Novel 3H-1,2,3-Dithiaphosphole and Unprecedented 1,3,2,4-Dithiadiphosphinane Heterocycles: Unanticipated Cyclization Reactions of Lawesson's Reagent and Alkynes

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OriginalspracheEnglisch
Aufsatznummere202500219
FachzeitschriftEuropean Journal of Organic Chemistry
Jahrgang28
Ausgabenummer29
Frühes Online-Datum29 Apr. 2025
PublikationsstatusVeröffentlicht - 20 Aug. 2025

Abstract

The treatment of Lawesson's reagent with selected alkyl or aryl alkynes results in the formation of cyclization products such as 3H-1,2,3-dithiaphosphole-3-sulfide or unprecedented 1,3,2,4-dithiadiphosphinane-2,4-disulfide derivatives. The new heterocycles are characterized spectroscopically and in two cases by crystal structure analyses. Density functional theory (DFT) computations (PW6B95D3/6-311 + G(d,p)-PCM(toluene)//B97D3/6-31 G*) explain the formation of the dithiaphosphole product from alkynes and Lawesson's reagent via a sequence of [2 + 2] addition, electrocyclic ring opening, S-S bond forming ring closure, and P(III) oxidation by sulfur transfer from Lawesson's reagent. Based on DFT calculations, the formation of a 1,3,2,4-dithiadiphosphinane-2,4-disulfide is rationalized by a sequence of cyclization, electrocyclic ring opening, and dipolar cyclization steps.

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Novel 3H-1,2,3-Dithiaphosphole and Unprecedented 1,3,2,4-Dithiadiphosphinane Heterocycles: Unanticipated Cyclization Reactions of Lawesson's Reagent and Alkynes. / Blüm, Felix; Goldfuss, Bernd; Butenschön, Holger.
in: European Journal of Organic Chemistry, Jahrgang 28, Nr. 29, e202500219, 20.08.2025.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

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abstract = "The treatment of Lawesson's reagent with selected alkyl or aryl alkynes results in the formation of cyclization products such as 3H-1,2,3-dithiaphosphole-3-sulfide or unprecedented 1,3,2,4-dithiadiphosphinane-2,4-disulfide derivatives. The new heterocycles are characterized spectroscopically and in two cases by crystal structure analyses. Density functional theory (DFT) computations (PW6B95D3/6-311 + G(d,p)-PCM(toluene)//B97D3/6-31 G*) explain the formation of the dithiaphosphole product from alkynes and Lawesson's reagent via a sequence of [2 + 2] addition, electrocyclic ring opening, S-S bond forming ring closure, and P(III) oxidation by sulfur transfer from Lawesson's reagent. Based on DFT calculations, the formation of a 1,3,2,4-dithiadiphosphinane-2,4-disulfide is rationalized by a sequence of cyclization, electrocyclic ring opening, and dipolar cyclization steps.",
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author = "Felix Bl{\"u}m and Bernd Goldfuss and Holger Butensch{\"o}n",
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T1 - Novel 3H-1,2,3-Dithiaphosphole and Unprecedented 1,3,2,4-Dithiadiphosphinane Heterocycles

T2 - Unanticipated Cyclization Reactions of Lawesson's Reagent and Alkynes

AU - Blüm, Felix

AU - Goldfuss, Bernd

AU - Butenschön, Holger

N1 - Publisher Copyright: © 2025 The Author(s). European Journal of Organic Chemistry published by Wiley-VCH GmbH.

PY - 2025/8/20

Y1 - 2025/8/20

N2 - The treatment of Lawesson's reagent with selected alkyl or aryl alkynes results in the formation of cyclization products such as 3H-1,2,3-dithiaphosphole-3-sulfide or unprecedented 1,3,2,4-dithiadiphosphinane-2,4-disulfide derivatives. The new heterocycles are characterized spectroscopically and in two cases by crystal structure analyses. Density functional theory (DFT) computations (PW6B95D3/6-311 + G(d,p)-PCM(toluene)//B97D3/6-31 G*) explain the formation of the dithiaphosphole product from alkynes and Lawesson's reagent via a sequence of [2 + 2] addition, electrocyclic ring opening, S-S bond forming ring closure, and P(III) oxidation by sulfur transfer from Lawesson's reagent. Based on DFT calculations, the formation of a 1,3,2,4-dithiadiphosphinane-2,4-disulfide is rationalized by a sequence of cyclization, electrocyclic ring opening, and dipolar cyclization steps.

AB - The treatment of Lawesson's reagent with selected alkyl or aryl alkynes results in the formation of cyclization products such as 3H-1,2,3-dithiaphosphole-3-sulfide or unprecedented 1,3,2,4-dithiadiphosphinane-2,4-disulfide derivatives. The new heterocycles are characterized spectroscopically and in two cases by crystal structure analyses. Density functional theory (DFT) computations (PW6B95D3/6-311 + G(d,p)-PCM(toluene)//B97D3/6-31 G*) explain the formation of the dithiaphosphole product from alkynes and Lawesson's reagent via a sequence of [2 + 2] addition, electrocyclic ring opening, S-S bond forming ring closure, and P(III) oxidation by sulfur transfer from Lawesson's reagent. Based on DFT calculations, the formation of a 1,3,2,4-dithiadiphosphinane-2,4-disulfide is rationalized by a sequence of cyclization, electrocyclic ring opening, and dipolar cyclization steps.

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