Origin of voltage decay in high-capacity layered oxide electrodes

M. Sathiya, A. M. Abakumov, D. Foix, G. Rousse, K. Ramesha, M. Saubanère, M. L. Doublet, H. Vezin, C. P. Laisa, A. S. Prakash, D. Gonbeau, G. Vantendeloo, J. M. Tarascon

Research output: Contribution to journalArticlepeer-review

620 Citations (Scopus)


Although Li-rich layered oxides (Li1+x Niy Coz Mn 1-x-y-z O2 > 250 mAh g-1) are attractive electrode materials providing energy densities more than 15% higher than today's commercial Li-ion cells, they suffer from voltage decay on cycling. To elucidate the origin of this phenomenon, we employ chemical substitution in structurally related Li2 RuO3 compounds. Li-rich layered Li2 Ru1-y Tiy O3 phases with capacities of ∼240 mAh g-1 exhibit the characteristic voltage decay on cycling. A combination of transmission electron microscopy and X-ray photoelectron spectroscopy studies reveals that the migration of cations between metal layers and Li layers is an intrinsic feature of the charge-discharge process that increases the trapping of metal ions in interstitial tetrahedral sites. A correlation between these trapped ions and the voltage decay is established by expanding the study to both Li2 Ru1-y Sny O3 and Li2 RuO3; the slowest decay occurs for the cations with the largest ionic radii. This effect is robust, and the finding provides insights into new chemistry to be explored for developing high-capacity layered electrodes that evade voltage decay.

Original languageEnglish
Pages (from-to)230-238
Number of pages9
JournalNature Materials
Issue number2
Publication statusPublished - Feb 2015
Externally publishedYes


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