Catalytic combustion of toluene over platinum supported on Ce–Zr–O solid solution modified by Y and Mn

A series of CeO₂–ZrO₂ mixed oxides were prepared using coprecipitation method and characterized by BET, oxygen storage capacity (OSC), X-ray diffraction (XRD) and H₂-temperature-programmed reduction (H₂-TPR). The catalytic activities toward toluene combustion were investigated in a micro-reactor. The results demonstrate that the catalytic activity of Pt/γ-Al₂O₃/Ce_0.50Zr_0.50O₂ monolithic catalyst can be greatly improved by doping metal into Ce_0.50Zr_0.50O₂. When doping Y and Mn into Ce_0.50Zr_0.50O₂ simultaneously, the catalyst Pt/γ-Al₂O₃/Ce_0.40Zr_0.40Y_0.10Mn_0.10O_X shows the highest activity. The T₁₀ (the temperature of 10% toluene conversion) and the complete conversion temperature (the temperature of 90% toluene conversion) of toluene are 443 and 489 K, respectively. Gas hourly space velocity (GHSV) results show that the prepared catalyst can be applied in a wide range of GHSV (from 12,000 to 20,000 h⁻¹). The catalyst prepared shows great potential for practical application.     

Preparation of platinum nanoparticle and its catalytic activity for toluene oxidation

Colloidal Pt nanoparticles are prepared using H2PtCl6 as a precursor, polyvinylpyrrolidone (PVP: molecular weight = 10,000 and 40,000) and hydrogen as a stabilizing agent and a reducing agent, respectively. The amounts of the precursor and the stabilizing agent and the molecular weight of PVP have an effect on the formation of Pt nanoparticles. Supported Pt catalyst (CSPt) is prepared from colloidal Pt nanoparticles and y-Al2O3. Another supported Pt catalyst (ISPt) is prepared by using the conventional incipient wetness impregnation method with an aqueous H2PtCl6 solution and gamma-Al2O3. The catalytic activities of CSPt and ISPt catalysts are compared for VOC (toluene) oxidation. Transmission Electron Microscopy (TEM), UV-vis, X-ray diffraction (XRD) and temperature programmed reduction (TPR) are used to characterize CSPt and ISPt catalysts. The experimental results reveal that the catalytic activity of CSPt is superior to that of ISPT.     

催化剂MnCe（y）Ox/TiO2的制备及其催化燃烧甲苯的活性

以TiO2为载体,采用浸渍法制备了不同配比的MnCe复合型催化剂,并采用X射线衍射(XRD)、氧气的程序升温脱附(O2-TPD)和氢气的程序升温还原(H2-TPR)对制备的催化剂进行表征,比较了催化剂催化氧化(燃烧)甲苯的活性。研究结果表明,所制备的催化剂MnCe(y)Ox/TiO2对甲苯有明显的催化活性。当Ce/(Mn+Ce)的摩尔比为0.1时,催化剂MnCe(0.1)Ox/TiO2的催化活性最高,甲苯的转化率达到90%时的温度为254℃。在催化剂MnOx/TiO2中掺杂少量的Ce元素,有利于活性组分Mn物种在载体表面上以更小颗粒而且更高的分散度存在,从而提高催化剂的催化活性。     

The catalytic oxidation of aromatic hydrocarbons over supported metal oxide

The catalytic activity of metals (Cu, Mn, Fe, V, Mo, Co, Ni, Zn)/gamma-Al2O3 was investigated to bring about the complete oxidation of benzene, toluene and xylene (BTX). Among them, Cu/gamma-Al2O3 was found to be the most promising catalyst based on activity. X-ray diffraction (XRD), Brunauer Emmett Teller method (BET), electron probe X-ray micro analysis (EPMA) and temperature programmed reduction (TPR) by H2 were used to characterize a series of supported copper catalysts. Increasing the calcination temperature resulted in decreasing the specific surface areas of catalysts and, subsequently, the catalytic activity. Copper loadings on gamma-Al2O3 had a great effect on catalytic activity, and 5 wt.% Cu/gamma-Al2O3 catalyst was observed to be the most active, which might be contributed to the well-dispersed copper surface phase. Using TiO2 (anatase), TiO2 (rutile), SiO2 (I) and SiO2 (II) as support instead of gamma-Al2O3, the activity sequence of 5 wt.% Cu with respect to the support was gamma-Al2O3 > TiO2 (rutile) > TiO2 (anatase)>SiO2 (I) > SiO2 (II), and this appeared to be correlated with the distribution of copper on support rather than with the specific surface area of the catalyst. The smaller particle size of copper, due to its high dispersion on support, had a positive effect on catalytic activity. The activity of 5 wt.% Cu/gamma-Al2O3 with respect to the VOC molecule was observed to follow this sequence: toluene > xylene > benzene. Increasing the reactant concentration exerted an inhibiting effect on the catalytic activity.     

