Citation: MENG Peng-tong, FAN Chao, LÜ Wen-ting, WU Zhi-wei, JIAO Wei-yong, LI Jun-fen, QIN Zhang-feng, FAN Wei-bin, WANG Jian-guo. Preparation of monolithic cordierite supported Cu-SSZ-13 catalyst and its performance in the selective catalytic reduction of NO_x with NH₃[J]. Journal of Fuel Chemistry and Technology, ;2020, 48(10): 1216-1223. shu

Preparation of monolithic cordierite supported Cu-SSZ-13 catalyst and its performance in the selective catalytic reduction of NO_x with NH₃

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: LI Jun-fen, lijunfen@sxicc.ac.cn QIN Zhang-feng, qzhf@sxicc.ac.cn
Received Date: 9 July 2020
Revised Date: 8 August 2020

Fund Project: The Strategic Program of Coal-based Technology of Shanxi Province of China MQ2014-10The project was supported by the Strategic Program of Coal-based Technology of Shanxi Province of China ( MQ2014-11, MQ2014-10) and the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21020500).The Strategic Program of Coal-based Technology of Shanxi Province of China MQ2014-11The Strategic Priority Research Program of the Chinese Academy of Sciences XDA21020500

Figures(6)

A series of monolithic cordierite supported Cu-SSZ-13 catalysts (Cu-SSZ-13/Cordierite) was prepared by coating the Cu-SSZ-13 molecular sieves on the cellular cordierite through ultrasonic dispersion with polyvinyl alcohol (PVA) or pseudo boehmite powder (SB) as assisting agent and used in the selective catalytic reduction of NO_x with NH₃ (NH₃-SCR). With the help of XRD, nitrogen sorption, SEM and H₂-TPR characterization techniques, the influence of coating assistant agent on the firmness of the Cu-SSZ-13 layer, catalytic activity in the NH₃-SCR of NO, hydrothermal stability and resistance against SO₂ poisoning was then investigated. The results indicate that by using PVA as the coating assistant agent, a firm layer of Cu-SSZ-13 can be formed on the surface of monolithic Cu-SSZ-13/Cordierite catalyst. Moreover, the Cu-SSZ-13(PVA)/Cordierite exhibits high catalytic activity in the NH₃-SCR of NO_x (close to that of the pristine Cu-SSZ-13 molecular sieve), high hydrothermal stability and good tolerance to SO₂, displaying great potential as a practicable catalyst for the removal of NO_x from exhausts of both the mobile and the stationary sources.
- Cu-SSZ-13,
- cordierite,
- monolithic catalyst,
- selective catalytic reduction of NO_x with NH₃,
- denitrification
1. [1]
  BOSCH H, JANSSEN F. Formation and control of nitrogen oxides[J]. Catal Today, 1988,2(4):369-379.
2. [2]
  HERNÁNDEZ-GIMÉNEZ A M, LOZANO-CASTELLÓ D, BUENO-LÓPEZ A. Effect of CO₂, H₂O and SO₂ in the ceria-catalyzed combustion of soot under simulated diesel exhaust conditions[J]. Appl Catal B:Environ, 2014,148-149:406-414.
3. [3]
  LIU Xiao-wen, LI Jun, LI Jia-xing, NI Zhong-xiao, YI Xiu-le, LU Xin. Overview of flue gas denitrification technology[J]. Guangzhou Chem Ind (China), 2019,47(24):53-55.
4. [4]
  QI G, YANG R, RINALDI F. Selective catalytic reduction of nitric oxide with hydrogen over Pd-based catalysts[J]. J Catal, 2006,237(2):381-392.
5. [5]
  LI J, CHANG H, MA L, HAO J, YANG R T. Low-temperature selective catalytic reduction of NO_x with NH₃ over metal oxide and zeolite catalysts-A review[J]. Cataly Today, 2011,175(1):147-156.
6. [6]
  BRANDENBERGER S, KRÖCHER O, TISSLER A, ALTHOFF R. The state of the art in selective catalytic reduction of NO_x by ammonia using metal-exchanged zeolite catalysts[J]. Catal Rev-Sci Eng, 2008,50(4):492-531.
7. [7]
