A La-modified Al2O3 catalyst was prepared with deposition-precipitation method. The effect of calcination temperature on the reactivity for vapor phase hydrofluorination of acetylene to vinyl fluoride. The catalysts c...A La-modified Al2O3 catalyst was prepared with deposition-precipitation method. The effect of calcination temperature on the reactivity for vapor phase hydrofluorination of acetylene to vinyl fluoride. The catalysts calcined at different temperatures were characterized using NH3-TPD, pyridine-FTIR, X-ray diffraction, and Raman techniques. It was found that the calcination process could not only change the structure of these catalysts but also modify the amount of surface acidity on the catalysts. The catalyst calcined at 400 ℃ exhibited the highest conversion of acetylene （94.6%） and highest selectivity to vinyl fluoride （83.4%） and lower coke deposition selectivity （0.72%）. The highest activity was related to the largest amount of surface acidity on the catalyst, and the coke deposition was also related to the total amount of surface acidic sites.展开更多
The catalytic performances of Co3O4/SiO2 catalysts prepared by incipient wetness impregnation for CO oxidation were investigated using three kinds of silica as carriers with different pore sizes of 7.7,14.0 and 27.0 n...The catalytic performances of Co3O4/SiO2 catalysts prepared by incipient wetness impregnation for CO oxidation were investigated using three kinds of silica as carriers with different pore sizes of 7.7,14.0 and 27.0 nm.The effects of calcination temperature on the catalyst surface and micro structure properties as well as catalytic performance for the oxidation of carbon monoxide were also studied.All catalysts were characterized by N2 adsorption-desorption,XRD,XPS,FTIR,H2-TPR and O2-TPD.It was found that the properties and crystal size of cobalt-containing species strongly depended on the pore size of silica carrier.While the silica pore size increased from 7.7 to 27.0 nm,the Co3O4 crystal size increased from 8.5 to 13.5 nm.Moreover,it was demonstrated that if the spinel crystal structure of Co3O4 was obtained at a calcination temperature as low as 150℃,the catalyst sample would have a high Co3O4 surface dispersion and an increase of surface active species,and thus exhibit a high activity for the oxidation of carbon monoxide.展开更多
The acidic modulations of a series of HZSM-5 catalysts were successfully made by calcination at different treatment temperatures, i.e. 500, 600, 650, 700 and 800 ℃, respectively. The results indicated that the total ...The acidic modulations of a series of HZSM-5 catalysts were successfully made by calcination at different treatment temperatures, i.e. 500, 600, 650, 700 and 800 ℃, respectively. The results indicated that the total acid amounts, their density and the amount of B-type acid of HZSM-5 catalysts rapidly decreased, while the amounts of L-type acid had almost no change and thus the ratio of L/B was obviously enhanced with the increase of calcination temperature （excluding 800 ℃）. The catalytic performances of modified HZSM-5 catalysts for the cracking of n-butane were also investigated. The main properties of these catalysts were characterized by means of XRD, N2 adsorption at low temperature, NH3-TPD, FTIR of pyridine adsorption and BET surface area measurements. The results showed that HZSM-5 zeolite pretreated at 800 ℃ had very low catalytic activity for n-butane cracking. In the calcination temperature range of 500-700 ℃, the total selectivity to olefins, propylene and butene were increased with the increase of calcination temperature, while, the selectivity for arene decreased with the calcination temperature. The HZSM-5 zeolite calcined at 700 ℃ produced light olefins with high yield, at the reaction temperature of 650 ℃ the yields of total olefins and ethylene were 52.8% and 29.4%, respectively. Besides, the more important role is that high calcination temperature treatment improved the duration stability of HZSM-5 zeolites. The effect of calcination temperature on the physico-chemical properties and catalytic performance of HZSM-5 for cracking of n-butane was explored. It was found that the calcination temperature had large effects on the surface area, crystallinity and acid properties of HZSM-5 catalyst, which further affected the catalytic performance for n-butane cracking.展开更多
CuSO4/TiO2 catalysts with high catalytic activity and excellent resistant to SO2 and H2 O,were thought to be promising catalysts used in Selective catalytic reduction of nitrogen oxides by NH3.The performance of catal...CuSO4/TiO2 catalysts with high catalytic activity and excellent resistant to SO2 and H2 O,were thought to be promising catalysts used in Selective catalytic reduction of nitrogen oxides by NH3.The performance of catalysts is largely affected by calcination temperature.Here,effects of calcination temperature on physicochemical property and catalytic activity of CuSO4/TiO2 catalysts were investigated in depth.Catalyst samples calcined at different temperatures were prepared first and then physicochemical properties of the catalyst were characterized by N2 adsorption-desorption,X-ray diffraction,thermogravimetric analysis,Raman spectra,Fourier-transform infrared spectroscopy,X-ray photoelectron spectroscopy,temperature-pro grammed desorption of NH3,temperature-programmed reduction of H2 and in situ diffuse reflectance infrared Fourier transform spectroscopy.Results revealed that high calcination temperature had three main effects on the catalyst.First,sintering and anatase transform into rutile with increase of calcination temperature,causing a decrement of specific surface area.Second,decomposition of CuSO4 under higher calcination temperature,resulting in disappears of Br(?)nsted acid sites(S-OH),which had an adverse effect on surface acidity.Third,CuO from the decomposition of CuSO4 changed surface reducibility of the catalyst and favored the process of NH3 oxidation to nitrogen oxides(NOx).Thus,catalytic activity of the catalyst calcined under high temperatures(≥600℃)decreased largely.展开更多
