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Catalytic Performance and Characterization of Ce-Modified Fe Catalysts Supported on Al2O3 for SCR-C3H8

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Abstract

In order to further improve the resistance of the catalysts to H2O and SO2 during the selective catalytic reduction of NO with C3H8 (SCR-C3H8), Ce was used to modify the Fe-based catalysts. Sol–gel and impregnation methods were adopted to prepare the monolithic cordierite Ce–Fe/Al2O3 catalysts and the SCR-C3H8 testes were carried out in a flow reactor, electrically heated up to 600 °C, and with simulated a flue gas rate of 1.5 L/min. The physical chemical properties of the catalysts were characterized by XRD, N2 adsorption–desorption, SEM, H2-TPR and FT-IR spectra of adsorbed pyridine, etc. Results show that the introduction of Cerium notably enhances the resistance of the Fe/Al2O3/Cordierite catalysts to SO2. 3.5Ce–Fe/Al2O3/Cordierite has the highest C3H8-SCR activity, e.g., the NO reductions are 96.5% and 93% at 600 °C when there was no and 0.02% SO2 in the flue gas, respectively. While the NO reduction by Fe/Al2O3/Cordierite decreased from 88 to 80% in the presence of 0.02% SO2. The addition of Cerium to iron oxide leads to an increase in the Lewis acid sites and the redox property of the catalysts. However, an overload of cerium will reduce the crystallinity of iron oxide nanorods and inhibit the formation of the NO2/NO3− species in the C3H8-SCR reaction, resulting in a decrease in the NO reduction.

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References

  1. Richter A, Burrows JP, Nüss H, Granier C, Niemeir U (2005) Increase in tropospheric nitrogen dioxide over China observed from space. Nature 437:129–132

    CAS  PubMed  Google Scholar 

  2. Liu F, Shan W, Shi X, He H (2012) Vanadium-based catalysts for the selective catalytic reduction of NOx with NH3. Prog Chem 24:445–455

    Google Scholar 

  3. Iwamoto M (1990) Selective reduction of NO by lower hydrocarbons in the presence of O2 and SO2 over copper ion-exchanged zeolites. Catalyst 32:430–433

    CAS  Google Scholar 

  4. Held W, König A, Richter T, Puppe L (1990) Catalytic NOx reduction in net oxidizing exhaust gas. SAE Trans 99:209–216

    Google Scholar 

  5. Rivallan M, Berlier G, Ricchiardi G, Zecchina A, Nechita MT, Olsbye U (2008) Characterisation and catalytic activity in de-NOx reactions of Fe-ZSM-5 zeolites prepared via ferric oxalate precursor. Appl Catal B 84:204–213

    CAS  Google Scholar 

  6. Shi Y, Pan H, Zhang Y, Li W (2008) Promotion of MgO addition on SO2 tolerance of Ag/Al2O3 for selective catalytic reduction of NOx with methane at low temperature. Catal Commun 9:796–800

    CAS  Google Scholar 

  7. Miyahara Y, Takahashi M, Masuda T, Imamura S, Kanai H, Iwamoto S, Watanabe T, Inoue M (2008) Selective catalytic reduction of NO with C1–C3 reductants over solvothermally prepared Ga2O3-Al2O3 catalysts: effects of water vapor and hydrocarbon uptake. Appl Catal B 84:289–296

    CAS  Google Scholar 

  8. Yang T, Bi H, Cheng X (2011) Effects of O2, CO2 and H2O on NOx adsorption and selective catalytic reduction over Fe/ZSM-5. Appl Catal B 102:163–171

    CAS  Google Scholar 

  9. Li L, Guan N (2009) HC-SCR reaction pathways on ion exchanged ZSM-5 catalysts. Microporous Mesoporous Mater 117:450–457

    CAS  Google Scholar 

  10. Zhou H, Su Y, Deng W, Zhong F (2015) A review of HC-SCR over metal-based zeolite catalysts. Envir Sci Tech 38:64–73

    CAS  Google Scholar 

  11. Zhou H, Su Y, Deng W, Zhong F (2016) A review of HC-SCR over metal oxides-based catalysts. Envir Sci Tech 39:93–100

    CAS  Google Scholar 

  12. Shimizu K, Satsuma A, Hattori T (2000) Catalytic performance of Ag-Al2O3 catalyst for the selective catalytic reduction of NO by higher hydrocarbons. Appl Catal B 25:239–247

