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Efficiency of Site-Specific Clicked Laccase-Carbon Nanotubes Biocathodes towards O 2 Reduction.

Authors :
Gentil S
Rousselot-Pailley P
Sancho F
Robert V
Mekmouche Y
Guallar V
Tron T
Le Goff A
Source :
Chemistry (Weinheim an der Bergstrasse, Germany) [Chemistry] 2020 Apr 09; Vol. 26 (21), pp. 4798-4804. Date of Electronic Publication: 2020 Mar 30.
Publication Year :
2020

Abstract

A maximization of a direct electron transfer (DET) between redox enzymes and electrodes can be obtained through the oriented immobilization of enzymes onto an electroactive surface. Here, a strategy for obtaining carbon nanotube (CNTs) based electrodes covalently modified with perfectly control-oriented fungal laccases is presented. Modelizations of the laccase-CNT interaction and of electron conduction pathways serve as a guide in choosing grafting positions. Homogeneous populations of alkyne-modified laccases are obtained through the reductive amination of a unique surface-accessible lysine residue selectively engineered near either one or the other of the two copper centers in enzyme variants. Immobilization of the site-specific alkynated enzymes is achieved by copper-catalyzed click reaction on azido-modified CNTs. A highly efficient reduction of O <subscript>2</subscript> at low overpotential and catalytic current densities over -3 mA cm <superscript>-2</superscript> are obtained by minimizing the distance from the electrode surface to the trinuclear cluster.<br /> (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Details

Language :
English
ISSN :
1521-3765
Volume :
26
Issue :
21
Database :
MEDLINE
Journal :
Chemistry (Weinheim an der Bergstrasse, Germany)
Publication Type :
Academic Journal
Accession number :
31999372
Full Text :
https://doi.org/10.1002/chem.201905234