JP2001152023A - Composition for film formation - Google Patents

Abstract

PROBLEM TO BE SOLVED: To obtain a composition for film formation useful as an interlaminar insulating film in a semiconductor element, etc., having a low dielectric constant of coating film and uniformity of coating film, excellent low foaming properties in shaking in a solution, etc. SOLUTION: This composition for film formation is characterized in that the composition comprises (A) a polymer obtained by hydrolyzing at least one kind of compound selected from (A-1) a compound of general formula (1): R1aSi(OR2)4-a (R1 is a hydrogen atom, a fluorine atom or a monofunctional organic group; R2 is a monofunctional organic group; (a) is an integer of 0 to 2) and (A-2) a compound of general formula (2): R3b(R4O)3-bSi-(R7)d-Si(OR5)3-cR6c (R3, R4, R5 and R6 may be the same or different and are each a monofunctional organic group; b and c may be the same or different and are each a number of 0 to 2; R7 is an oxygen atom or (CH2)n; d is 0 or 1; n is a number of 1 to 6) in the presence of a metal chelate compound of general formula (3): R8e(MCOR9)f-e (R8 is a chelating agent; M is a metal atom; R9 is a 2-5C alkyl group or a 6-20C aryl group; f is a valence of metal M; e is an integer of 1 to f) and (B) a silicone surfactant.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a film-forming composition, and more particularly, to a film having a low dielectric constant, uniformity of a coating film, and a solution as an interlayer insulating film material in a semiconductor device. The present invention relates to a film-forming composition having excellent low foaming properties.

[0002]

2. Description of the Related Art Conventionally, a silica (SiO2) film formed by a vacuum process such as a CVD method has been frequently used as an interlayer insulating film in a semiconductor element or the like. In recent years, for the purpose of forming a more uniform interlayer insulating film, a coating-type insulating film mainly composed of a hydrolysis product of tetraalkoxylan, which is called an SOG (Spin on Glass) film, may be used. It has become. 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 and multilayering of semiconductor devices and the like, more excellent electrical insulation between conductors is required, and therefore,
There has been a demand for an interlayer insulating film material having a lower dielectric constant, a uniform coating film, and a lower foaming property when the solution is shaken.

[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, when a metal chelate compound such as titanium or zirconium is combined with the silane compound as described above, the low dielectric constant of the coating film, the uniformity of the coating film, the low foaming property when the solution is shaken down, etc. It does not have a good balance.

[0007]

The present invention relates to a film-forming composition for solving the above-mentioned problems, and more particularly, to a low dielectric constant of a coating film or a coating film as an interlayer insulating film in a semiconductor device or the like. An object of the present invention is to provide a material for an interlayer insulating film which is excellent in uniformity and low foaming property when a solution is shaken.

The present invention relates to (A) (A-1) a compound represented by the following general formula (1): R ¹ _a Si (OR ² ) _4-a (1) wherein R ¹ is hydrogen An atom, a fluorine atom or a monovalent organic group, R ² represents a monovalent organic group, a represents an integer of 0 to 2) and (A-2) represented by the following general formula (2) Compound R ³ _b (R ⁴ O) _3-b Si— (R ⁷ ) _d —Si (OR ⁵ ) _3-c R ⁶ _c (2) (R ³ , R ⁴ , R ⁵ and R ⁶ may be the same or different and each represents a monovalent organic group, b and c may be the same or different and each represent a number of 0 to 2, and R ⁷ represents an oxygen atom or-( CH ₂ ) _n- , d is 0 or 1
And n represents a number of 1 to 6. ) Is a metal chelate compound represented by the following general formula (3): R ⁸ _e M (OR ⁹ ) _fe (3) (R ⁸ is a chelating agent, M is a metal Atom, R ⁹ has 2 to 5 carbon atoms
Represents an alkyl group or an aryl group having 6 to 20 carbon atoms, f represents the valence of the metal M, and e represents an integer of 1 to f. )
And (B) a silicone surfactant, and a film-forming composition and a material for forming an insulating film.

[0009]

BEST MODE FOR CARRYING OUT THE INVENTION

Component (A) Component (A-1) In the general formula (1), examples of the monovalent organic group represented by R ¹ and R ² include an alkyl group, an aryl group, an allyl group, and a glycidyl group. Can be. Further, in the general formula (1), R ¹ is preferably a monovalent organic group, particularly an alkyl group or a phenyl group. Here, examples of the alkyl group include a methyl group, an ethyl group, a propyl group, a butyl group and the like, preferably having 1 to 5 carbon atoms, and these alkyl groups may be chain-like or branched, Further, a hydrogen atom may be substituted with a fluorine atom or the like. In the general formula (1), as the aryl group,
Examples include a phenyl group, a naphthyl group, a methylphenyl group, an ethylphenyl group, a chlorophenyl group, a bromophenyl group, and a fluorophenyl group.

