A pitch-based carbon fiber composite material with interfacial thermal conductivity and its preparation method and application

Abstract

The present invention relates to an asphalt-based carbon fiber composite material with interfacial thermal conductivity, a preparation method and an application thereof, which solves the technical problem of unsatisfactory thermal conductivity of materials in the prior art. The composite material is radially arranged from the inside to the outside in the order of asphalt-based carbon fiber, an inner layer of aromatic condensed ring molecules, a graphene middle layer and an outer layer of aromatic condensed ring molecules. The graphene middle layer contains graphene, which is dispersed on the surface of the asphalt-based carbon fiber and forms the graphene middle layer through the π-π conjugation between the aromatic condensed ring molecules and the graphene. The aromatic condensed ring molecules have amino groups at the end of NH3 + The hydrogen bonds between the atoms act on the graphene surface to form an outer layer of aromatic condensed ring molecules. The material prepared by the present invention can be used in the fields of aerospace structural function integration and electronic and electrical materials.

Description

Technical Field

[0001] The present invention relates to a composite material, a preparation method and an application thereof, and in particular to an asphalt-based carbon fiber composite material with interface thermal conductivity, a preparation method and an application thereof. Background Art

[0002] The highly oriented structure formed by the large graphite crystallites on the surface of pitch-based carbon fibers imparts excellent thermal conductivity, but also makes the surface chemically inert, resulting in poor interfacial wettability and compatibility with the resin matrix. This easily creates a large number of micropores at the resin-fiber interface. This not only affects stress transfer within the composite, but the presence of micropores also increases the likelihood of carrier phonon scattering, thereby increasing interfacial thermal resistance and reducing the composite's thermal conductivity. To improve the thermal conductivity of composites, thermally conductive particles are often added to the resin matrix to create a thermal pathway. A paper (Polymer Testing, 2015, 45:132-138) reported the addition of graphene nanosheets to CBT resin, effectively improving both the in-plane and out-of-plane thermal conductivity of pitch-based carbon fiber composites. However, the addition of nanofillers also introduces interfacial thermal resistance between the filler and the resin matrix. Excessive filler can cause agglomeration, resulting in larger defects at the cross-section between the resin matrix and the pitch-based carbon fibers. Therefore, surface modification of pitch-based carbon fibers to construct a thermally conductive network is an effective approach to reducing interfacial thermal resistance and improving interfacial thermal conductivity in composites.

[0003] The surface modification of pitch-based carbon fibers is mainly divided into covalent modification by plasma treatment and oxidation treatment and non-covalent modification represented by molecular assembly. Covalent modification requires surface functionalization of the fiber. The Chinese patent (CN111979757A) obtains surface carboxylation of pitch-based carbon fibers by nitric acid treatment, and then grafts dopamine and polyetheramine on the surface of the pitch-based carbon fibers by covalent action, effectively improving the interface strength of the pitch-based carbon fiber / resin composite material. However, the acidification treatment of the pitch-based carbon fibers in advance will destroy the graphite structure on the fiber surface, which will cause a decrease in thermal conductivity. Non-covalent modification is represented by aromatic condensed ring molecules. The literature (Composites Part A: Applied Science and Manufacturing, 2016, 87: 212-219) introduces hydroxyl-containing aromatic condensed ring molecules on the surface of pitch-based carbon fibers through non-covalent bonding such as π-π stacking and hydrogen bonding. Under the premise of not damaging the graphite microcrystalline structure of the pitch-based carbon fibers, its surface activity is improved, effectively improving the interface bonding between the fiber and the resin. However, the low thermal conductivity of polymer as the interface layer limits the improvement of the interface thermal conductivity of asphalt-based carbon fiber composites.

[0004] The Chinese patent application with publication number CN109851999A impregnates carbon fibers with a carbon nanomaterial / aromatic condensed ring assembly liquid. The carbon nanomaterial and aromatic condensed ring molecules form an interface assembly transition layer on the fiber surface through a π-π stacking effect, thereby improving the wetting performance with the resin matrix and ultimately improving the interface bonding strength of the composite material.

[0005] However, this method has the following problems: (1) the carbon fiber graphite structure used is irregular and the thermal conductivity is not high; (2) the carbon nanomaterials and aromatic condensed ring molecules in the molecular assembly liquid are assembled due to π-π conjugation, which easily agglomerates on the carbon fiber surface, thereby affecting the interface bonding. At the same time, the gaps between the aggregated particles will destroy the integrity of the thermal conduction path, limiting the improvement of the thermal conductivity of the composite material. Summary of the Invention

[0006] The present invention aims to solve the technical problem of unsatisfactory thermal conductivity of materials in the prior art, and to provide an asphalt-based carbon fiber composite material with good interface thermal conductivity, as well as its preparation method and application.

