Identification of the Electronic and Structural Dynamics of Catalytic Centers in Single-Fe-Atom Material

Xuning Li, Chang Su Cao, Sung Fu Hung, Ying Rui Lu, Weizheng Cai, Alexandre I. Rykov, Shu Miao, Shibo Xi, Hongbin Yang, Zehua Hu, Junhu Wang, Jiyong Zhao, Esen Ercan Alp, Wei Xu, Ting Shan Chan, Haoming Chen, Qihua Xiong, Hai Xiao, Yanqiang Huang*, Jun LiTao Zhang, Bin Liu

*Corresponding author for this work

研究成果: Article同行評審

4 引文 斯高帕斯(Scopus)

摘要

The lack of model single-atom catalysts (SACs) and atomic-resolution operando spectroscopic techniques greatly limits our comprehension of the nature of catalysis. Herein, based on the designed model single-Fe-atom catalysts with well-controlled microenvironments, we have explored the exact structure of catalytic centers and provided insights into a spin-crossover-involved mechanism for oxygen reduction reaction (ORR) using operando Raman, X-ray absorption spectroscopies, and the developed operando 57Fe Mössbauer spectroscopy. In combination with theoretical studies, the N-FeN4C10 moiety is evidenced as a more active site for ORR. Moreover, the potential-relevant dynamic cycles of both geometric structure and electronic configuration of reactive single-Fe-atom moieties are evidenced via capturing the peroxido (∗O2) and hydroxyl (∗OH) intermediates under in situ ORR conditions. We anticipate that the integration of operando techniques and SACs in this work shall shed some light on the electronic-level insight into the catalytic centers and underlying reaction mechanism.

原文English
頁(從 - 到)3440-3454
頁數15
期刊Chem
6
發行號12
DOIs
出版狀態Published - 3 十二月 2020

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