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CH bond activation in CH sub 4 and t-BuO(ads) by oxygen chemisorbed on Ag(110). Molecular orbital theory

Journal Article · · Journal of the American Chemical Society; (United States)
DOI:https://doi.org/10.1021/ja00176a021· OSTI ID:5379754
;  [1]
  1. Case Western Reserve Univ., Cleveland, OH (USA)
Activation of the CH bond in CH{sub 4} and t-BuO(ads) by H{sup {sm bullet}} transfer to O adsorbed on the Ag(110) surface has been studied by the atom-superposition and electron-delocalization molecular orbital theory. Both abstractions are found to proceed with a low-energy barrier because of the presence of low-lying empty Ag surface orbitals at the Fermi level. Transfer of an electron to the Fermi level alleviates the initial closed-shell repulsion between the CH {sigma}-bond electron pair and the surface O (which is formally O{sup 2{minus}}) lone-pair orbital that ultimately forms the OH {sigma} bond. It is concluded that surface O behaves like a radical anion O{sup {sm bullet}{minus}} or R{sub 3}O{sup {sm bullet}} in its ability to form a single bond. These calculations also suggest the possibility that surface oxygen atoms might insert into CH bonds to form alcohols, which is a result of their ability to exhibit O atom or carbene (R{sub 2}C:) bonding properties.
OSTI ID:
5379754
Journal Information:
Journal of the American Chemical Society; (United States), Journal Name: Journal of the American Chemical Society; (United States) Vol. 112:20; ISSN 0002-7863; ISSN JACSA
Country of Publication:
United States
Language:
English