Structure and bonding of a site-isolated transition metal complex: Rhodium dicarbonyl in highly dealuminated zeolite y

Journal of the American Chemical Society

Volumn 122, Issue 33, 2000, Pages 8056-8066

  Goellner, Jesse F ^a   Gates, Bruce C ^a   Vayssilov, Georgi N ^b,c   Rösch, Notker ^b  

^a UNIVERSITY OF CALIFORNIA   (United States)

^b TECHNICAL UNIVERSITY OF MUNICH   (Germany)

^c UNIVERSITY OF SOFIA   (Bulgaria)

Author keywords

[No Author keywords available]

Indexed keywords

RHODIUM DERIVATIVE; ZEOLITE;

ARTICLE; CHEMICAL BINDING; CHEMICAL STRUCTURE; INFRARED SPECTROSCOPY; QUANTUM MECHANICS; STRUCTURE ANALYSIS; X RAY ANALYSIS;

EID: 0034705982     PISSN: 00027863     EISSN: None     Source Type: Journal    
DOI: 10.1021/ja001209f     Document Type: Article

References (67)

1. Kristen, M. O. Top. Cotal. 1999, 7, 89.
2. Kaminsky, W. Sci. Technol. Catal. 1998 1999, 121, 3.
3. Kaminsky, W. Angew. Makromol. Chem. 1994, 223, 101.
4. Roscoe, S. B.; Frechet, J. M. J., Walzer, J. F.; Dias, A. J. Science 1998, 280, 270.
5. Weber, W. A. Ph.D. Dissertation, University of California, Davis, 1998.
6. Miessner, H.; Burkhardt, I.; Gutschick, D.; Zecchina, A.; Morterra, C.; Spoto, G. J. Chem. Soc., Faraday Trans. I 1989, 85, 2113.
7. Binsted, N.; Evans, J.; Greaves, G. N.; Price, R. J. Organometallics 1989, 8, 613.
8. van't Blik, H. F. J.; van Zon, J. B. A. D.; Huzinga, T.; Vis, J. C.; Koningsberger, D. C.; Prins, R. J. Am. Chem. Soc. 1985, 107, 3139.
9. Hu, A.; Neyman, K. M.; Staufer, M.; Belling, T.; Gates, B. C.; Rösch, N. J. Am. Chem. Soc. 1999, 121, 4522.
10. Ferrari, A. M.; Neyman, K. M.; Mayer, M.; Staufer, M.; Gates, B. C.; Rösch, N. J. Phys. Chem. B 1999, 103, 5311.
11. Lamb, H. H.; Gates, B. C.; Knözinger, H. Angew. Chem., Int. Ed. Engl. 1988, 27, 1127.
12. Braterman, P. S. Metal Carbonyl Spectra; Academic Press: New York, 1975.
13. -1, indicating remnants of the acac ligand. However, such an infrared band would be obscured in the spectrum of the zeolite DAY-supported samples reported here by the absorption of the zeolite.
14. 2 from supported aggregates of rhodium metal, Miessner et al. observed peaks which correspond to acidic OH groups. Such peaks were not observed in the spectrum of our sample calcined at 300 °C. In contrast, the O-H stretching region characterizing our sample calcined at 120 °C, which had a higher concentration of surface water than that calcined at 300 °C, exhibits broad and muted OH features that do not allow clear identification of band positions (Figure 1 in Supporting Information).
15. Lytle, F. W.; Sayers, D. E.; Stern, E. A. Physica B 1989, 158, 701.
16. 2 showed that the probabilities that Model III describes the data better than Model I are only 51% and 50% for samples calcined at 300 and 120 °C, respectively. Similar values, with no probability exceeding 61%, were obtained for similar comparisons discriminating between the other models. Thus, there is little basis in the data for choosing one of these models over the other, each fits the data well.
17. Vaarkamp, M. Catal. Today 1998, 39, 271.
18. Alexeev, O.; Gates, B. C. Top. Catal. 2000, 10, 273.
19. The effect of multiple scattering as a consequence of the near linearity of the Rh-C-O* moiety (a shorter apparent bond distance than the actual distance) was accounted for, as well as possible, by using the Ru-O* reference described below.
20. 3. 8
21. short contribution. For the remaining parameters of the models fitting the EXAFS spectra, the generally accepted error bounds (mentioned above) are larger than those determined by solely considering cross-correlation.
22. 0 values in the characterization of this absorber-backscatterer pair.
23. Miessner, H. J. Am. Chem. Soc. 1994, 116, 11522.
24. Vayssilov, G. N.; Staufer, M.; Belling, T.; Neyman, K. M.; Knözinger, H.; Rösch, N. J. Phys. Chem. B 1999, 103, 7920.
25. Vayssilov, G. N.; Rösch, N. J. Catal. 1999, 186, 423.
26. asym to deduce the C-Rh-C angle, we obtained a value of 99°, although the angle employed in calculating the frequencies and intensities is 90.4°, as determined in the geometry optimization. This comparison shows that the estimate of the angle between two ligand molecules on the basis of the intensity ratio of the symmetric and antisymmetric vibrations is not accurate.
