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

Abstract

Abstract 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.

Keywords

• Localized high-concentration electrolytes
• Lithium batteries
• Theoretical calculation and computational simulation
• Density functional theory (DFT)
• Molecular dynamics (MD)
• Ab initio molecular dynamics (AIMD)