Performance of mesoporous CeO2-Cr2O3 mixed metal oxides applied to benzene catalytic combustion

In this paper,a hydrothermal method was used to prepare(Ce,Cr)-MOF with different Ce/Cr molar ratios and then a series of CeO₂-Cr₂O₃ mixed metal oxides(CeCr-MMO) with mesoporous structure were prepared by thermal decomposition of these MOFs at different temperatures.After a series of characterization techniques were applied to test the physicochemical properties of the materials,it is found that thermal decomposition temperature(TDT) and Ce/Cr molar ratios have i...     

MCM-41 supported nano-sized CuO-CeO_2 for catalytic combustion of chlorobenzene

In this paper,MCM-41 was synthesized by a soft template technique and MCM-41 supported CuO-CeO_2 nano-sized catalysts with different Cu/Ce molar ratios were prepared by a deposition-precipitation method.N_2 adsorption,HRTEM-EDS,H_2-TPR,XPS characterization,as well as catalytic activity and durability tests for the catalytic combustion of chlorobenzene(CB) were conducted to explore the relationship between the structure and catalytic performance of the catalysts.It is revealed that cuCe(6:1)/MCM-41 has the highest activity and can completely catalyze the degradation of CB at 260℃.The reasons for the high activity of the catalysts are as follows:MCM-41,a type of mesoporous material which has large pore size and large specific surface area,is suitable as a catalyst carrier.The average diameter of nano-sized CuO and CeO_2 particles is about 3-5 nm and adding CeO_2 improves the dispersion of active component CuO,which are highly and evenly dispersed on the surface of MCM-41.Characterization results also explain why MCM-41 supported CuO-CeO_2 with appropriate proportion can highly enhance the catalytic activity.The reason is that CeO_2 acting as an oxygen-rich material can improve the mobility of oxygen species through continuous redox between Ce~(4+)and Ce~(3+),and improve the catalytic performance of CuO for CB combustion.Besides,CuCe(6:1)/MCM-41 also displays good durability for CB combustion,both in the humid condition and in the presence of benzene,making it a promising catalytic material for the elimination of chlorinated VOCs.     

Support interaction of Pt/CeO_2 and Pt/SiC catalysts prepared by nano platinum colloid deposition for CO oxidation

The interaction between Pt and its various supports can regulate the intrinsic electronic structure of Pt particles and their catalytic performance.Herein,Pt/CeO_2 and Pt/SiC catalysts were successfully prepared via a facile Pt colloidal particle deposition method,and their catalytic performance in CO oxidation was investigated.XRD,TEM,XPS and H_2-TPR were used to identify the states of Pt particles on the support surface,as well as their effect on the performance of the catalysts.Formation of the Pt-O-Ce interaction is one of the factors controlling catalyst activity.Under the oxidative treatment at low temperature,the Pt-O-Ce interaction plays an important role in improving the catalytic activity.After calcining at high temperature,enhanced Pt-O-Ce interaction results in the absence of metallic Pt~0 on the support surface,as evidenced by the appearance of Pt~(2+) species.It is consistent with the XPS data of Pt/CeO_2,and is the main reason behind the deactivation of the catalyst.By contrast,either no interaction is formed between Pt and SiC or Pt nanoparticles remain in the metallic Pt~0 state on the SiC surface even after aging at 800℃in an oxidizing atmosphere.Thus,the Pt/SiC shows better thermal stability than Pt/CeO_2.The interaction between Pt and the active support may be concluded to be essential for CO oxidation at low temperature,but strong interactions may induce serious deactivation of catalytic activity.     

Low-temperature thermocatalytic particulate carbon decomposition via urea solution-combustion derived CeO_2 nanostructures

A facile,one-pot,urea solution combustion route was utilized to synthesize highly catalytic CeO_2 nanostructures.CeO_2 prepared under varying thermal conditions was characterized by electron microscopy,energy dispersive X-ray spectroscopy,X-ray diffraction,X-ray photoelectron spectroscopy,infrared and Raman techniques.As the synthesis temperature is raised from 400 to 1000℃,the crystallite size and dspacing of nanoparticles are observed to reduce while cell parameters remain in the same range.Particle size exhibits an accession from ～20 to ～50 nm along the process.Initial CeO_2 nanoparticles are detected as a composite structure of CeO_2 and graphitic carbon nitride(g-C_3 N_4) produced by the pyrolysis of urea.Concerning the solid carbon particulate oxidation capacity,an outstanding performance is exhibited by CeO_2 synthesized at 800℃ where the oxidation onset temperature is reduced by 27% compared with the others.The superior performance is attributed to the carbon nitride-generated unique CeO_2 nanomorphology consolidating ample reactive sites and facilitated oxygen delivery for a highly efficient thermocatalytic process.Concerning atmospheric pollution mitigation,synthesis of these CeO_2 nanostructures represents a cost effective and convenient abatement technique for carbon particulates in comparison to cost-intensive,environmentally detrimental and noble-metal based techniques.     

