Effect of loading content of copper oxides on performance of Mn-Cu mixed oxide catalysts for catalytic combustion of benzene

A series of Mn-Cu mixed oxide catalysts were prepared by precipitation method. The catalysts were characterized by N 2 adsorption-desorption, H 2 -TPR and XPS. When the loading ratio of manganese oxides to copper oxides was 8:2 or 7:3, the catalysts possessed better catalytic activity, and benzene was converted completely at 558 K. Results of H 2 -TPR showed that the loading of a small amount of copper oxides decreased the reduction temperature of catalysts. Results of XPS showed that the loading of a small amount of copper oxides increased the proportion of manganese and defective oxygen on the surface of catalysts, and stabilized manganese at higher oxidation state. And the catalyst with the loading ratio 7:3 was a little worse than 8:2, since the interaction between manganese oxides and copper oxides is too strong, copper oxides migrate to the surface of catalysts and manganese oxides in excess are immerged.     

In-situ synthesis of monolithic Cu-Mn-Ce/cordierite catalysts towards VOCs combustion

A monolithic series of Cu-Mn-Ce oxides supported on cordierites with different Cu/Mn/Ce molar ratios were prepared by the in-situ sol-gel method without any binder. The catalysts were characterized by scanning electron microscopy (SEM), energy dispersive spectrometer (EDS), X-ray diffraction (XRD), and Brunauer-Emmett-Teller method (BET) and examined in the catalytic combustion of volatile organic compounds (VOCs). The results showed that the well-dispersed nanometer particles of mixed oxides adhered firmly...     

Effect of metal doping into Ce0.5Zr0.5O2 on catalytic activity of MnOx/Ce0.5-xZr0.5-xM0.2xOy/Al2O3 for benzene combustion

The research investigated the effect of doping two metals separately or together into Ce0.5Zr0.5O2 on the catalytic activity of MnOx/Ce0.5–xZr0.5–xM0.2xOy/Al2O3 (M=Y, Mn, Y and Mn) for catalytic combustion of benzene. The prepared catalysts were characterized by X-ray diffraction (XRD), surface area analysis, oxygen storage capacity (OSC), and H2-temperature programmed reduction (H2-TPR). Cata-lytic test was performed on a conventional fixed bed flow reactor. The characterization results revealed that Y and Mn ions entered into the ceria-zirconia mixed oxides framework, which improved the textural properties and greatly promoted the MnOx dispersion on the support surface. The complete conversion temperature of benzene on MnOx/Ce0.4Zr0.4Y0.1Mn0.1Oy /Al2O3 was 563 K, and the selectivity of carbon dioxides was 99%. This catalyst could be applied in a wide range of GHSV and wide concentration condition, showing great potential for application.     

Palladium catalysts supported on novel CexY1-xO washcoats for toluene catalytic combustion

Novel CexY1-xO washcoats adhered on the cordierite honeycomb, used as supports for Pd catalysts, were prepared by an impregnation method. It was fotmd that the CexY1-xO washcoats had better adhesion and higher adsorption efficiency of H2PdCl4, and the optimal component of the washcoat was Ce0.8Y0.2O. Model reaction of catalytic combustion of toluene was chosen to evaluate the performance of the developed Pd/CexY1-xO/substrate catalysts. The results showed that the catalytic performance of the Pd/CexY1-xO/substrate catalysts depended on the component of the washcoats, with the Pd/Ce0.8Y0.2O/substrate catalyst giving the best catalytic activity and thermal stability.     

Promotional effects of cerium doping and NO_x on the catalytic soot combustion over MnMgAlO hydrotalcite-based mixed oxides

A series of MnMgAlO samples with different amounts of Ce doping were facilely prepared using coprecipitation method and their catalytic soot combustion activity was evaluated by temperature programmed oxidation reaction(TPO).The methods of X-ray diffraction(XRD),Brumauer-Emmett-Teller(BET),H2-TPR,NO-TPO and in situ IR were used to characterize the physiochemical properties of these samples.Dopant Ce improved the soot combustion performance of MnMgAlO catalyst due to the enhanced redox ability.Introduction of NOx led to the further increase of catalytic soot oxidation activity on these samples.Over Ce-containing samples,the catalytic activity was slightly decreased as the amount of dopant Ce increased in O2.Differently,in NO+O2,a certain amount of dopant Ce was much more favorable and excess amount of Ce resulted in a sharp drop of the catalytic soot combustion activity.Both NO2 and nitrates were found to have great contributions to the effects of NOx on the soot combustion activity of Ce-doped catalysts.More NO2 was generated as dopant Ce increased.When appropriate amount of Ce was introduced,the as-formed NO2 was stored as bridging bidentate nitrate on Mn-Ce site,which was confirmed to have higher reactivity with soot than nitrite or monodentate nitrate on Mn and/or Ce sites.Overall,Mn0.5Mg2.5Ce0.1Al0.9O was considered as the most potential catalyst for soot combustion.     

