Probing the intermediates in the MO + CH4 ↔ M + CH3OH reactions by matrix isolation infrared spectroscopy

In this review, we present our recent studies on the MO + CH 4 and M + CH 3 OH model reactions (M = transition metals) in order to provide quantitative information regarding the mechanisms for the catalytic methane-to-methanol conversion process. The reaction intermediates were trapped and probed by...

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Bibliographic Details
Published in:International reviews in physical chemistry 2008-01, Vol.27 (1), p.1-25
Main Authors: Wang, Guanjun, Zhou, Mingfei
Format: Article
Language:English
Subjects:
matrix isolation
methane-to-methanol conversion
reaction intermediate
reaction mechanism
transition metal
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Summary:In this review, we present our recent studies on the MO + CH 4 and M + CH 3 OH model reactions (M = transition metals) in order to provide quantitative information regarding the mechanisms for the catalytic methane-to-methanol conversion process. The reaction intermediates were trapped and probed by matrix isolation infrared absorption spectroscopy. Various important intermediates including OM(CH 4 ), M(CH 3 OH), CH 3 MOH, CH 3 M(O)H and CH 3 OMH are identified via isotopic substitution experiments in the MO + CH 4 and M + CH 3 OH reactions for selected early and late transition metals. Based on the observed reaction intermediates, some unprecedented reaction pathways are proposed. Complementary quantum chemical calculations support the intermediate identification and help to gain insight into the reaction mechanisms and periodic trends.
ISSN:0144-235X
1366-591X
DOI:10.1080/01442350701685946