HAL will be down for maintenance from Friday, June 10 at 4pm through Monday, June 13 at 9am. More information
Skip to Main content Skip to Navigation
Journal articles

Reversible H2 oxidation and evolution by hydrogenase embedded in a redox polymer film

Abstract : Efficient electrocatalytic energy conversion requires the devices to function reversibly, i.e. 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 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 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.
Document type :
Journal articles
Complete list of metadata

Contributor : Aurélia Bimbi Connect in order to contact the contributor
Submitted on : Monday, May 3, 2021 - 10:41:42 AM
Last modification on : Friday, April 1, 2022 - 3:46:45 AM
Long-term archiving on: : Wednesday, August 4, 2021 - 6:36:43 PM


Files produced by the author(s)




Steffen Hardt, Stefanie Stapf, Dawit Filmon, James Birrell, Olaf RÜdiger, et al.. Reversible H2 oxidation and evolution by hydrogenase embedded in a redox polymer film. Nature Catalysis, Nature Publishing Group, 2021, 4, pp.251 - 258. ⟨10.1038/s41929-021-00586-1⟩. ⟨hal-03215114⟩



Record views


Files downloads