Citation: 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]. Journal of Fuel Chemistry and Technology, ;2016, 44(5): 570-578. shu

Hydrodenitrogenation and hydrodesulfurization of coal tar on Ni-W catalysts with different metal loadings

MENG Xin-xin ^1,2 ,
QIU Ze-gang ³ ,
GUO Xing-mei ^1,*,, ,
LI Zhen-rong ² ,
HU Nai-fang ² ,
SONG Mao-ning ^1,2 ,
ZHAO Liang-fu ^2,*,,

1.
College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, China
2.
Laboratory of Applied Catalysis and Green Chemical Engineering Institute of Coal Chemistry Chinese Academy of Sciences, Taiyuan 030001, China
3.
College of Chemistry and Chemical Engineering, Xi'an University of Petroleum, Xi'an 710065, China

Corresponding author: GUO Xing-mei, linyrain@163.com ZHAO Liang-fu, lfzhao@sxicc.ac.cn
Received Date: 23 October 2015
Revised Date: 2 February 2016

Fund Project: the Strategic Science and Technology Project of Chinese Academy of Science XDA07020200the Development of Gasification Coal Tar Hydrogenation in Furnace of Lu Qi CFBYKJ-JSFW-01-2014

Figures(7)

The γ-Al₂O₃ supported Ni-W catalysts with different metal contents for the hydroprocessing of low and middle-temperature coal tar were prepared and characterized by the X-ray diffractogram (XRD), X-ray photoelectron spectroscopy (XPS), temperature programmed desorption of NH₃ (NH₃-TPD), N₂ adsorption and high resolution transmission electron microscopy (HRTEM). The hydrodenitrogenation (HDN) and hydrodesulfurization (HDS) performances of the catalysts were evaluated by using low and middle temperature coal tar. The results show that the sulfidation degree of the catalysts increases with increasing metal content within a certain range, while the amount of total acid that mainly consists of intermediate acid decreases. The HDN activity of the catalysts with Ni/W atomic ratio of 0.786 increases initially and reaches an optimum value at 24% WO₃, and then decreases, while the HDS activity increases gradually.
- coal tar,
- hydrodenitrogenation and hydrodesulfurization,
- Ni-W,
- catalyst
1. [1]
  MA Bao-qi, REN Pei-jian, YANG Zhan-biao, WANG Shu-kuan. Preparation of Fuel Oil from Coal Tar[M]. Beijing: Chemical Industry Press, 2011.
2. [2]
  LI Da-dong. Hydrotreating Technology and Engineering[M]. Beijing: China Petrochemical Press, 2004.
3. [3]
  SHI Lei, ZHANG Zeng-hui, QIU Ze-gang, GUO Fang, ZHANG Wei, ZHAO Liang-fu. Effect of phosphorus modification on the catalytic properties of Mo-Ni/Al₂O₃ in the hydrodenitrogenation of coal tar[J]. J Fuel Chem Technol, 2015,43(1):74-80. doi: 10.1016/S1872-5813(15)60007-X
4. [4]
  GRANGE P, VANHAEREAN X. Hydrotreating catalysts, an old story with new chanllenges[J]. Catal Today, 1997,36(4):375-391. doi: 10.1016/S0920-5861(96)00232-5
5. [5]
  WANG Yong-gang, ZHANG Hai-yong, ZHANG Pei-zhong, XU De-ping, ZHAO Kuan, WANG Fang-jie. Hydroprocessing of low temperature coal tar on NiW/γ-Al₂O₃ catalyst[J]. J Fuel Chem Technol, 2012,40(12):1492-1497.
6. [6]
  LAREDO S G C, DELOSREYES H J A, LUISCANO D J. Inhibition effects of nitrogen compounds on the hydrodesulfurization of dibenzothiophene[J]. Appl Catal A: Gen, 2001,207(1/2):103-112.
7. [7]
  LAREDO S G C, MONTESINOS A, ANTONIO DE LOS REYES J. Inhibition effects observed between dibenzothiophene and carbazole during the hydrotreating process[J]. Appl Catal A: Gen, 2004,265(2):171-183. doi: 10.1016/j.apcata.2004.01.013
8. [8]
  ZHANG Hai-yong, WANG Yong-gang, ZHANG Pei-zhong, LIN Xiong-chao, ZHU Yu-fei. Preparation of NiW catalysts with alumina and zeolite Y for hydroprocessing of coal tar[J]. J Fuel Chem Technol, 2013,41(9):1085-1091. doi: 10.1016/S1872-5813(13)60046-8
9. [9]
  LAREDOS G C, ALTAMIRANO E, DELOSREYES J. Inhibition effects of nitrogen compounds on the hydrodesulfurization of dibenzothiophene: Part 2[J]. Appl Catal A: Gen, 2003,243(2):207-214. doi: 10.1016/S0926-860X(02)00321-6
10. [10]
