Amorphous Li-La-Zr-O films are considered very attractive as a solid-state electrolyte in future batteries due to their low processing temperatures and resistance to Li-dendrite formation. The knowledge of amorphous Li-La-Zr-O phases is limited and thick films and bulk samples of amorphous Li-La-Zr-O have yet to be explored. Only thin film forms (~0.5 μm) of these amorphous Li-La-Zr-O phases have been prepared. In this work, we investigated the Li-ion transport properties of amorphous/crystalline mixtures of Li-La-Zr-Nb-O thick films (30 to 55 μm) prepared by the suspension plasma spray process. The process was manipulated to alter the amorphous Li-La-Zr-Nb-O content in the as-deposited films. Properties of the films that contained mostly amorphous Li-La-Zr-Nb-O (~76 wt%) were compared vs. mostly cubic Li garnet-type oxide (~55 wt%). The latter showed Li-ion transport properties that were similar to previously reported properties of cubic Li-garnet type oxides whereas the amorphous Li-La-Zr-Nb-O films exhibited significantly different properties. Their AC conductivity spectra show a Jonscher power law (JPL) behavior with the dimensionless exponent of ~0.92 that is followed by superlinear power law (SLPL) behavior with the dimensionless exponent of ~1.65 in the high frequency regime. These behaviors have not been reported earlier for the amorphous Li-La-Zr-Nb-O phases. Both of the JPL and SLPL behaviors have thermally activated characteristic with the activation energies of 0.76 eV and 0.64 eV, respectively. A lower value of ~0.45 eV was evaluated for the activation energy by solid-state ⁷Li NMR spectroscopy. The effect of temperature on the Li-ion dynamic process was studied by scaling the conductivity spectra and it was found to be temperature independent.

非晶 Li-La-Zr-O 薄膜因其低加工温度和抗锂枝晶形成而被认为是未来电池中非常有吸引力的固态电解质。非晶态 Li-La-Zr-O 相的知识是有限的，非晶态 Li-La-Zr-O 的厚膜和大块样品还有待探索。仅制备了这些非晶 Li-La-Zr-O 相的薄膜形式（~0.5 μm）。在这项工作中，我们研究了 Li-La-Zr-Nb-O厚的非晶/结晶混合物的锂离子传输特性通过悬浮等离子喷涂工艺制备的薄膜（30 至 55 μm）。操纵该过程以改变沉积薄膜中的无定形 Li-La-Zr-Nb-O 含量。将主要包含非晶 Li-La-Zr-Nb-O (~76 wt%) 的薄膜的性能与主要包含立方锂石榴石型氧化物 (~55 wt%) 的性能进行了比较。后者显示出的锂离子传输特性类似于先前报道的立方锂石榴石型氧化物的特性，而无定形 Li-La-Zr-Nb-O 薄膜表现出显着不同的特性。他们的交流电导谱显示了 Jonscher 幂律 (JPL) 行为，其无量纲指数约为 0.92，随后是超线性幂律 (SLPL) 行为，其在高频范围内的无量纲指数约为 1.65。对于非晶态 Li-La-Zr-Nb-O 相，这些行为之前没有报道过。JPL 和 SLPL 行为都具有热激活特性，激活能分别为 0.76 eV 和 0.64 eV。固态活化能评估为~0.45 eV的较低值⁷ Li 核磁共振波谱。通过缩放电导率光谱研究了温度对锂离子动态过程的影响，发现它与温度无关。