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Speciation and decomposition pathways of ruthenium catalysts used for selective C–H hydroxylation

Authors
Type
Published Article
Journal
Advances in Chemical Engineering and Science
Publisher
"Scientific Research Publishing, Inc."
Publication Date
Jan 14, 2014
Volume
5
Issue
8
Pages
3309–3314
Identifiers
DOI: 10.1039/C4SC01050G
Source
CCHF
License
White

Abstract

Mechanistic insight into a C–H hydroxylation reaction catalysed by [(Me3tacn)RuCl3] has been obtained using desorption electrospray ionization mass spectrometry (DESI-MS) to identify reactive intermediates and to determine the fate of the starting metal complex. Our studies provide direct evidence for the formation of a high-valent dioxo-Ru(VI) species, which is believed to be the active oxidant. Other unexpected Ru-oxo intermediates, however, have been identified and may also function as competent hydroxylating agents. Mass spectral data that substantiate putative mechanisms for catalyst arrest and highlight reactivity differences between [(Me3tacn)RuCl3] and the corresponding tribromide adduct are also described.

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