In Situ Engineering of the Cu+/Cu0 Interface to Boost C2+ Selectivity in CO2 Electroreduction

作者：Du, Ruian; Li, Tan^*; Wu, Qiqi; Wang, Peng; Yang, Xianfeng; Fan, Yan; Qiu, Yongcai; Yan, Keyou; Wang, Pei; Zhao, Yun^*; Zhao, Wei-Wei^*; Chen, Guangxu^*

来源：ACS applied materials & interfaces, 2022, 14(32): 36527-36535.

DOI：10.1021/acsami.2c05992

• CO2 electroreduction
• oxide-derived Cu catalysts
• Cu+/Cu-0 interface
• halide
• C(2+)product

The Cu+/Cu(0 )interface in the Cu-based electrocatalyst is essential to promote the electrochemical reduction of carbon dioxide (ERCO2) to produce multi-carbon hydrocarbons and alcohols with high selectivity. However, due to the high activity of the Cu+/Cu-0 interface, it is easy to be oxidized in the air. How to control and prepare a Cu-based electrocatalyst with an abundant and stable Cu+/Cu(0 )interface in situ is a huge challenge. Here, combined with density functional theory (DFT) calculations and experimental studies, we found that the trace halide ions adsorbed on Cu2O can slow the reduction kinetics of Cu+ -> Cu-0, which allowed us to in-situ well control the synthesis of the CuO-derived electrocatalyst with rich Cu+/Cu0 interfaces. Our Cu catalyst with a rich Cu+/Cu-0 interface exhibits excellent ERCO2 performance. Under the operation potential of -0.98 V versus RHE, the Faraday efficiency of C(2)H(4 )and C2+ products are 55.8 and 75.7%, respectively, which is about 16% higher than that of CuO-derived electrocatalysts that do not use halide ions. The high + FEC2 comes from the improvement of the coupling efficiency of reaction intermediates such as CO-CO, which is proved by DFT calculations, and the suppression of hydrogen evolution reaction. Therefore, we provide an in-situ engineering strategy, which is simple and effective for the design and preparation of high-performance ERCO2 catalysts.

• 单位
  华中农业大学; y; 南京大学