Epoxy resin compound and preparation method thereof

Abstract

The invention discloses an epoxy resin compound and a preparation method thereof, the epoxy resin compound is a cured product of a compound of epoxy resin, a first heat-conducting filler, a second heat-conducting filler, a phase-change material and a third heat-conducting filler under the action of a curing agent, the epoxy resin accounts for 30-50 parts by weight, the second heat-conducting filler accounts for 30-50 parts by weight, and the phase-change material accounts for 30-50 parts by weight. The first heat-conducting filler accounts for 56-63 parts, the second heat-conducting filler accounts for 6.2-6.5 parts, the third heat-conducting filler compound accounts for 0-7 parts, the phase-change material accounts for 0-7 parts, the curing agent accounts for 7.5-12.5 parts, and the third heat-conducting filler compound comprises a mesoporous material, an organic silicon phosphorus flame retardant, a silane coupling agent and liquid metal. The epoxy resin compound has low viscosity and high thermal conductivity.

Description

Technical Field

[0001] This application relates to the field of thermally conductive materials, and more particularly to a low-viscosity, high-thermal-conductivity epoxy resin composite and its preparation method. Background Technology

[0002] With the advent of the digital age, electronic devices are developing towards miniaturization, high power, and integration. Electronic components are being tightly concentrated in small spaces, and the power density of various devices is constantly increasing. During operation, a large amount of heat is constantly generated and accumulated. If heat cannot be dissipated in time, it may lead to problems such as device lag, performance degradation, or even malfunction. In severe cases, excessively high temperatures can damage electronic devices or even cause fires, greatly increasing the probability of safety accidents. Thermally conductive polymer materials, due to their good processing properties and low manufacturing costs, are widely used in various fields such as intelligent electronic devices, aerospace, electrical cables, and energy heat exchange.

[0003] Epoxy resin (EP) is often used as an electronic packaging material due to its excellent mechanical properties, superior electrical insulation, chemical resistance, and ease of processing. However, with the increasing power density and integration of electronic devices, the low thermal conductivity of traditional epoxy resins fails to meet the heat dissipation requirements of modern electronic products. Therefore, constructing more efficient thermal conductive networks and preparing epoxy resin-based high thermal conductivity composite materials with excellent overall performance is crucial for the development of next-generation high-performance electronic products. Summary of the Invention

[0004] The technical problem to be solved by this application is to provide a low-viscosity, high-thermal-conductivity epoxy resin composite and its preparation method, so that the epoxy resin composite has better thermal conductivity.

[0005] This application provides an epoxy resin composite, which is a cured product of epoxy resin, a first thermally conductive filler, a second thermally conductive filler, a phase change material, and a third thermally conductive filler composite under the action of a curing agent. By weight, the epoxy resin accounts for 30 to 50 parts, the first thermally conductive filler accounts for 56 to 63 parts, the second thermally conductive filler accounts for 6.2 to 6.5 parts, the third thermally conductive filler composite accounts for 0 to 7 parts, the phase change material accounts for 0 to 7 parts, and the curing agent accounts for 7.5 to 12.5 parts. The first thermally conductive filler includes at least one of alumina, zinc oxide, magnesium oxide, and beryllium oxide; the second thermally conductive filler includes at least one of silicon carbide, boron carbide, boron nitride, and aluminum nitride; the phase change material includes at least one of vanadium oxide, tungsten-doped vanadium oxide, titanium-doped vanadium oxide, and tungsten-titanium-doped vanadium oxide; and the third thermally conductive filler composite includes a mesoporous material, an organosilicon-phosphorus flame retardant, a silane coupling agent, and liquid metal.

[0006] In some embodiments of this application, the mesoporous material includes at least one of mesoporous silica, mesoporous alumina, mesoporous titanium dioxide, and mesoporous zirconium oxide; the organosilicone phosphorus flame retardant includes at least one of polysiloxane-type organosilicone phosphorus flame retardant, POSS-based organosilicone phosphorus flame retardant, DOPO derivative organosilicone phosphorus flame retardant, and small molecule organosilicone phosphorus compound; the liquid metal includes at least one of rubidium, gallium, gallium indium tin alloy, sodium potassium alloy, gallium indium alloy, bismuth indium tin alloy, and gallium indium tin zinc alloy; the silane coupling agent includes at least one of γ-aminopropyltriethoxysilane (KH-550), N-β-aminoethyl-γ-aminopropyltrimethoxysilane (KH-792), γ-glycidoxypropyltrimethoxysilane (KH-560), vinyltriethoxysilane (A-151), and vinyltrimethoxysilane (VTMO).

[0007] In some embodiments of this application, the epoxy resin includes at least one of bisphenol A diglycidyl ether, bisphenol F type epoxy resin, polyphenol type glycidyl ether epoxy resin, and aliphatic glycidyl ether epoxy resin.

[0008] In some embodiments of this application, the curing agent is an amine curing agent or an acid anhydride curing agent.

[0009] In some embodiments of this application, the curing agent includes at least one selected from ethylenediamine, hexamethylenediamine, m-phenylenediamine, 4,4'-diaminodiphenylmethane, 4,4-diaminodiphenyl sulfone, maleic anhydride, and phthalic anhydride.

[0010] This application also provides a method for preparing an epoxy resin composite, comprising: uniformly mixing epoxy resin, a first thermally conductive filler, a second thermally conductive filler, a phase change material, and a third thermally conductive filler composite to form a first mixture; adding a curing agent to the first mixture; and, under the action of the curing agent, causing each component in the first mixture to undergo a curing reaction to form a cured product. By weight, the epoxy resin accounts for 30 to 50 parts, the first thermally conductive filler accounts for 56 to 63 parts, the second thermally conductive filler accounts for 6.2 to 6.5 parts, and the third thermally conductive filler... The composite material comprises 0 to 7 parts, the phase change material comprises 0 to 7 parts, and the curing agent comprises 7.5 to 12.5 parts. The first thermally conductive filler comprises at least one of alumina, zinc oxide, magnesium oxide, and beryllium oxide. The second thermally conductive filler comprises at least one of silicon carbide, boron carbide, boron nitride, and aluminum nitride. The phase change material comprises at least one of vanadium oxide, tungsten-doped vanadium oxide, titanium-doped vanadium oxide, and tungsten-titanium-doped vanadium oxide. The third thermally conductive filler composite comprises mesoporous material, organosilicon phosphorus flame retardant, silane coupling agent, and liquid metal.

