期刊文献+

以硫化态前驱物制备的NiMoS/γ-Al_2O_3催化剂表面活性相HRTEM研究 被引量:15

INVESTIGATION OF ACTIVE PHASE OF NiMoS/γ-Al_2O_3 PREPARED BY THIOSALT AS PRECURSOR THROUGH HRTEM
下载PDF
导出
摘要 采用硫化态前驱物四硫代钼酸铵溶液浸渍载体γ-Al2O3制备了硫化态NiMoS/γ-Al2O3加氢精制催化剂,对催化剂进行了XRD和HRTEM表征,并以FCC柴油为原料,考察了催化剂的加氢精制性能。结果表明,该加氢催化剂的活性组分与载体γ-Al2O3的相互作用较弱,不存在难以还原硫化的Mo—O—Al桥键,催化剂表面MoS2分散度较好,MoS2的晶粒较大,堆积层数较高,大部分MoS2以Ⅱ型的NiMoS相存在;硫化态NiMoS/γ-Al2O3加氢精制催化剂具有优于工业催化剂CK-2的脱硫、脱氮和脱芳烃性能。 Sulfide NiMoS/γ-Al2O3 hydrotreating catalyst was prepared through impregnating sulfide precursor ammonium tetrathiomolybdate aqua solution into carrier γ-Al2O3 and the catalyst was investigated by means of XRD and high resolution electron microscopy (HRTEM) to get a better understanding of the nature of the active phase. The hydrotreating performance of the catalyst was evaluated with the FCC gas oil as the feed. The results of XRD and HRTEM characterizations indicated that interaction between active components and carrier γ-Al2O3 was weaker through sulfide precursor (ATTM) than that through oxidation precursor, the catalyst prepared by this method could not come into being Mo--O--Al anchors, which were difficult to be reduce-sulfided. The dispersion of MoS2 on NiMoS/γ-Al2O3 catalyst surface was well, and the slab size of MoS2 on NiMoS/γ-Al2O3 surface was bigger and the stacking degree of MoS2 was higher than that on the surface of CK-2, a commercial catalyst, and those MoS2 presented in type Ⅱ NiMoS active phase in a great measure. The evaluation results of FCC gas oil hydrotreating experiment indicated that the performance of sulfide NiMoS/γ-Al2O3 hydrotreating catalyst was a little better than that of commercial catalyst CK-2.
出处 《石油学报(石油加工)》 EI CAS CSCD 北大核心 2007年第3期20-26,共7页 Acta Petrolei Sinica(Petroleum Processing Section)
基金 国家重点基础研究发展规划"973"项目(2004CB217807) 中国石油集团公司应用基础研究重点项目(B04A50502)资助
关键词 四硫代钼酸铵 前驱物 加氢精制催化剂 活性相 高分辨透射电镜(HRTEM) ammonium tetrathiomolybdate precursors hydrotreating catalysts active phases high resolution transmission electron microscope (HRTEM)
  • 相关文献

参考文献30

  • 1DUFRESNE P.Catalyst presulphuration process using two different presulphuration agents:US,5985787[P].1999.
  • 2LABRUYERE F,DUFRESNE P,LACROIX M,et al.Ex-situ sulfidation by alkylpolysulfides:A route for the preparation of highly dispersed supported sulfides[J].Catal Today,1998,43(1-2):111-116.
  • 3BREYSSE M,AFANASIEV P,GEANTET C,et al.Overview of support effects in hydrotreating catalysts[J].Catal Today,2003,86(1-4):5-16.
  • 4TANAKA H,BOULINGUIEZ M,VRINAT M.Hydrodesulfurization of thiophene,dibenzothiophene and gas oil on various Co-Mo/TiO2-Al2O3 catalysts[J].Catal Today,1996,29(1-4):209-213.
  • 5REINHOUDT H R,SIE S T,MOULIJN J A,et al.On the difference between gas-and liquid-phase hydrotreating test reactions[J].Appl Catal A,2001,207(1-2):25-36.
  • 6WANG X Y,ZHAO B Y,XIE Y C,et al.Monolayer dispersion of MoO3,NiO and their precursors on γ-Al2O3[J].Appl Catal A,1999,188(1-2):201-209.
  • 7HILLEROVAE,MORISHIGE H,INAMURA K,et al.Formation of monolayer of molybdena over alumina by unconventional slurry impregnation or solvent assisted spreading method[J].Appl Catal A,1997,156(1):1-17.
  • 8MORROW B A,MCFARLAN A J.Chemical reactions at silica surfaces[J].J Non-Crystal Solids,1990,120 (1-3):61-71.
  • 9HENSEN E J M,DE BEER V H J,VAN VEEN J A R,et al.A refinement on the notion of type Ⅰ and Ⅱ (Co) MoS phases in hydrotreating catalysts[J].Catal Lett,2002,84(1-2):59-67.
  • 10HINNEMANN B,NORSKOV J K,TOPSOE H,et al.A density functional study of the shemical differences between type Ⅰ and type Ⅱ MoS2-Based structures in hydrotreating catalysts[J].J Phys Chem B,2005,109(6):2245-2253.

二级参考文献17

  • 1[1]Marroquin-Sanchez G,Ancheyta-Juarez J.Catalytic hydrotreating of middle distillates blends in a fixed-bed pilot reactor[J].Applied Catalysis A:General,2001,207(1):407-420.
  • 2[2]Macaud M,Milenkovic A,Schulz E,et al.Hydrodesulfurization of alkyldibenzothiophenes:Evidence of highly unreactive aromatic sulfur compounds[J].Journal of Catalysis,2000,193(1),255-263.
  • 3[3]Laudau M V.Deep hydrotreating of middle distillates from crude and shale oils[J].Catalysis Today,1997,36(4):393-429.
  • 4[4]Girgis M J,Gates B C.Reactivities,reaction,networks,and kinetics in high-pressure catalytic hydroprocessing[J].Ind Eng Chem Res,1991,30(9):2021-2058.
  • 5[5]Gilman H,Jcoby A L.Dibenzothiophene:Orientation and derivatives[J].J Org Chem,1938,3:108-119.
  • 6[6]Kuchm-Caubere C,Adach-Becker S,Fort Y,et al.Expeditious and efficient syntheses of pure 4-methyl and 4,6-disubstituted dibenzothiophene[J].Tetrahedron,1996,52(27):9087-9092.
  • 7[7]Bataille F,Lemberton J L,Michaud P,et al.Alkyldibenzothiophene hydrodesulfurization-promoter effect,reactivity,and reaction mechanism[J].Journal of Catalysis,2000,191(1):409-422.
  • 8刘法.柴油馏分超深度加氢脱硫动力学模型研究[D].北京:石油化工科学研究院,2005.
  • 9Joyner R W,Santen R A.Elementary Reaction Steps in Heterogeneous Catalysis[M].Netherlands:Kluwer Academic Publishers,1993.
  • 10Lipsch J M J G,Schuit G C A.The CoO-MoO3-Al2O3 catalyst:Catalytic properties[J].J Catal,1969,15(2):179-189.

共引文献66

同被引文献126

引证文献15

二级引证文献44

相关作者

内容加载中请稍等...

相关机构

内容加载中请稍等...

相关主题

内容加载中请稍等...

浏览历史

内容加载中请稍等...
;
使用帮助 返回顶部