Unlocking anionic redox activity in O3-type sodium 3d layered oxides via Li substitution

Qing Wang, Sathiya Mariyappan, Gwenaëlle Rousse, Anatolii V. Morozov, Benjamin Porcheron, Rémi Dedryvère, Jinpeng Wu, Wanli Yang, Leiting Zhang, Mohamed Chakir, Maxim Avdeev, Michaël Deschamps, Young Sang Yu, Jordi Cabana, Marie Liesse Doublet, Artem M. Abakumov, Jean Marie Tarascon

Research output: Contribution to journalArticlepeer-review

66 Citations (Scopus)

Abstract

Sodium ion batteries, because of their sustainability attributes, could be an attractive alternative to Li-ion technology for specific applications. However, it remains challenging to design high energy density and moisture stable Na-based positive electrodes. Here, we report an O3-type NaLi1/3Mn2/3O2 phase showing anionic redox activity, obtained through a ceramic process by carefully adjusting synthesis conditions and stoichiometry. This phase shows a sustained reversible capacity of 190 mAh g−1 that is rooted in cumulative oxygen and manganese redox processes as deduced by combined spectroscopy techniques. Unlike many other anionic redox layered oxides so far reported, O3-NaLi1/3Mn2/3O2 electrodes do not show discernible voltage fade on cycling. This finding, rationalized by density functional theory, sheds light on the role of inter- versus intralayer 3d cationic migration in ruling voltage fade in anionic redox electrodes. Another practical asset of this material stems from its moisture stability, hence facilitating its handling and electrode processing. Overall, this work offers future directions towards designing highly performing sodium electrodes for advanced Na-ion batteries.

Original languageEnglish
Pages (from-to)353-361
Number of pages9
JournalNature Materials
Volume20
Issue number3
DOIs
Publication statusPublished - Mar 2021

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