Clinically, biofilm-associated infections commonly form on intravascular catheters and other hydrogel surfaces. The overuse of antibiotics to treat these infections has led to the spread of antibiotic resistance and underscores the importance of developing alternative strategies that delay the onset of biofilm formation. Previously, it has been reported that during surface contact, bacteria can detect surfaces through subtle changes in the function of their motors. However, how the stiffness of a polymer hydrogel influences the initial attachment of bacteria is unknown. Systematically, we investigated poly(ethylene glycol) dimethacrylate (PEGDMA) and agar hydrogels that were twenty times thicker than the cumulative size of bacterial cell appendages, as a function of Young’s moduli. Soft (44.05 – 308.5 kPa), intermediate (1495 – 2877 kPa), and stiff (5152 – 6489 kPa) hydrogels were synthesized. Escherichia coli and Staphylococcus aureus attachment onto the hydrogels was analyzed using confocal microscopy after 2 and 24 hr incubation periods. Independent of hydrogel chemistry and incubation time, E. coli and S. aureus attachment correlated positively to increasing hydrogel stiffness. For example, after a 24 hr incubation period, there were 52% and 82% less E. coli adhered to soft PEGDMA hydrogels, than to the intermediate and stiff PEGDMA hydrogels, respectively. A 62% and 79% reduction in the area coverage by the Gram-positive microbe S. aureus occurred after 24 hr incubation on the soft versus intermediate and stiff PEGDMA hydrogels. We suggest that hydrogel stiffness is an easily tunable variable that, potentially, could be used synergistically with traditional antimicrobial strategies to reduce early bacterial adhesion, and therefore the occurrence of biofilm-associated infections.
Hydration is central to mitigating surface fouling by oil and microorganisms. Immobilization of hydrophilic polymers on surfaces promotes retention of water and a reduction of direct interactions with potential foulants. While conventional surface modification techniques are surface-specific, mussel-inspired adhesives based on dopamine effectively coat many types of surfaces and thus hold potential as a universal solution to surface modification. Here, we describe a facile, one-step surface modification strategy that affords hydrophilic, and underwater superoleophobic, coatings by the simultaneous deposition of polydopamine (PDA) with poly(methacryloyloxyethyl phosphorylcholine) (polyMPC). The resultant composite coating features enhanced hydrophilicity (i.e., water contact angle of ~10° in air) and antifouling performance relative to PDA coatings. PolyMPC affords control over coating thickness and surface roughness, and results in a nearly 10 fold reduction in Escherichia coli adhesion relative to unmodified glass. The substrate-independent nature of PDA coatings further promotes facile surface modification without tedious surface pretreatment, and offers a robust template for codepositing polyMPC to enhance biocompatibility, hydrophilicity and fouling resistance.
By combining antifouling shark-skin patterns with antibacterial titanium dioxide (TiO2) nanoparticles (NPs), we present a simple route toward producing durable multifunctional surfaces that decrease microbial attachment and inactivate attached microorganisms. Norland Optical Adhesive, a UV-crosslinkable adhesive material, was loaded with 0, 10, or 50 wt % TiO2 NPs from which shark-skin microstructures were imprinted using solvent-assisted soft nanoimprint lithography on a poly(ethylene terephthalate) (PET) substrate. To obtain coatings with an exceptional durability and an even higher concentration of TiO2 NPs, a solution containing 90 wt % TiO2 NPs and 10 wt % tetraethyl orthosilicate was prepared. These ceramic shark-skin-patterned surfaces were fabricated on a PET substrate and were quickly cured, requiring only 10 s of near infrared (NIR) irradiation. The water contact angle and the mechanical, antibacterial, and antifouling characteristics of the shark-skin-patterned surfaces were investigated as a function of TiO2 composition. Introducing TiO2 NPs increased the contact angle hysteresis from 30 to 100° on shark-skin surfaces. The hardness and modulus of the films were dramatically increased from 0.28 and 4.8 to 0.49 and 16 GPa, respectively, by creating ceramic shark-skin surfaces with 90 wt % TiO2 NPs. The photocatalytic shark-skin-patterned surfaces reduced the attachment of Escherichia coli by ~70% compared with smooth films with the same chemical composition. By incorporating as low as 10 wt % TiO2 NPs into the chemical matrix, over 95% E. coli and up to 80% Staphylococcus aureus were inactivated within 1 h UV light exposure because of the photocatalytic properties of TiO2. The photocatalytic shark-skin-patterned surfaces presented here were fabricated using a solution-processable and roll-to-roll compatible technique, enabling the production of large-area high-performance coatings that repel and inactivate bacteria.
