How to estimate solid-electrolyte interphase features when screening electrolyte materials

TL;DR

This paper introduces automated estimators for solid-electrolyte interphase formation and graphite exfoliation, enabling systematic screening of electrolyte materials through quantum chemistry calculations of thermodynamic and kinetic effects.

Contribution

It presents a novel combinatorial approach combining quantum chemistry and heuristic methods to evaluate complex interfacial features in electrolyte screening.

Findings

Automated estimators for SEI formation and graphite exfoliation.

Systematic first assessment of electrolyte properties.

Application to large compound datasets.

Abstract

Computational screening of battery electrolyte components is an extremely challenging task because very complex features like solidelectrolyte-interphase (SEI) formation and graphite exfoliation need to be taken into account at least at the final screening stage. We present estimators for both SEI formation and graphite exfoliation based on a combinatorial approach with quantum chemistry calculations on model system reactions, which can be applied automatically for a large number of compounds and thus allows for a systematic first assessment of the relevant properties within screening approaches. Thermodynamic effects are assessed with quantum mechanical calculations, a more heuristic approach is used to estimate kinetic effects.