CHEMICAL DESIGN AND SYNTHESIS OF ADVANCED MATERIALS FOR OVERCOMING LIMITATIONS IN SOLID-STATE LITHIUM-SULFUR
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dissertation
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University of Wisconsin-Milwaukee
Abstract
Solid-state lithium–sulfur (Li–S) batteries have emerged as a promising candidate in the quest for high-energy-density, safe, and long-lasting energy storage systems. Compared to conventional liquid-electrolyte Li–S batteries, their solid-state counterparts offer notable advantages, including the elimination of volatile organic solvents and improved safety due to enhanced thermal and electrochemical stability. However, despite these merits, solid-state electrolytes often suffer from intrinsic drawbacks such as sluggish ion transport, poor interfacialcontact, and limited mechanical compliance, those factors that severely hinder practical performance. In this work, we report a composite electrolyte strategy that integrates a newly synthesized UV-curable solid polymer electrolyte (PUA-based SPE) with a sulfide-based solid inorganic electrolyte (SIE), forming a dual-layer ion-conductive structure known as an inorganic/polymer hybrid electrolyte (IPHE). The PUA-based polymer, prepared via a facile one-pot method, provides excellent interfacial contact with the lithium metal anode due to its flexible nature and strong interfacial compatibility with the electrode. Simultaneously, the sulfide SIE layer maintains high ionic conductivity and effectively blocks polysulfide crossover. When combined, this IPHE architecture synergistically addresses the limitations of each individual component, resulting in improved electrochemical performance, enhanced mechanical strength, and increased resistance to lithium dendrite penetration.