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High-capacity electrode materials for rechargeable lithium batteries: Li₃NbO₄-based system with cation-disordered rocksalt structure

Proceedings of the National Academy of Sciences - PNAS, 2015-06, Vol.112 (25), p.7650-7655 [Peer Reviewed Journal]

Volumes 1–89 and 106–112, copyright as a collective work only; author(s) retains copyright to individual articles ;ISSN: 0027-8424 ;EISSN: 1091-6490 ;DOI: 10.1073/pnas.1504901112 ;PMID: 26056288

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  • Title:
    High-capacity electrode materials for rechargeable lithium batteries: Li₃NbO₄-based system with cation-disordered rocksalt structure
  • Author: Yabuuchi, Naoaki ; Takeuchi, Mitsue ; Nakayama, Masanobu ; Shiiba, Hiromasa ; Ogawa, Masahiro ; Nakayama, Keisuke ; Ohta, Toshiaki ; Endo, Daisuke ; Ozaki, Tetsuya ; Inamasu, Tokuo ; Sato, Kei ; Komaba, Shinichi
  • Subjects: Physical Sciences
  • Is Part Of: Proceedings of the National Academy of Sciences - PNAS, 2015-06, Vol.112 (25), p.7650-7655
  • Description: Rechargeable lithium batteries have rapidly risen to prominence as fundamental devices for green and sustainable energy development. Lithium batteries are now used as power sources for electric vehicles. However, materials innovations are still needed to satisfy the growing demand for increasing energy density of lithium batteries. In the past decade, lithium-excess compounds, Li₂MeO₃ (Me = Mn⁴⁺, Ru⁴⁺, etc.), have been extensively studied as high-capacity positive electrode materials. Although the origin as the high reversible capacity has been a debatable subject for a long time, recently it has been confirmed that charge compensation is partly achieved by solid-state redox of nonmetal anions (i.e., oxide ions), coupled with solid-state redox of transition metals, which is the basic theory used for classic lithium insertion materials, such as LiMeO₂ (Me = Co³⁺, Ni³⁺, etc.). Herein, as a compound with further excess lithium contents, a cation-ordered rocksalt phase with lithium and pentavalent niobium ions, Li₃NbO₄, is first examined as the host structure of a new series of high-capacity positive electrode materials for rechargeable lithium batteries. Approximately 300 mAh·g⁻¹ of high-reversible capacity at 50 °C is experimentally observed, which partly originates from charge compensation by solid-state redox of oxide ions. It is proposed that such a charge compensation process by oxide ions is effectively stabilized by the presence of electrochemically inactive niobium ions. These results will contribute to the development of a new class of high-capacity electrode materials, potentially with further lithium enrichment (and fewer transition metals) in the close-packed framework structure with oxide ions.
  • Publisher: United States: National Academy of Sciences
  • Language: English
  • Identifier: ISSN: 0027-8424
    EISSN: 1091-6490
    DOI: 10.1073/pnas.1504901112
    PMID: 26056288
  • Source: GFMER Free Medical Journals
    PubMed Central
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