removed by methods such as filtration, evaporation, or sublimation to obtain silica particles as a solid powder, which may then be blended with a resin. can.

○ Preparation method The composition of the present invention may be prepared by any method as long as the silica particles and resin can be mixed and dispersed uniformly, and any known mixing method can be adopted. For example, the following method may be used. prepared by the method. Examples include a method of simply stirring and mixing silica particles or a silica particle dispersion with a solution in which a resin having a hydroxyl group is dissolved in a solvent as necessary, using an appropriate stirring device, and at that time, heating at 60 to 200°C as necessary. You may. In particular, a method in which one or more alkoxysilane compounds are added and hydrolyzed in the presence of a catalyst in a liquid state in which a resin having a hydroxyl group is dissolved or dispersed in a solvent as necessary is a This is a preferred method because the properties of the resulting resin composition are particularly excellent. The composition produced by such a method can be used as it is in a solution state or in a form from which the solvent has been removed.

○Blending ratio As for the blending ratio of resin and silica particles in the composition of the present invention, the ratio of resin to silica particles is 99/1 to 2 by weight.
0/80 is preferable, more preferably 95/5 to 40
/60. If the blending ratio of silica particles is small, the effect of blending the silica particles may not be obtained, and if the blending ratio is high, the composition may become brittle.

In particular, when producing an alkoxysilane by hydrolyzing it with a basic catalyst in the presence of a resin having a hydroxyl group, the blending ratio of the resin and the alkoxysilane is from 1/100 to 1000/100 by weight. The ratio is preferably 5/100 to 500/100.

Additives Appropriate additives can be added to the composition of the present invention depending on the purpose. As additives, those widely used in the field can be used. , specifically, for example, carbon black, titanium oxide, zinc white,
White lead, yellow lead, aluminum hydroxide, calcium carbonate, talc, clay, kaolin, white carbon, molybdenum disulfide, alumina, mica, glass fiber, zinc powder,
Examples include pigments such as aluminum powder, fillers, reinforcing agents, and various other additives such as viscosity modifiers, antifoaming agents, leveling agents, antioxidants, ultraviolet absorbers, and lubricants. Such additives can be added at an appropriate stage during the preparation of the composition of the present invention.

○Applications The composition of the present invention has excellent strength by itself and also has excellent adhesion to other base materials, so it can be used as a molding material, rubber material, film material, paint, and surface treatment. It can be used as an agent, adhesive, sealant, etc. in various applications such as machinery, electrical equipment, automobiles, transportation vehicles, metals, and architecture. Furthermore, since the composition of the present invention is manufactured in a solution state or a molten state by heating, it can be easily formed into various shapes by cooling after melting and molding, or by drying and removing the solvent after coating the solution. It can be molded or applied to various base materials. Such methods are known in the art.

[0029]

[Operation] The composition of the present invention is composed of a resin having a hydroxyl group and silica particles produced by a sol-gel method, and can also be called a silica composite resin, and the form of the composite has not been clearly defined. However, it is presumed that the effects of the composition of the present invention are produced by the following mechanism.

■ Active Si OH groups remain on the surface of the silica particles precipitated during hydrolysis by the sol-gel method, and the Si
Reactions between OH groups and hydroxyl groups in the resin occur actively, especially during hydrolysis of alkoxysilane, and the resin component and silica particle component become highly complex.

(2) Since the silica particles precipitated during hydrolysis by the sol-gel method have a uniform particle size and are uniformly dispersed in a solution state, a composite resin is formed that is uniformly dispersed even after the solvent is removed.

(2) The physical properties of the resin are improved due to the reinforcing effect of the silica particles as crosslinking points.

■ Active SiOH on the surface of the precipitated silica particles
Because the group remains, when applied to various substrates, it exhibits extremely excellent adhesion to those substrates.

[0034] A specific example will be explained below.

[0035]

[Example] Synthesis example of silica particles Silica particle dispersion A A reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device was charged with 80 parts of tetraethoxysilane and 100 parts of isopropanol, and after raising the temperature to 70°C, ethylamine A mixed solution of 0.5 parts of silica, 15.3 parts of pure water, and 40 parts of isopropanol was gradually added dropwise, and the mixture was allowed to react at 70°C for 3 hours to obtain a cloudy liquid in which fine silica particles with an average particle size of 0.1 μm were precipitated. Ta. Furthermore, this cloudy liquid was concentrated under reduced pressure, and the heating residue was adjusted to 10%. The heating residue was determined by placing 1 g of the cloudy liquid in an aluminum cup, heating it at 150° C. for 20 minutes, and calculating its residual rate.