[0011] In some embodiments of this application, the mesoporous material includes at least one of mesoporous silica, mesoporous alumina, mesoporous titanium dioxide, mesoporous zirconium oxide, and graphene porous materials; the organosilicone phosphorus flame retardant includes at least one of polysiloxane-type organosilicone phosphorus flame retardant, POSS-based organosilicone phosphorus flame retardant, DOPO derivative organosilicone phosphorus flame retardant, and small molecule organosilicone phosphorus compound; the liquid metal includes at least one of rubidium, gallium, gallium indium tin alloy, sodium potassium alloy, gallium indium alloy, bismuth indium tin alloy, and gallium indium tin zinc alloy; the silane coupling agent includes at least one of γ-aminopropyltriethoxysilane (KH-550), N-β-aminoethyl-γ-aminopropyltrimethoxysilane (KH-792), γ-glycidoxypropyltrimethoxysilane (KH-560), vinyltriethoxysilane (A-151), and vinyltrimethoxysilane (VTMO).

[0012] In some embodiments of this application, the liquid metal is prepared by heating gallium metal to 50°C, then adding indium metal, and heating the mixture of the two metals to 190°C while stirring for several hours to obtain the liquid metal.

[0013] In some embodiments of this application, the preparation method of the third thermally conductive filler composite includes: Drying removes water molecules from the surface of the mesoporous material and the pores of the mesoporous material, exposing the active sites in the mesoporous material. The mesoporous material is made into a colloidal suspension in a first organic solvent. Then, the organosilicon-phosphorus flame retardant is added to the colloidal suspension, and the organosilicon-phosphorus molecules in the organosilicon-phosphorus flame retardant undergo a condensation reaction with the groups in the active sites on the surface of the mesoporous material to form a covalent compound, thereby obtaining an organosilicon-phosphorus functionalized mesoporous material hybrid flame retardant, denoted as SiP-J. The SiP-J is mixed with liquid metal, and under oil bath and ultrasonic conditions, a portion of the liquid metal is embedded in the channels of the SiP-J, while the other portion forms a metal coating on the surface of the SiP-J, forming mesoporous spheres. The filling rate of the liquid metal in the channels of the mesoporous spheres is 60-80%. The mesoporous spheres are crushed to a set particle size and uniformity. The mesoporous spheres are mixed with the silane coupling agent and then activated to allow the silane coupling agent to be chemically grafted onto the surface of the intermediate product, forming the third thermally conductive filler composite.

[0014] In some embodiments of this application, before pulverizing the mesoporous balls to a set particle size and uniformity, the method further includes: controlling the rotation speed and time of the ball mill to increase the filling rate of the liquid metal in the channels of the mesoporous balls to 80-95%.

[0015] In some embodiments of this application, in the third thermally conductive filler composite, the weight ratio of the mesoporous material to the sum of the weights of the organosilicone-phosphorus flame retardant and the silane coupling agent ranges from 1:(0.02~3); the molar ratio of the organosilicone-phosphorus flame retardant to the silane coupling agent ranges from 1:(1~3). Compared with the prior art, the technical solution of this application has the following beneficial effects: The third thermally conductive filler composite provided in this embodiment combines the flowability and thermal conductivity of liquid metal. Under oil bath and ultrasonic conditions, a portion of the liquid metal is embedded within the channels of the SiP-J, while another portion forms a metal coating on the surface of the SiP-J, thereby controlling the physical state of the third thermally conductive filler composite. When heat is generated, the temperature rises, and the liquid metal embedded in the channels of the mesoporous material spontaneously flows out, connecting different thermally conductive particles to form a through-connected thermally conductive network, thereby improving the thermal conductivity of the epoxy resin composite. Furthermore, the addition of the organosilicon-phosphorus flame retardant also lays a good foundation for improving the flame retardant properties of the epoxy resin composite.

[0016] Furthermore, if only one type of thermally conductive filler is added to the epoxy resin, the addition and dispersion of the thermally conductive filler will negatively affect the thermal conductivity pathway of the epoxy resin. In this embodiment, a thermally conductive epoxy resin composite, such as a bisphenol A diglycidyl ether thermally conductive epoxy composite, is formed by solution blending of a first thermally conductive filler, a second thermally conductive filler, a phase change material, and a third thermally conductive filler. This results in high thermal conductivity and low viscosity. Therefore, the epoxy resin composite formed in this application has advantages such as high thermal conductivity, low viscosity, low electrical conductivity, and flame retardancy, which can further expand the application range of epoxy resin in electronic packaging materials. Attached Figure Description

[0017] Figure 1 This is a schematic diagram of the structure of the third thermally conductive filler composite formed in an embodiment of this application. Detailed Implementation

[0018] The following description provides specific application scenarios and requirements for this application, intended to enable those skilled in the art to make and use the content of this application. Various partial modifications to the disclosed embodiments will be apparent to those skilled in the art, and the general principles defined herein can be applied to other embodiments and applications without departing from the spirit and scope of this application. Therefore, this application is not limited to the embodiments shown, but rather to the widest scope consistent with the claims.

[0019] This application provides an epoxy resin composite, which is a cured product of epoxy resin, a first thermally conductive filler, a second thermally conductive filler, a phase change material, and a third thermally conductive filler composite under the action of a curing agent. By weight, the epoxy resin accounts for 30 to 50 parts, the first thermally conductive filler accounts for 56 to 63 parts, the second thermally conductive filler accounts for 6.2 to 6.5 parts, the third thermally conductive filler composite accounts for 0 to 7 parts, the phase change material accounts for 0 to 7 parts, and the curing agent accounts for 7.5 to 12.5 parts. The first thermally conductive filler includes at least one of alumina, zinc oxide, magnesium oxide, and beryllium oxide; the second thermally conductive filler includes at least one of silicon carbide, boron carbide, boron nitride, and aluminum nitride; the phase change material includes at least one of vanadium oxide, tungsten-doped vanadium oxide, titanium-doped vanadium oxide, and tungsten-titanium-doped vanadium oxide; and the third thermally conductive filler composite includes a mesoporous material, an organosilicon-phosphorus flame retardant, a silane coupling agent, and liquid metal.

