High‐Throughput Computational Screening of New Li‐Ion Battery Anode Materials

Abstract

We use density functional theory (DFT) in conjunction with grand canonical linear programming (GCLP), a powerful automated tool for analyzing ground state thermodynamics, to exhaustively enumerate the 515 thermodynamically stable lithiation reactions of transition metal silicides, stannides and phosphides, and compute cell potential, volume expansion, and capacity for each. These reactions comprise an exhaustive list of all possible thermodynamically stable ternary conversion reactions for these transition metal compounds. The reactions are calculated based on a library DFT energies of 291 compounds, including all transition metal silicides, phosphides and stannides found in the Inorganic Crystal Structure Database (ICSD). We screen our computational database for the most appealing anode properties based on gravimetric capacity, volumetric capacity, cell potential, and volume expansion when compared with graphitic carbon anodes. This high‐throughput computational approach points towards several promising anode compositions with properties significantly superior to graphitic carbon, including CoSi 2, TiP and NiSi 2.