期刊
NANO-MICRO LETTERS
卷 12, 期 1, 页码 -出版社
SHANGHAI JIAO TONG UNIV PRESS
DOI: 10.1007/s40820-020-00456-8
关键词
Atomic dispersion; Iron-nitrogen moiety; Electronic structure; Sulfur doping; Oxygen reduction
资金
- National Natural Science Foundation of China
- Beijing University of Chemical Technology [buctrc201901]
- Ministry of Foreign Affairs and International Cooperation, Italy [NSFC-MAECI 51861135202]
- National Key Research and Development Project [2018YFB1502401, 2018YFA0702002]
- Royal Society
- Newton Fund through the Newton Advanced Fellowship award [NAF\ R1\191294]
- Program for Changjiang Scholars and Innovation Research Team in the University [IRT1205]
- Fundamental Research Funds for the Central Universities
- Ministry of Finance and the Ministry of Education of PRC
Immobilizing metal atoms by multiple nitrogen atoms has triggered exceptional catalytic activity toward many critical electrochemical reactions due to their merits of highly unsaturated coordination and strong metal-substrate interaction. Herein, atomically dispersed Fe-NC material with precise sulfur modification to Fe periphery (termed as Fe-NSC) was synthesized, X-ray absorption near edge structure analysis confirmed the central Fe atom being stabilized in a specific configuration of Fe(N-3)(N-C-S). By enabling precisely localized S doping, the electronic structure of Fe-N-4 moiety could be mediated, leading to the beneficial adjustment of absorption/desorption properties of reactant/intermediate on Fe center. Density functional theory simulation suggested that more negative charge density would be localized over Fe-N-4 moiety after S doping, allowing weakened binding capability to *OH intermediates and faster charge transfer from Fe center to O species. Electrochemical measurements revealed that the Fe-NSC sample exhibited significantly enhanced oxygen reduction reaction performance compared to the S-free Fe-NC material (termed as Fe-NC), showing an excellent onset potential of 1.09 V and half-wave potential of 0.92 V in 0.1 M KOH. Our work may enlighten relevant studies regarding to accessing improvement on the catalytic performance of atomically dispersed M-NC materials by managing precisely tuned local environments of M-N-x moiety.
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