[0020] In some embodiments of this application, the mesoporous material includes at least one of mesoporous silica, mesoporous alumina, mesoporous titanium dioxide, and mesoporous zirconium oxide porous materials; the organosilicone phosphorus flame retardant includes at least one of polysiloxane-type organosilicone phosphorus flame retardant, POSS-based organosilicone phosphorus flame retardant, DOPO derivative organosilicone phosphorus flame retardant, and small molecule organosilicone phosphorus compound; the liquid metal includes at least one of rubidium, gallium, gallium indium tin alloy, sodium potassium alloy, gallium indium alloy, bismuth indium tin alloy, and gallium indium tin zinc alloy; the silane coupling agent includes at least one of γ-aminopropyltriethoxysilane (KH-550), N-β-aminoethyl-γ-aminopropyltrimethoxysilane (KH-792), γ-glycidoxypropyltrimethoxysilane (KH-560), vinyltriethoxysilane (A-151), and vinyltrimethoxysilane (VTMO).

[0021] In some embodiments of this application, by weight, the epoxy resin composite comprises 35 parts of the epoxy resin, 62 parts of the first thermally conductive filler, 6.3 parts of the second thermally conductive filler, 3 parts of the third thermally conductive filler composite, 5 parts of the phase change material, and 8 parts of the curing agent. The first thermally conductive filler is beryllium oxide, the second thermally conductive filler is a mixture of boron carbide and boron nitride, the phase change material is tungsten-titanium doped vanadium oxide, and the third thermally conductive filler composite comprises a mesoporous material (mesoporous zirconium oxide), an organosilicon phosphorus flame retardant, a silane coupling agent vinyltriethoxysilane, and a liquid metal (a mixture of gallium indium alloy and bismuth indium tin alloy).

[0022] In some embodiments of this application, by weight, the epoxy resin composite comprises 40 parts of the epoxy resin, 57 parts of the first thermally conductive filler, 6.3 parts of the second thermally conductive filler, 5 parts of the third thermally conductive filler composite, 6 parts of the phase change material, and 10.5 parts of the curing agent. The first thermally conductive filler is a mixture of zinc oxide and magnesium oxide, the second thermally conductive filler is boron carbide, the phase change material is tungsten-doped vanadium oxide, and the third thermally conductive filler composite comprises a mesoporous material (mesoporous silica), an organosilicon phosphorus flame retardant (DOPO derivative organosilicon phosphorus flame retardant), a silane coupling agent N-β-aminoethyl-γ-aminopropyltrimethoxysilane, and liquid gallium metal.

[0023] In some other embodiments of this application, the epoxy resin composite comprises 45 parts of the epoxy resin, 60 parts of the first thermally conductive filler, 6.4 parts of the second thermally conductive filler, 3 parts of the third thermally conductive filler composite, 4 parts of the phase change material, and 9 parts of the curing agent. The first thermally conductive filler is alumina, the second thermally conductive filler is silicon carbide, the phase change material is vanadium oxide, and the third thermally conductive filler composite comprises a mesoporous material (mesoporous alumina), an organosilicon phosphorus flame retardant (DOPO derivative organosilicon phosphorus flame retardant), a silane coupling agent γ-aminopropyltriethoxysilane, and a liquid gallium indium tin alloy.

[0024] In some embodiments of this application, the epoxy resin includes at least one of bisphenol A diglycidyl ether, bisphenol F type epoxy resin, polyphenolic glycidyl ether epoxy resin, and aliphatic glycidyl ether epoxy resin. For example, a blend of bisphenol A diglycidyl ether and bisphenol F type epoxy resin, or a blend of polyphenolic glycidyl ether epoxy resin and aliphatic glycidyl ether epoxy resin.

[0025] In some embodiments of this application, the curing agent is an amine curing agent or an acid anhydride curing agent.

[0026] In some embodiments of this application, the curing agent includes at least one selected from ethylenediamine (EDA), hexamethylenediamine (HMD), m-phenylenediamine (m-PDA), 4,4'-diaminodiphenylmethane (DDM), 4,4-diaminodiphenyl sulfone (DDS), maleic anhydride (MA), and phthalic anhydride (PA).

[0027] This application also provides a method for preparing an epoxy resin composite, comprising: uniformly mixing epoxy resin, a first thermally conductive filler, a second thermally conductive filler, a phase change material, and a third thermally conductive filler composite to form a first mixture; adding a curing agent to the first mixture; and, under the action of the curing agent, causing each component in the first mixture to undergo a curing reaction to form a cured product. By weight, the epoxy resin accounts for 30 to 50 parts, the first thermally conductive filler accounts for 56 to 63 parts, the second thermally conductive filler accounts for 6.2 to 6.5 parts, and the third thermally conductive filler composite... The compound comprises 0 to 7 parts, the phase change material comprises 0 to 7 parts, and the curing agent comprises 7.5 to 12.5 parts. The first thermally conductive filler comprises at least one of alumina, zinc oxide, magnesium oxide, and beryllium oxide. The second thermally conductive filler comprises at least one of silicon carbide, boron carbide, boron nitride, and aluminum nitride. The phase change material comprises at least one of vanadium oxide, tungsten-doped vanadium oxide, titanium-doped vanadium oxide, and tungsten-titanium-doped vanadium oxide. The third thermally conductive filler compound comprises mesoporous material, organosilicon phosphorus flame retardant, silane coupling agent, and liquid metal.

[0028] The mesoporous material includes at least one of mesoporous silica, mesoporous alumina, mesoporous titanium dioxide, and mesoporous zirconium oxide; the organosilicone phosphorus flame retardant includes at least one of polysiloxane-type organosilicone phosphorus flame retardant, POSS-based organosilicone phosphorus flame retardant, DOPO derivative organosilicone phosphorus flame retardant, and small molecule organosilicone phosphorus compound; the liquid metal includes at least one of rubidium, gallium, gallium indium tin alloy, sodium potassium alloy, gallium indium alloy, bismuth indium tin alloy, and gallium indium tin zinc alloy; the silane coupling agent includes at least one of γ-aminopropyltriethoxysilane (KH-550), N-β-aminoethyl-γ-aminopropyltrimethoxysilane (KH-792), γ-glycidoxypropyltrimethoxysilane (KH-560), vinyltriethoxysilane (A-151), and vinyltrimethoxysilane (VTMO).

