Coulombic self-ordering upon charging a large-capacity layered cathode material for rechargeable batteries

Benoit Mortemard de Boisse, Marine Reynaud, Jiangtao Ma, Jun Kikkawa, Shin-ichi Nishimura, Montse Casas-Cabanas, Claude Delmas, Masashi Okubo and Atsuo Yamada ()
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Benoit Mortemard de Boisse: The University of Tokyo
Marine Reynaud: CIC energiGUNE, Parque Tecnológico de Álava
Jiangtao Ma: The University of Tokyo
Jun Kikkawa: Advanced Key Technologies Division, National Institute for Materials Science
Shin-ichi Nishimura: The University of Tokyo
Montse Casas-Cabanas: CIC energiGUNE, Parque Tecnológico de Álava
Claude Delmas: Institut de Chimie de la Matière Condensée de Bordeaux (ICMCB)
Masashi Okubo: The University of Tokyo
Atsuo Yamada: The University of Tokyo

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: Abstract Lithium- and sodium-rich layered transition-metal oxides have recently been attracting significant interest because of their large capacity achieved by additional oxygen-redox reactions. However, layered transition-metal oxides exhibit structural degradation such as cation migration, layer exfoliation or cracks upon deep charge, which is a major obstacle to achieve higher energy-density batteries. Here we demonstrate a self-repairing phenomenon of stacking faults upon desodiation from an oxygen-redox layered oxide Na2RuO3, realizing much better reversibility of the electrode reaction. The phase transformations upon charging A2MO3 (A: alkali metal) can be dominated by three-dimensional Coulombic attractive interactions driven by the existence of ordered alkali-metal vacancies, leading to counterintuitive self-repairing of stacking faults and progressive ordering upon charging. The cooperatively ordered vacancy in lithium-/sodium-rich layered transition-metal oxides is shown to play an essential role, not only in generating the electro-active nonbonding 2p orbital of neighbouring oxygen but also in stabilizing the phase transformation for highly reversible oxygen-redox reactions.

Date: 2019
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DOI: 10.1038/s41467-019-09409-1

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