Atomistic modelling approaches to understanding the interfaces of ionic liquid electrolytes for batteries and electrochemical devices

Interface stability is a core issue in battery research. However, interfacial problems are the most complex dilemma to solve, and molecular modelling becomes increasingly indispensable today in the study of interface problems. This work reviews the atomistic computational methods currently used to understand electrolyte-electrode interfaces, with a particular interest in ionic liquid electrolytes which have shown promising prospects in the development of new generation high-energy-density batteries. Understanding their interfacial behaviour is critical for optimizing electrolyte composition. These methods have primarily been applied to the following four research topics: (1) understanding the ionic liquid electrolyte double layer at the electrolyte/electrode interface; (2) understanding the electrolyte composition near the electrodes and the early formation of solid electrolyte interphases; (3) predicting the components of the solid electrolyte interphases and modelling their growth; and (4) understanding ion transport across the interfaces and interphases.