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CN-122013240-A - Preparation method and application of nonmetallic edge doped graphene nano-plate electrocatalyst

CN122013240ACN 122013240 ACN122013240 ACN 122013240ACN-122013240-A

Abstract

The invention provides a preparation method and application of a nonmetal edge doped graphene nano-plate electrocatalyst. The preparation method of the nonmetallic edge doped graphene nano plate electrocatalyst comprises the following steps of (1) mixing and loading graphite powder, a nonmetallic doping element precursor and an organic solvent according to a preset proportion, adding the mixture into a reactor, uniformly mixing, sealing the reactor, and (2) mechanically stripping and doping, namely applying preset mechanical shearing force to a reaction system in the step (1) to strip graphite layers to form graphene nano plates, and synchronously realizing that nonmetallic doping elements are doped at the edges of the graphene nano plates in the stripping process, (3) purifying and collecting, namely collecting the mixture treated in the step (2), washing to remove impurities, and then drying to obtain the nonmetallic edge doped graphene nano plate electrocatalyst. The invention has the advantages of low cost, broad spectrum, high activity, high two-electron oxygen reduction selectivity and the like.

Inventors

  • WANG XIAOXIONG
  • LIU XURAN

Assignees

  • 清华大学深圳国际研究生院

Dates

Publication Date
20260512
Application Date
20260414

Claims (11)

  1. 1. The preparation method of the nonmetallic edge doped graphene nano-plate electrocatalyst is characterized by comprising the following steps of: (1) Mixing and loading, namely adding graphite powder, a nonmetallic doping element precursor and an organic solvent into a reactor according to a preset proportion, and sealing the reactor after uniform mixing; (2) Applying a preset mechanical shearing force to the reaction system in the step (1) to strip graphite layers to form graphene nano plates, and synchronously realizing that the nonmetallic doping elements in the nonmetallic doping element precursor are doped at the edges of the graphene nano plates in the stripping process; (3) And (3) purifying and collecting, namely collecting the mixture treated in the step (2), washing to remove impurities, and drying to obtain the nonmetallic edge doped graphene nano-plate electrocatalyst.
  2. 2. The method according to claim 1, wherein in the step (1), the particle size of the graphite powder is 10 to 5000 mesh.
  3. 3. The preparation method of the non-metal doped element precursor, according to the preparation method of the non-metal doped element precursor, is characterized in that in the step (1), the mass ratio of the graphite powder to the non-metal doped element precursor is 1 (1-10), and the organic solvent is absolute ethyl alcohol.
  4. 4. The method according to claim 1, wherein in the step (1), the reactor is a ball mill tank containing a grinding medium, and in the step (2), a predetermined mechanical shearing force is applied by subjecting the reaction system to a mechanical ball milling treatment.
  5. 5. The method according to claim 4, wherein the mass ratio of the grinding medium to the graphite powder is (50-150): 1, the rotational speed of the mechanical ball milling treatment is 100 rpm-500 rpm, and the continuous ball milling time is 8-48 hours.
  6. 6. The preparation method of the water-based organic electroluminescent display device according to claim 1, wherein in the step (3), the specific operation of washing and impurity removal is that absolute ethyl alcohol washing, acid liquor soaking and ultrapure water washing are sequentially used, and the acid liquor is an HCl solution of 1M.
  7. 7. The method according to claim 1, wherein in the step (1), the nonmetallic doping element in the nonmetallic doping element precursor is at least one of N, P, S, B, F, and the nonmetallic doping element precursor is solid or gas.
  8. 8. A non-metallic edge doped graphene nanoplate electrocatalyst made by the method of any one of claims 1 to 6.
  9. 9. An electrode comprising a conductive substrate and the non-metallic edge doped graphene nanoplate electrocatalyst according to claim 8 supported on the conductive substrate.
  10. 10. The electrode of claim 9, wherein the non-metallic edge doped graphene nanoplate electrocatalyst is supported on the conductive substrate at a loading of 0.1 mg/cm 2 to 0.5 mg/cm 2 .
  11. 11. Use of the non-metallic edge doped graphene nanoplate electrocatalyst of claim 8 in two-electron oxygen reduction to generate hydrogen peroxide.

