Highly Stereoselective Diels-Alder Reactions Catalyzed by Diboronate Complexes

Angew Chem Int Ed Engl. 2023 Aug 14;62(33):e202303075. doi: 10.1002/anie.202303075. Epub 2023 Jul 6.

Abstract

A highly enantioselective catalytic system for exo-Diels-Alder reactions was developed based on the newly discovered bispyrrolidine diboronates (BPDB). Activated by various Lewis or Brønsted acids, BPDB can catalyze highly stereoselective asymmetric exo-Diels-Alder reactions of monocarbonyl-based dienophiles. When 1,2-dicarbonyl-based dienophiles are used, the catalyst can sterically distinguish between the two binding sites, which leads to highly regioselective asymmetric Diels-Alder reactions. BPDB can be prepared as crystalline solids on a large scale and are stable under ambient condition. Single-crystal X-ray analysis of the structure for acid-activated BPDB indicated that its activation involves cleavage of a labile B←N bond.

Keywords: Asymmetric Catalysis; Bispyrrolidine Diboronates; Diels-Alder Reaction; Exo-Selectivity; Pericyclic Reaction.