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21. Sonochemical synthesis of Pr-doped ZnO nanoparticles for sonocatalytic degradation of Acid Red 17 [2015]
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KHATAEE, Alireza, KARIMI, Atefeh, AREFI-OSKOUI, Samira, REZA DARVISHI CHESHMEH SOLTANI, HANIFEHPOUR, Younes, SOLTANI, Behzad, and SANG WOO JOO
- Ultrasonics sonochemistry. 22:371-381
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General chemistry, physical chemistry, Chimie générale, chimie physique, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Sonochimie, Ultrasonic chemistry, Etat colloïdal et états dispersés, Colloidal state and disperse state, Etudes physiques et chimiques. Granulométrie. Phénomènes électrocinétiques, Physical and chemical studies. Granulometry. Electrokinetic phenomena, Composé binaire, Binary compound, Compuesto binario, Acide, Acids, Acido, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Colorant, Dyes, Colorante, Dégradation, Degradation, Degradación, Nanoparticule, Nanoparticle, Nanopartícula, Sonochimie, Sonochemistry, Sonoquímica, Sonolyse, Sonolysis, Sonólisis, Synthèse, Synthesis, Síntesis, Textile, Textil, Ultrason, Ultrasound, Ultrasonido, Nanocatalyseur, Nanocatalyst, O Zn, Sonocatalyse, Sonocatalysis, ZnO, Sonochemical synthesis, Textile dye, Ultrasonic degradation, and ZnO nanocatalyst
- Abstract
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Undoped and Pr-doped ZnO nanoparticles were prepared using a simple sonochemical method, and their sonocatalytic activity was investigated toward degradation of Acid Red 17 (AR17) under ultrasonic (US) irradiation. Synthesized nanoparticles were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) techniques. The extent of sonocatalytic degradation was higher compared with sonolysis alone. The decolorization efficiency of sonolysis alone, sonocatalysis with undoped ZnO and 5% Pr-doped ZnO was 24%, 46% and 100% within reaction time of 70 min, respectively. Sonocatalytic degradation of AR17 increased with increasing the amount of dopant and catalyst dosage and decreasing initial dye concentration. Natural pH was favored the sonocatalytic degradation of AR17. With the addition of chloride, carbonate and sulfate as radical scavengers, the decolorization efficiency was decreased from 100% to 65%, 71% and 89% at the reaction time of 70 min, respectively, indicating that the controlling mechanism of sonochemical degradation of AR17 is the free radicals (not pyrolysis). The addition of peroxydisulfate and hydrogen peroxide as enhancer improved the degradation efficiency from 79% to 85% and 93% at the reaction time of 50 min, respectively. The result showed good reusability of the synthesized sonocatalyst.
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KHATAEE, Alireza, SHEYDAEI, Mohsen, HASSANI, Aydin, TASEIDIFAR, Mojtaba, and KARACA, Semra
- Ultrasonics sonochemistry. 22:404-411
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General chemistry, physical chemistry, Chimie générale, chimie physique, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Sonochimie, Ultrasonic chemistry, Argile, Clay, Arcilla, Composé de métal de transition, Transition element compounds, Colorant organique, Organic dye, Colorante orgánico, Dégradation, Degradation, Degradación, Epuration eau usée, Waste water purification, Depuración aguas servidas, Montmorillonite, Montmorilonita, Nanocomposite, Nanocompuesto, Oxyde de titane, Titanium oxide, Titanio óxido, Sonochimie, Sonochemistry, Sonoquímica, Sonolyse, Sonolysis, Sonólisis, Ultrason, Ultrasound, Ultrasonido, Sonocatalyse, Sonocatalysis, Cationic dyes, Modified nanoclay, Sonocatalytic degradation, and Wastewater treatment
- Abstract
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The sonocatalytic performance of the synthesized TiO2/Montmorillonite K10 (TiO2/MMT) nanocomposite was studied in removal of Basic Blue 3 (BB3) from water. The TiO2/MMT nanocomposite was prepared by hydrothermal method. Scanning electron microscope, X-ray diffraction and Fourier transform infrared were used to characterize the synthesized nanocomposite. The average size of TiO2 nanoparticles decreased from 60-80 nm to 40-60 nm through the immobilization of this semiconductor on the surface of MMT. The obtained results indicated that the sonocatalytic activity of TiO2/MMT nanocomposite was higher than that of pure TiO2 nanoparticles and MMT particles. Furthermore, the main influence factors on the sonocatalytic activity such as the BB3 concentration, pH of solution, TiO2/MMT dose, power of ultrasonic generator, and inorganic salts were studied. The intermediates of BB3 degradation during the sonocatalytic process in the presence of the TiO2/MMT nanocomposite have been monitored by gas chromatography-mass spectrometry.