[0007] To this end, the present invention provides an interfacial thermally conductive asphalt-based carbon fiber composite material, wherein the composite material is radially arranged from the inside to the outside in sequence asphalt-based carbon fiber, an inner layer of aromatic condensed ring molecules, a graphene middle layer, and an outer layer of aromatic condensed ring molecules, wherein the graphene middle layer contains graphene, which is dispersed on the surface of the asphalt-based carbon fiber and forms a graphene middle layer through the π-π conjugation of aromatic condensed ring molecules and graphene, and finally the pH value is adjusted to adjust the end amino group -NH3 of the aromatic condensed ring molecules. + The hydrogen bonds between the atoms form an outer layer of aromatic fused ring molecules on the graphene surface.

[0008] Preferably, the aromatic fused ring molecule is prepared from an aromatic dianhydride and an organic diamine; the aromatic dianhydride is one or a combination of pyromellitic dianhydride, biphenyltetracarboxylic dianhydride, 1,4,5,8-naphthalenetetracarboxylic dianhydride, and 3,4,9,10-perylenetetracarboxylic dianhydride; the organic diamine is one or a combination of aliphatic diamine, aromatic diamine, and alicyclic diamine.

[0009] The present invention also provides a method for preparing an asphalt-based carbon fiber composite material with interfacial thermal conductivity, which comprises the following steps: (1) preparing an aromatic condensed ring molecule: dissolving an aromatic dibasic anhydride and an organic diamine in a polar solvent to which a catalyst is added, reacting at 150 to 180° C. for 9 to 15 hours, washing, filtering, and drying to obtain an amino-terminated aromatic condensed ring molecule powder, wherein the molar ratio of the aromatic dibasic anhydride to the organic diamine is 1:(2 to 4), and the mass fraction of the catalyst is 0.1 to 0.2 wt% of the aromatic dibasic anhydride; (2) constructing an asphalt-based carbon fiber. The inner layer of aromatic condensed ring molecules on the surface: the aromatic condensed ring molecule powder obtained in the step (1) is dissolved in a polar solvent, ultrasonically dispersed, and a suspension solution with a concentration of 10 to 20 mg / ml is prepared. The unsized asphalt-based carbon fiber is reacted in the suspension solution at 150 to 180°C for 18 to 24 hours, and vacuum dried to obtain an asphalt-based carbon fiber with an aromatic condensed ring molecule assembly layer, wherein the mass fraction of the aromatic condensed ring molecule inner layer is 0.5 to 2 wt% of the unsized asphalt-based carbon fiber; (3) constructing a graphene intermediate layer on the surface of the asphalt-based carbon fiber: the peeled and layered graphene is dissolved in a polar solvent. The asphalt-based carbon fibers are immersed in a polar solvent of a dispersant and ultrasonically treated for 3 to 7 hours to obtain a graphene dispersion. Finally, the asphalt-based carbon fibers obtained in the step (2) are immersed in the graphene dispersion for 15 to 24 hours and vacuum-dried to obtain asphalt-based carbon fibers with secondary surface assembly, wherein the total mass fraction of the assembly layer after secondary assembly is 2 to 3 wt% of the unsized asphalt-based carbon fibers in the step (1); (4) constructing an outer layer of aromatic condensed ring molecules on the surface of the asphalt-based carbon fibers: dissolving the powder obtained in the step (1) in a polar solvent and ultrasonically dispersing the powder to a concentration of 1 to 5 mg / m l suspension, adding alkaline solution to control the pH value to 7-9, placing the asphalt-based carbon fiber obtained in the step (3) in the suspension to react for 6-12 hours, and after vacuum drying, finally obtaining asphalt-based carbon fiber with three-times surface assembly, wherein the total mass fraction of the assembled layer after three times assembly is 2.5-4wt% of the unsized asphalt-based carbon fiber in the step (1); (5) Preparation of interface thermal conductive composite material: compounding the asphalt-based carbon fiber obtained in the step (4) with a resin system, curing and heating, to obtain an asphalt-based carbon fiber composite material with good interface thermal conductivity.

[0010] Preferably, the polar solvent in steps (1) to (4) is a combination of one or more of N,N-dimethylformamide, N-methylpyrrolidone, dimethyl sulfoxide, formamide, methanol, and ethanol.

