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Russian Chemical Bulletin

, Volume 42, Issue 6, pp 1032–1038 | Cite as

Synthesis of hydrocarbons from CO and H2 on SiO2 supported iron-cobalt clusters

  • V. I. Koval'chuk
  • B. N. Kuznetsov
  • N. M. Mikova
  • A. A. Efremov
  • N. I. Bakhmutova
Physical Chemistry
  • 36 Downloads

Abstract

Bimetallic catalysts (Fe+Co)/SiO2 were prepared by impregnation of SiO2 with solutions of carbonyl clusters [FeCo3(CO)12][(C2H5)4N], [Fe3Co(CO)13][(C2H5)4N], HFeCo3(CO)12, [Fe5CoC(CO)16][(C2H5)4N], and Co2(CO)8, Fe(CO)5. At 20 °C, no reaction occurs between the compounds supported and the surface of the support. The stability of the supported clusters to thermodecarboxylation in a hydrogen atmosphere depends on their composition and is the highest for the catalyst [FeCo3(CO)12]/SiO2. The catalytic properties of supported clusters in CO hydrogenation are mostly determined by the preactivation technique. The properties of Fe-Co catalysts which were pretreated at high temperatures, are in general similar to those of standard metal catalysts. Product distribution for the same samples prepared without preactivation does not fit the Schulz-Flory equation. The catalyst HFeCo3(CO)12/SiO2 favors the formation ofC1–C11 hydrocarbons in the temperature range of 468–473 K; the catalyst [Fe3Co(CO)13]/SiO2 gives ethylene in the temperature range of 453–473 K.

Key words

carbonyl clusters supported silica gel carbon monoxide hydrogen hydrogenation olefins thermodesorption 

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References

  1. 1.
    J. Zwart and R. Snel,J. Mol. Catal., 1985,30, 305.Google Scholar
  2. 2.
    A. L. Lapidus and M. M. Savel'ev,Usp. Khim., 1988,57, 29 [Russ. Chem. Rev., 1988,57 (Engl. Transl.)].Google Scholar
  3. 3.
    A. S. Lisitsyn, A. V. Golovin, A. L. Chuvilin, V. L. Kuznetsov, A. V. Romanenko, A. F. Danilyuk, and Yu. I. Yermakov,Appl. Catal., 1989,55, 235.Google Scholar
  4. 4.
    J. M. Basset, J. P. Candy, A. Choplin, M. Leconte, and A. Theolier,Aspects Homogen. Catal., 7, Dordrecht etc., 1990. 85.Google Scholar
  5. 5.
    A. Fukuoka, T. Kimura, N. Kosugi, H. Kuroda, Y. Minai, Y. Sakai, T. Tominaga, and M. Ichikawa,J. Catal., 1990,126, 434.Google Scholar
  6. 6.
    R. Hemmerich, W. Keim, and M. Roper,J. Chem. Soc., Chem. Commun., 1983, 428.Google Scholar
  7. 7.
    M. Roper, R. Hemmerich, and W. Keim,Chem. Ing. Techn., 1984,56, 152.Google Scholar
  8. 8.
    R. S. Armstrong, T. Bell, A. L. Chaffee, V. W. Chin, H. J. Loeh, A. B. J. Lucchese, A. F. Masters, and M. A. Williams,Appl. Catal., 1989,47, 243.Google Scholar
  9. 9.
    A. A. Chen, M. Kaminsky, G. L. Geoffroy, and M. A. Vannice,J. Phys. Chem., 1986,90, 4810.Google Scholar
  10. 10.
    Yu. V. Maksimov, V. V. Matveev, I. P. Suzdalev, A. A. Slinkin, E. A. Fedorovskaya, T. I. Khomenko, N. A. Kutyreva, and A. A. Kadushin,Kinet. Katal, 1989,30, 1188 [Rinet. and Catal., 1989,30 (Engl. Transl.)].Google Scholar
  11. 11.
    R. B. King and F. G. A. Stone,Inorg. Synth., 1963,7, 193.Google Scholar
  12. 12.
    P. C. Steinhardt, W. L. Gladfelter, D. Harlcy, J. Fox, and G. L., Geoffroy,Inorg. Chem., 1980,19, 332.Google Scholar
  13. 13.
    P. Chini, L. Colli, and M. Peraldo,Gazz. Chim. Ital., 1960,90, 1005.Google Scholar
  14. 14.
    V. E. Lopatin, M. Ts. Tsybenov, N. M. Mikova, and S. P. Gubin,Koordinats. Khim., 1985,11, 1099 [Sov. Coordinat. Chem., 1985,11 (Engl. Transl.)].Google Scholar
  15. 15.
    E. Gudlielminotti, D. Osella, and P. L. Stanghellini,J. Organometal. Chem., 1985,281, 291.Google Scholar
  16. 16.
    A. Choplin, L. Huang, J. M. Basset, R. Mathieu, U. Siriwardane, and S. G. Shore,Organometallics, 1986,5, 1547.Google Scholar
  17. 17.
    A. L. Lapidus, M. M. Savel'ev, L. T. Kondrat'ev, L. M. Muranova, I. G. Borisovich, and V. E. Wasserberg,Khimicheskii sintez na osnove odnouglerodnych molekul. Tez, dokl. Vses. soveshch., [Chemical Synthesis on the Basis of C 1 Molecules, All-Union Workshop, Abstracts], Nauka, Moscow, 1984, 4 (in Russian).Google Scholar
  18. 18.
    A. Choplin, L. Huang, A. Theolier, P. Gallezot, and J. M. Basset,J. Am. Chem. Soc., 1986,108, 4224.Google Scholar
  19. 19.
    M. Kaminsky, K. L. Yoon, G. L. Geoffroy, and M. A. Vannice,J. Catal., 1985,91, 338.Google Scholar
  20. 20.
    T. Shigematsu, K. Kodama, and N. Nakanishi,Chemistry Express, 1987,2, 317.Google Scholar
  21. 21.
    M. E. Dry,Catalysis, Science and Technology,1, Eds. J. R. Anderson and M. Boudart, Springer-Verlag, Berlin, 1989, 159.Google Scholar
  22. 22.
    L. Bruce, G. Hope, and T. W. Turney,React. Kinet. Catal. Lett., 1981,20, 175.Google Scholar
  23. 23.
    J. M. Basset, B. Besson, A. Choplin, F. Hugues, M. Leconte, D. Rojas, A. K. Smith, A. Theolier, Y. Chaovin, D. Commereuc, R. Psaro, R. Ugo, and G. M. Zanderighi,Fundam. Res. Homogeneous Catal.,4, New York-London, 1984, 19.Google Scholar
  24. 24.
    P. Biloen,Rec. Trav. Chim. Phys.-Bas., 1980,99, 33.Google Scholar

Copyright information

© Plenum Publishing Corporation 1994

Authors and Affiliations

  • V. I. Koval'chuk
    • 1
  • B. N. Kuznetsov
    • 1
  • N. M. Mikova
    • 1
  • A. A. Efremov
    • 1
  • N. I. Bakhmutova
    • 1
  1. 1.Institute of Chemistry of Natural Organic Raw MaterialsRussian Academy of SciencesKrasnoyarskRussian Federation

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