TiOz nanotubes （TiO2-NTs） were synthesized by the hydrothermal method. Co and Mo active components were supported on a series of the as-prepared TiO2-NTs samples which were calcined at different temperatures. The ef...TiOz nanotubes （TiO2-NTs） were synthesized by the hydrothermal method. Co and Mo active components were supported on a series of the as-prepared TiO2-NTs samples which were calcined at different temperatures. The effects of support calcination temperature of CoMo/TiOz- NTs catalysts on their catalytic performance were investigated for selective hydrodesulfurization （HDS）. The samples were characterized by means of the scanning electron microscopy （SEM）, the transmission electron microscopy （TEM）, N2 adsorption-desorption, X-ray diffraction （XRD）, Raman spectroscopy and H2 temperature-programmed reduction （Hz-TPR）. The experimental results revealed that TiOz-NTs support calcined under 500℃ can maintain the nanotubular structure with higher surface area and pore volume. Meanwhile, the obtained supported CoMo/TiO2-NTs catalysts exhibited weak metal-support interaction, more octahedral Mo6＋ species and high catalytic performance in selective HDS.展开更多
In this research,a solid 1%Li/Ca-La mixed oxide catalyst was prepared using co-precipitation method followed by wet impregnation.The prepared catalyst was used in the transesterification reaction of canola oil and met...In this research,a solid 1%Li/Ca-La mixed oxide catalyst was prepared using co-precipitation method followed by wet impregnation.The prepared catalyst was used in the transesterification reaction of canola oil and methanol for biodiesel synthesis.The effects of calcination and reaction temperatures were investigated on the activity of the catalyst.In addition,rate of the reaction was studied through a kinetic model for which parameters were determined.Surface properties and structure of the catalyst were characterized through the powder X-ray diffraction(XRD),thermogravimetry/derivative thermogravimetry(TG/DTG),and Fourier transform infrared spectroscopy analysis.All these emphasized that the performance of the catalyst corresponded to the generation of the active sites and their thermal activation.展开更多
The effects of calcination temperature on the physicochemical properties of manganese oxide catalysts prepared by a precipitation method were assessed by X-ray diffraction,N2 adsorption-desorption,X-ray photoelectron ...The effects of calcination temperature on the physicochemical properties of manganese oxide catalysts prepared by a precipitation method were assessed by X-ray diffraction,N2 adsorption-desorption,X-ray photoelectron spectroscopy,H2 temperature-programmed reduction,O2 temperature-programmed desorption,and thermogravimetry-differential analysis.The catalytic performance of each of these materials during the selective oxidation of cyclohexane with oxygen in a solvent-free system was subsequently examined.It was found that the MnOx-500 catalyst,calcined at 500 °C,consisted of a Mn2O3 phase in addition to Mn5O8 and Mn3O4 phases and possessed a low surface area.Unlike MnOx-500,the MnOx-400 catalyst prepared at 400 °C was composed solely of Mn3O4 and Mn5O8 and had a higher surface area.The pronounced catalytic activity of this latter material for the oxidation of cyclohexene was determined to result from numerous factors,including a higher concentration of surface adsorbed oxygen,greater quantities of the surface Mn4＋ ions that promote oxygen mobility and the extent of O2 adsorption and reducibility on the catalyst.The effects of various reaction conditions on the activity of the MnOx-400 during the oxidation of cyclohexane were also evaluated,such as the reaction temperature,reaction time,and initial oxygen pressure.Following a 4 h reaction at an initial O2 pressure of 0.5 MPa and 140 °C,an 8.0% cyclohexane conversion and 5.0% yield of cyclohexanol and cyclohexanone were achieved over the MnOx-400 catalyst.In contrast,employing MnOx-500 resulted in a 6.1% conversion of cyclohexane and 75% selectivity for cyclohexanol and cyclohexanone.After being recycled through 10 replicate uses,the catalytic activity of the MnOx-400 catalyst was unchanged,demonstrating its good stability.展开更多
Co3O4/SiO2 catalysts for CO oxidation were prepared by conventional incipient wetness impregnation followed by calcination at various temperatures. Their structures were char- acterized with X-ray diffraction （XRD）,...Co3O4/SiO2 catalysts for CO oxidation were prepared by conventional incipient wetness impregnation followed by calcination at various temperatures. Their structures were char- acterized with X-ray diffraction （XRD）, laser Raman spectroscopy, X-ray photoelectron spectroscopy （XPS）, temperature-programmed reduction （TPR） and X-ray absorption fine structure （XAFS） spectroscopy. Both XRD and Raman spectroscopy only detect the existence of Co3O4 crystallites in all catalysts. However, XPS results indicate that excess Co2＋ ions are present on the surface of Co3O4 in Co3O4（200）/Si02 as compared with bulk Co3O4. Meanwhile, TPR results suggest the presence of surface oxygen vacancies on Co3O4 in Co3O4（200）/SiO2, and XAFS results demonstrate that Co3O4 in Co3O4（200）/SIO2 contains excess Co2＋. Increasing calcination temperature results in oxidation of excess Co2＋ and the decrease of the concentration of surface oxygen vacancies, consequently the for- mation of stoichiometric Co3O4 on supported catalysts. Among all Co3O4/SiO2 catalysts, Co3O4（200）/SiO2 exhibits the best catalytic performance towards CO oxidation, demonstrating that excess Co2＋ and surface oxygen vacancies can enhance the catalytic activity of Co3O4 towards CO oxidation. These results nicely demonstrate the effect of calcination temperature on the structure and catalytic performance towards CO oxidation of silicasupported Co3O4 catalysts and highlight the important role of surface oxygen vacancies on Co3O4.展开更多
