Mechanism of Selective Adsorption of O2 / N2 Based on TM-N-C Coordination Relationship
Faculty of Materials Metallurgy and Chemistry, Jiangxi University of Science and Technology, Ganzhou 341000, China
| Abstract: | The burning of fossil fuels has caused increasingly serious environmental pollution. As a new energy conversion device, fuel cell involves oxygen electrocatalytic reaction, but these reaction processes are complicated and high overpotential, so it is necessary to find suitable catalyst to promote the smooth reaction. The reactants O2 and N2 of oxygen reduction reaction (ORR) and nitrogen reduction reaction (NRR) all come from air, while the products H2O and NH3 are important chemical resources. In this paper, the selective adsorption of O2/N2 by 13 kinds of non-expensive transition metals (TM) anchored by graphene under different N concentration doping conditions was studied by calculation. It was concluded that the higher the content of N in single-vacancy and double-vacancy structures, the better the stability of the substrate, and the stability of the double-vacancy structure is better than that of the single vacancy. The ZrN4 catalytic substrate with the best stability was mainly studied. Through the Mulliken charge distribution and partial wave density of state (PDOS), it was found that its charge distribution was symmetrical and the electron transfer was obvious. Further analysis of the deformed state density of the substrate adsorbing O2 and H2O shows that the catalytic substrate has excellent adsorption and desorption capacity. Except CuN0C4, ZnN0C4, CdN4C0, CdN2C2-o and ZnN2C1 substrates, the other structures have moderate adsorption capacity of reactant O2 and desorption capacity of product H2O, which are potential sources of ORR catalysts in acidic environment. |
| Keywords: | Graphene; Oxygen Reduction Reaction; Nitrogen Reduction Reaction; Density Functional Theory; Single-Atom Doping |
| DOI: | 10.57237/j.mater.2022.02.004 |
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Received: 11 November 2022
Accepted: 29 December 2022
Published Online: 5 January 2023
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