Specific examples of the compound represented by the general formula (1) include trimethoxysilane, triethoxysilane, tri-n-propoxysilane, tri-iso-propoxysilane, tri-n-butoxysilane and tri-silane. sec-butoxysilane, tri-tert-butoxysilane, triphenoxysilane, fluorotrimethoxysilane, fluorotriethoxysilane, fluorotri-n-propoxysilane, fluorotri-iso-propoxysilane,
Fluorotri-n-butoxysilane, fluorotri-s
ec-butoxysilane, fluorotri-tert-butoxysilane, fluorotriphenoxysilane, tetramethoxysilane, tetraethoxysilane, tetra-n-propoxysilane, tetra-iso-propoxysilane,
Tetra-n-butoxysilane, tetra-sec-butoxysilane, tetra-tert-butoxysilane, tetraphenoxysilane, etc .; methyltrimethoxysilane, methyltriethoxysilane, methyltri-n-propoxysilane, methyltri-iso-propoxysilane, methyltrimethylsilane -N-butoxysilane, methyltri-sec-butoxysilane, methyltri-tert-butoxysilane,
Methyltriphenoxysilane, ethyltrimethoxysilane, ethyltriethoxysilane, ethyltri-n-propoxysilane, ethyltri-iso-propoxysilane, ethyltri-n-butoxysilane, ethyltri-s
ec-butoxysilane, ethyltri-tert-butoxysilane, ethyltriphenoxysilane, vinyltrimethoxysilane, vinyltriethoxysilane, vinyltri-n-propoxysilane, vinyltri-iso-propoxysilane, vinyltri-n-butoxysilane, vinyltri- sec-butoxysilane, vinyl tri-tert
-Butoxysilane, vinyltriphenoxysilane, 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, γ-aminopropyltriethoxysilane, γ-glycidoxypropyltrimethoxysilane, γ-glycidoxypropyltriethoxysilane, γ-trifluoropropyltrimethoxysilane, γ-trifluoropropyltriethoxysilane, etc .; dimethyldimethoxysilane , Dimethyldiethoxysilane, dimethyl-di-n-propoxysilane, dimethyl-di-iso-propoxysilane, dimethyl-di-n-butoxysilane, dimethyl-di-sec
-Butoxysilane, dimethyl-di-tert-butoxysilane, dimethyldiphenoxysilane, diethyldimethoxysilane, diethyldiethoxysilane, diethyl-di-n-propoxysilane, diethyl-di-iso-propoxysilane, diethyl-di-n -Butoxysilane, diethyl-di-sec-butoxysilane, diethyl-di-
tert-butoxysilane, diethyldiphenoxysilane, di-n-propyldimethoxysilane, di-n-propyldiethoxysilane, di-n-propyl-di-n-propoxysilane, di-n-propyl-di-iso- 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-i
so-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-sec-
Butoxysilane, di-iso-propyl-di-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-butoxysilane, di-s
ec-butyl-di-sec-butoxysilane, di-se
c-butyl-di-tert-butoxysilane, di-se
c-butyl-di-phenoxysilane, di-tert-butyldimethoxysilane, di-tert-butyldiethoxysilane, di-tert-butyl-di-n-propoxysilane, di-tert-butyl-di-iso-propoxy Silane, di-tert-butyl-di-n-butoxysilane, di-tert-butyl-di-sec-butoxysilane, di-tert-butyl-di-tert-butoxysilane, di-tert-butyl-di-phenoxy Silane, diphenyldimethoxysilane, diphenyl-di-ethoxysilane, diphenyl-di-n-propoxysilane, diphenyl-di-iso-propoxysilane, diphenyl-di-n-butoxysilane, diphenyl-di-s
ec-butoxysilane, diphenyl-di-tert-butoxysilane, diphenyldiphenoxysilane, divinyltrimethoxysilane, γ-aminopropyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ
-Glycidoxypropyltrimethoxysilane, γ-glycidoxypropyltriethoxysilane, γ-trifluoropropyltrimethoxysilane, γ-trifluoropropyltriethoxysilane, and the like. Preferably, tetramethoxysilane, tetraethoxysilane, tetra-n-propoxysilane, tetra-iso-
Propoxysilane, tetraphenoxysilane, methyltrimethoxysilane, methyltriethoxysilane, methyltri-n-propoxysilane, methyltri-iso-propoxysilane, ethyltrimethoxysilane, ethyltriethoxysilane, vinyltrimethoxysilane, vinyltriethoxysilane , Phenyltrimethoxysilane, phenyltriethoxysilane, dimethyldimethoxysilane, dimethyldiethoxysilane, diethyldimethoxysilane, diethyldiethoxysilane, diphenyldimethoxysilane, diphenyldiethoxysilane, trimethylmonomethoxysilane, trimethylmonoethoxysilane, triethylmono Methoxysilane, triethylmonoethoxysilane, triphenylmonomethoxysilane, triphenylmonoethoxysila It is. These may be used alone or in combination of two or more.

