Preparation method of high-thermal-conductivity epoxy resin composite material filled with core-shell structure filler

Abstract

The invention discloses a preparation method of a high-thermal-conductivity epoxy resin composite material filled with core-shell structure filler, and relates to the technical field of preparation of epoxy resin composite materials. The invention aims to solve the problems of low efficiency and discontinuity of construction of a heat conduction path in a traditional epoxy resin-based composite material. According to the invention, E51 epoxy resin is taken as a matrix, h-BN coated Al2O3 is taken as a filler and added into the matrix, the surface of a core layer h-BN is coated with shell layer Al2O3, and an Al2O3 thermal resistance transition layer is constructed at the interface of the h-BN and the epoxy resin, so that the interface thermal resistance between the filler and the epoxy resin is reduced, and the probability of mutual lap joint between the core-shell filler is greater than that of mutual lap joint of two-dimensional sheet-shaped h-BN; and a high-efficiency continuous heat conduction path can be constructed in the epoxy resin. The invention can obtain the preparation method of the high-thermal-conductivity epoxy resin composite material filled with the core-shell structure filler.

Description

Technical Field

[0001] The present invention relates to the technical field of preparing epoxy resin composites, and particularly relates to a method for preparing a highly thermally conductive epoxy resin composite filled with a core-shell structure filler. Background Art

[0002] Epoxy resin is widely used in power equipment such as dry-type transformers due to its excellent insulation performance, mechanical properties and thermal stability. However, researchers have found that the thermal conductivity of epoxy resin is relatively low, which makes the heat generated during the operation of dry-type transformers unable to be released quickly, and a large amount of heat accumulated inside the equipment seriously affects its stable operation. At present, the method of doping inorganic highly thermally conductive fillers is commonly used in engineering to improve the thermal conductivity of epoxy resin composites. However, the thermal resistance at the interface between epoxy resin and ordinary thermally conductive fillers varies greatly, and most of the fillers are dispersed in the epoxy matrix and cannot form a continuous thermal conduction path, which restricts the improvement of the thermal conductivity of epoxy resin composites.

[0003] Therefore, studying how to modify the fillers to achieve the preparation of highly thermally conductive epoxy resin-based composites has important practical significance for realizing the stable operation of dry-type transformers and conforming to the development trend of high voltage, large capacity and miniaturization. Summary of the Invention

[0004] The purpose of the present invention is to provide a method for preparing a highly thermally conductive epoxy resin composite filled with a core-shell structure filler to solve the problem of inefficient and discontinuous construction of thermal conduction paths in traditional epoxy resin-based composites.

[0005] A method for preparing a highly thermally conductive epoxy resin composite filled with a core-shell structure filler is carried out according to the following steps:

[0006] Step S1: Prepare a sodium aluminate solution:

[0007] Put Al(OH) 3 solid and NaOH solid into a reaction kettle with a polytetrafluoroethylene inner lining, then add deionized water into the reaction kettle, seal it and stir and heat it at a constant temperature to obtain a sodium aluminate solution;

[0008] Step S2: Prepare a boehmite sample:

[0009] Add aluminum sulfate octadecahydrate solid into deionized water, stir magnetically until the aluminum sulfate octadecahydrate solid is completely dissolved to obtain an aluminum sulfate octadecahydrate solution; while stirring, drop the sodium aluminate solution obtained in step S1 into the aluminum sulfate octadecahydrate solution, stop dropping the sodium aluminate solution until the pH value of the mixed solution remains stable, and then stir the liquid product until it is completely dissolved; then filter, wash and dry the mixed solution to obtain a boehmite sample;

[0010] Step S3: Prepare h-BN@Al 2 O 3 Composite filler:

[0011] Mix the boehmite sample obtained in Step S2 with the hexagonal boron nitride suspension, dry it after sufficient magnetic stirring, and finally calcine it to obtain h-BN@Al 2 O 3 Composite filler;

[0012] Step S4: Prepare a high thermal conductivity epoxy resin composite filled with core-shell structure fillers:

[0013] After fully mixing the epoxy resin with methylhexahydrophthalic anhydride, add the h-BN@Al 2 O 3 Composite filler, after ultrasonic dispersion, add 2,4,6-tris(dimethylaminomethyl)phenol to obtain a suspension; pour the suspension into a mold and perform gradient curing to obtain a high thermal conductivity epoxy resin composite filled with core-shell structure fillers;

[0014] The mass fraction of h-BN@Al 2 O 3 Composite filler in the high thermal conductivity epoxy resin composite filled with core-shell structure fillers is 10%, 15%, 20% or 25%.