[0029] The curing reaction occurs at a temperature range of 60°C to 80°C. The mixture of epoxy resin, first thermally conductive filler, second thermally conductive filler, phase change material and third thermally conductive filler composite is continuously stirred for 1 to 2 hours until all components are uniformly mixed to form the first mixture.

[0030] Then, a curing agent is added to the first mixture. Under the action of the curing agent, the components in the first mixture undergo a curing reaction at a temperature of 60°C to 80°C to form a cured product, including: Step S21: Add 7.5 to 12.5 parts by weight of curing agent to the first mixture, heat until the curing agent is completely dissolved, and then perform degassing to form a second mixture. The degassing process can be, for example, placing the mixture of the first mixture and the curing agent in a vacuum oven, drawing the vacuum to the bottom, and then performing degassing in the vacuum oven.

[0031] Step S22: Pour the second mixture into a curing device and cure it at a temperature of 120°C to 160°C for 2 to 6 hours to form the cured product. In some embodiments of this application, the second mixture is poured into a curing device and cured at a temperature of 140°C for 5 hours to form the cured product.

[0032] In some embodiments of this application, the second mixture is poured into a curing device and cured at a temperature of 120°C to 160°C for 2 to 6 hours to form the cured product. The process can be performed in steps. For example, the second mixture is poured into a curing device preheated to 80°C, first cured at 120°C for 2 hours, then the curing temperature is adjusted to 160°C and cured for 3 hours to form the cured product. After the cured product cools to room temperature, it is removed from the curing device.

[0033] In the embodiments of this application, the curing agent is an amine curing agent or an anhydride curing agent, including at least one of ethylenediamine (EDA), hexamethylenediamine (HMD), m-phenylenediamine (m-PDA), 4,4'-diaminodiphenylmethane (DDM), 4,4-diaminodiphenyl sulfone (DDS), maleic anhydride (MA), and phthalic anhydride (PA).

[0034] In this embodiment, the epoxy resin includes at least one of bisphenol A diglycidyl ether (DGEBA), bisphenol F type epoxy resin (BPF), polyphenol type glycidyl ether epoxy resin, or aliphatic glycidyl ether epoxy resin.

[0035] The silane coupling agent is an aminosilane, epoxysilane, or vinylsilane coupling agent, including at least one of γ-aminopropyltriethoxysilane (KH-550), N-β-aminoethyl-γ-aminopropyltrimethoxysilane (KH-792), γ-glycidoxypropyltrimethoxysilane (KH-560), vinyltriethoxysilane (A-151), and vinyltrimethoxysilane (VTMO); and / or the liquid metal includes at least one of rubidium, gallium, gallium-indium-tin alloy, sodium-potassium alloy, gallium-indium alloy, bismuth-indium-tin alloy, and gallium-indium-tin-zinc alloy.

[0036] In some embodiments of this application, the third thermally conductive filler composite is synthesized from mesoporous materials, organosilicone-phosphorus flame retardants, liquid metals, and silane coupling agents as raw materials. The mesoporous materials are at least one of mesoporous silica, mesoporous alumina, mesoporous titanium dioxide, and mesoporous zirconium oxide. The organosilicone-phosphorus flame retardants include at least one of polysiloxane-type organosilicone-phosphorus flame retardants, POSS-based organosilicone-phosphorus flame retardants, DOPO derivative organosilicone-phosphorus flame retardants, and small molecule organosilicone-phosphorus compounds. The metal in the state is at least one of rubidium, gallium, gallium-indium-tin alloy, sodium-potassium alloy, gallium-indium alloy, bismuth-indium-tin alloy, and gallium-indium-tin-zinc alloy; the silane coupling agent monomer includes any one of γ-aminopropyltriethoxysilane (KH-550), N-β-aminoethyl-γ-aminopropyltrimethoxysilane (KH-792), γ-glycidoxypropyltrimethoxysilane (KH-560), vinyltriethoxysilane (A-151), and vinyltrimethoxysilane (VTMO).

[0037] In some embodiments of this application, the preparation method of the third thermally conductive filler composite includes: Drying removes water molecules from the surface of the mesoporous material and the pores within the mesoporous material, exposing active sites in the mesoporous material, such as silanol groups (Si-OH). The mesoporous material is made into a colloidal suspension in a first organic solvent. Then, the organosilicon-phosphorus flame retardant is added to the colloidal suspension, and the organosilicon-phosphorus molecules in the organosilicon-phosphorus flame retardant undergo a condensation reaction with the groups in the active sites on the surface of the mesoporous material to form a covalent compound, thereby obtaining an organosilicon-phosphorus functionalized mesoporous material hybrid flame retardant, denoted as SiP-J. The SiP-J is mixed with liquid metal, and under oil bath and ultrasonic conditions, a portion of the liquid metal is embedded in the channels of the SiP-J, while the other portion forms a metal coating on the surface of the SiP-J, forming mesoporous spheres. The filling rate of the liquid metal in the channels of the mesoporous spheres is 60-80%. The mesoporous spheres are crushed to a set particle size and uniformity. The mesoporous spheres are mixed with the silane coupling agent and then activated to allow the silane coupling agent to be chemically grafted onto the surface of the intermediate product, forming the third thermally conductive filler composite.

[0038] In some embodiments of this application, before pulverizing the mesoporous balls to a set particle size and uniformity, the method further includes: controlling the rotation speed and time of the ball mill to increase the filling rate of the liquid metal in the channels of the mesoporous balls to 80-95%.

[0039] In some embodiments of this application, in the third thermally conductive filler composite, the ratio of the weight of the mesoporous material to the sum of the weights of the organosilicone-phosphorus flame retardant and the silane coupling agent is in the range of 1:(0.02~3); the molar ratio of the organosilicone-phosphorus flame retardant to the silane coupling agent is in the range of 1:(1~3).

