Citation: DONG Shi-lin, SU Ya-xin, LIU Xin, LI Qian-cheng, YUAN Min-hao, ZHOU Hao, DENG Wen-yi. Experimental study on selective catalytic reduction of NO by C₃H₆ over Fe/Ti-PILC catalysts[J]. Journal of Fuel Chemistry and Technology, ;2018, 46(10): 1231-1239. shu

Experimental study on selective catalytic reduction of NO by C₃H₆ over Fe/Ti-PILC catalysts

1.
School of Environmental Science and Engineering, Donghua University, Shanghai 201620, China
2.
Changzhou Vocational Institude of Engineering, Changzhou 203164, China

Corresponding author: SU Ya-xin, suyx@dhu.edu.cn
Received Date: 8 May 2018
Revised Date: 9 August 2018

Fund Project: Jiangsu Province Prospective Joint Research Projects BY2015032-02the National Natural Science Foundation of China 51278095The project was supported by the National Natural Science Foundation of China (51278095) and Jiangsu Province Prospective Joint Research Projects (BY2015032-02)

Figures(7)

Ti-pillared interlayer clay (PILC)-based catalysts ion exchanged with Fe were prepared and used for selective catalytic reduction of NO_x using propylene as the reducing agent under oxygen-rich conditions. The relationship between structure and properties of the catalysts was studied using N₂-adsorption/desorption, XRD, UV-vis, H₂-TPR, and Py-FTIR. The results show that the prepared 19Fe/Ti-PILC catalyst can achieve complete removal of NO at 400 ℃, and N₂ selectivity can reach over 90% and has better resistance to water vapor and SO₂. N₂-isothermal adsorption/desorption and XRD results show that structure of montmorillonite is opened, cross-linked pillars are effective, and a large specific surface area and pore volume are formed. UV-vis results show that the denitrification activity of the catalyst is related to content of oligomeric Fe_xO_y. Py-FTIR results show that both Lewis acid and Brønsted acid are presented on the catalyst surface. Fe³⁺ loading into the pillared clay can significantly increase the Lewis acid content. Lewis acid is one of the influencing factors on the denitrification activity of the catalyst. H₂-TPR indicates that the catalyst has a strong reduction ability at about 400 ℃, and the reduction ability of the catalyst is mainly represented by the reduction of Fe³⁺→Fe²⁺.
- oxygen-rich conditions,
- pillared clay,
- selective catalytic reduction,
- propylene
1. [1]
  IWAMOTO M, YAHIRO H, YU U Y. Selective reduction of NO by lower hydrocarbons in the presence of O₂ and SO₂ over copper ion-exchanged zeolites[J]. Catal, 1990,32(6):430-433.
2. [2]
  HELD W, KOENIG A, RICHTER T, PUPPE L. Catalytic NO_x reduction in net oxidizing exhaust gas[J]. SAE Trans, 1990,99(4):209-216.
3. [3]
  ZHOUs Hao, SU Ya-xin, DENG Wen-yi, ZHONG Fang-chuan. A review of HC-SCR over metal oxides-based catalysts[J]. Environ Sci Technol, 2016,39(1):93-100.
4. [4]
  WANG Qi-yin, WEN Yan-bing, DONG Xin-fa, LIN Wei-ming. Crosslinked clay synthesis and its application in selective catalytic reduction of NO_x with C₃H₆[J]. J Chem Eng Chin Univ, 2006,20(4):598-603. doi: 10.3321/j.issn:1003-9015.2006.04.019
