Abstract
NASICON-type solid electrolytes with excellent stability in moisture are promising in all-solid-state batteries and redox flow batteries. However, NASIOCN LiZr2(PO4)3 (LZP), which is more stable with lithium metal than the commercial Li1.3Al0.3Ti1.7(PO4)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 Y3+ doping at room temperature, and the hot-pressing technique is employed to further improve the density of the pellet. The dense Li1.1Y0.1Zr1.9(PO4)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 LiZr2(PO4)3. The in-situ formed Li3P layer on the surface of Li1.1Y0.1Zr1.9(PO4)3 after contact with the lithium metal increases the wettability of the pellet by the metallic lithium anode. Moreover, the Li1.1Y0.1Zr1.9(PO4)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.
Highlights
Rechargeable Li-metal batteries with a high-voltage cathode and Li-metal as an anode have much higher energy density than conventional rechargeable Li-ion batteries with a graphite anode
Research on solid electrolytes is focusing on polymer electrolytes, ceramic electrolytes, and polymer/composite electrolytes
The X-ray diffraction (XRD) patterns of as-synthesized powders in a regular box furnace were compared in Figure 1a; dopant-free LiZr2 (PO4 )3 exhibited a monoclinic phase at room temperature, which is consistent with a previous report [46]
Summary
Rechargeable Li-metal batteries with a high-voltage cathode and Li-metal as an anode have much higher energy density than conventional rechargeable Li-ion batteries with a graphite anode. Developing all-solid-state Li-metal batteries by replacing the liquid electrolyte with a high Li-ion conductive solid-state electrolyte is one of the most effective strategies to improve the safety and energy density of the batteries. M = Al, Ge) [20,21,22,23,24,25,26], perovskite-type (e.g., Li3x La(2/3)−x (1/3)−2x TiO3 ) [27,28,29,30,31], and antiperovskite-type electrolytes (e.g., Li2 OHX, X = Cl, Br) [32,33,34,35,36,37,38] have been reported to have high Li-ion conductivities at room temperature because of the suitable Li-ion transport channel inside the framework. Replacing the Ti4+ by other stable metal ions may improve the stability of the perovskite and NASICON electrolytes with lithium metal. The XPS depth profiles revealed that a passivation layer with a thickness of less than 100 nm formed on the surface of the pellet, which improved the cycling of the symmetric cell
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