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1.
A series of MoO3 doped Fe2O3 catalysts prepared by the co-precipitation method were investigated in the selective catalytic reduction of NO by NH3 (NH3-SCR). The catalysts displayed excellent catalytic activity from 225 to 400°C and high tolerance to SO2/H2O poisoning at 300°C. To characterize the catalysts the N2-BET, XRD, Raman, NO-TPD, NH3-TPD and in situ DRIFTS were carried out. It was found that the main reason explaining a high NH3-SCR performance might be the synergistic effect between Fe and Mo species in the catalyst that could enhance the dispersion of Fe2O3 and increase NH3 adsorption on the catalyst surface.  相似文献   

2.
Selective catalytic reduction (SCR) with ammonia has been considered as the most promising technology, as its effect deals with the NOX. Novel Fe-doped V2O5/TiO2 catalysts were prepared by sol–gel and impregnation methods. The effects of iron content and reaction temperature on the catalyst SCR reaction activity were explored by a test device, the results of which revealed that catalysts could exhibit the best catalytic activity when the iron mass ratio was 0.05%. It further proved that the VTiFe (0.05%) catalyst performed the best in denitration and its NOX conversion reached 99.5% at 270 °C. The outcome of experimental procedures: Brunauer–Emmett–Teller surface area, X-ray powder diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, temperature-programmed reduction and adsorption (H2-TPR, NH3-TPD) techniques showed that the iron existed in the form of Fe3+ and Fe2+ and the superior catalytic performance was attributed to the highly dispersed active species, lots of surface acid sites and absorbed oxygen. The modified Fe-doped catalysts do not only have terrific SCR activities, but also a rather broad range of active temperature which also enhances the resistance to SO2 and H2O.  相似文献   

3.
Ce-Ti-W-O x catalysts were prepared and applied to the NH3-selective catalytic reduction (SCR) reaction. The experimental results showed that the Ce-Ti-W-O x catalyst prepared by the hydrothermal method exhibited higher NO conversion than those synthesised via the sol-gel and impregnating methods, while the optimal content of WO3 and molar ratio of Ce/Ti were 20 mass % and 4: 6, respectively. Under these conditions, the catalyst exhibited the highest level of catalytic activity (the NO conversion reached values higher than 90 %) across a wide temperature range of 225–450°C, with a range of gas hourly space velocity (GHSV) of 40000–140000 h?1. The catalyst also exhibited good resistance to H2O and SO2. The influences of morphology, phase structure, and surface properties on the catalytic performance were investigated by N2 adsorption-desorption measurement, XRD, XPS, H2-TPR, and SEM. It was found that the high efficiency of NO removal was due to the large BET surface area, the amorphous surface species, the change to element valence states, and the strong interaction between Ce, Ti, and W.  相似文献   

4.
Higher alcohol has been considered as a potential fuel additive. Higher alcohol, including C2–C4 alcohol was synthesized by catalytic conversion of syngas (with a ratio of CO/H2?=?1) derived from natural gas over modified Cu/ZnO/Al2O3 catalyst. Modified Cu/ZnO/Al2O3 catalysts promoted by alkali metal (Li) for higher alcohol synthesis (HAS) were prepared at different pH (6, 6.5, 7, 8, and 9) by co-precipitation to control Cu surface area and characterized by N2 physisorption, XRD, SEM, H2-TPR and TPD. The HAS reaction was carried out under a pressure of 45 bar, GHSV of 4000 h?1, ratio of H2/CO?=?1, and temperature ranges of 240 and 280 °C. It was found that the malachite phase of copper causes the size of copper to be small, which is suitable for methanol synthesis. Methanol and HAS share a common catalytic active site and intermediate. It was also found that the productivity to higher alcohol was correlated with Cu surface area.  相似文献   

