摘要
根据纳米自组装机理,分别采用正向胶束法和反向胶束法制备了Mo-Ni-P和Mo-NiNH3浸渍体系的渣油加氢催化剂,考察了不同模板剂对催化剂样品性质及加氢活性的影响。利用氮吸附法、电子探针法对催化剂进行了表征。结果表明,以吐温-80作为模板剂制备的Mo-Ni-P和MoNi-NH3,催化剂FP-ZT 8和FN-ZP 8加氢活性最佳。FP-ZT 8的孔体积为0.34 m L/g,比表面积为187 m~2/g,活性金属质量分数为26.68%,其硫、氮、残炭的脱除率分别达到62.3%,58.9%,50.3%;FN-ZP 8的孔体积为0.38 m L/g,比表面积为185 m~2/g,活性金属质量分数为23.78%,其硫、氮、残炭的脱除率分别达到55.2%,50.9%,44.3%。
Based on nano- self- assembly mechanism,Mo- Ni- P and Mo- Ni- NH3 catalysts were prepared for residue hydrogenation by positive or negative micelle impregnation methods,the obtained catalysts were characterized by N2- adsorption and electron microprobe methods,and the influence of different template agents on properties and activities of the catalysts was investigated. The results showed that FP- ZT 8 and FN- ZP 8 catalysts with Tween- 80 as template agent had the best activity. The pore volume of FP- ZT 8 was 0. 34 m L /g,specific area 187 m2/ g,mass fraction of active metal 26. 68%,and its removal rate of sulfur,nitrogen and carbon residue reached 62. 3%,58. 9%,50. 3% respectively; the pore volume of FN- ZP 8was 0. 38 m L / g,specific area 185 m2/ g,the mass fraction of active metal 23. 87%,and its removal rate of sulfur,nitrogen and carbon residue reached55. 2%,50. 9% and 44. 3% separately.
引文
[1]Bartley G J,Burch R.Zr-containing pillared interlayer clays partⅢinfluence of method of preparation on the thermal and hydrothermal stability[J].Applied Catal,1985,19(2):175-178.
[2]Cooper B H,Donnis B B L.Reaction site on oxygenated metal surfaces[J].Applied Catalysis A:General,1996,137(1):203-205.
[3]Wang D C.In situ synthesis of nano particles via supersolubilizing micelle self-assembly[J].Sci China Ser B:Chem,2007,50(1):105-113.
[4]Schafer E,Thurn A T,Russell T P,et a1.Electrically induced structure formation and pattern transfer[J].Nature,2004,403(3):874-877.
[5]Dale S,Elaine C.Hydrogen cost and issues:Gasification vs SMR[C].NPRA 2008 Annual Meeting,Salt Lake City:NPRA,2008.
[6]王鼎聪.纳米自组装合成大孔容介孔氧化铝[J].中国科学B辑(化学),2009,39(5):420-431.
[7]张凯,王鼎聪.第三次纳米自组装制备大孔主客体催化材料[J].中国科学B辑(化学),2013,43(1):1-9.
[8]Gao R,Wang L D,Geng Y,et al.Effects of an intercalation nanocomposite at the photoanode/electrolyte interface in quasi-solid dye-sensitized solar cells[J].The Journal of Physical Chemistry C,2011,115(1):17986-17992.
[9]Breen T L,Tien J,Oliver S R J,et a1.Design and self-assembly of open regular 3D-mesostructures[J].Science,1999,284(5):948-951.
[10]Zhong B Y,Ming H Q,He X L,et al.Preparation of amorphous Ni-Co-B alloys and the effect of cobalt on their hydrogenation activity[J].Applied Catalysis A:General,1997,163(1/2):1-13.
[11]Ono T,Ohguchi Y,Togari O.Stud Surf Sci Catal[M].Amsterdam:Elsevier Science,1983:631-641.
[12]Topsoe H,Ramasse Q M,Brorson M,et al.Visualizing the stoichiometry of industrial-style co-mo-s catalysts with singleatom sensitivity[J].Angewandte Chemie,2014,53(40):10723-10727.