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Physical Crosslinking in Double Network Hydrogels: Structural Design, Toughening Mechanisms, and Functional Diversity
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DOI：10.1016/j.progpolymsci.2026.102104.png)
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Abstract
En 中文
Physically crosslinked double-network (DN) hydrogels offer a compelling strategy for developing tough, resilient, and multifunctional soft materials. Their unique architecture—comprising two interpenetrating yet independently crosslinked polymer networks stabilized by reversible physical interactions—confers exceptional mechanical robustness and functional adaptability under diverse deformation and stimulus conditions. Compared to their chemically crosslinked counterparts, physically crosslinked DN hydrogels address key limitations such as irreparable mechanical failure and irreversible fatigue damage by leveraging dynamic, non-covalent bonding. Achieving such performance, however, requires innovative molecular design and synthesis strategies to identify compatible polymer pairs capable of forming stable, reversible networks during gelation. This review synthesizes recent and important findings to provide a fundamental overview of the advancements in physically crosslinked DN hydrogels, focusing on their design concepts, synthesis strategies, network structures, mechanical toughening and recovery mechanisms, and functional applications associated with physical bonds. It systematically categorizes physical crosslinking mechanisms—including hydrogen bonding, hydrophobic association, ionic coordination, host–guest interactions, and hybrid approaches—and discusses their roles in network formation, toughening, and recovery. Representative strategies are examined to highlight the integration of sacrificial bonds and network topologies that enable energy dissipation, self-recovery, and fatigue resistance. Furthermore, the review explores diverse applications of these materials, spanning biomedical devices, flexible electronics, and environmental systems. Finally, current challenges and future opportunities are discussed, emphasizing the potential for machine learning and molecular simulations to guide rational design. This work aims to advance the fundamental understanding and practical utility of physically crosslinked DN hydrogels across interdisciplinary domains.
Keywords:
Physical crosslinking
Double-network hydrogels
Mechanical toughening
Functional applications
Network design
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26.1
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1.4K
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