Defective Bimetallic Selenides for Selective CO<sub>2</sub> Electroreduction to CO
Jiajun Wang, Xuerong Zheng, Guangjin Wang, Yanhui Cao, Wenlong Ding, Jinfeng Zhang, Han‐Chun Wu, Jia Ding, Huilin Hu, Xiaopeng Han, Tianyi Ma, Yida Deng, Wenbin Hu
Abstract
Abstract CO 2 electroreduction (CO 2 RR) to CO is promising for the carbon cycle but still remains challenging. Au is regarded as the most selective catalyst for CO 2 RR, but its high cost significantly hinders its industrial application. Herein, the bimetallic CuInSe 2 is found to exhibit an Au‐like catalytic feature: i) the interaction of Cu and In orbitals induces a moderate adsorption strength of CO 2 RR intermediates and favors the reaction pathway; and ii) the hydrogen evolution is energetically unfavorable on CuInSe 2 , as a surface reconstruction along with high energy change will occur after hydrogen adsorption. Furthermore, the Se vacancy is found to induce an electron redistribution, slightly tune the band structure, and optimize the CO 2 RR route of bimetallic selenide. Consequently, the Se‐defective CuInSe 2 (V‐CuInSe 2 ) achieves a highly selective CO production ability that is comparable to noble metals in aqueous electrolyte, and the V‐CuInSe 2 cathode shows a satisfactory performance in an aqueous Zn–CO 2 cell. This work demonstrates that designing cost‐effective catalysts with noble‐metal‐like properties is an ideal strategy for developing efficient electrocatalysts. Moreover, the class of transition bimetallic selenides has shown promising prospects as active and cost‐effective electrocatalysts owing to their unique structural, electronic, and catalytic properties.