Linked Life Data

20923156

Source:http://linkedlifedata.com/resource/pubmed/id/20923156

Statements in which the resource exists as a subject.
PredicateObject
rdf:type
lifeskim:mentions
pubmed:issue
42
pubmed:dateCreated
2010-10-21
pubmed:abstractText
The reactive oxidizing species in the selective oxidation of methane to methanol in oxygen activated Cu-ZSM-5 was recently defined to be a bent mono(?-oxo)dicopper(II) species, [Cu(2)O](2+). In this communication we report the formation of an O(2)-precursor of this reactive site with an associated absorption band at 29,000 cm(-1). Laser excitation into this absorption feature yields a resonance Raman (rR) spectrum characterized by (18)O(2) isotope sensitive and insensitive vibrations, ?O-O and ?Cu-Cu, at 736 (?(18)O(2) = 41 cm(-1)) and 269 cm(-1), respectively. These define the precursor to be a ?-(?(2):?(2)) peroxo dicopper(II) species, [Cu(2)(O(2))](2+). rR experiments in combination with UV-vis absorption data show that this [Cu(2)(O(2))](2+) species transforms directly into the [Cu(2)O](2+) reactive site. Spectator Cu(+) sites in the zeolite ion-exchange sites provide the two electrons required to break the peroxo bond in the precursor. O(2)-TPD experiments with (18)O(2) show the incorporation of the second (18)O atom into the zeolite lattice in the transformation of [Cu(2)(O(2))](2+) into [Cu(2)O](2+). This study defines the mechanism of oxo-active site formation in Cu-ZSM-5.
pubmed:grant
pubmed:language
eng
pubmed:journal
pubmed:citationSubset
IM
pubmed:chemical
pubmed:status
MEDLINE
pubmed:month
Oct
pubmed:issn
1520-5126
pubmed:author
pubmed:issnType
Electronic
pubmed:day
27
pubmed:volume
132
pubmed:owner
NLM
pubmed:authorsComplete
Y
pubmed:pagination
14736-8
pubmed:dateRevised
2011-10-27
pubmed:meshHeading
pubmed:year
2010
pubmed:articleTitle
Oxygen precursor to the reactive intermediate in methanol synthesis by Cu-ZSM-5.
pubmed:affiliation
Department of Chemistry, Stanford University, Stanford, California 94305, USA.
pubmed:publicationType
Journal Article, Research Support, Non-U.S. Gov't, Research Support, N.I.H., Extramural