Atomic-scale structure defect repairing method

Abstract

The invention provides an atomic-scale structure defect repairing method, and belongs to the technical field of atomic defect repairing methods.The atomic-scale structure defect repairing method comprises the steps that defective graphene is added into an organic solvent containing a catalyst to be dispersed, and graphene dispersion liquid is obtained; a substrate is cleaned, and then the graphene dispersion liquid is evenly sprayed to the surface of the substrate through a spraying method; according to the invention, the specific catalyst is introduced to synergistically repair the defects of the graphene structure, so that the efficient migration of carbon atoms is realized, and the repair of the amorphous structure is greatly accelerated; the catalyst plays a role in fixing a graphene sheet layer, thermal expansion in the thermal reduction process is reduced, and the stability of graphene during repairing is effectively improved; according to the method, stable conversion of graphene sp2 and repairing of in-plane structural crystal lattices are achieved by using an ultra-high-temperature defect repairing method, so that graphene microdefects are fully repaired, and the heat conductivity coefficient is increased to 1500 W / m.K or above.

Description

Technical Field

[0001] The present invention belongs to the technical field of atomic defect repair methods, and in particular relates to an atomic level structural defect repair method. Background Art

[0002] The defect of the atomic structure model is that the positive charge in the atom is not evenly distributed, but concentrated in the central nuclear region (nucleus), the electrons are moving at high speed instead of being stationary, and the electron arrangement has orbits.

[0003] Graphene's unique two-dimensional crystal structure gives it many excellent properties such as ultra-high specific surface area, high electron mobility and thermal conductivity, and high mechanical strength. As a new type of low-dimensional functional carbon material, graphene has broad and far-reaching application potential in solar cells, electronic devices, transistors, supercapacitors, transparent conductive electrodes, photosensitive elements, biomedicine and gene sequencing, antibacterial devices and other fields. Therefore, high-quality graphene with a perfect structure has become the goal pursued by researchers.

[0004] In the prior art, a large number of amorphous structural defects such as intralayer topological structures and nanopores will remain in the internal structure of graphene after thermal reduction, resulting in many carbon atoms being unable to effectively form a regular six-membered ring structure, which seriously affects the improvement of the thermal conductivity of the graphene film. Summary of the invention

[0005] The purpose of the present invention is to provide a method for repairing atomic-level structural defects, aiming to solve the problem in the prior art that a large number of amorphous structural defects such as intralayer topological structures and nanopores are left in the internal structure of graphene after thermal reduction, resulting in many carbon atoms being unable to effectively form a regular six-membered ring structure, seriously affecting the improvement of the thermal conductivity of the graphene film.

[0006] To achieve the above object, the present invention provides the following technical solutions: A method for repairing atomic-level structural defects comprises the following steps: S1, adding defective graphene into an organic solvent containing a catalyst for dispersion to obtain a graphene dispersion; S2, cleaning the substrate, and then evenly spraying the graphene dispersion onto the surface of the substrate by a spraying method to obtain a fluffy graphene film; S3, drying the graphene film obtained in step S2, and then placing it in a vacuum environment and introducing hydrogen for high-temperature repair. After the repair is completed, cooling it to room temperature, and then removing the graphene film to obtain a repaired graphene film.

[0007] As a preferred solution of the present invention, the catalyst is prepared by mixing one or more of ethanol, γ-mercaptopropyltrimethoxysilane, phenyltriethoxysilane, tetraethylammonium hydroxide, tetrahydrofuran and methanol in any proportion.

[0008] As a preferred solution of the present invention, the organic solvent is prepared by mixing one or more of xylene, ethanol, n-butanol and N-methylpyrrolidone in any proportion.

[0009] As a preferred solution of the present invention, the substrate in step S2 is SiC.

[0010] As a preferred solution of the present invention, the substrate cleaning in step S2 includes the following steps: S21, preparing a mixed solution; S22 Place the SiC substrate in the mixed solution and soak it at a constant temperature for 15-30 minutes. S23, then rinse the SiC substrate with deionized water, and then blow dry with nitrogen gas to complete the cleaning of the SiC substrate.

[0011] As a preferred solution of the present invention, in step S21, 30 ml of H2SO4 is poured into a polytetrafluoroethylene container, and 10 ml of H2O2 is added under stirring to prepare a mixed solution.

[0012] As a preferred solution of the present invention, the temperature of the mixed solution in step S22 is 70-90°C.

[0013] As a preferred solution of the present invention, the spraying method in step S2 is to apply the graphene dispersion on the substrate at a rotation speed of 600-1600600 rpm.

