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Nano Research 2023, 16(7): 8729-8736 https://doi.org/10.1007/s12274-023-5513-5
Communication | Issue | Published: 02 April 2023

Isolated Cu-Sn diatomic sites for enhanced electroreduction of CO2 to CO

Show Author's Information Wei Liu1,3,§,  Haoqiang Li4,§,  Pengfei Ou5,§,  Jing Mao6,  Lili Han1,2( ),  Jun Song5,  Jun Luo4,  Huolin L. Xin2( )
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
Department of Physics and Astronomy, University of California, Irvine, CA 92697, USA
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
School of Materials Science and Engineering, Tianjin Key Lab of Photoelectric Materials & Devices, Tianjin University of Technology, Tianjin 300384, China
Department of Mining and Materials Engineering, McGill University, Montreal H3A 0C5, Canada
Teaching and Analytical Instrumentation Center, School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China

§ Wei Liu, Haoqiang Li, and Pengfei Ou contributed equally to this work.

Keywords:
density functional theory (DFT) calculation, CO2 reduction reaction, Cu-Sn active site, CO product, dual-atom electrocatalyst
Topics:
Electrocatalysts
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Liu W, Li H, Ou P, et al. Isolated Cu-Sn diatomic sites for enhanced electroreduction of CO2 to CO. Nano Research, 2023, 16(7): 8729-8736. https://doi.org/10.1007/s12274-023-5513-5
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Abstract Full text Electronic supplementary material About this article

Electrochemical CO2 reduction reaction (CO2RR) to high-value product, CO, not only provides a key feedstock for the well-established Fischer–Tropsch process but also mitigates the greenhouse effect. However, it suffers from sluggish reaction kinetics, competitive hydrogen evolution reaction, and low selectivity. Herein, we report non-precious Cu-Sn diatomic sites anchored on nitrogen-doped porous carbon (CuSn/NPC) as an efficient catalyst for CO2RR to CO. The catalyst exhibits outstanding selectivity with CO Faradaic efficiency (FE) up to 99.1%, much higher than those of individual Cu (66.2%) and Sn (51.3%) single-atom catalysts. Moreover, high stability is confirmed by consecutive 24 h electrolysis with high selectivity from CO2 to CO. Theoretical calculations reveal an obvious activation of CO2 with weakened C–O bonds and distorted CO2 configuration upon chemisorption on the CuSn/NPC catalyst. It is also suggested CuSn/NPC is more selective for the CO2RR with dominant CO production during the electrolysis, rather than the competing hydrogen evolution reaction.


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Electronic supplementary material
About this article

Isolated Cu-Sn diatomic sites for enhanced electroreduction of CO2 to CO

Show Author's information Wei Liu1,3,§, Haoqiang Li4,§, Pengfei Ou5,§, Jing Mao6, Lili Han1,2( ), Jun Song5, Jun Luo4, Huolin L. Xin2( )
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
Department of Physics and Astronomy, University of California, Irvine, CA 92697, USA
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
School of Materials Science and Engineering, Tianjin Key Lab of Photoelectric Materials & Devices, Tianjin University of Technology, Tianjin 300384, China
Department of Mining and Materials Engineering, McGill University, Montreal H3A 0C5, Canada
Teaching and Analytical Instrumentation Center, School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China

§ Wei Liu, Haoqiang Li, and Pengfei Ou contributed equally to this work.

Abstract

Electrochemical CO2 reduction reaction (CO2RR) to high-value product, CO, not only provides a key feedstock for the well-established Fischer–Tropsch process but also mitigates the greenhouse effect. However, it suffers from sluggish reaction kinetics, competitive hydrogen evolution reaction, and low selectivity. Herein, we report non-precious Cu-Sn diatomic sites anchored on nitrogen-doped porous carbon (CuSn/NPC) as an efficient catalyst for CO2RR to CO. The catalyst exhibits outstanding selectivity with CO Faradaic efficiency (FE) up to 99.1%, much higher than those of individual Cu (66.2%) and Sn (51.3%) single-atom catalysts. Moreover, high stability is confirmed by consecutive 24 h electrolysis with high selectivity from CO2 to CO. Theoretical calculations reveal an obvious activation of CO2 with weakened C–O bonds and distorted CO2 configuration upon chemisorption on the CuSn/NPC catalyst. It is also suggested CuSn/NPC is more selective for the CO2RR with dominant CO production during the electrolysis, rather than the competing hydrogen evolution reaction.

Keywords: density functional theory (DFT) calculation, CO2 reduction reaction, Cu-Sn active site, CO product, dual-atom electrocatalyst

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Publication history
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Acknowledgements

Publication history

Received: 24 October 2022
Revised: 05 January 2023
Accepted: 17 January 2023
Published: 02 April 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the startup funding of H. L. X. The XAFS/EXAFS spectra obtained from beamline TPS 44A at National Synchrotron Radiation Research Center (NSRRC) are appreciated. The authors thank Hsiao-Tsu Wang, Wei-Xuan Lin, Chih-Wen Pao, and Way-Faung Pong for the acquisition and analysis of the XAFS data.

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