    CAS  Google Scholar 

  13. Satsuma A, Shimizu K (2003) In situ FT/IR study of selective catalytic reduction of NO over alumina-based catalysts. Prog Energy Combust 29:71–84

    CAS  Google Scholar 

  14. Kumar PA, Reddy MP, Ju LK, Hyun-Sook B, Phil HH (2008) Low temperature propylene SCR of NO by copper alumina catalyst. J Mol Catal A 291:66–74

    CAS  Google Scholar 

  15. Long QN, Salim C, Hinode H (2008) Performance of nano-sized Au/TiO2 for selective catalytic reduction of NOx by propene. Appl Catal A 347:94–99

    Google Scholar 

  16. Baidya T, Gupta A, Deshpandey PA, Madras G, Hegde MS (2009) High oxygen storage capacity and high rates of CO oxidation and NO reduction catalytic properties of Ce1−xSnxO2 and Ce0.78Sn0.2Pd0.02O2-δ. J Phys Chem C 113:4059–4068

    CAS  Google Scholar 

  17. Narasimharao K, Malik MA, Mokhtar MM, Basahel SN, Al-Thabaiti SA (2014) Iron oxide supported sulfated TiO2 nanotube catalysts for NO reduction with propane. Ceram Int 40:4039–4053

    CAS  Google Scholar 

  18. Gradoń B, Lasek J (2010) Investigations of the reduction of NO to N2 by reaction with Fe. Fuel 89:3505–3509

    Google Scholar 

  19. Su Y, Su A, Cheng H (2013) Experimental study on direct catalytic reduction of NO by metallic iron. J China Coal Soc 38(s1):206–210

    CAS  Google Scholar 

  20. Su Y, Lu Z, Zhou H, Dou Y, Deng W (2014) Experimental study on NO reduction by propane over iron. J Fuel Chem Technol 42:1470–1477

    CAS  Google Scholar 

  21. Su Y, Ren L, Su A, Deng W (2013) NO reduction by mathane over irons oxides and the mechanism. J Fuel Chem Technol 41:1129–1135

    CAS  Google Scholar 

  22. Dou Y, Su Y, Lu Z, Zhou H, Deng W (2015) Experimental study of NO reduction by ethane over iron. J Fuel Chem Technol 10:1273–1280

    Google Scholar 

  23. Su Y, Su A, Ren L, Deng W (2014) Effect of SO2 on the reduction of NO by methane over iron catalyst. J Fuel Chem Technol 42:377–384

    CAS  Google Scholar 

  24. Zhou H, Su Y, Su A, Qi Y, Deng W (2014) Effect of water vapor on NO reduction by methane over iron. J Fuel Chem Technol 42:1377–1386

    Google Scholar 

  25. Zhou H, Su Y, Liao W, Deng W, Zhong F (2015) Preparation, characterization, and properties of monolithic Fe/Al2O3/cordierite catalysts for NO reduction with C2H6. Appl Catal A 505:402–409

    CAS  Google Scholar 

  26. Zhou H, Su Y, Liao W, Deng W, Zhong F (2016) NO reduction by propane over monolithic cordierite-based Fe/Al2O3 catalyst: reaction mechanism and effect of H2O/SO2. Fuel 182:352–360

    CAS  Google Scholar 

  27. Qiu L, Meng J, Pang D, Zhang C, Ouyang F (2015) Reaction and characterization of Co and Ce Doped Mn/TiO2 catalysts for low-temperature SCR of NO with NH3. Catal Lett 145:1500–1509

    CAS  Google Scholar 

  28. Mendes AN, Zholobenko VL, Thibault-Starzyk F, Costa PD, Henriques C (2016) On the enhancing effect of Ce in Pd-MOR catalysts for NOx CH4-SCR: a structure-reactivity study. Appl Catal B 195:121–131

