Catalytic activity of Cu-SSZ-13 prepared with different methods for NH_3-SCR reaction
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摘要
A series of Cu-SSZ-13 catalysts with the same Cu loading were prepared by different methods of incipient wetness impregnation [Cu-SSZ-13(IWI)], ion exchange[Cu-SSZ-13(IE)] and hydro-thermal synthesis [Cu-SSZ-13(HTS)]. Their activity for selective catalytic reduction of nitrogen oxides(NO_x) with NH3 was determined. The results show that the Cu-SSZ-13(HTS) catalyst exhibits a better ammonia selective catalytic reduction(NH3-SCR)activity compared with the other two catalysts, over which more than 90% NO conversion is obtained at 215-600℃under the space velocity of 180,000 h~(-1). The characterization results reveal that the Cu-SSZ-13(HTS) catalyst possesses more amount of stable Cu~(2+) in the six-membered ring and high ability for NH3 and NO adsorption, leading to its high NH3-SCR activity, although this catalyst has low surface area. On the other hand, the activity of Cu-SSZ-13(IE) catalyst is almost the same as that of Cu-SSZ-13(IWI) catalyst at the temperature lower than 400 ℃, but the activity of the former is much higher than that of the latter at > 400 ℃ due to the high activity of Cu-SSZ-13(IWI) catalyst for NH3 oxidation.
A series of Cu-SSZ-13 catalysts with the same Cu loading were prepared by different methods of incipient wetness impregnation [Cu-SSZ-13(IWI)], ion exchange[Cu-SSZ-13(IE)] and hydro-thermal synthesis [Cu-SSZ-13(HTS)]. Their activity for selective catalytic reduction of nitrogen oxides(NO_x) with NH3 was determined. The results show that the Cu-SSZ-13(HTS) catalyst exhibits a better ammonia selective catalytic reduction(NH3-SCR)activity compared with the other two catalysts, over which more than 90% NO conversion is obtained at 215-600℃under the space velocity of 180,000 h~(-1). The characterization results reveal that the Cu-SSZ-13(HTS) catalyst possesses more amount of stable Cu~(2+) in the six-membered ring and high ability for NH3 and NO adsorption, leading to its high NH3-SCR activity, although this catalyst has low surface area. On the other hand, the activity of Cu-SSZ-13(IE) catalyst is almost the same as that of Cu-SSZ-13(IWI) catalyst at the temperature lower than 400 ℃, but the activity of the former is much higher than that of the latter at > 400 ℃ due to the high activity of Cu-SSZ-13(IWI) catalyst for NH3 oxidation.
A series of Cu-SSZ-13 catalysts with the same Cu loading were prepared by different methods of incipient wetness impregnation [Cu-SSZ-13(IWI)], ion exchange[Cu-SSZ-13(IE)] and hydro-thermal synthesis [Cu-SSZ-13(HTS)]. Their activity for selective catalytic reduction of nitrogen oxides(NO_x) with NH3 was determined. The results show that the Cu-SSZ-13(HTS) catalyst exhibits a better ammonia selective catalytic reduction(NH3-SCR)activity compared with the other two catalysts, over which more than 90% NO conversion is obtained at 215-600℃under the space velocity of 180,000 h~(-1). The characterization results reveal that the Cu-SSZ-13(HTS) catalyst possesses more amount of stable Cu~(2+) in the six-membered ring and high ability for NH3 and NO adsorption, leading to its high NH3-SCR activity, although this catalyst has low surface area. On the other hand, the activity of Cu-SSZ-13(IE) catalyst is almost the same as that of Cu-SSZ-13(IWI) catalyst at the temperature lower than 400 ℃, but the activity of the former is much higher than that of the latter at > 400 ℃ due to the high activity of Cu-SSZ-13(IWI) catalyst for NH3 oxidation.
引文
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[2] Huang JW, Li YR, Xia YF, Zhu JT, Yi QH, Wang H, Xiong J,Sun YH, Zou G F. Flexible cobalt phosphide network electrocatalyst for hydrogen evolution at all pH values. Nano Res.2017;10(3):1010.
[3] Burch R, Breen JP, Hill CJ, Krutzsch B, Konrad B, Jobson E,Cider L, Eranen K, Klingstedt F, Lindfors LE. Exceptional activity for NO_x reduction at low temperatures using combinations of hydrogen and higher hydrocarbons on Ag/Al_2O_3 catalysts. Top Catal. 2004;30-31(1):19.