Promotional effects of cerium doping and NOx on the catalytic soot combustion over MnMgAIO hydrotalcite-based mixed oxides

A series of MnMgA10 samples with different amounts of Ce doping were facilely prepared using coprecipitation method and their catalytic soot combustion activity was evaluated by temperature programmed oxidation reaction （TPO）. The methods of X-ray diffraction （XRD）, Brumauer-Emmett-Teller （BET）, H2-TPR, NO-TPO and in situ 1R were used to characterize the physio- chemical properties of these samples. Dopant Ce improved the soot combustion performance of MnMgA10 catalyst due to the en- hanced redox ability. Introduction of NOx led to the further increase of catalytic soot oxidation activity on these samples. Over Ce-containing samples, the catalytic activity was slightly decreased as the amount of dopant Ce increased in 02. Diftbrently, in NO＋O2, a certain amount of dopant Ce was much more favorable and excess amount of Ce resulted in a sharp drop of the catalytic soot combustion activity. Both NO： and nitrates were found to have great contributions to the effects of NOx on the soot combustion activity of Ce-doped catalysts. More NO2 was generated as dopant Ce increased. When appropriate amount of Ce was introduced, the as-formed NO2 was stored as bridging bidentate nitrate on Mn-Ce site, which was confirmed to have higher reactivity with soot than nitrite or monodentate nitrate on Mn and/or Ce sites. Overall, Mno.sMg2.sCeo.lAlo.90 was considered as the most potential catalyst for soot combustion.     

In-situ DRIFT assessment on strengthening effect of cerium over FeO_x/TiO_2 catalyst for selective catalytic reduction of NO_x with NH_3

Fe-based catalysts have a great potential to be used for selective catalytic reduction(SCR) of NO_x with NH3 reaction due to their low cost,nontoxicity and excellent catalytic activity.The aim of this paper is to investigate Ce doping effect on activity of NH_3-SCR over the FeO_x/TiO_2 catalyst.In-situ diffuse reflectance infrared fourier transform(DRIFT) technology was utilized to verity the adsorbed species on the surface of FeO_x/TiO_2 and FeO_x-CeO_2/TiO_2 catalysts.With respect to the obtained results,among the four catalysts studied,the FeO_x-CeO_2/TiO_2 with the FeO_x/CeO_2 ratio of 3/8 shows the best NO conversion more than 98%in the temperature range of 230—350℃,The active centers for NH_3 adsorption and activation are assigned to Lewis acid sites over the FeO_x-CeO_2/TiO_2 and monodentate nitrates can act as the key intermediate in the NH3-SCR.Moreover,both of Langmuir-Hinshelwood and Eley-Rideal mechanisms are observed over the FeO_x-CeO_2/TiO_2 catalysts in the SCR.     

Influence of preparation method on performance of a metal supported perovskite catalyst for combustion of methane

A different method was employed for the preparation of a metal supported perovskite catalyst for the catalytic combustion of methane.The prepared metallic catalysts were characterized by means of X-ray diffractometer(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),and also by ultrasonic and thermal shock tests and catalytic activity.It was found that the process factors during the preparation,e.g.the preparation of the catalyst precursor and the coating slurry,the calcination te...     

Low-temperature catalytic oxidation of NO over Mn-Ce-O_x catalyst

A series of manganese-cerium oxide catalysts were prepared by different methods and used for low-temperature catalytic oxidation of NO in the presence of excess O2.Their surface properties were evaluated by means of BET and were characterized by using scanning electron microscopy(SEM) and X-ray diffractometer(XRD).The activity test of Mn-Ce-Ox catalysts showed that addition of Ce enhanced the activities of NO oxidation.The most active catalysts with a molar Ce/(Mn+Ce) ratio of 0.3 were prepared by co-precipitation method.The results showed that NO conversion reached 60% at 150 °C with a high space velocity of 50902 h-1.The effect of doping different rare earth oxides was also investigated and the addition of small amount of Ce not only increased the surface area of MnOx but also enhanced the dispersion of Mn species in the catalyst shown by BET,SEM and XRD.     

