Heat-conducting polyphenyl ether composite material and preparation method thereof

Abstract

The invention discloses a heat-conducting polyphenyl ether composite material and a preparation method thereof, and relates to the technical field of polymer composite material processing. The preparation method of the heat-conducting polyphenyl ether composite material comprises the following steps: S1, preparation of an azobenzene group blend: mixing functionalized UHMWPE (Ultra High Molecular Weight Polyethylene), functionalized polystyrene and an antioxidant to obtain the azobenzene group blend; and S2, preparation of the heat-conducting polyphenyl ether composite material: uniformly mixing PPO and the azobenzene group blend prepared in the step S1 to obtain the heat-conducting polyphenyl ether composite material. According to the heat-conducting polyphenyl ether composite material and the preparation method thereof disclosed by the invention, an azobenzene unit and an acrylate unit are respectively introduced into a polystyrene chain and an ultra-high molecular weight polyethylene chain through free radical copolymerization and reactive melting processing, and are further compounded with polyphenyl ether resin, so that a composite system is constructed, and strong interface interaction among the components is realized; the high strength and toughness of ultrahigh molecular weight polyethylene are exerted, and the impact resistance of the composite material is improved.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of polymer composite material processing, and particularly relates to a heat-conducting polyphenyl ether composite material and a preparation method thereof. BACKGROUND

[0002] With the rapid development of modern industry and information technology, especially the rapid rise of 5G communication, new energy vehicles and high-end electronic equipment, the demand for high-performance heat-conductive materials has surged, and the requirements for the comprehensive performance of the materials have become increasingly stringent. Traditional heat-conductive materials such as metals and ceramics have excellent heat-conductive performance, but they still face problems such as high processing cost and complex forming process in practical applications. Polymer-based heat-conductive composite materials have become a research hotspot in the field of material science due to their easy processing, light weight, corrosion resistance, low cost and other advantages. As one of the five engineering plastics, polyphenyl ether (PPO) has good dielectric properties, high heat resistance, good mechanical properties and temperature dimensional properties, and is widely used in electronic packaging, electronic device / battery heat dissipation, printed circuit boards and mobile communication technologies.

[0003] There are few reports on PPO-based heat-conductive composite materials: Chinese patent CN202411215279.5 uses boron nitride and basalt fiber to modify PPO resin, and improves the interaction between PPO and fillers through a compatibilizer, so as to prepare a PPO composite material with good heat-conductive performance, dielectric properties and thermal stability; Chinese patent CN202210730051.4 introduces aluminum nitride, graphite and other heat-conductive fillers into the PPO system, and the thermal conductivity of the PPO composite material is increased to 4.2 W / m·K; Chinese patent CN202210625214.2 uses boron nitride / silicon carbide and flaky graphite powder to optimize the heat-conductive performance of PPO, and the thermal conductivity of the prepared composite material can reach 1.3 W / m·K. In summary, at present, the fillers used to improve the heat-conductive performance of PPO resin are mainly inorganic fillers such as aluminum nitride, graphite, boron nitride and silicon carbide. Such fillers lack interaction between the PPO matrix, are prone to interface debonding, and lead to deterioration of other properties of the composite material, thereby limiting the practical application thereof. SUMMARY

[0004] To solve the above technical problems, the purpose of the present application is to provide a heat-conducting polyphenyl ether composite material and a preparation method thereof, which has the characteristics that azobenzene groups and acrylate units are introduced into the polyphenyl ether resin by free radical copolymerization and reactive melt processing, and the composite system is further compounded with polyphenyl ether resin to build strong interfacial interaction between the components of the composite system, play the high toughness of the ultra-high molecular weight polyethylene, and improve the impact resistance of the composite material; the azobenzene groups are fixed in the composite system by using the high molecular entanglement structure of the ultra-high molecular weight polyethylene, so that they are enriched in the entanglement structure area, and then the azobenzene groups are self-assembled to form highly oriented crystalline microzones through π-π stacking, which significantly improves the phonon coupling and transmission efficiency, increases the average free path of phonons, and establishes an efficient heat transfer network, giving the polyphenyl ether good thermal conductivity.

