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          Institute: MPI für bioanorganische Chemie     Collection: MPI für bioanorganische Chemie     Display Documents



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ID: 712824.0, MPI für bioanorganische Chemie / MPI für bioanorganische Chemie
Mechanism of Protection of Catalysts Supported in Redox Hydrogel Films
Authors:Fourmond, Vincent; Stapf, Stefanie; Li, Huaiguang; Buesen, Darren; Birrell, James A.; Rüdiger, Olaf; Lubitz, Wolfgang; Schuhmann, Wolfgang; Plumere, Nicolas; Leger, Christophe
Language:English
Date of Publication (YYYY-MM-DD):2015
Title of Journal:Journal of the American Chemical Society
Journal Abbrev.:J.Am.Chem.Soc.
Volume:137
Issue / Number:16
Start Page:5494
End Page:5505
Review Status:Internal review
Audience:Experts Only
Abstract / Description:The use of synthetic inorganic complexes as supported catalysts is a key route in energy production and in industrial synthesis. However, their intrinsic oxygen sensitivity is sometimes an issue. Some of us have recently demonstrated that hydrogenases, the fragile but very efficient biological catalysts of H2 oxidation, can be protected from O-2 damage upon integration into a film of a specifically designed redox polymer. Catalytic oxidation of H-2 produces electrons which reduce oxygen near the film/solution interface, thus providing a self-activated protection from oxygen [Plumere et al., Nat Chem. 2014, 6, 822-827]. Here, we rationalize this protection mechanism by examining the time-dependent distribution of species in the hydrogenase/polymer film, using measured or estimated values of all relevant parameters and the numerical and analytical solutions of a realistic reaction-diffusion scheme. Our investigation sets the stage for optimizing the design of hydrogenase-polymer films, and for expanding this strategy to other fragile catalysts.
Comment of the Author/Creator:Date: 2015, APR 29 2015
External Publication Status:published
Document Type:Article
Communicated by:N. N.
Affiliations:MPI für bioanorganische Chemie
External Affiliations:[Fourmond,V.; Leger,C.] Aix Marseille Univ., Lab Bioenerget & Ingn Prot, CNRS, BIP UMR 7281, F-13402 Marseille, France.
[Stapf,S.; Li,H.; Buesen,D.; Plumere,N.] Ruhr Univ.Bochum, Ctr Electrochem Sci Mol Nanostruct, D-44780 Bochum, Germany.
[Schuhmann,W. ] Ruhr Univ.Bochum, CES, Analyt Chem, Elektroanalyt & Sensor, D-44780 Bochum, Germany.
Identifiers:ISI:000353931500042 [ID No:1]
ISSN:0002-7863 [ID No:2]
DOI:10.1021/jacs.5b01194 [ID No:3]
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