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固态锂电池因其高能量密度和安全性成为新一代关键储能技术。复合固态电解质作为较具商业化前景的固态电解质，其性能突破是促进固态锂电池发展的关键。层状结构硅酸盐矿物因具有独特的纳米结构、高比表面积和可控的化学性质，在提升复合固态电解质的离子电导率、力学性能和界面稳定性方面展现出巨大潜力。本文首先系统探讨了层状结构硅酸盐矿物的结构特性及其功能化对复合固态电解质的离子传输、界面稳定及力学性能等性能的影响；深入分析了层状结构硅酸盐矿物晶体结构、微观形貌及表界面性质对复合固态电解质离子迁移机制、力学性能增强机制及界面稳定性调控机制的影响规律。在此基础上，综述了近年来层状结构硅酸盐矿物及其功能化改性在复合固态电解质领域中的最新研究进展。最后，基于对现有研究的系统梳理与综合分析，归纳了当前层状结构硅酸盐矿物复合固态电解质研究存在的关键科学问题与技术挑战，提出了未来研究重点与发展方向，旨在为高性能层状结构硅酸盐矿物复合固态电解质的设计与应用提供科学依据和技术参考。
Abstract：Solid-state lithium batteries(SSLBs) represent a transformative advancement in energy storage technology, playing a pivotal role in achieving global “dual carbon” goals. These batteries also offer a significant breakthrough in overcoming the energy density and safety limitations inherent in conventional lithium-ion batteries. Unlike conventional liquid electrolytes, solid electrolytes mitigate some critical issues such as electrolyte leakage and flammability, thus substantially enhancing the safety of SSLBs. Among various solid-state electrolyte candidates, composite solid electrolytes(CSEs) have attracted much attention due to their potential for commercial viability. Nevertheless, three major challenges remain to be addressed for the practical application of CSEs, i.e.,(ⅰ) limitations in ionic conduction dynamics. Most CSEs exhibit room-temperature ionic conductivities ranging from 10-6 to 10-3 S·cm-1, which are one to three orders of magnitude lower than those of liquid electrolytes(i.e., ～10-2 S·cm-1), severely restricting the rate and low-temperature performance of SSLBs;(ⅱ) poor mechanical properties. Despite some CSEs possessing high Young's moduli, localized current concentration at micro-defects can lead to lithium dendrite formation and propagation, posing a significant risk of internal short circuits; and(ⅲ) solid–solid interfacial compatibility issues. Physical defects and chemical side reactions at the electrode–CSE interface can lead to continuous increases in interfacial impedance, thereby compromising the cycle life and stability of SSLBs. Layered silicate minerals, including montmorillonite, attapulgite, and halloysite, are naturally occurring silicates with unique nanoscale structures. These minerals are abundant, cost-effective, and readily available in regions such as China. Layered silicates present a substantial potential for enhancing the ionic conductivity, mechanical properties, and interfacial stability of CSEs due to their high specific surface area, tunable chemical properties, and distinct nano-structural characteristics. This review systematically explores the structural characteristics of layered silicate minerals and their functionalization strategies to enhance ion transport, interfacial stability, and mechanical properties within CSEs. The crystal structures, micro-morphologies, and surface/interface properties of layered silicates affect ion migration mechanisms, reinforcement of mechanical properties, and regulation of interfacial stability in composite electrolytes. In addition, the review also represents recent advancements on utilizing layered silicate minerals and their functional modifications for improving CSEs. Layered silicate minerals offer several unique advantages in CSEs, i.e.,(ⅰ) Their unique structural properties provide excellent pathways for ion conduction, with some even exhibiting inherent ion-conductive behavior;(ⅱ) As inorganic fillers, they promote the dissociation of lithium salts through Lewis acid-base interactions, while suppressing polymer crystallization, significantly boosting the ionic conductivity of the composite electrolyte; and(ⅲ) The high modulus and thermal stability of layered silicate minerals improve the mechanical properties and thermal stability of CSEs. Summary and Prospects Layered silicate mineral-based composite solid electrolytes have an immense potential for advancing solid-state battery technologies. However, several scientific and technical challenges remain. First, the complexity of material composition and structural stability are key factors that restrict the performance. Variations in the batch-to-batch properties of layered silicate minerals result in compositional inhomogeneity. Furthermore, their high surface energy leads to agglomeration, disrupting ion conduction channels and stress distribution, which negatively impacts ionic conductivity and interfacial compatibility. The presence of impurities in the minerals, which are difficult to eliminate, may also induce side reactions that degrade the electrolyte-electrode interface, hindering performance improvement. Second, ion transport in these materials is constrained by small interlayer spacings and suboptimal interface compatibility, leading to a low ionic conductivity at room and low temperatures. This limits the realization of high conductivity. Moreover, the trade-off between mechanical properties and ionic conductivity complicates the simultaneous enhancement. The electrolyte stability under extreme conditions(such as low temperatures and high-voltage environments) is also a challenge. Polymer crystallization and interlayer contraction at low temperatures significantly reduce conductivity, while high-voltage conditions lead to electrolyte decomposition and electrode compatibility issues. To overcome these challenges, a future research should focus on the following aspects, i.e., ⅰ) Multistage purification and interface modification to address heterogeneity and agglomeration, improving ionic conductivity and stability through interdisciplinary collaboration; ⅱ) Control of interlayer spacing and surface modification, using ionic liquids and silane coupling agents to expand interlayer spacing and enhance interface properties, thereby improving ion transport efficiency; ⅲ) Design of three-dimensional network structures, integrating layered silicate minerals with various morphologies to construct ordered 3D networks, enhancing both the mechanical and electrochemical properties of the composite material; ⅳ) Extreme-condition adaptability, developing stable electrolytes for low-temperature and high-voltage environments through functionalization and additive optimization; and ⅴ) Scalable, environmentally friendly fabrication techniques, such as water-based dispersion and UV curing, to reduce production costs and improve batch-to-batch consistency. Layered silicate mineral-based composite solid electrolytes will play a crucial role in the development of solid-state battery technologies and accelerate their commercialization via advancing research in these aspects.
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基本信息:
DOI：10.14062/j.issn.0454-5648.20250510
中图分类号:O646;TM912
引用信息:
[1]张建强,韩文强,杨燕飞,等.层状结构硅酸盐矿物基复合固态电解质研究进展[J].硅酸盐学报,2025,53(12):3634-3649.DOI:10.14062/j.issn.0454-5648.20250510.
基金信息:
国家自然科学基金（22305255,22275200）; 甘肃省拔尖领军人才; 甘肃省重点研发计划-工业领域（25YFGA010）