Computational Modelling Study on Stability of Li-S/Se System

Li-ion batteries have transformed portable electronics and will play a key role in the electrification of transport. However, the highest energy storage possible for Li-ion batteries is insufficient for the long-term needs of society. Here we consider a study on rechargeable lithium−sulfur (Li−S) batteries which hold great potential for high-performance energy storage systems because they have a high theoretical specific energy, low cost, and are eco-friendly. This work employs computational modelling methods to explore stability, structural and electronic properties of discharge products formed in the Li-S/Se battery, especially Li 2 S/Se, which has potential to offer higher theoretical specific energy and remedies the challenges that Li-S battery encounters. First principle methods were used to calculate thermodynamic properties of Li 2 S and Li 2 Se, which agreed with available experimental results. A cluster expansion technique generated new stable phases of Li 2 S/Se system and Monte Carlo simulations determined concentration and temperature ranges in which the systems mix. Interatomic Born Meyer potential models for Li 2 S and Li 2 Se were derived and validated and used to explore high temperature structural and transport properties of Li 2 S/Se.