(A-2) Component In the above general formula (2), examples of the monovalent organic group include the same organic groups as those in the above general formula (1).
In the general formula (2), as the compound in which R ⁷ is an oxygen atom, hexamethoxydisiloxane, hexaethoxydisiloxane, hexaphenoxydisiloxane, 1,1,1
1,3,3-pentamethoxy-3-methyldisiloxane, 1,1,1,3,3-pentaethoxy-3-methyldisiloxane, 1,1,1,3,3-pentamethoxy-
3-phenyldisiloxane, 1,1,1,3,3-pentaethoxy-3-phenyldisiloxane, 1,1,3,
3-tetramethoxy-1,3-dimethyldisiloxane,
1,1,3,3-tetraethoxy-1,3-dimethyldisiloxane, 1,1,3,3-tetramethoxy-1,3
-Diphenyldisiloxane, 1,1,3,3-tetraethoxy-1,3-diphenyldisiloxane, 1,1,3
-Trimethoxy-1,3,3-trimethyldisiloxane, 1,1,3-triethoxy-1,3,3-trimethyldisiloxane, 1,1,3-trimethoxy-1,3,3
3-triphenyldisiloxane, 1,1,3-triethoxy-1,3,3-triphenyldisiloxane, 1,3
Dimethoxy-1,1,3,3-tetramethyldisiloxane, 1,3-diethoxy-1,1,3,3-tetramethyldisiloxane, 1,3-dimethoxy-1,1,3,3
Examples thereof include 3-tetraphenyldisiloxane and 1,3-diethoxy-1,1,3,3-tetraphenyldisiloxane. Of these, hexamethoxydisiloxane, hexaethoxydisiloxane, 1,1,
3,3-tetramethoxy-1,3-dimethyldisiloxane, 1,1,3,3-tetraethoxy-1,3-dimethyldisiloxane, 1,1,3,3-tetramethoxy-
1,3-diphenyldisiloxane, 1,3-dimethoxy-1,1,3,3-tetramethyldisiloxane, 1,3
-Diethoxy-1,1,3,3-tetramethyldisiloxane, 1,3-dimethoxy-1,1,3,3-tetraphenyldisiloxane, 1,3-diethoxy-1,1,
Preferred examples include 3,3-tetraphenyldisiloxane. In the general formula (2), d
Are 0, hexamethoxydisilane, hexaethoxydisilane, hexaphenoxydisilane, 1,
1,1,2,2-pentamethoxy-2-methyldisilane, 1,1,1,2,2-pentaethoxy-2-methyldisilane, 1,1,1,2,2-pentamethoxy-2-
Phenyldisilane, 1,1,1,2,2-pentaethoxy-2-phenyldisilane, 1,1,2,2-tetramethoxy-1,2-dimethyldisilane, 1,1,2,2-
Tetraethoxy-1,2-dimethyldisilane, 1,1,
2,2-tetramethoxy-1,2-diphenyldisilane, 1,1,2,2-tetraethoxy-1,2-diphenyldisilane, 1,1,2-trimethoxy-1,2,2
-Trimethyldisilane, 1,1,2-triethoxy-
1,2,2-trimethyldisilane, 1,1,2-trimethoxy-1,2,2-triphenyldisilane, 1,1,
2-triethoxy-1,2,2-triphenyldisilane, 1,2-dimethoxy-1,1,2,2-tetramethyldisilane, 1,2-diethoxy-1,1,2,2-tetramethyldisilane, 1,2-dimethoxy-1,1,1
Examples of the compound in which R ⁷ is — (CH ₂ ) _n — in the general formula (2) include 2,2-tetraphenyldisilane and 1,2-diethoxy-1,1,2,2-tetraphenyldisilane. (Hexamethoxysilyl) methane, bis (hexaethoxysilyl) methane, bis (hexaphenoxysilyl) methane, bis (dimethoxymethylsilyl) methane, bis (diethoxymethylsilyl) methane, bis (dimethoxyphenylsilyl) methane, bis ( Diethoxyphenylsilyl) methane, bis (methoxydimethylsilyl) methane, bis (ethoxydimethylsilyl) methane,
Bis (methoxydiphenylsilyl) methane, bis (ethoxydiphenylsilyl) methane, bis (hexamethoxysilyl) ethane, bis (hexaethoxysilyl) ethane, bis (hexaphenoxysilyl) ethane, bis (dimethoxymethylsilyl) ethane, bis ( Diethoxymethylsilyl) ethane, bis (dimethoxyphenylsilyl)
Ethane, bis (diethoxyphenylsilyl) ethane, bis (methoxydimethylsilyl) ethane, bis (ethoxydimethylsilyl) ethane, bis (methoxydiphenylsilyl) ethane, bis (ethoxydiphenylsilyl) ethane, 1,3-bis (hexa Methoxysilyl) propane,
1,3-bis (hexaethoxysilyl) propane, 1,
3-bis (hexaphenoxysilyl) propane, 1,3
-Bis (dimethoxymethylsilyl) propane, 1,3-
Bis (diethoxymethylsilyl) propane, 1,3-bis (dimethoxyphenylsilyl) propane, 1,3-bis (diethoxyphenylsilyl) propane, 1,3-bis (methoxydimethylsilyl) propane, 1,3- Examples thereof include bis (ethoxydimethylsilyl) propane, 1,3-bis (methoxydiphenylsilyl) propane, and 1,3-bis (ethoxydiphenylsilyl) propane. Of these, hexamethoxydisilane,
Hexaethoxydisilane, hexaphenixidisilane,
1,1,2,2-tetramethoxy-1,2-dimethyldisilane, 1,1,2,2-tetraethoxy-1,2-dimethyldisilane, 1,1,2,2-tetramethoxy-
1,2-diphenyldisilane, 1,1,2,2-tetraethoxy-1,2-diphenyldisilane, 1,2-dimethoxy-1,1,2,2-tetramethyldisilane, 1,
2-diethoxy-1,1,2,2-tetramethyldisilane, 1,2-dimethoxy-1,1,2,2-tetraphenyldisilane, 1,2-diethoxy-1,1,2,2-
Tetraphenyldisilane, bis (hexamethoxysilyl) methane, bis (hexaethoxysilyl) methane, bis (dimethoxymethylsilyl) methane, bis (diethoxymethylsilyl) methane, bis (dimethoxyphenylsilyl) methane, bis (diethoxyphenyl) Preferred examples include (silyl) methane, bis (methoxydimethylsilyl) methane, bis (ethoxydimethylsilyl) methane, bis (methoxydiphenylsilyl) methane, and bis (ethoxydiphenylsilyl) methane.
In the present invention, the component (A) includes the above (A-1)
Component and / or Component (A-2) are used, and Component (A-1) and Component (A-2) are 2
More than one species can be used.

