Intermediate honeycomb ordering to trigger oxygen redox chemistry in layered battery electrode

Benoit Mortemard De Boisse, Guandong Liu, Jiangtao Ma, Shin Ichi Nishimura, Sai Cheong Chung, Hisao Kiuchi, Yoshihisa Harada, Jun Kikkawa, Yoshio Kobayashi, Masashi Okubo, Atsuo Yamada

Research output: Contribution to journalArticlepeer-review

99 Citations (Scopus)

Abstract

Sodium-ion batteries are attractive energy storage media owing to the abundance of sodium, but the low capacities of available cathode materials make them impractical. Sodium-excess metal oxides Na2MO3 (M: transition metal) are appealing cathode materials that may realize large capacities through additional oxygen redox reaction. However, the general strategies for enhancing the capacity of Na2MO3 are poorly established. Here using two polymorphs of Na2RuO3, we demonstrate the critical role of honeycomb-type cation ordering in Na2MO3. Ordered Na2RuO3 with honeycomb-ordered [Na1/3Ru2/3]O2 slabs delivers a capacity of 180 mAh g-1 (1.3-electron reaction), whereas disordered Na2RuO3 only delivers 135 mAh g-1 (1.0-electron reaction). We clarify that the large extra capacity of ordered Na2RuO3 is enabled by a spontaneously ordered intermediate Na1RuO3 phase with ilmenite O1 structure, which induces frontier orbital reorganization to trigger the oxygen redox reaction, unveiling a general requisite for the stable oxygen redox reaction in high-capacity Na2MO3 cathodes.

Original languageEnglish
Article number11397
JournalNature communications
Volume7
DOIs
Publication statusPublished - 2016 Apr 18
Externally publishedYes

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

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