[0005] Specifically, the technical solutions include the following: In a first aspect, a preparation method of a heat-conducting polyphenyl ether composite material is provided, comprising the following steps: S1. Preparation of azobenzene group blend: (1) mixing ultra-high molecular weight polyethylene (UHMWPE), ultraviolet light initiator, reactive monomer 1 and solvent 1 uniformly, treating with ultraviolet light, and then cleaning with N,N-dimethylformamide and deionized water to obtain functionalized UHMWPE; (2) dissolving styrene and reactive monomer 2 in solvent 2, adding a free radical copolymerization initiator to react, obtaining a reaction solution, and finally adding methanol to the reaction solution to obtain functionalized polystyrene; (3) mixing the functionalized UHMWPE, the functionalized polystyrene and the antioxidant to obtain the azobenzene group blend; S2. Preparation of the heat-conducting polyphenyl ether composite material: mixing PPO and the azobenzene group blend prepared in step S1 uniformly to obtain the heat-conducting polyphenyl ether composite material.

[0006] Further, in step S1, the average entanglement molar mass of the ultra-high molecular weight polyethylene is 300-1000 g / mol; the ultraviolet light initiator is selected from one of 2-hydroxy-2-methyl-1-phenyl-1-propanone, 1-hydroxycyclohexyl phenyl ketone, 2-hydroxy-4'-(2-hydroxyethoxy)-2-methylpropiophenone, benzophenone, 2,4,6-trimethylbenzoyl-diphenyl phosphine oxide, bis(2,4,6-trimethylbenzoyl) phenyl phosphine oxide, and isopropyl thioxanthone.

[0007] Further, in step S1, the reactive monomer 1 is selected from one of hydroxyethyl methacrylate, isobutyl methacrylate, n-butyl methacrylate, ethyl methacrylate, methyl methacrylate, glycidyl methacrylate, ethylene glycol dimethacrylate, triethylene glycol dimethacrylate, allyl methacrylate, dimethylaminoethyl methacrylate, and siloxane methacrylate; and the solvent 1 is selected from one of dimethyl sulfoxide, dimethylbenzene, isopropyl alcohol, n-butyl alcohol, ethyl acetate, butyl acetate, N,N-dimethylformamide, methyl ethyl ketone, and cyclohexanone.

[0008] Further, in step S1, the reactive monomer 2 is selected from one of amino-4'- methacrylate azobenzene, 4-methacryloyloxy-4'-methoxyazobenzene, 4,4'-bis(methacryloyloxy)azobenzene, (1-4'-butylazophenoxy-6-hexanol) methacrylate, 11-[4-(4-butylphenylazo)phenoxy]undecyl methacrylate, 4-methacryloyloxyazobenzene, bis-methacrylate azobenzene, and 4,4'-di(6''-acryloyloxyhexyloxy)azobenzene; and the solvent 2 is selected from one of n-hexane, cyclohexane, toluene, xylene, dichloromethane, chloroform, carbon tetrachloride, diethyl ether, tetrahydrofuran, isopropyl alcohol, and n-butyl alcohol.

[0009] Further, in step S1, the free radical copolymerization initiator is selected from one of azobisisobutyronitrile, benzoyl peroxide, dicumyl peroxide, peroxide dicarbonate, and azobisisoheptyl nitrile; and the antioxidant is selected from one of tetrakis[β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionic acid]pentaerythritol ester, β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionic acid octadecyl ester, 2,6-di-tert-butyl-p-cresol, tris(2,4-di-tert-butylphenyl)phosphite, bis(2,4-di-tert-butylphenyl)pentaerythritol diphosphite, dilauryl thiodipropionate, and N-isopropyl-N'-phenyl-p-phenylenediamine.

[0010] Further, in step S1, the functionalized UHMWPE is prepared by mixing 100 parts of ultra-high molecular weight polyethylene, 0.5-10 parts of an ultraviolet light initiator, 1-30 parts of the reactive monomer 1, and 100-300 parts of the solvent 1 at 50-70°C, stirring and mixing uniformly, treating under a nitrogen atmosphere for 20-60 min using an ultraviolet lamp with a power of 500-5000 W, and then cleaning with N,N-dimethylformamide and deionized water, and drying at 110°C for 3 hours under vacuum.

[0011] Further, in step S1, the functionalized polystyrene is prepared by dissolving 100 parts of styrene, 40-100 parts of reactive monomer 2 in 100-200 parts of solvent 2, adding 0.5-10 parts of free radical copolymerization initiator, and reacting at 80°C for 12 hours under a nitrogen atmosphere to obtain a reaction solution, and finally adding 5-20 parts of methanol dropwise to the reaction solution to precipitate, filter, and dry at 90°C under vacuum for 4 hours.