In the present invention, the above component (A) is converted into a solvent represented by the following general formula (4): R ¹⁰ O (R ¹² O) _g R ¹¹ (4) (where R ¹⁰ and R ¹¹ are And each independently represents a hydrogen atom, an alkyl group having 1 to 4 carbon atoms or a monovalent organic group selected from CH ₃ CO—, R ¹² represents an alkylene group, and g represents an integer of 1 to 2. ) In the presence of In the general formula (4), the alkyl group of R ¹⁰ and R ¹¹ is a methyl group, an ethyl group, an n-propyl group, an I-propyl group,
Examples of the alkylene group represented by R ¹² include a butyl group and the like, and examples thereof include an ethylene group, an n-propylene group, and an isopropylene group. Specific examples of the solvent represented by the general formula (4) include propylene glycol monomethyl ether, propylene glycol monoethyl ether, propylene glycol monopropyl ether, propylene glycol monobutyl ether, propylene glycol dimethyl ether, propylene glycol diethyl ether, and propylene glycol diether. Propyl ether, propylene glycol dibutyl ether, dipropylene glycol monomethyl ether, dipropylene glycol monoethyl ether, dipropylene glycol monopropyl ether,
Dipropylene glycol monobutyl ether, dipropylene glycol dimethyl ether, dipropylene glycol diethyl ether, dipropylene glycol dipropyl ether, dipropylene glycol dibutyl ether, 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, dipropylene glycol monopropyl ether acetate, dipropylene glycol monobutyl ether acetate, propylene glycol diacetate,
Dipropylene glycol diacetate, propylene glycol, etc., and particularly propylene glycol monomethyl ether, propylene glycol monoethyl ether, propylene glycol monopropyl ether, propylene glycol monobutyl ether, propylene glycol dimethyl ether, propylene glycol diethyl ether, propylene glycol monomethyl ether acetate Propylene glycol monoethyl ether acetate and propylene glycol monopropyl ether acetate are preferred. These can be used alone or in combination of two or more.

In the present invention, the component (A) is added in the presence of a solvent,
The metal chelate compound and water are added to hydrolyze the component (A). When the above component (A) is hydrolyzed and condensed, the components (A-1) and (A-2) have
It is preferable to use 0.25 to 3 mol of water per 1 mol of the group represented by 2O-, R4O- and R5O-,
It is particularly preferred to add 0.3 to 2.5 mol of water.
When the amount of water to be added falls within the range of 0.25 to 3 mol, there is no possibility that the uniformity of the coating film is reduced, and the storage stability of the film-forming composition is less likely to be reduced. That's why. Further, the water is preferably added intermittently or continuously.

The component (A-1) and / or (A-2)
When the components are hydrolyzed and condensed, a metal chelate compound (B) represented by the general formula (3) is used.

Examples of the metal chelate compound include triethoxy mono (acetylacetonate) titanium, tri-n-propoxy mono (acetylacetonate) titanium, tri-i-propoxy mono (acetylacetonate) titanium, -N-butoxy mono (acetylacetonate) titanium, tri-sec-butoxy mono (acetylacetonate) titanium, tri-t-butoxy mono (acetylacetonate) titanium, diethoxy.
Bis (acetylacetonato) titanium, di-n-propoxybis (acetylacetonato) titanium, di-i-
Propoxy bis (acetylacetonate) titanium, di-n-butoxybis (acetylacetonate) titanium, di-sec-butoxybis (acetylacetonato) titanium, di-t-butoxybis (acetylacetonate) Titanium, monoethoxy-tris (acetylacetonato) titanium, mono-n-propoxy-tris (acetylacetonato) titanium, mono-i-propoxy.
Tris (acetylacetonate) titanium, mono-n-butoxytris (acetylacetonate) titanium, mono-sec-butoxytris (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) Acetate) titanium, tri-s
ec-butoxy mono (ethyl acetoacetate) titanium, tri-t-butoxy mono (ethyl acetoacetate) titanium, diethoxy bis (ethyl acetoacetate) titanium, di-n-propoxy bis (ethyl acetoacetate) titanium, Di-i-propoxy bis (ethyl acetoacetate) titanium, di-n-butoxy bis (ethyl acetoacetate) titanium, di-sec-butoxy bis (ethyl acetoacetate) titanium, di-t
-Butoxy bis (ethyl acetoacetate) titanium,
Monoethoxy tris (ethyl acetoacetate) titanium, mono-n-propoxy tris (ethyl acetoacetate) titanium, mono-i-propoxy tris (ethyl acetoacetate) titanium, mono-n-butoxy tris (ethyl acetoacetate) ) Titanium, mono-sec
-Butoxy-tris (ethylacetoacetate) titanium, mono-t-butoxytris (ethylacetoacetate) titanium, tetrakis (ethylacetoacetate)
Titanium chelate compounds such as titanium, mono (acetylacetonato) tris (ethylacetoacetate) titanium, bis (acetylacetonato) bis (ethylacetoacetate) titanium, tris (acetylacetonato) mono (ethylacetoacetate) titanium; triethoxy・ Mono (acetylacetonate) zirconium, tri-
n-propoxy mono (acetylacetonato) zirconium, tri-i-propoxy mono (acetylacetonato) zirconium, tri-n-butoxy mono (acetylacetonato) zirconium, tri-sec-butoxy mono (acetylacetonate) Nart) zirconium,
Tri-t-butoxy mono (acetylacetonate) zirconium, diethoxybis (acetylacetonato) zirconium, di-n-propoxybis (acetylacetonato) zirconium, di-i-propoxy.
Bis (acetylacetonate) zirconium, di-n-
Butoxy bis (acetylacetonate) zirconium, di-sec-butoxy bis (acetylacetonate) zirconium, di-t-butoxybis (acetylacetonate) zirconium, monoethoxy tris (acetylacetonate) zirconium, mono -N-propoxy tris (acetylacetonate) zirconium, mono-i-propoxy tris (acetylacetonate) zirconium, mono-n-butoxy tris (acetylacetonate) zirconium, mono-sec-butoxy tris (acetyl) (Acetonate) zirconium, mono-t-butoxy tris (acetylacetonate) zirconium, tetrakis (acetylacetonate) zirconium, triethoxy mono (ethylacetoacetate) zirconium Tri -n- propoxy mono (ethylacetoacetate) 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 (ethylacetoacetate) zirconium, diethoxybis (ethylacetoacetate) zirconium, di-n-propoxybis (ethylacetoacetate) 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
-Propoxy tris (ethyl acetoacetate) zirconium, mono-i-propoxy tris (ethyl acetoacetate) 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 chelate compounds such as zirconium and tris (acetylacetonate) mono (ethylacetoacetate) zirconium; aluminum chelate compounds such as tris (acetylacetonate) aluminum and tris (ethylacetoacetate) aluminum; and titanium. A particularly preferred example is a metal chelate compound containing

