[FeFe]-hydrogenases and photobiological hydrogen production

Maria L. Ghirardi; Jordi Cohen; Paul King; Klaus Schulten; Kwiseon Kim; Michael Seibert

doi:10.1117/12.683767

8 September 2006 [FeFe]-hydrogenases and photobiological hydrogen production

Maria L. Ghirardi, Jordi Cohen, Paul King, Klaus Schulten, Kwiseon Kim, Michael Seibert

Proceedings Volume 6340, Solar Hydrogen and Nanotechnology; 63400X (2006) https://doi.org/10.1117/12.683767
Event: SPIE Optics + Photonics, 2006, San Diego, California, United States

Abstract

The promise of efficient, economic and renewable H₂ photoproduction from water can potentially be met by green algae. These organisms are able to functionally link photosynthetic water oxidation to the catalytic recombination of protons and electrons to generate H₂ gas through the activity of the hydrogenase enzyme. Green algal hydrogenases contain a unique metallo-catalytic H-cluster that performs the reversible H₂ oxidation /evolution reactions. The H-cluster, located in the interior of the protein structure is irreversibly inactivated by O₂, the by-product of water oxidation. We developed an Escherichi coli expression system to produce [FeFe]-hydrogenases from different biological sources and demonstrated that clostridial [FeFe]-hydrogenases have higher tolerance to O₂ inactivation compared to their algal counterparts. We have been using computational simulations of gas diffusion within the Clostridium pasteurianum CpI hydrogenase to identify the pathways through which O₂ can reach its catalytic site. Subsequently, we modify the protein structure at specific sites along the O₂ pathways (identified by the computational simulations) by site-directed mutagenesis with the goal of generating recombinant enzymes with higher O₂ tolerance. In this paper, we review the computational simulation work and report on preliminary results obtained through this strategy.

Citation Download Citation

Maria L. Ghirardi, Jordi Cohen, Paul King, Klaus Schulten, Kwiseon Kim, and Michael Seibert "[FeFe]-hydrogenases and photobiological hydrogen production", Proc. SPIE 6340, Solar Hydrogen and Nanotechnology, 63400X (8 September 2006); https://doi.org/10.1117/12.683767

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