A Facile Two-Step Thermal Process for Producing a Dense, Phase-Pure, Cubic Ta-Doped Lithium Lanthanum Zirconium Oxide Electrolyte for Upscaling

Abstract

An inorganic solid electrolyte is the most favorable candidate for replacing flammable liquid electrolytes in lithium batteries. Lithium lanthanum zirconium oxide (LLZO) is considered a promising solid electrolyte due to its safe operating potential window (0–5 V) combined with its good electrochemical stability. In this work, 250 g batches of pre-sintered Ta-doped LLZO (Li7La3Zr1.6Ta0.4O12, Ta-LLZO) were synthesized for bulk production of a dense LLZO electrolyte. A simple two-step thermal treatment process was developed. The first thermal step at 950 °C initiates nucleation of LLZO, with carefully controlled process parameters such as heating atmosphere, temperature, and dopant concentration. In the second thermal step at 1150 °C, sintered discs were obtained as solid electrolytes, with relative densities of 96%. X-ray diffraction analysis confirmed the phase purity of the sintered Ta-LLZO disc, and refined data were used to calculate the lattice parameter (12.944 Å). Furthermore, the presence of the Ta dopant in the disc was confirmed through X-ray photoelectron spectroscopy (XPS) analysis. The ionic and electronic conductivity values of the Ta-LLZO disc were 10−4 S cm−1 and 10−10 S cm−1, respectively. These values confirm that the prepared (Ta-LLZO) discs exhibit ionic conductivity while being electronically insulating, being suitable for use as solid electrolytes with the requisite electrical properties.

Keywords

• solid electrolyte
• lithium batteries
• LLZO
• solid-state batteries
• lithium metal