Binding of deuterium to icosahedral nickel and cobalt clusters

Surface Science

Volumn 355, Issue 1-3, 1996, Pages 127-139

  Parks, E K ^a   Nieman, G C ^a,b   Riley, S J ^a  

^a ARGONNE NATIONAL LABORATORY   (United States)

^b MONMOUTH COLLEGE   (United States)

Author keywords

Clusters; Cobalt; Hydrides; Nickel

Indexed keywords

CHEMISORPTION; COBALT; DEUTERIUM; ELECTRON ENERGY LEVELS; HYDRIDES; NICKEL; SATURATION (MATERIALS COMPOSITION);

ICOSAHEDRAL CLUSTERS;

CHEMICAL BONDS;

EID: 0030169994     PISSN: 00396028     EISSN: None     Source Type: Journal    
DOI: 10.1016/0039-6028(95)01364-4     Document Type: Article

References (45)

1. For general reviews of cluster studies, see: Clusters of Atoms and Molecules, I and II, Ed. H. Haberland (Springer, New York, 1994); Physics and Chemistry of Finite Systems: From Clusters to Crystals, Vols. I and II, Eds. P. Jena, S.N. Khanna and B.K. Rao (Kluwer, Boston, 1991).
2. For general reviews of cluster studies, see: Clusters of Atoms and Molecules, I and II, Ed. H. Haberland (Springer, New York, 1994); Physics and Chemistry of Finite Systems: From Clusters to Crystals, Vols. I and II, Eds. P. Jena, S.N. Khanna and B.K. Rao (Kluwer, Boston, 1991).
3. T.D. Klots, B.J. Winter, E.K. Parks and S.J. Riley J. Chem. Phys. 95 (1991) 8919.
4. 147 may not.
5. On a given face of an icosahedron, the packing from the central atom out is essentially fee, with an ABCABC. . . layering. However, the initial atoms that add to a closed-shell icosahedron add to three-fold sites that form an ABA layer with a conversion to the ABC layering occurring when a sufficient number of metal atoms are present on the cluster's surface.
6. (a) J.A. Northby, J. Chem. Phys. 87 (1987) 6166;
7. (b) E.K. Parks and S.J. Riley, Z. Phys. D 33 (1995) 59.
8. W. Miehle, O. Kandler, T. Leisner and O. Echt, J. Chem. Phys. 91 (1989) 5940.
9. (a) E.K. Parks, B.J. Winter, T.D. Klots and S.J. Riley, J. Chem. Phys. 94 (1991) 1882;
10. (b) E.K. Parks, T.D. Klots, B.J. Winter and S.J. Riley, J. Chem. Phys. 99 (1993) 5831.
11. The surfaces of icosahedral clusters are stretched relative to an ideal close-packed geometry.
12. G. Pacchioni, S.-C. Chung, S. Krüger and N. Rösch, Chem. Phys. 184 (1994) 125; C.L. Cleveland and U. Landmann, J. Chem. Phys. 94 (1991) 7376.
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16. (b) P.S. Bechthold, E.K. Parks, B.H. Weiller, L.G. Pobo and S.J. Riley, Z. Phys. Chem. N.F. 169 (1990) 1669;
17. (c) E.K. Parks and S.J. Riley, in: The Chemical Physics of Atomic and Molecular Clusters, Ed. G. Scoles (North-Holland, Amsterdam, 1990), p. 761.
18. At the low temperatures, clusters may be formed in a number of different structures, each with its own saturation level, thus leading to a broadening of the in distribution. Similar effects have been seen with nitrogen adsorption at low temperature (see E.K. Parks, L. Zhu, J. Ho and S.J. Riley, J. Chem. Phys. 102 (1995) 7377).
19. The effective mass resolution degrades with increasing temperature, both due to the increasing level of water impurity and its effect on H/D exchange, as well as due to the increased velocity spread of the clusters as they exit the nozzle.
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21. E.K. Parks, G.C. Nieman, L.G. Pobo and S.J. Riley, J. Chem. Phys. 86 (1987) 1066; 88 (1988) 6260.
22. 2 desorption from the cluster during the flight from the FTR to the mass spectrometer.
23. 2 pressures are considerably higher.
24. J. Ho, L. Zhu, E.K. Parks and S.J. Riley, J. Chem. Phys. 99 (1993) 140.
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26. 71 is the capped icosahedron, resulting from the addition of a 16-atom cap to the 55-atom icosahedron in either a ABC or ABA configuration. The experiments on water and ammonia adsorption in Ref. [2] cannot distinguish between the two 71-atom isomers. Experiments on nitrogen adsorption have suggested that the ABA cap rather than the icosahedral ABC cap is the most stable for the bare nickel clusters; see Ref. [5(b)]. Clusters larger than ∼80 atoms probably form entirely with an icosahedral rather than an ABA third shell; see Ref. [5a].
27. 71, the closed shell occurs at 81 atoms.
28. See Ref. [2] for model drawings of the clusters.
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31. Apex atoms on closed subshells refer to any of the 12 apex atoms on the 55 or 147-atom icosahedra that are exposed, as long as they do not lie along the edge of the emerging third shell.
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34. K. Christmann, Surf. Sci. Rep. 9 (1988) 1.
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38. P.E.M. Seigbahn, M.R.A. Blomberg and C.W. Bauschlicher, Jr., J. Chem. Phys. 81 (1984) 2103; I. Panas, P. Seigbahn and U. Wahlgren, Theoret. Chim. Acta 74 (1988) 167; T.N. Truong, D.G. Truhlar and B.C. Garrett, J. Phys. Chem. 93 (1989) 8227; T.N. Truong and D.G. Truhlar, J. Phys. Chem. 94 (1990) 8262.
39. K.H. Rieder and H. Wilson, Surf. Sci. 131 (1983) 245.
40. 2.
41. Yang and Whitten (Ref. [22]) find that three-fold sites bind H atoms 10.5 kJ/mol more strongly than bridge sites on Ni(III).
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43. E.K. Parks and S.J. Riley J. Chem. Phys. 99 (1993) 5898.
44. E.K. Parks, L. Zhu, J. Ho and S.J. Riley, J. Chem. Phys. 100 (1994) 7206.
45. J. Jellinek, Z. Phys. D 26 (1993) 304.