Advertisement

Rare Metals

, Volume 38, Issue 3, pp 210–220 | Cite as

Catalytic activity of Cu–SSZ-13 prepared with different methods for NH3-SCR reaction

  • Meng-Jie Han
  • Yun-Lei Jiao
  • Chun-Hong Zhou
  • Yang-Long Guo
  • Yun Guo
  • Guan-Zhong Lu
  • Li Wang
  • Wang-Cheng ZhanEmail author
Article
  • 49 Downloads

Abstract

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 (NOx) 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 °C 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 Cu2+ 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 °C, but the activity of the former is much higher than that of the latter at > 400 °C due to the high activity of Cu–SSZ-13(IWI) catalyst for NH3 oxidation.

Graphical abstract

Three kinds of Cu–SSZ-13 with the same amount of Cu loading were prepared by different methods. The catalyst prepared by hydrothermal synthesis displayed the better NH3-SCR activity due to more isolated Cu2+ in six-membered ring of the CHA structure.

Keywords

SSZ-13 zeolite Selective catalytic reduction Nitrogen oxides Preparation method Cu2+ 

Notes

Acknowledgements

This work was financially supported by the National Key Research and Development Program of China (No. 2016YFC0204300), the National Natural Science Foundation of China (Nos. 21577034 and 21333003) and the Science and Technology Commission of Shanghai Municipality (No. 16ZR1407900).

