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Reaction model for methane oxidation on reduced SnO 2 (110) surface
Author(s) -
Yamaguchi Yoichi,
Nagasawa Yosuke,
Shimomura Satoshi,
Tabata Kenji
Publication year - 1999
Publication title -
international journal of quantum chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.484
H-Index - 105
eISSN - 1097-461X
pISSN - 0020-7608
DOI - 10.1002/(sici)1097-461x(1999)74:4<423::aid-qua6>3.0.co;2-r
Subject(s) - x ray photoelectron spectroscopy , chemistry , methanol , formaldehyde , methane , hydrogen atom abstraction , yield (engineering) , hydrogen , molecule , thermodynamics , chemical engineering , organic chemistry , physics , engineering
A reaction model for methane oxidation on a reduced SnO 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 2 surface are via the reactant complex CH 3 OH 2 O and via the secondary production of methanol oxidation, respectively. It is also found that CH 3 O − is a stable anion on the surface due to having the high barriers of about 70 kcal/mol in both hydrogen abstraction with O − and thermal decomposition, which is favorable to yield methanol and also is consistent with X‐ray photoelectron spectroscopy (XPS) experiments. ©1999 John Wiley & Sons, Inc. Int J Quant Chem 74: 423–433, 1999