Proton hop paving the way for hydroxyl migration: Theoretical elucidation of fluxionality in transition-metal oxide clusters

Journal of Physical Chemistry Letters

Volumn 1, Issue 20, 2010, Pages 3066-3071

  Ramabhadran, Raghunath O ^a   Mayhall, Nicholas J ^a   Raghavachari, Krishnan ^a  

^a INDIANA UNIVERSITY   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

BRIDGING OXYGEN; ELECTRONIC STRUCTURE THEORY; ENHANCED CATALYTIC ACTIVITY; FLUXIONALITY; HYDROGEN EVOLUTION; HYDROXYL GROUPS; INTERCONVERSIONS; MECHANISTIC STUDIES; RELATIVE POSITIONS; TRANSITION-METAL OXIDES;

CATALYST ACTIVITY; CHEMISORPTION; ELECTRONIC STRUCTURE; ISOMERS; METALLIC COMPOUNDS; OXYGEN; TRANSITION METALS;

PROTONS;

EID: 77958454917     PISSN: None     EISSN: 19487185     Source Type: Journal    
DOI: 10.1021/jz1012033     Document Type: Article

References (42)

1. Rao, C. N. R.; Raveau, B. Transition Metal Oxides; Wiley-VCH: New York, 1998.
2. - (y = 2-5) with Methane J. Phys. Chem. A 2007, 111, 8211-8217 and references therein.
3. 2 Sequential Oxidation Reaction: An Exploration of Kinetic versus Thermodynamic Effects J. Chem. Phys. 2009, 131, 144306/1-144306/8
4. 2 Production and Kinetic Traps J. Chem. Phys. 2009, 131, 144302/1-144302/8
5. - Angew. Chem., Int. Ed. 2007, 46, 4277-4280
6. 2 (110) Angew. Chem., Int. Ed. 2006, 45, 4786-4789
7. 2 with Reduced W sites on Tungsten Oxide Surfaces Angew. Chem., Int. Ed. 2006, 45, 657-660
8. Huang, X.; Zhai, H. J.; Kiran, B.; Wang, L. S. Observation of d-Orbital Aromaticity Angew. Chem., Int. Ed. 2005, 44, 7251-7254
9. 2- (M=Mo, W) J. Phys. Chem. A 2007, 111, 11093-11099
10. n Clusters (M=Mo, W; n =3-5): A Photoelectron Spectroscopy and ab initio Study J. Am. Chem. Soc. 2004, 126, 16134-16141
11. 2 (M=Nb, Ta) J. Am. Chem. Soc. 2007, 129, 13270-13276
12. 4 J. Phys. Chem. A 1999, 103, 1585-1591
13. Sun, Q.; Rao, B. K.; Jena, P.; Stolcic, D.; Kim, Y. D.; Gantefor, G.; Castleman, A. W., Jr. Appearance of Bulk Properties in Small Tungsten Oxide Clusters J. Chem. Phys. 2004, 121, 9417-9422
14. - (M=Cr, W), from Photoelectron Spectroscopy and Quantum Chemical Calculations J. Phys. Chem. A. 2009, 113, 11273-11288
15. Bergeron, D. E.; Castleman, A. W., Jr.; Jones, N. O.; Khanna, S. N. Stable Cluster Motifs for Nanoscale Chromium Oxide Materials Nano Lett. 2004, 111, 261-265
16. n (n = 1-8) J. Phys. Chem. A 2009, 113, 9804-9813
17. n (n =1-5) from Photoelectron Spectroscopy and Density Functional Theory Calculations J. Chem. Phys. 2001, 115, 7935-7944
18. - (M, M? = Cr, Mo, W) J. Phys. Chem. A 2005, 109, 10512-10520
19. - (n = 1-7) using photoelectron spectroscopy J. Chem. Phys. 2006, 125, 164315/1-164315/9
20. Li, S. G.; Dixon, D. A. Molecular and Electronic Structures, Bronsted Basicities, and Lewis Acidities of Group VIB Transition Metal Oxide Clusters J. Phys. Chem. A 2006, 110, 6231-6244
21. Li, S. G.; Hennigan, J. M.; Peterson, K. A.; Dixon, D. A. Accurate Thermochemistry for Transition Metal Oxide Clusters J. Phys. Chem. A 2009, 113, 7861-7877
22. Gong, Y.; Zhou, M.; Andrews, L. Spectroscopic and Theoretical Studies of Transition Metal Oxides and Dioxygen Complexes Chem. Rev. 2009, 109, 6765-6808 and references therein.