References

  1. [1]
    Huang JW, Sun YH, Zhang YD, Zou GF, Yan CY, Cong S, Lei TY, Dai X, Guo J, Lu RF, Li YR, Xiong J. A new member of electrocatalysts based on nickel metaphosphate nanocrystals for efficient water oxidation. Adv Mater. 2018;30(5):1705045.Google Scholar
  2. [2]
    Huang JW, Li YR, Xia YF, Zhu JT, Yi QH, Wang H, Xiong J, Sun YH, Zou GF. Flexible cobalt phosphide network electrocatalyst for hydrogen evolution at all pH values. Nano Res. 2017;10(3):1010.Google Scholar
  3. [3]
    Burch R, Breen JP, Hill CJ, Krutzsch B, Konrad B, Jobson E, Cider L, Eranen K, Klingstedt F, Lindfors LE. Exceptional activity for NOx reduction at low temperatures using combinations of hydrogen and higher hydrocarbons on Ag/Al2O3 catalysts. Top Catal. 2004;30–31(1):19.Google Scholar
  4. [4]
    Han J, Meeprasert J, Maitarad P, Nammuangruk S, Shi LY, Zhang DS. Investigation of the facet-dependent catalytic performance of Fe2O3/CeO2 for the selective catalytic reduction of NO with NH3. J Phys Chem C. 2016;120(3):1523.Google Scholar
  5. [5]
    Gu L, Chen X, Zhou Y, Zhu QL, Huang HF, Lu HF. Propene and CO oxidation on Pt/Ce–Zr–SO42–diesel oxidation catalysts: effect of sulfate on activity and stability. Chin J Catal. 2017;38(3):607.Google Scholar
  6. [6]
    Gao RH, Zhang DS, Maitarad P, Shi LY, Rungrotmongkol T, Li HR, Zhang JP, Cao WG. Morphology-dependent properties of MnOx/ZrO2–CeO2 nanostructures for the selective catalytic reduction of NO with NH3. J Phys Chem C. 2013;117(20):10502.Google Scholar
  7. [7]
    Wan HQ, Li D, Dai Y, Hu YH, Liu B, Dong L. Catalytic behaviors of CuO supported on Mn2O3 modified γ-Al2O3 for NO reduction by CO. J Mol Catal A Chem. 2010;332(1–2):32.Google Scholar
  8. [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.Google Scholar
  9. [9]
    Liu FD, Shan WP, Pan DW, Li TY, He H. Selective catalytic reduction of NOx by NH3 for heavy-duty diesel vehicle. Chin J Catal. 2014;35(9):1438.Google Scholar
  10. [10]
    Meng DM, Zhan WC, Guo Y, Guo YL, Wang L, Lu GZ. A highly effective catalyst of Sm-MnOx for the NH3-SCR of NOx at low temperature: promotional role of Sm and its catalytic performance. ACS Catal. 2015;5:5973.Google Scholar
  11. [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 NOx with ammonia: effect of the calcination temperature. J Mol Catal A Chem. 2016;420:272.Google Scholar
  12. [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.Google Scholar
  13. [13]
    Yates M, Martin JA, Martin-Luengo MA, Suarez S, Blanco J. N2O formation in the ammonia oxidation and in the SCR process with V2O5-WO3 catalysts. Catal Today. 2005;107–108(15):120.Google Scholar
  14. [14]
    Krishnan AT, Boehman AL. Selective catalytic reduction of nitric oxide with ammonia at low temperatures. Appl Catal B. 1998;18(3–4):189.Google Scholar
  15. [15]
    Meng DM, Xu Q, Jiao YL, Guo Y, Guo YL, Wang L, Lu GZ, Zhan WC. Spinel structured CoaMnbOx mixed oxide catalyst for the selective catalytic reduction of NOx with NH3. Appl Catal B. 2018;221:652.Google Scholar
  16. [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.Google Scholar
  17. [17]
    Chen HY, Sachtler WMH. Activity and durability of Fe/ZSM-5 catalysts for lean burn NOx reduction in the presence of water vapor. Catal Today. 1998;42(1–2):73.Google Scholar
  18. [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 NOx with NH3: effect of the atmosphere during the preparation of catalysts. J Mol Catal A Chem. 2016;424:232.Google Scholar
  19. [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.Google Scholar
  20. [20]
    Weng XL, Dai XX, Zeng QS, Liu Y, Wu ZB. DRIFT studies on promotion mechanism of H3PW12O40 in selective catalytic reduction of NO with NH3. J Colloid Interface Sci. 2016;461:9.Google Scholar
  21. [21]
    Seo CK, Choi B, Kim H, Lee CH, Lee CB. Effect of ZrO2 addition on de-NOx performance of Cu-ZSM-5 for SCR catalyst. Chem Eng J. 2012;191(19):331.Google Scholar
  22. [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.Google Scholar
  23. [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 NOx with NH3. RSC Adv. 2015;5(110):90235.Google Scholar
  24. [24]
    Chen HY, Sachtler WMH. Promoted Fe/ZSM-5 catalysts prepared by sublimation: de-NOx activity and durability in H2O-rich streams. Catal Lett. 1998;50(3–4):125.Google Scholar
