催化作用
介电谱
电化学
钴
金属
过渡金属
材料科学
吸收光谱法
吸附
光谱学
化学
光化学
氧化还原
无机化学
氧气
电极
物理化学
有机化学
冶金
物理
量子力学
作者
Hsiang-Ting Lien,Shinn‐Jen Chang,Po‐Tuan Chen,Deniz Wong,Yu-Chung Chang,Ying-Rei Lu,Chung‐Li Dong,Chenhao Wang,Kuei‐Hsien Chen,Li‐Chyong Chen
标识
DOI:10.1038/s41467-020-17975-y
摘要
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–N x /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 Co 2+ center, with end-on coordination forming a Co 2+ -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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