Issue

Vol. 12 (2020)

Atomically Dispersed Fe-N4 Modified with Precisely Located S for Highly Efficient Oxygen Reduction

https://doi.org/10.1007/s40820-020-00456-8
Yin Jia
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, People’s Republic of China
Xuya Xiong
Interdisciplinary Nanoscience Center (INANO), Sino‑Danish Center for Education and Research (SDC), Aarhus University, 8000 Aarhus C, Denmark
Danni Wang
Shandong University of Science and Technology, Electrical Engineering and Automation, Tsingtao 266590, People’s Republic of China
Xinxuan Duan
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, People’s Republic of China
Kai Sun
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, People’s Republic of China
Yajie Li
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, People’s Republic of China
Lirong Zheng
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, People’s Republic of China
Wenfeng Lin
Department of Chemical Engineering, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
Mingdong Dong
Interdisciplinary Nanoscience Center (INANO), Sino‑Danish Center for Education and Research (SDC), Aarhus University, 8000 Aarhus C, Denmark
Guoxin Zhang
Shandong University of Science and Technology, Electrical Engineering and Automation, Tsingtao 266590, People’s Republic of China
Wen Liu
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, People’s Republic of China
Xiaoming Sun
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, People’s Republic of China

Corresponding Author: Xiaoming Sun

sunxm@mail.buct.edu.cn

Nano-Micro Letters, Vol. 12 (2020), Article Number: 116

Abstract

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(N3)(N–C–S). By enabling precisely localized S doping, the electronic structure of Fe-N4 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-N4 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-Nx moiety.


Highlights:


1 Precisely located S doping of atomic Fe-N4 in Fe(N3)(N–C–S) motif was realized.
2 This S doping renders weakened *OH binding and faster charge transfer on Fe-N4.
3 Fe-NSC showed excellent oxygen reduction reaction performance with onset potential ~ 1.09 V and half-wave potential ~ 0.92 V.

Keywords

Atomic dispersion Iron–nitrogen moiety Electronic structure Sulfur doping Oxygen reduction
Jia, Yin, Xuya Xiong, Danni Wang, Xinxuan Duan, Kai Sun, Yajie Li, Lirong Zheng, Wenfeng Lin, Mingdong Dong, Guoxin Zhang, Wen Liu, and Xiaoming Sun. 2020. “Atomically Dispersed Fe-N4 Modified With Precisely Located S for Highly Efficient Oxygen Reduction”. Nano-Micro Letters 12 (May):116. https://doi.org/10.1007/s40820-020-00456-8.
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