Catalytic properties of MnOx-FeOx complex oxide （hereafter denoted as Mn-Fe） catalysts modified with different loadings of chromium oxide were investigated by using the combination of physico-cbemical techniques, su...Catalytic properties of MnOx-FeOx complex oxide （hereafter denoted as Mn-Fe） catalysts modified with different loadings of chromium oxide were investigated by using the combination of physico-cbemical techniques, such as N2 physisorption, X-ray diffraction （XRD）, high-resolution transmission electron microscope （HRTEM）, in situ Fourier transform infrared spectroscopy （in situ FT-IR） and temperature-programmed reduction （TPR） and their catalytic activities were evaluated with the selective catalytic reduction （SCR） of NOx by NH3. It was found that with the addition of Cr, more NO could be removed in the low-temperature window （below 120 ℃）. Among the tested catalysts, Mn-Fe- Cr （2 ： 2 ： 1） catalyst exhibited the best catalytic performance at 80 ℃ with the NO conversion higher than 90%. The combination of the reaction and characterization results indicated that （1） the strong interaction among tertiary metal oxides existed in the catalysts when Cr was appropriately added, which made the active components better dispersed with less agglomeration and sintering and the largest BET specific surface area could be obtained; （2） Cr improved the low-temperature reducibility of the catalyst and promoted the formation of the active intermediate （-NH3＋）, which favored the low-temperature SCR reaction.展开更多
Monolithic catalysts of Pt/La-Al2O3 and Pt/Ce0.67Zr0.3302 were prepared to investigate methane selective catalytic reduction （SCR） of NO. The results indicate that Pt/Ce0.67Zr0.33O2 shows high activity and both NO a...Monolithic catalysts of Pt/La-Al2O3 and Pt/Ce0.67Zr0.3302 were prepared to investigate methane selective catalytic reduction （SCR） of NO. The results indicate that Pt/Ce0.67Zr0.33O2 shows high activity and both NO and CH4 can be converted completely at 450℃. Meanwhile, NO and CH4 can be converted completely when there exists excess oxygen. The Pt/Ce0.67Zr0.33O2 catalyst were further investigated by using methane as reducing agent to SCR NO in a novel equipment which combined the CH4 selective catalytic reduction of NO with methane combustion. The result shows that the catalyst is high active and the novel equipment is very effective. The conversion of NO is above 92% under the conditions used in this work. The prepared burner and catalysts have great potential for application.展开更多
We rationally designed a high performance denitration(De-NOx) catalyst based on a micrometer-sized spherical Mn–Ce–Fe–Ti(CP-SD)catalyst for selective catalytic reduction(SCR). This was prepared by a co-precipitatio...We rationally designed a high performance denitration(De-NOx) catalyst based on a micrometer-sized spherical Mn–Ce–Fe–Ti(CP-SD)catalyst for selective catalytic reduction(SCR). This was prepared by a co-precipitation and spray drying(CP-SD) method. The catalyst was systematically characterized, and its morphological structure and surface properties were identified. Compare with conventional Mn–Ce–Fe–Ti(CP) catalysts, the Mn–Ce–Fe–Ti(CP-SD) catalyst had superior surface-adsorbed oxygen leading to enhanced 'fast NH3-SCR' reaction. The asobtained Mn–Ce–Fe–Ti(CP-SD) catalyst offered excellent NO conversion and N2 selectivity of 100.0% and 84.8% at 250℃, respectively, with a gas hourly space velocity(GHSV) of 40,000 h-1. The porous micro-spherical structure provides a larger surface area and more active sites to adsorb and activate the reaction gases. In addition, the uniform distribution and strong interaction of manganese, iron, cerium, and titanium oxide species improved H2O and SO2 resistance. The results showed that the Mn–Ce–Fe–Ti(CP-SD) catalyst could be used prospectively as a denitration(De-NOx) catalyst.展开更多
Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybde...Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybdenum oxide,tungsten oxide,and cerium oxide were used to reconfigure the redox sites and acid sites of red mud based catalyst.When activated red mud was reconfigured by cerium-tungsten oxide(Ce-W@RM),the NOx conversion kept above 90%at 219-480℃.The existence of Ce^(3+)/Ce^(4+) redox electron pairs provided more surface adsorbed oxygen(O_(α)) and served as a redox cycle.Positive interactions between Ce,W species and Fe oxide in red mud occurred,which led to the formation of unsaturated chemical bond and promoted the activation of adsorbed NH_(3) species.WO_(3) and Ce_(2)(WO_(4))_(3)(formed by solid-state reaction between Ce and W species)could provide more Brønsted acid sites(W-O modes of WO_(3),W=O or W-O-W modes of Ce_(2)(WO_(4))_(3)).CeO_(2) species could provide more Lewis acid sites.The Langmuir-Hinshelwood(L-H)routes and Eley-Rideal(E-R)routes occurred in the low-temperature SCR reaction on the Ce-W@RM surface.NH_(4)^(+) species on Brønsted acid sites,NH_(3) species on Lewis acid sites,bidentate nitrate and bridging nitrate species were key active intermediates species.展开更多
