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1.
The physicochemical, surface and catalytic properties of 10 and 20 wt% CuO, NiO or (CuO–NiO) supported on cordierite (commercial grade) calcined at 350–700 °C were investigated using XRD, EDX, nitrogen adsorption at −196 °C and CO oxidation by O 2 at 220–280 °C. The results obtained revealed that the employed cordierite preheated at 350–700 °C was well-crystallized magnesium aluminum silicate (Mg 2Al 4Si 5O 18). Loading of 20 wt% CuO or NiO on the cordierite surface followed by calcination at 350 °C led to dissolution of a limited amount of both CuO and NiO in the cordierite lattice. The portions of CuO and NiO dissolved increased upon increasing the calcination temperature. Treating a cordierite sample with 20 wt% (CuO–NiO) followed by heating at 350 °C led to solid–solid interaction between some of the oxides present yielding nickel cuprate. The formation of NiCuO 2 was stimulated by increasing the calcination temperature above 350 °C. However, raising the temperature up to ≥550 °C led to distortion of cuprate phase. The chemical affinity towards the formation of NiCuO 2 acted as a driving force for migration of some of copper and nickel oxides from the bulk of the solid towards their surface by heating at 500–700 °C. The SBET of cordierite increased several times by treating with small amounts of NiO, CuO or their binary mixtures. The increase was, however, less pronounced upon treating the cordierite support with CuO–NiO. The catalytic activity of the cordierite increased progressively by increasing the amount of oxide(s) added. The mixed oxides system supported on cordierite and calcined at 450–700 °C exhibited the highest catalytic activity due to formation of the nickel cuprate phase. However, the catalytic activity of the mixed oxides system reached a maximum limit upon heating at 500 °C then decreased upon heating at temperature above this limit due to the deformation of the nickel cuprate phase. 相似文献
2.
Nanosized particles dispersed uniformly on Al 2O 3 particles were prepared from the decomposition of precursor Cr(CO) 6 by metal organic chemical vapor deposition (MOCVD) in a fluidized chamber. These nanosized particles consisted of Cr 2O 3, CrC 1−x, and C. A solid solution of Al 2O 3–Cr 2O 3 and an Al 2O 3–Cr 2O 3/Cr 3C 2 nanocomposite were formed when these fluidized powders were pre-sintered at 1000 and 1150 °C before hot-pressing at 1400 °C, respectively. In addition, an Al 2O 3–Cr 2O 3/Cr-carbide (Cr 3C 2 and Cr 7C 3) nanocomposite was formed when the particles were directly hot pressed at 1400 °C. The interface between Cr 3C 2 and Al 2O 3 is non-coherent, while the interface between Cr 7C 3 and Al 2O 3 is semi-coherent. 相似文献
3.
The effects of cobalt and manganese oxides-doping on surface and catalytic properties of Cr 2O 3/MgO system have been investigated. The dopant concentration was changed between 1 and 5 mol% cobalt and manganese oxides. Pure and variously doped solids were subjected to heat treatment at 400 and 700 °C. The techniques employed were X-ray diffraction (XRD), nitrogen adsorption at –196 °C, catalytic conversion of iso-propanol at 200–400 °C using flow technique and catalytic decomposition of H 2O 2 at 20–40 °C. The results revealed that the doping process of the system investigated followed by calcinations at 400 or 700 °C, enhanced the solid–solid interactions between catalyst constituents yielding (-MgCrO 4, β-MgCrO 4) and MgCr 2O 4, respectively. Furthermore, manganese and cobalt oxide-doping for Cr 2O 3/MgO system increased its catalytic activity much towards H 2O 2-decomposition. The increase was, however, more pronounced in the case of manganese-doping. Opposite results have been observed in the case of iso-propanol conversion, which proceeds via dehydrogenation and dehydration reaction. The SBET of the investigated system was found to decrease by increasing the dopant concentration. The doping process did not modify the activation energy of the catalyzed reaction, but rather changed the concentration of the catalytically active constituents without changing their energetic nature. 相似文献
4.
