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Ionogel with Synergistic Dual Dynamic Bonds for High Self-healing and Ionic Conductivity
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DOI：10.11777/j.issn1000-3304.2025.25292.png)
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Abstract
En 中文
Ionogels, known for their high safety and wide electrochemical windows, show great potential in energy storage. However, existing ionogels often struggle to balance high strength with dynamic properties,making it difficult to achieve an optimal combination of mechanical performance, self-healing capability, and ionic conductivity. To address this challenge, this study presents a novel ionogel electrolyte that integrates good flexibility, high mechanical strength, a wide electrochemical window, and rapid self-healing functionality. The self-healing system of the electrolyte is constructed through a dual dynamic crosslinking mechanism: on one hand, imidazole-zinc (Im-Z) metal coordination is introduced to form a dynamic high-strength crosslinked network; on the other hand, ion-dipole (Ion-D) interactions between the ionic liquid (IL) and & horbar;CF3 groups on the polymer chains are utilized to regulate chain segment mobility, thereby optimizing ion transport performance.Owing to this structure, the ionogel achieved a high self-healing efficiency of 94% and a tensile strength of 80 kPa. Moreover, the material exhibits a high ionic conductivity of 0.36 mS/cm, lithium-ion transference number of 0.46, and wide electrochemical window of 4.32 V, all of which contribute to the comprehensive improvements in the performance of solid-state lithium batteries. A Li/LiFePO4 full cell assembled with this ionogel maintained a capacity retention rate as high as 80 % after 500 cycles at 0.5 C. This study elucidates the regulatory mechanism of supramolecular structural design on ion transport behavior and chain segment dynamics in ionogels, providing a theoretical basis for developing high-performance energy storage materials
Keywords:
Self-healing performance
Metal ligand
Ion-dipole
Ionogel
Solid-state lithium battery
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