Advertisement

Springer Nature is making SARS-CoV-2 and COVID-19 research free. View research | View latest news | Sign up for updates

Kinetics and mechanism of the oxidative dehydrogenation of ethane over Li/Dy/Mg/O/(Cl) mixed oxide catalysts

The microkinetic reaction network of the oxidative dehydrogenation of ethane to ethene over Li/Dy/Mg/O and Li/Dy/Mg/O/Cl catalysts was investigated. With Li/Dy/Mg/O catalysts, the reaction kinetics is compatible with a heterogeneous-homogeneous radical based reaction mechanism. The formation of ethyl radicals on the surface is concluded to be the rate-determining step. In contrast, the reaction kinetics for Li/Dy/Mg/O/Cl is in line with a purely surface catalyzed reaction mechanism. However, also in this case, alkane activation is rate determining.

This is a preview of subscription content, log in to check access.

References

  1. 1

    T. Blasco J.M. Lopez Nieto (1997) Appl. Catal. A: Gen. 157 117 Occurrence Handle10.1016/S0926-860X(97)00029-X Occurrence Handle1:CAS:528:DyaK2sXkvVOqt7w%3D

  2. 2

    R. Burch E.M. Crabb (1993) Appl. Catal. A: Gen. 97 49 Occurrence Handle10.1016/0926-860X(93)80066-Y Occurrence Handle1:CAS:528:DyaK3sXitlCms7o%3D

  3. 3

    M.A. Bañares (1999) Catal. Today 51 319 Occurrence Handle10.1016/S0920-5861(99)00053-X

  4. 4

    H.H. Kung M.C. Kung (1997) Appl. Catal. A: Gen. 157 105 Occurrence Handle10.1016/S0926-860X(97)00028-8 Occurrence Handle1:CAS:528:DyaK2sXkvVOqt78%3D

  5. 5

    E.A. Mamedov V. Cortés Corberán (1995) Appl. Catal. A: Gen. 127 1 Occurrence Handle10.1016/0926-860X(95)00056-9 Occurrence Handle1:CAS:528:DyaK2MXmtVygtb8%3D

  6. 6

    K. Ruth R. Burch R. Kieffer (1998) J. Catal. 175 27 Occurrence Handle10.1006/jcat.1998.1976 Occurrence Handle1:CAS:528:DyaK1cXis1Ojsro%3D

  7. 7

    S.J. Conway D.J. Wang J.H. Lunsford (1991) Appl. Catal. A: Gen. 79 L1 Occurrence Handle10.1016/0926-860X(91)85001-E Occurrence Handle1:CAS:528:DyaK38XisVeguw%3D%3D

  8. 8

    S. Fuchs L. Leveles K. Seshan L. Lefferts A. Lemonidou J.A. Lercher (2001) Top. Catal. 15 169 Occurrence Handle10.1023/A:1016662101839 Occurrence Handle1:CAS:528:DC%2BD3MXlsV2nurw%3D

  9. 9

    M.V. Landau M.L. Kaliya A. Gutman L.O. Kogan M. Herskowitz P.F. Oosterkamp Particlevan den (1997) Stud. Surf. Sci. Catal. 110 315 Occurrence Handle1:CAS:528:DyaK1cXptlegsA%3D%3D

  10. 10

    M.V. Landau M.L. Kaliya M. Herskowitz P.F. Oosterkamp Particlevan den P.S.G. Bocqué (1996) CHEMTECH 26 24 Occurrence Handle1:CAS:528:DyaK28XpslOlsg%3D%3D

  11. 11

    M. Herskowitz, M.V. Landau and M.L. Kaliya, German Patent DE 19502747C1, 1997.

  12. 12

    L. Leveles (2002) Oxidative dehydrogenation of lower alkanes to olefins Print Partners Ipskamp Enschede

  13. 13

    L. Leveles S. Fuchs K. Seshan J.A. Lercher L. Lefferts (2002) Appl. Catal. A: Gen. 227 287 Occurrence Handle10.1016/S0926-860X(01)00944-9 Occurrence Handle1:CAS:528:DC%2BD38XhtlGisLo%3D

  14. 14

    S. Gaab M. Machli J. Find R.K. Grasselli J.A. Lercher (2003) Top. Catal. 23 151 Occurrence Handle10.1023/A:1024836707308 Occurrence Handle1:CAS:528:DC%2BD3sXls1SmtbY%3D

  15. 15

    R.C. Weast M.J. Astle W.H. Beyer (1986) Handbook of Chemistry and Physics EditionNumber66 CRC Press Florida

  16. 16

    A. Levins M. Straumanis K. Karlsons (1938) Zeitschr. Phys. Chem. B40 146

  17. 17

    M. Straumanis A. Levins K. Karlsons (1938) Zeitschr. Anorg. Allg. Chem. 238 175 Occurrence Handle10.1002/zaac.19382380203 Occurrence Handle1:CAS:528:DyaA1cXlsFOmsQ%3D%3D

  18. 18

    Data on the thermodynamic stability of LiOCl are found in NIST Standard Reference Database 69, June 2005 Release: NIST Chemistry WebBook.

