Efficiency of Site‐Specific Clicked Laccase–Carbon Nanotubes Biocathodes towards O2 Reduction

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 O2 at low overpotential and catalytic current densities over −3 mA cm−2 are obtained by minimizing the distance from the electrode surface to the trinuclear cluster.

Références

Titre
Efficiency of Site‐Specific Clicked Laccase–Carbon Nanotubes Biocathodes towards O2 Reduction
Type de publication
Article de revue
Année de publication
2020
Revue
Chemistry – A European Journal
Volume
26
Ticket
21
Start Page
4798-4804
ISSN
0947-6539
Soumis le 10 juillet 2020