[0015] Advantages of the present invention:

[0016] (1) For the preparation method of a high thermal conductivity epoxy resin composite filled with core-shell structure fillers of the present invention, using E51 epoxy resin as the matrix and adding h-BN@Al 2 O 3 as a filler, by coating the core layer h-BN with a shell layer of Al 2 O 3 , a thermal resistance transition layer of Al 2 O 3 is constructed at the interface between h-BN and the epoxy resin, reducing the interfacial thermal resistance between the filler and the epoxy resin. At the same time, the probability of mutual overlap between the prepared core-shell fillers is greater than that of two-dimensional flaky h-BN, which is conducive to constructing an efficient continuous heat conduction path in the epoxy resin, effectively solving the problem that the improvement of the thermal conductivity of the epoxy resin composite is not obvious due to the difficulty in constructing the heat conduction path.

[0017] (2) The epoxy resin composite prepared by the method of the present invention has a higher thermal conductivity compared to directly doping h-BN and Al 2 O 3The composite material has a significantly improved thermal conductivity and excellent dielectric properties, which provides a new idea for the development of epoxy resin composites with excellent thermal and dielectric properties and is of great significance for the development of dry-type transformers towards high voltage, large capacity and miniaturization.

[0018] The present invention can obtain a preparation method of a highly thermally conductive epoxy resin composite material filled with core-shell structure fillers. Brief Description of the Drawings

[0019] Figure 1 It represents the thermal conductivity values after different fillers are doped into the epoxy resin matrix at different filling amounts in the present invention;

[0020] Figure 2 It represents the dielectric spectroscopy diagrams of five groups of different epoxy resin materials in the present invention;

[0021] Figure 3 It represents the SEM image of untreated h-BN;

[0022] Figure 4 It represents the SEM image of the highly thermally conductive epoxy resin composite material filled with core-shell structure fillers in the present invention;

[0023] Figure 5 It represents the X-ray diffraction pattern of the highly thermally conductive epoxy resin composite material with different doping amounts of h-BN@Al 2 O 3 ; Detailed Description of the Invention

[0024] Detailed Description of the Invention One: A preparation method of a highly thermally conductive epoxy resin composite material filled with core-shell structure fillers in this embodiment is carried out according to the following steps:

[0025] Step S1: Prepare a sodium aluminate solution:

[0026] Put Al(OH) 3 solid and NaOH solid into a reaction kettle with a polytetrafluoroethylene inner lining, then add deionized water into the reaction kettle, seal it and stir and heat it at a constant temperature to obtain a sodium aluminate solution;

[0027] Step S2: Prepare a boehmite sample:

[0028] Add aluminum sulfate octadecahydrate solid into deionized water, stir magnetically until the aluminum sulfate octadecahydrate solid is completely dissolved to obtain an aluminum sulfate octadecahydrate solution; while stirring, drop the sodium aluminate solution obtained in Step S1 into the aluminum sulfate octadecahydrate solution, stop dropping the sodium aluminate solution when the pH value of the mixed solution remains stable, and then stir the liquid product until it is completely dissolved; then filter, wash and dry the mixed solution to obtain a boehmite sample;

[0029] Step S3: Prepare h-BN@Al 2 O 3 Composite filler:

[0030] Mix the boehmite sample obtained in Step S2 with the hexagonal boron nitride suspension, dry it after sufficient magnetic stirring, and finally calcine it to obtain h-BN@Al 2 O 3 Composite filler;

[0031] Step S4: Prepare a highly thermally conductive epoxy resin composite filled with core-shell structure fillers:

[0032] After thoroughly mixing the epoxy resin with methylhexahydrophthalic anhydride, add the h-BN@Al 2 O 3 Composite filler obtained in Step S3. After ultrasonic dispersion, add 2,4,6-tris(dimethylaminomethyl)phenol to obtain a suspension; pour the suspension into a mold and perform gradient curing to obtain a highly thermally conductive epoxy resin composite filled with core-shell structure fillers;

[0033] In the highly thermally conductive epoxy resin composite filled with the core-shell structure fillers, the mass fraction of the h-BN@Al 2 O 3 Composite filler is 10%, 15%, 20% or 25%.

