Preparation method of graphene composite coating with multifunctional characteristic

Abstract

The invention discloses a preparation method of a graphene composite coating with multifunctional characteristics, which comprises the following steps: processing a substrate, coating a carbon source polymer solution on the surface of a substrate material to form a polymer liquid film, and treating a polymer to form a polymer film; laser induction: carbonizing the polymer film by using laser to form a laser-induced graphene (LIG) coating; functional particles are added, nanoparticles are doped on the surface of the LIG coating in a coating mode, and a composite structure is formed; integrating the multifunctional coating, and forming the graphene-based multifunctional composite coating through post-treatment.

Description

TECHNICAL FIELD

[0001] The application belongs to the technical field of graphene functional coating preparation, and particularly relates to a graphene composite coating preparation method with multifunctional characteristics. BACKGROUND

[0002] The statements herein are provided only to aid in the understanding of the present application, and do not necessarily constitute prior art.

[0003] With the rapid development of electronic information, national defense and military industry, intelligent equipment, new energy and other fields, the demand for functional coatings has been expanded from single function to "multifunctional integration, performance synergy, and process light weight". Graphene has shown application potential in the field of functional coatings due to its excellent electrical, thermal, mechanical and other properties, but single graphene coating has problems such as single function and insufficient synergy. Although carbon nanomaterials, metal particles and other functional materials have unique performance advantages, the existing preparation processes all face the difficulties of uneven dispersion, weak functional synergy, complex process, and difficult structure control when preparing multiple materials, which restricts the integration and practicalization process of multifunctional composite coatings.

[0004] Specifically, the existing graphene composite coating preparation methods can be mainly divided into two categories: surface deposition method and blending coating method. The surface deposition method forms a graphene film on the surface of the substrate through chemical vapor deposition CVD, mechanical transfer, electrochemical method and other processes; the blending coating method disperses graphene as a filler in liquid resin to form a mixed coating, and then forms a graphene coating on the surface of the substrate material through a coating method. However, the above-mentioned CVD method and other methods involve high-temperature, high-pressure environment and complex processes such as template etching and removal (CVD method is to crack organic carbon at high temperature, then deposit on the surface of the template to form a film, then remove the template to obtain graphene); similarly, the blending coating method involves the dispersion of graphene in polymers. Due to the characteristics of easy agglomeration and difficult dispersion of graphene, the whole process is time-consuming and complex, which seriously affects the preparation period and cost. At the same time, due to the factors such as multiple processes and harsh processing conditions of the above-mentioned methods, the graphene formation process is complex, and the macro / micro structure is affected by many factors such as template type, processing time, temperature, dispersion liquid concentration, etc. Therefore, the obtained graphene coating is mostly full-coverage film, and it is difficult to realize local patterning and customized structure, thereby limiting the application of the substrate material in more scenarios.

[0005] In recent years, with the development of laser processing technology, researchers have successfully prepared graphene functional coatings using graphene oxide, high molecular polymers, wood and other carbon sources as precursors through laser processing technology due to the advantages of digital processing, pattern design, rich raw materials, controllable structure, no need for masks and additional chemical reagents. For example, in the preparation method of a composite material surface graphene sensor disclosed in Chinese patent application CN201810753060.9, a carbon precursor film is first formed by spraying an oxidized graphene solution, and then a graphene coating is obtained by laser reduction. The obtained graphene coating exhibits excellent piezoresistive sensing characteristics and can realize large-area stress and strain monitoring of an epoxy resin matrix. However, there are still significant deficiencies in the preparation process and performance control: (1) The preparation process of graphene oxide requires long-time dispersion, making it difficult to form a homogeneous solution, and thus the coating performance may vary due to uneven dispersion during spraying; (2) It is difficult to achieve patterned customization, and there are problems such as weak coating adhesion, single function and difficulty in mass production. Similarly, in the preparation method of tungsten carbide / graphene composite material disclosed in Chinese patent application CN114988716 A, tungsten source is first dispersed in an aromatic polyimide precursor, and then a polyimide composite film is formed, and a graphene composite film is obtained by laser carbonization. However, there are still significant deficiencies in the preparation method and performance control: (1) The viscosity of the polyimide precursor solution can reach 6000 mPa·s, so it is difficult to form a homogeneous dispersion system by continuously stirring and dispersing the tungsten source in the polyimide solution for a long time, and thus the performance of the obtained graphene composite film may be uneven; (2) In the above coating process, the spin coating method is used, which can only form a large-area film and cannot form a patterned film, so it is difficult to form a customized composite film.

