Citation: WANG Dong, WU Jing-kun, NIU Sheng-li, LU Chun-mei, XU Li-ting, YU He-wei, LI Jing. Structural property of γ-Fe₂O₃ catalysts doped with Sn and Ti and their activity in the selective catalytic reduction of NO_x[J]. Journal of Fuel Chemistry and Technology, ;2015, 43(7): 876-883. shu

Structural property of γ-Fe₂O₃ catalysts doped with Sn and Ti and their activity in the selective catalytic reduction of NO_x

WANG Dong ^1,2 ,
WU Jing-kun ¹ ,
NIU Sheng-li ^1,2 ,
LU Chun-mei ^1,2,, ,
XU Li-ting ^1,2 ,
YU He-wei ¹ ,
LI Jing ³

1.
1. School of Energy and Power Engineering, Shandong University, Jinan 250061, China;

Corresponding author: LU Chun-mei,
Received Date: 10 May 2015
Available Online: 26 June 2015
Fund Project: 国家自然科学基金(51276101) (51276101) 高等学校博士学科点专项科研基金(20120131110022) (20120131110022) 山东大学基本科研业务费专项资金(2015JC024)。 (2015JC024)

A series of γ-Fe₂O₃ catalysts doped with Sn and Ti (γ-Fe_0.95Ti_0.05O_z, γ-Fe_0.95Sn_0.05O_z, and γ-Fe_0.95Sn_0.025Ti_0.025O_z) were prepared by the microwave assisted co-precipitation method. The crystal phase, pore structure, surface element distribution and microscopic morphology of the doped γ-Fe₂O₃ catalysts were characterized by X-ray diffraction (XRD), N₂ sorption, energy dispersive spectrometer (EDS) and scanning electron microscope (SEM); the influence of Sn and Ti doping on their activity in the selective catalytic reduction (SCR) of NO_x was investigated. The results indicated that Sn and Ti are highly dispersed as amorphous species in crystal lattice of γ-Fe₂O₃, forming sosoloid with Fe. Through doping with Ti, the γ-Fe_0.95Ti_0.05O_z catalyst exhibits a high de-NO_x efficiency of above 90% at 250~400 ℃, with a maximum of 98.3%; the addition of Ti is effective to reduce the crystallization degree of γ-Fe₂O₃, improve the pore structure of 2~100 nm, and suppress the formation of α-Fe₂O₃ phase, which are of benefits to get tiny and uniform discrete γ-Fe₂O₃ particles with high activity in SCR. However, Sn as an additive may aggravate the sintering and derogate pore structure of 2~6 nm for the γ-Fe_0.95Sn_0.05O_z catalyst, which is detrimental to SCR. The incorporation of both Sn and Ti leads to a decrease of the surface O/Fe atomic ratio from 1.83 to 1.33; the dramatic decrease of surface lattice oxygen content due to the synergistic effect between Sn and Ti may restrain the SCR activity of γ-Fe_0.95Sn_0.025Ti_0.025O_z.
- selective catalytic reduction (SCR),
- de-NO_x,
- catalyst,
- γ-Fe₂O₃,
- additives doped
1. [1]
  [1] CAO F, XIANG J, SU S, WANG P Y, SUN L S, HU S, LEI S Y. The activity and characterization of MnO_x-CeO₂-ZrO₂/g-Al₂O₃ catalysts for low temperature selective catalytic reduction of NO with NH₃[J]. Chem Eng J, 2014, 243: 347-354.
2. [2]
  [2] 杨晓燕, 沈伯雄, 马宏卿, 刘亭, 左琛. 前驱物对Mn-Ce/Ti-PILC低温SCR脱硝的影响[J]. 燃料化学学报, 2012, 40(1): 119-123. (YANG Xiao-yan, SHEN Bo-xiong, MA Hong-qing, LIU Ting, ZUO Chen. Study on the effect of Mn-Ce/Ti-PILC on low temperature SCR activity prepared with different precursors[J]. J Fuel Chem Technol, 2012, 40(1): 119-123.)
3. [3]