  19. 19

    S.J. Conway J.H. Lunsford (1991) J. Catal. 131 513 Occurrence Handle10.1016/0021-9517(91)90283-A Occurrence Handle1:CAS:528:DyaK3MXls1altb8%3D

  20. 20

    J.A. Roos S.J. Korf R.H.J. Veehof J.G. Ommen Particlevan J.R.H. Ross (1989) Catal. Today 4 441 Occurrence Handle10.1016/0920-5861(89)85040-0 Occurrence Handle1:CAS:528:DyaL1MXitFGqtbg%3D

  21. 21

    J.A. Roos S.J. Korf R.H.J. Veehof J.G. Ommen Particlevan J.R.H. Ross (1989) Appl. Catal. A: Gen. 52 147 Occurrence Handle10.1016/S0166-9834(00)83378-3 Occurrence Handle1:CAS:528:DyaL1MXltFOqsb4%3D

  22. 22

    E. Morales J.H. Lunsford (1989) J. Catal. 118 255 Occurrence Handle10.1016/0021-9517(89)90315-1 Occurrence Handle1:CAS:528:DyaL1MXlsFKgurw%3D

  23. 23

    Y. Ng Lee F. Spina E. Martinez J.V. Folgado V. Cortés Corberán (1997) Stud. Surf. Sci. Catal. 110 747 Occurrence Handle10.1016/S0167-2991(97)81037-3

  24. 24

    F. Cavani F. Trifirò (1995) Catal. Today 24 307 Occurrence Handle10.1016/0920-5861(95)00051-G Occurrence Handle1:CAS:528:DyaK2MXlvFKht7g%3D

  25. 25

    L. Leveles K. Seshan J.A. Lercher L. Lefferts (2003) J. Catal. 218 307 Occurrence Handle10.1016/S0021-9517(03)00113-1 Occurrence Handle1:CAS:528:DC%2BD3sXlsVWkurs%3D

  26. 26

    L. Leveles K. Seshan J.A. Lercher L. Lefferts (2003) J. Catal. 218 296 Occurrence Handle10.1016/S0021-9517(03)00112-X Occurrence Handle1:CAS:528:DC%2BD3sXlsVWkuro%3D

  27. 27

    T. Ito J.-X. Wang (1985) J. Am. Chem. Soc. 107 5062 Occurrence Handle10.1021/ja00304a008 Occurrence Handle1:CAS:528:DyaL2MXkvVOgtrs%3D

  28. 28

    S.C. Bhumkar L.L. Lobban (1992) Ind. Eng. Chem. Res. 31 1856 Occurrence Handle10.1021/ie00008a004 Occurrence Handle1:CAS:528:DyaK38Xkslars74%3D

  29. 29

    V.Y. Bychkov M.Y. Sinev V.N. Korchak E.L. Aptekar O.V. Krylov (1989) Kinet. Catal. 30 989

  30. 30

    E. Morales J.H. Lunsford (1989) J. Catal. 118 255 Occurrence Handle10.1016/0021-9517(89)90315-1 Occurrence Handle1:CAS:528:DyaL1MXlsFKgurw%3D

  31. 31

    V.R. Choudhary V.H. Rane S.T. Chaudhari (1998) React. Kinet. Catal. Lett. 63 371 Occurrence Handle10.1007/BF02475414 Occurrence Handle1:CAS:528:DyaK1cXjsFWgsLs%3D

  32. 32

    M.Y. Sinev V.Y. Bychkov V.N. Korchak E.L. Aptekar O.V. Krylov (1989) Kinet. Catal. 30 1236

  33. 33

    M.Y. Sinev V.Y. Bychkov (1993) Kinet. Catal. 34 309 Occurrence Handle1:CAS:528:DyaK2cXjvFamsQ%3D%3D

  34. 34

    V.A. Volkovich T.R. Griffiths D.J. Fray R. Thied (2000) J. Nucl. Mater. 282 152 Occurrence Handle10.1016/S0022-3115(00)00427-X Occurrence Handle1:CAS:528:DC%2BD3cXoslSrsLs%3D

  35. 35

    V.A. Volkovich T.R. Griffiths D.J. Fray M. Fields (1997) J. Chem. Soc., Faraday Trans. 93 3819 Occurrence Handle10.1039/a704450j Occurrence Handle1:CAS:528:DyaK2sXnsVars74%3D

  36. 36

    M.V. Landau A. Gutman M. Herskowitz R. Shuker Y. Bitton D. Mogilyansky (2001) J. Mol. Catal. A: Chem. 176 127 Occurrence Handle10.1016/S1381-1169(01)00241-2 Occurrence Handle1:CAS:528:DC%2BD3MXnvVSjt7k%3D

Download references

Author information

Correspondence to Johannes A. Lercher.

Rights and permissions

Reprints and Permissions

About this article

Cite this article

Gaab, S., Find, J., Müller, T.E. et al. Kinetics and mechanism of the oxidative dehydrogenation of ethane over Li/Dy/Mg/O/(Cl) mixed oxide catalysts. Top Catal 46, 101–110 (2007). https://doi.org/10.1007/s11244-007-0320-x

Download citation

Keywords

  • oxidative dehydrogenation
  • ethane
  • ethene
  • mixed oxide