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Title: Surface science investigation of the water-gas shift reaction on Cu(111)

Abstract

The authors have studied the kinetics of the water-gas shift reaction on a clean Cu(111) single-crystal surface using an apparatus which allows rapid transfer of the catalyst between a microreactor and an ultrahigh-vacuum chamber for surface preparation and postreaction surface analyses (AES), XPS, LEED). At 10 Torr H/sub 2/O, 26 Torr CO, and 612 K, the reaction proceeds with an activation energy of 17 kcal/mole and reaction orders in H/sub 2/O and CO pressures of zero and 0.5-1.0, respectively. The surface appears completely metallic and relatively free of adsorbed species in postreaction analysis, even when heavily preoxidized. The kinetics compare favorably with data for high-surface-area Cu/ZnO or Cu-based catalysts, indicating that metallic Cu is the active ingredient in these. The rate is limited by dissociative adsorption of water under their conditions. The authors were unable to produce significant coverages of oxygen species on Cu(111) by dosing pure H/sub 2/O at 10 Torr and 500-650 K. The mechanism is discussed in light of surface science measurements on Cu surfaces. The Cu(111) surface was also dosed with Zn from aqueous solution, and the resulting ZnO/sub x/Cu(111) surfaces were tested for activity as water-gas shift catalysts. No marked changes in activity compared tomore » clean Cu(111) were observed. A new method for increasing gas chromatographic sensitivities for low sampling pressures (< 1 atm) is also described. 46 references.« less

Authors:
;
Publication Date:
Research Org.:
Indiana Univ., Bloomington
OSTI Identifier:
5450008
Resource Type:
Journal Article
Journal Name:
J. Catal.; (United States)
Additional Journal Information:
Journal Volume: 104:1
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 10 SYNTHETIC FUELS; AMMONIA; SYNTHESIS; COPPER; CATALYTIC EFFECTS; HYDROGEN PRODUCTION; WATER GAS PROCESSES; CHEMICAL REACTION KINETICS; ACTIVATION ENERGY; AUGER ELECTRON SPECTROSCOPY; CARBON MONOXIDE; ELECTRON DIFFRACTION; GAS CHROMATOGRAPHY; PHOTOELECTRON SPECTROSCOPY; SURFACE PROPERTIES; WATER; X-RAY SPECTROSCOPY; ZINC; CARBON COMPOUNDS; CARBON OXIDES; CHALCOGENIDES; CHEMICAL REACTIONS; CHROMATOGRAPHY; COHERENT SCATTERING; DIFFRACTION; ELECTRON SPECTROSCOPY; ELEMENTS; ENERGY; HYDRIDES; HYDROGEN COMPOUNDS; KINETICS; METALS; NITROGEN COMPOUNDS; NITROGEN HYDRIDES; OXIDES; OXYGEN COMPOUNDS; REACTION KINETICS; SCATTERING; SEPARATION PROCESSES; SPECTROSCOPY; TRANSITION ELEMENTS; 080104* - Hydrogen- Production- Water Gas Processes; 090300 - Inorganic Hydrogen Compound Fuels- (-1989)

Citation Formats

Campbell, C T, and Daube, K A. Surface science investigation of the water-gas shift reaction on Cu(111). United States: N. p., 1987. Web. doi:10.1016/0021-9517(87)90341-1.
Campbell, C T, & Daube, K A. Surface science investigation of the water-gas shift reaction on Cu(111). United States. https://doi.org/10.1016/0021-9517(87)90341-1
Campbell, C T, and Daube, K A. 1987. "Surface science investigation of the water-gas shift reaction on Cu(111)". United States. https://doi.org/10.1016/0021-9517(87)90341-1.
@article{osti_5450008,
title = {Surface science investigation of the water-gas shift reaction on Cu(111)},
author = {Campbell, C T and Daube, K A},
abstractNote = {The authors have studied the kinetics of the water-gas shift reaction on a clean Cu(111) single-crystal surface using an apparatus which allows rapid transfer of the catalyst between a microreactor and an ultrahigh-vacuum chamber for surface preparation and postreaction surface analyses (AES), XPS, LEED). At 10 Torr H/sub 2/O, 26 Torr CO, and 612 K, the reaction proceeds with an activation energy of 17 kcal/mole and reaction orders in H/sub 2/O and CO pressures of zero and 0.5-1.0, respectively. The surface appears completely metallic and relatively free of adsorbed species in postreaction analysis, even when heavily preoxidized. The kinetics compare favorably with data for high-surface-area Cu/ZnO or Cu-based catalysts, indicating that metallic Cu is the active ingredient in these. The rate is limited by dissociative adsorption of water under their conditions. The authors were unable to produce significant coverages of oxygen species on Cu(111) by dosing pure H/sub 2/O at 10 Torr and 500-650 K. The mechanism is discussed in light of surface science measurements on Cu surfaces. The Cu(111) surface was also dosed with Zn from aqueous solution, and the resulting ZnO/sub x/Cu(111) surfaces were tested for activity as water-gas shift catalysts. No marked changes in activity compared to clean Cu(111) were observed. A new method for increasing gas chromatographic sensitivities for low sampling pressures (< 1 atm) is also described. 46 references.},
doi = {10.1016/0021-9517(87)90341-1},
url = {https://www.osti.gov/biblio/5450008}, journal = {J. Catal.; (United States)},
number = ,
volume = 104:1,
place = {United States},
year = {1987},
month = {3}
}