Methane activation and exchange by titanium-carbon multiple bonds

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We demonstrate that a titanium-carbon multiple bond, specifically an alkylidyne ligand in the transient complex, (PNP) Ti equivalent to(CBu)-Bu-t (A) (PNP- = N[2-P(CHMe2)(2)-4-methylphenyl](2)), can cleanly activate methane at room temperature with moderately elevated pressures to form (PNP)Ti=(CHBu)-Bu-t(CH3). Isotopic labeling and theoretical studies suggest that the alkylidene and methyl hydrogens exchange, either via tautomerization invoking a methylidene complex, (PNP)Ti=CH2((CH2Bu)-Bu-t), or by forming the methane adduct (PNP)Ti equivalent to(CBu)-Bu-t(CH4). The thermal, fluxional and chemical behavior of (PNP)Ti=(CHBu)-Bu-t(CH3) is also presented in this study.
Publisher
ROYAL SOC CHEMISTRY
Issue Date
2011
Language
English
Article Type
Article
Keywords

C-H ACTIVATION; TUNGSTEN ALKYLIDENE COMPLEXES; ALKANE METATHESIS; COMPUTATIONAL PERSPECTIVE; HYDROCARBON ACTIVATION; AMBIENT-TEMPERATURES; AGOSTIC INTERACTIONS; THERMAL-ACTIVATION; BENZENE ACTIVATION; OLEFIN METATHESIS

Citation

CHEMICAL SCIENCE, v.2, no.8, pp.1457 - 1462

ISSN
2041-6520
DOI
10.1039/c1sc00138h
URI
http://hdl.handle.net/10203/203312
Appears in Collection
CH-Journal Papers(저널논문)
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