Citation: Leiming Tao, Penghu Guo, Weiling Zhu, Tianle Li, Xiantai Zhou, Yongqing Fu, Changlin Yu, Hongbing Ji. Highly efficient mixed-metal spinel cobaltite electrocatalysts for the oxygen evolution reaction[J]. Chinese Journal of Catalysis, ;2020, 41(12): 1855-1863. doi: 10.1016/S1872-2067(20)63638-5 shu

Highly efficient mixed-metal spinel cobaltite electrocatalysts for the oxygen evolution reaction

a School of Science, Guangdong University of Petrochemical Technology, Maoming 525000, Guangdong, China;
b Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China;
c Faculty of Engineering and Environment, Northumbria University, Newcastle upon Tyne, NE1 8ST, UK;
d Fine Chemical Industry Research Institute, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, Guangdong, China

Received Date: 11 March 2020
Revised Date: 14 April 2020

Fund Project: This work was supported by the National Natural Science Foundation of China (21938001, 21576302, 21878344, 21961160741), Natural Science Foundation of China-SINOPEC Joint Fund (U1663220), Featured Innovation Project of Guangdong Education Department (2018KTSCX144, 2016KTSCX087), Guangdong Provincial Key R&D Programme (2019B110206002), the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (2017BT01C102), Scientific Research Fund of Natural Science Foundation of Guangdong University of Petrochemical Technology (2019rc019, 2019rc053), Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme (2019), Key Natural Science Research Projects of Guangdong Provincial Universities (2019KZDXM010), Guangdong Basic and Applied Basic Research Foundation (2019A1515011249), the UK Engineering and Physical Sciences Research Council (EPSRC) for support under grant EP/P018998/1, and Newton Mobility Grant (IE161019) through the Royal Society and the National Natural Science Foundation of China.

Cation substitution in spinel cobaltites (e.g., ACo₂O₄, in which A=Mn, Fe, Co, Ni, Cu, or Zn) is a promising strategy to precisely modulate their electronic structure/properties and thus improve the corresponding electrochemical performance for water splitting. However, the fundamental principles and mechanisms are not fully understood. This research aims to systematically investigate the effects of cation substitution in spinel cobaltites derived from mixed-metal-organic frameworks on the oxygen evolution reaction (OER). Among the obtained ACo₂O₄ catalysts, FeCo₂O₄ showed excellent OER performance with a current density of 10 mA·cm^-2 at an overpotential of 164 mV in alkaline media. Both theoretical calculations and experimental results demonstrate that the Fe substitution in the crystal lattice of ACo₂O₄ can significantly accelerate charge transfer, thereby achieving enhanced electrochemical properties. The crystal field of spinel ACo₂O₄, which determines the valence states of cations A, is identified as the key factor to dictate the OER performance of these spinel cobaltites.
- Cation-substituted spinel cobaltites,
- Crystal field,
- Oxygen evolution reaction,
- Water-splitting,
- Electrocatalysis
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