A Redox Hydrogel Protects the O2-Sensitive [FeFe]-Hydrogenase from Chlamydomonas reinhardtii from Oxidative Damage

Alaa Alsheikh Oughli; Felipe Conzuelo; Martin Winkler; Thomas Happe; Wolfgang Lubitz; Wolfgang Schuhmann; Olaf Rüdiger; Nicolas Plumeré

doi:10.1002/anie.201502776

A Redox Hydrogel Protects the O₂-Sensitive [FeFe]-Hydrogenase from Chlamydomonas reinhardtii from Oxidative Damage

Alaa Alsheikh Oughli, Felipe Conzuelo, Martin Winkler, Thomas Happe, Wolfgang Lubitz, Wolfgang Schuhmann, Olaf Rüdiger, Nicolas Plumeré

Research output: Contribution to journal › Article › peer-review

88 Scopus citations

Abstract

The integration of sensitive catalysts in redox matrices opens up the possibility for their protection from deactivating molecules such as O₂. [FeFe]-hydrogenases are enzymes catalyzing H₂ oxidation/production which are irreversibly deactivated by O₂. Therefore, their use under aerobic conditions has never been achieved. Integration of such hydrogenases in viologen-modified hydrogel films allows the enzyme to maintain catalytic current for H₂ oxidation in the presence of O₂, demonstrating a protection mechanism independent of reactivation processes. Within the hydrogel, electrons from the hydrogenase-catalyzed H₂ oxidation are shuttled to the hydrogel-solution interface for O₂ reduction. Hence, the harmful O₂ molecules do not reach the hydrogenase. We illustrate the potential applications of this protection concept with a biofuel cell under H₂/O₂ mixed feed.

Original language	English
Pages (from-to)	12329-12333
Number of pages	5
Journal	Angewandte Chemie International Edition in English
Volume	54
Issue number	42
DOIs	https://doi.org/10.1002/anie.201502776
State	Published - 1 Oct 2015
Externally published	Yes

Keywords

O protection
biocatalysis
biofuel cells
hydrogenases
viologen hydrogel

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title = "A Redox Hydrogel Protects the O2-Sensitive [FeFe]-Hydrogenase from Chlamydomonas reinhardtii from Oxidative Damage",

abstract = "The integration of sensitive catalysts in redox matrices opens up the possibility for their protection from deactivating molecules such as O2. [FeFe]-hydrogenases are enzymes catalyzing H2 oxidation/production which are irreversibly deactivated by O2. Therefore, their use under aerobic conditions has never been achieved. Integration of such hydrogenases in viologen-modified hydrogel films allows the enzyme to maintain catalytic current for H2 oxidation in the presence of O2, demonstrating a protection mechanism independent of reactivation processes. Within the hydrogel, electrons from the hydrogenase-catalyzed H2 oxidation are shuttled to the hydrogel-solution interface for O2 reduction. Hence, the harmful O2 molecules do not reach the hydrogenase. We illustrate the potential applications of this protection concept with a biofuel cell under H2/O2 mixed feed.",

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AU - Oughli, Alaa Alsheikh

AU - Conzuelo, Felipe

AU - Winkler, Martin

AU - Happe, Thomas

AU - Lubitz, Wolfgang

AU - Schuhmann, Wolfgang

AU - Rüdiger, Olaf

AU - Plumeré, Nicolas

PY - 2015/10/1

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N2 - The integration of sensitive catalysts in redox matrices opens up the possibility for their protection from deactivating molecules such as O2. [FeFe]-hydrogenases are enzymes catalyzing H2 oxidation/production which are irreversibly deactivated by O2. Therefore, their use under aerobic conditions has never been achieved. Integration of such hydrogenases in viologen-modified hydrogel films allows the enzyme to maintain catalytic current for H2 oxidation in the presence of O2, demonstrating a protection mechanism independent of reactivation processes. Within the hydrogel, electrons from the hydrogenase-catalyzed H2 oxidation are shuttled to the hydrogel-solution interface for O2 reduction. Hence, the harmful O2 molecules do not reach the hydrogenase. We illustrate the potential applications of this protection concept with a biofuel cell under H2/O2 mixed feed.

AB - The integration of sensitive catalysts in redox matrices opens up the possibility for their protection from deactivating molecules such as O2. [FeFe]-hydrogenases are enzymes catalyzing H2 oxidation/production which are irreversibly deactivated by O2. Therefore, their use under aerobic conditions has never been achieved. Integration of such hydrogenases in viologen-modified hydrogel films allows the enzyme to maintain catalytic current for H2 oxidation in the presence of O2, demonstrating a protection mechanism independent of reactivation processes. Within the hydrogel, electrons from the hydrogenase-catalyzed H2 oxidation are shuttled to the hydrogel-solution interface for O2 reduction. Hence, the harmful O2 molecules do not reach the hydrogenase. We illustrate the potential applications of this protection concept with a biofuel cell under H2/O2 mixed feed.

KW - O protection

KW - biocatalysis

KW - biofuel cells

KW - hydrogenases

KW - viologen hydrogel

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A Redox Hydrogel Protects the O₂-Sensitive [FeFe]-Hydrogenase from Chlamydomonas reinhardtii from Oxidative Damage

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Keywords

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