Nature has perfected the conversion of light energy to chemical energy in photosynthesis through a finely tuned network of protein-based reaction centers.  In photosynthetic cells, the association of Photosystem I and Photosystem II allows the extraction of electrons from water in the presence of sunlight to facilitate the formation of energy dense sugars and macromolecules from carbon dioxide.  Photosystem I (PSI) is a large thylakoid-centralized, molecular complex composed of several cross-membrane protein domains and associated bioorganic pigments and light absorbing compounds.  Upon excitation by light, PSI undergoes complex unidirectional electron transfers across multiple redox centers within the protein.  This light-induced charge separation is then utilized in the production of energy in the plant in the form of NAD(P)H.  The focus of our research is the decoupling of this photosynthetic pathway of PSI to allow the production of molecular hydrogen, rather than NAD(P)H, through a fusion with inorganic materials to produce a photocatalytic hydrogen-evolving system.This presentation illustrates our work in understanding PSI for solar energy conversion, and our progress in developing this system using computational chemistry, electrochemistry, and molecular biology approaches.  Areas of interest to our collaboration include the controlled surface assembly of wild-type and modified PSI complexes onto electrodes, the use of computational chemistry approaches to identify the binding site of cytochrome c6 to PSI and optimize charge transfer across that interface, and the design of chimeric PSI protein domains and cytochrome c6 oligomers.

Re-engineering Photosystem I as a photocatalytic hydrogen producing reactor

243rd National Meeting (2012)

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