目前，智能电子、电动汽车等领域对储能产品的需求不断增长。为进一步满足市场需求，开发具有优异机械/热稳定性以及高功率和高能量密度的新型可充电电池成为必然趋势。锂离子电池（LIBs）因高能量密度、长循环稳定性和高输出功率等优点被广泛应用在日常电子产品中。虽然传统 LIBs 在室温下表现出低界面电阻和良好的离子电导率，然而，由于电解液的泄漏和挥发以及不可逆的容量衰减导致的热稳定性差和易燃爆等安全问题亟待解决。因此，基于固体电解质的LIBs因其高安全性的优势成为极具潜力的下一代可充电电池。然而，制造出具有低界面电阻、高电导率和能抑制锂枝晶的固体电解质仍然是一个长期存在的挑战。本论文提出，将核壳金属有机框架（MOF）纳米粒子用于固体电解质，以促进Li⁺的传输，并提高固态电解质对电极的电化学稳定性。与原始MOF材料相比，核壳MOF纳米颗粒作为固体电解质时在离子传输方面具有明显优势。同时，系统研究并揭示了每种电解质的离子传输机理。主要发现如下：

1. 使用联苯二甲酸（H₂-BPDC）作为连接体，制备了核壳型MOF-in-MOF纳米粒子UIO-66@67，该材料用途广泛并展现出在储能领域实际应用的可能性。该研究工作旨在检验UIO-66@67作为一种独特的双功能电解质主体，能够提高固体电解质的离子电导率、Li⁺迁移数和界面稳定性。

2. 核壳UIO-66@67作为锂离子电池中一种吸附离子液体的主体材料。核壳UIO-66@67/锂离子液体（CSIL）设计中的壳结构（UIO-67）具有较大的比表面积和较大的孔径，可促进离子液体（IL）电解液的吸收，从而提高锂离子电导率。与IL离子尺寸相比，UIO-66结构的孔径更小，能够捕获体积较大的阴离子，限制阴离子的运动并促进Li⁺的迁移。CSIL的新颖结构设计使其能够实现高Li⁺迁移数(0.63)，展现优异的离子电导率（2.1×10^-3 S cm^-1）和高初始容量（158 mAh g^-1），在25 °C下循环100次后其容量保持率为99%。此外，基于CSIL的Li对称电池在1000 µA cm^-2下循环1000小时后仍保持28 mV的稳定极化。

3. 通过控制纳米粒子的形状首次合成了一种新型仿生类脑纳米结构（BBLN）固体聚合物电解质。与传统的聚合物基复合电解质相比，这种BBLN固体聚合物电解质的制备是在聚合物电解质中加入球形核壳（UIO-66@67）填料，该球形UIO-66@67填料有利于消除聚合物电解质在凝固过程中的应力和变形，赋予BBLN固体聚合物电解质高度均匀的连续结构，应用潜力巨大。此外，球形UIO-66@67纳米粒子可显著降低聚合物电解质的结晶度，增强聚合物链的分段运动，为快速离子转移提供连续输运路径。该工作中制备的BBLN聚合物电解质表现出优异的离子电导率（9.2×10^-4 S cm^-1）、高锂离子迁移数（0.74）和优异的锂电极循环稳定性（室温下稳定超过6500小时）。此外，基于BBLN固体聚合物电解质组装的LIBs在25 °C下循环200次后表现出155 mAh g^-1的优异容量。

4. 通过调控掺入纳米颗粒的密度合成了一种新型的异质多层结构固体电解质（HLSE）。与传统的聚合物基复合电解质相比，这种HLSE是将球形核壳UIO-66@67和无机陶瓷LLZO填料加入到聚合物电解质中制备而成。一方面，球形UIO-66@67纳米粒子利于消除聚合物电解质在凝固过程中的应力和变形，增强锂离子的迁移效率；另一方面，LLZO纳米粒子的引入可以提高固体聚合物电解质的机械强度，抑制锂枝晶的生长。因此，本工作所制备的HLSE表现出优异的离子电导率（7.1×10^-4 S cm^-1）、高锂迁移数（0.65），在室温1600 µA cm^-2电流密度下锂-锂循环超过1650次。基于HLSE组装的LIB在25 °C循环125次后比容量仍保持在159 mAh g^-1。

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