Flame-retardant polyphenylene ether resin composition, copper clad plate and method for producing the same

Abstract

The application provides a flame-retardant polyphenyl ether resin composition, a copper-clad plate and a preparation method thereof. The flame-retardant polyphenyl ether resin composition comprises 100 parts of polyphenyl ether with unsaturated double bonds at the end, 10-30 parts of a polyolefin compound, 10-30 parts of a POSS compound and 5-20 parts of an initiator in terms of weight parts. The thermosetting polyphenyl ether is modified by using the POSS, so that the temperature resistance of the resin system is ensured, the flame-retardant requirement is reached, the material has good phosphorus-free and halogen-free flame-retardant performance and low thermal expansion rate. In addition, the amount of each component is controlled in the above range, which is also beneficial to improving the overall mechanical properties of the material. In addition, the dielectric constant of the POSS is low, and the influence on the excellent dielectric properties of the polyphenyl ether is small. The above reasons make the flame-retardant polyphenyl ether resin composition of the application very suitable for use in the field of high-frequency and high-speed printed circuit boards, and meet the green environmental protection requirements.

Description

Technical Field

[0001] This invention relates to the field of material modification technology, and more specifically, to a flame-retardant polyphenylene ether resin composition, copper-clad laminate, and a method for preparing the same. Background Technology

[0002] With the rapid development of modern electronics, information processing in electronic products such as mobile communications, servers, and cloud storage is constantly evolving towards higher frequency and higher speed digitalization, which continuously increases the performance requirements for copper clad laminates. The copper clad laminate substrate material is required to not only have good dielectric properties, but also high heat resistance, low coefficient of thermal expansion, and good processability. Therefore, developing a high-performance PCB-compatible material is a current research focus.

[0003] Thermosetting polyphenylene ether resins are preferred materials for high-performance circuit boards due to their excellent comprehensive properties, such as active end groups (e.g., active double bonds), low dielectric constant, and low dielectric loss. However, existing thermosetting polyphenylene ethers do not perform well in terms of flame retardancy and heat resistance. Therefore, flame retardants, such as phosphorus-containing or halogenated flame retardants, are added to the resin composition.

[0004] Patent CN107868188 A, entitled "Phosphorus-containing vinyl polyphenylene ether, resin composition containing the phosphorus-containing vinyl polyphenylene ether and its products," describes a process of reacting a phosphorus-containing vinyl compound with vinyl polyphenylene ether to obtain phosphorus-containing vinyl polyphenylene ether. The resulting resin products possess excellent properties such as low coefficient of thermal expansion, high heat resistance, high flame retardancy, low dielectric constant, and low dielectric loss. However, the use of phosphorus-containing and halogen-containing flame retardants is not environmentally friendly and can no longer meet the requirements for flame retardant modification.

[0005] Introducing silicon into resin compositions can improve their heat resistance and flame retardancy. For example, patent CN108250716A provides a polysiloxane-allyl compound modified polyphenylene ether resin composition and its prepreg, laminate, and printed circuit board. This composition exhibits low dielectric constant and low dielectric loss, excellent heat resistance and moisture absorption, and good flame retardant properties without the addition of additional flame retardants, achieving a halogen-free and phosphorus-free flame retardant effect. However, when this modified polyphenylene ether resin composition is applied to copper-clad laminates, its thermal expansion coefficient and other properties still do not meet requirements, and its tensile strength and other mechanical properties need further improvement.

[0006] Therefore, how to modify polyphenylene ether to meet the requirements of phosphorus-free and halogen-free flame retardancy, low thermal expansion rate, and high mechanical properties in the use of copper clad laminates is crucial. Summary of the Invention

[0007] The main objective of this invention is to provide a flame-retardant polyphenylene ether resin composition, copper-clad laminate, and its preparation method, so as to solve the problem that the modified polyphenylene ether used in copper-clad laminates in the prior art cannot simultaneously achieve properties such as phosphorus-free and halogen-free flame retardancy, low thermal expansion coefficient, and high mechanical properties.

[0008] To achieve the above objectives, according to one aspect of the present invention, a flame-retardant polyphenylene ether resin composition is provided, comprising, by weight, 100 parts of polyphenylene ether with unsaturated double bonds at the ends, 10 to 30 parts of a polyolefin compound, 10 to 30 parts of a POSS compound, and 5 to 20 parts of an initiator.

[0009] Furthermore, by weight, the flame-retardant polyphenylene ether resin composition also includes 4 to 7 parts of a crosslinking agent, 60 to 200 parts of a filler, and 100 to 200 parts of a solvent.

