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Approaching the limits of cationic and anionic electrochemical activity with the Li-rich layered rocksalt Li3IrO4

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  • Arnaud J. Perez

    (Collège de France, Chimie du Solide et Energie, UMR 8260, 11 place Marcelin Berthelot
    Sorbonne Universités - UPMC Univ. Paris 06, 4 Place Jussieu
    Réseau sur le Stockage Electrochimique de l’Energie (RS2E), FR CNRS 3459)

  • Quentin Jacquet

    (Collège de France, Chimie du Solide et Energie, UMR 8260, 11 place Marcelin Berthelot
    Sorbonne Universités - UPMC Univ. Paris 06, 4 Place Jussieu
    Réseau sur le Stockage Electrochimique de l’Energie (RS2E), FR CNRS 3459)

  • Dmitry Batuk

    (Collège de France, Chimie du Solide et Energie, UMR 8260, 11 place Marcelin Berthelot
    EMAT, University of Antwerp, Groenenborgerlaan 171)

  • Antonella Iadecola

    (Réseau sur le Stockage Electrochimique de l’Energie (RS2E), FR CNRS 3459)

  • Matthieu Saubanère

    (Réseau sur le Stockage Electrochimique de l’Energie (RS2E), FR CNRS 3459
    Institut Charles Gerhardt, CNRS UMR 5253, Université Montpellier, Place E. Bataillon)

  • Gwenaëlle Rousse

    (Collège de France, Chimie du Solide et Energie, UMR 8260, 11 place Marcelin Berthelot
    Sorbonne Universités - UPMC Univ. Paris 06, 4 Place Jussieu
    Réseau sur le Stockage Electrochimique de l’Energie (RS2E), FR CNRS 3459)

  • Dominique Larcher

    (Réseau sur le Stockage Electrochimique de l’Energie (RS2E), FR CNRS 3459
    Laboratoire de Réactivité et Chimie des Solides, UMR CNRS 7314, 33 Rue Saint Leu)

  • Hervé Vezin

    (Réseau sur le Stockage Electrochimique de l’Energie (RS2E), FR CNRS 3459
    Université Lille 1, CNRS UMR 8516-LASIR)

  • Marie-Liesse Doublet

    (Réseau sur le Stockage Electrochimique de l’Energie (RS2E), FR CNRS 3459
    Institut Charles Gerhardt, CNRS UMR 5253, Université Montpellier, Place E. Bataillon)

  • Jean-Marie Tarascon

    (Collège de France, Chimie du Solide et Energie, UMR 8260, 11 place Marcelin Berthelot
    Sorbonne Universités - UPMC Univ. Paris 06, 4 Place Jussieu
    Réseau sur le Stockage Electrochimique de l’Energie (RS2E), FR CNRS 3459)

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 O2 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.

Suggested Citation

  • Arnaud J. Perez & Quentin Jacquet & Dmitry Batuk & Antonella Iadecola & Matthieu Saubanère & Gwenaëlle Rousse & Dominique Larcher & Hervé Vezin & Marie-Liesse Doublet & Jean-Marie Tarascon, 2017. "Approaching the limits of cationic and anionic electrochemical activity with the Li-rich layered rocksalt Li3IrO4," Nature Energy, Nature, vol. 2(12), pages 954-962, December.
    • Handle: RePEc:nat:natene:v:2:y:2017:i:12:d:10.1038_s41560-017-0042-7
    DOI: 10.1038/s41560-017-0042-7
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    Cited by:

    1. Xuelong Wang & Liang Yin & Arthur Ronne & Yiman Zhang & Zilin Hu & Sha Tan & Qinchao Wang & Bohang Song & Mengya Li & Xiaohui Rong & Saul Lapidus & Shize Yang & Enyuan Hu & Jue Liu, 2023. "Stabilizing lattice oxygen redox in layered sodium transition metal oxide through spin singlet state," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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