Citation: LI Yun-he, HONG Xin, GAO Chang, NIU Xiao-qing, TANG Ke. Preparation of heteroatom-containing mesoporous MCM-41 molecular sieves and their performance in the adsorption denitrification of quinoline in model diesel oil[J]. Journal of Fuel Chemistry and Technology, ;2019, 47(10): 1195-1204. shu

Preparation of heteroatom-containing mesoporous MCM-41 molecular sieves and their performance in the adsorption denitrification of quinoline in model diesel oil

School of Chemical and Environment Engineersity, Liaoning University of Technology, Jinzhou 121001, China

Corresponding author: HONG Xin, hongxin12@sohu.com
Received Date: 19 July 2019
Revised Date: 25 August 2019

Fund Project: The project was supported by the Liaoning Provincial Key Research and Development Guidance Project (2018230006) and Liaoning Provincial Natural Science Foundation of China (20180550639, 2019ZD0699)Liaoning Provincial Natural Science Foundation of China 2019ZD0699Liaoning Provincial Natural Science Foundation of China 20180550639the Liaoning Provincial Key Research and Development Guidance Project 2018230006

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The mesoporous MCM-41 molecular sieve and heteroatom (Zn, Ba, and Ce) containing mesoporous MCM-41 molecular sieves were synthesized and characterized by X-ray diffraction (XRD), FT-infrared spectroscopy (FT-IR) and N₂ sorption; their performance in the adsorption denitrification of quinoline in model diesel oil was investigated. The results indicate that all the synthesized molecular sieves take typical mesoporous structure and heteroatoms are successfully incorporated into the molecular sieves framework. An 8T cluster model for the MCM-41 molecular sieves was built by using the Materials Studio software; the simulated XRD spectrum is basically consistent with the experimental spectrum, proving the accuracy of cluster model. The adsorption of quinoline on the heteroatom-containing mesoporous MCM-41 molecular sieves were then simulated and the adsorption energy and the distance between the adsorbed molecule and the adsorption center (d_(N-M)) were calculated. The results suggest that the adsorption denitrification performance of various molecular sieves follows the order of Zn-MCM-41 > Ce-MCM-41 > Ba-MCM-41 > MCM-41; that is, Zn-MCM-41 exhibits the best adsorption denitrification performance, with the highest adsorption energy and shortest distance between the adsorption molecule and the adsorption center. Moreover, the adsorption time has a significant influence on the denitrification efficiency, whereas the effect of adsorption temperature is relatively minor; the optimal adsorption times for Zn-MCM-41, Ba-MCM-41 and Ce-MCM-41 are 40, 10 and 30 min, respectively, whereas the optimal adsorption temperatures for three molecular sieves are 40, 30 and 40℃, respectively.
- heteroatoms,
- mesoporous molecular sieves,
- MCM-41,
- molecular simulation,
- adsorption denitrification,
- adsorption energy
1. [1]
  WANG Di. Research on the type and distribution of nitrogen compounds in FCC process[D]. Beijing: Institute of petrochemical sciences, 2016.
2. [2]
  CHENG X G, ZHAO T, FU X G, HU Z D. Identification of nitrogen compounds in RFCC diesel oil by mass spectrometry[J]. Fuel Process Technol, 2003,85:1463-1472.
3. [3]
  GEORGINA C L, SARA L, REGINA A, MA T M, JEUSUS C, LIUS N. Nitrogen compounds characterization in atmospheric gas oil and light cycle oil from a blend of mexican crudes[J]. Fuel, 2002,81(10):1341-1350. doi: 10.1016/S0016-2361(02)00047-9
4. [4]
  MA Yun-jie. Study on preparation of catalyst active alumina[D]. Changsha: Agricultural University of Hunan, 2012.
