Stabilizing Cu0-Cu+ sites by Pb-doping for highly efficient CO2 electroreduction to C2 products

Authors：Ma, Xiaodong; Song, Xinning; Zhang, Libing; Wu, Limin; Feng, Jiaqi; Jia, Shunhan; Tan, Xingxing; Xu, Liang; Sun, Xiaofu^*; Han, Buxing^*

Source：Green Chemistry, 2023, 25(19): 7635-7641.

DOI：10.1039/d3gc01506h

• CARBON-DIOXIDE

The electrochemical CO2 reduction reaction (CO2RR) can convert CO2 to C-2 hydrocarbons and oxyge-nate over Cu-based catalysts, and has great potential to store renewable energy and close the carbon cycle. Developing a facile method to modify the local electronic structure of Cu is a useful way to design efficient catalysts. Herein, we design a Pb-doping Cu2O catalyst with controllable Cu-0-Cu+ sites. The catalyst generated a high C-2 faradaic efficiency (FE) of 83.9% with a current density of 203.8 mA cm(-2) at -1.1 V vs. RHE in a flow cell. In situ X-ray absorption spectroscopy and Raman spectroscopy revealed that the Pb doping in Cu2O could stabilize the Cu-0-Cu+ structure and enhance the CO adsorption and C-C coupling, leading to high activity for C-2 product formation. Theoretical calculations also show that Pb doping could reduce the energy barrier for both CO2 activation and C-C coupling processes.

• Institution
  中国科学院; 中国科学院研究生院