Silica particle dispersion B: 60 parts of tetramethoxysilane and 110 parts of propylene glycol monoethyl ether were charged into a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device, and the temperature was raised to 40°C.
A mixed solution of 0.5 parts of ethylamine, 9.2 parts of pure water, and 30 parts of propylene glycol monomethyl ether was gradually added dropwise and allowed to react at 40°C for 3 hours, with an average particle size of 0.
A cloudy white liquid in which fine silica particles of 0.02 μm were precipitated was obtained. Furthermore, this cloudy liquid was concentrated under reduced pressure, and the heating residue was reduced to 10%.
Adjusted to.

Silica particle dispersion C: 60 parts of tetraethoxysilane, 16.8 parts of zirconium tetrakis (acetylacetonate), and 130 parts of methyl ethyl ketone were charged into a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device, and the temperature was raised to 70°C. After heating, a mixed solution of 0.3 parts of ethylamine, 10.0 parts of pure water, and 20 parts of methyl ethyl ketone was gradually added dropwise and reacted at 70°C for 4 hours to precipitate composite silica with an average particle size of 0.05 μm. A cloudy liquid was obtained. Furthermore, this cloudy liquid was concentrated under reduced pressure,
The heating residue was adjusted to 10%.

Silica Particles D 40 parts of a partial condensate of tetraethoxysilane (manufactured by Tama Chemical Industry Co., Ltd., trade name "Ethylsilicate-40"), propylene glycol monomethyl were placed in a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device. After charging 100 parts of ether and raising the temperature to 70°C, add 0.3 parts of ethylamine and 1 part of pure water.
0.0 part, propylene glycol monomethyl ether 2
5.0 parts of the mixed solution was gradually added dropwise and heated to 70℃ for 3 minutes.
A white cloudy liquid in which fine silica particles were precipitated was obtained by reacting for a period of time. 2.8 parts of tetra-i-propoxytitanium was diluted with 10 parts of propylene glycol monomethyl ether to the resulting solution, and the mixture was gradually added dropwise to the solution, and the mixture was reacted at 70°C for 2 hours to form composite silica with an average particle size of 0.1 μm. A white cloudy liquid was obtained. Furthermore, this cloudy liquid was concentrated under reduced pressure to obtain silica particles in the form of white fine powder solid.

Example 1 180 parts of a mixed solvent of propylene glycol/methyl ethyl ketone = 1/1 (weight ratio) was charged into a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device. company)
45.0 parts of was dissolved. 180 parts of silica dispersion A was blended, and after mixing and stirring at room temperature, a slightly cloudy resin liquid in which silica particles were dispersed was obtained. The heating residue of this liquid was 20%.

Example 2 A reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device was charged with 209.2 parts of a mixed solvent of propylene glycol methyl ether/methyl ethyl ketone = 1/1 (weight ratio), and polyvinyl butyral resin S-LEC BLM ( (manufactured by Sekisui Chemical Co., Ltd.) was dissolved. 112.0 parts of silica particle dispersion B was added to this, and 3 parts were added at 70°C.
After stirring and mixing for a period of time, a uniform pale white resin liquid was obtained. The heating residue of this liquid was 20%.

Comparative Example 1 A resin liquid was prepared by dissolving the polyvinyl butyral resin used in Example 1 using the same mixed solvent so that the residual amount on heating was 20%.

Comparative Example 2 310 parts of propylene glycol methyl ether/methyl ethyl ketone = 1/1 (weight ratio) was charged into a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device, and polyvinyl butyral resin S-LEC BLM (Sekisui Chemical Co., Ltd.) was charged. 52.3 parts of (manufactured by) were dissolved. Further, fine particulate silica particles Aerosil #200 (manufactured by Nippon Aerosil Industries Co., Ltd.) produced by a gas phase method were heated as they were at 70° C. for 3 hours to obtain a transparent resin liquid in which fine silica particles were dispersed. Furthermore, this liquid was concentrated under reduced pressure to adjust the heating residue to 20%.

Test Example 1 An electrogalvanized steel plate (0.5 mm x 70 mm x 15
0mm) to a dry film thickness of 20μm,
It was dried by heating at 0° C. for 10 minutes. This coated board was subjected to the following tests. The test results are summarized in Table 1.

