Catalytic Partial Oxidation of Methane over Ni/CeO2-ZrO2-Al2O3

Nickel catalysts supported on CeO2-ZrO2-CeO2,ZrO2-Al2O3 and Al2O3 were prepared and characterized by means of X-ray diffraction（XRD）,BET areas,H2 temperature-programmed reduction（H2-TPR）,and X-ray photoelectron spectroscopy（XPS）.Through the test of catalytic partial oxidation of methane（CPOM）,Ni/CeO2-ZrO2-Al2O3 displayed the highest activity,which resulted from its largest BET area and best NiO dispersion.Furthermore,Ni/CeO2-ZrO2-Al2O3 maintained a long-time stability in CPOM,which was attributed to its best coking resistance among all the prepared catalysts.     

Effect of Fe2O3 Loading Amount on Catalytic Properties of Monolithic Fe2O3/Ce0.67Zr0.33O2 -Al2O3 Catalyst for Methane Combustion

Ce0.67Zr0.33O2-Al2O3 solid solution was prepared by the co-precipitation method. Fe2O3-based catalysts supported on the solid solution were obtained by the impregnation method. The article revealed that the optimal loading amount of Fe2O3 on Ce0.67Zr0.33 O2-Al2O3 in our experimental condition for catalytic combustion of methane was 8% （ mass fraction）. The prepared catalysts were characterized by BET, TPR, XRD analyses, and their catalytic activity was investigated after being calcined at 873 K and after being aged in water gas at 1273 K. When the loading amount of Fe203 was 8% （ mass fraction）, the catalyst held the highest activity, and the best temperature speciality and thermal stability. The complete-conversion temperature of methane for fresh and aged sample was 788 and 838 K, respectively. The range between the light-off temperature and the complete-conversion temperature was only 15 K. The characterization results of XRD indicated that Fe2O3 was well dispersed on the Ce0.67Zr0.33O2-Al2O3 matrix. The results of BET and TPR were in good harmony with the catalytic activity results.     

Fabrication of CeZrO2 on Ni/SiO2 and promoted catalysis for methane autothemal reforming in a fluidized bed reactor

The methane autothermal reforming in the present of oxygen was studied over cerium-and zirconium-promoted Ni/SiO2 catalysts in a fluidized bed reactor. The addition of CeZrO2 resulted in a significant improvement in the initial activity of the catalysis as well as an in-crease in the stability. The long-term activity of the promoted catalyst was dependent upon the rapid redox properties between the oxidative zone and the reductive zone in a fluidized bed reactor. H2 temperature-programmed reduction (H2-TPR) and temperature-progranmaed sur-face reaction (TPSR) studies demonstrated that addition of the CeZrO2 resulted in an increase in the reducibility and oxygen transfer ability of the support, Ni/Ce0.5ZrO0.5O2-SiO2 showed improved redox properties compared with Ni/SiO2 due to a low-temperature reduction. X-ray diffraction (XRD) of the fresh and spent catalysts showed that the promoter enhanced the nickel dispersion and retarded metal particle growth during reaction at high temperature, and surface Ni was gradually oxidized by remaining O2, leading to Ni deactivation.     

Characterization of CuO Species and Thermal Solid-Solid Interaction in CuO/CeO2-Al2O3 Catalyst by In-Situ XRD, Raman Spectroscopy and TPR

Transference of CuO species and thermal solid-solid interaction in CuO/CeO2-Al2O3 catalyst prepared by an impregnation method were characterized by in-situ XRD, Raman spectroscopy and H2-TPR techniques. For the catalyst calcined at 300℃, two kinds of CuO species coexist on the surface, that is, highly dispersed and bulk CuO crystalline phase. Four kinds of CuO species are present for the catalyst calcined at 600 ℃, ： （1） highly dispersed CuO, （2） bulk CuO on the surface, （3） bulk CuO in the internal layer of CeO2, and （4） CuAl2O4 formed from CuO-Al2O3 interaction. For the catalyst calcined at 800 ℃,C, besides very little highly dispersed and bulk CuO on the surface, most of the CuO has transferred into the internal layer of CeO2 and the mass of CuAl2O4 are increased. At 900 ℃,, all of CuO has diffused into the internal layer of CeO2 and formed CuAl2O4. The results show that the distribution of CuO species in the catalysts depends on the calcination temperature; the different CuO species can be effectively confirmed by in-situ XRD, Raman spectroscopy and H2-TPR techniques.     

