What question did this study set out to answer?

To enhance the performance of lithium-sulfur batteries through improved gel polymer electrolytes and reaction kinetics.

May 7, 2026Advanced Functional Materials1 citations

In Situ Crosslinking Polymerization and Redox Mediators for Gel‐Polymer Electrolyte‐Based Lithium‐Sulfur Batteries With Excellent Reaction Kinetics and Thermal Stability

XLX J LiShanghai University JYJiaqi YuShanghai University YLYalan LiaoShanghai University

Key Points

To enhance the performance of lithium-sulfur batteries through improved gel polymer electrolytes and reaction kinetics.
Developed a dual-function modification strategy integrating in situ cross-linking polymerization and redox mediators.
Designed a TMPDOL copolymer electrolyte with improved thermal stability.
Implemented SnF2 and 2-ethylanthraquinone for enhanced performance in Li-S batteries.
Achieved a record thermal stability with a decomposition temperature of 392°C.
Demonstrated a discharge specific capacity of 718 mAh g−1 at 3 C.
Maintained excellent cycling stability over 500 cycles at 1 C.

Abstract

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.

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