Ionic gel (IG) electrolytes are emerging as promising components for the development of next-generation supercapacitors (SCs), offering benefits in terms of safety, cost-effectiveness, and flexibility. The ionic conductivity, stability, and mechanical properties of the gel electrolyte are relevant factors to be considered and the key to improving the performance of the SC. However, the structure–activity relationship between the internal structure of IGs and their SC properties is not fully understood. In the current study, the intuitive and regular structure–activity relationship between the structure and properties of IGs was revealed combining computational simulation and experiment. In terms of conductivity, the ionic liquid (IL) ([EMIM][TFSI]) in the IG has a high self-diffusion coefficient calculated by molecular dynamics simulation (MDS), which is conductive to transfer and then improves the conductivity. The radial distribution function of the MDS shows that the larger the () between the particles in the polymer network, the stronger the interaction. For stability, IGs based on [EMIM][TFSI] and [EOMIM][TFSI] ILs have higher density functional theory calculated binding energy, which is reflected in the excellent thermal stability and excellent capacitor cycle stability. Based on the internal pore size distribution and stress-strain characterization of the gel network ([ME3MePy][TFSI] and [BMIM][TFSI] as additives), the highly crosslinked aggregate network significantly reduces the internal mesoporous distribution and plays a leading role in improving the mechanical properties of the network. By using this strategy, it will be possible to design the ideal structure of the IG and achieve excellent performance.

中文翻译：

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基于双三氟甲磺酰亚胺盐的超级电容器离子凝胶电解质构效关系的实验和计算分析

离子凝胶（IG）电解质正在成为开发下一代超级电容器（SC）的有前景的组件，在安全性、成本效益和灵活性方面具有优势。凝胶电解质的离子电导率、稳定性和机械性能是需要考虑的相关因素，也是提高SC性能的关键。然而，IG 的内部结构与其 SC 特性之间的构效关系尚不完全清楚。本研究结合计算模拟和实验，揭示了IGs结构与性能之间直观、规律的构效关系。在电导率方面，IG中的离子液体（IL）（[EMIM][TFSI]）通过分子动力学模拟（MDS）计算出具有较高的自扩散系数，有利于转移，进而提高电导率。 MDS的径向分布函数表明，聚合物网络中颗粒之间的()越大，相互作用越强。在稳定性方面，基于[EMIM][TFSI]和[EOMIM][TFSI]IL的IG具有更高的密度泛函理论计算的结合能，这体现在优异的热稳定性和优异的电容器循环稳定性。基于凝胶网络的内部孔径分布和应力应变表征（[ME3MePy][TFSI]和[BMIM][TFSI]作为添加剂），高度交联的聚集体网络显着降低了内部介孔分布并发挥主导作用提高网络的机械性能。通过采用这种策略，将有可能设计出理想的IG结构并获得优异的性能。