5. [5]
  YASHNIK S A, SALNIKOV A V, VASENIN N T, ANUFRIENKO V F, ISMAGILOV Z R. Regulation of the copper-oxide cluster structure and DeNO_x activity of Cu-ZSM-5 catalysts by variation of OH/Cu²⁺[J]. Catal Today, 2012,197(1):214-227. doi: 10.1016/j.cattod.2012.08.033
6. [6]
  KUMAR P A, REDDY M P, JU LK, HYUN-SOOK B, PHIL H H. Low temperature propylene SCR of NO by copper alumina catalyst[J]. J Mol Catal A:Chem, 2008,291(1/2):66-74.
7. [7]
  LONG R Q, CHANG M T, YANG R T. Enhancement of activities by sulfation on Fe-exchanged TiO₂-pillared clay for selective catalytic reduction of NO by ammonia[J]. Appl Catal B:Environ, 2001,33(2):97-107. doi: 10.1016/S0926-3373(01)00173-4
8. [8]
  VAUGHAN D E W, LUSSIER R J, MAGEE J S. Pillared interlayered clay materials useful as catalysts and sorbents: CA, US4176090[P]. 1979.
9. [9]
  YANG R T, THARAPPIWATTANANON N, LONG R Q. Ion-exchanged pillared clays for selective catalytic reduction of NO by ethylene in the presence of oxygen[J]. Appl Catal B:Environ, 1998,19(3/4):289-304.
10. [10]
  VALVERDE J L, LUCAS A D, SÁNCHEZ P, DORADO F, ROMERO A. Cation exchanged and impregnated ti-pillared clays for selective catalytic reduction of NO_x by propylene[J]. Appl Catal B:Environ, 2003,43(1):43-56. doi: 10.1016/S0926-3373(02)00274-6
11. [11]
  LU G, LI X Y, QU Z P, ZHAO Q D, ZHAO L, CHEN G H. Copper-ion exchanged Ti-pillared clays for selective catalytic reduction of NO by propylene[J]. Chem Eng J, 2011,168(3):1128-1133. doi: 10.1016/j.cej.2011.01.095
12. [12]
  DOU Yi-feng, SU Ya-xin, LU Zhe-xing, ZHOU Hao, DENG Wen-yi. Experimental study of NO reduction by ethane over iron[J]. J Fuel Chem Technol, 2015,43(10):1273-1280. doi: 10.3969/j.issn.0253-2409.2015.10.017
13. [13]
  LIANG Jun-qing, SU Ya-xin, ZHOU Hao, DENG Wen-yi. Performance and mechanism of NO reduction by iron combined with propene[J]. J Fuel Chem Technol, 2016,44(8):977-984. doi: 10.3969/j.issn.0253-2409.2016.08.011
14. [14]
  SU Ya-xin, SU A-long, REN Li-ming, DENG Wen-yi. Effect of SO₂ on NO reduction by methane over iron[J]. J Fuel Chem Technol, 2014,42(3):377-384.
15. [15]
  ZHOU Hao, SU Ya-xin, QI Yue-zhou, LU Zhe-xing, DENG Wen-yi. Effect of water vapor on NO reduction by methane over iron[J]. J Fuel Chem Technol, 2014,42(11):1378-1386. doi: 10.3969/j.issn.0253-2409.2014.11.016
16. [16]
  QIAN Wen-yan, SU Ya-xin, YANG Xi, YUAN Min-hao, DENG Wen-yi, ZHAO Bing-tao. Experimental study on selective catalytic reduction of NO with propene over iron based catalysts supported on aluminum pillared clays[J]. J Fuel Chem Technol, 2017,45(12):1499-1507. doi: 10.3969/j.issn.0253-2409.2017.12.012
17. [17]
  YE Qing, YAN Li-na, HUO Fei-fei, WANG Hai-ping, CHENG Shui-yuan, KANG Tian-fang. Cu-supportedon Fe-pillared sepiolite:Characterization and selective catalytic reduction(SCR)of NO by propene[J]. Acta Chim Sin, 2011,69(13):1524-1532.
18. [18]
  YANG T T, BI H T, CHENG X. Effects of O₂, CO₂ and H₂O on NO_x adsorption and selective catalytic red uction over Fe/ZSM-5[J]. Appl Catal B:Environ, 2011,102(1/2):163-171.