5.
The effect of calcination temperature on the state of the active component of iron-containing catalysts prepared by the impregnation of silica gel with a solution of FeSO4 and on their catalytic properties in selective H2S oxidation to sulfur was studied. With the use of thermal analysis, XPS, and Mössbauer spectroscopy, it was found that an X-ray amorphous iron-containing compound of complex composition was formed on the catalyst surface after thermal treatment in the temperature range of 400–500°C. This compound contained Fe3+ cations in three nonequivalent positions characteristic of various oxy and hydroxy sulfates and oxide and sulfate groups as anions. Calcination at 600°C led to the almost complete removal of sulfate groups; as a result, the formation of an oxide structure came into play, and it was completed by the production of finely dispersed iron oxide in the ?-Fe2O3 modification (the average particle size of 3.2 nm) after treatment at 900°C. As the calcination temperature was increased from 500 to 700°C, an increase in the catalyst activity in hydrogen sulfide selective oxidation was observed because of a change in the state of the active component. A comparative study of the samples by temperature-programmed sulfidation made it possible to establish that an increase in the calcination temperature leads to an increase in the stability of the iron-containing catalysts to the action of a reaction atmosphere.  相似文献   

6.
Toward achieving selective catalytic reduction of NO x by hydrocarbons at low temperatures (especially lower than 200 °C), C2H2 selective reduction of NO x was explored on H-mordenite (H-MOR) catalysts in dielectric barrier discharge (DBD) plasma. This work reported significant synergistic effects of DBD plasmas and H-MOR catalysts for C2H2 selective reduction of NO x at low temperatures (100–200 °C ) and across a wide range of O2 content (0–15%). At 100 °C, NO x conversions were 3.3, 11.6 and 66.7% for the plasma alone, catalyst alone and in-plasma catalysis (IPC) cases (with a reactant gas mixture of 500 ppm NO, 500 ppm C2H2, 10% O2 in N2, GHSV = 12,000 h−1 and input energy density of 125 J L 1), respectively. At 200 °C, NO x conversions were 3.8, 54.0 and 91.4% for the above three cases, respectively. Also, strong signals of hydrogen cyanide (HCN) byproduct were observed in the catalyst alone system by an on-line mass spectrometer. By contrast, almost no HCN was detected in the IPC system.  相似文献   

7.
(1.2–8.3)%FeOх/Al2O3 monolith catalysts have been prepared by impregnating alumina with aqueous solutions of iron(III) nitrate and oxalate and have been tested in NH3 oxidation and in the selective decomposition of N2O in mixtures resulting from ammonia oxidation over a Pt–Rh gauze pack under conditions of nitric acid synthesis (800–900°C). In the case of the support calcined at 1200°C, the catalyst is dominated by bulk Fe2O3 particles localized on the Al2O3 surface. The activity of these samples in both reactions decreases with a decreasing active component content, thus limiting the potential of Fe2(C2O4)3 · 5H2O, an environmentally friendlier but poorly soluble compound, as a substitute for Fe(NO3)3 · 9H2O. Decreasing the support calcination temperature to 1000°C or below leads to the formation of a highly defective Fe–Al–O solid solution in the (1.2–2.7)%FeOх/Al2O3 catalysts. The surface layers of the solid solution are enriched with iron ions or stabilize ultrafine FeOх particles. The catalytic activity of these samples in both reactions is close to the activities measured for ~8%FeOх/Al2O3 samples prepared using iron nitrate.  相似文献   

8.
One-pot synthesis of R-1-phenyethylacetate at 70°C was investigated using three different catalysts simultaneously, namely a bimetallic PdZn/Al2O3 as a hydrogenation catalyst, an immobilized lipase as an acylation catalyst and Ru/Al2O3 as a racemization catalyst. The most active bimetallic catalyst was PdZn/Al2O3 calcined at 300°C and reduced at 400°C, whereas the most selective although less active catalyst was the one being calcined and reduced at 500°C. The highest selectivity to R-1-phenylethyl acetate over this catalyst was 32 at 48% conversion. Ru/Al2O3 was confirmed to have a positive effect on the formation of the desired product, although it was not very active in the racemization during one-pot synthesis.  相似文献   

