Abstract Solid electrolytes could address the increasingly urgent safety and energy density concerns of lithium-ion batteries. Among several kinds of solid electrolytes, Ta-doped Li7La3Zr2O12 (Ta-LLZO) became a research hotspot because of its high Li-ion conductivity and chemical stability against Li-metal and air. However, the preparation of high quality LLZO ceramic electrolyte via conventional air ambient sintering method is still a big challenge due to the serious “Li-loss” and abnormal grain growth phenomenon during the long-time high-temperature sintering process. Herein, a new rapid ultra-high-temperature air ambient sintering method without mother powder (MP) is put forward for the preparation of high quality Ta-LLZO ceramic electrolyte. The rapid sintering strategy can effectively restrain “Li-loss”. Furthermore, it is demonstrated that the none-mother-powder method is superior to traditional mother-powder method. Ta-LLZO ceramics sintered without MP via this rapid sintering method own small grain size, tight grain boundary, dense microstructure and high conductivity. Specifically, the Ta-LLZO ceramic sintered at 1360 °C for 10 min without MP exhibits high conductivity (8.5 × 10−4 S cm−1 at 25 °C) and high relative density (97%), which equate those made by hot pressing sintering method. Without MP, the sintering process can avoid a lot of material waste and simplify the operation process. Moreover, the rapid sintering process can sharply shorten sintering time and reduce energy consumption. Therefore, this low-cost high-efficient sintering strategy can be effectively used in the large-scale production of high-quality Ta-LLZO ceramic electrolyte.

中文翻译：

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高导电Li7La3Zr2O12陶瓷电解质的快速烧结方法

摘要 固体电解质可以解决锂离子电池日益紧迫的安全性和能量密度问题。在多种固体电解质中，Ta掺杂的Li7La3Zr2O12（Ta-LLZO）因其高锂离子电导率和对锂金属和空气的化学稳定性而成为研究热点。然而，由于长时间高温烧结过程中存在严重的“Li损失”和异常晶粒长大现象，通过传统的空气环境烧结方法制备高质量的LLZO陶瓷电解质仍然是一个很大的挑战。在此，提出了一种无需母粉（MP）的快速超高温空气常温烧结新方法，用于制备高质量的Ta-LLZO陶瓷电解质。快速烧结策略可以有效抑制“Li-loss”。此外，证明无母粉法优于传统母粉法。通过这种快速烧结方法在无 MP 的情况下烧结的 Ta-LLZO 陶瓷具有晶粒小、晶界紧密、微观结构致密和高电导率的特点。具体而言，Ta-LLZO 陶瓷在没有 MP 的情况下在 1360°C 下烧结 10 分钟表现出高电导率（25°C 时为 8.5 × 10−4 S cm−1）和高相对密度（97%），这与热制造的陶瓷相当压制烧结法。没有MP，烧结过程可以避免大量的材料浪费，简化操作过程。此外，快速烧结工艺可以大幅缩短烧结时间，降低能耗。因此，这种低成本高效的烧结策略可以有效地用于大规模生产高质量的Ta-LLZO陶瓷电解质。