Super-tough hydrogels from shape-memory polyurethane with wide-adjustable mechanical properties

Feng Wu, Lei Chen, Yangling Li, Ka I. Lee, Bin Fei

Research output: Journal article publicationJournal articleAcademic researchpeer-review

20 Citations (Scopus)


Recoverable hydrogels with high strength and toughness have been fabricated from hydrophilic and thermoplastic polyurethane (HTPU), which chains consist of hydrophilic polyethylene glycol (PEG) segment of high crystallinity and hydrophobic segment with strong hydrogen-bonding groups. This HTPU absorbed high amount of water, during which the PEG crystals swollen and dissolved, while the hydrophobic segments still held the adjacent chains together, forming a stable hydrogel. Even at equilibrium swelling state (89 wt% water), the HTPU hydrogel exhibited high modulus (0.4 MPa), high strength (2.6 MPa), and large strain at break (~500%). The effect of water content on the tensile properties of HTPU hydrogels was carefully studied at different levels of swelling. Interestingly, the hydrogels demonstrated a transition from a typical tough plastic to a tough elastomer when the water content reached 35 wt% of the hydrogel, with breaking strength of 10.0 MPa and fracture energy of 59.7 MJ/m3at maximum strain over 1600%. The results from differential scanning calorimetry, Fourier transform infrared spectroscopy, and microscope measurements showed that the wide adjustability of this HTPU mechanical property was a result of the changes in its crystallinity, hydrogen-bonding, and hydrophobic association. Furthermore, the shape-memory performance of the HTPU was studied with heat and water stimuli and found faster at heating to 70 °C than that by immersion in water: 10 s versus 10 min. This study may widen the application of HTPU biodegradable polymers and provide new frontiers for the design of tough hydrogels by network structure control.
Original languageEnglish
Pages (from-to)4421-4434
Number of pages14
JournalJournal of Materials Science
Issue number8
Publication statusPublished - 1 Apr 2017

ASJC Scopus subject areas

  • Materials Science(all)
  • Mechanics of Materials
  • Mechanical Engineering


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