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CN-122013246-A - Electrode for hydrogen evolution of electrolyzed water, preparation method thereof and application of electrode in water electrolysis device

CN122013246ACN 122013246 ACN122013246 ACN 122013246ACN-122013246-A

Abstract

The invention discloses an electrode for hydrogen evolution of electrolyzed water, which takes carbon cloth as a substrate, wherein micron-order linear N, N-dimethylformamide complex derived cobalt-based metal oxide grows on the surface of the carbon cloth. The invention also provides a preparation method of the electrode for hydrogen evolution of the electrolyzed water. The electrode provided by the invention has a micron-sized linear structure, enhances the regulation and control on the micro-environment of a catalyst-electrolyte interface, can promote the rapid transfer and delivery of interface water molecules, protons separated from reaction intermediates and product oxygen molecules in electrolyte so as to maintain higher catalytic activity and current stability in a severe acidic environment, and the formation of N, N-dimethylformamide complex optimizes the electronic structure of cobalt-based metal oxide, improves the interface of the catalyst-electrolyte and improves the intrinsic activity and stability, so that the electrode is expected to overcome the severe conditions in the acidic environment and has important practical significance for realizing the large-scale development of green hydrogen production from electrolyzed water.

Inventors

  • DONG BIN
  • YU NING
  • CHAI YONGMING

Assignees

  • 中国石油大学(华东)

Dates

Publication Date
20260512
Application Date
20260203

Claims (10)

  1. 1. An electrode for hydrogen evolution of electrolyzed water is characterized in that carbon cloth is used as a substrate, and micron-scale linear N, N-dimethylformamide complex-derived cobalt-based metal oxide grows on the surface of the carbon cloth.
  2. 2. A method of producing an electrode for hydrogen evolution from electrolyzed water according to claim 1, comprising the steps of: 1) Carrying out hydrothermal treatment on the carbon cloth in a cobalt-containing mixed solution, and then carrying out calcination treatment to obtain cobalt-based metal oxide; 2) And (3) carrying out electrochemical activation treatment on the prepared cobalt-based metal oxide in an N, N-dimethylformamide solution to obtain the electrode containing the cobalt-based metal oxide derived from the N, N-dimethylformamide complex.
  3. 3. The method for producing an electrode for hydrogen evolution from electrolyzed water according to claim 1, wherein the cobalt-containing mixed solution in step 2) is a mixed solution composed of cobalt salt, fluorine salt and urea.
  4. 4. The method for preparing an electrode for hydrogen evolution from electrolyzed water according to claim 3, wherein the cobalt salt is one or more of cobalt nitrate, cobalt chloride and cobalt sulfate, the fluorine salt comprises ammonium fluoride, and the molar ratio of the cobalt salt, the fluorine salt and urea is 0.5-1.5:1.5-2.5:4-6.
  5. 5. The method for preparing an electrode for hydrogen evolution from electrolyzed water according to claim 4, wherein the hydrothermal treatment in the step 2) is performed under the process condition that the reaction is maintained for 4-12 hours at a hydrothermal temperature of 120-180 ℃.
  6. 6. The method for producing an electrode for electrolytic water hydrogen evolution according to claim 5, wherein the process conditions of the calcination treatment in step 2) are calcination in an air atmosphere at a temperature of 250 to 350 ℃ for 1.5 to 2.5 hours.
  7. 7. The method for producing an electrode for hydrogen evolution from electrolyzed water according to claim 6, wherein the activation treatment of cobalt-based metal oxide is carried out in N, N-dimethylformamide by a constant voltage method in step 3).
  8. 8. The method for preparing an electrode for hydrogen evolution from electrolyzed water according to claim 7, wherein the N, N-dimethylformamide solution is AR not less than 99.5%, the activated voltage interval is 1.8-2.4V vs. SHE, and the activation time is 5-20 minutes.
  9. 9. The method for producing an electrode for hydrogen evolution from electrolyzed water according to claim 1, further comprising vacuum drying the N, N-dimethylformamide complex-derived cobalt-based metal oxide produced in step 3).
  10. 10. A water electrolysis apparatus comprising the electrode for hydrogen evolution from electrolyzed water according to claim 1 or the electrode for hydrogen evolution from electrolyzed water prepared by the preparation method according to any one of claims 2 to 9.