9.
Various amounts and different types of heteropolyacids promoted 5Ag15Cu/Al2O3 catalysts were prepared by impregnation method and analyzed through many techniques. The synthesized catalysts were evaluated for hydrogenolysis of glycerol to propanediols. The results demonstrated that heteropolyacids loading facilitated the reduction, promoted the dispersion, enhanced the acidity, and increased Broensted acid sites of the AgCu catalysts, which benefited the generation of 1,3-propanediol. Compared with phosphotungstic acid and phosphomolybdic acid, silicotungstic acid promoted AgCu catalyst had a better performance for 1,3-propanediol due to the better Cu dispersion and higher Broensted acidity. In addition, when the reaction was performed at 220 °C under 3.5 MPa for 8 h, the chosen 5Ag15Cu-10HSiW/Al2O3 achieved a 69.6% glycerol conversion with 35.6% 1,2-propanediol selectivity and 21.5% 1,3-propanediol selectivity.  相似文献   

10.
One-pot synthesis of R-1-phenyethylacetate at 70°C was investigated using three different catalysts simultaneously, namely a bimetallic PdZn/Al2O3 as a hydrogenation catalyst, an immobilized lipase as an acylation catalyst and Ru/Al2O3 as a racemization catalyst. The most active bimetallic catalyst was PdZn/Al2O3 calcined at 300°C and reduced at 400°C, whereas the most selective although less active catalyst was the one being calcined and reduced at 500°C. The highest selectivity to R-1-phenylethyl acetate over this catalyst was 32 at 48% conversion. Ru/Al2O3 was confirmed to have a positive effect on the formation of the desired product, although it was not very active in the racemization during one-pot synthesis.  相似文献   

11.
Global warming, fossil fuel depletion and fuel price increases have motivated scientists to search for methods for the storage and reduction of the amount of greenhouse gases, especially CO2. The hydrogenation process has been introduced as an emerging method of CO2 capture and convertion into value-added products. In this study, new types of catalysts are introduced for CO2 hydrogenation and are compared based on catalytic activity and product selectivity. The physical properties of the samples are specified using BET. Iron catalysts supported on γ-Al2O3 with different metal promoters (X = Ni, K, Mn, Cu) are prepared through the impregnation method. Moreover, Fe–Ni catalysts supported on HZSM5-Al2O3 and Ce–Al2O3 are synthesized. Samples are reduced by pure H2 and involved in hydrogenation reaction in a fixed bed reactor (H2/CO2 = 3, total pressure = 10 MPa, temperature = 523 K, GHSV = 2000, 1250 nml/min). All catalysts provide high conversion in hydrogenation reactions and the results illustrate that the selectivity of light hydrocarbons is higher than that of methane and CO. It is found that Ni has a promoting effect on the conversion fluctuations throughout the reaction with 66.13% conversion. Using combined supported catalysts leads to enhancing catalytic performance. When Fe–Ni/γ–Al2O3—HZSM5 is utilized, CO2 conversion is 81.66% and the stability of the Fe–Ni catalyst supported on Al2O3 and Ce–Al2O3 furthey improves.  相似文献   

12.
A H3PW12O40/ZrO2 catalyst for effective dimethyl carbonate (DMC) formation via methanol carbonation was prepared using the sol–gel method. X-ray photoelectron spectra showed that reactive and dominant (63%) W(VI) species, in WO3 or H2WO4, enhanced the catalytic performances of the supported ZrO2. The mesoporous structure of H3PW12O40/ZrO2 was identified by nitrogen adsorption–desorption isotherms. In particular, partial sintering of catalyst particles in the duration of methanol carbonation caused a decrease in the Brunauer–Emmett–Teller surface area of the catalyst from 39 to 19 m2/g. The strong acidity of H3PW12O40/ZrO2 was confirmed by the desorption peak observed at 415 °C in NH3 temperature-programmed desorption curve. At various reaction temperatures (T?=?110, 170, and 220 °C) and CO2/N2 volumetric flow rate ratios (CO2/N2?=?1/4, 1/7, and 1/9), the calculated catalytic performances showed that the optimal methanol conversion, DMC selectivity, and DMC yield were 4.45, 89.93, and 4.00%, respectively, when T?=?170 °C and CO2/N2?=?1/7. Furthermore, linear regression of the pseudo-first-order model and Arrhenius equation deduced the optimal rate constant (4.24?×?10?3 min?1) and activation energy (Ea?=?15.54 kJ/mol) at 170 °C with CO2/N2?=?1/7 which were favorable for DMC formation.  相似文献   