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SOFIANOU, Maria-Veronica, TASSI, Maria, PSYCHARIS, Vassilis, BOUKOS, Nikos, THANOS, Stavros, VAIMAKIS, Tiverios, JIAGUO YU, and TRAPALIS, Christos
- Applied catalysis. B, Environmental. 162:27-33
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Photochimie, Photochemistry, Aldéhyde, Aldehyde, Aldehído, Composé de métal de transition, Transition element compounds, Acétaldéhyde, Acetaldehyde, Acetaldehído, Anatase, Anatasa, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Décomposition, Decomposition, Descomposición, Nanoplaque, Nanoplate, Nanoplaca, Oxydation, Oxidation, Oxidación, Oxyde de titane, Titanium oxide, Titanio óxido, Photocatalyse, Photocatalysis, Fotocatálisis, Protection environnement, Environmental protection, Protección medio ambiente, Synthèse solvothermale, Solvothermal synthesis, Síntesis solvotermal, Acetaldehyde decomposition, Anatase nanoplates, Mn4+/TiO2, NO oxidation, and {0 0 1} facets
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The photocatalytic activity of TiO2 and manganese doped TiO2 nanoplates with various manganese atomic percentages, in the range of 2-7%, was studied. The undoped and doped nanoplates with exposed {0 0 1} facets were produced by a solvothermal method. The crystal structure as well as the shape of the TiO2 and Mn4+/TiO2 anatase nanoparticles was determined with X-ray powder diffraction (XRD) and transmission electron microscopy (TEM). Both techniques revealed that the nanocrystals are in the form of plates. Moreover, the anisotropic peak broadening of the X-ray diffraction patterns was studied using the Rietveld refining method. Chemical analysis of the photocatalyst that was carried out with X-ray photoelectron spectroscopy (XPS) showed the presence of manganese ions in the TiO2 anatase matrix. The Density Functional Theory (DFT) calculations exhibited a decrease in the energy gap and an increase in the density of the electronic stated inside the gap for the doped TiO2. These observations were in agreement with the results of the UV-visible diffuse reflectance spectroscopy (DRS) that demonstrated an adsorption shift towards the visible region for the same samples. The photocatalytic activity of the synthesized catalysts was investigated by the photocatalytic oxidation of the gaseous nitric oxide (NO) and decomposition of the gaseous acetaldehyde (CH3CHO) under visible light irradiation. The optimal concentration of dopant that improves the photocatalytic activity of the nanoplates was determined.
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YOUNG KWANG KIM, SEUNGHOON LEE, JUNGHO RYU, and HYUNWOONG PARK
- Applied catalysis. B, Environmental. 163:584-590
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Photochimie, Photochemistry, Composé de métal de transition, Transition element compounds, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Conversion, Conversión, Déchet, Wastes, Desperdicio, Eau mer, Seawater, Agua mar, Electrode, Electrodes, Electrodo, Energie solaire, Solar energy, Energía solar, Oxyde de titane, Titanium oxide, Titanio óxido, Photocatalyse, Photocatalysis, Fotocatálisis, Protection environnement, Environmental protection, Protección medio ambiente, Rayonnement solaire, Solar radiation, Radiación solar, Réduction chimique, Chemical reduction, Reducción química, Uranium, Uranio, Metal reduction, Nuclear wastes, Photocatalytic, and Superoxide
- Abstract
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Uranium(VI) spiked in natural seawater was photoelectrochemically reduced using porous TiO2 film electrodes at varying potential biases (EbiasS) and pH values. Linear sweep voltammograms of TiO2 electrodes in seawater with U(VI) at pH 8.2 exhibited the characteristic reduction peaks at -0.95 VSCE and anodic peaks at -0.75 VSCE. These peaks shifted anodically and became less pronounced with decreasing pH values from 8.2 to 3. At the natural seawater pH of 8.2, photoelectrochemical (PEC) treatment (Ebias = -1.0VSCE; AM 1.5 G) was found to be considerably more effective in reducing U(VI) than photocatalytic (PC) treatment (without Ebias) and electrochemical (EC) treatment (without irradiation), and even the combination of the two treatment processes. The synergistic effect of the PEC U(VI) reduction varied depending on the EbiasS and pH values, and was further confirmed by the Faradaic efficiency (e), which was close to 100%. Inductively coupled plasma spectroscopy (ICP) and detailed surface analyses of the TiO2 using various techniques (TEM/EDX, SEM/EDX, and XPS) indicated that ∼95% of uranium in the PEC-treated experiment was adsorbed on TiO2 with 57% as U4.6+ and 14% as U4+, whereas ∼98% of uranium in the EC-treated experiment remained in solution, containing 62% as U4.6+ and 12% as U4+. Under certain conditions (e.g., at a pH of 3.0 and/or with N2-purging), no reduction of U(VI) was observed irrespective of the Ebias and irradiation. To further investigate the observed lack of U(VI) reduction, surface chemistry and energetics between TiO2 and U(VI) were studied as a function of pH. Finally, a role of superoxide radicals as an electron shuttle between TiO2 and U(VI) was established as a primary U(VI) reduction mechanism.
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ZABILSKIY, Maxim, DJINOVIC, Petar, ERJAVEC, Boštjan, DRAZIC, Goran, and PINTAR, Albin
- Applied catalysis. B, Environmental. 163:113-122
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Etat colloïdal et états dispersés, Colloidal state and disperse state, Etudes physiques et chimiques. Granulométrie. Phénomènes électrocinétiques, Physical and chemical studies. Granulometry. Electrokinetic phenomena, Composé binaire, Binary compound, Compuesto binario, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur, Catalyst, Catalizador, Composé de lanthanide, Lanthanide compound, Lantánido compuesto, Composé de métal de transition, Transition element compounds, Décomposition, Decomposition, Descomposición, Nanoparticule, Nanoparticle, Nanopartícula, Nanosphère, Nanosphere, Nanosfera, Oxyde d'azote, Nitrogen oxide, Nitrógeno óxido, Oxyde de cérium, Cerium oxide, Cerio óxido, Particule sphérique, Spherical particle, Partícula esférica, Protection environnement, Environmental protection, Protección medio ambiente, Protoxyde d'azote, Nitrogen protoxide, Nitrógeno protóxido, Réaction catalytique, Catalytic reaction, Reacción catalítica, CeO2, CuO, CeO2 nanospheres, CuO-CeO2 catalysts, N2O decomposition, Small CuO clusters, and Synergetic effect
- Abstract
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High surface area CeO2 nanospheres as an active catalyst support were synthesized using glycothermal approach. Different loadings of copper (4, 6, 10 and 15 wt.%) were supported by wet impregnation method. Prepared materials were characterized by means of TEM, SEM-EDX, XRD, UV-Vis diffuse reflectance, N2 adsorption/desorption, DRIFT and H2-TPR techniques, and tested for the catalytic reaction of nitrous oxide decomposition. The best activity in the N2O degradation was found for the sample containing 10 wt.% of Cu that can be attributed to the highest number of small CuO clusters on the catalyst surface. Further increase of copper content strongly affects the dispersion and leads to the formation of less active segregated CuO phase, which was confirmed by XRD, UV-Vis and H2-TPR results. Accordingly to UV-Vis examination and DRIFT analysis using CO as a probe molecule, all solids contain Cu+1 ions which play a crucial role in the N2O decomposition mechanism. The synthesized catalysts were also tested in wet or NO containing atmospheres, where an inhibiting effect takes place and leads to shifting of conversion profiles to higher temperature by 65 and 10 °C, correspondingly. It was found out that the formation of a new, crystalline CuO·3H2O phase occurs in water vapour containing atmosphere, which can result in catalyst deactivation. However, this effect is fully reversible and the catalyst is able to replenish initial activity in dry atmosphere. Potentiality of CuO/CeO2 materials in catalytic N2O decomposition in industrial processes was confirmed by long-term stability tests performed in the period of 50 h in the presence of inhibiting gas components.
