We report the covalent functionalization of graphene by photochemical chlorination. The gas-phase photochlorination of graphene, followed by the structural transformation of the C-C bonds from sp(2) to sp(3) configuration, could remove the conducting π-bands and open up a band gap in graphene. X-ray photoelectron spectroscopy revealed that chlorine is grafted to the basal plane of graphene, with about 8 atom % chlorine coverage. Raman spectroscopy, atomic force microscopy, and transmission electron microscopy all indicated that the photochlorinated graphene is homogeneous and nondestructive. The resistance increases over 4 orders of magnitude and a band gap appears upon photochlorination, confirmed by electrical measurements. Moreover, localized photochlorination of graphene can facilitate chemical patterning, which may offer a feasible approach to the realization of all-graphene circuits.
The worldwide emergence of multidrug-resistant (MDR) and extensively drug-resistant (XDR) tuberculosis threatens to make this disease incurable. Drug resistance mechanisms are only partially understood, and whether the current understanding of the genetic basis of drug resistance in M. tuberculosis is sufficiently comprehensive remains unclear. Here we sequenced and analyzed 161 isolates with a range of drug resistance profiles, discovering 72 new genes, 28 intergenic regions (IGRs), 11 nonsynonymous SNPs and 10 IGR SNPs with strong, consistent associations with drug resistance. On the basis of our examination of the dN/dS ratios of nonsynonymous to synonymous SNPs among the isolates, we suggest that the drug resistance-associated genes identified here likely contain essentially all the nonsynonymous SNPs that have arisen as a result of drug pressure in these isolates and should thus represent a near-complete set of drug resistance-associated genes for these isolates and antibiotics. Our work indicates that the genetic basis of drug resistance is more complex than previously anticipated and provides a strong foundation for elucidating unknown drug resistance mechanisms.
The shape-controlled synthesis of nano- and microstructured materials has opened up new possibilities to improve their physical and chemical properties. In this work, new types of Bi(2)WO(6) with complex morphologies, namely, flowerlike, tyre- and helixlike, and platelike shapes, have been controllably synthesized by a facile hydrothermal process. The benefits of the present work also stem from the first report on the transformation of Bi(2)WO(6) from three-dimensional (3D) flowerlike superstructures to 2D platelike structures, and on the formation of tyre- and helixlike Bi(2)WO(6) superstructures. UV/Vis absorption spectra show that the optical properties of Bi(2)WO(6) samples are relevant to their size and shape. More importantly, the photocatalytic activities of Bi(2)WO(6) nano- and microstructures are strongly dependent on their shape, size, and structure for the degradation of Rhodamine B (RhB) under visible-light irradiation. The reasons for the differences in the photocatalytic activities of these Bi(2)WO(6) nano- and microstructures are further investigated.
A novel flower-like Bi 2 WO 6 superstructure was successfully realized by a facile hydrothermal process without any surfactant or template. Based on the evolution of this morphology as a function of hydrothermal time, the formation mechanism was proposed to be as follows: (1) self-aggregation of nanoparticles; (2) formation of crystalline nanoplates by Ostwald ripening; and (3) organization of the in situ-formed nanoplates into spherical superstructures. The pretty flower-like superstructure of Bi 2 WO 6 was retained after calcination at 550 uC for 4 h. Both the uncalcined and calcined Bi 2 WO 6 exhibited excellent visible-light-driven photocatalytic efficiencies for the degradation of Rhodamine B (RhB), up to 84 and 97% within 60 minutes, respectively, which were much higher than those of TiO 2 (P-25) and Bi 2 WO 6 sample prepared by solid-state reaction (SSR-Bi 2 WO 6 ). Close investigation indicated that plenty of pores with different sizes existed in the Bi 2 WO 6 superstructures, which could serve as hierarchical transport paths for small molecules and might greatly improve their photocatalytic activities.
By introducing VO(3)(-) into the reaction system, uniform hierarchical nanostructures of Bi(2)O(3) have been successfully synthesized by a template-free aqueous method at 60-80 degrees C for 6 h. The as-prepared hierarchitectures are composed of 2D nanosheets, which intercross with each other. Based on the electron microscope observations, the growth of such hierarchitectures has been proposed as an Ostwald ripening process followed by self-assembly. The nucleation, growth, and self-assembly of Bi(2)O(3) nanosheets could be readily tuned, which brought different morphologies and microstructures to the final products. Pore-size distribution analysis revealed that both mesopores and macropores existed in the product. UV-vis spectroscopy was employed to estimate the band gap energies of the hierarchical nanostructures. The photocatalytic activities of as-prepared Bi(2)O(3) hierarchitectures were 6-10 times higher than that of the commercial sample, which was evaluated by the degradation of RhB dye under visible light irradiation (lambda>420 nm).
Mycobacterium tuberculosis is a hard-to-eradicate intracellular pathogen that infects one-third of the global population. It can live within macrophages owning to its ability to arrest phagolysosome biogenesis. Autophagy has recently been identified as an effective way to control the intracellular mycobacteria by enhancing phagosome maturation. In the present study, we demonstrate a novel role of miR-155 in regulating the autophagy-mediated anti-mycobacterial response. Both in vivo and in vitro studies showed that miR-155 expression was significantly enhanced after mycobacterial infection. Forced expression of miR-155 accelerated the autophagic response in macrophages, thus promoting the maturation of mycobacterial phagosomes and decreasing the survival rate of intracellular mycobacteria, while transfection with miR-155 inhibitor increased mycobacterial survival. However, macrophage-mediated mycobacterial phagocytosis was not affected after miR-155 overexpression or inhibition. Furthermore, blocking autophagy with specific inhibitor 3-methyladenine or silencing of autophagy related gene 7 (Atg7) reduced the ability of miR-155 to promote autophagy and mycobacterial elimination. More importantly, our study demonstrated that miR-155 bound to the 3′-untranslated region of Ras homologue enriched in brain (Rheb), a negative regulator of autophagy, accelerated the process of autophagy and sequential killing of intracellular mycobacteria by suppressing Rheb expression. Our results reveal a novel role of miR-155 in regulating autophagy-mediated mycobacterial elimination by targeting Rheb, and provide potential targets for clinical treatment.
Single-crystalline bismuth vanadate (BiVO 4 ) microtubes, with novel square cross-sections and flower-like morphology constructed by several tubes radiating from the center, were synthesized by a facile reflux method at 80 °C. No surfactants or templates were involved in the shaping process. The microtubes are of monoclinic structure with a [010] growth direction with a side length of ca. 800 nm and a wall thickness of ca.100 nm. A series of morphology evolutions of BiVO 4 from nanoparticles, to microrods, and then to microtubes have been arrested. The growth mechanism for the BiVO 4 microtubes is proposed to be a dissolutionrecrystallization-induced concentration depletion mechanism, which is different from other micro/nanotubes formed by layered structure materials reported previously. The presence of NaHCO 3 is crucial in forming the tubular structure by the equilibrium of the formation and dissociation of carbonic acid. Optical absorption experiments revealed the BiVO 4 microtubes had strong absorption in the visible light region in addition to the UV light region, and the energy of the band gap was estimated to be 2.36 eV. The as-synthesized microtubes exhibited higher photocatalytic activity under visible light irradiation (λ > 400 nm) than that of the reference sample prepared by solid-state reaction, which may be ascribed to the special single-crystalline tubular structure and/or flower-like morphology.
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