Solar-powered electrocatalysis provides a carbon netural means of reducing greenhouse gases and ultimately producing useful chemical fuels and feedstocks. We have adapted an optically transparent thin-layer electrochemical cell to transmission-mode two-dimensional infrared (2D-IR) spectroscopy to characterize structure and dynamics in electrocatalysis intermediates generated under operando conditions. This approach allows us to measure the full range of ultrafast dynamics, such as vibrational relaxation, vibrational energy redistribution, and spectral diffusion for species that are in a steady state under electrochemical potential. We also have found that it is possible to determine spectral diffusion dynamics when the electrochemistry is not at a steady state by monitoring the linear absorbance prior to recording each 2D spectrum. We will present our recent results for CO2 reduction by rhenium tricarbonyl bipyridine complexes.

2D-IR spectroelectrochemistry of CO2 reduction catalysis

ACS Fall 2021

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