Radiosynthesis and evaluation of a fluorine-18 labeled radioligand targeting vesicular acetylcholine transporter

Bioorg Med Chem Lett. 2018 Nov 15;28(21):3425-3430. doi: 10.1016/j.bmcl.2018.09.030. Epub 2018 Sep 24.

Abstract

Vesicular acetylcholine transporter (VAChT) is a reliable biomarker for assessing the loss of cholinergic neurons in the brain that is associated with cognitive impairment of patients. 5-Hydrotetralin compound (±)-5-OH-VAT is potent (Ki = 4.64 ± 0.32 nM) and selective for VAChT (>1800-fold and 398-fold for σ1 and σ2 receptor, respectively) with favorable hydrophilicity (LogD = 1.78), while (-)-5-OH-VAT originally serves as the radiolabeling precursor of (-)-[18F]VAT, a promising VAChT radiotracer with a logD value of 2.56. To evaluate (-)-5-OH-[18F]VAT as a radiotracer for VAChT, we performed in vitro binding assay to determine the potency of the minus enantiomer (-)-5-OH-VAT and plus enantiomer (+)-5-OH-VAT, indicating that (-)-5-OH-VAT is a more potent VAChT enantiomer. Radiosynthesis of (-)-5-OH-[18F]VAT was explored using three strategies. (-)-5-OH-[18F]VAT was achieved with a good yield (24 ± 6%) and high molar activity (∼37 GBq/µmol, at the end of synthesis) using a microwave assisted two-step one-pot procedure that started with di-MOM protected nitro-containing precursor (-)-6. MicroPET studies in the brain of nonhuman primate (NHP) suggest that (-)-5-OH-[18F]VAT readily penetrated the blood brain barrier and specifically accumulated in the VAChT-enriched striatum with improved washout kinetics from striatum compared to [18F]VAT. Nevertheless, the lower target to non-target ratio may limit its use for in vivo measurement of the VAChT level in the brain.

Keywords: Fluorine-18; PET imaging; Radiolabeling; Vesicular acetylcholine transporter.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Corpus Striatum / metabolism
  • Fluorine Radioisotopes
  • Kinetics
  • Ligands
  • Macaca fascicularis
  • Male
  • Piperidines / chemical synthesis
  • Piperidines / chemistry
  • Piperidines / metabolism*
  • Piperidines / pharmacokinetics
  • Positron-Emission Tomography
  • Protein Binding
  • Radiopharmaceuticals / chemical synthesis
  • Radiopharmaceuticals / chemistry
  • Radiopharmaceuticals / metabolism*
  • Radiopharmaceuticals / pharmacokinetics
  • Stereoisomerism
  • Tetrahydronaphthalenes / chemical synthesis
  • Tetrahydronaphthalenes / chemistry
  • Tetrahydronaphthalenes / metabolism*
  • Tetrahydronaphthalenes / pharmacokinetics
  • Vesicular Acetylcholine Transport Proteins / metabolism*

Substances

  • Fluorine Radioisotopes
  • Ligands
  • Piperidines
  • Radiopharmaceuticals
  • Tetrahydronaphthalenes
  • Vesicular Acetylcholine Transport Proteins
  • Fluorine-18