Lysine-Triggered Polymeric Hydrogels with Self-Adhesion, Stretchability, and Supportive Properties

Hydrogels, recognized for their flexibility and diverse characteristics, are extensively used in medical fields such as wearable sensors and soft robotics. However, many hydrogel sensors derived from biomaterials lack mechanical strength and fatigue resistance, emphasizing the necessity for enhanced formulations. In this work, we utilized acrylamide and polyacrylamide as the primary polymer network, incorporated chemically modified poly(ethylene glycol) (DF-PEG) as a physical crosslinker, and introduced varying amounts of methacrylated lysine (LysMA) to prepare a series of hydrogels. This formulation was labeled as poly(acrylamide)-DF-PEG-LysMA, abbreviated as pADLx, with x denoting the weight/volume percentage of LysMA. We observed that when the hydrogel contained 2.5% w/v LysMA (pADL2.5), compared to hydrogels without LysMA (pADL0), its stress increased by 642 ± 76%, strain increased by 1790 ± 95%, and toughness increased by 2037 ± 320%. Our speculation regarding the enhanced mechanical performance of the pADL2.5 hydrogel revolves around the synergistic effects arising from the co-polymerization of LysMA with acrylamide and the formation of multiple intermolecular hydrogen bonds within the network structures. Moreover, the acid, amine, and amide groups present in the LysMA molecules have proven to be instrumental contributors to the self-adhesion capability of the hydrogel. The validation of the pADL2.5 hydrogel's exceptional mechanical properties through rigorous tensile tests further underscores its suitability for use in strain sensors. The outstanding stretchability, adhesive strength, and fatigue resistance demonstrated by this hydrogel affirm its potential as a key component in the development of robust and reliable strain sensors that fulfill practical requirements.