Redox-Active Glyconanoparticles as Electron Shuttles for Mediated Electron Transfer with Bilirubin Oxidase in Solution

We demonstrate self-assembly, characterization and bioelectrocatalysis of redox-active cyclodextrin-coated nanoparticles. The nanoparticles with host–guest functionality are easy to assemble and permit entrapment of hydrophobic redox molecules in aqueous solution. Bis-pyrene-ABTS encapsulated nanopa...

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Bibliographic Details
Published in:Journal of the American Chemical Society 2017-11, Vol.139 (45), p.16076-16079
Main Authors: Gross, Andrew J, Chen, Xiaohong, Giroud, Fabien, Travelet, Christophe, Borsali, Redouane, Cosnier, Serge
Format: Article
Language:English
Subjects:
Analytical chemistry
Benzothiazoles - chemistry
Biosensing Techniques
Catalysis
Chemical Sciences
Cyclodextrins - chemistry
Electrochemical Techniques
Electrodes
Electron Transport
Electrons
Hypocreales - enzymology
Models, Molecular
Nanoparticles - chemistry
Oxidation-Reduction
Oxidoreductases Acting on CH-CH Group Donors - chemistry
Pyrenes - chemistry
Sulfonic Acids - chemistry
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Summary:We demonstrate self-assembly, characterization and bioelectrocatalysis of redox-active cyclodextrin-coated nanoparticles. The nanoparticles with host–guest functionality are easy to assemble and permit entrapment of hydrophobic redox molecules in aqueous solution. Bis-pyrene-ABTS encapsulated nanoparticles were investigated electrochemically and spectroscopically. Their use as electron shuttles is demonstrated via an intraelectron transfer chain between neighboring redox units of clustered particles (D h,DLS = 195 nm) and the mono- and trinuclear Cu sites of bilirubin oxidases. Enhanced current densities for mediated O2 reduction are observed with the redox nanoparticle system compared to equivalent bioelectrode cells with dissolved mediator. Improved catalytic stability over 2 days was also observed with the redox nanoparticles, highlighting a stabilizing effect of the polymeric architecture. Bioinspired nanoparticles as mediators for bioelectrocatalysis promises to be valuable for future biofuel cells and biosensors.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.7b09442