JP2000303023A - Production of film-forming composition - Google Patents

Abstract

PROBLEM TO BE SOLVED: To obtain a film-forming composition which can give a coating film having an excellent balance among uniformity, dielectric properties, cracking resistance, hygroscopicity, or the like, by hydrolytically condensing a first organosilane in the presence of a previously prepared hydrolytic condensate of the first organosilane with a second organosilane having another structure. SOLUTION: A solution is prepared by dissolving 100 pts.wt. mixture of 50-95 mol% (A) organosilane represented by formula I (e.g. methyltrimethoxysilane) with 5-50 mol% (B) organosilane represented by formula II (e.g. tetramethoxysilane) in 20-4,000 pts.wt. organic solvent (e.g. n-pentane). After the addition of 0.01-0.2 mol, per mol of components A and B, water and 0.001-20 pts.wt., per 100 pts.wt. components A and B, catalyst (e.g. organic acid), the solution is subjected to a hydrolytic condensation reaction. After the addition of 0.005-0.5 mol of component A, water, and a catalyst, the reaction mixture is further subjected to a hydrolytic condensation reaction to obtain a composition having a weight-average molecular weight of 1,000-120,000. In the formulae, R1 is a monovalent organic group; and R2 is an alkyl, or the like.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

The present invention relates to a method for producing a film-forming composition, and more particularly to a method for forming a film having an appropriate uniform thickness as an interlayer insulating film in a semiconductor device or the like. The present invention relates to a method for producing a film-forming composition having excellent dielectric constant characteristics, crack resistance of a coating film, and low moisture absorption.

[0002]

2. Description of the Related Art Conventionally, a silica (SiO ₂ ) film formed by a vacuum process such as a CVD method has been frequently used as an interlayer insulating film in a semiconductor device or the like. And in recent years,
In order to form a more uniform interlayer insulating film, S
A coating type insulating film called a OG (Spin on Glass) film, which is mainly composed of a hydrolysis product of tetraalkoxylan, has been used. Also, with the high integration of semiconductor elements and the like, an interlayer insulating film having a low dielectric constant and mainly containing polyorganosiloxane called organic SOG has been developed. However, with higher integration of semiconductor devices and the like, better electrical insulation between conductors is required, and therefore, an interlayer insulating film material having a lower dielectric constant is required.

[0003] Japanese Patent Application Laid-Open No. 6-181201 discloses a coating composition for forming an insulating film having a lower dielectric constant as an interlayer insulating film material. The coating type composition has a low water absorption and is intended to provide an insulating film of a semiconductor device having excellent crack resistance.
Titanium, zirconium, niobium and tantalum; an organometallic compound containing at least one element selected from the group consisting of polycondensation of an organosilicon compound having at least one alkoxy group in the molecule; This is a coating composition for forming an insulating film, which is mainly composed of an oligomer.

[0004] WO96 / 00758 also discloses that
A silica-based coating-type insulating film that is used for forming an interlayer insulating film of a multilayer wiring board and that is made of an alkoxysilane, a metal alkoxide other than silane, and an organic solvent, and that can be applied in a thick film and has excellent oxygen plasma resistance. A forming material is disclosed.

Further, Japanese Patent Application Laid-Open No. Hei 3-20377 discloses a coating liquid for forming an oxide film, which is useful for flattening the surface of electronic parts and the like and for interlayer insulation. The coating solution for forming an oxide film provides a uniform coating solution without generation of a gel-like substance. Further, by using this coating solution, curing at a high temperature and treatment by oxygen plasma are performed. Even so, the purpose is to obtain a good oxide film without cracks. The composition is a coating solution for forming an oxide film obtained by hydrolyzing and polymerizing a predetermined silane compound and a predetermined chelate compound in the presence of an organic solvent.

However, as described above, when a metal chelate compound such as titanium or zirconium is combined with a silane compound, the uniformity of the coating film is not excellent, and the dielectric constant, crack resistance, low hygroscopicity and the like are well-balanced. Not something.

[0007]

SUMMARY OF THE INVENTION The present invention provides a method for producing a film-forming composition which is excellent in balance among uniformity, dielectric constant, crack resistance and low moisture absorption of a coating film. The purpose is to:

[0008]

Means for Solving the Problems The present invention relates to a process for preparing an aqueous solution of an organosilane (I) represented by the following general formula (I) and an organosilane (II) represented by the following general formula (II) in a solvent. In the presence of a decomposition condensate (hereinafter also referred to as "hydrolysis condensate"), an organosilane (I) represented by the following general formula (I)
And a method for producing a film-forming composition, wherein the composition is further hydrolyzed and condensed. R ¹ Si (OR ² ) ₃ ... (I) (wherein, R ¹ represents a monovalent organic group, and R ² represents the same or different and represents an alkyl group, an aryl group, or an acyl group.) Si (OR ² ) ₄ ... (II) (wherein R ² is the same or different and represents an alkyl group, an aryl group, or an acyl group.)

[0009]

BEST MODE FOR CARRYING OUT THE INVENTION According to the present invention, a hydrolyzed condensate of an organosilane (I) or (II) as a base polymer for forming a film is dissolved in a solvent, and in this presence, the organosilane (I) is further dissolved. , The hydrolysis / condensation of the organosilane (I) having three alkoxy groups and the organosilane (II) having four alkoxysilanes results in a three-dimensional structure. In this structure, the organosilane (I) further comprises
By repeating hydrolysis and condensation, a polyorganosiloxane having a high three-dimensional structure and a high molecular weight is produced. Then, when the composition of the present invention containing the produced polyorganosiloxane as a base polymer is applied to a substrate such as a silicon wafer by dipping or spin coating, for example,
The grooves between the fine patterns can be sufficiently filled, and when the organic solvent is removed by heating and thermal condensation polymerization is performed, a vitreous or macromolecular film can be formed. The obtained film has a low dielectric constant, does not cause cracks, and can form a thick insulator having a low water absorption. Hereinafter, the hydrolysis condensate, organosilane (I), organosilane (II), solvent and the like used in the present invention will be described, and then the production method of the present invention will be described in detail.

Hydrolytic condensate The hydrolytic condensate used in the present invention is obtained by hydrolyzing and condensing organosilane (I) and organosilane (II) in the presence of a solvent. In the present invention, the organosilane (I) and the organosilane (II)
Need to be hydrolyzed and condensed. By using this hydrolyzed condensate, an effect of obtaining a coating film having excellent crack resistance and a low water absorption can be obtained. The use of the organosilane (I) or the organosilane (II) itself before hydrolysis and condensation is not preferred because crack resistance is poor.

