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1. The durability of carbon supported Pt nanowire as novel cathode catalyst for a 1.5 kW PEMFC stack [2015]
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BING LI, HIGGINS, Drew C, QIANGFENG XIAO, DAIJUN YANG, CUNMAN ZHNG, MEI CAI, ZHONGWEI CHEN, and JIANXIN MA
- Applied catalysis. B, Environmental. 162:133-140
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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, Electrochimie, Electrochemistry, Cinétique et mécanisme des réactions, Kinetics and mechanism of reactions, Carbone, Carbon, Carbono, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur, Catalyst, Catalizador, Durabilité, Durability, Durabilidad, Dynamique, Dynamics, Dinámica, Electrocatalyse, Electrocatalysis, Electrocatálisis, Nanofil, Nanowires, Protection environnement, Environmental protection, Protección medio ambiente, Support, Soporte, Dynamic drive cycle testing, PEMFCs, PtNW/C electrocatalyst, and Stack
- Abstract
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Carbon supported platinum nanowires (PtNW/C) synthesized by a simple and inexpensive template-free methodology has been used for the first time as a cathode catalyst in a 15 cell with an active area of 250 cm2, 1.5 kW proton exchange membrane fuel cell (PEMFC) stack. Drive cycle testing along with in-situ and ex-situ accelerated degradation testing (ADT) showed that the PtNW/C catalyst exhibited better durability than commercial Pt/C. After a 420 h dynamic drive cycle durability testing, the PEMFC stacks exhibited a performance degradation rate of 14.4% and 17.9% for PtNW/C and commercial Pt/C based cathodes, respectively. It was found that the majority of performance loss was due to degradation of the commercial Pt/C anode materials, resulting from the rapidly changing load frequencies used in the testing protocol, ultimately leading to harsh fuel/air starvation conditions and subsequent Pt nanoparticle growth and agglomeration. Notably, based on post-testing characterization, the structure, electrochemically active surface area (ECSA) and oxygen reduction activity of the PtNW/C cathode catalyst remained unchanged during the drive cycling, indicating its excellent stability under these practical conditions. Conversely, when using commercial Pt/C as a cathode catalyst, significant Pt nanoparticle growth and agglomeration were observed, resulting in the reduced PEMFC stack durability. Therefore, PtNW/C materials are presented as promising replacements to conventional Pt/C as cathode electrocatalysts for PEMFCs, and particularly demonstrate improved stability under the practical conditions encountered for automotive applications.
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PALUDO, Natalia, ALVES, Joana S, ALTMANN, Cintia, AYUB, Marco A. Z, FERNANDEZ-LAFUENTE, Roberto, and RODRIGUES, Rafael C
- Ultrasonics sonochemistry. 22:89-94
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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, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Enzyme immobilisée, Immobilized enzyme, Enzima inmovilizada, Estérification, Esterification, Esterificación, Réaction catalytique, Catalytic reaction, Reacción catalítica, Sonochimie, Sonochemistry, Sonoquímica, Stabilité, Stability, Estabilidad, Synthèse, Synthesis, Síntesis, Tamis moléculaire, Molecular sieve, Tamiz molecular, Ultrason, Ultrasound, Ultrasonido, Butyrique acide ester éthyle, Esterification reactions, Lipases, Lipozyme TL-IM, Molecular sieves, and Operational stability
- Abstract
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In this work, the combined use of ultrasound energy and molecular sieves was investigated for the synthesis of ethyl butyrate, ester with mango and banana notes, catalyzed by the immobilized lipase from Thermomyces lanuginosus (Lipozyme TL-IM). Initially, the best concentrations of biocatalysts (35%) and butyric acid (0.7 M) were tested using ultrasound as an alternative to mechanical agitation. The amount of acid in the reaction could be increased by 2-fold when compared to previous works where mechanical agitation was used. In the next step, substrate molar ratio and reaction temperature were optimized and the best conditions were at their lowest levels: 1:1 (acid:alcohol), and 30 °C, reaching 61% of conversion in 6 h. Molecular sieves (3 A) were added to optimized reaction medium in order to remove the formed water and improve the maximum yield. The reaction yield increased 1.5 times, reaching 90% of conversion in 6 h, when 60 mg of molecular sieves per mmol of butyric acid was used. Finally, the reuse of Lipozyme TL-IM for the ultrasound-assisted synthesis of ethyl butyrate was verified for 10 batches, without any appreciable loss of activity, whereas in systems using mechanical agitation, the biocatalyst was completely inactivated after 5 batches. These results suggest that the combined use of ultrasound and molecular sieves greatly improve esterification reactions by stabilizing the enzyme and increasing yields.
