Citation: YANG Jia-ke, ZUO Tong-jiu, LU Yu-ying, ZENG Wu-song, LU Jiang-yin. Catalytic performance of NiMo/Al₂O₃-USY in the hydrocracking of low-temperature coal tar[J]. Journal of Fuel Chemistry and Technology, ;2019, 47(9): 1053-1066. shu

Catalytic performance of NiMo/Al₂O₃-USY in the hydrocracking of low-temperature coal tar

Key Laboratory of Oil & Gas Fine Chemicals, Ministry of Education, Xinjiang University, Urumqi 830046, China

Corresponding author: LU Jiang-yin, jiangyinlu6410@163.com
Received Date: 28 May 2019
Revised Date: 4 July 2019

Fund Project: The project was supported by the National Natural Science Foundation of China (21366030)the National Natural Science Foundation of China 21366030

Figures(15)

A series of NiMo/Al₂O₃-USY catalysts with different MoO₃ contents were prepared through incipient wetness method and further modified with NH₄F. The NiMo/Al₂O₃-USY catalysts were characterized by XRD, XPS, HR-TEM, NH₃-TPD, H₂-TPR and N₂ adsorption and their catalytic performance in the hydrocracking of low-temperature coal tar (LTCT) was investigated in a 200 mL fixed-bed reactor. The results indicate that the appropriate MoO₃ content is 15% (mass ratio); higher MoO₃ content may lead to the agglomeration of active metals on the support, although it has little influence on the sulfidation degree of Mo species and the conversion of coal tar upon hydrocracking. In addition, the amount of strong acid sites and pore diameter decrease gradually with a further increase in the MoO₃ content, which is disadvantageous for deep hydrocracking. The modification of USY zeolite with NH₄F solution can enlarge the average pore diameter of resultant NiMo/Al₂O₃-USY catalysts and then improve the residue conversion of coal tar. However, the amount of strong acid sites decreases obviously when the concentration of NH₄F solution exceeds 0.6 mol/L, which may lead to an increase of the sulfur content in the hydrocracking product. Over the NiMo/Al₂O₃-USY catalyst modified with 0.6 mol/L NH₄F solution, the residue conversion of coal tar reaches 87.65%; the sulfur contents in the gasoline fraction (< 180 ℃) and diesel fraction (180-320 ℃) are 5.96 and 34.98 mg/kg, respectively.
- low-temperature coal tar,
- hydrocracking,
- modified USY,
- sulfur content,
- NiMo/Al₂O₃-USY
1. [1]
  YAN Lun-jing. Analysis on converting gaseous tar to light arenes by catalytic cracking[D]. Taiyuan: Taiyuan University of Technology, 2016.
2. [2]
  SUN J M, LI D, YAO R Q, SUN Z H, LI X K, LI W H. Modeling the hydrotreatment of full range medium temperature coal tar by using a lumping kinetic approach[J]. React Kinet Mech Catal, 2015,114(2):451-471. doi: 10.1007/s11144-014-0791-2
3. [3]
  MA Bao-qi. Preparation of Fuel Oil from Coal Tar[M]. Beijing:Chemical Industry Press, 2011.
4. [4]
  CUI W G, ZHENG H A, NIU M L, ZHANG S J, LI D, QIAO J, LI W H. Product compositions from catalytic hydroprocessing of low temperature coal tar distillate over three commercial catalysts[J]. React Kinet Mech Catal, 2016,119(2):491-509. doi: 10.1007/s11144-016-1068-8
5. [5]
  XIA Liang-yan. Study on hydroprocessing technology and catalysts of LTCT from polygeneration[D]. Hangzhou: Zhejiang University, 2015.