19. [19]
  MARTÍNEZ-HERNÁNDEZ A, FUENTES G A. Redistribution of cobalt species in Co-ZSM-5 during operation under wet conditions in the reduction of NO_x by propane[J]. Appl Catal B:Environ, 2005,57(3):167-174. doi: 10.1016/j.apcatb.2004.10.018
20. [20]
  KOMVOKIS V G, ILIOPOULOU E F, VASALOS I A, TRIANTAFYLLIDIS K S, MARSHALL C L. Development of optimized Cu-ZSM-5 deNO_x catalytic materials both for HC-SCR applications and as FCC catalytic additives[J]. Appl Catal A:Environ, 2007,325(2):345-352. doi: 10.1016/j.apcata.2007.02.035
21. [21]
  KIM B S, LEE S H, PARK Y T, HAM S W, CHAE H J, NAM I S. Selective catalytic reduction of NO_x, by propene over copper-exchanged pillared clays[J]. Korean J Chem Eng, 2001,18(5):704-710. doi: 10.1007/BF02706390
22. [22]
  LONG R Q, YANG R T. Selective catalytic reduction of NO with ammonia over V₂O₅doped TiO₂ pillared clay catalysts[J]. Appl Catal B:Environ, 2000,24(1):13-21. doi: 10.1016/S0926-3373(99)00092-2
23. [23]
  GREGG S J, SING K S W. Adsorption, Surface Area and Porosity[M]. New York:Academic Press Inc, 1982.
24. [24]
  LONG R Q, YANG R T. Selective catalytic reduction of nitrogen oxides by ammonia over Fe³⁺-exchanged TiO₂-pillared clay catalysts[J]. J Catal, 1999,186(2):254-268. doi: 10.1006/jcat.1999.2558
25. [25]
  CHMIELARZ L, PIWOWARSKA Z, KUŚTROWSKI P, WEGRZYN A, GIL B, KOWALCZYK A, DUDEK B, DZIEMBAJ R, MICHALIK M. Comparison study of titania pillared interlayered clays and porous clay heterostructures modified with copper and iron as catalysts of the DeNO_x process[J]. Appl Clay Sci, 2011,53(2):164-173. doi: 10.1016/j.clay.2010.12.009
26. [26]
  SHEN Bo-xiong, MA Hong-qing, YANG Xiao-yan, YAO Yan. Study on preparation, characterization and de-NO activity of Mn-CeO_x/Ti-PILC[J]. J Fuel Chem Technol, 2012,40(5):615-620. doi: 10.3969/j.issn.0253-2409.2012.05.017
27. [27]
  OLIVEIRA L C A, RIOS R V R A, FABRIS J D, SAPAG K, GARG V K, LAGO R M. Clay-iron oxide magnetic composites for the adsorption of contaminants in water[J]. Appl Clay Sci, 2003,22(4):169-177. doi: 10.1016/S0169-1317(02)00156-4
28. [28]
  KUMAR M S, SCHWIDDER M, GRÜNERT W, BRUCKNER A. On the nature of different iron sites and their catalytic role in Fe-ZSM-5 DeNO_x, catalysts:New insights by a combined EPR and UV/VIS spectroscopic approach[J]. J Catal, 2004,227(2):384-397. doi: 10.1016/j.jcat.2004.08.003
29. [29]
  BRANDENBERGER S, KRÖCHER 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]. J Catal, 2009,268(2):297-306. doi: 10.1016/j.jcat.2009.09.028
30. [30]
  DATKA J, TUREK A M, JEHNG J M, WACHS I E. Acidic properties of supported niobium oxide catalysts:An infrared spectroscopy investigation[J]. J Catal, 1992,135(135):186-199.
31. [31]
  SULTANA A, HANEDA M, FUJITANI T, HAMADA H. Influence of Al₂O₃ support on the activity of Ag/Al₂O₃ catalysts for SCR of NO with decane[J]. Catal Lett, 2007,114(1):96-102.
32. [32]
