Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.018
Publication date: 6th July 2018
There is a need to rationalise the catalytic mechanisms occurring during solar fuels production if the design rules for improved materials are to be identified. With both direct solar to fuels materials (e.g. photoelectrodes) and indirect systems (e.g. PV driven electrolysis) there is a common challenge – how to characterise short-lived intermediates that are present only at the electrode surface in the presence of a high concentration of bulk solvent/reagent.
IR-Vis Sum-Frequency Generation (SFG) spectroscopy specifically probes molecules at interfaces offering a sensitive probe of only the catalytically relevant species at the electrode surface. SFG has been widely used to study model electrochemical systems but rarely to explore the mechanisms of carbon dioxide reduction and water oxidation. Here I will describe both early experiments to examine photoelectrode surfaces and our recent reports on the mechanisms of carbon dioxide reduction by group 6 and 7 transition metal electrocatalysts which allow for the identification of new catalytic intermediates and the first in-situ observation of the “protonation-first” pathway by [Mn(bpy)(CO)3Br]. We will also discuss how the potential and light dependence of the non-resonant response recorded during the SFG experiment can provide important insights into the changing nature of the double layer structure during the study of solar fuels materials.
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