Publication date: 15th December 2014
Solar photocatalytic water splitting is most certainly a blooming research area with an ever increasing (and unkown) number of research groups working worldwide very actively in this field. Hence, this presentation does not aim to present an overview of these activities which appears to be an (almost) impossible task. I will rather discuss some crucial issues that according to my judgement are frequently overlooked when working in this field with great enthusiasm. In principle, the photocatalytic system seems to be ideal for basic investigations as it mimics a short-circuited photoelectrochemical device which definitely should be the final target of all such efforts. Unfortunately, however, as stoichiometric photocatalytic water splitting is rarely observed most published work fucuses on so-called sacrificial systems that include molecules other than H2O to be oxidized (e.g., CH3OH) or reduced (e.g., Ag+), respectively. The - often very interesting - results of these studies, however, cannot really be appreciated if the entire chemistry of the (now even more complex) system is not understood, i.e., complete material balances definitely need to be provided! Several possible mechanisms of the chemical transformation of these sacrificial reagents will thus be discussed. Moreover, details of the mechanisms of the two or four electron transfer processes finally resulting in the formation of molecular hydrogen or molecular oxygen, respectively, are also still far from being understood. Herein, examples of kinetic studies will be presented aiming to identify reaction intermediates, their chemical (and thermodynamic) nature and their final fate. I am convinced that without a detailed knowledge of these processes it will be difficult (if not impossible) to improve their efficiency. Based upon the work of our own laboratories this lecture will be mainly concerned with photocatalytic reactions occuring at metal oxide particles such as titanium dioxide, hematite, or sodium tantalates. However, many of the proposed mechanisms are considered to be quite universal.
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