TWI873765B - Manufacturing methods of a laminated board and a printed circuit board - Google Patents

Abstract

The present disclosure provides manufacturing methods of a laminated board and a printed circuit board. The method of manufacturing the laminated board includes disposing a thermosetting resin composition on a reinforcing material to form a prepreg; laminating a plurality of the prepregs to form a resin substrate; and disposing a metal foil layer on at least one surface of the resin substrate to form the laminate. The manufacturing method of the printed circuit board includes forming the printed circuit layer from the metal foil layer of the laminate by etching or electroplating process. The manufacturing methods of a laminated board and a printed circuit board of the present disclosure have specific components and proportions of the thermosetting resin composition, and provide the characteristics of low dielectric constant, low dielectric loss, and high peel strength of electronic circuit substrates.

Description

Manufacturing method of laminate and printed circuit board

The present invention relates to a method for manufacturing a laminate and a printed circuit board, and in particular to a method for manufacturing a laminate and a printed circuit board containing a thermosetting resin composition of a specific composition.

The advancement of modern information processing technology has prompted digital circuits to enter the stage of high-speed information processing and high-frequency signal transmission. In high-frequency circuits, electrical signal transmission loss is represented by the sum of dielectric loss, conductor loss, and radiation loss. The higher the frequency of the electrical signal, the greater the electrical signal transmission loss.

Since transmission loss will cause electrical signals to attenuate and destroy the reliability of electrical signals, dielectric loss, conductor loss and radiation loss must be reduced. The dielectric loss of electrical signals is proportional to the product of the dielectric loss angle of the insulator forming the circuit and the frequency of the electrical signal used. Therefore, by selecting insulating materials with a small dielectric loss angle, the transmission loss of electrical signals can be reduced.

US Patent US9428646B2 discloses the use of unsaturated polyphenylene ether and polybutadiene resin to control the dielectric properties of the insulating plate, but the compatibility of unsaturated polyphenylene ether and butadiene is poor, and the mixed product is prone to precipitation. Furthermore, bismaleimide is added to provide better copper bonding, however, the laminates prepared from these materials have a relatively high dissipation factor.

US Patent US5223568A discloses a laminate made of polybutadiene, polyisoprene and thermoplastic elastomer, and the obtained laminate has the characteristic of low loss. However, the polybutadiene sheet has poor peel strength when bonded to copper foil, and other properties such as mechanical strength, flammability and heat resistance are even worse.

Therefore, it is necessary to provide a manufacturing method for laminates and printed circuit boards used in electronic circuits to meet the requirements of electronic circuit products for comprehensive performance such as low dielectric constant, low dielectric loss, and high peeling strength.

The main purpose of the present invention is to provide a method for manufacturing a laminate, which includes: disposing a thermosetting resin composition on a reinforcing material to form a semi-cured adhesive sheet; pressing a plurality of the semi-cured adhesive sheets to form a resin substrate; and disposing a metal foil layer on at least one surface of the resin substrate to form the laminate. Specifically, the thermosetting resin composition comprises, with a total weight of 100 parts by weight, (A) 30 to 50 parts by weight of an unsaturated polyphenylene ether resin; (B) 10 to 30 parts by weight of a styrene-butylene block copolymer; (C) 5 to 25 parts by weight of a cycloolefin compound; (D) 1 to 10 parts by weight of a vinylphenyl compound; and (E) 5 to 25 parts by weight of a crosslinking agent; wherein the unsaturated polyphenylene ether resin comprises at least one carbon-carbon double bond or carbon-carbon triple bond, and at least one carboxyl group, and the carboxyl group is selected from the group consisting of carboxylic acids, anhydrides, amides and esters.

In one embodiment of the present invention, the reinforcing material is E-glass fiber (E-glass), NE-glass fiber (NE-glass) or polystyrene fiber cloth (PS-glass).

In one embodiment of the present invention, the styrene-butylene block copolymer is a block copolymer derived from an alkenyl aromatic compound block and a conjugated diene block.

In one embodiment of the present invention, the styrene-butylene block copolymer is a styrene-butylene block copolymer grafted with maleic anhydride.

In one embodiment of the present invention, the styrene-butylene block copolymer is at least one selected from the group consisting of styrene-butadiene diblock copolymer (SB), styrene-butadiene-styrene triblock copolymer (SBS), styrene-isoprene diblock copolymer (SI), styrene-isoprene-styrene triblock copolymer (SIS), styrene-(ethylene-butylene)-styrene triblock copolymer (SEBS), styrene-(ethylene-propylene)-styrene triblock copolymer (SEPS) and styrene-(ethylene-butylene) diblock copolymer (SEB).

