Unlocking All-Solid-State Lithium Conductivity with Dynamic Poly(Triazolium) Electrolytes
When and Where
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Abstract
To meet the growing demand for safer, high-performance batteries, Solid Polymer Electrolytes (SPEs) have emerged as promising alternatives to conventional liquid electrolytes because of their mechanical robustness and improved interfacial stability. However, many SPEs suffer from low Li-ion conductivity and require liquid additives or plasticizers, which compromise mechanical integrity and increase leakage risk.
To address these challenges, we developed a covalent adaptable network (CAN)-based SPE. CANs combine the mechanical strength of thermosets with the processability of thermoplastics through reversible covalent bonds that rearrange upon heating while remaining stable under operating conditions.
This work utilizes cationic poly(triazolium) dynamic bonds to develop a CAN-based SPE (PT-Li) with good mechanical properties, processability, and electrochemical performance. The crosslinked network provides dimensional stability during battery cycling, while the dynamic bonds enable reprocessing. Importantly, the cationic triazolium groups suppress anion mobility, resulting in a high lithium-ion transference number (τLi+ = 0.74) and improved ion transport. PT-Li was successfully integrated into an all-solid-state Li|PT-Li|LiFePO4 cell, delivering high coulombic efficiency (>99%) and stable charge/discharge cycling for over 200 cycles. The combination of tunable properties, recyclability, and strong battery performance highlights PT-Li as a promising platform for sustainable and manufacturable all-solid-state batteries.
References
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