○Pencil hardness test Using Mitsubishi Pencil Uni, according to JIS K-5400,
The scratches and peeling of the paint film were evaluated.

Cylindrical bending test After bending the test plate at 180 degrees using a 2 mm diameter cylinder, the bent portion was peeled off with cellophane tape. The presence or absence of peeling was observed. ○: No peeling △: Slight peeling ×: Peeling

Adhesion Test In the adhesion test, primary adhesion and secondary adhesion were tested. The primary adhesion test was performed by applying 10
The evaluation was carried out by cutting 0 goblets and attaching cellophane tape to these goblets and peeling them off. ○: No peeling △: Peeling 10% or less ×: Peeling 10% or more

○Salt water spray test After making cross cuts on the test plate, salt water spray test (JI
S-Z-2317) It was carried out for 120 hours. This result is shown in Table 2.
summarized in. For comparison, we also conducted tests on uncoated products, but 2
After 40 hours, red rust had appeared on almost the entire surface. The evaluation criteria was the width of corrosion on one side from the crosscut section as shown below. ○: No rust △: White rust 2mm or less ×: White rust 2mm or more

[0048]

[Table 1]

Example 3 37.7 parts of polyester resin PES-360 (manufactured by Toagosei Chemical Industry Co., Ltd.) and methyl ethyl ketone/toluene were placed in a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device.
Add 225 parts of a mixed solvent of 1/1 (weight ratio) and heat to 70°C.
After heating and dissolving the mixture, 112.5 parts of silica dispersion C was added dropwise, and the mixture was reacted at 70°C for 3 hours. This liquid was cooled to room temperature, and 17.5 parts of urea resin Cymel 303 (manufactured by Mitsui Toatsu Chemical Industries, Ltd.) was blended to obtain a pale white resin liquid in which fine silica particles were dispersed. The heating residue of this liquid is 20%
Met.

Example 4 37.7 parts of polyester resin PES-360 (manufactured by Toagosei Chemical Industry Co., Ltd.), methyl ethyl ketone/toluene/
After charging and dissolving 315 parts of a mixed solvent of propylene glycol methyl ether = 1/1/1 (weight ratio),
22.5 parts of silica particles D were blended and stirred and mixed at room temperature for 3 hours. Furthermore, 17.5 parts of urea resin Cymel 303 (manufactured by Mitsui Toatsu Chemical Industries, Ltd.) was blended to obtain a pale white resin liquid in which fine silica particles were dispersed. The heating residue of this liquid is 2
It was 0%.

Comparative Example 3 The polyester resin PES-360 used in Example 3 was
2.5 parts of Cymel 303, 17.5 parts of methyl ethyl ketone/toluene = 1/1 (weight ratio) mixed solvent 28
A resin solution dissolved in 0 parts was prepared.

Comparative Example 4 In a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device, 37.7 parts of polyester resin PES-360 (manufactured by Toagosei Chemical Industry Co., Ltd.), methyl ethyl ketone/toluene/
After charging and dissolving 315 parts of a mixed solvent of propylene glycol methyl ether = 1/1/1 (weight ratio),
Silica fine particles Aerosil R972 manufactured by vapor phase method (
(manufactured by Nippon Aerosil Industries Co., Ltd.) 22.5 parts,
The mixture was stirred and mixed at room temperature for 3 hours. Furthermore, urea resin Cymel 3
03 (manufactured by Mitsui Toatsu Chemical Industries, Ltd.) was blended to obtain a transparent resin liquid in which fine silica particles were dispersed. The heating residue of this liquid was 20%.

Test Example 2 The resin liquids prepared in Examples 3 and 4 and Comparative Examples 3 and 4 were subjected to the same test as Test Example 1. The results are shown in Table 2.

[0054]

[Table 2]

Example 5 310 parts of propylene glycol methyl ether/methyl ethyl ketone = 1/1 (weight ratio) was charged into a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device, and polyvinyl butyral resin S-LEC BLM (Sekisui Chemical Co., Ltd.) was charged. 52.3 parts of (manufactured by) were dissolved. After blending 80 parts of tetraethoxysilane and raising the temperature to 70°C, a mixed solution of 0.4 parts of ethylamine, 15.3 parts of pure water, and 40 parts of isopropanol was gradually added dropwise, and the mixture was left at 70°C. The reaction was carried out for 3 hours to obtain a slightly milky white resin liquid in which fine silica particles were precipitated. This liquid was concentrated under reduced pressure, and the heating residue was adjusted to 20%.

