A series CeO2(ZrO2)/TiO2 catalysts were modified with Er using a sol-gel method.The catalytic activity of the obtained catalysts in the selective catalytic reduction(SCR) of NO with NH3 was investigated to determi...A series CeO2(ZrO2)/TiO2 catalysts were modified with Er using a sol-gel method.The catalytic activity of the obtained catalysts in the selective catalytic reduction(SCR) of NO with NH3 was investigated to determine the appropriate Er dosage.The catalysts were characterized using X-ray diffraction,N2 adsorption,NH3 temperature-programmed desorption,H2 temperature-programmed reduction,photoluminescence spectroscopy,electron paramagnetic resonance spectroscopy,and X-ray photoelectron spectroscopy.The results showed that the optimum Er/Ce molar ratio was 0.10;this catalyst had excellent resistance to catalyst poisoning caused by vapor and sulfur and gave more than 90% NO conversion at 220–395 ℃ and a gas hourly space velocity of 71 400 h^-1.Er incorporation increased the Ti^3+ concentrations,oxygen storage capacities,and oxygen vacancy concentrations of the catalysts,resulting in excellent catalytic performance.Er incorporation also decreased the acid strength and inhibited growth of TiO2 and CeO2 crystal particles,which increased the catalytic activity.The results show that high oxygen vacancy concentrations and oxygen storage capacities,large amounts of Ti^3+,and low acid strengths give excellent SCR activity.展开更多
The Mn-Ce-Nb-O_x/P84 catalytic filter for removal of particulates and NO simultaneous was prepared by a novel method(foam coating method). The process parameters including the concentrations of PTFE emulsion, particle...The Mn-Ce-Nb-O_x/P84 catalytic filter for removal of particulates and NO simultaneous was prepared by a novel method(foam coating method). The process parameters including the concentrations of PTFE emulsion, particle size of catalyst and calcination temperature for preparation of catalytic filters were analyzed. In addition, the physical properties and performance for removal of NO(NH_3-SCR) and particulates of Mn-Ce-Nb-O_x/P84 catalytic filter prepared under the optimized parameters, were also systematic studied. Results show that the process parameters had significant influences on stability and performance of catalytic filter, The Mn-Ce-Nb-O_x/P84 catalytic filter prepared by foam coating method under the optimized parameters, has satisfactory physical properties and catalytic performance for removal of NO and particulates at 140-220 ℃. The NO removal efficiency of catalytic filter can reach95.3% at 200 ℃ as the catalyst loading amount is 450 g/m^2, Moreover,the dust removal efficiency of MnGe-Nb-O_x/P84 catalytic filter reaches as high as 99.98%, and the PM2.5 removal efficiency also reaches99.98%. The anti-sulfur performance of Mn-Ce-Nb-O_x catalytic filter is also attractive, after injecting150 ppm SO_2, the NO removal efficiency still retains up to 85%. It is indicated that the foam coating method can not only make a bond of high strength between catalyst and filter, but also make the catalytic filter possessing an excellent and stable performance for removal of NO and particulates.展开更多
Nb doped MnCe0.2Ox complex oxides catalysts prepared via a homogeneous precipitation method were investigated for synergistic catalytic removal of NOx and chlorobenzene(CB)at low temperatures.The MnNb0.4Ce0.2Ox cataly...Nb doped MnCe0.2Ox complex oxides catalysts prepared via a homogeneous precipitation method were investigated for synergistic catalytic removal of NOx and chlorobenzene(CB)at low temperatures.The MnNb0.4Ce0.2Ox catalyst with a molar ratio of Nb/Mn=0.4 exhibits excellent activity and the NOx and CB removal efficiency reaches 94.5%and 96%at 220℃,respectively.Furthermore,the NOx and CB removal efficiency