Planar Chlorination Engineering A Strategy of Completely Breaking the Geometric Symmetry of Fe-N4 Site for Boosting Oxygen Electroreduction

Planar Chlorination Engineering : A Strategy of Completely Breaking the Geometric Symmetry of Fe-N4 Site for Boosting Oxygen Electroreduction

© 2024 Wiley‐VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 31 vom: 01. Aug., Seite e2404692
1. Verfasser: Wei, Shengjie (VerfasserIn)
Weitere Verfasser: Yang, Rongyan, Wang, Ziyi, Zhang, Jijie, Bu, Xian-He
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article Fe‐N4 site with broken geometric symmetry Zn‐air battery oxygen reduction reaction planar chlorination engineering
Beschreibung
Zusammenfassung:© 2024 Wiley‐VCH GmbH.
Introducing asymmetric elements and breaking the geometric symmetry of traditional metal-N4 site for boosting oxygen reduction reaction (ORR) are meaningful and challenging. Herein, the planar chlorination engineering of Fe-N4 site is first proposed for remarkably improving the ORR activity. The Fe-N4/CNCl catalyst with broken symmetry exhibits a half-wave potential (E1/2) of 0.917 V versus RHE, 49 and 72 mV higher than those of traditional Fe-N4/CN and commercial 20 wt% Pt/C catalysts. The Fe-N4/CNCl catalyst also has excellent stability for 25 000 cycles and good methanol tolerance ability. For Zn-air battery test, the Fe-N4/CNCl catalyst has the maximum power density of 228 mW cm-2 and outstanding stability during 150 h charge-discharge test, as the promising substitute of Pt-based catalysts in energy storage and conversion devices. The density functional theory calculation demonstrates that the adjacent C─Cl bond effectively breaks the symmetry of Fe-N4 site, downward shifts the d-band center of Fe, facilitates the reduction and release of OH*, and remarkably lowers the energy barrier of rate-determining step. This work reveals the enormous potential of planar chlorination engineering for boosting the ORR activity of traditional metal-N4 site by thoroughly breaking their geometric symmetry
Beschreibung:Date Revised 01.08.2024
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202404692