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Fluoride-assisted detection of glutathione by surface Ce3+/Ce4+ engineered nanoceria

hal.structure.identifierGlobal Innovative Center for Advanced Nanomaterials [GICAN]
dc.contributor.authorPATEL, Vaishwik
hal.structure.identifierGlobal Innovative Center for Advanced Nanomaterials [GICAN]
dc.contributor.authorJOSE, Linta
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
dc.contributor.authorPHILIPPOT, Gilles
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
dc.contributor.authorAYMONIER, Cyril
hal.structure.identifierL.N. Gumilyov Eurasian National University
hal.structure.identifierNational University of Science and Technology [MISIS]
dc.contributor.authorINERBAEV, Talgat
hal.structure.identifierSchool of Engineering
dc.contributor.authorMCCOURT, Luke
hal.structure.identifierSchool of Engineering
dc.contributor.authorRUPPERT, Michael
hal.structure.identifierCentre for Materials Science
dc.contributor.authorQI, Dongchen
hal.structure.identifierCentre for Materials Science
dc.contributor.authorLI, Wei
hal.structure.identifierSchool of Physics [Sydney]
dc.contributor.authorQU, Jiangtao
hal.structure.identifierSchool of Physics [Sydney]
dc.contributor.authorZHENG, Rongkun
hal.structure.identifierSchool of Physics [Sydney]
dc.contributor.authorCAIRNEY, Julie
hal.structure.identifierGlobal Innovative Center for Advanced Nanomaterials [GICAN]
dc.contributor.authorYI, Jiabao
hal.structure.identifierGlobal Innovative Center for Advanced Nanomaterials [GICAN]
dc.contributor.authorVINU, Ajayan
hal.structure.identifierGlobal Innovative Center for Advanced Nanomaterials [GICAN]
dc.contributor.authorKARAKOTI, Ajay
dc.date.issued2022
dc.identifier.issn2050-750X
dc.description.abstractEnNanoceria has evolved as a promising nanomaterial due to its unique enzyme-like properties, including excellent oxidase mimetic activity, which significantly increases in the presence of fluoride ions. However, this significant increase in oxidase activity has never been utilised as a signal enhancer for the detection of biological analytes partly because of the lack of understanding of the mechanism involved in this process. In this study, we show that the surface oxidation state of cerium ions plays a very crucial role in different enzymatic activities, especially the oxidase mimetic activity by engineering nanoceria with three different surface Ce 4+ /Ce 3+ compositions. Using DFT calculations combined with Bader charge analysis, it is demonstrated that stoichiometric ceria registers a higher oxidase mimetic activity than oxygen-deficient ceria with a low Ce 4+ /Ce 3+ ratio due to a higher charge transfer from a substrate, 3,3 0 ,5,5 0 tetramethylbenzidine (TMB), to the ceria surface. We also show that the fluoride ions can significantly increase the charge transfer from the TMB surface to ceria irrespective of the surface Ce 4+ /Ce 3+ ratio. Using this knowledge, we first compare the fluoride sensing properties of nanoceria with high Ce 4+ and mixed Ce 4+ /Ce 3+ oxidation states and further demonstrate that the linear detection range of fluoride ions can be extended to 1-10 ppm for nanoceria with mixed oxidation states. Then, we also demonstrate an assay for fluoride assisted detection of glutathione, an antioxidant with elevated levels during cancer, using nanoceria with a high surface Ce 4+ /Ce 3+ ratio. The addition of fluoride ions in this assay allows the detection of glutathione in the linear range of 2.5-50 ppm with a limit of detection (LOD) of 3.8 ppm. These studies not only underpin the role of the surface Ce 4+ /Ce 3+ ratio in tuning the fluoride assisted boost in the oxidase mimetic activity of nanoceria but also its strategic application in designing better colourimetric assays.
dc.language.isoen
dc.publisherRoyal Society of Chemistry
dc.title.enFluoride-assisted detection of glutathione by surface Ce3+/Ce4+ engineered nanoceria
dc.typeArticle de revue
dc.identifier.doi10.1039/D2TB01135B
dc.subject.halChimie/Matériaux
dc.subject.halChimie/Chimie analytique
bordeaux.journalJournal of materials chemistry‎ B
bordeaux.page9855-9868
bordeaux.volume10
bordeaux.issue47
bordeaux.peerReviewedoui
hal.identifierhal-03907011
hal.version1
hal.popularnon
hal.audienceInternationale
hal.origin.linkhttps://hal.archives-ouvertes.fr//hal-03907011v1
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