Study of CuSb bimetallic flow-through gas diffusion electrodes for efficient electrochemical CO2 reduction to CO

Azeem Mustafa; Bachirou Guene Lougou; Yong Shuai; Zhijiang Wang; Haseeb Ur-Rehman; Samia Razzaq; Wei Wang; Ruming Pan; Fanghua Li; Lei Han

doi:10.1016/j.jcis.2023.11.168

Study of CuSb bimetallic flow-through gas diffusion electrodes for efficient electrochemical CO₂ reduction to CO

J Colloid Interface Sci. 2024 Mar:657:363-372. doi: 10.1016/j.jcis.2023.11.168. Epub 2023 Nov 30.

Authors

Azeem Mustafa¹, Bachirou Guene Lougou², Yong Shuai³, Zhijiang Wang⁴, Haseeb Ur-Rehman⁵, Samia Razzaq⁶, Wei Wang¹, Ruming Pan¹, Fanghua Li⁷, Lei Han⁸

Affiliations

¹ Key Laboratory of Aerospace Thermophysics of MIIT, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China; School of Energy Science and Engineering, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China.
² Key Laboratory of Aerospace Thermophysics of MIIT, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China; School of Energy Science and Engineering, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China; MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China. Electronic address: lougou@hit.edu.cn.
³ Key Laboratory of Aerospace Thermophysics of MIIT, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China; School of Energy Science and Engineering, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China. Electronic address: shuaiyong@hit.edu.cn.
⁴ MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China.
⁵ Mechanical Engineering Department, University of Engineering and Technology, 47050, Taxila, Pakistan.
⁶ School of Aerospace, Mechanical and Mechatronics Engineering, University of Sydney, Sydney 2006, Australia.
⁷ Department of Environmental Science and Engineering, Harbin Institute of Technology, Harbin 150090, China.
⁸ School of Energy Science and Engineering, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China.

PMID: 38043238
DOI: 10.1016/j.jcis.2023.11.168

Abstract

Electrochemical CO₂ reduction (eCO₂R) to industrially important feedstock has received great attention, but it faces different challenges. Among them, the poor CO₂ mass transport due to low intrinsic CO₂ solubility significantly limits the rate of reduction reactions, leading to lower catalytic performance; thereby, commercially relevant current densities can't be achieved. Moreover, the poor activity and selectivity of high-cost monometallic catalysts, including Cu, Zn, Ag, and Au, undermine the efficiency of eCO₂R. Flow-through gas diffusion electrodes (FTGDE), a newly developed class of GDEs, can potentially solve the issue of poor CO₂ mass transport because they directly feed the CO₂ to the catalyst layer. In addition, abundant surface area, porous structure, and improved triple-phase interface make them an excellent candidate for extremely high rate eCO₂R. Antimony, a low-cost and abundant metalloid, can be effectively tuned with Cu to produce useful products such as CO, formate, and C₂H₄ through eCO₂R. Herein, a series of porous binary CuSb FTGDEs with different Sb compositions are fabricated for the electrocatalytic reduction of CO₂ to CO. The results show that the catalytic performance of CuSb FTGDEs improved with increasing Sb content up to a certain threshold, beyond which it started to decrease. The CuSb FTGDE with 5.4 g of antimony demonstrated higher current density (206.4 mA/cm²) and faradaic efficiency (72.82 %) at relatively lower overpotentials. Compared to gas diffusion configuration, the poor catalytic activity and selectivity achieved by CuSb FTGDE in non-gas diffusion configuration signifies the importance of improved local CO₂ concentration and improved triple-phase interface formation in GDE configuration. The several hours stable operation of CuSb FTGDEs during eCO₂R demonstrates its potential for efficient electrocatalytic conversion applications.

Keywords: CO(2) electroreduction; CuSb; Flow-through structure; Gas diffusion electrode; Local CO(2) concentration.