In one embodiment of the present invention, the cycloolefin compound is at least one selected from the group consisting of dicyclopentadiene (DCPD) monomer, dicyclopentadiene polymer, norbornene monomer and 5-norbornene polymer.

In one embodiment of the present invention, the vinylphenyl compound is selected from diphenylethylene and/or bromostyrene.

In one embodiment of the present invention, the crosslinking agent is at least one selected from the group consisting of triallyl isocyanurate, triallyl cyanurate, dimaleimide resin and divinylbenzene.

In one embodiment of the present invention, the thermosetting resin composition further comprises: an accelerator, which is selected from di-tert-butyl peroxide, dilauryl peroxide, dibenzoyl peroxide, tert-butyl peroxyacetate, tert-butyl peroxybenzoate, 1,1-di-tert-butyl peroxy-3,5,5-trimethylcyclohexane, 1,1-di-tert-butyl peroxycyclohexane, 2,2-di(tert-butylperoxy)butane , bis(4-tert-butylcyclohexyl) peroxydicarbonate, hexadecyl peroxydicarbonate, tetradecyl peroxydicarbonate, dipentylhexyl peroxide, diisopropylbenzene peroxide, bis(tert-butylperoxyisopropyl)benzene, 2,5-dimethyl- 2,5-di-tert-butylperoxyhexane, 2,5-dimethyl-2,5-di-tert-butylperoxyhexyne and diisopropylbenzene hydroperoxide.

In one embodiment of the present invention, the thermosetting resin composition further comprises: an inorganic filler, wherein the inorganic filler is at least one selected from the group consisting of silicon dioxide, aluminum oxide, aluminum hydroxide, magnesium oxide, magnesium hydroxide, calcium carbonate, aluminum nitride, boron nitride, aluminum silicon carbide, silicon carbide, titanium dioxide, zinc oxide, zirconium oxide, barium sulfate, magnesium carbonate, barium carbonate, mica, talc and graphene.

Another object of the present invention is to provide a method for manufacturing a printed circuit board, which includes forming a printed circuit line layer from the metal foil layer of the laminated board prepared by the method for manufacturing a laminated board of the present invention by etching or electroplating.

One of the beneficial effects of the present invention is that the manufacturing method of the laminate and printed circuit board provided by the present invention can provide and meet the requirements of the electronic circuit substrate for comprehensive performance such as low dielectric constant, low dielectric loss, and high peel strength through the technical scheme of "the reinforcing material is E-glass fiber (E-glass), NE-glass fiber (NE-glass) or polystyrene fiber cloth (PS-glass)", "the unsaturated polyphenylene ether resin includes at least one carbon-carbon double bond or carbon-carbon triple bond, and at least one carboxyl group" and a specific formula ratio.

P:Printed circuit board

L: Laminated board

1: Resin substrate

2: Metal foil layer

11: Semi-cured adhesive film

111: Reinforcement materials

112: Thermosetting resin composition

FIG1 is a flow chart of the manufacturing method of the laminated board of the present invention; FIG2 is a schematic diagram of the structure of the laminated board of the present invention; FIG3 is a flow chart of the manufacturing method of the printed circuit board of the present invention; and FIG4 is a schematic diagram of the structure of the printed circuit board of the present invention.

Referring to FIG. 1 , the technical solution adopted by the present invention is to provide a method for manufacturing a laminate, including: S100 arranging a thermosetting resin composition on a reinforcing material to form a semi-cured adhesive sheet; S200 pressing a plurality of semi-cured adhesive sheets to form a resin substrate; and S300 arranging a metal foil layer on at least one surface of the resin substrate to form the laminate.

More specifically, S100 can be to immerse the reinforcing material into a thermosetting resin composition or to wet the thermosetting resin composition with a roller coating, and then to bake to evaporate the solvent and semi-cure the resin, cool and roll it to form a semi-cured film. S200 presses multiple semi-cured films to form a resin substrate. S300 hot pressing treatment is to overlap the resin substrate with at least one metal foil layer (such as copper foil), and then press it at 220°C under vacuum conditions. Preferably, S300 hot pressing treatment is to overlap the resin substrate with two metal foil layers (such as copper foil), so that the resin substrate is sandwiched between the two metal foil layers.

