The development of hydrogen (H<sub>2</sub>) as an environmentally friendly fuel requires catalysts capable of efficient proton reduction. Ideally, these catalysts would be active in water near neutral pH, insensitive to oxygen, and insensitive to added ions and impurities. Biomolecules are attractive scaffolds to use for engineering artificial hydrogenases because of their compatibility with aqueous media and the wide range of derivatives that can be accessed using site-directed mutagenesis and protein chemistry. In this presentation, progress toward the development of biomolecular artificial hydrogenases will be presented. One class contains cobalt porphyrin active sites that display high activity and stability at neutral pH in the presence of air. Turnover numbers of over 100,000 have been achieved under electrocatalytic conditions. To demonstrate successful solar energy storage, a zinc porphyrin-based photosensitizer has been paired with cobalt porphyrin-based catalysts to yield hundreds of turnovers. The catalysts also display high activity in seawater, the world's most abundant proton source. Ongoing refinements are toward further increasing stability and lowering overpotential by engineering protein structure. A new class of artificial hydrogenases based on metallopeptides also will be presented.

Artificial hydrogenases for solar hydrogen production

249th National Meeting (2015)

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