Description

Preparation method and application of nonmetallic edge doped graphene nano-plate electrocatalyst Technical Field The invention relates to preparation of hydrogen peroxide, in particular to a nonmetallic edge doped graphene nano-plate electrocatalyst, and preparation and application thereof. Background Hydrogen peroxide (H 2O2) is used as a high-value green environment-friendly oxidant and disinfectant, and has irreplaceable strategic positions in the fields of chemical synthesis, metallurgical purification, electronic cleaning, papermaking bleaching, environmental management and the like. Currently, over 95% of the world's H 2O2 is dependent on the traditional anthraquinone process for mass production. However, the process has the problems of complicated flow, high energy consumption, organic waste liquid generation and the like, and meanwhile, the high-concentration H 2O2 has great potential safety hazard in the concentrated storage and transportation process, so that the ever-increasing requirements of miniaturization, dispersion and on-site production in production and use in modern industry are difficult to meet. In order to break the limitation of the traditional production mode, novel dispersive preparation approaches such as a direct oxyhydrogen synthesis method and a photocatalysis method have been widely studied in recent years. Although the methods are in agreement with the concept of instant production and instant use to a certain extent, the method has the fundamental defects that flammable and explosive hydrogen-oxygen mixture is needed to be used in the direct synthesis method of hydrogen-oxygen, the serious explosion risk exists, and the photocatalysis rule is limited by the problems of high photon-generated carrier recombination rate, low solar energy conversion efficiency and the like, so that the large-scale application is difficult to realize. In contrast, the electrocatalytic synthesis technology of H 2O2 based on two-electron oxygen reduction reaction (2 e - ORR) can realize the efficient, safe and in-situ production of H 2O2 by using air (or oxygen) and water as raw materials and being driven by electric energy at normal temperature and normal pressure, and is considered as the most promising green alternative. However, the efficiency of electrocatalytic 2e - ORR is highly dependent on the performance of the catalyst. At present, aiming at the technical requirements of electrocatalytic synthesis of hydrogen peroxide, the existing scheme mainly has three attempts, but has obvious defects that firstly noble metal catalysts such as palladium, platinum and the like are adopted, the activity is high, the cost is high, the secondary pollution of heavy metals is easy to cause, secondly the carbon materials are modified by strong acid oxidation, the conjugated network of a graphene basal plane can be seriously damaged by the method to cause sudden reduction of conductivity, waste acid pollution is large, the catalytic stability is poor, and thirdly the heteroatom doped carbon materials are prepared by adopting the traditional thermal pyrolysis method. In summary, the prior art is difficult to meet the requirements of low cost, high selectivity and environment protection on large-scale production. Therefore, the development of a novel nonmetal electrocatalyst with low cost, broad spectrum, high activity and high two-electron oxygen reduction selectivity becomes a key technical problem to be solved in urgent need for realizing the efficient green in-situ production of H 2O2. It should be noted that the information disclosed in the above background section is only for understanding the background of the application and thus may include information that does not form the prior art that is already known to those of ordinary skill in the art. Disclosure of Invention In order to make up the defects of the prior art, the invention provides a nonmetallic edge doped graphene nano-plate electrocatalyst with low cost, broad spectrum, high activity and high two-electron oxygen reduction selectivity, and preparation and application thereof. The invention adopts the following technical scheme: in a first aspect, a preparation method of a nonmetallic edge-doped graphene nano-plate electrocatalyst is provided, including the following steps: (1) Mixing and loading, namely adding graphite powder, a nonmetallic doping element precursor and an organic solvent into a reactor according to a preset proportion, and sealing the reactor after uniform mixing; (2) Applying a preset mechanical shearing force to the reaction system in the step (1) to strip graphite layers to form graphene nano plates, and synchronously realizing that the nonmetallic doping elements in the nonmetallic doping element precursor are doped at the edges of the graphene nano plates in the stripping process; (3) And (3) purifying and collecting, namely collecting the mixture treated in the step (2), washing to remove impurities, and drying to obtai