[0034] Specific Embodiment 2: The difference between this embodiment and Specific Embodiment 1 is that the mass ratio of the solid Al(OH) 3 Solid, NaOH solid and deionized water is (2.5 - 5):(6.25 - 10):(15 - 20).

[0035] Other steps are the same as those in Specific Embodiment 1.

[0036] Specific Embodiment 3: The difference between this embodiment and Specific Embodiment 1 or 2 is that after sealing in Step S1, it is placed in a constant temperature oil bath pot and heated at a temperature of 120 - 140 °C for 1 - 2 h, and the stirring speed is 20 - 30 r / min.

[0037] Other steps are the same as those in Specific Embodiment 1 or 2.

[0038] Specific Embodiment 4: The difference between this embodiment and one of Specific Embodiments 1 to 3 is that the mass ratio of the aluminum sulfate octadecahydrate solid to deionized water in Step S2 is 1:(3 - 4), and the pH value is 4 - 7.

[0039] Other steps are the same as those in Specific Embodiments 1 to 3.

[0040] Specific Embodiment 5: The difference between this embodiment and any one of Specific Embodiments 1 to 4 is that in step S2, the drying is carried out in an oven at 80-100°C for 10-12 hours.

[0041] Other steps are the same as those in Specific Embodiments 1 to 4.

[0042] Specific Embodiment 6: The difference between this embodiment and any one of Specific Embodiments 1 to 5 is that in step S3, the mass ratio of the boehmite sample to boron nitride in the boron nitride suspension is 1:(2-4), and the particle size of the boron nitride is 5-10 μm.

[0043] Other steps are the same as those in Specific Embodiments 1 to 5.

[0044] Specific Embodiment 7: The difference between this embodiment and any one of Specific Embodiments 1 to 6 is that in step S3, it is stirred at a temperature of 70-90°C for 6-8 hours, and then dried at 80-100°C for 6-12 hours.

[0045] Other steps are the same as those in Specific Embodiments 1 to 6.

[0046] Specific Embodiment 8: The difference between this embodiment and any one of Specific Embodiments 1 to 7 is that in step S3, the calcination is carried out at a temperature of 1000-1200°C for 2-3 hours, and the heating rate is 2-4°C / min.

[0047] Other steps are the same as those in Specific Embodiments 1 to 7.

[0048] Specific Embodiment 9: The difference between this embodiment and any one of Specific Embodiments 1 to 8 is that in step S4, the mass ratio of the epoxy resin, methylhexahydrophthalic anhydride, and 2,4,6-tris(dimethylaminomethyl)phenol is 10:(8-8.5):0.03; the mixing time of the epoxy resin and methylhexahydrophthalic anhydride is 20-30 minutes, and the ultrasonic dispersion time is 0.5-2 hours.

[0049] Other steps are the same as those in Specific Embodiments 1 to 8.

[0050] Specific Embodiment 10: The difference between this embodiment and any one of Specific Embodiments 1 to 9 is that in step S4, the gradient curing is to first heat up to 70-80°C and cure at 70-80°C for 1-2 hours; then heat up to 90-100°C and continue to cure at 90-100°C for 1-2 hours; then heat up to 110-120°C and continue to cure at 110-120°C for 3-4 hours.

[0051] Other steps are the same as those in Specific Embodiments 1 to 9.

[0052] The beneficial effects of the present invention are verified by the following examples:

[0053] Example 1: A preparation method of a highly thermally conductive epoxy resin composite filled with a core-shell structure filler is carried out according to the following steps:

[0054] Step S1: Prepare a sodium aluminate solution:

[0055] Put 2.5 g of solid Al(OH) 3 and 6.25 g of solid NaOH into a reaction kettle with a PTFE inner lining, then add 15 g of deionized water into the reaction kettle. After sealing, place it in a constant temperature oil bath, and stir and heat it at a constant temperature at 140 °C and a rotation speed of 30 r / min for 2 h to obtain a sodium aluminate solution. Take it out and cool it for standby;

[0056] The thickness of the reaction kettle is 1 mm, and the diameter is 5 cm;

[0057] Step S2: Prepare a boehmite sample:

