Highly selective catalytic reduction of NO_x by MnO_x–CeO_2–Al_2O_3 catalysts prepared by self-propagating high-temperature synthesis
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摘要
We first present preparation of MnOx–CeO_2–Al_2O_3 catalysts with varying Mn contents through a self-propagating high-temperature synthesis(SHS) method, and studied the application of these catalysts to the selective catalytic reduction of NOxwith NH3(NH_3-SCR).Using the catalyst with 18 wt.% Mn(18 MnCe1Al2), 100% NO conversion was achieved at 200°C and a gas hourly space velocity of 15384 hr-1, and the high-efficiency SCR temperature window, where NO conversion is greater than 90%, was widened to a temperature range of 150–300°C. 18 MnCe1Al2 showed great resistance to SO_2(100 ppm)and H_2O(5%) at 200°C. The catalysts were characterized using X-ray diffraction, X-ray photoelectron spectroscopy, Brunauer–Emmett–Teller(BET) analysis, scanning electron microscopy, Fourier transform infrared spectroscopy, and H_2 temperature programmed reduction. The characterization results showed that the surface atomic concentration of Mn increased with increasing Mn content, which led to synergism between Mn and Ce and improved the activity in the SCR reaction. 18 MnCe1Al2 has an extensive pore structure,with a BET surface area of approximately 135.4 m~2/g, a pore volume of approximately 0.16 cm~3/g, and an average pore diameter of approximately 4.6 nm. The SCR reaction on 18 MnCe1Al2 mainly followed the Eley-Rideal mechanism. The performances of the MnOx–CeO_2–Al_2O_3 catalysts were good, and because of the simplicity of the preparation process,the SHS method is applicable to their industrial-scale manufacture.
We first present preparation of MnOx–CeO_2–Al_2O_3 catalysts with varying Mn contents through a self-propagating high-temperature synthesis(SHS) method, and studied the application of these catalysts to the selective catalytic reduction of NOxwith NH3(NH_3-SCR).Using the catalyst with 18 wt.% Mn(18 MnCe1Al2), 100% NO conversion was achieved at 200°C and a gas hourly space velocity of 15384 hr-1, and the high-efficiency SCR temperature window, where NO conversion is greater than 90%, was widened to a temperature range of 150–300°C. 18 MnCe1Al2 showed great resistance to SO_2(100 ppm)and H_2O(5%) at 200°C. The catalysts were characterized using X-ray diffraction, X-ray photoelectron spectroscopy, Brunauer–Emmett–Teller(BET) analysis, scanning electron microscopy, Fourier transform infrared spectroscopy, and H_2 temperature programmed reduction. The characterization results showed that the surface atomic concentration of Mn increased with increasing Mn content, which led to synergism between Mn and Ce and improved the activity in the SCR reaction. 18 MnCe1Al2 has an extensive pore structure,with a BET surface area of approximately 135.4 m~2/g, a pore volume of approximately 0.16 cm~3/g, and an average pore diameter of approximately 4.6 nm. The SCR reaction on 18 MnCe1Al2 mainly followed the Eley-Rideal mechanism. The performances of the MnOx–CeO_2–Al_2O_3 catalysts were good, and because of the simplicity of the preparation process,the SHS method is applicable to their industrial-scale manufacture.
We first present preparation of MnOx–CeO_2–Al_2O_3 catalysts with varying Mn contents through a self-propagating high-temperature synthesis(SHS) method, and studied the application of these catalysts to the selective catalytic reduction of NOxwith NH3(NH_3-SCR).Using the catalyst with 18 wt.% Mn(18 MnCe1Al2), 100% NO conversion was achieved at 200°C and a gas hourly space velocity of 15384 hr-1, and the high-efficiency SCR temperature window, where NO conversion is greater than 90%, was widened to a temperature range of 150–300°C. 18 MnCe1Al2 showed great resistance to SO_2(100 ppm)and H_2O(5%) at 200°C. The catalysts were characterized using X-ray diffraction, X-ray photoelectron spectroscopy, Brunauer–Emmett–Teller(BET) analysis, scanning electron microscopy, Fourier transform infrared spectroscopy, and H_2 temperature programmed reduction. The characterization results showed that the surface atomic concentration of Mn increased with increasing Mn content, which led to synergism between Mn and Ce and improved the activity in the SCR reaction. 18 MnCe1Al2 has an extensive pore structure,with a BET surface area of approximately 135.4 m~2/g, a pore volume of approximately 0.16 cm~3/g, and an average pore diameter of approximately 4.6 nm. The SCR reaction on 18 MnCe1Al2 mainly followed the Eley-Rideal mechanism. The performances of the MnOx–CeO_2–Al_2O_3 catalysts were good, and because of the simplicity of the preparation process,the SHS method is applicable to their industrial-scale manufacture.
