Theoretical Studies of Metal-N-C for Oxygen Reduction and Hydrogen Evolution Reactions in Acid and Alkaline Solutions

Authors

Xue-Ping Qin, 1. Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, China;Follow
Shang-Qian Zhu, 1. Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, China;
Lu-Lu Zhang, 1. Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, China;
Shu-Hui Sun, 2. INRS-énergie, Matériaux et Télécommunications, 1650 Boulevard Lionel Boulet, Varennes, Québec, Canada J3X 1S2;
Min-Hua Shao, 1. Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, China;Follow

Corresponding Author

Xue-Ping Qin(xqinaa@connect.ust.hk);
Min-Hua Shao(kemshao@ust.hk)

Abstract

Single atom catalysts (SAC) have been regarded as the promising alternatives to platinum group metals due to their low costs and potentially high catalytic activities in various electrocatalytic reactions. The atomic mechanism understanding of activity discrepancy among different metal and nitrogen co-doped carbon-based catalysts is still lacking. Here, non-precious metal and nitrogen co-doped carbons (Me-N-C, Me = Fe and Co) as the model catalysts are investigated by combining experimental and theoretical studies to explore the catalytic activities and corresponding reaction mechanisms toward oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) at universal pHs. Atomic theoretical simulations suggest that Fe-N-C has higher ORR activity than Co-N-C due to its lower reaction barrier of the rate-determining step, while the activity trend is reversed for HER. Our simulation results are consistent with experimental observations.

Graphical Abstract

Keywords

oxygen reduction reaction, hydrogen evolution reaction, electrocatalysts, single atom catalysts, theoretical calculations

DOI Link

https://doi.org/10.13208/j.electrochem.201248

Publication Date

2021-04-28

Online Available Date

2021-03-20

Revised Date

2021-03-10

Received Date

2021-02-02

Recommended Citation

Xue-Ping Qin, Shang-Qian Zhu, Lu-Lu Zhang, Shu-Hui Sun, Min-Hua Shao. Theoretical Studies of Metal-N-C for Oxygen Reduction and Hydrogen Evolution Reactions in Acid and Alkaline Solutions[J]. Journal of Electrochemistry, 2021 , 27(2): 185-194.
DOI: 10.13208/j.electrochem.201248
Available at: https://jelectrochem.xmu.edu.cn/journal/vol27/iss2/4