RESEARCH ARTICLE
. State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, China.. School of Chemistry and Materials Science, Ludong University, Yantai 264025, China.. Center for Computational Chemistry and Molecular Simulation, College of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, China.. Oil & Gas Field Applied Chemistry Key Laboratory of Sichuan Province, College of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, China
收稿日期：
2020-12-31
录用日期：
2021-02-05
发布日期：
2021-02-05
摘要
In this work, the detailed oxygen reduction reaction (ORR) catalytic performance of M-N O (M= Fe, Co, and Ni; = 1–4) has been explored via the detailed density functional theory method. The results suggest that the formation energy of M-N O shows a good linear relationship with the number of doped O atoms. The adsorption manner of O on M-N O changed from end-on ( = 1 and 2) to side-on ( = 3 and 4), and the adsorption strength gradually increased. Based on the results for binding strength of ORR intermediates and the Gibbs free energy of ORR steps on the studied catalysts, we screened out two highly active ORR catalysts, namely Co-N O and Ni-N O , which possess very small overpotentials of 0.27 and 0.32 V, respectively. Such activities are higher than the precious Pt catalyst. Electronic structure analysis reveals one of the reasons for the higher activity of Co-N O and Ni-N O is that they have small energy gaps and moderate highest occupied molecular orbital energy levels. Furthermore, the results of the density of states reveal that the O doping can improve the electronic structure of the original catalyst to tune the adsorption of the ORR intermediates.
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