Computational approaches to electrolyte design for advanced lithium-ion batteries

Abstract

Theoretical calculations have shown great potential as an instructional, reliable, and robust tool for designing and optimizing electrolyte formulations for lithium-ion batteries. However, there is still a lack of clear understanding of the design principles and synergistic effects between each component of electrolytes, including lithium salts, solvents, additives, etc., especially on how to optimize each part of electrolytes from the atomic scale and molecular scale. In this review, we cover the quantum chemistry in lithium salt selection, functional additive design, solid electrolyte interphase film study, and reaction mechanism speculation; molecular dynamics simulations in solvation structures, interphase simulations, and dendrite growth studies; and high throughput simulations in functional electrolyte screening. Meanwhile, the limitations of each type of simulation are discussed. Finally, conclusions and an outlook regarding theoretical calculations for the electrolyte design of lithium-ion batteries are presented.