Structural evolution at the oxidative and reductive limits in the first electrochemical cycle of Li1.2Ni0.13Mn0.54Co0.13O2.

Nature Communications
Wei YinJean-Marie Tarascon

Abstract

High-energy-density lithium-rich materials are of significant interest for advanced lithium-ion batteries, provided that several roadblocks, such as voltage fade and poor energy efficiency are removed. However, this remains challenging as their functioning mechanisms during first cycle are not fully understood. Here we enlarge the cycling potential window for Li1.2Ni0.13Mn0.54Co0.13O2 electrode, identifying novel structural evolution mechanism involving a structurally-densified single-phase A' formed under harsh oxidizing conditions throughout the crystallites and not only at the surface, in contrast to previous beliefs. We also recover a majority of first-cycle capacity loss by applying a constant-voltage step on discharge. Using highly reducing conditions we obtain additional capacity via a new low-potential P" phase, which is involved into triggering oxygen redox on charge. Altogether, these results provide deeper insights into the structural-composition evolution of Li1.2Ni0.13Mn0.54Co0.13O2 and will help to find measures to cure voltage fade and improve energy efficiency in this class of material.

References

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Mar 8, 2011·Journal of the American Chemical Society·Naoaki YabuuchiShinichi Komaba
Jul 16, 2013·Nature Materials·M SathiyaJ-M Tarascon
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Mar 20, 2019·Nature Materials·Mouna Ben YahiaMarie-Liesse Doublet

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Citations

Oct 4, 2020·Nature Communications·Artem M AbakumovJean-Marie Tarascon
Jan 23, 2021·The Journal of Physical Chemistry Letters·Shehab E AliLaura Simonelli
Apr 8, 2021·Journal of the American Chemical Society·Antonin GrenierKarena W Chapman
Aug 3, 2021·The Journal of Physical Chemistry Letters·Jon Serrano-SevillanoAmaia Saracibar

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Methods Mentioned

BETA
X-ray
transmission
neutron powder diffraction
electron diffraction

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