Here, the hydrolyzate of the organosilanes (I) to (II) does not need to have all of the OR ² groups contained in the organosilanes (I) to (II) hydrolyzed. It may be one in which only one is hydrolyzed, one in which two or more are hydrolyzed, or a mixture thereof. In addition, the organosilanes (I) to (I)
The condensate of (I) is a product in which silanol groups of the hydrolyzate of organosilanes (I) to (II) are condensed to form a Si—O—Si bond. In the present invention, all of the silanol groups are condensed. It is not necessary that the condensation be performed, and the concept includes a mixture of a small amount of silanol groups condensed and a mixture of compounds having different degrees of condensation.

Organosilane (I) The hydrolytic condensate and the organosilane (I) used for the post-addition are represented by the general formula (I). In the general formula (I), R ¹ is a monovalent organic group, preferably a monovalent organic group having 1 to 8 carbon atoms, for example, a methyl group, an ethyl group, an n-propyl group, an i-propyl group , N-
Butyl group, i-butyl group, sec-butyl group, t-butyl group, n-hexyl group, n-heptyl group, n-octyl group, alkyl group such as 2-ethylhexyl group, acetyl group, propionyl group, butyryl group , Valeryl group, benzoyl group, acyl group such as trioil group, vinyl group, allyl group, cyclohexyl group, phenyl group, glycidyl group,
In addition to (meth) acryloxy, ureido, amide, fluoracetamide, and isocyanate groups,
Substituted derivatives of these groups can be mentioned.

Examples of the substituent in the substituted derivative of R ¹ include a halogen atom, a substituted or unsubstituted amino group, a hydroxyl group, a mercapto group, an isocyanate group, a glycidoxy group, a 3,4-epoxycyclohexyl group, a (meth) An acryloxy group, a ureido group, an ammonium base and the like can be mentioned. However, the carbon number of R ¹ composed of these substituted derivatives is 8 or less including the carbon atom in the substituent.

The alkyl group for R ² is preferably an alkyl group having 1 to 5 carbon atoms, for example, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-propyl group.
-Butyl group, sec-butyl group, t-butyl group, n-pentyl group, and the like. Examples of the aryl group include phenyl, methylphenyl, ethylphenyl, chlorophenyl, bromophenyl, and fluorophenyl. The acyl group is preferably an acyl group having 1 to 6 carbon atoms, for example, an acetyl group, a propionyl group, a butyryl group, a valeryl group,
And a caproyl group. General formula (I)
A plurality of R ^{2 's} may be the same or different from each other.

As the organosilane (I) represented by the general formula (I), specifically, methyltrimethoxysilane, methyltriethoxysilane, methyltri-n-propoxysilane, methyltri-iso-propoxysilane, Methyltri-n-butoxysilane, methyltri-s
ec-butoxysilane, methyltri-tert-butoxysilane, methyltriphenoxysilane, ethyltrimethoxysilane, ethyltriethoxysilane, ethyltri-n-propoxysilane, ethyltri-iso-propoxysilane, ethyltri-n-butoxysilane, ethyltri- sec-butoxysilane, ethyl tri-tert
-Butoxysilane, ethyltriphenoxysilane, n-
Propyltrimethoxysilane, n-propyltriethoxysilane, n-propyltri-n-propoxysilane,
n-propyltri-iso-propoxysilane, n-propyltri-n-butoxysilane, n-propyltri-
sec-butoxysilane, n-propyltri-tert
-Butoxysilane, n-propyltriphenoxysilane, i-propyltrimethoxysilane, i-propyltriethoxysilane, i-propyltri-n-propoxysilane, i-propyltri-iso-propoxysilane, i-propyltri- n-butoxysilane, i-propyltri-sec-butoxysilane, i-propyltri-tert-butoxysilane, i-propyltriphenoxysilane, n-butyltrimethoxysilane, n-butyltriethoxysilane, n-butyltri- n-propoxysilane, n-butyltri-iso-propoxysilane, n-butyltri-n-butoxysilane, n-butyltri-sec-butoxysilane, n-butyltri-te
rt-butoxysilane, n-butyltriphenoxysilane, sec-butyltrimethoxysilane, sec-butyl-i-triethoxysilane, sec-butyl-tri-
n-propoxysilane, sec-butyl-tri-iso
-Propoxysilane, sec-butyl-tri-n-butoxysilane, sec-butyl-tri-sec-butoxysilane, sec-butyl-tri-tert-butoxysilane, sec-butyl-triphenoxysilane, t-butyltrimethoxy Silane, t-butyltriethoxysilane, t-butyltri-n-propoxysilane, t-butyltri-iso-propoxysilane, t-butyltri-
n-butoxysilane, t-butyltri-sec-butoxysilane, t-butyltri-tert-butoxysilane, t-butyltriphenoxysilane, phenyltrimethoxysilane, phenyltriethoxysilane, phenyltri-n-propoxysilane, phenyltrisilane -Iso-
Propoxysilane, phenyltri-n-butoxysilane, phenyltri-sec-butoxysilane, phenyltri-tert-butoxysilane, phenyltriphenoxysilane, vinyltrimethoxysilane, vinyltriethoxysilane, γ-aminopropyltrimethoxysilane, one kind of γ-aminopropyltriethoxysilane, γ-glycidoxypropyltrimethoxysilane, γ-glycidoxypropyltriethoxysilane, γ-trifluoropropyltrimethoxysilane, γ-trifluoropropyltriethoxysilane, etc. Two or more types are mentioned.

Organosilane (II) Organosilane (II) used in the above hydrolyzed condensate
Is represented by the above general formula (II). In general formula (II), R ² has the same meaning as R ² in formula (I),
They may be different within the same meaning.

As the organosilane (II) represented by the general formula (II), specifically, tetramethoxysilane,
Tetraethoxysilane, tetra-n-propoxysilane, tetra-iso-propoxysilane, tetra-n-
One or more of butoxysisilane, tetra-sec-butoxysisilane, tetra-tert-butoxysisilane, tetraphenoxysisilane and the like can be mentioned.

The ratio of the organosilane (I) to the organosilane (II) in the hydrolysis condensate is 50 to 95 mol%, preferably 55 to 90 mol%, and 5 to 50 mol% of the organosilane (I). Mol%, preferably 10 to 45 mol% (provided that (I) + (II) = 100 mol%). If the organosilane (II) is less than 5 mol%, the crack resistance is poor, while if it exceeds 50 mol%, the storage stability of the solution may be degraded.