[0006] Therefore, it is of great technical innovation and industrial application value to develop a multifunctional graphene composite coating material that can realize multifunctional integration, process control and adaptation to multiple scenarios, and a preparation method thereof. SUMMARY

[0007] In view of the deficiencies of the prior art, in order to overcome the problems of single function, uneven dispersion, complex process, difficult structure control, weak functional synergy and other problems, and to meet more application scenarios, the present application provides a preparation method of a graphene composite coating with multifunctional characteristics. The method adopts a three-step method of "substrate coating construction-laser carbonization functionalization-multicomponent material composite". First, a polymer solution is used as a carbon source to form a precursor coating by extrusion printing, and then a laser-induced graphene (LIG) coating is generated by laser carbonization. Finally, nano functional particles are added to form a composite coating with functions of sensing, anti-icing / icing removal, high temperature resistance and electromagnetic shielding through multi-material synergy.

[0008] To achieve the above object, the present application is realized by the following technical solutions: The present application provides a preparation method of graphene composite coating with multifunctional characteristics, comprising the following steps: Substrate processing, forming a polymer liquid film on the surface of the substrate material by coating method, and high-temperature treating the polymer to form a polymer film; Laser induction, carbonizing the polymer film by laser to form a laser-induced graphene (LIG) coating; Adding functional particles, doping nanoparticles on the surface of the LIG coating by coating method to form a composite structure; Multifunctional coating integration, forming a graphene-based multifunctional composite coating by post-processing.

[0009] The carbon source polymer solution includes a solution of polyimide (PI), polyphenylene sulfide (PPS), polyetherimide (PEI), or polyether ether ketone (PEEK) powder in an organic solvent, and also includes a precursor solution of each of the above powders.

[0010] In a further technical solution, the coating method of the carbon source polymer solution is an automatic controllable extrusion molding method, the extrusion pressure is 0.1-100 psi, the extrusion speed is 10-100 mm / s, and the needle diameter is 0.1 mm-0.61 mm. By controlling the extrusion pressure, extrusion speed and needle diameter, the processing efficiency and the precision of the formed polymer film can be adjusted.

[0011] In a further technical solution, the substrate material includes composite materials, glass, plastic, metal, fabric and other materials.

[0012] In a further technical solution, the laser used in laser induction is a CO2 laser, and the laser focal length, scanning speed and pulse resolution of the CO2 laser are 33.1-43.1 mm, 2.54-203.2 mm / s and 1-1000 ppi / inch, respectively, and the laser power is 0.1-50 W. Laser carbonization can be carried out under room temperature atmospheric environment conditions. By adjusting the above parameters, the processing speed of the LIG film can be adjusted, and LIG with different microstructures can be obtained.

[0013] In a further technical solution, laser induction can be single laser induction or multiple laser inductions.

[0014] The coating obtained by substrate processing includes a large-area coated coating and a customizable patterned coating.

[0015] The LIG coating formed by laser carbonization can be a large-area coated LIG coating, a customized patterned coating, or an array of patterned coatings.

[0016] In a further technical solution, the nanoparticles include carbon nanotubes (CNT), MXene, polyaniline (PANI), Pt, Ni, and other metal particles.

[0017] In a further technical solution, the particulate nanomaterial or its corresponding solution is doped on the surface of the LIG coating by coating.

[0018] In a further technical solution, the coating method of the nanoparticles includes extrusion molding, spray pen spraying, doctor blade coating, and the like.

[0019] In a further technical solution, the specific steps of integrating the multifunctional coating are as follows: The solvent and the like are removed by a post-processing method to stably combine the nanoparticles with the LIG coating, and a graphene-based multifunctional composite coating is obtained.

[0020] In a further technical solution, the post-processing method includes heating, electrophoretic deposition, laser induction, and the like.

[0021] In a further technical solution, the functions of the multifunctional coating include sensing, anti-icing / icing removal, electromagnetic shielding, energy storage, high-temperature resistance, and the like. By adding functional particles with corresponding functions, the coating realizes the above-mentioned performances.

[0022] In a further technical solution, the structure and electrical properties of the coating can be realized by adjusting the laser power, the number of laser scanning, the laser focal length, and the content of the doped nanoparticles.

[0023] In a further technical solution, the thickness of the composite coating is (0-100) μm.