[0010] Furthermore, polyphenylene ethers with unsaturated double bonds at the ends have the structure shown in Formula I:

[0011]

[0012] In Formula I, Y is -CH2-, -CH(CH3)-, -C(CH3)2-, -O-, or carbonyl; m and n are independently selected from integers from 1 to 15; R1 to R 16 Each is independently selected from hydrogen, methyl, halogen atoms, C1 to C2 atoms. 10 Alkyl or C1-C 10 alkyl-substituted aryl groups; R0 is a group with an unsaturated double bond.

[0013] Furthermore, the number-average molecular weight of the polyphenylene ether with unsaturated double bonds at the ends is 500–10000 g / mol, preferably 1000–3500 g / mol.

[0014] Furthermore, the polyphenylene ether with unsaturated double bonds at the end is selected from one or more of methacrylate polyphenylene ether, divinyl benzyl polyphenylene ether resin, and vinyl benzyl etherified modified bisphenol A polyphenylene ether.

[0015] Further, the polyolefin compound is selected from polyethylene compounds, preferably from one or more of styrene-butadiene copolymers, polybutadiene, styrene, butadiene-styrene-divinylbenzene branched terpolymers, epoxidized polybutadiene, maleic anhydride-modified polybutadiene, methacrylated polybutadiene, maleic anhydride-modified polybutadiene-styrene copolymers, hydroxyl-terminated polybutadiene, and epoxidized hydroxyl-terminated polybutadiene; preferably, the POSS compound is selected from one or more of octavinyl POSS, propylene POSS, and methpropylene POSS. Preferably, the initiator is selected from organic peroxide initiators, and more preferably, the initiator is selected from one or more of the following: dicumyl peroxide, benzoyl peroxide, tert-butyl peroxyacetate, tert-butyl peroxyisobutyrate, tert-butyl peroxy-3,5,5-trimethylhexanoate, cumyl peroxyneodecanate, tert-butyl peroxyneodecanate, tert-pentyl peroxypentate, tert-butyl peroxybenzoate, 2,5-di(2-ethylhexanoylperoxy)-2,5-dimethylhexane, tert-butyl hydroperoxide, tert-butyl peroxide, dicumyl peroxide, peroxycarbonate, and tert-butyl 2-ethylhexanoate.

[0016] Further, the crosslinking agent is selected from one or more of aminotriazine phenolic resin, melamine cyanurate, and tri-hydroxyethyl isocyanate; preferably, the filler is selected from one or more of crystalline silica, amorphous silica, hollow silica, glass powder, aluminum nitride, boron nitride, silicon carbide, aluminum hydroxide, magnesium hydroxide, strontium titanate, barium titanate, zinc oxide, zirconium oxide, aluminum oxide, barium sulfate, calcium titanate, calcium silicate, spherical silica, polyethersulfone, polytetrafluoroethylene powder, polyimide, polyethersulfone, and titanium dioxide; preferably, the solvent includes one or more of methanol, ethanol, toluene, xylene, acetone, methyl ethyl ketone, methyl isobutyl ketone, cyclohexanone, ethyl acetate, N,N-dimethylformamide, and propylene glycol methyl ether.

[0017] Further, by weight, the flame-retardant polyphenylene ether resin composition comprises 100 parts of polyphenylene ether with unsaturated double bonds at the end, 10 to 30 parts of polyolefin compound, 20 to 25 parts of POSS compound, 12 to 18 parts of initiator, 5 to 7 parts of co-crosslinking agent, 70 to 100 parts of filler and 140 to 180 parts of solvent.

[0018] According to another aspect of the present invention, a copper-clad laminate is also provided, comprising a copper foil and a resin fiber cloth located on the copper foil, the resin fiber cloth comprising a resin base layer and a fiber cloth located in the resin base layer, wherein the resin base layer is formed by impregnation and curing of the above-mentioned flame-retardant polyphenylene ether resin composition.

[0019] According to another aspect of the present invention, a method for preparing the above-mentioned copper-clad laminate is also provided, which includes the following steps: impregnating a fiber cloth in the above-mentioned flame-retardant polyphenylene ether resin composition, removing it, and baking it to obtain a prepreg; placing the prepreg between two layers of copper foil, and hot-pressing to cure it to obtain a copper-clad laminate.

