Probing the active site in single-atom oxygen reduction catalysts via operando X-ray and electrochemical spectroscopy
學年 109
學期 1
出版(發表)日期 2020-08-25
作品名稱 Probing the active site in single-atom oxygen reduction catalysts via operando X-ray and electrochemical spectroscopy
作品名稱(其他語言)
著者 H. T. Lien; S. T. Chang; P. T. Chen; D. P. Wong; Y. C. Chang; Y. R. Lu; C. L. Dong; C. H. Wang; K. H. Chen; L. C. Chen
單位
出版者
著錄名稱、卷期、頁數 Nature Communications 11, 4233 (8 pages)
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.
關鍵字 Characterization and analytical techniques;Electrocatalysis;Fuel cells
語言 en_US
ISSN 2041-1723
期刊性質 國外
收錄於 SCI
產學合作
通訊作者
審稿制度
國別 GBR
公開徵稿
出版型式 ,電子版
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機構典藏連結 ( http://tkuir.lib.tku.edu.tw:8080/dspace/handle/987654321/120712 )