Molecular-scale perspective of water-catalyzed methanol dehydrogenation to formaldehyde

ACS Nano

Volumn 7, Issue 7, 2013, Pages 6181-6187

  Boucher, Matthew B ^a   Marcinkowski, Matthew D ^b   Liriano, Melissa L ^b   Murphy, Colin J ^b   Lewis, Emily A ^b   Jewell, April D ^b   Mattera, Michael F G ^b   Kyriakou, Georgios ^b,c   Flytzani Stephanopoulos, Maria ^a   Sykes, E Charles H ^b  

^a Tufts University   (United States)

^b TUFTS UNIVERSITY   (United States)

^c UNIVERSITY OF HULL   (United Kingdom)

Author keywords

alloy; copper; methanol; palladium; steam reforming; water

Indexed keywords

CHEMICAL TRANSFORMATIONS; COPPER CATALYST; METALLIC COPPER; METHANOL CONVERSION; METHANOL DEHYDROGENATION; METHANOL STEAM REFORMING; OXYGEN ADATOMS; WATER MOLECULE;

ALLOYING; CARBON DIOXIDE; CERIUM ALLOYS; COPPER; FORMALDEHYDE; HYDROGEN PRODUCTION; PALLADIUM; STEAM REFORMING; SURFACE REACTIONS; WATER;

METHANOL;

COPPER; FORMALDEHYDE; HYDROGEN; METHANOL; NANOMATERIAL; WATER;

CATALYSIS; CHEMISTRY; ISOLATION AND PURIFICATION; MATERIALS TESTING; PARTICLE SIZE; ULTRASTRUCTURE; ARTICLE;

CATALYSIS; COPPER; FORMALDEHYDE; HYDROGEN; MATERIALS TESTING; METHANOL; NANOSTRUCTURES; PARTICLE SIZE; WATER;

EID: 84880826077     PISSN: 19360851     EISSN: 1936086X     Source Type: Journal    
DOI: 10.1021/nn402055k     Document Type: Article

References (39)

