Stabilizing the Interface of NASICON Solid Electrolyte against Li Metal with Atomic Layer Deposition

Solid-state batteries have been considered as one of the most promising next-generation energy storage systems because of their high safety and energy density. Solid-state electrolytes are the key component of the solid-state battery, which exhibit high ionic conductivity, good chemical stability, and wide electrochemical windows. LATP [Li1.3Al0.3Ti1.7 (PO4)3] solid electrolyte has been widely investigated for its high ionic conductivity. Nevertheless, the chemical instability of LATP against Li metal has hindered its application in solid-state batteries. Here, we propose that atomic layer deposition (ALD) coating on LATP surfaces is able to stabilize the LATP/Li interface by reducing the side reactions. In comparison with bare LATP, the Al2O3-coated LATP by ALD exhibits a stable cycling behavior with smaller voltage hysteresis for 600 h, as well as small resistance. More importantly, on the basis of advanced characterizations such as high-resolution transmission electron spectroscope-electron energy loss spectroscopy, the lithium penetration into the LATP bulk and Ti4+ reduction are significantly limited. The results suggest that ALD is very effective in improving solid-state electrolyte/electrode interface stability.