Comparison of computational methods for the electrochemical stability window of solid-state electrolyte materials

Abstract

Superior stability and safety are key promises attributed to all-solid-state batteries (ASSBs) containing solid-state electrolyte (SSE) compared to their conventional counterparts utilizing liquid electrolyte. To unleash the full potential of ASSBs, SSE materials that are stable when in contact with the low and high potential electrodes are required. The electrochemical stability window is conveniently used to assess the SSE-electrode interface stability. In the present work, we review the most important methods to compute the SSE stability window. Our analysis reveals that the stoichiometry stability method represents a bridge between HOMO-LUMO method and phase stability method (grand canonical phase diagram). Moreover, we provide computational implementations of these methods for SSE material screening. We compare their results for the relevant Li- and Na-SSE materials LGPS, LIPON, LLZO, LLTO, LATP, LISICON, and NASICON, and we discuss their relation to published experimental stability windows.

References in corpus (6)

• Optimized norm-conserving Vanderbilt pseudopotentials
• Optimization Algorithm for the Generation of ONCV Pseudopotentials
• Thermal Contraction and Disordering of the Al(110) Surface
• Precision and efficiency in solid-state pseudopotential calculations
• Understanding Band Gaps of Solids in Generalized Kohn-Sham Theory
• AiiDA: Automated Interactive Infrastructure and Database for Computational Science

Cited by in corpus (3)

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