Activation of anionic redox in d0 transition ...
Type de document :
Article dans une revue scientifique
URL permanente :
Titre :
Activation of anionic redox in d0 transition metal chalcogenides by anion doping
Auteur(s) :
Leube, Bernhard T. [Auteur]
Robert, Clara [Auteur]
Foix, Dominique [Auteur]
Porcheron, Benjamin [Auteur]
Dedryvère, Remi [Auteur]
Rousse, Gwenaëlle [Auteur]
Salager, Elodie [Auteur]
Cabelguen, Pierre-Etienne [Auteur]
Abakumov, Artem M. [Auteur]
Vezin, Herve [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Doublet, Marie-Liesse [Auteur]
Tarascon, Jean-Marie [Auteur]
Robert, Clara [Auteur]
Foix, Dominique [Auteur]
Porcheron, Benjamin [Auteur]
Dedryvère, Remi [Auteur]
Rousse, Gwenaëlle [Auteur]
Salager, Elodie [Auteur]
Cabelguen, Pierre-Etienne [Auteur]
Abakumov, Artem M. [Auteur]
Vezin, Herve [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Doublet, Marie-Liesse [Auteur]
Tarascon, Jean-Marie [Auteur]
Titre de la revue :
Nature Communications
Nom court de la revue :
Nat Commun
Numéro :
12
Pagination :
5485
Éditeur :
Springer Nature
Date de publication :
2021-09-16
ISSN :
2041-1723
Discipline(s) HAL :
Chimie/Matériaux
Chimie/Polymères
Chimie/Chimie théorique et/ou physique
Chimie/Chimie analytique
Chimie/Polymères
Chimie/Chimie théorique et/ou physique
Chimie/Chimie analytique
Résumé en anglais : [en]
Expanding the chemical space for designing novel anionic redox materials from oxides to sulfides has enabled to better apprehend fundamental aspects dealing with cationic-anionic relative band positioning. Pursuing with ...
Lire la suite >Expanding the chemical space for designing novel anionic redox materials from oxides to sulfides has enabled to better apprehend fundamental aspects dealing with cationic-anionic relative band positioning. Pursuing with chalcogenides, but deviating from cationic substitution, we here present another twist to our band positioning strategy that relies on mixed ligands with the synthesis of the Li2TiS3-xSex solid solution series. Through the series the electrochemical activity displays a bell shape variation that peaks at 260 mAh/g for the composition x = 0.6 with barely no capacity for the x = 0 and x = 3 end members. We show that this capacity results from cumulated anionic (Se2−/Sen−) and (S2−/Sn−) and cationic Ti3+/Ti4+ redox processes and provide evidence for a metal-ligand charge transfer by temperature-driven electron localization. Moreover, DFT calculations reveal that an anionic redox process cannot take place without the dynamic involvement of the transition metal electronic states. These insights can guide the rational synthesis of other Li-rich chalcogenides that are of interest for the development of solid-state batteries.Lire moins >
Lire la suite >Expanding the chemical space for designing novel anionic redox materials from oxides to sulfides has enabled to better apprehend fundamental aspects dealing with cationic-anionic relative band positioning. Pursuing with chalcogenides, but deviating from cationic substitution, we here present another twist to our band positioning strategy that relies on mixed ligands with the synthesis of the Li2TiS3-xSex solid solution series. Through the series the electrochemical activity displays a bell shape variation that peaks at 260 mAh/g for the composition x = 0.6 with barely no capacity for the x = 0 and x = 3 end members. We show that this capacity results from cumulated anionic (Se2−/Sen−) and (S2−/Sn−) and cationic Ti3+/Ti4+ redox processes and provide evidence for a metal-ligand charge transfer by temperature-driven electron localization. Moreover, DFT calculations reveal that an anionic redox process cannot take place without the dynamic involvement of the transition metal electronic states. These insights can guide the rational synthesis of other Li-rich chalcogenides that are of interest for the development of solid-state batteries.Lire moins >
Langue :
Anglais
Audience :
Internationale
Vulgarisation :
Non
Projet Européen :
Établissement(s) :
Université de Lille
CNRS
CNRS
Collections :
Équipe(s) de recherche :
Propriétés magnéto structurales des matériaux (PMSM)
Date de dépôt :
2021-09-16T11:51:45Z
2021-10-06T14:48:11Z
2021-10-06T14:48:11Z
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