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Wiring of photosystem II to hydrogenase for photoelectrochemical water splitting

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Mersch, Dirk, Lee, Chong-Yong, Zhang, Jenny Zhenqi, Brinkert, Katharina, Fontecilla-Camps, Juan C., Rutherford, A. William and Reisner, Erwin (2015) Wiring of photosystem II to hydrogenase for photoelectrochemical water splitting. Journal of the American Chemical Society, 137 (26). pp. 8541-8549. doi:10.1021/jacs.5b03737

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Official URL: http://dx.doi.org/10.1021/jacs.5b03737

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Abstract

In natural photosynthesis, light is used for the production of chemical energy carriers to fuel biological activity. The re-engineering of natural photosynthetic pathways can provide inspiration for sustainable fuel production and insights for understanding the process itself. Here, we employ a semiartificial approach to study photobiological water splitting via a pathway unavailable to nature: the direct coupling of the water oxidation enzyme, photosystem II, to the H2 evolving enzyme, hydrogenase. Essential to this approach is the integration of the isolated enzymes into the artificial circuit of a photoelectrochemical cell. We therefore developed a tailor-made hierarchically structured indium–tin oxide electrode that gives rise to the excellent integration of both photosystem II and hydrogenase for performing the anodic and cathodic half-reactions, respectively. When connected together with the aid of an applied bias, the semiartificial cell demonstrated quantitative electron flow from photosystem II to the hydrogenase with the production of H2 and O2 being in the expected two-to-one ratio and a light-to-hydrogen conversion efficiency of 5.4% under low-intensity red-light irradiation. We thereby demonstrate efficient light-driven water splitting using a pathway inaccessible to biology and report on a widely applicable in vitro platform for the controlled coupling of enzymatic redox processes to meaningfully study photocatalytic reactions.

Item Type: Journal Article
Subjects: Q Science > QK Botany
Divisions: Faculty of Science > Life Sciences (2010- )
Library of Congress Subject Headings (LCSH): Photosynthesis, Hydrogenase
Journal or Publication Title: Journal of the American Chemical Society
Publisher: American Chemical Society
ISSN: 0002-7863
Official Date: 2015
Dates:
DateEvent
2015Published
5 June 2015Available
5 June 2015Accepted
Volume: 137
Number: 26
Page Range: pp. 8541-8549
DOI: 10.1021/jacs.5b03737
Status: Peer Reviewed
Publication Status: Published
Access rights to Published version: Open Access
RIOXX Funder/Project Grant:
Project/Grant IDRIOXX Funder NameFunder ID
EP/H00338X/2[EPSRC] Engineering and Physical Sciences Research Councilhttp://dx.doi.org/10.13039/501100000266
EP/G037221/1[EPSRC] Engineering and Physical Sciences Research Councilhttp://dx.doi.org/10.13039/501100000266
BB/K002627/1[BBSRC] Biotechnology and Biological Sciences Research Councilhttp://dx.doi.org/10.13039/501100000268
BB/K010220/1[BBSRC] Biotechnology and Biological Sciences Research Councilhttp://dx.doi.org/10.13039/501100000268
PIEF-GA-2013-62503Marie Curie Cancer Carehttp://dx.doi.org/10.13039/501100000654
PIIF-GA-2012-328085 RPSIIMarie Curie Cancer Carehttp://dx.doi.org/10.13039/501100000654
UNSPECIFIED[CNRS] Centre National de la Recherche Scientifiquehttp://dx.doi.org/10.13039/501100004794
Wolfson Merit Award[RS] Royal Societyhttp://dx.doi.org/10.13039/501100000288
UNSPECIFIEDUniversité de Grenoblehttp://viaf.org/viaf/154496835

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