Mixed oxides of alumina and zirconia having a relative composition of 50, 80 and 100% Zr 2O were synthesized by means of sol–gel methods. The catalysts were sulfated with H 2SO 4 1N, and were loaded with 0.3% Pt metal using the incipient wetness technique. The characterization of the physicochemical properties was carried out using XRD, N 2-adsorption at 78 K, and SEM. The catalytic properties of the Al 2O 3–ZrO 2 series were studied by means of dehydration of 2-propanol at 180°C and isomerization of n-hexane at 250°C, 1 atm. The sulfated solids presented a high surface acidity and a limited crystallinity, together with high activity for alcohol dehydration (i.e. 2-propanol). On the other hand, the Al 2O 3–ZrO 2 solid solutions (i.e. those having a 20–80% composition) turned out to be the most active ones for the isomerization of n-hexane. 相似文献
5.
Dispersing La 2O 3 on δ- or γ-Al 2O 3 significantly enhances the rate of NO reduction by CH 4 in 1% O 2, compared to unsupported La 2O 3. Typically, no bend-over in activity occurs between 500° and 700°C, and the rate at 700°C is 60% higher than that with a Co/ZSM-5 catalyst. The final activity was dependent upon the La 2O 3 precursor used, the pretreatment, and the La 2O 3 loading. The most active family of catalysts consisted of La 2O 3 on γ-Al 2O 3 prepared with lanthanum acetate and calcined at 750°C for 10 h. A maximum in rate (mol/s/g) and specific activity (mol/s/m 2) occurred between the addition of one and two theoretical monolayers of La 2O 3 on the γ-Al 2O 3 surface. The best catalyst, 40% La 2O 3/γ-Al 2O 3, had a turnover frequency at 700°C of 0.05 s −1, based on NO chemisorption at 25°C, which was 15 times higher than that for Co/ZSM-5. These La 2O 3/Al 2O 3 catalysts exhibited stable activity under high conversion conditions as well as high CH 4 selectivity (CH 4 + NO vs. CH 4 + O 2). The addition of Sr to a 20% La 2O 3/γ-Al 2O 3 sample increased activity, and a maximum rate enhancement of 45% was obtained at a SrO loading of 5%. In contrast, addition of SO =4 to the latter Sr-promoted La 2O 3/Al 2O 3 catalyst decreased activity although sulfate increased the activity of Sr-promoted La 2O 3. Dispersing La 2O 3 on SiO 2 produced catalysts with extremely low specific activities, and rates were even lower than with pure La 2O 3. This is presumably due to water sensitivity and silicate formation. The La 2O 3/Al 2O 3 catalysts are anticipated to show sufficient hydrothermal stability to allow their use in certain high-temperature applications. 相似文献
6.
The activity of the various CuO species found in supported copper catalysts and the effect of the presence of reaction products, CO 2 and H 2O, was studied during the complete oxidation of methane. Series of copper catalysts supported on ZrO 2, Al 2O 3 and SiO 2 with different metal concentrations were analyzed under identical experimental conditions of reactant concentration and temperature. The catalysts were characterized by TPR, UV–vis spectroscopy and XRD. The results show that the activity of supported CuO is closely related to the kind of Cu species formed on the different supports. It was found that the Cu species formed on ZrO 2 and Al 2O 3 are dependent on the metal loading/support's surface area ratio, and that the activity of highly dispersed Cu is substantially higher than that of bulk CuO. In the case of silica, only the formation of bulk CuO was detected, accounting for the low activity of CuO/SiO 2 catalysts. The activity of highly dispersed Cu species formed on ZrO 2 is higher than those formed over Al 2O 3, and it is not significantly affected by the formation of bulk CuO on the surface. On the contrary, the activity of copper species formed on alumina decreases continuously as the Cu loading is increased. Thus, for the range of copper loading studied in this work, the activity of the catalysts, per gram of loaded Cu, follows the sequence: CuO/ZrO 2 > CuO/Al 2O 3 CuO/SiO 2. It was also found that CO 2 does not inhibits the activity of the CuO/ZrO 2 catalysts, while water inhibits the combustion reaction of methane, with an estimated reaction order of about −0.2 for temperatures between 360 °C and 420 °C. 相似文献
7.
