In search of high performance anode materials for Mg batteries: computational studies of Mg in Ge, Si, and Sn

Abstract: We present ab initio studies of structures, energetics, and diffusion properties of Mg in Si, Ge, and Sn diamond structures to evaluate their potential as insertion type anode materials for Mg batteries. We show that Si could provide the highest specific capacities (3817 mAh g-1) and the lowest average insertion voltage (~0.15 eV vs. Mg) for Mg storage. Nevertheless, due to its significant percent lattice expansion (~216%) and slow Mg diffusion, Sn and Ge are more attractive; both anodes have lower lattice expansions (~120 % and ~178 %, respectively) and diffusion barriers (~0.50 and ~0.70 eV, respectively for single-Mg diffusion) than Si. We show that Mg-Mg interactions at different stages of charging can decrease significantly the diffusion barrier compared to the single atom diffusion, by up to 0.55 eV.