The Asymmetrical Fe-O-Se Bonds in Fe 2 O(SeO 3 ) 2 Boosting Bifunctional Oxygen Electrocatalytic Performance for Zinc-Air Battery

Zinc-air batteries (ZABs) have the advantages of high energy density and rich zinc raw materials. It is a low-cost, green and sustainable energy storage device. At present, one of the key technologies that hinder the large-scale application of ZABs is the design and fabrication oxygen evolution reac...

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Veröffentlicht in:Angewandte Chemie International Edition 2024-12, Vol.63 (51), p.e202412025
Hauptverfasser: Xu, Hui-Min, Yue, Kai-Hang, Song, Lian-Jie, Zhang, Hong-Cheng, Zhu, Hong-Rui, Zhang, Zhi-Jie, Li, Gao-Ren
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Sprache:eng
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Zusammenfassung:Zinc-air batteries (ZABs) have the advantages of high energy density and rich zinc raw materials. It is a low-cost, green and sustainable energy storage device. At present, one of the key technologies that hinder the large-scale application of ZABs is the design and fabrication oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) bifunctional catalysts with excellent performance, especially the non-platinum-based catalysts. Here N-doped carbon-coated Fe-based selenium oxide catalyst Fe O(SeO ) /Fe C@NC with high performance has been fabricated by a one-step pyrolysis and then the electrochemical oxidization. The experimental results confirmed that the existence of Fe-O-Se bonds in Fe O(SeO ) crystal phase of Fe O(SeO ) /Fe C@NC, and the Fe-O-Se bonds could obviously enhance ORR and OER catalytic performance of Fe O(SeO ) /Fe C@NC. Density functional theoretical calculations (DFT) confirmed that the Fe O(SeO ) in Fe O(SeO ) /Fe C@NC had a higher d-band center of Fe atom and a lower p-orbital coupling degree with its own lattice O atom than Fe O , which leads to Fe site of Fe O(SeO ) being more likely to adsorb external oxygen intermediates. The Fe-O-Se bonds in Fe O(SeO ) results in the modification of coordination environment of Fe atoms and optimizes the adsorption energy of Fe site for oxygen intermediates. Compared with Fe O /Fe C@NC, the Fe O(SeO ) /Fe C@NC showed the obvious enhancements of ORR/OER catalytic activities with a half-wave potential of 0.91 V for ORR in 0.1 M KOH electrolyte and a low overpotential of 345 mV for OER at 10 mA cm in a 1.0 M KOH electrolyte. The peak power density and specific capacity of Fe O(SeO ) /Fe C@NC-based ZABs are higher than those of Pt/C+RuO -ZABs. The above results demonstrate that the asymmetrical Fe-O-Se bonds in Fe O(SeO ) plays a key role in improving the bifunctional catalytic activities of ORR/OER for ZABs.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202412025