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LIUJIA LU, FEI TENG, SENTAPAS, DIANYU QI, LINGZHI WANG, and JINLONG ZHANG
- Applied catalysis. B, Environmental. 163:9-15
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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, Matériaux poreux, Porous materials, Composé binaire, Binary compound, Compuesto binario, Composé de métal de transition, Transition element compounds, Matériau poreux, Porous material, Material poroso, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Mésoporosité, Mesoporosity, Mesoporosidad, Oxyde de titane, Titanium oxide, Titanio óxido, Photocatalyse, Photocatalysis, Fotocatálisis, Protection environnement, Environmental protection, Protección medio ambiente, Silice, Silica, Sílice, Synthèse, Synthesis, Síntesis, Photocatalyseur, Photocatalyst, SiO2, Hierarchical macro-mesoporous silica, Si-Cr-Ti, and Visible-light driven photocatalysis
- Abstract
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Hierarchical macro-mesoporous silica materials co-incorporated with Crand Ti were directly synthesized by adopting close-packed array of polystyrene microsphere as hard template for macropore through a simple soaking-calcination way, where Si/Ti ratio was fixed at 200 and Si/Cr ratio was set between 200 and 10. Ti specie is highly dispersed in porous matrix and Cr specie mainly exists as tetra-coordinated CrO3 at higher Si/Cr ratio (Si/Cr ≥ 50), which transforms to a mixture of CrO3 and crystallized hexa-coordinated Cr2O3when Si/Cr ratio is below 50. This highly interconnected porous material co-incorporated with Cr and Ti presents highest visible-light driven photocatalytic activity at Si/Cr = 20 toward degradation of A07. Moreover, macro-mesoporous photocatalyst presents higher activity than those of macroporous and mesoporous ones at the same Si/Cr ratio. The improved visible light driven catalytic activity is mainly attributed to effective metal to metal charge transfer from Cr(VI) to Ti(IV) benefitted from the uniform dispersion of these two species in hierarchical porous silica matrix.
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CHOUDHARY, Hemant, NISHIMURA, Shun, and EBITANI, Kohki
- Applied catalysis. B, Environmental. 162:1-10
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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, Acide carboxylique, Carboxylic acid, Acido carboxílico, Composé de métal de transition, Transition element compounds, Acide formique, Formic acid, Fórmico ácido, Acide lactique, Lactic acid, Láctico ácido, Acide organique, Organic acids, Acido orgánico, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Condition hydrothermale, Hydrothermal condition, Condición hidrotermal, Magnésie, Magnesia, Oxyde de cuivre, Copper oxide, Cobre óxido, Protection environnement, Environmental protection, Protección medio ambiente, Réaction catalytique, Catalytic reaction, Reacción catalítica, Sucre, Sugar, Azúcar, Synthèse, Synthesis, Síntesis, Alkaline hydrothermal synthesis, Copper oxide catalysis, and Sugars
- Abstract
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Design of a suitable catalyst for the conversion of inedible-biomass, a renewable resource, into high-value chemicals is an immense and important area of research in an era of energy crisis. This paper demonstrates batch conversion of sugars into lactic acid (LA) and formic acid (FA) employing a supported copper catalyst. A magnesia-supported copper catalyst was synthesized by a hydrothermal methodology using CTAB as the capping agent (denoted as CuCTAB/MgO). We found that the CuCTAB/MgO not only dramatically boosted the yields of LA and FA from sugars but also decreased the energy demand of the process by decreasing the reaction temperature from 523 K to 393 K. The high yields of LA (70%) in the presence of NaOH and of FA (65%) in the presence of H2O2 were achieved from glucose at 393 K in water using a CuCTAB/MgO catalyst, which could be recycled without any significant loss of activity. The copper catalyst was also found to exhibit excellent activity for the transformation of other sugars. The catalyst was characterized using PXRD, H2-TPR, N2 adsorption-desorption, and other analytical techniques to investigate the active Cu species and propose a plausible mechanistic pathway to LA.