The amount of the metal chelate compound used is
Total amount of component (A) (in terms of complete hydrolysis condensate) 100
It is usually in the range of 0.001 to 10 parts by weight, preferably 0.01 to 10 parts by weight, based on parts by weight. Further, the metal chelate compound may be added in the solvent in advance, or may be dissolved or dispersed in water at the time of adding water. In the present invention, the hydrolysis means the above (A)
R ² O—, R ⁴ O—, and R ⁵ O—
It is not necessary that all of the groups be hydrolyzed, for example, only one is hydrolyzed, two or more are hydrolyzed, or a mixture thereof. In the production method of the present invention, the component (A) may be condensed after hydrolysis. In the present invention, condensation refers to condensation of a silanol group of the hydrolyzate of the component (A) to form a Si—O—Si bond. In the present invention, however, it is not necessary that all of the silanol groups are condensed. The concept encompasses the formation of a mixture of a small amount of silanol groups and a mixture of those having different degrees of condensation. In the present invention, the temperature at which the component (A) is hydrolyzed is usually 0 to 100 ° C, preferably 15 to 100 ° C.
８０80 ° C.

The film-forming composition of the present invention is a composition obtained by the above-mentioned production method, and the content of alcohol having a boiling point of 100 ° C. or less in the composition is 20% by weight or less, particularly 5% by weight or less. Preferably, there is. The alcohol having a boiling point of 100 ° C. or lower may be generated during hydrolysis and / or condensation of the component (A-1) and the component (A-2), and the content thereof is 20% by weight or less, preferably 5% by weight. %
It is preferable to remove by distillation or the like so as to be as follows.

The film-forming composition of the present invention may further contain the following organic solvent in addition to the solvent represented by the general formula (4). As the organic solvent used in the present invention, for example, n-pentane, i-pentane, n-hexane, i-hexane, n-heptane, i-heptane, 2,
Aliphatic hydrocarbon solvents such as 2,4-trimethylpentane, n-octane, i-octane, cyclohexane and methylcyclohexane; benzene, toluene, xylene,
Aromatic hydrocarbon solvents such as ethylbenzene, trimethylbenzene, methylethylbenzene, n-propylbenzene, i-propylbenzene, diethylbenzene, i-butylbenzene, triethylbenzene, di-i-propylbenzene, n-amylnaphthalene, and trimethylbenzene ; 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-
Ketone solvents such as hexyl ketone, di-i-butyl ketone, trimethylnonanone, cyclohexanone, 2-hexanone, methylcyclohexanone, 2,4-pentanedione, acetonylacetone, diacetone alcohol, acetophenone and fenchone; ethyl ether; i-
Propyl ether, n-butyl ether, n-hexyl ether, 2-ethylhexyl ether, ethylene oxide, 1,2-propylene oxide, dioxolane,
-Methyl dioxolane, dioxane, dimethyl dioxane, 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,
Ethers such as 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, tripropylene glycol monomethyl ether, tetrahydrofuran, and 2-methyltetrahydrofuran System solvent: 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-ethylhexyl acetate, benzyl acetate, cyclohexyl acetate, methyl acetate Tylcyclohexyl, 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 ether acetate, diethylene glycol mono-n-butyl ether acetate, propylene acetate Glycol monomethyl ether, methoxytriglycol acetate, ethyl propionate, n-butyl propionate, i-amyl propionate, diethyl oxalate, di-n-butyl oxalate, methyl lactate, ethyl lactate, n-butyl lactate, n-lactic acid n Ester solvents such as amyl, diethyl malonate, dimethyl phthalate and diethyl phthalate; N-methylformamide, N, N-dimethylformamide, N, N Nitrogen-containing solvents such as diethylformamide, acetamide, N-methylacetamide, N, N-dimethylacetamide, N-methylpropionamide, N-methylpyrrolidone; dimethyl sulfide, diethyl sulfide, thiophene, tetrahydrothiophene, dimethyl sulfoxide, sulfolane, Examples thereof include sulfur-containing solvents such as 1,3-propane sultone. These can be used alone or in combination of two or more.

The silicone surfactant used in the present invention includes, for example, SH7PA, SH21PA, SH30
PA, ST94PA (both by Dow Corning Toray)
Silicone Co., Ltd. can be used. Among these, a polymer represented by the following general formula (5) corresponding to SH28PA and SH30PA is particularly preferable.

