Synthesis, X-ray crystallography, and pharmacokinetics of novel azomethine prodrugs of (R)-alpha-methylhistamine: highly potent and selective histamine H3 receptor agonists

J Med Chem. 1995 Sep 29;38(20):4070-9. doi: 10.1021/jm00020a022.

Abstract

Since various neuroregulatory functions of the histamine H3 receptor have been proved during the last few years, the H3 receptor is of current interest. Azomethine derivatives of the highly potent histamine H3 receptor agonist (R)-alpha-methylhistamine (1) were prepared as lipophilic prodrugs to improve the bioavailability of the hydrophilic drug, particularly its entry into the brain. Additionally, azomethine derivatization provides protection against histamine methyltransferase, the major metabolizing enzyme in man, and thus efficiently enhances the bioavailability of 1. The molecular conformations of (R)-2(-)[[N(-)[1-(1H-imidazol-4-yl)-2-propyl]- imino]phenylmethyl]phenol (9a) and (R)-4-fluoro-2(-)[[N(-)[1-(1H-imidazol-4-yl)-2-propyl[imino]- (4-chlorophenyl)methyl]phenol (9p) were determined by X-ray structure analysis. An intramolecular hydrogen bond which is essential for the stability of these azomethines was thereby confirmed. Moreover, the pharmacokinetic parameters of the prodrugs were investigated in vitro as well as in vivo. The halogenated azomethines have an effect following peroral administration in mice, and some of them seem to be highly potent for the central nervous system (CNS) delivery of 1. At present the most potent prodrug of 1 is (R)-4-chloro-2(-)[[N(-)[1-(1H-imidazol-4-yl)-2-propyl]imino](4- chlorophenyl)methyl]phenol (9q), reaching by far the highest CNS level of 1 (Cmax = 71 ng/g). Prodrugs of this type are not only valuable pharmacological tools but may also become H3 histaminergic drugs for therapeutic use.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Crystallography, X-Ray
  • Histamine Agonists / chemical synthesis*
  • Histamine Agonists / chemistry
  • Histamine Agonists / pharmacokinetics
  • Male
  • Methylhistamines / chemical synthesis*
  • Methylhistamines / chemistry
  • Methylhistamines / pharmacokinetics
  • Mice
  • Prodrugs / chemical synthesis*
  • Prodrugs / chemistry
  • Prodrugs / pharmacokinetics

Substances

  • Histamine Agonists
  • Methylhistamines
  • Prodrugs
  • alpha-methylhistamine