[0058] Add 33 g of aluminum sulfate octadecahydrate solid into a beaker, and add 100 g of deionized water. Place the beaker on a magnetic stirring device and stir magnetically until the aluminum sulfate octadecahydrate solid is completely dissolved to obtain an aluminum sulfate octadecahydrate solution; while stirring, use a separatory funnel to drop the sodium aluminate solution obtained in step S1 into the aluminum sulfate octadecahydrate solution until the pH value of the mixed solution is 4 and remains stable, then stop dropping the sodium aluminate solution, and stir the liquid product until it is completely dissolved; then filter and wash the mixed solution, place it in an oven, and dry it at 80 °C for 12 h to obtain a boehmite sample;

[0059] Step S3: Prepare h-BN@Al 2 O 3 composite filler:

[0060] Mix 1 g of the boehmite sample obtained in step S2 with a hexagonal boron nitride (h-BN) suspension (the mass of hexagonal boron nitride is 4 g, and the particle size is 10 μm), stir on a magnetic stirrer at a temperature of 70 °C for 8 h, then dry it at 100 °C for 12 h. Finally, put the dried powder into an alumina crucible, and then put it into a muffle furnace, heat it at a rate of 4 °C / min to 1200 °C, and calcine it at 1200 °C for 3 h to obtain h-BN@Al 2 O 3 composite filler;

[0061] Step S4: Prepare a highly thermally conductive epoxy resin composite filled with a core-shell structure filler:

[0062] Put 10 g of E51 epoxy resin (EP) into an oven preheated to 60 °C and preheat for 30 min. Then add 8.5 g of methylhexahydrophthalic anhydride (MHHPA), and use a powerful stirrer to stir for 30 min at 60 °C. After that, add the h-BN@Al 2 O 3 composite filler. After ultrasonic dispersion for 2 h, then use a syringe to drop 0.03 g of 2,4,6-tris(dimethylaminomethyl)phenol to obtain a suspension; pour the suspension into a mold, first heat up to 80 °C and cure for 2 h at 80 °C; then heat up to 100 °C and continue to cure for 2 h at 100 °C; then heat up to 120 °C and continue to cure for 4 h at 120 °C to finally obtain the h-BN@Al 2 O 3 / EP high thermal conductivity epoxy resin material.

[0063] In the high thermal conductivity epoxy resin composite filled with the core-shell structure filler, the mass fraction of the h-BN@Al 2 O 3 composite filler is 10%. It was measured that the thermal conductivity of the composite material obtained under the conditions of this example is shown in Table 1.

[0064] Table 1: Thermal conductivity of the composite material added with 10% h-BN@Al 2 O 3 composite filler;

[0065] Filler mass fraction Filler type Thermal conductivity λ (W / (m·K)) h-BN 0.367 10％ <![CDATA[h-BN&Al 2 O 3 > 0.38 <![CDATA[h-BN@Al 2 O 3 > 0.443

[0066] Example 2:

[0067] In this example, the mass fraction of the added h-BN@Al 2 O 3 composite filler is 15%, and all other experimental conditions are the same as those in Example 1. It was measured that the thermal conductivity of the composite material obtained under the conditions of this example is shown in Table 2.

[0068] Table 2: Thermal conductivity of the composite material added with 15% h-BN@Al 2 O 3 composite filler;

[0069] Filler mass fraction Filler type Thermal conductivity λ (W / (m·K)) h-BN 0.452 15％ <![CDATA[h-BN&Al 2 O 3 > 0.523 <![CDATA[h-BN@Al 2 O 3 > 0.585

[0070] Example 3:

[0071] In this example, the mass fraction of the added h-BN@Al 2 O 3 composite filler is 20%, and all other experimental conditions are the same as those in Example 1. It was measured that the thermal conductivity of the composite material obtained under the conditions of this example is shown in Table 3.

[0072] Table 3: Thermal conductivity of the composite material with 20% h-BN@Al 2 O 3 composite filler;

[0073] Filler mass fraction Filler type Thermal conductivity λ (W / (m·K)) h-BN 0.518 20％ <![CDATA[h-BN&Al 2 O 3 > 0.824 <![CDATA[h-BN@Al 2 O 3 > 0.917

[0074] Example 4:

[0075] In this example, the mass fraction of h-BN@Al 2 O 3 composite filler added is 25%, and other experimental conditions are the same as those in Example 1. After measurement, the thermal conductivity of the composite material obtained under the conditions of this example is shown in Table 4.