As the hydrolyzed condensate, a product obtained by previously hydrolyzing and condensing organosilanes (I) to (II) can be used, but the organosilane (I) can be used in the presence of the solvent used in the present invention. ) To (II) and further adding an appropriate amount of water to the organosilane (I).
To (II) are preferably hydrolyzed and condensed to obtain a hydrolyzed condensate. The polystyrene-equivalent weight average molecular weight (hereinafter also referred to as “Mw”) of the hydrolyzed condensate is preferably from 800 to 100,000, more preferably 1,
000 to 50,000.

On the other hand, the organosilane (I) added later in the solvent in the presence of the above hydrolyzed condensate is the same as the organosilane (I) used in the hydrolyzed condensate. The organosilane (I) is further mixed in the presence of the above hydrolyzed condensate and subjected to hydrolysis and condensation, whereby the organosilane (I) is further reduced in the three-dimensional structure of the hydrolyzed condensate. Is repeatedly hydrolyzed and condensed to form a macromolecule. The ratio of the organosilane (I) added later to the condensate is determined by the amount of the organosilane (I) used in the hydrolyzed condensate.
To (II): 1 to 1 mol, and 0.05 to 0.5
Mole, preferably 0.05-0.4 mole. 0.
If the amount is less than 05 mol, the hygroscopicity of the coating film may be deteriorated. On the other hand, if it exceeds 0.5 mol, the crack resistance becomes poor.

In the present invention, the use of the organosilanes (I) to (II) used in the hydrolysis condensate and the organosilane (I) added later in the above range allows
A film-forming composition capable of forming a cured product having a better balance between heat resistance and low dielectric properties is obtained.

In the present invention, an organosilane (III) represented by the following general formula (III) may be used in the reaction system at an optional stage in an amount of about 20 mol% or less in all the organosilanes. it can. (R ¹ ) ₂ Si (OR ² ) ₂ ... (III) (wherein R ¹ is the same or different and represents a monovalent organic group, R ² is the same or different, and is an alkyl group or an aryl group. Or an acyl group.) In the general formula (III), R ¹
And R ² have the same meanings as R ¹ and R ² in formula (I), and may be different within the same meaning.

Specific examples of the organosilane (III) represented by the general formula (III) include dimethyldimethoxysilane, dimethyldiethoxysilane, dimethyl-di-n-propoxysilane, and dimethyl-di-iso-propoxysilane. Silane, dimethyl-di-n-butoxysilane, dimethyl-
Di-sec-butoxysilane, dimethyl-di-tert
-Butoxysilane, dimethyldiphenoxysilane, diethyldimethoxysilane, diethyldiethoxysilane, diethyl-di-n-propoxysilane, diethyl-di-i
so-propoxysilane, diethyl-di-n-butoxysilane, diethyl-di-sec-butoxysilane, diethyl-di-tert-butoxysilane, diethyldiphenoxysilane, di-n-propyldimethoxysilane, di-n-propyl Diethoxysilane, di-n-propyl-
Di-n-propoxysilane, di-n-propyl-di-i
so-propoxysilane, di-n-propyl-di-n-
Butoxysilane, di-n-propyl-di-sec-butoxysilane, di-n-propyl-di-tert-butoxysilane, di-n-propyl-di-phenoxysilane,
Di-iso-propyldimethoxysilane, di-iso-
Propyldiethoxysilane, di-iso-propyl-di-n-propoxysilane, di-iso-propyl-di-
iso-propoxysilane, di-iso-propyl-di-n-butoxysilane, di-iso-propyl-di-s
ec-butoxysilane, di-iso-propyl-di-t
tert-butoxysilane, di-iso-propyl-di-
Phenoxysilane, di-n-butyldimethoxysilane,
Di-n-butyldiethoxysilane, di-n-butyl-di-n-propoxysilane, di-n-butyl-di-iso
-Propoxysilane, di-n-butyl-di-n-butoxysilane, di-n-butyl-di-sec-butoxysilane, di-n-butyl-di-tert-butoxysilane,
Di-n-butyl-di-phenoxysilane, di-sec-
Butyldimethoxysilane, di-sec-butyldiethoxysilane, di-sec-butyl-di-n-propoxysilane, di-sec-butyl-di-iso-propoxysilane, di-sec-butyl-di-n-butoxy Silane,
Di-sec-butyl-di-sec-butoxysilane, di-sec-butyl-di-tert-butoxysilane, di-sec-butyl-di-phenoxysilane, di-ter
t-butyldimethoxysilane, di-tert-butyldiethoxysilane, di-tert-butyl-di-n-propoxysilane, di-tert-butyl-di-iso-propoxysilane, di-tert-butyl-di-n -Butoxysilane, di-tert-butyl-di-sec-butoxysilane, di-tert-butyl-di-tert-butoxysilane, di-tert-butyl-di-phenoxysilane, diphenyldimethoxysilane, diphenyl-di-ethoxy Silane, diphenyl-di-n-propoxysilane, diphenyl-di-iso-propoxysilane, diphenyl-di-n-butoxysilane, diphenyl-di-
sec-butoxysilane, diphenyl-di-tert-
One or more kinds such as butoxysilane and diphenyldiphenoxysilane are exemplified.

