Jui-Che Lin

Reducing hospital-acquired infections, especially those related to medical devices, is essential not only to improve patients’ well-being but also to reduce healthcare costs. Among various antibacterial approaches, creating bactericidal device surfaces has been advocated as it reduces the likelihood of antibiotic-resistant strains emerging when antibiotics are used. Functionalizing the device surface with cationic groups, such as quaternary ammonium terminal groups, has been considered an effective approach for killing microbes upon contact. Nonetheless, multiple steps, some of which may require harsh chemical reactions and toxic solvents, are generally required to attach the cationic quaternary ammonium functionalities to the surface. Inspired by the mussel’s capability to bind to various substrates, various novel biomimetic cationic catechol-terminated small molecules having the quaternary ammonium functionality with different alkyl chain lengths were synthesized for the first time. These compounds were used for surface modification of medical-grade titanium using simple immersion approaches: a single-layer procedure or a two-layer approach, in which the first layer was prepared by dopamine immersion, followed by a second immersion in the compound of interest. The surface characteristics and antimicrobial capability against the Gram-negative E. coli and Gram-positive S. aureus were assessed. The likely effects of the alkyl chain length and modification schemes on the surface properties and antibacterial activity are discussed and compared. The highest antimicrobial activity against E. coli was noted on the modified surfaces prepared by the two-layer approach with the cationic compound having the shortest alkyl chain, C1, at 2 mg/mL (DA_C1-2) and 8 mg/mL (DA_C1-8). The DA_C1-8 surface also exhibited the highest antimicrobial activity against S. aureus. These findings indicated that the antibacterial activity of titanium can be greatly improved by selecting the appropriate compound and a proper, facile immersion procedure.

Healthcare-associated infection, mainly through medical device-associated infection, remains a critical issue in hospital care. Bacterial adhesion, proliferation, and biofilm formation on the device surface have been considered the foremost cause of medical device-associated infection. Different means have been explored to reduce microbial attachment and proliferation, including forming a bactericidal or microbial adhesion-resistant surface layer. Fear of limited bactericidal capability if the dead microbes remained adhered to the surface has withheld the widespread use of a bactericidal surface in medical devices if it was intended for long-term use. By contrast, constructing a microbial adhesion-resistant or antifouling surface, such as a surface with zwitterionic functionality, would be more feasible for devices intended to be used for the long term. Nevertheless, a sophisticated multi-step chemical reaction process would be needed. Instead, a simple immersion method that utilized a novel mussel-inspired catechol compound with zwitterionic sulfobetaine functionality, ZDS, was explored in this investigation for the surface modification of substrates with distinctively different surface characteristics, including titanium and polyvinyl chloride. Dopamine, NaIO₄ oxidants, and chemicals that could affect ionic interactions (NaCl and polyethyleneimine) were added to the ZDS-containing immersion solution to compare their effects on modifying titanium and PVC substrates. Furthermore, a layer-by-layer immersion method, in which the substrate was first immersed in the no-ZDS-added dopamine-containing solution, followed by the ZDS-containing solution, was also attempted on the PVC substrate. By properly selecting the immersion solution formulation and additional NaIO₄ oxidation modification, the antibacterial capability of ZDS-modified substrates can be optimized without causing cytotoxicity. The maximum antibacterial percentages against S. aureus were 84.2% and 81.7% for the modified titanium and PVC substrate, respectively, and both modified surfaces did not show any cytotoxicity.

Medical device-associated infection remains a critical problem in the healthcare setting. Different clinical- or device-related methods have been attempted to reduce the infection rate. Among these approaches, creating a surface with bactericidal cationic functionality has been proposed. To do so, a sophisticated multi-step chemical procedure would be needed. Instead, a simple immersion approach was utilized in this investigation to render the titanium and polypropylene surface with the quaternary ammonium functionality by using a mussel-inspired novel lab-synthesized biomimetic catechol-terminated polymer, PQA-C8. The chemical oxidants, CuSO₄/H₂O₂, as well as dopamine, were added into the novel PQA-C8 polymer immersion solution for one-step surface modification. Additionally, a two-step immersion scheme, in which the polypropylene substrate was first immersed in the dopamine solution and then in the PQA-C8 solution, was also attempted. Surface analysis results indicated the surface characteristics of the modified substrates were affected by the immersion solution formulation as well as the procedure utilized. The antibacterial assay has shown the titanium substrates modified by the one-step dopamine + PQA-C8 mixtures with the oxidants added and the polypropylene modified by the two-step scheme exhibited bacterial reduction percentages greater than 90% against both Gram-positive S. aureus and Gram-negative E. coli and these antibacterial substrates were non-cytotoxic.