  25. [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.Google Scholar
  26. [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.Google Scholar
  27. [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.Google Scholar
  28. [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.Google Scholar
  29. [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.Google Scholar
  30. [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 NOx by NH3. Chem Commun. 2011;47(35):9789.Google Scholar
  31. [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 NOx with NH3. Environ Sci Technol. 2014;48(1):566.Google Scholar
  32. [32]
    Korhonen ST, Fickel DW, Lobo RF, Weckhuysen BM, Beale AM. Isolated Cu2+ ions: active sites for selective catalytic reduction of NO. Chem Commun. 2011;47(2):800.Google Scholar
  33. [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.Google Scholar
  34. [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.Google Scholar
  35. [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.Google Scholar
  36. [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 NOx from diesel engine exhaust. Appl Catal B. 2012;126:9.Google Scholar
  37. [37]
    Treacy MMJ, Higgins JB. Collection of Simulated XRD Powder Patterns for Zeolites. 5th ed. Amsterdam: USA Elsevier; 2007. 112.Google Scholar
  38. [38]
    Ma L, Cheng YS, Cavataio GV, McCabe RW, Fu LX, Li JH. Characterization of commercial Cu–SSZ-13 and Cu-SAPO-34 catalysts with hydrothermal treatment for NH3-SCR of NOx in diesel exhaust. Chem Eng J. 2013;225(3):323.Google Scholar
  39. [39]
    Ismagilov ZR, Yashnik SA, Anufrienko VF, Larina TV, Vasenin NT, Bulgakov NN, Vosel SV, Tsykoza LT. Linear nanoscale clusters of CuO in Cu-ZSM-5 catalysts. Appl Surf Sci. 2004;226(1–3):88.Google Scholar
  40. [40]
    Dedecek J, Wichterlova B. Role of hydrated Cu ion complexes and aluminum distribution in the framework on the Cu ion siting in ZSM-5. J Phys Chem B. 1997;101(49):10233.Google Scholar
  41. [41]
    Giordanino F, Vennestrom PNR, Lundegaard LF, Stappen FN, Mossin S, Beato P, Bordiga S, Lamberti C. Characterization of Cu-exchanged SSZ-13: a comparative FTIR, UV–Vis, and EPR study with Cu-ZSM-5 and Cu-β with similar Si/Al and Cu/Al ratios. Dalton Trans. 2013;42(35):12741.Google Scholar
  42. [42]
    Lezcano-Gonzalez I, Deka U, Bij HEVD, Paalanenb P, Arstad B, Weckhuysen BM, Beale AM. Chemical deactivation of Cu–SSZ-13 ammonia selective catalytic reduction (NH3-SCR) systems. Appl Catal B. 2014;154–155(1):339.Google Scholar
  43. [43]
    El-Trass A, El-Shamy H, El-Mehasseb I, El-Kemary M. CuO nanoparticles: synthesis, characterization, optical properties and interaction with amino acids. Appl Surf Sci. 2012;258(7):2997.Google Scholar
  44. [44]
    Zhang RR, Li YH, Zhen TL. Ammonia selective catalytic reduction of NO over Fe/Cu–SSZ-13. RSC Adv. 2014;4(94):52130.Google Scholar
  45. [45]
    Velu S, Suzuki K, Vijayaraj M, Barman S, Gopinath CS. In situ XPS investigations of Cu1–xNixZnAl-mixed metal oxide catalysts used in the oxidative steam reforming of bio-ethanol. Appl Catal B. 2005;55(4):287.Google Scholar
  46. [46]
    Figueiredo RT, Martınez-Arias A, Granados ML, Fierro JLG. Spectroscopic evidence of Cu–Al interactions in Cu–Zn–Al mixed oxide catalysts used in CO hydrogenation. J Catal. 1998;178(1):146.Google Scholar
  47. [47]
    Ghodselahi T, Vesaghi MA, Shafiekhani A, Baghizadeh A, Lameii M. XPS study of the Cu@Cu2O core–shell nanoparticles. Appl Surf Sci. 2008;255(5):2730.Google Scholar
  48. [48]
    Kim MH, Nam IS, Kim YG. Characteristics of mordenite-type zeolite catalysts deactivated by SO2 for the reduction of NO with hydrocarbons. J Catal. 1998;179(2):350.Google Scholar
  49. [49]
    Wagner CD. II. Standard ESCA Spectra of the Elements and Line Energy Information. In: Muilenberg GE, editor. Handbook of X-ray Photoelectron Spectroscopy, 1st edn. Waltham: Perkin-Elmer, Physical Electronics; 1979. 74.Google Scholar
  50. [50]
    Chadwick D, Hashemi T. Adsorbed corrosion inhibitors studied by electron spectroscopy: benzotriazole on copper and copper alloys. Corros Sci. 1978;18(1):39.Google Scholar
  51. [51]
