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Photo-Driven Hydrogen Evolution by an Artificial Hydrogenase Utilizing the Biotin-Streptavidin Technology

Keller, Sascha G. and Probst, Benjamin and Heinisch, Tillmann and Alberto, Roger and Ward, Thomas R.. (2018) Photo-Driven Hydrogen Evolution by an Artificial Hydrogenase Utilizing the Biotin-Streptavidin Technology. Helvetica Chimica Acta, 101 (4). e1800036.

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Official URL: https://edoc.unibas.ch/70597/

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Abstract

Photocatalytic hydrogen evolution by an artificial hydrogenase based on the biotin-streptavidin technology is reported. A biotinylated cobalt pentapyridyl-based hydrogen evolution catalyst (HEC) was incorporated into different mutants of streptavidin. Catalysis with [Ru(bpy)(3)]Cl-2 as a photosensitizer (PS) and ascorbate as sacrificial electron donor (SED) at different pH values highlighted the impact of close lying amino acids that may act as a proton relay under the reaction conditions (Asp, Arg, Lys). In the presence of a close-lying lysine residue, both, the rates were improved, and the reaction was initiated much faster. The X-ray crystal structure of the artificial hydrogenase reveals a distance of 8.8 angstrom between the closest lying Co-moieties. We thus suggest that the hydrogen evolution mechanism proceeds via a single Co centre. Our findings highlight that streptavidin is a versatile host protein for the assembly of artificial hydrogenases and their activity can be fine-tuned via mutagenesis.
Faculties and Departments:05 Faculty of Science > Departement Chemie > Chemie > Bioanorganische Chemie (Ward)
UniBasel Contributors:Ward, Thomas R. R. and Keller, Sascha and Heinisch, Tillmann
Item Type:Article, refereed
Article Subtype:Research Article
Publisher:Wiley
ISSN:0018-019X
e-ISSN:1522-2675
Note:Publication type according to Uni Basel Research Database: Journal article
Language:English
Identification Number:
Last Modified:23 May 2019 15:24
Deposited On:23 May 2019 12:30

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