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<p>Polymer hydrogels with variable stiffness demonstrate immense practical application value, particularly when utilizing water as a trigger medium, which significantly expands their prospects in soft robotics, bioelectronics, and artificial muscles. However, existing water-induced stiffening hydrogel rely on ionic liquids and inorganic salts, posing leakage risks during prolonged use. Here, we proposed a strategy for mechanically strengthening hydrogel through water-induced phase separation. By designing a polymer matrix featuring hydrophilic oligomeric ethylene glycol methacrylate (OEGMA) and hydrophobic methyl methacrylate (MMA) moieties, this poly[methyl methacrylate-<i>co</i>-poly(ethylene glycol) methacrylate] [P(MMA<sub><i>x</i></sub>-<i>co</i>-OEGMA<sub><i>y</i></sub>)] hydrogel exhibited reversible stiffness switching across four orders of magnitude (from 1.88×10<sup>−2</sup> MPa to 201.63 MPa) upon water stimulation. This abrupt stiffness enhancement stemmed from strong hydrogen bonding between water molecules and hydrophilic OEGMA segments, facilitating spontaneous aggregation and phase separation of hydrophobic MMA segments. The resulting hydrophobic MMA domains formed dynamic physical crosslinking points, thereby enhancing the hydrogel’s stiffness. Furthermore, the hydrogel exhibited a time-dependent, multi-stage stiffness enhancement during water swelling. As proof of concept, it was employed as a shape-memory component to explore its application in the controllable programming of multi-stage complex shapes, offering novel design insights for developing environmentally friendly, high-mechanical-performance smart hydrogel materials.</p>

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Water Swelling-induced Stiffness Enhancement of Polymer Hydrogels

  • 期刊论文

  • 发表日期：

    2026年4月17日

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  • Yi Yu,
  • Wei Zhou,
  • Tao Chen,
  • Wei Lu

摘要

Polymer hydrogels with variable stiffness demonstrate immense practical application value, particularly when utilizing water as a trigger medium, which significantly expands their prospects in soft robotics, bioelectronics, and artificial muscles. However, existing water-induced stiffening hydrogel rely on ionic liquids and inorganic salts, posing leakage risks during prolonged use. Here, we proposed a strategy for mechanically strengthening hydrogel through water-induced phase separation. By designing a polymer matrix featuring hydrophilic oligomeric ethylene glycol methacrylate (OEGMA) and hydrophobic methyl methacrylate (MMA) moieties, this poly[methyl methacrylate-co-poly(ethylene glycol) methacrylate] [P(MMAx-co-OEGMAy)] hydrogel exhibited reversible stiffness switching across four orders of magnitude (from 1.88×10−2 MPa to 201.63 MPa) upon water stimulation. This abrupt stiffness enhancement stemmed from strong hydrogen bonding between water molecules and hydrophilic OEGMA segments, facilitating spontaneous aggregation and phase separation of hydrophobic MMA segments. The resulting hydrophobic MMA domains formed dynamic physical crosslinking points, thereby enhancing the hydrogel’s stiffness. Furthermore, the hydrogel exhibited a time-dependent, multi-stage stiffness enhancement during water swelling. As proof of concept, it was employed as a shape-memory component to explore its application in the controllable programming of multi-stage complex shapes, offering novel design insights for developing environmentally friendly, high-mechanical-performance smart hydrogel materials.