Surface chemical properties of typical commercial coal-based activated cokes were characterized by Xray photoelectron spectroscopy(XPS) and acid-base titration, and then the influence of surface chemical properties on...Surface chemical properties of typical commercial coal-based activated cokes were characterized by Xray photoelectron spectroscopy(XPS) and acid-base titration, and then the influence of surface chemical properties on catalytic performance of activated cokes of NO reduction with NH3 was investigated in a fixed-bed quartz micro reactor at 150 ℃. The results indicate that the selective catalytic reduction(SCR) activity of activated cokes with the increase of its surface acidic sites and oxygen content,obviously, a correlation between catalytic activity and surface acidic sites content by titration has higher linearity than catalytic activity and surface oxygen content by XPS. While basic sites content by acid-base titration have not correlation with SCR activity. It has been proposed that surface basic sites content measured by titration may not be on adjacent of acidic surface oxides and then cannot form of NO2-like species, thus the reaction of reduction of NO with NH3 have been retarded.展开更多
Catalytic performance of W/HZSM-5 in selective catalytic reduction of NO by acetylene was investigated in a reaction system with 1600 ppm of NO, 800 ppm of C2H2, and 9.95% of O2 in He. It was found that promotional ef...Catalytic performance of W/HZSM-5 in selective catalytic reduction of NO by acetylene was investigated in a reaction system with 1600 ppm of NO, 800 ppm of C2H2, and 9.95% of O2 in He. It was found that promotional effect of tungsten on the reaction is strongly affected by catalyst preparation conditions and Si/Al ratio of the parent zeolite. A better dispersion of tungsten on HZSM-5 and relatively more monomeric tungsten species were found on 8%W/HZSM-5 prepared by impregnation of the zeolite with lower SiO2/A1203 ratio （25） in ammonic ammonium tungstate solution and calcination of the resulting material at higher temperature （550 ℃）. The highest NO conversion to N2 of 86.3% in the reaction system was obtained at 350 ℃ over the catalyst thus prepared. The mechanism of monomeric tungsten species improving the C2H2-SCR can be attributed to accelerating the formation of active nitrate species.展开更多
The removal of nitrogen oxides from exhaust gases has attracted greatattention in recent years, and many approaches have been developed depending on the application.Methane, the main component of natural gas, has grea...The removal of nitrogen oxides from exhaust gases has attracted greatattention in recent years, and many approaches have been developed depending on the application.Methane, the main component of natural gas, has great potential as a NO reductant. In this paper, anumber of catalysts previous reported for this catalytic reduction of NO have been reviewed,including a direct comparison of the relative activities and effective factors of the catalysts.Reaction mechanisms have also been explored preliminarily.展开更多
The presented work reports the selective catalytic reduction(SCR)of NO_(x) assisted by dielectric barrier discharge plasma via simulating marine diesel engine exhaust,and the experimental results demonstrate that the ...The presented work reports the selective catalytic reduction(SCR)of NO_(x) assisted by dielectric barrier discharge plasma via simulating marine diesel engine exhaust,and the experimental results demonstrate that the low-temperature activity of NH_(3)-SCR assisted by non-thermal plasma is enhanced significantly,particularly in the presence of a C_(3)H_(6) additive.Simultaneously,CeMnZrO_(x)@TiO_(2) exhibits strong tolerance to SO_(2) poisoning and superior catalytic stability.It is worthwhile to explore a new approach to remove NO_(x) from marine diesel engine exhaust,which is of vital significance for both academic research and practical applications.展开更多
The Cu-Mo/ZSM-5 catalysts with different Cu/Mo ratios were prepared by wetimpregnation method, and their catalytic performance for selective catalytic reduction of NO_x wasstudied. The results showed that Cu-Mo/ZSM-5 ...The Cu-Mo/ZSM-5 catalysts with different Cu/Mo ratios were prepared by wetimpregnation method, and their catalytic performance for selective catalytic reduction of NO_x wasstudied. The results showed that Cu-Mo/ZSM-5 is a very effective catalyst for NO_x catalyticreduction with ammonia, especially when Cu/Mo molar ratio is about 1.5. It not only exhibited theextremely high catalytic activity, but also showed good stability for O_2. The bulk phase structureof Cu-Mo/ZSM-5 catalysts was determined by XRD technique, and the results indicated that there is amaximum dispersion for Cu species when Cu/Mo molar ratio is 1.5, and an interaction between Cu andMo along with HZSM-5 may be present in Cu-Mo/ZSM-5, which may possibly result in a special structurefavorable for the catalytic reduction of NO_x over Cu-Mo/ZSM-5 catalyst.展开更多
