Probing the active site in single-atom oxygen reduction catalysts via operando X-ray and electrochemical spectroscopy

Hsiang-Ting Lien, Sun-Tang Chang, Po-Tuan Chen, Deniz P. Wong, Yu-Chung Chang, Ying-Rei Lu, Chung-Li Dong, Chen-Hao Wang, Kuei-Hsien Chen () and Li-Chyong Chen ()
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Hsiang-Ting Lien: National Taiwan University
Sun-Tang Chang: National Taiwan University of Science and Technology
Po-Tuan Chen: National Taiwan University
Deniz P. Wong: Institute of Atomic and Molecular Sciences, Academia Sinica
Yu-Chung Chang: National Taiwan University
Ying-Rei Lu: National Synchrotron Radiation Research Center
Chung-Li Dong: Tamkang University
Chen-Hao Wang: National Taiwan University of Science and Technology
Kuei-Hsien Chen: National Taiwan University
Li-Chyong Chen: National Taiwan University

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract Nonnoble metal catalysts are low-cost alternatives to Pt for the oxygen reduction reactions (ORRs), which have been studied for various applications in electrocatalytic systems. Among them, transition metal complexes, characterized by a redox-active single-metal-atom with biomimetic ligands, such as pyrolyzed cobalt–nitrogen–carbon (Co–Nx/C), have attracted considerable attention. Therefore, we reported the ORR mechanism of pyrolyzed Vitamin B12 using operando X-ray absorption spectroscopy coupled with electrochemical impedance spectroscopy, which enables operando monitoring of the oxygen binding site on the metal center. Our results revealed the preferential adsorption of oxygen at the Co2+ center, with end-on coordination forming a Co2+-oxo species. Furthermore, the charge transfer mechanism between the catalyst and reactant enables further Co–O species formation. These experimental findings, corroborated with first-principle calculations, provide insight into metal active-site geometry and structural evolution during ORR, which could be used for developing material design strategies for high-performance electrocatalysts for fuel cell applications.

Date: 2020
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DOI: 10.1038/s41467-020-17975-y

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