[0014] As a preferred solution of the present invention, the vacuum environment in step S3 is in a vacuum deposition furnace.

[0015] As a preferred solution of the present invention, the temperature in the vacuum deposition furnace is 700-920°C and the pressure is 0.01-55Pa.

[0016] Compared with the prior art, the present invention has the following beneficial effects: 1. In the present invention, by introducing a specific catalyst, the structural defects of graphene are repaired in a coordinated manner, the efficient migration of carbon atoms is achieved, and the repair of the amorphous structure is greatly accelerated; 2. In the present invention, the catalyst plays a role in fixing the graphene sheets, reducing the thermal expansion during the thermal reduction process, and effectively improving the stability of the graphene during repair; 3. In the present invention, by using an ultra-high temperature defect repair method, the stable transformation of graphene sp2 and the repair of the in-plane structural lattice are achieved, so that the graphene microscopic defects are fully repaired and the thermal conductivity is increased to above 1500W / m·K. BRIEF DESCRIPTION OF THE DRAWINGS

[0017] The accompanying drawings are used to provide a further understanding of the present invention and constitute a part of the specification. Together with the embodiments of the present invention, they are used to explain the present invention and do not constitute a limitation of the present invention. In the accompanying drawings: Figure 1 The figure is a process flow chart of the atomic-level structural defect repair method of the present invention. DETAILED DESCRIPTION

[0018] The following will be combined with the drawings in the embodiments of the present invention to clearly and completely describe the technical solutions in the embodiments of the present invention. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without creative work are within the scope of protection of the present invention.

[0019] Example 1 See also Figure 1 , the present invention provides the following technical solutions: A method for repairing atomic-level structural defects comprises the following steps: S1, adding defective graphene into an organic solvent containing a catalyst for dispersion to obtain a graphene dispersion; The catalyst is prepared by mixing one or more raw materials selected from ethanol, γ-mercaptopropyltrimethoxysilane, phenyltriethoxysilane, tetraethylammonium hydroxide, tetrahydrofuran and methanol in any proportion; the organic solvent is prepared by mixing one or more raw materials selected from xylene, ethanol, n-butanol and N-methylpyrrolidone in any proportion; graphene is added to an organic solvent containing a catalyst for dispersion, a specific catalyst is introduced, and structural defects of graphene are repaired in a coordinated manner, efficient migration of carbon atoms is achieved, and repair of amorphous structures is greatly accelerated; the catalyst plays a role in fixing graphene sheets, reduces thermal expansion during thermal reduction, and effectively improves the stability of graphene during repair; S2, cleaning the substrate, and then evenly spraying the graphene dispersion onto the surface of the substrate by a spraying method to obtain a fluffy graphene film; The following steps will be included: S21, preparing a mixed solution; A mixed solution was prepared by pouring 30 ml of H2SO4 into a polytetrafluoroethylene container and adding 10 ml of H2O2 while stirring; S22 Place the SiC substrate in a mixed solution at 70-90°C, heat at a constant temperature, and soak for 15-30 minutes. S23, then rinse the SiC substrate with deionized water, and then blow dry with nitrogen gas, thus completing the cleaning of the SiC substrate; When the graphene dispersion is sprayed onto the SiC substrate, the SiC substrate is first rotated at 600 rpm to fully disperse the solution on the SiC substrate, and then the rotation speed is increased to 800 rpm to thin the prepared film, and finally the rotation speed is increased to 1600 rpm to accelerate the evaporation of the solvent, so that the film is easy to dry and easy to remove; S3, drying the graphene film obtained in step S2, and then introducing hydrogen into the vacuum environment of a vacuum deposition furnace for high-temperature repair. After the repair is completed, cooling to room temperature, and then removing the graphene film to obtain a repaired graphene film; Among them, the dried graphene film is removed and placed in a vacuum deposition furnace with a vacuum environment, and the temperature is raised to 700-920°C, hydrogen is introduced, and high-temperature repair is performed. The temperature in the vacuum deposition furnace is always controlled to be between 700-920°C and the pressure is between 0.01-55Pa.

[0020] Specifically, the catalyst is prepared by mixing one or more of ethanol, γ-mercaptopropyltrimethoxysilane, phenyltriethoxysilane, tetraethylammonium hydroxide, tetrahydrofuran and methanol in any proportion.

[0021] In this embodiment:

[0022] Specifically, the organic solvent is prepared by mixing one or more raw materials selected from the group consisting of xylene, ethanol, n-butanol and N-methylpyrrolidone in any proportion.