Effects of ZrO2 Content on Structure and Performance of Cu/CeO2-ZrO2 Catalysts for Water-Gas Shift Reaction

Water-gas shift(WGS)is a critical step in fuelprocessors for preli minary COclean-up and additionalhydrogen generation prior to the CO clean-up stage,which opened up new potential applications for WGScatalysts.Recently several formulations of noble-met-al…     

Catalytic Oxidative Properties and Characterization of CuO／CeO2 Catalysts

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Modification of Cu/ZSM-5 catalyst with CeO_2 for selective catalytic reduction of NO_x with ammonia

Cu/ZSM-5 and CeO_2-modified Cu/ZSM-5 catalysts were prepared by a wetness impregnation method. The addition of CeO_2 was found to enhance the NO_x selective catalytic reduction(SCR) activity of the catalyst at low temperatures, but the high-temperature activity was weakened. The catalysts were characterized by X-ray diffraction(XRD), nitrogen physisorption, inductively coupled plasma optical emission spectrometry(ICP-OES), X-ray photoelectron spectroscopy(XPS), electron paramagnetic resonance(EPR), H_2 temperature-programmed reduction(TPR) and NH_3 temperature-programmed desorption(TPD). The results showed that more CuO clusters instead of isolated Cu~(2+) species were obtained on the modified catalyst. These active CuO clusters, as well as the Cu-Ce synergistic effect, improved the redox property of the catalyst and low-temperatures SCR activity via promoting the oxidation of NO to NO_2 and fast SCR reaction. The loss in high-temperatures activity was attributed to the enhanced competitive oxidation of NH_3 by O_2 and decreased surface acidity of the catalyst.     

Synthesis of neodymium modified CeO2-ZrO2-Al2O3 support materials and their application in Pd-only three-way catalysts

Ce-Zr-Al-Nd2O3 (CZAN) support materials were prepared by co-precipitation and impregnation methods, respectively. They were characterized by X-ray diffraction (XRD), low temperature nitrogen adsorption-desorption, oxygen pulsing technique, H2-temperature pro-grammed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS). The Pd-only three-way catalysts (Pd-TWC) supported on these materials were prepared by incipient wetness method and studied by activity tests. The results demonstrated that the CZAN supports obtained by the two methods showed better structural, textural and redox properties than the CZA without Nd2O3, and the addition of Nd2O3 improved the catalytic activity of TWC. Especially, the CZAN-i support prepared by impregnation method had better thermal stability and redox prop-erty. Meanwhile, the Pd/CZAN-i catalyst exhibited the best catalytic performance. XPS measurements indicated that the Nd-modified sam-ples possessed more Ce3+ and oxygen vacancies on the surface of samples, which led to a better redox property. The excellent redox property of support materials helped to improve the catalytic activity of TWC.     

Effect of yttrium addition on water-gas shift reaction over CuO/CeO2 catalysts

This paper presented a study on the role of yttrium addition to CuO/CeO2 catalyst for water-gas shift reaction. A single-step co-precipitation method was used for preparation of a series of yttrium doped CuO/CeO2 catalysts with yttrium content in the range of 0-5wt.%. Properties of the obtained samples were characterized and analyzed by X-ray diffraction (XRD), Raman spectroscopy, H2-TPR, cyclic voltammetry (CV) and the BET method. The results revealed that catalytic activity was increased with the yttrium content at first, but then decreased with the further increase of yttrium content. Herein, CuO/CeO2 catalyst doped with 2wt.% of yttrium showed the highest catalytic activity (CO conversion reaches 93.4% at 250℃) and thermal stability for WGS reaction. The catalytic activity was correlated with the surface area, the area of peak y of H2-TPR profile (I.e., the reduction of surface copper oxide (crystalline forms) interacted with surface oxygen vacancies on ceria), and the area of peak C2 and A1 (Cu0→Cu2+ in cyclic voltammetry process), respectively. Besides, Raman spectra provided evidences for a synergistic Cu-Ovacancy interaction, and it was indicated that doping yttrium may facilitate the formation of oxygen vacancies on ceria.     

从腐泥土型红土镍矿制备共掺杂MgFe2O4物相转化规律及催化性能

采用酸浸-水热-煅烧法从腐泥土型红土镍矿中制备磁性多金属共掺杂型MgFe₂O₄异相类芬顿(Fenton)催化剂.利用X射线衍射(XRD)、傅立叶红外光谱(FTIR)、扫描电子显微镜(SEM)和比表面积及孔径分布测定(BET-BJH)等手段, 考察了煅烧温度对所制备产物结构、形貌和比表面积及孔径分布的影响, 并研究了所制备产物作为异相Fenton催化剂降解罗丹明B (RhB)溶液的催化活性.结果表明, 水热合成产物为层状双(多)金属氢氧化物和尖晶石型MgFe₂O₄复合物.通过300℃的煅烧, 层状双(多)金属氢氧化物就能分解并生成MgFe₂O₄; 随着煅烧温度的提高, 产物结晶度增加、粒径尺寸变大, 形貌逐渐生长为近球型颗粒且分散度渐渐提高, 同时介孔数量减少、比表面积减小.经过500℃煅烧的试样H-C500显示出优异的催化降解活性.在体系反应温度为45℃、pH值为6.44、催化剂用量为0.625 g·L-1且H₂O₂体积分数为1.0%的条件下, 经过300 min, 10 mg·L-1的罗丹明B溶液降解率可达到97.8%, 同时总有机碳(TOC)去除率达到77.8%.重复使用3次后, 催化剂仍能保持较高活性, 降解率和TOC去除率减少量分别少于3.0%和5.0%.      

