| Literature DB >> 25044956 |
Sharmistha Karmakar1, Ayan Datta.
Abstract
At room temperature, 1,2-hydrogen-transfer reactions of N-heterocyclic carbenes, like the imidazol-2-ylidene to give imidazole is shown to occurr almost entirely (>90 %) by quantum mechanical tunneling (QMT). At 60 K in an Ar matrix, for the 2, 3-dihydrothiazol-2-ylidene→thiazole transformation, QMT is shown to increase the rate about 10(5) times. Calculations including small-curvature tunneling show that the barrier for intermolecular 1,2-hydrogen-transfer reaction is small, and QMT leads to a reduced rate of the forward reaction because of nonclassical reflections even at room temperature. A small barrier also leads to smaller kinetic isotope effects because of efficient QMT by both H and D. QMT does not always lead to faster reactions or larger KIE values, particularly when the barrier is small.Entities:
Keywords: N-heterocyclic carbenes; density functional calculations; dimerization; kinetics; quantum chemistry
Year: 2014 PMID: 25044956 DOI: 10.1002/anie.201404368
Source DB: PubMed Journal: Angew Chem Int Ed Engl ISSN: 1433-7851 Impact factor: 15.336