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RAY, Suman, MANNA, Priyabrata, and MUKHOPADHYAY, Chhanda
- Ultrasonics sonochemistry. 22:22-29
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General chemistry, physical chemistry, Chimie générale, chimie physique, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Sonochimie, Ultrasonic chemistry, Etat colloïdal et états dispersés, Colloidal state and disperse state, Etudes physiques et chimiques. Granulométrie. Phénomènes électrocinétiques, Physical and chemical studies. Granulometry. Electrokinetic phenomena, Matériaux poreux, Porous materials, Composé binaire, Binary compound, Compuesto binario, Matériau poreux, Porous material, Material poroso, Acide fluoroborique, Fluoroboric acid, Fluorobórico ácido, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur sur support, Supported catalyst, Catalizador sobre soporte, Mésoporosité, Mesoporosity, Mesoporosidad, Nanoparticule, Nanoparticle, Nanopartícula, Silice, Silica, Sílice, Sonication, Sonicación, Sonochimie, Sonochemistry, Sonoquímica, Support catalyseur, Catalyst support, Soporte catalizador, Synthèse, Synthesis, Síntesis, Ultrason, Ultrasound, Ultrasonido, SiO2, Mesoporous silica nanoparticles, Pyrroloacridinones, Sonication mediated synthesis, and Supported HBF4 catalyst
- Abstract
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Fluoroboric acid (HBF4) adsorbed on mesoporous silica nanoparticles of 600 nm dimension was synthesized and characterized by N2 adsorption, HRTEM, EDX, XPS. The applicability of silica-HBF4 was probed through the sonication assisted synthesis of pyrroloacridinones in ecofriendly solvent ethanol. Standard leaching experiment was performed to show that the reaction was heterogeneous with this recyclable catalyst.
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JUAN ZHOU, KE WU, WENJUAN WANG, YUXIANG HAN, ZHAOYI XU, HAIQIN WAN, SHOURONG ZHENG, and DONGQIANG ZHU
- Applied catalysis. B, Environmental. 162:85-92
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Composé binaire, Binary compound, Compuesto binario, Composé de métal de transition, Transition element compounds, Acide, Acids, Acido, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur sur support, Supported catalyst, Catalizador sobre soporte, Composé de lanthanide, Lanthanide compound, Lantánido compuesto, Hydrogénation, Hydrogenation, Hidrogenación, Oxyde de cérium, Cerium oxide, Cerio óxido, Oxyde de zirconium, Zirconium oxide, Zirconio óxido, Phase liquide, Liquid phase, Fase líquida, Protection environnement, Environmental protection, Protección medio ambiente, Réaction catalytique, Catalytic reaction, Reacción catalítica, Réduction chimique, Chemical reduction, Reducción química, Solution solide, Solid solution, Solución sólida, CeO2, ZrO2, CeO2-ZrO2 solid solutions, Liquid-phase catalytic hydrogenation, Simultaneous reduction of monochloroacetic acid and bromate, and Supported Pd catalysts
- Abstract
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Palladium catalysts supported on ZrO2, CeO2 and CeO2-ZrO2 solid solutions were prepared using the deposition-precipitation method, and individual and simultaneous reduction of monochloroacetic acid (MCAA) and bromate by liquid-phase catalytic hydrogenation on these catalysts was investigated. The catalysts were characterized by N2 adsorption-desorption, X-ray diffraction, measurement of point of zero charge, X-ray photoelectron spectroscopy and CO chemisorption. Characterization results showed that CeO2-ZrO2 solid solutions with varied Ce/Zr ratios had nearly identical points of zero charge to those of ZrO2 and CeO2. For supported Pd catalysts, the binding energy of Pd 3d5/2 of Pd/CeO2 was found to be higher than that of Pd/ZrO2, indicative of a stronger metal-support interaction in the former. Given a similar Pd loading, Pd dispersion of Pd/Ce1-xZrxO2 first increased and then decreased with CeO2 content, and the highest Pd dispersion was observed on Pd(0.86)/Ce0.8Zr0.2O2. Accordingly, Pd/Ce1-xZrxO2 exhibited much higher catalytic activities than Pd/ZrO2 at a Pd loading amount of around 0.85 wt.%, and the highest activity was identified on Pd(0.86)/Ce0.8Zr0.2O2 for individual reduction of bromate and MCAA. The turnover frequencies of Pd(0.86)/Ce0.8Zr0.2O2 for the reduction of bromate and MCAA were 0.69 and 0.23 s-1, respectively, which were one order of magnitude higher than the supported Pd catalysts previously reported. For the simultaneous reduction of MCAA and bromate, the presence of bromate completely suppressed MCAA reduction on Pd(0.85)/ZrO2, while both MCAA and bromate could be effectively reduced on Pd(0.86)/Ce0.8Zr0.2O2. Additionally, the simultaneous reduction of bromate and MCAA proceeded via a competitive reaction mechanism, and the reduction rate of bromate or MCAA was negatively correlated to the competitor concentration.
