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

• Published in: Chemistry of materials Vol. 37; no. 11; pp. 4085 - 4096
• Main Authors: Mandal, Subhankar, Anand, Shrinkhala, Mandal, Dipankar, Sinha, Akhoury Sudhir Kumar, Ojha, Umaprasana
• Format: Journal Article
• Language: English
• Published: American Chemical Society 10.06.2025
• ISSN: 0897-4756; 1520-5002
• DOI: 10.1021/acs.chemmater.5c00418

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.