[0020] This invention provides a flame-retardant polyphenylene ether resin composition, comprising, by weight, 100 parts of polyphenylene ether with terminal unsaturated double bonds, 10-30 parts of a polyolefin compound, 10-30 parts of a POSS compound, and 5-20 parts of an initiator. POSS is an organic-inorganic nano-hybrid material with a unique cage-like structure. Its incorporation into the polyphenylene ether resin composition promotes excellent thermal and flame-retardant properties in the final resin material. Therefore, modifying thermosetting polyphenylene ether with POSS ensures both the temperature resistance of the resin system and meets flame-retardant requirements, resulting in a material with both excellent phosphorus-free and halogen-free flame-retardant properties and a low thermal expansion coefficient. Controlling the amounts of each component within the aforementioned range also helps improve the overall mechanical properties of the material. Furthermore, the low dielectric constant of POSS has minimal impact on the excellent dielectric properties of polyphenylene ether. These factors make the flame-retardant polyphenylene ether resin composition of this invention highly suitable for use in the field of high-frequency, high-speed printed circuit boards, and it also meets green and environmentally friendly requirements. Detailed Implementation

[0021] It should be noted that, unless otherwise specified, the embodiments and features described in this application can be combined with each other. The present invention will now be described in detail with reference to the embodiments.

[0022] As described in the background section, the modified polyphenylene ether used in existing copper-clad laminates has the problem of not being able to simultaneously achieve properties such as phosphorus-free and halogen-free flame retardancy, low thermal expansion coefficient, and high mechanical properties.

[0023] To address the aforementioned problems, the present invention provides a flame-retardant polyphenylene ether resin composition, comprising, by weight, 100 parts of polyphenylene ether with unsaturated double bonds at the ends, 10-30 parts of a polyolefin compound, 10-30 parts of a POSS compound, and 5-20 parts of an initiator.

[0024] Polyhedral oligomeric semisiloxanes (POSS) are organic-inorganic nanocomposite materials with a unique cage-like structure. When incorporated into polyphenylene ether resin compositions, they can participate in the crosslinking reaction of thermosetting polyphenylene ethers, improve the compatibility between different components in the resin system, and increase the amount of inorganic filler added, resulting in a final resin material with excellent thermal and flame-retardant properties. Therefore, using POSS to modify thermosetting polyphenylene ethers ensures both the temperature resistance of the resin system and meets flame-retardant requirements, giving it excellent phosphorus-free and halogen-free flame-retardant properties and a low thermal expansion coefficient. Controlling the dosage of each component within the aforementioned range also helps improve the overall mechanical properties of the material. Furthermore, the low dielectric constant of POSS has minimal impact on the excellent dielectric properties of polyphenylene ether. These factors make the flame-retardant polyphenylene ether resin composition of this invention highly suitable for use in the field of high-frequency, high-speed printed circuit boards, and it also meets green and environmentally friendly requirements.

[0025] To further improve the various properties of the polyphenylene ether resin system and to give it a suitable viscosity for impregnation in the subsequent copper clad laminate manufacturing process, in a preferred embodiment, the flame-retardant polyphenylene ether resin composition further includes 4 to 7 parts by weight of a crosslinking agent, 60 to 200 parts by weight of a filler and 100 to 200 parts by weight of a solvent.

[0026] In a preferred embodiment, the polyphenylene ether with unsaturated double bonds at the ends has the structure shown in Formula I:

[0027]

[0028] In Formula I, Y is -CH2-, -CH(CH3)-, -C(CH3)2-, -O-, or carbonyl; m and n are independently selected from integers from 1 to 15; R1 to R 16 Each is independently selected from hydrogen, methyl, halogen atoms, C1 to C2 atoms. 10 alkyl or substituted aryl groups; R0 is a group with an unsaturated double bond.

[0029] The polyphenylene ether with the above-described structure exhibits better dielectric properties, and after POSS modification, it demonstrates superior performance in flame retardancy, heat resistance, low thermal expansion coefficient, and mechanical properties. More preferably, the polyphenylene ether with terminal unsaturated double bonds has a number-average molecular weight of 500–10000 g / mol, more preferably 1000–3500 g / mol. At this molecular weight, the composition viscosity is more suitable, facilitating impregnation during subsequent copper-clad laminate fabrication.

