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<p>Shape memory behavior with programmable recovery onset have been discovered very recently in poly(acrylic acid) hydrogels crosslinked by calcium ions. Their ability to undergo apparent autonomous and timed shape transformation, governed by thermal-sensitive phase evolution, has attracted growing interests particularly for the development of trigger-free biomedical devices. While copolymerization with various monomers can introduce multifunctional properties, this strategy often compromises the phase-separated microstructure and shortens the recovery onset period. Here we introduce hydrophobic acrylate comonomers with different lengths of aliphatic chains to investigate various properties of the copolymerized hydrogels. Upon the same comonomer weight percentage of 20 wt%, short alkyl chains disrupt the polymer aggregation and disable the timed recovery. In contrast, longer alkyl chains form hydrophobic domains which enhance the mechanical properties of the hydrogel and prolong the onset time. Quantitatively, the copolymer hydrogel provided excellent tensile strength of 5.25 MPa and maximum onset period of strikingly 800 min, which are respectively 16.7 and 35 times than the homopolymer hydrogel. This work advances the understanding of the hydrogel system with programmable recovery onset and provides a promising molecular modulation strategy for functionalization of hydrogels with responsive phase separation behavior.</p>

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Enhanced Mechanical Properties and Prolonged Recovery Onset Period of Timed Shape Memory Hydrogels via Hydrophobic Interaction

  • 期刊论文

  • 发表日期：

    2026年5月21日

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  • Xiao-Ting Jia,
  • Yi-Ting Sun,
  • Chu-Jun Ni,
  • Qian Zhao

摘要

Shape memory behavior with programmable recovery onset have been discovered very recently in poly(acrylic acid) hydrogels crosslinked by calcium ions. Their ability to undergo apparent autonomous and timed shape transformation, governed by thermal-sensitive phase evolution, has attracted growing interests particularly for the development of trigger-free biomedical devices. While copolymerization with various monomers can introduce multifunctional properties, this strategy often compromises the phase-separated microstructure and shortens the recovery onset period. Here we introduce hydrophobic acrylate comonomers with different lengths of aliphatic chains to investigate various properties of the copolymerized hydrogels. Upon the same comonomer weight percentage of 20 wt%, short alkyl chains disrupt the polymer aggregation and disable the timed recovery. In contrast, longer alkyl chains form hydrophobic domains which enhance the mechanical properties of the hydrogel and prolong the onset time. Quantitatively, the copolymer hydrogel provided excellent tensile strength of 5.25 MPa and maximum onset period of strikingly 800 min, which are respectively 16.7 and 35 times than the homopolymer hydrogel. This work advances the understanding of the hydrogel system with programmable recovery onset and provides a promising molecular modulation strategy for functionalization of hydrogels with responsive phase separation behavior.