Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries

Abstract

A passivation layer called the solid electrolyte interphase (SEI) is formed on electrode surfaces from decomposition products of electrolytes. The SEI allows Li + transport and blocks electrons in order to prevent further electrolyte decomposition and ensure continued electrochemical reactions. The formation and growth mechanism of the nanometer thick SEI films are yet to be completely understood owing to their complex structure and lack of reliable in situ experimental techniques. Significant advances in computational methods have made it possible to predictively model the fundamentals of SEI. This review aims to give an overview of state-of-the-art modeling progress in the investigation of SEI films on the anodes, ranging from electronic structure calculations to mesoscale modeling, covering the thermodynamics and kinetics of electrolyte reduction reactions, SEI formation, modification through electrolyte design, correlation of SEI properties with battery performance, and the artificial SEI design. Multiscale simulations have been summarized and compared with each other as well as with experiments. Computational details of the fundamental properties of SEI, such as electron tunneling, Li-ion transport, chemical/mechanical stability of the bulk SEI and electrode/(SEI/) electrolyte interfaces have been discussed. This review shows the potential of computational approaches in the deconvolution of SEI properties and design of artificial SEI. We believe that computational modeling can be integrated with experiments to complement each other and lead to a better understanding of the complex SEI for the development of a highly efficient battery in the future.

A Robust Solid Electrolyte Interphase Layer Augments the Ion Storage Capacity of Bimetallic‐Sulfide‐Containing Potassium‐Ion Batteries

“…[22][23][24] Further improvement in the electrochemical performance of transition-metal sulfides-specifically their potassium-ion storage properties-may be achieved with an appropriate electrolyte.T he organic salt, alkali bis(fluorosulfonyl) imide,i su sed widely in batteries because of its unique function in forming stable SEI layers. [22][23][24] Further improvement in the electrochemical performance of transition-metal sulfides-specifically their potassium-ion storage properties-may be achieved with an appropriate electrolyte.T he organic salt, alkali bis(fluorosulfonyl) imide,i su sed widely in batteries because of its unique function in forming stable SEI layers.…”

Improving the Stability of an RT‐NaS Battery via In Situ Electrochemical Formation of Protective SEI on a Sulfur–Carbon Composite Cathode

“…[18,19] SEI is an insulator but ion permeable layer composed of multiple components such as metal oxide, metal fluoride, polyolephines, and metal carbonate. [18,19] SEI is an insulator but ion permeable layer composed of multiple components such as metal oxide, metal fluoride, polyolephines, and metal carbonate.…”

Key Aspects of Lithium Metal Anodes for Lithium Metal Batteries

“…It is well known that the anode is always covered by a protective layer called an SEI film . An unstable SEI results in fast self‐discharge (short shelf‐life), increased impedance, irreversible capacity loss, dendrite formation, and an abnormal Coulombic efficiency of the cell . In early research, the Butler–Volmer equation was used to investigate the growth and behavior of the SEI film.…”

“…However, the SEI is a very complicated layer and its composition and properties may dependent on numerous factors including electrolyte composition/concentration, temperature, current density, etc . Research on SEI formation and composition has been well reviewed elsewhere …”