引文
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Gao,F.,Tang,X.,Yi,H.,Li,J.,Zhao,S.,Wang,J.,Chu,C.,Li,C.,2017.Promotional mechanisms of activity and SO2tolerance of Coor Ni-doped MnOx-CeO2catalysts for SCR of NOxwith NH3at low temperature.Chem.Eng.J.317,20-31.
Ge,C.,Liu,L.,Liu,Z.,Yao,X.,Cao,Y.,Tang,C.,Gao,F.,Dong,L.,2014.Improving the dispersion of CeO2onγ-Al2O3to enhance the catalytic performances of CuO/CeO2/γ-Al2O3catalysts for NO removal by CO.Catal.Commun.51,95-99.
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Li,C.,Zhang,X.,Wang,K.,Sun,X.,Liu,G.,Li,J.,Tian,H.,Li,J.,Ma,Y.,2016.Scalable self-propagating high-temperature synthesis of graphene for supercapacitors with superior power density and cyclic stability.Adv.Mater.690(4),1-8.
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Balle,P.,Geiger,B.,Kureti,S.,2009b.Selective catalytic reduction of NOxby NH3on Fe/HBEA zeolite catalysts in oxygen-rich exhaust.Appl.Catal.B Environ.85(3-4),109-119.
Boningari,T.,Ettireddy,P.R.,Somogyvari,A.,Yi,L.,Vorontsov,A.,Mcdonald,C.A.,Smirniotis,P.G.,2015.Influence of elevated surface texture hydrated titania on Ce-doped Mn/TiO2catalysts for the low-temperature SCR of NOxunder oxygen-rich conditions.J.Catal.325,145-155.
Büchel,R.,Strobel,R.,Baiker,A.,Pratsinis,S.E.,2009.Effect of the proximity of Pt to Ce or Ba in Pt/Ba/CeO2catalysts on NOx storage-reduction performance.Top.Catal.52(13-20),1709-1712.
Cao,J.L.,Yan,W.,Yuan,Z.Y.,Zhang,T.Y.,Wu,S.H.,2008.Preparation,characterization and catalytic behavior of nanostructured mesoporous CuO/Ce0.8Zr0.2O2catalysts for low-temperature CO oxidation.Appl.Catal.B Environ.78(1-2),120-128.
Deng,Y.X.,Chen,X.,Shao,R.,Hu,L.M.,Tang,J.,Wang,C.Q.,2016.V2O5-WO3/TiO2catalysts for low temperature NH3-SCR:Catalytic activity and characterization.Key Eng.Mater.697,275-278.
Devadas,M.,Kr?cher,O.,Elsener,M.,Wokaun,A.,Mitrikas,G.,S?ger,N.,Pfeifer,M.,Demel,Y.,Mussmann,L.,2007.Characterization and catalytic investigation of Fe-ZSM5 for urea-SCR.Catal.Today 119(1-4),137-144.
Djerad,S.,Tifouti,L.,Crocoll,M.,Weisweiler,W.,2004.Effect of vanadia and tungsten loadings on the physical and chemical characteristics of V2O5/WO3TiO2catalysts.J.Mol.Catal.AChem.208(1),257-265.
Dong,W.K.,Nam,K.B.,Hong,S.C.,2015.Influence of tungsten on the activity of a Mn/Ce/W/Ti catalyst for the selective catalytic reduction of NO with NH3at low temperatures.Appl.Catal.A497,160-166.
Fan,C.,Sheng,S.,Xiang,J.,Wang,P.,Song,H.,Sun,L.,Zhang,A.,2015.The activity and mechanism study of Fe-Mn-Ce/γ-Al2O3catalyst for low temperature selective catalytic reduction of NO with NH3.Fuel 139,232-239.
Forzatti,P.,Nova,I.,Tronconi,E.,Kustov,A.,Th?gersen,J.R.,2012.Effect of operating variables on the enhanced SCR reaction over a commercial V2O5-WO3/TiO2catalyst for stationary applications.Catal.Today 184(1),153-159.
Gao,F.,Tang,X.,Yi,H.,Li,J.,Zhao,S.,Wang,J.,Chu,C.,Li,C.,2017.Promotional mechanisms of activity and SO2tolerance of Coor Ni-doped MnOx-CeO2catalysts for SCR of NOxwith NH3at low temperature.Chem.Eng.J.317,20-31.
