Catalyst-Free Synthesis of a Mechanically Tailorable, Nitric-Oxide-Releasing Organohydrogel and Its Derived Underwater Superoleophobic Coatings

Organohydrogels are an emerging class of soft materials that mimick the mechanical durability and organic solvent affinity of organogels and the biocompatibility and water swelling ability characteristics of hydrogels for prospective biomedical applications. This work introduces a facile, catalyst-free one-step chemical approach to develop an organohydrogel with impeccable antibiofouling properties following the epoxy-amine ring-opening reaction under ambient conditions. The mechanical properties of the as-fabricated organohydrogel can be tailored depending on the concentration of the epoxy-based cross-linker, from 0.10 to 1.12 MPa (compressive modulus). The affinity of the as-developed organohydrogel to both organic solvents and water was exploited to incorporate the antimicrobial nitric oxide donor (NO) molecule, S-nitroso-<i>N</i>-acetylpenicillamine (SNAP) from ethanol, and subsequently, the water-sensitive NO-releasing behavior of the organohydrogels was analyzed. The SNAP-incorporated organohydrogels release physiologically active levels of NO with 3.13 ± 0.27 × 10^-10 and 0.36 ± 0.14 × 10^-10 mol cm^-2 min^-1 flux of NO release observed at 0 and 24 h, respectively. The as-reported organohydrogel demonstrated excellent antibacterial activity against <i>Escherichia coli</i> and <i>Staphylococcus aureus</i> with >99% and >87% reduction, respectively, without eliciting any cytotoxicity concerns. Moreover, the organohydrogel with remarkable water uptake capacity was extended as a coating on different medically relevant polymers to demonstrate transparent underwater superoleophobicity. Thus, the facile synthesis of the reported organohydrogel and its derived underwater antifouling coating can open avenues for utility in biomedical, energy, and environmental applications.