[0012] Further, in step S1, the azobenzene unit blend is prepared by adding 5-30 parts of functionalized UHMWPE, 70-95 parts of functionalized polystyrene, and 0.5-5 parts of antioxidant to a Banbury mixer, mixing at 200-230°C for 20-60 minutes, and then obtaining the azobenzene unit blend.

[0013] Further, in step S2, the heat-conducting polyphenyl ether composite material is prepared by uniformly mixing 100 parts of PPO and 20-60 parts of the azobenzene unit blend prepared in step S1, and then passing through a twin-screw extruder at an extrusion temperature of 250-310°C and a screw rotation speed of 150-200 rpm.

[0014] In a second aspect, a heat-conducting polyphenyl ether composite material is provided, which is prepared by the method for preparing a heat-conducting polyphenyl ether composite material according to the first aspect.

[0015] Preferably, the heat-conducting polyphenyl ether composite material has a thermal conductivity of 1.81 W / m·K and a notched Charpy impact strength of 14.45 kJ / m 2 .

[0016] The present application provides a heat-conducting polyphenyl ether composite material and a method for preparing the same, which has the following beneficial effects: (1) Unlike the traditional method of introducing inorganic heat-conducting fillers to improve the heat-conducting performance of polyphenyl ether, the azobenzene liquid crystal unit is chemically bonded into the composite system in the present application, and the highly entangled structure of the ultra-high molecular weight polyethylene is used as a physical crosslinking point to enrich and fix the azobenzene liquid crystal unit in the entangled network, thereby promoting the azobenzene unit to form highly oriented crystalline microzones through π-π stacking self-assembly, significantly improving the phonon coupling and transmission efficiency, establishing a high-efficiency heat transfer network, and endowing the polyphenyl ether with good heat-conducting performance.

[0017] (2) The azobenzene unit and the acrylate unit are introduced into the polystyrene and the ultra-high molecular weight polyethylene chains, respectively, through free radical copolymerization and reactive melt processing, and are further compounded with the polyphenyl ether resin, thereby constructing strong interfacial interactions between the components of the composite system, effectively exerting the high strength and toughness of the UHMWPE, and obtaining a polyphenyl ether composite material with good impact strength. DETAILED DESCRIPTION

[0018] The technical solutions in the embodiments of the present application will be clearly and completely described below. Obviously, the described embodiments are only some of the embodiments of the present application but not all the embodiments. Based on the embodiments in the present application, all other embodiments obtained by those skilled in the art without creative efforts should fall into the scope of the present application.

[0019] It should be understood that the terms "comprise" and "include" as used in the specification and the appended claims indicate the presence of the described features, integers, steps, operations, elements, and / or components but do not preclude the presence or addition of one or more other features, integers, steps, operations, elements, components, and / or groups thereof.

[0020] It should also be understood that the terms used in the present application specification are only for the purpose of describing specific embodiments and are not intended to limit the present application. As used in the present application specification and the appended claims, the singular forms "a", "an" and "the" are intended to include the plural forms unless the context clearly indicates otherwise.

[0021] It should be further understood that the term "and / or" as used in the present application specification and the appended claims means any combination of one or more of the associated listed items and all possible combinations, and includes these combinations.

[0022] In order to more fully understand the technical content of the present application, the technical solutions of the present application will be further introduced and described below in combination with specific embodiments.

[0023] The object of the present application is achieved by the following technical measures, wherein the parts of raw materials are parts by weight unless otherwise specified.

[0024] Embodiment 1 A heat-conducting polyphenyl ether composite material is prepared by the method for preparing the heat-conducting polyphenyl ether composite material.

