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231226s2022 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202202240
|2 doi
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|a pubmed24n1134.xml
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|a (DE-627)NLM34050983X
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|a (NLM)35522454
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|a eng
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|a Li, Yan
|e verfasserin
|4 aut
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|a Local Spin-State Tuning of Iron Single-Atom Electrocatalyst by S-Coordinated Doping for Kinetics-Boosted Ammonia Synthesis
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|c 2022
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
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|2 rdamedia
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|a ƒa Online-Ressource
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|2 rdacarrier
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|a Date Revised 14.07.2022
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2022 Wiley-VCH GmbH.
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|a 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
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|a Journal Article
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|a S-coordinated doping
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|a iron single atoms
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|a kinetics-boosted catalysis
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|a nitrogen reduction reaction
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|a tunable spin states
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|a Ji, Yaxin
|e verfasserin
|4 aut
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|a Zhao, Yingjie
|e verfasserin
|4 aut
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| 700 |
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|a Chen, Junxiang
|e verfasserin
|4 aut
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| 700 |
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|a Zheng, Sixing
|e verfasserin
|4 aut
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| 700 |
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|a Sang, Xiahan
|e verfasserin
|4 aut
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| 700 |
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|a Yang, Bin
|e verfasserin
|4 aut
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|a Li, Zhongjian
|e verfasserin
|4 aut
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| 700 |
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|a Lei, Lecheng
|e verfasserin
|4 aut
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| 700 |
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|a Wen, Zhenhai
|e verfasserin
|4 aut
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| 700 |
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|a Feng, Xinliang
|e verfasserin
|4 aut
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| 700 |
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|a Hou, Yang
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g 34(2022), 28 vom: 02. Juli, Seite e2202240
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnns
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| 773 |
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|g volume:34
|g year:2022
|g number:28
|g day:02
|g month:07
|g pages:e2202240
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|u http://dx.doi.org/10.1002/adma.202202240
|3 Volltext
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