Abstract
Electronic structure engineering is a powerful method to tailor the behavior of adsorbed intermediates on the surface of catalysts, thus regulating catalytic activity towards CO2 electroreduction. Herein, we prepared a series of P-doped Cu catalysts for CO2 electroreduction into multi-carbon (C2+) products by regulating the surface electronic structure of Cu. The introduction of P could stabilize the surface Cuδ+ species, enhancing the activity for C2+ products via adjusting the adsorbed strength of the CO intermediates (*CO). When the molar ratio of P to Cu was 8.3%, the catalyst exhibited a Faradaic efficiency of 64% for C2+ products, which was 1.9 times as high as that (33%) for Cu catalysts at the applied current density of 210 mA cm−2. Notably, at the applied current density of 300 mA cm−2, the P-doped Cu catalyst with the molar ratio of P to Cu of 8.3% exhibited the highest partial current density for C2+ products of 176 mA cm−2, whereas the partial current density for C2+ products over the Cu catalyst was only 84 mA cm−2. Mechanistic studies revealed that modulating the molar ratios of P to Cu regulated the adsorbed strength of *CO. A moderate adsorbed strength of *CO induced by appropriate P doping was responsible for the facilitated C-C coupling process.
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Acknowledgements
This work was supported by National Science Fund for Distinguished Young Scholars (21925204), the National Natural Science Foundation of China (U1932146, U19A2015, 21673214, and U1732272), National Key Research and Development Program of China (2019YFA0405600, 2017YFA0403402, and 2019YFA0405602), Key Research Program of Frontier Sciences of the CAS (QYZDB-SSW-SLH017), Fundamental Research Funds for the Central Universities, and USTC Research Funds of the Double First-Class Initiative (YD2340002002).
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Kong, X., Wang, C., Zheng, H. et al. Enhance the activity of multi-carbon products for Cu via P doping towards CO2 reduction. Sci. China Chem. 64, 1096–1102 (2021). https://doi.org/10.1007/s11426-020-9934-0
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DOI: https://doi.org/10.1007/s11426-020-9934-0