Effect of CeO2 doping on catalytic activity of Fe2O3/gamma-Al2O(3) catalyst for catalytic wet peroxide oxidation of azo dyes

In order to find a catalyst with high activity and stability for catalytic wet peroxide oxidation (CWPO) process under normal condition, with Fe(2)O(3)/gamma-Al(2)O(3) and Fe(2)O(3)-CeO(2)/gamma-Al(2)O(3) catalysts prepared by impregnation method, the effect of CeO(2) doping on the structure and catalytic activity of Fe(2)O(3)/gamma-Al(2)O(3) for catalytic wet peroxide oxidation of azo dyes at 25 degrees C and atmospheric pressure is evaluated using BET, SEM, XRF, XRD, XPS and chemical analysis techniques, and test results show that, better dispersion and smaller size of Fe(2)O(3) crystal can be achieved by adding CeO(2), and the content of chemisorbed oxygen can also be increased on the surface of catalyst. CWPO experimental results indicate that azo dyes in simulated wastewater can be efficiently mineralized and the catalytic activity of Fe(2)O(3)-CeO(2)/gamma-Al(2)O(3) can be increased by about 10% compared with that of Fe(2)O(3)/gamma-Al(2)O(3) because of the promotion of the structural and redox properties of the ferric oxide by ceria doped. Leaching tests indicate that Fe(2)O(3)/gamma-Al(2)O(3) and Fe(2)O(3)-CeO(2)/gamma-Al(2)O(3) are stable with a negligible amount of irons found in the aqueous solution after reaction for 2h. It can therefore be concluded from results and discussion that in comparison with Fe(2)O(3)/gamma-Al(2)O(3), Fe(2)O(3)-CeO(2)/gamma-Al(2)O(3) is a suitable catalyst, which can effectively degrade contaminants at normal temperature and atmospheric pressure.     

Effect of metal doping into Ce0.5Zr0.5O2 on photocatalytic activity of TiO2/Ce0.45Zr0.45M0.1OX (M=Y, La, Mn)

The paper demonstrates that the photocatalytic activity of TiO2 towards the decomposition of gaseous benzene in a batch reactor can be greatly improved by loading TiO2 on the surface of CeO(2)-ZrO(2). The research investigates the effects of three metals doping into Ce(0.5)Zr(0.5)O(2) on photocatalytic activity of TiO2/Ce(0.45)Zr(0.45)M(0.1)O(X) (M=Y, La, Mn). The prepared photocatalysts were characterized by BET, XRD, UV-vis diffuse reflectance and XPS analyses. BET surface area of TiO2/Ce(0.45)Zr(0.45)M(0.1)O(X) (M=Y, La, Mn) is smaller than that of Ce(0.5)Zr(0.5)O(2). XRD results reveal that the deposited titania is highly dispersed as in the CeO(2)-ZrO(2) matrix, doping M in the CeO(2)-ZrO(2) lattice causes the changing of lattice space and the diffraction peaks shift to higher 2theta position. Among these four catalysts, the band gap value of TiO(2)/Ce(0.45)Zr(0.45)La(0.1)O(X) is the lowest. The binding energy value of Ti 2p(3/2) of four catalysts transfers to a lower value. The order of photocatalytic activity is TiO2/Ce(0.45)Zr(0.45)La(0.1)O(X)>TiO2/Ce(0.45)Zr(0.45)Y(0.1)O(X)>TiO2/Ce(0.45)Zr(0.45)Mn(0.1)O(X)>TiO2/Ce(0.5)Zr(0.5)O(2)>TiO2. The proposed mechanism is of electron transfer and the stronger absorption in the region 210-400 nm.     