[0023] Specifically, the substrate in step S2 is SiC.

[0024] Specifically, the substrate cleaning in step S2 includes the following steps: S21, preparing a mixed solution; S22 Place the SiC substrate in the mixed solution and soak it at a constant temperature for 15-30 minutes. S23, then rinse the SiC substrate with deionized water, and then blow dry with nitrogen gas, thus completing the cleaning of the SiC substrate.

[0025] Specifically, in step S21, 30 ml of H2SO4 is poured into a polytetrafluoroethylene container, and 10 ml of H2O2 is added with stirring to prepare a mixed solution.

[0026] Specifically, the temperature of the mixed solution in step S22 is 70-90°C.

[0027] Specifically, the spraying method in step S2 is to apply the graphene dispersion on the substrate at a rotation speed of 600-1600600 rpm.

[0028] Specifically, the vacuum environment in step S3 is in a vacuum deposition furnace.

[0029] Specifically, the temperature in the vacuum deposition furnace is 700-920° C., and the pressure is 0.01-55 Pa.

[0030] In the present invention, by introducing a specific catalyst, the structural defects of graphene are repaired in a coordinated manner, the efficient migration of carbon atoms is achieved, and the repair of the amorphous structure is greatly accelerated; the catalyst plays a role in fixing the graphene sheets, reduces the thermal expansion during the thermal reduction process, and effectively improves the stability of the graphene during the repair; in the present invention, by using an ultra-high temperature defect repair method, the stable conversion of graphene sp2 and the repair of the in-plane structural lattice are achieved, the graphene microscopic defects are fully repaired, and the thermal conductivity is increased to above 1500W / m·K.

[0031] Finally, it should be noted that the above description is only a preferred embodiment of the present invention and is not intended to limit the present invention. Although the present invention has been described in detail with reference to the aforementioned embodiments, those skilled in the art can still modify the technical solutions described in the aforementioned embodiments or replace some of the technical features therein by equivalents. Any modification, equivalent replacement, improvement, etc. made within the spirit and principle of the present invention shall be included in the protection scope of the present invention.

Claims

1. A method for repairing atomic-level structural defects, characterized in that: The steps include: S1, adding defective graphene into an organic solvent containing a catalyst for dispersion to obtain a graphene dispersion; S2, cleaning the substrate, and then evenly spraying the graphene dispersion onto the surface of the substrate by a spraying method to obtain a fluffy graphene film; S3, drying the graphene film obtained in step S2, and then placing it in a vacuum environment and introducing hydrogen for high-temperature repair. After the repair is completed, cooling it to room temperature, and then removing the graphene film to obtain a repaired graphene film.

2. The method for repairing atomic-level structural defects according to claim 1, characterized in that: The catalyst is prepared by mixing one or more raw materials selected from ethanol, gamma-mercaptopropyltrimethoxysilane, phenyltriethoxysilane, tetraethylammonium hydroxide, tetrahydrofuran and methanol in any proportion.

3. The method for repairing atomic-level structural defects according to claim 2, characterized in that: The organic solvent is prepared by mixing one or more raw materials selected from the group consisting of xylene, ethanol, n-butanol and N-methylpyrrolidone in any proportion.

4. The method for repairing atomic-level structural defects according to claim 3, characterized in that: The substrate in step S2 is SiC.

5. The method for repairing atomic-level structural defects according to claim 4, characterized in that: The substrate cleaning in step S2 includes the following steps: S21, preparing a mixed solution; S22 Place the SiC substrate in the mixed solution and soak it at a constant temperature for 15-30 minutes. S23, then rinse the SiC substrate with deionized water, and then blow dry with nitrogen gas to complete the cleaning of the SiC substrate.

6. The method for repairing atomic-level structural defects according to claim 5, characterized in that: In the step S21, 30 ml of H2SO4 is poured into a polytetrafluoroethylene container, and 10 ml of H2O2 is added under stirring to prepare a mixed solution.

7. The method for repairing atomic-level structural defects according to claim 6, characterized in that: The temperature of the mixed solution in step S22 is 70-90°C.

8. The method for repairing atomic-level structural defects according to claim 7, characterized in that: The spraying method in step S2 is to apply the graphene dispersion on the substrate at a rotation speed of 600-1600600 rpm.

9. The method for repairing atomic-level structural defects according to claim 8, characterized in that: The vacuum environment in step S3 is in a vacuum deposition furnace.

10. The method for repairing atomic-level structural defects according to claim 9, characterized in that: The temperature in the vacuum deposition furnace is 700-920°C and the pressure is 0.01-55Pa.

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