Effect of calcination process on performance of 3DOM CeMnO_3 catalysts

A series of 3DOM CeMnO_3 perovskite catalysts were prepared by poly(methyl methacrylate) hardtemplating-excessive impregnation method at calcination temperature of x℃(x=600,700,800) and the heating rate of y ℃/min(y=1,2,5,10).The samples were characterized by Brunauer-Emmett-Teller method,scanning electron microscopy,transmission electron microscopy,H_2-temperature programmed reduction,X-ray photoelectron spectroscopy,X-ray diffraction,moreover,the effect of the calcination process on the catalytic activity of the samples were discussed by the catalytic combustion of toluene.The results show that the 3DOM CeMnO_3 catalysts calcined at 600℃ promote the formation of a perovskite structure,inhibit the reduction of the Mn~(4+) species in the catalyst with high temperature.The catalyst expresses the complete macroporous structure,large specific surface area(38.8 m~2/g),higher adsorption oxygen concentration and Mn~(4+) substance concentration,with a low T_(90%)=172℃.By preparing the catalysts at different calcination heating rates,it can be concluded that the catalyst possesses a high concentration of adsorbed oxygen and a low reduction temperature and a large specific surface area(40.42 m~2/g) greatly promotes adsorption stage catalytic oxidation reaction and catalytic combustion of toluene at low temperature under the heating rate of 5℃/min.When the heating rate is 1 ℃/min,the catalyst has a complete macroporous structure(250 nm),which is beneficial to the exchange of macromolecular substances during the catalytic reaction and the catalyst has a high concentration of lattice oxygen suitable for the catalysis of toluene in high temperature flue gas combustion.     

Catalytic combustion of soot over Ru-doped mixed oxides catalysts

We employed modified substrates as outer heterogeneous catalysts to reduce the soot originating from the incomplete diesel combustion. Here, we proposed that ceria（CeO2）-based catalysts could lower the temperature at which soot combustion occurred from 610 oC to values included in the operation range of diesel exhausts（270–400 oC）. Here, we used the sol-gel method to synthesize catalysts based on mixed oxides（ZnO：CeO2） deposited on cordierite substrates, and modified by ruthenium nanoparticles. The presence of ZnO in these mixed oxides produced defects associated with oxygen vacancies, improving thermal stability, redox potential, sulfur resistance, and oxygen storage. We evaluated the morphological and structural properties of the material by X-ray diffraction（XRD）, Brumauer-emmett-teller method（BET）, temperature programmed reduction（H2-TPR）, scanning electron microscopy（SEM）, and transmission electron microscopy（TEM）. We investigated how the addition of Ru（0.5 wt.%） affected the catalytic activity of ZnO：CeO2 in terms of soot combustion. Thermogravimetric analysis（TG/DTA） revealed that presence of the catalyst decreased the soot combustion temperature by 250 oC, indicating that the oxygen species arose at low temperatures, which was the main reason for the high reactivity of the oxidation reactions. Comparative analysis of soot emission by diffuse reflectance spectroscopy（DRS） showed that the catalyst containing Ru on the mixed oxide-impregnated cordierite samples efficiently oxidized soot in a diesel stationary motor： soot emission decreased 80%.     

Double perovskite anti-supported rare earth oxide catalyst CeO_2/La_2CoFeO_6 for efficient ventilation air methane combustion

Ventilation air methane is one of available resources with a massive reserve.However,most of ventilation air methane is discharged into the air and pollutes the environment.Catalysts with high temperature resistance(>800℃)for ventilation air methane are very essential for utilization of the ventilation air methane.We mainly prepared catalysts CeO₂/La₂CoFeO₆and La₂CoFeO₆/CeO₂and comparative samples CeO₂and La₂CoFeO₆by the simple sol-gel method and calcined them under 9000C,and tested the catalytic performance of ventilation air methane combustion under the condition of 5 vol%H₂O.The experimental results show that the light-off temperature(T_1O)and complete combustion temperature(T₉₀)of the ventilation air methane combustion reaction of CeO₂/La₂CoFeO₆catalyst are 417.4 and 587.7℃,respectively.T_1Oand Tgo of La₂CoFeO₆/CeO₂only reach 425.5 and 615.8℃.The T₁₀and T_9Oof CeO₂/La₂CoFeO₆are 417.4 and 587.7℃,which are lower than those of La₂CoFeO₆[T₁₀=452.4℃and T₉₀=673.0℃)and La₂CoFeO₆/CeO₂(T₁₀=425.5℃and T₉₀=615.8℃).Therefore,the catalytic performance of the anti-supported rare earth oxide catalyst CeO₂/La₂CoFeO₆is better than that of La₂CoFeO₆and supported catalyst La₂CoFeO₆/CeO₂.     

