1. In-situ spectroscopic probe of the intrinsic structure feature of single-atom center in electrochemical CO/CO 2 reduction to methanol.
- Author
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Ren X, Zhao J, Li X, Shao J, Pan B, Salamé A, Boutin E, Groizard T, Wang S, Ding J, Zhang X, Huang WY, Zeng WJ, Liu C, Li Y, Hung SF, Huang Y, Robert M, and Liu B
- Subjects
- Spectroscopy, Fourier Transform Infrared, Adsorption, Carbon, Carbon Dioxide, Methanol
- Abstract
While exploring the process of CO/CO
2 electroreduction (COx RR) is of great significance to achieve carbon recycling, deciphering reaction mechanisms so as to further design catalytic systems able to overcome sluggish kinetics remains challenging. In this work, a model single-Co-atom catalyst with well-defined coordination structure is developed and employed as a platform to unravel the underlying reaction mechanism of COx RR. The as-prepared single-Co-atom catalyst exhibits a maximum methanol Faradaic efficiency as high as 65% at 30 mA/cm2 in a membrane electrode assembly electrolyzer, while on the contrary, the reduction pathway of CO2 to methanol is strongly decreased in CO2 RR. In-situ X-ray absorption and Fourier-transform infrared spectroscopies point to a different adsorption configuration of *CO intermediate in CORR as compared to that in CO2 RR, with a weaker stretching vibration of the C-O bond in the former case. Theoretical calculations further evidence the low energy barrier for the formation of a H-CoPc-CO- species, which is a critical factor in promoting the electrochemical reduction of CO to methanol., (© 2023. The Author(s).)- Published
- 2023
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