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    元素钇掺杂对Li3InCl6 卤化物电解质性能的影响

    Impact of doping of yttrium elements on the performance of Li3InCl6 electrolyte

    • 摘要: 新型卤化物固态电解质的开发是当今能源电化学领域的一个研究热点,如何进一步提高离子电导率和界面相容性,是卤化物电解质开发所面对的两大技术挑战。本文针对Li3InCl6(LIC)卤化物电解质与锂金属负极界面相容性差的问题开展研究。采用高能球磨结合后退火法制备了一系列元素钇(Y)掺杂改性的新型卤化物电解质(Li3In1-xYxCl6(0≤x≤0.5))。通过X射线衍射(XRD)、扫描电子显微镜(SEM)、差示扫描量热(DSC)、热重分析(TGA)、电化学阻抗谱(EIS)、直流极化(DC)、线性扫描伏安(LSV)及对称/全电池充放电循环测试等方法,系统地探究了元素(Y)掺杂对Li3InCl6电解质的晶体结构、热稳定性、离子/电子电导率及其与锂金属负极界面稳定性等性能的影响机制。研究结果表明:掺杂适量的元素Y,虽然使得Li3InCl6电解质的室温离子电导率有所降低,但会显著地降低Li3InCl6 电解质的电子电导率,提升Li3InCl6 电解质的热稳定性和电化学稳定性,特别是明显地改善了Li3InCl6 电解质与金属锂之间的界面相容性,提高了全固态电池的长循环性能。本研究为设计高稳定性卤化物固态电解质,提供了一种有效的技术改进策略。

       

      Abstract: The development of new halide solid-state electrolyte is a research hotspot in the field of energy electrochemistry. Low ionic conductivity and poor interfacial compatibility are two major technical challenges for the exploitation of halide electrolyte. This work has focused on how to further improve the interface compatibility between the halide electrolyte of Li3InCl6 (LIC) and Li anode. A series of new kinds of halide electrolyte (Li3In1-xYxCl6 (0≤x≤0.5)) doped with yttrium element (Y) have been prepared by high-energy ball milling combined with annealing process subsequently. The mechanisms of element (Y) doping on Li3InCl6 electrolyte, including the crystal structure, thermal stability, ionic/electronic conductivity and interface compability with Li anode, are systematically explored. The testing methods contain X-ray diffraction (XRD), scanning electron microscopy (SEM), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), electrochemical impedance spectroscopy (EIS), direct current polarization (DC), linear scanning voltammetry (LSV), and charge/discharge tests of the symmetrical/full batteries. The research results show that doping of Y element may reduce the room-temperature ionic conductivity of the Li3InCl6 electrolyte to some extent. However, incorporating an appropriate amount of Y element into Li3InCl6 electrolyte can lower its electronic conductivity, enhancing its thermal stability and electrochemical stability availably. It has significantly promoted the interface compatibility between Li3InCl6 electrolyte and Li anode by doping of Y element, enhancing the long-cycle performance of all-solid-state lithium batteries. This study provides an effective improvement strategy for designing highly stable halide electrolytes.

       

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