Wang Yuwen, Wang Jiajun, Liu Shuang, Zhang Xuan, Jin Lin, Feng Lanlan, Kong Demeng, Zhang Chenxi, Wei Yajuan, Zhang Jingbo
Academy of Interdisciplinary Studies on Intelligent Molecules, Tianjin Key Laboratory of Structure and Performance for Functional Molecules, College of Chemistry, Tianjin Normal University, Tianjin, 300387, China.
ChemSusChem. 2025 Apr 1;18(7):e202402097. doi: 10.1002/cssc.202402097. Epub 2024 Nov 27.
In recent years, the electrochemical reduction of carbon dioxide (CORR) has made many advances in C production. Cu/Cu site is beneficial for C-C coupling process, but the oxidation state of copper cannot be well maintained during the reaction process, resulting in a decrease in catalyst activity. Based on this consideration, in this work, transition metal oxide CeO with a hollow cube structure and oxygen vacancies was introduced to stabilize and increase Cu/Cu active sites (CeCu). The catalyst exhibits excellent CORR performance, with FE achieving 73.52 % and j >280 mA/cm at 1.26 V (vs. RHE). Ethanol is the main C product and FE reaches 39 % at 1.26 V. The experimental results indicate that the presence of CeO provides a large number of oxygen vacancies and forming Cu-O-Ce structure by the strong interaction of CeO and Cu NPs. The structure of Cu-O-Ce and abundant oxygen vacancies lay a good foundation for the CO adsorption. Moreover, it increases the content of Cu/Cu sites, effectively inhibiting hydrogen evolution reaction, promoting the C-C coupling interaction, thereby facilitating the generation of C products. The DFT theoretical calculation further demonstrates that CeCu is more inclined towards the ethanol pathway, confirming its high selectivity for ethanol.