6. [6]
  FENG X, LI D, CHEN J H, NIU M L, LIU X, LESTER L T, LI W H. Kinetic parameter estimation and simulation of trickle-bed reactor for hydrodesulfurization of whole fraction low-temperature coal tar[J]. Fuel, 2018,230:113-125. doi: 10.1016/j.fuel.2018.05.023
7. [7]
  ZHANG Shi-wan. Study on light-end products of coal tar with catalytic hydrogenation and catalyst[D]. Shanghai: East China University of Science and Technology, 2012.
8. [8]
  ZHANG H Y, CHEN G W, BAI L, CHANG N, WANG Y G. Selective hydrogenation of aromatics in coal-derived liquids over novel NiW and NiMo carbide catalysts[J]. Fuel, 2019,244:359-365. doi: 10.1016/j.fuel.2019.02.015
9. [9]
  VAN N B, DOROTHEE L, PAVEL A, CHRISTOPHE G. Hydrodeoxygenation of guaiacol with CoMo catalysts. Part Ⅰ:Promoting effect of cobalt on HDO selectivity and activity[J]. Appl Catal B:Environ, 2011,101(3/4):239-245.
10. [10]
  ZHANG D Q, DUAN A J, ZHAO Z, WANG X Q, JIANG G Y, LIU J, WANG C Y. Synthesis, characterization and catalytic performance of meso-microporous material Beta-SBA-15-supported NiMo catalysts for hydrodesulfurization of dibenzothiophene[J]. Catal Today, 2011,175(1):477-484. doi: 10.1016/j.cattod.2011.03.060
11. [11]
  XU Nan, LIANG Nai-sen, ZHANG Shun-guang, DUAN Yan, HOU Kai-hu. Synthesis of β-MCM-41 and its application in gasoline isomerization/hydrodesulfurization[J]. Acta Pet Sin(Pet Process Sect), 2012,28(6):913-919. doi: 10.3969/j.issn.1001-8719.2012.06.005
12. [12]
  MENG J P, WANG Z Y, MA Y H, LU J Y. Hydrocracking of low-temperature coal tar over NiMo/Beta-KIT-6 catalyst to produce gasoline oil[J]. Fuel Process Technol, 2017,165:62-71. doi: 10.1016/j.fuproc.2017.05.009
13. [13]
  KAZAKOV M O, NADEINA K A, DANILOVA I G, DIK P P, KLIMOV O V, PEREYMA V Y, PAUKSHTIS E A, GOLUBEV I S, PROSVIRIN I P, GERASIMOV E Y, DOBRYAKOVA I V, KNYAZEVA E E, IVANOVA I I, NOSKOV A S. Influence of USY zeolite recrystallization on physicochemical properties and catalytic performance of NiMo/USY-Al₂O₃ hydrocracking catalysts[J]. Catal Today, 2019,329:108-115. doi: 10.1016/j.cattod.2019.01.003
14. [14]
  RAYO P, TORRES M P, CENTENTO G, FERNANDO A, JOSE A D, ANCHEYTA J. Effect of silicon incorporation method in the supports of NiMo catalysts for hydrotreating reactions[J]. Fuel, 2019,239:1293-1303. doi: 10.1016/j.fuel.2018.10.102
15. [15]
  FERRAZ S, ZOTIN F, ARAUJO L. Influence of support acidity of NiMoS catalysts in the activity for hydrogenation and hydrocracking of tetralin[J]. Appl Catal A:Gen, 2010,384(1):51-57.
16. [16]
  CHEN Song, XU Jie, YANG Yong-rong, WANG Jing-dai, ZHANG Xiao-ping, ZHANG Kui-xi. Nanometer β zeolite made from mesoporous zeolite and its hydrocracking performance[J]. Chin J Catal, 2006,27(3):255-258. doi: 10.3321/j.issn:0253-9837.2006.03.013
17. [17]
  ZHANG Xue-jun, WANG Zong-xian, GUO Ai-jun, YUAN Zong-sheng, WANG Fu-cun. Modification of zeolite Y for preparation of the maxinizing middle distillates hydrocracking catalyst[J]. J Fuel Chem Technol, 2008,36(5):606-609. doi: 10.3969/j.issn.0253-2409.2008.05.017
18. [18]
  SHALI N B, SUGUNAN S. Influence of transition metals on the surface acidic properties of titania prepared by sol-gel route[J]. Mater Res Bull, 2007,42(9):1777-1783. doi: 10.1016/j.materresbull.2006.11.016
