The Decaheme Cytochrome MtrC as a Platform for Modular Biohybrid Photocatalysis

Piper, Samuel (2021) The Decaheme Cytochrome MtrC as a Platform for Modular Biohybrid Photocatalysis. Doctoral thesis, University of East Anglia.

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The development of technologies to store solar energy as fuel is a highly active field. So-called solar fuels have the potential to revolutionise humanity’s energy infrastructure and reduce our reliance on fossil fuels. Of particular interest is the use of living cells, typically bacteria, as catalysts for the production of such fuels due to their ability to repair and replicate themselves autonomously. Photocatalytic production of fuels (e.g. hydrogen) by bacteria requires a supply of electrons which must cross from light absorbers in the extracellular environment to enzymatic catalysts inside the cells. Most bacterial membranes are insulating however some specialised “electrogenic” bacteria readily transfer electrons across their membranes to support anaerobic growth. Such bacteria, in particular Shewanella oneidensis MR-1, can use porin:cytochrome complexes such as the MtrCAB complex as membrane-spanning molecular wires which could be adapted to provide the cell with photogenerated electrons.
The work presented in this thesis aimed to develop liposomal nanoreactors which use a photosensitised MtrCAB complex to transfer electrons across lipid bilayers to support catalysis by an encapsulated nitrous oxide reductase enzyme. This goal was pursued by first considering each component of the intended system, from the assembly and photochemistry of a photosensitised MtrCAB complex, to the requirements and encapsulation of the enzyme catalyst. Ultimately, the nanoreactors developed and produced were able to couple extraliposomal photochemistry to intraliposomal enzyme activity, a feat which to our knowledge has not been previously achieved. These nanoreactors serve as a proof-of-principle for the use of MtrCAB as a means of providing living cells with photogenerated electrons for the production of solar fuels.

Item Type: Thesis (Doctoral)
Faculty \ School: Faculty of Science > School of Chemistry
Depositing User: Nicola Veasy
Date Deposited: 06 Apr 2022 13:31
Last Modified: 31 Mar 2023 01:38


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