23. - Clusters toward Methane and Ethane J. Phys. Chem. A 2006, 110, 2157-2164 and references therein.
24. 2O Reactions J. Chem. Phys. 2009, 130, 124314/1-124314/8
25. Wyrwas, R. B.; Robertson, E. M.; Jarrold, C. C. Reactions between CO and Small Molybdenum Suboxide Cluster Anions J. Chem. Phys. 2007, 126, 214309/1-214309/8
26. - from Oligomerization of CO on Molybdenum Anions J. Am. Chem. Soc. 2006, 128, 13688-13689
27. Johnson, G. E.; Reveles, J. U.; Khanna, S. N.; Castleman, A. W., Jr. Reactivity Trends in the Oxidation of CO by Anionic Transition Metal Oxide Clusters J. Phys. Chem. C 2010, 114, 5438-5446
28. Johnson, G. E.; Mitric, R.; Nossler, M.; Tyo, E. C.; Koutecky, V. B.; Castleman, A. W., Jr. Influence of Charge State on Catalytic Oxidation Reactions at Metal Oxide Clusters Containing Radical Oxygen Centres J. Am. Chem. Soc. 2009, 131, 5460-5470 and references therein.
29. Johnson, G. E.; Reveles, J. U.; Reilly, N. M.; Tyo, E. C.; Khanna, S, N.; Castleman, A. W., Jr. Influence of Stoichiometry and Charge State on the Structure and Reactivity of Cobalt Oxide Clusters with CO J. Phys. Chem. A 2008, 112, 11330-11340
30. Johnson, G. E.; Reveles, J. U.; Reilly, N. M.; Castleman, A. W., Jr. Effect of Charge State and Stoichiometry on the Structure and Reactivity of Nickel Oxide Clusters with CO Int. J. Mass Spectrom. 2009, 280, 93-100
31. Johnson, G. E.; Tyo, E. C.; Castleman, A. W., Jr. Gas-Phase Reactivity of Gold Oxide Cluster Cations with CO J. Phys. Chem. C 2008, 112, 9730-9736
32. + (m =1,2; n =1-5) with CO J. Phys. Chem. C 2007, 111, 19086-19097
33. ± with Carbon Monoxide Chem. Phys. Lett. 2007, 435, 295-300
34. Buörgel, C.; Reilly, N. M.; Johnson, G. E.; Mitrić, R.; Kimble, M, L.; Castleman, A. W.; Bonac?ić-Koutecký, V. Influence of Charge State on the Mechanism of CO Oxidation on Gold Clusters J. Am. Chem. Soc. 2008, 130, 1694-1698 and references therein.
35. Landman, U.; Yoon, B.; Zhang, C.; Heiz, U.; Arenz, M. Factors in Gold Nanocatalysis: Oxidation of CO in the Non-Scalable Size Regime Top. Catal. 2007, 44, 145-158
36. For a classic review on the mechanism of fluxionality and examples featuring structural changes in the functional groups due to fluxionality, see: Band, E.; Muetterties, E. L. Mechanistic Features of Metal Cluster Rearrangements Chem. Rev. 1978, 78, 639-658
37. Heiz, U.; Bullock, E. L. Fundamental Aspects of Catalysis on Supported Metal Clusters J. Mater. Chem. 2004, 14, 566-577
38. Huheey, J. E.; Keiter, E. A.; Keiter, R. L. Inorganic Chemistry Principles of Structure and Reactivity. HarperCollins: New York, 1993.
39. Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Scalemani, G.; Barone, V.; Mennucci, B.; Petersson, G. A.; et al. Gaussian 09, revision h08; Gaussian, Inc.; Wallingford, CT, 2009.
40. Becke, A. D. Density-Functional Thermochemistry. III. The Role of Exact Exchange J. Chem. Phys. 1993, 98, 5648-5652
41. Lee, C. T.; Yang, W. T.; Parr, R. G. Devolopment of the Colle-Salvetti Correlation-Energy Formula into a Functional of the Electron Density Phys. Rev. B 1988, 37, 785-789
42. Andrae, D.; Hausserman, U.; Dolg, M.; Stoll, H.; Preuss, H. Energy-Adjusted Ab Initio Pseudopotentials for the 2nd and 3rd Row Transition-Elements Theor. Chem. Acc. 1990, 77, 123-141