  BONINGARI T, KOIRALA R, SMIRNIOTIS P G. Low-temperature selective catalytic reduction of NO with NH₃ over V/ZrO₂ prepared by flame-assisted spray pyrolysis:Structural and catalytic properties[J]. Appl Catal B:Environ, 2012,127:255-264.
8. [8]
  CHEN Z, YANG Q, LI H, LI X, WANG L, CHI TSANG S. Cr-MnO_x mixed-oxide catalysts for selective catalytic reduction of NO_x with NH₃ at low temperature[J]. J Catal, 2010,276(1):56-65.
9. [9]
  SCHNEIDER H, MACIEJEWSKI M, KOHLER K, WOKAUN A, BAIKER A. Chromia supported on titania:ⅣProperties of different chromium oxide phases in the catalytic reduction of no by NH₃ studied by in situ diffuse reflectance FTIR spectroscopy[J]. J Catal, 1995,157:312-320.
10. [10]
  SMIRNIOTIS P G, PENÃ D A, UPHADE B S. Low-temperature selective catalytic reduction (SCR) of NO with NH₃ by using Mn, Cr, and Cu oxides supported on hombikat TiO₂[J]. Angew Chem Int Ed, 2001,40(13):2479-2482.
11. [11]
  XIN Y, LI Q, ZHANG Z. Zeolitic materials for DeNO_x selective catalytic reduction[J]. ChemCatChem, 2018,10(1):29-41.
12. [12]
  CHEN L, LI J, GE M. DRIFT study on cerium-tungsten titiania catalyst for selective catalytic reduction of NO_x with NH₃[J]. Environ Sci Technol, 2010,44(24):9590-9596.
13. [13]
  LIU F, ASAKURA K, HE H, SHAN W, SHI X, ZHANG C. Influence of sulfation on iron titanate catalyst for the selective catalytic reduction of NO_x with NH₃[J]. Appl Catal B:Environ, 2011,103(3/4):369-377.
14. [14]
  ZHU Q, KONDO J N, OHNUMA R, KUBOTA Y, YAMAGUCHI M, TATSUMI T. The study of methanol-to-olefin over proton type aluminosilicate CHA zeolites[J]. Microporous Mesoporous Mater, 2008,112(1/3):153-161.
15. [15]
  BLEKEN F, BJØRGEN M, PALUMBO L, BORDIGA S, SVELLE S, LILLERUD K-P, OLSBYE U. The effect of acid strength on the conversion of methanol to olefins over acidic microporous catalysts with the CHA topology[J]. Top Catal, 2009,52(3):218-228.
16. [16]
  FICKEL D W, LOBO R F. Copper coordination in Cu-SSZ-13 and Cu-SSZ-16 investigated by variable-temperature XRD[J]. J Phys Chem C, 2010,114(3):1633-1640.
17. [17]
  DEKA U, JUHIN A, EILERTSEN E A, EMERICH H, GREEN M A, KORHONEN S T, WECKHUYSEN B M, BEALE A M. Confirmation of isolated Cu²⁺ ions in SSZ-13 zeolite as active sites in NH₃-selective catalytic reduction[J]. J Phys Chem C, 2012,116(7):4809-4818.
18. [18]
  FICKEL D W, D'ADDIO E, LAUTERBACH J A, LOBO R F. The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites[J]. Appl Catal B:Environ, 2011,102(3/4):441-448.
19. [19]
  BOGER T, HEIBEL A K, SORENSEN C M. Monolithic catalysts for the chemical industry[J]. Ind Eng Chem Res, 2004,43(16):4602-4611.
20. [20]
  LIU Q, LIU Z, WU W. Effect of V₂O₅ additive on simultaneous SO₂ and NO removal from flue gas over a monolithic cordierite-based CuO/Al₂O₃ catalyst[J]. Catal Today, 2009,147S:S285-S289.
21. [21]
  ZONES S I. Zeolite SSZ-13 and its method of preparation: US, 4544538[P]. 1985.
22. [22]
  FAN Chao, LUO Li, WU Zhi-wei, ZHU Hua-qing, QIN Zhang-feng. Preparation of monolithic Pd/ZSM-5/Cordierite catalyst for the combustion of lean methane[J]. J Shaanxi Normal Univ (Nat Sci Ed), 2019,47(1):94-100.
23. [23]
  HE D, WANG Z, DENG D, DENG S, HE H, LIU L. Synthesis of Cu-SSZ-13 catalyst by using different silica sources for NO-SCR by NH₃[J]. Mol Catal, 2020,484110738.
24. [24]
  WANG Y, XIE L, LIU F, RUAN W. Effect of preparation methods on the performance of CuFe-SSZ-13 catalysts for selective catalytic reduction of NO_x with NH₃[J]. J Environ Sci, 2019,81:195-204. doi: 10.1016/j.jes.2019.01.013
25. [25]
  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]. J Catal, 2007,245(1):11-24.
26. [26]
