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Fatigue, Memory and Training in Thermo-Responsive Hydrogels

Year: 2026
Type: preprint
Abstract: Responsive materials are a cornerstone of functional soft matter. Their functionality relies on switching between equilibrium states, a process generally assumed fully reversible over repeated cycles. Here we show that thermo-responsive hydrogels can instead develop progressive fatigue and irreversibility during repeated volume phase transitions. Viscoelastic phase separation generates mechanical stresses that drive permanent network rearrangements and trap phase-separated morphologies, creating a non-volatile structural memory. Consequently, classical responsive hydrogels become adaptive materials whose structure and mechanics evolve with their thermal history. By varying chemical composition and network connectivity, we identify conditions governing the transition from reversible to adaptive behavior. Mechanochemical network remodeling thus provides a route toward materials that acquire durable memory through repeated stimulation, while revealing design and operation principles for fatigue-free switchable soft materials.
Source: ChemRxiv
Language: English
Subfield: Biomaterials
Open Access status: green
OpenAlex ID: W7211899443
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