CeO_2/CuO catalysts using different template agent for preferential CO oxidation in H_2-rich stream

The CeO_2/CuO catalysts using different template agent(F68 L64, F127 and P123) were synthesized by the simple template and impregnation method. They were characterized by FESEM, XRD, N2 physisorption and H2-TPR techniques. It is found that the CeO_2/CuO catalysts are double pore distribution, and CeO_2 can enter into the gap of CuO supports and form the contact interface of copper and cerium. Among the asprepared catalysts, the CeO_2/CuO-F127 catalyst displays better activity at lower temperature and the CeO_2/CuO-P123 catalyst presents higher activity at higher temperature. The CeO_2/CuO-P123 catalyst has the smallest crystallite sizes of CuO and CeO_2 as well as the largest size of cubes, which may improve the interaction of copper and cerium and enhance the performance of CO oxidation.     

Methane Combustion and TPR/TPO Properties of Pd/CexZr1-xO2/Al2O3 Catalysts

Methane Combustion and TPR/TPO Properties of Pd/Ce_xZr_ 1-xO_2/Al_2O_3 Catalysts     

Partial oxidation of methane on Ni/CeO2-ZrO2/γ-Al2O3 prepared using different processes

The influences of CeO2-ZrO2 and γ-Al2O3 mixing methods on the catalytic activity and stability of partial oxidation of methane （POM） were investigated over Ni/Ce0.7Zr0.3O2-Al2O3 catalysts. The catalysts were characterized by XRD, TPR, H2-chemsorption, and TG-DTA. For fresh catalysts, the results showed that the salt precursor mixing catalyst （ATOM） presented better performance than the catalysts prepared by the precipitator mixing method （MOL） and the powder mechanically mixing method （MECH）. The result of XRD suggested that the interaction between CeO2-ZrO2 and Al2O3 in ATOM sample was stronger than the others, which led to more lattice defects and thereby better initial activity. Moreover, the MECH sample had the best stability and the least coke deposition in 24 h stability tests. The results of TPR and H2-chemsorption indicated that the intimate contact of Ni-Al in MECH sample enhanced the ability of resisting coke deposition and metal sintering.     

Synthesis and Photocatalytic Activity of TiO2/V2O5 Composite Catalyst Doped with Rare Earth Ions

TiO2/V2O5 catalyst doped with rare earth ions was prepared by sol-gel method. Titanium tetrapropoxide and vanadium pentoxide were used as precursor of the composite catalyst and rare earth ions were used as dopant. The crystal phases, crystalline sizes, microstructure, absorption spectra of doped composite catalyst were studied by XRD, EDS, FT-IR and UV-Vis. Photoactivity of the prepared catalyst under ultraviolet irradiation were evaluated by degradation of methyl orange （MO） in aqueous solution. It is shown that the prepared catalyst is composed of anatase and futile. The rare earth ions are highly dispersed in composite catalyst. All the doped catalysts appear higher photocatalytic activity than TiO2/V2O5 catalyst and catalyst doped with Ce^4＋ present the best activity to MO.     

Catalytic combustion of diesel soot over K2NiF4-type oxides La2-xKxCuO4

Nanostructure K2NiF4 type oxides La2-xKxCuO4 complex oxides were prepared using the Sol-Gel method, characterized by X-Ray Diffraction （XRD）, Fourier Transform Infrared （FT-IR）, and Scanning Electron Microscopy （SEM）. The catalytic activity for soot combustion was evaluated by the Temperature-Programmed Reaction （TPO） technique. The results demonstrated that the substitution quality of K^＋ for La^3＋ at the A-site would increase the catalytic activities of La2-xKxCuO4 for soot combustion greatly; the substitution quality affected the structure and catalytic activity obviously. The La1.8K0.2CuO4 complex oxides with tetrahedral structures had the best catalytic activity for soot combustion, and the ignition temperature of soot combustion was lowered from 490 to 320 ℃.     

Preparation, Characterization of CuO／CeO2 and Cu／CeO2 Catalysts and Their Applications in Low-Temperature CO Oxidation

CeO2 was synthesized via sol-gel process and used as supporter to prepare CuO/CeO2, Cu/CeO2 catalysts by impregnation method. The catalytic properties and characterization of CeO2, CuO/CeO2 and Cu/CeO2 catalysts were examined by means of a microreactor-GC system, HRTEM, XRD, TPR and XPS techniques. The results show that CuO has not catalytic activity and the activity of CeO2 is quite low for CO oxidation. However, the catalytic activity of CuO/CeO2 and Cu/CeO2 catalysts increases significantly. Furthermore, the activity of CuO/CeO2 is higher than that of Cu/CeO2 catalysts.     

