Evolution of LiNi0.8Mn0.1Co0.1O2 (NMC811) Cathodes for Li-Ion Batteries: An In Situ Electron Paramagnetic Resonance Study

IF 3.3 3区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry C Pub Date : 2025-04-11 DOI:10.1021/acs.jpcc.5c00275

Bin Wang, Edurne Redondo, Lewis W. Le Fevre, Adam Brookfield, Eric J. L. McInnes, Robert A. W. Dryfe

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Abstract

The rapid voltage and capacity fade of the otherwise promising Ni-rich layered LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) cathode are the primary obstacles to its successful commercialization in lithium-ion batteries (LIBs). Here, in situ electrochemical electron paramagnetic resonance (EPR) spectroscopy is employed to gain insight into the cation redox behavior of the NMC811 cathode during the cell charge/discharge process. Different oxidation states of Ni ions are detected by variations in the signal of the EPR spectra. Ex situ studies of NMC811 at different SOC levels also confirm changes in the local Mn–Ni environment. A comparison of in situ studies on fresh and cycled NMC811 electrodes demonstrates that the fundamental redox processes remain unchanged upon cycling of the material. Finally, dissolved Mn and Co ions from the bulk are found using ex situ EPR characterization of the cycled cathode and separator. The dissolution of these metal ions can accelerate the degradation of the entire battery.

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来源期刊

The Journal of Physical Chemistry C 化学-材料科学：综合

CiteScore

6.50

自引率

8.10%

发文量

2047

审稿时长

1.8 months

期刊介绍： The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.