[0024] In a further technical solution, the sheet resistance of the composite coating is 10-2000 (Ω / sq).

[0025] In a further technical solution, when the composite coating is used for structural health monitoring, the sensing coefficient (Gauge Factor) can be adjusted in the range of 0.6-650.

[0026] In a further technical solution, when the composite coating is used for anti-icing, the water contact angle can be adjusted in the range of 90-155°.

[0027] In a further technical solution, when the composite coating is used for Joule heating deicing, the surface temperature of the coating can reach 220℃ when the input power of the power supply is adjusted in the range of 0-4.5 W.

[0028] In a further technical solution, the composite coating can absorb 20db electromagnetic waves when used for electromagnetic shielding.

[0029] In a further technical solution, the specific capacitance of the composite coating can be up to 117.3mF / cm when used for supercapacitors. 2 .

[0030] The multifunctional graphene composite coating preparation method of the present application combines extrusion molding coating method and digital laser carbonization process during the preparation of the substrate LIG coating. Since the extrusion molding method controlled by program can directly coat the carbon source polymer solution on the substrate material according to the pre-set coating path, it is not necessary to disperse the carbon source in the polymer or other organic solvents, thereby avoiding the high-temperature and high-pressure environment of the traditional surface deposition method and the complex dispersion process of the blending coating method, and effectively improving the processing efficiency of the coating and adapting to the scale production demand.

[0031] The multifunctional graphene composite coating preparation method of the present application can directly or indirectly heat the substrate LIG coating, add nano functional particles by utilizing the Joule heat performance of the substrate LIG coating and the secondary laser induction method, and avoid the dispersion of nano functional particles in the carbon source substrate, so that the processing process is simple and controllable, and suitable for large-area processing of multifunctional coatings.

[0032] The multifunctional graphene composite coating preparation method of the present application uses automatic and controllable extrusion molding coating for substrate processing, and combines laser-induced carbonization technology, so that not only a large-area functional coating can be obtained, but also a customizable patterned coating can be obtained, the coating is locally functionalized, the problems of single function and expansion limitation are broken through, and the application scene is more flexible.

[0033] In the preparation process of the present application, no toxic and harmful chemicals are used, the laser carbonization is carried out at room temperature in an atmospheric environment, and there is no pollutant emission in the processing process, so that the present application is more in line with the green and environmental protection production requirements compared with the traditional process.

[0034] The coating substrate of the present application has a wide selection range, including metal, composite material, glass, fabric, etc., and has stronger adaptability.

[0035] The substrate coating of the present application is combined with the substrate material by heating, thereby improving the adhesion of the coating.

[0036] The raw materials of the coating of the present application are rich, including a solution formed by carbon source polyimide (PI), polyphenylene sulfide (PPS), polyetherimide (PEI) or polyether ether ketone (PEEK) powder in an organic solvent, and also including a precursor solution of the above-mentioned powder.

[0037] The multifunctional graphene composite coating preparation method of the application can realize the performance of the obtained coating by adjusting laser parameters or adjusting the concentration of doped nanoparticles. BRIEF DESCRIPTION OF DRAWINGS

[0038] The drawings accompanying the specification of the application form a part thereof and serve to further understand the application, the illustrative embodiments thereof and the description thereof, and do not constitute an improper limitation of the application.

[0039] Figure 1 Flow chart of the multifunctional graphene composite coating preparation method of the application; Figure 2 Processing schematic diagram of the graphene coating of the application; Figure 3 and Figure 4 Actual object diagram of the graphene coating obtained by the application; Figure 5 Actual object diagram of the graphene coating obtained by the application on different substrates; Figure 6 Processing schematic diagram of the graphene composite coating prepared by the spraying method of the application; Figure 7 Processing schematic diagram of the graphene composite coating prepared by the coating method of the application; Figure 8 Actual object diagram of the graphene / CNT composite coating obtained by the application; Figure 9 Actual object diagram of the graphene / Pt composite coating obtained by the application; Figure 10 SEM diagram of the graphene composite coating obtained by the application by regulating the number of laser scans; Figure 11 SEM diagram of the graphene composite coating obtained by the application by regulating the laser processing power; Figure 12 Raman diagram of the graphene / CNT composite coating obtained by the application; Figure 13 SEM diagram of the graphene composite coating obtained by the application by regulating the Pt content; Figure 14 Test result diagram of the graphene multifunctional coating for sensing of the application; Figure 15 Contact angle diagram of the hydrophobic graphene composite coating for active ice prevention obtained by the application; Figure 16 Test result diagram of the graphene multifunctional coating for heating deicing of the application; Figure 17 Test result diagram of the graphene multifunctional coating for supercapacitor of the application; Figure 18 Figure for test results of the graphene multifunctional coating for electromagnetic shielding of the present application; In the figure: the mutual distance or size is exaggerated to show the position of each part, and the schematic diagram is only for illustration. DETAILED DESCRIPTION

