Synthesis of beta-lactams by Ag+-induced ring expansion of 1-hydroxycyclopropylamines: a theoretical analysis

J Phys Chem A. 2005 Sep 1;109(34):7822-31. doi: 10.1021/jp052291+.

Abstract

A theoretical analysis of the silver-induced ring expansion of N-chloro-N-methyl-1-hydroxycyclopropylamine to form N-methyl-2-azetidinone, and of the Cl(-) elimination from this substrate without Ag(+) assistance, was performed using the B3LYP method and the 6-31+G(d) basis set for C, N, O, H, and Cl atoms and the relativistic effective core pseudopotential LANL2DZ complemented with one set of f polarization functions (zeta(f) = 0.473) for the Ag atom. The partial Ag(+)-assisted extrusion of Cl(-) at the rate-determining transition state provokes an important change in the nodal properties of the frontier molecular orbitals of the H(3)CClNCOHAg(+) fragment, thus making very stabilizing HOMO-LUMO interactions between this fragment and the C(2)H(4) moiety possible. This interaction leads to the ring opening and release of most of the strain energy, giving rise to a low energy barrier for the process. Also, by assisting the Cl(-) extrusion, Ag(+) avoids the elimination of the hydroxyl hydrogen atom, which would provoke the fragmentation of the system instead of the formation of the beta-lactam.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Cyclopropanes / chemistry*
  • Silver / chemistry*
  • beta-Lactams / chemical synthesis*

Substances

  • Cyclopropanes
  • beta-Lactams
  • Silver
  • cyclopropylamine