Effect of active oxygen on the performance of Pt/CeO2 catalysts for CO oxidation

This study was focused on the influence of active oxygen on the performance of Pt/CeO_2 catalysts for CO oxidation. A series of CeO_2 supports with different contents of active oxygen were obtained by adding surfactant at different synthesis steps. 0.25 wt% Pt was loaded on these CeO_2 supports by incipientwetness impregnation methods. The catalysts were characterized by N2 adsorption, X-ray diffraction(XRD), high-resolution transmission electron microscopy(HRTEM), H_2 temperature-programmed reduction(H_2-TPR), dynamic oxygen storage capacity(DOSC) and in-situ DRIFTS technologies. For S-f supports, the surfactant was added into the solution before spray-drying in the synthesis process, which facilitates more active oxygen formation on the surface of CeO_2. After loading Pt, the more active oxygen on CeO_2 contributes to dispersing Pt species and enhancing the CO oxidation activity. As for the aged samples,Pt-R-h shows the highest activity above 190 ℃ because of the presence of more partly oxidized Pt~(δ+) species. Thus the activity is also influenced by the states of Pt and the Pt~(δ+) species may contribute to the high activity at elevated temperature.     

Fabrication of La_(1-x)Ca_xFeO_3 perovskite-type oxides with macro-mesoporous structure via a dual-template method for highly efficient soot combustion

A series of three-dimensionally ordered macro-mesoporous(3DOMM) La_(1-x)Ca_xFeO_3(x=0-0.3)perovskite-type oxides were designed and successfully fabricated for the first time via a dual-template method.In which,PMMA and Brij-56 were employed as the hard template and soft template,respectively.It is found that 3 DOMM La_(1-x)Ca_xFeO_3 exhibits abundant wormlike mesoporous channels about 3 nm in diameter on macroporous skeleton walls.The excellent catalytic activity of soot combustion benefits from not only the well-designed hierarchical porous structure of catalyst,but also the redox electron pair of Fe~(3+)/Fe~(4+) induced by the doping of low-valent alkaline earth metal Ca to A-site of LaFeO_3.3DOMM La_(0.8)Ca_(0.2)FeO_3 exhibits superior catalytic performance for soot combustion,which shows T_(50) of396℃.It is 189℃lower than that without catalyst.A combination of structure and composition in the design of catalyst can be widely extended to other catalytic systems.     

Rh/CeO2 composites prepared by combining dealloying with calcination as an efficient catalyst for CO oxidation and CH4 combustion

In this paper, a series of Rh/CeO₂ catalysts with three-dimensional porous nanorod frameworks and large specific surface area were prepared by chemical dealloying Al–Ce–Rh precursor alloys and then calcining in pure O₂. The effects of the Rh content and calcination temperature on CO oxidation and CH₄ combustion were studied, and the results reveal that the Rh/CeO₂ catalysts produced by dealloying melt-spun Al_91.3Ce₈Rh_0.7 alloy ribbons and then calcining at 500 °C exhibit the best catalytic activity, the reaction temperatures for the complete conversion of CO and CH₄ are as low as 90 and 400 °C, respectively. Furthermore, after 150 h of continuous testing at high concentrations of H₂O and CO₂, the nature of the catalyst is not irreversibly destroyed and can still return to its initial level of activity. This excellent catalytic activity is attributed to a portion of Rh being uniformly distributed on the CeO₂ nanorod surface in the form of nanoparticles, forming strong Rh–CeO₂ interfacial synergy. Another portion of Rh permeated into the CeO₂ lattice, which results in a significant increase in the number of oxygen vacancies in CeO₂, thus allowing more surface active oxygen to be adsorbed and converted from the gas phase. Moreover, the catalytic reaction can proceed even in an oxygen-free environment due to the excellent oxygen storage performance of the Rh/CeO₂ catalyst.     