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RUIPING HU, XIN XIAO, SHUNHENG TU, XIAOXI ZUO, and JUNMIN NAN
- Applied catalysis. B, Environmental. 163:510-519
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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, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Dégradation photochimique, Photochemical degradation, Degradación fotoquímica, Microparticule, Microparticle, Micropartícula, Microsphère, Microsphere, Microsfera, Mécanisme, Mechanism, Mecanismo, Oxyde de bismuth, Bismuth oxide, Bismuto óxido, Particule sphérique, Spherical particle, Partícula esférica, Photocatalyse, Photocatalysis, Fotocatálisis, Protection environnement, Environmental protection, Protección medio ambiente, Précurseur, Precursor, Synthèse, Synthesis, Síntesis, Photodegradation mechanism, Visible-light photocatalysis, o-Phenylphenol, p-n junction, and β-Bi2O3/Bi2O2CO3 microspheres
- Abstract
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Novel flower-like heterostructured β-Bi2O3/Bi2O2CO3 microspheres are synthesized by calcining a Bi2O2CO3 self-sacrifice precursor for the visible-light photocatalytic degradation of o-phenylphenol (OPP. is a widely used fungicide and preservative agent). The Bi2O2CO3 microspheres are firstly prepared under hydrothermal conditions, and then converted to Bi2O3 by thermal treatment. With increasing the calcining temperature from 250 to 500 °C, an in situ stepwise decomposition reaction take place during the course of calcination, described as: Bi2O2CO3 → β-Bi2O3/Bi2O2CO3 → β-Bi2O3 → β-Bi2O3/α-Bi2O3 → α-Bi2O3. The β-Bi2O3/Bi2O2CO3 microspheres synthesized at 300 °C exhibit excellent photocatalytic activity under visible-light irradiation, which can degrade 99.8% OPP in 45 min. And the degradation rate of the heterostructured photocatalyst is approximately 2, 2.6, 6, 13, 80, and 827 times higher than that of single P-Bi2O3, mixed β-Bi2O3 and Bi2O2CO3, commercial β-Bi2O3, α-Bi2O3, N-doped TiO2, and Bi2O2CO3, respectively. The superior photoreactivity of the β-Bi2O3/Bi2O2CO3 is attributed to the enhanced charge separation and transfer due to the formation of p-n junction with large heterojunction interface, favorable band gap energy (2.27 eV), relatively high specific surface areas (12.5 m2 g-1), and flower-like hierarchical micro/nano structures. In addition, the degradation intermediates including ethyl phenethyl ether, phenyl acetaldehyde, and phenylacetic acid are identified. And the results also reveal that the photogenerated holes and •O2- radicals are primarily reactive species in the photocatalytic system, which are the key factors responsible for the nearly complete mineralization of OPP.