of MnNb0.4Ce0.2Ox still remains above 80%after injecting 300 ppm SO2 and 7 vol%H2 O for 36 h.In addition,the presence of CB and NOx+NH3 can improve the NOx and CB removal efficiency of MnNb0.4Ce0.2Ox,respectively.The analysis results from N2-BET,Py-IR,H2-TPR and NH3-TPD reveal that the introduction of Nb increases the average pore size,pore volume and surface area,promoted the growth of Lewis acid amount obviously,and enhances redox ability of MnCe0.2Ox at 100-250℃.Moreover,the molecular migration process of NOx,NH3,CB and SO2 in NH3-SCR and CB oxidation reaction over MnNb0.4Ce0.2Ox catalysts were systematically studied.In situ DRIFTS,FT-IR and XPS also confirm that the adsorption of sulfate species and SO2 on the surface of MnNb0.4Ce0.2Ox is inhibited effectively by the introduction of Nb in the presence of SO2 and H2 O.Moreover,Nb additives also enhance the structural stability of MnNb0.4Ce0.2Ox,due to the interactions among Mn,Nb and Ce.The NH3-TPD,H2-TPR and in situ DRIFTS results also confirm that the MnNb0.4Ce0.2Ox still retains abundant acid sites and high redox ability in the presence of SO2 and H2O.In summary,MnNb0.4Ce0.2Ox catalysts represent a promising and effective candidate for controlling NOx and CB at low temperatures.展开更多
A series of CeO2/Al2O3 catalysts was modified with praseodymium oxide using an extrusion method. The cata- lytic activities of the obtained catalysts were measured for the selective catalytic reduction of NO with NH3 ...A series of CeO2/Al2O3 catalysts was modified with praseodymium oxide using an extrusion method. The cata- lytic activities of the obtained catalysts were measured for the selective catalytic reduction of NO with NH3 to screen suitable addition of praseodymium oxide. These samples were characterized by XRD, N2-BET, NH3-TPD, NO-TPD, Py-IR, H2-TPR, Raman spectra and XPS, respectively. Results showed the optimal catalyst with the Pr/Ce molar ratio of 0.10 exhibited more than 90% NO conversion in a wide temperature range of 290-425℃ under GHSV of 5000 h i. The number of Lewis acid sites and the chemisorbed oxygen concentration of the catalysts would increase with the Pr incorporation, which was favorable for the excellent catalytic performance. In addition, the Pr incorporation inhibited growth of the Al2O3 crystal particles and led to the lattice expansion of CeO2, which increased catalytic activity. The results implied that the higher chemisorbed oxygen concentrations and the more Lewis acid sites were conductive to obtain the excellent SCR activity.展开更多
A series of Mn-Mo-W-O_x/TiO_2-SiO_2 catalysts was modified with CeO_2 using an extrusion molding method. The catalytic activities of the obtained catalysts were tested for the synergistic catalytic removals of CO, NO ...A series of Mn-Mo-W-O_x/TiO_2-SiO_2 catalysts was modified with CeO_2 using an extrusion molding method. The catalytic activities of the obtained catalysts were tested for the synergistic catalytic removals of CO, NO and C_3H_8. The ratio of catalyst composition on catalytic activities for NH_3-SCR was optimized, which reveals that the molar ratio of Ti/Si was 9:1 and the catalyst containing 1.5 wt% CeO_2 and 12 wt% Mn-Mo-W-O_x exhibits the best catalytic performances. These samples were characterized by XRD, N_2-BET, Py-IR, NH_3-TPD, SEM/element mapping, H_2-TPR and XPS, respectively. Results show that the optimal catalyst exhibits more than 99% NO conversion, 86% CO conversion and 100% C_3H_8 conversion under GHSV of 5000 h^(-1). In addition, the GHSV has little influence on removal of NO when it is less than 15,000 h^(-1). Furthermore, the addition of CeO_2 will enhance the surface acidity, increase Mn^(4+)concentration and inhibit the grain growth, which are favorable for the excellent catalytic performance.Anyway,the 1.5 wt% CeO_2-12 wt% Mn-Mo-W-O_x/TiO_2-SiO_2 possesses outstanding redox properties,abundant acid sites and high Mn^(4+) concentration, which provide a guarantee for synergistic catalytic removal of CO, NO and HC.展开更多