[0040] In a specific embodiment of this application, the method for preparing the third thermally conductive filler composite is as follows: The original mesoporous material is placed in a vacuum drying oven and dried continuously at 120°C and a constant vacuum (≤10 Pa) for 4 hours to completely remove physically adsorbed water molecules from the material surface and pores, thereby fully exposing the silanol groups (Si-OH) and providing active sites for subsequent surface modification. The dehydrated mesoporous material is transferred to a three-necked flask containing anhydrous ethanol and treated with a high-intensity ultrasonic cell disruptor (power ≥500 W, frequency 20 kHz) for 30 minutes to ensure that the mesoporous material forms a highly uniform and stable colloidal suspension in the solvent, avoiding uneven reaction caused by agglomeration. According to a precise stoichiometric ratio of 6:1 between the mesoporous material framework structure and the organosilicon phosphorus flame retardant, the flame retardant is slowly added dropwise to the above suspension. The reaction system is placed on a heat-collecting constant-temperature magnetic stirrer, heated to 78°C (ethanol reflux temperature), and continuously stirred for 12 hours under reflux conditions. During the reaction, a catalytic amount of protic acid (such as p-toluenesulfonic acid, concentration 0.1 mol%) is continuously added via a micro-injection pump to promote the hydrolysis of organosilicon phosphorus molecules and their condensation reaction with silanol groups on the mesoporous surface, forming strong covalent bonds. After the reaction, the mixture is transferred to a high-speed centrifuge (speed ≥10,000 rpm) for solid-liquid separation. The resulting solid precipitate is washed with anhydrous ethanol as the washing medium, and repeated centrifugation-redispersion cycles (at least 5 times) are performed to thoroughly remove physically adsorbed and unreacted organosilicon phosphorus species. Finally, the purified product is placed in a vacuum drying oven and dried at 80°C for 24 hours to obtain an organosilicon phosphorus functionalized mesoporous material hybrid flame retardant, denoted as SiP-J. SiP-J and liquid metal (such as gallium-based alloy) are weighed at a mass ratio of 4:1 to 5:1 and placed in a special high-temperature resistant beaker. The beaker is fixed to a precision oil bath heating system, and the oil bath temperature is controlled at 100°C. Under these conditions, a high-power ultrasonic processor (amplitude ≥80%, pulse mode) was used to treat the mixture, promoting the initial spreading and coating of liquid metal on the SiP-J surface. The ultrasonic pretreatment system was then transferred to a digitally temperature-controlled magnetic stirring platform and continuously stirred at a constant speed (800 rpm) for 2 hours under a constant temperature of 100℃ and an inert atmosphere to further fuse and disperse the two-phase interface. The stirred mixture was then poured into a high-performance planetary ball mill, using zirconia grinding balls (diameter gradient configuration), and subjected to high-energy ball milling under strictly controlled speed (300 rpm) and time (4 hours) to induce mechanochemical effects and strengthen the interfacial bonding between the packing materials. After ball milling, the material was removed and manually finely ground using an agate mortar to reduce particle size and improve uniformity.The ground intermediate product and a silane coupling agent with a specific structure (such as aminosilane) are added to a ball mill at a preset mass ratio (e.g., 10:1). A multi-stage ball milling program (including low-speed mixing and high-speed activation stages) is set for a total time of 6 hours to achieve chemical grafting of the coupling agent onto the surface of the composite filler. Finally, the product is ground again using an agate mortar to obtain the third thermally conductive filler composite. (Appendix to this application.) Figure 1 The diagram shows a structural schematic of the third thermally conductive filler composite. R1 includes... , , or Any one of them; R2 includes , or Any one of them.

[0041] In this embodiment of the application, the method for preparing the liquid metal may include: heating gallium metal to 50°C, then adding indium metal thereto, and heating the gallium and indium metal mixture to 190°C while stirring and maintaining stirring for several hours to obtain the liquid metal.

[0042] The third thermally conductive filler composite described in this application embodiment is formed by reacting liquid metal, organosilicon phosphorus flame retardant, silane coupling agent and mesoporous material to form a composite, wherein the liquid metal has high thermal conductivity and fluidity. Therefore, the third thermally conductive filler composite has both high thermal conductivity and low viscosity properties.

[0043] The third thermally conductive filler composite provided in this application embodiment combines the flowability and thermal conductivity of liquid metal. The physical state of the epoxy resin composite is controlled by embedding fluid liquid metal within a mesoporous material. When heat is generated, the temperature rises, and the liquid metal embedded in the pores spontaneously flows out, connecting different thermally conductive particles to form a continuous thermally conductive network, thereby improving the thermal conductivity of the epoxy resin.

[0044] Furthermore, if thermally conductive fillers are added alone to epoxy resin, the addition and dispersion of these fillers can negatively impact the thermal conductivity pathway. In this application, a composite of a first thermally conductive filler, a second thermally conductive filler, a phase change material, and a third thermally conductive filler is formed by solution blending to create a bisphenol A diglycidyl ether epoxy composite material, which exhibits high thermal conductivity and low viscosity. Therefore, the low-viscosity, high-thermal-conductivity bisphenol A diglycidyl ether epoxy composite material of this application possesses advantages such as high thermal conductivity, low viscosity, low electrical conductivity, and flame retardancy, which can further expand the application range of epoxy resin in electronic packaging materials.

[0045] The third thermally conductive filler composite provided in this embodiment combines the flowability and thermal conductivity of liquid metal. Under oil bath and ultrasonic conditions, a portion of the liquid metal is embedded within the channels of the SiP-J, while another portion forms a metal coating on the surface of the SiP-J, thereby controlling the physical state of the third thermally conductive filler composite. When heat is generated, the temperature rises, and the liquid metal embedded in the channels of the mesoporous material spontaneously flows out, connecting different thermally conductive particles to form a through-connected thermally conductive network, thereby improving the thermal conductivity of the epoxy resin composite. Furthermore, the addition of the organosilicon-phosphorus flame retardant also lays a good foundation for improving the flame retardant properties of the epoxy resin composite.