The oxidative coupling of methane(OCM)involves directly converting methane to C_(2+)hydrocarbons(such as ethylene and ethane)via a reaction with oxygen.This study elucidated the effect of the calcination temperature o...The oxidative coupling of methane(OCM)involves directly converting methane to C_(2+)hydrocarbons(such as ethylene and ethane)via a reaction with oxygen.This study elucidated the effect of the calcination temperature on the structure and catalytic performance of potassium-doped-cobalt oxide supported on an alumina(K-Co/Al2O3)catalyst for the OCM reaction.The catalyst was highly active at relatively low reactor temperatures(500-640℃).Four calcination temperatures(400,500,600,and 700℃)were investigated,with the results showing that the calcination temperature strongly affected catalytic properties,such as the crystalline phases,elemental distribution,physical properties,and catalytic basicity,leading to a wide range in catalytic performances.The catalyst calcined at 400℃ was superior among the catalysts,with 8.3%C_(2+)yield,24.8%C_(2+)selectivity,and 33.6%CH4 conversion at 640℃.Furthermore,the catalyst was robust over 24 h of testing.展开更多
The MnCeO_(x)catalysts were synthesized via the co-precipitation method,with calcination temperatures ranging from 300 to 850℃.The results demonstrate that MnCeO_(x)-350℃catalyst exhibits the optimal NO_(x)conversio...The MnCeO_(x)catalysts were synthesized via the co-precipitation method,with calcination temperatures ranging from 300 to 850℃.The results demonstrate that MnCeO_(x)-350℃catalyst exhibits the optimal NO_(x)conversion rate within the reaction temperature range of 175–325℃.To understand the reasons for the influence of calcination temperature on the performance of catalysts,four representative catalysts were chosen for detailed analysis:MnCeO_(x)-300℃,MnCeO_(x)-350℃,MnCeO_(x)-650℃,and MnCeO_(x)-750℃.The catalysts were characterized through various techniques including nitrogen physisorption analysis,X-ray diffraction,Raman spectroscopy,hydrogen temperature programmed reduction,ammonia temperature programmed desorption,X-ray photoelectron spectroscopy,and in situ diff use reflectance infrared Fourier transform spectroscopy experiments.In addition,we assessed the water and SO_(2)resistance of these catalysts.The results demonstrate that the reason why MnCeO_(x)-350℃has good performance is not only because of its lower crystallinity and higher specific surface area but also because the catalyst can provide more Br?nsted acid sites,higher content of Ce^(3+),Mn^(4+),and surface adsorbed oxygen.The synergistic effect between Mn^(4+)and Ce^(3+)is enhanced while the surface acidity is increased,which is conducive to the improvement of the denitrification performance of the catalyst at low temperatures.展开更多
Iron-based perovskite-type compounds modified by Ru were prepared through sol-gel process to study its catalytic activity of NOx direct decomposition at low temperature and evaluate the conversion of NO under the expe...Iron-based perovskite-type compounds modified by Ru were prepared through sol-gel process to study its catalytic activity of NOx direct decomposition at low temperature and evaluate the conversion of NO under the experimental conditions. The catalytic activity of La 0.9Ce 0.1Fe 0.8-nCo 0.2RunO3 （n=0.01,0.03,0.05,0.07,0.09）series for the NO, NO-CO two components, CO-HC-NO three components were also analyzed. The catalytic investigation evidenced that the presence of Ru is necessary for making highly activity in decomposition of nitric oxide even at low temperature（400 ℃）and La 0.9Ce 0.9Fe 0.75Co 0.2Ru 0.05O3 （n=0.05） has better activity in all the samples, the conversion of it is 58.5%. With the reducing gas（CO,C3H6）added into the gas, the catalyst displayed very high activity in decomposition of NO and the conversion of it is 80% and 92.5% separately.展开更多
Iron-based catalysts have been explored for selective catalytic reduction(SCR)of NO due to environmentally benign characters and good SCR activity.Mn-W-Sb modified siderite catalysts were prepared by impregnation meth...Iron-based catalysts have been explored for selective catalytic reduction(SCR)of NO due to environmentally benign characters and good SCR activity.Mn-W-Sb modified siderite catalysts were prepared by impregnation method based on siderite ore,and SCR perfor-mance of the catalysts was investigated.The catalysts were analyzed by X-ray diffrac-tion,H_(2)-temperature-programmed reduction,Brunauer-Emmett-Teller,Thermogravimetry-derivative thermogravimetry and in-situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS).The modified siderite catalysts calcined at 450℃ mainly consist of Fe_(2)O_(3),and added Mn,W and Sb species are amorphous.3Mn-5W-1.5Sb-siderite catalyst has a wide temperature window of 180-360℃ and good N_(2) selectivity at low temperatures.In-situ DRIFTS results show NH_(4)^(+),coordinated NH_(3),NH_(2),NO_(3)^(-)species(bidentate),NO_(2)-species(nitro,nitro-nitrito,monodentate),and adsorbed NO_(2) can be discovered on the sur-face of Mn-W-Sb modified siderite catalysts,and doping of Mn will enhance adsorbed NO_(2) formation by synergistic catalysis with Fe^(3+).In addition,the addition of Sb can inhibit sulfates formation on the surface of the catalyst in the presence of SO_(2) and H_(2)O.Time-dependent in-situ DRIFTS studies also indicate that both of Lewis and Br?nsted acid sites play a role in SCR of NO by ammonia at low temperatures.The mechanism of NO removal on the 3Mn-5W-1.5Sb-siderite catalyst can be discovered as a combination of Eley-Rideal and Langmuir-Hinshelwood mechanisms with three reaction pathways.The mechanism of NO,oxidized by synergistic catalysis of Fe^(3+)and Mn^(4+/3+)to form NO_(2) among three pathways,reveals the reason of high NO_(x) conversion of the catalyst at medium and low temperatures.展开更多
