The rapid growth of flexible quasi‐solid‐state thermocells (TECs) provides a fresh way forward for wearable electronics. However, their insufficient mechanical strength and power output still hinder their further applications. This work demonstrates a one‐stone‐two‐birds strategy to synergistically enhance the mechanical and thermoelectrochemical properties of the [Fe(CN)6]3−/4−‐based TECs. By introducing multiple non‐covalent interactions via betaine zwitterions, the mechanical strength of the conventional brittle gelatin hydrogel electrolytes is substantially improved from 50 to 440 kPa, with a high stretchability approaching 250%. Meanwhile, the betaine zwitterions strongly affect the solvation structure of [Fe(CN)6]3− ions, thus enlarging the entropy difference and raising the thermoelectrochemical Seebeck coefficient from 1.47 to 2.2 mV K−1. The resultant quasi‐solid‐state TECs exhibit a superior normalized output power density of 0.48 mW m−2 K−2, showing a notable improvement in overall performance compared to their counterparts without zwitterion regulation. In addition, the intrinsic thermo‐reversible property allows the TECs to repeatedly self‐recover through sol‐gel transformations, ensuring reliable energy output and even recycling of TECs in case of extreme mechanical damages. An energy‐autonomous smart glove consisting of eighteen individual TECs is further designed, which can simultaneously monitor the temperature of different positions of any touched object, demonstrating high potential in wearable applications.

中文翻译：

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坚固、高效、可恢复的热电池，采用两性离子增强水凝胶电解质，用于能量自主和可穿戴传感

柔性准固态热电池（TEC）的快速增长为可穿戴电子产品提供了一条新的前进方向。然而，它们机械强度和功率输出不足仍然阻碍了它们的进一步应用。这项工作展示了一种一石二鸟的策略，可以协同增强[Fe(CN)6]3−/4−基TEC的机械和热电化学性能。通过甜菜碱两性离子引入多种非共价相互作用，传统脆性明胶水凝胶电解质的机械强度从 50 kPa 大幅提高到 440 kPa，拉伸率接近 250%。同时，甜菜碱两性离子强烈影响[Fe(CN)6]3−离子的溶剂化结构，从而扩大了熵差并将热电化学塞贝克系数从1.47提高到2.2 mV K−1。由此产生的准固态 TEC 表现出 0.48 mW m−2 K−2 的优异归一化输出功率密度，与没有两性离子调节的同类产品相比，整体性能显着提高。此外，固有的热可逆特性允许TEC通过溶胶-凝胶转变反复自我恢复，确保可靠的能量输出，甚至在极端机械损坏的情况下回收TEC。进一步设计了由 18 个独立 TEC 组成的能量自主智能手套，它可以同时监测任何触摸物体不同位置的温度，在可穿戴应用中展现出巨大的潜力。