Two series of Mn/beta and Mn/ZSM‐5catalysts were prepared to study the influence of how different Mn precursors,introduced to the respective parent zeolites by wet impregnation,affected the selective catalytic reduct...Two series of Mn/beta and Mn/ZSM‐5catalysts were prepared to study the influence of how different Mn precursors,introduced to the respective parent zeolites by wet impregnation,affected the selective catalytic reduction(SCR)of NO by NH3across a low reaction temperature window of50–350°C.In this study,the catalysts were characterized using N2adsorption/desorption,X‐ray diffraction,X‐ray fluorescence,H2temperature‐programmed reduction,NH3temperature‐programmed desorption and X‐ray photoelectron spectroscopy.As the manganese chloride precursor only partially decomposed this primarily resulted in the formation of MnCl2in addition to the presence of low levels of crystalline Mn3O4,which resulted in poor catalytic performance.However,the manganese nitrate precursor formed crystalline MnO2as the major phase in addition to a minor presence of unconverted Mn‐nitrate.Furthermore,manganese acetate resulted principally in a mixture of amorphous Mn2O3and MnO2,and crystalline Mn3O4.From all the catalysts screened,the test performance data showed Mn/beta‐Ac to exhibit the highest NO conversion(97.5%)at240°C,which remained>90%across a temperature window of220–350°C.The excellent catalytic performance was ascribed to the enrichment of highly dispersed MnOx(Mn2O3and MnO2)species that act as the active phase in the NH3‐SCR process.Furthermore,together with a suitable amount of weakly acidic centers,higher concentration of surface manganese and a greater presence of surface labile oxygen groups,SCR performance was collectively enhanced at low temperature.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.展开更多
Cu–Mn bimetal catalysts were prepared to remove nitrogen oxides(NOx)from diesel engine exhaust at low temperatures.At a Cu/Mn ratio of 3:2,the NOx conversions at 200°C reached 65%and 90%on Cu–Mn/ZSM‐5 and Cu–...Cu–Mn bimetal catalysts were prepared to remove nitrogen oxides(NOx)from diesel engine exhaust at low temperatures.At a Cu/Mn ratio of 3:2,the NOx conversions at 200°C reached 65%and 90%on Cu–Mn/ZSM‐5 and Cu–Mn/SAPO‐34,respectively.After a hydrothermal treatment and reaction in the presence of C3H6,the activity of Cu–Mn/SAPO‐34 was more stable than that of Cu–Mn/ZSM‐5.No obvious variations in the crystal structure or dealumination were observed,whereas the physical structure was best maintained in Cu–Mn/SAPO‐34.The atomic concentration of Cu on the surface of Cu–Mn/SAPO‐34 was quite stable,and the consumption of octahedrally coordinated Cu2+could be recovered.Conversely,the proportion of octahedrally coordinated Cu2+on the surface of Cu–Mn/ZSM‐5 significantly decreased.Therefore,besides the structure,the redox cycle between Cu+and octahedrally coordinated Cu2+played an important role in the stability of the catalysts.展开更多
基金supported by the National Science and Technology Program of China(CDGC01-KT16)~~
文摘Two series of Mn/beta and Mn/ZSM‐5catalysts were prepared to study the influence of how different Mn precursors,introduced to the respective parent zeolites by wet impregnation,affected the selective catalytic reduction(SCR)of NO by NH3across a low reaction temperature window of50–350°C.In this study,the catalysts were characterized using N2adsorption/desorption,X‐ray diffraction,X‐ray fluorescence,H2temperature‐programmed reduction,NH3temperature‐programmed desorption and X‐ray photoelectron spectroscopy.As the manganese chloride precursor only partially decomposed this primarily resulted in the formation of MnCl2in addition to the presence of low levels of crystalline Mn3O4,which resulted in poor catalytic performance.However,the manganese nitrate precursor formed crystalline MnO2as the major phase in addition to a minor presence of unconverted Mn‐nitrate.Furthermore,manganese acetate resulted principally in a mixture of amorphous Mn2O3and MnO2,and crystalline Mn3O4.From all the catalysts screened,the test performance data showed Mn/beta‐Ac to exhibit the highest NO conversion(97.5%)at240°C,which remained>90%across a temperature window of220–350°C.The excellent catalytic performance was ascribed to the enrichment of highly dispersed MnOx(Mn2O3and MnO2)species that act as the active phase in the NH3‐SCR process.Furthermore,together with a suitable amount of weakly acidic centers,higher concentration of surface manganese and a greater presence of surface labile oxygen groups,SCR performance was collectively enhanced at low temperature.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.
基金supported by the National Natural Science Foundation of China(51008277)the Natural Science Foundation of Zhejiang Province(LY14E080001)the Key Project of Zhejiang Provincial Science and Technology Program(2012C03003-4)~~
文摘Cu–Mn bimetal catalysts were prepared to remove nitrogen oxides(NOx)from diesel engine exhaust at low temperatures.At a Cu/Mn ratio of 3:2,the NOx conversions at 200°C reached 65%and 90%on Cu–Mn/ZSM‐5 and Cu–Mn/SAPO‐34,respectively.After a hydrothermal treatment and reaction in the presence of C3H6,the activity of Cu–Mn/SAPO‐34 was more stable than that of Cu–Mn/ZSM‐5.No obvious variations in the crystal structure or dealumination were observed,whereas the physical structure was best maintained in Cu–Mn/SAPO‐34.The atomic concentration of Cu on the surface of Cu–Mn/SAPO‐34 was quite stable,and the consumption of octahedrally coordinated Cu2+could be recovered.Conversely,the proportion of octahedrally coordinated Cu2+on the surface of Cu–Mn/ZSM‐5 significantly decreased.Therefore,besides the structure,the redox cycle between Cu+and octahedrally coordinated Cu2+played an important role in the stability of the catalysts.
基金supported by the National Natural Science Foundation of China(No.21073131)Shanxi Provincial Science and Technology Projects(No.20140313002-2)+1 种基金State Key Laboratory Breeding Base of Coal Science and Technology Co-founded by Shanxi Province and the Ministry of Science and TechnologyTaiyuan University of Technology(No.MKX201301)~~