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FENG GAO, WALTER, Eric D, WASHTON, Nancy M, SZANYI, János, and PEDEN, Charles H. F
- Applied catalysis. B, Environmental. 162:501-514
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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, Ammoniac, Ammonia, Amoníaco, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur, Catalyst, Catalizador, Chabazite, Chabasita, Echange ion, Ion exchange, Cambio iónico, Etat solide, Solid state, Estado sólido, Moteur diesel, Diesel engine, Motor diesel, Oxyde d'azote, Nitrogen oxide, Nitrógeno óxido, Protection environnement, Environmental protection, Protección medio ambiente, Réaction catalytique, Catalytic reaction, Reacción catalítica, Réaction one pot, One pot reaction, Reacción one pot, Réduction chimique, Chemical reduction, Reducción química, Synthèse, Synthesis, Síntesis, Zéolite, Zeolite, Zeolita, SAPO-34, Cu/SAPO-34, Emission control, NOx, and Selective catalytic reduction
- Abstract
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Cu/SAPO-34 catalysts are synthesized using two methods: solid-state ion exchange (SSIE) and one-pot synthesis. SSIE is conducted by calcining SAPO-34/CuO mixtures at elevated temperatures. For the one-pot synthesis method, Cu-containing chemicals (CuO and CuSO4) are added during gel preparation. A high-temperature calcination step is also needed for this latter method. Catalysts are characterized with surface area/pore volume measurements, temperature programmed reduction (TPR), electron paramagnetic resonance (EPR) and nuclear magnetic resonance (NMR) spectroscopies, and scanning electron microscopy (SEM). Catalytic properties are examined using standard ammonia selective catalytic reduction (NH3-SCR) and ammonia oxidation reactions. For Cu/SAPO-34 samples prepared by SSIE, Cu presents both as isolated Cu2+ ions and unreacted CuO. The former are highly active and selective in NH3-SCR, while the latter catalyzes a side reaction; notably, the non-selective oxidation of NH3 above 350°C. Using the one-pot method followed by a high-temperature aging treatment, it is possible to form Cu/SAPO-34 samples with predominately isolated Cu2+ ions at low Cu loadings. However at much higher Cu loadings, isolated Cu2+ ions that bind weakly with the CHA framework and CuO clusters also form. These Cu moieties are very active in catalyzing non-selective NH3 oxidation above 350°C. At very low reaction temperature temperatures (<155°C), standard NH3-SCR over Cu/SAPO-34 catalysts appears to be kinetically limited. However at higher temperatures, multiple rate limiting factors are possible.
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7. Synthesis and application of layered titanates in the photocatalytic degradation of phenol [2015]
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IVANOVA, Svetlana, PENKOVA, Anna, DEL CARMEN HIDALGO, María, NAVIO, José Antonio, ROMERO-SARRIA, Francisca, CENTENO, Miguel Angel, and ODRIOZOLA, José Antonio
- Applied catalysis. B, Environmental. 163:23-29
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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, Alcool, Alcohol, Composé benzénique, Benzenic compound, Compuesto bencénico, Composé de métal de transition, Transition element compounds, Autoorganisation, Self organization, Autoorganización, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Dégradation photochimique, Photochemical degradation, Degradación fotoquímica, Nanotube, Nanotubo, Oxyde de titane, Titanium oxide, Titanio óxido, Phénol, Phenol, Fenol, Phénols, Phenols, Fenoles, Protection environnement, Environmental protection, Protección medio ambiente, Synthèse, Synthesis, Síntesis, Titanate, Titanates, Titanato, Photocatalytic degradation of phenol, and Self organized TiO2 nanotube layers
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This study proposes a direct synthetic route to single titanate sheets through the mild and versatile conditions of the chimie douce. The stages of the production include the complexation of the titanium alkoxide precursor by benzoic acid, the formation of titanium oxo-clusters and their controlled transformation into single sheet titanates during the hydrolysis stage. The resulted material appears to be an excellent precursor for self-organized TiO2 nanotubes formation which presents an excellent activity as photocatalyst in the photo-degradation of phenol.