  CHMIELARZ L, PIWOWARSKA Z, KUŚTROWSKIP , WEGRZYN A, GIL B, KOWALCZYK A, DUDEK B, DZIEMBAJ R, MICHALIK M. Comparison study of titania pillared interlayered clays and porous clay heterostructures modified with copper and iron as catalysts of the DeNO_x process[J]. Appl Clay Sci, 2011,53(2):164-173. doi: 10.1016/j.clay.2010.12.009
33. [33]
  TOLEDO-ANTONIO J A, CORTÉS-JÁCOME M A, NAVARRETE J, ANGELES-CHAVEZ C, LOPEZ-SALINAS E, RENDON-RIVERA A. Morphology induced CO, pyridine and lutidine adsorption sites on TiO₂:Nanoparticles, nanotubes and nanofibers[J]. Catal Today, 2010,155(3/4):247-254.
1. [1]
  Yu Wang , Haiyang Shi , Zihan Chen , Feng Chen , Ping Wang , Xuefei Wang . 具有富电子Pt^δ^-壳层的空心AgPt@Pt核壳催化剂：提升光催化H₂O₂生成选择性与活性. Acta Physico-Chimica Sinica, 2025, 41(7): 100081-. doi: 10.1016/j.actphy.2025.100081
2. [2]
  Yaping ZHANG , Tongchen WU , Yun ZHENG , Bizhou LIN . Z-scheme heterojunction β-Bi₂O₃ pillared CoAl layered double hydroxide nanohybrid: Fabrication and photocatalytic degradation property. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 531-539. doi: 10.11862/CJIC.20240256
3. [3]
  Guojie Xu , Fang Yu , Yunxia Wang , Meng Sun . Introduction to Metal-Catalyzed β-Carbon Elimination Reaction of Cyclopropenones. University Chemistry, 2024, 39(8): 169-173. doi: 10.3866/PKU.DXHX202401060
4. [4]
  Zhuoyan Lv , Yangming Ding , Leilei Kang , Lin Li , Xiao Yan Liu , Aiqin Wang , Tao Zhang . Light-Enhanced Direct Epoxidation of Propylene by Molecular Oxygen over CuO_x/TiO₂ Catalyst. Acta Physico-Chimica Sinica, 2025, 41(4): 100038-. doi: 10.3866/PKU.WHXB202408015
5. [5]
  Xingyang LI , Tianju LIU , Yang GAO , Dandan ZHANG , Yong ZHOU , Meng PAN . A superior methanol-to-propylene catalyst: Construction via synergistic regulation of pore structure and acidic property of high-silica ZSM-5 zeolite. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1279-1289. doi: 10.11862/CJIC.20240026
6. [6]
  Shihui Shi , Haoyu Li , Shaojie Han , Yifan Yao , Siqi Liu . Regioselectively Synthesis of Halogenated Arenes via Self-Assembly and Synergistic Catalysis Strategy. University Chemistry, 2024, 39(5): 336-344. doi: 10.3866/PKU.DXHX202312002
7. [7]
  .
  CCS Chemistry | 超分子活化底物为自由基促进高效选择性光催化氧化
  . CCS Chemistry, 2025, 7(10.31635/ccschem.025.202405229): -.
8. [8]
  Peng YUE , Liyao SHI , Jinglei CUI , Huirong ZHANG , Yanxia GUO . Effects of Ce and Mn promoters on the selective oxidation of ammonia over V₂O₅/TiO₂ catalyst. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 293-307. doi: 10.11862/CJIC.20240210
9. [9]
  Yunhao Zhang , Yinuo Wang , Siran Wang , Dazhen Xu . Progress in Selective Construction of Functional Aromatics from Nitrogenous Cycloalkanes. University Chemistry, 2024, 39(11): 136-145. doi: 10.3866/PKU.DXHX202401083
10. [10]
  Peiran ZHAO , Yuqian LIU , Cheng HE , Chunying DUAN . A functionalized Eu³⁺ metal-organic framework for selective fluorescent detection of pyrene. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 713-724. doi: 10.11862/CJIC.20230355
11. [11]
  Xilin Zhao , Xingyu Tu , Zongxuan Li , Rui Dong , Bo Jiang , Zhiwei Miao . Research Progress in Enantioselective Synthesis of Axial Chiral Compounds. University Chemistry, 2024, 39(11): 158-173. doi: 10.12461/PKU.DXHX202403106
