Sapkota Aasma, Shome Arpita, Crutchfield Natalie, Moses Joseph Christakiran, Martinez Isabel, Handa Hitesh, Brisbois Elizabeth J
School of Chemical, Materials, & Biomedical Engineering, University of Georgia, Athens 30602, Georgia, United States.
Pharmaceutical and Biomedical Sciences Department, College of Pharmacy, University of Georgia, Athens, Georgia 30602, United States.
ACS Appl Mater Interfaces. 2025 Apr 2;17(13):19335-19347. doi: 10.1021/acsami.4c21695. Epub 2025 Mar 19.
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--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 and 0.36 ± 0.14 × 10 mol cm min flux of NO release observed at 0 and 24 h, respectively. The as-reported organohydrogel demonstrated excellent antibacterial activity against and 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.
有机水凝胶是一类新兴的软材料，它模仿了有机凝胶的机械耐久性和有机溶剂亲和力，以及水凝胶的生物相容性和水溶胀能力特性，具有潜在的生物医学应用前景。这项工作介绍了一种简便的、无催化剂的一步化学方法，在环境条件下通过环氧-胺开环反应来开发一种具有无可挑剔的抗生物污损性能的有机水凝胶。所制备的有机水凝胶的机械性能可以根据环氧基交联剂的浓度进行调整，压缩模量从0.10到1.12兆帕。利用所开发的有机水凝胶对有机溶剂和水的亲和力，从乙醇中引入抗菌一氧化氮供体（NO）分子S-亚硝基-N-乙酰青霉胺（SNAP），随后分析了有机水凝胶对水敏感的NO释放行为。在0小时和24小时时，分别观察到掺入SNAP的有机水凝胶释放具有生理活性水平的NO，NO释放通量分别为3.13±0.27×10和0.36±0.14×10摩尔/平方厘米·分钟。所报道的有机水凝胶对大肠杆菌和金黄色葡萄球菌表现出优异的抗菌活性，分别减少>99%和>87%，且没有引起任何细胞毒性问题。此外，具有显著吸水能力的有机水凝胶被扩展为不同医学相关聚合物上的涂层，以展示透明的水下超疏油性。因此，所报道的有机水凝胶及其衍生的水下防污涂层的简便合成可为生物医学、能源和环境应用开辟途径。