Homogeneous-eutectic microstructure of Y 3Al 5O 12–Al 2O 3 system without coarse primary crystals was formed at an off-eutectic composition. This method utilizes a low migration rate in an amorphous phase. A mixture of Y 2O 3 and Al 2O 3 having the off-eutectic composition was melted and quenched rapidly to form an amorphous phase. A heat-treatment of the amorphous phase at 1000 °C and 1300 °C for 30 min formed Y 3Al 5O 12 and Al 2O 3 phases. SEM observation of this material, which was formed from the amorphous phase at 1300 °C for 30 min, showed homogeneous eutectic-like microstructure. The formation of the primary crystals (coarse Al 2O 3), which are always observed in the off-eutectic compositions by ordinary method, was completely suppressed. 相似文献
8.
Coprecipitated Fe-Al 2O 3, Fe-Co-Al 2O 3 and Fe-Ni-Al 2O 3 catalysts is shown to be very efficient in carbon deposition during methane decomposition at moderate temperatures (600–650 °C). The carbon capacity of the most efficient bimetallic catalysts containing 50–65 wt.% Fe, 5–10 wt.% Co (or Ni) and 25–40 wt.% Al 2O 3 is found to reach 145 g/g cat. Most likely, their high efficiency is due to specific crystal structures of the metal particles and formation of optimum particle size distribution. According to the TEM data, catalytic filamentous carbon (CFC) is formed on them as multiwall carbon nanotubes (MWNTs). The phase composition of the catalysts during methane decomposition is studied using a complex of physicochemical methods (XRD, REDD, Mössbauer spectroscopy and EXAFS). Possible mechanisms of the catalyst deactivation are discussed. 相似文献
9.
In this work, different procedures, namely carbonate coprecipitation and modified solid–solid diffusion, were used to prepare hexaaluminate samples, unsupported or supported onto θ-Al 2O 3. These samples were used as catalyst for the methane total oxidation as synthesized or after impregnation of 1 wt% Pd. It was observed that the modified solid–solid diffusion procedure is an efficient method to obtain the hexaaluminate structure. At a theoretical ratio x of hexaaluminate onto Al 2O 3 less than 0.6 ( xLa 0.2Sr 0.3Ba 0.5MnAl 11O 19 + (1− x)·Al 2O 3, with x = 0.25, 0.60), samples with high specific surface area and θ-Al 2O 3 structure are then obtained. Large differences in catalytic activity can be observed among the series of sample synthesized. All the pure oxide samples (i.e. without palladium) present low catalytic activity for methane total oxidation compared to a reference Pd/Al 2O 3 catalyst. The highest activity was obtained for the samples presenting a θ-Al 2O 3 structure (with x = 0.60) and a high surface area. Impregnation of 1 wt% palladium resulted in an increase in catalytic activity, for all the solids synthesized in this work. Even if the lowest light-off temperature was obtained on the reference sample, similar methane conversions at high temperature (700 °C) were obtained on the stabilized θ-Al 2O 3 solids ( x = 0.25, 0.60). Moreover, the reference sample is found to strongly deactivate with reaction time at the temperature of test (700 °C), due to a progressive reduction of the PdO x active phase into the less active Pd° phase, whereas excellent stabilities in reaction were obtained on the pure and palladium-doped hexaaluminate and supported θ-Al 2O 3 samples. This clearly showed the beneficial effect of the support for the stabilization of the PdO x active phase at high reaction temperature. These properties are discussed in term of oxygen transfer from the support to the palladium particle. Oxygen transfer is directly related to the Mn 3+/Mn 2+ redox properties (in the case of the hexaaluminate and stabilized θ-Al 2O 3 samples), that allows a fast reoxidation of the metal palladium sites since palladium sites reoxidation cannot occur directly by gaseous dioxygen adsorption and dissociation on the surface. 相似文献
10.
