New Insights into the Compositional Dependence of Li-Ion Transport in Polymer–Ceramic Composite Electrolytes,ACS Applied Materials & Interfaces

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New Insights into the Compositional Dependence of Li-Ion Transport in Polymer–Ceramic Composite Electrolytes
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2018-01-16 00:00:00 , DOI: 10.1021/acsami.7b17301
Jin Zheng ₁ , Yan-Yan Hu _{1,

2}

Affiliation

Composite electrolytes are widely studied for their potential in realizing improved ionic conductivity and electrochemical stability. Understanding the complex mechanisms of ion transport within composites is critical for effectively designing high-performance solid electrolytes. This study examines the compositional dependence of the three determining factors for ionic conductivity, including ion mobility, ion transport pathways, and active ion concentration. The results show that with increase in the fraction of ceramic Li₇La₃Zr₂O₁₂ (LLZO) phase in the LLZO–poly(ethylene oxide) composites, ion mobility decreases, ion transport pathways transit from polymer to ceramic routes, and the active ion concentration increases. These changes in ion mobility, transport pathways, and concentration collectively explain the observed trend of ionic conductivity in composite electrolytes. Liquid additives alter ion transport pathways and increase ion mobility, thus enhancing ionic conductivity significantly. It is also found that a higher content of LLZO leads to improved electrochemical stability of composite electrolytes. This study provides insight into the recurring observations of compositional dependence of ionic conductivity in current composite electrolytes and pinpoints the intrinsic limitations of composite electrolytes in achieving fast ion conduction.

中文翻译：

聚合物-陶瓷复合电解质中锂离子输运组成依赖性的新见解

复合电解质在实现改善的离子电导率和电化学稳定性方面的潜力得到了广泛的研究。了解复合物中离子传输的复杂机制对于有效设计高性能固体电解质至关重要。这项研究检查了三个决定性因素对离子电导率的成分依赖性，包括离子迁移率，离子迁移途径和活性离子浓度。结果表明，随着陶瓷Li ₇ La ₃ Zr ₂ O ₁₂含量的增加，LLZO-聚环氧乙烷复合材料中的（LLZO）相，离子迁移率降低，离子传输路径从聚合物迁移到陶瓷路径，并且活性离子浓度增加。离子迁移率，传输途径和浓度的这些变化共同解释了复合电解质中观察到的离子电导率趋势。液体添加剂可改变离子传输途径并增加离子迁移率，从而显着提高离子电导率。还发现较高的LLZO含量可改善复合电解质的电化学稳定性。这项研究提供了对当前复合电解质中离子电导率组成依赖性反复观察的见解，并指出了复合电解质在实现快速离子传导方面的固有局限性。

更新日期：2018-01-16

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