Abstract
The application of Mössbauer emission spectroscopy to study cobalt based Fischer–Tropsch catalysts for the gas-to-liquids process was investigated. It was shown that Mössbauer emission spectroscopy could be used to study the oxidation of cobalt as a deactivation mechanism of high loading cobalt based Fischer–Tropsch catalysts. Oxidation was observed under conditions that are in contradiction with the bulk cobalt phase thermodynamics. This can be explained by oxidation of small cobalt crystallites or by surface oxidation. The formation of re-reducible Co3+ species was observed as well as the formation of irreducible Co3+ and Co2+ species that interact strongly with the alumina support. The formation of the different cobalt species depends on the oxidation conditions. Iron was used as a probe nuclide to investigate the cobalt catalyst preparation procedure. A high-pressure Mössbauer emission spectroscopy cell was designed and constructed, which creates the opportunity to study cobalt based Fischer–Tropsch catalysts under realistic synthesis conditions.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Eisberg, B. and Fiato, R. A., Stud. Surf. Sci. Catal. 199 (1998), 961.
Senden, M. M. G., Punt, A. D. and Hoek, A., Stud. Surf. Sci. Catal. 199 (1998), 943.
van Berge, P. J., Barradas, S., Caricato, E. A., Sigwebela, B. H. and van de Loosdrecht, J., Proc.Worldwide Catalyst Industry Conference CatCon2000, 12–13 June 2000, Houston, USA.
Espinoza, R. L., Steynberg, A. P., Jager, B. and Vosloo, A. C., Appl. Catal. A 186 (1999), 13.
van Berge, P. J. and Everson, R. C., Stud. Surf. Sci. Catal. 107 (1997), 207.
Leviness, S., Mart, C. J., Behrmann, W. C., Hsia, S. J. and Neskora, D. R., WO 98/50487.
Iglesia, E., Soled, S. L., Fiato, R. A. and Via, G. H., J. Catal. 141 (1993), 345.
Schanke, D., Hilmen, A. M., Bergene, E., Kinnari, K., Rytter, E., Adnanes, E. and Holmen, A., Catal. Lett. 34 (1995), 269.
Anderson, R. B., In: P. H. Emmett (ed.), Catalysis, Vol. IV, Reinhold, New York, 1956.
Bolt, H., Ph.D. thesis, University of Utrecht, The Netherlands, 1994.
Hoff, A., Blekkan, E. A., Holmen, A. and Schanke, D., Proceedings of the 10th International Congress on Catalysis, 19–24 July 1992, Budapest, Hungary, Elsevier Science Publishers B.V., 1993, p. 2067.
Iglesia, E., Stud. Surf. Sci. Catal. 107 (1997), 153.
Hilmen, A. M., Schanke, D., Hanssen, K. F. and Holmen, A., Appl. Catal. A 186 (1999), 169.
Niemantsverdriet, J. W., Stud. Surf. Sci. Catal. 79 (1993), 393.
Delgass, W. N., Haller, G. L., Kellerman, R. and Lunsford, J. H., Spectroscopy in Heterogeneous Catalysis, Academic Press, New York, San Fransico, London, 1979.
Niemantsverdriet, J. W., van der Kraan, A. M. and Delgas, W. N., J. Catal. 89 (1984), 138.
van der Kraan, A. M., Nonnekens, R. C. H., Stoop, F. and Niemantsverdriet, J.W., Appl. Catal. 27 (1986), 285.
van de Loosdrecht, J., van Dillen, A. J., van der Horst, A. A., van der Kraan, A. M. and Geus, J. W., Top. Catal. 2(1–4) (1995), 29.
Topsøe, H. and Clausen, B. S., Catal. Rev. – Sci. Eng. 26 (1984), 395.
Crajé, M. W. J., de Beer, V. H. J., van Veen, J. A. R. and van der Kraan, A. M., In: M. L. Occelli and R. R. Chianelli (eds.), Hydrotreating Technology for Pollution Control, Chemical Industries Series, Vol. 67, Marcel Dekker, New York, 1996, p. 95.
Bartholomew, C. H., Neubauer, L. R. and Smith, P. A., Proceedings of the 10th International Congress on Catalysis, 19–24 July 1992, Budapest, Hungary, Elsevier Science Publishers B.V. 1993, p. 821.
van Berge, P. J., van de Loosdrecht, J., Barradas, S. and van der Kraan, A. M., Catal. Today 58 (2000), 321.
Crajé, M. W. J., de Beer, V. H. J., van Veen, J. A. R. and van der Kraan, A. M., J. Catal. 143 (1993), 601.
van der Kraan, A. M. and Niemantsverdriet, J. W., In: G. J. Long and J. G. Stevens (eds), Industrial Application of the Mössbauer Effect, Plenum Press, New York, 1986, p. 609.
Wivel, C., Clausen, B. S., Candia, R., Mørup, S. and Topsøe, H., J. Catal. 87 (1984), 497.
Spencer, C. D. and Schroerr, D., Phys. Rev. B 9 (1974), 3658.
Schulz, H. and Geertsema, A., Erdöl und Kohle 30 (1969), 193.
Espinoza, R. L., Visagie, J. L., van Berge, P. J. and Bolder, F. H., US patent 5,733,839, 1998.
Chanenchuk, C. A., Yates, I. C. and Satterfield, C. N., Energy and Fuels 5 (1991), 847.
Yates, I. C. and Satterfield, C. N., Energy and Fuels 5 (1991), 168.
Crajé, M. W. J., van der Kraan, A. M., van de Loosdrecht, J. and van Berge, P. J., Catal. Today 71 (2002), 369.
Author information
Authors and Affiliations
Rights and permissions
About this article
Cite this article
van de Loosdrecht, J., van Berge, P.J., Crajé, M.W.J. et al. The Application of Mössbauer Emission Spectroscopy to Industrial Cobalt Based Fischer–Tropsch Catalysts. Hyperfine Interactions 139, 3–18 (2002). https://doi.org/10.1023/A:1021265701186
Issue Date:
DOI: https://doi.org/10.1023/A:1021265701186