Removal of Cooking Fume by Catalytic Combustion on Pt/La-Al2O3 ＋ Ce0.5 Zr0.5O2 Catalyst

Four monolithic catalysts with low concentration of noble metal were prepared by the immersion method [ Pt/La- Al2O3, Pt/La-Al2O3 ＋ Pt/OSM （2 ： 1 ）, Pt/La-Al2O3 ＋ Pt/OSM （ 1 ： 1 ） Pt/La-Al2O3 ＋ Pt/OSM （ 1 ： 2） ], and measurements of their activity were carded out in a conventional fixed-bed flow reactor. The results show that the oxygen storage material （OSM） that is added can promote the activity of the prepared catalysts and can decrease the complete conversion temperature of cooking fume. When the ratio between La-Al2O3 and OSM is 1 ： 1, the catalyst has the highest activity, and the complete conversion temperature of cooking fume is 270℃ ; the catalyst thus prepared can be applied in a wide range of gas hourly space velocity （GHSV） [from 10000 to 60000 h^-1]. The catalyst obtained shows great potential for practical application.     

Photocatalytic activity of cerium-doped mesoporous TiO2 coated Fe3O4 magnetic composite under UV and visible light

A novel kind of magnetically separable photocatalyst of cerrium-doped mesoporous titanium dioxide coated magnetite (Ce/MTiO2/ Fe3O4) was prepared and its activities under UV and visible light were reported. The catalysts with Ce/MTiO2 shell and Fe3O4 core were pre-pared by coating photoactive Ce/MTiO2 onto a magnetic Fe3O4 core through the hydrolysis of tetrabutyltitanate (Ti(OBu)4, TBT) with pre-cursors of ammonium ceric nitrate and TBT in the presence of Fe3O4 particles. The MTiO2 shell was for photocatalysis, the Fe3O4 core was for separation by the magnetic field and the doped Ce was used to enhance the photocatalytic activity of MTiO2. The morphological, struc-tural and optical properties of the prepared samples were characterized by Brunauer-Emmett-Teller (BET) surface area, transmission electron microscopy (TEM), X-ray diffraction (XRD) and UV-vis absorption spectroscopy. The effect of cerrium-doped content on the photocatalytic activity was studied and the result revealed that 0.5 mol.% Ce/MTiO2/Fe3O4 exhibited highest photoactivity. The photocatalytic activities of obtained photocatalysts under UV and visible light were estimated by measuring the degradation rate of methylene blue (MB, 50 mg/L) in an aqueous solution. The results showed that the prepared photocatalyst was activated by visible light and used as effective catalyst in photooxi-dation reactions. In addition, the possibility of cyclic usage of the prepared photocatalyst was also confirmed. Moreover, Ce/MTiO2 was tightly bound to Fe3O4 and could be easily recovered from the medium by an external magnetic filed. So, the photocatalyst can be reused without any mass loss. It can therefore be potentially applied for the treatment of water contaminated by organic pollutants.     

Catalytic performance for methane combustion of supported Mn-Ce mixed oxides

A series of supported Mn-Ce mixed oxide catalysts were prepared by the impregnation method and used for the oxidation of methane. The catalysts were characterized by N2 adsorption （BET）, X-ray diffraction （XRD）, laser Raman spectrum （LRS）, and temperature programmed reduction （TPR） techniques. The XRD and LRS results confirmed the high dispersion of active components or formation of solid solution between manganese and cerium oxides in the bulk and on the surface of mixed oxide catalysts. The reducibility was remarkably promoted by the stronger synergistic interaction between the two oxides from H2-TPR measurements. As expected, all the experimental mixed oxide catalysts showed excellent activity for methane combustion at low temperature. Especially, for the catalyst with Mn-Ce ratio 3：7, methane conversion reached 92% at a temperature as low as 470 ℃.     

Structure and Catalytic Behavior of CuO-ZrO-CeO2 Mixed Oxides

The effect of doping CuO on the structure and properties of zirconia-ceria mixed oxide was studied. The results show that addition of CuO decreases the reduction temperature of ceria, and stabilizes the cubic structure of mixed oxides, and enhances catalytic activity of CuO-ZrO-CeO2 mixed oxides for CO oxidation. Increasing ceria content in the mixed oxides can enhance the catalytic activity, but some impurities such as sulfate make catalytic activity falling. There is little effect of calcination temperature on catalytic activities, implying that these catalysts are effective with good thermal stability.