Description

Electrode for hydrogen evolution of electrolyzed water, preparation method thereof and application of electrode in water electrolysis device Technical Field The invention belongs to the technical field of materials, and particularly relates to an electrode for hydrogen evolution of electrolyzed water, and further relates to an electrode containing a catalyst of cobalt-based metal oxide derived from N, N-dimethylformamide complex, a preparation method thereof and application thereof in a water electrolysis device. Background In the context of energy conversion, the potential of hydrogen as a clean energy source is increasingly prominent, and efficient hydrogen production technology is key. Proton Exchange Membrane Water Electrolysis (PEMWE) is a very promising technology for producing hydrogen from water electrolysis due to its efficient proton transport capacity. However, the Oxygen Evolution Reaction (OER) of its anode presents a serious challenge to the catalyst in strongly acidic environments. In the acidic OER process, the rapid accumulation of protons on the catalyst surface accelerates the electron depletion at the active metal sites, leading to irreversible excessive oxidation and even dissolution deactivation of the metal. Traditional strategies, such as doping and hybridization, mainly focus on regulating and controlling the electronic structure of a catalyst body to optimize the adsorption energy of an intermediate, but often neglect the key role of a real place where the reaction of a catalyst-electrolyte interface occurs, and in recent years, research discovers that the interface microenvironment has a decisive influence on the reaction efficiency, and the combination of the optimization of the intrinsic activity of the catalyst and the precise regulation of the interface microenvironment is an effective way for breaking through the bottleneck of acid OER dynamics. In addition to the intrinsic activity of the catalyst and the interfacial microenvironment, the behavior of the gas bubbles generated during oxygen evolution is also a central but often neglected factor affecting the efficiency and stability of the PEMWE. If oxygen bubbles generated on the surface of the electrode cannot be desorbed in time, a gas covering layer can be formed, active sites are physically shielded, the system resistance is increased, and more serious, the bubbles can generate huge tensile stress on catalyst particles in the slow growth and desorption processes, so that pulverization and falling of the catalytic layer are directly caused. Thus, efficient bubble management is critical to maintaining catalyst macro-stability. Disclosure of Invention The present invention aims to solve at least one of the technical problems in the related art to some extent. To this end, the main object of the present invention is to provide an electrode for the hydrogen evolution of electrolyzed water with high catalytic activity and long-term stability. The invention aims to provide a preparation method of the electrode for hydrogen evolution of electrolyzed water. The invention further provides a water electrolysis device containing the electrolytic water hydrogen-evolution electrode. The invention aims at realizing the following technical scheme: An electrode for hydrogen evolution of electrolyzed water takes carbon cloth as a substrate, and micron-scale linear N, N-dimethylformamide complex-derived cobalt-based metal oxide grows on the surface of the carbon cloth. As the same inventive concept, the invention also provides a preparation method of an electrode for hydrogen evolution of electrolyzed water, comprising the following steps: 1) Carrying out hydrothermal treatment on the carbon cloth in a cobalt-containing mixed solution, and then carrying out calcination treatment to obtain cobalt-based metal oxide; 2) And (3) carrying out electrochemical activation treatment on the prepared cobalt-based metal oxide in an N, N-dimethylformamide solution to obtain the electrode of the cobalt-based metal oxide derived from the N, N-dimethylformamide complex. The N, N-dimethylformamide is a DMF polar aprotic solvent, the carbonyl oxygen atom of the DMF polar aprotic solvent has stronger coordination capacity, and under the action of an electric field, when the cobalt atom on the surface is oxidized to a high valence state, the chemical bond of the DMF polar aprotic solvent is shortened and unstable, and DMF molecules can adsorb and coordinate to the high valence cobalt sites to form a Co-DMF surface complex intermediate. In certain embodiments, the cobalt-containing mixed solution is a mixed solution of cobalt salt, fluoride salt and urea. The ammonia and CO 2 are slowly decomposed and released by urea at high temperature to provide alkaline environment, while the ammonium fluoride is used as a key morphology control agent, F - ions can be selectively adsorbed on the specific surface of the crystal to inhibit the lateral growth of the crystal,