[0011] Preferably, the exfoliated and layered graphene in step (3) is graphene obtained after high-temperature carbonization treatment, cell disruption and freeze-drying treatment, wherein the number of graphene layers is 5 to 10.

[0012] Preferably, the alkaline solution in step (4) is a combination of one or more of triethylamine, sodium hydroxide and potassium hydroxide.

[0013] Preferably, the resin system in step (5) is one of epoxy resin, phenolic resin, bismaleimide, and cyanate resin.

[0014] The present invention also provides an application of an interfacial thermally conductive asphalt-based carbon fiber composite material in aerospace structural and functional integrated materials, such as satellite radiators, hypersonic aircraft, etc.

[0015] The present invention also provides an application of an interfacial thermally conductive asphalt-based carbon fiber composite material in electronic and electrical materials, such as a heat conducting sheet of a mobile phone, a heat dissipation part of an integrated circuit, and the like.

[0016] The present invention has the following beneficial effects:

[0017] 1. The present invention constructs an aromatic fused ring / graphene alternating assembly layer structure through the design of molecular coplanar conjugated structure, and realizes the surface three-dimensional assembly of asphalt-based carbon fiber. First, the inner assembly layer of aromatic fused ring molecules is constructed on the surface of asphalt-based carbon fiber, which is conducive to the dispersion of graphene on the fiber surface, and the graphene middle layer is formed through the π-π conjugation between the fused rings. Finally, the terminal amino group -NH3 is regulated by pH value. + The inter-hydrogen bonds form the outer assembly layer of the aromatic fused ring molecules.

[0018] 2. The present invention non-covalently modifies asphalt-based carbon fibers through aromatic condensed ring molecules, which effectively improves the surface activity of the fibers without damaging their graphite structure, and is more conducive to the adsorption and dispersion of graphene molecules. At the same time, the outer layer of aromatic condensed ring molecules can effectively improve the wettability with the resin matrix, thereby achieving good interface bonding between the fibers and the resin matrix.

[0019] 3. The alternating assembly layer structure of aromatic fused ring molecules / graphene of the present invention can maintain the integrity of the graphene structure, which helps to improve its thermal conductivity. At the same time, it constructs a thermal conductive network structure, reduces the possibility of carrier phonon scattering, reduces the interfacial thermal resistance between the fiber and the resin matrix, and realizes the effective transfer of heat in the interfacial phase, thereby improving the thermal conductivity of the composite material. BRIEF DESCRIPTION OF THE DRAWINGS

[0020] Figure 1 This is a process diagram for constructing alternating assembly layers of aromatic condensed ring molecules / graphene on the surface of pitch-based carbon fibers in the present invention;

[0021] Figure 2A 、 Figure 2B 、 Figure 2C This is the SEM image of the surface morphology of asphalt-based carbon fiber after alternating assembly of PDI / graphene / PDI; Figure 2AThe surface of asphalt-based carbon fiber after PDI assembly, Figure 2B The surface of asphalt-based carbon fiber after PDI and graphene assembly, Figure 2C The surface of pitch-based carbon fiber after PDI / graphene / PDI assembly;

[0022] Figure 3 is the transverse fiber bundle tensile strength of the bundled fiber composite;

[0023] Figure 4 is the thermal conductivity in the thickness direction of the unidirectional composite material. DETAILED DESCRIPTION

[0024] The present invention will be further described below with reference to the embodiments.

[0025] Example 1

[0026] (1) Design and preparation of aromatic fused ring molecules: 3,4,9,10-perylenetetracarboxylic dianhydride and octanediamine were added to N,N-dimethylformamide solvent containing triethylamine catalyst at a molar ratio of 1:4, reacted at 180°C for 9 h, washed and dried to obtain amino-terminated perylene imide powder. The amount of triethylamine used was 0.2 wt% relative to the mass of the dianhydride.

[0027] (2) Construction of the inner layer of aromatic condensed ring molecules on the surface of pitch-based carbon fibers: Perylene imide powder was dissolved in N,N-dimethylformamide and ultrasonically dispersed to prepare a suspension with a concentration of 20 mg / ml. Unsized pitch-based carbon fibers were reacted in the suspension at 180°C for 18 h and vacuum dried to obtain modified pitch-based carbon fibers.