Referring to FIG. 2 , the laminate L prepared by the laminate manufacturing method of the present invention includes: a resin substrate 1 and a metal foil layer 2 disposed on at least one surface of the resin substrate. The resin substrate 1 includes a plurality of semi-cured adhesive sheets 11, and each of the semi-cured adhesive sheets 11 is made of a reinforcing material 111 coated with a thermosetting resin composition 112.

More specifically, the thermosetting resin composition comprises, with a total weight of 100 parts by weight, (A) 30 to 50 parts by weight of an unsaturated polyphenylene ether resin; (B) 10 to 30 parts by weight of a styrene-butylene block copolymer; (C) 5 to 25 parts by weight of a cycloolefin compound; (D) 1 to 10 parts by weight of a vinylphenyl compound; and (E) 5 to 25 parts by weight of a crosslinking agent; wherein the unsaturated polyphenylene ether resin comprises at least one carbon-carbon double bond or carbon-carbon triple bond, and at least one carboxyl group.

In one embodiment of the present invention, the reinforcing material is E-glass, NE-glass or polystyrene fiber cloth (PS-glass). E-glass, also known as alkali-free glass, is a borosilicate glass with good electrical insulation and mechanical properties, and is widely used in the production of glass fibers for electrical insulation. NE-glass has the characteristics of low dielectric constant and low dielectric loss factor. Compared with the reinforcing materials of polyethylene and polypropylene fibers with low melting points, the present invention selects a specific reinforcing material to maintain the CTE and heat resistance of the laminate.

Specifically, polyphenylene ether (PPE) resin has good mechanical properties and excellent dielectric properties, with a Dk/Df of about 2.45/0.0007 at a frequency of 1 MHz. It is the preferred resin material for substrates of high-frequency printed circuit boards. Preferably, the unsaturated polyphenylene ether resin used in the present invention is modified and includes the following multifunctional compounds: at least one carbon-carbon double bond or carbon-carbon triple bond, and at least one carboxyl group, for example, carboxylic acid, anhydride, amide, ester. More specifically, the unsaturated polyphenylene ether resin used in the present invention can be selected from terminal vinyl benzyl modified polyphenylene ether resin or difunctional methacrylate modified polyphenylene ether resin.

The styrene-butylene block copolymer includes a block copolymer of (A) a block derived from an alkenyl aromatic compound and (B) a block derived from a conjugated diene. More specifically, the styrene-butylene block copolymer can be selected from at least one of the group consisting of styrene-butadiene diblock copolymer (SB), styrene-butadiene-styrene triblock copolymer (SBS), styrene-isoprene diblock copolymer (SI), styrene-isoprene-styrene triblock copolymer (SIS), styrene-(ethylene-butylene)-styrene triblock copolymer (SEBS), styrene-(ethylene-propylene)-styrene triblock copolymer (SEPS) and styrene-(ethylene-butylene) diblock copolymer (SEB). In a specific embodiment of the present invention, the styrene-butylene block copolymer is a styrene-butylene block copolymer grafted with maleic anhydride.

The vinyl phenyl compound is selected from stilbene and/or bromostyrene compounds, for example, Saytex 3010 bromostyrene purchased from Albemarle Commercial. More specifically, the bromostyrene compound provides high flame retardancy, thermal stability, good compatibility, and no precipitation.

The cycloolefin is at least one selected from the group consisting of dicyclopentadiene (DCPD) monomers, dicyclopentadiene polymers, norbornene monomers and norbornene polymers having a bridging cycloolefin or a combination thereof.

Preferably, the crosslinking agent can be at least one selected from the group consisting of triallyl isocyanurate (TAIC), triallyl cyanurate (TAC), dimaleimide resin and divinylbenzene. If the proportion of the crosslinking agent is too high, the thermal conductivity of the crosslinked resin composition will be reduced (such as reducing the thermal conductivity coefficient K value). If the proportion of the crosslinking agent is too low, the thermal properties of the crosslinked resin composition will be poor (such as reducing the glass transition temperature Tg).