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HU, S. W, YANG, L. W, TIAN, Y, WEI, X. L, DING, J. W, ZHONG, J. X, and CHU, P. K
- Applied catalysis. B, Environmental. 163:611-622
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Photochimie, Photochemistry, Electrochimie, Electrochemistry, Photoélectrochimie. Electrochimiluminescence, Photoelectrochemistry. Electrochemiluminescence, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Dopage, Doping, Graphite, Grafito, In situ, Nanostructure, Nanoestructura, Nitrure de carbone, Carbon nitrides, Photocatalyse, Photocatalysis, Fotocatálisis, Photoélectrochimie, Photoelectrochemistry, Fotoelectroquímica, Protection environnement, Environmental protection, Protección medio ambiente, Nanofeuillet, Nanosheet, Graphite-like carbon nitride, Heterojunction, Mott-Schottky effect, and Nanosheets
- Abstract
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A novel mesoporous ternary photocatalyst consisting of g-C3N4 nanosheets, metallic silver and MoS2 nanosheets is prepared using AgNO3 as a multifunctional modifier during thermal polymerization of melamine and few-layer MoS2 in a simple one-pot process. The gas bubbles from AgNO3 form an extra soft templates to in situ alter the polymerization behavior of melamine, creating thin g-C3N4 nanosheets and large porous structure that exhibit enhanced light absorption. The solution-based, soft-chemical synthesis enables homogeneous inclusion of metallic silver in the g-C3N4 nanosheets and high dispersibility of ultrathin MoS2 nanosheets in the obtained nanocomposite. In situ coupling between metallic silver and g-C3N4 nanosheets produces nanoscale Mott-Schottky effect, provides an effective channel for charge separation and transfer, and tunes energy band of the latter. More importantly, modulated energy band of g-C3N4 nanosheets synergistically expedites the separation and transfer of photogenerated electron-hole pairs at the interface of two-dimensional g-C3N4/MoS2 heterojunction. As a result, the ternary nanocomposite exhibits improved photoelectrochemical performance and photocatalytic activity under simulated sunlight irradiation compared with other reference materials. Our results provide new insights into the design and large-scale production of semiconductor photocatalyst.
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DOS SANTOS XAVIER, Leandro P, RICO-PEREZ, Verónica, HERNANDEZ-GIMENEZ, Ana M, LOZANO-CASTELLO, Dolores, and BUENA-LOPEZ, Agustín
- Applied catalysis. B, Environmental. 162:412-419
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Composé binaire, Binary compound, Compuesto binario, Composé de lanthanide, Lanthanide compound, Lantánido compuesto, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur, Catalyst, Catalizador, Composé de métal de transition, Transition element compounds, Hydrocarbure, Hydrocarbon, Hidrocarburo, Monoxyde de carbone, Carbon monoxide, Carbono monóxido, Néodyme, Neodymium, Neodimio, Oxydation, Oxidation, Oxidación, Oxyde de cérium, Cerium oxide, Cerio óxido, Protection environnement, Environmental protection, Protección medio ambiente, Réaction catalytique, Catalytic reaction, Reacción catalítica, Suie, Soot, Hollín, Zircone, Zirconia, Zircona, CeO2, ZrO2, Ceria-zirconia catalyst, Diesel soot, Hydrocarbons, and Neodymium-ceria catalyst
- Abstract
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Ce0.73-xZr0.27NdxO2 mixed oxides (x ≤ 0.3) were prepared, characterized by XRD, Raman spectroscopy, N2 adsorption isotherms and H2-TPR, and tested for simultaneous CO, propylene, benzene and soot oxidation in a gas mixture containing O2, NOx, H2O, CO2, CO, propylene (model aliphatic hydrocarbon) and benzene (model aromatic hydrocarbon) that simulates a diesel exhaust. Ce-Zr mixed oxide doping with a low atomic fraction of neodymium (0.01 ≤ x ≤ 0.09) promotes the creation of oxygen vacancies, has a minor effect in the BET specific surface areas of the oxides, increases the surface ceria reducibility and has a positive effect in the catalytic activity. On the contrary, higher neodymium atomic fractions (x = 0.2 and 0.3) promote sintering, with a drastic decrease of the BET specific surface area, surface reducibility and catalytic activity. The Ce0.73-xZr0.27NdxO2 catalysts with x ≤ 0.09 are able to accelerate simultaneously soot, propylene and benzene combustion, and as a general trend, the catalytic behavior of Ce0.73Zr0.27O2 is improved by low atomic fraction neodymium doping (0.01 ≤ x ≤ 0.09). These Ce0.73-xZr0.27NdxO2 mixed oxides with 0.01 ≤ x ≤ 0.09 are also able to accelerate CO oxidation in a certain extent, but there is a net production of CO during soot combustion because the oxidation capacity of these oxides is not high enough to oxidize all CO released as soot combustion product.
