The ability to use carbon dioxide (CO2) as a precursor for renewably powered electrosynthesis is an exciting approach for mitigating climate change as well as for synthesizing high value chemical products with less-carbon intensive energy inputs. To achieve this goal requires the development of catalysts that both efficiently and selectively reduce CO2. Toward this end, Au and Cu nanoparticles (both unary and alloyed) have been shown to reduce CO2 to carbon monoxide (CO) with high selectivity and at relatively low overpotentials. The continued development of these catalysts requires an intimate understanding of the surface species present at different potentials in addition to how those species change in different local environments. Spectroelectrochemical surface enhanced Raman spectroscopy provides a chemically specific tool for monitoring how surface species change as a function of catalyst composition, potential, electrolyte conditions, and ligand choice; particularly those related to CO electrosynthesis. Plane wave density functional theory (DFT) calculations are used to provide additional insight into those structural and environmental factors that control intermediate binding strength.

Monitoring surface species during carbon dioxide reduction using in situ Raman spectroscopy

253rd National Meeting (2017)

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