13.
A series of Co-modified Ce0.5Zr0.5O2 catalysts with different concentrations of Co (mass %: 0, 2, 4, 6, 8, 10) was investigated for diesel soot combustion. Ce0.5Zr0.5O2 was prepared using the coprecipitation method and Co was loaded onto the oxide using the incipient wetness impregnation method. The activities of the catalysts were evaluated by thermogravimetric (TG) analysis and temperature-programmed oxidation (TPO) experiments. The results showed the soot combustion activities of the catalysts to be effectively improved by the addition of Co, 6 % Co/Ce0.5Zr0.5O2 and that the 8 % Co/Ce0.5Zr0.5O2 catalysts exhibited the best catalytic performance in terms of lower soot ignition temperature (Ti at 349°C) and maximal soot oxidation rate temperature (Tm at 358°C). The reasons for the improved activity were investigated by X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), H2 temperature-programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). These results revealed that the presence of Co could lower the reduction temperature due to the synergistic effect between Co and Ce, thereby improving the activity of the catalysts in soot combustion. The 6 % Co catalyst exhibited the best catalytic performance, which could be attributed to the greater amounts of Co3+ and surface oxygen species on the catalyst.  相似文献   

14.
Copper or iron supported on commercially available oxides, such as γ-Al2O3, TiO2 (anatase) and monoclinic tetragonal ZrO2 (mt-ZrO2) were tested as catalysts for selective catalytic oxidation of ammonia into nitrogen and water vapour (NH3-SCO) in the low temperature range. Different commercial oxides were used in this study to determine the influence of the specific surface area, acidic nature of the support and crystalline phases as well as of the type of species and aggregation state of transition metals on the catalytic performance in selective ammonia oxidation. Copper modified oxide supports were found to be more active and selective to nitrogen than catalysts impregnated with iron. Activities of both transition metal modified samples decreased in the following order: mt-ZrO2, TiO2 (anatase), γ-Al2O3. Quantitative total ammonia conversion was achieved with the Cu/ZrO2 catalytic system at 400°C. Characterisation techniques, e.g. H2-temperature programmed reduction, UV-VIS-diffuse reflectance spectroscopy, suggest that easily reducible copper oxide species are important in achieving high catalytic performances at low temperatures.  相似文献   

15.
Palygorskite (PG)-supported manganese oxide catalysts (MnOx/PG) were prepared for the selective catalytic reduction (SCR) of NO with ammonia in the presence of SO2 at low temperature. The influence of gaseous SO2 on the performance of the catalyst was studied by means of specific surface area (Brunauer-Emmett-Teller, BET) analysis, scanning electron microscopy (SEM), thermogravimetric (TG) analysis, temperature-programmed desorption (TPD) and X-ray photoelectron spectroscopy (XPS). The results showed that the SCR activity of Mn10/PG was significantly inhibited by gaseous SO2 at temperatures below 300°C. However, the SCR activity of Mn10/PG was markedly promoted by SO2 in a higher temperature range of 300°C to 500°C. The sulphating of surface active species (MnOx) was suggested to inhibit the oxidation of NH3 to NO leading to enhancement of the SCR activity at a higher temperature range of 300°C to 500°C and decrease in the SCR activity at temperatures below 300°C.  相似文献   

16.
It is shown that palladium–cobalt oxide–cerium catalyst deposited on cordierite catalyzes the reduction of nitrogen(II) oxide with carbon monoxide, and cobalt–iron catalysts in simultaneous reduction of NO + N2O with C3-C4 alkanes retained high activity in the presence of water vapor and sulfur dioxide. The Pd-Co3O4/cordierite catalyst exceeds the Pt-Co3O4/codierite catalyst in the conversion of NO and CO in the reaction mixture CO + NO + O2 + H2O + SO2. Modification of the Pd-Co3O4/cordierite with cerium oxide considerably increases its sulfur resistance.  相似文献   