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VITA, Antonio, CRISTIANO, Giuseppe, ITALIANO, Cristina, PINO, Lidia, and SPECCHIA, Stefania
- Applied catalysis. B, Environmental. 162:551-563
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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, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur, Catalyst, Catalizador, Composé de lanthanide, Lanthanide compound, Lantánido compuesto, Cordiérite, Cordierite, Cordierita, Gaz synthèse, Synthesis gas, Gas síntesis, Méthane, Methane, Metano, Oxyde de cérium, Cerium oxide, Cerio óxido, Protection environnement, Environmental protection, Protección medio ambiente, Reformage vapeur, Steam reforming, Reformación vapor, CeO2, CH4 oxy-steam reforming, Ceria carrier, Cordierite monoliths, Rh Pt Ni catalysts, and Syngas production
- Abstract
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The deposition of catalytic layers as Rh, Pt, Ni (noble metals load equal to 1.5 wt.%, Ni load equal to 7.5 wt.%) on CeO2, over cordierite monoliths (400 cpsi, diameter 1 cm, length 1.5 cm), prepared through a combination of the solution combustion synthesis followed by the Wet Impregnation technique, was investigated. The performances of the structured catalysts were evaluated towards the methane Oxy-Steam Reforming (OSR) reaction. The physicochemical properties of the catalysts at powder level were investigated by X-ray Diffraction, CO chemisorption and nitrogen adsorption (BET), whereas the characteristics of the structured catalysts in terms of thickness and coating integrity were investigated by Scanning Electron Microscopy (SEM), mechanical strength and pressure drop tests. Moreover, the morphology of catalytic layers was investigated by Transmission Electron Microscopy (TEM) on the powder obtained by mechanically scraping the monoliths internal walls. The prepared structured catalysts were tested and compared towards the CH4 OSR reaction varying the temperature (500-800°C), the weight space velocity (WSV = 33,000-400,000 Nml gcat-1 h-1), at fixed molecular oxygen-to-carbon (O/C = 0.55) and steam-to-carbon (S/C = 1.2) molar ratios. The catalytic monoliths presented a uniform thin coating with thickness between 20 and 25 μm, high mechanical strength and low pressure drop. Regarding the catalytic activity, at low WSV all of the structured catalysts showed similar performances. Instead, increasing the WSV, the catalytic monolith loaded with 1.5 wt.% Rh/CeO2 performed slightly better than the other samples, maintaining almost constant the methane conversion and the CO selectivity even at 400,000 Nml gcat-1 h-1.
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HAMEED, Abdul, ASLAM, Muhammad, ISMAIL, Iqbal M. I, SALAH, Numan, and FORNASIERO, Paolo
- Applied catalysis. B, Environmental. 163:444-451
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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, Alcool, Alcohol, Composé benzénique, Benzenic compound, Compuesto bencénico, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Chlorophénol, Chlorophenol, Clorofenol, Composé du chlore, Chlorine compounds, Cloro compuesto, Dégradation, Degradation, Degradación, Minéralisation, Mineralization, Mineralización, Nanocomposite, Nanocompuesto, Oxyde de bismuth, Bismuth oxide, Bismuto óxido, Photocatalyse, Photocatalysis, Fotocatálisis, Phénols, Phenols, Fenoles, Protection environnement, Environmental protection, Protección medio ambiente, Photocatalyseur, Photocatalyst, 2-Chlorophenol degradation, 2-Nitrophenol degradation, Bi2O3 based photocatalyst, and Sunlight photocatalysis
- Abstract
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The photocatalytic mineralization of 2-chlorophenol (2-CP) and 2-nitrophenol (2-NP) was investigated using α-Bi2O3. The experiments were performed both in complete spectrum and in the visible region (420-800 nm) of the sunlight. The materials were fully characterized by means of UV-vis diffuse reflectance spectroscopy (DRS), photoluminescence (PL), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) analysis and field emission scanning electron microscopy (FESEM). α-Bi2O3 showed considerably higher activity for the mineralization of 2-nitrophenol and 2-chlorophenol under natural sunlight exposure, however still appreciable activity was observed in the visible region. Formation of surface nanocomposites Bi2O4-x-Bi2O3 was observed under sunlight irradiation due to the presence of UV light. The sunlight exposed Bi2O3, i.e. Bi2O4-xBi2O3 composite, showed excellent activity for the degradation and mineralization of 2-CP and 2-NP in the visible region of sunlight. A key role of both hydroxyl and superoxide anion radicals was evidenced in the degradation and mineralization processes under sunlight while only hydroxyl radicals were identified as major facilitators under visible light irradiation.