[0028] (3) Construction of a graphene intermediate layer on the surface of asphalt-based carbon fiber: The graphene after peeling and delamination is dispersed in an N,N-dimethylformamide solvent with polyvinyl pyrrolidone added, and after ultrasonic treatment for 7 hours, the asphalt-based carbon fiber modified in step (2) is immersed in the graphene dispersion for 24 hours, and vacuum dried to obtain the asphalt-based carbon fiber with secondary surface assembly;

[0029] (4) Construction of the outer layer of aromatic condensed ring molecules on the surface of asphalt-based carbon fibers: Perylene imide powder was dissolved in N,N-dimethylformamide, and ultrasonic dispersion was performed to prepare a suspension with a concentration of 5 mg / ml. NaOH solution was added to adjust the pH value to 9. The asphalt-based carbon fibers after secondary surface assembly were reacted in the solution for 6 h. After vacuum drying, asphalt-based carbon fibers with alternating perylene imide / graphene assembly layers on the surface were finally obtained.

[0030] (5) Preparation of interfacial thermally conductive composite materials: Pitch-based carbon fibers containing an alternating perylene imide / graphene assembly structure were compounded with an epoxy resin system and heated to a curing temperature to obtain an asphalt-based carbon fiber composite material with both good interfacial bonding and thermal conductivity. According to the transverse fiber bundle tensile strength test, the transverse fiber bundle tensile strength of the bundled composite material was 26.72 MPa. According to the laser flash test, the thermal conductivity of the unidirectional composite material in the thickness direction was 2.59 W / m·K.

[0031] Example 2

[0032] (1) Design and preparation of aromatic fused ring molecules: 1,4,5,8-naphthalenetetracarboxylic dianhydride and decanediamine were added to an ethanol solvent containing a triethylamine catalyst at a molar ratio of 1:2, reacted at 150°C for 15 h, washed and dried to obtain amino-terminated naphthalimide powder. The amount of triethylamine used was 0.1 wt% relative to the mass of the dianhydride.

[0033] (2) Construction of the inner layer of aromatic fused ring molecules on the surface of pitch-based carbon fibers: Naphthalimide powder was dissolved in ethanol solvent and ultrasonically dispersed to prepare a suspension with a concentration of 10 mg / ml. Unsized pitch-based carbon fibers were reacted in the suspension at 150°C for 24 h and vacuum dried to obtain modified pitch-based carbon fibers.

[0034] (3) Construction of a graphene intermediate layer on the surface of asphalt-based carbon fiber: The graphene after peeling and delamination is dispersed in an ethanol solvent with polyvinyl pyrrolidone added, and after ultrasonic treatment for 3 hours, the asphalt-based carbon fiber modified in step (2) is immersed in the graphene dispersion for 15 hours, and vacuum dried to obtain the asphalt-based carbon fiber with secondary surface assembly;

[0035] (4) Construction of the outer layer of aromatic condensed ring molecules on the surface of pitch-based carbon fibers: Naphthalimide powder was dissolved in ethanol solvent and ultrasonically dispersed to prepare a suspension with a concentration of 1 mg / ml. KOH solution was added to adjust the pH value to 7. The pitch-based carbon fibers after secondary surface assembly were reacted in the solution for 12 h. After vacuum drying, pitch-based carbon fibers with alternating naphthalimide / graphene assembly layers on the surface were finally obtained.

[0036] (5) Preparation of interfacial thermally conductive composite materials: Pitch-based carbon fibers containing an alternating naphthaleneimide / graphene assembly structure were compounded with a bismaleimide resin system and heated to a curing temperature to obtain an asphalt-based carbon fiber composite material with both good interfacial bonding and thermal conductivity. According to the transverse fiber bundle tensile strength test, the transverse fiber bundle tensile strength of the bundled composite material was 23.42 MPa. According to the laser flash test, the thermal conductivity of the unidirectional composite material in the thickness direction was 2.08 W / m·K.

[0037] Example 3

[0038] (1) Design and preparation of aromatic fused ring molecules: Pyromellitic dianhydride and p-phenylenediamine were added to N-methylpyrrolidone solvent containing triethylamine catalyst at a molar ratio of 1:3, reacted at 170°C for 12 h, washed and dried to obtain amino-terminated pyromellitic imide powder. The amount of triethylamine used was 0.15% relative to the mass of the dianhydride.

[0039] (2) Construction of the inner layer of aromatic fused ring molecules on the surface of pitch-based carbon fibers: phthalimide powder was dissolved in N-methylpyrrolidone solvent, and a suspension with a concentration of 15 mg / ml was prepared by ultrasonic dispersion. Unsized pitch-based carbon fibers were reacted in the suspension at 170°C for 21 h, and vacuum dried to obtain modified pitch-based carbon fibers.

