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Computationally Unravelling the Mechanism and Selectivity of Five and Six membered N-Heterocyclic Carbene- Catalyzed Alkyne Hydrochalcogenation
  • Jayasree Elambalassery,
  • Sobhana Reshma,
  • Mohanan Aswathy
Jayasree Elambalassery
University of Kerala

Corresponding Author:[email protected]

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Sobhana Reshma
University of Kerala
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Mohanan Aswathy
University of Kerala
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Abstract

The present work is intended to bring to the forefront a relatively less explored area of N-Heterocyclic Carbene (NHC) catalyzed alkyne hydro- thiolation and selenation reactions. The present work can be regarded as the first ever computational investigation on the catalytic activity of the NHC catalyzed hydro- thiolation and selenation reactions by exploring the reaction mechanism. Reaction mechanism involves chalcogenol activation followed by alkyne insertion and the second step is found to be the rate determining step. A comparison with the reported uncatalyzed gas phase reaction showed that a simple imidazol-2-ylidene catalyst can lower the free energy barrier by 19.62 and 14.63 kcal/mol respectively for acetylene hydro- thiolation and selenation reaction. All the employed NHCs are proved to be better catalyst for both hydrothiolation and hydroselenation. Effects of factors such as changing the heterocycle, increasing the conjugation, ring expansion and electronic/steric substitution were also investigated. Effect of solvent polarity on the reaction energetics and selectivity has also been analyzed employing THF, DMSO and MeOH as the solvents.
02 Dec 2020Submitted to International Journal of Quantum Chemistry
03 Dec 2020Submission Checks Completed
03 Dec 2020Assigned to Editor
08 Dec 2020Reviewer(s) Assigned
29 Dec 2020Review(s) Completed, Editorial Evaluation Pending
04 Jan 2021Editorial Decision: Revise Major
13 Feb 20211st Revision Received
16 Feb 2021Submission Checks Completed
16 Feb 2021Assigned to Editor
16 Feb 2021Reviewer(s) Assigned
23 Feb 2021Review(s) Completed, Editorial Evaluation Pending
23 Feb 2021Editorial Decision: Accept