[0021]

Embedded image (In the formula, R ¹³ is a hydrogen atom or an alkyl group having 1 to 5 carbon atoms, n is an integer of 1 to 20, and x and y are each independently an integer of 2 to 100.)

The ratio of the silicone surfactant to 100 parts by weight of the component (A) (completely hydrolyzed condensate) is 0.1%.
002 to 0.5 parts by weight, more preferably 0.00
5 to 0.2 parts by weight. If the amount of the silicone surfactant is less than 0.002 parts by weight, the uniformity of the coating film may be poor, and if it exceeds 0.5 part by weight, the dielectric constant of the coating film may increase.

The film-forming composition of the present invention may further contain the following components. β-diketones β-diketones include acetylacetone, 2,4-hexanedione, 2,4-heptanedione, 3,5-heptanedione, 2,4-octanedione, 3,5-octanedione, 2,4- Nonanedione, 3,5-nonanedione, 5-methyl-2,4-hexanedione, 2,2
6,6-tetramethyl-3,5-heptanedione, 1,
One or more kinds such as 1,1,5,5,5-hexafluoro-2,4-heptanedione. In the present invention, the β-diketone content in the film-forming composition,
Total amount of component (A) (in terms of complete hydrolysis condensate) 100
It is usually in the range of 0.1 to 100 parts by weight, preferably 0.2 to 80 parts by weight based on parts by weight. Β in such a range
Addition of a diketone can provide a certain storage stability and reduce the risk of deterioration of properties such as coating uniformity of the film-forming composition. This β-diketone is preferably added after the hydrolysis and condensation reaction of the component (A).

Other Additives Components such as colloidal silica, colloidal alumina, and organic polymers may be further added to the film-forming composition obtained in the present invention. Colloidal silica, for example,
It is a dispersion in which high-purity silicic acid is dispersed in the hydrophilic organic solvent, and usually has an average particle size of 5 to 30 mμ, preferably 10 to 20 mμ, and a solid concentration of about 10 to 40% 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 sol 5 manufactured by Nissan Chemical Industries, Ltd.
20, 100 and 200; alumina clear sol, alumina sol 10, manufactured by Kawaken Fine Chemical Co., Ltd.
132 and the like. As the organic polymer, for example, a compound having a polyalkylene oxide structure,
A compound having a sugar chain structure, a vinylamide polymer, a (meth) acrylic polymer, an aromatic vinyl compound, a dendrimer, a polyimide, a polyamic acid, a polyarylene,
Examples thereof include polyamide, polyquinoxaline, polyoxadiazole, and fluoropolymer.

The total solid content of the film-forming composition of the present invention is preferably 2 to 30% by weight, and is appropriately adjusted depending on the purpose of use. When the total solid content of the composition is 2 to 30
When it is% by weight, the thickness of the coating film is in an appropriate range, and the storage stability is more excellent. The weight average molecular weight of all the polyorganosiloxane components [the hydrolyzed condensate of the component (A)] in the composition thus obtained is as follows:
Usually 1,000 to 120,000, preferably 1,2
It is about 100 to 100,000.

The composition of the present invention is prepared by adding silicon wafer, Si
When applying to a substrate such as an O2 wafer or a SiN wafer, a coating method such as spin coating, dipping, roll coating, or spraying is used.

In this case, the 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, a 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. As a heating atmosphere, the heating is performed in the atmosphere, a nitrogen atmosphere, an argon atmosphere, a vacuum, a reduced pressure in which the oxygen concentration is controlled, or the like. Can be.

The interlayer insulating film thus obtained is excellent in insulating properties, uniformity of coating film, dielectric constant, crack resistance of coating film, and surface hardness of coating film.
System L, DRAM, SDRAM, RDRAM, D
-It is useful for applications such as interlayer insulating films for semiconductor devices such as RDRAMs, protective films such as surface coat films for semiconductor devices, interlayer insulating films for multilayer wiring boards, protective films for liquid crystal display devices, and insulating films.

[0029]

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.

The weight average molecular weight (Mw) was measured by gel permeation chromatography (GPC) under the following conditions. Sample: Prepared by dissolving 1 g of a hydrolyzed condensate in 100 cc of tetrahydrofuran using tetrahydrofuran as a solvent. Standard polystyrene: Standard polystyrene manufactured by Pressure Chemical Co., USA was used. Apparatus: High-temperature, high-speed gel permeation chromatogram (model 150-C ALC / GPC) manufactured by Waters, Inc. Column: SHOdex A-80M manufactured by Showa Denko KK
(Length 50cm) Measurement temperature: 40 ° C Flow rate: 1cc / min

A composition sample was applied on a silicon wafer having a dielectric constant of 8 inches by a spin coating method, and was coated on a hot plate at 100 ° C. for 4 hours.
For 4 minutes at 250 ° C.
The substrate was baked in a vacuum oven for 120 minutes. Aluminum was vapor-deposited on the obtained substrate to produce a substrate for permittivity evaluation. Dielectric constants were measured using an HP16451B electrode manufactured by Yokogawa-Hewlett-Packard Co., Ltd. and an HP4284A.
It was calculated from the capacitance value at 10 kHz using a precision LCR meter.

