JPH03275760A - Polyphenylene oxide resin composition and metal-plated laminate board - Google Patents

Abstract

PURPOSE:To provide the subject composition having a low dielectric constant, excellent adhesivity to laminates, excellent bleeding resistance, etc., and suitable for the circuit boards of electric equipments, etc., by compounding the prepolymer of triallyl isocyanurate and/or triallylcyanurate, etc. CONSTITUTION:A composition comprises polyphenylene oxide [e.g. poly(2,6- dimethyl-1,4-phenylene oxide)], the prepolymer of triallylisocyanurate and/or triallylcyanurate, a crosslinking polymer, a crosslinking monomer and, if necessary, a flame retardant or a mixture thereof with flame retardant auxiliary. The composition is formed into a sheet and/or a prepreg and subsequently laminated to a metal foil to form a laminate, which is, if necessary, further formed into a multi-layered laminate.

Description

DETAILED DESCRIPTION OF THE INVENTION (Industrial Field of Application) The present invention relates to a polyphenylene oxide resin composition and a gold-gold laminate using the same.

More specifically, the present invention is applicable to wiring boards used in electrical equipment, children's equipment, etc., as well as their conductivity properties, as well as their leak resistance, bleedability, and flame retardancy. The present invention relates to a polyphenylene oxide-based III fat composition and a metal-clad laminate using the same.

(Conventional technology VW) For wiring boards used in precision instruments, electronic computers, communication devices, etc., there are increasing demands for faster calculation processing, higher reliability, higher circuit density, and smaller size. In order to meet these demands, wiring boards are rapidly becoming more multi-layered and more precisely miniaturized.

Conventionally, such i! Epoxy resins, polyimide resins, and low dielectric constant resins such as fluorine resins and polybutadiene resins have been used for IA wire boards, and efforts are being made to improve their properties. It's coming.

(Problems to be Solved by the Invention) However, such conventional resins have not been able to fully satisfy the various characteristics required for high-density wiring boards.

For example, as wiring density increases, it is becoming essential for resins used in multilayer wiring boards to have excellent adhesion and bleed properties, and to be flame retardant.

However, in the conventional TA#3, there remained points to be further improved regarding such adhesion and bleeding properties.

Traditional resins are also generally flammable, so
A flame retardant is added to the fM resin used for wiring boards in order to efficiently and reliably make it flame retardant.

However, even if the resin itself has a low dielectric constant, adding a flame retardant will increase the resin dielectric constant. J6i! There is a problem in that it cannot correspond to the high-speed signal processing required for i-devices and computer-related equipment.

For this reason, high-speed signal processing can be performed stably with a low dielectric constant, and it also has excellent adhesion and bleedability in multilayer boards, as well as excellent flame retardancy, making it possible to increase the density of multilayer wiring. There has been a strong desire to create a new resin composition for laminates that can be used as a laminate, and a laminate using the same.

This invention was made to solve the problems of conventional laminates as described above, and it provides a resin composition that has a low dielectric constant, excellent adhesion and bleedability of multilayer boards, and is flame retardant. The purpose of the present invention is to provide a laminate using the same.

(Means for Solving the Problem) The present invention solves the above problems by using a prepolymer, a crosslinkable polymer, and a crosslinkable monomer of polyphenylene oxide, triallyl isocyanurate, and/or triallyl cyanurate. To provide a polyphenylene oxide resin composition characterized in that the polyphenylene oxide resin composition is blended with a polyphenylene oxide resin composition. The present invention also provides a flame retardant polyphenylene oxide resin composition comprising a flame retardant, or a flame retardant and a flame retardant aid.

As a laminate using these resin compositions, the present invention forms a sheet and/or prepreg from the above-mentioned polyphenylene oxide resin composition, and
Alternatively, the present invention also provides a polyphenylene oxide-based metal-clad laminate characterized by being formed by integrally laminating prepreg and metal foil.

