Guo, Yafei, Gao, Yuxuan, Guo, Benshuai, Luo, Yangna, Zhao, Guoyang, Sun, Jian, Li, Weiling, Wang, Ruilin, and Zhao, Chuanwen
Electrochemical CO2reduction (ECR) to value-added products is regarded as a sustainable strategy to mitigate global warming and energy crisis, and designing highly efficient and robust catalysts is essential. In this work, transition metal sulfides (TMS)-decorated CuS microflower-like structures were prepared via the one-pot hydrothermal synthesis method for ECR to CO, and the influence of TMS doping on ECR performance was demonstrated. Characterization of the catalysts was performed using XRD, FESEM-EDS, N2physisorption, and XPS, revealing the successful loading of TMS, the formation of microflower-like architectures and the generation of sulfur vacancies. Electrochemical tests demonstrated that doping ZnS, Bi2S3, CdS and MoS2improved the intrinsic CO2reduction activity of the CuS catalyst. Particularly, the MoS2-CuS composite catalyst with imperfect petal-like structure showed uniform distribution of edge Mo sites, which worked synergistically with the formed grain boundaries (GBs) and undercoordinated S vacancy sites in promoting CO2activation, stabilizing *COOH adsorption, facilitating *CO desorption, and lowering the energy barrier of the potential-limiting step for improved CO selectivity. The MoS2-CuS catalyst achieved a maximum CO selectivity of 83.2% at –0.6 V versus the reversible hydrogen electrode (RHE) and a high CO cathodic energetic efficiency of 100%. At this potential, the catalyst maintained stable catalytic activity and CO selectivity during a 333-min electrolysis process. The findings will offer a promising avenue for the development of efficient and stable catalysts for CO production from ECR.