Concise Synthesis of (+)-[13 C4 ]-Anatoxin-a by Dynamic Kinetic Resolution of a Cyclic Iminium Ion

Angew Chem Int Ed Engl. 2020 Jul 6;59(28):11364-11368. doi: 10.1002/anie.202004464. Epub 2020 May 11.

Abstract

An asymmetric total synthesis of [13 C4 ]-anatoxin-a ([13 C4 ]-1) has been developed from commercially available ethyl [13 C4 ]-acetoacetate ([13 C4 ]-15). The unique requirements associated with isotope incorporation inspired a new, robust, and highly scalable route, providing access to 0.110 g of this internal standard for use in the detection and precise quantification of anatoxin-a in freshwater. A highlight of the synthesis is a method that leverages a cyclic iminium ion racemization to achieve dynamic kinetic resolution in an enantioselective Morita-Baylis-Hillman (MBH) cyclization.

Keywords: cyclization; isotopes; natural products; rearrangements; total synthesis.

Publication types

  • Research Support, N.I.H., Extramural

MeSH terms

  • Carbon Isotopes / chemistry
  • Cyanobacteria Toxins
  • Cyclization
  • Imines / chemistry*
  • Kinetics
  • Stereoisomerism
  • Tropanes / chemical synthesis*
  • Tropanes / chemistry

Substances

  • Carbon Isotopes
  • Cyanobacteria Toxins
  • Imines
  • Tropanes
  • anatoxin a