Literature DB >> 25044956

Tunneling assists the 1,2-hydrogen shift in N-heterocyclic carbenes.

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.
© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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


  2 in total

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Journal:  RSC Adv       Date:  2018-01-16       Impact factor: 3.361

2.  Beyond static structures: Putting forth REMD as a tool to solve problems in computational organic chemistry.

Authors:  Riccardo Petraglia; Adrien Nicolaï; Matthew D Wodrich; Michele Ceriotti; Clemence Corminboeuf
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  2 in total

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