[0030] In a preferred embodiment, the polyphenylene ether with unsaturated double bonds at the ends includes, but is not limited to, one or more selected from methacrylate polyphenylene ether, divinyl benzyl polyphenylene ether resin, and vinyl benzyl etherified modified bisphenol A polyphenylene ether. Specifically, methacrylate polyphenylene ether can be SA 9000 (Sabic), methyl methacrylate modified polyphenylene ether MX9000 (Sabic), divinyl benzyl polyphenylene ether resin can be OPE-2st (Mitsubishi Gas Chemical), and vinyl benzyl etherified modified bisphenol A polyphenylene ether can be styrene-modified polyphenylene ether St-PPE-1 (Mitsubishi Gas Chemical) or allyl-modified polyphenylene ether resin PP-501 (Taiwan Jin Yi Chemical). Using the above-mentioned types of polyphenylene ethers is more beneficial to improving the overall performance of the resin composition.

[0031] The aforementioned polyolefin compounds function as rubber co-adhesives or toughening agents to increase the crosslinking density of the resin system, resulting in better toughness and lower dielectric properties in the cured resin. In a preferred embodiment, the polyolefin compound is selected from polyethylene compounds, and more preferably from one or more of the following: styrene-butadiene copolymer, polybutadiene, styrene, butadiene-styrene-divinylbenzene branched terpolymer, epoxidized polybutadiene, maleic anhydride-modified polybutadiene, methacrylated polybutadiene, maleic anhydride-modified polybutadiene-styrene copolymer, hydroxyl-terminated polybutadiene, and epoxidized hydroxyl-terminated polybutadiene. Using the above-mentioned types of polyolefin compounds provides a more significant improvement in the toughness of the resin system while maintaining lower dielectric properties.

[0032] POSS is a class of substances containing a mixed inorganic-organic structure. The inorganic framework is composed of Si-O-Si bonds, with the chemical formula [RSiO1.5]n. POSS structures include amorphous, trapezoidal, cage-like, semi-cage-like, and bipyramidal types. The inorganic framework structure endows it with superior heat resistance, flame retardancy, and radiation resistance, while the organic groups ensure excellent compatibility with organic polymer systems. To further leverage these advantages, preferably, the POSS compound is selected from one or more of octavinyl POSS, allyl POSS, and methacryl POSS. These types of POSS have a better modification effect on polyphenylene ether resin compositions, resulting in superior comprehensive properties such as heat resistance, flame retardancy, electrical insulation, weather resistance, and low thermal expansion coefficient after curing.

[0033] Preferably, the initiator is selected from organic peroxide initiators, and more preferably, the initiator is selected from one or more of the following: dicumyl peroxide, benzoyl peroxide, tert-butyl peroxyacetate, tert-butyl peroxyisobutyrate, tert-butyl peroxy-3,5,5-trimethylhexanoate, cumyl peroxyneodecanate, tert-butyl peroxyneodecanate, tert-pentyl peroxypentate, tert-butyl peroxybenzoate, 2,5-di(2-ethylhexanoylperoxy)-2,5-dimethylhexane, tert-butyl hydroperoxide, tert-butyl peroxide, dicumyl peroxide, peroxycarbonate, and tert-butyl 2-ethylhexanoate. The above initiators have better initiation efficiency, allowing for more complete cross-linking and curing of the composition during the preparation of the copper-clad laminate using a hot-pressing process.

[0034] To further improve the crosslinking speed, adjust the crosslinking density, and give the cured resin better mechanical properties, in a preferred embodiment, the co-crosslinking agent is selected from one or more of aminotriazine phenolic resin, melamine cyanuric acid value, and tri-hydroxyethyl isocyanate; preferably, the filler is selected from one or more of crystalline silica, amorphous silica, hollow silica, glass powder, aluminum nitride, boron nitride, silicon carbide, aluminum hydroxide, magnesium hydroxide, strontium titanate, barium titanate, zinc oxide, zirconium oxide, aluminum oxide, barium sulfate, calcium titanate, calcium silicate, spherical silica, polyethersulfone, polytetrafluoroethylene powder, polyimide, polyethersulfone, and titanium dioxide.

[0035] Preferably, the solvent includes one or more of methanol, ethanol, toluene, xylene, acetone, butanone, methyl isobutyl ketone, cyclohexanone, ethyl acetate, N,N-dimethylformamide, and propylene glycol methyl ether. Using these solvents allows the numerical composition to form a more suitable and uniform adhesive system, facilitating subsequent impregnation.

[0036] To further improve the overall performance of the resin composition after curing, in a preferred embodiment, the flame-retardant polyphenylene ether resin composition comprises, by weight, 100 parts of polyphenylene ether with unsaturated double bonds at the end, 10-30 parts of polyolefin compound, 20-25 parts of POSS compound, 12-18 parts of initiator, 5-7 parts of co-crosslinking agent, 70-100 parts of filler, and 140-180 parts of solvent.