17.
CuCr2O4 spinel powders were synthesized starting from different chromium sources, namely (i) chromium oxide (α-Cr2O3) and (ii) ammonium dichromate ((NH4)2Cr2O7). The copper source was a Cu(II) carboxylate-type complex. The Cu(II) carboxylate complex was obtained by the redox reaction between Cu(NO3)2·3H2O and 1,3-propanediol (1,3PG) at 130 °C. In the first case (i), we have started from a mixture of α-Cr2O3, Cu(NO3)2·3H2O and 1,3PG that upon heating formed the copper malonate complex, which decomposed around 220 °C forming an oxide mixture (CuO + α-Cr2O3). In the second case (ii), (NH4)2Cr2O7, Cu(NO3)2·3H2O and 1,3PG were homogenously mixed. Heating this mixture at 130 °C resulted, in situ, in the Cu(II) complex. On controlled temperature increase, the violent decomposition of (NH4)2Cr2O7 took place at 180 °C along with the decomposition of the Cu(II) complex, leading to an amorphous oxide mixture of Cr2O3+x and CuO. By annealing the samples in the temperature range 400–1000 °C, the spinel phase (CuCr2O4) was obtained in both cases: (i) at 800 °C and (ii) at 600 °C as a result of the interactions between the precursors used, when the oxide system was amorphous and highly reactive. The presence of CuCr2O4 was highlighted by XRD and FTIR analyses.  相似文献   

18.
Steady State Isotopic Transient Kinetic Analysis (SSITKA) experiments using on-line Mass Spectrometry (MS) and in situ Diffuse Reflectance Infrared Fourier-Transform Spectroscopy (DRIFTS) have been performed to study essential mechanistic aspects of the Selective Catalytic Reduction of NO by H2 under strongly oxidizing conditions (H2-SCR) in the 120–300°C range over a novel 0.1 wt % Pt/MgO-CeO2 catalyst. The N-path of reaction from NO to the N2 gas product was probed by following the 14NO/H2O215NO/H2/O2 switch (SSITKA-MS and SSITKA-DRIFTS) at 1 bar total pressure. It was found that the N-pathway of reaction involves the formation of two active NO x species different in structure, one present on MgO and the other one on the CeO2 support surface. Inactive adsorbed NO x species were also found on both the MgO-CeO2 support and the Pt metal surfaces. The concentration (mol/g cat) of active NO x leading to N2 was found to change only slightly with reaction temperature in the 120–300°C range. This leads to the conclusion that other intrinsic kinetic reasons are responsible for the volcano-type conversion of NO versus the reaction temperature profile observed.  相似文献   

19.
Transition metal catalysts have been considerably used for NH3 decomposition because of the potential application in COx-free H2 generation for fuel cells. However, most transition metal catalysts prepared via traditional synthetic approaches performed the inferior stability due to the agglomeration of active components. Here, we adopted an efficient method, aerosol-assisted self-assembly approach (AASA), to prepare the optimized cobalt-alumina (Co3O4-Al2O3) catalysts. The Co3O4-Al2O3 catalysts exhibited excellent catalytic performance in the NH3 decomposition reaction, which can reach 100% conversion at 600 °C and maintain stable for 72 h at a gaseous hourly space velocity (GHSV) of 18000 cm3 gcat?1 h?1. The catalysts were characterized by various techniques including transmission electron microscope (TEM), scanning electron microscope (SEM), nitrogen sorption, temperature-programmed reduction by hydrogen (H2-TPR), ex-situ/in-situ Raman and ex-situ/in-situ X-ray diffraction (XRD) to obtain the information about the structure and property of the catalysts. H2-TPR and in-situ XRD results show that there is strong interaction between the cobalt and alumina species, which influences the redox properties of the catalysts. It is found that even a low content of alumina (10 at%) is able to stabilize the catalysts due to the adequate dispersion and rational interaction between different components, which ensures the high activity and superior stability of the cobalt-alumina catalysts.  相似文献   

20.
It has been established that oxides of the rare-earth elements with moderate redox potentials (La2O3, CeO2) increased the activity and working stability of Ni-Al2O3/cordierite catalysts in the reactions of deep and partial oxidation of methane. In the presence of the (NiO + La2O3 + Al2O3)/cordierite catalyst the process of carbon dioxide conversion of methane can be intensified by introduction of oxygen into the reaction gas mixture which decreases the temperature to achieve high conversion to 75–100 °C and has practically no effect on selectivity with respect to H2. Translated from Teoreticheskaya i éksperimental'naya Khimiya, Vol. 44, No. 6, pp. 359–364, November–December, 2008.  相似文献   

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