Work

A Descriptor for Non‐Arrhenius Ion Transport Enables Design of Sulfide Superionic Conductors

Year: 2026

Type: article

Abstract: ABSTRACT Non‐Arrhenius ion transport is increasingly observed in solid electrolytes but remains difficult to compare across materials or use in screening. A curated database of 867 conductivity‐temperature entries from thio‐LISICON and LGPS‐type sulfides is used to introduce Meyer–Neldel deviation (MND), a physics‐informed, material‐level descriptor of temperature‐dependent changes in apparent activation energy. More than 40% of the analyzed sulfide electrolytes show notable deviations from linear Arrhenius behavior. MND separates low‐conductivity/high‐barrier and superionic/low‐barrier regimes associated with ionic‐radius mismatch, electronegativity difference, configurational entropy, and mixing thermodynamics, while providing a more informative learning target than single‐value activation energies. Sensitivity analyses indicate that material‐level trends remain reasonably robust to variations in conductivity, reference temperature, and sampling density. Application to a reprocessed dataset of 160 compositions and 2,410 conductivity‐temperature entries across seven electrolyte families supports broader applicability. MND‐guided screening of 171 Li 10 Ge x Si y Sn z P 2 S 12 compositions prioritizes Li 10 Ge 0.3 Si 0.15 Sn 0.55 P 2 S 12 , which exhibits a room‐temperature conductivity of 7.21 mS cm − 1 , an apparent activation energy of 0.288 eV, and weak non‐Arrhenius behavior consistent with prediction. Evaluation of a second composition further supports the multistage screening strategy. These results position MND as a chemically interpretable representation for quantifying, learning, and screening temperature‐dependent ion transport.

Source: Angewandte Chemie International Edition

DOI: 10.1002/anie.4940262