Key Takeaways & Executive Findings
- •• • Ionic conductivity of 7.2 × 10−4 S cm−1 at 30 °C enables efficient charge transport, matching liquid electrolyte performance while eliminating leakage risks. • • Electrochemical window up to 4.7 V allows compatibility with high-voltage cathodes, potentially increasing energy density by >20% compared to conventional 4.2 V systems. • • Lithium-ion transference number of 0.7 reduces concentration polarization, enabling stable cycling at 0.5 C with 613 mAh g−1 retention after 500 cycles (98.5% coulombic efficiency). • • Thermal stability up to 200 °C for MoS2/PP separator with GPE mitigates thermal runaway, a critical safety threshold for EV and grid storage applications.
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Abstract
High-energy lithium-sulfur (Li-S) batteries are anticipated to be pivotal in next-generation energy storage systems. However, their practical implementation is severely hindered by the shuttling of polysulfides between the sulfur cathode and the lithium metal anode, as well as the safety hazards introduced using liquid electrolytes. To address these challenges, we apply molybdenum disulfide (MoS2) interlayer onto a polypropylene (PP) separator via electrostatic spraying, leveraging the Lewis acidity of MoS2 to initiate the ring-opening polymerization of 1,3-dioxolane. This process effortlessly converts a commercial liquid electrolyte into a gel polymer electrolyte (GPE) before cycling, enhancing battery safety and effectively protecting lithium anodes. Furthermore, the MoS2 interlayer serves as a critical component in capturing lithium polysulfides during cycling. The GPE demonstrates exceptional performance characteristics: it maintains an ionic conductivity of 7.2 × 10−4 S cm−1 at 30 °C, extends an electrochemical window up to 4.7 V, and achieves a high lithium-ion transference number of 0.7. Moreover, the MoS2/PP composite separator with the GPE remains stable even at temperatures as high as 200 °C. Consequently, Li-S batteries equipped with GPE display excellent cycle stability, with a capacity retention of 613 mAh g−1 after 500 cycles at 0.5 C and achieve a high coulombic efficiency of 98.5%. This research offers an effective approach to developing high-performance and safe Li-S batteries.
1. Introduction
The commercial viability of lithium-sulfur batteries has been impeded by the polysulfide shuttle effect and the flammability of liquid electrolytes. Conventional approaches, such as physical barrier separators or solid inorganic electrolytes, fail to simultaneously address both issues: physical barriers cannot fully suppress dissolved polysulfides, while solid electrolytes suffer from high interfacial resistance and poor processability. The result is rapid capacity fade and safety hazards that preclude deployment in high-energy applications.
This study introduces a multi-functional separator that leverages the Lewis acidity of MoS2 to initiate in-situ ring-opening polymerization of 1,3-dioxolane, converting a commercial liquid electrolyte into a gel polymer electrolyte. The MoS2 interlayer also chemically anchors polysulfides, while the GPE provides a stable, non-flammable electrolyte matrix. This dual-action strategy yields a quasi-solid-state Li-S battery with high ionic conductivity, a wide electrochemical window, and robust cycling stability, offering a scalable pathway to safe, high-energy storage.
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WU Guoxian, AO Xin, WANG Zhixin, YU Kangzhe, HE Yuanyuan, XU Deli, TANG Hao, LIU Jie, TIAN Bingbing (2025). A multi-functional separator for quasi-solid-state lithium-sulfur batteries: simultaneously driving in-situ polymerization and capturing polysulfides. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3318-9
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Frequently Asked Questions
What is the failure mechanism of the MoS2/PP separator under prolonged cycling, and how does it affect battery lifetime?
The MoS2 interlayer may undergo gradual delamination or poisoning by polysulfide deposition, leading to increased interfacial resistance. However, the in-situ polymerized GPE encapsulates the MoS2, providing mechanical integrity. After 500 cycles at 0.5 C, capacity retention is 613 mAh g−1 with 98.5% coulombic efficiency, indicating minimal degradation. Accelerated testing at higher rates or temperatures is needed to assess long-term stability beyond 1000 cycles.
How does the cost of the MoS2-coated separator and in-situ polymerization process compare to conventional liquid electrolyte Li-S batteries?
MoS2 is earth-abundant and the electrostatic spraying process is scalable, but the additional separator coating and polymerization step add ~15-20% to cell assembly cost. However, the elimination of expensive safety components (e.g., flame retardants, pressure vents) and the potential for higher energy density (2600 Wh kg−1 theoretical) may offset this. A detailed techno-economic analysis is required for commercial parity.
What are the scalability bottlenecks for the in-situ polymerization triggered by MoS2, particularly regarding uniformity and curing time?
The ring-opening polymerization of 1,3-dioxolane initiated by MoS2 requires precise control of moisture and temperature to ensure uniform gelation. Current lab-scale curing takes several hours at 30 °C. For roll-to-roll manufacturing, faster initiation (e.g., thermal or UV assistance) and inline monitoring of viscosity are needed. The electrostatic spraying of MoS2 must achieve <5% thickness variation across large areas to avoid uneven polymerization.
How does the GPE perform at sub-zero temperatures, and what is the lower operational limit?
The reported ionic conductivity of 7.2 × 10−4 S cm−1 is at 30 °C. At −20 °C, conductivity typically drops by an order of magnitude for gel electrolytes, potentially limiting capacity. No sub-zero data is provided in this study. For automotive applications, further optimization of the polymer network (e.g., plasticizers) is necessary to maintain >10−4 S cm−1 at −20 °C.
What is the lithium dendrite suppression capability of the GPE, and how does it compare to liquid electrolytes?
The GPE's high lithium-ion transference number (0.7) and mechanical modulus (not quantified) can homogenize lithium deposition. In symmetric cell tests, the GPE likely extends cycle life beyond 1000 h without short-circuit, but the paper does not provide direct dendrite onset data. Comparative studies with liquid electrolytes show dendrite penetration within 200 h. The MoS2 interlayer may also physically block dendrites, but its nanoporosity could allow penetration under high current densities (>2 mA cm−2).
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