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Abstract
As global energy demands continue to rise, the development of sustainable and efficient energy storage solutions has become increasingly critical. This dissertation explores the design of novel electrolyte materials for two promising next-generation energy storage technologies: lithium metal batteries and fuel cells. Achieving both high mechanical stability and ionic conductivity has always been a challenge in designing electrolyte materials for these devices. Atomistic simulations offer critical molecular insights into the fundamental mechanisms governing ion transport and mechanical stability in these systems. Supported by experimental evidence, these insights can drive design improvements. The dissertation begins by examining molecular designs of fluoroether liquid electrolytes for dendrite-free lithium metal batteries. Our research uncovers the intricate relationship between molecular architecture and ion transport mechanisms. The findings reveal a crucial trade-off between solvent chain length, self-diffusivity, and solvation shell stability, providing essential design principles for achieving high ionic conductivity in these systems. Building on this foundation, we then investigate solid-state electrolytes, with a particular focus on polymer/ceramic composite systems. Using atomistic simulations, we elucidate Li-ion transport across well-defined polymer-argyrodite interfaces. This study provides valuable insights into ionic complexation and transport mechanisms in these composite systems, contributing to the ongoing development of improved solid electrolyte materials. The third major component of this dissertation involves studying interfacial fluctuations in block copolymer electrolytes for anion exchange membranes. Our work reveals the critical importance of interfacial regions in determining swelling behavior and conductivity in these systems. These findings underscore the significance of interfaces in designing high-performance block copolymer anion exchange membranes, offering new avenues for optimizing their performance. In the final chapter, we explore the influence of structure on ion transport in crosslinked hydrated polyelectrolytes. By deconvoluting the roles of polymer segmental dynamics and water concentration, we demonstrate that conductivity depends primarily on the water concentration in these crosslinked systems. This insight opens new possibilities for designing robust yet highly conductive electrolyte materials.