title: Visualization of O-O peroxo-like dimers in high-capacity layered oxides for Li-ion batteries.
abstract: Lithium-ion (Li-ion) batteries that rely on cationic redox reactions are the primary energy source for portable electronics. One pathway toward greater energy density is through the use of Li-rich layered oxides. The capacity of this class of materials (>270 milliampere hours per gram) has been shown to be nested in anionic redox reactions, which are thought to form peroxo-like species. However, the oxygen-oxygen (O-O) bonding pattern has not been observed in previous studies, nor has there been a satisfactory explanation for the irreversible changes that occur during first delithiation. By using Li2IrO3 as a model compound, we visualize the O-O dimers via transmission electron microscopy and neutron diffraction. Our findings establish the fundamental relation between the anionic redox process and the evolution of the O-O bonding in layered oxides.
authors.affiliation: Collège de France, Chimie du Solide et de l'Energie, FRE 3677, 11 Place Marcelin Berthelot, 75231 Paris Cedex 05, France. ALISTORE-European Research Institute, FR CNRS 3104, 80039 Amiens, France. Réseau sur le Stockage Electrochimique de l'Energie (RS2E), FR CNRS 3459, France. National Institute of Chemistry, Hajdrihova 19, SI-1000 Ljubljana, Slovenia.
authors.forename: Eric
authors.initials: E
authors.lastname: McCalla
authors.affiliation: Electron Microscopy for Materials Science (EMAT), University of Antwerp, Groenenborgerlaan 171, B-2020, Antwerp, Belgium. Center for Electrochemical Energy Storage, Skolkovo Institute of Science and Technology, 3 Nobel Street, 143026 Moscow, Russia.
authors.forename: Artem M
authors.initials: AM
authors.lastname: Abakumov
authors.affiliation: ALISTORE-European Research Institute, FR CNRS 3104, 80039 Amiens, France. Réseau sur le Stockage Electrochimique de l'Energie (RS2E), FR CNRS 3459, France. Institut Charles Gerhardt, CNRS UMR 5253, Université Montpellier, Place Eugène Bataillon, 34 095 Montpellier, France.
authors.forename: Matthieu
authors.initials: M
authors.lastname: Saubanère
authors.affiliation: ALISTORE-European Research Institute, FR CNRS 3104, 80039 Amiens, France. Réseau sur le Stockage Electrochimique de l'Energie (RS2E), FR CNRS 3459, France. IPREM/ECP (UMR 5254), University of Pau, 2 Avenue Pierre Angot, 64053 Pau Cedex 9, France.
authors.forename: Dominique
authors.initials: D
authors.lastname: Foix
authors.affiliation: Electrochemistry Laboratory, Paul Scherrer Institut, CH-5232 Villigen PSI, Switzerland.
authors.forename: Erik J
authors.initials: EJ
authors.lastname: Berg
authors.affiliation: Collège de France, Chimie du Solide et de l'Energie, FRE 3677, 11 Place Marcelin Berthelot, 75231 Paris Cedex 05, France. Réseau sur le Stockage Electrochimique de l'Energie (RS2E), FR CNRS 3459, France. Sorbonne Universités-UPMC Univ Paris 06, 4 Place Jussieu, F-75005 Paris, France.
authors.forename: Gwenaelle
authors.initials: G
authors.lastname: Rousse
authors.affiliation: ALISTORE-European Research Institute, FR CNRS 3104, 80039 Amiens, France. Réseau sur le Stockage Electrochimique de l'Energie (RS2E), FR CNRS 3459, France. Institut Charles Gerhardt, CNRS UMR 5253, Université Montpellier, Place Eugène Bataillon, 34 095 Montpellier, France.
authors.forename: Marie-Liesse
authors.initials: ML
authors.lastname: Doublet
authors.affiliation: ALISTORE-European Research Institute, FR CNRS 3104, 80039 Amiens, France. Réseau sur le Stockage Electrochimique de l'Energie (RS2E), FR CNRS 3459, France. IPREM/ECP (UMR 5254), University of Pau, 2 Avenue Pierre Angot, 64053 Pau Cedex 9, France.
authors.forename: Danielle
authors.initials: D
authors.lastname: Gonbeau
authors.affiliation: Electrochemistry Laboratory, Paul Scherrer Institut, CH-5232 Villigen PSI, Switzerland.
authors.forename: Petr
authors.initials: P
authors.lastname: Novák
authors.affiliation: Electron Microscopy for Materials Science (EMAT), University of Antwerp, Groenenborgerlaan 171, B-2020, Antwerp, Belgium.
authors.forename: Gustaaf
authors.initials: G
authors.lastname: Van Tendeloo
authors.affiliation: National Institute of Chemistry, Hajdrihova 19, SI-1000 Ljubljana, Slovenia.
authors.forename: Robert
authors.initials: R
authors.lastname: Dominko
authors.affiliation: Collège de France, Chimie du Solide et de l'Energie, FRE 3677, 11 Place Marcelin Berthelot, 75231 Paris Cedex 05, France. ALISTORE-European Research Institute, FR CNRS 3104, 80039 Amiens, France. Réseau sur le Stockage Electrochimique de l'Energie (RS2E), FR CNRS 3459, France. Sorbonne Universités-UPMC Univ Paris 06, 4 Place Jussieu, F-75005 Paris, France. jean-marie.tarascon@college-de-france.fr.
authors.forename: Jean-Marie
authors.initials: JM
authors.lastname: Tarascon