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1.
This study focuses on the loading of catalytic materials, e.g., palladium on the surface of supporting materials, with the aim to obtain catalysts with high activity for methane combustion. The catalyst PdO/CeO 2-Al 2O 3 was prepared by impregnation under ultrasonic condition. The effect of different activation methods on the activity of catalysts for methane catalytic combustion was tested. The properties of reaction and adsorption of oxygen species on catalyst surface were characterized by H 2-temperature programmed reduction (H 2-TPR), and O 2-temperature programmed desorption (O 2-TPD). Furthermore, the sulfur tolerance and sulfur poisoning mode were investigated. The results indicate that the catalyst PdO/CeO 2-Al 2O 3 activated with rapid activation shows higher activity for methane combustion and better sulfur tolerance. The result of sulfur content analysis shows that there is a large number of sulfur species on the catalyst’s surface after reactivation at high temperature. It proves that the activity of catalysts cannot be fully restored by high-temperature reactivation. 相似文献
2.
Micro-channel plates with dimension of 1 mm × 0.3 mm × 48 mm were prepared by chemical etching of stainless steel plates followed by wash coating of CeO 2 and Al 2O 3 on the channels. After coating the support on the plate, Pt, Co, and Cu were added to the plate by incipient wetness method. Reaction experiments of a single reactor showed that the micro-channel reactor coated with CuO/CeO 2 catalyst was highly selective for CO oxidation while the one coated with Pt-Co/Al 2O 3 catalyst was highly active for CO oxidation. The 7-layered reactors coated with two different catalysts were prepared by laser welding and the performances of each reactor were tested in large scale of PROX conditions. The multi-layered reactor coated with Pt-Co/Al 2O 3 catalyst was highly active for PROX and the outlet concentration of CO gradually increased with the O 2/CO ratio due to the oxidation of H 2 which maintained the reactor temperature. The multi-layered reactor coated with CuO/CeO 2 showed lower catalytic activity than that coated with Pt catalyst, but its selectivity was not changed with the increase of O 2/CO ratios due to the high selectivity. In order to combine advantages (high activity and high selectivity) of the two individual catalysts (Pt-Co/Al 2O 3, CuO/CeO 2), a serial reactor was prepared by connecting the two multi-layered micro-channel reactors with different catalysts. The prepared serial reactor exhibited excellent performance for PROX. 相似文献
3.
The role of ceria, niobium and molybdenum oxides on the promotion of the NO reduction by CO was studied. A bifunctional mechanism was discussed as a function of both the nature of interaction between metal oxide and palladium and the redox properties of each metal oxide. The NO dissociation was better on the Pd/MoO3/Al2O3 catalyst than on the Pd/CeO2/Al2O3 and Pd/Nb2O5/Al2O3 catalysts. The explanation for the very high N2 production on Pd–Mo catalyst during the TPD analysis may be attributed to the NO+Meδ+ stoichiometric reaction. The promoting effect of a reducible oxide for the NO+CO reaction at low temperature can be ascribed mainly to its easiness for a redox interchange and its interaction with the noble metal particles. This would increase the surface redox ability and favor the dynamic equilibrium needed for high N2 selectivity. 相似文献
4.
Regeneration of S-poisoned Pd/Al 2O 3 catalysts for the abatement of methane emissions from natural gas vehicles was addressed in this work. Investigations were devoted to determine the temperature threshold allowing for catalyst reactivation under different CH4 containing atmospheres. Under lean combustion conditions in the presence of excess O2, partial regeneration took place only above 750 °C after decomposition of stable sulphate species adsorbed on the support. Short CH4-reducing, O2-free pulses led to partial catalyst reactivation already at 550 °C and to practically complete regeneration at 600 °C. Also in this case reactivation was associated with SO2 release due to the decomposition of stable support sulphates likely promoted by CH4 activation onto the reduced metallic Pd surface. Rich combustion pulses with CH4/O2 = 2 were equally effective to CH4-reducing pulses in catalyst regeneration. These results suggest that a regeneration strategy based on periodical natural gas pulses fed to the catalyst by a by-pass line might be efficient in limiting the effects of S-poisoning of palladium catalysts for the abatement of CH4 emissions from natural gas engine. 相似文献
5.
