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Hybrid Amyloid-Based Redox Hydrogel for Bioelectrocatalytic H2 Oxidation

Nicolas Duraffourg 1 Maxime Leprince 1 Serge Crouzy 2 Olivier Hamelin 1 Yves Husson 3 Luca Signor 4 Christine Cavazza 5 Vincent Forge 6 Luca Albertin 1, *
* Corresponding author
1 BioCE - Catalyse Bioinorganique et Environnement
LCBM - UMR 5249 - Laboratoire de Chimie et Biologie des Métaux
2 COMX - Chimie computationnelle, modélisation et rayons X
LCBM - UMR 5249 - Laboratoire de Chimie et Biologie des Métaux
5 BEE - BioEnergie et Environnement
LCBM - UMR 5249 - Laboratoire de Chimie et Biologie des Métaux
6 SolHyCat - Solar fuels, hydrogen and catalysis
LCBM - UMR 5249 - Laboratoire de Chimie et Biologie des Métaux
Abstract : An artificial amyloid-based redox hydrogel was designed for mediating electron transfer between a [NiFeSe] hydrogenase and an electrode. Starting from a mutated prion-forming domain of fungal protein HET-s, a hybrid redox protein containing a single benzyl methyl viologen moiety was synthesized. This protein was able to self-assemble into structurally homogenous nanofibrils. Molecular modeling confirmed that the redox groups are aligned along the fibril axis and are tethered to its core by a long, flexible polypeptide chain that allows close encounters between the fibril-bound oxidized or reduced redox groups. Redox hydrogel films capable of immobilizing the hydrogenase under mild conditions at the surface of carbon electrodes were obtained by a simple pH jump. In this way, bioelectrodes for the electrocatalytic oxidation of H2 were fabricated that afforded catalytic current densities of up to 270 μA cm−2, with an overpotential of 0.33 V, under quiescent conditions at 45 °C.
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https://hal.archives-ouvertes.fr/hal-03241503
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Submitted on : Friday, May 28, 2021 - 5:00:44 PM
Last modification on : Tuesday, September 7, 2021 - 3:56:01 PM
Long-term archiving on: : Sunday, August 29, 2021 - 7:39:27 PM

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Nicolas Duraffourg, Maxime Leprince, Serge Crouzy, Olivier Hamelin, Yves Husson, et al.. Hybrid Amyloid-Based Redox Hydrogel for Bioelectrocatalytic H2 Oxidation. Angewandte Chemie International Edition, Wiley-VCH Verlag, 2021, 60 (26), pp.14488-14497. ⟨10.1002/anie.202101700⟩. ⟨hal-03241503⟩

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