Achieving high selectivity and activity of CO2 electroreduction to formate by in-situ synthesis of single atom Pb doped Cu catalysts

Yurui Xu; Xiao Liu; Minghui Jiang; Bichuan Chi; Yue Lu; Jin Guo; Ziming Wang; Suping Cui

doi:10.1016/j.jcis.2024.03.137

Achieving high selectivity and activity of CO₂ electroreduction to formate by in-situ synthesis of single atom Pb doped Cu catalysts

J Colloid Interface Sci. 2024 Jul:665:365-375. doi: 10.1016/j.jcis.2024.03.137. Epub 2024 Mar 26.

Authors

Yurui Xu¹, Xiao Liu², Minghui Jiang³, Bichuan Chi⁴, Yue Lu⁵, Jin Guo⁶, Ziming Wang³, Suping Cui³

Affiliations

¹ College of Materials Science & Engineering, Beijing University of Technology, Beijing 100124, China; Institute of Disaster Prevention, Sanhe 065201, China.
² College of Materials Science & Engineering, Beijing University of Technology, Beijing 100124, China. Electronic address: liux@bjut.edu.cn.
³ College of Materials Science & Engineering, Beijing University of Technology, Beijing 100124, China.
⁴ China Institute of Building Standard Design and Research, Beijing 100048, China.
⁵ Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing 100124, China.
⁶ State Key Laboratory of Mechanical Behavior and System Safety of Traffic Engineering Structures, Shijiazhuang Tiedao University, Shijiazhuang 050043, China.

PMID: 38537585
DOI: 10.1016/j.jcis.2024.03.137

Abstract

Exploring highly selective and stable electrocatalysts is of great significance for the electrochemical conversion of CO₂ into fuel. Herein, a three-dimensional (3D) nanostructure catalyst was developed by doping Pb single-atom (Pb_SA) in-situ on carbon paper (Pb_SA100-Cu/CP) through a low-energy and economical method. The designed catalyst exhibited abundant active sites and was beneficial to CO₂ adsorption, activation, and subsequent conversion to fuel. Interestingly, Pb_SA100-Cu/CP showed a prominent Faraday efficiency (FE) of 97 % at -0.9 V versus reversible hydrogen electrode (vs. RHE) and a high partial current density of 27.9 mA·cm^-2 for formate. Also, the catalyst remained significantly stable for 60 h during the durability test. The reaction mechanism was investigated by density functional theory (DFT), demonstrating that the doping Pb_SA induced the electrons redistribution, promoted the formate generation, reduced the rate-determining step (RDS) energy barrier, and inhibited the hydrogen evolution reaction. The study aims to provide a new strategy for developing of single-atom catalysts with high selectivity and stability, which will help reduce environmental pressure and alleviate energy problems.

Keywords: CO(2) reduction; Catalyst; Formate; High selectivity; Single atom.