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Photochemistry: Light-Activated Molecular Wires and Solar Fuels.


Multiheme cytochromes are proposed as Nature’s solution to long-range electron transfer. These novel proteins enable electrons to be transported within, between and outside of bacteria, sometimes over distances greatly exceeding cellular dimensions. Electron transfer is through complementary Fe(III) to Fe(II) transitions of neighbouring hemes which are arranged as chains spanning the proteins’ structures. We apply a rational approach to activate multiheme cytochromes for light-driven long-range electron transfer whereby synthetic photosensitisers absorb visible-light creating energised electrons that are passed into the multiheme cytochromes. The resulting biohybrid materials aims to combine long-range electron transfer through renewable molecules with synthetic materials having that prospects of improved absorption over the incident solar spectrum and photostability when compared to natural Photosystems. Our photosensitised multiheme cytochromes are studied to reveal fundamental characteristics of electron transfer within these proteins and to inspire design concepts for technology delivering solar chemicals, including fuels.  

Our primary focus for these studies are the multiheme cytochromes of Shewanella oneidensis. This bacterium is a model organism for resolving the biochemistry and biophysics of multiheme cytochromes and a chassis for biotechnology exploiting electron transfer across the extracellular envelope.


Selected Publications

1. Rational Design of Covalent Multiheme Cytochrome-Carbon Dot Biohybrids for Photoinduced Electron Transfer

Adv. Funct. Mater. 2023

2. Photocatalytic Removal of the Greenhouse Gas Nitrous Oxide by Liposomal Microreactors

Angew. Chemie. Int. Ed. 2022

3. Nanosecond Heme-to-Heme Electron Transfer Rates in a Multiheme Cytochrome Nanowire Reported by a Spectrally Unique His/Met-Ligated Heme

Proc. Nat. Acad. Sci. USA 2021

4. Ultrafast Light-Driven Electron Transfer in a Ru(II)tris(bipyridine)-Labelled Multiheme Cytochrome.

JACS 2019

5. Towards Compartmentalized Photocatalysis: Multiheme Proteins as Transmembrane Molecular Electron Conduits.

Faraday Discuss 2019

6. Photosensitised Multiheme Cytochromes as Light‐Driven Molecular Wires and Resistors.

ChemBioChem 2018

7. Light-Driven H2-Evolution and C=C or C=O Bond Hydrogenation by Shewanella oneidensis: A Versatile Strategy for Photocatalysis by Nonphotosynthetic Microorganisms.

ACS Catalysis 2017

8. Carbon Dots as Versatile Photosensitizers for Solar-Driven Catalysis with Redox Enzymes.

JACS 2016

9. Photoreduction of Shewanella oneidensis Extracellular Cytochromes by Organic Chromophores and Dye-Sensitized TiO2. 

ChemBioChem 2016


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