JP2000143983A - Laminated material for circuit - Google Patents

Abstract

PROBLEM TO BE SOLVED: To obtain the subject material having a low dielectric constant, excellent heat resistance, sufficient peel strength at a room temperature, not causing scattering of resin in cutting, etc., having excellent handleability by laminating an adhesion layer of a specific composition to one side of a releasable film. SOLUTION: This material is obtained by laminating an adhesion layer composed of (A) a siloxane-modified polyimide, (B) a compound containing three allyl groups or methylallyl groups of formula I (R is H or methyl) and (C) a compound containing two or more maleimides to one side of a releasable film or a metal foil. A siloxane-modified polyimide comprising 90-40 mol% of a unit of formula II (X is O, CO or the like; Ar is a bifunctional group such as a group of formula III or the like) and 10-60 mol% of a unit of formula IV (R is -CH2OC6H4- in which methylene is bonded to Si or a 1-10C alkylene; n is 1-20) is preferable as the component A. Preferably the total of the components B and C is 10-900 pts.wt. based on 100 pts.wt. of the component A and the amount of methylallyl of the component B is 0.1-2 mol equivalent based on 1 mol equivalent maleimide of the component C.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a releasable film which has a low dielectric constant and a low dielectric loss tangent for use in a printed wiring board, has excellent adhesion to metal, and has very little resin scattering during operation. The present invention relates to a circuit laminate material provided with an adhesive layer on a metal foil.

[0002]

2. Description of the Related Art A multilayer printed wiring board used for electronic equipment and the like is a wiring board having an electric circuit also in an inner layer.
This multi-layer printed wiring board is composed of a circuit formed on the outer layer of a multi-layer copper-clad laminate containing an inner circuit obtained by hot-pressing an inner circuit board having a circuit formed in advance and a copper foil for an outer circuit with a prepreg interposed therebetween. Obtained by forming. Conventionally, a glass cloth-based epoxy resin prepreg is used for the prepreg. In recent years, the signal speed and operating frequency of electronic devices have been dramatically increased, so that electronic devices used in a high-frequency region, especially electronic devices required to be small and light, require heat resistance to form fine wiring. Excellent,
There is a demand for a thin circuit laminate material having a low dielectric constant and a low dielectric loss tangent. Since a thin circuit laminate material using a low dielectric material can increase the propagation speed of an electric signal, the signal can be processed at a higher speed.

At present, a thin multilayer printed wiring board has three
A thin glass cloth base epoxy resin prepreg having a thickness of 0 to 100 μm is used. However, the cross eyes are easy to emerge, and the unevenness of the inner layer circuit board cannot be absorbed inside the prepreg, and the unevenness tends to appear on the outer layer surface.
The smoothness of the surface is impaired, which hinders the formation of fine wiring. Therefore, instead of using a conventional glass cloth base epoxy resin prepreg, a method of using an adhesive film containing no glass cloth as a prepreg, or a resin-coated copper in which an adhesive layer is preliminarily laminated on one side of an outer layer copper foil. There is a method of using a foil as a copper foil for an outer layer circuit and a prepreg. Resins having film forming ability are used for these adhesive films and resin-attached copper foils, and usable resins are limited to resins having film forming ability. . If it does not have the ability to form a film, troubles such as cracking or chipping of the resin are likely to occur in the process of transporting, cutting, and laminating the adhesive film. Occasionally, the interlayer insulating layer becomes abnormally thin in the portion where the inner layer circuit is present, or the troubles such as a decrease in interlayer insulating resistance and a short circuit are liable to occur. Examples of the resin having film forming ability include thermoplastic polyimide adhesive film (US Pat. No. 4,543,295), high molecular weight epoxy resin (JP-A-4-120135), acrylonitrile-butadiene copolymer / phenol resin (JP-A-4-29).
393), phenolic resin / butyral resin (Japanese Unexamined Patent Application Publication No.
-36366), acrylonitrile butadiene copolymer / epoxy resin (JP-A-4-41581), and the like. However, these resins have a problem in the dielectric constant characteristics and cannot process signals at a higher speed.

As the low dielectric resin, fluorine resin, polyphenylene ether resin, polybutadiene resin having thermosetting 1,2-polybutadiene as a main component, 1,2-polybutadiene resin 5 to 20 parts by weight per 100 parts by weight of polyphenylene ether resin are used. 1 part by weight, a composition containing 5 to 10 parts by weight of a crosslinkable monomer and a radical crosslinking agent.
-83224) have been proposed, but are inferior in heat resistance, workability and non-film forming ability, and have problems in practical use.

[0005]

SUMMARY OF THE INVENTION An object of the present invention is to provide a thermosetting low-dielectric resin composition having a low dielectric constant, a low dielectric loss tangent, excellent adhesion to metal, and film-forming ability for use in printed wiring. An object of the present invention is to provide a circuit laminate material using a product.

[0006]

According to the present invention, there is provided a composition comprising a component (a) on one surface of a peelable film or at least one surface of a metal foil.
A siloxane-modified polyimide and a component (b) represented by the following formula (1)
(C) a circuit laminate material comprising an adhesive layer comprising a compound containing three allyl groups or methylallyl groups and a compound containing two or more maleimide groups as the component (c).

[0007]

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Further, in the present invention, the total amount of the components (b) and (c) is 10 to 900 parts by weight with respect to 100 parts by weight of the component (a).
An adhesive layer comprising 0.1 to 2.0 molar equivalents of the allyl group or methylallyl group of the component (b) with respect to 1 molar equivalent of the maleimide group is particularly preferably used.

[0009]

DESCRIPTION OF THE PREFERRED EMBODIMENTS First, the resin composition of the present invention is a thermosetting low dielectric resin composition. This resin composition is
It comprises (a) a siloxane-modified polyimide, component (b) a compound represented by the formula (1) containing three allyl groups or methylallyl groups, and component (c) a compound containing two or more maleimide groups. By using the siloxane-modified polyimide, the film forming ability of the resin composition is improved, and the scattering of the resin during operation is extremely reduced.
When manufacturing printed wiring boards, handling becomes better,
The yield is improved. The siloxane-modified polyimide used in the present invention contains 90 to 40 mol% of at least one structural unit represented by the following formula (2a) and the following formula (2b)
At least one structural unit represented by the formula:

[0010]

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(Wherein X is a direct bond, -O-, -SO
_{2 -, - CO -, -} C (CH 3) 2 -, - C (CF 3)
_{2 -, - COOCH 2 CH 2} OCO- either showed binding, Ar is a divalent group selected from Group having a structure according to formula with an aromatic ring (3), R is the methylene group Si Bound —CH ₂ OC ₆ H ₄ — or carbon number 1-10
And n represents an integer of 1 to 20. ).

