Unraveling electrolyte solvation architectures for high-performance lithium-ion batteries

The design of advanced electrolytes hinges critically on a comprehensive comprehension of lithium-ion migration mechanisms within these electrochemical systems. Fluorination generally improves the stability and reduces the reactivity of organic compounds, making them potentially suitable for use in harsh conditions such as those found in a battery electrolyte. However, the specific properties, such as the solvation power, diffusivity, ion mobility, and so forth, would depend on the exact nature and extent of the fluorination. In this work, we introduce a theoretical framework designed to facilitate the autonomous creation of electrolyte molecular structures and craft methodologies to compute transport coefficients, providing a physical interpretation of fluoride systems. Taking fluorinated-1,2-diethoxyethanes as electrolyte solvents, we present and analyze the relationship between the electronic properties and atomic structures, and further correlate these properties to the transport coefficients, resulting in a good alignment with the experimental diffusion behaviors and Li-solvation structures. The insights derived from this research contribute to the methodological basis for high-throughput evaluation of prospective electrolyte systems, and consequently, propose strategic directions for the improvement of electrochemical cycle characteristics. This comprehensive exploration of the transport mechanisms enhances our understanding, offering avenues for further advancements in the field of lithium-ion battery technology.