Our research program investigates fundamental mechanisms for coupling photons to fuels by comparing structure and function in natural and artificial photosynthesis. We recently demonstrated a milestone by achieving self-assembled, non-covalent coupling of hydrogen-evolving catalysts to photosynthetic electron transfer in photosystem I. (Utschig et. al. 2011 JACS 133: 16334)  This work suggests a strategy for chemically 'repairing' solar fuels inefficiencies in photosynthesis.  A comparison of rates for light-driven hydrogen production with photosystem I hybrids and a series of artificial photochemical systems that use cobaloxime-based catalysts suggests opportunities to achieve enhanced efficiencies in supramolecular assemblies by coupling hydrogen-evolving catalysts to light-harvesting and charge-transfer relays. Further, we demonstrate opportunities to use in-situ X-ray structural approaches for investigation of structure-function relationships in solar energy conversion. In one example, structural analyses of catalysts in 'artificial leaf' solar catalysts devices will be shown to provide insights and possible concepts for the design of molecular systems for solar fuels conversion.

Structure-function analyses of solar fuels catalysts in natural and artificial photosynthesis

245th National Meeting (2013)

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