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Cu2−xS derived copper nanoparticles: A platform for unraveling the role of surface reconstruction in efficient electrocatalytic CO2-to-C2H4 conversion

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Abstract

Cu-based electrocatalysts have provoked much attention for their high activity and selectivity in carbon dioxide (CO2) conversion into multi-carbon hydrocarbons. However, during the electrochemical reaction, Cu catalysts inevitably undergo surface reconstruction whose impact on CO2 conversion performance remains contentious. Here we report that polycrystalline Cu nanoparticles (denoted as Cu-s) with rich high-index facets, derived from Cu2−xS through desulphurization and surface reconstruction, offer an excellent platform for investigating the role of surface reconstruction in electrocatalytic CO2 conversion. During the formation of Cu-s catalyst, the two stages of desulphurization and surface reconstruction can be clearly resolved by in situ X-ray absorption spectroscopy and OH− adsorption characterizations, which are well correlated with the changes in electrocatalytic performance. It turns out that the high CO2 conversion performance, achieved by the Cu-s catalyst (Faradic efficiency of 68.6% and partial current density of 40.8 mA/cm2 in H-cell toward C2H4 production), is attributed to the increased percentage of high-index facets in Cu-s during the surface reconstruction. Furthermore, the operando electrochemical Raman spectroscopy further reveals that the conversion of the CO2 into the C2H4 on Cu-s is intermediated by the production of *COCHO. Our findings manifest that the surface reconstruction is an effective method for tuning the reaction intermediate of the CO2 conversion toward high-value multicarbon (C2+) chemicals, and highlight the significance of in situ characterizations in enhancing the understanding of the surface structure and its role in electrocatalysis.

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Acknowledgements

This work was financially supported in part by the National Key R&D Program of China (Nos. 2017YFA0207301 and 2017YFA0403402), the National Natural Science Foundation of China (Nos. 21725102, 91961106, U1832156, and 22075267), Science and Technological Fund of Anhui Province for Outstanding Youth (No. 2008085J05), Youth Innovation Promotion Association of CAS (No. 2019444), Young Elite Scientist Sponsorship Program by CAST, China Postdoctoral Science Foundation (Nos. 2019M652190 and 2020T130627), Users with Excellence Program of Hefei Science Center CAS (No. 2020HSC-UE003) and DNL Cooperation Fund, CAS (No. DNL201922). The in situ XAS measurements were employed on beamlines 1W1B (BSRF) and BL14W1 (SSRF). We thank the support from USTC Center for Micro- and Nanoscale Research and Fabrication.

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  1. Chaohua He, Delong Duan, and Jingxiang Low contributed equally to this work.

Authors and Affiliations

  1. Hefei National Laboratory for Physical Sciences at the Microscale, Frontiers Science Center for Planetary Exploration and Emerging Technologies, School of Chemistry and Materials Science, and National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026, China

    Chaohua He, Delong Duan, Jingxiang Low, Yu Bai, Yawen Jiang, Xinyu Wang, Shuangming Chen, Ran Long, Li Song & Yujie Xiong

  2. Hefei Comprehensive National Science Center, 350 Shushanhu Rd., Hefei, 230031, China

    Chaohua He & Yujie Xiong

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  1. Chaohua He
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Correspondence to Ran Long or Yujie Xiong.

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Cu2−xS derived copper nanoparticles: A platform for unraveling the role of surface reconstruction in efficient electrocatalytic CO2-to-C2H4 conversion

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He, C., Duan, D., Low, J. et al. Cu2−xS derived copper nanoparticles: A platform for unraveling the role of surface reconstruction in efficient electrocatalytic CO2-to-C2H4 conversion. Nano Res. 16, 4494–4498 (2023). https://doi.org/10.1007/s12274-021-3532-7

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