Publication date: 15th December 2025
Solid electrolyte-based batteries are seen as a new breakthrough technology to exceed by 50% the energy density of current Li-ion batteries, due to the use of lithium metal as negative electrode [1]. Sulfide solid electrolytes, and especially the argyrodite Li6PS5Cl, are the most considered candidates for this application, thanks to their good shaping ability and high ionic conductivity (>10-3 S/cm) [2]. However, they exhibit a narrow electrochemical stability window, causing their oxidation at its interface with most of common positive electrodes [3]. A Li+ ions blocking interphase then forms and causes a fast capacity loss that hinders the use of this electrolyte.
The approach of this work is to develop a highly conformal nanometer-thick coating on the Li6PS5Cl electrolyte, in order to prevent its decomposition on contact with the positive electrode, while allowing Li+ to cross this layer. These coatings are deposited using Atomic Layer Deposition (ALD), with a tool specially designed for powder deposition under pure argon atmosphere. Lithium phosphates (LixPyOz) coatings were chosen because of their electrochemical stability, ionic conduction and electronic insulation. This deposition is made following the process by Hämäläinen et al. using lithium hexamethyldisilazide (LiHMDS) and trimethyl phosphate (TMP) [4].
Silicon wafers were used as first-approach substrates to characterize the thin film synthesis. Ellipsometry, X-ray photoelectron spectroscopy (XPS) and scanning transmission electron microscopy (STEM) confirmed the controlled conformal growth of a Li3PO4 material at a rate of 0.6 Å/cycle. After demonstration of the stability of the solid electrolyte in ALD conditions, the first coatings could be synthesised on the targeted powder substrate. STEM-EDX imaging and XPS analysis revealed that the expected Li3PO4 layer was successfully obtained at various thicknesses on all particles. Together with electrochemical impedance spectroscopy (EIS), these characterizations provide valuable insights for a further integration of this coated argyrodite into all-solid-state-batteries.
The authors acknowledge support from the French state financial through the National Research Agency under reference ANR-22-PEBA-0004.
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