期刊
CHEMICAL SCIENCE
卷 2, 期 8, 页码 1457-1462出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c1sc00138h
关键词
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资金
- National Science Foundation [CHE-0848248, CHE-0645381]
- Alexander von Humboldt Stiftung
- Research Corporation
- CONACYT
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.
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