The effect of Al 2O 3 levels on the properties of NiO in coprecipitated NiO–Al 2O 3 samples were investigated, using samples with up to 60.7 wt.% Al 2O 3 that had been calcined in the range 300–700°C. Characterization techniques included BET surface area of fresh and reduced catalysts, X-ray diffraction analysis of structure and crystallite size, magnetic susceptibility measurements, oxidizing power, and reducibility in H 2. Only NiO was detected in samples with up to 4.1 wt.% Al 2O 3 for all sample calcination temperatures. Surface areas were similar for all fresh samples but decreased rapidly after calcination at high temperatures. The surface area loss was less for the higher Al 2O 3-containing samples. Nickel oxide crystallite sizes increased at higher calcination temperatures, but remained approximately the same for each Al 2O 3 level. The NiO was nonstoichiometric (NiO1+x), with x decreasing at higher calcination temperatures and increasing with small amounts of added Al2O3 through a maximum at about 3 wt.% Al2O3. However, this did not correlate well with microstrain in the NiO crystallites nor with reducibility, which decreased with Al2O3 addition. At higher levels of Al2O3 (13.6 wt.% and above), surface areas increased with higher Al2O3 loadings, but NiO crystallite sizes remained approximately the same, independent of both Al2O3 content and calcination temperature. X-ray diffraction patterns were very diffuse, and it was not possible to rule out the presence of pseudo-spinel combinations of NiO and Al2O3. Reducibility was more difficult than with low Al2O3 levels, and nonstoichiometry was low and independent of Al2O3 content. Reducibilities of all samples calcined at 300°C correlated well with the final BET surface area of the reduced samples, indicating that more dispersed NiO crystallites are more difficult to reduce, a conclusion that supports a model for reduction proposed previously. 相似文献
11.
Well crystallised aluminium borate Al 18B 4O 33 has been synthesised from alumina and boric acid with a BET area of 18 m 2/g after calcination at 1100 °C. Afterwards, 2 wt.% Pd/Al 18B 4O 33 was prepared by conventional impregnation of Pd(NO 3) 2 aqueous solution and calcination in air at 500 °C. The catalytic activity of Pd/Al 18B 4O 33 in the complete oxidation of methane was measured between 300 and 900 °C and compared with that of Pd/Al 2O 3. Pd/Al 18B 4O 33 exhibited a much lower activity than Pd/Al 2O 3 when treated in hydrogen at 500 °C or aged in O 2/H 2O (90:10) at 800 °C prior to catalytic testing. Surprisingly, a catalytic reaction run up to 900 °C in the reaction mixture induced a steep increase of the catalytic activity of Pd/Al 18B 4O 33 which became as active as Pd/Al 2O 3. Moreover, the decrease of the catalytic activity observed around 750 °C for Pd/Al 2O 3 and attributed to PdO decomposition into metallic Pd was significantly shifted to higher temperatures (820 °C) in the case of Pd/Al 18B 4O 33. The existence of two distinct types of PdO species formed on Al 18B 4O 33 and being, respectively, responsible for the improvement of the activity at low and high temperature was proposed on the basis of diffuse reflectance spectroscopy and temperature-programmed desorption of O 2. 相似文献
12.
The phase diagram of the Al 2O 3–ZrO 2–Nd 2O 3 system was constructed in the temperature range 1250–2800 °C. The liquidus surface of the phase diagram reflects the preferentially eutectic interaction in the system. Two new ternary and one new binary eutectics were found. The minimum melting temperature is 1675 °C and it corresponds to the ternary eutectic Nd 2O 3·11Al 2O 3 + F-ZrO 2 + NdAlO 3. The solidus surface projection and the schematic of the alloy crystallization path confirm the preferentially congruent character of phase interaction in the ternary system. The polythermal sections present the complete phase diagram of the Al 2O 3–ZrO 2–Nd 2O 3 system. No ternary compounds or regions of remarkable solid solution were found in the components or binaries in this ternary system. 相似文献
13.