[0025] The method for preparing the heat-conducting polyphenyl ether composite material comprises the following steps: S1. Preparation of azobenzene unit blend: (1) 100 parts of ultra-high molecular weight polyethylene (UHMWPE, average entanglement molar mass of 1000 g / mol), 2.5 parts of UV initiator (2-hydroxy-2-methyl-1-phenyl-1-propanone), 10 parts of reactive monomer 1 (methyl methacrylate) and 100 parts of solvent 1 (dimethyl sulfoxide) are mixed uniformly at 50°C by stirring, treated with a UV lamp for 20 min under a nitrogen atmosphere, the power of the UV lamp is 5000 W, then washed with N,N-dimethylformamide and deionized water, and dried in a vacuum at 110°C for 3 hours to obtain a functionalized UHMWPE; (2) 100 parts of styrene, 40 parts of reactive monomer 2 are dissolved in 100 parts of solvent 2 (isopropyl alcohol), 2 parts of free radical copolymerization initiator (azobisisobutyronitrile) is added, and the reaction liquid is prepared by reacting at 80°C for 12 hours under a nitrogen atmosphere, and finally 5-20 parts of methanol is added dropwise for precipitation, filtration, and vacuum drying at 90°C for 4 hours to obtain a functionalized polystyrene; the reactive monomer 2 is (1-4'-butylazobenzeneoxy-6-hexanol) methacrylic acid; (3) 30 parts of functionalized UHMWPE, 70 parts of functionalized polystyrene and 0.5 parts of antioxidant (tetra[β-(3,5-di-tert-butyl-4-hydroxyphenyl) propionic acid] pentaerythritol ester) are added to a banbury mixer, mixed at 200°C for 60 min to obtain an azobenzene unit blend; S2. Preparation of thermally conductive polyphenylene ether composite material: 100 parts of PPO and 20 parts of the azobenzene unit blend prepared in step S1 are uniformly mixed, and a thermally conductive polyphenylene ether composite material is prepared by a twin-screw extruder at an extrusion temperature of 250°C and a screw rotation speed of 150 rpm.

[0026] Example 2 A thermally conductive polyphenylene ether composite material is prepared by the method for preparing a thermally conductive polyphenylene ether composite material.

[0027] The method for preparing a thermally conductive polyphenylene ether composite material comprises the following steps: S1. Preparation of azobenzene moiety blend: (1) 100 parts of ultra-high molecular weight polyethylene (UHMWPE, average entanglement molar mass of 700 g / mol), 5 parts of UV initiator, 20 parts of reactive monomer 1 (ethylene glycol dimethacrylate) and 200 parts of solvent 1 (N,N-dimethylformamide) were mixed uniformly at 60°C, treated with a UV lamp under a nitrogen atmosphere for 40 min, the power of the UV lamp was 2500 W, then washed with N,N-dimethylformamide and deionized water, and dried in a vacuum at 110°C for 3 hours to obtain functionalized UHMWPE; the UV initiator was 2-hydroxy-4'-(2-hydroxyethoxy)-2-methylpropiophenone; (2) 100 parts of styrene and 70 parts of reactive monomer 2 (4-methacryloyloxy-4'-methoxyazobenzene) were dissolved in 150 parts of solvent 2 (dichloromethane), 4 parts of free radical copolymerization initiator (benzoyl peroxide) was added, and the reaction was carried out at 80°C for 12 hours under a nitrogen atmosphere to obtain a reaction solution, then 10 parts of methanol was added dropwise to the reaction solution for precipitation, filtration and vacuum drying at 90°C for 4 hours to obtain functionalized polystyrene; (3) 15 parts of functionalized UHMWPE, 85 parts of functionalized polystyrene and 2 parts of antioxidant were added to a banbury mixer, mixed at 210°C for 30 min to obtain an azobenzene moiety blend; the antioxidant was β-(3,5-di-tert-butyl-4-hydroxyphenyl) octadecyl propionate; S2. Preparation of thermally conductive polyphenylene ether composite material: 100 parts of PPO and 40 parts of the azobenzene moiety blend prepared in step S1 were uniformly mixed, and a thermally conductive polyphenylene ether composite material was prepared by a twin-screw extruder at an extrusion temperature of 250°C and a screw rotation speed of 150 rpm.

[0028] Example 3 A thermally conductive polyphenylene ether composite material is prepared by the method for preparing a thermally conductive polyphenylene ether composite material.

