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Asymmetric Coordination Regulating D‐Orbital Spin‐Electron Filling in Single‐Atom Iron Catalyst for Efficient Oxygen Reduction.
- Source :
-
Angewandte Chemie . 7/8/2024, Vol. 136 Issue 28, p1-9. 9p. - Publication Year :
- 2024
-
Abstract
- The single‐atom Fe−N−C catalyst has shown great promise for the oxygen reduction reaction (ORR), yet the intrinsic activity is not satisfactory. There is a pressing need to gain a deeper understanding of the charge configuration of the Fe−N−C catalyst and to develop rational modulation strategies. Herein, we have prepared a single‐atom Fe catalyst with the co‐coordination of N and O (denoted as Fe−N/O−C) and adjacent defect, proposing a strategy to optimize the d‐orbital spin‐electron filling of Fe sites by fine‐tuning the first coordination shell. The Fe−N/O−C exhibits significantly better ORR activity compared to its Fe−N−C counterpart and commercial Pt/C, with a much more positive half‐wave potential (0.927 V) and higher kinetic current density. Moreover, using the Fe−N/O−C catalyst, the Zn‐air battery and proton exchange membrane fuel cell achieve peak power densities of up to 490 and 1179 mW cm−2, respectively. Theoretical studies and in situ electrochemical Raman spectroscopy reveal that Fe−N/O−C undergoes charge redistribution and negative shifting of the d‐band center compared to Fe−N−C, thus optimizing the adsorption free energy of ORR intermediates. This work demonstrates the feasibility of introducing an asymmetric first coordination shell for single‐atom catalysts and provides a new optimization direction for their practical application. [ABSTRACT FROM AUTHOR]
- Subjects :
- *IRON catalysts
*PROTON exchange membrane fuel cells
*OXYGEN reduction
Subjects
Details
- Language :
- English
- ISSN :
- 00448249
- Volume :
- 136
- Issue :
- 28
- Database :
- Academic Search Index
- Journal :
- Angewandte Chemie
- Publication Type :
- Academic Journal
- Accession number :
- 178178676
- Full Text :
- https://doi.org/10.1002/ange.202405334