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MEROUANI, Slimane, HAMDAOUI, Oualid, REZGUI, Yacine, and GUEMINI, Miloud
- Ultrasonics sonochemistry. 22:41-50
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General chemistry, physical chemistry, Chimie générale, chimie physique, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Sonochimie, Ultrasonic chemistry, Bulle, Bubble, Ampolla, Gaz, Gases, Gas, Radical libre, Free radical, Simulation ordinateur, Computer simulation, Simulación computadora, Sonochimie, Sonochemistry, Sonoquímica, Ultrason, Ultrasound, Ultrasonido, Computer simulations, OH radical, Saturating gas, Single-bubble sonochemistry, and Ultrasonic frequency
- Abstract
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Central events of ultrasonic action are the bubbles of cavitation that can be considered as powered microreactors within which high-energy chemistry occurs. This work presents the results of a comprehensive numerical assessment of frequency and saturating gases effects on single bubble sonochemistry. Computer simulations of chemical reactions occurring inside a bubble oscillating in liquid water irradiated by an ultrasonic wave have been performed for a wide range of ultrasonic frequencies (213-1100 kHz) under different saturating gases (O2, air, N2 and H2). For O2 and H2 bubbles, reactions mechanism consisting in 25 reversible chemical reactions were proposed for studying the internal bubble-chemistry whereas 73 reversible reactions were taken into account for air and N2 bubbles. The numerical simulations have indicated that radicals such as ·OH, H·, HO2· and O are created in the bubble during the strong collapse. In all cases, hydroxyl radical (·OH) is the main oxidant created in the bubble. The production rate of the oxidants decreases as the driving ultrasonic frequency increases. The production rate of ·OH radical followed the order O2 > air > N2 > H2 and the order becomes more remarkable at higher ultrasonic frequencies. The effect of ultrasonic frequency on single bubble sonochemistry was attributed to its significant impact on the cavitation process whereas the effects of gases were attributed to the nature of the chemistry produced in the bubble at the strong collapse. It was concluded that, in addition to the gas solubility, the nature of the internal bubble chemistry is another parameter of a paramount importance that controls the overall sonochemical activity in aqueous solutions.
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FENG BIN, XIAOLIN WEI, BO LI, and KWAN SAN HUI
- Applied catalysis. B, Environmental. 162:282-288
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Physicochimie de surface, Surface physical chemistry, Echange d'ions, Ion-exchange, Zéolites: préparations et propriétés, Zeolites: preparations and properties, Atmosphère, Atmosphere, Atmósfera, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur, Catalyst, Catalizador, Combustion, Combustión, Monoxyde de carbone, Carbon monoxide, Carbono monóxido, Protection environnement, Environmental protection, Protección medio ambiente, Réaction catalytique, Catalytic reaction, Reacción catalítica, Zéolite ZSM5, Catalytic activity, Cu-Ce/ZSM-5, and Self-sustained combustion
- Abstract
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The Cu/ZSM-5, Ce/ZSM-5 and Cu-Ce/ZSM-5 catalysts were prepared and characterized in this investigation and the catalytic activity of carbon monoxide (CO) combustion under these catalysts was determined by temperature-programmed oxidation. The activity for the CO combustion follows the decreasing order: Cu-Ce/ZSM-5 > Cu/ZSM-5 > Ce/ZSM-5, indicated by lower ignition, light-off, extinction temperature and broader hysteresis determined via both heating and cooling feeding process. The CO adsorbed on the copper sites to form Cu+-CO complexes, monodentate and bidentate carbonates was considered to be the crucial step for CO catalytic combustion. At the CO concentration ≥5 vol.%, the CO self-sustained combustion was achieved over the Cu-Ce/ZSM-5 catalyst. One reason is due to formation of Cu2+ ions incorporated into cerium oxides, which are more reducible than the copper clusters, minicrystals and bulk CuO particles. Another reason is attributable to the formation of Ce4+/Ce3+ redox couple, which facilitates oxygen transport on the catalyst surface.
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LING ZHANG, WENZHONG WANG, SONGMEI SUN, DONG JIANG, and ERPING GAO
- Applied catalysis. B, Environmental. 162:470-474
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Photochimie, Photochemistry, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Dépôt, Deposition, Depósito, Photocatalyse, Photocatalysis, Fotocatálisis, Protection environnement, Environmental protection, Protección medio ambiente, Dissociation de l'eau, Water splitting, BiOCl, Photo-deposition, Photocatalytic, and Selective transport
- Abstract
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The efficient spatial transport of photo-generated electrons and holes to different facets is critical to construct an efficient solar energy conversion system. BiOCl@Au/MnOx hierarchical structure was fabricated by depositing the Au and MnOx on the {0 0 1} and {1 1 0} crystal facets of BiOCl, respectively. The internal electric field (EIEF) along the 〈0 0 1〉 direct, and strong local electric field (ELEF) induced by the fast formed Au nanoparticles have been proposed as the intrinsic driving force for the spatial separation and transport of charge carriers in the BiOCl semiconductor, which resulted in significant enhancement of solar-driven photocatalytic activity for the pure water splitting without any sacrificial agent. The special structure of selective deposition of redox cocatalysts on the different facets of a single crystal should be promising and intriguing for designing highly efficient solar energy conversion photocatalyst.
