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1.
The role of plasma processing on NO x reduction over γ-alumina and a basic zeolite, NaY was examined. During the plasma treatment NO is oxidized to NO 2 and propylene is partially oxidized to CO, CO 2, acetaldehyde, and formaldehyde. With plasma treatment, NO as the NO x gas, and a NaY catalyst, the maximum NO x conversion was 70% between 180 and 230 °C. The activity decreased at higher and lower temperatures. As high as 80% NOx removal over gamma alumina was measured by a chemiluminescent NOx meter with plasma treatment and NO as the NOx gas. For both catalysts a simultaneous decrease in NOx and aldehydes concentrations was observed, which suggests that aldehyde may be important components for NOx reduction in plasma-treated exhaust. 相似文献
2.
The release and reduction of NO x in a NO x storage-reduction (NSR) catalyst were studied with a transient reaction analysis in the millisecond range, which was made possible by the combination of pulsed injection of gases and time resolved time-of-flight mass spectrometry. After an O 2 pulse and a subsequent NO pulse were injected into a pellet of the Pt/Ba/Al 2O 3 catalyst, the time profiles of several gas products, NO, N 2, NH 3 and H 2O, were obtained as a result of the release and reduction of NO x caused by H 2 injection. Comparing the time profiles in another analysis, which were obtained using a model catalyst consisting of a flat 5 nmPt/Ba(NO 3) 2/cordierite plate, the release and reduction of NO x on Pt/Ba/Al 2O 3 catalyst that stored NO x took the following two steps; in the first step NO molecules were released from Ba and in the second step the released NO was reduced into N 2 by H 2 pulse injection. When this H 2 pulse was injected in a large amount, NO was reduced to NH 3 instead of N 2. A only small amount of H2O was detected because of the strong affinity for alumina support. We can analyze the NOx regeneration process to separate two steps of the NOx release and reduction by a detailed analysis of the time profiles using a two-step reaction model. From the result of the analysis, it is found that the rate constant for NOx release increased as temperature increase. 相似文献
3.
NO x reduction with NO 2 as the NO x gas in the absence of plasma was compared to plasma treated lean NO x exhaust where NO is converted to NO 2 in the plasma. Product nitrogen was measured to prove true chemical reduction of NO x to N 2. With plasma treatment, NO as the NO x gas, and a NaY catalyst, the maximum conversion to nitrogen was 50% between 180 and 230 °C. The activity decreased at higher and lower temperatures. At 130 °C a complete nitrogen balance could be obtained, however between 164 and 227 °C less than 20% of the NO x is converted to a nitrogen-containing compound or compounds not readily detected by gas chromatograph (GC) or Fourier transform infrared spectrometer (FT-IR) analysis. With plasma treatment, NO 2 as the NO x gas, and a NaY catalyst, a complete nitrogen balance is obtained with a maximum conversion to nitrogen of 55% at 225 °C. For γ-alumina, with plasma treatment and NO2 as the NOx gas, 59% of the NOx is converted to nitrogen at 340 °C. A complete nitrogen balance was obtained at these conditions. As high as 80% NOx removal over γ-alumina was measured by a chemiluminescent NOx meter with plasma treatment and NO as the NOx gas. When NO is replaced with NO2 and the simulated exhaust gases are not plasma treated, the maximum NOx reduction activity of NaY and γ-alumina decreases to 26 and 10%, respectively. This is a large reduction in activity compared to similar conditions where the simulated exhaust was plasma treated. Therefore, in addition to NO2, other plasma-generated species are required to maximize NOx reduction. 相似文献
4.
