Preparation method of efficient heat-conducting electromagnetic shielding material

Abstract

The invention relates to an efficient heat-conducting electromagnetic shielding composite material and a preparation method thereof.The preparation method specifically comprises the steps that APTES is adopted for modifying tetrapod-like ZnO whiskers, the tetrapod-like ZnO whiskers are grafted with graphene oxide through an EDC / NHS system, graphene oxide grafted tetrapod-like ZnO whiskers are obtained, and the dispersity and the heat-conducting property are improved; secondly, preparing a Ti3C2Tx nanosheet by adopting an HF etching method, and introducing amino groups through isocyanate-ethylenediamine modification, so that the chemical stability and the interfacial compatibility are improved; and finally, inducing oxidation polymerization of aniline through FeCl3 to obtain a graphene oxide graft / Ti < 3 > C < 2 > T < x > grafted polyaniline composite material, and constructing a uniform conductive network. The material has high thermal conductivity, high shielding performance, flexibility and stability, and is suitable for high-power electronic devices and flexible shielding materials.

Description

Technical Field

[0001] The present invention relates to a preparation method of an efficient heat-conducting electromagnetic shielding material, belonging to the technical fields of inorganic materials and composite materials. Background Art

[0002] With the rapid development of technologies such as 5G communication, Internet of Things (IoT), electric vehicles (EV), and high-performance computing (HPC), the density of electronic devices has been continuously increasing, and the problem of electromagnetic interference (EMI) has become increasingly serious. In modern electronic systems, the problems of electromagnetic interference (EMI) and electromagnetic compatibility (EMC) directly affect the stable operation of devices, and may even lead to signal attenuation, data loss, or device failure. Therefore, in order to ensure the normal operation of electronic devices, efficient, lightweight, and environmentally friendly electromagnetic shielding materials have become the focus of research and application.

[0003] Although electromagnetic shielding materials have been widely used, traditional materials still have the following technical bottlenecks: 1) Most traditional electromagnetic shielding materials are metals (such as copper, aluminum, nickel). Although they have high shielding efficiency, they have high density and are prone to corrosion, making them unsuitable for lightweight electronic devices and flexible electronics; 2) The shielding efficiency of existing carbon-based shielding materials (such as graphene, carbon nanotube CNT) is limited and it is difficult to cover the high-frequency band of 8-18 GHz, unable to meet the application requirements of 5G and millimeter waves; 3) The high integration and high power of modern electronic devices lead to an increase in device temperature. The insufficient thermal conductivity of electromagnetic shielding materials cannot effectively solve the problem of heat accumulation, affecting the device life and stability. Although traditional metal shielding materials have good thermal conductivity, they are heavy and have poor flexibility, while the thermal conductivity of polymer shielding materials is often lower than 1 W / m·K, unable to meet the thermal management requirements of high-power devices. There are interfacial thermal resistance and dispersion problems between conductive fillers (such as metals, MXene, graphene) and polymer matrices, resulting in a decrease in the overall thermal conductivity of the materials. Agglomeration is likely to occur between conductive fillers, affecting the shielding effect and reducing the mechanical strength and long-term stability of the materials. In order to overcome the above problems of traditional shielding materials, thermally conductive electromagnetic shielding materials have become a research hotspot in recent years. Such materials provide good thermal conductivity while ensuring high-efficiency electromagnetic shielding to meet the thermal management requirements of high-power electronic devices. Graphene, carbon nanotubes (CNTs), and MXene have become the most promising shielding materials due to their high conductivity, high specific surface area, and excellent thermal conductivity. Through layered structure arrangement and interface engineering optimization, an EMI shielding efficiency of >40 dB can be achieved, and the thermal conductivity can reach 10-100 W / m·K. Researchers have explored the combination of MXene, zinc oxide (ZnO), and silicon carbide (SiC) with polymers to achieve the synergistic effect of conductive loss and dielectric loss and improve the electromagnetic shielding efficiency. However, it has been found in the research that the compatibility between carbon-based materials, Mxene, and inorganic fillers is poor and the thermal conduction channels are incomplete, restricting the improvement of their performance. Therefore, how to develop materials with high thermal conductivity and high-efficiency electromagnetic shielding has become a research hotspot. Summary of the Invention

