View PDF Version
 
DOI: 10.1039/A705333I (Paper) Reference Section for: J. Mater. Chem., 1998, 8, 751-759

N,N-Dialkylcarbamato complexes as precursors for the chemical implantation of metal cations on a silica support

(Note: The full text of this document is currently only available in the PDF Version )

Luigi Abis, Daniela Belli Dell'amico, Carlo Busetto, Fausto Calderazzo, Ruggero Caminiti, Carmine Ciofi, Fabio Garbassi and Guglielmo Masciarelli

Abstract

Implantation of platinum(ii) on a commercial silica has been carried out under mild conditions by usingN,N-dialkylcarbamato complexes as reactive precursors, in a biphasic liquid/solid system, carbon dioxide and secondary amine being released during the reaction with the acidic silanol groups of the support. Information about the coordination sphere of the silica-supported platinum(ii) has been obtained by IR, XPS, solid-state NMR spectroscopy and WAXS measurements, which agree with chemical evidence. Reduction, either thermal or with dihydrogen, produces platinum nanoparticles, which were studied by conventional techniques and shown to be catalytically active in the hydrogenation of cyclohexene.

References

  1. (a) L. Abis, D. Belli Dell' Amico, F. Calderazzo, R. Caminiti, F. Garbassi, S. Ianelli, G. Pelizzi, P. Robino and A. Tomei, J. Mol. Catal., 1996, 108, L113 Search PubMed; (b) P. Rabette, A. M. Deane, A. J. Tench and M. Che, Chem. Phys. Lett., 1979, 60, 348 CrossRef CAS; (c) M. Che and C. O. Bennett, Adv. Catal., 1989, 36, 55 CAS.
  2. (a) E. Agostinelli, D. Belli Dell' Amico, F. Calderazzo, D. Fiorani and G. Pelizzi, Gazz. Chim. Ital., 1988, 118, 729 CAS; (b) P. B. Arimondo, F. Calderazzo, U. Englert, C. Maichle-Mössmer, G. Pampaloni and J. Strähle, J. Chem. Soc., Dalton Trans., 1996, 311 RSC; (c) D. Belli Dell' Amico, F. Calderazzo, F. Marchetti and G. Pampaloni, Stoichiometric and Exhaustive Hydrolysis of N,N-Dialkylcarbamates, in, Aqueous Organometallic Chemistry and Catalysis, ed. I. T. Horváth and F. Joó, Kluwer Academic, Dordrecht Boston London, 1995 and references therein Search PubMed; (d) D. Belli Dell' Amico, F. Calderazzo and G. Pampaloni, Chem. Rev., to be submitted Search PubMed.
  3. Handbook of Chemistry and Physics, ed. D. R. Lide, 75th ed., CRC Press, Boca Raton Ann Arbor London Tokyo, 1994–1995, p. 8 21 Search PubMed.
  4. L. Abis, D. Belli Dell' Amico, C. Busetto, F. Calderazzo, R. Caminiti, F. Garbassi and A. Tomei, manuscript in preparation.
  5. J. Schwartz, Acc. Chem. Res., 1985, 18, 302 CrossRef CAS; P. Dufour, C. C. Santini, C. Houtman and J. M. Basset, J. Mol. Catal., 1991, 66, L23 CrossRef CAS; T. J. Marks, Acc. Chem. Res., 1992, 25, 57 CrossRef CAS; F. Quignard, C. Lecuyer, C. Bougault, F. Lefebvre, A. Choplin, D. Olivier and J.-M. Basset, Inorg. Chem., 1992, 31, 928 CrossRef CAS; P. Dufour, C. Houtman, C. C. Santini, C. Nédez, J. M. Basset, L. Y. Hsu and S. G. Shore, J. Am. Chem. Soc., 1992, 114, 4248 CrossRef CAS; F. Quignard, C. Lecuyer, C. Bougault, F. Lefebvre, A. Choplin, D. Olivier and J. M. Basset, Inorg. Chem., 1992, 31, 928 CrossRef CAS; P. Dufour, S. L. Scott, C. C. Santini, F. Lefebvre and J. M. Basset, ibid., 1994, 33, 2509 Search PubMed; M. Taoufik, C. C. Santini, J.-P. Candy, A. de Mallmann and J. M. Basset, J. Am. Chem. Soc., 1996, 118, 4167 CrossRef CAS; V. Vidal, A. Théolier, J. Thivolle-Cazat, J.-M. Basset and J. Croker, ibid., 1996, 118, 4595 Search PubMed.