[0040] (3) Construction of graphene intermediate layer on the surface of asphalt-based carbon fiber: The graphene after peeling and delamination is dispersed in N-methylpyrrolidone solvent with polyvinylpyrrolidone added, and after ultrasonic treatment for 5 hours, the asphalt-based carbon fiber modified in step (2) is immersed in the graphene dispersion for 21 hours, and vacuum dried to obtain the asphalt-based carbon fiber with secondary surface assembly;

[0041] (4) Construction of the outer layer of aromatic condensed ring molecules on the surface of asphalt-based carbon fibers: dissolve phthalimide powder in N-methylpyrrolidone solvent, ultrasonically disperse and prepare a suspension with a concentration of 3 mg / ml, add triethylamine solution to adjust the pH value to 8, and react the asphalt-based carbon fibers after secondary surface assembly in the solution for 9 h. After vacuum drying, asphalt-based carbon fibers with alternating phthalimide / graphene assembly layers on the surface are finally obtained;

[0042] (5) Preparation of an interfacial thermally conductive composite material: Pitch-based carbon fibers containing an alternating phthalimide / graphene assembly structure were compounded with a cyanate ester resin system and heated to a curing temperature to obtain an asphalt-based carbon fiber composite material with both good interfacial bonding and thermal conductivity. According to a transverse fiber bundle tensile strength test, the transverse fiber bundle tensile strength of the bundled composite material was 20.56 MPa. According to a laser flash test, the thermal conductivity of the unidirectional composite material in the thickness direction was 1.88 W / m·K.

[0043] Comparative Example 1

[0044] Unsized pitch-based carbon fibers were compounded with an epoxy resin system and heated to a curing temperature to produce a unidirectional pitch-based carbon fiber composite. Transverse fiber bundle tensile strength testing revealed a 5.55 MPa transverse fiber bundle tensile strength, and laser flash testing revealed a thermal conductivity of 0.78 W / m·K through the thickness of the unidirectional composite.

[0045] Comparative Example 2

[0046] The method of the patent application with publication number CN109851999A is used as comparative example 2. (1) 1,4,5,8-naphthalenetetracarboxylic dianhydride and octanediamine are added to an ethanol solvent in which a triethylamine catalyst is dissolved in a molar ratio of 1:2, reacted at 80°C for 16 hours, washed and dried to obtain an amino-terminated naphthalene diimide powder, wherein the amount of triethylamine used is 0.1wt% relative to the mass of the dianhydride; (2) carbon nanotubes are ultrasonically dispersed in the solution of step (1), and then a NaOH solution is added to adjust the pH value to 9, and the mass concentration of carbon nanotubes in the molecular assembly solution is 0.3mg / mL; (3) unsized asphalt-based carbon fibers are immersed in the above molecular assembly solution for 2 minutes, and vacuum dried to obtain asphalt-based carbon fibers with surface carbon nanotube / naphthalene diimide assembly; (4) the asphalt-based carbon fibers containing the carbon nanotube / naphthalene diimide assembly structure are compounded with an epoxy resin system and heated according to the curing temperature to obtain a unidirectional asphalt-based carbon fiber composite material. According to the transverse fiber bundle tensile strength test, the transverse fiber bundle tensile strength of the filament composite material is 19.24MPa. According to the laser flash test, the thermal conductivity of the unidirectional composite material in the thickness direction is 1.75W / m·K.

[0047] However, the above description is merely a specific embodiment of the present invention and should not be used to limit the scope of implementation of the present invention. Therefore, the replacement of equivalent components, or equivalent changes and modifications made according to the scope of protection of the present invention should still fall within the scope covered by the claims of the present invention.

Claims

1. A pitch-based carbon fiber with a three-dimensional surface assembly, characterized in that: The asphalt-based carbon fiber assembled three times on the surface is radially arranged from the inside to the outside in order: asphalt-based carbon fiber, inner layer of aromatic condensed ring molecules, middle layer of graphene and outer layer of aromatic condensed ring molecules; the middle layer of graphene contains graphene, and the graphene is dispersed on the surface of the asphalt-based carbon fiber, and the graphene middle layer is formed by the π-π conjugation between aromatic condensed ring molecules and graphene; the terminal amino group of aromatic condensed ring molecules -NH3 + The hydrogen bonds between them act on the graphene surface to form an outer layer of aromatic fused ring molecules.