NiMnO3 perovskite catalysts supported on cordierite modified by CexZr(1-x)O2 coatings were prepared using impregnation and sol-gel methods for catalytic combustion of single/double component VOCs at different concen...NiMnO3 perovskite catalysts supported on cordierite modified by CexZr(1-x)O2 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, H2-TPR and O2-TPD. After coating modification, the specific surface area of catalysts is improved obviously.Among the catalysts, the Ce(0.75)Zr(0.25)O2 coating modified NiMnO3 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)O2 coating can promote more lattice distortion and defects and smaller crystal size, which improve oxygen transfer capability and dispersion of active component.展开更多
Zr-doped-TiO2 loaded glass fiber(ZT/GF) composite photocatalysts with different Zr/Ti ratios were prepared with a sol–gel process. Zr4+can replace Ti4+in the TiO2 lattice, which is conducive to forming the anatas...Zr-doped-TiO2 loaded glass fiber(ZT/GF) composite photocatalysts with different Zr/Ti ratios were prepared with a sol–gel process. Zr4+can replace Ti4+in the TiO2 lattice, which is conducive to forming the anatase phase and reducing the calcination temperature. The glass fiber carrier was responsible for better dispersion and loading of Zr-doped-TiO2 particles, improving the applicability of the Zr-doped-TiO2. The ZT/GF photocatalysts were characterized by X-ray diffraction(XRD), scanning electron microscope(SEM), Fourier transform infrared spectroscopy(FT-IR), ultraviolet–visible spectroscopy(UV–vis) and Barrett–Joyner–Halenda(BJH). The performance of photocatalysts with different loading was evaluated in formaldehyde degradation under visible light at room temperature. ZT/GF0.2exhibited the highest activity, with a formaldehyde removal rate as high as 95.14% being observed, which is better than that of the photocatalyst particles alone. The stability of the catalyst was also tested, and ZT/GF exhibited excellent catalytic performance with 94.38%removal efficiency, even after seven uses.展开更多
基金supported by the National Natural Science Foundation of China(51272105)Jiangsu Provincial Science and Technology Supporting Program(BE2013718)+1 种基金Research Subject of Environmental Protection Department of Jiangsu Province of China(2013006)Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)~~
文摘A series CeO2(ZrO2)/TiO2 catalysts were modified with Er using a sol-gel method.The catalytic activity of the obtained catalysts in the selective catalytic reduction(SCR) of NO with NH3 was investigated to determine the appropriate Er dosage.The catalysts were characterized using X-ray diffraction,N2 adsorption,NH3 temperature-programmed desorption,H2 temperature-programmed reduction,photoluminescence spectroscopy,electron paramagnetic resonance spectroscopy,and X-ray photoelectron spectroscopy.The results showed that the optimum Er/Ce molar ratio was 0.10;this catalyst had excellent resistance to catalyst poisoning caused by vapor and sulfur and gave more than 90% NO conversion at 220–395 ℃ and a gas hourly space velocity of 71 400 h^-1.Er incorporation increased the Ti^3+ concentrations,oxygen storage capacities,and oxygen vacancy concentrations of the catalysts,resulting in excellent catalytic performance.Er incorporation also decreased the acid strength and inhibited growth of TiO2 and CeO2 crystal particles,which increased the catalytic activity.The results show that high oxygen vacancy concentrations and oxygen storage capacities,large amounts of Ti^3+,and low acid strengths give excellent SCR activity.
