Journal
CHEMISTRY OF MATERIALS
Volume 33, Issue 4, Pages 1238-1248Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.0c04014
Keywords
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Funding
- ISCF Faraday Challenge project SOLBAT [FIRG007]
- Henry Royce Institute (through UK Engineering and Physical Science Research Council) [EP/R010145/1]
- Advanced Photon Source (APS) [DE-AC02-06CH11357]
- National Research Foundation of Korea [NRF2019R1A6A3A03031343]
- Shanghai Sailing Program [20YF1452300]
- Fundamental Research Funds for the Central Universities
- EPSRC [EP/R010145/1, EP/S003053/1] Funding Source: UKRI
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By synergistically pairing hollow-structured LNMO with an ionic liquid electrolyte, stable cycling performance and improved rate capability were achieved, allowing for high energy density and low cost. This comprehensive design strategy provides insights to enhance the electrochemical performance of high-voltage cathode materials.
The high-voltage (4.7 V vs Li+/Li) spinel lithium nickel manganese oxide (LiNi0.5Mn1.5O4, LNMO) is a promising candidate for the next generation of lithium-ion batteries due to its high energy density, low cost, and low 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, 1 M lithium bis(fluorosulfonyl)imide (LiFSI) in N-propyl-N-methylpyrrolidinium bis( fluorosulfonyl)imide (Pyr(1,3)FSI), to achieve stable cycling performance and improve the rate capability. The optimized cathode-electrolyte system exhibits extended cycling performance (>85% capacity retention after 300 cycles) and high rate performance (106.2 mAh g(-1) at 5C) even at an elevated temperature of 65 degrees 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.
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