Supramolecular Polymer‐Based Ionogels Enable Large‐Scale Fabrication of Stable Smart Windows with Room‐Temperature Closed‐Loop Recyclability and Self‐Healing Capability

Abstract

Current self‐healing ionogels are unable to undergo closed‐loop recycling and are unsuitable for large‐scale fabrication, which increases their manufacturing costs and limits their practical applications. In this study, self‐healing thermochromic ionogels with room‐temperature closed‐loop recyclability and self‐healing capability are large‐scale prepared by the in situ synthesis of imine bond cross‐linked supramolecular polymers in binary ionic liquids. The resulting ionogels show excellent mechanical and environmental stability, high solar modulation capability, and long service life, which can provide spontaneous solar modulation for buildings and vehicles to reduce cooling‐related energy consumption. The temperature‐responsive hydrogen bonding between supramolecular polymers and ionic liquids influences the dissolution state of the supramolecular polymers, allowing the self‐healing thermochromic ionogels to switch between transparent and opaque states through reversible agglomeration of ILs inside the ionogels. Dynamic imine bonds enable the ionogels to spontaneously heal themselves at room temperature and to be depolymerized into monomers in an extremely high yield and purity under hydrochloric acid catalysis at room temperature. The recovered monomers can be used to re‐manufacture self‐healing thermochromic ionogels without losing their original mechanical properties or thermochromic capability. This study provides a new route for developing functional self‐healing ionogels that can be large‐scale fabricated and closed‐loop recycled.

A Highly Effective Self-Healing Waterborne Polyurethane Vitrimer Containing Conjugated Schiff Base Bonds Driven by Photothermal

“…Nevertheless, this strategy has limitations, such as the limited number of self-healing cycles . However, intrinsic healing materials contain reversible dynamic chemical bonds that can break and regenerate when stimulated by external conditions such as pH, heat, or visible light, − allowing for self-healing of the material. Commonly used reversible dynamic bonds include imine, disulfide, Diels–Alder, and hydrogen bonds. − In recent years, there has been a growing interest in intrinsic self-healing materials as a research focus due to their ability to heal without the need for external agents, as well as their ability to completely heal multiple times .…”

Ligand Dissociation of Metal-Complex Photocatalysts toward pH-Photomanipulation in Dynamic Covalent Hydrogels for Printing Reprocessable and Recyclable Devices

“…Dynamic polymers have garnered significant attention due to their unique dynamic features and similar mechanical performances to traditional static polymers. − Their reversible networks allow them to reconfigure and restructure, with potential applications in high-performance smart materials, soft devices, electronics, and other fields. − For example, programmatically controlling the dynamic equilibrium in polymers enables precise shape-memory behavior in specific environments. − Their dynamic nature gives them excellent self-healing, reprocessable, and recyclable properties under external stimuli. − Especially dynamic hydrogels, with their water-rich and porous structures, offer biomimetic microenvironments, while reversible bonding provides mechanical dynamics for stiffness control in cell culture, tissue repair, and conformable bioelectronics fabrication. − Moreover, dynamic polymer hydrogels with covalent bonding interactions demonstrate superior mechanical performance to those with noncovalent interactions. Combining hydrogel preparation with emerging additive manufacturing technologies can further extend their advanced applications with complex structures. , Therefore, developing high-performance dynamic covalent hydrogels is essential and presents an intriguing topic in related fields.…”