[0012]

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(Wherein R ₁ , R ₂ , R ₃ and R ₄ may be the same or different and each represent a hydrogen atom, an alkyl group having 1 to 4 carbon atoms or an alkoxy group. It cannot be a hydrogen atom at the same time.) More preferably, the siloxane-modified polyimide has 90 to 40 mol% of at least one structural unit represented by the following formula (4a) and 1 to 40 mol% of the structural unit represented by the following formula (4b).
0-60 mol% is contained.

[0014]

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(Wherein X is a tetravalent aromatic group, 3,3 ′,
4,4′-diphenyl sulfone structure, 3,3 ′, 4
In any of the 4′-biphenyl structure and 2,3 ′, 3,4′-biphenyl structure, Ar has the same meaning as Ar in the formula (3), and R represents an alkylene group having 1 to 10 carbon atoms or a methylene group. -CH ₂ OC ₆ H _4- bonded to Si, and n
Represents an integer of 1 to 20. ). The siloxane-modified polyimide of the present invention has a weight average molecular weight of 5,000 to 50.
It is preferable that the material has a glass transition temperature of 150 ° C. or less and a dielectric constant of 3.0 or less. Weight average molecular weight of 5,
000-300,000, glass transition temperature 140 ° C
Hereinafter, it is more preferable that the dielectric constant is 3.0 or less, and it is further preferable that the weight average molecular weight is 10,000 to 300,000, the glass transition temperature is 130 ° C. or less, and the dielectric constant is 3.0 or less. When the weight average molecular weight is less than the lower limit of the above range, the thermal stability becomes poor, the heat resistance is reduced, and when the weight average molecular weight is larger than the upper limit of the above range, the melt viscosity increases. Property becomes poor. If the glass transition point temperature is higher than 150 ° C., the melting temperature will increase, leading to an increase in working temperature or poor adhesion. If the dielectric constant exceeds 3.0, the resin composition cannot be reduced in dielectric constant, and is not suitable for high-speed signal processing. In the present invention, the glass transition point temperature is a temperature measured as described below. Measurement conditions of glass transition temperature (Tg): Apparatus: Shear modulus measurement apparatus (Rheo Stress RS7 manufactured by HAAKE)
5) Measurement temperature range: -10 ° C to 300 ° C Heating rate: 3 ° C / min. Measurement frequency: 1 Hz Distortion rate: 0.01% ± 0.0025%.

The siloxane-modified polyimide used in the present invention
Can be obtained by using a general polyimide manufacturing method.
Can be obtained. That is, for each repeating structural unit
Tetracarboxylic dianhydride and each repeating structural unit
Production from diamine or diisocyanate corresponding to
it can. Specifically, as tetracarboxylic dianhydride
Pyromellitic dianhydride, 3,3 ', 4,4'-diphenyl
Rusulfonetetracarboxylic dianhydride, 3,3 ‘, 4
4'-benzophenonetetracarboxylic dianhydride, 3,
3 ', 4,4'-biphenyltetracarboxylic dianhydride
, 2,3 ', 3,4'-biphenyltetracarboxylic acid
Dianhydride, bis (3,4-dicarboxyphenyl) A
Terdianhydride, 4,4'-bis (3,4-dicarboxy)
Phenoxy) diphenyl sulfone dianhydride, ethylene glycol
Recall bis trimellitate dianhydride, 2,2-bis
[4- (3,4-dicarboxyphenoxy) phenyl]
And propane dianhydride and the like, more preferably 3,3 ', 4.
4'-diphenylsulfonetetracarboxylic dianhydride,
3,3 ', 4,4'-biphenyltetracarboxylic acid
Water, 2,3 ', 3,4'-biphenyltetracarboxylic
An acid dianhydride is used as a compound represented by the above formula (3) and
Reacting with the siloxane compound represented by the formula (6)
It can be manufactured by the following. (Wherein, R has the same meaning as R in formula (2b))

In the siloxane compound represented by the formula (6) used as a raw material for producing polyimide, the diamines in which the functional group Y is an amino group include bis (3-aminopropyl) tetramethyldisiloxane and bis (3-aminopropyl) tetramethyldisiloxane. 10
-Aminodecamethylene) tetramethyldisiloxane, aminopropyl-terminated dimethylsiloxane tetramer, octamer, bis (3-aminophenoxymethyl) tetramethyldisiloxane, etc., and these can be used in combination. .

In the compounds represented by the formula (6), as the diisocyanates wherein the functional group Y is an isocyanate group, in the diamines shown above, "amino" is replaced by "isocyanate". Can be mentioned. In the compound represented by the above formula (6), diisocyanates in which the functional group Y is an isocyanate group can be easily produced by reacting the corresponding diamine illustrated above with phosgene according to a conventional method. it can.

The siloxane-modified polyimide contains at least one structural unit represented by the formula (2a) in an amount of 90 to 40 mol%.
And at least one of the structural units represented by the formula (2b) is preferably 10 to 60 mol%. Equation (2
The diamines capable of constituting Ar represented by a) are more specifically exemplified as follows. 1,3-bis [1-
(3-Aminophenyl) -1-methylethyl] benzene, 1,3-bis [1- (4-aminophenyl) -1-
Methylethyl] benzene, 1,4-bis [1- (3-aminophenyl) -1-methylethyl] benzene, 1,4
-Bis [1- (4-aminophenyl) -1-methylethyl] benzene, bis [4- (3-aminophenoxy) phenyl] sulfone, bis [4- (4-aminophenoxy) phenyl] sulfone, 2,2 -Bis [3- (3-aminophenoxy) phenyl] propane, 2,2-bis [3- (4-aminophenoxy) phenyl] propane,
2,2-bis [4- (3-aminophenoxy) phenyl] propane, 2,2-bis [4- (4-aminophenoxy) phenyl] propane, 2,2-bis [3- (3-
Aminophenoxy) phenyl] hexafluoropropane, 2,2-bis [3- (4-aminophenoxy) phenyl] hexafluoropropane, 2,2-bis [4-
(3-Aminophenoxy) phenyl] hexafluoropropane, 2,2-bis [4- (4-aminophenoxy)
Phenyl] hexafluoropropane, 4,4'-diamino-3,3 ', 5,5'-tetramethyldiphenylmethane, 4,4'-diamino-3,3', 5,5'-tetraethyldiphenylmethane, 4 , 4'-Diamino-3,
3 ′, 5,5′-tetrapropyldiphenylmethane,
4,4′-diamino-3,3 ′, 5,5′-tetraisopropyldiphenylmethane, 4,4′-diamino-3,
3 ′, 5,5′-tetrabutyldiphenylmethane 4,
4'-diamino-3,3'-diethyl-5,5'-dimethyldiphenylmethane, 4,4-diamino-3,3'-
Dimethyldiphenylmethane, 4,4'-diamino-3,
3'-diethyldiphenylmethane, 4,4'-diamino-3,3 ', 5-5'-tetramethoxydiphenylmethane, 4,4'-diamino-3,3', 5,5'-tetraethoxydiphenylmethane, 4, 4'-diamino-3,
3 ′, 5,5′-tetrapropoxydiphenylmethane,
4,4-diamino-3,3 ', 5,5'-tetrabutoxydiphenylmethane, 4,4'-diamino-3,3'-
And dimethoxydiphenylmethane.

