Local Spin-State Tuning of Iron Single-Atom Electrocatalyst by S-Coordinated Doping for Kinetics-Boosted Ammonia Synthesis

Bibliographische Detailangaben
Veröffentlicht in:	Advanced materials (Deerfield Beach, Fla.). - 1998. - 34(2022), 28 vom: 02. Juli, Seite e2202240
1. Verfasser:	Li, Yan (VerfasserIn)
Weitere Verfasser:	Ji, Yaxin, Zhao, Yingjie, Chen, Junxiang, Zheng, Sixing, Sang, Xiahan, Yang, Bin, Li, Zhongjian, Lei, Lecheng, Wen, Zhenhai, Feng, Xinliang, Hou, Yang
Format:	Online-Aufsatz
Sprache:	English
Veröffentlicht:	2022
Zugriff auf das übergeordnete Werk:	Advanced materials (Deerfield Beach, Fla.)
Schlagworte:	Journal Article S-coordinated doping iron single atoms kinetics-boosted catalysis nitrogen reduction reaction tunable spin states

Beschreibung
Zusammenfassung:	© 2022 Wiley-VCH GmbH. The electrochemical nitrogen reduction reaction (e-NRR) is envisaged as alternative technique to the Haber-Bosch process for NH3 synthesis. However, how to develop highly active e-NRR catalysts faces daunting challenges. Herein, a viable strategy to manipulate local spin state of isolated iron sites through S-coordinated doping (FeSA -NSC) is reported. Incorporation of S in the coordination of FeSA -NSC can induce the transition of spin-polarization configuration with the formation of a medium-spin-state of Fe (t2g 6 eg 1), which is beneficial for facilitating eg electrons to penetrate the antibonding π-orbital of nitrogen. As a consequence, a record-high current density up to 10 mA cm-2 can be achieved, together with a high NH3 selectivity of ≈10% in a flow cell reactor. Both experimental and theoretical analyses indicate that the monovalent Fe(I) atomic center in the FeSA -NSC after the S doping accelerates the N2 activation and protonation in the rate-determining step of N2 to NNH
Beschreibung:	Date Revised 14.07.2022 published: Print-Electronic Citation Status PubMed-not-MEDLINE
ISSN:	1521-4095
DOI:	10.1002/adma.202202240