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W. Unterberger, Harald Gabasch, K. Hayek, B. Klötzer (2005)
Catalytic Oxidation of Ethene on Polycrystalline Palladium: Influence of the Oxidation State of the SurfaceCatalysis Letters, 104
Matthias Morkel, V. Kaichev, G. Rupprechter, H. Freund, I. Prosvirin, V. Bukhtiyarov (2004)
Methanol dehydrogenation and formation of carbonaceous overlayers on Pd(111) studied by high-pressure SFG and XPS spectroscopyJournal of Physical Chemistry B, 108
S. Bertarione, D. Scarano, A. Zecchina, V. Johánek, J. Hoffmann, S. Schauermann, J. Libuda, G. Rupprechter, H. Freund (2004)
Surface reactivity of Pd nanoparticles supported on polycrystalline substrates as compared to thin film model catalysts: infrared study of CH3OH adsorptionJournal of Catalysis, 223
J. Lee, D. Trimm (1995)
Catalytic combustion of methaneFuel Processing Technology, 42
Harald Gabasch, K. Hayek, B. Klötzer, A. Knop‐Gericke, R. Schlögl (2006)
Carbon incorporation in Pd(111) by adsorption and dehydrogenation of ethene.The journal of physical chemistry. B, 110 10
Yi-Fan Han, D. Kumar, C. Sivadinarayana, Abraham Clearfield, D. Goodman (2004)
The Formation of PdCx over Pd-Based Catalysts in Vapor-Phase Vinyl Acetate Synthesis: Does a Pd–Au Alloy Catalyst Resist Carbide Formation?Catalysis Letters, 94
S. Shaikhutdinov, M. Frank, M. Bäumer, S. Jackson, R. Oldman, J. Hemminger, H. Freund (2002)
Effect of Carbon Deposits on Reactivity of Supported Pd Model CatalystsCatalysis Letters, 80
D. Ciuparu, E. Altman, L. Pfefferle (2001)
Contributions of Lattice Oxygen in Methane Combustion over PdO-Based CatalystsJournal of Catalysis, 203
D. King, M. Wells (1972)
Molecular Beam Investigation of Adsorption Kinetics on Bulk Metal Targets: Nitrogen on TungstenSurface Science, 29
M. Sock, A. Eichler, S. Surnev, J. Andersen, B. Klötzer, K. Hayek, M. Ramsey, F. Netzer (2003)
High-resolution electron spectroscopy of different adsorption states of ethylene on Pd(111)Surface Science, 545
B. Klötzer, W. Unterberger, K. Hayek (2003)
Adsorption and hydrogenation of CO on Pd(1 1 1) and Rh(1 1 1) modified by subsurface vanadiumSurface Science, 532
L. Kesmodel, J. Gates (1981)
Ethylene Adsorption and Reaction on Pd(111): An Angle-Dependent EELS Analysis.Surface Science, 111
D. Teschner, E. Vass, M. Hävecker, S. Zafeiratos, P. Schnörch, H. Sauer, A. Knop‐Gericke, R. Schlögl, Mounir Chamam, A. Wootsch, A. Canning, J. Gamman, S. Jackson, J. McGregor, L. Gladden (2006)
Alkyne hydrogenation over Pd catalysts: A new paradigmJournal of Catalysis, 242
S. Ziemecki, G. Jones, D. Swartzfager, R. Harlow, J. Faber (1985)
Formation of interstitial palladium-carbon phase by interaction of ethylene, acetylene, and carbon monoxide with palladiumJournal of the American Chemical Society, 107
L. KesmodelL, A. GatesJ (1981)
Pd(111)上へのエチレン吸着と反応 角度依存EELS解析Surface Science, 111
J. Mccarty (1995)
Kinetics of PdO combustion catalysisCatalysis Today, 26
M. Bozack, L. Muehlhoff, J. Russell, W. Choyke, J. Yates (1987)
Methods in semiconductor surface chemistryJournal of Vacuum Science and Technology, 5
Yi-fan Han, D. Kumar, C. Sivadinarayana, D. Goodman (2004)
Kinetics of ethylene combustion in the synthesis of vinyl acetate over a Pd/SiO2 catalystJournal of Catalysis, 224
Jinhai Xie, Qinglin Zhang, K. Chuang (2004)
A Study of Hydrophobic Pd/SDB Catalyst for Ethylene Partial Oxidation to Acetic AcidCatalysis Letters, 93
S. Oh, P. Mitchell, R. Siewert (1991)
Methane oxidation over alumina-supported noble metal catalysts with and without cerium additivesJournal of Catalysis, 132
A. Evnin, J. Rabo, P. Kasai (1973)
Heterogeneously catalyzed vapor-phase oxidation of ethylene to acetaldehydeJournal of Catalysis, 30
P. Salomonsson, S. Johansson, B. Kasemo (1995)
