Toward Bottom-Up Understanding of Transport in Concentrated Battery Electrolytes

Bottom-up understanding of transport describes how molecular changes alter species concentrations and electrolyte voltage drops in operating batteries. Such an understanding is essential to predictively design electrolytes for desired transport behavior. We herein advocate building a structure-property-performance relationship as a systematic approach to accurate bottom-up understanding. To ensure generalization across salt concentrations as well as different electrolyte types and cell configurations, the property-performance relation must be described using Newman's concentrated solution theory. It uses Stefan-Maxwell diffusivity, ij, to describe the role of molecular motions at the continuum scale. The key challenge is to connect ij to the structure. We discuss existing methods for making such a connection, their peculiarities, and future directions to advance our understanding of electrolyte transport.