The photooxidation of NO with oxygen over Hycom TiO 2 and zeolite (A and Y form zeolite: TiO 2-AZ and TiO 2-YZ) composite catalysts was studied to remove NO x in the atmosphere. The photocatalytic oxidation activity of the titania in the composite catalyst in a proportion of AZ:TiO 2=3:7 is about three times larger than that in the bare titania. The adsorption behaviors of NO and NO 2 for the bare titania sample obey Langmuir adsorption equations of NO and NO 2, respectively. In the titania–zeolite composite catalysts, the adsorption data indicate the increase in the amount of NO adsorption on the TiO 2 phase and the decrease in the amount of NO 2 adsorption, compared with the bare titania. The acceleration of NO photooxidation rate, resulting from the increase in the amount of NO adsorbed and the decrease in the amount of NO 2 adsorbed, thus occurs on the TiO 2 phase. IR spectra, when irradiating the catalysts with UV, showed the immediate formation of nitrate and NO 2 species on the catalyst. The results lead to the conclusion that the zeolites promote the photocatalytic oxidation of NO over the titania. 相似文献
5.
This paper deals with the activity of bimetallic potassium–copper and potassium–cobalt catalysts supported on alumina for the reduction of NO x with soot from simulated diesel engine exhaust. The effect of the reaction temperature, the soot/catalyst mass ratio and the presence of C 3H 6 has been studied. In addition, the behavior of two monometallic catalysts supported on zeolite beta (Co/beta and Cu/beta), previously used for NO x reduction with C 3H 6, as well as a highly active HC-SCR catalyst (Pt/beta) has been tested for comparison. The preliminary results obtained in the absence of C 3H 6 indicate that, at temperatures between 250 and 400 °C, the use of bimetallic potassium catalysts notably increases the rate of NO x reduction with soot evolving N 2 and CO 2 as main reaction products. At higher temperatures, the catalysts mainly favor the direct soot combustion with oxygen. In the presence of C 3H 6, an increase in the activity for NO x reduction has been observed for the catalyst with the highest metal content. At 450 °C, the copper-based catalysts (Cu/beta and KCu2/Al 2O 3) show the highest activity for both NO x reduction (to N 2 and CO 2) and soot consumption. The Pt/beta catalyst does not combine, at any temperature, a high NO x reduction with a high soot consumption rate. 相似文献
6.
The catalytic oxidation of unsymmetrical dimethylhydrazine (UDMH) by air has been studied in a vibro-fluidized catalyst bed laboratory kinetic setup over catalysts Cu xMg 1−xCr 2O 4/γ-Al 2O 3, 32.9%Ir/γ-Al 2O 3 and β-Si 3N 4 in a temperature range 150–400 °C. The catalyst Cu xMg 1−xCr 2O 4/γ-Al 2O 3 was found to be optimal regarding high yields of CO 2 and low yields of NO x. A probable mechanism of UDMH heterogeneous catalytic oxidation is proposed. Catalyst Cu xMg 1−xCr 2O 4/γ-Al 2O 3 has been further used in the pilot plant specially designed for the destruction of UDMH. Results of testing the main fluidized bed catalytic reactor for UDMH oxidation and the reactor for selective catalytic reduction of NO x with NH 3 are presented. These results prove that the developed UDMH destruction technology is highly efficient and environmentally safe. 相似文献
7.
The lean selective catalytic reduction of NO x by methane over protonic palladium loaded ZSM-5, FER and MOR, as well as, on bimetallic Pd–Pt-HMOR was examined. Special emphasis was paid on the combined effects of water and SO 2 in the feed stream. Under dry conditions and in the absence of SO 2, the degree of NO x conversion at 450°C decreases as follows: Pd-HZSM-5>Pd-HMOR>Pd-HFER. Sulfur dioxide alone has no apparent effect on the activity for NO x reduction, but the coexistence of water and SO 2 inhibits both NO x and methane conversions. The extent of inhibition by water and SO 2 on NO x reduction is Pd-HFER>Pd-HZSM-5>Pd-HMOR. Acid mordenite doped with low levels of Pt and Pd leads to an active catalyst that is more tolerant to the presence of either water or SO 2 than the corresponding monometallic Pt- and Pd-HMOR. Nevertheless, NO x reduction is also inhibited at temperatures below 450°C when SO 2 and water are both present. TPD experiments of water over calcined samples of protonic Pd supported pentasil zeolites, Pd/γ-Al 2O 3 and Pt–Pd-HMOR with and without pretreatment in SO 2+O 2 indicate that sulfation of the surface increases water chemisorption by the support. Therefore, the observed decrease of NO x reduction on Pd-loaded zeolite catalysts when SO 2 and H 2O coexist in the feed stream may be due to enhanced water inhibition and presumably active site poisoning. 相似文献
8.
