Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 105, Issue 47, Pages 18114-18119Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0801849105
Keywords
bond activation; kinetic isotope effects; mass spectrometry
Categories
Funding
- Cluster of Excellence
- Czech Academy of Sciences [Z40550506]
- Deutsche Forschungsgemeinschaft [SFB 658]
- Agency of the Academy of Sciences of the Czech Republic [KJB400550704, 203/08/1487]
- Fonds der Chemischen Industrie
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Motivated by the search for ways of a more efficient usage of the large, unexploited resources of methane, recent progress in the gas-phase activation of methane by ligated transition-metal ions is discussed. Mass spectrometric experiments demonstrate that the ligands can crucially influence both reactivity and selectivity of transition-metal cations in bond-activation processes, and the most reactive species derive from combinations of transition metals with the electronegative elements fluorine, oxygen, and chlorine. Furthermore, the collected knowledge about intramolecular kinetic isotope effects associated with the activation of C-H(D) bonds of methane can be used to distinguish the nature of the bond activation as a mere hydrogen-abstraction, a metal-assisted mechanism or more complex reactions such as formation of insertion intermediates or sigma-bond metathesis.
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