The polyphenylene oxide used in the polyphenylene oxide resin composition of the present invention has a relatively high glass transition point, low dielectric constant, and low dielectric loss. It has attracted attention in recent years because it is a fat and is inexpensive. However, until now, it has been difficult to improve adhesion and bleed properties and to achieve flame retardancy when multilayering, so it has not been put to practical use as a resin for high-density wiring boards. .

However, in the present invention, a prepolymer of triallyl isocyanurate and/or triallyl cyanurate is added to the polyphenylene oxide resin composition.
A crosslinkable polymer and a crosslinkable monomer are blended, and further,
By adding a flame retardant or a flame retardant and a flame retardant aid, it is possible to improve the adhesion and bleedability of the multilayer wiring board while maintaining its low dielectric property, thereby making it flame retardant. Furthermore, the resin has excellent properties such as heat resistance, chemical resistance, processability, and dimensional stability.

The polyphenylene oxide used in this invention has, for example, the following general formula (1) [R represents hydrogen or a hydrocarbon group having 1 to 3 carbon atoms,
Each R is represented by 2, which may be the same or different; for example, poly(2
, 6-dimethyl-1,4-phenylene oxide), poly(3,5-dimethyl-1,4-)unicine oxide), and the like.

The molecular weight is not particularly limited, but if the weight average molecular weight (Mw) is about 50,000 and the molecular weight distribution Mw/Mn=4.2 (Mn is the number average molecular weight), cr tI 'F=Illustrated as an example, two and two are possible.

A popular polyphenysine oxide, likened to 2-poly(2,6-dimethyl-1,4-)unisine oxide)
In the case of 2.6-'! It can be obtained by subjecting Ersilenol to an oxidative coupling reaction with an oxygen-containing gas and methanol in the presence of a catalyst. here,
As a catalyst, a copper(I) compound, N,N'-diter
Can include t-butylethylenediamine, butyldimethylamine and hydrogen bromide. Also, methanol is 2 to 15' based on tt! jL 1% water is added to the reaction mixture system, and the total of methanol and water is 5 to 25 weight 1%.
It can be used as a polymerization solvent.

Further, the triallyl isocyanurate (TAIC) or triallyl cyanurate (TAC) blend to be incorporated into the composition of the present invention can be produced by solution polymerization or bulk polymerization.

In solution polymerization, the reaction is milder than in bulk polymerization, and molecular JIH adjustment is easier. In this method, a triallyl isocyanurate monomer and/or a triallyl cyanurated monomer are dissolved in a solvent, a radical initiator is mixed in, and the mixture is reacted with stirring until an appropriate molecular weight is reached, followed by heating if necessary. By doing this, you can do a knee jerk.

At this time, it is preferable to carry out the reaction using a reflux vessel and in an atmosphere free of oxygen.

The reaction atmosphere may be, for example, a nitrogen flowing atmosphere. In addition, as a solvent, benzene, toluene, xylene, methanol, ethanol, acetone,
Methyl ethyl getone, heptane, carbon tetrachloride, diku-3
0 methane, trichlorethylene, etc. can be used.

As the radical initiator, any suitable radical initiator can be used, including conventionally known ones. 2, benzoyl peroxide, 2,5-dimethyl-2,5-di(
Examples include benzoylperoxy)hexane, t-butylperoxybenzoate, and dicumyl peroxide.

Even if R1 is the triallylisocyanurate bleed polyester mentioned above? - can be produced as follows. (Example 1) 280 g of triallyl isocyanurate monomer, 11 g of benzoyl peroxide, and 1087 g of benzene.

was added and reacted for 6 hours while boiling under a nitrogen atmosphere using a reactor equipped with a stirrer and a reflux vessel. After benzene is recovered under reduced pressure, methanol is added, and the polymer is recovered and dried under reduced pressure. 139 g of polymer are obtained. The number average molecular weight is approximately 10.000.

(Example 2) Add 10 ir of dicumyl peroxide and 527 g of toluene to 225 g of triallylisocyanurate, and prepare poly'? − is obtained. Number average molecular weight is approximately 4,000
It is.

parable! Is it triallyl isocyanurate or triallyl cyanurate bleed poly that can be produced as described above? - It is preferable that the molecular strain of several thousand molecules is 10.000 or less.This triallyl isocyanurate and triallyl cyanurate are chemically structurally isomers, and have similar reactivity. , either or both can be used to exhibit polymer properties.

