Electrografted Interfaces on Metal Oxide Electrodes for Enzyme Immobilization and Bioelectrocatalysis

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dc.contributor.authorHarris, Tomos G. A. A.
dc.contributor.authorHeidary, Nina
dc.contributor.authorFrielingsdorf, Stefan
dc.contributor.authorRauwerdink, Sander
dc.contributor.authorTahraoui, Abbes
dc.contributor.authorLenz, Oliver
dc.contributor.authorZebger, Ingo
dc.contributor.authorFischer, Anna
dc.date.accessioned2021-06-24T14:44:45Z
dc.date.available2021-06-24T14:44:45Z
dc.date.issued2021-03-11
dc.date.updated2021-06-01T14:53:01Z
dc.description.abstractIn 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.en
dc.description.sponsorshipDFG, 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 Produkteen
dc.description.sponsorshipDFG, 390540038, EXC 2008: Unifying Systems in Catalysis "UniSysCat"en
dc.identifier.eissn2196-0216
dc.identifier.urihttps://depositonce.tu-berlin.de/handle/11303/13284
dc.identifier.urihttp://dx.doi.org/10.14279/depositonce-12076
dc.language.isoenen
dc.rights.urihttps://creativecommons.org/licenses/by-nc-nd/4.0/en
dc.subject.ddc540 Chemie und zugeordnete Wissenschaftende
dc.subject.othertransparent conducting oxidesen
dc.subject.otherelectrograftingen
dc.subject.other[NiFe] hydrogenaseen
dc.subject.otherATR-IR spectroscopyen
dc.subject.otherbioelectrocatalysisen
dc.titleElectrografted Interfaces on Metal Oxide Electrodes for Enzyme Immobilization and Bioelectrocatalysisen
dc.typeArticleen
dc.type.versionpublishedVersionen
dcterms.bibliographicCitation.doi10.1002/celc.202100020en
dcterms.bibliographicCitation.issue7en
dcterms.bibliographicCitation.journaltitleChemElectroChemen
dcterms.bibliographicCitation.originalpublishernameWileyen
dcterms.bibliographicCitation.originalpublisherplaceNew York, NYen
dcterms.bibliographicCitation.pageend1336en
dcterms.bibliographicCitation.pagestart1329en
dcterms.bibliographicCitation.volume8en
tub.accessrights.dnbfreeen
tub.affiliationVerbundforschung::Exzellenzcluster (EXC)::EXC - UniCatde
tub.affiliation.facultyVerbundforschungde
tub.affiliation.groupEXC - UniCatde
tub.affiliation.instituteExzellenzcluster (EXC)de
tub.publisher.universityorinstitutionTechnische Universität Berlinen

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