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Oxygen-resistant [FeFe]hydrogenases: new biocatalysis tools for clean energy and cascade reactions

Valetti, Francesca; Morra, Simone; Barbieri, Lisa; Dezzani, Sabrina; Ratto, Alessandro; Catucci, Gianluca; Sadeghi, Sheila J.; Gilardi, Gianfranco

Authors

Francesca Valetti

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

Lisa Barbieri

Sabrina Dezzani

Alessandro Ratto

Gianluca Catucci

Sheila J. Sadeghi

Gianfranco Gilardi



Abstract

The use of enzymes to generate hydrogen, instead of using rare metal catalysts, is an exciting area of study in modern biochemistry and biotechnology, as well as biocatalysis driven by sustainable hydrogen. Thus far, the oxygen sensitivity of the fastest hydrogen-producing/exploiting enzymes, [FeFe]hydrogenases, has hindered their practical application, thereby restricting innovations mainly to their [NiFe]-based, albeit slower, counterparts. Recent exploration of the biodiversity of clostridial hydrogen-producing enzymes has yielded the isolation of representatives from a relatively understudied group. These enzymes possess an inherent defense mechanism against oxygen-induced damage. This discovery unveils fresh opportunities for applications such as electrode interfacing, biofuel cells, immobilization, and entrapment for enhanced stability in practical uses. Furthermore, it suggests potential combinations with cascade reactions for CO2 conversion or cofactor regeneration, like NADPH, facilitating product separation in biotechnological processes. This work provides an overview of this new class of biocatalysts, incorporating unpublished protein engineering strategies to further investigate the dynamic mechanism of oxygen protection and to address crucial details remaining elusive such as still unidentified switching hot-spots and their effects. Variants with improved kcat as well as chimeric versions with promising features to attain gain-of-function variants and applications in various biotechnological processes are also presented.

Citation

Valetti, F., Morra, S., Barbieri, L., Dezzani, S., Ratto, A., Catucci, G., …Gilardi, G. (2024). Oxygen-resistant [FeFe]hydrogenases: new biocatalysis tools for clean energy and cascade reactions. Faraday Discussions, https://doi.org/10.1039/d4fd00010b

Journal Article Type Article
Acceptance Date Feb 21, 2024
Online Publication Date Feb 21, 2024
Publication Date 2024
Deposit Date Apr 19, 2024
Journal Faraday Discussions
Print ISSN 1359-6640
Electronic ISSN 1364-5498
Publisher Royal Society of Chemistry
Peer Reviewed Peer Reviewed
DOI https://doi.org/10.1039/d4fd00010b
Keywords Physical and Theoretical Chemistry
Public URL https://nottingham-repository.worktribe.com/output/33838034
Publisher URL https://pubs.rsc.org/en/content/articlelanding/2024/fd/d4fd00010b