Discovery of main group single Sb–N4 active sites for CO2 electroreduction to formate with high efficiency

Zhuoli Jiang; Tao Wang; Jiajing Pei; Huishan Shang; Danni Zhou; Haijing Li; Juncai Dong; Yu Wang; Rui Cao; Zhongbin Zhuang; Wenxing Chen; Dingsheng Wang; Jiatao Zhang; Yadong Li

doi:10.1039/D0EE01486A

Discovery of main group single Sb–N₄ active sites for CO₂ electroreduction to formate with high efficiency†

Zhuoli Jiang,‡^a Tao Wang,

‡^b Jiajing Pei,‡^c Huishan Shang,^a Danni Zhou,^a Haijing Li,^d Juncai Dong,^d Yu Wang,^e Rui Cao,^f Zhongbin Zhuang,

^c Wenxing Chen,

*^a Dingsheng Wang,

*^g Jiatao Zhang

*^a and Yadong Li

^g

Author affiliations

* Corresponding authors

^a Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
E-mail: wxchen@bit.edu.cn, zhangjt@bit.edu.cn

^b SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, California 94305, USA

^c College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China

^d Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China

^e Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai 201800, China

^f Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

^g Department of Chemistry, Tsinghua University, Beijing 100084, China
E-mail: wangdingsheng@mail.tsinghua.edu.cn

Abstract

Main group antimony (Sb) species are promising electrocatalysts that promote the CO₂ reduction reaction (CO₂RR) to formate, which is an important hydrogen storage material and a key chemical intermediate in many industrial reactions. Herein, we discovered that an Sb single atom (SA) material consisting of Sb–N₄ moieties anchored on N-doped carbon (NC) nanosheets (named Sb SA/NC) could serve as a CO₂RR catalyst to produce formate with high efficiency. Sb SA/NC exhibited a formate faradaic efficiency of 94.0% at −0.8 V vs. RHE. In situ X-ray absorption fine structure (XAFS) investigations and density functional theory (DFT) calculations demonstrated that the excellent CO₂RR activity originated from the positively charged Sb^δ+–N₄ (0 < δ < 3) active sites. Our results present significant guidelines for the rational design and accurate modulation of main group metal (Sb, In, Sn, Bi, etc.) catalysts for the CO₂RR at the atomic scale.

Energy & Environmental Science

Discovery of main group single Sb–N₄ active sites for CO₂ electroreduction to formate with high efficiency†

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Discovery of main group single Sb–N₄ active sites for CO₂ electroreduction to formate with high efficiency

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