Improving Energy Density and Structural Stability of Manganese Oxide Cathodes for Na-Ion Batteries by Structural Lithium Substitution

Ezequiel De La Llave, Elahe Talaie, Elena Levi, Prasant Kumar Nayak, Mudit Dixit, Penki Tirupathi Rao, Pascal Hartmann, Frederick Chesneau, Dan Thomas Major, Miri Greenstein, Doron Aurbach, Linda F. Nazar

Research output: Contribution to journalArticlepeer-review

200 Scopus citations


We report excellent cycling performance for P2-Na0.6Li0.2Mn0.8O2, an auspicious cathode material for sodium-ion batteries. This material, which contains mainly Mn4+, exhibits a long voltage plateau on the first charge, similar to that of high-capacity lithium and manganese-rich metal oxides. Electrochemical measurements, X-ray diffraction, and elemental analysis of the cycled electrodes suggest an activation process that includes the extraction of lithium from the material. The "activated" material delivers a stable, high specific capacity up to ∼190 mAh/g after 100 cycles in the voltage window between 4.6-2.0 V versus Na/Na+. DFT calculations locate the energy states of oxygen atoms near the Fermi level, suggesting the possible contribution of oxide ions to the redox process. The addition of Li to the lattice improves structural stability compared to many previously reported sodiated transition-metal oxide electrode materials, by inhibiting the detrimental structural transformation ubiquitously observed with sodium manganese oxides during cycling. This research demonstrates the prospect of intercalation materials for Na-ion battery technology that are active based on both cationic and anionic redox moieties.

Original languageEnglish
Pages (from-to)9064-9076
Number of pages13
JournalChemistry of Materials
Issue number24
StatePublished - 27 Dec 2016

Bibliographical note

Publisher Copyright:
© 2016 American Chemical Society


L.F.N and D.A gratefully acknowledge funding from BASF SE for ongoing support through the BASF Research Network in Electrochemistry and Batteries. L.F.N. also thanks the Natural Sciences and Engineering Council of Canada for partial financial support of this work through their Discovery and Canada Research Chair programs. D.A. and D.T.M. also thank the Israel Science Foundation (ISF) for a partial financial support of this work.

FundersFunder number
Natural Sciences and Engineering Research Council of Canada
Israel Science Foundation


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