  6. B. Kauffman and D. O. Cowan, Inorg. Synth., 1960, 6, 211.
  7. Yu. N. Kukushkin and S. C. Dhara, Indian J. Chem., 1970, 8, 184 Search PubMed; F. D. Rochon and P. C. Kong, Can. J. Chem., 1986, 64, 1894 CAS.
  8. (a) B. Sanna, Thesis, Degree in Chemistry, Università di Pisa, 1992–1993; (b) L. Marchetti, Thesis, Degree in Chemistry, Università di Pisa, 1994–1995.
  9. R. Alessio, D. Belli Dell' Amico, F. Calderazzo and U. Englert, Gazz. Chim. Ital., 1993, 123, 719 CAS.
  10. (a) J. B. Peri, J. Phys. Chem., 1966, 70, 2937 CAS and references therein; (b) F. Boccuzzi, S. Coluccia, G. Ghiotti, C. Morterra and A. Zecchina, ibid., 1978, 82, 1298 Search PubMed; (c) B. A. Morrow and A. J. McFarlan, ibid., 1992, 96, 1395 Search PubMed; (d) A. Zecchina, S. Bordiga, G. Spoto, L. Marchese, G. Petrini, G. Leofanti and M. Padovan, ibid., 1992, 96, 4991 Search PubMed; (e) ibid., 1992, 96, 4985 Search PubMed; (f) A. Zecchina and C. O. Arean, Catal. Rev. Sci. Eng., 1993, 35, 261 Search PubMed.
  11. (a) G. E. Maciel and D. W. Sindorf, J. Am. Chem. Soc., 1980, 102, 7606 CrossRef CAS; (b) D. W. Sindorf and G. E. Maciel, ibid., 1983, 105, 1487 Search PubMed; (c) J. Phys. Chem., 1983, 87, 5516 Search PubMed; (d) J. Am. Chem. Soc., 1983, 105, 3767 Search PubMed.
  12. F. Calderazzo and F. A. Cotton, Inorg. Chem., 1962, 1, 30 CrossRef CAS.
  13. J. F. Moulder, W. F. Stickle, P. E. Sobol and K. D. Bomben, Handbook of X-Ray Photoelectron Spectroscopy, ed. J. Chastain, Perkin-Elmer Corporation, Eden Prairie, MN, 1994 Search PubMed.
  14. (a) R. Caminiti, C. Sadun, V. Rossi, F. Cilloco and R. Felici, 25th Italian Congress of Physical Chemistry, Cagliari, Italy, June 17–21, 1991 Search PubMed; Ital. Pat. Appl. RM/93 A000410, June 23rd, 1993 Search PubMed; (b) M. Carbone, R. Caminiti and C. Sadun, J. Mater. Chem., 1996, 6, 1709 RSC.
  15. R. W. James, The Optical Principles of the Diffraction of X-Rays, G. Bell & Sons Ltd, London, 1950 Search PubMed.
  16. C. E. Briant, G. R. Hughes, P. C. Minshall and D. M. P. Mingos, J. Organomet. Chem., 1980, 202, C18 CrossRef CAS.
  17. R. D. Shannon, Acta Crystallogr., Sect. A, 1976, 32, 751 CrossRef.
  18. A. Anillo, D. Belli Dell' Amico, F. Calderazzo, M. Nardelli, G. Pelizzi and L. Rocchi, J. Chem. Soc., Dalton Trans., 1991, 2845 RSC.
  19. O. Glatter and O. Kratky, Small Angle X-Ray Scattering, Academic Press, London, 1982 Search PubMed.
  20. We thank Prof. G. Pelizzi, Università di Parma, for this X-ray experiment on a single crystal of trans-Pt(O2CNEt2)2(NHEt2)2.
  21. See ref. 3, p. 8–45.
  22. (a) F. Basolo and R. G. Pearson, Mechanisms of Inorganic Reactions, J. Wiley, New York London Sydney, 2nd edn., 1967 Search PubMed; (b) M. L. Tobe, Inorganic Reaction Mechanisms, Nelson, London, 1972 Search PubMed.
  23. Y. Asakura, M. Yamada and Y. Iwasawa, Chem. Lett., 1985, 511.
  24. H. F. J. van't Blik, J. B. A. D. van Zon, T. Huizinga, J. C. Vis, D. C. Koningsberger and R. Prins, J. Am. Chem. Soc., 1985, 107, 3139 CrossRef.
  25. N. Binsted, J. Evans, G. N. Greaves and R. J. Price, Organometallics, 1989, 8, 613 CrossRef CAS.
  26. P. S. Kirlin, F. B. M. van Zon, D. C. Koningsberger and B. C. Gates, J. Phys. Chem., 1990, 94, 8439 CrossRef CAS.