Cross-linked poly? - as ζ, 1,2-polybutadiene, 1,4-polybutadiene, polystyrene,
Styrene butazinine polymer, modified 1゜2-polybutadiene (maleic modification, acrylic modification, epoxy modification),
Examples include rubber fabric, and each can be used alone or in combination of two or more. These polymers may be in the form of elastomers or rubbers.

Also, cross-linking mono? Examples of −acrylates such as ester acrylates, epoxy acrylates, urethane acrylates, ether acrylates, melamine acrylates, alkyd acrylates, and silicone acrylates, and triallyl cyanurate and triallyl isocyanurate. , ethylene glycol dimethacrylate, divinylbenzene, diallyl phthalate, etc. -1■ Vinyltoluene,
Monofunctional monomers such as ethylvinylbenzene, styrene, and paramethylstyrene? -1) Polyfunctional epoxies can be exemplified, and each can be used alone or in combination of two or more. These frames
:'s policy? - and the blending of monomers improves film-forming properties, bridge properties, adhesion, heat resistance, and dielectric properties.

Furthermore, a flame retardant or a flame retardant aid can be added to the composition of the present invention, but
In this case, the flame retardant is usually one that can reduce the relative dielectric constant of the polyphenylene oxide resin composition to 4.0 or less after adding the flame retardant together with the flame retardant aid, and has a flame retardant rating of UL94 flame retardant. It is preferable to use a material that has a property of V-1 or -C based on the sex test method.

For example, a brominated diphenyl ether system having the following formula (2) (wherein R represents hydrogen, an aromatic group, or an aliphatic group),
Or a brominated polycarbonate system having the following formula (3) (wherein R represents hydrogen, an aromatic group or an aliphatic group),
Alternatively, brominated bisphenol compounds having the following formula (4), and furthermore, brominated cyanuric acid compounds having the following formula (5) can be exemplified as flame retardants (in the formula, R3
and R2↓, each represents hydrogen, an aromatic group, an aliphatic group, or a group of any of the following formulas <1> to (1/l>).

iii〉　-0-Co-C口=CH.

CH.

<iv> OCH2CH20Co CH=C
H2(V>OCH2CH20CC!C
=C12C! (.

These flame retardants may be used alone or in combination.

If necessary, a flame retardant aid may be used together with such a flame retardant to provide a synergistic effect on flame retardation.

In this case, flame retardant aids include, for example, antimony oxide (antimony dioxide, antimony pentoxide), zirconium oxide, antimony soda, and the like.

These flame retardant aids may be used alone or in combination. Flame retardant aids may be used alone or in combination as flame retardants.

In addition, when using these flame retardant aids, it is preferable to disperse them in an organic solvent for ease of handling.

When blending the triallyl isocyanurate and/or triallyl cyanurate prepolymer, crosslinkable polymer, crosslinkable monomer, flame retardant, or flame retardant and flame retardant aid into polyphenylene oxide, an initiator may be added. Can be used.

As the initiator, the following two types can be selected depending on whether the polyphenylene oxide resin composition is an ultraviolet curing type or a thermosetting type, but the initiator is of course not limited to these.

Examples of the ultraviolet curing photoinitiator (that is, one that generates radicals by ultraviolet irradiation) include benzoin, benzyl, allyldiazonium fluorobalate, benzyl methyl ketal, 2,2-jethoxyacetophenone, benzoyl isobutyl ether, p-tert-butyltrichloroacetophinione, benzyl (0-ethoxycarbonyl α-monoxime, biacetyl, acetophninone, benzophenone, mipilar ketone, ketoramethylthiuram sulfide, azobisisobutyronitrile, etc.) can be used.