Furthermore, different promoters can be used depending on the physical property requirements of the product. Preferably, the promoter is a peroxide crosslinking promoter, more specifically, an organic peroxide free radical initiator. For example, the accelerator is at least one selected from the group consisting of di-tert-butyl peroxide, dilauryl peroxide, dibenzoyl peroxide, tert-butyl peroxyacetate, tert-butyl peroxybenzoate, 1,1-di-tert-butylperoxy-3,5,5-trimethylcyclohexane, 1,1-di-tert-butylperoxycyclohexane, 2,2-di(tert-butylperoxy)butane, bis(4-tert-butylcyclohexyl)peroxydicarbonate, hexadecyl peroxydicarbonate, tetradecyl peroxydicarbonate, dipentyl peroxide, diisopropylbenzene peroxide, di(tert-butylperoxyisopropyl)benzene, 2,5-dimethyl-2,5-di-tert-butylperoxyhexane, 2,5-dimethyl-2,5-di-tert-butylperoxyhexyne, and diisopropylbenzene hydroperoxide. In one embodiment, the accelerator is dicumyl peroxide (DCP) commercially available from Arkema.

Silane coupling agents can improve the metal adhesion of polyolefin materials. Silane coupling agents commonly used in the relevant technical field can be selected. For example, the inorganic functional group of the silane coupling agent is a trifunctional group, namely Si-(OR2). In one embodiment of the present invention, the silane coupling agent can be vinyl silane, amino silane, methacryloxy silane, etc.

Preferably, the flame retardant is a phosphorus-containing flame retardant and a brominated flame retardant. Examples of brominated flame retardants include ethylene-bis(tetrabromophenylene dicarboxamide), decabromodiphenylethane, and 2,4,6-tris(2,4,6-tribromophenoxy)-1,3,5-triazine. Examples of phosphorus-containing flame retardants include bisphenol diphenyl phosphate, ammonium polyphosphate, hydroquinone bis(diphenyl phosphate), bisphenol A bis(diphenyl phosphate), tri(2-carboxyethyl)phosphine (TCEP), tri(chloroisopropyl) phosphate, trimethyl phosphate (TMP), dimethyl methylphosphonate (DMMP), resorcinol bis(xylyl phosphate), phosphazene, melamine polyphosphate, 9,10-dihydro-9-oxo-10-phosphaphenanthrene-10-oxide (DOPO) and its derivatives or resins, melamine cyanurate, and trihydroxyethyl isocyanurate.

In one embodiment of the present invention, the flame retardant may be a DOPO compound, such as a DOPO resin (DOPO-HQ, DOPO-NQ, DOPO-PN or DOPO-BPN) and an epoxy resin containing DOPO. More specifically, DOPO-BPN may be selected from bisphenol-formaldehyde novolac compounds, such as DOPO-BPAN, DOPO-BPFN or DOPO-BPSN.

The inorganic filler is selected from the group consisting of silica, alumina, barium sulfate, talc, clay, mica powder, and boron nitride. More preferably, the inorganic filler is selected from the group consisting of fused silica, amorphous silica, and hollow silica, such as Lianrui D1028L spherical silica, which can adjust the dielectric constant, dielectric loss, and thermal expansion coefficient of the dielectric substrate layer. Specifically, the inorganic filler can increase the thermal conductivity of the resin composition, improve its thermal expansion and mechanical strength.

Referring to FIG. 3 , the present invention further provides a method for manufacturing a printed circuit board, which includes S400 using an etching or electroplating process to form a printed circuit line layer from the metal foil layer of the laminated board prepared by the present invention. In other words, S400 patterns the metal foil layer of the laminated board and forms a predetermined circuit.

Refer to Figure 4, which is a printed circuit board P prepared by the printed circuit board manufacturing method of the present invention. The metal foil layer 2 of the laminate L is patterned to form a printed circuit line layer.

[Implementation example]

Tables 1 to 3 of the present invention respectively provide the composition ratios of the thermosetting resin composition and the reinforcing material of Examples 1 to 14 and Comparative Examples 1 to 7. The thermosetting resin composition is prepared according to each composition ratio, and the reinforcing material is immersed in or wetted by roller coating the thermosetting resin composition. The solvent is evaporated by baking and the resin is semi-cured, cooled and rolled to form a semi-cured film. The plurality of semi-cured films are further subjected to heat pressing to form a dielectric substrate layer. Specifically, For example, the hot pressing process is to stack four semi-cured films and two 18μm copper foils (metal foil layers) from the same batch in the order of copper foil, four semi-cured films, and copper foil, and then press them at 220℃ for 2 hours under vacuum conditions to form a copper foil substrate, in which the four semi-cured films are cured to form an insulating layer between the two copper foils. The aforementioned copper foil is etched by a wet etching process to form a wiring pattern, forming a specific wiring circuit, and obtaining a printed circuit board.

