Ordered LiNi0.5Mn1.5O4 Cathode in Bis(fluorosulfonyl)imide-Based Ionic Liquid Electrolyte: Importance of the Cathode-Electrolyte Interphase

25 September 2020, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


The high voltage (4.7 V vs. Li+ /Li) spinel lithium nickel manganese oxide (LiNi0.5 Mn1.5 O4 , LNMO) is a promising candidate for the next-generation of lithium ion batteries due to its high energy density, low cost and environmental impact. However, poor cycling performance at high cutoff potentials limits its commercialization. Herein, hollow structured LNMO is synergistically paired with an ionic liquid electrolyte, 1M lithium bis(fluorosulfonyl)imide (LiFSI) in N-propyl-N-methylpyrrolidinium bis(fluorosulfonyl)imide (Pyr1,3 FSI) to achieve stable cycling performance and improved rate capability. The optimized cathode-electrolyte system exhibits extended cycling performance (>85% capacity retention after 300 cycles) and high rate performance (106.2mAhg–1 at 5C) even at an elevated temperature of 65 ◦C. X-ray photoelectron spectroscopy and spatially resolved x-ray fluorescence analyses confirm the formation of a robust, LiF-rich cathode electrolyte interphase. This study presents a comprehensive design strategy to improve the electrochemical performance of high-voltage cathode materials.


Lithium Nickel Manganese Oxide
Cathode Electrolyte Interphase
Ionic Liquid Electrolyte
X-ray fluorescence mapping
X-ray Photoelectron Spectroscopy
X-ray Fluorescence

Supplementary materials



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