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Author Perez, A.J.; Jacquet, Q.; Batuk, D.; Iadecola, A.; Saubanere, M.; Rousse, G.; Larcher, D.; Vezin, H.; Doublet, M.-L.; Tarascon, J.-M.
Title Approaching the limits of cationic and anionic electrochemical activity with the Li-rich layered rocksalt Li3IrO4 Type A1 Journal article
Year (down) 2017 Publication Nature energy Abbreviated Journal Nat Energy
Volume 2 Issue 12 Pages 954-962
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The Li-rich rocksalt oxides Li2MO3 (M = 3d/4d/5d transition metal) are promising positive-electrode materials for Li-ion batteries, displaying capacities exceeding 300 mAh g(-1) thanks to the participation of the oxygen non-bonding O(2p) orbitals in the redox process. Understanding the oxygen redox limitations and the role of the O/M ratio is therefore crucial for the rational design of materials with improved electrochemical performances. Here we push oxygen redox to its limits with the discovery of a Li3IrO4 compound (O/M = 4) that can reversibly take up and release 3.5 electrons per Ir and possesses the highest capacity ever reported for any positive insertion electrode. By quantitatively monitoring the oxidation process, we demonstrate the material's instability against O-2 release on removal of all Li. Our results show that the O/M parameter delineates the boundary between the material's maximum capacity and its stability, hence providing valuable insights for further development of high-capacity materials.
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Publisher Place of Publication Editor
Language Wos 000430218300001 Publication Date 2017-12-06
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2058-7546 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 55 Open Access Not_Open_Access
Notes ; We thank P. Pearce for providing the beta-Li<INF>2</INF>IrO<INF>3</INF> and L. Lemarquis for helping in the DEMS experiment. We are particularly grateful to S. Belin, V. Briois and L. Stievano for helpful discussions on XAS analysis and synchrotron SOLEIL (France) for providing beamtime at the ROCK beamline (financed by the French National Research Agency (ANR) as part of the 'Investissements d'Avenir' programme, reference: ANR-10-EQPX-45). A.J.P and A. I. acknowledge the GdR C(RS) 2 for the workshop organized on a chemometric approach for XAS data analysis. V. Nassif is acknowledged for her help during neutron diffraction experiments performed at Institut Laue Langevin on D1B. Use of the 11-BM mail service of the APS at Argonne National Laboratory was supported by the US Department of Energy under contract No. DE-AC02-06CH11357 and is gratefully acknowledged. This work has been performed with the support of the European Research Council (ERC) (FP/2014)/ERC Grant- Project 670116 ARPEMA. ; Approved Most recent IF: NA
Call Number UA @ lucian @ c:irua:150926 Serial 4962
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