Two-Nozzle Flame Spray Pyrolysis (FSP) Synthesis of CoMo/Al2O3 Hydrotreating Catalysts

被引:27
|
作者
Hoj, Martin [1 ]
Pham, David K. [2 ]
Brorson, Michael [3 ]
Maedler, Lutz [2 ]
Jensen, Anker Degn [1 ]
Grunwaldt, Jan-Dierk [1 ,4 ]
机构
[1] Tech Univ Denmark, Dept Chem & Biochem Engn, DK-2800 Lyngby, Denmark
[2] Univ Bremen, Fdn Inst Mat Sci IWT, Dept Prod Engn, D-28359 Bremen, Germany
[3] Haldor Topsoe Res Labs, DK-2800 Lyngby, Denmark
[4] Karlsruhe Inst Technol, Inst Chem Technol & Polymer Chem ICTP, D-76131 Karlsruhe, Germany
关键词
Flame spray pyrolysis; Hydrotreating; Cobalt-molybdenum; Nanoparticle; Sulfidation; CO-MO-S; HYDRODESULFURIZATION CATALYSTS; MOSSBAUER EMISSION; RAMAN; METAL; NANOCLUSTERS; BEHAVIOR; COMOO4; NIMOO4; PHASE;
D O I
10.1007/s10562-013-0990-x
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Two-nozzle frame spray analysis (FSP) synthesis of CoMo/Al2O3 where Co and Al are sprayed in separate flames was applied to minimize the formation of CoAl2O4 observed in one-nozzle flame spray pyrolysis (FSP) synthesis and the materials were characterized by N-2-adsorption (BET), X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy, Raman spectroscopy, transmission electron microscopy, and catalytic performances in hydrotreating. By varying the flame mixing distances (81-175 mm) the amount of CoAl2O4 could be minimized. As evidenced by UV-vis spectroscopy, CoAl2O4 was detected only at short flame mixing distances, where the flame conditions resemble one-nozzle FSP. Raman spectroscopy revealed that beta-CoMoO4 was a component of all the catalysts (in the as-prepared oxidic form) together with alumina supported MoOx surface species. The only phase detected with XRD was gamma-Al2O3. The FSP synthesized oxidic catalysts were activated by sulfidation without further heat treatments. The hydrodesulfurization activity of the best two-nozzle FSP catalysts, compared to the one-nozzle FSP catalysts, improved from 75 to 91 % activity relative to a commercial reference catalyst and the hydrodenitrogenation activity improved from 70 to 90 % relative activity. This suggests that better promotion of the active molybdenum sulfide phase was achieved when using two-nozzle FSP synthesis, probably due to less formation of the undesired phase CoAl2O4, which makes Co unavailable for promotion.
引用
收藏
页码:386 / 394
页数:9
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