Kinetics and mechanism of hydrolysis of N-acyloxymethyl derivatives of azetidin-2-one

J Org Chem. 2004 May 14;69(10):3359-67. doi: 10.1021/jo0358123.

Abstract

The pH-independent, acid-catalyzed and base-catalyzed hydrolyses of N-acyloxymethylazetidin-2-ones all occur at the ester function. The pH-independent hydrolysis involves rate-limiting alkyl C-O fission and formation of an exocyclic beta-lactam iminum ion. This iminium ion is then trapped by water at the exocyclic iminium carbon atom, rather than at the beta-lactam carbonyl carbon atom, to form the corresponding N-hydroxymethylazetidin-2-ones. Calculations carried out at the B3LYP/6-31+G(d) level of theory also support that nucleophilic attack by water takes place at the exocyclic carbon rather than at the beta-lactam carbonyl carbon of the iminium ion. The mechanism for the acid-catalyzed pathway involves a preequilibrium protonation, probably at the beta-lactam nitrogen, followed by rate-limiting alkyl C-O fission with formation of an exocyclic iminum ion. The base-catalyzed hydrolysis involves rate-limiting hydroxide attack at the ester carbonyl carbon. These results imply formation of a beta-lactam system containing a positively charged amide nitrogen atom that hydrolyzes via a pathway that preserves the beta-lactam structure in the product and provide further evidence that cleavage of the beta-lactam C-N bond is not as facile as is commonly imagined.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Acids / chemistry
  • Azetidines / chemistry*
  • Catalysis
  • Enzyme Inhibitors / chemistry
  • Hydrogen-Ion Concentration
  • Hydrolysis
  • Imines / chemistry
  • Kinetics
  • Lactams / chemistry
  • Molecular Structure

Substances

  • 2-azetidinone
  • Acids
  • Azetidines
  • Enzyme Inhibitors
  • Imines
  • Lactams