Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 5, Pages 1345-1349Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201811667
Keywords
adsorbate-adsorbate interactions; in situ studies; DFT; electrocatalysis; Raman spectroscopy
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Funding
- NWO
- NWO [016.Veni.172.034]
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Ag is a promising catalyst for the production of carbon monoxide (CO) via the electrochemical reduction of carbon dioxide (CO2ER). Herein, we study the role of the formate (HCOO-) intermediate *OCHO, aiming to resolve the discrepancy between the theoretical understanding and experimental performance of Ag. We show that the first coupled proton-electron transfer (CPET) step in the CO pathway competes with the Volmer step for formation of *H, whereas this Volmer step is a prerequisite for the formation of *OCHO. We show that *OCHO should form readily on the Ag surface owing to solvation and favorable binding strength. In situ surface-enhanced Raman spectroscopy (SERS) experiments give preliminary evidence of the presence of O-bound bidentate species on polycrystalline Ag during CO2ER which we attribute to *OCHO. Lateral adsorbate interactions in the presence of *OCHO have a significant influence on the surface coverage of *H, resulting in the inhibition of HCOO- and H-2 production and a higher selectivity towards CO.
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