Solvents The organic solvents used in the present invention include, for example, n-pentane, i-pentane, n-hexane, i-hexane, n-pentane
Aliphatic hydrocarbon solvents such as heptane, i-heptane, 2,2,4-trimethylpentane, n-octane, i-octane, cyclohexane and methylcyclohexane; benzene, toluene, xylene, ethylbenzene,
Trimethylbenzene, methylethylbenzene, n-propylbenzene, i-propylbenzene, diethylbenzene, i-butylbenzene, triethylbenzene, di-i
Aromatic hydrocarbon solvents such as -propylbenzene, n-amylnaphthalene and trimethylbenzene; methanol,
Ethanol, n-propanol, i-propanol, n
-Butanol, i-butanol, sec-butanol,
t-butanol, n-pentanol, i-pentanol, 2-methylbutanol, sec-pentanol, t
-Pentanol, 3-methoxybutanol, n-hexanol, 2-methylpentanol, sec-hexanol, 2-ethylbutanol, sec-heptanol, heptanol-3, n-octanol, 2-ethylhexanol, sec-octanol, n -Nonyl alcohol, 2,6-dimethylheptanol-4, n-decanol, sec-undecyl alcohol, trimethylnonyl alcohol, sec-tetradecyl alcohol, sec
-Monoalcohol solvents such as heptadecyl alcohol, phenol, cyclohexanol, methylcyclohexanol, 3,3,5-trimethylcyclohexanol, benzyl alcohol, phenylmethylcarbinol, diacetone alcohol, cresol; ethylene glycol, 1,2 Propylene glycol, 1,3-butylene glycol, pentanediol-2,4, 2-methylpentanediol-2,4, hexanediol-2,5,
Polyhydric alcohol solvents such as heptanediol-2,4,2-ethylhexanediol-1,3, diethylene glycol, dipropylene glycol, triethylene glycol, tripropylene glycol, glycerin; acetone, methyl ethyl ketone, methyl-n-propyl ketone , Methyl-n-butyl ketone, diethyl ketone, methyl-i-butyl ketone, methyl-n-pentyl ketone,
Ethyl-n-butyl ketone, methyl-n-hexyl ketone, di-i-butyl ketone, trimethylnonanone, cyclohexanone, methylcyclohexanone, 2-hexanone, 2,4-pentanedione, acetonylacetone, diacetone alcohol, acetophenone, phen Ketone solvents such as Chong; ethyl ether, i-propyl ether, n-butyl ether, n-hexyl ether;
-Ethylhexyl ether, ethylene oxide, 1,2
-Propylene oxide, dioxolan, 4-methyldioxolan, dioxane, dimethyldioxane, ethylene glycol monomethyl ether, ethylene glycol monoethyl ether, ethylene glycol diethyl ether, ethylene glycol mono-n-butyl ether, ethylene glycol mono-n-hexyl ether, ethylene Glycol monophenyl ether, ethylene glycol mono-2-ethyl butyl ether, ethylene glycol dibutyl ether, diethylene glycol monomethyl ether, diethylene glycol monoethyl ether,
Diethylene glycol diethyl ether, diethylene glycol mono-n-butyl ether, diethylene glycol di-n-butyl ether, diethylene glycol mono-n-hexyl ether, ethoxytriglycol,
Tetraethylene glycol di-n-butyl ether, propylene glycol monomethyl ether, propylene glycol monoethyl ether, propylene glycol monopropyl ether, propylene glycol monobutyl ether, dipropylene glycol monomethyl ether, dipropylene glycol monoethyl ether, tripropylene glycol monomethyl ether, Ether solvents such as tetrahydrofuran and 2-methyltetrahydrofuran; diethyl carbonate, methyl acetate, ethyl acetate, γ-butyrolactone, γ-valerolactone, n-propyl acetate, i-propyl acetate, n-butyl acetate, i-butyl acetate; Sec-butyl acetate, n-pentyl acetate, sec-pentyl acetate, 3-methoxybutyl acetate,
Methylpentyl acetate, 2-ethylbutyl acetate, 2-acetic acid
Ethylhexyl, benzyl acetate, cyclohexyl acetate,
Methyl cyclohexyl acetate, n-nonyl acetate, methyl acetoacetate, ethyl acetoacetate, ethylene glycol monomethyl ether acetate, ethylene glycol monoethyl ether acetate, diethylene glycol monomethyl ether acetate, diethylene glycol monoethyl acetate,
Diethylene glycol mono-n-butyl ether acetate,
Propylene glycol monomethyl ether acetate, propylene glycol monoethyl ether acetate, propylene glycol monopropyl ether acetate, propylene glycol monobutyl ether acetate, dipropylene glycol monomethyl ether acetate, dipropylene glycol monoethyl ether acetate, glycol diacetate, methoxytriglycol acetate, Ethyl propionate, propionate n
-Butyl, i-amyl propionate, diethyl oxalate, di-n-butyl oxalate, methyl lactate, ethyl lactate, n-butyl lactate, n-amyl lactate, diethyl malonate, dimethyl phthalate, diethyl phthalate and the like Ester solvents such as N-methylformamide, N, N-dimethylformamide, N, N-diethylformamide, acetamide, N-methylacetamide, N, N-dimethylacetamide, N-methylpropionamide, N-methylpyrrolidone, etc. Nitrogen-based solvents; examples thereof include sulfur-containing solvents such as dimethyl sulfide, diethyl sulfide, thiophene, tetrahydrothiophene, dimethyl sulfoxide, sulfolane, and 1,3-propane sultone. These can be used alone or in combination of two or more. These organic solvents can be used as the above-mentioned organosilane (I)
To (II), 100 to 100 parts by weight,
00 parts by weight, preferably 100 to 2,000 parts by weight.

[0025] In the production method of the composition of the water present invention is usually in addition to the above solvent, for hydrolysis of the organosilane (I) ~ (II), water is used. In the present invention, water, preferably ion-exchanged water, hydrolyzes and condenses organosilanes (I) to (II) in the above solvent in the presence of the above hydrolyzed condensate. , Continuously or intermittently or batchwise. When water is continuously added, the water is added in an amount of 0.5 equivalent / min or less, preferably 0.001 to 0.05, per 1 mol of the organosilane (I) to (II).
Equivalent / min, more preferably 0.001-0.01 equivalent /
Add at a rate of minutes. In the case of intermittent addition, the amount of water to be added at one time is from organosilane (I) to
(II) 0.01 to 0.2 mol, preferably 0.05 to 0.1 mol, per 1 mol, and 2 to 2 mol between each addition.
It is preferable to leave at least about 0 minutes. The total amount of water added to the mixture, a group [here represented by -OR ^2, as the -OR ² group, organosilane (I) ~ (I
I) all)
It is from 0.3 to 3 mol, preferably from 0.4 to 2.5 mol. If the value of the range the total amount of water added is based on per mole 0.3 to 3 mol represented by -OR ^2, uniformity of the coating film is not to be reduced, also for film formation This is because the storage stability of the composition is less likely to be reduced.

In the present invention, the water added to the reaction system is
It may contain an organic solvent. As the organic solvent to be contained in water, those similar to the above-mentioned solvents can be exemplified. The proportion of the organic solvent that can be contained in water is usually 0 to 20 times the weight of water, preferably 0.5 to 10 times the weight of water. By containing an organic solvent in water, it becomes easier to carry out hydrolysis and condensation of the organosilanes (I) to (II) while suppressing gelation.

When water is added to the reaction system continuously, intermittently or collectively, the temperature of the reaction system is usually from 10 to 9:
0 ° C, preferably 20-70 ° C. The addition of water is usually performed while stirring the mixture.

