A Multifunctional Potent Lewis Acid for In Situ Formation of Poly-Dioxolane Electrolytes Toward High-Performance Quasi-Solid State Lithium Metal Batteries #MMPMID41319298
Yu J; Hong S; Park M; Kwak M; Kim S; Heo J; Kim WB
Adv Sci (Weinh) 2025[Nov]; ? (?): e19181 PMID41319298show ga
Quasi-solid-state polymer electrolytes represent a promising strategy for Li metal batteries (LMBs) with superior safety and energy density. However, Li dendrite formation and unstable interfaces significantly hinder their practical application. Here, an AlCl(3)-initiated gel polymer electrolyte (AGPE) is developed via in situ ring-opening polymerization of 1,3-dioxolane (DOL) to directly generate poly(1,3-dioxolane) (PDOL) electrolyte in battery cells. AlCl(3) acts both as polymerization initiator and a multifunctional additive, enhancing polymer network stability and facilitating selective Li(+) transport through an AlCl(3)-mediated multi-coordination framework. Additionally, AlCl(3) spontaneously generates a hybrid SEI layer composed of LiF, LiCl, and LiAl, significantly enhancing interfacial stability and suppressing dendritic growth. Consequently, the AGPE achieves excellent ionic conductivity ( approximately 5.0 mS cm(-1) at room temperature) and an outstanding Li(+) transference number (t(Li+) = 0.75). Li||LiFePO(4) full cells employing AGPE exhibit superior electrochemical stability, retaining 92.7% capacity after 280 cycles at 0.5 C and delivering a high capacity of 118.2 mAh g(-1) at 5 C. These results highlight AGPE as an attractive quasi-solid electrolyte, demonstrating substantial promise for safe and high-performance next-generation LMBs.
Adv+Sci+(Weinh) 2025 ; ? (?): e19181