A mechanic insight into low-temperature catalytic combustion toward ethylene oxide over Pt-Ru/CuCeOx bimetallic catalyst

The catalytic oxidation performance toward ethylene oxide(EO) and the consequent mechanism were investigated on the Pt-Ru/CuCeO_x bimetallic catalyst,which was prepared by a distinct method combining stepwise adsorption and subsequent impregnation.The catalytic tests show that the introduction of Ru into the Pt catalyst,so as to form Pt-Ru bimetallic active sites,can greatly increase the oxidation activity of the catalyst,as evidenced by the extremely lower full oxidation temperature(1...     

Understanding the role of tungsten on Pt/CeO2 for vinyl chloride catalytic combustion

Spherical CeO₂ synthesized by the hydrothermal process was used as support to prepare Pt/WO₃/CeO₂,and the effects of tungsten(W) contents on activity,stability and polychlorinated by-products were investigated to understand the role of W for vinyl chloride(VC) catalytic oxidation.The introduction of12 wt% W to Pt/CeO₂(P12 WC) exhibits the highest catalytic activity with 90% conversion of VC at 250℃,meanwhile the stability improves and the polychlorinat...     

Catalytic combustion of toluene on Pt/Al2O3 and Pd/Al2O3 catalysts with CeO2,CeO2-Y2O3 and La2O3 as coatings

CeO₂,La₂O₃,and CeO₂-Y₂O₃ oxides were coated on the surface of spherical granular AI₂O₃(3-5 mm)through impregnation method,and proved as better supports of Pd and Pt catalysts.The influences of rare earth metal doping on the adsorption rates of Pd and Pt ions,as well as the catalytic performance,were investigated.Results show that the H₂PtCl₆·6H₂O adsorption rates of the Al     

Low-temperature catalytic combustion of trichloroethylene over MnOx-CeO2 mixed oxide catalysts

The cerium-based catalysts were investigated for the catalytic co mbustion of trichlo roethylene(TCE) and exhibit a surprising catalytic activity.MnO_x was doped into CeO₂ by a citric acid(CA) sol-gel method,and the effect of Mn content on the physicochemical properties and catalytic activities of MnO_x-CeO₂ mixed oxides was investigated systemically.The introduction of MnO_x into CeO₂ can evidently improve the catalytic activity and...     

Construction of mesoporous ceria-supported gold catalysts with rich oxygen vacancies for efficient CO oxidation

Bearing unique redox nature and high oxygen storage capacity, ceria (CeO₂) has always been a promising CO oxidation catalyst support for gold (Au) catalysts and the like. Herein, a series of Au–CeO₂–P (P stands for pH value) samples was prepared by a co-precipitation method with the assistance of an alkaline environment and amino groups functionalized ordered mesoporous polymer (OMP-NH₂). Afterward, all samples described above were characterized that the Au–CeO₂–P catalysts are made of Au–Ce–O solid solution and Au nanoparticles (NPs) supported on CeO₂. It turns out that OMP-NH₂ is not just a simple sacrificial template for mesoporous structure, but also plays an important role as an amino source, explaining the presence of rich oxygen vacancies. Due to the concentration of oxygen vacancies in Au–Ce–O solid solution is the key factor for the oxygen mobility of CO oxidation, the catalytic results also demonstrate that the catalytic activity of Au–CeO₂–P catalysts is related to the concentration of their oxygen vacancies. Moreover, Au–CeO₂-9.6 with a highest concentration of oxygen vacancies (as high as 13.98%) in Au–CeO₂–P catalysts exhibits the best catalytic activity (complete conversion at 10 °C).     

Catalytic decomposition of ethyl acetate over La-modified Cu-Mn oxide supported on honeycomb ceramic

The La-modified Cu-Mn spinel oxide was successfully coated onto honeycomb ceramic by a washcoating method for complete catalytic decomposition of ethyl acetate.The La-modified Cu-Mn oxides were characterized by X-ray diffraction,X-ray fluorescence,H_2-temperature programmed reduction,Brunauer-Emmett-Teller method,field-emission scanning electron microscopy and high-resolution transmission electron microscopy.The effects of different precipitants and rare earth doping on the structure and catalytic performance of the catalysts were investigated.The results show that the CuMn_2 O_4 spinel with(NH_4)_2 CO_3 as a precipitant can form a larger specific surface area and a suitable pore size,which is beneficial to the absorption of ethyl acetate.Although the rare earth doping does not significantly change the crystal phase structure of the catalyst,it improves its reducibility and lowers the temperature of the catalytic decomposition.With respect to the catalytic decomposition of ethyl acetate,the rare earth-modified Cu-Mn oxide supported on honeycomb ceramic shows excellent catalytic performance with 100% conversion under the conditions of 239℃,space velocity of 12500 h~(-1) and1000 ppm.And the ethyl acetate removal rate is still 100% after 1440 min of continuous reaction.     