The siloxane-modified polyimide used in the present invention can be produced as follows. When tetracarboxylic dianhydride and diamine are used as raw materials, they may be used in an organic solvent in the presence of a catalyst such as tributylamine, triethylamine, or triphenyl phosphite as needed (20 parts by weight or less of the reactant). ), Heating to 100 ° C. or higher, preferably 180 ° C. or higher to directly obtain a polyimide; a polyamic acid which is a precursor of polyimide by reacting tetracarboxylic dianhydride and diamine in an organic solvent at 100 ° C. or lower Is obtained, if necessary, a dehydration catalyst such as p-toluenesulfonic acid (1 to 5 times the molar amount of tetracarboxylic dianhydride) is added, and a polyimide is obtained by imidation by heating, or Polyamic acid is converted to an acid anhydride such as acetic anhydride, propionic anhydride or benzoic anhydride, or a carbodiimide compound such as dicyclohexylcarbodiimide. And a ring-closing catalyst such as pyridine, isoquinoline, imidazole, triethylamine (dehydration ring-closing agent and ring-closing catalyst are 2 to 10 moles of tetracarboxylic dianhydride) as needed. There is a method of chemically ring closing at a low temperature (from room temperature to about 100 ° C.).

As the organic solvent used in the above reaction, N
-Methyl-2-pyrrolidone, N, N-dimethylacetamide, N, N-dimethylformamide, dimethylsulfoxide, sulfolane, hexamethylphosphoric triamide,
Aprotic polar solvents such as 1,3-dimethyl-2-imidazolidone, phenol, cresol, xylenol,
Phenol solvents such as p-chlorophenol are exemplified. If necessary, benzene, toluene, xylene, methyl ethyl ketone, acetone, tetrahydrofuran, dioxane, monoglyme, diglyme, methyl cellosolve, cellosolve acetate, methanol, ethanol, isopropanol, methylene chloride, chloroform, trichlene, nitrobenzene, etc. Can also be used as a mixture. Further, when using tetracarboxylic dianhydride and diisocyanate as raw materials, it is possible to produce according to the method of directly obtaining the above polyimide, the reaction temperature at this time is room temperature or higher, In particular, the temperature is preferably 60 ° C. or higher. The reaction between tetracarboxylic dianhydride and diamine or diisocyanate can be carried out in an equimolar amount to obtain a polyimide having a high degree of polymerization. It is also possible to produce polyimide using an excess amount in the following range.

The compound represented by the formula (1) containing three allyl groups or three methylallyl groups improves the heat resistance and the dielectric constant after curing of the resin composition. This compound is generally commercially available and can be easily obtained.

As the compound containing two or more maleimide groups, any compound can be used.
From the viewpoint of solvent solubility and the like, the following formulas (5-1) to (5-
5) is particularly preferred. These compounds are generally commercially available and can be easily obtained. It can also be synthesized by a conventionally known method.

[0024]

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The mixing ratio of the thermosetting low dielectric resin composition is as follows:
The total of components (b) and (c) is 10 to 900 parts by weight, preferably 50, based on 100 parts by weight of component (a).
To 900, more preferably 100 to 900 parts by weight. When the total of the component (b) and the component (c) is less than the lower limit of the above range by weight, the resin composition is cured, and the heat resistance of the resin composition, particularly, Tg and Young's modulus are significantly reduced,
Not suitable for intended use. On the other hand, when the amount exceeds 900 parts by weight, when the resin composition is cured to the B stage, the resin composition itself becomes brittle and causes scattering of the resin.
The mixing ratio of the component (b) to the component (c) is such that the allyl group or methylallyl group of the component (b) is 0.1 to 2.0 molar equivalents per 1 molar equivalent of the maleimide group of the component (c). , Preferably from 0.3 to
It is set to 1.8 molar equivalents, more preferably 0.5 to 1.5 molar equivalents. When the allyl group or methylallyl group equivalent is less than the lower limit of the above range, after curing of the resin composition,
If the electrical reliability deteriorates and exceeds the upper limit of the above range, gelation occurs during mixing, and it becomes impossible to prepare an adhesive.

The mixing of the components (a), (b) and (c) can be carried out in a solvent in which they are dissolved.
As the solvent, for example, N-methyl-2-pyrrolidone,
N, N-dimethylacetamide, N, N-dimethylformamide, dimethylsulfoxide, sulfolane, hexamethylphosphoric triamide, 1,3-dimethyl-2-imidazolidone, hexane, benzene, toluene, xylene, methylethylketone, acetone, diethylether, Tetrahydrofuran, dioxane, 1,2-dimethoxymethane, diethylene glycol dimethyl ether,
Methyl cellosolve, cellosolve acetate, methanol, ethanol, propanol, isopropanol, methyl acetate, ethyl acetate, acetonitrile, methylene chloride, chloroform, carbon tetrachloride, chlorobenzene, dichlorobenzene, dichloroethane, trichloroethane, and the like. The type and amount are appropriately selected and used so that the components are dissolved.