In addition, as thermosetting initiators (that is, those that generate radicals by heat), dicumyl peroxide, t
ert-butylcumyl peroxide, benzoyl peroxide, di-tert-butyl peroxide, 2
．． 5-dimethyl-2,neezy<tert-butylperoxy)hexyne-3.2,5-dimethyl-2,5-
Di(tert-butylperoxy)hexane, α,
α′-bis(tert-butylperoxy-m-isopropyl)benzene [1.

peroxides such as 4〈or 1.3〉-bis(tert-butylperoxyisopropyl)benzene], 1-hydroxycyclohexylphenyledone, 2-
Hydroxy-2-methyl-1-phenyl-propane-1
-one, 1-(4-isopropylphenyl)-2-hydroxy-2-methylpropan-1-one, 2-chlorothio'r''nton, methylbenzoyl formate,
4,4-bisdimethylaminobenzophenone (Michlergeton), benzoin methyl ether, methyl-benzoyl benzoate, α-aziroxime ester, S
Biscum mill made by this oil and fat ■ can be used.

These initiators may be used alone or in combination of two or more.

Further, an initiator using ultraviolet rays and an initiator using heat may be used in combination.

The blending ratio of the above polyphenylene oxide, triallyl isocyanurate and/or triallyl cyanurate prepolymer, crosslinkable polymer and crosslinkable monomer, flame retardant or flame retardant, flame retardant aid, reaction initiator, etc. , usually preferably 5 to 95% by weight of polyphenylene oxide, triallyl isocyanurate and/or
or triallyl cyanurate prepolymer 1% to 95% by weight, crosslinkable polymer and crosslinkable polymer, 1% each
~95% by weight, flame retardant 1~90% by weight, and flame retardant aid 1~0% by weight.

Further, the blending ratio of the reaction initiator is preferably 0 to 10% by weight.

Of course, these blending ratios can be determined depending on the dielectric constant and resin properties required for the resin composition.

As described above, the polyphenylene oxide resin composition of the present invention contains polyphenylene oxide, triallyl isocyanurate and/or triallyl cyanurate prepolymer, a crosslinkable polymer and a crosslinkable monomer, and further a flame retardant and a crosslinkable monomer. Contains combustion aids, reaction initiators, etc., but by blending various inorganic fillers,
Its properties such as permittivity may be changed. What is the best example of such an inorganic filler? ．． Examples include the use of titanium oxide ceramics, barium titanate ceramics, lead titanate ceramics, strontium titanate ceramics, calcium titanate ceramics, lead zirconate ceramics, etc., singly or in combination.

The polyphenylene oxide resin composition of the present invention and its flame retardant composition as described above are usually dissolved and dispersed in a solvent and mixed. In this case, the amount of solvent used is 5 to 50% by weight of the polyphenylene oxide resin composition.
It is preferable to form a solution (or resin solid content in the range of 10 to 13% by weight based on the solvent). Examples of the solvent include halogenated hydrocarbons such as trichloroethylene, trichloroethane, chloroform, methylene chloride, and chlorobenzene, and benzene. , aromatic hydrocarbons such as toluene and xylene, acetone, carbon tetrachloride, etc., and trichloroethylene is particularly preferred. These can be used alone or in a mixture of two or more.

Next, to explain the polyphenylene oxide-based laminate of the present invention, a sheet is formed from the polyphenylene oxide-based resin composition as described above, or a prepreg is formed by impregnating the same into a base material, and if necessary, the sheet is , core materials etc. from prepreg! ! It can be manufactured by laminating and integrating it with other base materials, sheets, prepregs, metal foils, etc. in accordance with conventional methods.

Of course, multilayer board molding is also possible.

For example, a casting method can be used to form the sheet.

This casting method is a method in which a resin mixed with a solvent is formed into a thin layer by casting or coating, and then the solvent is removed to form a cured product. According to the casting method, a cured product can be obtained at a low temperature without using the costly calendar method. To explain this casting method specifically, polyphenylene oxide-based Il! is mixed in a solvent. For example, 5 to 700 (preferably 5 to 500) the fat composition is applied onto a mirror-treated iron plate or a carrier film for casting.
A sheet is obtained by casting (or coating) to a thickness of about μm and thoroughly drying to remove the solvent.

