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Title: Adsorption and Reaction of Methanol on Thin-film Cerium Oxide

Authors:
 [1];  [1];  [1]
  1. ORNL
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1003216
DOE Contract Number:
DE-AC05-00OR22725
Resource Type:
Journal Article
Resource Relation:
Journal Name: Surface Science; Journal Volume: 600; Journal Issue: 7
Country of Publication:
United States
Language:
English

Citation Formats

Mullins, David R, Robbins, Matthew D, and Zhou, Jing. Adsorption and Reaction of Methanol on Thin-film Cerium Oxide. United States: N. p., 2006. Web. doi:10.1016/j.susc.2006.02.011.
Mullins, David R, Robbins, Matthew D, & Zhou, Jing. Adsorption and Reaction of Methanol on Thin-film Cerium Oxide. United States. doi:10.1016/j.susc.2006.02.011.
Mullins, David R, Robbins, Matthew D, and Zhou, Jing. Sun . "Adsorption and Reaction of Methanol on Thin-film Cerium Oxide". United States. doi:10.1016/j.susc.2006.02.011.
@article{osti_1003216,
title = {Adsorption and Reaction of Methanol on Thin-film Cerium Oxide},
author = {Mullins, David R and Robbins, Matthew D and Zhou, Jing},
abstractNote = {},
doi = {10.1016/j.susc.2006.02.011},
journal = {Surface Science},
number = 7,
volume = 600,
place = {United States},
year = {Sun Jan 01 00:00:00 EST 2006},
month = {Sun Jan 01 00:00:00 EST 2006}
}
  • Formaldehyde adsorption and reaction have been studied on cerium oxide thin films that were vapor deposited on Ru(0 0 0 1). The formaldehyde behavior was examined as a function of temperature, exposure and Ce oxidation state. Formaldehyde chemisorbs on fully oxidized CeO{sub 2} as dioxymethylene, CH{sub 2}O{sub 2}. The dioxymethylene decomposes and desorbs as formaldehyde between 200 K and 400 K. No other products are formed. On reduced ceria, formaldehyde also adsorbs as dioxymethylene. In addition to the formaldehyde desorption between 200 K and 400 K, a more strongly bound form of dioxymethylene is formed that produces formaldehyde at 440more » K. Above 400 K, some of the dioxymethylene reacts to form formate and methoxy on the surface. These species decompose to produce H{sub 2}, CO and CH{sub 2}O above 500 K.« less
  • Formaldehyde adsorption and reaction have been studied on cerium oxide thin films that were vapor deposited on Ru(0 0 0 1). The formaldehyde behavior was examined as a function of temperature, exposure and Ce oxidation state. Formaldehyde chemisorbs on fully oxidized CeO{sub 2} as dioxymethylene, CH{sub 2}O{sub 2}. The dioxymethylene decomposes and desorbs as formaldehyde between 200 K and 400 K. No other products are formed. On reduced ceria, formaldehyde also adsorbs as dioxymethylene. In addition to the formaldehyde desorption between 200 K and 400 K, a more strongly bound form of dioxymethylene is formed that produces formaldehyde at 440more » K. Above 400 K, some of the dioxymethylene reacts to form formate and methoxy on the surface. These species decompose to produce H{sub 2}, CO and CH{sub 2}O above 500 K.« less
  • The adsorption and reaction of hydrogen sulfide, H{sub 2}S, have been studied on cerium oxide thin films that were vapor deposited on Ru(0 0 0 1). The behavior of the H{sub 2}S was examined as a function of Ce oxidation state. H{sub 2}S weakly chemisorbs on fully oxidized CeO{sub 2} desorbing near 155 K. Hydrogen from the H{sub 2}S reacts with the surface O to desorb as water between 200 K and 450 K. When ca. 20% of the Ce{sup 4+} is reduced to Ce{sup 3+} more H{sub 2}S dissociates to -OH and -SH and water is produced near 580more » K. When the ceria is ca. 70% reduced, water formation is suppressed and H{sub 2} desorbs near 580 K. S 2p photoelectron spectroscopy indicates the decomposition of H{sub 2}S into -SH and then -S as the sample is annealed from 100 K to 600 K. O 1s photoemission indicated the presence of H{sub 2}O and -OH.« less
  • The adsorption and reaction of methanethiol, CH{sub 3}SH, have been studied on cerium oxide thin films that were vapor deposited on Ru(0 0 0 1). The behavior of the CH{sub 3}SH was examined as a function of the Ce oxidation state. CH{sub 3}SH weakly interacts with fully oxidized CeO{sub 2}(1 1 1) forming both chemisorbed CH{sub 3}SH and CH{sub 3}S + OH. OH forms through the reaction of the sulfhydrol H with the surface O. These species recombine and desorb near 180 K leaving the surface virtually clean. When the ceria is ca. 50% reduced, the chemisorbed CH{sub 3}SH desorbsmore » near 150 K while the CH{sub 3}S + OH are stable to 400 K. These species react above 450 K to produce predominantly CH{sub 4} and CH{sub 3}SH. A small amount of CH{sub 2}O and water are also formed through reaction with the O in the ceria. Atomic S is left on the surface. S 2p, C 1s and O 1s soft X-ray photoelectron spectroscopy were used to identify the nature of the chemisorbed species and the adsorption site of the CH{sub 3}S or S.« less