Stability and thermodynamics of the PtCl2 type catalyst for activating methane to methanol: A computational study

Organometallics

Volumn 21, Issue 3, 2002, Pages 511-525

  Kua, Jeremy ^a   Xu, Xin ^a,b   Periana, Roy A ^c   Goddard III, William A ^a  

^a CALIFORNIA INSTITUTE OF TECHNOLOGY   (United States)

^b XIAMEN UNIVERSITY   (China)

^c UNIVERSITY OF SOUTHERN CALIFORNIA   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

ACTIVATION ANALYSIS; CATALYST ACTIVITY; CHEMICAL MODIFICATION; METHANE; METHANOL; OXIDATION; PLATINUM COMPOUNDS; THERMODYNAMIC STABILITY;

DENSITY FUNCTIONAL THEORY (DFT);

ORGANOMETALLICS;

EID: 0001430826     PISSN: 02767333     EISSN: None     Source Type: Journal    
DOI: 10.1021/om0101691     Document Type: Article

References (38)

1. Arnstden, B. A.; Bergman, R. G.; Mobley, T. A.; Peterson, T. H. Acc. Chem. Res. 1995, 28, 154.
2. Bromberg, S. E.; Yang, H.; Asplund, C. M.; Lian, T.; McNamara, K. B.; Kotz, K. T.; Yeston, J. S.; Wilkens, M.; Frei, H.; Bergman, R. G.; Harris, C. B. Science 1997, 278, 260.
3. Selective Hydrocarbon Activation; Davies, J. A., Watson, P. L., Liebman, J. L., Greenberg, A., Eds.; Wiley-VCH: New York, 1990.
4. Hall, C.; Perutz, R. N. Chem. Rev. 1996, 96, 3125.
5. Hill, C. L. Activation and Functionalization of Alkanes; Wiley-Interscience: New York, 1989.
6. Sen, A. Acc. Chem. Res. 1988, 21, 421.
7. Shilov, A. E.; Shul'pin, G. B. Chem. Rev. 1997, 97, 2879.
8. Sommer, J.; Bukala, J. Acc. Chem. Res. 1993, 26, 370.
9. Walktz, K. M.; Hartwig, J. F. Science 1997, 277, 211.
10. Shilov, A. E. Activation of Saturated Hydrocarbons by Transition Metal Complexes; D. Riedel: Dordrecht, The Netherlands, 1984.
11. Periana, R. A.; Taube, D. J.; Gamble, S.; Taube, H.; Satoh, T.; Fujii, H. Science 1998, 280, 560.
12. Periana, R. A.; Taube, D. J.; Evitt, E. R.; Loffler, D. G.; Wentrcek, P. R.; Voss, G.; Masuda, T. Science 1993, 259, 340.
13. Slater, J. C. Quantum Theory of Molecules and Solids; McGraw-Hill: New York, 1974; Vol. 4 (The Self-Consistent Field for Molecules and Solids).
14. Becke, A. D. J. Chem. Phys. 1993, 95, 5648.
15. Becke, A. D. Phys. Rev. A 1988, 38, 3098.
16. Vosko, S. H.; Wilk, L.; Nusair, M. Can. J. Phys. 1980, 58, 1200.
17. Lee, C.; Yang, W.; Parr, R. G. Phys. Rev. B 1988, 37, 785.
18. Goddard, W. A., III. Phys. Rev. 1968, 174, 659.
19. Melius, C. F.; Olafson, B. O.; Goddard, W. A., III. Chem. Phys. Lett. 1974, 28, 457.
20. Hay, P. J.; Wadt, W. R. J. Phys. Chem. 1985, 82, 299.
21. Jaguar 3.5; Schrodinger, Inc., Portland, OR, 1998.
22. Greeley, B. H.; Russo, T. V.; Mainz, D. T.; Friesner, R. A.; Langlois, J.-M.; Goddard, W. A., III; Honig, B. J. Am. Chem. Soc. 1994, 116, 11875.
23. Tannor, D. J.; Marten, B.; Murphy, R.; Friesner, R. A.; Sitkoff, D.; Nicholls, A.; Ringnalda, M.; Goddard, W. A., III; Honig, B. J. Am. Chem. Soc. 1994, 116, 11875.
24. Marten, B.; Kim, K.; Cortis, C.; Friesner, R, A.; Murphy, R. B.; Ringnalda, M. N.; Sitkoff, D.; Honig, B. J. Phys. Chem. 1996, 100, 11775.
25. Klassen, J. K.; Fiehrer, K. M.; Nathanson, G. M. J. Phys. Chem. B 1997, 101, 9098.
26. 3 at 20 °C obtained from ref 27.
27. Lide, D. R. Handbook of Chemistry and Physics, 74th ed.; CRC Press: Boca Raton, FL, 1993.
28. In free bipyrimidine the calculated angle between the pyrimidine places was 28.4°. The energy required to twist the planes parallel was calculated to be -2.7 kcal/mol, including solvation and zero-point energy corrections.
29. Siegbahn, P. E. M.; Crabtree, R. H. J. Am. Chem. Soc. 1996, 118, 4442.
30. Holtcamp, M. W.; Labinger, J. A.; Bercaw, J. E. J. Am. Chem. Soc. 1997, 119, 848.
31. Mylavaganam, K.; Backsay, G. B.; Hush, N. S. J. Am. Chem. Soc. 1999, 121, 4633.
32. Igel-Mann, G.; Stoll, H.; Preuss, H. Mol. Phys. 1988, 65, 1321.
33. Andrae, D.; Haussermann, U.; Dolg, M.; Stoll, H.; Preuss, H. Theor. Chim. Acta 1990, 77, 123.
34. Foresman, J. B.; Keith, T. A.; Wiberg, K. B.; Snoonian, J.; Frisch, M. J. J. Phys. Chem. 1996, 700, 16098.
35. Note that in calculating the kinetics all species are included; i.e., we do not calculate reactant fragments as separated species at infinity.
36. From our calculations on C-H activation barriers of small hydrocarbons on a Pt surface (Kua, J.; Goddard, W. A., III. Unpublished results), we find that DFT/B3LYP with the same basis set systematically overestimates barriers by ̃5 kcal/mol when compared to experiment. The numbers we report are the actual calculated numbers without any corrections.
37. This estimate presumes the pathway for the bisulfate ligand is very similar to that for chloride. Calculations with the bisulfate ligand are currently in progress (Philipp, D.; Xu, X.; Goddard, W. A., III. Manuscript in preparation).
38. Periana, R. A. Unpublished results.