Chromium oxide catalysts supported on TiO 2 and Al 2O 3 were examined in a fixed-bed flow reactor system for the removal of PCE (perchloroethylene), a simulant of 2,3,7,8-TCDD (2,3,7,8-tetrachlorodibenzo- p-dioxin), and in a pilot plant employing actual flue gas from a sintering plant for the removal of PCDDs/PCDFs (poly-chlorinated dibenzo-dioxin/poly-chlorinated dibenzo-furan). The 12.5 wt.% chromium oxides supported on TiO 2 and Al 2O 3 revealed excellent stability and performance of PCE removal in the feed gas stream containing water vapor. In a pilot plant study, the catalysts washcoated on the honeycomb reactor revealed 93–95% of PCDDs/PCDFs removal activity over CrO x/Al 2O 3-HC20 (CrO x/Al 2O 3 catalyst washcoated on 20 cell-honeycomb), and more than 99% of the decomposition activity over CrO x/TiO 2-HC20 (CrO x/TiO 2 catalyst washcoated on 20 cell-honeycomb) at 325 °C and 5000 h −1 of reactor space velocity without the de novo synthesis of PCDDs/PCDFs. In particular, CrO x/TiO 2-HC20 showed 94% of PCDDs/PCDFs decomposition activity even at 280 °C reaction temperature. The catalyst also exhibited significant NO removal activity. The chromium oxide seems to be a promising catalyst for the removal of PCDDs/PCDFs and NO x contained in the flue gas. 相似文献
9.
The behaviour of a Pt(1 wt.%) supported on CeO 2–ZrO 2(20 wt.%)/Al 2O 3(64 wt.%)–BaO(16 wt.%) as a novel NO x storage–reduction catalyst is studied by reactivity tests and DRIFT experiments and compared with that of Pt(1%)–BaO(15 wt.%) on alumina. The former catalyst, designed as a hydrothermally stable sample, is composed of an alumina modified with Ba ions and an overlayer of ceria-zirconia. The results pointed out that during the calcination barium ions migrates over the surface of the catalyst which thus show a good NO x storage–reduction behaviour comparable with that of Pt–BaO on alumina, although Ba ions result much better dispersed. 相似文献
10.
The selective catalytic reduction of NO+NO 2 (NO x) at low temperature (180–230°C) with ammonia has been investigated with copper-nickel and vanadium oxides supported on titania and alumina monoliths. The influence of the operating temperature, as well as NH 3/NO x and NO/NO 2 inlet ratios has been studied. High NO x conversions were obtained at operating conditions similar to those used in industrial scale units with all the catalysts. Reaction temperature, ammonia and nitrogen dioxide inlet concentration increased the N 2O formation with the copper-nickel catalysts, while no increase was observed with the vanadium catalysts. The vanadium-titania catalyst exhibited the highest DeNO x activity, with no detectable ammonia slip and a low N 2O formation when NH 3/NO x inlet ratio was kept below 0.8. TPR results of this catalyst with NO/NH 3/O 2, NO 2/NH 3/O 2 and NO/NO 2/NH 3/O 2 feed mixtures indicated that the presence of NO 2 as the only nitrogen oxide increases the quantity of adsorbed species, which seem to be responsible for N 2O formation. When NO was also present, N 2O formation was not observed. 相似文献
11.
