Multifunctional nitrile additives for inducing pseudo-concentration gel-polymer electrolyte: Enabling stable high-voltage lithium metal batteries

Chi Guo, Yaqing Guo, Shuhao Yao, Runming Tao, Xiaolang Liu, Jianxing Wang, Haifeng Li, Huiying Li, Chang Hong, Jiazhi Geng, Xiao Guang Sun, Jianlin Li, Jiyuan Liang

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

High-voltage lithium metal batteries (LMBs) are promising for next-generation high-energy storage systems. Unfortunately, their implementation has been severely plagued by the interfacial instability between the high-voltage cathodes/lithium metal (LM) anodes and electrolytes. To tackle these challenges, a novel nitrile additive, 1,4-dicyanobenzene (DCB) (Synonyms: terephthalonitrile), is added to the in situ polymerized pentaerythritol tetraacrylate-based gel polymer electrolyte (GPE). The DCB additive, as demonstrated both theoretically and experimentally, plays a crucial role in altering the Li+ coordinated solvation structure within the GPE. This alteration leads to the formation of a pseudo-concentrated electrolyte with a tightly packed Li+ cluster, expanding the electrochemical stability window of the electrolyte. Moreover, the DCB-included GPE significantly improves its compatibility with both LM anode and high-voltage cathode, attributed to the modified solvation structure and the generated LiF-rich electrolyte/electrode interphases. Accordingly, the GPE enables stable cyclic performance of LMBs based on a 4.9 V LiNi0.5Mn1.5O4 cathode at a low relative negative/positive ratio of 4, achieving a high reversible capacity of 123.8 mAh g−1 with a capacity retention of 87.7 % over 500 cycles at 0.5 C. This work provides new insights into enhancing the cyclability of high-voltage LMBs via the synergistic effect of additives and GPE.

Original languageEnglish
Article number103683
JournalEnergy Storage Materials
Volume71
DOIs
StatePublished - Aug 2024

Funding

This work is supported by the Natural Science Foundation of China ( 52277218 ), the Hubei Provincial Natural Science Foundation of China ( 2024AFA094 ) and the Excellent Discipline Cultivation Project by JHUN ( 2023XKZ009 ). The efforts Runming Tao and Jianlin Li contributed are completely independent and personal, which does not involve financial support from any funding agencies. The research of X.-G. S. was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract number DE-AC05-00OR22725 .

Keywords

  • Gel polymer electrolyte
  • High-voltage cathodes
  • Li metal battery
  • Li solvation structure
  • Nitrile additive

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