Despite their broad biomedical applications in orthopedics and dentistry, metallic implants are still associated with failures due to their lack of surface biofunctionality, leading to prosthesis-related microbial infections. In order to address this issue, the current study focuses on the fabrication and characterization of a novel type of antibacterial coating based on gallium (III)-chitosan (Ga (III)-CS) complex layers deposited on metallic substrates via electrophoretic deposition (EPD). Aiming for the production of homogeneous and monophasic coatings, a two step-procedure was applied: the first step involved the synthesis of the Ga (III)-CS complex, followed by EPD from suitable solutions in an acetic acid–aqueous solvent. The influence of Ga (III) concentration on the stability of the suspensions was evaluated in terms of zeta potential. Fourier transform infrared (FTIR) and energy dispersive X-ray (EDX) spectroscopic analyses indicated the chelation of CS with Ga (III) within the coatings, while scanning electron microscopy (SEM) confirmed that no additional metallic gallium deposited during EPD. Furthermore, the results demonstrated that the wettability, mechanical properties, swelling ability, and enzymatic degradation of the coatings were affected by the quantity of Ga (III) ions. Colony forming unit (CFU) tests showed a strong synergistic effect between CS and Ga (III) in inhibiting Escherichia coli strain growth compared to control CS samples. An in vitro study with MG-63 cells showed that Ga (III)-containing coatings were not toxic after 24 h of incubation.
In this research work, the fabrication of biphasic composite implants has been investigated. Porous, commercially available pure Ti (50 vol % porosity and pore distributions of 100−200, 250−355, and 355−500 μm) has been used as a cortical bone replacement, while different composites based on a polymer blend (gelatin and alginate) and bioactive glass (BG) 45S5 have been applied as a soft layer for cartilage tissues. The microstructure, degradation rates, biofunctionality, and wear behavior of the different composites were analyzed to find the best possible coating. Experiments demonstrated the best micromechanical balance for the substrate containing 200−355 μm size range distribution. In addition, although the coating prepared from alginate presented a lower mass loss, the composite containing 50% alginate and 50% gelatin showed a higher elastic recovery, which entails that this type of coating could replicate the functions of the soft tissue in areas of the joints. Therefore, results revealed that the combinations of porous commercially pure Ti and composites prepared from alginate/gelatin/45S5 BG are candidates for the fabrication of biphasic implants not only for the treatment of osteochondral defects but also potentially for any other diseases affecting simultaneously hard and soft tissues.
Zein coatings were obtained by electrophoretic deposition (EPD) on commercially pure titanium substrates in an as-received state and after various chemical treatments. The properties of the zein solution, zeta potential and conductivity, at varying pH values were investigated. It was found that the zein content and the ratio of water to ethanol of the solution used for EPD, as well as the process voltage value and time, significantly influence the morphology of coatings. The deposits obtained from the solution containing 150 g/L and 200 g/L of zein and 10 vol % of water and 90 vol % of ethanol, about 4–5 μm thick, were dense and homogeneous. The effect of chemical treatment of the Ti substrate surface prior to EPD on coating adhesion to the substrate was determined. The coatings showed the highest adhesion to the as-received and anodized substrates due to the presence of a thick TiO2 layer on their surfaces and the presence of specific surface features. Coated titanium substrates showed slightly lower electrochemical corrosion resistance than the uncoated one in Ringer’s solution. The coatings showed a well-developed surface topography compared to the as-received substrate, and they demonstrated hydrophilic nature. The present results provide new insights for the further development of zein-based composite coatings for biomedical engineering applications.
The objective of the present work was the development of cathodic electrophoretic deposition (EPD) to obtain composite coatings of mesoporous sol–gel glass (MSGG) particles embedded in a zein matrix on Ti-13Nb-13Zr substrates. To deposit robust and repeatable coatings, a direct current EPD and pulsed direct current EPD as well as the deposition kinetics were investigated, including the deposition yield and deposition rate. The stability of the suspension was determined based on the zeta potential and conductivity. Macroscopically homogeneous coatings with a thickness of about 10 µm and various volume fractions of MSGG were subjected to further examination. Coatings were uniform, exhibiting open porosity and showing excellent adhesion to the substrates. Both zein and MSGG particles revealed an amorphous structure. The coated substrates demonstrated greater resistance to electrochemical corrosion in Ringer's electrolyte in comparison with the virgin (non-coated) substrate. The coatings showed high roughness and moderate hydrophilicity. The incubation of the coated substrates in concentrated 1.5 simulated body fluid (1.5SBF) showed the formation of carbonate hydroxyapatite. The composite coatings showed improved antibacterial properties against gram-negative E. coli and gram-positive S. aureus bacteria compared to pure zein coatings. Electrophoretic MSGG/zein composite coatings should be further investigated in terms of their osteoconductive behavior, to confirm their suitability for medical applications in orthopedics.
Even though antibiotic treatment remains one of the most common tools to handle bacterial infections, the excessive antibiotic concentration at the target site may lead to undesired effects. Aiming at the fabrication of antibiotic-free biomaterials for antibacterial applications, in this work, we propose the synthesis of gallium (III)—chitosan (Ga (III)-CS) complexes with six different gallium concentrations via an in situ precipitation method. Fourier Transform infrared spectroscopy indicated the chelation of chitosan with Ga (III) by peak shifts and changes in the relative absorbance of key spectral bands, while energy-dispersive X-ray spectroscopy indicated the homogenous distribution of the metal ions within the polymer matrix. Additionally, similar to CS, all Ga (III)-CS complexes showed hydrophobic behavior during static contact-angle measurements. The antibacterial property of the complexes against both Gram-negative and Gram-positive bacteria was positively correlated with the Ga (III) concentration. Moreover, cell studies confirmed the nontoxic behavior of the complexes against the human osteosarcoma cell line (MG-63 cells) and mouse embryonic fibroblasts cell line (MEFs). Based on the results of this study, new antibiotic-free antibacterial biomaterials based on Ga (III)-CS can be developed, expanding the scope of CS applications in the biomedical field.
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