Engineering unsymmetrically coordinated Cu-S1N3 single atom sites with enhanced oxygen reduction activity

Huishan Shang, Xiangyi Zhou, Juncai Dong, Ang Li, Xu Zhao, Qinghua Liu, Yue Lin, Jiajing Pei, Zhi Li, Zhuoli Jiang, Danni Zhou, Lirong Zheng, Yu Wang, Jing Zhou, Zhengkun Yang, Rui Cao, Ritimukta Sarangi, Tingting Sun, Xin Yang, Xusheng Zheng, Wensheng Yan, Zhongbin Zhuang, Jia Li (), Wenxing Chen (), Dingsheng Wang (), Jiatao Zhang () and Yadong Li
Additional contact information
Huishan Shang: School of Materials Science and Engineering, Beijing Institute of Technology
Xiangyi Zhou: Tsinghua University
Juncai Dong: Institute of High Energy Physics, Chinese Academy of Sciences
Ang Li: Beijing University of Technology
Xu Zhao: University of Science and Technology of China
Qinghua Liu: University of Science and Technology of China
Yue Lin: University of Science and Technology of China
Jiajing Pei: Beijing University of Chemical Technology
Zhi Li: Tsinghua University
Zhuoli Jiang: School of Materials Science and Engineering, Beijing Institute of Technology
Danni Zhou: School of Materials Science and Engineering, Beijing Institute of Technology
Lirong Zheng: Institute of High Energy Physics, Chinese Academy of Sciences
Yu Wang: Shanghai Institute of Applied Physics, Chinese Academy of Science
Jing Zhou: Shanghai Institute of Applied Physics, Chinese Academy of Science
Zhengkun Yang: University of Science and Technology of China
Rui Cao: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory
Ritimukta Sarangi: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory
Tingting Sun: University of Science and Technology Beijing
Xin Yang: Tsinghua University
Xusheng Zheng: University of Science and Technology of China
Wensheng Yan: University of Science and Technology of China
Zhongbin Zhuang: Beijing University of Chemical Technology
Jia Li: Tsinghua University
Wenxing Chen: School of Materials Science and Engineering, Beijing Institute of Technology
Dingsheng Wang: Tsinghua University
Jiatao Zhang: School of Materials Science and Engineering, Beijing Institute of Technology
Yadong Li: Tsinghua University

Nature Communications, 2020, vol. 11, issue 1, 1-11

Abstract: Abstract Atomic interface regulation is thought to be an efficient method to adjust the performance of single atom catalysts. Herein, a practical strategy was reported to rationally design single copper atoms coordinated with both sulfur and nitrogen atoms in metal-organic framework derived hierarchically porous carbon (S-Cu-ISA/SNC). The atomic interface configuration of the copper site in S-Cu-ISA/SNC is detected to be an unsymmetrically arranged Cu-S1N3 moiety. The catalyst exhibits excellent oxygen reduction reaction activity with a half-wave potential of 0.918 V vs. RHE. Additionally, through in situ X-ray absorption fine structure tests, we discover that the low-valent Cuprous-S1N3 moiety acts as an active center during the oxygen reduction process. Our discovery provides a universal scheme for the controllable synthesis and performance regulation of single metal atom catalysts toward energy applications.

Date: 2020
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DOI: 10.1038/s41467-020-16848-8

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