Hierarchical high-throughput screening of alkaline-stable lithium-ion conductors combining machine learning and first-principles calculations

TL;DR

This paper presents a hierarchical high-throughput screening method combining machine learning and first-principles calculations to identify alkaline-stable lithium-ion conductors suitable for solid-state batteries in humid environments.

Contribution

It introduces a novel workflow that efficiently screens over 320,000 compositions, identifying 209 candidates with enhanced alkaline stability and elucidating stability mechanisms.

Findings

Identified 209 alkaline-stable lithium-ion conductors from 320,000+ candidates.

Revealed cation substitution strategies that improve stability in NASICON and garnet structures.

Highlighted trade-offs in composition optimization for stability, conductivity, and synthesizability.

Abstract

Solid-state batteries require lithium-ion conductors that combine high ionic conductivity with stability under harsh electrochemical and chemical conditions. Here, we investigate the chemical factors governing the stability of NASICON-type and garnet-type Li-ion conductors in highly alkaline environments. This is particularly relevant to solid-state Li-air cells operated under humidified air where alkaline conditions arise due to the formation of LiOH discharge products. We implement a hierarchical high-throughput screening workflow that consists of a pre-screening step using a universal machine-learning interatomic potential and a more accurate DFT-based screening. This approach enables rapid evaluation of over 320,000 compositions, from which 209 alkaline-stable candidates are identified. We identify specific cation substitutions that improve alkaline stability in NASICON and garnet compounds and reveal the underlying mechanism. More importantly, we highlight design trade-offs that require careful composition optimization to simultaneously enhance synthesizability, operational stability, and Li-ion/electronic conductivities for practical humid Li-air battery applications.