A series of antibacterial and antifungal amino acid-derived compounds and their cobalt(II), copper(II), nickel(II), and zinc(II) metal complexes have been synthesized and characterized by their elemental analyses, molar conductances, magnetic moments, and IR, and electronic spectral measurements. Ligands (L1)−(L5) were derived by condensation of β-diketones with glycine, phenylalanine, valine, and histidine and act as bidentate towards metal ions (cobalt, copper, nickel, and zinc) via the azomethine-N and deprotonated-O of the respective amino acid. The stoichiometric reaction between the metal(II) ion and synthesized ligands in molar ratio of M : L (1 : 1) resulted in the formation of the metal complexes of type [M(L)(H2O)4]Cl (where M = Co(II), Cu(II), and Zn(II)) and of M : L (1 : 2) of type [M(L)2(H2O)2] (where M = Co(II), Cu(II), Ni(II), and Zn(II)). The magnetic moment data suggested for the complexes to have an octahedral geometry around the central metal atom. The electronic spectral data also supported the same octahedral geometry of the complexes. Elemental analyses and NMR spectral data of the ligands and their metal(II) complexes agree with their proposed structures. The synthesized ligands, along with their metal(II) complexes, were screened for their in vitro antibacterial activity against four Gram-negative (Escherichia coli, Shigella flexeneri, Pseudomonas aeruginosa, and Salmonella typhi) and two Gram-positive (Bacillus subtilis and Staphylococcus aureus) bacterial strains and for in vitro antifungal activity against Trichophyton longifusus, Candida albicans, Aspergillus flavus, Microsporum canis, Fusarium solani, and Candida glaberata. The results of these studies show the metal(II) complexes to be more antibacterial/antifungal against one or more species as compared to the uncomplexed ligands. The brine shrimp bioassay was also carried out to study their in vitro cytotoxic properties. Five compounds, (3), (7), (10), (11), and (22), displayed potent cytotoxic activity as LD50 = 8.974 × 10−4, 7.022 × 10−4, 8.839 × 10−4, 7.133 × 10−4, and 9.725 × 10−4 M/mL, respectively, against Artemia salina.

Bacterial infection associated with medical implants is a major threat to healthcare. This work reports the fabrication of Copper(II)–Chitosan (Cu(II)–CS) complex coatings deposited by electrophoretic deposition (EPD) as potential antibacterial candidate to combat microorganisms to reduce implant related infections. The successful deposition of Cu(II)–CS complex coatings on stainless steel was confirmed by physicochemical characterizations. Morphological and elemental analyses by scanning electron microscopy (SEM) and energy-dispersive X-ray (EDX) spectroscopy verified the uniform distribution of copper in the Chitosan (CS) matrix. Moreover, homogeneous coatings without precipitation of metallic copper were confirmed by X-ray diffraction (XRD) spectroscopy and SEM micrographs. Controlled swelling behavior depicted the chelation of copper with polysaccharide chains that is key to the stability of Cu(II)–CS coatings. All investigated systems exhibited stable degradation rate in phosphate buffered saline (PBS)–lysozyme solution within seven days of incubation. The coatings presented higher mechanical properties with the increase in Cu(II) concentration. The crack-free coatings showed mildly hydrophobic behavior. Antibacterial assays were performed using both Gram-positive and Gram-negative bacteria. Outstanding antibacterial properties of the coatings were confirmed. After 24 h of incubation, cell studies of coatings confirms that up to a certain threshold concentration of Cu(II) were not cytotoxic to human osteoblast-like cells. Overall, our results show that uniform and homogeneous Cu(II)–CS coatings with good antibacterial and enhanced mechanical stability could be successfully deposited by EPD. Such antibiotic-free antibacterial coatings are potential candidates for biomedical implants.

In this study, silver–strontium-doped hydroxyapatite (AgSr-HA)/chitosan composite coatings were deposited on a 316L stainless steel (SS) substrate via electrophoretic deposition (EPD). The Taguchi design of experiment (DoE) approach was used to optimize the EPD parameters such as the applied voltage, interelectrode spacing, and deposition time. Furthermore, the concentration of AgSr-HA particles in the suspension was also optimized via the DoE approach. DoE results demonstrated that the “homogeneous” coatings were obtained at the deposition time of 7 min, deposition voltage of 20 V, and at a concentration of 5 g/L AgSr-HA particles in the suspension. Scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), antibacterial studies, contact angle, and roughness measurements were performed to characterize the optimized coatings. SEM images confirmed the deposition of chitosan/AgSr-HA on the SS substrate. The wettability studies indicated the hydrophilic nature of the chitosan/AgSr-HA composite coatings, which confirmed that the developed coatings are suitable for biomedical applications, e.g., orthopedics. The average surface roughness of the chitosan/AgSr-HA composite coatings was in a suitable range used to attach the bone marrow stromal cells. Chitosan/AgSr-HA composite coatings showed an effective antibacterial effect against Gram-positive and Gram-negative bacteria. Moreover, the coatings developed apatite crystals on their surface upon immersion in simulated body fluid.

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.

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