Rhodamine-Functionalized Mechanochromic and Mechanofluorescent Hydrogels with Enhanced Mechanoresponsive Sensitivity

Smart materials responsible to external stimuli such as temperature, pH, solvents, light, redox agents, and mechanical or electric/magnetic field, have drawn considerable attention recently. Herein, we described a novel rhodamine (Rh) mechanophore-based mechanoresponsive micellar hydrogel with excellent mechanochromic and mechanofluorescent properties. We found with astonishment that, due to the favorable activation of rhodamine spirolactam in the presence of water, together with the stress concentration effect, the mechanoresponsive sensitivity of this hydrogel was enhanced significantly. As a result, the stress needed to trigger the mechanochromic property of Rh in the hydrogel was much lower than in its native polymer matrix reported before. The hydrogel based on Rh, therefore, exhibited excellent mechanochromic property even at lower stress. Moreover, due to the reversibility of color on/off, the hydrogel based on Rh could be used as a reusable and erasable material for color printing/writing. Of peculiar importance is that the hydrogel could emit highly bright fluorescence under sufficient stress or strain. This suggested that the stress/strain of hydrogel could be detected quantificationally and effectively by the fluorescence data. We also found that the hydrogel could respond to acid/alkali and exhibited outstanding properties of acidichromism and acidifluorochromism. Up to now, hydrogels with such excellent mechanochromic and mechanofluorescent properties have rarely been reported. Our efforts may be essentially beneficial to the design of the mechanochromic and mechanofluorescent hydrogels with enhanced mechanoresponsive sensitivity, fostering their potential applications in a number of fields such as damage or stress/strain detection.