In the thermosetting low dielectric resin composition, diazabicyclooctane, methyl ethyl ketone peroxide, cyclohexane peroxide, 3, 3 3,5-trimethylcyclohexanone peroxide, methylcyclohexanone peroxide,
Methyl acetoacetate peroxide, acetylacetone peroxide, 1,1-bis (t-butylperoxy) -3,3.5-trimethylhexane, 1,1-bis (t-butylperoxy) -cyclohexane, 2,2-
Bis (t-butylperoxy) octane, n-butyl-
4,4-bis (t-butylperoxy) valate, 2,2
-Bis (t-butylperoxy) butane, t-butyl hydroperoxide, cumene hydroperoxide, di-isopropylbenzene hydroperoxide, p-menthane hydroperoxide, 2,5-dimethylhexane-2,5-di Hydroperoxide,
1,1,3,3-tetramethylbutyl hydroperoxide, di-t-butyl peroxide, t-butylcumyl peroxide, di-cumyl peroxide, α,
α'-bis (t-butylperoxy-m-isopropyl) benzene, 2,5-dimethyl-2,5-di (t-butylperoxy) hexane, 2,5-dimethyl-2,5-di (t -Butylperoxy) hexine, acetyl peroxide, isobutyl peroxide, octanoyl peroxide, decanoyl peroxide, benzoyl peroxide, lauroyl peroxide, 3,5,5-
Trimethylhexanoyl peroxide, succinic acid peroxide, 2,4-dichlorobenzoyl peroxide, m-toluoyl peroxide, di-
Isopropyl peroxydicarbonate, di-2-ethylhexylperoxydicarbonate, di-n-propylperoxydicarbonate, bis- (4-t-butylcyclohexyl) peroxydicarbonate, di-myristyl peroxydicarbonate, Di-2-ethoxyethyl peroxydicarbonate, di-methoxyisopropylperoxydicarbonate, di (3-methyl-3
-Methoxybutyl) peroxydicarbonate, di-allylperoxydicarbonate, t-butylperoxyacetate, t-butylperoxyisobutyrate, t
-Butylperoxypivalate, t-butylperoxyneodecanate, cumylperoxyneodecanate, t
-Butyl peroxy-2-ethyl hexanate, t-butyl peroxy-3,5,5-trimethyl hexanate,
t-butylperoxylaurate, t-butylperoxybenzoate, di-t-butylperoxyisophthalate, 2,5-dimethyl-2,5-di (benzoylperoxy) hexane, t-butylperoxymaleic acid , T
-Butylperoxyisopropyl carbonate, cumylperoxyoctate, t-hexylperoxyneodecanate, t-hexylperoxypivalate, t-butylperoxyneohexanate, acetylcyclohexylsulfonyl peroxide, t-butylperoxy Organic peroxides such as allyl carbonate, 1,2-dimethylimidazole, 1-methyl-2-ethylimidazole, 2-methylimidazole, 2-ethyl-4-methylimidazole, 2-undecylimidazole, 2-heptadecylimidazole , 2-phenylimidazole, 1
-Benzyl-2-methylimidazole, 1-benzyl-
2-phenylimidazole, 1-benzyl-2-phenylimidazole trimellitate, 1-benzyl-2
-Ethylimidazole, 1-benzyl-2-ethyl-5
-Methylimidazole, 2-ethylimidazole, 2-
Isopropylimidazole, 2-phenyl-4-benzylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-ethyl-4-methylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2- Isopropylimidazole, 1-cyanoethyl-2-phenylimidazole,
1-cyanoethyl-2-methylimidazolium trimellitate, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2,4-diamino-6- [2′-methylimidazolyl- (1 ′)]-ethyl-s -Triazine, 2,4-diamino-6- [2'-ethyl-4-methylimidazolyl- (1 ')]-ethyl-s-triazine, 2,4-diamino-6- [2'-undecylimidazolyl- (1 ′)]-Ethyl-s-triazine, 2-methylimidazolium isocyanuric acid adduct, 2-phenylimidazolium isocyanuric acid adduct, 2,4-
Diamino-6- [2'-methylimidazolyl-
(1 ′)]-Ethyl-s-triazine-isocyanuric acid adduct, 2-phenyl-4,5-dihydroxymethylimidazole, 2-phenyl-4-benzyl-5-hydroxymethylimidazole, 4,4′-methylene -Bis- (2-ethyl-5-methylimidazole), 1-aminoethyl-2-methylimidazole, 1-cyanoethyl-2-phenyl-4,5-di (cyanoethoxymethyl)
Imidazole, 1-dodecyl-2-methyl-3-benzylimidazolium chloride, 2-methylimidazole / benzotriazole adduct, 1-aminoethyl-2-
Ethyl imidazole, 1- (cyanoethylaminoethyl) -2-methylimidazole, N, N ′-[2-methylimidazolyl- (1) -ethyl] -adipoyldamide, N, N′-bis- (2-methyl Imidazolyl-1-
Ethyl) urea, N- (2-methylimidazolyl-1-ethyl) urea, N, N ′-[2-methylimidazolyl-
(1) -ethyl] dodecandioyldiamide, N, N '
-[2-Methylimidazolyl- (1) -ethyl] eicosanedioiled diamide, imidazoles such as 1-benzyl-2-phenylimidazole / hydrochloride, and reaction accelerators such as triphenylphosphine may also be added. it can.

The thermosetting low dielectric resin composition has an average particle diameter of 1 μm in order to stabilize the fluidity of the resin composition.
The following fillers can be included. The content of the filler is 5 to 70% by weight of the total solid, preferably 10 to 70% by weight.
It is set in the range of 60% by weight, more preferably 20 to 50% by weight. When the content is lower than the lower limit of the above range, the effect of stabilizing the fluidity is reduced, and when the content is higher than the upper limit, the adhesive strength of the laminate decreases, and the dielectric constant increases. As the filler, for example, silica, quartz powder, alumina, calcium carbonate, magnesium oxide, diamond powder, mica, fluororesin, zircon powder and the like are used.