  [3] 黄海凤, 陈一杰, 杨睿, 朱秋莲, 卢晗锋. Fe-V/TiO₂催化剂NH₃选择性催化还原柴油车尾气NO_x[J]. 燃料化学学报, 2014, 42(6): 751-757. (HUANG Hai-feng, CHEN Yi-jie, YANG Rui, ZHU Qiu-lian, LU Han-feng. Fe-V/TiO₂ catalysts for selective catalytic reduction of NO_x with NH₃ in diesel exhaust[J]. J Fuel Chem Technol, 2014, 42(6): 751-757.)
4. [4]
  [4] MA L, LI J H, KE R, FU L X. Catalytic performance, characterization and mechanism study of Fe(SO₄)₃/TiO₂ catalyst for selective catalytic reduction of NO_z by ammonia[J]. J Phys Chem C, 2011, 115(15): 7603-7612.
5. [5]
  [5] APOSTOLESCU N, GEIGER B, HIZBULLAH K, JANC M T, KURETIA S, REICHERTA D, SCHOTTA F, WEISWEILERA W. Selective catalytic reduction of nitrogen oxides by ammonia on iron oxide catalysts[J]. Appl Catal B: Environ, 2006, 62(1/2): 104-114.
6. [6]
  [6] LIU F D, HE H. Structure-activity relationship of iron titanate catalysts in the selective catalytic reduction of NO_x with NH₃[J]. J Phys Chem C, 2010, 114(40): 16929-16936.
7. [7]
  [7] YANG S J, LIU C X, CHANG H Z, MA L, QU Z, YAN N Q, WANG C Z, LI J H. Improvement of the activity of γ-Fe₂O₃ for the selective catalytic reduction of NO with NH₃ at high temperatures: NO reduction versus NH₃ oxidization[J]. Ind Eng Chem Res, 2013, 52(16): 5601-5610.
8. [8]
  [8] RAMIS G, YI L, BUSCA G, TURCO M, KOTUR E, WILLEY R J. Adsorption, activation and oxidation of ammonia over SCR catalysts[J]. J Catal, 1995, 157(2): 523-535.
9. [9]
  [9] YAO G H, WANG F, WANG X B, GUI K T. Magnetic field effects on selective catalytic reduction of NO by NH₃ over Fe₂O₃ catalyst in a magnetically fluidized bed[J]. Energy, 2010, 35(5): 2295-2300.
10. [10]
  [10] YANG S, GUO Y, YAN N, QU Z, XIE J K, YANG C, JIA J P. Capture of gaseous elemental mercury from flue gas using a magnetic and sulfur poisoning resistant sorbent Mn/γ-Fe₂O₃ at lower temperatures[J]. J Hazardous Mater, 2011, 186(1): 508-515.
11. [11]
  [11] 赵莉, 何青松, 李琳, 陆强, 董长青, 杨勇平. 改性SCR催化剂对Hg⁰催化氧化性能的研究[J]. 燃料化学学报, 2015, 43(5): 628-634. (ZHAO Li, HE Qing-song, LI Lin, LU Qiang, DONG Chang-qing, YANG Yong-ping. Research on the catalytic oxidation of Hg⁰ by modified SCR catalysts[J]. J Fuel Chem Technol, 2015, 43(5): 628-634.)
12. [12]
  [12] CHANG H Z, LI J H, CHEN X Y, MA L, YANG S J, SCHWANK J W, HAO J M. Effect of Sn on MnO_x-CeO₂ catalyst for SCR of NO_x by ammonia: Enhancement of activity and remarkable resistance to SO₂[J]. Catal Commun, 2012, 27: 54-57.
13. [13]
  [13] LIU C X, CHEN L, CHANG H Z, MA L, PENG Y, ARANDIYAN H R, LI J H. Characterization of CeO₂-WO₃ catalysts prepared by different methods for selective catalytic reduction of NO_x with NH₃[J]. Catal Commun, 2013, 40: 145-148.
14. [14]
  [14] WANG C Z, YANG S J, CHANG H Z, PENG Y, LI J H. Structural effects of iron spinel oxides doped with Mn, Co, Ni and Zn on selective catalytic reduction of NO with NH₃[J]. J Molecular Catal A, 2013, 376: 13-21.
15. [15]
  [15] LI X L, LI Y H, DENG S S, RONG T A. A Ce-Sn-O_x catalyst for the selective catalytic reduction of NO_x with NH₃[J]. Catal Commun, 2013, 40: 47-50.
16. [16]
  [16] XIONG Y, TAND C J, YAO X J, ZHANG L, LI L L, WANG X B, DENG Y, GAO F, DONG L. Effect of metal ions doping (M = Ti⁴⁺, Sn⁴⁺) on the catalytic performance of MnO_x/CeO₂ catalyst for low temperature selective catalytic reduction of NO with NH₃[J]. Appl Catal A :Gen, 2015, 495: 206-216.
