Tough, Self-Recoverable, Spiropyran (SP3) Bearing Polymer Beads Incorporated PAM Hydrogels with Sole Mechanochromic Behavior

Spiropyran-containing hydrogels that can respond to external stimuli such as temperature, light, and stress have attracted extensive attention in recent years. However, most of them are generally dual or multiple stimuli-responsive to external stimuli, and the interplay of different stimulus responses is harmful to their sensitivity. Herein, spiropyran bearing polymer beads incorporated PAM (poly(AM–co–MA/DMSP3)) hydrogels with sole mechanochromic properties were synthesized by emulsion polymerization of acrylamide (AM) and methyl acrylate (MA) in the presence of spiropyran dimethacrylate mechanophore (DMSP3) crosslinker. Due to the hydrophobic nature of MA and DMSP3, the resultant hydrogel afforded a rosary structure with DMSP3 bearing polymer beads incorporated in the PAM network. It is found that the chemical component (e.g., AM, MA, and DMSP3 concentrations) significantly affect the mechanical and mechanoresponsive properties of the as-obtained poly(AM–co–MA/DMSP3) hydrogel. Under optimal conditions, poly(AM–co–MA/DMSP3) hydrogel displayed high mechanical properties (tensile stress of 1.91 MPa, a tensile strain of 815%, an elastic modulus of 0.67 MPa, and tearing energy of 3920 J/m2), and a good self-recovery feature. Owing to the mechanoresponsive of SP3, the hydrogels exhibited reversible color changes under force-induced deformation and relaxed recovery states. More impressive, the poly(AM–co–MA/DMSP3) hydrogel showed a linear correlation between tensile strain and chromaticity (x, y) as well as a stain and resting time-dependent color recovery rate. This kind of hydrogel is believed to have great potential in the application of outdoor strain sensors.