Novel mixed polyanions lithium-ion battery cathode materials predicted by high-throughput ab initio computations

The discovery of new chemistries outperforming current lithium intercalation cathodes is of major technological importance. In this context, polyanionic systems with the potential to exchange multiple electrons per transition metal are particularly interesting because they could combine the safety of polyanion systems with higher specific energy. In this paper, we report on a series of new mixed polyanions compounds of formula A(x)M(YO3)(XO4) (with A = Na, Li; X = Si, As, P; Y = C, B; M = a redox active metal; and x 0 to 3) identified by high-throughput ab initio computing. The computed stability of both lithium and sodium-based compounds is analyzed along with the voltage, specific energy and energy density of the lithium-based compounds. This analysis suggests several novel carbonophosphates and carbonosilicates as potential high capacity (>200 mAh/g) and specific energy (> 700 Wh/kg) cathode materials for lithium-ion batteries.