Author(s): Zhao, Yang ; Zeng, Binwen ; Huang, Haoliang ; Yang, Huanhuan ; Yu, Zhipeng ; Song, Chao ; Wang, Jingwei ; Xu, Kaiyang ; Xiang, Xinyi ; Wang, Wei ; Lin, Fei ; Meng, Sheng ; Meng, Lijian ; Cui, Zhiming ; Liu, Lifeng
Date: 2025
Persistent ID: http://hdl.handle.net/10400.22/30592
Origin: Repositório Científico do Instituto Politécnico do Porto
Subject(s): Electrochemical CO2 reduction; Rare earth doping; CuO nanosheet; Strain engineering; Surface reconstruction
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.