Free energy minimization calculations are used to determine the thermodynamic equilibrium concentrations of NO x and other species in stoichiometric and lean gas mixtures over a range of temperatures and compositions. Under lean (excess N 2 and O 2) conditions, the NO decomposition (NO↔(1/2)N 2+(1/2)O 2) and NO oxidation (NO+(1/2)O 2↔NO 2) equilibria impose lower bounds on the NO x concentrations achievable by thermodynamic equilibration or NO x decomposition, and these equilibrium NO x concentrations can be practically significant. Assuming a perfect isothermal catalyst acting on a representative diesel exhaust stream collected over the federal test procedure (FTP) cycle, equilibrium NO x levels exceed upcoming California Low Emission Vehicle II (LEV-II) and Tier II NO x emissions standards for automobiles and trucks at temperatures above approximately 800 K. Consideration of a perfect adiabatic catalyst acting on the same diesel exhaust shows that equilibrium NO x values can fall below NO x emissions standards at lower temperatures, but to achieve these low concentrations would require the catalyst to attain 100% approach to equilibrium at very low temperatures. It is concluded that NO x removal based on a thermodynamic equilibrating catalyst under lean exhaust conditions is not practically viable for automotive application, and that to achieve upcoming NO x standards will require selective NO x catalysts that vigorously promote NO x reactions with reductant and do not promote NO decomposition or oxidation. Finally, the ability of a selective NO x catalyst system to reduce NO x concentrations to or below thermodynamic equilibrium values is proposed as a useful measure for selective catalytic reduction (SCR) activity. 相似文献
12.
The effect of SO 2 on the NO x storage capacity and oxidation and reduction activities of a model Pt/Rh/BaO/Al 2O 3 NO x storage catalyst was investigated. Addition of 2.5, 7.5 or 25 vol. ppm SO 2 to a synthetic lean exhaust gas caused deactivation of the NO x storage function, the oxidation activity and the reduction activity of the catalyst. The degree of deactivation of the NO x storage capacity was found to be proportional to the total SO 2 dose that the catalyst had been exposed to. SO 2 was found to be accumulated in the catalyst as sulphate. 相似文献
13.
On an anodic alumina supported silver catalyst with a low Ag loading (1.68 wt.%), NO x (NO/He, NO/O 2/He, NO 2/He) adsorption measurements and NO x-temperature programmed decomposition (TPD)/temperature programmed surface-reaction (TPSR) measurements in different gas streams (He, C 3H 6/He, C 3H 6/O 2/He) were conducted to investigate the formation, consumption and reactivity of surface adsorbed NO x species. During NO adsorption, no noticeable uptake of NO was detected. Introducing oxygen greatly improved the formation of ads-NOx species. A greater quantity of surface nitrate species was found after NO2 adsorption, accompanied with gaseous NO release. The result of TPSR demonstrates the surface nitrate species can be effectively and preferentially reduced by propene. When introducing oxygen into the propene gas stream of TPSR test, the significantly increased amount of reacted nitrate undoubtedly shows the importance of oxygen in activating propene. The pathway for the selective reduction of NOx in the presence of excess oxygen is proposed to pass through the selective reduction of the adsorbed nitrate species with the activated propene. The enhanced NOx conversion when replacing NO with NO2 was attributed to the stronger NOx adsorption capacity and oxidation ability of NO2, than those for NO. With increasing oxygen concentration, the difference between NO and NO2 would gradually decrease, and finally disappear in a high excess of oxygen. 相似文献
14.
