1. Surface Water as an Initial Proton Source for the Electrochemical CO Reduction Reaction on Copper Surfaces.
- Author
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Shao, Feng, Xia, Zhaoming, You, Futian, Wong, Jun Kit, Low, Qi Hang, Xiao, Hai, and Yeo, Boon Siang
- Subjects
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ELECTROLYTIC reduction , *PROTON transfer reactions , *SURFACE enhanced Raman effect , *COPPER surfaces , *SURFACE reactions , *PROTONS , *DENSITY functional theory , *RADIOLABELING , *SERS spectroscopy - Abstract
We have employed in situ electrochemical shell‐isolated nanoparticle‐enhanced Raman spectroscopy (SHINERS) and density functional theory (DFT) calculations to study the CO reduction reaction (CORR) on Cu single‐crystal surfaces under various conditions. Coadsorbed and structure‐/potential‐dependent surface species, including *CO, Cu−Oad, and Cu−OHad, were identified using electrochemical spectroscopy and isotope labeling. The relative abundance of *OH follows a "volcano" trend with applied potentials in aqueous solutions, which is yet absent in absolute alcoholic solutions. Combined with DFT calculations, we propose that the surface H2O can serve as a strong proton donor for the first protonation step in both the C1 and C2 pathways of CORR at various applied potentials in alkaline electrolytes, leaving adsorbed *OH on the surface. This work provides fresh insights into the initial protonation steps and identity of key interfacial intermediates formed during CORR on Cu surfaces. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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