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 CoSi2, TiP and NiSi2.

Surface phase diagram and stability of (001) and (111)LiMn2O4spinel oxides

“…[2][3][4][11][12][13][14][15][16][17][18][19][20][21][22][23] The LMO surface structure was not investigated until very recent years using DFT, 2 and there are notable discrepancies in the reported LMO surface energies. [2][3][4] For instance, the reported energies for the same (001) Li-terminated surface vary from 0.26 to 0.96 J/m 2 .…”

High-throughput screening of perovskite alloys for piezoelectric performance and thermodynamic stability

“…While these materials are reported to show a similar phase boundary as PZT, which is crucial for a high piezoelectric effect, the former material is expensive and difficult to synthesize due to problems with vaporization of potassium oxide during sintering [21,22], and the latter has a phase boundary that is very temperature dependent. To find new alloy compounds that reproduce the relevant properties of PZT provides a well-defined challenge for the growing community in highthroughput computational material design [23][24][25][26][27][28][29][30][31][32][33][34][35][36][37][38][39][40].…”

NixSi1-xAlloys Prepared by Mechanical Milling as Negative Electrode Materials for Lithium Ion Batteries

“…When made by sputtering or ball milling, such alloys typically form active Si / inactive matrix nanostructured composites, where the inactive matrix comprises a transition metal silicide. 3,7,[10][11][12][13][14][15][16][17][18][19][20][21] Although transition metal silicides are theoretically active with lithium from a thermodynamic basis, 10 most have been found to be completely inactive or have very limited capacity at room temperature. 3,[12][13][14][15][16][17] For instance, Fleischauer et al used a model based on effective heats of formation to explain the capacity behavior of (Fe, Mn, Cr+Ni, Co)-Si alloys.…”