The film-forming composition of the present invention is obtained by a hydrolysis / condensation reaction of an organosilane, and it is preferable to add a catalyst to accelerate the reaction. The catalyst used at this time includes a metal chelate compound, an organic acid,
Examples include inorganic acids, organic bases, and inorganic bases. Examples of the metal chelate compound include triethoxy mono (acetylacetonate) titanium, tri-n-propoxy mono (acetylacetonate) titanium, and tri-i.
-Propoxy mono (acetylacetonate) titanium,
Tri-n-butoxy mono (acetylacetonate) titanium, tri-sec-butoxy mono (acetylacetonate) titanium, tri-t-butoxy mono (acetylacetonate) titanium, diethoxybis (acetylacetonate) Titanium, di-n-propoxybis (acetylacetonato) titanium, di-i-propoxybis (acetylacetonato) titanium, di-n-butoxy.
Bis (acetylacetonato) titanium, di-sec-butoxybis (acetylacetonato) titanium, di-t
-Butoxy bis (acetylacetonate) titanium, monoethoxy tris (acetylacetonate) titanium,
Mono-n-propoxy tris (acetylacetonate) titanium, mono-i-propoxy tris (acetylacetonate) titanium, mono-n-butoxy tris (acetylacetonate) titanium, mono-sec-butoxy tris ( Acetylacetonate) titanium, mono-
t-butoxy tris (acetylacetonate) titanium, tetrakis (acetylacetonate) titanium, triethoxy mono (ethyl acetoacetate) titanium, tri-n-propoxy mono (ethyl acetoacetate)
Titanium, tri-i-propoxy mono (ethyl acetoacetate) titanium, tri-n-butoxy mono (ethyl acetoacetate) titanium, tri-sec-butoxy.
Mono (ethyl acetoacetate) titanium, tri-t-butoxy mono (ethyl acetoacetate) titanium, diethoxy bis (ethyl acetoacetate) titanium, di-
n-propoxybis (ethylacetoacetate) titanium, di-i-propoxybis (ethylacetoacetate) titanium, di-n-butoxybis (ethylacetoacetate) titanium, di-sec-butoxybis (ethylacetate) Acetate) titanium, di-t-butoxybis (ethylacetoacetate) titanium, monoethoxytris (ethylacetoacetate) titanium, mono-n-propoxytris (ethylacetoacetate) titanium,
Mono-i-propoxy tris (ethyl acetoacetate) titanium, mono-n-butoxy tris (ethyl acetoacetate) titanium, mono-sec-butoxy tris (ethyl acetoacetate) titanium, mono-t-butoxy tris ( Ethyl acetoacetate) titanium, tetrakis (ethyl acetoacetate) titanium, mono (acetylacetonate) tris (ethyl acetoacetate)
Titanium chelate compounds such as titanium, bis (acetylacetonate) bis (ethylacetoacetate) titanium, tris (acetylacetonate) mono (ethylacetoacetate) titanium; triethoxymono (acetylacetonato) zirconium, tri-n-propoxy Mono (acetylacetonato) zirconium, tri-i-propoxymono (acetylacetonato) zirconium, tri-n-butoxymono (acetylacetonato) zirconium, tri-sec-butoxymono (acetylacetonato) zirconium Tri-t-butoxy mono (acetylacetonate) zirconium, diethoxybis (acetylacetonate) zirconium,
Di-n-propoxybis (acetylacetonato) zirconium, di-i-propoxybis (acetylacetonato) zirconium, di-n-butoxybis (acetylacetonato) zirconium, di-sec-butoxybis ( Acetylacetonato) zirconium, di-t-butoxybis (acetylacetonato) zirconium, monoethoxytris (acetylacetonato) zirconium, mono-n-propoxytris (acetylacetonato) zirconium, mono-i-propoxy・ Tris (acetylacetonate) zirconium,
Mono-n-butoxy tris (acetylacetonate)
Zirconium, mono-sec-butoxy tris (acetylacetonate) zirconium, mono-t-butoxy tris (acetylacetonate) zirconium, tetrakis (acetylacetonate) zirconium, triethoxy mono (ethylacetoacetate) zirconium, tri- n-propoxy mono (ethyl acetoacetate) zirconium, tri-i-propoxy mono (ethyl acetoacetate) zirconium, tri-n-butoxy mono (ethyl acetoacetate) zirconium,
Tri-sec-butoxy mono (ethyl acetoacetate) zirconium, tri-t-butoxy mono (ethyl acetoacetate) zirconium, diethoxy bis (ethyl acetoacetate) zirconium, di-n-propoxy bis (ethyl acetoacetate) Zirconium, di-i-propoxybis (ethylacetoacetate) zirconium, di-n-butoxybis (ethylacetoacetate) zirconium, di-sec-butoxybis (ethylacetoacetate) zirconium, di-
t-butoxybis (ethylacetoacetate) zirconium, monoethoxytris (ethylacetoacetate) zirconium, mono-n-propoxytris (ethylacetoacetate) zirconium, mono-i-propoxytris (ethylacetoacetate) zirconium Mono-n-butoxy tris (ethyl acetoacetate) zirconium, mono-sec-butoxy tris (ethyl acetoacetate) zirconium, mono-t-
Butoxy / tris (ethylacetoacetate) zirconium, tetrakis (ethylacetoacetate) zirconium, mono (acetylacetonate) tris (ethylacetoacetate) zirconium, bis (acetylacetonate) bis (ethylacetoacetate) zirconium, tris (acetylacetate) Zirconium chelate compounds such as (nate) mono (ethylacetoacetate) zirconium; aluminum chelate compounds such as tris (acetylacetonate) aluminum and tris (ethylacetoacetate) aluminum;

Examples of the organic acid include acetic acid, propionic acid, butanoic acid, pentanoic acid, hexanoic acid, heptanoic acid, octanoic acid, nonanoic acid, decanoic acid, oxalic acid, maleic acid, methylmalonic acid, adipic acid and sebacin Acid, gallic acid, butyric acid, melitic acid, arachidonic acid, mykimic acid,
2-ethylhexanoic acid, oleic acid, stearic acid, linoleic acid, linoleic acid, salicylic acid, benzoic acid, p-
Aminobenzoic acid, p-toluenesulfonic acid, benzenesulfonic acid, monochloroacetic acid, dichloroacetic acid, trichloroacetic acid, trifluoroacetic acid, formic acid, malonic acid, sulfonic acid, phthalic acid, fumaric acid, citric acid, tartaric acid, and the like. it can. Examples of the inorganic acid include hydrochloric acid, nitric acid, sulfuric acid, hydrofluoric acid, phosphoric acid and the like.