A series of 3DOM CeMnO3 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...A series of 3DOM CeMnO3 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,H2-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 CeMnO3 catalysts calcined at 600℃promote the formation of a perovskite structure,inhibit the reduction of the Mn4+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 Mn4+substance concentration,with a low T90%=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.展开更多
Revealing the active species of the catalyst is conducive to the design of more efficient catalyst.Herein,we tried to demonstrate the roles of amorphous and crystalline structures on CePO_(4)catalyst during selective ...Revealing the active species of the catalyst is conducive to the design of more efficient catalyst.Herein,we tried to demonstrate the roles of amorphous and crystalline structures on CePO_(4)catalyst during selective catalytic reduction(SCR)of NO_(x)by NH_(3).Higher calcination temperature promotes the transfer of amorphous structure to crystalline structure on the surface of CePO_(4).Both amorphous and crystalline CePO_(4)species on CePO-X samples can provide acid sites for NH_(3)adsorption,but the former can provide more acid sites.The superior redox property of surface amorphous CePO_(4)species contributes to its high NH_(3)-SCR activity at low temperature,but it also leads to the decrease of high temperature(>350℃)NH_(3)-SCR activity due to the oxidation of NH_(3).In contrast,crystalline CePO_(4)species shows high activity only at high temperature because of its poor redox property.Therefo re,it can be inferred that amo rphous and crystalline structures on CePO_(4)catalyst can be the efficient active species of NH_(3)-SCR at low and high temperature,respectively.展开更多
A novel powder catalyst Cu-Cr-O applied to the synthesis of carbon nanotubes （CNTs） was developed, which was prepared via ammonia precipitation method. Techniques of thermo-gravimetric/ differential scanning calorim...A novel powder catalyst Cu-Cr-O applied to the synthesis of carbon nanotubes （CNTs） was developed, which was prepared via ammonia precipitation method. Techniques of thermo-gravimetric/ differential scanning calorimeter （TG-DSC）, X-ray diffraction （XRD） as well as scanning electron microscopy （SEM） and transmission electron microscopy （TEM） have been employed to characterize the thermal decomposition procedure, crystal phase and micro structural morphologies of the as-synthesized materials, respectively. The results show that carbon nanotubes are successfully synthesized using Cu-Cr-O as catalyst when the precursors are calcined at 400, 500, 600, and 700 ℃. The results indicate that the calcination of the Cu-Cr-O catalyst at 600 ℃ is an effective method to get MWCNT with few nano-tube defects or amorphous carbons.展开更多
Several ternary oxides CuCeZrO_(y)(CCZ)were synthesized by a facile grinding method followed by calcination at high temperatures,and used as catalysts for CO oxidation at low temperatures.The influences of calcination...Several ternary oxides CuCeZrO_(y)(CCZ)were synthesized by a facile grinding method followed by calcination at high temperatures,and used as catalysts for CO oxidation at low temperatures.The influences of calcination temperature(400-600℃)on the physicochemical properties of the assynthesized ternary oxides were investigated by thermogravimetric analysis/differential scanning calorimetry(TGA/DSC),X-ray diffraction(XRD),transmission electron microscopy(TEM),Raman,inductively coupled plasma-optical emission spectrometry(ICP-OES),N_(2) adsorption,H_(2)-temperature programmed reduction(H_(2)-TPR),and X-ray photoelectron spectroscopy(XPS)characterizations.The results show that the increase in calcination temperature from 400 to 500℃is conducive to the high dispersion of CuOx on catalyst surface and the incorporation of Cu species into the support to form the Cu-Ce-Zr-O solid solution.Further raising of calcination temperature from 500 to 600℃,however,leads to the segregation of Cu species from the solid solution to aggregate on support surface and growth of highly dispersed CuOx nanoparticles.The highest catalytic activity is acquired over the CCZ calcined at 500℃,which can be ascribed to the largest contents of Cu+species and oxygen vacancies owing to the formation of the maximum amount of Cu-Ce-Zr-O solid solution.展开更多
基金ACKNOWLEDGMENT This work was supported by the National Natural Science Foundation of China （No.20873125）,
文摘A La-modified Al2O3 catalyst was prepared with deposition-precipitation method. The effect of calcination temperature on the reactivity for vapor phase hydrofluorination of acetylene to vinyl fluoride. The catalysts calcined at different temperatures were characterized using NH3-TPD, pyridine-FTIR, X-ray diffraction, and Raman techniques. It was found that the calcination process could not only change the structure of these catalysts but also modify the amount of surface acidity on the catalysts. The catalyst calcined at 400 ℃ exhibited the highest conversion of acetylene （94.6%） and highest selectivity to vinyl fluoride （83.4%） and lower coke deposition selectivity （0.72%）. The highest activity was related to the largest amount of surface acidity on the catalyst, and the coke deposition was also related to the total amount of surface acidic sites.
