Dynamics of dissociative methane adsorption on metals: CH4 on Pt{110}(1×2)
J. Chem. Phys. 112, 4739 (2000); doi:10.1063/1.481030
Issue Date: 8 March 2000
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Supersonic molecular beams have been used to study methane dissociative adsorption on Pt{110}(1×2) at incident translational energies of 20 to 700 meV, incident vibrational temperatures of 300 to 800 K and surface temperatures from 400 to 1000 K. At Et
100 meV, the initial dissociative sticking probability, s0, rises sharply. The process is facilitated by vibrational excitation of the deformation modes and surface temperature. At Et>100 meV, an activated adsorption process becomes dominant, with an activation barrier of ~146 meV. At Et
230 meV, s0 attains a limiting value which is strongly enhanced by excitation of the CH stretch modes in the incident molecule. An increase in the surface temperature also enhances s0, at all incident translational energies. The mechanistic implications are discussed and it is concluded that the low translational energy process is a distinctive steering-assisted direct adsorption pathway. ©2000 American Institute of Physics.
100 meV, the initial dissociative sticking probability, s0, rises sharply. The process is facilitated by vibrational excitation of the deformation modes and surface temperature. At Et>100 meV, an activated adsorption process becomes dominant, with an activation barrier of ~146 meV. At Et
230 meV, s0 attains a limiting value which is strongly enhanced by excitation of the CH stretch modes in the incident molecule. An increase in the surface temperature also enhances s0, at all incident translational energies. The mechanistic implications are discussed and it is concluded that the low translational energy process is a distinctive steering-assisted direct adsorption pathway. ©2000 American Institute of Physics.
| History: | Received 2 July 1999; accepted 14 December 1999 |
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http://link.aip.org/link/?JCPSA6/112/4739/1 |
KEYWORDS and PACS
organic compounds,
adsorbed layers,
dissociation,
surface chemistry,
molecular beams,
molecule-surface impact,
vibrational states,
rotational-vibrational energy transfer,
chemisorption,
platinum
- 68.45.-v
Surfaces and interfaces; thin films and whiskers (structure and nonelectronic properties) Solidfluid interfaces - 82.65.My
Physical chemistry Surface and interface chemistry Chemisorption - 82.30.Lp
Physical chemistry Specific chemical reactions; reaction mechanisms Decomposition reactions (pyrolysis, dissociation, and group ejection) - 82.65.-i
Physical chemistry Surface and interface chemistry - 82.40.Dm
Physical chemistry Chemical kinetics and reactions: special regimes and techniques Atomic and molecular beam reactions - 34.50.Dy
Atomic and molecular collision processes and interactions Scattering of atoms, molecules, and ions Interactions of atoms, molecules, and their ions with surfaces; photon and electron emission; neutralization of ions - 33.15.Mt
Molecular properties and interactions with photons Properties of molecules and molecular ions Rotation, vibration, and vibrationrotation constants - 34.50.Ez
Atomic and molecular collision processes and interactions Scattering of atoms, molecules, and ions Rotational and vibrational energy transfer - 68.45.Da
Surfaces and interfaces; thin films and whiskers (structure and nonelectronic properties) Solidfluid interfaces Adsorption and desorption kinetics; evaporation and condensation - YEAR: 2000
RELATED DATABASES
PUBLICATION DATA
0021-9606 (print)
1089-7690 (online)
REFERENCES (56)
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- C. Kemball,
Proc. R. Soc. London, Ser. A 207, 539 (1951) . - R. S. Suhrmann, H. J. Busses, and G. Wedler, Z. Phys. Chem., Neue Folge 47, 1 (1965).
- C. N. Stewart and G. Ehrlich, J. Chem. Phys. 62, 4672 (1975).
- J. Yates, Jr., J. J. Zinck, S. Sheard, and W. H. Weinberg, J. Chem. Phys. 70, 2266 (1979).
- C. T. Rettner, H. E. Pfnür, and D. J. Auerbach, Phys. Rev. Lett. 54, 2716 (1985).
- C. T. Rettner, H. E. Pfnür, and D. J. Auerbach, J. Chem. Phys. 84, 4163 (1986).
- M. B. Lee, Q. Y. Yang, and S. T. Ceyer, J. Chem. Phys. 87, 2724 (1987).
- M. B. Lee, Q. Y. Yang, and S. T. Ceyer, J. Chem. Phys. 85, 1693 (1986).
- A. V. Hamza and R. J. Madix,
Surf. Sci. 179, 25 (1987) . - S. G. Brass and G. Ehrlich, J. Chem. Phys. 87, 4285 (1987).
- A. C. Luntz and D. S. Bethune, J. Chem. Phys. 90, 1274 (1989).
- G. R. Schoofs, C. R. Arumainayagam, M. C. McMaster, and R. J. Madix,
Surf. Sci. 215, 1 (1989) . - J. Harris, J. Simon, A. C. Luntz, C. B. Mullins, and C. T. Rettner, Phys. Rev. Lett. 67, 652 (1991).
- M. C. McMaster and R. J. Madix, J. Chem. Phys. 98, 9963 (1993).
