ORGS3-0295
Tailoring Bicontinuous Elastomeric Electrolytes for High-Performance Lithium Metal Batteries
When and Where
Nov 30, -0001
12:00am - 12:00am
Presenter(s)
Jaejoon Lee (KAIST)
Co-Author(s)
Abstract
We report an elastomeric electrolyte capable of stable lithium (Li) metal batteries (LMBs) operation over a wide temperature range, extending down to −20 °C. The electrolyte features a bicontinuous architecture composed of a hexafluorobutyl acrylate (HFBA) elastomer network and a succinonitrile (SN) plastic crystal phase, fabricated via polymerization-induced phase separation (PIPS). This design enables independent tuning of Li⁺ transport in the plastic crystal phase while maintaining high mechanical stretchability (~300 %), which is critical for accommodating Li volume changes and suppressing dendrite formation. Incorporation of 15 vol % adiponitrile (ADN) into SN enhances its reorientational dynamics, promoting faster Li⁺ hopping and resulting in high ionic conductivity (0.17 mS cm⁻¹) and a Li⁺ transference number of 0.71 at −20 °C. Simultaneously, increasing the crosslinker functionality from di- to hexa-functional refines the bicontinuous morphology, producing smaller, well-connected domains with reduced tortuosity. Under low-temperature conditions with high cathode loading (5 mg cm⁻²), the combined effects of ADN incorporation and optimized crosslinker functionality improve Li⁺ transport, homogenize ion flux, and reinforce mechanical integrity, yielding an initial discharge capacity of 158 mAh g⁻¹ with 75 % retention over 100 cycles. These findings establish a practical design strategy for bicontinuous elastomeric electrolytes that optimizes ion transport efficiency and mechanical robustness for high-performance LMBs under demanding operational conditions.
