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Stable and Efficient Single-Atom Zn Catalyst for CO2 Reduction to CH4

  • Lili Han
    Lili Han
    Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
    Department of Physics and Astronomy, University of California, Irvine, California 92697, United States
    More by Lili Han
  • Shoujie Song
    Shoujie Song
    Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
    More by Shoujie Song
  • Mingjie Liu
    Mingjie Liu
    Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States
    More by Mingjie Liu
  • Siyu Yao
    Siyu Yao
    Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
    More by Siyu Yao
  • Zhixiu Liang
    Zhixiu Liang
    Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
    More by Zhixiu Liang
  • Hao Cheng
    Hao Cheng
    Department of Physics and Astronomy, University of California, Irvine, California 92697, United States
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  • Zhouhong Ren
    Zhouhong Ren
    Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
    More by Zhouhong Ren
  • Wei Liu
    Wei Liu
    Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
    More by Wei Liu
  • Ruoqian Lin
    Ruoqian Lin
    Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
    More by Ruoqian Lin
  • Gaocan Qi
    Gaocan Qi
    School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
    More by Gaocan Qi
  • Xijun Liu*
    Xijun Liu
    Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
    *[email protected]
    More by Xijun Liu
  • Qin Wu*
    Qin Wu
    Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States
    *[email protected]
    More by Qin Wu
  • Jun Luo*
    Jun Luo
    Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
    *[email protected]
    More by Jun Luo
  • , and 
  • Huolin L. Xin*
    Huolin L. Xin
    Department of Physics and Astronomy, University of California, Irvine, California 92697, United States
    *[email protected]
Cite this: J. Am. Chem. Soc. 2020, 142, 29, 12563–12567
Publication Date (Web):June 14, 2020
https://doi.org/10.1021/jacs.9b12111
Copyright © 2020 American Chemical Society
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Abstract

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The development of highly active and durable catalysts for electrochemical reduction of CO2 (ERC) to CH4 in aqueous media is an efficient and environmentally friendly solution to address global problems in energy and sustainability. In this work, an electrocatalyst consisting of single Zn atoms supported on microporous N-doped carbon was designed to enable multielectron transfer for catalyzing ERC to CH4 in 1 M KHCO3 solution. This catalyst exhibits a high Faradaic efficiency (FE) of 85%, a partial current density of −31.8 mA cm–2 at a potential of −1.8 V versus saturated calomel electrode, and remarkable stability, with neither an obvious current drop nor large FE fluctuation observed during 35 h of ERC, indicating a far superior performance than that of dominant Cu-based catalysts for ERC to CH4. Theoretical calculations reveal that single Zn atoms largely block CO generation and instead facilitate the production of CH4.

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  • Experimental section, additional electrochemical data, and details of the characterization of catalysts (PDF)

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