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

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Abstract

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 N2-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 β-CoMoO4 was a component of all the catalysts (in the as-prepared oxidic form) together with alumina supported MoO x surface species. The only phase detected with XRD was γ-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.

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Acknowledgments

Financial support from The Danish Council for Strategic Research (DSF: 2106-08-0039) and the German Research Foundation (DFG: MA 3333/2-1) is acknowledged. We are very grateful to Pablo Beato (Haldor Topsøe A/S) for supporting the Raman measurements and to Thomas W. Hansen and Jakob B. Wagner (DTU-CEN) for supporting the TEM measurements. MH thanks DTU Chemical Engineering for co-funding a PhD scholarship.

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Authors and Affiliations

  1. Department of Chemical and Biochemical Engineering, Technical University of Denmark (DTU), Søltofts Plads, Building 229, 2800, Lyngby, Denmark

    Martin Høj, Anker Degn Jensen & Jan-Dierk Grunwaldt

  2. Department of Production Engineering, Foundation Institute of Material Science (IWT), University of Bremen, Badgasteiner Str. 3, 28359, Bremen, Germany

    David K. Pham & Lutz Mädler

  3. Haldor Topsøe A/S, Nymøllevej 55, 2800, Lyngby, Denmark

    Michael Brorson

  4. Institute for Chemical Technology and Polymer Chemistry (ICTP), Karlsruhe Institute of Technology (KIT), Engesserstr. 20, 76131, Karlsruhe, Germany

    Jan-Dierk Grunwaldt

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  1. Martin Høj
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  2. David K. Pham
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  3. Michael Brorson
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  4. Lutz Mädler
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  6. Jan-Dierk Grunwaldt
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Correspondence to Jan-Dierk Grunwaldt.

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Høj, M., Pham, D.K., Brorson, M. et al. Two-Nozzle Flame Spray Pyrolysis (FSP) Synthesis of CoMo/Al2O3 Hydrotreating Catalysts. Catal Lett 143, 386–394 (2013). https://doi.org/10.1007/s10562-013-0990-x

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