Among them, the copper foil substrate has been tested for physical properties and the corresponding records are in Tables 1 to 3.

[Physical property test]

Peel strength: Peel tensile test is performed according to industry standards.

Heat resistance of copper foil laminate (T288): Also known as "soldering result", the heat resistance test is based on the industry standard IPC-TM-650 2.4.24.1, which is to immerse the copper foil laminate in a 288℃ solder furnace until the time required for the board to explode.

Dielectric constant (Dk): Measured according to IPC-TM-650 2.5.5 test specification. The dielectric constant represents the electronic insulation properties of the produced film. The lower the value, the better the electronic insulation properties.

Dielectric loss (Df): Measured according to IPC-TM-650 2.5.5 test specification. Dielectric loss indicates the ability of a substance to absorb microwaves of a certain frequency at a certain temperature. Usually in the specifications of communication products, the lower the dielectric loss value, the better.

Coefficient of thermal expansion (CTE): measured according to IPC-TM-650-2.4.24 test standard.

OPE-2St 2200: Terminal vinyl benzyl-modified polyphenylene ether (Mw: about 3600, purchased from Mitsubishi Gas Chemical Co., Ltd.)

SA-9000: Bifunctional methacrylate modified polyphenylene ether (Mw: 1700, purchased from SABIC)

SA90: Unmodified polyphenylene ether (Mw: 1700, commercially available from Saudi Basic Industries Corporation Innovative Plastics Co., Ltd.)

PPO640: non-modified polyphenylene ether, (molecular weight: 18000, commercially available from Saudi Basic Industries Company Innovative Plastics Co., Ltd.)

D-1118: Solid SB-SBS copolymer (commercially available from Keten Polymers)

G1648: SEBS compound (commercially available from Keten Polymers)

KIC19-023: SEBS copolymer grafted with maleic anhydride (commercially available from Keten Polymers)

Saytex3010: Brominated styrene

DCPD monomer: dicyclopentadiene (purchased from Zibo Luhua Hongjin New Materials Co., Ltd.)

Topas COC 5013: Cyclic olefin copolymer with non-reactive functional groups

TAIC: Triallyl isocyanurate

MIR3000: Biphenyl BMI

DCP: dicumyl peroxide (commercially available from Arkema)

KBM503: Vinyl silane (purchased from Shin-Etsu Corporation, Japan)

saytex 8010: decabromodiphenylethane

D1028L: Spherical silica purchased from Lianrui Commercial

Referring to Table 1, Examples 1 to 4 and Comparative Examples 1 and 2 show that the dielectric properties of unmodified polyphenylene ether deteriorate due to the presence of hydroxyl groups. In addition, the unmodified polyphenylene ether has better heat resistance to bleaching.

Refer to Table 2, maleic anhydride modified styrene-butylene block copolymer can effectively improve the peel strength, and its effect on dielectric properties is relatively small. From Comparative Example 3, it can be seen that the decrease in the proportion of polyphenylene ether in the formula of the thermosetting resin composition will lead to poor heat resistance, while the addition of vinyl phenyl compounds and crosslinking agents (triallyl isocyanurate, TAIC) helps to improve heat resistance.

Refer to Table 3. Comparative Examples 6 and 7 respectively use polyethylene (PE) and polypropylene (PP) fiber reinforcement materials with low melting points. They melt during the pressing process (above 190 degrees), which will cause the CTE of the substrate to increase and the heat resistance to deteriorate.

The beneficial effect of the present invention is that the thermosetting resin composition provided by the present invention can provide and meet the requirements of electronic circuit substrates for comprehensive properties such as low dielectric constant, low dielectric loss, and high peel strength through the technical solution of "the unsaturated polyphenylene ether resin includes multifunctional groups: at least one carbon-carbon double bond or carbon-carbon triple bond, and at least one carboxyl group" and a specific formula ratio.

In more detail, the unsaturated polyphenylene ether resin modified with specific groups improves the low dielectric properties caused by the hydroxyl group in polyphenylene ether and increases the heat resistance. The styrene-butylene block copolymer modified with maleic anhydride further improves the peeling strength and maintains its dielectric properties.

The above is only a better specific example of the present invention, and does not limit the patent scope of the present invention. Therefore, all equivalent changes made by applying the content of the present invention are also included in the scope of the present invention and are hereby stated.