For the effective clinical antibacterial application of biomaterials, such as for wound management and tissue repair, the biomaterials need to show proper antibacterial capability as well as non-cytotoxicity. Furthermore, the material needs to have suitable mechanical characteristics for further medical use. Chitosan hydrogel is a potential candidate for various antibacterial biomedical applications due to its amine functionalities that lead to antimicrobial characteristics. Nevertheless, its antimicrobial capability is dependent upon the degree of protonation of amine groups caused by the pH value. Moreover, its mechanical compressive strength may not be high enough for clinical use if not chemically or physically crosslinked. This study utilized a novel chemical crosslinker, mercaptosuccinic acid, to improve its mechanical characteristics. The natural antibacterial agent, cinnamaldehyde, was grafted onto the crosslinked chitosan to improve its antimicrobial capability. Meanwhile, to take advantage of the thiol functionality in the mercaptosuccinic acid, the bactericidal silver nanoparticles were incorporated through silver-thiol covalent bounding. NMR analyses indicated the chitosan was successfully mercaptosuccinic acid-crosslinked and grafted with cinnamaldehyde at different ratios. Combined the results from the mechanical assessment, swelling experiments, antimicrobial assessment, and cytotoxicity assay, the chitosan hydrogel with the highest crosslinked degree and grafted with cinnamaldehyde and silver nanoparticles is of great promise for further clinical uses.

The combinations of alumina particle air abrasion (AA) and a 10-methacryloyloxyidecyl-dihyidrogenphosphate (MDP) primer and a tribochemical silica coating (TSC) and a silane–base primer are contemporary pre-cementation treatments for zirconia restorations for bonding with resin cements. However, the stability of zirconia resists the mechanical or chemical preparations. The purpose of this study was to develop an atmospheric-pressure oxygen plasma (OP)-aided silicatization method to enhance the adhesion of resin cements to zirconia. Zirconia discs were prepared to receive surface treatments of different combinations: (1) AA or TSC (2) with or without OP treatment, and (3) a chemical primer (no primer, silane, or a silane–MDP mixture). The surface morphology, hydrophilicity, and chemical compositions were characterized, and the resin–zirconia bond strengths were examined either after 24 h or a thermocycling test. The results indicated that the OP treatment after the TSC facilitated the homogeneous distribution of silane and crosslinking of silica particles, and effectively improved the hydrophilicity. The OP increased the O and Si and reduced the C elemental contents, while the combination of TSC, OP, and silane induced SiO_x generation. Among the groups, only the TSC-OP–silane treatment effectively enhanced the bond strength and maintained the adhesion after thermocycling. With these results, the OP aided the silicatization protocol effectively, generated silane crosslinking, and resulted in superior resin–zirconia bond strength and durability compared to the current treatments.

Blue light (BL) curing on dental resin composites results in gradient polymerization. By incorporating upconversion phosphors (UP) in resin composites, near-infrared (NIR) irradiation may activate internal blue emission and a polymerization reaction. This study was aimed to evaluate the competency of the NIR-to-BL upconversion luminance in polymerizing dental composites and to assess the appropriate UP content and curing protocol. NaYF₄ (Yb³⁺/Tm³⁺ co-doped) powder exhibiting 476-nm blue emission under 980-nm NIR was adapted and ball-milled for 4–8 h to obtain different particles. The bare particles were assessed for their emission intensities, and also added into a base composite Z100 (3M EPSE) to evaluate their ability in enhancing polymerization under NIR irradiation. Experimental composites were prepared by dispensing the selected powder and Z100 at different ratios (0, 5, 10 wt% UP). These composites were irradiated under different protocols (BL, NIR, or their combinations), and the microhardness at the irradiated surface and different depths were determined. The results showed that unground UP (d50 = 1.9 μm) exhibited the highest luminescence, while the incorporation of 0.4-μm particles obtained the highest microhardness. The combined 20-s BL and 20–120-s NIR significantly increased the microhardness on the surface and internal depths compared to BL correspondents. The 5% UP effectively enhanced the microhardness under 80-s NIR irradiation but was surpassed by 10% UP with longer NIR irradiation. The combined BL-NIR curing could be an effective approach to polymerize dental composites, while the intensity of upconversion luminescence was related to specific UP particle size and content. Incorporation of 5–10% UP facilitates NIR upconversion polymerization on dental composites.

Reducing microbial infections associated with biomedical devices or articles/furniture noted in a hospital or outpatient clinic remains a great challenge to researchers. Due to its stability and low toxicity, the N-halamine compound has been proposed as a potential antimicrobial agent. It can be incorporated into or blended with the FDA-approved biomaterials. Surface grafting or coating of N-halamine was also reported. Nevertheless, the hydrophobic nature associated with its chemical configuration may affect the microbial interactions with the chlorinated N-halamine-containing substrate. In this study, a polymerizable N-halamine compound was synthesized and grafted onto a polyurethane surface via a surface-initiated atom transfer radical polymerization (SI-ATRP) scheme. Further, using the sequential SI-ATRP reaction method, different hydrophilic monomers, namely poly (ethylene glycol) methacrylate (PEGMA), hydroxyethyl methacrylate (HEMA), and [2-(methacryloyloxy) ethyl] dimethyl-(3-sulfopropyl) ammonium hydroxide (SBMA), were also grafted onto the polyurethane (PU) substrate before the N-halamine grafting reaction to change the surface properties of the N-halamine-modified substrate. It was noted that the chains containing the hydrophilic monomer and the polymerizable N-halamine compound were successfully grafted onto the PU substrate. The degree of chlorination was improved with the introduction of a hydrophilic monomer, except the HEMA. All of these hydrophilic monomer-containing N-halamine-modified PU substrates demonstrated a more than 2 log CFU reduction after microbial incubation. In contrast, the surface modified with N-halamine only exhibited significantly less antimicrobial efficacy instead. This is likely due to the synergistic effects caused by the reduced chlorine content, as well as the reduced surface interactions with the microbes.