Metal-phenolic networks (MPNs) have recently attracted great interest in material chemistry and biomaterials because of their biocompatible, versatile, and multifunctional properties. In this paper, we describe a facile method for preparation of a designable antifouling, antimicrobial, and substrate-independent coating assembled from the coordination of metal ions and catecholic groups. Hydrophilic and catecholic polymers were synthesized by copolymerization of dopamine methacrylamide (DMA) and poly(ethylene glycol)methyl methacrylate (PEGMA) to afford p(PEGMA-co-DMA). To investigate the assembly and formation of MPN films, two different metal ions, that is, ferrous (Fe II ) and ferric (Fe III ) ions, to react with p(PEGMA-co-DMA) were compared. The binding constants between iron ions and p(PEGMA-co-DMA) have been investigated by ultraviolet−visible spectroscopy (UV−vis). Measurements with atomic force microscopy, contact angle goniometer, and X-ray photoelectron spectroscopy (XPS) were carried out to quantitatively analyze the surface morphology, wettability, and interfacial elemental compositions of coatings, respectively. Moreover, ellipsometric measurements were performed to obtain the film thickness and grafting density. In addition, the pH-responsive property of the MPN films was investigated at different pH values, showing fast disassembly of the networks at low pH. The antifouling properties of the obtained coatings were analyzed by exposing them to bacteria of Escherichia coli and Staphylococcus epidermidis and NIH-3T3 fibroblasts under observation of fluorescence microscopy and cell imaging analysis. The findings suggest that the MPN from complexation of p(PEGMA-co-DMA) and metal ions provides excellent antifouling, pH-responsive, and biocompatible properties on a wide range of substrates. Furthermore, the released iron ions can effectively suppress the growth of bacteria. Accordingly, the new coating architecture offers a universal feature to control surface properties and functionalization for various applications.
Tough and antimicrobial dual-crosslinked poly((trimethylamino)ethyl methacrylate chloride)-phytic acid hydrogel (pTMAEMA-PA) has been synthesized by adding a chemical crosslinker and docking a physical crosslinker of multivalent phytic acid into a cationic polyelectrolyte network. By increasing the loading concentration of PA, the tough hydrogel exhibits compressive stress of >1 MPa, along with high elasticity and fatigue-resistant properties. The enhanced mechanical properties of pTMAEMA-PA stem from the multivalent ion effect of PA via the formation of ion bridges within polyelectrolytes. In addition, a comparative study for a series of pTMAEMA-counterion complexes was conducted to elaborate the relationship between swelling ratio and mechanical strength. The study also revealed secondary factors, such as ion valency, ion specificity and hydrogen bond formation, holding crucial roles in tuning mechanical properties of the polyelectrolyte hydrogel. Furthermore, in bacteria attachment and disk diffusion tests, pTMAEMA-PA exhibits superior fouling resistance and antibacterial capability. The results reflect the fact that PA enables chelating strongly with divalent metal ions, hence, disrupting the outer membrane of bacteria, as well as dysfunction of organelles, DNA and protein. Overall, the work demonstrated a novel strategy for preparation of tough polyelectrolyte with antibacterial capability via docking PA to open up the potential use of PA in medical application.
Biomimetic catechol-functionalized hydrogels have attracted substantial attention due to their potential in a variety of biomedical applications, such as tissue repair and regeneration, drug delivery, and antimicrobial and antifouling applications. In this study, a one-pot strategy for fabrication of functional catecholic hydrogels using dopamine as a photoinitiator was developed. Under UV irradiation in an acidic solution, dopamine generates free radicals, likely semiquinone radicals, to trigger the addition polymerization, following pseudo-first-order kinetics. The dopamine-initiated photopolymerization provides a straightforward and facile approach and, in addition, prevents the undesirable oxidation to catecholic groups. Superhydrophilic sulfobetaine methacrylate (SBMA) was applied for developing biocompatible hydrogels. 1H nuclear magnetic resonance, UV–vis spectroscopy, gel permeation chromatography, and rheological studies were conducted to explore the polymerization mechanism and optimal experimental conditions in terms of pH, UV doses, and the concentration of dopamine. The unique properties of the resultant catechol-functionalized pSBMA hydrogels were demonstrated by enhanced mechanical properties through metal–catechol complexation, self-healing and injectable capability, high adhesiveness, and fouling resistance. Consequently, the synthetic strategy to design catecholic hydrogels can leverage the use of dopamine in a variety of applications.
Tough and antimicrobial dual-crosslinked poly((trimethylamino)ethyl methacrylate chloride)-phytic acid hydrogel (pTMAEMA-PA) has been synthesized by adding chemical crosslinker and docking physical crosslinker of multivalent phytic acid into a cationic polyelectrolyte network. By increasing the loading concentration of PA, the tough hydrogel exhibits compressive stress of >1 MPa, along with high elasticity and fatigue-resistant properties. The enhanced mechanical properties of pTMAEMA-PA were stem from multivalent ion effect of PA via the formation of ion bridges within polyelectrolytes. In addition, a comparative study for a series of pTMAEMA-counterion complexes was conducted to elaborate the relationship between swelling ratio and mechanical strength. The study also revealed secondary factors, such as ion valency, ion specificity and hydrogen bond formation, holding crucial roles in tuning mechanical properties of the polyelectrolyte hydrogel. Furthermore, in bacteria attachment and disk diffusion tests, pTMAEMA-PA exhibits superior fouling resistance and antibacterial capability. The results reflect the fact that PA enables chelating strongly with divalent metal ions, hence, disrupting the outer membrane of bacteria, as well as dysfunction of organelles, DNA and protein. Overall, the work demonstrated a novel strategy for preparation of tough polyelectrolyte with antibacterial capability via docking PA to open up the potential use of PA in medical application.
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