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Main Title: Electrografted Interfaces on Metal Oxide Electrodes for Enzyme Immobilization and Bioelectrocatalysis
Author(s): Harris, Tomos G. A. A.
Heidary, Nina
Frielingsdorf, Stefan
Rauwerdink, Sander
Tahraoui, Abbes
Lenz, Oliver
Zebger, Ingo
Fischer, Anna
Type: Article
Abstract: In this work, we demonstrate that diazonium electrografting of biocompatible interfaces on transparent conducting oxide indium tin oxide (ITO) can be controlled and optimized to achieve low charge transfer resistance, allowing highly efficient electron transfer to an immobilized model enzyme, the oxygen‐tolerant [NiFe]‐hydrogenase from Ralstonia eutropha. The use of a radical scavenger enables control of the interface thickness, and thus facilitates maximization of direct electron transfer processes between the enzyme's active center and the electrode. Using this approach, amine and carboxylic acid functionalities were grafted on ITO, allowing enzyme immobilization both under moderate electrostatic control and covalently via amide bond formation. Despite an initial decrease in catalytic activity, covalent immobilization led to an improvement in current stability compared to just electrostatically immobilized enzyme. Given the superior stability of electrografted interfaces in comparison to adsorbed or self‐assembled interfaces, we propose electrografting as an alternative approach for the functional immobilization of redox‐active enzymes on transparent conducting oxide (TCO) electrodes in bioelectronic devices.
Subject(s): transparent conducting oxides
[NiFe] hydrogenase
ATR-IR spectroscopy
Issue Date: 11-Mar-2021
Date Available: 24-Jun-2021
Language Code: en
DDC Class: 540 Chemie und zugeordnete Wissenschaften
Sponsor/Funder: DFG, 5451160, Untersuchungen der Eignung von Verbindungen mit binären Untereinheiten aus Elementen der Gruppen 14/16 und 15/16 zum Aufbau ternärer oder quaternärer Anionen durch Reaktionen mit Übergangsmetallverbindungen; experimentelle und theoretische Studien zu physikalischen Eigenschaften der Produkte
DFG, 390540038, EXC 2008: Unifying Systems in Catalysis "UniSysCat"
Journal Title: ChemElectroChem
Publisher: Wiley
Volume: 8
Issue: 7
Publisher DOI: 10.1002/celc.202100020
Page Start: 1329
Page End: 1336
EISSN: 2196-0216
TU Affiliation(s): Verbundforschung » Exzellenzcluster (EXC) » EXC - UniCat
Appears in Collections:Technische Universität Berlin » Publications

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