    CAS  Google Scholar 

  29. Wang M, Wang L, Liu J, Fei Z, Chen X, Tang J, Cui M, Qiao X (2017) Promoting effect of transition metal on low-temperature deNOx activity of CeO2@TiO2 catalyst for selective catalytic reduction. J Fuel Chem Technol 45:497–504

    CAS  Google Scholar 

  30. Shan W, Liu F, Yu Y, He H (2014) THe use of ceria for the selective catalytic reduction of NOx with NH3. Chin J Catal 35:1251–1259

    CAS  Google Scholar 

  31. Wu Z, Jin R, Wang H, Liu Y (2009) Effect of ceria doping on SO2 resistance of Mn/TiO2 for selective catalytic reduction of NO with NH3 at low temperature. Catal Commun 10:935–939

    CAS  Google Scholar 

  32. Carja G, Kameshima Y, Okada K, Madhusoodana CD (2007) Mn–Ce/ZSM5 as a new superior catalyst for NO reduction with NH3. Appl Catal B 73:60–64

    CAS  Google Scholar 

  33. Perez-Alonso FJ, Melián-Cabrera I, Granados ML, Kapteijn F, Fierro JLG (2006) Synergy of FexCe1−xO2 mixed oxides for N2O decomposition. J Catal 239:340–346

    CAS  Google Scholar 

  34. Joyner RW, Stockkenhuber M (1997) Unusual structure and stability of iron-oxygen nano-clusters in Fe-ZSM-5 catalysts. Catal Lett 45:15–19

    CAS  Google Scholar 

  35. Yang Q (2011) Low temperature selective catalytic reduction of NOx over Ce modified FeMnOx catalysts. South China University of Technology.

  36. González-Velasco JR, Ferret R, López-Fonseca R, Gutiérrez-Ortiz MA (2005) Influence of particle size distribution of precursor oxides on the synthesis of cordierite by solid-state reaction. Powder Technol 153:34–42

    Google Scholar 

  37. Chen Y (2009) Study on low-temperature selective catalytic reduction of NOx in flue gas by CeO2-Fe2O3/ACF catalyst. Hunan University.

  38. Bao H, Chen X, Fang J, Jiang Z, Huang W (2008) Structure-activity relation of Fe2O3-CeO2 composite catalysts in CO Oxidation. Catal Lett 125:160–167

    CAS  Google Scholar 

  39. Xin Q (2009) Modern catalytic research methods. Science Press, New York

    Google Scholar 

  40. Xiong Z, Lu C (2013) Study on the modification of iron-cerium mixed oxide catalyst for selective reduction of NO. J Fuel Chem Technol 41:361–367

    CAS  Google Scholar 

  41. Zhang Y, Liu F, Zhang J (2010) Structure-activity relationship of iron titanate catalysts in the selective catalytic reduction of NOx with NH3. J Phys Chem C 114:16929–16936

    Google Scholar 

  42. Su J, Liu Q, Liu Z, Huang Z (2008) Honeycomb CuO/Al2O3/cordierite catalyst for selective catalytic reduction of NO by NH3-Effect of Al2O3 coating. Ind Eng Chem Res 47:4295–4301

    CAS  Google Scholar 

  43. Liu Q, Liu Z, Wu W (2009) Effect of V2O5 additive on simultaneous SO2 and NO removal from flue gas over a monolithic cordierite-based CuO/Al2O3 catalyst. Catal Today 147:S285–S289

    CAS  Google Scholar 

  44. Zieliński J, Zglinicka I, Znak L, Kaszkur Z (2010) Reduction of Fe2O3 with hydrogen. Appl Catal A-Gen 381:191–196

    Google Scholar 

  45. Jozwiak WK, Kaczmarek E, Maniecki TP, Ignaczak W, Maniukiewicz W (2007) Reduction behavior of iron oxides in hydrogen and carbon monoxide atmospheres. Appl Catal A 326:17–27

    CAS  Google Scholar 

  46. Wang HL, Jin BF, Wang HB (2018) Study of Ag promoted Fe2O3@CeO2 as superior soot oxidation catalysts: the role of Fe2O3 crystal plane and tandem oxygen delivery. Appl Catal B 237:251–262