基金supported by the National Natural Science Foundation of China(NSFC 20776089)the 985 Project of Sichuan University
文摘The catalytic performances of Co3O4/SiO2 catalysts prepared by incipient wetness impregnation for CO oxidation were investigated using three kinds of silica as carriers with different pore sizes of 7.7,14.0 and 27.0 nm.The effects of calcination temperature on the catalyst surface and micro structure properties as well as catalytic performance for the oxidation of carbon monoxide were also studied.All catalysts were characterized by N2 adsorption-desorption,XRD,XPS,FTIR,H2-TPR and O2-TPD.It was found that the properties and crystal size of cobalt-containing species strongly depended on the pore size of silica carrier.While the silica pore size increased from 7.7 to 27.0 nm,the Co3O4 crystal size increased from 8.5 to 13.5 nm.Moreover,it was demonstrated that if the spinel crystal structure of Co3O4 was obtained at a calcination temperature as low as 150℃,the catalyst sample would have a high Co3O4 surface dispersion and an increase of surface active species,and thus exhibit a high activity for the oxidation of carbon monoxide.
基金The authors would like to thank the financial support from the National Basic Research Program of China fgrant No．2004CB 217806)the National Natural Science Foundation of China (Grant No．20373043) the Scientific Research Key Foundation for the Returned Overseas Chinese Scholars of State Education Ministry．
文摘The acidic modulations of a series of HZSM-5 catalysts were successfully made by calcination at different treatment temperatures, i.e. 500, 600, 650, 700 and 800 ℃, respectively. The results indicated that the total acid amounts, their density and the amount of B-type acid of HZSM-5 catalysts rapidly decreased, while the amounts of L-type acid had almost no change and thus the ratio of L/B was obviously enhanced with the increase of calcination temperature （excluding 800 ℃）. The catalytic performances of modified HZSM-5 catalysts for the cracking of n-butane were also investigated. The main properties of these catalysts were characterized by means of XRD, N2 adsorption at low temperature, NH3-TPD, FTIR of pyridine adsorption and BET surface area measurements. The results showed that HZSM-5 zeolite pretreated at 800 ℃ had very low catalytic activity for n-butane cracking. In the calcination temperature range of 500-700 ℃, the total selectivity to olefins, propylene and butene were increased with the increase of calcination temperature, while, the selectivity for arene decreased with the calcination temperature. The HZSM-5 zeolite calcined at 700 ℃ produced light olefins with high yield, at the reaction temperature of 650 ℃ the yields of total olefins and ethylene were 52.8% and 29.4%, respectively. Besides, the more important role is that high calcination temperature treatment improved the duration stability of HZSM-5 zeolites. The effect of calcination temperature on the physico-chemical properties and catalytic performance of HZSM-5 for cracking of n-butane was explored. It was found that the calcination temperature had large effects on the surface area, crystallinity and acid properties of HZSM-5 catalyst, which further affected the catalytic performance for n-butane cracking.
基金supported by the National Natural Science Foundation of China(Nos.21906127,21677114,21876139 and 21922606)the Key R&D Program of Shaanxi Province(Nos.2019SF-244 and 2019ZDLSF05-05-02)+4 种基金the China PostdoctoralScience Foundation(No.2016M602831)Natural Science Foundation of Shaanxi Province,China(No.2019JQ-502)the Fundamental Research Funds for the Central Universities(Nos.xjj2017113 and xjj2017170)financial supports from the China Scholarship Councilthe support of K.C.Wong Education Foundation
文摘CuSO4/TiO2 catalysts with high catalytic activity and excellent resistant to SO2 and H2 O,were thought to be promising catalysts used in Selective catalytic reduction of nitrogen oxides by NH3.The performance of catalysts is largely affected by calcination temperature.Here,effects of calcination temperature on physicochemical property and catalytic activity of CuSO4/TiO2 catalysts were investigated in depth.Catalyst samples calcined at different temperatures were prepared first and then physicochemical properties of the catalyst were characterized by N2 adsorption-desorption,X-ray diffraction,thermogravimetric analysis,Raman spectra,Fourier-transform infrared spectroscopy,X-ray photoelectron spectroscopy,temperature-pro grammed desorption of NH3,temperature-programmed reduction of H2 and in situ diffuse reflectance infrared Fourier transform spectroscopy.Results revealed that high calcination temperature had three main effects on the catalyst.First,sintering and anatase transform into rutile with increase of calcination temperature,causing a decrement of specific surface area.Second,decomposition of CuSO4 under higher calcination temperature,resulting in disappears of Br(?)nsted acid sites(S-OH),which had an adverse effect on surface acidity.Third,CuO from the decomposition of CuSO4 changed surface reducibility of the catalyst and favored the process of NH3 oxidation to nitrogen oxides(NOx).Thus,catalytic activity of the catalyst calcined under high temperatures(≥600℃)decreased largely.
