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Converting CO2 to ethanol on Ag nanowires with high selectivity investigated by operando Raman spectroscopy

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Abstract

Electrochemical conversion of CO2 into liquid fuels provides an efficient way to store the renewable energy in the production of fuels and chemicals. However, effectively converting CO2 to ethanol remains extremely challenging due to the low activity and selectivity. Herein, we achieve a high ethanol Faradaic efficiency (FE) as high as 85% on Ag nanowires (NWs) for CO2 electroreduction at −0.95 V. X-ray photoelectron spectroscopy and electrochemical experiments prove that such Ag NWs are partially oxidized. Operando Raman spectroscopy finds the important CO intermediate adsorbed on partially oxidized Ag NWs, facilitating the ethanol formation. Density functional theory calculations prove that the reaction energy of CO coupling with the *CHO to *COCHO intermediate on the partially oxidized Ag NWs is smaller than that on the surface of Cu, which explains why the ethanol FE of such partially oxidized Ag NWs can exceed that of Cu, and therefore is the most favorable pathway for the formation of C2 products on partially oxidized Ag NWs. This study provides a new insight to design efficient catalysts and investigate the mechanisms to improve the selectivity.

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Acknowledgements

This work was supported by grants from the National Natural Science Foundation of China (22174165, 21925404, 22002036, and 21908253), the Natural Science Foundation of Guangdong Province (2019A1515011117), Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme (2017), and the Natural Science Foundation of Henan Province (202300410234).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, The Key Lab of Low-carbon Chem & Energy Conservation of Guangdong Province, School of Chemistry, Sun Yat-sen University, Guangzhou, 510275, China

    Qiong Liu, Can-Jun Zou, Huan-Yu Chen & Ping-Ping Fang

  2. State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China

    Zi-Yu Du, Yu Zhao, Jin-Chao Dong & Jian-Feng Li

  3. Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, State Key College of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang, 453007, China

    Xia-Guang Zhang

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  1. Qiong Liu
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Correspondence to Ping-Ping Fang or Jian-Feng Li.

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The supporting information is available online at chem.scichina.com and link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Liu, Q., Zhang, XG., Du, ZY. et al. Converting CO2 to ethanol on Ag nanowires with high selectivity investigated by operando Raman spectroscopy. Sci. China Chem. 66, 259–265 (2023). https://doi.org/10.1007/s11426-022-1460-7

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  • DOI: https://doi.org/10.1007/s11426-022-1460-7

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