Multiresponsive Color-Changing and Tough Hydrogels Enabled by Self-Assembled Epoxy Oligomer Microspheres

The fabrication process of hydrogels often incorporates various strategies to achieve multiple responses and enhance strength, which always make the procedure complex and even hinder the incorporation. Here, we develop a facile and flexible method to simultaneously achieve multiresponsive color-changing and tough properties in hydrogels by introducing epoxy oligomer microspheres (DEPMS) to hydrophobic association (HA) hydrogels. DEPMS is responsive to both pH and solvents, showing color changes due to conversion to a conjugated structure. The obtained DEPMS composite hydrogels could demonstrate diverse color-changing patterns by simply adjusting the components and pH of the solvents. Meanwhile, amphiphilic DEPMS helps to disperse hydrophobic regions of the HA hydrogel, resulting in more uniform cross-linking and thereby contributing to the enhanced mechanical properties. The tensile strength and toughness of the composite hydrogels could be easily adjusted and reach 1.00 MPa and 11.18 MJ m–3, respectively. This work provides an approach to the design of multiple responsive and tough hydrogels while offering insights into the recycling of waste epoxy resins.