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Diversity-Oriented Synthesis of Spiropentadiene Pyrazolones and 1<i>H</i>-Oxepino[2,3-<i>c</i>]pyrazoles from Doubly Conjugated Pyrazolones via Intramolecular Wittig Reaction

Pankaj V. Khairnar, Chi-Yi Wu, Yi-Fang Lin, Athukuri Edukondalu, Yi‐Ru Chen, Wenwei Lin

2020Organic Letters30 citationsDOI

Abstract

An efficient method for the diversity-oriented synthesis of spiropentadiene pyrazolones and 1H-oxepino[2,3-c]pyrazoles is reported. The methodology attributes O-acylation of phosphorus zwitterions which were formed by a tandem phospha-1,6-addition of PBu3 to α,β,γ,δ-unsaturated pyrazolones, further generating betaine intermediates that preferentially resulted in the aforementioned cyclic products in a diversity-oriented manner. The mechanistic investigations revealed that formation of the betaines is the key step to provide the products via an intramolecular Wittig reaction or an unprecedented δ-C-acylation/cyclization/Wittig reaction.

Topics & Concepts

PyrazolonesChemistryWittig reactionIntramolecular forceAcylationBetaineStereochemistryCombinatorial chemistryOrganic chemistryCatalysisPhosphorus compounds and reactionsSynthesis and Reactivity of Sulfur-Containing CompoundsSynthesis and Reactivity of Heterocycles