Phase Composition, Density, and Ionic Conductivity of the Li₇La₃Zr₂O₁₂-Based Composites with LiPO₃ Glass Addition

Abstract

The glass-ceramic composite electrolytes based on tetragonal LiLaZrO (t-LLZ) and cubic Al-doped LiLaZrO (c-LLZ) with the LiPO glass additive have been prepared. The electrical conductivity and microstructure of the t-LLZ/LiPO and c-LLZ/LiPO composites have been investigated. The phase evolution of electrolytes has been studied using XRD, SEM, and Raman spectroscopy. It was indicated that the impurities formation depends on the composition of the composite. The phase composition of the solid electrolytes determines their thermal properties, which have been studied by the DSC method. The relative density of the obtained composite electrolytes was established to be higher than one of the sintered t-LLZ and c-LLZ. The Li conductivity of the t-LLZ-based composites gradually increased from 4.6 × 10 S cm (undoped t-LLZ) to 2.5 × 10 S cm (t-LLZ/5 wt % LiPO composite) at 25 °C. The highest total conductivity of the c-LLZ/LiPO composites has been achieved by introducing 1 wt % additive (0.11 mS cm at room temperature), whereas further doping resulted in the impurities formation.

Garnet Solid Electrolyte for Advanced All‐Solid‐State Li Batteries

“…[ 48,60 ] At the same time, adding sintering additives can decrease the sintering temperature to get stable c‐LLZO with high relative density, which is demonstrated by many reports. Li 4 SiO 4 , [ 61 ] Li 3 BO 3 , [ 62 ] Li 2 O, [ 63 ] LiPO 3 , [ 64 ] Li 2 O‐B 2 O 3 ‐SiO 2 , [ 65 ] La 2 Zr 2 O 7 , [ 66 ] and Li 2 O‐Y 2 O 3 ‐SiO 2 [ 67 ] were reported to be useful in decreasing the sintering temperature. To sum up, an ionic conductivity of 10 −3 –10 −4 S cm −1 can be obtained for the optimized LLZO electrolyte, which is considered to be enough to meet the requirement.…”

Impact of Li3BO3 Addition on Solid Electrode-Solid Electrolyte Interface in All-Solid-State Batteries

“…DSC curves of LTO and c-LLZ mixture with the same weight ratio were investigated to identify the possible products of their interaction, Figure 1. The endothermic peaks at ~250 and ~430 • C can be referred to as the removal of adsorbed water and CO 2 from the c-LLZ sample, respectively [45,46]. The endothermic peak at ~588 • C can be referred to the removal of lithium oxide leading to La 2 Zr 2 O 7 formation on the solid electrolyte powder surface, the reflections of which can be detected in the XRD patterns of the LTO and c-LLZ mixture annealed at temperatures above 600 • C, Figure 7a.…”

Constructing Stable Anodic Interphase for Quasi-Solid-State Lithium–Sulfur Batteries

“…Raman spectra are used to detect the phase composition and molecular structure in the range of 200-1200 cm −1 (Figure 5b), and the spectroscopy of LAGP is consistent with Pershina's analysis. 40,41 After 50 cycles, the LAGP/LE pellet presents several small impure peaks and two obvious peaks in 613 and 746 cm −1 except for peaks of bulk LAGP. As a comparison, the one with CuF 2 has no obvious change.…”