Catalytic action of rare earth oxide (La2O3, CeO2, Pr6O11) on electrochemical oxidation of activated carbon in molten KOH–NaOH

The oxidation of anode carbon fuel directly affects the electrochemical performance of molten hydroxide direct carbon fuel cell (MHDCFC). In general, the anode carbon fuel can be oxidized at high temperature, thus the direct carbon fuel cell (DCFC) can show great electrochemical performance. In this study, rare earth oxides (La₂O₃, CeO₂, Pr₆O₁₁) were prepared by the method of precipitation. Activated carbon was prepared by pretreatment of lignite. Rare earth oxides and activated carbon were mixed as anode carbon fuel, and rare earth oxides were used to catalyze the electrochemical oxidation of anode carbon fuel. The results show that CeO₂ has better electrocatalytic activity compared with La₂O₃ and Pr₆O₁₁ in the MHDCFC. The electrochemical test results show that the current density (at 0.4 V) increases from 81.02 to 112.90 mA/cm² and the maximum power density increases from 34.78 to 47.05 mW/cm² at 450 °C, when the mass fraction of CeO₂ is increased from 0 to 40%. When the mass fraction of CeO₂ is 30%, the current density (82.55 mA/cm² at 0.4 V) at 400 °C is higher than that (81.02 mA/cm² at 0.4 V) without CeO₂ at 450 °C. The electrochemical oxidation mechanism of CeO₂ catalyzed anode carbon fuel is discussed.     

Effect of synthesis time on morphology of CeO_2 nanoparticles and Au/CeO_2 and their activity in oxidative steam reforming of methanol

Ceria(CeO_2)supports,synthesized by hydrothermal treatment with different synthesis time(CeO_2-X h,where X is the synthesis time in h)in the presence of the surfactant cetyltrimethyl ammonium bromide,were used as supports for gold(Au)catalysts.The synthesis time significantly affects the morphological structure and crystallite size of CeO_2,where CeO_2-2 h has the smallest crystallite size with coexisting nanorods and nanoparticles.Transmission electron microscopy analysis confirms the morphology of CeO_2 with distinctive(110),(100)and(111)planes,in agreement with interplanar spacings of 0.19,0,27 and 0.31,respectively.However,the morphology of CeO_2-8 h and CeO_2-48 h is mainly a truncated octahedral with crystal planes(111)and(100)accompanied by an interplanar spacing of 0.31 and0.27 nm,respectively.The CeO_2-X h supports and those with a 3 wt%Au loading(Au/CeO_2-X h)were investigated in the oxidative steam reforming of methanol at temperatures between 200 and 400 ℃.The Au/CeO_2-2 h gave the highest methanol conversion level and hydrogen yield at a low temperature of 250 ℃.This superior catalytic performance results from the good interaction between the metal and support and the well-distributed Au species on the CeO_2 support.     

Effect of interaction between different CeO2 plane and platinum nanoparticles on catalytic activity of Pt/CeO2 in toluene oxidation

The plane exposure of support vitally affects the catalytic performance of the catalyst. In this work, CeO₂ nanorods ((110) plane exposure), nano-octahedrons ((111) plane exposure) and nano-cubes ((100) plane exposure) were prepared as the supports of Pt/CeO₂ samples to investigate the effect of CeO₂ plane exposure on total toluene oxidation. Characterizations reveal that the (110) plane of CeO₂ is more helpful to the dispersion of Pt species, followed by (111) face. The improved dispersion of Pt species can enhance the metal-supports interaction, which promotes the electron transfer of CeO₂ carrier to Pt nanoparticles and the adsorption-activation of O₂, thereby facilitating the total oxidation of toluene via the Langmuir–Hinshelwood (L-H) mechanism. Therefore, Pt/CeO₂-r (nanorods) sample expresses excellent catalytic performance of toluene oxidation. Finally, the procedure of toluene total oxidation was studied by in-situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy. We expect that this work can contribute to the development of an effective sample for the decomposition of volatile organic compounds (VOCs).     

Effect of CuO species and oxygen vacancies over CuO/CeO2 catalysts on low-temperature oxidation of ethyl acetate

The catalytic oxidation of ethyl acetate(EA) was studied over CuO/CeO₂ catalysts which were prepared by ball milling with different precursors(copper oxide,cerium acetate,cerium dioxide,copper acetate and cerium hydroxide).The CuO/CeO₂ catalyst(O-A) prepared with copper oxide and cerium acetate as precursors shows very high catalytic activity that 100% EA conversion is achieved at low temperature of 220℃.It is found that specific surface area(112.8 m²/g),particle...