17. [17]
  [17] YU M E, LI C T, ZENG G M, ZHOU Y, ZHANG X N, XIE Y E. The selective catalytic reduction of NO with NH₃ over a novel Ce-Sn-Ti mixed oxides catalyst: Promotional effect of SnO₂[J]. Appl Surface Sci, 2015, 342: 174-182.
18. [18]
  [18] 王栋, 路春美, 张信莉, 刘洪涛, 徐丽婷, 彭建升. 不同沉淀条件制备γ-Fe₂O₃催化剂的表征及其NH₃-SCR性能[J]. 燃烧科学与技术, 2014, 20(3): 245-251. (WANG Dong, LU Chu-mei, ZHANG Xin-li, LIU Hong-tao, XU Li-ting, PENG Jian-shang. De-NO_x performance and characterization of γ-Fe₂O₃ catalysts under various precipitation conditions[J]. J Combust Sci Technol, 2014, 20(3): 245-251.)
19. [19]
  [19] 王栋, 张信莉, 路春美, 韩奎华, 彭建升, 徐丽婷. 微波热解制备γ-Fe₂O₃催化剂及其SCR脱硝性能[J]. 化工学报, 2014, 65(12): 4805-4813. (WANG Dong, ZHANG Xin-li, LU Chu-mei, HAN Kui-hua, PENG Jian-sheng, XU Li-ting. Microwave-assisted preparation of γ-Fe₂O₃ as SCR catalysts[J]. CIESC J, 2014, 65(12): 4805-4813.)
20. [20]
  [20] XIONG Z B, LU C M, GUO D X, ZHANG X L, HAN K H. Selective catalytic reduction of NO_xwith NH₃ over iron-cerium mixed oxide catalyst: Catalytic performance and characterization[J]. J Chem Technol Biotechnol, 2013, 88(7): 1258-1265.
21. [21]
  [21] CHEN T, GUAN B, LIN H, ZHU L. In situ DRIFTS study of the mechanism of low temperature selective catalytic reduction over manganese-iron oxides[J]. Chin J Catal, 2014, 35(3): 294-301.
22. [22]
  [22] SHEN B X, WANG F M, LIU T. Homogeneous MnO_x-CeO₂ pellets prepared by one-step hydrolysis process for low-temperature NH₃-SCR[J]. Powder Technol, 2014, 253: 152-157.
23. [23]
  [23] 王芳, 姚桂焕, 归柯庭. 铁基催化剂选择性催化还原烟气脱硝特性比较研究[J]. 中国电机工程学报, 2009, 29(29): 47-51. (WANG Fang, YAO Gui-huan, GUI Ke-ting. Comparison about selective catalytic reduction of de-NO_x n iron-based magnetic materials[J]. Proceed CSEE, 2009, 29(29): 47-51.)
24. [24]
  [24] 高彦杰. 低温选择性催化还原脱硝催化剂的制备及性能研究. 南京: 南京理工大学, 2009. (GAO Yan-jie. Research on the preparation and denitrification performance of low temperature SCR catalyst. Nanjing: Nanjing University of Science & Technology, 2009.)
25. [25]
  [25] LIU F D, HE H. Structure-activity relationship of iron titanate catalysts in the selective catalytic reduction of NO_x with NH₃[J]. J Phys Chem C, 2010, 114(40): 16929-16936.
26. [26]
  [26] PIEROTTI R A, ROUQUEROL J. Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity[J]. Pure Appl Chem, 1985, 57(4): 603-619.
27. [27]
  [27] KOEBEL M, ELSENER M, MADIA G. Reaction pathways in the selective catalytic reduction process with NO and NO₂ at low temperature[J]. Ind Eng Chem Res, 2001, 40(1): 52-59.
28. [28]
  [28] YANG S J, LI J H, WANG C Z, CHEN J H, MA L, CHANG H Z, CHEN L, PENG Y, YAN N Q. Fe-Ti spinel for the selective catalytic reduction of NO with NH₃: Mechanism and structure activity relationship[J].Appl Catal B: Environ, 2012, 117-118: 73-80.
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Structural property of γ-Fe2O3 catalysts doped with Sn and Ti and their activity in the selective catalytic reduction of NOx

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Structural property of γ-Fe₂O₃ catalysts doped with Sn and Ti and their activity in the selective catalytic reduction of NO_x