5. [5]
  MINH T N, TAYAKOUT F M, FABIEN C, GERHARD D P, CRISTOPHE G. Use of kinetic modeling for investigating support acidity effects of NiMo sulfide catalysts on quinoline hydrodenitrogenation[J]. Appl Catal A:Gen, 2017,520:132-144.
6. [6]
  GUO Zhong-sen, ZU Yun, HUI Yu, QIN Yu-cai, WANG Huan, ZHANG Xiao-tong, SONG Li-juan. Influence of olefin on the mechanism of thiophene adsorption on the active species of Al-MCM-41 mesoporous zeolites[J]. J Fuel Chem Technol, 2019,47(4):474-483.
7. [7]
  MARTINEZ B E, AGUILAR J, GUTIERREZ M, MONTOYA J A, REYES D L. Ga and Al containing MCM-41 mesoporous molecular sieves:Structure and catalytic performance for the 4, 6 dimethyldibenzothiophene hydrodesulfurization[J]. Catal Today, 2013,212:45-51. doi: 10.1016/j.cattod.2012.08.028
8. [8]
  GUO Xiao-jun, LI Yu-tian, LI Jing. Performance of magnesium hydroxide-modified diatomite in adsorption of reactive red from aqueous solution[J]. Bull Chin Ceram, 2014,33(9):2170-2175.
9. [9]
  HONG Xin, LI Yun-he, GUAN Li-hua, SUN Cheng-yi, GAO Chang, TANG Ke. Adsorption removal and dynamics of aniline or pyridine from model diesel with silica gel-supported heteropoly acid[J]. Petrochem Technol, 2018,47(12):1356-1361. doi: 10.3969/j.issn.1000-8144.2018.12.010
10. [10]
  HE Qing-quan. Study on alumina porous media preparation and adsorption properties[D]. Wuhan: Wuhan Institute of Technology, 2015.
11. [11]
  MING Yang, WANG Lei, WANG Jun-feng, SUN Yu, YANG Jing. Study on hydrothermal stability of metal modified SBA-15mesoporous molecular sieves[J]. Spec Petrochem, 2017,34(3):30-35.
12. [12]
  ZHANG Z Q, YAN L, YUAN G, SHI W X, WANG W, ZHANG B, ZHANG R J, BAO X, WU S Y, CUI F Y. Pd and Pt nanoparticles supported on the mesoporous silica molecular sieve SBA-15 with enhanced activity and stability in catalytic bromate reduction[J]. Chem Eng J, 2018,344:114-123. doi: 10.1016/j.cej.2018.03.056
13. [13]
  CHENG Jun-jie, LI Zhen-rong, ZHAO Liang-fu. Catalytic performance of Ni-W supported on micro-mesoporous Hβ/Al-SBA-15 composite molecular sieves in the hydrocracking of naphthalene to BTX[J]. J Fuel Chem Technol, 2017,45(1):93-99. doi: 10.3969/j.issn.0253-2409.2017.01.013
14. [14]
  LIU Sha, CAI Yi-xi, FAN Yong-sheng, LI Xiao-hua, WANG Jia-jun. Synergistic catalysis of MCM-41 and HZSM-5 on rape straw pyrolysis[J]. J Fuel Chem Technol, 2016,44(10):1195-1202. doi: 10.3969/j.issn.0253-2409.2016.10.006
15. [15]
  GUO Wei, CAO Yang, LI Jin, LUO Nan, ZHAO Zi-wei. Preparation, characterization and catalytic performance of the new catalysts Ni_xP/Zr-MCM-41[J]. Acta Pet Sin (Pet Process Sect), 2016,32(5):891-897. doi: 10.3969/j.issn.1001-8719.2016.05.004
16. [16]
  ZHANG X B, DONG J X, HAO Z C, CAI W F, WANG F M. Fe-Mn/MCM-41:Preparation, characterization and catalytic activity for methyl orange in the process of heterogeneous fenton reaction[J]. Trans Tianjin Univ, 2018,24(4):361-369. doi: 10.1007/s12209-018-0122-1
17. [17]
  HE Xi-feng, SONG Wei-ming, AN Hong. Synthesis and characterization of mesoporous molecular sieve MCM-41 with metal dopin[J]. Fine Chem, 2014,31(10):1215-1219.