- V. A. Ukrainstev and I. Harrison,
Surf. Sci. Lett. 286, L571 (1993) . - A. C. Luntz and H. F. Winters, J. Chem. Phys. 101, 10 980 (1994).
- P. M. Holmblad, J. Wambach, and I. Chorkendorff, J. Chem. Phys. 102, 8255 (1995).
- Y. K. Sun and W. H. Weinberg,
J. Vac. Sci. Technol. A 8, 2445 (1990) . - R. W. Verhoef, D. Kelly, C. B. Mullins, and W. H. Weinberg,
Surf. Sci. 287/288, 94 (1993) . - D. C. Seets, M. C. Wheeler, and C. B. Mullins, Chin. Phys. 266, 431 (1997).
- D. C. Seets, M. C. Wheeler, and C. B. Mullins, J. Chem. Phys. 107, 3986 (1997).
- D. C. Seets, C. T. Reeves, B. A. Ferguson, M. C. Wheeler, and C. B. Mullins, J. Chem. Phys. 107, 10 229 (1997).
- T. A. Jachimowski, C. T. Hagedorn, and W. H. Weinberg,
Surf. Sci. 393, 126 (1997) . - D. A. King and M. G. Wells,
Proc. R. Soc. London, Ser. A 339, 245 (1974) . - A. C. Luntz and J. Harris,
Surf. Sci. 258, 397 (1991) . - M. Hand and J. Harris, J. Chem. Phys. 92, 7610 (1990).
- A. P. J. Jansen and H. Burghgraef,
Surf. Sci. 344, 149 (1995) . - M.-N. Carré and B. Jackson, J. Chem. Phys. 108, 3722 (1998).
- V. A. Ukrainstev and I. Harrison, J. Chem. Phys. 101, 1564 (1994).
- A. V. Walker and D. A. King, Phys. Rev. Lett. 82, 5156 (1999).
- A. Hopkinson, X.-C. Guo, J. M. Bradley, and D. A. King, J. Chem. Phys. 99, 8262 (1993).
- P. Hoffmann, S. R. Bare, and D. A. King,
Surf. Sci. 117, 245 (1982) . - M. Wilf and P. T. Dawson,
Surf. Sci. 65, 399 (1977) . - F. Solymosi,
Catal. Today 28, 193 (1996) . - M. Valden, N. Xiang, J. Pere, and M. Pessa,
Appl. Surf. Sci. 99, 83 (1996) . - D. H. Fairbrother, X. D. Peng, R. Viswanathan, P. C. Stair, M. Trenary, and F. Fan,
Surf. Sci. Lett. 285, L455 (1993) . - D. J. Oakes, H. E. Newell, F. J. M. Rutten, M. R. S. McCoustra, and M. A. Chesters,
J. Vac. Sci. Technol. A 14, 1439 (1996) . - F. Zaera and H. Hoffmann, J. Phys. Chem. 95, 6397 (1991).
- D. P. T. Watson and D. A. King (unpublished).
- J.-F. Paul and P. Sautet,
J. Phys. Chem. B 102, 1578 (1998) . - R. A. van Santen, A. de Koster, and T. Koerts,
Catal. Lett. 7, 1 (1990) . - C. Minot, M. A. van Hove, and G. A. Somorjai,
Surf. Sci. 127, 441 (1983) . - K. D. Rendulic and A. Winkler,
Surf. Sci. 299/300, 261 (1994) . - W. van Willigen,
Phys. Lett. A 28, 80 (1968) . - H. F. Winters, J. Chem. Phys. 62, 2454 (1975); ,
- T. C. Lo and G. Ehrlich,
Surf. Sci. 179, L19 (1987) . - T. P. Beebe, Jr., D. W. Goodman, B. D. Kay, and J. T. Yates, Jr., J. Chem. Phys. 87, 2305 (1987).
- R. J. Galagher and J. B. Fenn, J. Chem. Phys. 60, 3487 (1974).
- D. J. Auerbach, in Atomic and Molecular Beam Methods, edited by G. Scoles (Oxford University Press, Oxford, 1988).
- J. M. Bradley, X.-C. Guo, A. Hopkinson, and D. A. King, J. Chem. Phys. 104, 4283 (1996).
- D. R. Miller, in Atomic and Molecular Beam Methods, edited by G. Scoles (Oxford University Press, Oxford, 1988).
- D. A. King,
CRC Crit. Rev. Solid State Mater. Sci. 7, 167 (1978) . - A. T. Pasteur, St. J. Dixon-Warren, Q. Ge, and D. A. King, J. Chem. Phys. 106, 8896 (1997).
- J. Jellinek, in Metal-Ligand Interations, edited by N. Russo and D. R. Salahub (Kluwer Academic, New York, 1996).
- J. D. Beckerle, R. R. Cavanagh, M. D. Casassa, E. J. Heilweil, and J. C. Stephnson, J. Chem. Phys. 95, 5403 (1991).
- C. R. Arumainayagam, M. C. McMaster, G. R. Schoofs, and R. J. Madix,
Surf. Sci. 222, 213 (1989) .








