Issue 35, 2024

Experimental trends and theoretical descriptors for electrochemical reduction of carbon dioxide to formate over Sn-based bimetallic catalysts

Abstract

The electrochemical carbon dioxide reduction reaction (CO2RR) using renewable energy sources is a promising solution for mitigating CO2 emissions. In particular, CO2RR to formate represents a commercially profitable target. However, a comprehensive understanding of the catalytic mechanisms of Sn-based catalysts under reaction conditions, including the real-time structural evolution of catalysts and the role of all key reaction intermediates in influencing the CO2RR selectivity, is still lacking. The current study reports a framework to study the selectivity preference of Sn-based bimetallic catalysts using a combination of electrochemical measurements, in situ characterization, and density functional theory (DFT) calculations. The addition of a second metal (Co, Ni, Ag, Zn, Ga, Bi) was found to play a vital role in affecting the CO2RR performance. In situ X-ray absorption near edge structure (XANES) measurements revealed a dynamic evolution in the Sn valence state induced by different secondary metals. A multidimensional descriptor involving all the key reaction intermediates was developed to assess formate selectivity using a 2-dimensional volcano plot. This research offers an effective framework for understanding CO2RR catalytic selectivity by considering both the real-time structural evolution of catalysts and all the key intermediates involved.

Graphical abstract: Experimental trends and theoretical descriptors for electrochemical reduction of carbon dioxide to formate over Sn-based bimetallic catalysts

Supplementary files

Article information

Article type
Paper
Submitted
05 اپریل 2024
Accepted
31 جوٗلایی 2024
First published
31 جوٗلایی 2024

J. Mater. Chem. A, 2024,12, 23560-23569

Experimental trends and theoretical descriptors for electrochemical reduction of carbon dioxide to formate over Sn-based bimetallic catalysts

X. Han, B. Wu, Y. Wang, N. N. Nichols, Y. Kwon, Y. Yuan, Z. Xie, S. Kang, B. Gil, C. Wang, T. Mou, H. Lin, Y. Nian and Q. Chang, J. Mater. Chem. A, 2024, 12, 23560 DOI: 10.1039/D4TA02315C

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