Li/Fe substitution in Li-rich Ni, Co, Mn oxides for enhanced electrochemical performance as cathode materials

Juliette Billaud, Denis Sheptyakov, Sébastien Sallard, Daniela Leanza, Michael Talianker, Judith Grinblat, Hadar Sclar, Doron Aurbach, Petr Novák, Claire Villevieille

Research output: Contribution to journalArticlepeer-review

29 Scopus citations

Abstract

Li-rich nickel cobalt manganese (NCM) oxides are among the most promising cathode materials for lithium-ion batteries owing to their high specific charges and operating voltages. However, their crystal structures are unstable upon prolonged cycling, leading to a collapse of their electrochemical performance. In this study, we investigated Fe doping of Li-rich NCM materials and explored various Li/Fe ratios. Compared with the reference Li-rich NCM material, the Li1.16(Ni0.18Co0.10Mn0.52Fe0.02)O2 composition exhibited a higher specific charge, potential drop mitigation at fast cycling rates, and an enhanced rate capability. At a rate of 4C, this composition exhibited a specific charge of 150 mA h g-1, which was as much as 50% higher than that of the reference (100 mA h g-1). Neutron and X-ray diffraction data for compounds with different Fe doping concentrations indicated that the crystallographic structure was preserved with up to 2 mol% Fe without the formation of separate impurity phases. Furthermore, we found that the crystal structure of this Fe-doped material was less susceptible to the effects of prolonged cycling than the reference compound. Complementary investigations with X-ray photoelectron spectroscopy revealed that Fe was electrochemically active in the structure, which explains the beneficial effects observed with Fe doping of Li-rich NCM materials, such as an increased specific charge and more stable cycling.

Original languageEnglish
Pages (from-to)15215-15224
Number of pages10
JournalJournal of Materials Chemistry A
Volume7
Issue number25
DOIs
StatePublished - 2019

Bibliographical note

Funding Information:
This work is partly based on experiments performed at the Swiss spallation neutron source SINQ, Paul Scherrer Institute, Villi-gen, Switzerland. The authors are also grateful to BASF SE for funding. The authors gratefully thank Dr Boris Markovsky for fruitful discussions.

Publisher Copyright:
© 2019 The Royal Society of Chemistry.

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