27. Browning, J.; Goggin, P. L.; Goodfellow, R. J.; Norton, M. G.; Rattray, A. J. M.; Taylor, B. F.; Mink. J. J. Chem. Soc., Dalton Trans. 1977, 2061.
28. Yates, J. T., Jr.; Duncan, T. M.; Worley, S. D.; Vaughn, R. W. J. Chem. Phys. 1979, 70, 1219.
29. Solymosi, F.; Knözinger, H. J. Chem. Soc., Faraday Trans. 1990, 86, 389.
30. Sauer, J.; Ugliengo, P.; Garrone, E.; Saunders: V. R. Chem. Rev. 1994, 94, 2095.
31. van Santen, R. A.; Kramer, G. J. Chem. Rev. 1995, 95, 637.
32. 13CO peaks were not found in the spectrum although they are evident in the spectra of the present samples.
33. We recognize that the vibrational frequency of adsorbed CO is affected by long-range fields, such as the Madelung field. However, the assertion that the local effects dominate the position of the VCO bands is supported by the close agreement (Table 1) between the experimental frequencies and those calculated using only a localized fragment of the zeolite structure to represent the support.
34. 2 such a contribution was observed at about 2.5 Å. 5
35. Görling, A.; Trickey, S. B.; Gisdakis, P.; Rösch, N. In Topics in Organometallic Chemistry; Brown, J., Hofmann, P., Eds.; Springer: Heidelberg, 1999; Vol. 4, p 109.
36. Goellner, J. F.; Neyman, K. M.; Mayer, M.; Nörtemann, F.; Gates, B. C.; Rösch, N. Langmuir 2000, 16, 2736.
37. Deutsch, S. E.; Chang, J.-R.; Gates, B. C. Langmuir 1993, 9, 1284.
38. Papile, C. J.; Gates, B. C. Langmuir 1992, 8, 74.
39. Basset, J.-M.; Choplin, A. J. Mol. Catal. 1983, 21, 95.
40. 2(acac), is a square-planar 16-electron complex.
41. Jentoft, R. E.; Deutsch, S. E.; Gates, B. C. Rev. Sci. Instrum. 1996, 67, 2111.
42. ParaGauss 2.0, Belling, T.; Grauschopf, T.; Krüger, S.; Nörtemann, F.; Staufer, M.; Mayer, M.; Nasluzov, V. A.; Birkenheuer, U.; Rösch, N.; Technische Universität München: München, 1999.
43. (a) Becke, A. D. Phys. Rev. A 1988, 38, 3098.
44. (b) Perdew, J. P. Phys. Rev. B 1986, 33, 8822. Perdew, J. P. Phys. Rev. B 1986, 34, 7406.
45. (b) Perdew, J. P. Phys. Rev. B 1986, 33, 8822. Perdew, J. P. Phys. Rev. B 1986, 34, 7406.
46. (a) Ferrari, A. M.; Neyman, K. M.; Rösch, N. J. Phys. Chem. B 1997, 101, 9292.
47. (b) Godbout, N.; Salahub, D. R.; Andzelm, J.; Wimmer, E. Can. J. Chem. 1992, 70, 560.
48. Nasluzov, V. A.; Rösch, N. Chem. Phys. 1996, 210, 413.
49. Weber, W. A.; Gates, B. C. J. Phys. Chem. B 1997, 101, 10423.
50. van Zon, J. B. A. D.; Koningsberger, D. C.; van't Blik, H. F. J.; Sayers, D. E. J. Chem. Phys. 1985, 82, 5742.
51. Kirlin, P. S.; van Zon, F. B. M.; Koningsberger, D. C.; Gates, B. C. J. Phys. Chem. 1990, 94, 8439.
52. Vaarkamp, M.; Linders, J. C.; Koningsberger, D. C. Physica B 1995, 209, 159.
53. Ramaker, D. E.; Mojet, B. L.; Koningsberger, D. C.; O'Grady, W. E. J. Phys. Condens. Matter 1988. 10, 8753.
54. Ramaker, D. E.; Quan, X.; O'Grudy, W. E. Chem. Phvs. Lett. 1999, 299, 221.
55. Cook, J. W., Jr.; Sayers, D. E. J. Appl. Phys. 1981, 52, 5024.
56. Duivenvoorden, F. B. M.; Koningsberger, D. C.; Uh, Y. S.; Gates, B. C. J. Am. Chem. Soc. 1986, 108, 6254.
57. (a) Zabinsky, S. I.; Rehr, J. J.; Ankudinov, A.; Albers, R. C.; Eller, M. J. Phys. Rev. B. 1995, 52, 2995.
58. (b) Ankudinov, A. Ph.D, Dissertation, University of Washington, 1996.
59. Donnay, J. D. H.; Ondik, H. M. Crystal Data Determinative Tables, 3rd ed.; U.S. Department of Commerce. National Bureau of Standards and the Joint Committee on Powder Diffraction Standards: Washington, DC. 1973; Vol. II, p C-4.
60. van Zon, F. B. M.; Maloney, S. D.; Gates, B. C.; Koningsberger, D. C. J. Am. Chem. Soc. 1993, 115, 10317.
61. van Zon, J. B. A. D. Dissertation, Eindhoven University of Technology, The Netherlands, 1988.
62. van Zon, J. B. A. D.; Koningsberger, D. C; Gates, B. C. J. Chem. Phys. 1985, 82, 5742.
63. Wycoff, R. W. G., Ed. Crystal Structures. 2nd ed.; Wiley: New York, 1963; Vol. 1, p 10.
64. Coey, J. M. D. Acta Crystallogr. 1970, B26, 1876.
65. Mason, R.; Rae, A. I. M. J. Chem. Soc. A 1968, 778.
66. Martens, J. H. A.; Prins, R.; Zandberge, H.; Koningsberger, D. C. J. Phys. Chem. 1988, 92, 1903.
67. Rao, L.-F.; Fukuoka, A.; Kosugi, N.; Kuroda, H.; Ichikawa, M. J. Phys. Chem. 1990, 94, 5317.