To get the low temperature sulfur resistant V 2O 5/TiO 2 catalysts quantum chemical calculation study was carried out. After selecting suitable promoters (Se, Sb, Cu, S, B, Bi, Pb and P), respective metal promoted V 2O 5/TiO 2 catalysts were prepared by impregnation method and characterized by X-ray diffraction (XRD) and Brunner Emmett Teller surface area (BET-SA). Se, Sb, Cu, S promoted V 2O 5/TiO 2 catalysts showed high catalytic activity for NH 3 selective catalytic reduction (NH 3-SCR) of NO x carried at temperatures between 150 and 400 °C. The conversion efficiency followed in the order of Se > Sb > S > V 2O 5/TiO 2 > Cu but Se was excluded because of its high vapor pressure. An optimal 2 wt% ‘Sb’ loading was found over V 2O 5/TiO 2 for maximum NO x conversion, which also showed high resistance to SO 2 in presence of water when compared to other metal promoters. In situ electrical conductivity measurement was carried out for Sb(2%)/V 2O 5/TiO 2 and compared with commercial W(10%)V 2O 5/TiO 2 catalyst. High electrical conductivity difference (Δ G) for Sb(2%)/V 2O 5/TiO 2 catalyst with temperature was observed. SO 2 deactivation experiments were carried out for Sb(2%)/V 2O 5/TiO 2 and W(10%)/V 2O 5/TiO 2 at a temperature of 230 °C for 90 h, resulted Sb(2%)/V 2O 5/TiO 2 was efficient catalyst. BET-SA, X-ray photoelectron spectroscopy (XPS) and carbon, hydrogen, nitrogen and sulfur (CHNS) elemental analysis of spent catalysts well proved the presence of high ammonium sulfate salts over W(10%)/V 2O 5/TiO 2 than Sb(2%)/V 2O 5/TiO 2 catalyst. 相似文献
15.
NO and NO 2 (NO x) sorption, desorption and reduction by hydrogen, carbon monoxide and/or propene were investigated on a TiO 2-supported heteropolyacid, 12-tungstophosphoric acid hexahydrate (HPW), promoted by platinum. A model taking into account NO x sorption, desorption and reduction was established. Kinetic constants for NO x sorption, desorption and reduction were extracted by modelling for the investigated range of temperature (170–300 °C). 相似文献
16.
近年来,面对大气污染日益严峻的现状,用于燃煤烟气中SO 2、NO x和Hg 0的控制技术的研发显得尤为关键。鉴于高级氧化法在污水处理领域较好的应用效果,对于将其用于烟气处理的研究也已展开。本文主要从高级氧化法用于单独脱硝、脱汞和同时脱硫脱硝以及三者联合脱除这4个方面进行了较为详细的综述。重点分析了光催化氧化、蒸发Fenton试剂、多相催化剂、UV/Fenton技术等氧化法在烟气处理领域的研究现状。分析表明,通过对诸多影响因素以及催化剂选择和改性等方面的试验与调控,可使SO 2、NO x和Hg 0的脱除率达到90%左右甚至更高的水平,但仍然存在着·OH自由基量难控制以及脱除效率难维持等问题。由此指出,在今后对于将高级氧化法用于燃煤烟气联合脱除的研究中,需要进一步尝试基于多方法融合的完整、稳定、高效脱硫脱硝脱汞的新思路。 相似文献
17.
The development of a catalytically active filter element for combined particle separation and NO x removal or VOC total oxidation, respectively, is presented. For NO x removal by selective catalytic reduction (SCR) a catalytic coating based on a TiO 2–V 2O 5–WO 3 catalyst system was developed on a ceramic filter element. Different TiO 2 sols of tailor-made mean particle size between 40 and 190 nm were prepared by the sol–gel process and used for the impregnation of filter element cylinders by the incipient wetness technique. The obtained TiO 2-impregnated sintered filter element cylinders exhibit BET surface areas in the range between 0.5 and 1.3 m 2/g. Selected TiO 2-impregnated filter element cylinders of high BET surface area were catalytically activated by impregnation with a V 2O 5 and WO 3 precursor solution. The obtained catalytic filter element cylinders show high SCR activity leading to 96% NO conversion at 300 °C, a filtration velocity of 2 cm/s and an NO inlet concentration of 500 vol.-ppm. The corresponding differential pressures fulfill the requirements for typical hot gas filtration applications. For VOC total oxidation, a TiO 2-impregnated filter element support was catalytically activated with a Pt/V 2O 5 system. Complete oxidation of propene with 100% selectivity to CO 2 was achieved at 300 °C, a filtration velocity of 2 cm/s and a propene inlet concentration of 300 vol.-ppm. 相似文献
18.