[0076] Table 4: Thermal conductivity of the composite material with 25% h-BN@Al 2 O 3 composite filler;

[0077] Filler mass fraction Filler type Thermal conductivity λ (W / (m·K)) h-BN 0.53 25％ <![CDATA[h-BN&Al 2 O 3 > 0.934 <![CDATA[h-BN@Al 2 O 3 > 0.985

[0078] Comparative Example 1:

[0079] (1) Put 10 g of E51 epoxy resin into an oven preheated to 60 °C for 30 min, then add 8.5 g of MHHPA to it and stir the mixture with a force-increasing stirrer at 60 °C for 30 min. After that, add h-BN with different mass fractions to the mixture and ultrasonically disperse it for 2 h. Keeping the above conditions unchanged, slowly drop 0.03 g of DMP-30 into the mixture with a syringe to obtain a suspension;

[0080] (2) Pour the obtained suspension into a mold with a thickness of 1 mm and a diameter of 5 cm;

[0081] (3) Place the mold in a forced-air oven and cure the epoxy resin by gradient heating. The curing conditions are 80 °C for 2 h, 100 °C for 2 h, and 120 °C for 4 h to finally obtain h-BN / EP composite material.

[0082] After measurement, the thermal conductivity of the h-BN / EP composite material obtained under the conditions of this comparative example is lower than that under the core-shell structure composite filler.

[0083] Comparative Example 2:

[0084] (1) Put 10 g of E51 epoxy resin into an oven preheated to 60 °C for 30 min, then add 8.5 g of MHHPA to it and stir the mixture with a force-increasing stirrer at 60 °C for 30 min. After that, add h-BN&Al with different mass fractions to the mixture 2 O 3Mix the composite fillers and disperse them ultrasonically for 2 h. Keeping the above conditions unchanged, slowly drip 0.03 g of DMP-30 into the mixture with a syringe to obtain a suspension;

[0085] (2) Pour the obtained suspension into a mold with a thickness of 1 mm and a diameter of 5 cm;

[0086] (3) Place the mold in a forced-air oven and cure the epoxy resin by gradient heating. The curing conditions are curing at 80 °C for 2 h, 100 °C for 2 h, and 120 °C for 4 h, and finally obtain the h-BN&Al 2 O 3 / EP composite material.

[0087] Figure 1 represents the thermal conductivity values of the epoxy resin matrix doped with different fillers in different filling amounts in the present invention; as Figure 1 shown, with the increase of the filler content, the thermal conductivities of all kinds of epoxy resin composites have been significantly improved. The difference is that the epoxy resin composite doped with h-BN@Al 2 O 3 has a more obvious improvement in the thermal conductivity effect compared with the composite material directly doped with h-BN and Al 2 O 3 . Among them, when 25% of h-BN@Al 2 O 3 is added, the thermal conductivity of the epoxy resin composite reaches 0.985 W / (m·K).

[0088] Figure 2 represents the dielectric spectroscopy diagrams of five groups of different epoxy resin materials in the present invention; as Figure 2 shown, the relative dielectric constants of all samples show a downward trend with the increase of the frequency, which is mainly due to the fact that with the increase of the external electric field frequency, the dipole rotation polarization inside the material gradually cannot keep up with the change of the external electric field. After introducing h-BN@Al 2 O 3 , due to the relatively large dielectric constant of Al 2 O 3 itself, the dielectric constant of the epoxy resin composite has increased significantly; however, the introduction of h-BN@Al 2 O 3 limits the rotation of the dipoles of the epoxy resin, and the relaxation polarization decreases, so the loss factor decreases significantly and is relatively stable with the change of frequency.

[0089] Figure 3 represents the SEM image of untreated h-BN; as Figure 3 shown, h-BN presents a two-dimensional flaky structure with a particle size of about 10 μm, and the surface is smooth and the thickness is uniform.

[0090] Figure 4 SEM images of the highly thermally conductive epoxy resin composite filled with the core-shell structure filler of the present invention; as Figure 4 shown, after h-BN was coated with Al 2 O 3 , the morphology changed significantly, the particle size increased, and it was no longer the obvious two-dimensional flake structure as before. Obvious wrinkles appeared on the surface, and a layer of Al 2 O 3 .