    CAS  Google Scholar 

  47. Wang X, Jin BF, Feng RX (2019) A robust core-shell silver soot oxidation catalyst driven by Co3O4: effect of tandem oxygen delivery and Co3O4-CeO2synergy. Appl Catal B 250:132–142

    CAS  Google Scholar 

  48. Qi G, Yang RT, Chang R (2004) MnOx-CeO2 mixed oxides prepared by co-precipitation for selective catalytic reduction of NO with NH3 at low temperatures. Appl Catal B 51:93–106

    CAS  Google Scholar 

  49. Wu Z, Jin R, Liu Y, Wang H (2008) Ceria modified MnOx/TiO2 as a superior catalyst for NO reduction with NH3 at low-temperature. Catal Commun 9:2217–2220

    CAS  Google Scholar 

  50. Li N, Wang A, Zheng M, Wang X, Cheng R, Zhang T (2004) Probing into the catalytic nature of Co/sulfated zirconia for selective reduction of NO with methane. J Catal 225:307–315

    CAS  Google Scholar 

  51. Liu J, Li X, Zhao Q, Zhang D, Ndokoye P (2013) The selective catalytic reduction of NO with propene over Cu-supported Ti–Ce mixed oxide catalysts: promotional effect of ceria. J Mol Catal A 378:115–123

    CAS  Google Scholar 

  52. Jagtap N, Umbarkar SB, Miquel P, Granger P, Dongare MK (2009) Support modification to improve the sulphur tolerance of Ag/Al2O3 for SCR of NOx with propene under lean-burn conditions. Appl Catal B 90:416–425

    CAS  Google Scholar 

  53. Jing G, Li J, Yang D, Hao J (2009) Promotional mechanism of tungstation on selective catalytic reduction of NOx by methane over In/WO3/ZrO2[J]. Appl Catal B 91:123–134

    CAS  Google Scholar 

  54. Peña DA, Uphade BS, Smirniotis PG (2004) TiO2-supported metal oxide catalysts for low-temperature selective catalytic reduction of NO with NH3: I. Evaluation and characterization of first row transition metals. J Catal 221:421–431

    Google Scholar 

  55. Yuan D, Li X, Zhao Q, Zhao J, Tadé M, Liu S (2014) A novel CuTi-containing catalyst derived from hydrotalcite-like compounds for selective catalytic reduction of NO with C3H6 under lean-burn conditions. J Catal 309:268–279

    CAS  Google Scholar 

  56. Méndez M, Cedillo A (2013) Gas phase Lewis acidity and basicity scales for boranes, phosphines and amines based on the formation of donor–acceptor complexes. Comput Theor Chem 1011:44–56

    Google Scholar 

  57. Li J, Zhu Y, Rrui K, Hao J (2008) Improvement of catalytic activity and sulfur-resistance of Ag/TiO2–Al2O3 for NO reduction with propene under lean burn conditions. Appl Catal B 80:202–213

    CAS  Google Scholar 

  58. Zhou H, Li K, Zhao B, Deng W, Su Y, Zhong F (2017) Surface properties and reactivity of Fe/Al2O3/cordierite catalysts for NO reduction by C2H6: effects of calcination temperature. Chem Eng J 326:737–744

    CAS  Google Scholar 

  59. Fierro G, Moretti G, Ferraris G, Andreozzi GB (2011) A Mössbauer and structural investigation of Fe-ZSM-5 catalysts: Influence of Fe oxide nanoparticles size on the catalytic behaviour for the NO-SCR by C3H8. Appl Catal B 102:215–223

    CAS  Google Scholar 

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Acknowledgements

The work was sponsored by Natural Science Foundation of Shanghai (No. 19ZR1401800), which is gratefully acknowledged.

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  1. School of Environmental Science and Engineering, Donghua University, Shanghai, 201620, China

    Fengguo Tian, Kangkai Li & Yaxin Su

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Tian, F., Li, K. & Su, Y. Catalytic Performance and Characterization of Ce-Modified Fe Catalysts Supported on Al2O3 for SCR-C3H8. Catal Surv Asia 24, 239–249 (2020). https://doi.org/10.1007/s10563-020-09306-4

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