Media Polarity Control Strategy to Tailor Mechanical Behavior of Dual Monomer Single Network Hydrogels and Integrated Machine Learning Approach

Abstract

Facile and scalable procedures to enhance the toughness of hydrogels and tailor their material behavior simultaneously are notably limited in the literature. Especially, one-pot gelation of dual/multi monomer systems suffers from the issue of macrophase separation, which compromises the mechanical behavior of the resulting hydrogels. In this article, a facile media polarity control strategy is reported to enhance the stretchability and adhesive strength of a dual monomer single network hydrogel by promoting phase mixing in a one-pot procedure. As a proof of concept, acrylamidomethylpropanesulfonic acid and acrylamide (AAm)-based dual monomer single network hydrogel are synthesized in an isopropyl alcohol (IPA)/H₂O mixture and evaluated. The resulting hydrogel (PAMSAAm-IP0.1) exhibits superior extensibility (ε, 1050%), tensile strength (UTS, 110 kPa), and adhesive strength (0.25 MPa) compared to that of the control synthesized in H₂O (ε ≈ 230%, UTS ≈ 70 kPa and adhesive strength ≈ 0.03 MPa), supporting the viability of the strategy. Importantly, these compositions having IPA in the matrix retain their functional behavior at low temperature conditions, suggesting their viability under the said conditions. Subsequently, a number of hydrogel compositions are derived using various solvent mixtures, and a machine learning approach is utilized to predict the tensile behavior of the hydrogels based on the compositional ratios and cross-linking conditions.