Mei Guoliang, Zhai Yanling, Guo Weiwei, Liu Doudou, Fang Zijian, Xie Guixian, Duan Zongxia, Lang Xianzhen, Zhu Zhijun, Lu Xiaoquan, Tang Jianguo
Institute of Hybrid Materials, College of Materials Science and Engineering, Institute of Molecular Metrology, College of Chemistry and Chemical Engineering, Qingdao University, Qingdao, 266071, P. R. China.
Chemistry. 2025 Jan 14;31(3):e202403261. doi: 10.1002/chem.202403261. Epub 2024 Nov 25.
Electrochemical reduction of carbon dioxide (CO) can produce value-added chemicals such as carbon monoxide (CO) and multicarbon (C). However, the complex reaction pathways of CO electro-reduction reaction (CORR) greatly limit the product selectivity and conversion efficiency. Herein, the Cu-Cd bimetallic oxides catalyst was designed and applied for the CORR. The optimized 4.73 %Cd-CuO exhibits remarkable electrocatalytic CORR activity for selective CO production in H-cell using 0.5 M 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim]PF)/MeCN as electrolyte. The Faradaic efficiency of CO (FE(CO)) can be maintained above 90 % over a wide potential range of -2.0 to -2.4 V vs. Ag/Ag. Particularly, the catalyst achieves an impressive FE(CO) of 96.3 % with a current density of 60.7 mA cm at -2.2 V vs. Ag/Ag. Furthermore, scaling up the 4.73 %Cd-CuO catalyst into a flow cell can reach 56.64 % FE of C products (ethylene, ethanol and n-propanol) with a current density as high as 600 mA cm steadily. The excellent CORR performance of the as-synthesized 4.73 %Cd-CuO can be mainly attributed to the introduction of CdO to improve the ability of CuO to activate CO, the electronic interactions between Cu and Cd can boost the activation and conversion the key intermediates of CORR and ensure the continuous stability of the 4.73 %Cd-CuO in electrolysis process.
二氧化碳（CO₂）的电化学还原可以产生一氧化碳（CO）和多碳（C₂+）等增值化学品。然而，CO₂电还原反应（CORR）复杂的反应路径极大地限制了产物的选择性和转化效率。在此，设计了Cu-Cd双金属氧化物催化剂并将其应用于CORR。优化后的4.73 %Cd-CuO在使用0.5 M六氟磷酸1-丁基-3-甲基咪唑鎓（[Bmim]PF₆）/乙腈作为电解质的H型电解池中，对选择性生成CO表现出显著的电催化CORR活性。相对于Ag/Ag参比电极，在-2.0至-2.4 V的宽电位范围内，CO的法拉第效率（FE(CO)）可以保持在90 %以上。特别地，在相对于Ag/Ag参比电极-2.2 V时，该催化剂实现了令人印象深刻的96.3 %的FE(CO)，电流密度为60.7 mA cm⁻²。此外，将4.73 %Cd-CuO催化剂放大到流动池中，C₂+产物（乙烯、乙醇和正丙醇）的FE可以稳定达到56.64 %，电流密度高达600 mA cm⁻²。所合成的4.73 %Cd-CuO优异的CORR性能主要归因于引入CdO提高了CuO活化CO₂的能力，Cu和Cd之间的电子相互作用可以促进CORR关键中间体的活化和转化，并确保4.73 %Cd-CuO在电解过程中的持续稳定性。