The operating performance and products distribution of the catalytic oxidation of methyl-isobutyl-ketone over a Pt/gamma-Al2O3 catalyst

Catalytic oxidation is one of the cost-effective technologies to solve the troublesome volatile organic compounds. This study treated methyl-isobutyl-ketone (MIBK) by a commercial catalyst, Pt/gamma-Al(2)O(3), in a fixed-bed reactor. The effects of operating factors, such as operating temperature, MIBK concentration, space velocity, and O(2) concentration, on the performance of the catalyst were investigated. The products and reactants distributions from the oxidation of MIBK over Pt/gamma-Al(2)O(3) were observed. The results show that the products containing carbon atoms are CO, CO(2), and C(3)H(6)O. Two catalyst life-tests were also carried out to characterize the deactivation effect of MIBK. The result shows that the deactivation effect may be due to the coke on the catalyst surface at 423 K. From the statistical analysis, the operating temperature is the most effective factor on the conversion of MIBK. The catalysts were also characterized by surface area analysis and elemental analysis before and after the test. The results show that the catalytic deactivation may be due to carbon coating. At low temperature (423 K), the phenomenon of carbon coating was more obvious than that at high temperature (573 K). The product distributions from the oxidation of MIBK over Pt/gamma-Al(2)O(3) were analyzed by GC. The results indicate that the C(3)H(6)O is formed from the beginning, presenting a peak at 423 K, 6.54 ppm. The CO concentration also peaked at the same temperature, 6.84 ppm.     

Catalytic combustion of carbon tetrachloride

The catalytic combustion of carbon tetrachloride (CCl4) by metal oxide catalysts coated on the monolith support was investigated. The prepared catalysts were tested at temperatures between 300 and 800 degrees C and at varying gas hourly space velocity (GHSV) values with an excess air ratio of 3100%. The catalyst, whose composition was 18% Cr2O3, 2% Ce2O3 and 80% gamma-Al2O3, was found to almost completely oxidize CCl4. The operating conditions proposed are 5702 h(-1) for GHSV, 3100% excess air and a temperature slightly higher than 800 degrees C. The reaction rate expression was found to be independent of oxygen partial pressure but strongly dependent on CCl4 partial pressure.     

Mn、Fe和Cu氧化物在低温等离子体催化氧化甲苯体系中的活性比较

采用等体积浸渍法制备了MnOx/γ-Al2O3、FeOx/γ-Al2O3和CuOx/γ-Al2O3催化剂,测定了不同催化剂在低温等离子体场内分解甲苯的活性,用X射线衍射(XRD)、氢气程序升温还原(H2-TPR)技术对催化剂进行表征。结果表明催化剂分解甲苯的活性的顺序是MnOx/γ-Al2O3>FeOx/γ-Al2O3>CuOx/γ-Al2O3。催化剂分解臭氧的实验表明,不同催化活性组分对臭氧的催化分解性能顺序与对甲苯的分解性能顺序是一致的。MnOx/γ-Al2O3催化剂的Mn负载量对其催化活性有明显影响,Mn的含量为1%(质量分数)时,催化剂的活性最高,当能量密度为19J/L时,其对甲苯催化氧化的转化率接近100%。催化剂表征结果表明当Mn含量为1%(质量分数)时,氧化锰在载体γ-Al2O3上最接近单层分散量,此时活性组分与载体表面的相互结合力最强,在载体上有很好的分散性,从而表现出对甲苯分解的最好性能。     

Effect of controlling nano-sized copper by silver in copper-based catalyst on catalytic oxidation of toluene

Catalytic oxidation of VOC (toluene) over a copper based catalyst was carried out to assess its properties and performance. The Brunauer Emmett Teller (BET) method, X-ray diffraction (XRD), temperature programmed reduction (TPR), N2O pulse titration and energy dispersive spectroscopy (EDS) were used to characterize a series of 5 wt% Cu/gamma-Al2O3 catalysts modified with silver. The experimental results revealed that the addition of silver to 5 wt% Cu/gamma-Al2O3 catalyst highly enhanced its catalytic activity. With increasing addition amount of silver, the light-off curve for complete oxidation of toluene shifted to lower temperature. In addition, the increase of the addition amount of silver caused the copper particle size of 5 wt% Cu/gamma-Al2O3 catalyst to gradually increase. Subsequently, it demonstrated that the increase in the copper particle size is closely associated with the increase in catalytic activity.     