文摘TiOz nanotubes （TiO2-NTs） were synthesized by the hydrothermal method. Co and Mo active components were supported on a series of the as-prepared TiO2-NTs samples which were calcined at different temperatures. The effects of support calcination temperature of CoMo/TiOz- NTs catalysts on their catalytic performance were investigated for selective hydrodesulfurization （HDS）. The samples were characterized by means of the scanning electron microscopy （SEM）, the transmission electron microscopy （TEM）, N2 adsorption-desorption, X-ray diffraction （XRD）, Raman spectroscopy and H2 temperature-programmed reduction （Hz-TPR）. The experimental results revealed that TiOz-NTs support calcined under 500℃ can maintain the nanotubular structure with higher surface area and pore volume. Meanwhile, the obtained supported CoMo/TiO2-NTs catalysts exhibited weak metal-support interaction, more octahedral Mo6＋ species and high catalytic performance in selective HDS.
基金supported by the Iran National Science Foundation(INSF)
文摘In this research,a solid 1%Li/Ca-La mixed oxide catalyst was prepared using co-precipitation method followed by wet impregnation.The prepared catalyst was used in the transesterification reaction of canola oil and methanol for biodiesel synthesis.The effects of calcination and reaction temperatures were investigated on the activity of the catalyst.In addition,rate of the reaction was studied through a kinetic model for which parameters were determined.Surface properties and structure of the catalyst were characterized through the powder X-ray diffraction(XRD),thermogravimetry/derivative thermogravimetry(TG/DTG),and Fourier transform infrared spectroscopy analysis.All these emphasized that the performance of the catalyst corresponded to the generation of the active sites and their thermal activation.
基金supported by the National Basic Research Program of China(973 Program,2010CB732300)the National Natural Science Foundation of China(21103048)~~
文摘The effects of calcination temperature on the physicochemical properties of manganese oxide catalysts prepared by a precipitation method were assessed by X-ray diffraction,N2 adsorption-desorption,X-ray photoelectron spectroscopy,H2 temperature-programmed reduction,O2 temperature-programmed desorption,and thermogravimetry-differential analysis.The catalytic performance of each of these materials during the selective oxidation of cyclohexane with oxygen in a solvent-free system was subsequently examined.It was found that the MnOx-500 catalyst,calcined at 500 °C,consisted of a Mn2O3 phase in addition to Mn5O8 and Mn3O4 phases and possessed a low surface area.Unlike MnOx-500,the MnOx-400 catalyst prepared at 400 °C was composed solely of Mn3O4 and Mn5O8 and had a higher surface area.The pronounced catalytic activity of this latter material for the oxidation of cyclohexene was determined to result from numerous factors,including a higher concentration of surface adsorbed oxygen,greater quantities of the surface Mn4＋ ions that promote oxygen mobility and the extent of O2 adsorption and reducibility on the catalyst.The effects of various reaction conditions on the activity of the MnOx-400 during the oxidation of cyclohexane were also evaluated,such as the reaction temperature,reaction time,and initial oxygen pressure.Following a 4 h reaction at an initial O2 pressure of 0.5 MPa and 140 °C,an 8.0% cyclohexane conversion and 5.0% yield of cyclohexanol and cyclohexanone were achieved over the MnOx-400 catalyst.In contrast,employing MnOx-500 resulted in a 6.1% conversion of cyclohexane and 75% selectivity for cyclohexanol and cyclohexanone.After being recycled through 10 replicate uses,the catalytic activity of the MnOx-400 catalyst was unchanged,demonstrating its good stability.
文摘Co3O4/SiO2 catalysts for CO oxidation were prepared by conventional incipient wetness impregnation followed by calcination at various temperatures. Their structures were char- acterized with X-ray diffraction （XRD）, laser Raman spectroscopy, X-ray photoelectron spectroscopy （XPS）, temperature-programmed reduction （TPR） and X-ray absorption fine structure （XAFS） spectroscopy. Both XRD and Raman spectroscopy only detect the existence of Co3O4 crystallites in all catalysts. However, XPS results indicate that excess Co2＋ ions are present on the surface of Co3O4 in Co3O4（200）/Si02 as compared with bulk Co3O4. Meanwhile, TPR results suggest the presence of surface oxygen vacancies on Co3O4 in Co3O4（200）/SiO2, and XAFS results demonstrate that Co3O4 in Co3O4（200）/SIO2 contains excess Co2＋. Increasing calcination temperature results in oxidation of excess Co2＋ and the decrease of the concentration of surface oxygen vacancies, consequently the for- mation of stoichiometric Co3O4 on supported catalysts. Among all Co3O4/SiO2 catalysts, Co3O4（200）/SiO2 exhibits the best catalytic performance towards CO oxidation, demonstrating that excess Co2＋ and surface oxygen vacancies can enhance the catalytic activity of Co3O4 towards CO oxidation. These results nicely demonstrate the effect of calcination temperature on the structure and catalytic performance towards CO oxidation of silicasupported Co3O4 catalysts and highlight the important role of surface oxygen vacancies on Co3O4.
