Cyclization of the acyl glucuronide metabolite of a neutral endopeptidase inhibitor to an electrophilic glutarimide: synthesis, reactivity, and mechanistic analysis

J Med Chem. 2007 Nov 29;50(24):6165-76. doi: 10.1021/jm0706766. Epub 2007 Nov 7.

Abstract

The neutral endopeptidase inhibitor (2R)-2-[(1-{[(5-ethyl-1,3,4-thiadiazol-2-yl)amino]carbonyl}cyclopentyl)methyl]pentanoic acid 2 is metabolized to acyl glucuronide 3. Unprecedentedly, at pH 7.4, 3 does not undergo the O-acyl migration characteristic of acyl glucuronides but rapid, eliminative cyclization (t1/2 at 37 degrees C, 10.2 min) to glutarimide 4. Glucuronide 3 was synthesized efficiently via acylation of benzylglucuronate with N-benzyloxymethyl-protected 2. Glucuronide and imide reacted rapidly in aqueous solution, pH 7.4, with amino acids and glutathione to form stable amides and unstable thioesters. Imide 4 acylated eight lysine Nepsilon-amino groups of human serum albumin. Rapid cyclization of 3 was attributed to attack on the ester linkage by an unusually nucleophilic glutaramide NH (pKa in 2 = 9.76). N-propyl 3 was refractory to acyl migration and cyclization. This suggested a synthetic strategy for preparing analogues of 2 that form chemically stable acyl glucuronides.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Cyclization
  • Glucuronides / chemistry*
  • Humans
  • Hydrogen-Ion Concentration
  • Hydrolysis
  • Male
  • Neprilysin / antagonists & inhibitors*
  • Neprilysin / chemistry*
  • Pentanoic Acids / chemistry*
  • Pentanoic Acids / metabolism*
  • Piperidones / chemical synthesis*
  • Piperidones / chemistry
  • Piperidones / pharmacokinetics
  • Rats
  • Rats, Wistar
  • Serum Albumin / chemistry
  • Stereoisomerism
  • Thiadiazoles / chemical synthesis*
  • Thiadiazoles / chemistry*
  • Thiadiazoles / metabolism*
  • Thiadiazoles / pharmacokinetics

Substances

  • 2-(1-((2-ethyl-1,3,4-thiadiazol-5-yl)aminocarbonyl)cyclopentyl)pentanoic acid
  • 7-(5-ethyl-1,3,4-thiadiazol-2-yl)-9-propyl-7-azaspiro(4,5)decane-6,8-dione
  • Glucuronides
  • Pentanoic Acids
  • Piperidones
  • Serum Albumin
  • Thiadiazoles
  • Neprilysin