[0004] The purpose of the present invention is to provide a preparation method of a highly thermally conductive electromagnetic shielding material, and the purpose of the present invention is achieved through the following technical solutions: A preparation method of a highly thermally conductive electromagnetic shielding material includes the following steps: (1) Prepare graphene graft; (2) Prepare amino-modified Ti3C2T x nanosheets; (3) Dissolve aniline in 1 M HCl, and add the graphene graft prepared in step (1), sodium dodecylbenzenesulfonate, and the amino-modified Ti3C2T prepared in step (2) to the system xNanosheets were used to form dispersion A by magnetic stirring; FeCl3·6H2O was dissolved in 1 M HCl, and the FeCl3 solution was added dropwise to dispersion A. After reacting for 10 h, it was washed and dried to obtain the graphene grafted product / Ti3C2T x Nanosheet grafted polyaniline composite, namely the high-efficiency heat-conducting and electromagnetic shielding material described above.

[0005] Preferably, the preparation method of the graphene grafted product is as follows: (1) Tetrapod zinc oxide whiskers were added to an ethanol / water (volume ratio 1:1) solution and ultrasonically dispersed. 3-Aminopropyltriethoxysilane was added to the dispersion and reacted for 2 h to obtain aminated tetrapod zinc oxide whiskers; graphene oxide was ultrasonically dispersed in deionized water, and EDC (1-ethyl-3-(3-dimethylaminopropyl)carbodiimide) and NHS (N-hydroxysuccinimide) were added and reacted for 2 h. After centrifugation and washing with deionized water, activated graphene oxide was obtained; (2) The aminated tetrapod zinc oxide whiskers and activated graphene oxide prepared in step (1) were added to DMF and ultrasonically dispersed, and reacted at room temperature for 10 h to obtain graphene grafted tetrapod zinc oxide whiskers, namely the graphene grafted product.

[0006] Preferably, the mass ratio of the tetrapod zinc oxide whiskers to 3-aminopropyltriethoxysilane in step (1) is (1~3):(2~4).

[0007] Preferably, the mass ratio of the aminated tetrapod zinc oxide whiskers to the activated graphene oxide in step (2) is (3~6):(2~4).

[0008] Preferably, the preparation method of the amino-modified Ti3C2T x nanosheets is as follows: (1) Ti3AlC2 nanosheets were added to an HF (mass fraction 40%) solution and reacted by magnetic stirring for 24 h. After washing with deionized water until the pH of the supernatant was greater than 6, it was freeze-dried to obtain Ti3C2T x nanosheets; (2) The Ti3C2T x nanosheets prepared in step (1) were dispersed in DMF, and phenyl isocyanate was added and reacted at 70 °C for 6 h to obtain isocyanate-modified Ti3C2T x ; (3) The isocyanate-modified Ti3C2T x prepared in step (2) was dispersed in DMF, and ethylenediamine was added and stirred at 60 °C for 12 h to obtain amino-modified Ti3C2T x nanosheets.

[0009] Preferably, the Ti3C2T in step (2)x The mass ratio of the nanosheets to phenyl isocyanate is (3 - 5):(1 - 2).

[0010] Preferably, the mass ratio of the aniline, the graphene graft, and the amino-modified Ti3C2T x nanosheets is (5 - 10):(1 - 2):(1 - 2).

[0011] Preferably, the high-efficiency thermal conductive electromagnetic shielding material is applied in the fields of high-power electronic devices and flexible shielding materials.

