Accelerating cathode material discovery through <i>ab initio</i> random structure searching

The choice of cathode material in Li-ion batteries underpins their overall performance. Discovering new materials is a slow process, and all major commercial are still based on those identified the 1990s. Discovery using high-throughput calculations has attracted great research interest; however, reliance databases existing begs question whether these approaches applicable for finding truly novel materials. In this work, we demonstrate that ab initio random structure searching (AIRSS), first-principles prediction method does not rely any pre-existing data, can locate low energy structures complex efficiently only chemical composition. We use AIRSS to explore three Fe-containing polyanion compounds as low-cost cathodes. Using known quaternary LiFePO4 quinary LiFeSO4F cathodes examples, easily reproduce polymorphs, addition predicting other, hitherto unknown, polymorphs even polymorph more stable than ones. then phase space fluoroxalates, range redox-active phases yet be experimentally synthesized, demonstrating suitability tool accelerating discovery