Atomic Dispersion of Scandium in Electrochemically Reduced Copper Oxide Nanosheets for Efficient Electrocatalytic CO2 Reduction to C2+ Products

Converting CO2 into value-added chemicals and fuels through electrochemical CO2 reduction reaction (CO2RR) has been acknowledged as a disruptive technology for chemical industry and an important means to realizing carbon neutrality. However, it remains challenging to achieve high selectivity for C2+ products at a large current density with a low overpotential. Herein, we report a scandium (Sc) single-atom-doped CuO nanosheet (Sc1CuO NS) electrocatalyst for efficient and durable CO2-to-C2+ conversion. The optimal Sc1CuO NS catalyst achieves a maximal C2+ Faradaic efficiency of 73 ± 1.8 % at 475.2 mA cm−2 under an ultralow potential of −0.6 V versus the reversible hydrogen electrode (RHE) and maintains stable CO2-to-C2+ conversion at ∼206 mA cm−2 with a > 60 % Faradaic efficiency for 47 h without degradation. In-situ spectroscopy measurements combined with density functional theory (DFT) calculations reveal that the electron transfer from Sc to Cu enhances the activation of CO2 to *CO. Moreover, the in-situ electrochemical reduction of CuO generates abundant undercoordinated Cu0 sites, featuring tensile-strained Sc-(O)-Cu motifs, which serve as active centers that reduce the reaction barrier for Csingle bondC coupling. This work highlights the importance of rare-earth doping combined with in-situ electrochemical surface reconstruction of CuO as an effective catalyst design strategy to boost CO2-to-C2+ conversion performance.

Keywords

Electrochemical CO2 reduction Rare earth doping CuO nanosheet Strain engineering Surface reconstruction

URI

http://hdl.handle.net/10400.22/30592

Citation

Yang Zhao, Binwen Zeng, Haoliang Huang, Huanhuan Yang, Zhipeng Yu, Chao Song, Jingwei Wang, Kaiyang Xu, Xinyi Xiang, Wei Wang, Fei Lin, Sheng Meng, Lijian Meng, Zhiming Cui, Lifeng Liu, Atomic dispersion of scandium in electrochemically reduced copper oxide nanosheets for efficient electrocatalytic CO2 reduction to C2+ products, Chemical Engineering Journal, Volume 524, 2025, 169132, ISSN 1385-8947, https://doi.org/10.1016/j.cej.2025.169132.