Cationic dynamic elastomer electrolyte enabling all-solid-state lithium batteries

Cationic dynamic elastomer electrolyte enabling all-solid-state lithium batteries

Nano Energy

10.1016/j.nanoen.2025.111507

https://doi.org/10.1016/j.nanoen.2025.111507

Sirin Kamarulzaman, Dorsasadat Safanama, Zhi Yuan Lee, Ming Yan Tan, Carmen X.N. Lim, Mavis W.X. Low, Debbie H.L. Seng, Sheau Wei Chien, Jason Y.C. Lim, Shermin S. Goh, Derrick W.H. Fam

All-solid-state lithium batteries, Solid polymer electrolytes, Covalent adaptable networks, Dynamic covalent polymers, Polymeric ionic liquids, Triazolium

15 December 2025

Kamarulzaman, S., Safanama, D., Lee, Z. Y., Tan, M. Y., Lim, C. X. N., Low, M. W. X., Seng, D. H. L., Chien, S. W., Lim, J. Y. C., Goh, S. S., & Fam, D. W. H. (2025). Cationic dynamic elastomer electrolyte enabling all-solid-state lithium batteries. Nano Energy, 146, 111507. https://doi.org/10.1016/j.nanoen.2025.111507

Elastomeric solid polymer electrolytes (SPEs), exhibiting excellent toughness and interfacial stability with lithium (Li) metal anodes, are promising electrolytes for safe and durable all-solid-state Li-batteries. However, many elastomeric SPEs suffer from low conductivity, necessitating addition of liquid electrolytes which can compromise mechanical integrity and cause leakages. Herein, we introduce a fully solid-state elastomeric poly(triazolium) (PT-Li) SPE, which integrates the principles of poly(ionic liquid) (PIL) and covalent adaptable network (CAN) -based electrolytes to achieve enhanced performance characteristics. Like PILs, PT-Li possesses a wide electrochemical window (up to 5.2 V). Meanwhile, like CANs, dynamic triazolium crosslinking enables PT-Li to remain mechanically robust when cycling (shear loss factor ≤ 0.2 at 60 °C) while facilitating (re)processing under heat and pressure. Additionally, the cationic triazolium moieties facilitate Li+ -ion mobility (ionic conductivity, σ = 3.2 × 10−5 S cm−1 at 30 °C, 2 × 10−4 S cm−1 at 60 °C; lithium transference, TLi+ = 0.74). This enabled PT-Lis to exhibit excellent cycling performances in all-solid-state Li | LiFePO4 cells with uniform Li+ deposition at the Li anode interface and enhanced rate capability. The tunability and (re)processability enabled by dynamic covalent crosslinks represent a promising strategy for the development of robust all-solid-state lithium batteries.

Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0)

This research / project is supported by the A*STAR - Career Development Fund
Grant Reference no. : C233312026

This research / project is supported by the A*STAR - Manufacturing, Trade, and Connectivity Programmatic
Grant Reference no. : M22K9b0049

This research / project is supported by the A*STAR - Advanced Manufacturing and Engineering (AME) Programmatic
Grant Reference no. : M24N6b0043

https://oar.a-star.edu.sg/communities-collections/articles/22513

2211-2855

Institute of Materials Research and Engineering