[0040] It should be noted that the following detailed description is exemplary and is intended to provide further explanation of the present application. Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this application belongs.

[0041] It should be noted that the terms used herein are only for the purpose of describing specific embodiments and are not intended to limit exemplary embodiments according to the present application. As used herein, the singular form is intended to include the plural form unless the context clearly indicates otherwise, and it should also be understood that when the terms "comprise" and / or "include" are used in the specification, there is a reference to the presence of a feature, step, operation, device, component, and / or combinations thereof.

[0042] In a typical embodiment of the present application, as shown in Figure 1 A preparation method of a graphene composite coating with multifunctional properties is proposed, which specifically comprises the following steps: S1: substrate processing, forming a polymer liquid film on the surface of the substrate material by coating method, and high-temperature treating the polymer to form a polymer film; S2: laser induction, carbonizing the polymer film by laser to form a laser-induced graphene (LIG) coating; S3: adding functional particles, doping granular nanomaterials or their corresponding solutions on the surface of the LIG coating by spraying, extrusion molding, etc., to form a composite structure; S4: multifunctional coating integration, removing solvents, etc. by post-treatment methods such as post-heating and laser induction, so that the nanoparticles and the LIG coating are stably combined, and a graphene-based multifunctional composite coating is obtained.

[0043] In step S1, the high-temperature treatment of the polymer liquid film allows the liquid film to form a solid state, and also increases the bonding force between the PI film and the substrate. The high-temperature treatment can be oven heating or heating table heating.

[0044] Using the preparation method of the present application, graphene composite coatings with various morphologies can be prepared, and the obtained coating can be a large-area coating (as shown in Figure 3 and a patterned coating (as shown in Figure 4The application is suitable for more flexible and extensive application sites, and has simple processing process, short time consumption and low cost; the preparation method can not only uniformly disperse the material, but also has strong coating bonding force, and can be widely adapted to various substrates; and multifunctional integration of the graphene composite coating is realized, and the graphene composite coating has multiple strong synergistic functions such as sensing, ice prevention and removal, electromagnetic shielding and the like.

[0045] The preparation method of the application can obtain graphene composite coatings with different structures by adjusting laser power, scanning times and concentration of doped nanoparticles, so as to realize the adjustment of the electrical performance and functional performance of the coating. Figure 10 And Figure 11 The graphene coatings with different microstructures are obtained.

[0046] After the graphene coating is prepared, the graphene is compounded with functional nanoparticles, and the specific type of the functional nanoparticles can be selected according to the requirements of the use scene of the composite material, and the graphene / CNT composite coating and the graphene / Pt composite coating are further described through specific implementation examples. Embodiment

[0047] A preparation method of a graphene / CNT composite coating with piezoresistive sensing and ice prevention and removal characteristics, comprising the following steps: S1: substrate coating processing, a polyimide precursor solution PAA is formed into a PAA film on the surface of a glass fiber composite material by extrusion molding, and the polymer is subjected to imidization treatment to form a PI coating; S2: laser induction, a laser is used to perform single laser scanning on the PI coating in an air atmosphere at a power of 0.75 W, a scanning speed of 50 mm / s and a printing resolution of 500, to form a laser-induced graphene LIG coating; S3: adding functional particles, a CNT dispersion liquid is sprayed on the surface of the LIG by using a spray pen, and the LIG solvent is volatilized through the electrothermal effect of the LIG, to finally obtain a LIG / CNT composite coating, as shown in Figure 8 . Embodiment

