Rational design of metal single-site embedded porous graphitic carbon nitride (P-g-C 3 N 4 ) nanostructures exploiting maximum atom utilization is warranted to enhance the thermal CO oxidation (CO Ox ) reaction. Herein, a facile, green, one-pot, and template-free approach is developed to fabricate the hierarchical porous P-g-C 3 N 4 -crumpled ultrathin nanosheets atomically doped with copper single atoms (Cu−P-g-C 3 N 4 ). Mechanistically, the quick protonation of melamine and pyridine under acidic conditions induces deamination to form melem, which is polycondensed under heating. The interconnected pores, high surface area (240 m 2 g −1 ), and maximized exposed isolated Cu atomic active sites (1.8 wt %) coordinated with nitrogen atom P-g-C 3 N 4 are the salient features of Cu− P-g-C 3 N 4 that endowed complete conversion to CO 2 at 184 °C. In contrast, P-g-C 3 N 4 only converted 3.8% of CO even at 350 °C, implying the electronic effect of Cu single atoms. The abundant Cu-nitrogen moieties can drastically weaken the binding affinity of the CO-oxidation (CO Ox ) intermediates and products, thus accelerating the reaction kinetics at a low temperature. This study may promote the fabrication of P-g-C 3 N 4 doped with various single atoms for the oxidation of CO.
Mycobacterium tuberculosis ( M.tb) has the extraordinary ability to adapt to the administration of antibiotics through the development of resistance mechanisms. By rapidly exporting drugs from within the cytosol, these pathogenic bacteria diminish antibiotic potency and drive the presentation of drug-tolerant tuberculosis (TB). The membrane integrity of M.tb is pivotal in retaining these drug-resistant traits. Silver (Ag) and zinc oxide (ZnO) nanoparticles (NPs) are established antimicrobial agents that effectively compromise membrane stability, giving rise to increased bacterial permeability to antibiotics. In this work, biodegradable multimetallic microparticles (MMPs), containing Ag NPs and ZnO NPs, were developed for use in pulmonary delivery of antituberculous drugs to the endosomal system of M.tb-infected macrophages. Efficient uptake of MMPs by M.tb-infected THP1 cells was demonstrated using an in vitro macrophage infection model, with direct interaction between MMPs and M.tb visualized with the use of electron FIB-SEM tomography. The release of Ag NPs and ZnO NPs within the macrophage endosomal system increased the potency of the model antibiotic rifampicin by as much as 76%, realized through an increase in membrane disorder of intracellular M.tb. MMPs were effective at independently driving membrane destruction of extracellular bacilli located at the exterior face of THP1 macrophages. This MMP system presents as an effective drug delivery vehicle that could be used for the transport of antituberculous drugs such as rifampicin to infected alveolar macrophages, while increasing drug potency. By increasing M.tb membrane permeability, such a system may prove effectual in improving treatment of drug-susceptible TB in addition to M.tb strains considered drug-resistant.
Zinc oxide engineered nanomaterials (ZnO ENMs) are used in a variety of applications worldwide due to their optoelectronic and antibacterial properties with potential contaminant risk to the environment following their disposal. One of the main potential pathways for ZnO nanomaterials to reach the environment is via urban wastewater treatment plants. So far there is no technique that can provide spatiotemporal nanoscale information about the rates and mechanisms by which the individual nanoparticles transform. Fundamental knowledge of how the surface chemistry of individual particles change, and the heterogeneity of transformations within the system, will reveal the critical physicochemical properties determining environmental damage and deactivation. We applied a methodology based on spatially resolved in situ X-ray fluorescence microscopy (XFM), allowing observation of real-time dissolution and morphological and chemical evolution of synthetic template-grown ZnO nanorods (∼725 nm length, ∼140 nm diameter). Core−shell ZnO-ZnS nanostructures were formed rapidly within 1 h, and significant amounts of ZnS species were generated, with a corresponding depletion of ZnO after 3 h. Diffuse nanoparticles of ZnS, Zn 3 (PO 4 ) 2 , and Zn adsorbed to Fe-oxyhydroxides were also imaged in some nonsterically impeded regions after 3 h. The formation of diffuse nanoparticles was affected by ongoing ZnO dissolution (quantified by inductively coupled plasma mass spectrometry) and the humic acid content in the simulated sludge. Complementary ex situ X-ray absorption spectroscopy and scanning electron microscopy confirmed a significant decrease in the ZnO contribution over time. Application of time-resolved XFM enables predictions about the rates at which ZnO nanomaterials transform during their first stages of the wastewater treatment process.
