Hydrothermal synthesis of Ag-doped ZnO/sepiolite nanostructured material for enhanced photocatalytic activity.

This work is devoted to the development of Ag-ZnO/sepiolite photocatalysts as novel nanostructured materials by the immobilization of Ag-doped ZnO on the surface of fibrous clay. Herein, innovative Ag-ZnO/sepiolite photocatalysts were successfully prepared through a simple hydrothermal route using diverse Ag dopant concentrations (2 and 5%). Structural, morphological, and optical properties of the obtained photocatalysts were characterized by XRD, TEM, MEB, and DRS-UV-Vis spectroscopy. The results confirmed that Ag-doped ZnO nanoparticles with a diameter of 10-30 nm are homogeneously distributed on the sepiolite fibers' surface. The silver dopant was effectively incorporated into the zinc oxide, leading to a slight distortion of the hexagonal wurtzite structure and a reduction of the bandgap energy with increased silver doping. The photocatalytic activity towards the degradation of methylene blue (MB) dye was analyzed for all the samples under UV-Vis light. Compared to ZnO alone and undoped ZnO/SEP, the Ag-ZnO/SEP5% nanostructured materials exhibited a significantly improved photocatalytic activity, with full decolorization after 4 h of UV-Vis irradiation (60 W). The photocatalysis of organic pollutants matched well with a pseudo-first-order kinetic. The enhanced photocatalytic activity was ascribed to the low bandgap energy (3 eV), the reduction of the recombination of electron hole, and the sepiolite support.

Removal of two anionic reactive textile dyes by adsorption into MgAl-layered double hydroxide in aqueous solutions.

Textile dyes pose a significant challenge for water pollution due to the poor degradability of their complex aromatic structures (e.g., RR-120 and RBB-150). In order to minimize the harmful effects of RR-120 and RBB-150, the capacity of MgAl-layered double hydroxide for removing of these contaminants was studied herein. Batch adsorption experiments were conducted to investigate the effect of various operating parameters, such as solution pH, contact time, dye concentration, and temperature in order to provide optimal conditions for removal. Structural and morphological analyses were used to highlight the assembly and/or interaction LDH-dye. The state of equilibrium of RR-120 and RBB-150 adsorption was pH- and temperature-dependent and followed the pseudo-second-order rate model. Also, the equilibrium adsorption data of both dyes were found to adopt the Langmuir type isotherm model, which assumes a monolayer arrangement in LDH-dye. Furthermore, the effects of four major coexisting and competing mono- and divalent interlayer anions, such as NO3-, Cl-, CO32-, and SO42-, on the uptakes of RR-120 and RBB-150 were studied and the results showed that NO3- anions had insignificant effect on the uptakes of RR-120 and RBB-150 by MgAl. An equivalent study on the presence of both dyes in competitive trial adsorption/desorption from binary aqueous solution was investigated. And finally, the reuse operation of recovered material after dye adsorption was tested in up to 5 cycles of recyclability.

Adsorption of nisin into layered double hydroxide nanohybrids and in-vitro controlled release.

Layered double hydroxide (LDH) nanohybrid intercalated biomolecules, including oligonecluotides, genes and peptides/proteins, have attracted particular attention since they exhibit improved safety and effectiveness as successful delivery biosystems. The current study specifically investigated the adsorption of nisin peptide and precisely the control of the release of the payload. Adsorption occurred from peptide solution in contact with zinc-aluminum LDH at room temperature, looking out over the influence of the Zn2+/Al3+ ratio, the anion exchange capacity, the nature of the intercalated anion, the host matrix, and the host morphology. Higher adsorption was obtained, around 80% of the loaded nisin and successful intercalation was verified by X-ray diffraction. The in-vitro release tests of the nisin from the biohybrid formulation was held over 25days in PBS medium (0.01M, pH7,4) and showed that no burst release phenomenon occurred at the beginning step, in addition, a sustained-time release of nisin was obtained compared with the free nisin. Therefore, these preliminary results are encouraging for the development of bioprotectors based on nisin intercalated LDH and being implemented in the food and medical industries.