[0046] Furthermore, if only one type of thermally conductive filler is added to the epoxy resin, the addition and dispersion of the thermally conductive filler will negatively affect the thermal conductivity pathway of the epoxy resin. In this embodiment, a thermally conductive epoxy resin composite, such as a bisphenol A diglycidyl ether thermally conductive epoxy composite, is formed by solution blending of a first thermally conductive filler, a second thermally conductive filler, a phase change material, and a third thermally conductive filler. This results in high thermal conductivity and low viscosity. Therefore, the epoxy resin composite formed in this application has advantages such as high thermal conductivity, low viscosity, low electrical conductivity, and flame retardancy, which can further expand the application range of epoxy resin in electronic packaging materials. Specific Implementation Example 1: The raw mesoporous material was placed in a vacuum drying oven and dried continuously at 120°C and a constant vacuum (≤10 Pa) for 4 hours to completely remove physically adsorbed water molecules from the material surface and pores, thus fully exposing the silanol groups (Si-OH) and providing active sites for subsequent surface modification. The dehydrated mesoporous material was then transferred to a three-necked flask containing anhydrous ethanol and treated with a high-intensity ultrasonic cell disruptor (power ≥500 W, frequency 20 kHz) for 30 minutes to ensure the formation of a highly uniform and stable colloidal suspension in the solvent, avoiding uneven reaction due to agglomeration. Following a precise stoichiometric ratio of 6:1 (mesoporous material framework structure to organosilicon phosphorus flame retardant), the flame retardant was slowly added dropwise to the suspension. The reaction system was placed on a thermostatically heated magnetic stirrer and heated to 78°C (ethanol reflux temperature), and continuously stirred under reflux conditions for 12 hours. During the reaction, a catalytic amount of protic acid (such as p-toluenesulfonic acid, concentration 0.1 mol%) was continuously added via a micro-injection pump to promote the hydrolysis of organosilicon phosphorus molecules and their condensation reaction with silanol groups on the mesoporous surface, forming strong covalent bonds. After the reaction, the mixture was transferred to a high-speed centrifuge (speed ≥10,000 rpm) for solid-liquid separation. The resulting solid precipitate was washed with anhydrous ethanol and subjected to repeated centrifugation-redispersion cycles (at least 5 times) to thoroughly remove physically adsorbed and unreacted organosilicon phosphorus species. Finally, the purified product was placed in a vacuum drying oven and dried at 80°C for 24 hours to obtain an organosilicon phosphorus functionalized mesoporous material hybrid flame retardant, denoted as SiP-J.

[0048] Example 2: 75 g of metallic gallium is heated to 50°C, and then 48 g of metallic indium is added. The mixture of the two metals is heated to 190°C while stirring and kept stirring for 8 hours to obtain liquid metallic gallium-indium alloy (GaIn).

[0049] Example 3: SiP-J and liquid metal (such as gallium-based alloy) were weighed at a mass ratio of 4:1 to 5:1 and placed in a special high-temperature resistant beaker. The beaker was fixed to a precision oil bath heating system, and the oil bath temperature was controlled at 100°C. Under these conditions, a high-power ultrasonic processor (amplitude ≥80%, pulse mode) was used to process the mixture, promoting the initial spreading and coating of the liquid metal on the SiP-J surface. The ultrasonic pretreatment system was then transferred to a digitally temperature-controlled magnetic stirring platform and stirred continuously at a constant speed (800 rpm) for 2 hours under a constant temperature of 100°C and an inert atmosphere to further fuse and disperse the two phases at the interface. The stirred mixture was then poured into a high-performance planetary ball mill, using zirconia grinding balls (diameter gradient configuration), and high-energy ball milling was performed under strictly controlled speed (300 rpm) and time (4 hours) to induce mechanochemical effects and strengthen the interfacial bonding between the packings. After ball milling, the material was removed and manually finely ground using an agate mortar to reduce particle size and improve uniformity. The ground intermediate product and a silane coupling agent with a specific structure (such as aminosilane) were added to a ball mill at a preset mass ratio (e.g., 10:1). A multi-stage ball milling program (including low-speed mixing and high-speed activation stages) was set for a total duration of 6 hours to achieve chemical grafting of the coupling agent onto the surface of the composite filler. Finally, the product was ground again using an agate mortar to obtain the third thermally conductive filler composite.

[0050] Example 4: Preparation of the epoxy resin composite: The epoxy resin is bisphenol A diglycidyl ether (DGEBA) with an epoxy equivalent of 0.51 mol / 100g. The curing agent is an amine curing agent, 4,4'-diaminodiphenylmethane (DDM). The first thermally conductive filler is alumina, the second thermally conductive filler is boron nitride, the phase change material is vanadium dioxide, and the third thermally conductive filler composite is obtained by blending SiP-J, gallium indium alloy, and KH560 in a ratio of 4:1:2.5. All components are then cured to obtain a low-viscosity, high-thermal-conductivity epoxy resin composite. By weight, the epoxy resin matrix accounts for 50 parts, the first thermally conductive filler alumina accounts for 62.5 parts, the second thermally conductive filler boron nitride accounts for 6.94 parts, vanadium dioxide accounts for 5.56 parts, the third thermally conductive filler composite accounts for 1.39 parts, and the curing agent accounts for 12.5 parts. 50 parts epoxy resin, 62.5 parts alumina, 6.94 parts boron nitride, 5.56 parts vanadium dioxide, and 1.39 parts of the third thermally conductive filler composite were added in batches to a beaker and mechanically stirred at 80 °C for 1.5 h (600-800 r / min) to ensure thorough mixing. Then, 12.5 parts of curing agent were added and stirred continuously for 8 min until the curing agent was completely dissolved. The beaker was then placed in a vacuum oven and evacuated to the bottom for degassing. The degassed mixture was then poured into a mold preheated at 80 °C, cured at 120 °C for 2 h, and then cured at 160 °C for another 3 h to obtain the epoxy resin composite. The parts mentioned in this example are by weight.

[0051] The addition of liquid metal can improve the agglomeration problem caused by the addition of a large amount of thermally conductive filler, reduce the viscosity of epoxy resin composites, and the use of thermally conductive fillers of different shapes can form a connected thermally conductive network, which not only improves thermal conductivity but also reduces viscosity.

