Journal
CHEM
Volume 6, Issue 12, Pages 3440-3454Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2020.10.027
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Funding
- National Key Projects for Fundamental Research and Development of China [2016YFA0202804]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17000000]
- Nanyang Technological University [M4080977.120]
- Ministry of Education of Singapore (AcRF Tier 1) [M4011021.120, 2015-T1-002-108]
- National Natural Science Foundation of China [21590792, 91426302, 21433005]
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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 Fe-57 Mossbauer 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 (*0(2)(-)) 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.
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