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ZHENYI ZHANG, CAO, Shao-Wen, YUSEN LIAO, and CAN XUE
- Applied catalysis. B, Environmental. 162:204-209
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Photochimie, Photochemistry, Etat colloïdal et états dispersés, Colloidal state and disperse state, Etudes physiques et chimiques. Granulométrie. Phénomènes électrocinétiques, Physical and chemical studies. Granulometry. Electrokinetic phenomena, Acide carboxylique, Carboxylic acid, Acido carboxílico, Composé de métal de transition, Transition element compounds, Acide formique, Formic acid, Fórmico ácido, Alliage, Alloys, Aleación, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Décomposition, Decomposition, Descomposición, Electrofilage, Electrospinning, Electrohilado, Hydrogène, Hydrogen, Hidrógeno, Nanofibre, Nanofiber, Nanofibra, Nanoparticule, Nanoparticle, Nanopartícula, Oxyde de titane, Titanium oxide, Titanio óxido, Photocatalyse, Photocatalysis, Fotocatálisis, Protection environnement, Environmental protection, Protección medio ambiente, Résonance plasmon surface, Surface plasmon resonance, AuPd alloy, and Formic acid decomposition
- Abstract
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We present high-yield hydrogen production through selective photocatalytic decomposition of formic acid by using electrospun TiO2 nanofibers decorated with AuPd bimetallic alloy nanoparticles under simulated sunlight irradiation. By using only 5 mg of the AuPd/TiO2 nanofibers containing the 0.75% Au and 0.25% Pd, we could achieve an optimal H2 generation rate of 88.5 μmol h-1 with an apparent quantum yield at 365 nm as 15.6%. which is higher than that of the Pd/TiO2 and Au/TiO2 nanofibers by a factor of 1.6 and 4.5, respectively. The enhanced photocatalytic decomposition of formic acid for H2 generation could be attributed to the stronger electron-sink effect of AuPd alloy nanoparticles, the high selectivity of Pd for the dehydrogenation of formic acid, and the surface plasmon resonance effect of Au. More importantly, we demonstrate that the photocatalytic processes enable re-activation of the AuPd nanoparticles that were poisoned by CO during thermal decomposition of formic acid. As such, the presented AuPd/TiO2 nanofibers are promising materials for re-generation of H2 under mild conditions from liquid storage carrier of hydrogen. .
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YOSHIDA, Hiroshi, WATANABE, Kou, IWASA, Nobuhiro, FUJITA, Shin-Ichiro, and ARAI, Masahiko
- Applied catalysis. B, Environmental. 162:93-97
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Métal transition, Transition metal, Metal transición, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur, Catalyst, Catalizador, Dopage, Doping, Méthanation, Methanation, Metanación, Nickel, Niquel, Platine, Platinum, Platino, Protection environnement, Environmental protection, Protección medio ambiente, Smectite, Esmectita, CO removal, Platinum doping, and Selective methanation
- Abstract
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The selective methanation of CO in a H2-rich gas stream has been investigated with nickel catalysts including synthetic nickel-containing smectite (SM(Ni)) catalysts undoped and doped with platinum in small quantities and conventional nickel catalysts on SiO2, Al2O3, ZrO2, and MgO. The nickel content in SM(Ni) and the nickel loading in the other catalysts were the same, being 35wt.%. The CO conversion with SM(Ni) was smaller than those with the conventional supported nickel catalysts at temperatures of 150-300°C. However, the former showed the higher selectivity to the methanation of CO of >95% at 250°C or below compared to the latter catalysts. The low activity of SM(Ni) was ascribed to a small area of exposed nickel species. The area of exposed nickel species was improved by doping a reduction promoter of platinum to SM(Ni), resulting in an increase in the activity while keeping the high selectivity to the CO methanation. The influence of reduction temperature and platinum loading on the activity and selectivity was investigated.
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35. Selective catalytic reduction of NOx by ammonia over phosphate-containing Ce0.75Zr0.25O2 solids [2015]
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JUN YU, ZHICHUN SI, LEI CHEN, XIAODONG WU, and DUAN WENG
- Applied catalysis. B, Environmental. 163:223-232
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Ammoniac, Ammonia, Amoníaco, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Oxyde d'azote, Nitrogen oxide, Nitrógeno óxido, Oxygène, Oxygen, Oxígeno, Phosphate de zirconium, Zirconium phosphate, Zirconio fosfato, Protection environnement, Environmental protection, Protección medio ambiente, Réaction catalytique, Catalytic reaction, Reacción catalítica, Réduction chimique, Chemical reduction, Reducción química, Solide, Solid, Sólido, Ce0.75Zr0.25O2, Lattice oxygen, and NH3-SCR
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A zirconium phosphate @ Ce0.75Zr0.25O2 (ZP/CZ) catalyst was synthesized by impregnating zirconium phosphates on Ce0.75Zr0.25O2 microspheres. Catalysts with different structures were also synthesized by various methods to illustrate the structure advantage of ZP/CZ catalyst in selective catalytic reduction of NOx by ammonia (NH3-SCR). The catalysts were characterized by scanning electron microscope (SEM), X-ray diffraction (XRD), BET surface area, Infrared (IR) spectra, Ultraviolet-visible (UV-vis) spectroscopy, X-ray photoelectron spectroscopy (XPS), H2-temperature programmed reduction (TPR) and diffuse reflectance infrared Fourier transformed spectra (DRIFTS) of NH3/NOx adsorption. ZP/CZ catalyst presents excellent catalytic activity at 250-450 °C with a good N2 selectivity under high space velocity of 300,000 h-1. Firstly, the zirconium phosphate provides adsorption sites for ammonia on the surface of the catalyst and the cerium sites in the core act as the redox sites for NO oxidation. The pre-combination of zirconium and phosphate can reduce the strong interactions between phosphates and cerium ions. Therefore, the mobility of surface lattice oxygen on Ce0.75Zr0.25O2 catalyst is retained, which is essential to obtain a catalyst with high NH3-SCR activity at low temperatures. Moreover, NH4NO3 has proved to be an important intermediate for the NH3-SCR reaction on the surface of ceria based catalysts. The ZP/CZ catalyst preserves plenty of oxygen vacancies, facilitating the Ce4+ → Ce3+ redox circles and therefore promotes the nitrites/nitrates formation and desorption on catalyst. Two distinct adsorption sites for NH3 and NO, result in a close contact between ads-NH3/NH4+ and ads-NO3-/NO2- species on ZP/CZ catalyst, which can react with NO rapidly with the participation of active surface lattice oxygen.
