The splitting of water into hydrogen and oxygen gas via artificial photosynthesis (AP) has been attracting considerable attention as a promising way to convert and store solar energy in chemical bonds.1-3 The ultimate goal of such a carbon-free energy system based on photo-driven water splitting into hydrogen and oxygen still remains challenging despite extensive experimental investigations and mechanistic studies on these proton reduction systems over the past two decades. Herein, we will present our recent research on photocatalytic generation of hydrogen using Fe-based dithiolene complexes as catalysts, water-soluble CdSe nanocrystals as photosensitizer, and ascorbic acid (AA) as the sacrificial electron donor.4 The activities of these complexes correlate well with ligand electron donor ability. The resulting turnover numbers (TONs) range from thousands to hundreds of thousands depending on the catalysts used and experimental conditions. In addition, an approach with the goal of eliminating sacrificial electron donors involves the development of photoelectrochemical H2-generating device in which a engineered photocathode is constructed via sensitization of a p-type NiO semiconductor with tunable quantum dot light absorbers.5

Efficient photocatalytic and photoelectrochemical generation of hydrogen in noble-metal-free systems

256th National Meeting (2018)

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