Synthesis and preclinical characterization of 1-(6'-deoxy-6'-[18F]fluoro-β-d-allofuranosyl)-2-nitroimidazole (β-6'-[18F]FAZAL) as a positron emission tomography radiotracer to assess tumor hypoxia

Bioorg Med Chem. 2016 Nov 1;24(21):5326-5339. doi: 10.1016/j.bmc.2016.08.053. Epub 2016 Aug 29.

Abstract

Positron emission tomography (PET) using fluorine-18 (18F)-labeled 2-nitroimidazole radiotracers has proven useful for assessment of tumor oxygenation. However, the passive diffusion-driven cellular uptake of currently available radiotracers results in slow kinetics and low tumor-to-background ratios. With the aim to develop a compound that is actively transported into cells, 1-(6'-deoxy-6'-[18F]fluoro-β-d-allofuranosyl)-2-nitroimidazole (β-[18F]1), a putative nucleoside transporter substrate, was synthetized by nucleophilic [18F]fluoride substitution of an acetyl protected labeling precursor with a tosylate leaving group (β-6) in a final radiochemical yield of 12±8% (n=10, based on [18F]fluoride starting activity) in a total synthesis time of 60min with a specific activity at end of synthesis of 218±58GBq/μmol (n=10). Both radiolabeling precursor β-6 and unlabeled reference compound β-1 were prepared in multistep syntheses starting from 1,2:5,6-di-O-isopropylidene-α-d-allofuranose. In vitro experiments demonstrated an interaction of β-1 with SLC29A1 and SLC28A1/2/3 nucleoside transporter as well as hypoxia specific retention of β-[18F]1 in tumor cell lines. In biodistribution studies in healthy mice β-[18F]1 showed homogenous tissue distribution and excellent metabolic stability, which was unaffected by tissue oxygenation. PET studies in tumor bearing mice showed tumor-to-muscle ratios of 2.13±0.22 (n=4) at 2h after administration of β-[18F]1. In ex vivo autoradiography experiments β-[18F]1 distribution closely matched staining with the hypoxia marker pimonidazole. In conclusion, β-[18F]1 shows potential as PET hypoxia radiotracer which merits further investigation.

Keywords: Azomycin nucleosides; PET; Pimonidazole; β-6′-[(18)F]FAZAL.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Cell Line, Tumor
  • Dose-Response Relationship, Drug
  • Humans
  • Hypoxia / diagnostic imaging*
  • Hypoxia / pathology
  • Imidazoles / analysis*
  • Imidazoles / chemical synthesis
  • Imidazoles / chemistry*
  • Imidazoles / pharmacokinetics
  • Mice
  • Molecular Structure
  • Monosaccharides / analysis*
  • Monosaccharides / chemical synthesis
  • Monosaccharides / chemistry*
  • Monosaccharides / pharmacokinetics
  • Neoplasms / diagnostic imaging*
  • Neoplasms / pathology
  • Positron-Emission Tomography*
  • Radiopharmaceuticals / analysis*
  • Radiopharmaceuticals / chemical synthesis*
  • Radiopharmaceuticals / chemistry
  • Radiopharmaceuticals / pharmacokinetics
  • Structure-Activity Relationship
  • Tissue Distribution

Substances

  • 1-(6'-deoxy-6'-(18F)fluoro-beta-D-allofuranosyl)-2-nitroimidazole
  • Imidazoles
  • Monosaccharides
  • Radiopharmaceuticals