Surface orientation-dependent adhesion behavior in Na-cathode and solid- state electrolyte interfaces using machine learning interatomic potential

W Shin and J Kim and J Sun and J Hwang and J Kim and K Min, JOURNAL OF POWER SOURCES, 653, 237670 (2025).

DOI: 10.1016/j.jpowsour.2025.237670

The interfacial adhesion between the cathode and solid-state electrolyte (SSE) presents a critical hurdle in the advancement of all-solid-state sodium-ion batteries, directly impacting structural integrity and long- term cycling performance. This study investigates the adhesion characteristics of the cathode/SSE interface via Steered Molecular Dynamics (SMD) simulations, leveraging the accuracy of Machine Learning Interatomic Potentials (MLIP). Specifically, we selected Na3Zr2Si2PO12 (NZSP) and O3-NaNi0.5Mn0.5O2 as representative SSE and cathode materials, respectively, owing to their demonstrated chemical and electrochemical stability. Four distinct interfacial configurations were systematically constructed by pairing two crystallographically different surfaces from each material. MLIP-SMD simulations were employed to quantify interfacial adhesion by computing the maximum force, work of adhesion, and separation distance. The results reveal that the Cathode (100)/SSE(100) interface exhibits superior adhesion, characterized by a significantly increased separation distance and work of adhesion, compared to other configurations. These findings underscore the paramount influence of surface crystallographic orientation on the mechanical stability of the cathode-electrolyte interface, offering crucial insights for the rational design of mechanically robust interfaces in solid-state sodium-ion batteries.

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