Palladium-Catalyzed [3 + 2]-C-C/N-C Bond-Forming Annulation

Org Lett. 2018 Jul 6;20(13):4057-4061. doi: 10.1021/acs.orglett.8b01616. Epub 2018 Jun 13.

Abstract

The synthesis of bi- and tricyclic structures incorporating pyrrolidone rings is disclosed, starting from resonance-stabilized acetamides and cyclic α,β-unsaturated-γ-oxycarbonyl derivatives. This process involves an intermolecular Tsuji-Trost allylation/intramolecular nitrogen 1,4-addition sequence. Crucial for the success of this bis-nucleophile/bis-electrophile [3 + 2] annulation is its well-defined step chronology in combination with the total chemoselectivity of the former step. When the newly formed annulation product carries a properly located o-haloaryl moiety at the nitrogen substituent, a further intramolecular keto α-arylation can join the cascade, thereby forming two new cycles and three new bonds in the same synthetic operation.

Publication types

  • Research Support, Non-U.S. Gov't