Publication date: 15th December 2014
Understanding the kinetics of multistep electron transfer reactions involving minority carriers at semiconductor/electrolyte interfaces is essential if progress is to be made in light-driven water splitting. Unfortunately, the methods that are used to study interfacial electron electron transfer at metal electrodes are generally not directly applicable to minority carrier reactions at semiconductor electrodes. Furthermore, the problem becomes even more complex if the semiconductor electrode is nanostructured, since the processes of carrier generation, transport, recombination and interfacial transfer must be considered in three dimensions. Nevertheless, considerable progress has been achieved using photoelectrochemical and spectroscopic methods to follow minority carrier reactions. The key here is that the exciting stimulus involves perturbation of the minority carrier generation rate by illumination rather than (as is the case for metal electrodes) perturbation of the potential difference across the Helmholtz layer. In simple terms, we perturb the concentration (i.e. entropy) term rather than the internal energy term in the Gibbs free energy of the system. This talk will contrast the behaviour of metal and semiconductor electrodes and review some of the time and frequency-resolved methods that can be applied to study the kinetics of interfacial charge transfer and the way that interfacial electron transfer competes with surface electron-hole recombination in a photoelectrode reaction such as oxygen or hydrogen evolution.
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