Photosensitised Multiheme Cytochromes as Light‐Driven Molecular Wires and Resistors

van Wonderen, Jessica H., Li, Daobo, Piper, Samuel E. H., Lau, Cheuk Y., Jenner, Leon P., Hall, Christopher R., Clarke, Thomas A., Watmough, Nicholas J. and Butt, Julea N. (2018) Photosensitised Multiheme Cytochromes as Light‐Driven Molecular Wires and Resistors. ChemBioChem, 19 (20). pp. 2206-2215. ISSN 1439-4227

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Abstract

Multiheme cytochromes possess closely packed redox‐active hemes arranged as chains spanning the tertiary structure. Here we describe five variants of a representative multiheme cytochrome engineered as biohybrid phototransducers for converting light into electricity. Each variant possesses a single Cys sulfhydryl group near a terminus of the heme chain, and this was efficiently labelled with a RuII(2,2′‐bipyridine)3 photosensitiser. When irradiated in the presence of a sacrificial electron donor (SED) the proteins exhibited different types of behaviour. Certain proteins were rapidly and fully reduced. Other proteins were rapidly semi‐reduced but resisted complete photoreduction. These findings reveal that photosensitised multiheme cytochromes can be engineered to act as resistors, with intrinsic regulation of light‐driven electron accumulation, and also as molecular wires with essentially unhindered photoreduction. It is proposed that the observed behaviour arises from interplay between the site of electron injection and the distribution of heme reduction potentials along the heme chain.

Item Type: Article
Uncontrolled Keywords: small tetraheme cytochrome (stc),shewanella oneidensis,electron transfer,ruthenium tris bipyridine,photocatalysis
Faculty \ School: Faculty of Science > School of Chemistry
Faculty of Science > School of Biological Sciences
Depositing User: LivePure Connector
Date Deposited: 24 Jul 2018 12:30
Last Modified: 18 Sep 2020 00:18
URI: https://ueaeprints.uea.ac.uk/id/eprint/67837
DOI: 10.1002/cbic.201800313

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