Nanosized Pt-Co catalysts for the preferential CO oxidation

The preferential CO oxidation in the presence of excess hydrogen was studied over Pt-Co/gamma-Al2O3. CO chemisorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), energy dispersive X-ray spectrometer (EDX) and temperature programmed reduction (TPR) were conducted to characterize active catalysts. The catalytic activity for CO oxidation and methanation at low temperatures increased with the amounts of cobalt in Pt-Co/gamma-Al2O3. This accompanied the TPR peak shift to lower temperatures. The optimum molar ratio between Co and Pt was determined to be 10. The co-impregnated Pt-Co/gamma-Al2O3 appeared to be superior to Pt/Co/gamma-Al2O3 and Co/Pt/gamma-Al2O3. The reductive pretreatment at high temperature such as 773 K increased the CO2 selectivity over a wide reaction temperature. The bimetallic phase of Pt-Co seems to give rise to high catalytic activity in selective oxidation of CO in H2-rich stream.     

铈锆氧化物固溶体的制备、表征及三效催化性能

采用共沉淀技术制备了Ce0.6Zr0.4O2固溶体,并对其进行了XRD、Raman光谱和SEM表征.将其用于单钯三效催化剂的制备,考察了Ce06Zr0.4O2对三效催化剂性能的影响.结果表明:Ce0.6Zr0.4O2具有和CeO2相似的立方结构,并具有较高的热稳定性;与含CeO2的三效催化剂相比,含Ce06Zr0.4O2的三效催化剂经高温老化后,仍具有较高的HC、CO、NO转化率和较低的起燃温度.     

Steam reforming of glycerol into hydrogen over nano-size Ni-based hydrotalcite-like catalysts

Steam reforming (SR) of glycerol for the production of hydrogen was investigated over the nano-sized Ni-based catalysts. The Ni-based catalysts were prepared by solid phase crystallization and impregnation methods, and characterized by N2 physisorption, CO chemisorption, XRD, SEM, and TEM techniques. The Ni/gamma-Al2O3 catalyst showed higher conversion and H2 selectivity. However, it was slowly deactivated due to the carbon formation on the surface of catalyst and the sintering. It was found that the Ni based hydrotalcite-like catalyst (spc-Ni/MgAl) showed higher catalytic activity to prevent carbon formation than Ni/gamma-Al2O3 catalyst in the SR of glycerol.     

Aqueous phase reforming of glycerol over Ni-based catalysts for hydrogen production

Aqueous phase reforming of glycerol over Ni-based catalysts for hydrogen production was carried out at 225 degrees C, 23 bar and LHSV = 4 h(-1). The Ni-based catalyst was prepared by an incipient wetness impregnation method. The catalysts before and after the reaction were characterized by N2 physisorption, CO chemisorption, XRD, TPR, SEM and TEM techniques. It was found that Ni(20 wt%)-Co(3 wt%)/gamma-Al2O3 catalyst showed higher glycerol conversion and hydrogen selectivity than Ni(20 wt%)/gamma-Al2O3 catalyst. There are no major changes in Ni particles after the reaction over Ni-Co/gamma-Al2O3 catalyst. The results suggest that the Ni-Co/gamma-Al2O3 catalyst can be applied to the hydrogen production system using APR of glycerol.     

Catalytic decomposition of 1,2-dichlorobenzene using Pt-loaded nanoporous zeolite MFI catalyst

Nanoporous zeolite MFI was prepared by using HClO4 as a promoter. A significant proportion of the synthesized zeolite MFI nanoparticles exhibited nanoporous characteristics. Although the synthesis of the zeolite MFI was completed within 6 h, the crystallinity of all the zeolite MFI was shown to be high. The synthesis time of approximately 6 h used in this study was much shorter than the conventional hydrothermal method. The feasibility of the new nanoporous zeolite MFI towards the gas phase catalytic oxidation of a model for dioxin, 1,2-dichlorobenzene, was tested by comparing the catalytic activity of Pt/nanoporous zeolite MFI with that of a Pt/gamma-Al2O3 catalyst. The catalytic activity of the Pt/nanoporous zeolite MFI was higher than that of the Pt/gamma-Al2O3 catalyst. The internal surface area and acidity appears to be a major factor for the decomposition of 1,2-dichlorobenzene.     

