Journal of Chemical Physics
Feedback | Help | Exit
The Journal of Chemical Physics
Search:
   
 
 
 
Previous Article
The isotropic-nematic interface with an oblique anchoring condition
We present numerical and analytic results for uniaxial and biaxial orders at the isotropic-nematic interface within Ginzburg–Landau–de Gennes theory. We study the case where an oblique anc...
Next Article
Calculation of hydrogen storage capacity of metal-organic and covalent-organic frameworks by spillover
We have used accurate ab initio quantum chemistry calculations together with a simple model to study the hydrogen storage capacity of metal-organic and covalent-organic frameworks by spillover. Recent...

First-principles study of methane dehydrogenation on a bimetallic Cu/Ni(111) surface

J. Chem. Phys. 131, 174702 (2009); doi:10.1063/1.3254383

Published 2 November 2009

You are not logged in to this journal. Log in

Wei An,1 X. C. Zeng,2 and C. Heath Turner1
1Department of Chemical and Biological Engineering, The University of Alabama, P.O. Box 870203, Tuscaloosa, Alabama 35487-0203, USA
2Department of Chemistry, University of Nebraska-Lincoln, Lincoln, Nebraska 68588, USA
We present density-functional theory calculations of the dehydrogenation of methane and CHx (x=1–3) on a Cu/Ni(111) surface, where Cu atoms are substituted on the Ni surface at a coverage of (1/4) monolayer. As compared to the results on other metal surfaces, including Ni(111), a similar activation mechanism with different energetics is found for the successive dehydrogenation of CH4 on the Cu/Ni(111) surface. In particular, the activation energy barrier (Eact) for CH-->C+H is found to be 1.8 times larger than that on Ni(111), while Eact for CH4-->CH3+H is 1.3 times larger. Considering the proven beneficial effect of Cu observed in the experimental systems, our findings reveal that the relative Eact in the successive dehydrogenation of CH4 plays a key role in impeding carbon formation during the industrial steam reforming of methane. Our calculations also indicate that previous scaling relationships of the adsorption energy (Eads) for CHx (x=1–3) and carbon on pure metals also hold for several Ni(111)-based alloy systems. ©2009 American Institute of Physics
History: Received 13 August 2009; accepted 5 October 2009; published 2 November 2009
Permalink: http://link.aip.org/link/?JCPSA6/131/174702/1
BUY THIS ARTICLE   (US$24)
Download HTML Download Sectioned HTML Download PDF (1551 kB) View Cart

KEYWORDS and PACS

Keywords
PACS
  • 68.43.Bc
    Ab initio calculations of adsorbate structure and reactions
  • 82.65.+r
    Surface and interface chemistry; heterogeneous catalysis at surfaces
  • 68.43.Mn
    Adsorption kinetics
  • YEAR: 2009

PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
Publisher:
AIP is a member of CrossRef AIP