[0091] Figure 5 X-ray diffraction patterns of the highly thermally conductive epoxy resin composites with different doping amounts of h-BN@Al 2 O 3 ; as Figure 5 shown, the diffraction peaks of Al 2 O 3 can be observed, proving the successful preparation of h-BN@Al 2 O 3 .

Claims

1. A method for preparing a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler, characterized in that The preparation method is carried out according to the following steps: Step S1, preparing sodium aluminate solution: Al(OH)3 solid and NaOH solid are placed in a polytetrafluoroethylene-lined reactor, deionized water is added to the reactor, and the reactor is sealed, stirred and heated at a constant temperature to obtain a sodium aluminate solution; Step S2, preparing boehmite sample: Adding aluminum sulfate 18hydrate solid to deionized water, and stirring with a magnetic force until the aluminum sulfate 18hydrate solid is completely dissolved, to obtain an aluminum sulfate 18hydrate solution; while stirring, dropwise adding the sodium aluminate solution obtained in step S1 to the aluminum sulfate 18hydrate solution, until the pH value of the mixed solution is stable, stopping the dropwise addition of the sodium aluminate solution, and stirring the liquid product until it is completely dissolved; Then the mixed solution is filtered, washed and dried to obtain a boehmite sample; Step S3, preparing h-BN@Al2O3 composite filler: The boehmite sample obtained in step S2 is mixed with the hexagonal boron nitride suspension, fully magnetically stirred and then dried, and finally calcined to obtain a h-BN@Al2O3 composite filler; Step S4, preparing a high thermal conductivity epoxy resin composite material filled with core-shell structure fillers: After the epoxy resin and methyl hexahydrophthalic anhydride are fully mixed, the h-BN@Al2O3 composite filler obtained in step S3 is added, and after ultrasonic dispersion, 2,4,6-tris(dimethylaminomethyl)phenol is added to obtain a suspension; the suspension is poured into a mold and gradient cured to obtain a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler; The mass fraction of the h-BN@Al2O3 composite filler in the high thermal conductivity epoxy resin composite material filled with the core-shell structure filler is 10%, 15%, 20% or 25%.

2. The method for preparing a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler according to claim 1, characterized in that The mass ratio of Al(OH)3 solid, NaOH solid and deionized water described in step S1 is (2.5-5):(6.25-10):(15-20).

3. The method for preparing a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler according to claim 1, characterized in that After being sealed in step S1, the mixture is placed in a constant temperature oil bath and heated at 120-140° C. for 1-2 hours with a stirring speed of 20-30 r / min.

4. The method for preparing a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler according to claim 1, characterized in that The mass ratio of the aluminum sulfate 18hydrate solid to deionized water in step S2 is 1:(3-4), and the pH value is 4-7.

5. The method for preparing a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler according to claim 1, characterized in that The drying in step S2 is performed by placing the product in an oven at 80 to 100° C. for 10 to 12 hours.

6. The method for preparing a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler according to claim 1, characterized in that The mass ratio of the boehmite sample in step S3 to the hexagonal boron nitride in the hexagonal boron nitride suspension is 1:(2-4), and the particle size of the hexagonal boron nitride is 5-10 μm.

7. The method for preparing a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler according to claim 1, characterized in that In step S3, the mixture is stirred at a temperature of 70 to 90° C. for 6 to 8 hours, and then dried at 80 to 100° C. for 6 to 12 hours.

8. The method for preparing a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler according to claim 1, characterized in that The calcination in step S3 is carried out at a temperature of 1000-1200° C. for 2-3 hours, and the heating rate is 2-4° C. / min.

9. The method for preparing a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler according to claim 1, characterized in that The mass ratio of the epoxy resin, methylhexahydrophthalic anhydride and 2,4,6-tris(dimethylaminomethyl)phenol described in step S4 is 10:(8-8.5):0.03; the mixing time of the epoxy resin and methylhexahydrophthalic anhydride is 20-30 minutes, and the ultrasonic dispersion time is 0.5-2 hours.

10. The method for preparing a high thermal conductivity epoxy resin composite material filled with a core-shell structure filler according to claim 1, characterized in that In step S4, the gradient curing is firstly heated to 70-80°C and cured at 70-80°C for 1-2h; then heated to 90-100°C and continued to cure at 90-100°C for 1-2h; then heated to 110-120°C and continued to cure at 110-120°C for 3-4h.

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