[0048] A preparation method of a graphene / CNT composite coating with piezoresistive sensing and ice prevention and removal characteristics, comprising the following steps: S1: substrate coating processing, a polyimide precursor solution PAA is formed into a PAA film on the surface of a glass fiber composite material by extrusion molding, and the polymer is subjected to imidization treatment to form a PI coating; S2: laser induction, a laser is used to perform multiple laser scanning on the PI coating in an air atmosphere at a power of 0.75 W, a scanning speed of 50 mm / s and a printing resolution of 500, to form a laser-induced graphene LIG coating; S3; Add functional particles, use an airbrush to spray CNT dispersion onto LIG surface, and at the same time evaporate LIG solvent through the electrothermal effect of LIG to finally obtain LIG / CNT composite coating. Example

[0049] A method for preparing a graphene / CNT composite coating with piezoresistive sensing and anti-icing / de-icing properties includes the following steps: S1: Base coating processing, the polyimide precursor solution PAA is extruded to form a PAA film on the surface of the glass fiber composite material, and the polymer is imidized to form a PI coating. S2: Laser-induced, in an air atmosphere, a laser is used to perform a single laser scan on the PI coating at a power of 2W, a scanning speed of 50 mm / s and a printing resolution of 500 to form a laser-induced graphene LIG coating. S3: Add functional particles, use an airbrush to spray the CNT dispersion onto the LIG surface, and at the same time, use the electrothermal effect of LIG to evaporate the LIG solvent, finally obtaining a LIG / CNT composite coating.

[0050] The surface of the composite coating obtained in Example 1 was observed using a scanning electron microscope (SEM), and the results are as follows: Figure 10 As shown in (a), the LIG film surface is a plane composed of fibers during a single laser scan. The surface of the composite coating obtained in Example 2 was observed using a scanning electron microscope (SEM), and the results are as follows. Figure 10 As shown in (b), the LIG obtained after three laser scans gradually exhibits a convex shape along the laser scanning path and produces a microcrack structure. The surface of the composite coating obtained in Example 3 was observed using a scanning electron microscope (SEM), and the results are as follows. Figure 11 As shown in the figure, when the laser power is 2W, the LIG gradually exhibits a fibrous structure. Raman spectroscopy was used to characterize the coating structure, and the results are as follows. Figure 12 As shown in the figure. All of the above structures exhibit the D peak (1350 cm⁻¹) of graphene. -1 ), G peak (1580 cm) -1 ) and 2D peak (2700 cm) -1 This demonstrates that the preparation method of the present invention yields a graphene structure. The prepared composite coating was applied to a piezoresistive sensor, and the tested sensing performance results are as follows: Figure 14 As shown in the figure, the cyclic curve of resistance versus strain shows that the obtained coating exhibits excellent sensing performance, with a sensing coefficient reaching 690. When the prepared composite coating is used for active anti-icing, the tested contact angle is as follows. Figure 15 As shown in the figure, the contact angle between the coating and water can reach 155°. When the prepared composite coating is used for active anti-icing, the tested contact angle is as follows... Figure 15As shown in the figure, the contact angle between the coating and water can reach 155°. When the prepared composite coating was used for electrothermal de-icing, the test results were as follows... Figure 16 As shown in the figure, when the power input is 4W and the surface temperature of the graphene film is 200°C, the volume is 8 cm³. 3 The ice was successfully melted within 4 minutes. Example

[0051] A method for preparing a graphene / Pt composite coating with energy storage properties includes the following steps: S1: Base coating processing, the polyimide precursor solution PAA is extruded to form a PAA film on the surface of the glass fiber composite material, and the polymer is imidized to form a PI coating. S2: Laser-induced, in an air atmosphere, a laser is used to perform a single laser scan on the PI coating at a power of 1W, a scanning speed of 50 mm / s and a printing resolution of 500 to form a laser-induced graphene LIG coating. S3: Add functional particles, apply Pt powder to the surface of the above LIG coating by coating method, and then use laser to induce to form LIG / Pt composite coating.

[0052] The surface of the composite coating obtained in Example 4 was observed using a scanning electron microscope (SEM), and the results are as follows: Figure 13 As shown in the figure, the LIG film surface is a plane composed of fibers during a single laser scan. The prepared composite structure was applied to supercapacitor electrode materials, and the tested capacitor performance results are as follows. Figure 17 As shown in the figure, the cyclic volt-ampere characteristic curves reveal that the composite structure exhibits excellent energy storage performance and stability, achieving a maximum specific capacitance of 117.3 mF / cm². 2 . Example

[0053] A method for preparing a graphene / Ni composite coating with electromagnetic shielding properties includes the following steps: S1: Base coating processing, the polyimide precursor solution PAA is extruded to form a PAA film on the surface of the composite material, and the polymer is imidized to form a PI coating. S2: Laser-induced, in an air atmosphere, a laser is used to perform a single laser scan on the PI coating at a power of 1.5W, a scanning speed of 50 mm / s and a printing resolution of 500 to form a laser-induced graphene LIG coating. S3: Add functional particles, apply Pt powder to the surface of the above LIG coating by coating method, and then use laser to induce to form LIG / Ni composite coating.

