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 devices to function reversibly, that is, to deliver a substantial current at a minimal overpotential. Redox-active films can effectively embed and stabilize 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, which consists of [FeFe] hydrogenase embedded in a low-potential, 2,2′-viologen-modified hydrogel. When this catalytic film served as the anode material in a H2/O2 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 H2 evolution. We explained the catalytic properties using a kinetic model, which shows that reversibility can be achieved even though intermolecular electron transfer is slower than catalysis. This understanding of reversibility simplifies the design principles of highly efficient and stable bioelectrocatalytic films, advancing their implementation in energy conversion. [Figure not available: see fulltext.].
Item Type: | Article |
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Divisions: | 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: | 23 Nov 2022 11:48 |
URI: | http://repository.essex.ac.uk/id/eprint/34058 |
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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