1. Palo, D. R.; Dagle, R. A.; Holladay, J. D. Methanol Steam Reforming for Hydrogen Production Chem. Rev. 2007, 107, 3992-4021
2. 3 Catalysts. Part 2. A Comprehensive Kinetic Model Appl. Catal. A 1999, 179, 31-49
3. 3. Part 1: The Reaction Network Appl. Catal. A 1999, 179, 21-29
4. Takezawa, N.; Iwasa, N. Steam Reforming and Dehydrogenation of Methanol: Difference in the Catalytic Functions of Copper and Group VIII Metals Catal. Today 1997, 36, 45-56
5. Lindstrom, B.; Pettersson, L. J. Hydrogen Generation by Steam Reforming of Methanol over Copper-Based Catalysts for Fuel Cell Applications Int. J. Hydrogen Energy 2001, 26, 923-933
6. Bowker, M.; Madix, R. J. XPS, UPS and Thermal Desorption Studies of Alcohol Adsorption on Cu(110) Surf. Sci. 1980, 95, 190-206
7. 2CO on a Copper(110) Catalyst J. Catal. 1978, 53, 208-227
8. Bowker, M. Active Sites in Methanol Oxidation on Cu(110) Determined by STM and Molecular Beam Measurements Top. Catal. 1996, 3, 461-468
9. Davies, P. R.; Bowker, M. On the Nature of the Active Site in Catalysis: The Reactivity of Surface Oxygen on Cu(110) Catal. Today 2010, 154, 31-37
10. Liu, X.; Madix, R. J.; Friend, C. M. Unraveling Molecular Transformations on Surfaces: A Critical Comparison of Oxidation Reactions on Coinage Metals Chem. Soc. Rev. 2008, 37, 2243-2261
11. Russell, J. N.; Gates, S. M.; Yates, J. T. Reaction of Methanol with Cu(111) and Cu(111) + O(ads) Surf. Sci. 1985, 163, 516-540
12. Madix, R. J.; Telford, S. G. Primary and Secondary Kinetic Isotope Effects for Methoxy Dehydrogenation and Cu(110): Absence of Tunnelling Corrections Surf. Sci. 1995, 328, L576-L581
13. Leibsle, F. M.; Francis, S. M.; Haq, S.; Bowker, M. Aspects of Formaldehyde Synthesis on Cu(110) As Studied by STM Surf. Sci. 1994, 318, 46-60
14. Matsumoto, T.; Bennett, R. A.; Stone, P.; Yamada, T.; Domen, K.; Bowker, M. Scanning Tunneling Microscopy Studies of Oxygen Adsorption on Cu(111) Surf. Sci. 2001, 471, 225-245
15. Johnson, S.; Madix, R. J. Sulfur Induced Selectivity Changes for Methanol Decomposition on Ni(100) Surf. Sci. 1981, 103, 361-396
16. Johnston, S. M.; Mulligan, A.; Dhanak, V.; Kadodwala, M. The Structure of Methanol and Methoxy on Cu(111) Surf. Sci. 2003, 530, 111-119
17. Pan, M.; Pozun, Z. D.; Yu, W.-Y.; Henkelman, G.; Mullins, C. B. Structure Revealing H/D Exchange with Co-adsorbed Hydrogen and Water on Gold J. Phys. Chem. Lett. 2012, 3, 1894-1899
18. Brush, A. J.; Pan, M.; Mullins, C. B. Methanol O-H Bond Dissociation on H-Precovered Gold Originating from a Structure with a Wide Range of Surface Stability J. Phys. Chem. C 2012, 116, 20982-20989
19. Gomes, J. R. B.; Gomes, J. A. N. F.; Illas, F. First-Principles Study of the Adsorption of Formaldehyde on the Clean and Atomic Oxygen Covered Cu(111) Surface J. Mol. Catal. A 2001, 170, 187-193
20. Bryden, T. R.; Garrett, S. J. Adsorption and Polymerization of Formaldehyde on Cu(100) J. Phys. Chem. B 1999, 103, 10481-10488
21. Somorjai, G. A.; Li, Y. Introduction to Surface Chemistry and Catalysis; Wiley: New York, 2010; p 800.
22. Michaelides, A.; Morgenstern, K. Ice Nanoclusters at Hydrophobic Metal Surfaces Nat. Mater. 2007, 6, 597-601
23. Mehlhorn, M.; Carrasco, J.; Michaelides, A.; Morgenstern, K. Local Investigation of Femtosecond Laser Induced Dynamics of Water Nanoclusters on Cu(111) Phys. Rev. Lett. 2009, 103, 0261011-0261014
24. Mehlhorn, M.; Morgenstern, K. Faceting during the Transformation of Amorphous to Crystalline Ice Phys. Rev. Lett. 2007, 99, 2461011-2461014
25. Morgenstern, K.; Rieder, K.-H. Formation of the Cyclic Ice Hexamer via Excitation of Vibrational Molecular Modes by the Scanning Tunneling Microscope J. Chem. Phys. 2002, 116, 5746-5752
26. Lawton, T. J.; Carrasco, J.; Baber, A. E.; Michaelides, A.; Sykes, E. C. H. Hydrogen-Bonded Assembly of Methanol on Cu(111) Phys. Chem. Chem. Phys. 2012, 14, 11846-11852
27. Ren, J.; Meng, S. Atomic Structure and Bonding of Water Overlayer on Cu(110): The Borderline for Intact and Dissociative Adsorption J. Am. Chem. Soc. 2006, 128, 9282-9283
28. Andersson, K.; Ketteler, G.; Bluhm, H.; Yamamoto, S.; Ogasawara, H.; Pettersson, L. G. M.; Salmeron, M.; Nilsson, A. Bridging the Pressure Gap in Water and Hydroxyl Chemistry on Metal Surfaces: The Cu(110) Case J. Phys. Chem. C 2007, 111, 14493-14499
29. Andersson, K.; Gomez, A.; Glover, C.; Nordlund, D.; Ostrom, H.; Schiros, T.; Takahashi, O.; Ogasawara, H.; Pettersson, L. G. M.; Nilsson, A. Molecularly Intact and Dissociative Adsorption of Water on Clean Cu (110): A Comparison with the Water/Ru(001) System Surf. Sci. 2005, 585, L183-L189
30. Andersson, K.; Ketteler, G.; Bluhm, H.; Yamamoto, S.; Ogasawara, H.; Pettersson, L. G. M.; Salmeron, M.; Nilsson, A. Autocatalytic Water Dissociation on Cu(110) at Near Ambient Conditions J. Am. Chem. Soc. 2008, 130, 2793-2797
31. Chen, A. K.; Masel, R. Direct Conversion of Methanol to Formaldehyde in the Absence of Oxygen on Cu(210) Surf. Sci. 1995, 343, 17-23
32. Merte, L. R.; Peng, G.; Bechstein, R.; Rieboldt, F.; Farberow, C. A.; Grabow, L. C.; Kudernatsch, W.; Wendt, S.; Lægsgaard, E.; Mavrikakis, M. et al. Water-Mediated Proton Hopping on an Iron Oxide Surface Science 2012, 336, 889-893
33. Tierney, H. L.; Baber, A. E.; Kitchin, J. R.; Sykes, E. C. H. Hydrogen Dissociation and Spillover on Individual Isolated Palladium Atoms Phys. Rev. Lett. 2009, 103, 2461021-2461024
34. Tierney, H. L.; Baber, A. E.; Sykes, E. C. H. Atomic-Scale Imaging and Electronic Structure Determination of Catalytic Sites on Pd/Cu Near Surface Alloys J. Phys. Chem. C 2009, 113, 7246-7250
35. Kyriakou, G.; Boucher, M. B.; Jewell, A. D.; Lewis, E. A.; Lawton, T. J.; Baber, A. E.; Tierney, H. L.; Flytzani-Stephanopoulos, M.; Sykes, E. C. H. Isolated Metal Atom Geometries as a Strategy for Selective Heterogeneous Hydrogenations Science 2012, 335, 1209-1212
36. Baber, A. E.; Tierney, H. L.; Lawton, T. J.; Sykes, E. C. H. An Atomic-Scale View of Palladium Alloys and Their Ability To Dissociate Molecular Hydrogen ChemCatChem 2011, 3, 607-614
37. Marcinkowski, M. D.; Jewell, A. D.; Stamatakis, M.; Boucher, M. B.; Lewis, E. A.; Murphy, C. J.; Kyriakou, G.; Sykes, E. C. H. Controlling a Spillover Pathway with the Molecular Cork Effect Nat. Mater. 2013, 12, 523-528
38. Chen, J.-J.; Jiang, Z.-C.; Zhou, Y.; Chakraborty, B. R.; Winograd, N. Spectroscopic Studies of Methanol Decomposition on Pd(111) Surf. Sci. 1995, 328, 248-262
39. Kitchin, J.; Nørskov, J.; Barteau, M.; Chen, J. Role of Strain and Ligand Effects in the Modification of the Electronic and Chemical Properties of Bimetallic Surfaces Phys. Rev. Lett. 2004, 93, 156801-156806