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1.
Phys Chem Chem Phys ; 16(36): 19634-42, 2014 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-25110101

RESUMO

Chemical looping combustion (CLC) is a key technology for oxy-fuel combustion with inherent separation of CO2 from a flue gas, in which oxygen is derived from a solid oxygen carrier. Multi-cycle CLC performance and the product selectivity towards CO2 formation were achieved using mixed oxide of Cu and Mn (CuMn2O4) (Fd3[combining macron]m, a = b = c = 0.83 nm) as an oxygen carrier. CuMn2O4 was prepared by the co-precipitation method followed by annealing at 900 °C using copper(II) nitrate trihydrate and manganese(II) nitrate tetrahydrate as metal precursors. CuMn2O4 showed oxygen-desorption as well as reducibility at elevated temperatures under CLC conditions. The lattice of CuMn2O4 was altered significantly at higher temperature, however, it was reinstated virtually upon cooling in the presence of air. CuMn2O4 was reduced to CuMnO2, Mn3O4, and Cu2O phases at the intermediate stages, which were further reduced to metallic Cu and MnO upon the removal of reactive oxygen from their lattice. CuMn2O4 showed a remarkable activity towards methane combustion reaction at 750 °C. The reduced phase of CuMn2O4 containing Cu and MnO was readily reinstated when treated with air or oxygen at 750 °C, confirming efficient regeneration of the oxygen carrier. Neither methane combustion efficiency nor oxygen carrying capacity was altered with the increase of CLC cycles at any tested time. The average oxygen carrying capacity of CuMn2O4 was estimated to be 114 mg g(-1), which was not altered significantly with the repeated CLC cycles. Pure CO2 but no CO, which is one of the possible toxic by-products, was formed solely upon methane combustion reaction of CuMn2O4. CuMn2O4 shows potential as a practical CLC material both in terms of multi-cycle performance and product selectivity towards CO2 formation.

2.
J Environ Sci (China) ; 25(5): 1023-33, 2013 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-24218834

RESUMO

Pt supported on mesoporous silica SBA-15 was investigated as a catalyst for low temperature selective catalytic reduction (SCR) of NO by C3H6 in the presence of excess oxygen. The prepared catalysts were characterized by means of XRD, BET surface area, TEM, NO-TPD, NO/C3H6-TPO, NH3-TPD, XPS and 27Al MAS NMR. The effects of Pt loading amount, O2/C3H6 concentration, and incorporation of Al into SBA-15 have been studied. It was found that the removal efficiency increased significantly after Pt loading, but an optimal loading amount was observed. In particular, under an atmosphere of 150 ppm NO, 150 ppm C3H6, and 18 vol.% O2, 0.5% Pt/SBA-15 showed remarkably high catalytic performance giving 80.1% NOx reduction and 87.04% C3H6 conversion simultaneously at 140 degrees C. The enhanced SCR activity of Pt/SBA-15 is associated with its outstanding oxidation activities of NO to NO2 and C3H6 to CO2 in low temperature range. The research results also suggested that higher concentration of O2 and higher concentration of C3H6 favored NO removal. The incorporation of Al into SBA-15 improved catalytic performance, which could be ascribed to the enhancement of catalyst surface acidity caused by tetrahedrally coordinated AlO4. Moreover, the catalysts could be easily reused and possessed good stability.


Assuntos
Poluentes Atmosféricos/química , Alcenos/química , Alumínio/química , Óxido Nítrico/química , Platina/química , Dióxido de Silício/química , Poluição do Ar/prevenção & controle , Catálise , Oxirredução , Temperatura
3.
J Environ Sci (China) ; 23(1): 139-44, 2011.
Artigo em Inglês | MEDLINE | ID: mdl-21476353

RESUMO

The adsorption/plasma decomposition with the combination of adsorption honeycomb-sheets and a plasma element is a new technology for small-sized apparatuses to decompose volatile organic compounds (VOCs) at concentrations lower than about 100 ppm. The feasibility of the prototype adsorption/plasma decomposition apparatus was evaluated with the simulated exhausts containing one VOC component and with real exhausts from a painting booth and an adhesion factory. The apparatus decomposed VOCs effectively at the painting booth exhaust but not always satisfactorily at the adhesion factory exhaust. The performance test results with real exhausts were discussed with respect to the concentration and discharge pattern of the exhausts and the basic properties of the system such as cooperation of adsorption and plasma reaction and the concentration dependence of the performance.


Assuntos
Gases em Plasma/química , Reologia/métodos , Reologia/normas , Compostos Orgânicos Voláteis/química , Adsorção , Carbono/análise , Eletrodos , Emissões de Veículos
4.
Inorg Chem ; 49(24): 11362-9, 2010 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-21077663

RESUMO

The relationship between the photocatalytic activity and the arrangement of metal cations was investigated with Sr-Al-Nb-O double perovskite (SAN) synthesized at 1400 °C for various calcination times using a solid state reaction. Transmission electron microscopic observation revealed that SAN particles had a domain structure of completely B-site ordered (Sr(2)AlNbO(6)) and disordered (SrAl(0.5)Nb(0.5)O(3)) phases. The ordered phase fraction was determined using a newly proposed mixed-phase model for the Rietveld refinement and a method using the relative intensity of the superlattice line of powder X-ray diffraction. It turned out that the mass fraction of the ordered phase in SAN calcined at 1400 °C could be controlled by the calcination time as 33% (10 h), 37% (20 h), 44% (30 h), and 48% (50 h). Photocatalytic activities of SAN for the evolution of H(2) and O(2) respectively from aqueous solutions of methanol and AgF decreased with increasing the calcination time, that is, with increasing the fraction of the ordered phase. These results suggested that the photocatalytic activity of ordered Sr(2)AlNbO(6) should be lower than that of disordered SrAl(0.5)Nb(0.5)O(3). This is practically the first report to reveal the photocatalytic activity of SAN as well as the effect of cation ordering in oxides on the photocatalytic activity.

6.
Chem Commun (Camb) ; (17): 1844-5, 2002 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-12271637

RESUMO

Mesoporous carbonaceous materials with relatively high surface area have been synthesized by a new method composed of in situ polymerization of divinylbenzene in the hydrophobic phase of a hexagonally arrayed micelle/silicate nanocomposite and subsequent carbonization and hydrofluoric acid treatments, while rod-like carbons were obtained from a direct incorporation of divinylbenzene into the mesopores of MCM-41.

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