Amorphous Molybdenum Sulfide Chalcogels for Electrochemical Energy Storage— First-Principles Structure-Property Relationships

Lithium-sulfur (Li-S) batteries hold great promise for next-generation energy storage, yet their commercial viability is hindered by slow lithium diffusion and polysulfide shuttling, which compromise performance and longevity. Molybdenum sulfide-based (MoxSy) chalcogels have emerged as a compelling alternative, demonstrating enhanced stability and facilitating lithium diffusion, thereby addressing these limitations. In this study, we investigate the structure-property relationships of amorphous MoS2 and Mo3S13 chalcogels through ab initio molecular dynamics (AIMD) simulations. Our analyses focus on atomic arrangements, bonding characteristics, and their implications for electrochemical performance. Key findings reveal insights into the coordination environment of molybdenum and sulfur atoms within the chalcogel matrix, highlighting predominant Mo-S bonding interactions that contribute to structural stability. Additionally, we explore the impact of local structural disorder on ion transport, targeting lithium and sodium. By elucidating the relationships between atomic structure and electrochemical behavior, our findings advance understanding of MoxSy chalcogels and their potential applications in Li-S energy storage technologies.