ABSTRACT Lithium‐sulfur (Li‐S) batteries face critical challenges of lithium polysulfides (LiPSs) shuttling and lithium dendrites in liquid electrolytes, while conventional gel polymer electrolytes (GPE) suffer from low thermal stability (<110°C) and sluggish kinetics. This work pioneers a dual‐function modification strategy integrating in situ cross‐linking polymerization and a redox mediator for GPE‐based Li‐S batteries. A novel TMPDOL copolymer electrolyte is designed through selective crosslinking of trihydroxymethylpropane tris3‐(2‐methyl‐1‐aza‐cyclobutyane)propionate (TMP) with 3‐dioxopentane (DOL), achieving record thermal stability (392°C decomposition temperature), and it can also promote the dissociation of LiTFSI and accelerate lithium‐ion transport kinetics. Concurrently, the SnF 2 initiator generates a LiF/Li 13 Sn 5 ‐rich solid electrolyte interphase (SEI) enabling uniform lithium deposition, while the 2‐ethylanthraquinone (2‐EAQ) redox mediator catalytically accelerates polysulfide conversion kinetics and inhibits the shuttle of LiPSs. The Li‐S batteries exhibit a promising discharge specific capacity of 718 mAh g −1 at 3 C and excellent long‐term cycling stability over 500 cycles at 1 C. This work introduces new electrolyte engineering paradigms through molecular crosslinking for thermal resilience, dynamic redox mediation to overcome kinetics barriers, and multi‐functional initiators for stable interfaces, providing a scalable pathway for the development of GPE‐based Li‐S batteries with high dynamic, excellent thermal stability and safety.
Li et al. (Sat,) studied this question.
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