Aqueous phase reforming of glycerol over the Pd loaded Ni/Al2O3 catalysts

Bifunctional catalysts containing (0.5-1.5 wt%) palladium and 15 wt% of Nickel supported on gamma-Al2O3 were prepared via an impregnation technique and catalysts were characterzed by XRD BET surface area and SEM, respectively. The aqueous phase reforming of glycerol (APR) was conducted over alumina-supported catalysts at different reaction conditions for catalytic activity. Finally, we concluded that the 1.0 wt% Pd 15 wt% Ni/gamma-Al2O3 catalyst evidences higher conversion, hydrogen selectivity, lower alkane selectivity and CO production. This indicate that Pd loaded Ni/gamma-Al2O3 could be a potential catalyst for the APR of glycerol.     

Removal of oxygenated volatile organic compounds by catalytic oxidation over Zr-Ce-Mn catalysts

The composition-activity relationship of Zr-Ce-Mn-O materials was investigated for the catalytic removal of Oxygenated Volatile Organic Compounds (OVOC) emitted by stationary sources. Using a sol-gel method, very high surface specific areas, small crystallite sizes and high redox properties were obtained for Zr(0.4)Ce(0.6-x)Mn(x)O(2) catalytic systems after calcination at 500°C. The textural and redox properties were improved when Mn content increased in the material, especially for x=0.36. As a result the most active and selective catalyst in the butanol (model of OVOC) oxidation was obtained for the nominal composition Zr(0.4)Ce(0.24)Mn(0.36)O(2) due to a high oxygen mobility and surface Mn(4+) concentration.     

Mn-Cu-La/TiO_2低温催化剂催化还原氮氧化物性能研究

采用浸渍法制备了Mn-Cu-La/TiO2催化剂,研究了其组分配比、焙烧温度等制备条件和NO进口浓度、空速、O2含量、NH3/NO摩尔比等操作条件对Mn-Cu-La/TiO2上NH3低温还原NO活性的影响;探讨了H2O、SO2对Mn-Cu-La/TiO2活性的影响.结果表明,该催化剂具有很好的低温SCR活性,空速为10 000h-1,反应温度为150℃下时NO转化率接近99.6%.180℃下同时通SO2、H2O后的360min内,活性始终保持在95%以上;单独通入SO2时,该催化剂较容易中毒;单独通入体积分数10%的H2O对催化剂活性基本没有影响,转化率始终保持在98%以上.     

Oxidation treatment of diesel soot particulate on CexZr1-xO2

Catalytic oxidation of diesel soot particulate on Ce(x)Zr(1-x)O(2) catalysts was investigated. Results indicated that Ce/Zr ratios had a significant influence on the catalytic activities. Compared with the ignition temperature (T(i)) of uncatalyzed soot combustion, T(i) of Ce(0.5)Zr(0.5)O(2) with the best catalytic behavior decreased by 80 degrees C. The reactant gas compositions (O(2), H(2)O and NO) affected the catalytic activities too. O(2)-TPD, TG-DTA and XPS characterization results showed that Ce(x)Zr(1-x)O(2) released lattice oxygen continuously to promote the soot combustion even no gas oxygen occurred in the reaction atmosphere. The mechanisms of spill-over and reduction/oxidation functioned synergistically for soot catalytic combustion.     

Catalytic activity of CuOn-La2O3/gamma-Al2O3 for microwave assisted ClO2 catalytic oxidation of phenol wastewater

In order to develop a catalyst with high activity and stability for microwave assisted ClO2 catalytic oxidation, we prepared CuOn-La2O3/gamma-Al2O3 by impregnation-deposition method, and determined its properties using BET, XRF, XPS and chemical analysis techniques. The test results show that, better thermal ability of gamma-Al2O3 and high loading of Cu in the catalyst can be achieved by adding La2O3. The microwave assisted ClO2 catalytic oxidation process with CuOn-La2O3/gamma-Al2O3 used as catalyst was also investigated, and the results show that the catalyst has an excellent catalytic activity in treating synthetic wastewater containing 100 mg/L phenol, and 91.66% of phenol and 50.35% of total organic carbon (TOC) can be removed under the optimum process conditions. Compared with no catalyst process, CuOn-La2O3/gamma-Al2O3 can effectively degrade contaminants in short reaction time and with low oxidant dosage, extensive pH range. The comparison of phenol removal efficiency in the different process indicates that microwave irradiation and catalyst work together to oxidize phenol effectively. It can therefore be concluded from results and discussion that CuOn-La2O3/gamma-Al2O3 is a suitable catalyst in microwave assisted ClO2 catalytic oxidation process.