Surface Modification of 3D-Printed PCL/BG Composite Scaffolds via Mussel-Inspired Polydopamine and Effective Antibacterial Coatings for Biomedical Applications.

A wide variety of composite scaffolds with unique geometry, porosity and pore size can be fabricated with versatile 3D printing techniques. In this work, we fabricated 3D-printed composite scaffolds of polycaprolactone (PCL) incorporating bioactive glass (BG) particles (13-93 and 13-93B3 compositions) by using fused deposition modeling (FDM). The scaffolds were modified with a "mussel-inspired surface coating" to regulate biological properties. The chemical and surface properties of scaffolds were analyzed by Fourier transform infrared spectroscopy (FTIR), contact angle and scanning electron microscopy (SEM). Polydopamine (PDA) surface-modified composite scaffolds exhibited attractive properties. Firstly, after the surface modification, the adhesion of a composite coating based on gelatin incorporated with strontium-doped mesoporous bioactive glass (Sr-MBGNs/gelatin) was significantly improved. In addition, cell attachment and differentiation were promoted, and the antibacterial properties of the scaffolds were increased. Moreover, the bioactivity of these scaffolds was also significantly influenced: a hydroxyapatite layer formed on the scaffold surface after 3 days of immersion in SBF. Our results suggest that the promoting effect of PDA coating on PCL-BG scaffolds leads to improved scaffolds for bone tissue engineering.

Boswellia sacra Extract-Loaded Mesoporous Bioactive Glass Nano Particles: Synthesis and Biological Effects.

Bioactive glasses (BGs) are being increasingly considered for numerous biomedical applications. The loading of natural compounds onto BGs to increase the BG biological activity is receiving increasing attention. However, achieving efficient loading of phytotherapeutic compounds onto the surface of bioactive glass is challenging. The present work aimed to prepare novel amino-functionalized mesoporous bioactive glass nanoparticles (MBGNs) loaded with the phytotherapeutic agent Boswellia sacra extract. The prepared amino-functionalized MBGNs showed suitable loading capacity and releasing time. MBGNs (nominal composition: 58 wt% SiO2, 37 wt% CaO, 5 wt% P2O5) were prepared by sol-gel-modified co-precipitation method and were successfully surface-modified by using 3-aminopropyltriethoxysilane (APTES). In order to evaluate MBGNs loaded with Boswellia sacra, morphological analysis, biological studies, physico-chemical and release studies were performed. The successful functionalization and loading of the natural compound were confirmed with FTIR, zeta-potential measurements and UV-Vis spectroscopy, respectively. Structural and morphological evaluation of MBGNs was done by XRD, SEM and BET analyses, whereas the chemical analysis of the plant extract was done using GC/MS technique. The functionalized MBGNs showed high loading capacity as compared to non-functionalized MBGNs. The release studies revealed that Boswellia sacra molecules were released via controlled diffusion and led to antibacterial effects against S. aureus (Gram-positive) bacteria. Results of cell culture studies using human osteoblastic-like cells (MG-63) indicated better cell viability of the Boswellia sacra-loaded MBGNs as compared to the unloaded MBGNs. Therefore, the strategy of combining the properties of MBGNs with the therapeutic effects of Boswellia sacra represents a novel, convenient step towards the development of phytotherapeutic-loaded antibacterial, inorganic materials to improve tissue healing and regeneration.

Facile Synthesis of Gallium (III)-Chitosan Complexes as Antibacterial Biomaterial.

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.

Fabrication and Characterization of Ag-Sr-Substituted Hydroxyapatite/Chitosan Coatings Deposited via Electrophoretic Deposition: A Design of Experiment Study.

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.

Electrophoretic Deposition of Copper(II)-Chitosan Complexes for Antibacterial Coatings.

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.

A nanocomposite prepared from magnetite nanoparticles, polyaniline and carboxy-modified graphene oxide for non-enzymatic sensing of glucose.

The authors report on the synthesis of carboxy functionalized graphene oxide (fGO) decorated with magnetite (Fe3O4) nanoparticles. The resulting nanomaterial was used to prepare a composite with polyaniline (PANI) which was characterized by UV-vis, Fourier transform-infrared and Raman spectroscopies. Its surface morphologies were characterized by atomic force and scanning electron microscopies. A screen-printed carbon electrode was then modified with the nanocomposite to obtain an enzyme-free glucose sensor. The large surface of fGO and Fe3O4 along with the enhanced charge transfer capability of PANI warrant a pronounced electrochemical response (typically measured at 0.18 V versus Ag/AgCl) which is suppressed in the presence of glucose. This reduction of current by glucose was used to design a sensitive method for quantification of glucose. The response of the modified SPCE is linear in the 0.05 µM - 5 mM glucose concentration range, and the lower detection limit is 0.01 µM. Graphical abstract Schematic illustration of in-situ anchoring of Iron oxide on functionalized graphene oxide and synthesis of its polymeric nanocomposite for non-enzymatic detection of Glucose. The nanocomposite modified screen printed interface enabled monitoring of glucose at lower potential with higher precision. GO (graphene oxide), fGO (functionalized graphene oxide), PANI (polyaniline).