The role of vanadium oxide and palladium on the benzene oxidation reaction over Pd/V 2O 5/Al 2O 3 catalysts was investigated. The Pd/V 2O 5/Al 2O 3 catalysts were more active than V 2O 5/Al 2O 3 and Pd/Al 2O 3 catalysts. The increase of vanadium oxide content decreased the Pd dispersion and increased the benzene conversion. A strong Pd particle size effect on benzene oxidation reaction was observed. Although the catalysts containing high amount of V 4+ species were more active, the Pd particle size effect was responsible for the higher activity. 相似文献
6.
Reaction activities of several developed catalysts for NO oxidation and NO x (NO + NO 2) reduction have been determined in a fixed bed differential reactor. Among all the catalysts tested, Co 3O 4 based catalysts are the most active ones for both NO oxidation and NO x reduction reactions even at high space velocity (SV) and low temperature in the fast selective catalytic reduction (SCR) process. Over Co 3O 4 catalyst, the effects of calcination temperatures, SO 2 concentration, optimum SV for 50% conversion of NO to NO 2 were determined. Also, Co 3O 4 based catalysts (Co 3O 4-WO 3) exhibit significantly higher conversion than all the developed DeNO x catalysts (supported/unsupported) having maximum conversion of NO x even at lower temperature and higher SV since the mixed oxide Co-W nanocomposite is formed. In case of the fast SCR, N 2O formation over Co 3O 4-WO 3 catalyst is far less than that over the other catalysts but the standard SCR produces high concentration of N 2O over all the catalysts. The effect of SO 2 concentration on NO x reduction is found to be almost negligible may be due to the presence of WO 3 that resists SO 2 oxidation. 相似文献
7.
The effect of palladium incorporation on the performance of Cu–ZnO(Al 2O 3) during the hydrogenation of carbon dioxide has been assessed. Temperature-programmed reduction profiles and X-ray photoelectron spectra of copper revealed that Pd enhances copper oxide reduction. Carbon dioxide conversion and methanol yield were found to increase on Pd-loaded catalysts. The importance of the palladium incorporated to the base Cu–ZnO(Al 2O 3) catalyst in determining the catalytic activity is discussed in terms of the relative ease with which hydrogen is dissociated on the Pd particles and then spilt over the Cu–ZnO phase of the base catalyst. 相似文献
8.
Pt supported on CeO 2 and 10 wt.% La 3+-doped CeO 2 catalysts have been prepared, characterised and tested for soot oxidation by O 2 in TGA. The reaction mechanism has been studied in a TAP reactor with labelled O 2. Isotopic oxygen exchange between molecular O 2 and ‘O’ on the support/catalyst was observed and soot oxidation is being carried out by lattice oxygen. TAP studies further show that Pt improves O 2 adsorption and, therefore, 5 wt.% Pt-containing catalysts are more active for soot oxidation than the counterpart supports. In addition, CeO 2 doping by La 3+ leads to an improved support, since La 3+ stabilises the structure of CeO 2 when calcined at high temperature (1000 °C) and minimises sintering. In addition, La 3+ improves the Ce 4+/Ce 3+ reduction as deduced from H 2-TPR experiments and favours oxygen mobility into the lattice. A synergetic effect of Pt and La 3+ is observed, Pt-containing La 3+-doped CeO 2 being the most active catalyst for soot oxidation by O 2 among the samples studied. 相似文献
9.
