Synthesis and evaluation of technetium-99m-labeled bioreductive pharmacophores conjugated with amino acids and peptides for tumor imaging

Chem Biol Drug Des. 2015 Apr;85(4):504-17. doi: 10.1111/cbdd.12437. Epub 2014 Oct 25.

Abstract

Development of molecular imaging agents to target tumor has become a major trend in nuclear medicine. With the aim to develop new potential 99mTc-radiopharmaceuticals for targeting tumor, we have synthesized 5-nitroimidazolyl amino acids and RGD-coupled 2-nitroimidazoles. Technetium-99m radiolabeling with high radiochemical purity (>90%) was achieved for all the compounds. The radiolabeled complexes exhibited substantial in vitro stability in saline, serum, and histidine solution (10(-2) m). Cell binding studies in EAC and B16F10 cell lines also revealed rapid and comparatively high cellular internalization. Among all the compounds studied, the binding of 99mTc(CO)3-5 to B16F10 cells was moderately inhibited by the competitive peptide c[RGDfV], suggesting specificity of the radioligand toward αvβ3 receptor. However, no significant displacement of bound radioligand was observed when the binding of the 99mTc-labeled complexes to above cells was challenged with excess competitive peptide. Fluorescent microscopy study provided direct evidence of intracellular localization of 5(6)-carboxyfluorescein-labeled 2-nitroimidazolyl-RGD-peptide in αvβ3-positive B16F10 mouse melanoma cell line. The ligands caused only 8-13% of hemolysis toward rat erythrocytes at concentrations as high as 100 μm. Imaging and biodistribution studies were performed in Swiss albino mice bearing induced tumor. 99mTc-1 and 99mTc(CO)3-5 demonstrated a very favorable in vivo profile. Selective uptake and retention in tumor with encouraging tumor/muscle and tumor/blood ratio and significant cellular uptake of fluorescence-labeled-2-nitroimidazolyl RGD indicate the great potentiality of the pharmacophore for further evaluation as potential molecular imaging agent in cancer diagnosis.

Keywords: amino acids and peptides; bioreductive pharmacophore; technetium-99m labeling; tumor imaging.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Amino Acids / chemical synthesis
  • Amino Acids / chemistry*
  • Amino Acids / metabolism
  • Amino Acids / pharmacokinetics
  • Animals
  • Cell Line, Tumor
  • Mice
  • Molecular Imaging
  • Neoplasms / diagnosis*
  • Neoplasms / diagnostic imaging*
  • Neoplasms / metabolism
  • Oligopeptides / chemical synthesis
  • Oligopeptides / chemistry*
  • Oligopeptides / metabolism
  • Oligopeptides / pharmacokinetics
  • Organotechnetium Compounds / chemical synthesis
  • Organotechnetium Compounds / chemistry*
  • Organotechnetium Compounds / metabolism
  • Organotechnetium Compounds / pharmacokinetics
  • Radionuclide Imaging
  • Rats, Sprague-Dawley

Substances

  • Amino Acids
  • Oligopeptides
  • Organotechnetium Compounds
  • arginyl-glycyl-aspartic acid