Organic-inorganic interface in composite solid electrolyte could lead to increased ion transport for solid-state lithium batteries; however, most inorganic fillers have much larger size than polymer chains, which results in severe aggregation of inorganic fillers and poor ionic conductivity. Herein, functional sub-1 nm inorganic cluster chains were integrated with polymer chains to fabricate composite solid electrolyte with enhanced ionic conductivity. Different from all other inorganic fillers, the sub-1 nm inorganic cluster chains with diameter <1 nm have similar size and geometry compared with polymer chains, exhibiting polymer-like solution properties. A transparent sub-1 nm inorganic filler/polymer mixed solution was generated to realize monodispersion of cluster chains as functional fillers in polymer matrix. Meanwhile, abundant oxygen vacancies on cluster chains interact with polymer chains and lithium salts at molecular-scale, which decreases the complexation of polymer segments with Li and promote the dissociation of lithium salts, thereby improving Li transport. As a result, the composite solid electrolyte exhibits high ionic conductivity (0.4 mS cm) and large mobile Li distribution (50.8 %). This work pushes the size of nanofillers down to <1 nm, which is a unique approach to the molecular-scale interaction between nanofillers and polymers to boost ion transport in solid electrolytes.

中文翻译：

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亚1纳米簇链与高性能固体电解质聚合物之间的分子尺度相互作用

复合固体电解质中的有机-无机界面可以增加固态锂电池的离子传输；然而，大多数无机填料的尺寸远大于聚合物链，这导致无机填料严重聚集，离子电导率较差。在此，功能性亚1纳米无机簇链与聚合物链集成，以制造具有增强离子电导率的复合固体电解质。与所有其他无机填料不同，直径<1 nm的亚1 nm无机簇链与聚合物链相比具有相似的尺寸和几何形状，表现出类似聚合物的溶液特性。生成透明的亚1纳米无机填料/聚合物混合溶液，以实现簇链作为功能填料在聚合物基体中的单分散。同时，簇链上丰富的氧空位在分子尺度上与聚合物链和锂盐相互作用，减少了聚合物链段与锂的络合，促进了锂盐的解离，从而改善了锂的传输。结果，复合固体电解质表现出高离子电导率（0.4 mS cm）和大的移动锂分布（50.8％）。这项工作将纳米填料的尺寸降低至<1 nm，这是纳米填料和聚合物之间分子级相互作用以促进固体电解质中离子传输的独特方法。