[4] Han J, Meeprasert J, Maitarad P, Nammuangruk S, Shi LY,Zhang DS. Investigation of the facet-dependent catalytic performance of Fe_2O_3/Ce02 for the selective catalytic reduction of NO with NH3. J Phys Chem C. 2016;120(3):1523.
[5] Gu L, Chen X, Zhou Y, Zhu QL, Huang HF, Lu HF. Propene and CO oxidation on Pt/Ce-Zr-S042-diesel oxidation catalysts:effect of sulfate on activity and stability. Chin J Catal. 2017;38(3):607.
[6] Gao RH, Zhang DS, Maitarad P, Shi LY, Rungrotmongkol T, Li HR, Zhang JP, Cao WG. Morphology-dependent properties of MnO_x/ZrO_2-CeO_2 nanostructures for the selective catalytic reduction of NO with NH3. J Phys Chem C. 2013;117(20):10502.
[7] Wan HQ, Li D, Dai Y, Hu YH, Liu B, Dong L. Catalytic behaviors of CuO supported on Mn_2O_3 modifiedγ-Al_2O_3 for NO reduction by CO. J Mol Catal A Chem. 2010;332(1-2):32.
[8] Luo JY, Gao F, Kamasamudram K, Currier N, Peden CHF,Yezerets A. New insights into Cu/SSZ-13 SCR catalyst acidity.Part I:nature of acidic sites probed by NH3 titration. J Catal.2017;348:291.
[9] Liu FD, Shan WP, Pan DW, Li TY, He H. Selective catalytic reduction of NO_x by NH3 for heavy-duty diesel vehicle. Chin J Catal. 2014;35(9):1438.
[10] Meng DM, Zhan WC, Guo Y, Guo YL, Wang L, Lu GZ. A highly effective catalyst of Sm-MnO_x for the NH3-SCR of NO_x at low temperature:promotional role of Sm and its catalytic performance. ACS Catal. 2015;5:5973.
[11] Meng DM, Zhan WC, Guo Y, Guo YL, Wang YS, Wang L, Lu GZ. A highly effective catalyst of Sm-Mn mixed oxide for the selective catalytic reduction of NO_x with ammonia:effect of the calcination temperature. J Mol Catal A Chem. 2016;420:272.
[12] Grossale A, Nova I, Tronconi E. Study of a Fe-zeolite-based system as NH3-SCR catalyst for diesel exhaust after treatment.Catal Today. 2008;136(1-2):18.
[13] Yates M, Martin JA, Martin-Luengo MA, Suarez S, Blanco J.N_2O formation in the ammonia oxidation and in the SCR process with V_2O_5-WO_3 catalysts. Catal Today. 2005;107-108(15):120.
[14] Krishnan AT, Boehman AL. Selective catalytic reduction of nitric oxide with ammonia at low temperatures. Appl Catal B.1998;18(3-4):189.
[15] Meng DM, Xu Q, Jiao YL, Guo Y, Guo YL, Wang L, Lu GZ,Zhan WC. Spinel structured CoaMnbOx mixed oxide catalyst forthe selective catalytic reduction of NO_x with NH3. Appl Catal B.2018;221:652.
[16] Long RQ, Yang RT. Superior Fe-ZSM-5 catalyst for selective catalytic reduction of nitric oxide by ammonia. J Am Chem Soc.1999;121(23):5595.
[17] Chen HY, Sachtler WMH. Activity and durability of Fe/ZSM-5catalysts for lean burn NO_x reduction in the presence of water vapor. Catal Today. 1998;42(1-2):73.
[18] Lai SS, She Y, Zhan WC, Guo Y, Guo YL, Wang L, Lu GZ.Performance of Fe-ZSM-5 for selective catalytic reduction of NO_x with NH3:effect of the atmosphere during the preparation of catalysts. J Mol Catal A Chem. 2016;424:232.
[19] Xia Y, Zhan WC, Guo Y, Guo YL, Lu GZ. Activity of Fe-beta zeolite catalyst in selective catalytic reduction of nitrogen oxides:influence of Fe content. Chin J Catal. 2016;37(12):2069.
[20] Weng XL, Dai XX, Zeng QS, Liu Y, Wu ZB. DRIFT studies on promotion mechanism of H_3PW_(12)O_(40)in selective catalytic reduction of NO with NH3. J Colloid Interface Sci. 2016;461:9.