    Zhang T, Li JM, Liu J, Wang DX, Zhao Z, Cheng K, Li JH. High activity and wide temperature window of Fe–Cu–SSZ-13 in the selective catalytic reduction of NO with ammonia. AIChE J. 2015;61(11):3825.Google Scholar
  52. [52]
    Richter M, Fait M, Eckelt R, Schneider M, Radnik J, Heidemann D, Fricke R. Gas-phase carbonylation of methanol to dimethyl carbonate on chloride-free Cu-precipitated zeolite Y at normal pressure. J Catal. 2007;245(1):11.Google Scholar
  53. [53]
    Kefirov R, Penkova A, Hadjiivanov K, Dzwigaj S, Che M. Stabilization of Cu+ ions in BEA zeolite: study by FTIR spectroscopy of adsorbed CO and TPR. Microporous Mesoporous Mater. 2008;116(1–3):180.Google Scholar
  54. [54]
    Kwak JH, Zhu HH, Lee JH, Peden CHF, Szanyi J. Two different cationic positions in Cu–SSZ-13. Chem Commun. 2012;48(39):4758.Google Scholar
  55. [55]
    Cao Y, Zou S, Lan L, Yang ZZ, Xu HD, Lin T, Gong MC, Chen YG. Promotional effect of Ce on Cu-SAPO-34 monolith catalyst for selective catalytic reduction of NOx with ammonia. J Mol Catal A Chem. 2015;398:304.Google Scholar
  56. [56]
    Kim DJ, Wang J, Crocker M. Adsorption and desorption of propene on a commercial Cu–SSZ-13 SCR catalyst. Catal Today. 2014;231(4):83.Google Scholar
  57. [57]
    Deka U, Lezcano-Gonzalez I, Weckhuysen BM, Beale AM. Local environment and nature of Cu active sites in zeolite-based catalysts for the selective catalytic reduction of NOx. ACS Catal. 2013;3(3):413.Google Scholar
  58. [58]
    Sultana A, Sasaki M, Suzuki K, Hamada H. Tuning the NOx conversion of Cu–Fe/ZSM-5 catalyst in NH3-SCR. Catal Commun. 2013;41(21):21.Google Scholar
  59. [59]
    Ye Q, Wang LF, Yang RT. Activity, propene poisoning resistance and hydrothermal stability of copper exchanged chabazite-like zeolite catalysts for SCR of NO with ammonia in comparison to Cu/ZSM-5. Appl Catal A. 2012;427–428(1):24.Google Scholar
  60. [60]
    Rodríguez-González R, Hermes F, Bertmer M, Rodríguez Castellón E, Jiménez-López A, Simon U. The acid properties of H-ZSM-5 as studied by NH3-TPD and 27 Al-MAS-NMR spectroscopy. Appl Catal A. 2007;328(2):174.Google Scholar
  61. [61]
    Wang D, Jangjou Y, Liu Y, Sharma MK, Luo JY, Li JH, Kamasamudram K, Epling WS. A comparison of hydrothermal aging effects on NH3-SCR of NOx over Cu–SSZ-13 and Cu-SAPO-34 catalysts. Appl Catal B. 2015;165:438.Google Scholar
  62. [62]
    Wang J, Yu T, Wang X, Qi G, Xue J, Shen M, Li W. The influence of silicon on the catalytic properties of Cu/SAPO-34 for NOx reduction by ammonia-SCR. Appl Catal B. 2012;127(43):137.Google Scholar
  63. [63]
    Olsson L, Wijayanti K, Leistner K, Kumar A, Joshi SY, Kamasamudram K, Currier NW, Yezeretsb A. A multi-site kinetic model for NH3-SCR over Cu/SSZ-13. Appl Catal B Environ. 2015;174–175:212.Google Scholar
  64. [64]
    Despres J, Koebel M, Krocher O, Elsener M, Wokaun A. Adsorption and desorption of NO and NO2 on Cu-ZSM-5. Microporous Mesoporous Mater. 2003;58(2):175.Google Scholar
  65. [65]
    Lisi L, Pirone R, Russo G, Santamaria N, Stanzione V. Nitrates and nitrous oxide formation during the interaction of nitrogen oxides with Cu-ZSM-5 at low temperature. Appl Catal A. 2012;413–414(1):117.Google Scholar
  66. [66]
    Landi G, Lisi L, Pirone R, Russo G, Tortorelli M. Effect of water on NO adsorption over Cu-ZSM-5 based catalysts. Catal Today. 2012;191(1):138.Google Scholar
  67. [67]
    Gao F, Walter ED, Karp EM, Luo J, Tonkyn RG, Kwak JH, Szanyi J, Peden CHF. Structure-activity relationships in NH3-SCR over Cu–SSZ-13 as probed by reaction kinetics and EPR studies. J Catal. 2013;300(3):20.Google Scholar
  68. [68]
    Chen BH, Xu RN, Zhang RD, Liu N. An economical way to synthesize SSZ-13 with abundant ion-exchanged Cu+ for an extraordinary performance in selective catalytic reduction (SCR) of NOx by ammonia. Environ Sci Technol. 2014;48(23):13909.Google Scholar
  69. [69]
    Brandenberger S, Kröchera O, Wokaun A, Tissler A, Althoff R. The role of Brønsted acidity in the selective catalytic reduction of NO with ammonia over Fe-ZSM-5. J Catal. 2009;268(2):297.Google Scholar

Copyright information

© The Nonferrous Metals Society of China and Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  1. 1.Key Laboratory for Advanced Materials and Research Institute of Industrial CatalysisEast China University of Science and TechnologyShanghaiChina

Personalised recommendations