2. The surface-tertiary assembled pitch-based carbon fiber according to claim 1, characterized in that: The aromatic fused ring molecule is prepared from an aromatic dianhydride and an organic diamine; the aromatic dianhydride is one or a combination of pyromellitic dianhydride, biphenyltetracarboxylic dianhydride, 1,4,5,8-naphthalenetetracarboxylic dianhydride, and 3,4,9,10-perylenetetracarboxylic dianhydride; the organic diamine is one or a combination of aliphatic diamine, aromatic diamine, and alicyclic diamine.

3. A method for preparing an interfacially thermally conductive pitch-based carbon fiber composite material using the surface-tertiary assembled pitch-based carbon fiber according to claim 1 or 2, characterized in that: The steps include: (1) Preparation of aromatic fused ring molecules: dissolving aromatic dianhydride and organic diamine in a polar solvent with a catalyst, reacting at 150-180°C for 9-15 hours, washing, filtering, and drying to obtain amino-terminated aromatic fused ring molecule powder, wherein the molar ratio of the aromatic dianhydride to the organic diamine is 1:(2-4), and the mass fraction of the catalyst is 0.1-0.2 wt% of the aromatic dianhydride; (2) Constructing an inner layer of aromatic condensed ring molecules on the surface of asphalt-based carbon fibers: dissolving the aromatic condensed ring molecule powder obtained in step (1) in a polar solvent, ultrasonically dispersing the powder, and preparing a suspension with a concentration of 10 to 20 mg / ml. The unsized asphalt-based carbon fibers are reacted in the suspension at 150 to 180°C for 18 to 24 hours, and vacuum dried to obtain an asphalt-based carbon fiber with an aromatic condensed ring molecule assembly layer, wherein the mass fraction of the inner layer of aromatic condensed ring molecules is 0.5 to 2 wt% of the unsized asphalt-based carbon fibers. (3) Constructing a graphene intermediate layer on the surface of asphalt-based carbon fiber: dissolving the peeled and layered graphene in a polar solvent to which a dispersant is added, ultrasonically treating for 3 to 7 hours to obtain a graphene dispersion, and finally immersing the asphalt-based carbon fiber obtained in step (2) in the graphene dispersion for 15 to 24 hours, and vacuum drying to obtain a surface secondary assembled asphalt-based carbon fiber, wherein the total mass fraction of the assembled layer after secondary assembly is 2 to 3 wt% of the unsized asphalt-based carbon fiber in step (1); (4) Constructing an outer layer of aromatic condensed ring molecules on the surface of asphalt-based carbon fibers: dissolving the powder obtained in step (1) in a polar solvent, ultrasonically dispersing, and preparing a suspension with a concentration of 1 to 5 mg / ml. Adding an alkaline solution to control the pH value to 7 to 9, placing the asphalt-based carbon fibers obtained in step (3) in the suspension for reaction for 6 to 12 hours, and vacuum drying to obtain asphalt-based carbon fibers with three-fold assembly on the surface, wherein the total mass fraction of the assembled layer after three-fold assembly is 2.5 to 4 wt% of the unsized asphalt-based carbon fibers in step (1); (5) Preparation of interface thermal conductive composite material: The asphalt-based carbon fiber obtained in step (4) is compounded with a resin system, cured and heated to obtain an asphalt-based carbon fiber composite material with good interface thermal conductivity.

4. The method according to claim 3, characterized in that The polar solvent in steps (1) to (4) is a combination of one or more of N,N-dimethylformamide, N-methylpyrrolidone, dimethyl sulfoxide, formamide, methanol, and ethanol.

5. The method according to claim 3, characterized in that The exfoliated and layered graphene in step (3) is graphene obtained after high-temperature carbonization, cell disruption and freeze-drying, wherein the number of graphene layers is 5 to 10.

6. The method according to claim 3, characterized in that The alkaline solution in step (4) is a combination of one or more of triethylamine, sodium hydroxide and potassium hydroxide.

7. The method according to claim 3, characterized in that The resin system in step (5) is one of epoxy resin, phenolic resin, bismaleimide and cyanate resin.

8. A pitch-based carbon fiber composite material with interfacial thermal conductivity obtained by the method according to claim 3.

9. Use of the interfacial thermal conductive pitch-based carbon fiber composite material according to claim 8 in aerospace structural and functional integrated materials.

10. Use of the pitch-based carbon fiber composite material with interfacial thermal conductivity as claimed in claim 8 in electronic and electrical materials.

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