[0012] The principle of the present invention lies in: (1) 3-Aminopropyltriethoxysilane (APTES) is used to amino-functionalize the surface of the tetrapod-like ZnO whiskers, and the EDC / NHS system is used to promote the activation of the carboxyl groups on the surface of graphene oxide, enabling the ZnO whiskers to be stably grafted onto the graphene through amide bonds, thereby enhancing the interfacial binding force of the material, optimizing its dispersibility and thermal conductivity, and laying a foundation for the subsequent construction of the conductive network.

[0013] (2) The HF etching method is used to remove the Al layer in the Ti3AlC2 structure to obtain two-dimensional Ti3C2T x nanosheets, and through the reaction of isocyanate and ethylenediamine, amino groups are introduced onto its surface, which is beneficial for the subsequent grafting of aniline.

[0014] (3) FeCl3 is used to induce the oxidative polymerization of aniline monomers, enabling them to be grafted onto the Ti3C2T x nanosheets to form a uniform conductive polyaniline (PANI) layer.

[0015] Compared with the prior art, the present invention has the following beneficial effects: (1) In the present invention, the tetrapod-like ZnO whiskers are amino-functionalized by APTES and graphene oxide is crosslinked by EDC / NHS, so that a covalent bond is formed between the ZnO whiskers and the graphene. Compared with the traditional physical doping method, the dispersibility and interfacial binding force of the filler are improved, the interfacial thermal resistance is effectively reduced, and thus the thermal conductivity of the composite material is increased.

[0016] (2) The HF etching method is used to exfoliate the Ti3C2T x nanosheets, and further amino groups are introduced onto its surface by modification with isocyanate and ethylenediamine, improving its chemical stability and dispersibility, and avoiding the problems of easy agglomeration and degradation of the traditional Ti3C2T x materials. At the same time, the high conductivity of Ti3C2T x forms a conductive network with PANI, improving the electromagnetic shielding efficiency of the composite material in the 8 - 18 GHz frequency band, which is superior to the traditional single shielding material.

[0017] (3) In-situ polymerization of polyaniline on the graphene graft / Ti3C2T x composite material by FeCl3 oxidation polymerization method, avoiding the interfacial inhomogeneity problem caused by the traditional mechanical mixing method, realizing a uniform and continuous conductive network, improving the electrical conductivity, thermal stability and mechanical flexibility of the material, making it applicable to flexible electromagnetic shielding materials, heat dissipation shielding layers of 5G electronic devices and high-performance thermal conductive interface materials, and having better comprehensive performance compared with existing single conductive or thermal conductive materials. Brief Description of the Drawings

[0018] By reading the following detailed description of the non-limiting embodiments with reference to the accompanying drawings, other features, objects and advantages of the present invention will become more apparent: Figure 1 It is a preparation flow chart of the high-efficiency thermal conductive electromagnetic shielding material prepared in Example 1 of the present invention. Detailed Embodiments

[0019] The present invention will be described in detail below with reference to specific embodiments. The following embodiments will help those skilled in the art to further understand the present invention, but do not limit the present invention in any form. It should be noted that those of ordinary skill in the art can make several modifications and improvements without departing from the concept of the present invention. These all belong to the protection scope of the present invention. Example 1

[0020] (1) Preparation of graphene graft 0.5 g of tetrapod zinc oxide whiskers was added to 100 mL of ethanol / water (volume ratio 1:1) solution, and ultrasonicated for 30 min to ensure sufficient dispersion. 0.5 g of 3-aminopropyltriethoxysilane was added to the dispersion, and the reaction was magnetically stirred for 2 h. The product was filtered, washed and dried to obtain amino-functionalized tetrapod zinc oxide whiskers. 0.1 g of graphene oxide was dispersed in 100 mL of deionized water, and after ultrasonicating for 30 min to form a uniform suspension, 100 mM EDC (1-ethyl-3-(3-dimethylaminopropyl)carbodiimide) and 50 mM NHS (N-hydroxysuccinimide) were added, and the reaction was magnetically stirred for 2 h. After the reaction was completed, it was centrifuged and washed with deionized water to obtain activated graphene oxide. 0.5 g of amino-functionalized tetrapod zinc oxide whiskers and 0.3 g of activated graphene oxide were added to 100 mL of DMF, ultrasonically dispersed, and magnetically stirred at room temperature for 10 h. After the reaction was completed, it was centrifuged, washed and vacuum dried to obtain graphene-grafted tetrapod zinc oxide whiskers.

