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Rapid Synthesis of Self?Healing, pH?Responsive IA?Based Hydrogels via Frontal Polymerization

The present investigation addresses a gap in knowledge regarding the development of itaconic acid–based self?healing poly(IA?co?HPA?co?AAc) hydrogels. By employing a rapid frontal polymerization technique, this study successfully fabricates these hydrogels within 10?min, while simultaneously achieving excellent mechanical properties and pH?responsive behavior. The observed reinforcement in strength with increasing AAc content could potentially be attributed to the formation of additional hydrogen bonds within the hydrogel network. These hydrogen bonds may arise from interactions between the carboxylic acid groups (?COOH), hydroxyl groups (?OH), carbonyl groups (?C?O), or potentially other functional groups (?CO?NH?) present in the hydrogel network. The reversible nature of such non?covalent interactions (hydrogen bonding) plays a significant role in enhancing self?healing properties of materials. This reversibility allows for the dynamic rearrangement of intermolecular forces at the interface upon damage, facilitating reformation of the network structure and restoration of material integrity.ABSTRACTSelf?healing polymeric gels have emerged as a promising class of materials due to their ability to repair damage autonomously, offering significant advantages for various applications. Nevertheless, a major hurdle to their widespread practical use lies in their often?compromised mechanical strength and long reaction time. Herein, we present the synthesis of a new type of self?healing hydrogels using poly(itaconic acid?co?hydroxypropyl alcohol?co?acrylic acid), also known as poly(IA?co?HPA?co?AAc), by a frontal polymerization (FP) method. The rapid reaction rate of FP facilitates the swift and energy?efficient synthesis of the hydrogels within 10?min, eliminating the need for prolonged reaction times. Additionally, the results revealed that the synthesized hydrogels exhibited pH?dependent responsiveness, robust mechanical integrity, and autonomous self?healing capabilities, obviating the requirement for external stimuli. The exceptional self?healing properties can be attributed to the extensive hydrogen bonding network between the polymer chains, enabling them to recover up to 80% of their original mechanical strength. Rheological analysis confirmed the presence of a robust and stable gel network, evidenced by high storage modulus (G?) values across the entire frequency and strain sweep tests. This research addresses a significant knowledge gap in IA?based hydrogels by introducing a rapid, optimized method for constructing self?healing materials through hydrogen bonding interactions.