Nanostructured, uncharged liquid-crystalline (LC) electrolyte molecules having bicyclohexyl and cyclic carbonate moieties have been developed for application in Li-ion batteries as quasi-solid electrolytes, which suppress leakage and combustion. Towards the development of safe and high performance Li-ion batteries, we have designed Li-ion conductive LC materials with high oxidation resistance using density functional theory (DFT) calculation. The DFT calculation suggests that a mesogen with a bicyclohexyl moiety is suitable for the high-oxidation-resistance LC electrolytes compared to a mesogen containing phenylene moieties. A tri(oxyethylene) chain introduced between the cyclic carbonate and the bicyclohexyl moiety in the core part tunes the viscosity and the miscibility with Li salts. The designed Li-ion conductive LC molecules exhibit smectic LC phases over a wide temperature range, and they are miscible with added lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt up to 5 : 5 in molar ratio in their smectic phases. The resulting LC mixtures with LiTFSI show oxidation resistance above 4.0 V vs. Li/Li⁺ in cyclic voltammetry measurements. The enhanced oxidation resistance improves the performance of Li half-cells containing LC electrolytes.

中文翻译：

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具有高抗氧化性的纳米结构液晶锂离子导体：安全、高压运行锂离子电池的分子设计策略

具有双环己基和环状碳酸酯部分的纳米结构、不带电液晶（LC）电解质分子已被开发用于锂离子电池中作为准固体电解质，从而抑制泄漏和燃烧。为了开发安全、高性能的锂离子电池，我们利用密度泛函理论（DFT）计算设计了具有高抗氧化性的锂离子导电LC材料。DFT计算表明，与含有亚苯基部分的介晶相比，具有双环己基部分的介晶更适合高抗氧化性LC电解质。在环状碳酸酯和核心部分的双环己基部分之间引入的三(氧乙烯)链调节粘度和与Li盐的混溶性。设计的锂离子导电液晶分子在较宽的温度范围内表现出近晶液晶相，并且它们在近晶相中可与添加的双(三氟甲磺酰基)亚胺锂(LiTFSI)盐以高达5:5的摩尔比混溶。所得的含有 LiTFSI 的 LC 混合物在循环伏安法测量中相对于Li/Li ⁺表现出高于 4.0 V 的抗氧化性。增强的抗氧化性提高了含有液晶电解质的锂半电池的性能。