Citation: YAN Jing-sen, WANG Hai-yan, LI Su-kui, LI Xiao-hui. Effects of support on hydrodenitrogenation activity of nickel phosphide catalysts[J]. Journal of Fuel Chemistry and Technology, ;2014, 42(3): 362-369. shu

Effects of support on hydrodenitrogenation activity of nickel phosphide catalysts

YAN Jing-sen ^1,2,3 ,
WANG Hai-yan ^1,2,, ,
LI Su-kui ² ,
LI Xiao-hui ³

1.
1. China University of Petroleum (East China), Qingdao 266555, China;

Corresponding author: WANG Hai-yan,
Received Date: 19 August 2013
Available Online: 11 October 2013

The effects of the support on active site formation and hydrodenitrogenation(HDN) activity of nickel phosphide catalysts were examined, using TiO₂, Al₂O₃ and TiO₂-Al₂O₃, composite supports. A series of TiO₂-Al₂O₃ prepared by hydrolysis and deposition of tetrabutyl titanate on macropore Al₂O₃, and the supported nickel phosphide catalyst, were prepared by incipient wetness impregnation and in situ H₂ reduction method. The samples were characterized by X-ray diffraction(XRD), BET surface area, transmission electron microscopy(TEM) and H₂ temperature-programmed reduction(H₂-TPR).Their hydrodenitrogenation(HDN) performance were evaluated on a continuous-flow fixed-bed reactor by using quinoline as the model molecules. The results showed that the TiO₂-Al₂O₃ composite support still retained the pore properties of macropore Al₂O₃, and TiO₂ were well dispersed on the Al₂O₃ surface in the form of anatase. Different supports have great influence on the reduction behaviour of the oxidic precusors and HDN activity of phosphide catalysts. The main active phase after reduction was Ni₂P phase for the TiO₂ and TiO₂-Al₂O₃ supportd catalyst, but only Ni₁₂P₅ appeared for the Al₂O₃ supported catalyst. The order of HDN activities of nickel phosphide reduced at optimal reaction conditions was TiO₂-Al₂O₃ > Al₂O₃> TiO₂. TiO₂-Al₂O₃ supported catalyst with the Ti /Al atomic ratio of 1:8 exhibited the highest HDN activity among all catalysts. The presence of TiO₂ weakened the strong interaction between the Al₂O₃ and phosphate, and contributed to the formation of Ni₂P active phase and the improvement of HDN activity.
- nickel phosphide,
- titania,
- alumina,
- composite support,
- hydrodenitrogenation,
- quinoline
1. [1]
  [1] OYAMA S T. Novel catalysts for advanced hydroprocessing: Transition metal phosphides[J]. J Catal, 2003, 216(2): 343-352.
2. [2]
  [2] OYAMA S T, GOTT T, ZHAO H Y, LEE Y K. Transition metal phosphide hydroprocessing catalysts: A review[J]. Catal Today, 2009, 143(1/2): 94-107.
3. [3]
  [3] CLARK P, OYAMA S T. Alumina-supported molybdenum phosphide hydroprocessing catalysts[J]. J Catal, 2003, 218(1): 78-87.
4. [4]
  [4] SUN F X, WU W C, WU Z L, GUO J, WEI Z B, YANG Y X, JIANG Z X, TIAN F P, LI C. Dibenzothiophene hydrodesulfurization activity and surface sites of silica-supported MoP, Ni₂P, and NiMoP catalysts[J]. J Catal, 2004, 228(2): 298-310.
5. [5]
  [5] WANG A J, RUAN L F, TENG Y, LI X, LU M H, REN J, WANG Y, HU Y K. Hydrodesulfurization of dibenzothiophene over siliceous MCM-41-supported nickel phosphide catalysts[J]. J Catal, 2005, 229(2): 314-321.
6. [6]
  [6] SHU Y, OYAMA S T. Synthesis, characterization, and hydrotreating activity of carbon-supported transition metal phosphide[J]. Carbon, 2005, 43(7): 1517-1532.
7. [7]
  [7] KORANYI T I, VíT Z, PODUVAL D G, RYOO R, KIM H C, HENSEN E J M. SBA-15-supported nickel phosphide hydrotreationg catalysts[J]. J Catal, 2008, 253(1): 119-131.
8. [8]
  [8] RAMIREZ J, MACIAS G, CEDENO L, GUTIERREZ-ALEJANDRE, A, CUEVAS R, CASTULLO P. The role of titania in supported Mo, CoMo, NiMo and NiW hydrodesulfurization catalysts: Analysis of past and new evidences[J]. Catal Today, 2004, 98(1): 19-30.