Sulfidation of trimetallic CoNiMo/Al 2O 3 catalysts was studied by thermogravimetry at 400 °C under flow and pressure conditions. Results were compared with those obtained on prepared and industrial CoMo/Al 2O 3 and NiMo/Al 2O 3 catalysts. The amount of sorbed H 2S on the sulfided solids was measured at 300 °C in the H 2S pressure range 0–3.5 MPa at constant H 2 pressure (3.8 MPa). The adsorption isotherms were simulated using a model featuring dissociated adsorption of H 2S on supported metal sulfides and bare alumina. The amount of sulfur-vacancy sites could thus be determined under conditions close to industrial practice. A relationship with activity results for thiophene HDS and benzene hydrogenation was sought for. 相似文献
14.
The selective catalytic reduction of NO by H 2 under strongly oxidizing conditions (H 2-SCR) in the low-temperature range of 100–200 °C has been studied over Pt supported on a series of metal oxides (e.g., La 2O 3, MgO, Y 2O 3, CaO, CeO 2, TiO 2, SiO 2 and MgO-CeO 2). The Pt/MgO and Pt/CeO 2 solids showed the best catalytic behavior with respect to N 2 yield and the widest temperature window of operation compared with the other single metal oxide-supported Pt solids. An optimum 50 wt% MgO-50wt% CeO 2 support composition and 0.3 wt% Pt loading (in the 0.1–2.0 wt% range) were found in terms of specific reaction rate of N 2 production (mols N 2/g cat s). High NO conversions (70–95%) and N 2 selectivities (80–85%) were also obtained in the 100–200 °C range at a GHSV of 80,000 h −1 with the lowest 0.1 wt% Pt loading and using a feed stream of 0.25 vol% NO, 1 vol% H 2, 5 vol% O 2 and He as balance gas. Addition of 5 vol% H 2O in the latter feed stream had a positive influence on the catalytic performance and practically no effect on the stability of the 0.1 wt% Pt/MgO-CeO 2 during 24 h on reaction stream. Moreover, the latter catalytic system exhibited a high stability in the presence of 25–40 ppm SO 2 in the feed stream following a given support pretreatment. N 2 selectivity values in the 80–85% range were obtained over the 0.1 wt% Pt/MgO-CeO 2 catalyst in the 100–200 °C range in the presence of water and SO 2 in the feed stream. The above-mentioned results led to the obtainment of patents for the commercial exploitation of Pt/MgO-CeO 2 catalyst towards a new NO x control technology in the low-temperature range of 100–200 °C using H 2 as reducing agent. Temperature-programmed desorption (TPD) of NO, and transient titration of the adsorbed surface intermediate NO x species with H 2 experiments, following reaction, have revealed important information towards the understanding of basic mechanistic issues of the present catalytic system (e.g., surface coverage, number and location of active NO x intermediate species, NO x spillover). 相似文献
15.
The role of La 2O 3 loading in Pd/Al 2O 3-La 2O 3 prepared by sol–gel on the catalytic properties in the NO reduction with H 2 was studied. The catalysts were characterized by N 2 physisorption, temperature-programmed reduction, differential thermal analysis, temperature-programmed oxidation and temperature-programmed desorption of NO. The physicochemical properties of Pd catalysts as well as the catalytic activity and selectivity are modified by La2O3 inclusion. The selectivity depends on the NO/H2 molar ratio (GHSV = 72,000 h−1) and the extent of interaction between Pd and La2O3. At NO/H2 = 0.5, the catalysts show high N2 selectivity (60–75%) at temperatures lower than 250 °C. For NO/H2 = 1, the N2 selectivity is almost 100% mainly for high temperatures, and even in the presence of 10% H2O vapor. The high N2 selectivity indicates a high capability of the catalysts to dissociate NO upon adsorption. This property is attributed to the creation of new adsorption sites through the formation of a surface PdOx phase interacting with La2O3. The formation of this phase is favored by the spreading of PdO promoted by La2O3. DTA shows that the phase transformation takes place at temperatures of 280–350 °C, while TPO indicates that this phase transformation is related to the oxidation process of PdO: in the case of Pd/Al2O3 the O2 uptake is consistent with the oxidation of PdO to PdO2, and when La2O3 is present the O2 uptake exceeds that amount (1.5 times). La2O3 in Pd catalysts promotes also the oxidation of Pd and dissociative adsorption of NO mainly at low temperatures (<250 °C) favoring the formation of N2. 相似文献
16.
