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Revealing defects in crystalline lithium-ion battery electrodes by solid state NMR: applications to LiVPO4F

hal.structure.identifierConditions Extrêmes et Matériaux : Haute Température et Irradiation [CEMHTI]
hal.structure.identifierRéseau sur le stockage électrochimique de l'énergie [RS2E]
dc.contributor.authorMESSINGER, Robert J.
hal.structure.identifierRéseau sur le stockage électrochimique de l'énergie [RS2E]
hal.structure.identifierAdvanced Lithium Energy Storage Systems - ALISTORE-ERI [ALISTORE-ERI]
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
dc.contributor.authorMÉNÉTRIER, Michel
hal.structure.identifierRéseau sur le stockage électrochimique de l'énergie [RS2E]
hal.structure.identifierConditions Extrêmes et Matériaux : Haute Température et Irradiation [CEMHTI]
dc.contributor.authorSALAGER, Elodie
hal.structure.identifierLaboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux [LITEN]
dc.contributor.authorBOULINEAU, Adrien
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
dc.contributor.authorDUTTINE, Mathieu
hal.structure.identifierRéseau sur le stockage électrochimique de l'énergie [RS2E]
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
dc.contributor.authorCARLIER, Dany
hal.structure.identifierAdvanced Lithium Energy Storage Systems - ALISTORE-ERI [ALISTORE-ERI]
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
hal.structure.identifierLaboratoire réactivité et chimie des solides - UMR CNRS 7314 UPJV [LRCS]
dc.contributor.authorATEBA MBA, Jean-Marcel
hal.structure.identifierRéseau sur le stockage électrochimique de l'énergie [RS2E]
hal.structure.identifierAdvanced Lithium Energy Storage Systems - ALISTORE-ERI [ALISTORE-ERI]
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
dc.contributor.authorCROGUENNEC, Laurence
hal.structure.identifierRéseau sur le stockage électrochimique de l'énergie [RS2E]
hal.structure.identifierAdvanced Lithium Energy Storage Systems - ALISTORE-ERI [ALISTORE-ERI]
hal.structure.identifierLaboratoire réactivité et chimie des solides - UMR CNRS 7314 UPJV [LRCS]
dc.contributor.authorMASQUELIER, Christian
hal.structure.identifierConditions Extrêmes et Matériaux : Haute Température et Irradiation [CEMHTI]
dc.contributor.authorMASSIOT, Dominique
hal.structure.identifierConditions Extrêmes et Matériaux : Haute Température et Irradiation [CEMHTI]
hal.structure.identifierRéseau sur le stockage électrochimique de l'énergie [RS2E]
dc.contributor.authorDESCHAMPS, Michaël
dc.date.issued2015
dc.identifier.issn0897-4756
dc.description.abstractEnIdentifying and characterizing defects in crystalline solids is a challenging problem, particularly for lithium-ion intercalation materials, which often exhibit multiple stable oxidation and spin states as well as local ordering of lithium and charges. Here, we reveal the existence of characteristic lithium defect environments in the crystalline lithium-ion battery electrode LiVPO4F and establish the relative subnanometer-scale proximities between them. Well-crystallized LiVPO4F samples were synthesized with the expected tavorite-like structure, as established by X-ray diffraction (XRD) and scanning transmission electron microscopy (STEM) measurements. Solid-state 7Li nuclear magnetic resonance (NMR) spectra reveal unexpected paramagnetic 7Li environments that can account for up to 20% of the total lithium content. Multidimensional and site-selective solid-state 7Li NMR experiments using finite-pulse radio frequency-driven recoupling (fp-RFDR) establish unambiguously that the unexpected lithium environments are associated with defects within the LiVPO4F crystal structure, revealing the existence of dipole–dipole-coupled defect pairs. The lithium defects exhibit local electronic environments that are distinct from lithium ions in the crystallographic LiVPO4F site, which result from altered oxidation and/or spin states of nearby paramagnetic vanadium atoms. The results provide a general strategy for identifying and characterizing lithium defect environments in crystalline solids, including paramagnetic materials with short 7Li NMR relaxation times on the order of milliseconds.
dc.language.isoen
dc.publisherAmerican Chemical Society
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/
dc.title.enRevealing defects in crystalline lithium-ion battery electrodes by solid state NMR: applications to LiVPO4F
dc.typeArticle de revue
dc.identifier.doi10.1021/acs.chemmater.5b01234
dc.subject.halChimie/Matériaux
bordeaux.journalChemistry of Materials
bordeaux.page5212-5221
bordeaux.volume27
bordeaux.issue15
bordeaux.peerReviewedoui
hal.identifierhal-01200997
hal.version1
hal.popularnon
hal.audienceInternationale
hal.origin.linkhttps://hal.archives-ouvertes.fr//hal-01200997v1
bordeaux.COinSctx_ver=Z39.88-2004&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.jtitle=Chemistry%20of%20Materials&rft.date=2015&rft.volume=27&rft.issue=15&rft.spage=5212-5221&rft.epage=5212-5221&rft.eissn=0897-4756&rft.issn=0897-4756&rft.au=MESSINGER,%20Robert%20J.&M%C3%89N%C3%89TRIER,%20Michel&SALAGER,%20Elodie&BOULINEAU,%20Adrien&DUTTINE,%20Mathieu&rft.genre=article


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