  GAO F, WALTER E D, KARP E M, LUO J, TONKYN R G, KWAK J H, SZANYI J, PEDEN C H F. Structure-activity relationships in NH₃-SCR over Cu-SSZ-13 as probed by reaction kinetics and EPR studies[J]. J Catal, 2013,300:20-29. doi: 10.1016/j.jcat.2012.12.020
27. [27]
  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[J]. Microporous Mesoporous Mater, 2008,116(1/3):180-187.
28. [28]
  LIU Shi-cheng, QIN Rui-xiang, XIAO Rui, ZHANG Chun-xue, WANG Dan, LIU Tong, WANG Jin-bo. NH₃-SCR reaction of nitrogen oxides catalyzed by Cu-based ZSM-5 zeolite[J]. J Chongqing Univ Sci Technol(Nat Sci Ed), 2019,21(5):108-111.
29. [29]
  DOU B, LV G, WANG C, HAO Q, HUI K. Cerium doped copper/ZSM-5 catalysts used for the selective catalytic reduction of nitrogen oxide with ammonia[J]. Chem Eng J, 2015,270:549-556. doi: 10.1016/j.cej.2015.02.004
30. [30]
  SULTANA A, SASAKI M, SUZUKI K, HAMADA H. Tuning the NO_x conversion of Cu-Fe/ZSM-5 catalyst in NH₃-SCR[J]. Catal Commun, 2013,41:21-25. doi: 10.1016/j.catcom.2013.06.028
31. [31]
  SJÖVALL H, OLSSON L, FRIDELL E, BLINT R J. Selective catalytic reduction of NO_x with NH₃ over Cu-ZSM-5-The effect of changing the gas composition[J]. Appl Catal B:Environ, 2006,64:180-188.
32. [32]
  WANG C, WANG C, WANG J, WANG J, SHEN M, LI W. Effects of Na⁺ on Cu/SAPO-34 for ammonia selective catalytic reduction[J]. J Environ Sci, 2018,70:20-28.
33. [33]
  XIE K, LEISTNER K, WIJAYANTI K, KUMAR A, KAMASAMUDRAM K, OLSSON L. Influence of phosphorus on Cu-SSZ-13 for selective catalytic reduction of NO_x by ammonia[J]. Catal Today, 2017,297:46-52.
34. [34]
  HAMMERSHØI P S, JANGJOU Y, EPLING W S, JENSEN A D, JANSSENS T V W. Reversible and irreversible deactivation of Cu-CHA NH₃-SCRcatalysts by SO₂ and SO₃[J]. Appl Catal B:Environ, 2018,226:38-45.
35. [35]
  HAMMERSHØI P S, VENNESTRØM P N R, FALSIG H, JENSEN A D, JANSSENS T V W. Importance of the Cu oxidation state for the SO₂-poisoning of a Cu-SAPO-34 catalyst in the NH₃-SCR reaction[J]. Appl Catal B:Environ, 2018,236:377-383.
36. [36]
  JANGJOU Y, DO Q, GU Y, LIM L-G, SUN H, WANG D, KUMAR A, LI J, GRABOW L C, EPLING W S. Nature of Cu active centers in Cu-SSZ-13 and their responses to SO₂ exposure[J]. ACS Catal, 2018,8(2):1325-1337.
37. [37]
  ZHANG L, WANG D, LIU Y, KAMASAMUDRAM K, LI J, EPLING W. SO₂ poisoning impact on the NH₃-SCR reaction over a commercial Cu-SAPO-34 SCR catalyst[J]. Appl Catal B:Environ, 2014,156-157:371-377.
38. [38]
  JANGJOU Y, WANG D, KUMAR A, LI J, EPLING W S. SO₂ poisoning of the NH₃-SCR reaction over Cu-SAPO-34:Impact of ammonium sulfate versus other S-containing species[J]. ACS Catal, 2016,6(10):6612-6622.
39. [39]
  FERRIZZ R M, GORTE R J, VOHS J M. TPD and XPS investigation of the interaction of SO₂ with model ceria catalysts[J]. Catal Lett, 2002,82:123-129. doi: 10.1023/A:1020512713021
40. [40]
  KONG L, ZOU S, MEI J, GENG Y, ZHAO H, YANG S. Outstanding resistance of H₂S-modified Cu/TiO₂ to SO₂ for capturing gaseous Hg(0) from nonferrous metal smelting flue gas:Performance and reaction mechanism[J]. Environ Sci Technol, 2018,52(17):10003-10010.
41. [41]
  THEGE I K. DSC investigation of the thermal behaviour of (NH₄)₂SO₄, NH₄HSO₄ and NH₄NH₂SO₃[J]. Thermochim Acta, 1983,60(2):149-159.
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沈阳化工大学材料科学与工程学院沈阳 110142

Preparation of monolithic cordierite supported Cu-SSZ-13 catalyst and its performance in the selective catalytic reduction of NOx with NH3

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通讯作者: 陈斌, bchen63@163.com

Preparation of monolithic cordierite supported Cu-SSZ-13 catalyst and its performance in the selective catalytic reduction of NO_x with NH₃