Example 6 80 parts of a mixed solvent of toluene/methyl ethyl ketone = 1/1 (weight ratio) was charged into a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device, and polyvinyl butyral resin S-LEC BLM (Sekisui Chemical Co., Ltd.) was added. 39.2 parts of (manufactured by) were dissolved. Furthermore, after blending 60 parts of tetramethoxysilane and raising the temperature to 40°C, a mixed solution of 21.5 parts of an ammonia aqueous solution diluted to 10% and 50 parts of methyl alcohol was gradually added dropwise, and the mixture was kept at 40°C for 3 hours. The reaction was carried out for a period of time to obtain a slightly cloudy liquid in which fine silica particles were precipitated. Furthermore, this slightly milky white liquid was concentrated under reduced pressure, and the heating residue was adjusted to 20%.

Test Example 3 The resin liquids prepared in Examples 5 and 6 were subjected to the same test as in Test Example 1. The results are shown in Table 3 together with Comparative Examples 1 and 2.

[0058]

[Table 3]

Example 7 In a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device, 37.7 parts of polyester resin PES360 (manufactured by Toagosei Kagaku Kogyo Co., Ltd.) and a partial condensate of tetraethoxysilane (manufactured by Tama Chemical Industry Co., Ltd.) were added. Company product name “Ethyl silicate”
40 parts of methyl ethyl ketone, 160 parts of propylene glycol monomethyl ether, and 60 parts of toluene were heated to 70°C and dissolved, followed by 0.3 parts of ethylamine, 10.0 parts of pure water, and propylene glycol monomethyl ether. 25.0 parts of the mixed solution was gradually added dropwise and the reaction was continued at 70° C. for 3 hours to obtain a slightly milky white solution in which fine silica particles were precipitated.

Comparative Example 5 A resin liquid was prepared by dissolving the polyester resin used in Example 7 in a solvent of methyl ethyl ketone/toluene = 1/1 (weight ratio).

Comparative Example 6 In a reaction vessel equipped with a dropping funnel, a thermometer, and a stirring device, 37.7 parts of polyester resin PES360 (manufactured by Toagosei Kagaku Kogyo Co., Ltd.) and finely powdered silica particles Aerosil #30 were placed.
0 (manufactured by Nippon Aerosil Industries Co., Ltd.), 200 parts of methyl ethyl ketone, 160 parts of propylene glycol monomethyl ether, and 60 parts of toluene were heated to 70°C and dissolved, followed by 0.3 parts of ethylamine and 10 parts of pure water.
0 parts, propylene glycol monomethyl ether 25.
0 parts of the mixed solution was gradually added dropwise, and the mixture was heated as it was at 70° C. for 3 hours to obtain a transparent solution in which fine silica particles were dispersed.

Test Example 4 The solvent was removed from the solutions prepared in Example 7 and Comparative Examples 5 and 6 on a Teflon sheet under reduced pressure to obtain a dry film with a thickness of 100 μm. Aluminum plate made from this film (A1050, 0.6mm x 25mm x 100mm)
Place it between the two and heat press at 150℃
Heat bonding was performed for 3 minutes. After cooling, tensile shear strength and peel strength were measured at room temperature and in an atmosphere of 50°C. The results are summarized in Table 4.

[0063]

[Table 4]

[0064]

[Effects of the Invention] The present invention provides a resin composition that can be called a novel silica composite resin, which has the characteristics of organic materials such as flexibility and moldability, and the hardness, heat resistance, and durability of inorganic materials. This resin composition can be handled in liquid form and has good applicability, and also has an excellent balance of transparency, flexibility, and strength, and has other properties. Because of its excellent adhesion to materials, it can be used for various purposes such as molding materials, rubber materials, film materials, paints, surface treatment agents, adhesives, sealants, etc., and is widely used in various industries. It is a great contribution to this.

Claims (2)

[Claims] 1. A resin composition comprising a resin having a hydroxyl group and silica particles produced by a sol-gel method. Claim 2: In the coexistence of a resin having a hydroxyl group,
2. The method for producing a resin composition according to claim 1, wherein the alkoxysilane is hydrolyzed using a basic catalyst.