Next, the circuit laminate material of the present invention using the thermosetting low dielectric resin composition will be described. To produce the adhesive film and the resin-attached metal plate of the present invention,
The above resin composition may be applied to one or both surfaces of a metal foil or one surface of a peelable film and dried. At this time, the coating thickness is 5 to 100 μm, especially 1
It is preferably in the range of 0 to 70 μm. As the metal foil, a thickness of 10 to 200 μm, preferably 100 μm or less, particularly preferably 36 μm or less, copper, copper, silver, iron,
42 alloy and stainless steel are used. If the thickness is too large, it becomes difficult to form fine wiring, so the above range is preferable. The peelable film used for the adhesive film of the present invention has a thickness of 1 to 200 μm, preferably 10 to 1 μm.
Those having a size of 00 μm are used and act as a temporary support. Available peelable films include polypropylene film, fluororesin film, polyethylene film, polyethylene terephthalate film, paper,
And, in some cases, those obtained by imparting releasability to them with a silicone resin are exemplified. It is desirable that these peelable films have a 90 ° peel strength in the range of 0.01 to 7.0 g / cm. If the peel strength is smaller than the above range, there is a problem that the peelable film is easily peeled off during the adhesive tape conveyance, and if the peel strength is larger than the above range, the peelable film does not peel off cleanly from the adhesive layer,
Workability deteriorates. In the case of a metal foil with a resin in which the above-mentioned resin composition is applied to one or both surfaces of the metal foil to form an adhesive layer, a peelable protective film may be further provided on the adhesive layer. As the protective film, the same as the above-mentioned releasable film can be used.

Hereinafter, the present invention will be described in more detail with reference to examples.

EXAMPLES (Synthesis example of siloxane-modified polyimide) Synthesis example 1 2,2-bis [4- (4-aminophenoxy) phenyl]
29.42 g (72 mmol) of propane and 6.96 g (28 mmol) of diaminosiloxane represented by the above formula, wherein Y = NH 2, R = propyl and n = 1, and 3,3 ′,
35.83 g (100 mmol) of 4,4'-diphenylsulfonetetracarboxylic dianhydride and N-methyl-2
-Pyrrolidone (hereinafter referred to as "NMP") 300 ml
Was introduced under ice temperature, and stirring was continued for 1 hour. Next, this solution was reacted at room temperature for 2 hours to synthesize a polyamic acid. 50 ml of toluene and 1.
0 g of p-toluenesulfonic acid was added, the mixture was heated to 160 ° C., and an imidization reaction was carried out for 3 hours while separating water azeotropic with toluene as the reaction proceeded. Thereafter, toluene was distilled off, the obtained siloxane-modified polyimide varnish was poured into methanol, and the obtained precipitate was separated.
Through the steps of pulverization, washing and drying, the molar ratio of each structural unit represented by the above formula becomes (1a) :( 1
b) = molecular weight of 18,000, Tg = 72: 28
Siloxane-modified polyimide 6 having a dielectric constant of 2.8 at 30 ° C.
1.9 g (94% yield) was obtained. When the infrared absorption spectrum of the obtained siloxane-modified polyimide was measured,
Typical imide absorption was observed at 1718 cm ^-1 and 1783 cm ^-1 .

Synthesis Example 2 2,2-bis [4- (4-aminophenoxy) phenyl]
30.39 g (74 mmol) of propane, 19.94 g (26 mmol) of diaminosiloxane represented by the above formula, wherein Y = NH 2, R = propyl and n = 8, and 3,
29.42 g (100 mmol) of 3 ', 4,4'-biphenyltetracarboxylic dianhydride and 300 ml of NMP
In the same manner as in Synthesis Example 1, a siloxane-modified product having a molecular weight of (3a) :( 3b) = 74: 26, a molecular weight of 19,000, a Tg of 45 ° C., and a dielectric constant of 2.9 is obtained. 72.3 g (95% yield) of polyimide was obtained. When the infrared absorption spectrum of the obtained siloxane-modified polyimide was measured, typical imide absorption was observed at 1718 cm ^-1 and 1783 cm ^-1 .

Synthesis Example 3 2,2-bis [4- (4-aminophenoxy) phenyl]
Hexafluoropropane 41.48 g (80 mmol)
And 15.54 g (20 mmol) of diaminosiloxane represented by Y = NH 2, R = propyl and n = 8 in the above formula, and 29.42 g of 2,3 ′, 3,4′-biphenyltetracarboxylic dianhydride ( 100 mmol) and NMP
Siloxane having a molecular weight of 10,000, a Tg of 60 ° C. and a dielectric constant of 2.9, in which the molar ratio of each structural unit is (3a) :( 3b) = 80: 20, using 300 ml in the same manner as in Synthesis Example 1. 81.2 g (94% yield) of the modified polyimide was obtained. When the infrared absorption spectrum of the obtained siloxane-modified polyimide was measured, it was 1718 cm ^-1 and 178 cm ^-1.
Typical imide absorption was observed at 3 cm ^-1 .

(Preparation Example of Thermosetting Low Dielectric Resin Composition) Resin Composition Preparation Example 1 The siloxane-modified polyimide resin 10 obtained in Synthesis Example 3
0 parts by weight, 314 parts by weight of the compound represented by the formula (5-2), 86 parts by weight of the compound represented by the formula (1) in which R is a methyl group (the methyl allyl group relative to 1 mole equivalent of the maleimide group) The molar equivalent of 0.5) was added to tetrahydrofuran, sufficiently mixed and dissolved to obtain a resin composition varnish having a solid content of 30% by weight.

Resin Composition Preparation Example 2 The compound represented by the formula (5-2) was added to 259 parts by weight
Example 1 of preparing a resin composition except that the compound represented by the formula (1) in which R is a methyl group was replaced by 141 parts by weight (the molar equivalent of methylallyl group was 1.0 with respect to 1 molar equivalent of maleimide group). In the same manner as in above, a resin composition varnish was obtained.

Resin Composition Preparation Example 3 The compound represented by the formula (5-2) was added to 221 parts by weight of
Example 1 of preparing a resin composition except that the compound represented by the formula (1) in which R is a methyl group was replaced by 179 parts by weight (the molar equivalent of methylallyl group was 1.5 per mole equivalent of maleimide group). In the same manner as in above, a resin composition varnish was obtained.

Resin Composition Preparation Example 4 A compound represented by the above formula (5-2) was added to 64 parts by weight, and a compound represented by the above formula (1) wherein R was a methyl group was added to 36 parts by weight (maleimide A resin composition varnish was obtained in the same manner as in Preparation Example 1 of the resin composition except that the molar equivalent of methylallyl group was changed to 1.0) per 1 molar equivalent of the group.

Resin Composition Preparation Example 5 The compound represented by the formula (5-2) was added to 584 parts by weight
Example 1 of preparing a resin composition except that the compound represented by the formula (1) in which R is a methyl group was replaced by 316 parts by weight (the molar equivalent of methylallyl group was 1.0 with respect to 1 molar equivalent of maleimide group). In the same manner as in above, a resin composition varnish was obtained.