Claims (11)

A method for manufacturing a laminate, comprising: placing a thermosetting resin composition on a reinforcing material to form a semi-cured adhesive sheet; pressing a plurality of the semi-cured adhesive sheets to form a resin substrate; and placing a metal foil layer on at least one surface of the resin substrate to form the laminate; wherein the total weight of the thermosetting resin composition is 100 parts by weight, and the thermosetting resin composition comprises: (A) 43 to 50 parts by weight of unsaturated polystyrene ether resin; (B) 22 to 30 parts by weight of styrene-butylene block copolymer; (C) 5 to 25 parts by weight of cycloolefin compound; (D) 1 to 10 parts by weight of vinylphenyl compound; and (E) 5 to 25 parts by weight of crosslinking agent; wherein the unsaturated polyphenylene ether resin comprises a multifunctional group: at least one carbon-carbon double bond or carbon-carbon triple bond, and at least one carboxyl group, and the carboxyl group is selected from the group consisting of carboxylic acid, anhydride, amide and ester. A method for manufacturing a laminate as described in claim 1, wherein the reinforcing material is E-glass fiber (E-glass), NE-glass fiber (NE-glass) or polystyrene fiber cloth (PS-glass). The method for manufacturing a laminate as described in claim 1, wherein the styrene-butylene block copolymer is a block copolymer derived from an alkenyl aromatic compound block and a conjugated diene block. The method for manufacturing a laminate as described in claim 1, wherein the styrene-butylene block copolymer is a styrene-butylene block copolymer grafted with maleic anhydride. The manufacturing method of the laminate as described in claim 1, wherein the styrene-butylene block copolymer is at least one selected from the group consisting of styrene-butadiene diblock copolymer (SB), styrene-butadiene-styrene triblock copolymer (SBS), styrene-isoprene diblock copolymer (SI), styrene-isoprene-styrene triblock copolymer (SIS), styrene-(ethylene-butylene)-styrene triblock copolymer (SEBS), styrene-(ethylene-propylene)-styrene triblock copolymer (SEPS) and styrene-(ethylene-butylene) diblock copolymer (SEB). The method for manufacturing a laminate as described in claim 1, wherein the cycloolefin compound is at least one selected from the group consisting of dicyclopentadiene (DCPD) monomers, dicyclopentadiene polymers, norbornene monomers, and 5-norbornene polymers. The method for manufacturing a laminate as described in claim 1, wherein the vinylphenyl compound is diphenylethylene and/or bromostyrene. The method for manufacturing a laminate as described in claim 1, wherein the crosslinking agent is at least one selected from the group consisting of triallyl isocyanurate, triallyl cyanurate, dimaleimide resin and divinylbenzene. The manufacturing method of the laminate as described in claim 1, wherein the thermosetting resin composition further comprises: an accelerator, wherein the accelerator is selected from di-tert-butyl peroxide, dilauryl peroxide, dibenzoyl peroxide, tert-butyl peroxyacetate, tert-butyl peroxybenzoate, 1,1-di-tert-butyl peroxy-3,5,5-trimethylcyclohexane, 1,1-di-tert-butyl peroxycyclohexane, 2,2-di(tert-butyl peroxide) ) butane, bis(4-tert-butylcyclohexyl) peroxydicarbonate, hexadecyl peroxydicarbonate, tetradecyl peroxydicarbonate, dipentylhexyl peroxide, diisopropylbenzene peroxide, bis(tert-butylperoxyisopropyl)benzene, 2,5-dimethyl-2,5-di-tert-butylperoxyhexane, 2,5-dimethyl-2,5-di-tert-butylperoxyhexyne and diisopropylbenzene hydroperoxide. In the manufacturing method of the laminate as described in claim 1, the thermosetting resin composition further comprises: an inorganic filler, wherein the inorganic filler is at least one selected from the group consisting of silicon dioxide, aluminum oxide, aluminum hydroxide, magnesium oxide, magnesium hydroxide, calcium carbonate, aluminum nitride, boron nitride, aluminum silicon carbide, silicon carbide, titanium dioxide, zinc oxide, zirconium oxide, barium sulfate, magnesium carbonate, barium carbonate, mica, talc and graphene. A method for manufacturing a printed circuit board, comprising forming a printed circuit line layer from the metal foil layer of the laminate as described in claim 1 by etching or electroplating process.

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