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PreprintCC BY-NC-NDChemRxiv

Fatigue, Memory and Training in Thermo-Responsive Hydrogels

  1. 1Life-Like Materials and Systems, Department of Chemistry
  2. 2University of Mainz
  3. 3Max-Planck Institute for Polymer Research

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.

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BibTeX
@misc{ciardi2026fatigue,
  title = {{Fatigue, Memory and Training in Thermo-Responsive Hydrogels}},
  author = {Diego Ciardi and Davide Campagna and Daniel Hoenders and Johann Fritzen and Brigitta Dúzs and Andreas Walther},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15008367/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008367/v1},
  note = {CC BY-NC-ND},
}
RIS
TY  - UNPB
TI  - Fatigue, Memory and Training in Thermo-Responsive Hydrogels
AU  - Diego Ciardi
AU  - Davide Campagna
AU  - Daniel Hoenders
AU  - Johann Fritzen
AU  - Brigitta Dúzs
AU  - Andreas Walther
PY  - 2026
DA  - 2026/09/06
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15008367/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008367/v1
AB  - 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.
ER  -