Journal
CHEMCATCHEM
Volume 10, Issue 18, Pages 4067-4073Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201800681
Keywords
[Cp*Rh(bpy)Cl](+) mediator; dehydrogenase; NADH; co-immobilization; bioelectrocatalytic reactor
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Funding
- French PIA project Lorraine Universite d'Excellence [ANR-15-IDEX-04-LUE]
- CNRS
- Region Grand Est
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A bioelectrode for electroenzymatic synthesis was prepared, combining a layer for NADH regeneration and a renewable layer for enzymatic substrate reduction. The covalent immobilization of a rhodium complex mediator ([Cp*Rh(bpy)Cl](+)) on the surface of a bucky paper electrode was achieved by following an original protocol in two steps. A bipyridine ligand was first grafted on the electrode by electro-reduction of bipyridyl diazonium cations generated from 4-amino-2,2-bipyridine, and the complex was then formed by reaction with [RhCp*Cl-2](2). A turnover frequency of 1.3s(-1) was estimated for the electrocatalytic regeneration of NADH by this immobilized complex, with a Faraday efficiency of 83%. The bucky paper electrode was then overcoated by a bio-doped porous layer made of glassy fibers with immobilized D-sorbitol dehydrogenase. This assembly allowed for the efficient separation of the enzyme and the rhodium catalyst, which is a prerequisite for effective bioelectrocatalysis with such bioelectrochemical system, while allowing effective mass transport of NAD(+)/NADH cofactor from one layer to the other. Thereby, it was possible to reuse the same mediator-functionalized bucky paper with three different enzyme layers. The bioelectrode was applied to the electroenzymatic reduction of D-fructose to D-sorbitol. A turnover frequency of 0.19s(-1) for the rhodium complex was observed in the presence of 3mM D-fructose and a total turnover number higher than 12000 was estimated.
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