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Chemical Science Vol - 3 Issue - 9

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Mechanistic insight into catalytic oxidations of organic compounds by ruthenium(iv)-oxo complexes with pyridylamine ligands

Content Provider	Royal Society of Chemistry (RSC)
Author	Hirai, Yuichirou Ogura, Takashi Ohzu, Shingo Ishizuka, Tomoya Sakaguchi, Miyuki Fukuzumi, Shunichi Kojima, Takahiko Jiang, Hua
Copyright Year	2012
Abstract	A series of Ru(IV)-oxo complexes (4–6) were synthesized from the corresponding Ru(II)-aqua complexes (1–3) and fully characterized by 1H NMR and resonance Raman spectroscopies, and ESI-MS spectrometry. Based on the diamagnetic character confirmed by the 1H NMR spectroscopy in D2O, the spin states of 5 and 6 were determined to be S = 0 in the d4 configuration, in sharp contrast to that of 4 being in the S = 1 spin state. The aqua-complexes 1–3 catalyzed oxidation of alcohols and olefins using (NH4)2[CeIV(NO3)6] (CAN) as an electron-transfer oxidant in acidic aqueous solutions. Comparison of the reactivity of electrochemically generated oxo-complexes (4–6) was made in the light of kinetic analyses for oxidation of 1-propanol and a water-soluble ethylbenzene derivative. The oxo complexes (4–6) exhibited no significant difference in the reactivity for the oxidation reactions, judging from the similar catalytic rates and the activation parameters. The slight difference observed in the reaction rates can be accounted for by the difference in the reduction potentials of the oxo-complexes, but the spin states of the oxo-complexes have hardly affected the reactivity. The activation parameters and the kinetic isotope effects (KIE) observed for the oxidation reactions of methanol indicate that the oxidation reactions of alcohols with the RuIVO complexes proceed via a concerted proton-coupled electron transfer mechanism.
Starting Page	3421
Ending Page	3431
Page Count	11
File Format	HTM / HTML PDF
ISSN	20416520
Volume Number	3
Issue Number	12
Journal	Chemical Science
DOI	10.1039/c2sc21195e
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Ethylbenzene Isotope 1-Propanol Nuclear magnetic resonance spectroscopy Proton-coupled electron transfer Resonance Raman spectroscopy Diamagnetism Methanol
Content Type	Text
Resource Type	Article
Subject	Chemistry

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