Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.023
Publication date: 23rd September 2021
The kinetics of electrochemical reactions are typically analysed through Butler-Volmer analyses of current – voltage data. Such analyses have been very effective at determining electrochemical kinetics on metal electrodes. However their application to the kinetics of (photo)electrocatalytic water oxidation / reduction on metal oxides can be more challenging, due to multiple redox transitions observed in such metal oxides, the localised nature of these transitions and the complexity of the water oxidation / reduction reactions. In my talk I will address the potential of operando spectrochemistry to determine redox state population densities in metal oxides electrodes and photoelectrodes, and the use of such data to undertake rate law analyses of water oxidation / reduction. These studies will primarily be applied to Ni/Fe oxyhydroxide electrocatalysts and hematite photoanodes for water oxidation, as well as comparison with other metal oxide for both water oxidation and reduction. These studies will address the nature of the states driving water oxidation / reduction and the reaction kinetics and dependence upon population density. For example for Ni(M)OOH electrocatalysts, these studies will address the impact of metal (M) substitution on both the population densities and reaction rate constants, and how these together impact upon the overall current / voltage behaviour. A key conclusion of my talk will be that for the systems studied the kinetics of water / oxidation appear to be primarily driven by the population of states driving these reactions – and as such it more appropriate to employ rate law rather than Butler-Volmer models in analysing these kinetics.
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