Examples of the organic base include pyridine, pyrrole, piperazine, pyrrolidine, piperidine, picoline, trimethylamine, triethylamine, monoethanolamine, diethanolamine, dimethylmonoethanolamine, monomethyldiethanolamine, triethanolamine, diazabicyclooctane, Examples thereof include diazabicyclononane, diazabicycloundecene, and tetramethylammonium hydroxide. Examples of the inorganic base include ammonia, sodium hydroxide, potassium hydroxide, barium hydroxide, calcium hydroxide and the like. Among these catalysts, metal chelate compounds, organic acids, and inorganic acids are preferred,
More preferred are a titanium chelate compound and an organic acid. These may be used alone or in combination of two or more.

The amount of the above-mentioned catalyst used is usually based on 100 parts by weight of the total amount of the above-mentioned organosilanes (I) to (II).
0.001 to 20 parts by weight, preferably 0.005 to 20
It is in the range of parts by weight.

The film forming composition of the present invention may further contain the following components. β-diketone β-diketone functions as a stability improver of the composition. That is, the β-diketone is coordinated with the polyorganosiloxane to form a hydrolyzed condensate of the organosilanes (I) to (II) by this compound or a co-polymer of the hydrolyzed condensate with the organosilane (I). It is considered that by appropriately controlling the action of accelerating the condensation reaction, the action of further improving the storage stability of the obtained composition is achieved.

Examples of the β-diketone include acetylacetone, 2,4-hexanedione, 2,4-heptanedione, 3,5-heptanedione, 2,4-octanedione, 3,5-octanedione, 2,4 -Nonanion,
3,5-nonanedione, 5-methyl-2,4-hexanedione, 2,2,6,6-tetramethyl-3,5-heptanedione, 1,1,1,5,5,5-hexafluoro- One or more of 2,4-heptanedione, dimethyl malonate, diethyl malonate and the like. In the present invention, the content of β-diketone in the film-forming composition is preferably 1 to 50% by weight, more preferably 3 to 30% by weight of the total solvent. If the β-diketone is added in such a range, a certain storage stability can be obtained, and characteristics such as uniformity of the coating film of the film-forming composition are less likely to deteriorate. Β-diketone is an organosilane (I)
To 100 parts by weight of the total amount of
To 100 parts by weight, preferably 0.2 to 80 parts by weight. This β-diketone is preferably added after the hydrolysis and condensation reaction of the organosilane.

Other Additives Components such as colloidal silica, colloidal alumina, organic polymer and surfactant may be further added to the film-forming composition obtained in the present invention. Colloidal silica is, for example, a dispersion in which high-purity silicic anhydride is dispersed in the hydrophilic organic solvent, and usually has an average particle size of 5 to 30 m.
μ, preferably 10-20 μm, solid content concentration of 10-4
It is about 0% by weight. Examples of such colloidal silica include methanol silica sol and isopropanol silica sol manufactured by Nissan Chemical Industry Co., Ltd .; and Oscar manufactured by Catalyst Chemicals Co., Ltd. Examples of the colloidal alumina include alumina sols 520, 100, and 200 manufactured by Nissan Chemical Industries, Ltd .; and alumina clear sol, alumina sol 10, and 132 manufactured by Kawaken Fine Chemicals Co., Ltd. Examples of the organic polymer include a compound having a polyalkylene oxide structure, a compound having a sugar chain structure, a vinylamide polymer, a (meth) acrylate compound, an aromatic vinyl compound, a dendrimer, a polyimide, a polyamic acid, a polyarylene, and a polyamide. Examples thereof include polyquinoxaline, polyoxadiazole, and a fluoropolymer. Examples of the surfactant include a nonionic surfactant, an anionic surfactant, a cationic surfactant, an amphoteric surfactant, and the like. Further, a silicone surfactant, a polyalkylene oxide surfactant Agents, fluorine-containing surfactants and the like. In the film-forming composition obtained in the present invention, the sodium content in the film-forming composition is preferably set to a value within 20 ppb. By limiting the sodium content to such a range, there is no possibility that the reliability of an electric circuit or the like will be reduced even when used for a material for an interlayer insulating film such as a semiconductor.
Further, it is possible to form an interlayer insulating film having a uniform thickness while preventing the occurrence of corrosion more efficiently.

Further, in constituting the film forming composition, the content of the alcohol having a boiling point of 100 ° C. or less in the film forming composition is preferably 20% by weight or less, particularly preferably 5% by weight or less. The alcohol having a boiling point of 100 ° C. or lower may be generated during the hydrolysis and / or condensation of the above-mentioned organosilanes (I) to (III) or the co-condensation of the above-mentioned hydrolyzed condensate with the organosilane (I). , Is preferably removed by distillation or the like so that the content thereof is 20% by weight or less, preferably 5% by weight or less. When the content of the alcohol having a boiling point of 100 ° C. or less in the film forming composition is 20% by weight or less, there is no possibility that the uniformity of the coating film is reduced.

Method for Preparing Film-Forming Composition In preparing the film-forming composition of the present invention, the above-mentioned organosilane (I) is mixed in a solvent in the presence of the above-mentioned hydrolytic condensate, It only has to be hydrolyzed and condensed,
There is no particular limitation. However, when the above-mentioned metal chelate compound and β-diketones are used, a method of preparing the composition and then finally adding β-diketone is adopted.

Specific examples of the method for preparing the composition of the present invention include the following methods. A predetermined amount of water and a catalyst are added to a mixture comprising the organosilanes (I) to (II) and a required amount of an organic solvent to carry out a hydrolysis / condensation reaction.
, Water and a catalyst are added to carry out hydrolysis and condensation of (I). A predetermined amount of water and a catalyst are added to a mixture composed of the organosilanes (I) to (II) and a required amount of an organic solvent to carry out a hydrolysis / condensation reaction, and then an alcohol component produced by the reaction is removed under reduced pressure. , Organosilane (I)
, Water and a catalyst are added to carry out hydrolysis and condensation of (I).

