Pd-Catalyzed Asymmetric N-Allylation of Amino Acid Esters with Exceptional Levels of Catalyst Control: Stereo-Divergent Synthesis of ProM-15 and Related Bicyclic Dipeptide Mimetics

Chemistry. 2020 Mar 9;26(14):3049-3053. doi: 10.1002/chem.202000307. Epub 2020 Feb 18.

Abstract

A general and powerful method for the stereo-controlled Pd-catalyzed N-allylation of amino acid esters is reported, as a previously largely unsolved synthetic challenge. Employing a new class of tartaric acid-derived C2 -symmetric chiral diphosphane ligands the developed asymmetric amination protocol allows the conversion of various amino acid esters to the N-allylated products with highest levels of enantio- or diastereoselectivity in a fully catalyst-controlled fashion and predictable configuration. Remarkably, the in situ generated catalysts also exhibit outstanding levels of activity (ligand acceleration). The usefulness of the method was demonstrated in the stereo-divergent synthesis of a set of new conformationally defined dipeptide mimetics, which represent new modular building blocks for the development of peptide-inspired bioactive compounds.

Keywords: asymmetric catalysis; chiral diphosphine ligands; peptide mimetics; protein interactions; transition-metal catalysis.

MeSH terms

  • Alanine / chemistry
  • Amino Acids / chemistry*
  • Catalysis
  • Crystallography, X-Ray
  • Cycloaddition Reaction
  • Dipeptides / chemical synthesis*
  • Esters / chemistry*
  • Ligands
  • Models, Molecular
  • Molecular Structure
  • Oxidation-Reduction
  • Palladium / chemistry*
  • Proline / chemistry
  • Stereoisomerism

Substances

  • Amino Acids
  • Dipeptides
  • Esters
  • Ligands
  • Palladium
  • Proline
  • Alanine