Resin Composition Preparation Example 6 314 parts by weight of the compound represented by the formula (5-2) was added to 298 parts by weight of the compound represented by the formula (5-1), and In the same manner as in Resin Composition Preparation Example 1 except that 86 parts by weight of the compound in which R is a methyl group was replaced by 102 parts by weight (the molar equivalent of methylallyl group to 1 molar equivalent of maleimide group was 1.0) A composition varnish was obtained.

Resin Composition Preparation Example 7 314 parts by weight of the compound represented by the formula (5-2) was added to 278 parts by weight of the compound represented by the formula (5-3), and In the same manner as in Resin Composition Preparation Example 1, except that 86 parts by weight of the compound in which R is a methyl group was replaced by 122 parts by weight (the molar equivalent of methylallyl group to 1 molar equivalent of maleimide group was 1.0). A composition varnish was obtained.

Resin Composition Preparation Example 8 314 parts by weight of the compound represented by the formula (5-2) was added to 271 parts by weight of the compound represented by the formula (5-4) wherein p was 0 (zero). And the resin composition except that 86 parts by weight of the compound represented by the formula (1) in which R is a methyl group was replaced by 129 parts by weight (the molar equivalent of methylallyl group was 1.0 with respect to 1 molar equivalent of maleimide group). A resin composition varnish was obtained in the same manner as in Preparation Example 1.

Resin Composition Preparation Example 9 314 parts by weight of the compound represented by the formula (5-2) was added to 309 parts by weight of the compound represented by the formula (5-4) wherein p was 4, R of the compounds represented by (1)
Was replaced with 90 parts by weight (the molar equivalent of methylallyl group was 1.0 with respect to 1 molar equivalent of maleimide group) except that 86 parts by weight of the compound having a methyl group was a methyl group. I got a varnish.

Resin Composition Preparation Example 10 314 parts by weight of the compound represented by the formula (5-2) was added to 333 parts by weight of the compound represented by the formula (5-4) wherein p was 8, R of the compounds represented by (1)
Is a methyl group, except that 86 parts by weight of the compound is replaced by 67 parts by weight (the molar equivalent of methylallyl group to 1 mole equivalent of maleimide group is 1.0). I got a varnish.

Resin Composition Preparation Example 11 314 parts by weight of the compound represented by the formula (5-2) was added to 294 parts by weight of the compound represented by the formula (5-5), and In the same manner as in Resin Composition Preparation Example 1, except that 86 parts by weight of the compound in which R is a methyl group was replaced by 106 parts by weight (the molar equivalent of methylallyl group to 1 molar equivalent of maleimide group), A composition varnish was obtained.

Resin Composition Preparation Example 12 A resin composition was prepared in the same manner as in Resin Composition Preparation Example 2 except that the siloxane-modified polyimide obtained in Synthesis Example 3 was replaced with the siloxane-modified polyimide obtained in Synthesis Example 1. I got a varnish.

Resin Composition Preparation Example 13 A resin composition was prepared in the same manner as in Resin Composition Preparation Example 2 except that the siloxane-modified polyimide obtained in Synthesis Example 3 was replaced with the siloxane-modified polyimide obtained in Synthesis Example 2. I got a varnish.

Resin Composition Preparation Example 14 150 parts by weight of silica filler was dispersed in the resin composition varnish obtained in Resin Composition Preparation Example 2 to obtain a resin composition varnish.

Resin Composition Preparation Example 15 300 parts by weight of silica filler was dispersed in the resin composition varnish obtained in Resin Composition Preparation Example 2 to obtain a resin composition varnish.

Resin Composition Preparation Example 16 The siloxane-modified polyimide resin 10 obtained in Synthesis Example 3
0 parts by weight, 273 parts by weight of the compound represented by the formula (5-2), 127 parts by weight of the compound represented by the formula (1) wherein R is hydrogen (the mole of the allyl group relative to 1 mole equivalent of the maleimide group) (1.0 equivalent) was added to tetrahydrofuran, mixed and dissolved sufficiently to obtain a resin composition varnish having a solid content of 30% by weight.

Resin Composition Preparation Example 17 A compound represented by the above formula (5-2) was added to 68 parts by weight, and a compound represented by the above formula (1), wherein R was hydrogen, was added to 32 parts by weight (maleimide group). A resin composition varnish was obtained in the same manner as in Resin Composition Preparation Example 16 except that the molar equivalent of allyl group was changed to 1.0) per 1 molar equivalent.

Resin Composition Preparation Example 18 The compound represented by the formula (5-2) was added to 615 parts by weight
Resin composition Preparation Example 16 except that among the compounds represented by the formula (1), the compound in which R was hydrogen was replaced with 285 parts by weight (the molar equivalent of allyl group was 1.0 with respect to 1 molar equivalent of maleimide group). The same operation was performed to obtain a resin composition varnish.

Resin Composition Preparation Example 19 325 parts by weight of the compound represented by the formula (5-2) was added to 310 parts by weight of the compound represented by the formula (5-1), and Wherein R is hydrogen
A resin composition varnish was obtained by operating in the same manner as in Resin Composition Preparation Example 16 except that the parts by weight was changed to 90 parts by weight (the molar equivalent of the allyl group relative to 1 molar equivalent of the maleimide group was 1.0).

Resin Composition Preparation Example 20 325 parts by weight of the compound represented by the formula (5-2) was added to 291 parts by weight of the compound represented by the formula (5-3), and Wherein R is hydrogen
A resin composition varnish was obtained by operating in the same manner as in Resin Composition Preparation Example 16 except that the parts by weight was changed to 109 parts by weight (the molar equivalent of the allyl group relative to 1 molar equivalent of the maleimide group was 1.0).

Resin Composition Preparation Example 21 A resin composition was prepared in the same manner as in Resin Composition Preparation Example 16 except that the siloxane-modified polyimide obtained in Synthesis Example 3 was replaced with the siloxane-modified polyimide obtained in Synthesis Example 1. I got a varnish.

Resin Composition Preparation Example 22 A resin composition was prepared in the same manner as in Resin Composition Preparation Example 16 except that the siloxane-modified polyimide obtained in Synthesis Example 3 was replaced with the siloxane-modified polyimide obtained in Synthesis Example 2. I got a varnish.