Ge,C.,Liu,L.,Liu,Z.,Yao,X.,Cao,Y.,Tang,C.,Gao,F.,Dong,L.,2014.Improving the dispersion of CeO2onγ-Al2O3to enhance the catalytic performances of CuO/CeO2/γ-Al2O3catalysts for NO removal by CO.Catal.Commun.51,95-99.
Geng,Y.,Huang,H.,Chen,X.,Ding,H.,Yang,S.,Liu,F.,Shan,W.,2016.The effect of Ce on a high-efficiency CeO2/WO3-TiO2catalyst for the selective catalytic reduction of NOxwith NH3.Catal.Commun.40,47-50.
Haidi,X.U.,Fang,Z.,Cao,Y.,Kong,S.,Lin,T.,Gong,M.,Chen,Y.,Haidi,X.U.,Fang,Z.,Cao,Y.,2012.Influence of Mn/(Mn+Ce)ratio of MnOx-CeO2/WO3-ZrO2monolith catalyst on selective catalytic reduction of NOxwith ammonia.J.Catal.33(11-12),1927-1937.
Huang,H.Y.,Yang,R.T.,2001.Removal of NO by reversible adsorption on Fe-Mn based transition metal oxides.J.Langmuir 17(16),4997-5003.
Huang,Z.,Zhu,Z.,Liu,Z.,2002.Combined effect of H2O and SO2on V2O5/AC catalysts for NO reduction with ammonia at lower temperatures.Appl.Catal.B Environ.39(4),361-368.
Hui,C.,Zhang,Y.,Ying,X.,Qian,L.,Zhang,Z.,Zheng,J.,Ma,Y.,Hao,Z.,Jian,Z.,2015.Enhanced NOxconversion by coupling NOxstorage-reduction with Co adsorption-oxidation over the combined Pd-K/MgAlO and Pd/MgAlO catalysts.Catal.Today258,416-423.
Kapteijn,F.,Singoredjo,L.,Andreini,A.,Moulijn,J.A.,1994.Activity and selectivity of pure manganese oxides in the selective catalytic reduction of nitric oxide with ammonia.J.Cheminform.3(2-3),173-189.
Koebel,M.,Elsener,A.M.,Madia,G.,2013.Reaction pathways in the selective catalytic reduction process with NO and NO2at low temperatures.Ind.Eng.Chem.Res.40(1),52-59.
Li,C.,Zhang,X.,Wang,K.,Sun,X.,Liu,G.,Li,J.,Tian,H.,Li,J.,Ma,Y.,2016.Scalable self-propagating high-temperature synthesis of graphene for supercapacitors with superior power density and cyclic stability.Adv.Mater.690(4),1-8.
Liu,F.,He,H.,2010a.Selective catalytic reduction of NO with NH3over manganese substituted iron titanate catalyst:Reaction mechanism and H2O/SO2inhibition mechanism study.Catal.Today 153(3-4),70-76.
Liu,F.,He,H.,2010b.Structure-activity relationship of iron titanate catalysts in the selective catalytic reduction of NOx with NH3?.J.Phys.Chem.114(40),16929-16936.
Liu,Q.,Liu,Z.,Su,J.,2010.Al2O3-coated cordierite honeycomb supported CuO catalyst for selective catalytic reduction of NOby NH3:surface properties and reaction mechanism.Catal.Today 158(3-4),370-376.
Liu,Y.,Gu,T.,Weng,X.,Wang,Y.,Wu,Z.,Wang,H.,2012.Drift studies on the selectivity promotion mechanism of Ca modified Ce-Mn/TiO2catalysts for low-temperature NOreduction with NH3.J.Phys.Chem.A 116(31),16582-16592.
Liu,Z.,Zhu,J.,Li,J.,Ma,L.,Woo,S.I.,2014.Novel Mn-Ce-Ti mixedoxide catalyst for the selective catalytic reduction of NOxwith NH3.Appl.Mater.Interfaces 6(16),14500-14508.
Liu,R.,Xu,Y.F.,Ye,F.,Ji,L.C.,Guan,H.,Yang,M.,2016.Low-temperature selective catalytic reduction with NH3over MnOx-CeO2catalysts supported on nano tetragonal zirconia.Mater.Sci.Forum 582(4),293-299.
Madia,G.,Koebel,M.,Elsener,A.M.,Wokaun,A.,2002.Side reactions in the selective catalytic reduction of NOxwith various NO2fractions.Ind.Eng.Chem.Res.41(16),4008-4015.
Min,K.,Park,E.D.,Ji,M.K.,Yie,J.E.,2006.Cu-Mn mixed oxides for low temperature NO reduction with NH3.Catal.Today 111(3-4),236-241.
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