The composition for forming a uniform film thickness was applied onto an 8-inch silicon wafer by using a spin coater under the conditions of 1,000 rpm for 15 seconds. Thereafter, using a hot plate maintained at a temperature of 90 ° 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 (Ru).
Spec manufactured by dolph Technologies
(tra Laser 200), and 50 points were measured 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 15 nm ×: 3σ of coating film is 15 nm or more

The solution Solution screw tube bottle effervescent 100cc of added 50 cc,
The screw tube was shaken vigorously for 1 minute. The solution was allowed to stand, and the time until bubbles in the solution disappeared was measured. The foaming property of the solution was evaluated according to the following criteria. The foaming of the solution disappears within 5 minutes ×: foaming is observed in the solution even after 5 minutes

Synthesis Example 1 In a quartz separable flask, 154.1 g of methyltrimethoxysilane, 48.1 g of tetramethoxysilane and 0.96 g of tetrakis (acetylacetonato) titanium
And 200 g of propylene glycol monomethyl ether, and then stirred with a three-one motor to stabilize the solution temperature at 65 ° C. Next, 92 g of ion-exchanged water
Was added to the solution over 2 hours. Then, after reacting at 65 ° C. for 4 hours, the reaction solution was cooled to room temperature. To this reaction solution, propylene glycol monomethyl ether 299 was added.
g was added, and 299 g of a solution containing methanol was removed from the reaction solution at 50 ° C. by evaporation to obtain a reaction solution.
The weight average molecular weight of the condensate and the like thus obtained is
7,700.

Synthesis Example 2 In a quartz separable flask, 154.1 g of methyltrimethoxysilane, 48.1 g of tetramethoxysilane and 0.96 g of diisopropoxytitanium bisethylacetyl acetate were dissolved in 200 g of propylene glycol monopropyl ether. Thereafter, the solution was stirred with a three-one motor, and the solution temperature was stabilized at 65 ° C. Next, 92 g of ion-exchanged water was added to the solution over 2 hours. afterwards,
After reacting at 65 ° C. for 4 hours, the reaction solution was cooled to room temperature. 299 g of propylene glycol monopropyl ether was added to this reaction solution, and at 50 ° C., 299 g of a solution containing methanol was removed from the reaction solution by evaporation to obtain a reaction solution. The weight average molecular weight of the condensate and the like thus obtained was 8,700.

Synthesis Example 3 In a quartz separable flask, 154.1 g of methyltrimethoxysilane, 48.1 g of tetramethoxysilane, and 0.9 of aluminum tris (ethylacetoacetate) were added.
6 g of propylene glycol monopropyl ether 20
After dissolving in 0 g, the mixture was stirred with a three-one motor, and the solution temperature was stabilized at 65 ° C. Next, 92 g of ion-exchanged water was added to the solution over 2 hours. Then 65
After reacting at 4 ° C. for 4 hours, the reaction solution was cooled to room temperature. 299 g of propylene glycol monopropyl ether was added to this reaction solution, and at 50 ° C., 299 g of a solution containing methanol was removed from the reaction solution by evaporation to obtain a reaction solution. The weight average molecular weight of the condensate and the like thus obtained was 5,700.

Example 1 0.002 g of SH28PA manufactured by Dow Corning Toray Silicone Co., Ltd. was added to 50 g of the reaction solution obtained in Synthesis Example 1.
After the addition, the solution was filtered through a Teflon filter having a pore size of 0.2 μm to obtain a film-forming composition of the present invention. The obtained composition was applied on a silicon wafer by a spin coating method. The dielectric constant of the obtained coating film was as low as 2.65,
σ was as good as 7.8 nm. When the foaming property of the solution was evaluated, no foaming was observed in 3 minutes and 20 seconds.

Example 2 0.002 g of SH30PA manufactured by Dow Corning Toray Silicone Co., Ltd. was added to 50 g of the reaction solution obtained in Synthesis Example 1.
After the addition, the solution was filtered through a Teflon filter having a pore size of 0.2 μm to obtain a film-forming composition of the present invention. The obtained composition was applied on a silicon wafer by a spin coating method. The dielectric constant of the obtained coating film was as low as 2.64,
σ was as good as 7.9 nm. When the foaming property of the solution was evaluated, no foaming was observed in 3 minutes and 40 seconds.

Example 2 0.002 g of SH28PA manufactured by Dow Corning Toray Silicone Co., Ltd. was added to 50 g of the reaction solution obtained in Synthesis Example 1.
After the addition, the solution was filtered through a Teflon filter having a pore size of 0.2 μm to obtain a film-forming composition of the present invention. The obtained composition was applied on a silicon wafer by a spin coating method. The dielectric constant of the obtained coating film was as low as 2.67,
σ was as good as 7.5 nm. When the foaming property of the solution was evaluated, no foaming was observed in 3 minutes and 35 seconds.

Example 3 0.002 g of SH28PA manufactured by Dow Corning Toray Silicone Co., Ltd. was added to 50 g of the reaction solution obtained in Synthesis Example 1.
After the addition, the solution was filtered through a Teflon filter having a pore size of 0.2 μm to obtain a film-forming composition of the present invention. The obtained composition was applied on a silicon wafer by a spin coating method. The dielectric constant of the obtained coating film was as low as 2.58,
σ was as good as 8.3 nm. When the foaming property of the solution was evaluated, no foaming was observed in 3 minutes and 32 seconds.

Example 4 50 g of the reaction solution obtained in Synthesis Example 1 had a molecular weight of about 4,
5 g of polyisopropyl methacrylate and SH28PA manufactured by Dow Corning Toray Silicone Co., Ltd.
Evaluation was performed in the same manner as in Example 1 except that a solution containing 002 g was used. The dielectric constant of the obtained coating film is 2.3.
0, which was a very low value, and 3σ of the coating film was as good as 10.2 nm. Also, when the foaming property of the solution was evaluated,
After 3 minutes and 20 seconds, no foaming was observed.

