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First mixed-metal fluoride pyrochlores obtained by topotactic oxidation of ammonium fluorides under F2 gas

hal.structure.identifierInstitut des Molécules et Matériaux du Mans [IMMM]
dc.contributor.authorLEMOINE, Kévin
hal.structure.identifierInstitut des Molécules et Matériaux du Mans [IMMM]
dc.contributor.authorMOURY, Romain
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
dc.contributor.authorDURAND, Etienne
hal.structure.identifierDepartamento de Quimica Inorganica y Bioinorganica [Madrid]
dc.contributor.authorARROYO-DE DOMPABLO, Elena
hal.structure.identifierDepartamento de Quimica Inorganica y Bioinorganica [Madrid]
dc.contributor.authorMORÁN, Emilio
hal.structure.identifierInstitut des Molécules et Matériaux du Mans [IMMM]
dc.contributor.authorLEBLANC, Marc
hal.structure.identifierInstitut des Molécules et Matériaux du Mans [IMMM]
dc.contributor.authorHÉMON-RIBAUD, Annie
hal.structure.identifierInstitut des Molécules et Matériaux du Mans [IMMM]
dc.contributor.authorGRENECHE, Jean-Marc
hal.structure.identifierInstitut des Molécules et Matériaux du Mans [IMMM]
dc.contributor.authorGALVEN, Cyrille
hal.structure.identifierInstitut des Molécules et Matériaux du Mans [IMMM]
dc.contributor.authorGUNES, Veyis
hal.structure.identifierInstitut des Molécules et Matériaux du Mans [IMMM]
dc.contributor.authorLHOSTE, Jérôme
hal.structure.identifierInstitut des Molécules et Matériaux du Mans [IMMM]
dc.contributor.authorMAISONNEUVE, Vincent
dc.date.issued2021-02-03
dc.identifier.issn1528-7483
dc.description.abstractEnMetal fluorides with 3D open structures, pyrochlore (pyr) or hexagonal tungsten bronze (HTB), are promising materials as positive electrodes for rechargeable batteries or catalysts. Herein, we have developed a two-step synthesis procedure to obtain new anhydrous mixed-metal-cation fluorides crystallizing in the pyrochlore structure. The first step consists of preparing mixed-metal ammonium fluorides (NH4)M2+Fe3+F6 (M = Mn, Fe, Co Ni) using different synthesis strategies. For M = Mn, three allotropic varieties of (NH4)Mn2+Fe3+F6 are obtained; two phases adopt the expected pyrochlore network with either the cubic Fm3̅m or the orthorhombic Pnma space group, and the third phase exhibits a 3D network with narrow pseudotriangular cavities. 57Fe Mössbauer spectrometry indicates that the crystal structures are governed by the Fe3+/Mn2+ cationic order or disorder. The second step is a topotactic oxidation of pyr-(NH4)M2+Fe3+F6 under a molecular F2 flow. To better understand the reaction mechanism, the topotactic oxidation was followed by thermogravimetry, XRD, FTIR, and Mössbauer spectrometry. The successful synthesis of the first anhydrous pyr-M3+0.5Fe0.5F3 provides a new route to prepare anhydrous mixed-metal fluorides pyrochlore with empty cavities of the open framework.
dc.language.isoen
dc.publisherAmerican Chemical Society
dc.subject.enChemical structure
dc.subject.enAnions
dc.subject.enOxidation
dc.subject.enTransition metals
dc.subject.enCations
dc.title.enFirst mixed-metal fluoride pyrochlores obtained by topotactic oxidation of ammonium fluorides under F2 gas
dc.typeArticle de revue
dc.identifier.doi10.1021/acs.cgd.0c01279
dc.subject.halChimie/Matériaux
bordeaux.journalCrystal Growth & Design
bordeaux.page935-945
bordeaux.volume21
bordeaux.issue2
bordeaux.peerReviewedoui
hal.identifierhal-03167049
hal.version1
hal.popularnon
hal.audienceInternationale
hal.origin.linkhttps://hal.archives-ouvertes.fr//hal-03167049v1
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