Details
| Original language | English |
|---|---|
| Article number | 114709 |
| Journal | Journal of Chemical Physics |
| Volume | 125 |
| Issue number | 11 |
| Publication status | Published - 20 Sept 2006 |
Abstract
The adsorbate species present during partial oxidation of methanol on a Cu(110) surface have been investigated in the 10-5 mbar range with in situ x-ray photoelectron spectroscopy and rate measurements. Two reaction intermediates were identified, methoxy with a C 1s binding energy (BE) of 285.4 eV and formate with a C is BE of 287.7 eV. The c(2×2) overlayer formed under reaction conditions is assigned to formate. Two states of adsorbed oxygen were found characterized by O 1s BE's of 529.6 and 528.9 eV, respectively. On the inactive surface present at low T around 300-350 K formate dominates while methoxy is almost absent. Ignition of the reaction correlates with a decreasing formate coverage. A large hysteresis of ≈00 K occurs in T-cycling experiments whose correlation with adsorbate species was studied with varying oxygen and methanol partial pressures. The two branches of the hysteresis differ mainly in the amount of adsorbed oxygen, the methoxy species, and a carbonaceous species. Methoxy covers only a minor part of the catalytic surface reaching at most 20%. Above 650 K the surface is largely adsorbate-free.
ASJC Scopus subject areas
- Physics and Astronomy(all)
- General Physics and Astronomy
- Chemistry(all)
- Physical and Theoretical Chemistry
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In: Journal of Chemical Physics, Vol. 125, No. 11, 114709, 20.09.2006.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Adsorbate coverages and surface reactivity in methanol oxidation over Cu(110)
T2 - An in situ photoelectron spectroscopy study
AU - Günther, S.
AU - Zhou, L.
AU - Hävecker, M.
AU - Knop-Gericke, A.
AU - Kleimenov, E.
AU - Schlögl, R.
AU - Imbihl, R.
N1 - Funding Information: This work was supported by the DFG under the priority program 1091 “Bridging the gap between ideal and real systems in heterogeneous catalysis.”
PY - 2006/9/20
Y1 - 2006/9/20
N2 - The adsorbate species present during partial oxidation of methanol on a Cu(110) surface have been investigated in the 10-5 mbar range with in situ x-ray photoelectron spectroscopy and rate measurements. Two reaction intermediates were identified, methoxy with a C 1s binding energy (BE) of 285.4 eV and formate with a C is BE of 287.7 eV. The c(2×2) overlayer formed under reaction conditions is assigned to formate. Two states of adsorbed oxygen were found characterized by O 1s BE's of 529.6 and 528.9 eV, respectively. On the inactive surface present at low T around 300-350 K formate dominates while methoxy is almost absent. Ignition of the reaction correlates with a decreasing formate coverage. A large hysteresis of ≈00 K occurs in T-cycling experiments whose correlation with adsorbate species was studied with varying oxygen and methanol partial pressures. The two branches of the hysteresis differ mainly in the amount of adsorbed oxygen, the methoxy species, and a carbonaceous species. Methoxy covers only a minor part of the catalytic surface reaching at most 20%. Above 650 K the surface is largely adsorbate-free.
AB - The adsorbate species present during partial oxidation of methanol on a Cu(110) surface have been investigated in the 10-5 mbar range with in situ x-ray photoelectron spectroscopy and rate measurements. Two reaction intermediates were identified, methoxy with a C 1s binding energy (BE) of 285.4 eV and formate with a C is BE of 287.7 eV. The c(2×2) overlayer formed under reaction conditions is assigned to formate. Two states of adsorbed oxygen were found characterized by O 1s BE's of 529.6 and 528.9 eV, respectively. On the inactive surface present at low T around 300-350 K formate dominates while methoxy is almost absent. Ignition of the reaction correlates with a decreasing formate coverage. A large hysteresis of ≈00 K occurs in T-cycling experiments whose correlation with adsorbate species was studied with varying oxygen and methanol partial pressures. The two branches of the hysteresis differ mainly in the amount of adsorbed oxygen, the methoxy species, and a carbonaceous species. Methoxy covers only a minor part of the catalytic surface reaching at most 20%. Above 650 K the surface is largely adsorbate-free.
UR - http://www.scopus.com/inward/record.url?scp=33749051810&partnerID=8YFLogxK
U2 - 10.1063/1.2229198
DO - 10.1063/1.2229198
M3 - Article
AN - SCOPUS:33749051810
VL - 125
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 11
M1 - 114709
ER -