A Computational Review on Localized High-Concentration Electrolytes in Lithium Batteries

Electrolyte engineering plays a vital role in improving the battery performance of lithium batteries. The idea of localized high-concentration electrolytes that are derived by adding “diluent” in high-concentration electrolytes has been proposed to retain the merits and alleviate the disadvantages of high-concentration electrolytes, and it has become the focus of attention in high-voltage lithium batteries, flame-retardant lithium batteries, and low-temperature lithium batteries. Extensive efforts have been made to elucidate the fundamentals of localized high-concentration electrolytes. This review provides an overview of state-of-the-art computational progress in the studies of localized high-concentration electrolytes, focusing on the application of computational techniques to analyze the redox stability, solvation structures, and interface characteristics of lithium batteries with localized high-concentration electrolytes. Integrated with experimental approaches, complementing each other, computational methods are believed to be conducive to understanding the working mechanism and designing localized high-concentration electrolytes for better lithium batteries in the future.