基金Project supported by the National Natural Science Foundation of China(21501097,21272118,21577065)the Natural Science Foundation of Jiangsu Province(BK20170954)+2 种基金the Startup Foundation for Introducing Talent of NUIST(2017r073)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China,China(18KJB430019)University Science Research Project of Jiangsu Province(18KJB430019)
文摘The Mn-Ce-Nb-O_x/P84 catalytic filter for removal of particulates and NO simultaneous was prepared by a novel method(foam coating method). The process parameters including the concentrations of PTFE emulsion, particle size of catalyst and calcination temperature for preparation of catalytic filters were analyzed. In addition, the physical properties and performance for removal of NO(NH_3-SCR) and particulates of Mn-Ce-Nb-O_x/P84 catalytic filter prepared under the optimized parameters, were also systematic studied. Results show that the process parameters had significant influences on stability and performance of catalytic filter, The Mn-Ce-Nb-O_x/P84 catalytic filter prepared by foam coating method under the optimized parameters, has satisfactory physical properties and catalytic performance for removal of NO and particulates at 140-220 ℃. The NO removal efficiency of catalytic filter can reach95.3% at 200 ℃ as the catalyst loading amount is 450 g/m^2, Moreover,the dust removal efficiency of MnGe-Nb-O_x/P84 catalytic filter reaches as high as 99.98%, and the PM2.5 removal efficiency also reaches99.98%. The anti-sulfur performance of Mn-Ce-Nb-O_x catalytic filter is also attractive, after injecting150 ppm SO_2, the NO removal efficiency still retains up to 85%. It is indicated that the foam coating method can not only make a bond of high strength between catalyst and filter, but also make the catalytic filter possessing an excellent and stable performance for removal of NO and particulates.
基金Project supported by the National Natural Science Foundation of China(51902166)the Natural Science Foundation of Jiangsu Province(BK20190786+6 种基金BK20170954)the Key Research and Development Program of Jiangsu Province(BE2018074)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(18KJB430019)the Startup Foundation for Introducing Talent of NUIST(2017r073)the USA NIH/NIAID(R21AI107415)the NSF-PREM program(DMR 1827745)the Philadelphia Foundation。
文摘Nb doped MnCe0.2Ox complex oxides catalysts prepared via a homogeneous precipitation method were investigated for synergistic catalytic removal of NOx and chlorobenzene(CB)at low temperatures.The MnNb0.4Ce0.2Ox catalyst with a molar ratio of Nb/Mn=0.4 exhibits excellent activity and the NOx and CB removal efficiency reaches 94.5%and 96%at 220℃,respectively.Furthermore,the NOx and CB removal efficiency of MnNb0.4Ce0.2Ox still remains above 80%after injecting 300 ppm SO2 and 7 vol%H2 O for 36 h.In addition,the presence of CB and NOx+NH3 can improve the NOx and CB removal efficiency of MnNb0.4Ce0.2Ox,respectively.The analysis results from N2-BET,Py-IR,H2-TPR and NH3-TPD reveal that the introduction of Nb increases the average pore size,pore volume and surface area,promoted the growth of Lewis acid amount obviously,and enhances redox ability of MnCe0.2Ox at 100-250℃.Moreover,the molecular migration process of NOx,NH3,CB and SO2 in NH3-SCR and CB oxidation reaction over MnNb0.4Ce0.2Ox catalysts were systematically studied.In situ DRIFTS,FT-IR and XPS also confirm that the adsorption of sulfate species and SO2 on the surface of MnNb0.4Ce0.2Ox is inhibited effectively by the introduction of Nb in the presence of SO2 and H2 O.Moreover,Nb additives also enhance the structural stability of MnNb0.4Ce0.2Ox,due to the interactions among Mn,Nb and Ce.The NH3-TPD,H2-TPR and in situ DRIFTS results also confirm that the MnNb0.4Ce0.2Ox still retains abundant acid sites and high redox ability in the presence of SO2 and H2O.In summary,MnNb0.4Ce0.2Ox catalysts represent a promising and effective candidate for controlling NOx and CB at low temperatures.
文摘A series of CeO2/Al2O3 catalysts was modified with praseodymium oxide using an extrusion method. The cata- lytic activities of the obtained catalysts were measured for the selective catalytic reduction of NO with NH3 to screen suitable addition of praseodymium oxide. These samples were characterized by XRD, N2-BET, NH3-TPD, NO-TPD, Py-IR, H2-TPR, Raman spectra and XPS, respectively. Results showed the optimal catalyst with the Pr/Ce molar ratio of 0.10 exhibited more than 90% NO conversion in a wide temperature range of 290-425℃ under GHSV of 5000 h i. The number of Lewis acid sites and the chemisorbed oxygen concentration of the catalysts would increase with the Pr incorporation, which was favorable for the excellent catalytic performance. In addition, the Pr incorporation inhibited growth of the Al2O3 crystal particles and led to the lattice expansion of CeO2, which increased catalytic activity. The results implied that the higher chemisorbed oxygen concentrations and the more Lewis acid sites were conductive to obtain the excellent SCR activity.