Casting Gokya 1. The type of J-ar film is not particularly limited, but it is preferably one that is insoluble in the above solvents, such as polyethylene terephthalate (rPETJ) film, polyethylene film, polypropylene film, polyester film, polyimide film, etc. (-), those subjected to mold release treatment are preferred.

Drying is performed by air drying or hot air drying, etc. The upper limit of the temperature range in this case must be lower than the boiling point of the solvent or lower than the heat-resistant temperature of the carrier film for casting (no (when drying) is preferred, and the lower limit shall be determined depending on the drying time and processability. Even if R, trichlorethylene is used as a solvent and PET film is used as a carrier film for casting, the temperature from room temperature to about 80°C is preferred. It is preferable to set the temperature within this range; however, if the temperature is increased within this range, the drying time can be shortened.

When manufacturing a bulipung by impregnating a base material with a polyphenylene oxide resin composition, the following method can generally be used.

That is, even if the base material is immersed (dipped) in a solvent dispersion of a polyphenylene oxide resin composition,
For example, polyphenylene oxide is added to the base material!
Impregnating and adhering the J fat composition 6 Next, remove the solvent by drying or the like or semi-cure to obtain the B stage. In this case, the impregnation amount of the polyphenylene oxide resin composition is not particularly limited, but it is preferably 30 to 80% by weight.The base material can be impregnated with resin such as glass cloth, aramid cloth, polyester cloth, nylon cloth, etc. What are the loss-like materials made of these materials?
It is also possible to use la fibrous materials such as printed materials and/or non-woven fabrics, paper such as kraft paper, linter paper, etc., and the material is not limited to these materials.

As the metal foil for circuit formation used in forming the metal-clad laminate, a wide variety of metal foils that are used for ordinary wiring boards can be used. For example, metal foil such as copper foil, aluminum tin, etc. can be used. In this case, it is preferable that the metal foil has a smooth adhesive surface and good isoelectricity in order to improve the characteristics of the printed wiring board.

Such metal foil can be processed into a desired comb body by a subtractive method or the like. Further, it can also be processed into desired comb-shaped circuits, electrodes, etc. by vapor deposition, additive methods (Tru additive method, semi-additive method), etc.

As a method for producing a laminate using a core material, sheet, or blob produced from a polyphenylene oxide resin composition, the following method can be used, for example.

That is, a predetermined number of appropriately dried sheets and/or prepregs are combined to achieve a predetermined design thickness, and if necessary, metal foil for the wiring type is also combined and laminated, and resin is formed by heating and compressing. are melted and bonded to each other in combinations such as sheets, sheets and prepreg or core material, bulipungu, sheets and metal foil, prepreg and metal foil, etc. to form a laminate. Furthermore, a multi-layered laminate is formed. Strong adhesion is obtained by this W& adhesion, but if the heating at this time causes a crosslinking reaction by the reaction initiator, a strong adhesion state can be obtained. The crosslinking reaction can be carried out by photocrosslinking such as ultraviolet irradiation, thermal crosslinking, radiation irradiation, and the like.

Note that such adhesion may be performed using an adhesive in combination.

There are no particular restrictions on the combination of sheets, brills, and core materials, but a symmetrical combination is recommended for secondary processing (etching, etc.) after molding.
This is preferable from the viewpoint of preventing warping due to the metal foil, and it is preferable to combine the sheet so that it is placed on the adhesive interface with the metal foil because the adhesion force will be increased.

The temperature during heat pressing depends on the combination of metal foil and sheet or prepreg, but for example, the heat fusion properties of the sheet can be used to bond metal foil and sheet, so the lamination pressing temperature depends on the sheet. Above the glass transition point, for example 160
It is preferable to set the temperature range to about 300°C.

Also, the polyphenylene oxide type of this invention! ! When crosslinking a 1-fat composition by placing it in a dryer and heating it, the crosslinking reaction depends on the reaction temperature of the initiator, so the heating temperature and heating time should be adjusted depending on the type of initiator. It is preferable to choose.

For example, the temperature is 150 to 300°C and the time is about 10 to 60 minutes.

