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NASICON-type solid electrolytes with excellent stability in moisture are promising in all-solid-state batteries and redox flow batteries. However, NASIOCN LiZr 2 (PO 4 ) 3  (LZP), which is more stable with lithium metal than the commercial Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 , exhibits a low Li-ion conductivity of 10 −6  S cm −1  because the fast conducting rhombohedral phase only exists above 50 °C. In this paper, the high-ionic conductive rhombohedral phase is stabilized by Y 3+  doping at room temperature, and the hot-pressing technique is employed to further improve the density of the pellet. The dense Li 1.1 Y 0.1 Zr 1.9 (PO 4 ) 3  pellet prepared by hot-pressing shows a high Li-ion conductivity of 9 × 10 −5  S cm −1 , which is two orders of magnitude higher than that of LiZr 2 (PO 4 ) 3 . The in-situ formed Li 3 P layer on the surface of Li 1.1 Y 0.1 Zr 1.9 (PO 4 ) 3  after contact with the lithium metal increases the wettability of the pellet by the metallic lithium anode. Moreover, the Li 1.1 Y 0.1 Zr 1.9 (PO 4 ) 3  pellet shows a relatively small interfacial resistance in symmetric Li/Li and all-solid-state Li-metal cells, providing these cells a small overpotential and a long cycling life.

Rhombohedral Li1+xYxZr2-x(PO4)3 Solid Electrolyte Prepared by Hot-Pressing for All-Solid-State Li-Metal Batteries