Abstract
Photoelectrocatalysis offers a way to generate hydrogen and oxygen from water under ambient light. Here, a series of hydrogen evolving photocatalysts based on a ruthenium(II) bipyridyl sensitiser covalently linked to platinum or palladium catalytic centres were adsorbed onto mesoporous nickel oxide and tested for hydrogen evolution in a photoelectrochemical half-cell. The electrolyte buffer was varied and certain catalysts performed better at pH 7 than pH 3 (for example, PC3 with photocurrent density = 8 μA cm–2), which is encouraging for coupling with an oxygen evolving photoanode in tandem water splitting devices. The molecular catalysts were surprisingly robust when integrated into devices, but the overall performance appears to be limited by rapid recombination at the photocatalyst|NiO interface. Our findings provide further insight towards basic design principles for hydrogen evolving photoelectrochemical systems and guidelines for further development.
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