Structure and antibacterial activity relationships of native and amyloid fibril lysozyme loaded on layered double hydroxide.

Lysozyme from hen egg white is composed by a unique linear chain of 129 amino acids. It is known to inhibit Gram positive bacteria and to form amyloid fibrils at low pH, under 75°C. This work investigates the effect of the fibrillation and/or adsorption onto a layered double hydroxide material on the antibacterial properties of lysozyme. The kinetics of adsorption follows a behavior of pseudo second order model. The X-ray diffraction and the Fourier transform infrared spectroscopy highlight that adsorption occurs only on the external surface of the material. Interestingly, the amyloid fibrils of lysozyme retain their antibacterial properties when they are adsorbed on the layered double hydroxide; even if their activity is lowered, the active site of the enzyme is not fully denatured and is still accessible. This is confirmed by the study of the tryptophan using time-resolved fluorescence spectroscopy.

Delivery system for berberine chloride based on the nanocarrier ZnAl-layered double hydroxide: Physicochemical characterization, release behavior and evaluation of anti-bacterial potential.

Layered double hydroxide (LDH) has attracted major interest as one of the most versatile drug delivery systems especially for adsorption capacity and/or controlled delivery property of bioactive agents owing to their combining features of biohybrid. ZnAl synthesized layered double hydroxide can offer a platform to immobilize various types of bioactive compounds, particularly berberine chloride (BBC). However, the immobilization reaction of berberine chloride into ZnAl-LDH was performed by direct co-precipitation method at different ratios of BBC/LDH. BBC-ZnAl-LDH biohybrids were characterized in terms of structure, surface morphology, in vitro drug release profile and antibacterial assay against various bacterial cells. The BBC biomolecules were attached by coordinate bond. Structural and microstructural characterization confirms that interaction of BBC with ZnAl-LDH occurs by adsorption rather than intercalation of BBC within LDH layers. The BBC release profiles from BBC-ZnAl-LDH had a longer release duration compared to the physical mixture, and the drug release seemed faster with the low ratio of BBC/LDH. BBC-ZnAl-LDH can be internalized into bacterial cells. In vitro experiments in PBS medium showed that BBC-ZnAl-LDH biohybrid had higher cytotoxicity and inhibitory effects against three pathogenic bacteria; Staphylococcus aureus CIP 543154, Pseudomonas aeruginosa A22 and Bacillus subtilus ILP 1428B upon the drug release profiles and its destructive potential depends on the loading BBC on the LDH layers. Nonetheless these results prove that the prepared BBC-ZnAl-LDH biohybrids retain the anti-bacterial character of the BBC molecules and are therefore potential modified drug delivery system (DDS).

Preparation and optimization of a drug delivery system based on berberine chloride-immobilized MgAl hydrotalcite.

Hydrotalcite (HT), also known as a layered double hydroxide (LDH) compound, has been widely used in past years in the formulation of drugs due to its specific properties including good biocompatibility, null toxicity, high chemical stability and pH-dependent solubility which aid in drug controlled release. In this work, berberine chloride (BBC) class antibacterial agent was immobilized into magnesium-aluminum LDH in order to improve the drug efficiency as well as to achieve the controlled release property. BBC molecules were immobilized into MgAl LDH through a conventional ion exchange reaction and co-precipitation method. The ion-exchange experiments of BBC on MgAl LDH were investigated with particular attention paid to the influence of the layer charge, the nature of the intercalated anion and the morphology. The immobilization efficiency was dependent upon the LDH properties and the immobilization process. Characterization by powder x-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy and contact angle measurements revealed that the interaction of BBC with MgAl LDH occurs by adsorption rather than intercalation of BBC within LDH layers. In vitro anti-bacterial tests were carried out using disc diffusion assay to prove the effectiveness of these novel biohybrid beads as a controlled drug delivery method. Consequently, the BBC-LDH co-precipitated formulation revealed an enhanced anti-bacterial activity compared to the ion-exchanged formulation not only due to an improvement of chemical stability and retained amount of BBC molecules but also due to the release property.