[0021] (2) Amino modification of Ti3C2T x Preparation of nanosheets At room temperature, 1 g of Ti3AlC2 nanosheets was slowly added to 50 mL of HF (40% by mass) solution, and the reaction was carried out under magnetic stirring for 24 h. After the reaction, the above corrosion products were washed with deionized water until the pH of the centrifuged supernatant was greater than 6. The product was freeze-dried to obtain Ti3C2T x nanosheets. 0.3 g of Ti3C2Tx nanosheets was dispersed in 100 mL of DMF, 0.1 g of phenyl isocyanate was added, and the reaction was carried out under magnetic stirring at 70 °C for 6 h. The unreacted substances were removed by washing with ethanol and deionized water to obtain isocyanate-modified Ti3C2T x . 0.2 g of isocyanate-modified Ti3C2T x was dispersed in 100 mL of DMF, 0.5 g of ethylenediamine was added, and the mixture was stirred at 60 °C for 12 h. The product was washed repeatedly with DMF, ethanol, and deionized water to remove the unreacted substances, and then dried in vacuo to obtain amino-modified Ti3C2T x nanosheets.

[0022] (3)Preparation of Graphene Graft / Ti3C2T x nanosheet Grafted Polyaniline Composite 1.5 g of aniline was dissolved in 100 mL of 1 M HCl solution, and the solution was formed by magnetic stirring for 10 min. 0.2 g of graphene graft, 1 g of sodium dodecylbenzenesulfonate, and 0.2 g of amino-modified Ti3C2T x nanosheets were added to the solution, and a dispersion A was formed by magnetic stirring. 2 g of FeCl3·6H2O was dissolved in 100 mL of 1 M HCl, and an FeCl3 solution was formed by magnetic stirring for 10 min. Under the condition of an ice bath at 3 °C, the FeCl3 solution was added dropwise to dispersion A, and the addition was completed within 15 min. Subsequently, the reaction was continued with magnetic stirring for 10 h. After the reaction, it was left standing for 1 h to promote precipitation, and then washed repeatedly with deionized water and ethanol (1:1) 3-5 times to remove the unreacted FeCl3 and by-products, and dried in vacuo to obtain graphene graft / Ti3C2T x nanosheet grafted polyaniline composite. The preparation process is as Figure 1 shown.

[0023] The electromagnetic shielding effectiveness of this composite material is 61.2 dB (in the frequency band of 0.03 - 18 GHz), the thermal conductivity is 1.8 W / m·k, and it has high thermal conductivity, effectively inhibits signal interference, and improves the equipment life. Example 2

[0024] (1)Preparation of Graphene Graft 0.4 g of tetrapod-like zinc oxide whiskers were added to 100 mL of ethanol / water (volume ratio 1:1) solution and sonicated for 30 min to ensure sufficient dispersion. 0.6 g of 3-aminopropyltriethoxysilane was added to the dispersion, and the mixture was magnetically stirred for 2 h. The product was filtered, washed, and dried to obtain amino-functionalized tetrapod-like zinc oxide whiskers. 0.1 g of graphene oxide was dispersed in 100 mL of deionized water and sonicated for 30 min to form a homogeneous suspension. Then, 100 mM of EDC (1-ethyl-3-(3-dimethylaminopropyl)carbodiimide) and 50 mM of NHS (N-hydroxysuccinimide) were added, and the mixture was magnetically stirred for 2 h. After the reaction was completed, the product was centrifuged and washed with deionized water to obtain activated graphene oxide. 0.6 g of amino-functionalized tetrapod-like zinc oxide whiskers and 0.3 g of activated graphene oxide were added to 100 mL of DMF, sonicated for dispersion, and magnetically stirred at room temperature for 10 h. After the reaction ended, the product was centrifuged, washed, and vacuum dried to obtain graphene-grafted tetrapod-like zinc oxide whiskers.