The effect of the Pd addition method into the fresh Pd/(OSC + Al 2O 3) and (Pd + OSC)/Al 2O 3 catalysts (OSC material = Ce xZr 1−xO 2 mixed oxides) was investigated in this study. The CO + NO and CO + NO + O 2 model reactions were studied over fresh and aged catalysts. The differences in the fresh catalysts were insignificant compared to the aged catalysts. During the CO + NO reaction, only small differences were observed in the behaviour of the fresh catalysts. The light-off temperature of CO was about 20 °C lower for the fresh Pd/(OSC + Al 2O 3) catalyst than for the fresh (Pd + OSC)/Al 2O 3 catalyst during the CO + NO + O 2 reaction. For the aged catalysts lower NO reduction and CO oxidation activities were observed, as expected. Pd on OSC-containing alumina was more active than Pd on OSC material after the agings. The activity decline is due to a decrease in the number of active sites on the surface, which was observed as a larger Pd particle size for aged catalysts than for fresh catalysts. In addition, the oxygen storage capacity of the aged Pd/(OSC + Al 2O 3) catalyst was higher than that of the (Pd + OSC)/Al 2O 3 catalyst. 相似文献
10.
Ni/Al_2O_3催化剂是甲烷二氧化碳重整反应制取合成气研究最多、最具应用潜力的一种催化剂。通过对催化剂进行CO_2-TPD研究,考察还原态Ni/Al_2O_3催化剂的CO_2脱附特性。结果表明,浸渍法制备的Ni/Al_2O_3催化剂CO_2脱附曲线呈现双峰,分别在(60~65)℃和(350~380)℃出现高低温两个活性位;高温CO_2吸附量为3.0 cm~3·g~(-1),低温CO_2吸附量为24.0 cm~3·g~(-1)。催化剂的CO_2吸附量与其Ni含量无关。考察选用不同载体的CO_2脱附行为,发现以Al_2O_3为载体的催化剂CO_2吸附量是MgO和SiO_2为载体催化剂的2~4倍,以TiO_2为载体的催化剂几乎不吸附CO_2。 相似文献
11.
This work investigates performances of supported transition-metal oxide catalysts for the catalytic reduction of SO 2 with C 2H 4 as a reducing agent. Experimental results indicate that the active species, the support, the feed ratio of C 2H 4/SO 2, and pretreatment are all important factors affecting catalyst activity. Fe 2O 3/γ-Al 2O 3 was found to be the most active catalyst among six γ-Al 2O 3-supported metal oxide catalysts tested. With Fe 2O 3 as the active species, of the supports tested, CeO 2 is the most suitable one. Using this Fe 2O 3/CeO 2 catalyst, we found that the optimal Fe content is 10 wt.%, the optimal feed ratio of C 2H 4/SO 2 is 1:1, and the catalyst presulfidized by H 2+H 2S exhibits a higher performance than those pretreated with H 2 or He. Although the feed concentrations of C 2H 4:SO 2 being 3000:3000 ppm provide a higher conversion of SO 2, the sulfur yield decreases drastically at temperatures above 300 °C. With higher feed concentrations, maximum yield appears at higher temperatures. The C 2H 4 temperature-programmed desorption (C 2H 4-TPD) and SO 2-TPD desorption patterns illustrate that Fe 2O 3/CeO 2 can adsorb and desorb C 2H 4 and SO 2 more easily than can Fe 2O 3/γ-Al 2O 3. Moreover, the SO 2-TPD patterns further show that Fe 2O 3/γ-Al 2O 3 is more seriously inhibited by SO 2. These findings may properly explain why Fe 2O 3/CeO 2 has a higher activity for the reduction of SO 2. 相似文献
12.
Methane partial oxidation (MPO) is considered as an alternative method to produce hydrogen because it is an exothermic reaction to afford a suitable H 2/CO ratio of 2. However, carbon deposition on a catalyst is observed as a major cause of catalyst deactivation in MPO. In order to find suitable catalysts that prevent the carbon deposition, NiO-MgO/Ce 0.75Zr 0.25O 2 (CZO) supported catalysts were prepared via the co-impregnation (C) and sequential incipient wetness impregnation (S) methods. The amount of Ni loading was fixed at 15 wt-% whereas the amount of MgO loading was varied from 5 to 15 wt-%. The results revealed that the addition of MgO shifted the light-off temperatures to higher temperatures. This is because the Ni surface was partially covered with MgO, and the strong interaction between NiO and NiMgO 2 over CZO support led to the difficulty in reducing NiO to active Ni 0 and thus less catalytic activity. However, among the catalysts tested, the 15Ni5Mg/CZO (S) catalyst exhibited the best catalytic stability for MPO after 18 h on stream at 750°C. Moreover, this catalyst had a better resistance to carbon deposition due to its high metallic Ni dispersion at high temperature. 相似文献
13.
