(3+2)-Cycloadditions of Levoglucosenone (LGO) with Fluorinated Nitrile Imines Derived from Trifluoroacetonitrile: An Experimental and Computational Study DOI Creative Commons
Grzegorz Mlostoń, Katarzyna Urbaniak, Marcin Palusiak

et al.

Molecules, Journal Year: 2023, Volume and Issue: 28(21), P. 7348 - 7348

Published: Oct. 30, 2023

The in situ-generated N-aryl nitrile imines derived from trifluoroacetonitrile smoothly undergo (3+2)-cycloadditions onto the enone fragment of levoglucosenone molecule, yielding corresponding, five-membered cycloadducts. In contrast to ‘classic’ C(Ph),N(Ph) imine, reactions with fluorinated C(CF3),N(Ar) analogues lead stable pyrazolines a chemo- and stereoselective manner. Based on result X-ray single crystal diffraction analysis, their structures were established as exo-cycloadducts location N-Ar terminus 1,3-dipole at α-position moiety. DFT computation demonstrated that observed reaction pathway results strong dominance kinetic control over thermodynamic control.

Language: Английский

Diastereoselective (8+3)‐Cycloadditions of Donor‐Acceptor Cyclopropanes with Tropothione DOI
Grzegorz Mlostoń, Mateusz Kowalczyk, Marcin Palusiak

et al.

European Journal of Organic Chemistry, Journal Year: 2023, Volume and Issue: 27(6)

Published: Dec. 27, 2023

Abstract Reactions of dimethyl 2‐arylcyclopropane‐1,1‐dicarboxylates, used as representatives D‐A cyclopropanes, with tropothione were carried out in the presence scandium triflate a catalyst, under mild conditions (CH 2 Cl solution, rt). The anticipated (8+3)‐cycloaddition products, cycloheptatriene fused thiopyrans, obtained good to excellent yields. Cycloadditions occurred complete diastereoselectivity and all cases single diastereomers formed. Structures isolated cycloadducts established based on spectroscopic data two they unambiguously confirmed by crystal X‐ray diffraction analysis. In contrast an analogous reported for parent tropone, which was performed Ni(ClO 4 ) , no 1,3‐ H shift leading products possessing CH moiety located within seven‐membered ring observed.

Language: Английский

Citations

9

Expedient sulfurization with elemental sulfur and an unexpected conversion of 2,3-diarylcyclopropenethiones using tetrabutylammonium fluoride (TBAF) as a source of the fluoride anion DOI
Grzegorz Mlostoń, Jakub Wręczycki,

Amelia Robak

et al.

Journal of Fluorine Chemistry, Journal Year: 2023, Volume and Issue: 270, P. 110170 - 110170

Published: July 31, 2023

Language: Английский

Citations

4

(3+2)-Cycloadditions of Levoglucosenone (LGO) with Fluorinated Nitrile Imines Derived from Trifluoroacetonitrile: An Experimental and Computational Study DOI Creative Commons
Grzegorz Mlostoń, Katarzyna Urbaniak, Marcin Palusiak

et al.

Molecules, Journal Year: 2023, Volume and Issue: 28(21), P. 7348 - 7348

Published: Oct. 30, 2023

The in situ-generated N-aryl nitrile imines derived from trifluoroacetonitrile smoothly undergo (3+2)-cycloadditions onto the enone fragment of levoglucosenone molecule, yielding corresponding, five-membered cycloadducts. In contrast to ‘classic’ C(Ph),N(Ph) imine, reactions with fluorinated C(CF3),N(Ar) analogues lead stable pyrazolines a chemo- and stereoselective manner. Based on result X-ray single crystal diffraction analysis, their structures were established as exo-cycloadducts location N-Ar terminus 1,3-dipole at α-position moiety. DFT computation demonstrated that observed reaction pathway results strong dominance kinetic control over thermodynamic control.

Language: Английский

Citations

1