With the increasing demand for higher energy density Lithium-ion batteries, the battery safety issue has gained growing attention. Solid-state electrolytes (SSEs) are considered a promising solution to the volatilization and inflammable problems of the traditional liquid electrolytes. In this work, we propose a novel solvent-free modification process using stearic acid as a modifying agent for LLZTO/PEO hybrid electrolytes. Compared to the conventional solvent-casting process, the new one integrates surface modification and composite in a successive solvent-free step, so it can greatly improve the process efficiency and meet the requirement of green chemistry. Fourier Transform Infrared spectrometry (FTIR), X-Ray Diffraction (XRD) and Transmission Electron Microscope (TEM) observation confirm the structure of the uniform coating layer. The solvent-free modification and composite process are proved to significantly inhibit the agglomeration of LLZTO particles and the side reactions on particle surfaces in the polymer matrix by using Scanning Electron Microscope (SEM) and Thermal Gravimetric-Differential Thermal Analysis (TG-DTA) characterization. Thus, the prepared electrolyte has the ionic conductivity of up to 8.3 × 10⁻⁴ S cm⁻¹ at 70 °C. It has better electrochemical stability as well, which can achieve about 900 cycles in Li symmetric cells with a current density of 0.1 mA cm⁻².

随着对更高能量密度的锂离子电池的日益增长的需求，电池安全问题日益受到关注。固态电解质（SSE）被认为是解决传统液态电解质挥发和易燃问题的有前途的解决方案。在这项工作中，我们提出了一种使用硬脂酸作为LLZTO / PEO混合电解质的改性剂的新型无溶剂改性方法。与传统的溶剂浇铸工艺相比，该新工艺在连续的无溶剂步骤中整合了表面改性和复合材料，因此可以大大提高工艺效率并满足绿色化学的要求。傅里叶变换红外光谱（FTIR），X射线衍射（XRD）和透射电子显微镜（TEM）的观察证实了均匀涂层的结构。通过扫描电子显微镜（SEM）和热重差热分析（​​TG-DTA）表征，证明了无溶剂改性和复合工艺可显着抑制LLZTO颗粒的团聚和聚合物基质中颗粒表面的副反应。 。因此，制备的电解质具有高达8.3×10的离子电导率在70°C下为^-4  S cm ^-1。它还具有更好的电化学稳定性，在电流密度为0.1 mA cm ^-2的Li对称电池中可以实现约900次循环。