[0025] (2)Amino-modified Ti3C2T x Preparation of nanosheets At room temperature, 1 g of Ti3AlC2 nanosheets was slowly added to 50 mL of HF (mass fraction 40%) solution, and the mixture was magnetically stirred for 24 h. After the reaction ended, the corrosion product was washed with deionized water until the pH of the centrifuged supernatant was greater than 6. The product was freeze-dried to obtain Ti3C2T x nanosheets. 0.4 g of Ti3C2T x nanosheets were dispersed in 100 mL of DMF, 0.15 g of phenyl isocyanate was added, and the mixture was magnetically stirred at 70 °C for 6 h. The product was washed with ethanol and deionized water to remove the unreacted substances, and isocyanate-modified Ti3C2T x was obtained. 0.2 g of isocyanate-modified Ti3C2T x was dispersed in 100 mL of DMF, 0.5 g of ethylenediamine was added, and the mixture was stirred at 60 °C for 12 h. The product was repeatedly washed with DMF, ethanol, and deionized water to remove the unreacted substances, and vacuum dried to obtain amino-modified Ti3C2T x nanosheets.

[0026] (3)Graphene graft / Ti3C2T x Preparation of graphene graft / Ti3C2T 1.8 g of aniline was dissolved in 100 mL of 1 M HCl solution and magnetically stirred for 10 min to form a solution. 0.15 g of graphene graft, 1 g of sodium dodecylbenzenesulfonate, and 0.15 g of amino-modified Ti3C2T were added to the solution xNanosheets were used to form dispersion A by magnetic stirring. 2 g of FeCl3·6H2O was dissolved in 100 mL of 1 M HCl, and magnetic stirring was carried out for 10 min to form a FeCl3 solution. Under the condition of an ice bath at 3 °C, the FeCl3 solution was added dropwise to dispersion A, and the addition was completed within 15 min. Subsequently, magnetic stirring was continued for 10 h. After the reaction ended, it was left standing for 1 h to promote precipitation, and then washed repeatedly 3 - 5 times with deionized water and ethanol (1:1) to remove unreacted FeCl3 and by-products, and then dried under vacuum to obtain graphene grafted / Ti3C2T x Nanosheet grafted polyaniline composite. The preparation process is as Figure 1 shown

[0027] The electromagnetic shielding effectiveness of this composite material is 63.9 dB (in the frequency band of 0.03 - 18 GHz), and the thermal conductivity is 1.7 W / m·k. It has high thermal conductivity, can effectively suppress signal interference, and improve the service life of equipment Example 3

[0028] (1) Preparation of graphene grafted material 0.5 g of tetrapod-like zinc oxide whiskers was added to 100 mL of ethanol / water (volume ratio 1:1) solution, and ultrasonic treatment was carried out for 30 min to ensure sufficient dispersion. 0.6 g of 3-aminopropyltriethoxysilane was added to the dispersion, and magnetic stirring reaction was carried out for 2 h. The product was filtered, washed and dried to obtain amino-functionalized tetrapod-like zinc oxide whiskers. 0.1 g of graphene oxide was dispersed in 100 mL of deionized water, and after ultrasonic treatment for 30 min to form a uniform suspension, 100 mM EDC (1-ethyl-3-(3-dimethylaminopropyl)carbodiimide) and 50 mM NHS (N-hydroxysuccinimide) were added, and magnetic stirring was carried out for 2 h. After the reaction was completed, it was centrifuged and washed with deionized water to obtain activated graphene oxide. 0.6 g of amino-functionalized tetrapod-like zinc oxide whiskers and 0.4 g of activated graphene oxide were added to 100 mL of DMF, ultrasonically dispersed, and magnetic stirring reaction was carried out at room temperature for 10 h. After the reaction ended, it was centrifuged, washed, and dried under vacuum to obtain graphene grafted tetrapod-like zinc oxide whiskers

