Abstract

Efficient production of solar fuels is an imperative for meeting future fossil-fuel-free energy demands. Hydrogen that is derived from the splitting of water by solar energy is clearly attractive as a clean energy vector, and there have been many attempts to construct viable molecular and biomolecular devices for photohydrogen production. A common approach in the construction of such devices is the utilization of tris(bipyridine)ruthenium, zinc porphyrin, or related molecular materials as photosensitizers in conjunction with a tethered or free electrocatalyst or enzymic system. Apart from cost, such systems suffer from having limited lifetimes, which may be attributed at least in part to the intrinsic reactivity of the organic N-donor ligands in the radical anion form of the photoexcited state and photodegradation pathways.

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