First-principles material modeling of solid-state electrolytes with the spinel structure

Maarten J Mees; Geoffrey Pourtois; Fabio Rosciano; Brecht Put; Philippe M Vereecken; André Stesmans

doi:10.1039/c3cp54610a

First-principles material modeling of solid-state electrolytes with the spinel structure

Phys Chem Chem Phys. 2014 Mar 21;16(11):5399-406. doi: 10.1039/c3cp54610a.

Authors

Maarten J Mees¹, Geoffrey Pourtois, Fabio Rosciano, Brecht Put, Philippe M Vereecken, André Stesmans

Affiliation

¹ Department of Physics, University of Leuven, Celestijnenlaan 200 D, B-3001 Leuven, Belgium. meesm@imec.be.

PMID: 24503944
DOI: 10.1039/c3cp54610a

Abstract

Ionic diffusion through the novel (AlxMg1-2xLix)Al2O4 spinel electrolyte is investigated using first-principles calculations, combined with the Kinetic Monte Carlo algorithm. We observe that the ionic diffusion increases with the lithium content x. Furthermore, the structural parameters, formation enthalpies and electronic structures of (AlxMg1-2xLix)Al2O4 are calculated for various stoichiometries. The overall results indicate the (AlxMg1-2xLix)Al2O4 stoichiometries x = 0.2…0.3 as most promising. The (AlxMg1-2xLix)Al2O4 electrolyte is a potential candidate for the all-spinel solid-state battery stack, with the material epitaxially grown between well-known spinel electrodes, such as LiyMn2O4 and Li4+3yTi5O12 (y = 0…1). Due to their identical crystal structure, a good electrolyte-electrode interface is expected.