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KATARZYNA MORAWA EBLAGON and EDMAN TSANG, S. C
- Applied catalysis. B, Environmental. 163:599-610
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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, Sciences appliquees, Applied sciences, Energie, Energy, Combustibles, Fuels, Combustibles de remplacement. Production et utilisation, Alternative fuels. Production and utilization, Hydrogène, Hydrogen, Métal transition, Transition metal, Metal transición, Platinoïde, Platinoid, Platinoide, Carbone, Carbon, Carbono, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur, Catalyst, Catalizador, Hydrogénation, Hydrogenation, Hidrogenación, Hydrure, Hydrides, Hidruro, Hétérocycle, Heterocyclic compound, Heterociclo, Liquide, Liquid, Líquido, Protection environnement, Environmental protection, Protección medio ambiente, Ruthénium, Ruthenium, Rutenio, Réaction catalytique, Catalytic reaction, Reacción catalítica, Réactivité chimique, Chemical reactivity, Reactividad química, Stockage hydrogène, Hydrogen storage, Structure, Estructura, Substitution, Substitución, Heterocyclic compounds, Liquid organic hydride, and Ruthenium catalysts
- Abstract
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The effect of the type of heteroatom in the structure on the recyclability of possible candidate compounds for application as LOC (liquid organic carriers) was studied by comparing the rate and selectivity obtained in hydrogenation of carbazole, dibenzothiophene, dibenzofuran and fluorene. The effect of a partial saturation of the compound on its hydrogenation yield and reaction pathway was also considered by studying hydrogenation of 1,2,3,4-tetrahydrocarbazole. Using Ru black catalyst, the rate of hydrogenation was found to decrease in order; dibenzofuran > 1,2,3,4-tetrahydrocarbazole > carbazole » fluorene. No reaction was observed in the hydrogenation of dibenzothiophene under the conditions studied which was attributed to the immediate poisoning of ruthenium metal by sulphur compounds. The rate of hydrogenation of fluorene was around 3 times lower as compared to carbazole and over 8 times lower as compared to that of dibenzofuran under the same reaction conditions. With the exeption of S containing dibenzothiophene, the presence of the heteroatom in the structure was found to be beneficial in terms of increasing the rate of hydrogen loading step. Additionally, a higher reaction rate was obtained in the hydrogenation of the partially saturated 1,2,3,4-tetrahydrocarbazole as compared to the substrate carbazole. The structure and stability of intermediates was found to be significantly influenced by the type and presence of a heteroatom in the structure. A stable octahydro-intermediate was observed only with N-heterocycles, whereas a stable hexahydro-intermediate was produced in the polyaromatic hydrocarbon-fluorene. Additionally, the theoretically obtained lowest total enthalpies using DFT calculations agreed well with the stable intermediates observed experimentally in the hydrogenation of fluorene. Theoretical DFT differences in enthalpies also indicated the products of hydrogenolysis of perhydro-dibenzofuran to be the most favourable products of its hydrogenation, which agreed well with the experimental observations. Overall, taking into account the recyclability of LOC, substitution of carbon with a N heteroatom was demonstrated to be one of the promising approaches to improve the kinetics of the hydrogen loading step.
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HOANG, T. M. C, GEERDINK, B, STURM, J. M, LEFFERTS, L, and SESHAN, K
- Applied catalysis. B, Environmental. 163:74-82
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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, Acide carboxylique, Carboxylic acid, Acido carboxílico, Composé binaire, Binary compound, Compuesto binario, Composé de lanthanide, Lanthanide compound, Lantánido compuesto, Métal transition, Transition metal, Metal transición, Acide acétique, Acetic acid, Acético ácido, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Composé de métal de transition, Transition element compounds, Gazéification, Gasification, Gasificación, Matière volatile, Volatiles, Materia volátil, Nickel, Niquel, Oxyde de cérium, Cerium oxide, Cerio óxido, Protection environnement, Environmental protection, Protección medio ambiente, Reformage vapeur, Steam reforming, Reformación vapor, Zircone, Zirconia, Zircona, CeO2, ZrO2, Ceria-zirconia, and Humin
- Abstract
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Acetic acid and phenols are the major components of the condensable by-products in the low temperature de-volatilisation stage of humin during gasification. Catalytic steam reforming of acetic acid using supported Ni on ceria-zirconia mixed oxide prepared via the hydrothermal route is discussed. The influence of steam reforming temperatures, steam/carbon ratios were studied. The catalyst showed high activity and good stability. Furthermore, activity improvement was achieved with multiple redox cycles as relevant to recycling the catalysts. Characterisation of the fresh and used catalyst by various techniques (e.g., LEIS, Raman spectroscopy, TPO/TPR) revealed the modification of metal-oxygen bond on the support under the steam reforming conditions. It in turn improved the oxygen mobility of the catalyst.