18. [18]
  ZHANG Jia-dong, ZU Yun, QIN Yu-cai, SONG Li-juan. Study on selective adsorption desulfurization mechanism on aluminum modified MCM-41 Zeolite[J]. Pet Process Petrochem, 2017,48(8):51-57. doi: 10.3969/j.issn.1005-2399.2017.08.012
19. [19]
  LI Yun-he, HONG Xin, LI Xiang-long, NIU Xiao-qing, TANK Ke. Preparation of molecular sieve Ni-MCM-41 and its adsorptive denitrogenation performance of Simulated Diesel[J]. Pet Process Petrochem, 2019,50(6):40-45. doi: 10.3969/j.issn.1005-2399.2019.06.009
20. [20]
  HONG Xin, TANG Ke. Preparation and adsorption denitrification of heteroatoms mesoporous molecular sieve Co-MCM-41[J]. J Fuel Chem Technol, 2015,43(6):720-727. doi: 10.3969/j.issn.0253-2409.2015.06.012
21. [21]
  China Petrochemical Co Ltd. Science and Technology Development Department. Industry Standards for Petroleum Products[M]. Beijing:China Petrochemical Press, 2005:402-405.
22. [22]
  AN Xiao-wei. The theoretica calculation for CO₂ capture Using hydroxypyridine-based ionic liquids and its immobilization on molecular sieve MCM-41[D]. Taiyuan: Taiyuan University of Technology, 2017.
23. [23]
  ABREU T H, MEYER C I, PADRO C, MARTINS L. Acidic V-MCM-41 catalysts for the liquid-phase ketalization of glycerol with acetone[J]. Microporous Mesoporous Mater, 2019,273:219-225. doi: 10.1016/j.micromeso.2018.07.006
24. [24]
  LI Ya-nan. Synthesis, characterization and catalytic activity of Me-MCM-41 for oxidative dehydrogenation of ethane to ethylene with CO₂[D]. Jilin: Jilin University, 2006.
25. [25]
  LIU Jia, SUI Ming-hao, SHENG Li. Hydrothermal synthesis, characterization and catalytic performance of Mn-MCM-41 mesoporous molecular sieve[J]. Modern Chem Ind, 2018,38(7):93-97.
26. [26]
  YI, BAI, Zhao-ri-ge-tu. Preparation of Pd/MCM-41 and its photocatalytic performance for benzene hydroxylation[J]. J Mol Catal, 2016,30(16):583-593.
27. [27]
  YAN C Y, CHEN Q C, CHANG Q, PENG Y B. Microwave-assisted hydrothermal synthesis, characterization and photocatalytic activities of Ti-MCM-41[J]. Acta Scientiae Circumstantiae, 2014,34(5):1220-1227.
28. [28]
  JIANG T S, TANG Y J, ZHAO Q, YIN H B. Effect of Ni-doping on the pore structure of pure silica MCM-41 mesoporous molecular sieve under microwave irradiation[J]. Colloid Surface A, 2018,315:299-303.
29. [29]
  Bai Jia-ning, Li Hui-peng, Zhao Hua. Study on adsorptive denitrogennation of Ce-MCM-41 molecular sieve[J]. J Liaoning Univ Pet Chem Technol, 2018,38(1):16-19. doi: 10.3969/j.issn.1672-6952.2018.01.003
30. [30]
  WU Qi-sheng, CHEN Yi-lin. Synthesis, characterization, and de-NO_x performance of lanthanum-doped MCM-41[J]. Inorg Chem Ind, 2014,46(7):71-74. doi: 10.3969/j.issn.1006-4990.2014.07.020
31. [31]
  ZHAO Q, CHU J Y, JIANG T S, YIN H B. Hydrothermal synthesis and stability of Ni-MCM-41[J]. J Chin Ceram Soc, 2008,9(36):1256-1261.