通过浸渍法制备了Al_2O_3负载的Pd和Pt催化剂,考察催化剂的甲烷、乙烷和丙烷催化燃烧活性,以及助剂Ba对催化性能的影响。对于Pd/Al_2O_3催化剂,加入Ba使活性物种PdO颗粒变大和还原温度升高,形成更稳定的PdO活性物种,是Pd-Ba/Al_2O_3催化剂活性提升的主要原因。对于Pt/Al_2O_3催化剂,加入Ba助剂使活性物种Pt0含量降低,PtO_x与Al_2O_3载体相互作用增强,使PtO_x物种更难被还原为Pt~0,导致Pt-Ba/Al_2O_3催化剂活性降低。Pd和Pt催化剂催化烷烃氧化反应活性规律一致:丙烷乙烷甲烷。Pd/Al_2O_3催化剂有利于C—H键活化,Pt/Al_2O_3催化剂有利于C—C键活化。Pt/Al_2O_3催化剂对C1-C3烷烃氧化活性的差别明显大于Pd/Al_2O_3催化剂。Pt/Al_2O_3催化剂对碳比例高的烷烃活性更高。 相似文献
14.
分别采用合成的铝镍类水滑石和其焙烧后复合氧化物为载体,负载K_2CO_3制得负载型固体碱催化剂,并用于催化食用菜籽油制生物柴油的反应。考察甲醇与菜籽油物质的量比、反应时间和反应温度对催化性能的影响,结果表明,在甲醇与菜籽油物质的量比10∶1、反应温度60℃、反应时间6 h和催化剂用量为油质量的5%条件下,生物柴油产率最高,为82.4%,且催化剂可重复使用,具有稳定的催化作用。 相似文献
15.
A series of CeO 2 promoted cobalt spinel catalysts were prepared by the co-precipitation method and tested for the decomposition of nitrous oxide (N 2O). Addition of CeO 2 to Co 3O 4 led to an improvement in the catalytic activity for N 2O decomposition. The catalyst was most active when the molar ratio of Ce/Co was around 0.05. Complete N 2O conversion could be attained over the CoCe0.05 catalyst below 400 °C even in the presence of O 2, H 2O or NO. Methods of XRD, FE-SEM, BET, XPS, H 2-TPR and O 2-TPD were used to characterize these catalysts. The analytical results indicated that the addition of CeO 2 could increase the surface area of Co 3O 4, and then improve the reduction of Co 3+ to Co 2+ by facilitating the desorption of adsorbed oxygen species, which is the rate-determining step of the N 2O decomposition over cobalt spinel catalyst. We conclude that these effects, caused by the addition of CeO 2, are responsible for the enhancement of catalytic activity of Co 3O 4. 相似文献
16.
The current work is devoted to study of CO interaction with PdO/Al 2O 3–(Ce x–Zr 1−x)O 2 catalysts. Ceria–zirconia–alumina supports with different Ce/Zr ratio were prepared by sol–gel technique. The FT-IR characterization of CO adsorbed at −120 and 25 °C on oxidized and reduced samples revealed that Ce/Zr ratio modifies the surface properties of support and oxidation state of palladium. The catalyst with Ce/Zr molar ratio 0.5/0.5 was characterized with the highest ability to stabilize palladium in oxide state and the highest activity to oxidize CO. Redox treatment of catalysts improves their catalytic activity. 相似文献
17.
