Oxygen vacancies in crystal have important impacts on the electronic properties of ZnO. With ZnO(2) as precursors, we introduce a high concentration of oxygen vacancies into ZnO successfully. The obtained ZnO exhibits a yellow color, and the absorption edge shifts to longer wavelength. Raman and XPS spectra reveal that the concentration of oxygen vacancies in the ZnO decreased when the samples are annealed at higher temperature in air. It is consistent with the theory calculation. The increasing of oxygen vacancies results in a narrowing bandgap and increases the visible light absorption of the ZnO. The narrowing bandgap can be confirmed by the enhancement of the photocurrent response when the ZnO was irradiated with visible light. The ZnO with oxygen vacancies are found to be efficient for photodecomposition of 2,4-dichlorophenol under visible light irradiation.
The chemical structure and electronic properties of two-dimensional (2D) carbon-supported TiO₂, TiO₂-graphdiyne, and TiO₂-graphene composites have been studied by first-principles density functional theory. Calculation results show that TiO₂(001)-graphdiyne composites possess superior charge separation and oxidation properties, having the longest lifetimes of photoexcited carriers among all of the 2D composites containing TiO₂ of different facets. Our experimental results further proved that TiO₂(001)-graphdiyne composites could be a promising photocatalyst. For photocatalytic degradation of methylene blue, the rate constant of the TiO₂(001)-graphdiyne composite is 1.63 ± 0.15 times that of the pure TiO₂(001) and 1.27 ± 0.12 times that of the TiO₂(001)-graphene composite.
Health-relevant microorganisms present in natural surface waters and engineered treatment systems that are exposed to sunlight can be inactivated by a complex set of interacting mechanisms. The net impact of sunlight depends on the solar spectral irradiance, the susceptibility of the specific microorganism to each mechanism, and the water quality; inactivation rates can vary by orders of magnitude depending on the organism and environmental conditions. Natural organic matter (NOM) has a large influence, as it can attenuate radiation and thus decrease inactivation by endogenous mechanisms. Simultaneously NOM sensitizes the formation of reactive intermediates that can damage microorganisms via exogenous mechanisms. To accurately predict inactivation and design engineered systems that enhance solar inactivation, it is necessary to model these processes, although some details are not yet sufficiently well understood. In this critical review, we summarize the photo-physics, -chemistry, and -biology that underpin sunlight-mediated inactivation, as well as the targets of damage and cellular responses to sunlight exposure. Viruses that are not susceptible to exogenous inactivation are only inactivated if UVB wavelengths (280-320 nm) are present, such as in very clear, open waters or in containers that are transparent to UVB. Bacteria are susceptible to slightly longer wavelengths. Some viruses and bacteria (especially Gram-positive) are susceptible to exogenous inactivation, which can be initiated by visible as well as UV wavelengths. We review approaches to model sunlightmediated inactivation and illustrate how the environmental conditions can dramatically shift the inactivation rate of organisms. The implications of this mechanistic understanding of solar inactivation are discussed for a range of applications, including recreational water quality, natural treatment systems, solar disinfection of drinking water (SODIS), and enhanced inactivation via the use of sensitizers and photocatalysts. Finally, priorities for future research are identified that will further our understanding of the key role that sunlight disinfection plays in natural systems and the potential to enhance this process in engineered systems.
Environmental signicanceThe manuscript provides a comprehensive synthesis of the current understanding of the mechanisms by which sunlight causes damage to microorganisms, ultimately leading to inactivation. This topic is important for understanding the fate and transport of microbiological contaminants in all sunlit surface waters, including fresh and marine ecosystems, as well as engineered treatment systems.
Photocatalysis has attracted a lot of attention owing to its great potential to solving energy and environmental problems. Although great efforts have been made in the last few decades, the poor efficiency still fails to meet the requirement of practical applications. With the aim to improve further the photocatalytic efficiency and promote their practical applications, in this work we reviewed briefly the progress of the strategies on extending the light absorption spectra of photocatalysts from the aspect of solar energy harvesting. Based on the analyses and discussions of photocatalytic performances, and the mechanisms, advantages and disadvantages of these strategies, some perspectives and interpretations of the future development of photocatalysis were proposed based on our own understanding and experience. We hope it will be helpful for our colleagues that work in the field of photocatalysis.
We prepared BiOCl(1-x)Br(x) (x=0-1) solid solutions and characterized their structures, morphologies, and photocatalytic properties by X-ray diffraction, diffuse reflectance spectroscopy, scanning electron microscopy, Raman spectroscopy, photocurrent and photocatalytic activity measurements and also by density functional theory calculations for BiOCl, BiOBr, BiOCl(0.5)Br(0.5). Under visible-light irradiation BiOCl(1-x)Br(x) exhibits a stronger photocatalytic activity than do BiOCl and BiOBr, with the activity reaching the maximum at x=0.5 and decreasing gradually as x is increased toward 1 or decreased toward 0. This trend is closely mimicked by the photogenerated current of BiOCl(1-x)Br(x) , indicating that the enhanced photocatalytic activity of BiOCl(1-x)Br(x) with respect to those of BiOCl and BiOBr originates from the trapping of photogenerated carriers. Our electronic structure calculations for BiOCl(0.5)Br(0.5) with the anion (O(2-), Cl(-), Br(-)) and cation (Bi(3+)) vacancies suggest that the trapping of photogenerated carriers is caused most likely by Bi(3+) cation vacancies, which generate hole states above the conduction band maximum.
A radial stagnation point flow (RSPF) system combined with a microscope was used to determine the deposition kinetics of Cryptosporidium parvum oocysts on quartz surfaces and silica surfaces coated with Suwannee River natural organic matter (SRNOM) in solutions with different ionic strengths. Microscopic evidence of C. parvum oocysts entrapped in the secondary minimum energy well was presented to show that among the entrapped C. parvum oocysts some were washed away by the radial flow and some were able to transfer to deep primary minima and become irreversibly deposited. Experimental data were compared with simulation results obtained by the convective-diffusion equation and Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. The experimental results suggested that surface charge heterogeneity led to a higher attachment efficiency at low ionic strength. In addition, the maximum attachment efficiency was less than 1 at high ionic strength due to steric interaction.
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