32. [32]
  KARTHIK M, TRIPATHI A K, GUPTA N M, VINU A, HARTMANN M, PALANICHA M Y, MURUGESAN V. Characterization of Co, Al-MCM-41 and its activity in the t-butylation of phenol using isobutanol[J]. Appl Catal A:Gen, 2004,268:139-149. doi: 10.1016/j.apcata.2004.03.028
33. [33]
  WANG Jun-feng, SHEN Jian, REN Tie-qiang. Preparation of Ce-SBA-15 catalyst and its performance on phenol alkylation with methanol[J]. J Mol Catal A Chem (China), 2016,30(6):523-531.
34. [34]
  YANG Xiao-dong, WANG Xin-miao, GAO Shan-bin, WANG An-jie. Hydrodesulfurization performances of Pd catalysts supported on ZSM-5/MCM-41 composite zeolite[J]. Acta Chim Sin, 2017,75:479-484.
35. [35]
  SUO Yan-hua, WANG Juan, WANG Ying-jun, CHEN Yan-guang, CHEN Gang. HPMo-Ni/La-MCM-41 catalyst for n-Heptane hydroisomerization[J]. Acta Pet Sin (Pet Process Sect), 2015,31(4):875-882. doi: 10.3969/j.issn.1001-8719.2015.04.007
36. [36]
  SZEGEDI Á, KÍNYA Z, MÉHN D, SOLYMÁRE , PÁLBORBÉLYG , HORVÁTH Z E, BIRÍ LP, KIRICSI I. Spherical mesoporous MCM-41 materials containing transition metals:Synthesis and characterization[J]. Appl Catal A:Gen, 2004,272:257-266. doi: 10.1016/j.apcata.2004.05.057
37. [37]
  HAN Lei, OUYANG Ying, LUO Yi-bin, DA Zhi-jian. Application of modified ZSM-5 zeolite with different elements in catalytic cracking of light hydrocarbon[J]. Acta Pet Sin (Pet Process Sect), 2018,34(2):419-429. doi: 10.3969/j.issn.1001-8719.2018.02.025
38. [38]
  ZHANG Jun-tao, SONG Jing, ZHEN Xing, SHEN Zhi-bing, LIANG Sheng-rong. Synthesis of MCM-41/MOR composite molecular sieves and its catalytic properties for isomerization of alkane[J]. J Fuel Chem Technol, 2017,45(6):675-681. doi: 10.3969/j.issn.0253-2409.2017.06.005
39. [39]
  SHU U H, SHAO Y M, WEI X Y. Synthesis and characterization of Ni-MCM-41 for methyl blue adsorption[J]. Microporous Mesoporous Mater, 2015,204:88-94.
40. [40]
  ZHOU Dan-hong, WANG Yu-qing, HE Ning, YANG Gang. The π-complexation mechanisms of Cu(I), Ag(I)/Zeolites for desulfurization[J]. Acta Phys Chim Sin, 2006,22(5):542-547. doi: 10.3866/PKU.WHXB20060506
41. [41]
  HONG Xin, TANG Ke, DING Shi-hong. Preparation and deep adsorption denitrification from diesel oil of heteroatoms mesoporous molecular sieve Co-MCM-41[J]. J Fuel Chem Technol, 2016,44(1):99-105. doi: 10.3969/j.issn.0253-2409.2016.01.014
42. [42]
  XU Ru-ren, PANG Wen-qin, HUO Qi-sheng, YU Ji-hong, CHEN Jie-sheng, SU Bao-lian, QIU Shi-lun, YAN Wen-fu. Chemistry-Zeolite and Porous Materials[M]. Beijing:Science Press, 2015.
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