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Title: Reaction model for methane oxidation on reduced SnO{sub 2} (110) surface

Abstract

A reaction model for methane oxidation on a reduced SnO{sub 2} (110) crystal surface has been proposed theoretically using a point-charge model. The geometric and electronic structures for all the molecules along the four reaction channels have been calculated by means of the MP2/6-311 + G(2d, p) level of theory. On the basis of the optimized geometries in the gas phase, the single-point calculations of the energies on the point-charge model are carried out. The results indicate that the energetically favorable reaction paths to yield methanol and formaldehyde on the reduced SnO{sub 2} surface are via the reactant complex CH{sub 3}O-H{sub 2}O and via the secondary production of methanol oxidation, respectively. It is also found that CH{sub 3}O{sup {minus}} is a stable anion on the surface due to having the high barriers of about 70 kcal/mol in both hydrogen abstraction with O{sup {minus}} and thermal decomposition, which is favorable to yield methanol and also is consistent with X-ray photoelectron spectroscopy (XPS) experiments.

Authors:
; ; ;
Publication Date:
Research Org.:
Kansai Research Inst., Kyoto (JP)
OSTI Identifier:
20000405
Resource Type:
Journal Article
Journal Name:
International Journal of Quantum Chemistry
Additional Journal Information:
Journal Volume: 74; Journal Issue: 4; Other Information: PBD: 5 Sep 1999; Journal ID: ISSN 0020-7608
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; 10 SYNTHETIC FUELS; METHANE; OXIDATION; MATHEMATICAL MODELS; CHEMICAL REACTION KINETICS; TIN OXIDES; CATALYTIC EFFECTS; METHANOL; FORMALDEHYDE; SYNTHESIS

Citation Formats

Yamaguchi, Yoichi, Nagasawa, Yosuke, Shimomura, Satoshi, and Tabata, Kenji. Reaction model for methane oxidation on reduced SnO{sub 2} (110) surface. United States: N. p., 1999. Web. doi:10.1002/(SICI)1097-461X(1999)74:4<423::AID-QUA6>3.0.CO;2-R.
Yamaguchi, Yoichi, Nagasawa, Yosuke, Shimomura, Satoshi, & Tabata, Kenji. Reaction model for methane oxidation on reduced SnO{sub 2} (110) surface. United States. doi:10.1002/(SICI)1097-461X(1999)74:4<423::AID-QUA6>3.0.CO;2-R.
Yamaguchi, Yoichi, Nagasawa, Yosuke, Shimomura, Satoshi, and Tabata, Kenji. Sun . "Reaction model for methane oxidation on reduced SnO{sub 2} (110) surface". United States. doi:10.1002/(SICI)1097-461X(1999)74:4<423::AID-QUA6>3.0.CO;2-R.
@article{osti_20000405,
title = {Reaction model for methane oxidation on reduced SnO{sub 2} (110) surface},
author = {Yamaguchi, Yoichi and Nagasawa, Yosuke and Shimomura, Satoshi and Tabata, Kenji},
abstractNote = {A reaction model for methane oxidation on a reduced SnO{sub 2} (110) crystal surface has been proposed theoretically using a point-charge model. The geometric and electronic structures for all the molecules along the four reaction channels have been calculated by means of the MP2/6-311 + G(2d, p) level of theory. On the basis of the optimized geometries in the gas phase, the single-point calculations of the energies on the point-charge model are carried out. The results indicate that the energetically favorable reaction paths to yield methanol and formaldehyde on the reduced SnO{sub 2} surface are via the reactant complex CH{sub 3}O-H{sub 2}O and via the secondary production of methanol oxidation, respectively. It is also found that CH{sub 3}O{sup {minus}} is a stable anion on the surface due to having the high barriers of about 70 kcal/mol in both hydrogen abstraction with O{sup {minus}} and thermal decomposition, which is favorable to yield methanol and also is consistent with X-ray photoelectron spectroscopy (XPS) experiments.},
doi = {10.1002/(SICI)1097-461X(1999)74:4<423::AID-QUA6>3.0.CO;2-R},
journal = {International Journal of Quantum Chemistry},
issn = {0020-7608},
number = 4,
volume = 74,
place = {United States},
year = {1999},
month = {9}
}