Activation and adsorption of multiple H2 molecules on a Pd5 cluster: A density functional study

Journal of Physical Chemistry A

Volumn 107, Issue 24, 2003, Pages 4929-4939

  Moc, Jerzy ^a,b   Musaev, Djamaladdin G ^b   Morokuma, Keiji ^b  

^a UNIVERSITY OF WROC AW   (Poland)

^b EMORY UNIVERSITY   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

ADSORPTION; ATOMS; CHEMICAL ACTIVATION; HYDROGEN; HYDROGENATION; MOLECULAR STRUCTURE; PALLADIUM; PROBABILITY DENSITY FUNCTION; REACTION KINETICS; SATURATION (MATERIALS COMPOSITION); THERMODYNAMIC STABILITY;

CORE STRUCTURE; MOLECULAR ADSORPTION; NON-HYDROGEN SATURATED SPECIES; TRIGONAL BIPYRAMIDAL CLUSTER;

MOLECULAR PHYSICS;

EID: 0037561545     PISSN: 10895639     EISSN: None     Source Type: Journal    
DOI: 10.1021/jp0343436     Document Type: Article

References (35)

1. Arakawa, H.; Aresta, M.; Armor, J. N.; Barteau, M. A.; Beckman, E. J.; Bell, A. T.; Bercaw J. E.; Creutz, C.; Dinjus, E.; Dixon, D. A.; Domen, K.; DuBois, D. L.; Eckert, J.; Fujita, E.; Gibson, D. H.; Goddard, W. A.; Goodman, D. W.; Keller, J.; Kubas, G. J.; Kung, H. H.; Lyons, J. E.; Manzer, L. E.; Marks, T. J.; Morokuma, K.; Nicholas, K. M.; Periana, R.; Que, L.; Rostrup-Nielson, J.; Sachtler, W. M. H.; Schmidt, L. D.; Sen, A.; Somoriai, G. A.; Stair, P. C.; Stults, B. R.; Tumas, W. Chem. Rev. 2001, 101, 953.
2. (a) Wicke, E.; Brodowsky, H. In Hydrogen in Metals; Alefeld, G., Völkl, J., Eds.; Springer: Berlin, 1978; Vol. 2, p 73.
3. (b) Farias, D.; Schilbe, P.; Patting, M.; Rieder, K.-H. J. Chem. Phys. 1999, 110, 559 and references therein.
4. (c) Okuyama, H.; Siga, W.; Takagi, N.; Nishijima, M.; Aruga, T. Surf. Sci. 1998, 401, 344.
5. (d) Behm, R. J.; Christmann, K.; Ertl, G. Surf. Sci. 1980, 99, 320.
6. Efremenko, I.; Sheintuch, M. Surf. Sci. 1998, 414, 148 and references therein.
7. Fayet, P.; Kaldor, A.; Cox, D. M. J. Chem. Phys. 1990, 92, 254.
8. (a) Thomas, J. M. Angew. Chem., Int. Ed. Engl. 1988, 27, 1673.
9. (b) Thomas, J. M. Angew. Chem., Int. Ed. Engl. 1994, 33, 913.
10. (c) Cox, D. M.; Fayet, P.; Brickman, R.; Hahn, M. Y.; Kaldor, A. Catal. Lett. 1990, 4, 271.
11. Knickelbein, M. B.; Koretsky, G. M.; Jackson, K. A.; Pederson, M. R.; Hajnal, Z. J. Chem. Phys. 1998, 109, 10692 and references therein.
12. For a comprehensive set of the representative references, the reader is referred to our previous paper.
13. Cui, Q.; Musaev, D. G.; Morokuma, K. J. Chem. Phys. 1998, 108, 8418.
14. Cui, Q.; Musaev, D. G.; Morokuma, K. J. Phys. Chem. A 1998, 102, 6373.
15. Moc, J.; Musaev, D. G.; Morokuma, K. J. Phys. Chem. A 2000, 104, 11606.
16. (a) Becke, A. D. Phys. Rev. A 1988, 38, 3098.
17. (b) Lee, C.; Yang, W.; Parr, R. G. Phys. Rev. B 1988, 37, 785.
18. (c) Becke, A. D. J. Chem. Phys. 1993, 98, 5648.
19. Hay, P. J.; Wadt, W. R. J. Chem. Phys. 1985, 82, 299.
20. Dunning, T. H., Jr. J. Chem. Phys. 1970, 53, 2823.
21. Andrae, D.; Haussermann, U.; Dolg, M.; Stoll, H.; Preuss, H. Theor. Chim. Acta 1990, 77, 123.
22. Dunning, T. H., Jr. J. Chem. Phys. 1989, 90, 1007. Note that d functions on H were excluded from the correlation-consistent basis set.
23. (a) Gonzalez, C.; Schlegel, H. B. J. Chem. Phys. 1989, 90, 2154.
24. (b) Gonzalez, C.; Schlegel, H. B. J. Phys. Chem. 1990, 94, 5523.
25. The choice of low temperature (70 K) was explained in our previous work. Note that the actual cluster temperature in the experiment by Cox et al. was not reported.
26. Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Zakrzewski, V. G.; Montgomery, J. A., Jr.; Stratmann, R. E.; Burant, J. C.; Dapprich, S.; Millam, J. M.; Daniels, A. D.; Kudin, K. N.; Strain, M. C.; Farkas, O.; Tomasi, J.; Barone, V.; Cossi, M.; Cammi, R.; Mennucci, B.; Pomelli, C.; Adamo, C.; Clifford, S.; Ochterski, J.; Petersson, G. A.; Ayala, P. Y.; Cui, Q.; Morokuma, K.; Malick, D. K.; Rabuck, A. D.; Raghavachari, K.; Foresman, J. B.; Cioslowski, J.; Ortiz, J. V.; Stefanov, B. B.; Liu, G.; Liashenko, A.; Piskorz, P.; Komaromi, I.; Gomperts, R.; Martin, R. L.; Fox, D. J.; Keith, T.; Al-Laham, M. A.; Peng, C. Y.; Nanayakkara, A.; Gonzalez, C.; Challacombe, M.; Gill, P. M. W.; Johnson, B. G.; Chen, W.; Wong, M. W.; Andres, J. L.; Head-Gordon, M.; Replogle, E. S.; Pople, J. A. Gaussian 98, revision A.1; Gaussian, Inc.: Pittsburgh, PA, 1998.
27. Fahmi, A.; van Santen, R. A. J. Phys. Chem. 1996, 100, 5676.
28. 5 with equatorial and axial Pd-Pd edges of 3.05 and 2.61 Å, respectively.
29. 3E′) structure was not considered by these authors.
30. 5(1) of 146.1 kcal/mol can be compared with the MRSDCI (MRSDCI + Q) values of 146 (161) kcal/mol.
31. LaJohn, L. A.; Christiansen, P. A.; Ross, R. B.; Atashroo, T.; Ermler, W. C. J. Chem. Phys. 1987, 87, 2812.
32. 3A) TS, the IRC calculation generated only one point and stopped (both directions); this was followed by the geometry optimizations started at the indicated "forward" and "backward" IRC structures.
33. 2).
34. 2), have been found (at the geometry-optimization level) to be 9.1 and 7.7 kcal/mol less favorable, respectively, than the most stable singlet complex of this type, Pd5_2_a_(f, f′).
35. 2 is entrained in the primary helium gas and exposed to the laser initiated plasma".