基金supported by:the National Research Council of Thailand through the Fundamental Fund under the Kasetsart University Research and Development Institute(KURDI),Bangkok,Thailand,through Grant No.FF(KU)38.67the Center of Excellence on Petrochemical and Materials Technology+2 种基金and the National Research Council of Thailand through the Research Team Promotion Grant/Senior Research Scholar(Grant No.N42A640324)support by the Austrian Science Fund(FWFSFB TACO F81-P08).
文摘The oxidative coupling of methane(OCM)involves directly converting methane to C_(2+)hydrocarbons(such as ethylene and ethane)via a reaction with oxygen.This study elucidated the effect of the calcination temperature on the structure and catalytic performance of potassium-doped-cobalt oxide supported on an alumina(K-Co/Al2O3)catalyst for the OCM reaction.The catalyst was highly active at relatively low reactor temperatures(500-640℃).Four calcination temperatures(400,500,600,and 700℃)were investigated,with the results showing that the calcination temperature strongly affected catalytic properties,such as the crystalline phases,elemental distribution,physical properties,and catalytic basicity,leading to a wide range in catalytic performances.The catalyst calcined at 400℃ was superior among the catalysts,with 8.3%C_(2+)yield,24.8%C_(2+)selectivity,and 33.6%CH4 conversion at 640℃.Furthermore,the catalyst was robust over 24 h of testing.
基金The financial supports of the National Natural Science Foundation of China(22076180)the Key Project of Science and Technology Talent and Independent Innovation of Beibei District Science and Technology Bureau,Chongqing(2024-18)Chongqing Bayu Scholar program(Young Scholar,YS2020048)are gratefully acknowledged。
文摘The MnCeO_(x)catalysts were synthesized via the co-precipitation method,with calcination temperatures ranging from 300 to 850℃.The results demonstrate that MnCeO_(x)-350℃catalyst exhibits the optimal NO_(x)conversion rate within the reaction temperature range of 175–325℃.To understand the reasons for the influence of calcination temperature on the performance of catalysts,four representative catalysts were chosen for detailed analysis:MnCeO_(x)-300℃,MnCeO_(x)-350℃,MnCeO_(x)-650℃,and MnCeO_(x)-750℃.The catalysts were characterized through various techniques including nitrogen physisorption analysis,X-ray diffraction,Raman spectroscopy,hydrogen temperature programmed reduction,ammonia temperature programmed desorption,X-ray photoelectron spectroscopy,and in situ diff use reflectance infrared Fourier transform spectroscopy experiments.In addition,we assessed the water and SO_(2)resistance of these catalysts.The results demonstrate that the reason why MnCeO_(x)-350℃has good performance is not only because of its lower crystallinity and higher specific surface area but also because the catalyst can provide more Br?nsted acid sites,higher content of Ce^(3+),Mn^(4+),and surface adsorbed oxygen.The synergistic effect between Mn^(4+)and Ce^(3+)is enhanced while the surface acidity is increased,which is conducive to the improvement of the denitrification performance of the catalyst at low temperatures.
基金Sponsored by the National Natural Science Foundation of China(Grant No.20271019 and 20576027), Natural Science Foundation of Heilongjiang Prov-ince(Grant No.B200504), Postdoctoral Foundationof Heilongjiang Province(Grant No.LBH-Z05066) and Education Department Foundation of Hei-longjiang Province(Grant No.11511270).
文摘Iron-based perovskite-type compounds modified by Ru were prepared through sol-gel process to study its catalytic activity of NOx direct decomposition at low temperature and evaluate the conversion of NO under the experimental conditions. The catalytic activity of La 0.9Ce 0.1Fe 0.8-nCo 0.2RunO3 （n=0.01,0.03,0.05,0.07,0.09）series for the NO, NO-CO two components, CO-HC-NO three components were also analyzed. The catalytic investigation evidenced that the presence of Ru is necessary for making highly activity in decomposition of nitric oxide even at low temperature（400 ℃）and La 0.9Ce 0.9Fe 0.75Co 0.2Ru 0.05O3 （n=0.05） has better activity in all the samples, the conversion of it is 58.5%. With the reducing gas（CO,C3H6）added into the gas, the catalyst displayed very high activity in decomposition of NO and the conversion of it is 80% and 92.5% separately.
基金This work was supported by the National Natural Science Foundation of China(Nos.51406077 and 51276039).