  27. (a) J. R. Chang, L. U. Gron, A. Honji, K. M. Sanchez and B. C. Gates, J. Phys. Chem., 1991, 95, 9944 CrossRef CAS; (b) A. Masson, B. Bellamy, G. Colomer, M. M'bedi, P. Rabette and M. Che, Proc. Int. 8th Congr. Catal., 1984, 4, 333 Search PubMed; quoted from ref. 1(c), p. 75; (c) S. D. Jackson, J. Willis, G. D. McLellan, G. Webb, M. B. T. Keegan, R. B. Moyes, S. Simpson, P. B. Wells and R. Whyman, J. Catal., 1993, 139, 191 CrossRef CAS; (d) M. Muhler, Z. Paàl and R. Schlögl, Appl. Surf. Sci., 1991, 47, 281 CrossRef CAS; (e) D. M. Hercules and J. C. Klein, Electron Spectroscopy for Chemical Analysis Applied to Heterogeneous Catalysis, in, Applied Electron Spectroscopy for Chemical Analysis, ed. H. Windawi and F. F.-L. Ho, J. Wiley, New York, NY, 1982, p. 147 Search PubMed.
  28. R. R. Schrock and G. W. Parshall, Chem. Rev., 1976, 76, 243 CrossRef CAS.
  29. (a) J. M. Mayer, C. J. Curtis and J. E. Bercaw, J. Am. Chem. Soc., 1983, 105, 2651 CrossRef CAS; (b) G. Parkin, E. Bunel, B. J. Burger, M. S. Trimmer, A. van Asselt and J. E. Bercaw, J. Mol. Catal., 1987, 41, 21 CrossRef CAS.
  30. (a) H. E. Bryndza, J. C. Calabrese, M. Marsi, D. C. Roe, W. Tam and J. E. Bercaw, J. Am. Chem. Soc., 1986, 108, 4805 CrossRef CAS; (b) A. Sacco and P. Mastrorilli, J. Chem. Soc., Dalton Trans., 1994, 2761 RSC; (c) O. Blum and D. Milstein, J. Am. Chem. Soc., 1995, 117, 4582 CrossRef CAS.
  31. (a) V. B. Kazansky, V. Yu. Borovkov, N. Sokolova, N. I. Jaeger and G. Schulz-Ekloff, Catal. Lett., 1994, 23, 263 CAS; (b) C. Besoukhanova, J. Guidot and D. Barthomeuf, J. Chem. Soc., Faraday Trans., 1981, 77, 1595 RSC; (c) R. P. Eischens and W. A. Pliskin, Adv. Catal., 1958, 10, 1 CAS; (d) T. M. Tri, J.-P. Candy, P. Gallezot, J. Massardier, M. Primet, J. C. Védrine and B. Imelik, J. Catal., 1983, 79, 396 CAS; (e) C. De La Cruz and N. Sheppard, Spectrochim. Acta, Part A, 1994, 50, 271 CrossRef; (f) M. Vaarkamp, B. L. Mojet, M. J. Kappers, J. T. Miller and D. C. Koningsberger, J. Phys. Chem., 1995, 99, 16067 CrossRef CAS; (g) J. C. Calabrese, L. F. Dahl, A. Cavalieri, P. Chini, G. Longoni and S. Martinengo, J. Am. Chem. Soc., 1974, 96, 2614 CrossRef CAS; (h) G. Longoni and P. Chini, ibid., 1976, 98, 7225 Search PubMed; (i) D. M. Washecheck, E. J. Wucherer, L. F. Dahl, A. Ceriotti, G. Longoni, M. Manassero, M. Sansoni and P. Chini, ibid., 1979, 101, 6110 Search PubMed; (j) D. M. P. Mingos and R. W. M. Wardle, Transition Met. Chem., 1985, 10, 441 CAS.
  32. JCPDS, Joint Committee on Powder Diffraction Standards, 1601 Park Lane, Swarthmore, PA, Card No. 4–0802.
  33. (a) T. E. Whyte, Jr., Catal. Rev., 1973, 8, 117; (b) T. Gacoin, F. Chaput, J. P. Boilot and G. Jaskierowicz, Chem. Mater., 1993, 5, 1150 CrossRef CAS.
  34. (a) J. P. Bucher, J. Buttet, J. J. van der Klink and M. Graetzel, Surf. Sci., 1989, 214, 347 CrossRef CAS; (b) Y. Takasu, M. Teramoto and Y. Matsuda, J. Chem. Soc., Chem. Commun., 1983, 1329 RSC.
  35. (a) M. Boudart, A. Aldag, J. E. Benson, N. A. Dougharty and C. G. Harkins, J. Catal., 1966, 6, 92 CAS; (b) G. Leclercq and M. Boudart, ibid., 1981, 71, 127 Search PubMed.
  36. (a) R. F. Baddour, M. Modell and R. L. Goldsmith, J. Phys. Chem., 1970, 74, 1787 CrossRef CAS; (b) T. Engel and G. Ertl, Adv. Catal., 1979, 28, 1 CAS.
Click here to see how this site uses Cookies. View our privacy policy here.