A predetermined amount of water and a catalyst are added to a mixture comprising the organosilanes (I) to (II) and a required amount of an organic solvent to carry out a hydrolysis / condensation reaction, and then the organosilane (I), water and A method comprising adding a catalyst, hydrolyzing and condensing (I), and removing the alcohol component produced by the reaction under reduced pressure. A predetermined amount of water and a catalyst are added to a mixture composed of the organosilanes (I) to (II) and a required amount of an organic solvent to carry out a hydrolysis / condensation reaction, and then an alcohol component produced by the reaction is removed under reduced pressure. , Organosilane (I)
, Water and a catalyst, hydrolyzing and condensing (I), and removing an alcohol component produced by the reaction under reduced pressure.

A predetermined amount of water and a catalyst are added to a mixture comprising the organosilanes (I) to (II) and a required amount of an organic solvent to carry out a hydrolysis / condensation reaction, and then the organosilane (I), water and A method comprising adding a catalyst, hydrolyzing and condensing (I), and then adding a β-diketone to the resulting composition. A predetermined amount of water and a catalyst are added to a mixture composed of the organosilanes (I) to (II) and a required amount of an organic solvent to carry out a hydrolysis / condensation reaction, and then an alcohol component produced by the reaction is removed under reduced pressure. , Organosilane (I)
, Water and a catalyst, hydrolyzing and condensing (I), and then adding a β-diketone to the resulting composition.

A predetermined amount of water and a catalyst are added to a mixture comprising the organosilanes (I) to (II) and a required amount of an organic solvent to carry out a hydrolysis / condensation reaction, and then the organosilane (I), water and A method comprising adding a catalyst, hydrolyzing and condensing (I), removing an alcohol component produced by the reaction under reduced pressure, and then adding β-diketone to the resulting composition. A predetermined amount of water and a catalyst are added to a mixture composed of the organosilanes (I) to (II) and a required amount of an organic solvent to carry out a hydrolysis / condensation reaction, and then an alcohol component produced by the reaction is removed under reduced pressure. , Organosilane (I)
, Water and a catalyst, hydrolyzing and condensing (I), removing an alcohol component produced by the reaction under reduced pressure, and then adding a β-diketone to the resulting composition.

The total solid content of the composition of the present invention thus obtained is preferably 2 to 30% by weight,
It is appropriately adjusted according to the purpose of use. When the total solid content of the composition is less than 2% by weight, the thickness of the obtained coating film becomes too thin, and when it exceeds 30% by weight, the storage stability tends to decrease. The weight average molecular weight of all the polyorganosilane components [(I) to (II)] in the composition thus obtained is usually 1,000 to 120,000, preferably 1,200 to 100,000. It is about 000.

When the composition of the present invention thus obtained is applied to a substrate such as a silicon wafer, a SiO ₂ wafer or a SiN wafer, a spin coating method, a dipping method,
A coating means such as a roll coating method and a spray method is used.

In this case, a dry film thickness may be about 0.05 to 1.5 μm in a single coating, and about 0.1 to 3 μm in a double coating. it can. Thereafter, by drying at room temperature, or by heating at a temperature of about 80 to 600 ° C., usually for about 5 to 240 minutes, the glassy or macromolecular insulating film can be formed. As a heating method at this time, a hot plate, an oven, a furnace, or the like can be used, and as a heating atmosphere, the heating is performed in the atmosphere, a nitrogen atmosphere, an argon atmosphere, a vacuum, a reduced pressure with controlled oxygen concentration, or the like. Can be.

The film thus obtained is excellent in insulating properties, uniformity of the coating film, dielectric constant, crack resistance of the coating film and low moisture absorption of the coating film.
, DRAM, SDRAM, RDRAM, D-RDRA
It is useful for applications such as an interlayer insulating film for semiconductor devices such as M, a protective film such as a surface coat film of a semiconductor device, an interlayer insulating film for a multilayer wiring board, a protective film for a liquid crystal display device, and an insulating prevention film.

[0045]

The present invention will now be described more specifically with reference to examples. Parts and% in Examples and Comparative Examples are parts by weight and% by weight, respectively, unless otherwise specified. Further, the evaluation of the film-forming composition in the examples was measured as follows.

<Film Thickness Uniformity> The film-forming composition was applied on an 8-inch silicon wafer by using a spin coater under the conditions of a rotation speed of 2,000 rpm and 20 seconds. Thereafter, using a hot plate maintained at a temperature of 80 ° C., the silicon wafer coated with the film-forming composition was heated for 5 minutes to disperse the organic solvent. Next, using a hot plate maintained at a temperature of 200 ° C., the silicon wafer coated with the film-forming composition was heated for 5 minutes to form a coating film on the silicon wafer. The film thickness of the coating film thus obtained is measured by an optical film thickness meter (Rudolph Tech).
Spectra Laser2 manufactured by Nologies
00) were measured at 50 points in the coating film surface. 3σ of the obtained film thickness was calculated and evaluated according to the following criteria. ：: 3σ of coating film is less than 100 nm ×: 3σ of coating film is 100 nm or more

<Dielectric constant> On an 8-inch silicon wafer,
The composition sample was applied by spin coating, the substrate was dried on a hot plate at 80 ° C. for 5 minutes and at 200 ° C. for 5 minutes, and further baked in a nitrogen atmosphere oven at 440 ° C. for 60 minutes. Aluminum was vapor-deposited on the obtained substrate to produce a substrate for permittivity evaluation. The dielectric constant was calculated from the capacitance value at 100 kHz using an HP16451B electrode manufactured by Yokogawa-Hewlett-Packard Co., Ltd. and an HP4284A precision LCR meter.

<Crack Resistance> A composition sample was applied on an 8-inch silicon wafer by a spin coating method, and the substrate was dried on a hot plate at 80 ° C. for 5 minutes and at 200 ° C. for 5 minutes. The substrate was baked in a nitrogen atmosphere oven at 60 ° C. for 60 minutes. Final coating thickness is 1.0μ
m. The appearance of the obtained coating film was observed with a 350,000 lux surface observation lamp, and evaluated according to the following criteria. ：: No crack is observed on the coating film surface. ×: Crack is observed on the coating film surface.

