期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 132, 期 40, 页码 14239-14250出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja1061505
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资金
- ANR [BLAN07-2_182861]
- CNRS [LEA 368]
- Royal Society
- ICIQ Foundation
- Spanish MICINN [CTQ2008-06866-CO2-02/BQU, CSD2006-0003]
- Engineering and Physical Sciences Research Council [EP/C534425/1, EP/C534425/2] Funding Source: researchfish
We report the synthesis of a niobium cyclopropyl complex, Tp(Me2)NbMe(c-C3H5)(MeCCMe), and show that thermal loss of methane from this compound generates an intermediate that is capable of activating both aliphatic and aromatic C-H bonds. Isotopic labeling, trapping studies, a detailed kinetic analysis, and density functional theory all suggest that the active intermediate is an eta(2)-cyclopropene complex formed via beta-hydrogen abstraction rather than an isomeric cyclopropylidene species. C-H activation chemistry of this type represents a rather unusual reactivity pattern for eta(2)-alkene complexes but is favored in this case by the strain in the C-3 ring which prevents the decomposition of the key intermediate via loss of cyclopropene.
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