Synthesis and biological evaluation of alpha-halogenated bisphosphonate and phosphonocarboxylate analogues of risedronate

J Med Chem. 2007 Nov 29;50(24):5967-75. doi: 10.1021/jm0702884. Epub 2007 Nov 2.

Abstract

Alpha-halogenated analogues of the anti-resorptive bisphosphonate risedronate (5, Ris) and its phosphonocarboxylate cognate (7, 3-PEHPC) were synthesized and compared with 5, 7, and the corresponding desoxy analogues in bone mineral affinity and mevalonate pathway inhibition assays. The Ris (5e-h) and 3-PEHPC (7e-h) analogues had decreased bone mineral affinity, confirming that the alpha-OH group in 5 and 7 enhances bone affinity. The 5 alpha-halo-analogues potently inhibited farnesyl pyrophosphate synthase (FPPS) with IC50 values from 16 (alpha-F) to 340 (alpha-Br) nM (5, 6 nM). In contrast, 7 alpha-halo-analogues were ineffective versus FPPS (IC50 > 600 microM), but inhibited Rab geranylgeranyl transferase (RGGT) (IC50 = 16-35 microM) similarly to 7 itself (IC50 = 24 microM). The alpha-F analogue 7e was 1-2 times as active as 7 in J774 cell viability and Rab11 prenylation inhibition assays.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Alkyl and Aryl Transferases / antagonists & inhibitors
  • Animals
  • Bone Density Conservation Agents / chemical synthesis*
  • Bone Density Conservation Agents / chemistry
  • Bone Density Conservation Agents / pharmacology
  • Cell Line
  • Cell Proliferation
  • Cell Survival / drug effects
  • Chromatography, Liquid
  • Diphosphonates / chemical synthesis*
  • Diphosphonates / chemistry
  • Diphosphonates / pharmacology
  • Durapatite / chemistry
  • Etidronic Acid / analogs & derivatives*
  • Etidronic Acid / chemical synthesis
  • Etidronic Acid / chemistry
  • Etidronic Acid / pharmacology
  • Geranyltranstransferase / antagonists & inhibitors
  • Mice
  • Organophosphonates / chemical synthesis*
  • Organophosphonates / chemistry
  • Organophosphonates / pharmacology
  • Propionates / chemical synthesis*
  • Propionates / chemistry
  • Propionates / pharmacology
  • Protein Prenylation / drug effects
  • Pyridines / chemical synthesis*
  • Pyridines / chemistry
  • Pyridines / pharmacology
  • Risedronic Acid
  • Structure-Activity Relationship

Substances

  • 1-fluoro-2-(3-pyridinyl)ethylidene-1,1-bisphosphonic acid
  • 2-(3-pyridinyl)-1-hydroxyethylidene-1,1-phosphonocarboxylic acid
  • 2-fluoro-3-(3-pyridinyl)-2-phosphonopropionic acid
  • Bone Density Conservation Agents
  • Diphosphonates
  • Organophosphonates
  • Propionates
  • Pyridines
  • Durapatite
  • Alkyl and Aryl Transferases
  • Rab geranylgeranyltransferase
  • Geranyltranstransferase
  • Risedronic Acid
  • Etidronic Acid