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CHAO HE, JIANWEI ZHENG, KE WANG, HAIQIANG LIN, WANG, Jing-Yuan, and YANHUI YANG
- Applied catalysis. B, Environmental. 162:401-411
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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, Métal transition, Transition metal, Metal transición, Adsorption, Adsorción, Carbone, Carbon, Carbono, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Catalyseur mixte, Mixed catalyst, Catalizador mixto, Gaz à l'eau, Water gas, Gas con agua, Glycérol, Glycerol, Glicerol, Hydrogène, Hydrogen, Hidrógeno, Nanotube multifeuillet, Multiwalled nanotube, Nanotubo pared múltiple, Nickel, Niquel, Palladium, Paladio, Platine, Platinum, Platino, Platinoïde, Platinoid, Platinoide, Protection environnement, Environmental protection, Protección medio ambiente, Reformage, Reforming, Reformación, Sorption, Sorción, Support, Soporte, Bimetallic catalyst, CO2 removal, Platinum-nickel, Platinum-palladium, and Water-gas shift
- Abstract
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In this study, multi-walled carbon nanotubes supported Pt and Pt-based bimetallic catalysts were prepared and their catalytic activities were investigated to screen effective and economical catalyst for H2 production in catalytic aqueous phase reforming (CAPR) of glycerol. Nickel promoted Pt catalyst with optimized Ni:Pt molar ratio afforded highest glycerol conversion rate (81.21%) and carbon conversion to gas (15.3%) although hydrogen gasification ratio (7.2%) was poorer than that of noble metals promoted Pt-based bimetallic catalysts. Adding CaO significantly enhanced the fraction and selectivity of H2 over Pt-Ni catalyst and those of CH4 were reduced to a negligible level, which was possibly attributed to the facilitated water-gas shift reaction and inhibited methanation through in-situ CO2 sorption via carbonation. Results suggested that Pt-Ni bimetallic catalysts improved dehydrogenation-decarboxylation and dehydration-hydrogenation reactions, leading to high glycerol conversions. Introducing CaO further favored C-C bond cleavage towards high H2 yield. The catalytic performance can be completely recovered after regenerating the catalyst and adding sacrificial CaO. In terms of reduced consumption of precious metal catalyst, excellent catalyst performance and hydrothermal stability, combination of Pt-Ni bimetallic catalyst and CaO additive was identified as an effective catalytic system for H2 production in CAPR of glycerol.
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SAFAEI-GHOMI, Javad and AKBARZADEH, Zeinab
- Ultrasonics sonochemistry. 22:365-370
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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, Catalyse hétérogène, Heterogeneous catalysis, Catálisis heterogénea, Chimie verte, Green chemistry, Química verde, Iodure de cuivre, Copper iodide, Cobre ioduro, Nanoparticule, Nanoparticle, Nanopartícula, Protection environnement, Environmental protection, Protección medio ambiente, Réaction catalytique, Catalytic reaction, Reacción catalítica, Sonochimie, Sonochemistry, Sonoquímica, Synthèse, Synthesis, Síntesis, Ultrason, Ultrasound, Ultrasonido, Couplage de Sonogashira, Aryl ethynyl linked triarylamines, Cul nanoparticles, Sonogashira coupling, and Ultrasonic irradiation
- Abstract
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A simple and green method was performed to the preparation of copper iodide nanoparticles by ultrasound approach. Consequently the synthesis of aryl ethynyl linked triarylamines was carried out through the Sonogashira coupling between iodo-substituted triarylamine and aryl acetylenes in the presence of CuI nanoparticles/Pd(PPh3)2Cl2 as an efficient catalytic system and triethylamine as the base under ultrasonic irradiation. Good to excellent yields of products and short reaction times are some of the important advantages of this solvent free protocol which were attained by both nano CuI and ultrasound conditions.
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14. 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
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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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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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