基金supported by Jiangsu Natural Science Foundation (No. BK2012347)the National High Technology and Development Program of China (863 Programs, No.2007AA061802)
文摘Catalytic properties of MnOx-FeOx complex oxide （hereafter denoted as Mn-Fe） catalysts modified with different loadings of chromium oxide were investigated by using the combination of physico-cbemical techniques, such as N2 physisorption, X-ray diffraction （XRD）, high-resolution transmission electron microscope （HRTEM）, in situ Fourier transform infrared spectroscopy （in situ FT-IR） and temperature-programmed reduction （TPR） and their catalytic activities were evaluated with the selective catalytic reduction （SCR） of NOx by NH3. It was found that with the addition of Cr, more NO could be removed in the low-temperature window （below 120 ℃）. Among the tested catalysts, Mn-Fe- Cr （2 ： 2 ： 1） catalyst exhibited the best catalytic performance at 80 ℃ with the NO conversion higher than 90%. The combination of the reaction and characterization results indicated that （1） the strong interaction among tertiary metal oxides existed in the catalysts when Cr was appropriately added, which made the active components better dispersed with less agglomeration and sintering and the largest BET specific surface area could be obtained; （2） Cr improved the low-temperature reducibility of the catalyst and promoted the formation of the active intermediate （-NH3＋）, which favored the low-temperature SCR reaction.
基金Supported by the National High Technology Research and Development Program of China (863 Program, 2006AA06Z347)the NationalNatural Science Foundation of China (20773090).
文摘Monolithic catalysts of Pt/La-Al2O3 and Pt/Ce0.67Zr0.3302 were prepared to investigate methane selective catalytic reduction （SCR） of NO. The results indicate that Pt/Ce0.67Zr0.33O2 shows high activity and both NO and CH4 can be converted completely at 450℃. Meanwhile, NO and CH4 can be converted completely when there exists excess oxygen. The Pt/Ce0.67Zr0.33O2 catalyst were further investigated by using methane as reducing agent to SCR NO in a novel equipment which combined the CH4 selective catalytic reduction of NO with methane combustion. The result shows that the catalyst is high active and the novel equipment is very effective. The conversion of NO is above 92% under the conditions used in this work. The prepared burner and catalysts have great potential for application.
基金supported by Major Scientific and Technological Project of Bingtuan (No.2018AA002)the Program for Changjiang Scholars and Innovative Research Team in University (No. IRT_15R46)
文摘We rationally designed a high performance denitration(De-NOx) catalyst based on a micrometer-sized spherical Mn–Ce–Fe–Ti(CP-SD)catalyst for selective catalytic reduction(SCR). This was prepared by a co-precipitation and spray drying(CP-SD) method. The catalyst was systematically characterized, and its morphological structure and surface properties were identified. Compare with conventional Mn–Ce–Fe–Ti(CP) catalysts, the Mn–Ce–Fe–Ti(CP-SD) catalyst had superior surface-adsorbed oxygen leading to enhanced 'fast NH3-SCR' reaction. The asobtained Mn–Ce–Fe–Ti(CP-SD) catalyst offered excellent NO conversion and N2 selectivity of 100.0% and 84.8% at 250℃, respectively, with a gas hourly space velocity(GHSV) of 40,000 h-1. The porous micro-spherical structure provides a larger surface area and more active sites to adsorb and activate the reaction gases. In addition, the uniform distribution and strong interaction of manganese, iron, cerium, and titanium oxide species improved H2O and SO2 resistance. The results showed that the Mn–Ce–Fe–Ti(CP-SD) catalyst could be used prospectively as a denitration(De-NOx) catalyst.
基金supported by the National Natural Science Foundation of China(21906090)the National Key Research and Development Program(2017YFC0210200,2017YFC0212800)Primary Research&Development Project of Shandong Province(2018GSF117034,2019JZZY020305).
文摘Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybdenum oxide,tungsten oxide,and cerium oxide were used to reconfigure the redox sites and acid sites of red mud based catalyst.When activated red mud was reconfigured by cerium-tungsten oxide(Ce-W@RM),the NOx conversion kept above 90%at 219-480℃.The existence of Ce^(3+)/Ce^(4+) redox electron pairs provided more surface adsorbed oxygen(O_(α)) and served as a redox cycle.Positive interactions between Ce,W species and Fe oxide in red mud occurred,which led to the formation of unsaturated chemical bond and promoted the activation of adsorbed NH_(3) species.WO_(3) and Ce_(2)(WO_(4))_(3)(formed by solid-state reaction between Ce and W species)could provide more Brønsted acid sites(W-O modes of WO_(3),W=O or W-O-W modes of Ce_(2)(WO_(4))_(3)).CeO_(2) species could provide more Lewis acid sites.The Langmuir-Hinshelwood(L-H)routes and Eley-Rideal(E-R)routes occurred in the low-temperature SCR reaction on the Ce-W@RM surface.NH_(4)^(+) species on Brønsted acid sites,NH_(3) species on Lewis acid sites,bidentate nitrate and bridging nitrate species were key active intermediates species.