REFERENCES (89)
View in Separate Window/Tab
For access to fully linked references, you need to log in. For access to fully linked references, you need to Log in.
  1. I. E. Agency, Hydrogen and Fuel Cells: Review of National R&D Programs (OECD, Paris, France, 2004).
  2. J. N. Armor, Appl. Catal., A 176, 159 (1999).
  3. J. R. Rostrup-Nielsen and R. Nielsen, Catal. Rev. - Sci. Eng. 46, 247 (2004).
  4. J. R. Rostrup-Nielsen, Steam Reforming Catalysts (Danish Technical, Copenhagen, 1975).
  5. H. S. Bengaard, J. K. Norskov, J. Sehested, B. S. Clausen, L. P. Nielsen, A. M. Molenbroek, and J. R. Rostrup-Nielsen, J. Catal. 209, 365 (2002).
  6. H. S. Bengaard, I. Alstrup, I. Chorkendorff, S. Ullmann, J. R. Rostrup-Nielsen, and J. K. Norskov, J. Catal. 187, 238 (1999).
  7. F. Abild-Pedersen, J. Greeley, and J. K. Norskov, Catal. Lett. 105, 9 (2005).
  8. F. Abild-Pedersen, O. Lytken, J. Engbaek, G. Nielsen, I. Chorkendorff, and J. K. Norskov, Surf. Sci. 590, 127 (2005).
  9. C. T. Au, C. F. Ng, and M. S. Liao, J. Catal. 185, 12 (1999).
  10. H. L. Abbott and I. Harrison, J. Catal. 254, 27 (2008).
  11. I. M. Ciobica, F. Frechard, R. A. van Santen, A. W. Kleyn, and J. Hafner, Chem. Phys. Lett. 311, 185 (1999).
  12. I. M. Ciobica, F. Frechard, R. A. van Santen, A. W. Kleyn, and J. Hafner, J. Phys. Chem. B 104, 3364 (2000).
  13. R. C. Egeberg and I. Chorkendorff, Catal. Lett. 77, 207 (2001).
  14. J. H. Larsen, P. M. Holmblad, and I. Chorkendorff, J. Chem. Phys. 110, 2637 (1999).
  15. J. M. Wei and E. Iglesia, J. Catal. 225, 116 (2004).
  16. J. M. Wei and E. Iglesia, J. Phys. Chem. B 108, 7253 (2004).
  17. A. Kokalj, N. Bonini, S. de Gironcoli, C. Sbraccia, G. Fratesi, and S. Baroni, J. Am. Chem. Soc. 128, 12448 (2006).
  18. A. Kokalj, N. Bonini, C. Sbraccia, S. de Gironcoli, and S. Baroni, J. Am. Chem. Soc. 126, 16732 (2004).
  19. C. T. Au, M. S. Liao, and C. F. Ng, Chem. Phys. Lett. 267, 44 (1997).
  20. B. S. Bunnik and G. J. Kramer, J. Catal. 242, 309 (2006).
  21. G. Henkelman and H. Jonsson, Phys. Rev. Lett. 86, 664 (2001).
  22. H. L. Abbott and I. Harrison, J. Phys. Chem. B 109, 10371 (2005).
  23. G. Henkelman, A. Arnaldsson, and H. Jonsson, J. Chem. Phys. 124, 044706 (2006).
  24. J. M. Wei and E. Iglesia, Angew. Chem., Int. Ed. 43, 3685 (2004).
  25. M. S. Liao, C. T. Au, and C. F. Ng, Chem. Phys. Lett. 272, 445 (1997).
  26. M. S. Liao and Q. E. Zhang, J. Mol. Catal. A: Chem. 136, 185 (1998).
  27. C. J. Zhang and P. Hu, J. Chem. Phys. 116, 322 (2002).
  28. J. F. Paul and P. Sautet, J. Phys. Chem. B 102, 1578 (1998).
  29. A. T. Anghel, D. J. Wales, S. J. Jenkins, and D. A. King, Phys. Rev. B 71, 113410 (2005).
  30. A. Bukoski, H. L. Abbott, and I. Harrison, J. Chem. Phys. 123, 094707 (2005).
  31. M. A. Petersen, S. J. Jenkins, and D. A. King, J. Phys. Chem. B 108, 5909 (2004).
