A Master Key for Accessible Solid Electrolyte Design

ChemRxiv

Abstract

The solid electrolyte design currently relies on heuristic approaches, lacking a unified framework to correlate atomistic lattice features with the accessible bulk ion transport properties. Nor could the rich literature be interpreted consistently to provide a definitive perspective on new solidelectrolyte engineering by design, with refined composition and lattice information. To address these needs and challenges, here we found a master key (Fig. S1), opening a door for accessible solid electrolyte design by encoding the composition-structure-property relationship validated by Li 10 GeP 2 S 12 (LGPS) and Li 4 GeS 4 (thio-LISICON) solid electrolytes with a new concept called “intrinsic lattice formation strain” (ILFS) (Fig. 1), which originates from the chemical bond formation and lattice relaxation from perfect symmetry of the unit cell. The master key uses Gibbs free energy terms expressed in ILFS to describe the ion transport properties of solid electrolytes that follow the Arrhenius law, correlating the experimental composition-structure-property trends across the open-literature sulfide solid electrolyte database with R 2 > 0.90 for LGPS and > 0.86 for thio-LISICON, respectively. The master key thus offers an intelligent pathway to guide new solid electrolyte design and discovery.

Authors 4

1. Han Zhou Aachen Institute of Physical Chemistry

   RWTH Aachen University · Forschungszentrum Jülich

   Affiliation as printed

   Institute of Energy Technologies -Fundamental Electrochemistry (IET-1) , Forschungszentrum Jülich , 52428 Jülich , Germany

   Institute of Physical Chemistry , RWTH Aachen University , 52074 Aachen , Germany

2. Shicheng Yu

   Forschungszentrum Jülich

   Affiliation as printed

   Institute of Energy Technologies -Fundamental Electrochemistry (IET-1) , Forschungszentrum Jülich , 52428 Jülich , Germany

3. Bor Yann Liaw

   Forschungszentrum Jülich

   Affiliation as printed

   High Power Research Laboratory , LLC , Idaho Falls , ID 83404 , USA

   Institute of Energy Technologies -Fundamental Electrochemistry (IET-1) , Forschungszentrum Jülich , 52428 Jülich , Germany

4. Rüdiger‐A. Eichel