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Advancements in Separator Modification and Quasi-Solid Electrolytes for Sulfurized Polyacrylonitrile-Based Lithium-Sulfur Batteries : A Comprehensive Study / 亞潘.

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This dissertation explores separator modifications and quasi-solid-state electrolytes (QSSE) to improve the electrochemical performance of sulfurized polyacrylonitrile-based (SPAN) lithium-sulfur (Li-S) batteries. The research focuses on enhancing safety and efficiency by incorporating functional materials into separators and electrolytes. In the first study, ZIF67 nanoparticles were integrated onto glass-fiber (GF) separators, creating a ZIF67@GF separator. This modification improved electrolyte absorption, wettability, and ion transport, leading to better electrochemical performance. Cells with ZIF67@GF separators demonstrated low polarization and long-term cycling stability, retaining high capacity over 600 cycles at 2C/2C. In the second study, quasi-solid-state Li-S batteries (QSSLSB) were developed using a hybrid solid-state electrolyte (HSE) membrane, containing LiTa2PO8 (LTPO) fillers within a PVDF-HFP matrix. By adding a small amount of liquid electrolyte to the HSE, the system promoted Li⁺ transport, improved electrolyte distribution, and enhanced interface stability. This approach aims to gradually phase out liquid electrolytes in favor of safer solid-state systems. Cells with the LTPO-HSE membrane exhibited smooth Li plating/stripping behavior, significantly lower exothermic heat generation, and improved cycling stability compared to conventional liquid-electrolyte systems. Finally, a polypropylene-based separator, PP|SC-NCM|PP was developed with a single crystal NCM811 (SC-NCM) layer. This trilayer separator improved electrolyte uptake, ionic conductivity, and Li+ ion transference number. In long-term cycling at 1C/1C, the cells with PP|SC-NCM|PP separator achieved 80% capacity retention over 500 cycles, as compared to 37% for the standard PP separator, and demonstrated improved performance under high-temperature conditions. Overall, the cells combination of ZIF67@GF separators, LTPO-HSE membranes, and PP|SC-NCM|PP separators significan

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