(Examples) Examples 1 to 22 A copper foil having a thickness of 18 μm so that the adhesive layer after drying the resin composition varnish obtained in each of the resin composition preparation examples 1 to 22 has a thickness of 60 μm. And dried at 140 ° C. for 5 minutes in a hot-air circulation dryer to prepare a resin-coated copper foil. The created resin-coated copper foil has no resin cracking and scattering in the resin near the cutting point when cutting with a cutter knife,
The handleability was good. On the other hand, resin composition preparation example 1
The resin composition varnish obtained in No. 22 to No. 22 is impregnated with 100 parts by weight of an aromatic polyester nonwoven fabric (thickness: 0.1 mm, manufactured by Kuraray Co., Ltd.) so as to have a solid content of 120 parts by weight, and dried at 140 ° C. The prepreg was dried in an oven for 5 minutes. Four prepregs are superimposed on each other, and a copper foil of 18 μm is arranged on the upper and lower outermost layers.
At a pressure of m ² , a double-sided copper-clad laminate of 0.4 mm was obtained at 200 ° C., and unnecessary portions of the copper foil on both sides were removed by etching to form an inner layer circuit board. Then, the resin-coated copper foil is stacked so that the resin surface faces the inner layer circuit, and
It was molded under a heating condition of 200 ° C. and 2 hours under a pressure of kg / cm ² to prepare a multilayer copper-clad laminate having an inner layer circuit. Table 1 shows the test results.

Example 23 The resin obtained in Resin Composition Preparation Example 2 was used and had a thickness of 18
A multilayer metal-clad laminate with an inner layer circuit was prepared in the same manner as in Examples 1 to 22, except that the μm copper foil was replaced by a 42 μm-thick 42 alloy foil. Table 1 shows the test results.

Example 24 One side of a 38 μm thick polyethylene terephthalate film obtained by subjecting the resin composition varnish obtained in Resin Composition Preparation Example 2 to a release treatment so that the thickness of the adhesive layer after drying was 60 μm was obtained. It was applied and dried at 140 ° C. for 5 minutes in a hot air circulation type drier to form an adhesive film. The produced adhesive film had no resin cracking or scattering in the resin in the vicinity of the cut portion when cut with a cutter knife, and the handleability was good. On the other hand, the resin composition varnish obtained in Resin Composition Preparation Example 2 was applied to an aromatic polyester nonwoven fabric (with a thickness of 0.1 mm).
1 mm, manufactured by Kuraray Co., Ltd.)
It was impregnated to 20 parts by weight and dried in a drying oven at 140 ° C. for 5 minutes to prepare a prepreg. Four prepregs are stacked on top of each other, and 18 μm
m of copper foil, and at a pressure of 20 kg / cm ² , 200
A 0.4 mm double-sided copper-clad laminate at 0.4 ° C. was obtained, and unnecessary portions of the copper foil on both sides were removed by etching to prepare an inner circuit board. Then, the resin film of the adhesive film is superimposed on both surfaces of the inner circuit board so that the resin surface faces the inner circuit, and 20 kg
/ Cm ² under a heating condition of 200 ° C. for 2 hours to produce a multilayer copper-clad laminate having an inner circuit. Table 1 shows the test results.

Comparative Example 1 Siloxane-modified polyimide resin 10 obtained in Synthesis Example 3
0 parts by weight and 400 parts by weight of the compound represented by the formula (5-2) are added to tetrahydrofuran and mixed well.
Using a resin composition having a solid content of 30% by weight, the same operation as in Examples 1 to 22 was performed to prepare a multilayer copper-clad laminate having an inner circuit. Table 1 shows the test results.

Comparative Example 2 179 parts by weight of the compound represented by the formula (5-2) and 168 parts by weight of the compound represented by the formula (1) in which R is a methyl group (methylallyl relative to 1 mole equivalent of the maleimide group) The molar equivalent of the group is 1.0), added to tetrahydrofuran, thoroughly mixed and dissolved, and using a resin composition having a solid content of 30% by weight, operating in the same manner as in Examples 1 to 22, to form the inner layer. A multilayer copper-clad laminate with a circuit was prepared. Table 1 shows the test results.

Comparative Example 3 Using a resin composition varnish obtained in the same manner as in Resin Composition Preparation Example 1 except that the siloxane-modified polyimide obtained in Synthesis Example 3 was replaced with an acrylonitrile-butadiene copolymer. In the same manner as in Examples 1 to 22, a multilayer copper-clad laminate containing an inner layer circuit was prepared. Table 1 shows the test results.

Table 1 Characteristics Dielectric constant Peel strength Hunter heat resistance Spattering property PCBT Example 1 2.9 1.3 kg / cm No abnormality No cracking No short-circuiting Example 2 2.8 1.2 kg / cm No abnormality No burring No short-circuiting Example 3 2.9 1.3 kg / cm No abnormality No cracking No short circuit Example 4 2.9 1.2 kg / cm No abnormality No cracking No short circuit Example 5 3.0 1.2 kg / cm No abnormality No cracking No short circuit Example 6 3.0 1.3 kg / cm No abnormality No burr No short circuit Example 7 3.0 1.3 kg / cm No abnormality No crack No short circuit Example 8 2.8 1.3 kg / cm No abnormality No crack No short circuit Example 9 9 1.2 kg / cm No abnormality No crack No short circuit Example 10 2.8 1.2 kg / cm No abnormality No crack No short example 11 2.9 1.2 kg / cm No abnormality No crack No short Example 12 2.8 1.2 kg / cm No abnormality No crack No short example Example 13 3.0 1.3 kg / cm No abnormality No crack No short Example 14 2.9 1.3 kg / cm No abnormality No crack No short example 15 2.8 1.2 kg / cm No abnormality No crack No short circuit Example 16 2.9 1.2 kg / cm No abnormality No crack No short example 17 2.9 1.4 kg / cm No abnormality No crack No short circuit Example 183 2.0 1.4 kg / cm No abnormalities No irregularities No short-circuit Example 19 3.0 1.4 kg / cm No abnormalities No irregularities No short-circuits Example 20 2.9 1.3 kg / cm No abnormalities No irregularities No shorts

Table 1 (continued) Characteristics Dielectric constant Peel strength Hunter heat resistance Spattering property PCBT Example 21 2.9 1.4 kg / cm No abnormality No cracking No short circuit Example 22 2.9 1.2 kg / cm No abnormality No cracking No short circuit Example 23 2.9 1.2 kg / cm No abnormality No cracking No short circuit Example 24 2.8 1.3 kg / cm No abnormality No cracking No short comparative example 1 3.3 1.4 kg / cm Copper foil blister No cracking Short None Comparative Example 2 2.8 1.3 kg / cm No abnormality No cracking No short circuit Comparative Example 3 3.5 1.2 kg / cm No abnormality No cracking No short circuit