[0037] According to another aspect of the present invention, a copper-clad laminate is also provided, comprising a copper foil and a resin fiber cloth located on the copper foil. The resin fiber cloth comprises a resin base layer and a fiber cloth located within the resin base layer, wherein the resin base layer is formed by impregnation and curing of the aforementioned flame-retardant polyphenylene ether resin composition. The use of POSS to modify thermosetting polyphenylene ether ensures both the temperature resistance of the resin system and meets flame-retardant requirements, giving it both excellent phosphorus-free and halogen-free flame-retardant properties and a low thermal expansion coefficient. Furthermore, controlling the dosage of each component within the aforementioned range also helps improve the overall mechanical properties of the material. In addition, the low dielectric constant of POSS has minimal impact on the excellent dielectric properties of polyphenylene ether. For these reasons, the flame-retardant polyphenylene ether resin composition of the present invention is very suitable for use in the field of high-frequency and high-speed printed circuit boards and meets green environmental protection requirements.

[0038] The fiber cloth mentioned above can be of a type commonly used in the art, with electronic glass fiber cloth being preferred to better meet the requirements of copper clad laminates.

[0039] In addition, the present invention also provides a method for preparing the above-mentioned copper-clad laminate, which includes the following steps: impregnating a fiber cloth in the above-mentioned flame-retardant polyphenylene ether resin composition, taking it out, and baking it to obtain a prepreg; placing the prepreg between two layers of copper foil, and hot-pressing to cure it to obtain a copper-clad laminate.

[0040] Specifically, the copper-clad laminate is preferably prepared using the above method: a flame-retardant polyphenylene ether resin composition is adjusted into an adhesive solution, which is then impregnated onto electronic glass fiber cloth and baked to obtain a prepreg. The prepregs are then stacked together, coated with copper foil on both sides, and hot-pressed under specific temperature and pressure to obtain the copper-clad laminate. Here, "prepreg" refers to a state where most of the solvent in the flame-retardant polyphenylene ether resin composition has evaporated, leaving it in a state where it can adhere to the fiber cloth but is not cross-linked.

[0041] The present application will be further described in detail below with reference to specific embodiments, which should not be construed as limiting the scope of protection claimed in the present application.

[0042] Example

[0043] Flame-retardant polyphenylene ether resin compositions with different components and ratios are provided, and the specific formulations are shown in Table 1:

[0044] Table 1

[0045]

[0046]

[0047] The prepreg is cut to the required size, stacked, and cured using a vacuum press to obtain a substrate for PCB.

[0048] The physical properties of the substrates used in the examples and comparative examples were measured:

[0049] Tensile strength: tested according to D638 standard;

[0050] Thermal expansion effect: CTE z-axis, dimensional expansion and contraction rate measurement range: 50 to 260℃, measured by TMA instrument, the lower the dimensional expansion and contraction rate (%), the better;

[0051] Heat resistance: T288, measured by TMA thermomechanical analysis instrument: the time it takes for a copper foil plate to not explode when heated to 288 degrees Celsius;

[0052] Peel strength test: Tested according to IPC-TM-650 2.4.8;

[0053] Glass transition temperature testing: 40-280℃, thermomechanical analysis instrument;

[0054] Dielectric constant: Dk, measured by AET microwave electrochemical analyzer. The lower the Dk value, the better the dielectric properties.

[0055] Dielectric loss: Df, measured by AET microwave electrochemical analyzer. The lower the Df value, the better the dielectric properties.

[0056] Flame retardancy: UL94, with V-0 being better than V-1 in the rating ranking.

[0057] Note: Except for the tests of dielectric constant, dielectric loss and mechanical properties (tensile strength and peel strength) which use a substrate without copper foil, all other tests require copper foil to be laid on the substrate using conventional methods.

[0058] The performance test results are shown in Table 2 below:

[0059] Table 2-1

[0060]

[0061] Table 2-2

[0062]

[0063]

[0064] The above description is merely a preferred embodiment of the present invention and is not intended to limit the invention. Various modifications and variations can be made to the present invention by those skilled in the art. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the scope of protection of the present invention.