The clamping pressure can be, for example, about 30 to 80 kg/'d.

The above-described heat-pressing method involves heating and laminating a predetermined number of the sheets and/or prepregs in advance, overlapping metal foil on one or both sides of the sheets, and
It is also possible to heat and press it again.

<Function> The resin composition of the present invention is a polyphenylene oxide resin #f16. It has excellent heat resistance, 1-method stability, chemical resistance of 8 degrees, and low dielectric constant, and has excellent adhesion and bleedability during multilayer board molding, as well as flame retardancy. Become.

Therefore, a laminate using the polyphenylene oxide resin composition of the present invention can be easily processed with high precision.
It is suitable for high-speed signal processing and can realize high-density multilayering.

EXAMPLES Next, Examples will be shown and the polyphenylene oxide resin composition of the present invention and a metal-clad laminate using the same will be explained in more detail.

(Example) Example 1 (A) Production of flame-retardant polyphenylene oxide-based resin composition In a reactor equipped with a pressure reduction device, 30% by weight of polyphenylene oxide (GE PP0) and styrene-butadiene copolymer (
Asahi Kasei ■: Turprene T406>4% by weight, triallyl isocyanurate (Nippon Kasei M; TAIC) 35% by weight, polytriallyl isocyanurate 4.5% by weight,
Add 20% by weight of flame retardant GX-6145 (Daiichi Kogyo Seiyaku) and 5% by weight of antimony pentoxide, a flame retardant aid, and then add toluene and stir thoroughly until a homogeneous solution is obtained. A polyphenylene oxide-based resin composition is obtained.

(B) Molding of laminate Next, the obtained flame-retardant polyphenylene oxide resin composition was coated onto a PET film using a coating machine to a thickness of 5.
Coat to a thickness of 00 μm.

After drying this at 50°C for about 10 minutes, the resulting film was released from the PET film and dried at 120°C for an additional 30 minutes to completely remove toluene, resulting in a crude flame-retardant polyphenylene oxide resin. Got a sheet. The thickness of this sheet was approximately 150 μm.

Stack 4 of these sheets, heat at 190℃, 50&t+r
Heat and press for 30 minutes under /'cd conditions to completely cure.
As shown in FIG. 1, a laminate is produced by laminating and fixing four sheets (1) together. A metal foil is laminated on this to obtain a metal-clad laminate.

Further, as shown in FIG. 2, a metal-clad laminate can also be obtained by manufacturing a prepreg (2) and laminating a metal foil (3) thereon.

Regarding the obtained laminate, the dielectric constant, dielectric loss tangent, soldering heat resistance, I! R foil peel strength, flame retardance, etc. were evaluated. The results are shown in Table 1, and these characteristics were extremely good.

Examples 2 to 9 Various resin compositions were prepared in the +IM manner in the same manner as in Example 1, with the formulations of flame-retardant polyphenylene oxide resin compositions as shown in Table 1. In addition, a laminate was similarly produced using the IJ resin composition.

The physical properties of the obtained laminate were similarly evaluated in terms of dielectric constant, dielectric loss tangent, solder heat resistance, copper foil peel strength, flame retardance, etc. The results are also shown in Table 1. As is clear from the comparison with the comparative example described below, the characteristics of the laminate of the present invention were very good.

Comparative Example 1 A resin composition as shown in Table 1 was produced in the same manner as in Example 1 without adding polytriallyl isocyanurate, a flame retardant, and a flame retardant aid. In addition, a laminate was produced using the resin composition, and its physical properties were evaluated.

It was inferior to the Examples in terms of properties such as adhesion and flame retardancy.