  QIAN E W, ABE S, KAGAWA Y, IKEDA H. Hydrodenitrogenation of porphyrin on Ni-Mo based catalysts[J]. Chin J Catal, 2013,34(1):152-158. doi: 10.1016/S1872-2067(11)60514-7
11. [11]
  LEWANDOWSKI M, SARBAK Z. The effect of boron addition on hydrodesulfurization and hydrodenitrogenation activity of NiMo/Al₂O₃ catalysts[J]. Fuel, 2000,79(5):487-495. doi: 10.1016/S0016-2361(99)00151-9
12. [12]
  SHI Lei. Studies on the performance of Mo-Ni/Al₂O₃ catalyst in the hydrodenitrogenation of coal tar[D]. Tauyuan: Institute of Coal Chemistry Chinese Aacdemy of Sciences, 2014.
13. [13]
  ZHANG L, AFANASIEV P, LI D D, LONG X Y, VRINAT M. Solution synthesis of the unsupported Ni-Wsulfide hydrotreating catalysts[J]. Catal Today, 2007,130(1):24-31.
14. [14]
  KARAKONSTANTIS L, MATRALIS H, KORDULIS C. Tungsten-oxo-species deposited on alumina. 2. Characterization and catalytic activity of unpromoted W-(Ⅵ)/gamma-Al₂O₃catalysts prepared by equilibrium deposition filtration (EDF) at various pH's and non-dry impregnation (NDI)[J]. J Catal, 1996,162(2):306-319. doi: 10.1006/jcat.1996.0288
15. [15]
  ZHENG Lu-bin. New Solid Acid and Alkali as Well as Their Interaction[M]. Beijing: Chemical Industry Press, 2011.
16. [16]
  DING L H, ZHENG Y, ZHANG Z S, RING Z, CHEN J W. Hydrotreating of light cycle oil using WNi catalysts containing hydrothermally and chemically treated zeolite Y[J]. Catal Today, 2007,125(3):229-238.
17. [17]
  DUGULAN A I, HENSEN E J M, VAN VEEN J A R. Effect of pressure on the sulfidation behavior of NiW catalysts: A 182W Mossbauer spectroscopy study[J]. Today, 2010,150(3/4):224-230.
18. [18]
  HENSENE J M, VAN DER MEER Y, VAN VEEN J A R. Insight into the formation of the active phases in supported NiW hydrotreating catalysts[J]. Appl Catal A: Gen, 2007,322:16-32. doi: 10.1016/j.apcata.2007.01.003
19. [19]
  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.
20. [20]
  NIE Hong, LONG Xiang-yun, LIU Qing-he, LI Da-dong. Effect of citric acid on sulfidation behavior of NiW/Al₂O₃ hydrodesulfurization catalyst[J]. Acta Pet Sin (Pet Process Sect), 2010,26(3):329-335.
21. [21]
  ENGELEN C W R, WOLTHUIZEN J P, VANHOOFF J H C. Reactions of propane over a bifunctional Pt/H-ZSM-5 catalyst[J]. Appl Catal, 1985,19(1):153-163. doi: 10.1016/S0166-9834(00)82677-9
22. [22]
  BRAGIN O V, SHPIRO E S, PREOBRAZGHENSKY A V, PALISHKINA N V, VASINA TV, DYUSENBINA B B, ANTOSHIN G V, MINACHEV K M. The state of platinum in high-silica zeolites and its catalytic activity in ethane aromatization[J]. Bull Acad Sci USSR Div Chem Sci, 1986,35(1):10-15. doi: 10.1007/BF00952835
23. [23]
  SATTERFIELD C N, MODELL M, MAYER J F. Interactions between catalytic hydrodenitrogenation of Hydrodesulfurization thiopene and hydrodenitrogenation of Pyridine[J]. AIChE J, 1975,21(6):1100-1107. doi: 10.1002/(ISSN)1547-5905
24. [24]
  STANISLAUS A, MARAFI A, RANA M S. Recent advances in the science and technology of ultra low sulfur diesel (ULSD) production[J]. Catal Today, 2010,153(1/2):1-68.
25. [25]
  EGOROVA M, PRINS R. Competitive hydrodesulfurization of 4, 6-dimethyl dibenzothiophene, hydrodenitrogenation of 2-methylpyridine, and hydrogenation of naphthalene over sulfided NiMo/γ-Al₂O₃[J]. J Catal, 2004,244(2):278-287.
26. [26]
  EGOROVA M, ROEL P. Mutual influence of the HDS of dibenzothiophene and HDN of 2-methylpyridine[J]. J Catal, 2004,221(1):11-19. doi: 10.1016/S0021-9517(03)00264-1
27. [27]
  SUNDARAMURTHY V, DALAI AK, ADJAYE J. The effect of phosphorus on hydrotreating property of NiMo/γ-Al₂O₃ nitride catalyst[J]. Appl Catal A: Gen, 2008,335(2):204-210. doi: 10.1016/j.apcata.2007.11.024
28. [28]
  JIAN M, PRINS R. Existence of different catalytic sites in HDN catalysts[J]. Catal Today, 1996,30(1/3):127-134.
29. [29]
  HOUALLA M, NAG N K, SAPRE A V. Hydrodesulfurization of dibenzothiophenes catalyzed by sulfided CoMo/γ-Al₂O₃[J]. React Net, 1978,24(4):1015-1021.
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