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|
|Date of Publication (YYYY-MM-DD):||2015|
|Title of Journal:||Journal of the American Chemical Society|
|Issue / Number:||16|
|Review Status:||Internal review|
|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|
|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]
The scope and number of records on eDoc is subject
to the collection policies defined by each institute
- see "info" button in the collection browse view.