Computational Design of Electrode-Electrolyte Interfaces for Solid-State Lithium Ion Batteries

Abstract

All-solid-state lithium-ion batteries have attracted significant interest for their enhanced safety compared with conventional batteries employing an organic liquid electrolyte. However interfacial reactions between the electrodes and the electrolyte can increase the impedance of charge carrier transfer, degrading battery performance. In this work, we present a systematic high-throughput screening method to identify coatings for interfaces based on thermodynamic phase equilibria to maintain long-term interface stability during battery operation. Using Monte Carlo simulated ab initio phase diagrams, our approach can incorporate metastable phases in the coating materials screening and identify potential multi-layer coatings. We identified single- and double-layer coatings for 56 combinations of common electrode and electrolyte materials from existing databases of inorganic materials. Top protective coatings were further evaluated on their electrical resistance, ionic conductivity and electrochemical stability. Our work provides a general approach to mitigating interfacial reactions and optimizing battery performance by rational coating design.