The capability of flame-made Rh/Ce 0.5Zr 0.5O 2 nanoparticles catalyzing the production of H 2- and CO-rich syngas from butane was investigated for different Rh loadings (0–2.0 wt% Rh) and two different ceramic fibers (Al 2O 3/SiO 2 and SiO 2) as plugging material in a packed bed reactor for a temperature range from 225 to 750 °C. The main goal of this study was the efficient processing of butane at temperatures between 500 and 600 °C for a micro-intermediate-temperature SOFC system. Our results showed that Rh/Ce 0.5Zr 0.5O 2 nanoparticles offer a very promising material for butane-to-syngas conversion with complete butane conversion and a hydrogen yield of 77% at 600 °C. The catalytic performance of packed beds strongly depended on the use of either Al 2O 3/SiO 2 or SiO 2 fiber plugs. This astonishing effect could be attributed to the interplay of homogeneous and heterogeneous chemical reactions during the high-temperatures within the reactor. 相似文献
17.
A method to quantify DRIFT spectral features associated with the in situ adsorption of gases on a NO x adsorber catalyst, Pt/K/Al 2O 3, is described. To implement this method, the multicomponent catalyst is analysed with DRIFT and chemisorption to determine that under operating conditions the surface comprised a Pt phase, a pure γ-Al 2O 3 phase with associated hydroxyl groups at the surface, and an alkalized-Al 2O 3 phase where the surface –OH groups are replaced by –OK groups. Both DRIFTS and chemisorption experiments show that 93–97% of the potassium exists in this form. The phases have a fractional surface area of 1.1% for the 1.7 nm-sized Pt, 34% for pure Al 2O 3 and 65% for the alkalized-Al 2O 3. NO 2 and CO 2 chemisorption at 250 °C is implemented to determine the saturation uptake value, which is observed with DRIFTS at 250 °C. Pt/Al 2O 3 adsorbs 0.087 μmol CO 2/m 2and 2.0 μmol NO 2/m 2, and Pt/K/Al 2O 3 adsorbs 2.0 μmol CO 2/m 2and 6.4 μmol NO 2/m 2. This method can be implemented to quantitatively monitor the formation of carboxylates and nitrates on Pt/K/Al 2O 3 during both lean and rich periods of the NO x adsorber catalyst cycle. 相似文献
18.
A comparison study was carried out on non-thermal plasma (NTP)-assisted selective catalytic reduction (SCR) of NO x by propene over Ag/USY and Ag/Al 2O 3 catalysts. Ag/USY was almost inactive in thermal SCR while it showed obvious activities in NTP-assisted SCR at 100 °C–200 °C. Although the NO x conversion over Ag/Al 2O 3 was also enhanced at 300 °C–400 °C by the assistance of NTP, it was ineffective below 250 °C. The intermediates over Ag/USY and Ag/Al 2O 3 were investigated using in situ DRIFTS method. It was found that key intermediates in HC-SCR, such as NCO, CN, oxygenates and some N-containing organic species were enriched after the assistance of NTP. The differences in the behaviors of above intermediates were not found between these two kinds of catalysts. However, some evidences suggested that different properties of the absorbed NO x species resulted in the distinction of SCR reactions over Ag/USY and Ag/Al 2O 3. TPD profiles of Ag/Al 2O 3 showed that nitrates formed over the catalyst were quite stable at low temperatures, which might occupy the active sites and were unfavorable to SCR reactions. The nitrates over Ag/USY were unstable, among which the unidentate nitrate species is probably contributed to the SCR reactions at low temperatures. 相似文献
19.