[0029] The method for preparing a thermally conductive polyphenylene ether composite material comprises the following steps: S1. Preparation of azobenzene moiety blend: (1) 100 parts of ultra-high molecular weight polyethylene (UHMWPE, average entanglement molecular weight of 300 g / mol), 8 parts of UV initiator (2,4,6-trimethylbenzoyl-diphenyl phosphine oxide), 30 parts of reactive monomer 1 (triethylene glycol dimethacrylate) and 300 parts of solvent 1 (ethyl acetate) were mixed uniformly at 70°C, treated with a UV lamp under a nitrogen atmosphere for 60 min, the power of the UV lamp was 1000 W, then cleaned with N,N-dimethylformamide and deionized water, and dried in a vacuum at 110°C for 3 hours to obtain functionalized UHMWPE; (2) 100 parts of styrene and 100 parts of reactive monomer 2 were dissolved in 200 parts of solvent 2 (xylene), 8 parts of free radical copolymerization initiator (dicumyl peroxide) was added, and the reaction liquid was prepared by reacting at 80°C for 12 hours under a nitrogen atmosphere, and finally 20 parts of methanol was added dropwise for precipitation, filtration, and vacuum drying at 90°C for 4 hours to obtain functionalized polystyrene; the reactive monomer 2 is 11-[4-(4-butyl phenylazo) phenoxy] undecyl methacrylate; (3) 10 parts of functionalized UHMWPE, 90 parts of functionalized polystyrene and 5 parts of antioxidant were added to a banbury mixer, mixed at 230°C for 20 min to obtain an azobenzene moiety blend; the antioxidant is bis(2,4-di-tert-butylphenyl) pentaerythritol diphosphite; S2. Preparation of thermally conductive polyphenylene ether composite material: 100 parts of PPO and 60 parts of the azobenzene moiety blend prepared in step S1 were uniformly mixed, and a thermally conductive polyphenylene ether composite material was prepared by a twin-screw extruder at an extrusion temperature of 310°C and a screw rotation speed of 200 rpm.

[0030] Comparative Example 1 Comparative Example 1 is different from Example 1 in that the preparation of the thermally conductive polyphenylene ether composite material in step S2: 100 parts of PPO and 20 parts of functionalized UHMWPE were directly compounded, and the other components, preparation steps and parameters were consistent.

[0031] Comparative Example 2 Comparative Example 2 is different from Example 3 in that the preparation of the thermally conductive polyphenylene ether composite material in step S2: 100 parts of PPO and 60 parts of functionalized polystyrene were directly compounded, and the other components, preparation steps and parameters were consistent.

[0032] Comparative Example 3 Comparative Example 3 is different from Example 3 in that the average entanglement molecular weight of UHMWPE added in step S1 is 1500 g / mol, and the other components, preparation steps and parameters are consistent.

[0033] Comparative Example 4 Comparative Example 4 is different from Example 3 in that the reactive monomer 2 in step S1 is 10 parts by weight of 11-[4-(4-butylphenylazo)phenoxy]undecyl methacrylate is added, and the rest of the components, preparation steps and parameters are consistent.

[0034] The thermal conductive polyphenyl ether composite materials prepared in Examples 1-3 and Comparative Examples 1-4 are tested for thermal conductivity according to GB / T 3399 1982 Plastic Thermal Conductivity Test Method Heat Shield Flat Plate Method, and for Charpy notched impact strength according to ISO 179 2000 Determination of the Charpy Impact Strength of Rigid Plastics Materials, and the test results are shown in Table 1.

