Photosensitised Multiheme Cytochromes as Light-Driven Molecular Wires and Resistors

Chembiochem : a European Journal of Chemical Biology
Jessica H van WonderenJulea N Butt

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.

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Citations

Aug 28, 2019·Journal of the American Chemical Society·Jessica H van WonderenJulea N Butt
Nov 4, 2020·The Journal of Physical Chemistry Letters·Zdenek FuteraJochen Blumberger
Sep 25, 2021·Proceedings of the National Academy of Sciences of the United States of America·Jessica H van WonderenJulea N Butt
Oct 6, 2021·Materials Horizons·Jiayu ZengXuemei Wang

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