Citation: Mingliang Wu, Yehui Zhang, Zhanzhao Fu, Zhiyang Lyu, Qiang Li, Jinlan Wang. Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction[J]. Acta Physico-Chimica Sinica, ;2023, 39(1): 220700. doi: 10.3866/PKU.WHXB202207007 shu

Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction

1.
School of Physics, Southeast University, Nanjing, 211189, China
2.
Jiangsu Key Laboratory for Design and Manufacture of Micro-Nano Biomedical Instruments, School of Mechanical Engineering, Southeast University, Nanjing 211189, China

Corresponding author: Qiang Li, qiang.li@seu.edu.cn Jinlan Wang, jlwang@seu.edu.cn
Received Date: 5 July 2022
Revised Date: 31 July 2022
Accepted Date: 31 July 2022
Available Online: 9 August 2022
Fund Project: the National Key Research and Development Program of China 2021YFA1500700National Natural Science Foundation of China 22033002National Natural Science Foundation of China 22173018

Understanding the origin of the active site activity in the oxygen evolution reaction (OER) electrocatalysts is key for developing efficient electrocatalysts. However, crucial challenges remain due to the complexity of catalyst structure-activity relationships. Herein, various Co-N-C configurations, including single atoms, diatoms, and clusters, were designed to establish structure-activity relationships by first-principles calculations. It was revealed that the Co-N₄ exhibited the best reactivity due to the high coordination number of the metal center and moderate adsorption energies for all reaction intermediates. The diatom and cluster activities originate from the highly coordinated structures formed with reaction intermediates, which serve as coordination ligands. Furthermore, other factors influencing the OER activity based on the Co-N₄ configuration are discussed. For example, the weak metal-metal interaction can further optimize the adsorption of oxygen-containing intermediates by tuning antibonding energy levels of Co-O. Subsequently, an ultralow overpotential of 0.23 V for the OER in CoNi-type4 systems can be obtained by extrapolation of the volcano plot derived from the established structure-adsorption-activity relationships. This work uncovers the underlying OER activity mechanisms of Co-N-C catalysts, which helps to further understanding of high-performance of M-N-C base catalysts and will aid in the future design of high-efficiency OER catalysts.
- Electrocatalysis,
- Oxygen evolution reaction,
- First-principles calculations,
- Structure-activity relationship,
- Weak metal-metal interaction
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