[0035] Table 1 Thermal conductivity and notched impact strength of Examples 1-3 and Comparative Examples 1-4 As can be seen from Table 1, for Examples 1-3, the functionalized UHMWPE and the functionalized polystyrene are introduced into the PPO composite system to build strong interfacial interactions between the components of the composite system, to play the high strength and toughness of the ultra-high molecular weight polyethylene, and to improve the impact resistance of the composite material. At the same time, the highly entangled structure of the ultra-high molecular weight polyethylene can fix the azobenzene units in the composite system, making them rich in the entangled structure region, and then promoting the azobenzene units to form highly oriented crystalline microzones through π-π stacking self-assembly, significantly improving the phonon coupling and transmission efficiency, and establishing a high-efficiency heat transfer network, giving the polyphenyl ether good thermal conductivity. The thermal conductivity of the polyphenyl ether composite material can reach 1.29-1.81 W / m·K, and the Charpy notched impact strength can reach 12.76-14.45 kJ / m 2 . For Comparative Example 1, only the functionalized UHMWPE is compounded with the PPO resin, and the thermal conductivity of the composite material is significantly reduced to 0.45 W / m·K, and the Charpy notched impact strength is 11.12 kJ / m 2 . For Comparative Example 2, only the functionalized polystyrene is compounded with the PPO resin, at this time the movement ability of the azobenzene units is stronger, and it is difficult to form highly oriented crystalline microzones through π-π stacking self-assembly, the phonon coupling and transmission efficiency is reduced, the thermal conductivity of the polyphenyl ether composite material is only 0.68 W / m·K, and the Charpy notched impact strength is reduced to 9.06 kJ / m 2 . For Comparative Example 3, the average entanglement molar mass of the added UHMWPE is 1500 g / mol, the average molecular entanglement density of the UHMWPE is reduced, the fixing ability of the azobenzene units is weakened, the highly oriented crystalline microzone structure is reduced, the phonon coupling and transmission efficiency is reduced, the thermal conductivity of the polyphenyl ether composite material is reduced to 0.96 W / m·K, and the Charpy notched impact strength is 12.53 kJ / m2 For the comparative example 4, only 10 parts of 11-[4-(4-butylphenylazo) phenoxy] undecyl methacrylate was added, and less 11-[4-(4-butylphenylazo) phenoxy] undecyl methacrylate cannot form a heat conduction network in the PPO composite system, and the thermal conductivity of the polyphenylene ether composite material is only 0.54 W / m·K, and the simply supported beam notched impact strength is 12.62 kJ / m 2 .

[0036] In summary, the present application provides a kind of heat-conducting polyphenylene ether composite material and preparation method thereof, by radical copolymerization and reactive melt processing, azobenzene group and acrylate unit are introduced into polystyrene and ultra-high molecular weight polyethylene chain respectively, and further composite with polyphenylene ether resin, build strong interface interaction between each component of composite system, play the high toughness of ultra-high molecular weight polyethylene, improve the impact resistance of composite material.Using the high molecular entanglement structure of ultra-high molecular weight polyethylene, azobenzene group is fixed in the composite system, and it is enriched in the entanglement structure area, and then promote azobenzene group to form highly oriented crystalline micro area by π-π stacking self-assembly, significantly improve the phonon coupling and transmission efficiency, establish high-efficiency heat transfer network, give polyphenylene ether good thermal conductivity, widen its application in electronic devices, power battery and other fields.

[0037] The above is only a specific embodiment of the present application, but the protection scope of the present application is not limited to this, any skilled person in the art can easily think of various equivalent modifications or replacements within the technical range disclosed by the present application, and these modifications or replacements should be covered in the protection scope of the present application. Therefore, the protection scope of the present application should be subject to the protection scope of claims.

Claims

1. A method for preparing a thermally conductive polyphenylene ether composite material, characterized in that, Includes the following steps: S1. Preparation of azophenyl blend: (1) Mix ultra-high molecular weight polyethylene, ultraviolet photoinitiator, reactive monomer 1 and solvent 1 evenly, treat with ultraviolet lamp, and then clean with N,N-dimethylformamide and deionized water to obtain functionalized UHMWPE; (2) Dissolve styrene and reactive monomer 2 in solvent 2, add free radical copolymerization initiator to react, prepare reaction solution, and finally add methanol dropwise to the reaction solution to obtain functionalized polystyrene; (3) Mix functionalized UHMWPE, functionalized polystyrene and antioxidant to obtain azophenyl blend; S2. Preparation of thermally conductive polyphenylene ether composite material: PPO and the azophenyl blend obtained in step S1 are mixed evenly to obtain thermally conductive polyphenylene ether composite material.

2. The method for preparing the thermally conductive polyphenylene ether composite material as described in claim 1, characterized in that, In step S1, the average entanglement molar mass of the ultra-high molecular weight polyethylene is 300~1000 g / mol; the ultraviolet photoinitiator is selected from one of 2-hydroxy-2-methyl-1-phenyl-1-propanone, 1-hydroxycyclohexylphenyl ketone, 2-hydroxy-4'-(2-hydroxyethoxy)-2-methylphenylpropanone, benzophenone, 2,4,6-trimethylbenzoyl-diphenylphosphine oxide, bis(2,4,6-trimethylbenzoyl)phenylphosphine oxide, and isopropylthioxanthraphenone.

