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Issue 31, 2018
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Viologen-modified electrodes for protection of hydrogenases from high potential inactivation while performing H2 oxidation at low overpotential

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Abstract

In this work we present a viologen-modified electrode providing protection for hydrogenases against high potential inactivation. Hydrogenases, including O2-tolerant classes, suffer from reversible inactivation upon applying high potentials, which limits their use in biofuel cells to certain conditions. Our previously reported protection strategy based on the integration of hydrogenase into redox matrices enabled the use of these biocatalysts in biofuel cells even under anode limiting conditions. However, mediated catalysis required application of an overpotential to drive the reaction, and this translates into a power loss in a biofuel cell. In the present work, the enzyme is adsorbed on top of a covalently-attached viologen layer which leads to mixed, direct and mediated, electron transfer processes; at low overpotentials, the direct electron transfer process generates a catalytic current, while the mediated electron transfer through the viologens at higher potentials generates a redox buffer that prevents oxidative inactivation of the enzyme. Consequently, the enzyme starts the catalysis at no overpotential with viologen self-activated protection at high potentials.

Graphical abstract: Viologen-modified electrodes for protection of hydrogenases from high potential inactivation while performing H2 oxidation at low overpotential

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Publication details

The article was received on 12 Mar 2018, accepted on 25 May 2018 and first published on 25 May 2018


Article type: Paper
DOI: 10.1039/C8DT00955D
Citation: Dalton Trans., 2018,47, 10685-10691
  • Open access: Creative Commons BY license
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    Viologen-modified electrodes for protection of hydrogenases from high potential inactivation while performing H2 oxidation at low overpotential

    A. A. Oughli, M. Vélez, J. A. Birrell, W. Schuhmann, W. Lubitz, N. Plumeré and O. Rüdiger, Dalton Trans., 2018, 47, 10685
    DOI: 10.1039/C8DT00955D

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