[0052] Example 5: An epoxy resin composite was prepared by comprising 50 parts epoxy resin, 56.25 parts alumina thermally conductive filler, 6.25 parts boron nitride thermally conductive filler, and 12.5 parts curing agent. The remaining implementation process was the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0053] Example 6: The epoxy resin composite is prepared by comprising 50 parts epoxy resin, 62.5 parts alumina thermally conductive filler, 6.94 parts boron nitride thermally conductive filler, 6.94 parts a third thermally conductive filler composite, and 12.5 parts curing agent. The remaining implementation process is the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0054] Example 7: An epoxy resin composite was prepared by comprising 50 parts epoxy resin, 62.5 parts alumina thermally conductive filler, 6.94 parts boron nitride thermally conductive filler, 6.94 parts vanadium dioxide, and 12.5 parts curing agent. The remaining implementation process was the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0055] Example 8: The epoxy resin composite is prepared by comprising 50 parts epoxy resin, 62.5 parts alumina thermally conductive filler, 6.94 parts boron nitride thermally conductive filler, 6.25 parts vanadium dioxide, 0.69 parts a third thermally conductive filler composite, and 12.5 parts curing agent. The remaining implementation process is the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0056] Example 9: The epoxy resin composite is prepared by comprising 50 parts epoxy resin, 62.5 parts alumina thermally conductive filler, 6.94 parts boron nitride thermally conductive filler, 5.9 parts vanadium dioxide, 1.04 parts a third thermally conductive filler composite, and 12.5 parts curing agent. The remaining implementation process is the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0057] Example 10: The epoxy resin composite is prepared by comprising 50 parts epoxy resin, 62.5 parts alumina thermally conductive filler, 6.94 parts boron nitride thermally conductive filler, 3.47 parts vanadium dioxide, 3.47 parts a third thermally conductive filler composite, and 12.5 parts curing agent. The remaining implementation process is the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0058] Example 11: The epoxy resin composite is prepared by comprising 50 parts epoxy resin, 62.5 parts alumina thermally conductive filler, 6.94 parts boron nitride thermally conductive filler, 1.39 parts vanadium dioxide, 5.56 parts a third thermally conductive filler composite, and 12.5 parts curing agent. The remaining implementation process is the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0059] Example 12: An epoxy resin composite was prepared by comprising 50 parts epoxy resin and 12.5 parts curing agent, and the remaining process was the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0060] Example 13: An epoxy resin composite was prepared by comprising 50 parts epoxy resin, 56 parts zinc oxide thermally conductive filler, 6.25 parts boron nitride thermally conductive filler, and 12.5 parts curing agent. The remaining process was the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0061] Example 14: The epoxy resin composite is prepared by comprising 50 parts epoxy resin, 62.5 parts zinc oxide thermally conductive filler, 6 parts boron nitride thermally conductive filler, 6.94 parts third thermally conductive filler composite, and 12.5 parts curing agent. The remaining process is the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0062] Example 15: An epoxy resin composite was prepared by comprising 50 parts epoxy resin, 62.5 parts zinc oxide thermally conductive filler, 4.94 parts boron nitride thermally conductive filler, 6.94 parts vanadium dioxide, and 12.5 parts curing agent. The remaining implementation process was the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0063] Example 16: The epoxy resin composite is prepared by comprising 50 parts epoxy resin, 62.5 parts zinc oxide thermally conductive filler, 6.94 parts boron nitride thermally conductive filler, 6.25 parts vanadium dioxide, 0.69 parts a third thermally conductive filler composite, and 12.5 parts a curing agent. The remaining implementation process is the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0064] Example 17: The epoxy resin composite is prepared by comprising 50 parts epoxy resin, 62.5 parts zinc oxide thermally conductive filler, 6.94 parts boron nitride thermally conductive filler, 4.9 parts vanadium dioxide, 1.04 parts a third thermally conductive filler composite, and 12.5 parts a curing agent. The remaining implementation process is the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0065] Example 18: An epoxy resin composite was prepared by comprising 50 parts epoxy resin, 56.25 parts magnesium oxide thermally conductive filler, 6.25 parts aluminum nitride thermally conductive filler, and 12.5 parts curing agent. The remaining process was the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0066] Example 19: The epoxy resin composite is prepared by comprising 50 parts epoxy resin, 62.5 parts magnesium oxide thermally conductive filler, 6.94 parts aluminum nitride thermally conductive filler, 6.94 parts a third thermally conductive filler composite, and 12.5 parts a curing agent. The remaining implementation process is the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0067] Example 20: An epoxy resin composite was prepared by comprising 50 parts epoxy resin, 62.5 parts magnesium oxide thermally conductive filler, 6.94 parts aluminum nitride thermally conductive filler, 6.54 parts vanadium dioxide, and 12.5 parts curing agent. The remaining implementation process was the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0068] Example 21: An epoxy resin composite was prepared by comprising 50 parts epoxy resin, 56.25 parts alumina thermally conductive filler, 6.25 parts aluminum nitride thermally conductive filler, and 12.5 parts curing agent. The remaining process was the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0069] Example 22: The epoxy resin composite is prepared by comprising 50 parts epoxy resin, 42.5 parts zinc oxide thermally conductive filler, 6.94 parts aluminum nitride thermally conductive filler, 5.9 parts vanadium dioxide, 1.04 parts a third thermally conductive filler composite, and 12.5 parts a curing agent. The remaining implementation process is the same as in Example 4 of this application. The parts mentioned in this example are by weight.

[0070] The epoxy resin composites prepared in Examples 4 to 22 were subjected to thermal conductivity tests, which were performed at 25°C using laser thermal conductivity measurement. Viscosity tests were performed at 25°C using a rotational rheometer. The test results are shown in Table 1.

[0071] Table 1

[0072] As can be seen from the data in Table 1, the epoxy resin composites prepared in Examples 4 to 22 have good thermal conductivity and low viscosity.

[0073] Finally, it should be understood that the embodiments disclosed herein are illustrative of the principles of the embodiments of this application. Other modified embodiments are also within the scope of this application. Therefore, the embodiments disclosed herein are merely examples and not limitations. Those skilled in the art can implement the applications in this application by adopting alternative configurations based on the embodiments in this application. Therefore, the embodiments of this application are not limited to those embodiments precisely described in the application.

Claims

1. An epoxy resin composite, characterized by, The epoxy resin composite is a cured product of an epoxy resin, a first thermal conductive filler, a second thermal conductive filler, a phase change material, and a third thermal conductive filler composite under the action of a curing agent, wherein the epoxy resin accounts for 30-50 parts by weight, the first thermal conductive filler accounts for 56-63 parts by weight, the second thermal conductive filler accounts for 6.2-6.5 parts by weight, the third thermal conductive filler composite accounts for 0-7 parts by weight, the phase change material accounts for 0-7 parts by weight, and the curing agent accounts for 7.5-12.5 parts by weight, wherein the first thermal conductive filler comprises at least one of aluminum oxide, zinc oxide, magnesium oxide, and beryllium oxide, the second thermal conductive filler comprises at least one of silicon carbide, boron carbide, boron nitride, and aluminum nitride, the phase change material comprises at least one of vanadium oxide, tungsten-doped vanadium oxide, titanium-doped vanadium oxide, and tungsten-titanium-doped vanadium oxide, and the third thermal conductive filler composite comprises a mesoporous material, an organosilicon phosphorus flame retardant, a silane coupling agent, and a liquid metal.