3. The method for preparing the thermally conductive polyphenylene ether composite material as described in claim 1, characterized in that, In step S1, the reactive monomer 1 is selected from one of hydroxyethyl methacrylate, isobutyl methacrylate, n-butyl methacrylate, ethyl methacrylate, methyl methacrylate, glycidyl methacrylate, ethylene glycol dimethacrylate, triethylene glycol dimethacrylate, allyl methacrylate, dimethylaminoethyl methacrylate, and siloxane methacrylate; the solvent 1 is selected from one of dimethyl sulfoxide, xylene, isopropanol, n-butanol, ethyl acetate, butyl acetate, N,N-dimethylformamide, methyl ethyl ketone, and cyclohexanone.

4. The method for preparing the thermally conductive polyphenylene ether composite material as described in claim 1, characterized in that, In step S1, the reactive monomer 2 is selected from one of amino-4'-methacrylate-based azobenzene, 4-methacryloyloxy-4'-methoxyazobenzene, 4,4'-bis(methacryloyloxy)azobenzene, (1-4'-butylazophenoxy-6-hexanol)methacrylate, 11-[4-(4-butylphenylazo)phenoxy]undecyl methacrylate, 4-methacryloyloxyazobenzene, bismethacrylate-based azobenzene, and 4,4'-bis(6''-acryloyloxyhexyloxy)azobenzene; the solvent 2 is selected from one of n-hexane, cyclohexane, toluene, xylene, dichloromethane, chloroform, carbon tetrachloride, diethyl ether, tetrahydrofuran, isopropanol, and n-butanol.

5. The method for preparing the thermally conductive polyphenylene ether composite material as described in claim 1, characterized in that, In step S1, the free radical copolymerization initiator is selected from one of azobisisobutyronitrile, benzoyl peroxide, dicumyl peroxide, dicarbonate peroxide, and azobisisoheptanenitrile; the antioxidant is selected from one of pentaerythritol tetrakis[β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate], octadecyl β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate, 2,6-di-tert-butyl-p-cresol, tris(2,4-di-tert-butylphenyl) phosphite, bis(2,4-di-tert-butylphenyl) pentaerythritol diphosphite, dilauryl thiodipropionate, and N-isopropyl-N'-phenyl-p-phenylenediamine.

6. The method for preparing the thermally conductive polyphenylene ether composite material as described in claim 1, characterized in that, In step S1, the functionalized UHMWPE is prepared by mixing 100 parts by weight of ultra-high molecular weight polyethylene, 0.5-10 parts by weight of ultraviolet photoinitiator, 1-30 parts by weight of reactive monomer 1 and 100-300 parts by weight of solvent 1 at 50-70°C, treating with ultraviolet light for 20-60 minutes under a nitrogen atmosphere with a power of 500-5000W, then cleaning with N,N-dimethylformamide and deionized water, and drying under vacuum at 110°C for 3 hours.

7. The method for preparing the thermally conductive polyphenylene ether composite material according to claim 1, characterized in that, In step S1, the functionalized polystyrene is prepared by dissolving 100 parts of styrene and 40-100 parts of reactive monomer 2 in 100-200 parts of solvent 2 by weight, adding 0.5-10 parts of free radical copolymerization initiator, reacting at 80°C for 12 hours under a nitrogen atmosphere to obtain a reaction solution, and finally adding 5-20 parts of methanol dropwise to the reaction solution for precipitation, filtering, and drying under vacuum at 90°C for 4 hours.

8. The method for preparing the thermally conductive polyphenylene ether composite material as described in claim 1, characterized in that, In step S1, the azophenyl blend is prepared by adding 5-30 parts by weight of functionalized UHMWPE, 70-95 parts by weight of functionalized polystyrene and 0.5-5 parts by weight of antioxidant into an internal mixer and mixing at 200-230°C for 20-60 minutes.

9. The method for preparing the thermally conductive polyphenylene ether composite material as described in claim 1, characterized in that, The thermally conductive polyphenylene oxide composite material in step S2 is prepared by mixing 100 parts by weight of PPO and 20-60 parts by weight of the azophenyl blend obtained in step S1, and then extruding it through a twin-screw extruder at an extrusion temperature of 250-310℃ and a screw speed of 150-200rpm.

10. A thermally conductive polyphenylene ether composite material, characterized in that, It is prepared by the method of any one of claims 1-9 for the preparation of thermally conductive polyphenylene ether composite material.

Images