Li$_{14}$Mn$_{2}$S$_{9}$ and Li$_{10}$Si$_{2}$S$_{9}$ as a pair of all-electrochem-active electrode and solid-state electrolyte with chemical compatibility and low interface resistance

TL;DR

This paper introduces a compatible pair of all-electrochem-active electrode and solid-state electrolyte, Li$_{14}$Mn$_{2}$S$_{9}$ and Li$_{10}$Si$_{2}$S$_{9}$, designed to improve interface stability in solid-state batteries through computational validation.

Contribution

It proposes a novel pair of structurally compatible AEA-electrode and SSE with confirmed interface stability using advanced simulations.

Findings

Confirmed chemical compatibility via AIMD simulations.

Validated interface stability with MLIP-based MD simulations.

Provides a new approach for stable solid-state battery interfaces.

Abstract

In solid-state batteries (SSBs), improving the physical contact at the electrode-electrolyte interface is essential for achieving better performance and durability. On the one hand, it is necessary to look for solid-state electrolytes (SSEs) with high ionic conductivity and no reaction with the electrode, on the other hand, to design the all-electrochem-active (AEA) electrodes that contain no SSEs and other non-active substances. In this work, we proposed a pair of AEA-electrode and SSE with the same structural framework and excellent interface compatibility, Li$_{14}$Mn$_{2}$S$_{9}$ and Li$_{10}$Si$_{2}$S$_{9}$, and confirmed the feasibility by ab-initio molecular dynamics (AIMD) simulations and machine learning interatomic potential based molecular dynamics (MLIP-based MD) simulations, providing a new approach to promote interfacial stability in SSBs.