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Application of a Synthetic Ferredoxin‐Inspired [4Fe4S]‐Peptide Maquette as the Redox Partner for an [FeFe]‐Hydrogenase

Bombana, Andrea; Shanmugam, Muralidharan; Collison, David; Kibler, Alexander J.; Newton, Graham N.; Jäger, Christof M.; Croft, Anna K.; Morra, Simone; Mitchell, Nicholas J.

Application of a Synthetic Ferredoxin‐Inspired [4Fe4S]‐Peptide Maquette as the Redox Partner for an [FeFe]‐Hydrogenase Thumbnail


Authors

Andrea Bombana

Muralidharan Shanmugam

David Collison

Alexander J. Kibler

Christof M. Jäger

Anna K. Croft

Profile image of SIMONE MORRA

SIMONE MORRA SIMONE.MORRA@NOTTINGHAM.AC.UK
Assistant Professor in Chemical &environmental Engineering



Abstract

‘Bacterial-type’ ferredoxins host a cubane [4Fe4S]2+/+ cluster that enables these proteins to mediate electron transfer and facilitate a broad range of biological processes. Peptide maquettes based on the conserved cluster-forming motif have previously been reported and used to model the ferredoxins. Herein we explore the integration of a [4Fe4S]-peptide maquette into a H2-powered electron transport chain. While routinely formed under anaerobic conditions, we illustrate by electron paramagnetic resonance (EPR) analysis that these maquettes can be reconstituted under aerobic conditions by using photoactivated NADH to reduce the cluster at 240 K. Attempts to tune the redox properties of the iron-sulfur cluster by introducing an Fe-coordinating selenocysteine residue were also explored. To demonstrate the integration of these artificial metalloproteins into a semi-synthetic electron transport chain, we utilize a ferredoxin-inspired [4Fe4S]-peptide maquette as the redox partner in the hydrogenase-mediated oxidation of H2.

Citation

Bombana, A., Shanmugam, M., Collison, D., Kibler, A. J., Newton, G. N., Jäger, C. M., …Mitchell, N. J. (2023). Application of a Synthetic Ferredoxin‐Inspired [4Fe4S]‐Peptide Maquette as the Redox Partner for an [FeFe]‐Hydrogenase. ChemBioChem, 24(18), Article e202300250. https://doi.org/10.1002/cbic.202300250

Journal Article Type Article
Acceptance Date Jun 28, 2023
Online Publication Date Jun 30, 2023
Publication Date Sep 15, 2023
Deposit Date Jul 14, 2023
Publicly Available Date Jul 1, 2024
Journal ChemBioChem
Print ISSN 1439-4227
Electronic ISSN 1439-7633
Publisher Wiley
Peer Reviewed Peer Reviewed
Volume 24
Issue 18
Article Number e202300250
DOI https://doi.org/10.1002/cbic.202300250
Keywords Iron-sulfur; Peptide; Maquette; hydrogenase; EPR
Public URL https://nottingham-repository.worktribe.com/output/22989411
Publisher URL https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cbic.202300250

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