2. The epoxy resin composite according to claim 1, characterized in that In the third thermal conductive filler composite, the mesoporous material comprises at least one of mesoporous silicon dioxide, mesoporous aluminum oxide, mesoporous titanium oxide, and mesoporous zirconium oxide; the organosilicon phosphorus flame retardant comprises at least one of a polysiloxane type organosilicon phosphorus flame retardant, a POSS-based organosilicon phosphorus flame retardant, a DOPO derivative organosilicon phosphorus flame retardant, and a small molecule organosilicon phosphorus compound; the liquid metal comprises at least one of rubidium, gallium, a gallium-indium-tin alloy, a sodium-potassium alloy, a gallium-indium alloy, a bismuth-indium-tin alloy, and a gallium-indium-tin-zinc alloy; and the silane coupling agent comprises at least one of γ-aminopropyltriethoxysilane, N-β-aminoethyl-γ-aminopropyltrimethoxysilane, γ-glycidyl ether oxypropyltrimethoxysilane, vinyltriethoxysilane, and vinyltrimethoxysilane.

3. The epoxy resin composite of claim 1, wherein The epoxy resin comprises at least one of bisphenol A diglycidyl ether, bisphenol F type epoxy resin, polyphenol type glycidyl ether epoxy resin, and aliphatic glycidyl ether epoxy resin.

4. The epoxy resin composite of claim 1, wherein The curing agent is an amine curing agent or an acid anhydride curing agent.

5. The epoxy resin composite according to claim 4, characterized in that The curing agent comprises at least one of ethylenediamine, hexamethylenediamine, m-phenylenediamine, 4,4'-diaminodiphenyl methane, 4,4-diaminodiphenyl sulfone, maleic anhydride, and phthalic anhydride.

6. A method of preparing an epoxy resin composite, characterized by, Comprise: The epoxy resin, the first thermal conductive filler, the second thermal conductive filler, the phase change material and the third thermal conductive filler compound are mixed uniformly to form a first mixture, and a curing agent is added to the first mixture, and under the action of the curing agent, the components in the first mixture undergo a curing reaction to form a cured product, wherein the epoxy resin accounts for 30-50 parts, the first thermal conductive filler accounts for 56-63 parts, the second thermal conductive filler accounts for 6.2-6.5 parts, the third thermal conductive filler compound accounts for 0-7 parts, the phase change material accounts for 0-7 parts, and the curing agent accounts for 7.5-12.5 parts, wherein the first thermal conductive filler includes at least one of aluminum oxide, zinc oxide, magnesium oxide and beryllium oxide, the second thermal conductive filler includes at least one of silicon carbide, boron carbide, boron nitride and aluminum nitride, the phase change material includes at least one of vanadium oxide, tungsten-doped vanadium oxide, titanium-doped vanadium oxide and tungsten-titanium-doped vanadium oxide, and the third thermal conductive filler compound includes mesoporous material, organosilicon phosphorus flame retardant, silane coupling agent and liquid metal.

7. The method for preparing the epoxy resin composite according to claim 6, characterized in that, In the third thermal conductive filler compound, The mesoporous material includes at least one of mesoporous silica, mesoporous alumina, mesoporous titania and mesoporous zirconia; the organosilicon phosphorus flame retardant includes at least one of polysiloxane organosilicon phosphorus flame retardant, POSS-based organosilicon phosphorus flame retardant, DOPO derivative organosilicon phosphorus flame retardant and small-molecule organosilicon phosphorus compound; the liquid metal includes at least one of rubidium, gallium, gallium-indium-tin alloy, sodium-potassium alloy, gallium-indium alloy, bismuth-indium-tin alloy and gallium-indium-tin-zinc alloy; and the silane coupling agent includes at least one of γ-aminopropyl triethoxysilane, N-β-aminoethyl-γ-aminopropyl trimethoxysilane, γ-glycidyl ether propyl trimethoxysilane, vinyl triethoxysilane and vinyl trimethoxysilane.

8. The method for preparing the epoxy resin composite according to claim 6, characterized in that, The preparation method of the third thermal conductive filler compound includes: Drying to remove water molecules on the surface of the mesoporous material and in the pores of the mesoporous material, and exposing active sites in the mesoporous material; Forming a colloidal suspension of the mesoporous material in a first organic solvent, then adding the organosilicon phosphorus flame retardant to the colloidal suspension, and allowing the organosilicon phosphorus molecules in the organosilicon phosphorus flame retardant to hydrolyze and condense with the groups in the active sites on the surface of the mesoporous material to form a covalent bond compound, obtaining an organosilicon phosphorus functionalized mesoporous material hybrid flame retardant, denoted as SiP-J; Mixing the SiP-J with the liquid metal and embedding a part of the liquid metal in the pores of the SiP-J and forming a metal coating on the surface of the SiP-J under oil bath and ultrasonic conditions to form a mesoporous sphere, wherein the filling rate of the liquid metal in the pores of the mesoporous sphere is 60-80%; Pulverizing the mesoporous sphere to a set particle size and uniformity; Mixing the mesoporous sphere with the silane coupling agent to initiate a chemical grafting reaction on the surface of the mesoporous sphere, and forming the third thermal conductive filler compound.

9. The method for preparing the epoxy resin composite according to claim 8, characterized in that, The method further comprises: increasing the filling rate of the liquid metal in the channels of the mesoporous spheres to 80-95% by controlling the rotation speed and time of the ball mill before crushing the mesoporous spheres to a set particle size and uniformity.

10. The method for preparing the epoxy resin composite according to claim 8, characterized in that, In the third heat-conductive filler compound, the ratio of the weight of the mesoporous material to the sum of the weights of the organosilicon phosphorus flame retardant and the silane coupling agent ranges from 1:(0.02-3); and the molar ratio of the organosilicon phosphorus flame retardant to the silane coupling agent ranges from 1:(1-3).

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