Synthesis and characterization of aluminum and AI/REE pillared clays and supported palladium catalysts for benzene oxidation

Volatile organic compounds (VOCs) are considered as a major pollutant in indoor and outdoor air.More stringent environmental regulations have been implemented in order to reduce the VOC emissions.One of the techniques available for destructive removal of VOCs is catalytic oxidation.In the present work,Al/Rare Earths (REE: Y,Ce,La,Pr and Nd) pillared clays (PILCs) were used to support 0.2 wt.% of palladium for the complete oxidation of low concentration of benzene.The supports and catalysts were characterized by XRD,N2 adsorp-tion/desorption,FTIR spectroscopy,HRTEM and H2-TPR techniques.The results indicated that after Al and Al/REE pillaring,the basal spac-ing,SBET,Amic and Vmic of Al and AlREE-PILC had a considerable increase compared with those of Na-mmt.Activity tests of deep oxidation of benzene showed that the catalytic activity of Pd catalysts supported on Al and AlREE-PILC were much higher than that on initial clays,which was due to the fact that optimized structure of PILCs,such as large basal spacing,high SBET and porosity,improved Pd dispersion and increased the active sites of Pd.Especially for Pd/AlCe-PILC,the temperature of complete oxidation was about 280 oC,exhibiting the highest catalytic activity.     

Promotional effect of CeO2 and Y2O3 on CuO/ZrO2 catalysts for methane combustion

Catalytic combustion of methane was conducted by using a Cu-based catalyst prepared by the plasma-assisted impregnation method. The properties of the catalysts were surveyed by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and temperature-programmed reduction (H2-TPR). The results showed that the activity of CuO/ZrO2 with the CeO2 and Y2O3 was obviously increased compared with the CuO/ZrO2 catalyst, which was examined in relation to the structure and surface characteristics and might be correlated with their surface oxygen species and redox properties. Among the investigated catalysts, the Ce-CuO/ZrO2 sample exhibited the highest activity for methane combustion.     

Synthesis and characterization of aluminum and Al/REE pillared clays and supported palladium catalysts for benzene oxidation

Volatile organic compounds (VOCs) are considered as a major pollutant in indoor and outdoor air.More stringent environmental regulations have been implemented in order to reduce the VOC emissions.One of the techniques available for destructive removal of VOCs is catalytic oxidation.In the present work,Al/Rare Earths (REE: Y,Ce,La,Pr and Nd) pillared clays (PILCs) were used to support 0.2 wt.% of palladium for the complete oxidation of low concentration of benzene.The supports and catalysts were characterize...     

Preparation of ultrafine Ce-based oxide nanoparticles and their catalytic performances for diesel soot combustion

The ultrafine Ce-based oxide nanoparticles with different element dopings （Zr, Y） were synthesized by the method of mi- cropores-diffused coprecipitation （MDC） using ammonia solution as the precipitation agent. The activities of the catalysts for soot oxidation were evaluated by the temperature-programmed oxidation （TPO） reaction. Ce-based oxides prepared in this study exhibited high catalytic activity for soot oxidation under tile condition of loose contact between soot particles and catalysts, and the catalytic ac- tivity ofultrafine Ce0.gZr0 iO2 nanoparticle for soot combustion was the highest, whose/＂10, Ts0 and Sco2m was 364, 442 ~C and 98.3%, respectively. All catalysts were systematically characterized by means of X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission electron microscopy （TEM）, Brumauer-Emett-Teller （BET）, Fourier transform infrared spectroscopy （FT-IR） and UV-Vis diffuse reflectance spectroscopy （UV-Vis DRS）. It was indicated that the MDC method could prepare the ultrafine Ce-bascd oxide nanoparticles whose the crystal lattice were perfect, and the BET surface area and average crystal size of the ultrafine nanoparticles changed with the different element dopings （Zr, Y）. The H2-TPR measurements showed that the ultrafine Ce-based ox- ide nanoparticles with the doping-Zr cation could be favorable for improving the redox property of the catalysts.     