19. [19]
  RAJAGOPAL S, MARZARI J A, MIRANDA R. Silica-alumina-supported Mo oxide catalysts:Genesis and demise of Brønsted-Lewis acidity[J]. J Catal, 1995,151(1):192-203. doi: 10.1006/jcat.1995.1021
20. [20]
  JOSE E, MARIA C B, ANA W G, MARIA A, CORTES J, CARLOS A C, JOSE A T. Highly active P-doped sulfided NiMo/alumina HDS catalysts from Mo-blue by using saccharose as reducing agents precursor[J]. Appl Catal B:Environ, 2018,237:708-720. doi: 10.1016/j.apcatb.2018.06.034
21. [21]
  KLIMOV O V, NADEINA K A, DIK P P, KORYAKINA G I, PEREYMA V Y, KAZAKOV M O, BUDUKVA S V, GERASIMOV E Y, PROSVIRIN I P, KOCHUBEY D I, NOSKOV A S. CoNiMo/Al₂O₃ catalysts for deep hydrotreatment of vacuum gasoil[J]. Catal Today, 2016,271:56-63. doi: 10.1016/j.cattod.2015.11.004
22. [22]
  MENG Xin-xin, QIU Ze-gang, GUO Xing-mei, LI Zhen-rong, HU Nai-fang, SONG Mao-ning, ZHAO Liang-fu. Hydrodenitrogenation and hydrodesulfurization of coal tar on Ni-W catalysts with different metal loadings[J]. J Fuel Chem Technol, 2016,44(5):570-578. doi: 10.3969/j.issn.0253-2409.2016.05.009
23. [23]
  BERIT H, N R J K, HENRSK T E. A density functional study of the chemical differences between Type Ⅰ and Type Ⅱ MoS2-based structures in hydrotreating catalysts[J]. J Phys Chem B, 2005,109(6):2245-2253. doi: 10.1021/jp048842y
24. [24]
  YIN H L, ZHOU T N, LLU Y Q, CHAI Y M, LIU C G. NiMo/Al₂O₃ catalyst containing nano-sized zeolite Y for deep hydrodesulfurization and hydrodenitrogenation of diesel[J]. J Nat Gas Chem, 2011,20(4):441-448. doi: 10.1016/S1003-9953(10)60204-6
25. [25]
  YU F, HAN X, GANG S, LIU H Y, QIAN Y, WANG T H, GONG G B, BAO X J. Citrc acid-assisted hydrothermal method for preparing NiW/USY-Al₂O₃ ultradeep hydrodesulfurization catalysts[J]. J Catal, 2011,279(5):27-35.
26. [26]
  FANG Xiang-chen. Hydrocracking[M]. Beijing:China Petrochemical Press, 2008.
27. [27]
  ZHANG Deng-qian. Synthesis of meso-microporous composite materials and their applications in the catalysts for the hydrodesulfurization of diesel[D]. Beijing: China University of Petroleum, 2010.
28. [28]
  REN Liang, MAO Yi-chao, LIU Kun-hong, NIE Hong. Hydrocracking of decane on different acidity Y zeolite catalysts[J]. Acta Pet Sin(Pet Process Sect), 2009,25(1):31-35. doi: 10.3969/j.issn.1001-8719.2009.01.006
29. [29]
  AROLDY P, JONGE J C M D, MOULIJNN J A. Temperature-programed reduction of molybdenum(Ⅵ) oxide and molybdenum(Ⅳ) oxide[J]. J Phys Chem, 1985,89(21):4517-4526. doi: 10.1021/j100267a021
30. [30]
  HENKER M, WENDLANDT K P, VALYON J, BORNMANN P. Structure of MoO₃/Al₂O₃-SiO₂ catalysts[J]. Appl Catal, 1991,69(1):205-220. doi: 10.1016/S0166-9834(00)83303-5
31. [31]
  SHEILA G A, FATIMA M, LUCIA R, RADDI A, JOSE L Z. Influence of support acidity of NiMoS catalysts in the activity for hydrogenation and hydrocracking of tetralin[J]. Appl Catal A:Gen, 2010,384(1/2):51-57.
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Catalytic performance of NiMo/Al2O3-USY in the hydrocracking of low-temperature coal tar

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通讯作者: 陈斌, bchen63@163.com

Catalytic performance of NiMo/Al₂O₃-USY in the hydrocracking of low-temperature coal tar