Shewanella oneidensis as a living electrode for controlled radical polymerization

Metabolic engineering has facilitated the production of pharmaceuticals, fuels, and soft materials but is generally limited to optimizing well-defined metabolic pathways. We hypothesized that the reaction space available to metabolic engineering could be expanded by coupling extracellular electron t...

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Bibliographic Details
Published in:Proceedings of the National Academy of Sciences - PNAS 2018-05, Vol.115 (18), p.4559-4564
Main Authors: Fan, Gang, Dundas, Christopher M., Graham, Austin J., Lynd, Nathaniel A., Keitz, Benjamin K.
Format: Article
Language:English
Subjects:
Biological Sciences
Catalysis
Catalysts
Coupling (molecular)
E coli
Electron transfer
Electron transport
Fuels
Metabolic engineering
Metabolic pathways
Metabolism
Molecular weight
Optimization
Pharmaceuticals
Physical Sciences
Polydispersity
Polymer chemistry
Polymerization
Proteins
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Summary:Metabolic engineering has facilitated the production of pharmaceuticals, fuels, and soft materials but is generally limited to optimizing well-defined metabolic pathways. We hypothesized that the reaction space available to metabolic engineering could be expanded by coupling extracellular electron transfer to the performance of an exogenous redox-active metal catalyst. Here we demonstrate that the electroactive bacterium Shewanella oneidensis can control the activity of a copper catalyst in atom-transfer radical polymerization (ATRP) via extracellular electron transfer. Using S. oneidensis, we achieved precise control over the molecular weight and polydispersity of a bioorthogonal polymer while similar organisms, such as Escherichia coli, showed no significant activity. We found that catalyst performance was a strong function of bacterial metabolism and specific electron transport proteins, both of which offer potential biological targets for future applications. Overall, our results suggest that manipulating extracellular electron transport pathways may be a general strategy for incorporating organometallic catalysis into the repertoire of metabolically controlled transformations.
ISSN:0027-8424
1091-6490
DOI:10.1073/pnas.1800869115