<Wet and Heat Resistance> A composition sample was applied on an 8-inch silicon wafer by spin coating, and the substrate was dried on a hot plate at 80 ° C. for 5 minutes and at 200 ° C. for 5 minutes, and further dried at 440 ° C. 6 in a nitrogen atmosphere oven
The substrate was baked for 0 minutes. PCT (Pressure)
Cooker Test device (PC, manufactured by Hirayama Seisakusho)
-242HS-A), 127 ° C, 100% R
The wet heat treatment was performed under the conditions of H, 2.5 atm and 2 hours. Thereafter, the coating film subjected to the wet heat treatment is subjected to JIS K54
A cross-cut test (tape peel test) was performed in accordance with No. 00. Then, an average value (n) of the number of grids which did not peel from the silicon wafer as a base without peeling out of the 100 grids was calculated and evaluated as adhesion to the ground. ：: n is 100 Δ: n is 50 or more ×: n is less than 50

Example 1 Preparation of Film Forming Composition 203 parts of methyltrimethoxysilane (MTMSi), 50 parts of tetramethoxysilane (TMSi), isopropoxytitanium tetraethylacetyl acetate (TiEA)
A) After mixing 1 part with 140 parts of propylene glycol monopropyl ether (PFG), the mixture was stirred with a three-one motor, and the liquid temperature was stabilized at 50 ° C. next,
A mixed solution of 100 parts of ion-exchanged water and 100 parts of PFG was continuously added over 1 hour. Thereafter, the reaction solution was reacted at 50 ° C. for 4 hours. The weight average molecular weight of this hydrolysis condensate was 4,900. Next, 50 parts of MTMSi was further added to this reaction system,
After reacting at 50 ° C. for 2 hours, acetylacetone (A
cAc) 50 parts was added, and the mixture was further reacted at 50 ° C. for 1 hour. After allowing the reaction solution to cool to room temperature, PF
150 parts of G were added. Finally, a film-forming composition was obtained by removing 150 parts of a solvent containing methanol from the reaction solution by evaporation. The methanol content of the obtained film-forming composition was measured by gas chromatography and found to be 2% or less. The weight average molecular weight of the above organosilane condensate was 5,900. Evaluation of Film Forming Composition The uniformity of thickness, dielectric constant, crack resistance and hygroscopicity of the coating film were evaluated and measured under the above-described evaluation conditions. Table 1 shows the measurement results.

Example 2 Preparation of Film Forming Composition 203 parts of MTMSi, 70 parts of TMSi, TiEAA1
And 140 parts of PFG, and the mixture was stirred with a three-one motor to stabilize the liquid temperature at 50 ° C. next,
A mixed solution of 100 parts of ion-exchanged water and 100 parts of PFG was continuously added over 1 hour. Thereafter, the reaction solution was reacted at 50 ° C. for 4 hours. The weight average molecular weight of this hydrolysis condensate was 5,400. Next, 50 parts of MTMSi was further added to this reaction system,
After reacting at 50 ° C. for 2 hours, acetylacetone (A
cAc) 50 parts was added, and the mixture was further reacted at 50 ° C. for 1 hour. After allowing the reaction solution to cool to room temperature, PF
150 parts of G were added. Finally, a film-forming composition was obtained by removing 150 parts of a solvent containing methanol from the reaction solution by evaporation. The methanol content of the obtained film-forming composition was measured by gas chromatography and found to be 2% or less. Evaluation of Film Forming Composition Under the same conditions as in Example 1, the thickness uniformity, dielectric constant, crack resistance and moisture absorption of the coating film were evaluated and measured.
Table 1 shows the measurement results.

Example 3 Preparation of Film Forming Composition 203 parts of MTMSi, 70 parts of TMSi, and PFG240
After mixing, the mixture was stirred with a three-one motor to stabilize the liquid temperature at 50 ° C. Next, a solution in which 30 parts of oxalic acid was dissolved in 100 parts of ion-exchanged water was continuously added over 1 hour. Thereafter, the reaction solution was heated at 50 ° C., 4
The reaction was performed under the condition of time. The weight average molecular weight of this hydrolysis condensate was 3,200. Next, 50 parts of MTMSi was further added to the reaction system and reacted at 50 ° C. for 2 hours. After allowing the reaction solution to cool to room temperature, PFG
Was added. Finally, a film-forming composition was obtained by removing 150 parts of a solvent containing methanol from the reaction solution by evaporation. The methanol content of the obtained film-forming composition was measured by gas chromatography and found to be 2% or less. Evaluation of Film Forming Composition Under the same conditions as in Example 1, the thickness uniformity, dielectric constant, crack resistance and moisture absorption of the coating film were evaluated and measured.
Table 1 shows the measurement results.

Comparative Example 1 A film-forming composition was prepared in the same manner as in Example 1, except that MTMSi to be added later was added to the reaction system from the beginning. Table 1 shows the results. The weight average molecular weight of the organosilane condensate was 4,100.

Comparative Example 2 A film-forming composition was prepared in the same manner as in Example 2, except that MTMSi to be added later was added to the reaction system from the beginning. Table 1 shows the results. The weight average molecular weight of the above organosilane condensate was 4,400.

[0055]

[Table 1]

[0056]

According to the method for producing a film-forming composition of the present invention, a filterable film-forming composition can be obtained.
It is possible to provide a film-forming composition having an excellent balance of thickness uniformity, dielectric constant, crack resistance, low moisture absorption and the like in a coating film.

 ──────────────────────────────────────────────────続 き Continuing on the front page (72) Inventor Jun Shiota 2--11-24 Tsukiji, Chuo-ku, Tokyo Inside JSR Co., Ltd. (72) Kinji Yamada 2-11-24 Tsukiji, Chuo-ku, Tokyo JSR (72) Inventor Kohei Goto 2-11-24 Tsukiji, Chuo-ku, Tokyo FSR in JSR Corporation (reference) 4J002 CP031 FD010 FD030 FD310 GQ01 HA08 4J035 AA03 BA13 CA04N CA041 EA01 EB02 GA01 GB02 GB08 LA05 LA07 LB20 4J038 DB171 DG291 DL051 GA01 GA02 GA03 GA06 GA07 GA08 GA09 GA11 GA12 GA13 NA01 NA07 NA11 NA12 NA21 5F058 AA02 AA04 AB04 AC03 AF04 AH02 5G303 AA07 AB06 AB20 BA03 BA07 CA01 CA09 CB30 DA01 DA06

Claims (1)

[Claims] 1. In a solvent, in the presence of a hydrolytic condensate of an organosilane (I) represented by the following general formula (I) and an organosilane (II) represented by the following general formula (II): A method for producing a film-forming composition, which further comprises adding an organosilane (I) represented by the following general formula (I), followed by hydrolysis and condensation. R ¹ Si (OR ² ) ₃ ... (I) (wherein, R ¹ represents a monovalent organic group, and R ² represents the same or different and represents an alkyl group, an aryl group, or an acyl group.) Si (OR ² ) ₄ ... (II) (wherein R ² is the same or different and represents an alkyl group, an aryl group, or an acyl group.)