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QI CAO, RENCHAO CHE, and NAN CHEN
- Applied catalysis. B, Environmental. 162:187-195
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Photochimie, Photochemistry, Etat colloïdal et états dispersés, Colloidal state and disperse state, Etudes physiques et chimiques. Granulométrie. Phénomènes électrocinétiques, Physical and chemical studies. Granulometry. Electrokinetic phenomena, Autoassemblage, Self assembly, Autoensamble, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Dégradation photochimique, Photochemical degradation, Degradación fotoquímica, Nanoparticule, Nanoparticle, Nanopartícula, Photocatalyse, Photocatalysis, Fotocatálisis, Protection environnement, Environmental protection, Protección medio ambiente, Sulfure, Sulfides, Sulfuro, Superréseau, Superlattice, Superred, Synthèse, Synthesis, Síntesis, Cuprous sulfide, Photocatalytic degradation, Scalable synthesis, and Self-assembly
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Size- and shape-tunable Cu2S nanoparticles were successfully synthesized via a facile one-pot solvothermal process and appreciable yields at gram-scale were achieved in every single reaction. By meticulous observation with a high resolution transmission electron microscope, intensively existing atomic-level superlattice structures were identified and perceived as a result of the coexistence of both chalcocite and chalcocite-M phase in as-obtained Cu2S nanoparticles. Further, 3D ordered self-assemblies of pristine Cu2S nanoparticles were obtained by introducing the polar solvent, ethanol, into the non-polar colloidal dispersion systems during the post-treatment process, and thereby the double-superlattice (DSL) nanoparticle systems consisted of both atomic- and particle-level superlattice structures were achieved. And as promising photocatalysts, although the photocatalytic activity was influenced mutually by the size, shape, crystallinity, atomic-level superlattice structures of pristine Cu2S nanoparticles and their self-assembling behavior, the novel structured DSL nanoparticle systems finally demonstrated highly enhanced photocatalytic efficiency towards the degradation of methylene blue.
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LEI ZHAO, WEICHAO MA, JUN MA, GANG WEN, and QIANLIANG LIU
- Ultrasonics sonochemistry. 22:198-204
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General chemistry, physical chemistry, Chimie générale, chimie physique, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Sonochimie, Ultrasonic chemistry, Benzène(nitro), Dégradation, Degradation, Degradación, Ozonation, Ozonization, Ozonización, Ozone, Ozono, Radical hydroxyle, Hydroxyl radicals, Réaction catalytique, Catalytic reaction, Reacción catalítica, Solution aqueuse, Aqueous solution, Solución acuosa, Sonochimie, Sonochemistry, Sonoquímica, Ultrason, Ultrasound, Ultrasonido, Catalytic ozonation, Hydroxyl radical (·OH), Multiple-field ultrasound, and Nitrobenzene
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The synergetic effect between ozone and ultrasound can enhance the degradation of nitrobenzene and removal efficiency of TOC in aqueous solution, and the degradation of nitrobenzene follows the mechanism of hydroxyl radical (.OH) oxidation. Under the same total ultrasonic power input condition, the degradation rate of nitrobenzene (kNB), the volumetric mass transfer coefficient of ozone (kLa), and the initiation rate of .OH (k.OH) increases with introduction of additional ultrasonic field (1-4) in the process of ozone/ultrasound. The increasing amount of ultrasonic fields accelerates the decomposition of ozone, leading to the rapid appearance of the maximum equilibrium value and the decrease in the accumulation concentration of ozone in aqueous solution with the increasing reaction time. The increase in mass transfer of gaseous ozone dissolved into aqueous solution and the acceleration in the decomposition of ozone in aqueous solution synchronously contribute to the increase of kLa. The investigation of mechanism confirms that the increasing amount of ultrasonic fields yields the increase in cavitation activity that improves the mass transfer and decomposition of ozone, resulting in acceleration of .OH initiation, which determines the degradation of nitrobenzene in aqueous solution.
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QINGHUA LI, XIAA JIN, XUWEI YANG, CHANGYANG CHEN, ZIHAN CHEN, YUANCHENG QIN, WEI, Tai-Huei, and WEIFU SUN
- Applied catalysis. B, Environmental. 162:524-531
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Métal transition, Transition metal, Metal transición, Argent, Silver, Plata, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Dopage, Doping, Energie, Energy, Energía, Matériau hybride, Hybrid material, Material híbrido, Protection environnement, Environmental protection, Protección medio ambiente, Rayonnement solaire, Solar radiation, Radiación solar, Transfert électron, Electron transfer, Transferencia electrón, Energy level control, Organic/inorganic hybrid solar cells, Photoexcited electron transfer, and Silver doping
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The photoexcited electron transfer rate represents one of the most important properties required for photovoltaic devices. However, the fabrication of solar cells with a faster electron transfer remains a technological challenge. Regulating the energy level alignment of acceptor-donor system by the incorporation of foreign ions is one of the most promising strategies to achieve this aim. Herein we demonstrate that the incorporation of silver ions into TiO2 nanocrystals results in a remarkable reduction of energy offset between the conduction band edge of acceptor and the lowest unoccupied molecular orbital of donor. In particular, the electron transfer life time was shortened from 30.2 to 18.3 ps, i.e., almost 40% faster than pure TiO2 acceptor, thus leading to a notable enhancement of power conversion efficiency by almost 38% in organic/inorganic hybrid solar cells. The reduction of the 'excess' energy offset accelerates the electron transfer, which is expected to have an important role in applications of solar energy conversion and photon detectors.
