Proceedings of nanoGe Fall Meeting19 (NFM19)
Publication date: 18th July 2019
Water oxidation reaction, also denoted as oxygen evolution reaction (OER), is a key step in natural and artificial photosynthesis. For direct coupling with CO2 reduction reactions (CO2RR), OER needs to proceed in the neutral pH regime. Here, amorphous CoCat catalyst is chosen as a model to understand electrokinetics and the catalytic mechanism.[1] We report three parallel trial sets with varying phosphate buffer (KPi) concentration based on chronoamperometry measurement in the potential range from 1.1 V to 1.6 V vs NHE. It was found that the catalytic current was affected by the KPi concentration on specific operation conditions.
In detail, at low potential, the catalytic current is almost independent on the phosphate buffer concentration, even if additional KNO3 was added to the solution or the solution was stirred. However, increasing the potential to values above 1.2 V significantly ramps the catalytic current, because the buffer plays a key role in accelerating the proton transfer. In contrast, adding KNO3 has no major impact in the current density, which elucidates that increasing the electrical conductivity alone (without increasing the number of protons) does not improve the catalytic efficiency. Stirring, however, enhances the diffusion of phosphate resulting in increased current densities, reducing the formation of local pH gradients, which would hamper catalysis. Finally, combining high voltages with high buffer concentrations and high rate of particle convection (i.e. stirring) leads to the highest current densities. Operando Raman and X-ray absorption spectroscopy are undergoing to analyse near-surface pH gradients and determine redox kinetics.
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