12. [12]
  Jiakun BAI , Ting XU , Lu ZHANG , Jiang PENG , Yuqiang LI , Junhui JIA . A red-emitting fluorescent probe with a large Stokes shift for selective detection of hypochlorous acid. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1095-1104. doi: 10.11862/CJIC.20240002
13. [13]
  Qinjin DAI , Shan FAN , Pengyang FAN , Xiaoying ZHENG , Wei DONG , Mengxue WANG , Yong ZHANG . Performance of oxygen vacancy-rich V-doped MnO₂ for high-performance aqueous zinc ion battery. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 453-460. doi: 10.11862/CJIC.20240326
14. [14]
  Jun LUO , Baoshu LIU , Yunchang ZHANG , Bingkai WANG , Beibei GUO , Lan SHE , Tianheng CHEN . Europium(Ⅲ) metal-organic framework as a fluorescent probe for selectively and sensitively sensing Pb²⁺ in aqueous solution. Chinese Journal of Inorganic Chemistry, 2024, 40(12): 2438-2444. doi: 10.11862/CJIC.20240240
15. [15]
  Hailian Tang , Siyuan Chen , Qiaoyun Liu , Guoyi Bai , Botao Qiao , Fei Liu . Stabilized Rh/hydroxyapatite Catalyst for Furfuryl Alcohol Hydrogenation: Application of Oxidative Strong Metal-Support Interactions in Reducing Conditions. Acta Physico-Chimica Sinica, 2025, 41(4): 100036-. doi: 10.3866/PKU.WHXB202408004
16. [16]
  Hailang JIA , Hongcheng LI , Pengcheng JI , Yang TENG , Mingyun GUAN . Preparation and performance of N-doped carbon nanotubes composite Co₃O₄ as oxygen reduction reaction electrocatalysts. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 693-700. doi: 10.11862/CJIC.20230402
17. [17]
  Jie ZHAO , Sen LIU , Qikang YIN , Xiaoqing LU , Zhaojie WANG . Theoretical calculation of selective adsorption and separation of CO₂ by alkali metal modified naphthalene/naphthalenediyne. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 515-522. doi: 10.11862/CJIC.20230385
18. [18]
  Junjie Zhang , Yue Wang , Qiuhan Wu , Ruquan Shen , Han Liu , Xinhua Duan . Preparation and Selective Separation of Lightweight Magnetic Molecularly Imprinted Polymers for Trace Tetracycline Detection in Milk. University Chemistry, 2024, 39(5): 251-257. doi: 10.3866/PKU.DXHX202311084
19. [19]
  Baitong Wei , Jinxin Guo , Xigong Liu , Rongxiu Zhu , Lei Liu . Theoretical Study on the Structure, Stability of Hydrocarbon Free Radicals and Selectivity of Alkane Chlorination Reaction. University Chemistry, 2025, 40(3): 402-407. doi: 10.12461/PKU.DXHX202406003
20. [20]
  Jun Huang , Pengfei Nie , Yongchao Lu , Jiayang Li , Yiwen Wang , Jianyun Liu . 丝光沸石负载自支撑氮掺杂多孔碳纳米纤维电容器及高效选择性去除硬度离子. Acta Physico-Chimica Sinica, 2025, 41(7): 100066-. doi: 10.1016/j.actphy.2025.100066

Get Citation

PDF

XML

Metrics

PDF Downloads(7)
Abstract views(960)
HTML views(91)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Experimental study on selective catalytic reduction of NO by C3H6 over Fe/Ti-PILC catalysts

Metrics

通讯作者: 陈斌, bchen63@163.com

Experimental study on selective catalytic reduction of NO by C₃H₆ over Fe/Ti-PILC catalysts