Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 54, Issue 42, Pages 12329-12333Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201502776
Keywords
biocatalysis; biofuel cells; hydrogenases; O-2 protection; viologen hydrogel
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Funding
- Deutsche Forschungsgemeinschaft (DFG) [EXC1069, HA 255/2-1]
- Max Planck Society
- Volkswagen Foundation [LigH2t]
- BMBF [Sun2Chem]
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The integration of sensitive catalysts in redox matrices opens up the possibility for their protection from deactivating molecules such as O-2. [FeFe]-hydrogenases are enzymes catalyzing H-2 oxidation/production which are irreversibly deactivated by O-2. 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 H-2 oxidation in the presence of O-2, demonstrating a protection mechanism independent of reactivation processes. Within the hydrogel, electrons from the hydrogenase-catalyzed H-2 oxidation are shuttled to the hydrogel-solution interface for O-2 reduction. Hence, the harmful O-2 molecules do not reach the hydrogenase. We illustrate the potential applications of this protection concept with a biofuel cell under H-2/O-2 mixed feed.
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