Example 5 50 g of the reaction solution obtained in Synthesis Example 2 was added with a molecular weight of about 2,2.
0.002 of polyethylene glycol 5g and SH28PA manufactured by Dow Corning Toray Silicone Co., Ltd.
Evaluation was performed in the same manner as in Example 1 except that the solution to which g was added was used. The obtained coating film had a very low dielectric constant of 2.25, and the coating had a good 3σ of 9.2 nm. When the foaming property of the solution was evaluated,
No foaming was observed in seconds.

Example 6 To 50 g of the reaction solution obtained in Synthesis Example 2 was added 1 g of acetylacetone and SH manufactured by Dow Corning Toray Silicone Co., Ltd.
Evaluation was performed in the same manner as in Example 1 except that a solution to which 0.002 g of 28PA was added was used. The dielectric constant of the obtained coating film was as low as 2.62, and 3σ of the coating film was 5.2.
nm. When the foaming property of the solution was evaluated, no foaming was observed in 2 minutes and 40 seconds.

COMPARATIVE EXAMPLE 1 Except that only the reaction solution obtained in Comparative Synthesis Example 1 was used,
Evaluation was performed in the same manner as in Example 1. The dielectric constant of the obtained coating film was a low value of 2.69, but 3σ of the coating film was 2
It was inferior to 3 nm.

Comparative Example 2 The procedure of Example 1 was repeated except that 0.002 g of a fluorine-based surfactant Megafax F-172 (manufactured by Dainippon Ink and Chemicals) was added to 50 g of the reaction solution obtained in Comparative Synthesis Example 2. Evaluation was performed in the same manner. The dielectric constant of the obtained coating film is 2.68.
The value of 3σ of the coating film was as good as 10.3 nm. However, when the foaming property of the solution was evaluated, foaming was observed in the solution even after 5 minutes had passed.

[0046]

According to the present invention, an alkoxysilane is hydrolyzed in the presence of a metal chelate compound and an acid catalyst, thereby achieving an excellent balance among dielectric constant, coating uniformity, and low foaming property of a solution. Composition for film formation (material for interlayer insulating film)
It is possible to provide.

──────────────────────────────────────────────────続 き Continued on the front page (51) Int.Cl. ⁷ Identification symbol FI Theme coat ゛ (Reference) C09D 133/00 C09D 133/00 171/02 171/02 183/06 183/06 183/12 183/12 H01L 21/312 H01L 21/312 C 21/316 21/316 G (72) Inventor Mayumi Tsunoda 2-11-24 Tsukiji, Chuo-ku, Tokyo Inside JS Suare Co., Ltd. (72) Inventor Kentaro Tamaki Tsukiji, Chuo-ku, Tokyo 2-11-11-24 JAE S.R. Ltd. EA016 EA056 EC046 ED026 EE036 EE047 EH036 EH037 FD010 FD206 FD312 GH01 GQ01 4J038 CG002 DF002 DL051 DL052 DL071 DL101 JA34 JC32 JC38 KA06 KA09 NA21 PB09 PC03 PC08 5F058 AA03 AA10 AC03 AF04 AG01 AH01 AH02

Claims (7)

[Claims] (A) (A-1) a compound represented by the following general formula (1): R ¹ _a Si (OR ² ) _4-a (1) (R ¹ is a hydrogen atom, A fluorine atom or a monovalent organic group, R ² represents a monovalent organic group, a represents an integer of 0 to 2) and (A-2) a compound represented by the following general formula (2) _{^{R 3 b (R 4 O)}} 3-b Si- (R 7) d -Si (oR 5) 3-c R 6 c ····· (2) (R 3, R 4, R 5 and R ⁶ May be the same or different and each represents a monovalent organic group, b and c may be the same or different and each represents a number of 0 to 2, and R ⁷ represents an oxygen atom or — (CH ₂ ) _{Represents n-} , d is 0 or 1
And n represents a number of 1 to 6. ) Is a metal chelate compound represented by the following general formula (3): R ⁸ _e M (OR ⁹ ) _fe (3) (R ⁸ is a chelating agent, M is a metal Atom, R ⁹ has 2 to 5 carbon atoms
Represents an alkyl group or an aryl group having 6 to 20 carbon atoms, f represents the valence of the metal M, and e represents an integer of 1 to f. )
A film-forming composition comprising a polymer hydrolyzed in the presence of (A) and (B) a silicone surfactant. Wherein the solvent R ¹⁰ O (R ¹² 0) of the hydrolysis reaction represented by the following general formula ^{_{(4) g R 11 ····· (}} 4) (R 10 and R ¹¹ are each independently A hydrogen atom, an alkyl group having 1 to 4 carbon atoms or a monovalent organic group selected from CH ₃ CO—, R ¹² represents an alkylene group, and g represents an integer of 1 to 2.) The composition for forming a film according to claim 1, wherein the composition is used. 3. The film-forming composition according to claim 1, wherein M in the general formula (3) is at least one selected from titanium, zirconium and aluminum. 4. The film-forming composition according to claim 1, wherein the silicone surfactant is a polymer containing a dimethylsiloxane group and an oxyalkylene group. 5. A silicone surfactant having a ratio of 0.1 to 100 parts by weight of component (A) (completely hydrolyzed and condensed).
2. The composition according to claim 1, wherein the amount is 002 to 0.5 parts by weight.
The composition for forming a film according to the above. 6. The film-forming composition according to claim 1, wherein β-
A film-forming composition, comprising at least one compound selected from the group consisting of a diketone, a compound having a polyalkylene oxide structure, and a (meth) acrylic polymer. 7. An insulating film forming material comprising the film forming composition according to claim 6.