  32. M. A. Petersen, S. J. Jenkins, and D. A. King, J. Phys. Chem. B 108, 5920 (2004).
  33. J. M. Wei and E. Iglesia, J. Phys. Chem. B 108, 4094 (2004).
  34. C. J. Zhang and P. Hu, J. Chem. Phys. 116, 4281 (2002).
  35. H. Burghgraef, A. P. J. Jansen, and R. A. van Santen, J. Chem. Phys. 101, 11012 (1994).
  36. H. Burghgraef, A. P. J. Jansen, and R. A. van Santen, J. Chem. Phys. 103, 6562 (1995).
  37. H. Burghgraef, A. P. J. Jansen, and R. A. van Santen, Surf. Sci. 324, 345 (1995).
  38. A. Groß, Top. Catal. 37, 29 (2006).
  39. H. Yang and J. L. Whitten, Surf. Sci. 289, 267 (1993).
  40. F. Besenbacher, I. Chorkendorff, B. S. Clausen, B. Hammer, A. M. Molenbroek, J. K. Norskov, and I. Stensgaard, Science 279, 1913 (1998).
  41. P. M. Holmblad, J. H. Larsen, I. Chorkendorff, L. P. Nielsen, F. Besenbacher, I. Stensgaard, E. Laegsgaard, P. Kratzer, B. Hammer, and J. K. Norskov, Catal. Lett. 40, 131 (1996).
  42. P. M. Holmblad, J. H. Larsen, and I. Chorkendorff, J. Chem. Phys. 104, 7289 (1996).
  43. P. Kratzer, B. Hammer, and J. K. Norskov, J. Chem. Phys. 105, 5595 (1996).
  44. E. Nikolla, A. Holewinski, J. Schwank, and S. Linic, J. Am. Chem. Soc. 128, 11354 (2006).
  45. E. Nikolla, J. Schwank, and S. Linic, J. Catal. 263, 220 (2009).
  46. E. Nikolla, J. Schwank, and S. Linic, J. Am. Chem. Soc. 131, 2747 (2009).
  47. S. Saadi, B. Hinnemann, S. Helveg, C. C. Appel, F. Abild-Pedersen, and J. K. Norskov, Surf. Sci. 603, 762 (2009).
  48. E. Nikolla, J. Schwank, and S. Linic, J. Catal. 250, 85 (2007).
  49. E. Nikolla, J. W. Schwank, and S. Linic, Catal. Today 136, 243 (2008).
  50. A. Christensen, A. V. Ruban, P. Stoltze, K. W. Jacobsen, H. L. Skriver, J. K. Norskov, and F. Besenbacher, Phys. Rev. B 56, 5822 (1997).
  51. J. R. Rostrup-Nielsen and I. Alstrup, Catal. Today 53, 311 (1999).
  52. M. T. Tavares, C. A. Bernardo, I. Alstrup, and J. R. Rostrupnielsen, J. Catal. 100, 545 (1986).
  53. C. A. Bernardo, I. Alstrup, and J. R. Rostrupnielsen, J. Catal. 96, 517 (1985).
  54. D. W. Blaylock, T. Ogura, W. H. Green, and G. J. O. Beran, J. Phys. Chem. C 113, 4898 (2009).
  55. G. Kresse and J. Hafner, J. Phys.: Condens. Matter 6, 8245 (1994).
  56. G. Kresse, J. Furthmuller, and J. Hafner, Phys. Rev. B 50, 13181 (1994).
  57. G. Kresse and J. Furthmuller, Phys. Rev. B 54, 11169 (1996).
  58. J. P. Perdew, K. Burke, and M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996).
  59. G. Kresse and D. Joubert, Phys. Rev. B 59, 1758 (1999).
  60. M. Methfessel and A. T. Paxton, Phys. Rev. B 40, 3616 (1989).
  61. I. Alstrup, M. T. Tavares, C. A. Bernardo, O. Sorensen, and J. R. Rostrup-Nielsen, Mater. Corros. 49, 367 (1998).
  62. G. Henkelman, B. P. Uberuaga, and H. Jonsson, J. Chem. Phys. 113, 9901 (2000).
  63. C. A. Menning and J. G. G. Chen, J. Chem. Phys. 130, 174709 (2009).
