Abstract
Cu-based electrocatalysts with favorable facets and Cu+ can boost CO2 reduction to valuable multicarbon products. However, the inevitable Cu+ reduction and the phase evolution usually result in poor performance. Herein, we fabricate CuI nanodots with favorable (220) facets and a stable Cu+ state, accomplished by operando reconstruction of Cu(OH)2 under CO2- and I−-containing electrolytes for enhanced CO2-to-C2H4 conversion. Synchrotron X-ray absorption spectroscopy (XAS), in-situ Raman spectroscopy and thermodynamic potential analysis reveal the preferred formation of CuI. Vacuum gas electroresponse and density functional theory (DFT) calculations reveal that CO2-related species induce the exposure of the (220) plane of CuI. Moreover, the small size of nanodots enables the adequate contact with I−, which guarantees the rapid formation of CuI instead of the electroreduction to Cu0. As a result, the resulting catalysts exhibit a high C2H4 Faradaic efficiency of 72.4% at a large current density of 800 mA cm−2 and robust stability for 12 h in a flow cell. Combined in-situ ATR-SEIRS spectroscopic characterizations and DFT calculations indicate that the (220) facets and stable Cu+ in CuI nanodots synergistically facilitate CO2/*CO adsorption and *CO dimerization.
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Acknowledgements
This work is financially supported by The National Key Research and Development Program of China (2021YFA1600800), the Start-up Funding of the Huazhong University of Science and Technology (HUST), the Program for HUST Academic Frontier Youth Team, the National Natural Science Foundation of China (22075092), the National 1000 Young Talents Program of China and The Innovation and Talent Recruitment Base of New Energy Chemistry and Device (B21003).
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Xue, W., Liu, H., Chen, X. et al. Operando reconstruction towards stable CuI nanodots with favorable facets for selective CO2 electroreduction to C2H4. Sci. China Chem. 66, 1834–1843 (2023). https://doi.org/10.1007/s11426-023-1591-6
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DOI: https://doi.org/10.1007/s11426-023-1591-6