Claims

1. A flame-retardant polyphenylene ether resin composition, characterized in that, By weight, the flame-retardant polyphenylene ether resin composition comprises 100 parts of polyphenylene ether with unsaturated double bonds at the end, 10-30 parts of polyolefin compound, 10-30 parts of POSS compound and 5-20 parts of initiator. The flame-retardant polyphenylene ether resin composition further comprises 4 to 7 parts by weight of a crosslinking agent, 60 to 200 parts by weight of a filler and 100 to 200 parts by weight of a solvent. The polyolefin compound is selected from one or more of styrene-butadiene copolymer, polybutadiene, butadiene-styrene-divinylbenzene branched terpolymer, epoxidized polybutadiene, maleic anhydride-modified polybutadiene, methacrylated polybutadiene, maleic anhydride-modified polybutadiene-styrene copolymer, hydroxyl-terminated polybutadiene, and epoxidized hydroxyl-terminated polybutadiene; the POSS compound is selected from one or more of octavinyl POSS, propylene POSS, and methpropylene POSS; the filler is selected from one or more of crystalline silica, amorphous silica, and spherical silica; and the co-crosslinking agent is triallyl isocyanurate (TAIC).

2. The flame-retardant polyphenylene ether resin composition according to claim 1, characterized in that, The polyphenylene ether with unsaturated double bonds at the ends has the structure shown in Formula I: Formula I In Formula I, Y is -CH2-, -CH(CH3)-, -C(CH3)2-, -O-, or a carbonyl group; m and n are each independently selected from integers from 1 to 15; R1 to R 16 Each is independently selected from hydrogen, methyl, halogen atoms, C1~C 10 Alkyl or C1~C 10 alkyl-substituted aryl groups; R0 is a group with an unsaturated double bond.

3. The flame-retardant polyphenylene ether resin composition according to claim 2, characterized in that, The polyphenylene ether with unsaturated double bonds at the ends has a number average molecular weight of 500~10000 g / mol.

4. The flame-retardant polyphenylene ether resin composition according to claim 2, characterized in that, The polyphenylene ether with unsaturated double bonds at the ends has a number average molecular weight of 1000~3500 g / mol.

5. The flame-retardant polyphenylene ether resin composition according to claim 2, characterized in that, The polyphenylene ether with unsaturated double bonds at the end is selected from one or more of methacrylate polyphenylene ether, divinyl benzyl polyphenylene ether resin, and vinyl benzyl etherified modified bisphenol A polyphenylene ether.

6. The flame-retardant polyphenylene ether resin composition according to claim 1, characterized in that, The initiator is selected from organic peroxide initiators.

7. The flame-retardant polyphenylene ether resin composition according to claim 6, characterized in that, The initiator is selected from one or more of the following: dicumyl peroxide, benzoyl peroxide, tert-butyl peroxyacetate, tert-butyl peroxyisobutyrate, tert-butyl peroxy-3,5,5-trimethylhexanoate, cumyl peroxyneodecanate, tert-butyl peroxyneodecanate, tert-pentyl peroxypentate, tert-butyl peroxybenzoate, 2,5-bis(2-ethylhexanoylperoxy)-2,5-dimethylhexane, tert-butyl hydroperoxide, tert-butyl peroxide, dicumyl peroxide, and peroxycarbonate.

8. The flame-retardant polyphenylene ether resin composition according to claim 1, characterized in that, The solvent includes one or more of methanol, ethanol, toluene, xylene, acetone, butanone, methyl isobutyl ketone, cyclohexanone, ethyl acetate, N,N-dimethylformamide, and propylene glycol methyl ether.

9. The flame-retardant polyphenylene ether resin composition according to claim 1, characterized in that, By weight, the flame-retardant polyphenylene ether resin composition comprises 100 parts of the polyphenylene ether with unsaturated double bonds at the ends, 10-30 parts of the polyolefin compound, 20-25 parts of the POSS compound, 12-18 parts of an initiator, 5-7 parts of a co-crosslinking agent, 70-100 parts of a filler, and 140-180 parts of a solvent.

10. A copper-clad laminate, characterized in that, The copper-clad laminate includes a copper foil and a resin fiber cloth on the copper foil. The resin fiber cloth includes a resin base layer and a fiber cloth located in the resin base layer, wherein the resin base layer is formed by impregnation and curing of the flame-retardant polyphenylene ether resin composition according to any one of claims 1 to 9.

11. A method for preparing the copper-clad laminate according to claim 10, characterized in that, The preparation method includes the following steps: The fiber cloth is impregnated in the flame-retardant polyphenylene ether resin composition according to any one of claims 1 to 9, and after being removed, it is baked to obtain a semi-cured sheet; The prepreg is placed between two layers of copper foil and then hot-pressed to cure, thus obtaining the copper-clad laminate.

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