Surface carbonyl species of copper supported on dealuminated Y zeolite

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Hans Miessner, Holger Landmesser, Nils Jaeger and Klaus Richter


Abstract

Well defined surface carbonyls of CuI with unusually narrow (ν1/2<5 cm-1) IR carbonyl bands are formed during the interaction of CO with copper supported on highly dealuminated Y zeolite. A CuI monocarbonyl with an IR band at 2159 cm-1 forms, with additional CO, a dicarbonyl with well resolved IR bands at 2179 and 2153 cm-1. Isotopic exchange experiments combined with corresponding force field calculations reveal the C2v structure of the dicarbonyl and a correlation of the integrated carbonyl intensities shows the mutual conversion of mono- and di-carbonyl at the same CuI site. The reversible equilibrium between the two species is dependent on both the temperature and the CO pressure, with a formation energy of the CuI(CO)2 of 37 kJ mol-1. The bond angle between the carbonyl groups in the dicarbonyl is estimated to be 113°. Using a controlled hydration, several aquacarbonyls could be observed dependent on the water content. An aquacarbonyl species with a carbonyl band at 2141 cm-1 is observed when the first doses of water are added. It is transformed, with more water, into species with IR bands at 2136, 2129 and, finally, 2123 cm-1, which contain probably more than one water and/or hydroxy ligand coordinated to the CuI.


References

  1. M. Iwamoto and H. Hamada, Catal. Today, 1991, 10, 57 CrossRef CAS.
  2. M. Iwamoto and H. Yahiro, Catal. Today, 1994, 22, 5 CrossRef CAS.
  3. Y. J. Li and J. N. Armor, Appl. Catal. B, 1992, 1, L21 CrossRef CAS.
  4. Y. Y. Huang, J. Am. Chem. Soc., 1973, 95, 6636 CrossRef CAS.
  5. Y. Y. Huang, J. Catal., 1973, 30, 187 CrossRef CAS.
  6. G. Coudurier, T. Decamp and H. Praliaud, J. Chem. Soc., Faraday Trans. 1, 1982, 78, 2661 RSC.
  7. H. Förster and U. Witten, Zeolites, 1987, 7, 517 CrossRef.
  8. J. Howard and J. M. Nicol, Zeolites, 1988, 8, 142 CAS.
  9. J. Howard and J. M. Nicol, J. Chem. Soc., Faraday Trans. 1, 1989, 85, 1233 RSC.
  10. J. Sarkany, J. L. Ditri and W. M. H. Sachtler, Catal. Lett., 1992, 16, 241 CrossRef CAS.
  11. J. Sarkany and W. M. H. Sachtler, Zeolites, 1994, 14, 7 CrossRef CAS.
  12. G. Spoto, A. Zecchina, S. Bordiga, G. Ricchiardi, G. Martra, G. Leofanti and G. Petrini, Appl. Catal. B, 1994, 3, 151 CrossRef CAS.
  13. Z. Chajar, M. Primet, H. Praliaud, M. Chevrier, C. Gauthier and F. Mathis, Appl. Catal. B, 1994, 4, 199 CrossRef CAS.
  14. T. Pieplu, F. Poignant, A. Vallet, J. Saussey, J. C. Lavalley and J. Mabilon, Stud. Surf. Sci. Catal., 1995, 96, 619 CAS.
  15. G. D. Borgard, S. Molvik, P. Balaraman, T. W. Root and J. A. Dumesic, Langmuir, 1995, 11, 2065 CrossRef.
  16. V. Y. Borovkov and H. G. Karge, J. Chem. Soc., Faraday Trans., 1995, 91, 2035 RSC.
  17. K. I. Hadjiivanov, M. M. Kantcheva and D. G. Klissurski, J. Chem. Soc., Faraday Trans., 1996, 92, 4595 RSC.
  18. Y. Hoshino and M. Iwamoto, Chem. Lett., 1996, 631 CAS.
  19. I. C. Hwang, D. H. Kim and S. I. Woo, Catal. Lett., 1996, 42, 177 CrossRef CAS.
  20. M. Iwamoto and Y. Hoshino, Inorg. Chem., 1996, 35, 6918 CrossRef CAS.
  21. H. J. Jang, W. K. Hall and J. dItri, J. Phys. Chem., 1996, 100, 9416 CrossRef CAS.
  22. C. Lamberti, S. Bordiga, M. Salvalaggio, G. Spoto, A. Zecchina, F. Geobaldo, G. Vlaic and M. Bellatreccia, J. Phys. Chem. B, 1997, 101, 344 CrossRef.
  23. Y. Kuroda, H. Maeda, Y. Yoshikawa, R. Kumashiro and M. Nagao, J. Phys. Chem. B, 1997, 101, 1312 CrossRef CAS.
  24. I. Burkhardt, D. Gutschick, U. Lohse and H. Miessner, J. Chem. Soc., Chem. Commun., 1987, 291 RSC.
  25. H. Miessner, I. Burkhardt, D. Gutschick, A. Zecchina, C. Morterra and G. Spoto, J. Chem. Soc., Faraday Trans. 1, 1989, 85, 2113 RSC.
  26. H. Miessner, I. Burkhardt and D. Gutschick, J. Chem. Soc., Faraday Trans., 1990, 86, 2329 RSC.
  27. H. Miessner, I. Burkhardt, D. Gutschick, A. Zecchina, C. Morterra and G. Spoto, J. Chem. Soc., Faraday Trans., 1990, 86, 2321 RSC.
  28. H. Miessner, J. Chem. Soc., Chem. Commun., 1994, 927 RSC.
  29. H. Miessner, J. Am. Chem. Soc., 1994, 116, 11522 CrossRef CAS.
  30. P. S. Braterman, Metal Carbonyl Spectra, Academic Press, London, 1975 Search PubMed.
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