Methane oxidation over PdOx: on the mechanism for the hysteresis in activity and oxygen contentCatalysis Letters, 33
Harald Gabasch, K. Hayek, B. Klötzer, W. Unterberger, E. Kleimenov, D. Teschner, S. Zafeiratos, M. Hävecker, A. Knop‐Gericke, R. Schlögl, B. Aszalos-Kiss, D. Zemlyanov (2007)
Methane Oxidation on Pd(111): In Situ XPS Identification of Active PhaseJournal of Physical Chemistry C, 111
R. Heck, R. Farrauto, S. Gulati (1994)
Catalytic Air Pollution Control: Commercial Technology
D. Stacchiola, F. Calaza, L. Burkholder, W. Tysoe (2004)
Vinyl acetate formation by the reaction of ethylene with acetate species on oxygen-covered Pd(111).Journal of the American Chemical Society, 126 47
K. Sano, H. Uchida, Syoichirou Wakabayashi (1999)
A new process for acetic acid production by direct oxidation of ethyleneCatalysis Surveys from Asia, 3
M. Kaltchev, A. Thompson, W. Tysoe (1997)
Reflection-absorption infrared spectroscopy of ethylene on palladium (111) at high pressureSurface Science, 391
J. Seoane (1980)
Ethylene oxidation to acetic acid with Pd-V2O5 catalysts: II. Kinetics of the catalytic reactionJournal of Catalysis, 63
F. Leisenberger, G. Koller, M. Sock, S. Surnev, M. Ramsey, F. Netzer, B. Klötzer, K. Hayek (2000)
Surface and subsurface oxygen on Pd(111)Surface Science, 445
M. Bowker, C. Morgan, N. Perkins, R. Holroyd, E. Fourré, F. Grillo, Alexander MacDowall (2005)
Ethene adsorption, dehydrogenation and reaction with Pd(110): Pd as a carbon 'sponge'.The journal of physical chemistry. B, 109 6
Harald Gabasch, W. Unterberger, K. Hayek, B. Klötzer, G. Kresse, C. Klein, M. Schmid, P. Varga (2006)
Growth and decay of the Pd(111)-Pd5O4 surface oxide : Pressure-dependent kinetics and structural aspectsSurface Science, 600
The catalytic oxidation of ethene was studied on Pd(111) in the 10−7–10−6 mbar pressure range by a molecular beam TPR hysteresis experiment between 400 K and 1,000 K. Two important effects were identified: the reaction-blocking effect of a dense chemisorbed adlayer of oxygen and the promotional effect of dissolved carbon segregating back to the surface and efficiently reducing the adsorbed oxygen. A strong dependence of the catalytic activity on the oxygen partial pressure is explained by the inhibiting effect of oxygen adsorption; high oxygen pressures in fact extinguish the reaction. The presence of oxygen-free metal surface area, where ethene can dissociate, is necessary for high activity. During heating the highest activity is observed at T ∼ 620 K, where a combination of oxygen clean-off by carbon segregating back to the surface is combined with a high ethene adsorption rate, thus forming additional reaction sites and additional reaction products. During heating this carbon-induced clean-off of O(ad) is very efficient because the dissolved C atoms rather accumulate in the surface-near region and largely segregate back to the surface at T > 600 K. In contrast, during cooling from higher temperatures a high surface-near carbon bulk concentration does not build up because the bulk mobility of C atoms is also high and the faster diffusion of C into deeper layers counteracts carbon enrichment in the surface-near metal bulk. This effect favours a higher oxygen surface coverage and a stronger deactivation during cooling. If the carbon loading of the surface-near region was increased by decomposition of clean ethene prior to the reaction experiment, the promotional effect during the heating cycle was strongly enhanced, but the cooling cycle showed no memory of the C presaturation. Generally, the observed hysteresis effects stem from an interplay of combined oxygen site blocking and carbon diffusion effects.
Catalysis Letters – Springer Journals
Published: Jul 31, 2007
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