Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 8, Pages 10141-10148Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c00661
Keywords
lithium metal batteries; ether-based electrolyte; nonflammable; high-voltage cathodes; SEI layer
Funding
- Taishan Scholars Program of Shandong Province [tsqn201812002, ts20190908]
- National Natural Science Foundation of China [51972198]
- Natural Science Foundation of Shandong Province [ZR2020JQ19]
- Young Scholars Program of Shandong University [2016WLJH03]
- State Key Program of National Natural Science of China [61633015]
- Shenzhen Fundamental Research Program [JCYJ20190807093405503]
- Project of the Taishan Scholar [ts201511004]
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The high reactivity between lithium metal and traditional carbonate electrolytes poses a challenge for the long-term cycling ability of lithium metal batteries. Ether-based electrolytes offer better stability towards lithium metal anodes but have limited oxidation stability below 4V and high flammability. This study introduces a high-voltage, nonflammable ether-based electrolyte with HFPN as a cosolvent, which effectively inhibits flame and stabilizes the lithium/electrolyte interface, achieving a capacity retention of around 95% for high-voltage lithium metal batteries.
The high reactivity between lithium metal and traditional carbonate electrolytes is a great obstacle to realize the long-term cycling ability of lithium metal batteries. Ether-based electrolytes have good stability toward lithium metal anodes. However, the oxidation stability of ether-based electrolytes is generally lower than 4 V, which limits the application of high-voltage (>4 V) cathodes and restricts the energy density. The high flammability of ether is another key issue that hinders the commercialization of ether-based electrolytes. To address these issues, herein, we report a high-voltage, nonflammable ether-based electrolyte with F-, N-, and P-rich hexafluorocyclotriphosphazene (HFPN) as a cosolvent. HFPN can not only act as a highly efficient flame-retarding agent but also form a dense and homogeneous solid electrolyte interphase (SEI) layer rich in LiF and Li3N on the lithium metal anode, which stabilizes the lithium/electrolyte interface and inhibits the formation of lithium dendrites. Moreover, the HFPN-based electrolyte has a wider potential window than 4 V. As a result, with this electrolyte, high-voltage lithium metal batteries exhibit a capacity retention of similar to 95% after 100 cycles. This study may provide a new pathway for developing safe, high-energy, and dendrite-free lithium metal batteries.
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