Hardt, Steffen and Stapf, Stefanie and Filmon, Dawit T and Birrell, James A and Rüdiger, Olaf and Fourmond, Vincent and Léger, Christophe and Plumeré, Nicolas (2021) Reversible H₂ Oxidation and Evolution by Hydrogenase Embedded in a Redox Polymer Film. Nature Catalysis, 4 (3). pp. 251-258. DOI https://doi.org/10.1038/s41929-021-00586-1
Hardt, Steffen and Stapf, Stefanie and Filmon, Dawit T and Birrell, James A and Rüdiger, Olaf and Fourmond, Vincent and Léger, Christophe and Plumeré, Nicolas (2021) Reversible H₂ Oxidation and Evolution by Hydrogenase Embedded in a Redox Polymer Film. Nature Catalysis, 4 (3). pp. 251-258. DOI https://doi.org/10.1038/s41929-021-00586-1
Hardt, Steffen and Stapf, Stefanie and Filmon, Dawit T and Birrell, James A and Rüdiger, Olaf and Fourmond, Vincent and Léger, Christophe and Plumeré, Nicolas (2021) Reversible H₂ Oxidation and Evolution by Hydrogenase Embedded in a Redox Polymer Film. Nature Catalysis, 4 (3). pp. 251-258. DOI https://doi.org/10.1038/s41929-021-00586-1
Abstract
Efficient electrocatalytic energy conversion requires the devices to function reversibly, <i>i.e.</i> deliver a significant current at minimal overpotential. Redox-active films can effectively embed and stabilise molecular electrocatalysts, but mediated electron transfer through the film typically makes the catalytic response irreversible. Here, we describe a redox-active film for bidirectional (oxidation or reduction) and reversible hydrogen conversion, consisting of [FeFe] hydrogenase embedded in a low-potential, 2,2'-viologen modified hydrogel. When this catalytic film served as the anode material in a H<sub>2</sub>/O<sub>2</sub> biofuel cell, an open circuit voltage of 1.16 V was obtained - a benchmark value near the thermodynamic limit. The same film also acted as a highly energy efficient cathode material for H<sub>2</sub> evolution. We explained the catalytic properties using a kinetic model, which shows that reversibility can be achieved despite intermolecular electron transfer being slower than catalysis. This understanding of reversibility simplifies the design principles of highly efficient and stable bioelectrocatalytic films, advancing their implementation in energy conversion.
Item Type: | Article |
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Divisions: | Faculty of Science and Health Faculty of Science and Health > Life Sciences, School of |
SWORD Depositor: | Unnamed user with email elements@essex.ac.uk |
Depositing User: | Unnamed user with email elements@essex.ac.uk |
Date Deposited: | 23 Nov 2022 11:48 |
Last Modified: | 07 Aug 2024 20:16 |
URI: | http://repository.essex.ac.uk/id/eprint/34058 |
Available files
Filename: Reversible Hsub2sub Oxidation and Evolution by Hydrogenase Embedded in a Redox Polymer Film.pdf
Licence: Creative Commons: Attribution-Noncommercial-No Derivative Works 3.0