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

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作者
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
Li-Chyong Chen
机构
[1] National Taiwan University,Center for Condensed Matter Sciences
[2] National Taiwan University,Center of Atomic Initiative for New Materials
[3] National Taiwan University of Science and Technology,Department of Materials Science and Engineering
[4] National Taipei University of Technology,Department of Vehicle Engineering
[5] Institute of Atomic and Molecular Sciences,Department of Physics
[6] Academia Sinica,undefined
[7] National Synchrotron Radiation Research Center,undefined
[8] Tamkang University,undefined
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Nature Communications | / 11卷
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摘要
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.
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