Biopolymer-based hydrogels have several advantages, including robust mechanical, high biocompatibility, and excellent properties. These hydrogels can be ideal wound dressing materials and advantageous to repair and regenerate skin wounds. In this work, we have reported fabricated of composite hydrogels from gelatin and graphene oxide-f unctionalized-bacterial cellulose (synthesized by hydrothermal method) (GO-f-BC) and crosslinked with tetraethyl orthosilicate (TEOS). The hydrogels were characterized using Fourier transform infrared spectroscopy, scanning electron microscopy, atomic force microscopy, and water contact angle analyses to explore functional groups and their interactions, surface morphology, and wetting behavior, respectively. The swelling, biodegradation, and water retention were tested to respond to biofluid. Maximum swelling was exhibited by samle with maximum amount of GO (GBG-4) in all media (aqueous = 1902.83%, PBS = 1546.63%, and electrolyte = 1367.32%). The hemolysis of all hydrogel samples is less than 0.5%, and the blood coagulation time decreased as the hydrogel concentration increased. The composite hydrogels were found to be hemocompatible as they have less than 0.5% hemolysis for all hydrogel samples under in vitro standard conditions. These hydrogels performed unusual antimicrobial activities against Gram (positive and negative) bacterial strains. The cell viability and proliferation were increased with an increased GO amount, and maximum values were found for GBG-4 against fibroblast (3T3) cell lines. The mature and well-adhered cell morphology of 3T3 cells was found against all hydrogel samples. Hence, based on these results findings, these hydrogels would be potential wound dressing skin materials for wound healing applications.
The aim of this study is to compare the graphene produced using a biotechnological method (Escherichia coli) with the graphene produced by Hummers’ method (a chemical method) and to study the effect on the energy consumption and environment. The results indicated that the chemical reduction process has higher energy consumption, approximately 1642 Wh, than the energy consumption of the biotechnological reduction process, which is 5 Wh. The potential of global warming (GWP 100) improved by 71% using the biotechnological route for the production of graphene. Abiotic depletion, the photochemical ozone creation potential, and marine aquatic ecotoxicity potential were improved when the biological route was employed, compared with the chemical route. The eutrophication potential, terrestrial ecotoxicity, and ozone depletion layer changed very little since the main variables involved in the production of graphene oxide and waste management are the same. The biotechnological method can be considered a green technique for the production of graphene, especially given the reduction in the negative effects on global warming, abiotic depletion, the photochemical ozone creation potential, and the marine aquatic ecotoxicity potential.
Fullerene-containing materials have the ability to store and release electrical energy. Therefore, fullerenes may ultimately find use in high-voltage equipment devices or as super capacitors for high electric energy storage due to this ease of manipulating their excellent dielectric properties and their high volume resistivity. A series of structured fullerene (C60) polymer nanocomposites were assembled using the thiol-ene click reaction, between alkyl thiols and allyl functionalized C60 derivatives. The resulting high-density C60-urethane-thiol-ene (C60-Thiol-Ene) networks possessed excellent mechanical properties. These novel networks were characterized using standard techniques, including infrared spectroscopy (FTIR), differential scanning calorimetry (DSC), dynamic mechanical analysis (DMA), and thermal gravimetric analysis (TGA). The dielectric spectra for the prepared samples were determined over a broad frequency range at room temperature using a broadband dielectric spectrometer and a semiconductor characterization system. The changes in thermo-mechanical and electrical properties of these novel fullerene-thiol-ene composite films were measured as a function of the C60 content, and samples characterized by high dielectric permittivity and low dielectric loss were produced. In this process, variations in chemical composition of the networks were correlated to performance characteristics.
Anisotropic polymer/nanoparticle composites display unique mechanical, thermal, electrical, and optical properties depending on confirmation and configuration control of the composing elements. Processes, such as vapor deposition, ice-templating, nanoparticle self-assembly, additive manufacturing, or layer-by-layer casting, are explored to design and control nanoparticle microstructures with desired anisotropy or isotropy. However, limited attempts are made toward nanoparticle patterning during continuous fiber spinning due to the thin-diameter cross section and 1D features. Thus, this research focuses on a new patterning technique to form ordered nanoparticle assembly in layered composite fibers. As a result, distinct layers can be retained with innovative tool design, unique material combinations, and precise rheology control during fiber spinning. The layer multiplyingenabled nanoparticle patterning is demonstrated in a few material systems, including polyvinyl alcohol (PVA)-boron nitride (BN)/PVA, polyacrylonitrile (PAN)-aluminum (Al)/PAN, and PVA-BN/graphene nanoplatelet (GNP)/ PVA systems. This approach demonstrates an unprecedentedly reported fiber manufacturing platform for well-managed layer dimensions and nanoparticle manipulations with directional thermal and electrical properties that can be utilized in broad applications, including structural supports, heat exchangers, electrical conductors, sensors, actuators, and soft robotics.
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