A new NO x storage-reduction electrochemical catalyst has been prepared from a polycrystalline Pt film deposited on 8 mol% Y 2O 3-stabilized ZrO 2 (YSZ) solid electrolyte. BaO has been added onto the Pt film by impregnation method. The NO x storage capacity of Pt-BaO/YSZ system was investigated at 350 °C and 400 °C under lean conditions. Results have shown that the electrochemical catalyst was effective for NO x storage. When nitric oxides are fully stored, the catalyst potential is high and reaches its maximum. On the other hand, when a part of NO and also NO 2 desorb to the gas phase, the catalyst potential remarkably drops and finally stabilizes when no more NO x storage occurs but only the reaction of NO oxidation into NO 2. Furthermore, the investigation has clearly demonstrated that the catalyst potential variation versus temperature or chemical composition is an effective indicator for in situ following the NO x storage-reduction process, i.e. the storage as well as the regeneration phase. The catalyst potential variations during NO x storage process was explained in terms of oxygen coverage modifications on the Pt. 相似文献
19.
We have investigated the regeneration of a nitrated or sulphated model Pt/Ba-based NO x trap catalyst using different reductants. H 2 was found to be more effective at regenerating the NO x storage activity especially at lower temperature, but more importantly over the entire temperature window after catalyst ageing. When the model NO x storage catalyst is sulphated in SO 2 under lean conditions at 650 °C almost complete deactivation can be seen. Complete regeneration was not achieved, even under rich conditions at 800 °C in 10% H 2/He. Barium sulphate formed after the high temperature ageing was partly converted to barium sulphide on reduction. However, if the H 2 reduced sample was exposed to a rich condition in a gas mixture containing CO 2 at 650 °C, the storage activity can be recovered. Under these rich conditions the S 2− species becomes less stable than the CO 32−, which is active for storing NO x. Samples which were lean aged in air containing 60 ppm SO 2 at <600 °C, after regeneration at λ=0.95 at 650 °C, have a similar activity window to a fresh catalyst. It is, therefore, important that CO 2 is present during the rich regenerations of the sulphated model samples (as of course it would be under real conditions), as suppression of carbonate formation can lead to sulphide formation which is inactive for NO x storage. 相似文献
20.
NH 3 stored on zeolites in the form of NH 4+ ions easily reacts with NO to N 2 in the presence of O 2 at temperatures <373 K under dry conditions. Wet conditions require a modification of the catalyst system. It is shown that MnO 2 deposited on the external surface of zeolite Y by precipitation considerably enhances the NO x conversion by zeolite fixed NH 4+ ions in the presence of water at 400–430 K. Particle-size analysis, temperature-programmed reduction, textural characterization, chemical analysis, ESR and XRD gave a subtle picture of the MnO 2 phase structure. The MnO 2 is a non-stoichiometric, amorphous phase that contains minor amounts of Mn 2+ ions. It loses O 2 upon inert heating up to 873 K, but does not crystallize or sinter. The phase is reducible by H 2 in two stages via intermediate formation of Mn 3O 4. The manufacture of extrudates preserving stored NH 4+ ions for NO x reduction is described. It was found that MnO 2 can oxidize NO by bulk oxygen. This enables the reduction of NO to N 2 by the zeolitic NH 4+ ions without gas-phase oxygen for limited time periods. The composite catalyst retains storage capacity for both, oxygen and NH 4+ ions despite the presence of moisture and allows short-term reduction of NO without gaseous O 2 or additional reductants. The catalyst is likewise suitable for steady-state DeNO x operation at higher space velocities if gaseous NH 3 is permanently supplied. 相似文献
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