Properties of La0.9Sr0.1MnO3 and tourmaline compound catalytic materials for methane combustion

A novel catalytic material Lao.9Sr0.1MnO3 and tourmaline compound catalytic material was synthesized in the base of traditional catalytic material La0.9Sr0.1MnO3 which exhibited excellent catalytic activity for methane combustion. Different contents of toumaaline were added to give a series ofLa0.9Sr0.1MnO3 and tourmaline catalytic material through a sol-gel method. Samples above were characterized and analyzed by means of X-ray diffraction （XRD）, scanning electron microscopy （SEM）, Brunauer-Emmett-Teller method （BET）, temperaalre programmed reduction （TPR）, catalytic activity test and contact angle test. The as-prepared sample with 2% （m/m） tourmaline showed good homogeneity surface morphology and displayed the optimal catalytic activity. The light-off temperature reduced by 10 ℃ and the T90 decreased by 15 ℃. In addition, the mechanism of the reinforcement of catalytic activity was explored.     

Effect of intermediate layer on the activity and adhesion stability of metal monolith supported LaMn-hexaaluminate catalyst for methane combustion

Al2O3 and La2O3 layers were coated respectively on a FeCrAl alloy foil by a dip-coating technique and used as the second support for the active LaMnAl11O19 hexaaluminate (HA) phase in a metallic monolithic catalyst. A sample without an intermediate layer was employed for comparison. The properties and performances of the catalyst were examined with X-ray diffraction (XRD), scanning electron microscopy (SEM), ultrasonic vibration and thermal shock techniques. Methane catalytic combustion was performed to evaluate the activity of the catalyst. The results showed that the activity and adhesion of the HA to the alloy foil could be improved with the introduction of the intermediate layer. Al2O3 provided a strong adhesion, while La2O3 weakened the interaction between the active component and alloy foil. For the activity, the catalysts made with the two different intermediate materials also showed difference.     

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 ℃.     

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.     

Effect of coating modification of cordierite carrier on catalytic performance of supported NiMnO3 catalysts for VOCs combustion

NiMnO_3 perovskite catalysts supported on cordierite modified by Ce_xZr_(1-x)O_2 coatings were prepared using impregnation and sol-gel methods for catalytic combustion of single/double component VOCs at different concentrations and GHSV of 15,000 h~(-1), which were characterized by BET, XRD, SEM, FT-IR, H_2-TPR and O_2-TPD. After coating modification, the specific surface area of catalysts is improved obviously.Among the catalysts, the Ce_(0.75)Zr_(0.25)O_2 coating modified NiMnO_3 catalyst exhibits the best catalytic activity for VOCs combustion with 95.6% conversion at 275 ℃ and has stable activity when catalyst is embalmed at 800 ℃. In addition, the catalyst also presents the excellent water-resistant and conversion stability over time-on-stream condition. The reason is that Ce_(0.75)Zr_(0.25)O_2 coating can promote more lattice distortion and defects and smaller crystal size, which improve oxygen transfer capability and dispersion of active component.     

Promotional effect of CO pretreatment on CuO/CeO2 catalyst for catalytic reduction of NO by CO

The CuO/CeO2 catalysts were investigated by means of X-ray diffraction(XRD),laser Raman spectroscopy(LRS),X-ray photoelectronic spectroscopy(XPS),temperature-programmed reduction(TPR),in situ Fourier transform infrared spectroscopy(FTIR) and NO+CO reaction.The results revealed that the low temperature(150 °C) catalytic performances were enhanced for CO pretreated samples.During CO pretreatment,the surface Cu+/Cu0 and oxygen vacancies on ceria surface were present.The low valence copper species activated the adsorbed CO and surface oxygen vacancies facilitated the NO dissociation.These effects in turn led to higher activities of CuO/CeO2 for NO reduction.The current study provided helpful understandings of active sites and reaction mechanism in NO+CO reaction.     

氧化铈粒度控制研究

以碳化铈为前驱体,通过对沉淀条件的控制及填加剂的使用,控制碳酸盐的粒度,在850℃条件下灼烧后一次性得到D 50=4～7μm理想粒度的氧化铈,并可实现连续的工业化生产.