Enolonium Species-Umpoled Enolates

Angew Chem Int Ed Engl. 2017 Mar 1;56(10):2599-2603. doi: 10.1002/anie.201610274. Epub 2017 Jan 27.

Abstract

Enolonium species/iodo(III)enolates of carbonyl compounds have been suggested to be intermediates in a wide variety of hypervalent iodine induced chemical transformations of ketones, including α-C-O, α-C-N, α-C-C, and α-carbon-halide bond formation, but they have never been characterized. We report that these elusive umpoled enolates may be made as discrete species that are stable for several minutes at -78 °C, and report the first spectroscopic identification of such species. It is shown that enolonium species are direct intermediates in C-O, C-N, C-Cl, and C-C bond forming reactions. Our results open up chemical space for designing a variety of new transformations. We showcase the ability of enolonium species to react with prenyl, crotyl, cinnamyl, and allyl silanes with absolute regioselectivity in up to 92 % yield.

Keywords: allylation; enolonium species; ketones; polarity inversion; umpolung.

Publication types

  • Research Support, Non-U.S. Gov't