(Note) *a) Polyphenylene oxide (GE PPO3 *b) Triallylisocyanurate (Nippon Kasei TAIC) *C) Styrene-butadiene copolymer (Asahi Kasei Trubulen T406) *cl) GX-6142 (Dai-Kogyo Rai) R -250 (Daiichi Kogyo Seiyaku) BC-58; Great Lakes *e) PBP (Barbutyl 91 NOF) α, α-
Bis(t-butyl-peroxy-m-isopropyl) Benzene P25B (Vervexin 25B, NOF) 2,5-dimethyl-2,mean(t-butyl-peroxy) Hexane-3 Examples 10 to 18 <A) Polyphenylene oxide Production of polyphenylene oxide (GE) based resin
Toluene (Gyudon Kagaku) is added to PP0), polyallylisocyanurate and U/or polytriallyl cyanurate, crosslinking polymer and crosslinking monomer, flame retardant, flame retardant aid, etc. to form a homogeneous solution. The polyphenysine oxide resin composition shown in Table 2 is obtained by stirring thoroughly until the mixture becomes saturated with air and defoaming.

(B) Molding of laminate Next, the obtained polyphenylene oxide tree! 111
Impregnate a glass cloth with the 1 composition using an impregnating device,
The toluene is removed by drying at 10° C. for about 7 minutes to produce prepung with a resin content of 60%.

Four sheets of this prepreg are stacked together, and electrolysis #! with a thickness of 18 μm is applied on both sides. Layer the foil, 200'C150b
As shown in Fig. 2, four sheets of prepreg (2) and two sheets of copper foil (3) were pressed for 30 minutes under the conditions of t/aA.
A metal-clad laminate is produced by laminating and fixing the two together.

The properties of the obtained laminate were evaluated in the same manner as in Example 1, and excellent results as shown in Table 2 were obtained.

<C) Forming of a multilayer board Also, the metal-clad laminate thus obtained is formed into a multilayer and subjected to processing such as etching, through-hole processing, and other plating by ordinary methods to form 4 to 10 sheets that can be put to practical use.
Produce a multilayer board of layers. When this multilayer board was used as a wiring board for a high-speed signal processing circuit, signal delays were suppressed and good results were obtained. Varnish stability, bleedability, moldability, interlayer adhesion, oven heat resistance, through-hole reliability, etc. were also evaluated. The results are shown in Table 2. All had good multilayer board characteristics.

Comparative Examples 2 to 8 Polyphenylene oxide-based ms compositions were manufactured using the resin composition formulations shown in Table 2. Further, a metal-clad laminate was created using the resin composition, and its physical properties were measured in the same manner as in Examples 10-18.

As shown in Table 2, the flame retardance was poor, as well as the multilayer board's adhesion, bleedability, and other properties.

<Effects of the invention> Polyphenylene oxide, a prepolymer of triallyl isocyanurate and/or triallyl cyanurate, a crosslinkable polymer and a crosslinkable monomer, and further a flame retardant and a flame retardant aid, if necessary. By blending a reaction initiator accordingly, it has excellent heat resistance, dimensional stability, chemical resistance, good processability, low dielectric constant, and good adhesion and bleedability of multilayer plates. To obtain a resin at-material for laminates having excellent flame retardancy and the like.

Therefore, the laminate formed using the polyphenylene oxide resin composition of the present invention can be processed with high precision as a wiring board, has excellent heat resistance and chemical resistance during mounting, and has excellent flame retardancy. Furthermore, since it has good dielectric properties, it is also advantageous as a high-density multilayer wiring board for high-speed signal processing.

[Brief explanation of drawings]

FIGS. 1 and 2 are cross-sectional views showing embodiments of the laminate of the present invention, respectively. 1...Sheet 2...Prepreg 3...Metal foil

Claims (4)

[Claims] (1) A polyphenylene oxide resin composition comprising a prepolymer of polyphenylene oxide, triallyl isocyanurate and/or triallyl cyanurate, a crosslinkable polymer, and a crosslinkable monomer. (2) A flame-retardant polyphenylene oxide-based resin composition, characterized in that the composition according to claim (1) is blended with a flame retardant, or a flame retardant and a flame retardant aid. (3) A sheet and/or prepreg is formed from the polyphenylene oxide resin composition according to claim (1) or (2), and this sheet and/or prepreg is laminated and integrated with metal foil. Polyphenylene oxide metal clad laminate. (4) A claim characterized in that the product is formed by multilayer lamination molding (
3) The polyphenylene oxide metal-clad multilayer laminate described above.