  64. J. R. Rostrup-Nielsen, J. Sehested, and J. K. Norskov, Adv. Catal. 47, 65 (2002).
  65. M. B. Lee, Q. Y. Yang, and S. T. Ceyer, J. Chem. Phys. 87, 2724 (1987).
  66. M. B. Lee, Q. Y. Yang, S. L. Tang, and S. T. Ceyer, J. Chem. Phys. 85, 1693 (1986).
  67. S. T. Ceyer, J. D. Beckerle, M. B. Lee, S. L. Tang, Q. Y. Yang, and M. A. Hines, J. Vac. Sci. Technol. A 5, 501 (1987).
  68. P. M. Holmblad, J. Wambach, and I. Chorkendorff, J. Chem. Phys. 102, 8255 (1995).
  69. L. Hanley, Z. Xu, and J. T. Yates, Surf. Sci. 248, L265 (1991).
  70. R. D. Beck, P. Maroni, D. C. Papageorgopoulos, T. T. Dang, M. P. Schmid, and T. R. Rizzo, Science 302, 98 (2003).
  71. P. Maroni, D. C. Papageorgopoulos, M. Sacchi, T. T. Dang, R. D. Beck, and T. R. Rizzo, Phys. Rev. Lett. 94, 246104 (2005).
  72. L. B. F. Juurlink, R. R. Smith, D. R. Killelea, and A. L. Utz, Phys. Rev. Lett. 94, 208303 (2005).
  73. D. R. Killelea, V. L. Campbell, N. S. Shuman, and A. L. Utz, Science 319, 790 (2008).
  74. T. P. Beebe, D. W. Goodman, B. D. Kay, and J. T. Yates, J. Chem. Phys. 87, 2305 (1987).
  75. H. Yang and J. L. Whitten, J. Chem. Phys. 96, 5529 (1992).
  76. R. M. Watwe, H. S. Bengaard, J. R. Rostrup-Nielsen, J. A. Dumesic, and J. K. Norskov, J. Catal. 189, 16 (2000).
  77. Q. Y. Yang, K. J. Maynard, A. D. Johnson, and S. T. Ceyer, J. Chem. Phys. 102, 7734 (1995).
  78. H. Yang and J. L. Whitten, J. Am. Chem. Soc. 113, 6442 (1991).
  79. M. P. Kaminsky, N. Winograd, G. L. Geoffroy, and M. A. Vannice, J. Am. Chem. Soc. 108, 1315 (1986).
  80. A. Michaelides and P. Hu, J. Chem. Phys. 112, 6006 (2000).
  81. A. Michaelides and P. Hu, J. Chem. Phys. 112, 8120 (2000).
  82. F. Abild-Pedersen, J. Greeley, F. Studt, J. Rossmeisl, T. R. Munter, P. G. Moses, E. Skulason, T. Bligaard, and J. K. Norskov, Phys. Rev. Lett. 99, 016105 (2007).
  83. D. L. Trimm, Catal. Today 37, 233 (1997).
  84. B. Hammer and J. K. Norskov, Surf. Sci. 343, 211 (1995).
  85. B. Hammer, Top. Catal. 37, 3 (2006).
  86. G. Jones, T. Bligaard, F. Abild-Pedersen, and J. K. Norskov, J. Phys.: Condens. Matter 20, 064239 (2008).
  87. G. Jones, J. G. Jakobsen, S. S. Shim, J. Kleis, M. P. Andersson, J. Rossmeisl, F. Abild-Pedersen, T. Bligaard, S. Helveg, B. Hinnemann, J. R. Rostrup-Nielsen, I. Chorkendorff, J. Sehested, and J. K. Norskov, J. Catal. 259, 147 (2008).
  88. F. Studt, F. Abild-Pedersen, T. Bligaard, R. Z. Sorensen, C. H. Christensen, and J. K. Norskov, Science 320, 1320 (2008).
  89. E. M. Fernandez, P. G. Moses, A. Toftelund, H. A. Hansen, J. I. Martinez, F. Abild-Pedersen, J. Kleis, B. Hinnemann, J. Rossmeisl, T. Bligaard, and J. K. Norskov, Angew. Chem., Int. Ed. 47, 4683 (2008).

CITING ARTICLES
For access to citing articles, you need to log in.
For access to citing articles, you need to Log in.


Copyright © American Institute of Physics