The effects of carbon dioxide on the dehydrogenation of C 3H 8 to produce C 3H 6 were investigated over several Cr 2O 3 catalysts supported on Al 2O 3, active carbon and SiO 2. Carbon dioxide exerted promoting effects only on SiO 2-supported Cr 2O 3 catalysts. The promoting effects of carbon dioxide over a Cr 2O 3/SiO 2 catalyst were to enhance the yield of C 3H 6 and to suppress the catalyst deactivation. 相似文献
18.
Oxidation activity and stability under reaction was investigated for a series of mixed oxide catalysts, doped or not by a precious metal (Pd, Pt). The reaction feedstock, containing CO, H 2, CH 4, CO 2 and H 2O, simulated gases issued from H 2 production processes for fuel cells. Contrarily to conventional noble metal catalysts, mixed oxide samples present generally good stability under reaction at high temperature. The activities measured for the perovskite and hexaaluminate catalysts, are however largely lower than that of the reference Pd/Al 2O 3 catalyst. High activities were obtained after impregnation of 1.1 wt.% Pd or 0.8 wt.% Pt on the hexaaluminates samples. Even if Pd/Al 2O 3 was found to present a high activity, this sample suffered from drastic deactivation at 700 °C. Better stability were obtained on perovskite. Furthermore, doping hexaaluminate by Pt led to samples with good activities and high stability. Even if better activities were obtained by doping the hexaaluminate samples by Pd, the Pd/BaAl 12O 19 strongly deactivated, as it was previously observed for the reference catalyst. Interestingly, this Pd deactivation was not observed when Pd was impregnated on the Mn substituted hexaaluminate, leading to a stable and active catalyst. This suggests that it is possible to stabilize the palladium in its oxidized form at high temperature (700 °C) on the surface of some supports. 相似文献
19.
The importance of the hydrodearomatisation (HDA) is increasing together with tightening legislation of fuel quality and exhaust emissions. The present study focuses on hydrogenation (HYD) kinetics of the model aromatic compound naphthalene, found in typical diesel fraction, in n-hexadecane over a NiMo (nickel molybdenum), Ni (nickel) and Ru (ruthenium) supported on trilobe alumina (Al 2O 3) catalysts. Kinetic reaction expressions based on the mechanistic Langmuir–Hinshelwood (L–H) model were derived and tested by regressing the experimental data that translated the effect of both naphthalene and hydrogen concentration at a constant temperature (523.15 and 573.15 K over the NiMo catalyst and at 373.15 K over the Ni and Ru/Al 2O 3 catalysts) on the initial reaction rate. The L–H equation, giving an adequate fit to the experimental data with physically meaningful parameters, suggested a competitive adsorption between hydrogen and naphthalene over the presulphided NiMo catalyst and a non-competitive adsorption between these two reactants over the prereduced Ni and Ru/Al 2O 3 catalysts. In addition, the adsorption constant values indicated that the prereduced Ru catalyst was a much more active catalyst towards naphthalene HYD than the prereduced Ni/Al 2O 3 or the presulphided NiMo/Al 2O 3 catalyst. 相似文献
20.
We have been developed novel catalysts for gasification of biomass with much higher energy efficiency than conventional methods (non-catalyst, dolomite, commercial steam reforming Ni catalyst). From the result of the gasification of cellulose over novel Rh/CeO 2/SiO 2 catalysts, it is found that the gasification process consists of the reforming of tar and the combustion of solid carbon. We also tested novel Rh/CeO 2/SiO 2 in the gasification with air, pyrogasification, and steam reforming of cedar wood. As a result, Rh/CeO 2/SiO 2 gave higher yield of syngas than the conventional steam reforming Ni catalyst. Furthermore, we compared the performance between single and dual bed reactors. Single bed reactor was effective in the gasification of cedar, however, it was not suitable for the gasification of rice straw since a rapid deactivation was observed. Gasification of rice straw, jute stick, baggase using the fluidized dual-bed reactor and Rh/CeO 2/SiO 2 was also investigated. Especially, the catalyst stability in the gasification of rice straw clearly was enhanced by using the fluidized dual bed reactor. 相似文献
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