Despite lacking visual, auditory, and olfactory perception, bacteria sense and attach to surfaces. Many factors including, the chemistry, topography, and mechanical properties of a surface, are known to alter bacterial attachment, and in this study, using a library of nine protein-resistant poly(ethylene glycol) (PEG) hydrogels immobilized on glass slides, we demonstrate that the thickness or amount of polymer concentration also matters. Hydrated atomic force microscopy and rheological measurements corroborated that thin (15 μm), medium (40 μm), and thick (150 μm) PEG hydrogels possessed Young’s moduli in three distinct regimes, soft (20 kPa), intermediate (300 kPa), and stiff (1000 kPa). The attachment of two diverse bacteria, flagellated gram-negative Escherichia coli and non-motile gram-positive Staphylococcus aureus was assessed after a 24 h incubation on the nine PEG hydrogels. On the thickest PEG hydrogels (150 μm), E. coli and S. aureus attachment increased with increasing hydrogel stiffness. However, when hydrogel’s thickness was reduced to 15 μm, a substantially greater adhesion of E. coli and S. aureus was observed. Twelve times fewer S. aureus and eight times fewer E. coli adhered to thin-soft hydrogels than to thick-soft hydrogels. Though a full mechanism to explain this behavior is beyond the scope of this paper, we suggest that because the Young’s moduli of thin-soft and thick-soft hydrogels were statistically equivalent, potentially, the very stiff underlying glass slide was causing the thin-soft hydrogels to feel stiffer to the bacteria. These findings suggest a key takeaway design rule; to optimize fouling-resistance, hydrogel coatings should be thick and soft.
In this study, we exploit the excellent fouling resistance of polymer zwitterions and present electrospun nanofiber mats surface-functionalized with poly(2-methacryloyloxyethyl phosphorylcholine) (polyMPC). This zwitterionic polymer coating maximizes the accessibility of the zwitterion to effectively limit biofouling on nanofiber membranes. Two facile, scalable methods yielded a coating on a cellulose nanofiber platform: (i) a two-step sequential deposition featuring dopamine polymerization followed by the physioadsorption of polyMPC; and (ii) a one-step codeposition of polydopamine (PDA) with polyMPC. While the sequential and codeposited nanofiber mat assemblies have an equivalent average fiber diameter, hydrophilic contact angle, surface chemistry, and stability, the topography of nanofibers prepared by codeposition were smoother. Protein and microbial antifouling performance of the zwitterion modified nanofiber mats along with two controls, cellulose (unmodified) and PDA coated nanofiber mats were evaluated by dynamic protein fouling and prolonged bacteria exposure experiments. Following 21 days of exposure to bovine serum albumin, the sequential nanofiber mats significantly resisted protein fouling, as indicated by their 95% flux recovery ratio in a water flux experiment, 300% improvement over the cellulose nanofiber mats. When challenged with two model microbes Escherichia coli and Staphylococcus aureus for 24 hr, both zwitterion modifications demonstrated superior fouling resistance by statistically reducing microbial attachment over the two controls. This study demonstrates that by decorating the surfaces of chemically and mechanically robust cellulose nanofiber mats with polyMPC, we can generate high performance, free-standing nanofiber mats that hold potential in applications where antifouling materials are imperative, such as tissue engineering scaffolds and water purification technologies.
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