[21] Seo CK, Choi B, Kim H, Lee CH, Lee CB. Effect of Zr02addition on de-NO_x performance of Cu-ZSM-5 for SCR catalyst.Chem Eng J. 2012;191(19):331.
[22] Qi GS, Yang RT. Ultra-active Fe/ZSM-5 catalyst for selective catalytic reduction of nitric oxide with ammonia. Appl Catal B.2005;60(1-2):13.
[23] Lai SS, Meng DM, Zhan WC, Guo Y, Guo YL, Zhang ZG, Lu GZ. The promotional role of Ce in Cu/ZSM-5 and in situ surface reaction for selective catalytic reduction of NO_x with NH_3. RSC Adv. 2015;5(110):90235.
[24] Chen HY, Sachtler WMH. Promoted Fe/ZSM-5 catalysts prepared by sublimation:de-NO_x activity and durability in H_2O-rich streams. Catal Lett. 1998;50(3-4):125.
[25] Carja G, Delahay G, Signorile C, Coq B. Fe-Ce-ZSM-5 a new catalyst of outstanding properties in the selective catalytic reduction of NO with NH3. Chem Commun. 2004;10(12):1404.
[26] Smith LJ, Davidson A, Cheetham AK. A neutron diffraction and infrared spectroscopy study of the acid form of the aluminosilicate zeolite, chabazite(H-SSZ-13). Catal Lett. 1997;49(3-4):143.
[27] Fickel DW, D'Addio E, Lauterbach JA, Lobo RF. The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites. Appl Catal B. 2011;102(3-4):441.
[28] Jeon HY, Shin CH, Jung HJ, Hong SB. Catalytic evaluation of small-pore molecular sieves with different framework topologies for the synthesis of methylamines. Appl Catal A. 2006;305(1):70.
[29] Kwak JH, Tran D, Burton SD, Szanyi J, Lee JH, Peden CHF.Effects of hydrothermal aging on NH3-SCR reaction over Cu/zeolites. J Catal. 2012;287(3):203.
[30] Ren LM, Zhu LF, Yang CG, Chen YM, Sun Q, Zhang HY, Li CJ, Nawaz FS, Meng XJ, Xiao FS. Designed copper-amine complex as an efficient template for one-pot synthesis of Cu-SSZ-13 zeolite with excellent activity for selective catalytic reduction of NO_x by NH3. Chem Commun. 2011;47(35):9789.
[31] Xie LJ, Liu FD, Ren LM, Shi XY, Xiao FS, He H. Excellent performance of one-pot synthesized Cu-SSZ-13 catalyst for the selective catalytic reduction of NO_x with NH3. Environ Sci Technol. 2014;48(1):566.
[32] Korhonen ST, Fickel DW, Lobo RF, Weckhuysen BM, Beale AM. Isolated Cu~(2+)ions:active sites for selective catalytic reduction of NO. Chem Commun. 2011;47(2):800.
[33] Bates SA, Verma AA, Paolucci C, Parekh AA, Anggara T,Yezerets A, Schneider WF, Miller JT, Delgass WN, Ribeiro FH.Identification of the active Cu site in standard selective catalytic reduction with ammonia on Cu-SSZ-13. J Catal. 2014;312(15):87.
[34] Fickel DW, Lobo RF. Copper coordination in Cu-SSZ-13 and Cu-SSZ-16 investigated by variable-temperature XRD. J Phys Chem C. 2010;114(3):1633.
[35] Deka U, Lezcano-Gonzalez I, Warrender SJ, Picone AL, Wright PA, Weckhuysen BM, Beale AM. Changing active sites in Cu-CHA catalysts:deNOx selectivity as a function of the preparation method. Microporous Mesoporous Mater. 2013;166(166):144.
[36] Kim YJ, Kwon HJ, Heo I, Nam I, Cho BK, Choung JW, Cha M,Yeo GK. Mn-Fe/ZSM5 as a low-temperature SCR catalyst to remove NO_x from diesel engine exhaust. Appl Catal B. 2012;126:9.
[37] Treacy MMJ, Higgins JB. Collection of Simulated XRD Powder Patterns for Zeolites. 5th ed. Amsterdam:USA Elsevier; 2007.112.
[38] Ma L, Cheng YS, Cavataio GV, McCabe RW, Fu LX, Li JH.Characterization of commercial Cu-SSZ-13 and Cu-SAPO-34catalysts with hydrothermal treatment for NH3-SCR of NO_x in diesel exhaust. Chem Eng J. 2013;225(3):323.
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