[0029] (2) Amino modification of Ti3C2T x Preparation of nanosheets At room temperature, 1 g of Ti3AlC2 nanosheets was slowly added to 50 mL of HF (mass fraction 40%) solution, and magnetic stirring was carried out for 24 h. After the reaction ended, the corrosion product was washed with deionized water until the pH of the centrifuged supernatant was greater than 6. The product was freeze-dried to obtain Ti3C2T x Nanosheets. 0.45 g of Ti3C2T xThe nanosheets were dispersed in 100 mL of DMF, 0.2 g of phenyl isocyanate was added, and the mixture was magnetically stirred at 70 °C for 6 h. The unreacted substances were removed by washing with ethanol and deionized water to obtain isocyanate-modified Ti3C2T x 0.2 g of isocyanate-modified Ti3C2T x was dispersed in 100 mL of DMF, 0.5 g of ethylenediamine was added, and the mixture was stirred at 60 °C for 12 h. The product was repeatedly washed with DMF, ethanol, and deionized water to remove the unreacted substances, and then dried under vacuum to obtain amino-modified Ti3C2T x nanosheets.

[0030] (3)Graphene grafted / Ti3C2T x Preparation of graphene grafted / Ti3C2T 1.6 g of aniline was dissolved in 100 mL of 1 M HCl solution and magnetically stirred for 10 min to form a solution. 0.18 g of graphene grafted, 1 g of sodium dodecylbenzenesulfonate, and 0.2 g of amino-modified Ti3C2T x nanosheets were added to the solution, and a dispersion A was formed by magnetic stirring. 2 g of FeCl3·6H2O was dissolved in 100 mL of 1 M HCl and magnetically stirred for 10 min to form an FeCl3 solution. Under the condition of an ice bath at 3 °C, the FeCl3 solution was added dropwise to dispersion A, and the addition was completed within 15 min. Subsequently, magnetic stirring was continued for 10 h. After the reaction was completed, the mixture was allowed to stand for 1 h to promote precipitation, and then repeatedly washed 3-5 times with deionized water and ethanol (1:1) to remove the unreacted FeCl3 and by-products, and then dried under vacuum to obtain graphene grafted / Ti3C2T x nanosheets grafted with polyaniline composite. The preparation process is as Figure 1 shown.

[0031] The electromagnetic shielding effectiveness of this composite material is 58.9 dB (in the frequency band of 0.03-18 GHz), and the thermal conductivity is 1.7 W / m·k. It has high thermal conductivity, effectively suppresses signal interference, and improves the service life of the device. Comparative Example 1

[0032] The difference from Example 1 is that: step (1) was omitted. In step (3), "graphene" was directly used instead of "graphene grafted" to finally obtain graphene Ti3C2T x nanosheets grafted with polyaniline composite. The electromagnetic shielding effectiveness of this composite material is 63.7 dB (in the frequency band of 0.03-18 GHz), and the thermal conductivity is 0.3 W / m·k. Comparative Example 2

[0033] The difference from Example 1 is that step (3) is omitted, the addition amount of polyaniline is 0, and finally graphene grafted / Ti3C2T x nanosheet composite is obtained. The electromagnetic shielding effectiveness of this composite material is 50.1 dB (0.03 - 18 GHz frequency band), and the thermal conductivity is 1.6 W / m·k. Comparative Example 3

[0034] The difference from Example 1 is that step (2) is omitted, and "Ti3C2T x nanosheets" is directly used in step (3) to replace "amino modified Ti3C2T x nanosheets", and finally graphene grafted / Ti3C2T x nanosheet / polyaniline composite is obtained. The electromagnetic shielding effectiveness of this composite material is 54.2 dB (0.03 - 18 GHz frequency band), and the thermal conductivity is 1.7 W / m·k.