(Evaluation Method) Dielectric constant: Measured according to JIS C6481 (relative dielectric constant and dielectric loss tangent), and measured by measuring the capacitance at a frequency of 1 MHz. Peel strength: Measured according to JIS C6481 (peeling strength). Solder heat resistance: Measured according to JIS C6481 (solder heat resistance), and the solder heat resistance was checked for any abnormal appearance at 260 ° C. PCBT: 100 μm between lines by etching on the surface of the laminate
A pattern of 0.1m thick on the pattern
m of prepreg were laminated, and heated and pressed at a pressure of 20 kg / cm 2 and a temperature of 200 ° C. for 2 hours to prepare a test body. 5V applied to test specimen, 121 ° C, 2 atm, 100% R
H, the presence or absence of a short between the patterns was examined under the conditions of 1000 hours. Scatterability: The semi-cured resin-coated copper foil was punched out with a mold, and the end face was observed.

[0065]

According to the present invention, low dielectric constant, excellent heat resistance, sufficient peel strength at room temperature, no resin cracking and scattering in the vicinity of the cut portion at the time of cutting, and good handleability. Is provided. The circuit laminate material of the present invention is suitable for use in printed wiring boards and the like.

──────────────────────────────────────────────────続 き Continued on the front page (51) Int.Cl. ⁷ Identification symbol FI Theme coat ゛ (Reference) C08L 35/00 C08L 35/00 4J100 39/04 39/04 C09J 7/02 C09J 7/02 Z 179/08 179/08 Z H05K 1/03 610 H05K 1/03 610N (72) Inventor Ken Sato 3-1, Yomuneha-cho, Shizuoka-shi, Shizuoka Prefecture Electronic Materials Division, Hamakawa Paper Co., Ltd. (72) Daisuke Orino F-1 Term (Reference) 4-3, Yomune-cho, Yomunecho, Shizuoka City, Shizuoka Pref., Ltd. CA04 CA06 CA08 CC02 DA04 DB02 DB03 FA05 4J040 EH031 EH032 EK111 EK112 FA061 FA062 FA181 FA182 FA191 FA192 JA09 JB02 LA09 MA02 MB03 NA20 4J043 PA04 PA08 PC01 6 PC116 QB26 QB58 RA34 SA06 SA11 SA72 SB02 TA22 TB01 UA122 UA131 UA141 UA151 UA231 UA262 UB011 UB022 UB061 UB062 UB122 UB131 UB141 UB152 UB172 UB301 UB302 WA09 XA14 XA15 XA16 XA18 XA XB18 XA18 XA18 XA18 XA18 XA18BA JA43

Claims (12)

[Claims] 1. A component (a) a siloxane-modified polyimide, a component (b) a compound containing three allyl groups or methyl allyl groups represented by the following formula (1), and a component (a) c) A circuit laminate material characterized by laminating an adhesive layer comprising a compound containing two or more maleimide groups. Embedded image 2. The composition according to claim 1, wherein each component is component (a) 1.
The total amount of the component (b) and the component (c) is 10 to 900 parts by weight with respect to 00 parts by weight, and the amount of the methylallyl group of the component (b) is 0.1 to 1 mol equivalent to 1 mole equivalent of the maleimide group of the component (c). 2. The circuit laminate material according to claim 1, having a molar equivalent of 2.0. 3. The siloxane-modified polyimide of the component (a) contains 90 to 40 mol% of at least one of the structural units represented by the following formula (2a) and at least one of the structural units represented by the following formula (2b): The circuit laminate material according to claim 1, wherein one kind of the laminate material is contained in an amount of 10 to 60 mol%. (Wherein X is a direct _{bond, -O -, - SO 2 -} , - CO-,
—C (CH ₃ ) ₂ —, —C (CF ₃ ) ₂ —, —COOCH ₂
CH ₂ OCO—indicates any bond, Ar represents a divalent group selected from a group of groups having a structure of the following formula (3) having an aromatic ring, and R represents —CH in which a methylene group is bonded to Si. _Two
It represents OC ₆ H ₄ — or an alkylene group having 1 to 10 carbon atoms, and n represents an integer of 1 to 20. ) Formula (3) (In the formula, R ₁ , R ₂ , R ₃ and R ₄ may be the same or different and each represent a hydrogen atom, an alkyl group having 1 to 4 carbon atoms or an alkoxy group. Is not.) 4. The siloxane-modified polyimide of the component (a) comprises 90 to 40 mol% of at least one of the structural units represented by the following formula (4a) and at least one of the structural units represented by the following formula (4b): 4. The circuit laminate material according to claim 3, wherein one kind is contained in an amount of 10 to 60 mol%. (Wherein X is a tetravalent aromatic group, 3,3 ′, 4,4′-diphenylsulfone structure, 3,3 ′, 4,4′-biphenyl structure, 2,3 ′, 3,4′- Ar is a divalent group selected from a group having the structure represented by the formula (3), R is an alkylene group having 1 to 10 carbon atoms or a methylene group bonded to Si. -CH ₂ OC ₆ H
₄ - shows a, n represents an integer of 1 to 20. ). 5. The siloxane-modified polyimide of component (a) has a dielectric constant of 3.0 or less.
The described circuit laminate material. 6. The circuit laminate material according to claim 1, wherein the siloxane-modified polyimide as the component (a) has a glass transition temperature of 150 ° C. or lower. 7. The circuit laminate material according to claim 1, wherein the weight average molecular weight of the siloxane-modified polyimide of the component (a) is 5,000 to 500,000. 8. The compound of the component (c) containing two or more maleimide groups is represented by the following formulas (5-1) to (5-5): The circuit laminate material according to claim 1, which is a compound represented by the formula: 9. The circuit laminate material according to claim 1, wherein a filler having an average particle size of 1 μm or less is contained in an amount of 5 to 70% of the total solid of the resin. 10. The material of the metal foil is copper, white copper, silver, iron,
The circuit laminate material according to claim 1, wherein the material is at least one selected from two alloys and stainless steel. 11. The metal foil has a thickness of 10 μm to 300 μm.
2. The circuit laminate material according to claim 1, wherein m is in the range of m. 12. A circuit laminate material, wherein a release film is provided on the surface of the adhesive layer according to claim 1.