[0054] The prepared composite structure was applied to electromagnetic shielding materials, and the tested capacitor performance results are as follows: Figure 18 As shown in the figure, the cyclic volt-ampere characteristic curves show that the composite structure exhibits microwave shielding performance, achieving an electromagnetic shielding effectiveness of 20 dB.

[0055] It should be understood that the foregoing only illustrates some embodiments, and changes, modifications, additions, and / or variations can be made without departing from the scope and spirit of the disclosed embodiments. These embodiments are illustrative and not restrictive. Furthermore, the described embodiments relate to those currently considered most practical and preferred, and should be understood as not being limited to the disclosed embodiments, but rather intended to cover different modifications and equivalent arrangements included within the spirit and scope of those embodiments. Moreover, the various embodiments described above can be used in conjunction with other embodiments; for example, an aspect of one embodiment can be combined with an aspect of another embodiment to achieve yet another embodiment. Additionally, individual features or components of any given component can constitute another embodiment.

[0056] The above description is merely a preferred embodiment of the present invention and is not intended to limit the invention. Various modifications and variations can be made to the present invention by those skilled in the art. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the scope of protection of the present invention.

Claims

1. A method for preparing a graphene composite coating having multifunctional properties, characterized in that, The method comprises the following steps: a substrate processing step, in which a carbon source polymer solution is coated on a surface of a substrate material to form a polymer liquid film, and the polymer is treated to form a polymer film; a laser induction step, in which the polymer film is carbonized by laser to form a laser-induced graphene (LIG) coating; a functional particle adding step, in which nanoparticles are doped on the surface of the LIG coating by coating to form a composite structure; a multifunctional coating integration step, in which a graphene-based multifunctional composite coating is formed by post-processing.

2. The method of claim 1, wherein the graphene composite coating is prepared by a process comprising: The carbon source polymer solution is a solution of polyimide, polyphenylene sulfide, polyetherimide or polyether ether ketone powder in an organic solvent, or a precursor solution of each of the powders.

3. The method for preparing the graphene composite coating as described in claim 1, characterized in that, The coating method of the carbon source polymer solution is an automatic controllable extrusion molding method, the extrusion pressure is 0.1-100 psi, the extrusion speed is 10-100 mm / s, and the needle diameter is 0.1-0.61 mm.

4. The method for preparing the graphene composite coating as described in claim 1, characterized in that, The substrate material is a glass fiber composite material, glass, plastic, metal or fabric.

5. The method for preparing the graphene composite coating as described in claim 1, characterized in that, The polymer is treated at a high temperature to form a polymer film.

6. The method for preparing the graphene composite coating as described in claim 1, characterized in that, The laser induction adopts a CO2 laser, the laser focal length, scanning speed and pulse resolution of the CO2 laser are 33.1-43.1 mm, 2.54-203.2 mm / s and 1-1000 ppi / inch respectively, the laser power is 0.1-50 W, and the laser carbonization is performed at room temperature in an atmospheric environment.

7. The method for preparing the graphene composite coating as described in claim 1, characterized in that, The nanoparticles are carbon nanotubes, MXene, polyaniline, Pt or Ni metal particles; when the functional particles are added, the particulate nanomaterial or its corresponding solution is doped on the surface of the LIG coating by coating.

8. The method for preparing graphene composite coating as described in claim 1 or 7, characterized in that, The coating method of the nanoparticles includes extrusion molding, spray pen spraying or doctor blade coating.

9. The method for preparing the graphene composite coating as described in claim 1, characterized in that, The specific steps of the multifunctional coating integration include: removing the solvent by a post-processing method to stably combine the nanoparticles with the LIG coating, and obtaining a graphene-based multifunctional composite coating.

10. The method for preparing the graphene composite coating as described in claim 1, characterized in that, The post-processing method includes heating, electrophoretic deposition and laser induction; the functions of the multifunctional coating include sensing, anti-icing / icing removal, electromagnetic shielding, energy storage and high temperature resistance.

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