Theoretical Study on B-doped FeN4 Catalyst for Potential-Dependent Oxygen Reduction Reaction |
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| Authors: | Ziwei Wang Dr. Yanyang Qin Dr. Tiantian Wu Dr. Jianrui Zhang Prof. Shujiang Ding Prof. Yaqiong Su |
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| Affiliation: | School of Chemistry, Engineering Research Center of Energy Storage Materials and Devices of Ministry of Education, State Key Laboratory of Electrical Insulation and Power Equipment, National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology, Xi'an Jiaotong University, Xi'an, 710049 China |
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| Abstract: | Electrochemical reactions mostly take place at a constant potential, but traditional DFT calculations operate at a neutral charge state. In order to really model experimental conditions, we developed a fixed-potential simulation framework via the iterated optimization and self-consistence of the required Fermi level. The B-doped graphene-based FeN4 sites for oxygen reduction reaction were chosen as the model to evaluate the accuracy of the fixed-potential simulation. The results demonstrate that *OH hydrogenation gets facile while O2 adsorption or hydrogenation becomes thermodynamically unfavorable due to the lower d-band center of Fe atoms in the constant potential state than the neutral charge state. The onset potential of ORR over B-doped FeN4 by performing potential-dependent simulations agree well with experimental findings. This work indicates that the fixed-potential simulation can provide a reasonable and accurate description on electrochemical reactions. |
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| Keywords: | boron doping constant potential states density functional calculations electrochemical reaction modelling oxygen reduction reaction |
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