Fluorinated-oligomeric ionic liquids for high-performance wide-temperature solid zinc batteries

Ze Chen, Tong Liu, Zhiquan Wei, Yiqiao Wang, Ao Chen, Zhaodong Huang, Duanyun Cao*, Nan Li*, Chunyi Zhi*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

1 Citation (Scopus)

Abstract

Zn-based solid polymer electrolytes (SPEs) hold immense potential for developing high-performance and safe zinc ion batteries (ZIBs) that can operate effectively even at high temperatures. However, typical plasticizers like ionic liquids (ILs) exhibit limitations regarding Zn2+ ion transport and compatibility with the polymer matrix, causing a low Zn2+ transference number (tZn2+) and serious phase separation in SPEs. In this study, we develop a novel fluorinated IL (F-IL) plasticizer containing an imidazole cation with a fluoro alkyl substituent as an extended side chain for zinc-based SPEs. This innovative imidazole cation effectively modifies the Zn2+ solvation structure. It significantly enhances the compatibility between ILs and the polymer matrix, enabling fast Zn2+ ion transport (with a notable tZn2+ of 0.46 and high ionic conductivity of 2.8 × 10−3 S cm−1) when incorporated in SPEs. Using the F-ILs-based SPE, we achieve dendrite-free Zn plating/stripping cycling over 2000 h, even at high temperatures. A Zn‖Cl4Q battery assembled with the designed SPE outperforms other solid ZIBs, demonstrating a wide working temperature range (−15 °C to 120 °C) and a long cycling life (capacity retention 70.9% after 2000 cycles at 90 °C). In addition, the pouch cell exhibits a remarkable shelf life (90 days) and a low self-discharge rate (capacity loss of 0.09% per day) at 60 °C, thanks to the high thermal and chemical stability of the SPE during operation. The F-IL-based SPE, with its advanced ion transport structure, provides solid ZIBs with significant performance improvement, high safety, and enduring durability.

Original languageEnglish
Pages (from-to)3296-3304
Number of pages9
JournalEnergy and Environmental Science
Volume18
Issue number7
DOIs
Publication statusPublished - 20 Feb 2025
Externally publishedYes

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