[0035] The specific embodiments of the present invention have been described above. It should be understood that the present invention is not limited to the above specific embodiments, and those skilled in the art can make various deformations or modifications within the scope of the claims, which do not affect the essence of the present invention.

Claims

1. A method for preparing a high-efficiency thermal conductive electromagnetic shielding material, characterized in that: The steps include: (1) Preparation of graphene grafted materials; (2) Preparation of amino-modified Ti3C2T x Nanosheets; (3) Aniline was dissolved in 1 M HCl, and the graphene grafted product prepared in step (1), sodium dodecylbenzene sulfonate, and amino-modified Ti3C2T prepared in step (2) were added to the system. x Nanosheets were magnetically stirred to form dispersion A; FeCl3·6H2O was dissolved in 1M HCl, and the FeCl3 solution was added dropwise to dispersion A for 10 h, washed, and dried to obtain graphene grafted Ti3C2T x Nanosheet grafted polyaniline composite, namely the highly efficient thermal conductive electromagnetic shielding material; The preparation method of the graphene grafted material is: (1) Tetrapod-shaped zinc oxide whiskers were added to an ethanol / water (volume ratio 1:1) solution and ultrasonically dispersed. 3-aminopropyltriethoxysilane was added to the dispersion and reacted for 2 h to obtain amino-modified tetrapod-shaped zinc oxide whiskers. Graphene oxide was ultrasonically dispersed in deionized water, and EDC (1-ethyl-3-(3-dimethylaminopropyl)carbodiimide) and NHS (N-hydroxysuccinimide) were added and reacted for 2 h. The mixture was centrifuged and washed with deionized water to obtain activated graphene oxide. (2) adding the aminated tetrapod-shaped zinc oxide whiskers and activated graphene oxide obtained in step (1) into DMF, dispersing them by ultrasonication, and reacting them at room temperature for 10 h to obtain graphene-grafted tetrapod-shaped zinc oxide whiskers, i.e., the graphene grafted product; The mass ratio of the tetrapod-shaped zinc oxide whiskers and 3-aminopropyltriethoxysilane in step (1) is (1-3): (2-4); The mass ratio of the amino-modified tetrapod-shaped zinc oxide whiskers and the activated graphene oxide in step (2) is (3-6): (2-4); The amino-modified Ti3C2T x The preparation method of nanosheets is: (1) Ti3AlC2 nanosheets were added to HF (mass fraction 40%) solution and reacted with magnetic stirring for 24 h. The solution was washed with deionized water until the pH of the supernatant was greater than 6 and freeze-dried to obtain Ti3C2T x Nanosheets; (2) Ti3C2T prepared in step (1) x The nanosheets were dispersed in DMF, phenyl isocyanate was added, and the reaction was carried out at 70 °C for 6 h to obtain isocyanate-modified Ti3C2T x ; (3) The isocyanate-modified Ti3C2T prepared in step (2) x Dispersed in DMF, added ethylenediamine, stirred at 60 °C for 12 h, and amino-modified Ti3C2T x Nanosheets; Step (2) Ti3C2T x The mass ratio of nanosheets to phenyl isocyanate is (3~5):(1~2).

2. The method for preparing a high-efficiency thermal conductive electromagnetic shielding material according to claim 1, characterized in that: The aniline, graphene grafted product, amino-modified Ti3C2T x The mass ratio of the nanosheets is (5~10):(1~2):(1~2).

3. The method for preparing a high-efficiency thermal conductive electromagnetic shielding material according to claim 1, characterized in that: The high-efficiency heat-conductive electromagnetic shielding material is used in the fields of high-power electronic devices and flexible shielding materials.

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