Quasi-solid-state ionic thermoelectric (i-TE) cells have attracted increasing interest due to their high thermopower and easy solution processability for flexible and wearable thermoelectric devices. However, many i-TE gels have drawbacks of a narrow working temperature range (ΔT_max) and low power density. In this study, we introduced glutaraldehyde into the gelatin-KCl-FeCN^4−/3− matrix, forming strong covalent bonds and interconnected porous structures, which significantly improve ΔT_max from 9 °C to 23 °C. The formed gelatin/GTA polymer network increases the entropy difference between the redox couples of FeCN^4−/3−, thereby enhancing its thermopower. For the first time, a high thermopower of 24.7 mV K⁻¹, a record-high power density of 9.6 mW m⁻² K⁻² and a 2 h energy density (E_2h) of 198 J m⁻² are achieved simultaneously in a quasi-solid-state i-TE cell. The i-TE cell exhibits good cycling performance in long-term power generation, corresponding to an average E_2h value of 175 J m⁻² after the whole cycling process. A flexible and wearable device consisting of 16 i-TE cells can generate a high voltage of 3.6 V and an output power of 115 μW by harvesting body heat. This work provides a general route to increase the working temperature range and output power density of gel-based i-TE cells through a molecular-level approach.

中文翻译：

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通过扩展工作温度范围，在柔性明胶/GTA-KCl-FeCN4−/3− 离子热电电池中实现创纪录的高输出功率

准固态离子热电 (i-TE) 电池由于其高热功率和易于溶液加工的柔性和可穿戴热电设备而受到越来越多的关注。然而，许多 i-TE 凝胶存在工作温度范围 (Δ T _max ) 窄和功率密度低的缺点。在这项研究中，我们将戊二醛引入到明胶-KCl-FeCN ^4−/3−基质中，形成强共价键和相互连接的多孔结构，显着提高了 Δ T _max从 9 °C 到 23 °C。形成的明胶/GTA 聚合物网络增加了 FeCN ^4−/3−氧化还原对之间的熵差，从而增强了其热电势。首次实现了 24.7 mV K 的高热电势⁻¹时，准固态 i-TE 电池同时实现了^{9.6 mW m −2} K ⁻²的创纪录高功率密度198 J m ⁻²的 2 h 能量密度 ( E _{2h )。}i-TE电池在长期发电中表现出良好的循环性能，对应于整个循环过程后的平均E _2h值为175 J m ^{-2 。}由 16 个 i-TE 电池组成的柔性可穿戴设备可以通过收集体热产生 3.6 V 的高压和 115 μW 的输出功率。这项工作提供了通过分子水平方法增加基于凝胶的 i-TE 电池的工作温度范围和输出功率密度的一般途径。