基金Project supported by the National Key Research and Development Program of China(2016YFC0205500)National Natural Science Foundation of China(51772149)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘A series of Mn-Mo-W-O_x/TiO_2-SiO_2 catalysts was modified with CeO_2 using an extrusion molding method. The catalytic activities of the obtained catalysts were tested for the synergistic catalytic removals of CO, NO and C_3H_8. The ratio of catalyst composition on catalytic activities for NH_3-SCR was optimized, which reveals that the molar ratio of Ti/Si was 9:1 and the catalyst containing 1.5 wt% CeO_2 and 12 wt% Mn-Mo-W-O_x exhibits the best catalytic performances. These samples were characterized by XRD, N_2-BET, Py-IR, NH_3-TPD, SEM/element mapping, H_2-TPR and XPS, respectively. Results show that the optimal catalyst exhibits more than 99% NO conversion, 86% CO conversion and 100% C_3H_8 conversion under GHSV of 5000 h^(-1). In addition, the GHSV has little influence on removal of NO when it is less than 15,000 h^(-1). Furthermore, the addition of CeO_2 will enhance the surface acidity, increase Mn^(4+)concentration and inhibit the grain growth, which are favorable for the excellent catalytic performance.Anyway,the 1.5 wt% CeO_2-12 wt% Mn-Mo-W-O_x/TiO_2-SiO_2 possesses outstanding redox properties,abundant acid sites and high Mn^(4+) concentration, which provide a guarantee for synergistic catalytic removal of CO, NO and HC.
基金Project supported by the Science and Technology Department of Jiangsu Province(BE2016769)the Natural Science Foundation of China(51172107)+2 种基金Natural Science Foundation of the Jiangsu Higher Education Institutions of China(14KJB430014)Open fund by Jiangsu Engineering Technology Research Center of Environmental Cleaning Materials(KFK1503)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘NiMnO3 perovskite catalysts supported on cordierite modified by CexZr(1-x)O2 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, H2-TPR and O2-TPD. After coating modification, the specific surface area of catalysts is improved obviously.Among the catalysts, the Ce(0.75)Zr(0.25)O2 coating modified NiMnO3 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)O2 coating can promote more lattice distortion and defects and smaller crystal size, which improve oxygen transfer capability and dispersion of active component.
基金financially supported by the Project of Science and Technology Department of Jiangsu Province (BE2016769)the Natural Science Foundation of China (No. 51608261)+2 种基金Six talent peaks project in Jiangsu Province (2016)Open fund by Jiangsu Engineering Technology Research Center of Environmental Cleaning Materials (KFK1503)A Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
文摘Zr-doped-TiO2 loaded glass fiber(ZT/GF) composite photocatalysts with different Zr/Ti ratios were prepared with a sol–gel process. Zr4+can replace Ti4+in the TiO2 lattice, which is conducive to forming the anatase phase and reducing the calcination temperature. The glass fiber carrier was responsible for better dispersion and loading of Zr-doped-TiO2 particles, improving the applicability of the Zr-doped-TiO2. The ZT/GF photocatalysts were characterized by X-ray diffraction(XRD), scanning electron microscope(SEM), Fourier transform infrared spectroscopy(FT-IR), ultraviolet–visible spectroscopy(UV–vis) and Barrett–Joyner–Halenda(BJH). The performance of photocatalysts with different loading was evaluated in formaldehyde degradation under visible light at room temperature. ZT/GF0.2exhibited the highest activity, with a formaldehyde removal rate as high as 95.14% being observed, which is better than that of the photocatalyst particles alone. The stability of the catalyst was also tested, and ZT/GF exhibited excellent catalytic performance with 94.38%removal efficiency, even after seven uses.