文摘Iron-based catalysts have been explored for selective catalytic reduction(SCR)of NO due to environmentally benign characters and good SCR activity.Mn-W-Sb modified siderite catalysts were prepared by impregnation method based on siderite ore,and SCR perfor-mance of the catalysts was investigated.The catalysts were analyzed by X-ray diffrac-tion,H_(2)-temperature-programmed reduction,Brunauer-Emmett-Teller,Thermogravimetry-derivative thermogravimetry and in-situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS).The modified siderite catalysts calcined at 450℃ mainly consist of Fe_(2)O_(3),and added Mn,W and Sb species are amorphous.3Mn-5W-1.5Sb-siderite catalyst has a wide temperature window of 180-360℃ and good N_(2) selectivity at low temperatures.In-situ DRIFTS results show NH_(4)^(+),coordinated NH_(3),NH_(2),NO_(3)^(-)species(bidentate),NO_(2)-species(nitro,nitro-nitrito,monodentate),and adsorbed NO_(2) can be discovered on the sur-face of Mn-W-Sb modified siderite catalysts,and doping of Mn will enhance adsorbed NO_(2) formation by synergistic catalysis with Fe^(3+).In addition,the addition of Sb can inhibit sulfates formation on the surface of the catalyst in the presence of SO_(2) and H_(2)O.Time-dependent in-situ DRIFTS studies also indicate that both of Lewis and Br?nsted acid sites play a role in SCR of NO by ammonia at low temperatures.The mechanism of NO removal on the 3Mn-5W-1.5Sb-siderite catalyst can be discovered as a combination of Eley-Rideal and Langmuir-Hinshelwood mechanisms with three reaction pathways.The mechanism of NO,oxidized by synergistic catalysis of Fe^(3+)and Mn^(4+/3+)to form NO_(2) among three pathways,reveals the reason of high NO_(x) conversion of the catalyst at medium and low temperatures.
基金Project supported by Natural Science Foundation of Shandong Province(ZR2019MEE112)。
文摘A series of 3DOM CeMnO3 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,H2-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 CeMnO3 catalysts calcined at 600℃promote the formation of a perovskite structure,inhibit the reduction of the Mn4+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 Mn4+substance concentration,with a low T90%=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.
基金Project supported by the Fundamental Research Funds for the Central Universities(30919011220)the Key Project of Jiangsu Province Programs for Research and Development(BE2019115)Top-notch Academic Programs Project of Jiangsu Higher Education Institutions。
文摘Revealing the active species of the catalyst is conducive to the design of more efficient catalyst.Herein,we tried to demonstrate the roles of amorphous and crystalline structures on CePO_(4)catalyst during selective catalytic reduction(SCR)of NO_(x)by NH_(3).Higher calcination temperature promotes the transfer of amorphous structure to crystalline structure on the surface of CePO_(4).Both amorphous and crystalline CePO_(4)species on CePO-X samples can provide acid sites for NH_(3)adsorption,but the former can provide more acid sites.The superior redox property of surface amorphous CePO_(4)species contributes to its high NH_(3)-SCR activity at low temperature,but it also leads to the decrease of high temperature(>350℃)NH_(3)-SCR activity due to the oxidation of NH_(3).In contrast,crystalline CePO_(4)species shows high activity only at high temperature because of its poor redox property.Therefo re,it can be inferred that amo rphous and crystalline structures on CePO_(4)catalyst can be the efficient active species of NH_(3)-SCR at low and high temperature,respectively.
基金Supported by National Natural Science Foundation of China(No.51201107)Key Basic Research Project of Shanghai Committee of Science and Technology in China(10JC1411800)
文摘A novel powder catalyst Cu-Cr-O applied to the synthesis of carbon nanotubes （CNTs） was developed, which was prepared via ammonia precipitation method. Techniques of thermo-gravimetric/ differential scanning calorimeter （TG-DSC）, X-ray diffraction （XRD） as well as scanning electron microscopy （SEM） and transmission electron microscopy （TEM） have been employed to characterize the thermal decomposition procedure, crystal phase and micro structural morphologies of the as-synthesized materials, respectively. The results show that carbon nanotubes are successfully synthesized using Cu-Cr-O as catalyst when the precursors are calcined at 400, 500, 600, and 700 ℃. The results indicate that the calcination of the Cu-Cr-O catalyst at 600 ℃ is an effective method to get MWCNT with few nano-tube defects or amorphous carbons.
基金Project supported by the National Natural Science Foundation of China(21273150)。
文摘Several ternary oxides CuCeZrO_(y)(CCZ)were synthesized by a facile grinding method followed by calcination at high temperatures,and used as catalysts for CO oxidation at low temperatures.The influences of calcination temperature(400-600℃)on the physicochemical properties of the assynthesized ternary oxides were investigated by thermogravimetric analysis/differential scanning calorimetry(TGA/DSC),X-ray diffraction(XRD),transmission electron microscopy(TEM),Raman,inductively coupled plasma-optical emission spectrometry(ICP-OES),N_(2) adsorption,H_(2)-temperature programmed reduction(H_(2)-TPR),and X-ray photoelectron spectroscopy(XPS)characterizations.The results show that the increase in calcination temperature from 400 to 500℃is conducive to the high dispersion of CuOx on catalyst surface and the incorporation of Cu species into the support to form the Cu-Ce-Zr-O solid solution.Further raising of calcination temperature from 500 to 600℃,however,leads to the segregation of Cu species from the solid solution to aggregate on support surface and growth of highly dispersed CuOx nanoparticles.The highest catalytic activity is acquired over the CCZ calcined at 500℃,which can be ascribed to the largest contents of Cu+species and oxygen vacancies owing to the formation of the maximum amount of Cu-Ce-Zr-O solid solution.