The effectiveness of Ag/Al 2O 3 catalyst depends greatly on the alumina source used for preparation. A series of alumina-supported catalysts derived from AlOOH, Al 2O 3, and Al(OH) 3 was studied by means of X-ray diffraction (XRD), scanning electron microscopy (SEM), ultraviolet–visible (UV–vis) spectroscopy, diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy, O 2, NO + O 2-temperature programmed desorption (TPD), H 2-temperature programmed reduction (TPR), thermal gravimetric analysis (TGA) and activity test, with a focus on the correlation between their redox properties and catalytic behavior towards C 3H 6-selective catalytic reduction (SCR) of NO reaction. The best SCR activity along with a moderated C 3H 6 conversion was achieved over Ag/Al 2O 3 (I) employing AlOOH source. The high density of Ag–O–Al species in Ag/Al 2O 3 (I) is deemed to be crucial for NO selective reduction into N 2. By contrast, a high C 3H 6 conversion simultaneously with a moderate N 2 yield was observed over Ag/Al 2O 3 (II) prepared from a γ-Al 2O 3 source. The larger particles of Ag mO ( m > 2) crystallites were believed to facilitate the propene oxidation therefore leading to a scarcity of reductant for SCR of NO. An amorphous Ag/Al 2O 3 (III) was obtained via employing a Al(OH) 3 source and 500 °C calcination exhibiting a poor SCR performance similar to that for Ag-free Al 2O 3 (I). A subsequent calcination of Ag/Al 2O 3 (III) at 800 °C led to the generation of Ag/Al 2O 3 (IV) catalyst yielding a significant enhancement in both N 2 yield and C 3H 6 conversion, which was attributed to the appearance of γ-phase structure and an increase in surface area. Further thermo treatment at 950 °C for the preparation of Ag/Al 2O 3 (V) accelerated the sintering of Ag clusters resulting in a severe unselective combustion, which competes with SCR of NO reaction. In view of the transient studies, the redox properties of the prepared catalysts were investigated showing an oxidation capability of Ag/Al 2O 3 (II and V) > Ag/Al 2O 3 (IV) > Ag/Al 2O 3 (I) > Ag/Al 2O 3 (III) and Al 2O 3 (I). The formation of nitrate species is an important step for the deNO x process, which can be promoted by increasing O 2 feed concentration as evidenced by NO + O 2-TPD study for Ag/Al 2O 3 (I), achieving a better catalytic performance. 相似文献
20.
A multi-component NO x-trap catalyst consisting of Pt and K supported on γ-Al 2O 3 was studied at 250 °C to determine the roles of the individual catalyst components, to identify the adsorbing species during the lean capture cycle, and to assess the effects of H 2O and CO 2 on NO x storage. The Al 2O 3 support was shown to have NO x trapping capability with and without Pt present (at 250 °C Pt/Al 2O 3 adsorbs 2.3 μmols NO x/m 2). NO x is primarily trapped on Al 2O 3 in the form of nitrates with monodentate, chelating and bridged forms apparent in Diffuse Reflectance mid-Infrared Fourier Transform Spectroscopy (DRIFTS) analysis. The addition of K to the catalyst increases the adsorption capacity to 6.2 μmols NO x/m 2, and the primary storage form on K is a free nitrate ion. Quantitative DRIFTS analysis shows that 12% of the nitrates on a Pt/K/Al 2O 3 catalyst are coordinated on the Al 2O 3 support at saturation. When 5% CO2 was included in a feed stream with 300 ppm NO and 12% O2, the amount of K-based nitrate storage decreased by 45% after 1 h on stream due to the competition of adsorbed free nitrates with carboxylates for adsorption sites. When 5% H2O was included in a feed stream with 300 ppm NO and 12% O2, the amount of K-based nitrate storage decreased by only 16% after 1 h, but the Al2O3-based nitrates decreased by 92%. Interestingly, with both 5% CO2 and 5% H2O in the feed, the total storage only decreased by 11%, as the hydroxyl groups generated on Al2O3 destabilized the K–CO2 bond; specifically, H2O mitigates the NOx storage capacity losses associated with carboxylate competition. 相似文献
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