基金the High Technology Research and Development Program of China(No.2011AA060803)the Beijing Key Laboratory Annual Program(No.Z121103009212039)
文摘Surface chemical properties of typical commercial coal-based activated cokes were characterized by Xray photoelectron spectroscopy(XPS) and acid-base titration, and then the influence of surface chemical properties on catalytic performance of activated cokes of NO reduction with NH3 was investigated in a fixed-bed quartz micro reactor at 150 ℃. The results indicate that the selective catalytic reduction(SCR) activity of activated cokes with the increase of its surface acidic sites and oxygen content,obviously, a correlation between catalytic activity and surface acidic sites content by titration has higher linearity than catalytic activity and surface oxygen content by XPS. While basic sites content by acid-base titration have not correlation with SCR activity. It has been proposed that surface basic sites content measured by titration may not be on adjacent of acidic surface oxides and then cannot form of NO2-like species, thus the reaction of reduction of NO with NH3 have been retarded.
基金the National Natural Science Foundation of China(20677006)
文摘Catalytic performance of W/HZSM-5 in selective catalytic reduction of NO by acetylene was investigated in a reaction system with 1600 ppm of NO, 800 ppm of C2H2, and 9.95% of O2 in He. It was found that promotional effect of tungsten on the reaction is strongly affected by catalyst preparation conditions and Si/Al ratio of the parent zeolite. A better dispersion of tungsten on HZSM-5 and relatively more monomeric tungsten species were found on 8%W/HZSM-5 prepared by impregnation of the zeolite with lower SiO2/A1203 ratio （25） in ammonic ammonium tungstate solution and calcination of the resulting material at higher temperature （550 ℃）. The highest NO conversion to N2 of 86.3% in the reaction system was obtained at 350 ℃ over the catalyst thus prepared. The mechanism of monomeric tungsten species improving the C2H2-SCR can be attributed to accelerating the formation of active nitrate species.
文摘The removal of nitrogen oxides from exhaust gases has attracted greatattention in recent years, and many approaches have been developed depending on the application.Methane, the main component of natural gas, has great potential as a NO reductant. In this paper, anumber of catalysts previous reported for this catalytic reduction of NO have been reviewed,including a direct comparison of the relative activities and effective factors of the catalysts.Reaction mechanisms have also been explored preliminarily.
基金supported by National Key Research and Development Project of China(No.2019YFC1805503)National Engineering Laboratory for Mobile Source Emission Control Technology(No.NELMS2019A13)+1 种基金the Open Project Program of the State Key Laboratory of Petroleum Pollution Control(No.PPC2019013)Major Science and Technology Projects of Shanxi Province(No.20181102017)。
文摘The presented work reports the selective catalytic reduction(SCR)of NO_(x) assisted by dielectric barrier discharge plasma via simulating marine diesel engine exhaust,and the experimental results demonstrate that the low-temperature activity of NH_(3)-SCR assisted by non-thermal plasma is enhanced significantly,particularly in the presence of a C_(3)H_(6) additive.Simultaneously,CeMnZrO_(x)@TiO_(2) exhibits strong tolerance to SO_(2) poisoning and superior catalytic stability.It is worthwhile to explore a new approach to remove NO_(x) from marine diesel engine exhaust,which is of vital significance for both academic research and practical applications.
文摘The Cu-Mo/ZSM-5 catalysts with different Cu/Mo ratios were prepared by wetimpregnation method, and their catalytic performance for selective catalytic reduction of NO_x wasstudied. The results showed that Cu-Mo/ZSM-5 is a very effective catalyst for NO_x catalyticreduction with ammonia, especially when Cu/Mo molar ratio is about 1.5. It not only exhibited theextremely high catalytic activity, but also showed good stability for O_2. The bulk phase structureof Cu-Mo/ZSM-5 catalysts was determined by XRD technique, and the results indicated that there is amaximum dispersion for Cu species when Cu/Mo molar ratio is 1.5, and an interaction between Cu andMo along with HZSM-5 may be present in Cu-Mo/ZSM-5, which may possibly result in a special structurefavorable for the catalytic reduction of NO_x over Cu-Mo/ZSM-5 catalyst.