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XIN SUN, HAOBO XU, JING SHEN, SHUYUAN GUO, SA SHI, JUHUA DAN, FANG TIAN, YANFENG TIAN, and YE TIAN
- Ultrasonics sonochemistry. 22:7-14
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General chemistry, physical chemistry, Chimie générale, chimie physique, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Physicochimie des réactions induites par rayonnements, particules et ultrasons, Physical chemistry of induced reactions (with radiations, particles and ultrasonics), Sonochimie, Ultrasonic chemistry, Etat colloïdal et états dispersés, Colloidal state and disperse state, Membranes, Acide, Acids, Acido, Détection, Detection, Detección, Mitochondrie, Mitochondria, Mitocondria, Potentiel membrane, Membrane potential, Potencial membrana, Sonochimie, Sonochemistry, Sonoquímica, Thérapie, Therapy, Terapia, Ultrason, Ultrasound, Ultrasonido, 5-Aminolevulinic acid, Macrophage, Mitochondrial membrane potential, Reactive oxygen species, and Sonodynamic therapy
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Reactive oxygen species (ROS) elevation and mitochondrial membrane potential (MMP) loss have been proven recently to be involved in sonodynamic therapy (SDT)-induced macrophage apoptosis and necrosis. This study aims to develop an experimental system to monitor intracellular ROS and MMP in real-time during ultrasonic irradiation in order to achieve optimal effect in SDT. Cultured THP-1 derived macrophages were incubated with 5-aminolevulinic acid (ALA), and then sonicated at different intensities. Intracellular ROS elevation and MMP loss were detected in real-time by fluorospectrophotometer using fluorescence probe DCFH-DA and jc-1, respectively. Ultrasound at low intensities (less than 0.48 W/cm2) had no influence on ROS and MMP in macrophages, whereas at an intensity of 0.48 W/cm2, ROS elevation and MMP loss were observed during ultrasonic irradiation. These effects were strongly enhanced in the presence of ALA. Quantitative analysis showed that ROS elevation and MMP loss monotonically increased with the rise of ultrasonic intensity between 0.48 and 1.16 W/cm2. SDT at 0.48 and 0.84 W/cm2 induced mainly apoptosis in THP-1 macrophages while SDT at 1.16 W/cm2 mainly cell necrosis. This study supports the validity and potential utility of real-time ROS and MMP detection as a dosimetric tool for the determination of optimal SDT.
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QI HUANG, MENGHUA CAO, ZHIHUI AI, and LIZHI ZHANG
- Applied catalysis. B, Environmental. 162:319-326
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General chemistry, physical chemistry, Chimie générale, chimie physique, Environment, Environnement, Sciences exactes et technologie, Exact sciences and technology, Chimie, Chemistry, Chimie generale et chimie physique, General and physical chemistry, Théorie des réactions, cinétique générale. Catalyse. Nomenclature, documentation chimique, informatique chimique, Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry, Catalyse, Catalysis, Alcool, Alcohol, Composé benzénique, Benzenic compound, Compuesto bencénico, Composé binaire, Binary compound, Compuesto binario, Métal transition, Transition metal, Metal transición, Acide, Acids, Acido, Activation, Activación, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Chlorophénol, Chlorophenol, Clorofenol, Composé de métal de transition, Transition element compounds, Composé du chlore, Chlorine compounds, Cloro compuesto, Dégradation, Degradation, Degradación, Echelle nanométrique, Nanometer scale, Fer, Iron, Hierro, Mécanisme, Mechanism, Mecanismo, Nanofil, Nanowires, Oxyde de fer, Iron oxide, Hierro óxido, Oxygène, Oxygen, Oxígeno, Phénols, Phenols, Fenoles, Protection environnement, Environmental protection, Protección medio ambiente, Fe O, Fe2O3, 4-Chlorophenol, Degradation mechanism, Diethylenetriaminepentacetate acid, Molecular oxygen activation, and Nanoscale zero-valent iron
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In this study, an environmentally benign polyaminocarboxylic ligand diethylenetriamine pentacetate (DTPA) was first used to promote the aerobic 4-chlorophenol (4-CP) degradation with Fe@Fe2O3 core-shell nanowires, and then compared with the most used counterpart ethylenediamine tetraacetate (EDTA) of poor biodegradability. Although the 4-CP removal rate in the Fe@Fe2O3/DTPA/Air system was slower owing to the preferential degradation of DTPA, the total organic carbon removal rate in the Fe@Fe2O3/DTPA/4-CP/Air system was much faster than that in the Fe@Fe2O3/EDTA/4-CP/Air system. We interestingly found that hydroxyl radicals could more easily react with DTPA to produce DTPA radicals than with EDTA to produce EDTA radicals. Ligands (DTPA or EDTA) could significantly accelerate the hydroxyl radicals production with Fe@Fe2O3, while more hydroxyl radicals were generated in the Fe@Fe2O3/DTPA/Air system. We also employed gas chromatography-mass spectrometry and ion chromatography to detect organic intermediates and chloride ions to probe the 4-chlorophenol degradation pathways, and found its degradation pathways were dependent on the reactive oxygen species generated in the different systems. This study can clarify the roles of polyaminocarboxylic ligands on the molecular oxygen activation with nanoscale zero-valent iron, and also provide a green chlorophenols removal method.
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