9. [9]
  [9] DAMYANOVA S, SPOJAKINA A, JIRATIVA K. Effect of mixed titania-alumina supports on the phase composition of NiMo/TiO₂-Al₂O₃ catalysts[J]. Appl Catal A: Gen, 1995, 125(2): 257-269.
10. [10]
  [10] 鲁墨弘, 王安杰, 李翔, 胡永康, 单玉华. TiO₂的加入对非负载的Ni₂P催化剂加氢脱氮性能的促进作用[J]. 石油学报(石油加工), 2009, 25(4): 522-526. (LU Mo-hong, WANG An-jie, LI Xiang, HU Yong-kang. Effect of TiO₂ addition methods on hydrodenitrogenation performance of nickel phosphide[J]. Acta Petrolei Sinica(Petroleum Processing Section.), 2009, 25(4): 496-502.)
11. [11]
  [11] 宋华, 于洪坤, 武显春, 郭云涛. TiO₂-Al₂O₃载体的制备及Ni₂P/TiO₂-Al₂O₃催化剂上的同时加氢脱硫和加氢脱氮反应[J]. 催化学报, 2010, 31(4): 447-453. (SONG Hua, YU Hong-kun, WU Xian-chun, GUO Yun-tao. Preparation of TiO₂-Al₂O₃ support and simutaneous hydrodesulfurization and hydrodenitrogenation over Ni₂P/TiO₂-Al₂O₃ catalyst[J]. Chinese Journal of Catalysis, 2010, 31(4): 447-453.)
12. [12]
  [12] OYAMA S T, WANG X, LEE Y K, BANDO K, REQUEJO F G. Effect of phosphorus content in nickel phosphide catalysts studied by XAFS and other techniques[J]. J Catal, 2002, 210(1): 207-217.
13. [13]
  [13] WANG X, CLARK P, OYAMA S T. Synthesis, characterization, and hydrotreating activity of several iron group transition metal phosphides[J]. J Catal, 2002, 208(2): 321-331.
14. [14]
  [14] SCHEFFER B, ARNOLDY P, MOULIJN J A. Sulfidability and hydrodesulfurization activity of Mo catalysts supported on alumina, silica and carbon[J]. J Catal, 1988, 112(2): 516-527.
15. [15]
  [15] 辛勤, 罗孟飞. 现代催化研究方法[M]. 北京: 科学出版社, 2009: 1-41. (XIN Qin, LUO Meng-fei. Modern catalysis research methods[M]. Beijing: Science Press, 2009: 1-41.)
16. [16]
  [16] 史媛媛. 载体焙烧温度对氧化铝负载磷化镍结构及HDC 性能的影响[D]. 天津: 天津大学, 2010. (SHI Yuan-yuan. Effect of support calcination temperature on structure and performance of Al₂O₃-supported nickel phosphide catalysts[D]. Tianjin: University of Tianjin, 2010.)
17. [17]
  [17] CLARK P A, OYAMA S T. Alumina-supported molybdenum phosphidehydroprocessing catalysts[J]. J Catal, 2003, 218(1): 78-87.
18. [18]
  [18] KAO C, TSAI S, BAHL M. Electronic properties, structure and temperature-dependent composition of nickel deposited on rutile titanium dioxide(110) surfaces[J]. Surf Sci, 1980, 95(1): 1-14.
19. [19]
  [19] ARMBRUSTER T. Phase relations and exsolution phenomena in the system NiO-TiO₂[J]. Solid State Chem, 1981, 36(3): 275-288.
20. [20]
  [20] LI M F, LI H F. Effect of surface characteristics of different alumina on metal-support interaction and hydrodesulfurization activity[J]. Fuel, 2009, 88: 1281-1285.
21. [21]
  [21] 鲁墨弘.磷化镍催化剂的制备及其加氢脱氮反应性能研究[D].大连: 大连理工大学, 2007. (LU Mo-hong. Preparation and performance of nickel phosphide catalyst for hydrodenitrogenation[D]. Beijing: Dalian University of Technology, 2007.)
22. [22]
  [22] 曲本连, 柴永明, 相春娥, 张景成, 刘晨光.磷化镍和磷化钼催化剂的原位XRD研究[J].石油学报(石油加工), 2009, 25(4): 496-502. (QU Ben-lian, CHAI Yong-ming, XIANG Chun-e, ZHANG Jing-cheng. In-situ XRD study of nickel phosphide and molebednum phosphide catalysts[J]. Acta Petrolei Sinica(Petroleum Processing Section.), 2009, 25(4): 496-502.
23. [23]
  [23] KUMAR S R, PILLAI S C, HAREESH U S, MUKUNDAN P, WARRIER K G K. Synthesis of thermally stable, high surface area anatase-alumina mixed oxides[J]. Mater Lett, 2000, 286: 43-46.
24. [24]
  [24] SATTERFIELD C N, COCCHETTO J F. Reaction network and kinetics of the vapor-phase catalytic hydrodenitrogenation of quinoline[J]. Ind Eng Chem Proc Des Dev, 1981, 20(1): 53-62.
25. [25]
  [25] JIAN M, PRINS R. Mechanism of the hydrodenitrogenation of quinoline over NiMo(P)/Al₂O₃ catalysts[J]. J Catal, 1998, 179(1): 18-27.
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