Yang Lijuan, Chen Jiawei, He Wenjun, Li Guimei, Xie Chunxia, Wang Wei, Han Dongxue, Han Cheng-Gong, Niu Li
Center for Advanced Analytical Science, Guangzhou Key Laboratory of Sensing Materials and Devices, Guangdong Engineering Technology Research Center for Photoelectric Sensing Materials and Devices, Key Laboratory of Optoelectronic Materials and Sensors in Guangdong Provincial Universities, School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou, 510006, P.R. China.
School of Chemical Engineering and Technology, Sun Yat-Sen University, Zhuhai, 519000, P.R. China.
Angew Chem Int Ed Engl. 2025 Jul 30:e202511293. doi: 10.1002/anie.202511293.
Gel thermocell can directly convert heat into electricity by ions as energy carriers, capable of low-grade heat harvesting. However, ionic thermoelectric performance, including ionic thermopower, output power density, and energy density, needs to be significantly improved to meet practical applications. To date, it still lacks an effective strategy to focus on gels to achieve the overall high performance. Herein, an adhesive and self-healing cationic high-entropy gel (CHEG) G-FeCN-K-Na-Li-Gdm-Cs in a multi-ion cooperative chemical environment has been designed by the interaction between multications and anions, improving the entropy change of redox reaction, exchange current density, and ionic conductivity, thereby achieving an overall high ionic thermoelectric performance. The CHEG thermocell using the synergy of thermogalvanic and thermodiffusion effects showed a total ionic thermopower of 41 mV K with 2.3 mV K for the former, and delivered a maximum output power density of 14.3 mW m K and an energy density of 4.5 J m K. In addition, an ultrahigh maximum output power density of 4.13 mW m K was obtained in the CHEG device that was assembled by connecting four thermocells in series, which could realize electrocatalytic degradation of rhodamine B. This work demonstrates a feasible way to design high-performance ionic thermoelectric gels and provides a new application in water pollution treatments.
凝胶热电池能够通过离子作为能量载体将热量直接转化为电能，可实现低品位热能收集。然而，离子热电性能，包括离子热功率、输出功率密度和能量密度，仍需大幅提高以满足实际应用需求。迄今为止，仍缺乏一种有效的策略来专注于凝胶以实现整体高性能。在此，通过多阳离子与阴离子之间的相互作用，设计了一种处于多离子协同化学环境中的粘性且可自愈的阳离子高熵凝胶（CHEG）G-FeCN-K-Na-Li-Gdm-Cs，改善了氧化还原反应的熵变、交换电流密度和离子电导率，从而实现了整体高离子热电性能。利用热电流效应和热扩散效应协同作用的CHEG热电池，前者的总离子热功率为41 mV K，其中热电流效应贡献2.3 mV K，其最大输出功率密度为14.3 mW m² K，能量密度为4.5 J m² K。此外，通过串联连接四个热电池组装而成的CHEG装置获得了4.13 mW m² K的超高最大输出功率密度，该装置可实现罗丹明B的电催化降解。这项工作展示了一种设计高性能离子热电凝胶的可行方法，并为水污染处理提供了新的应用。
