Hetero-Diels-Alder and CuAAC Click Reactions for Fluorine-18 Labeling of Peptides: Automation and Comparative Study of the Two Methods

Molecules. 2024 Jul 5;29(13):3198. doi: 10.3390/molecules29133198.

Abstract

Radiolabeled peptides are valuable tools for diagnosis or therapies; they are often radiofluorinated using an indirect approach based on an F-18 prosthetic group. Herein, we are reporting our results on the F-18 radiolabeling of three peptides using two different methods based on click reactions. The first one used the well-known CuAAC reaction, and the second one is based on our recently reported hetero-Diels-Alder (HDA) using a dithioesters (thia-Diels-Alder) reaction. Both methods have been automated, and the 18F-peptides were obtained in similar yields and synthesis time (37-39% decay corrected yields by both methods in 120-140 min). However, to obtain similar yields, the CuAAC needs a large amount of copper along with many additives, while the HDA is a catalyst and metal-free reaction necessitating only an appropriate ratio of water/ethanol. The HDA can therefore be considered as a minimalist method offering easy access to fluorine-18 labeled peptides and making it a valuable additional tool for the indirect and site-specific labeling of peptides or biomolecules.

Keywords: CuAAC; automated synthesis; cycloaddition; fluorine-18; hetero-Diels–Alder; labeling; peptide; radiochemistry.

Publication types

  • Comparative Study

MeSH terms

  • Automation
  • Catalysis
  • Click Chemistry* / methods
  • Copper* / chemistry
  • Cycloaddition Reaction*
  • Fluorine Radioisotopes* / chemistry
  • Isotope Labeling / methods
  • Peptides* / chemistry
  • Radiopharmaceuticals / chemical synthesis
  • Radiopharmaceuticals / chemistry

Substances

  • Fluorine Radioisotopes
  • Peptides
  • Fluorine-18
  • Copper
  • Radiopharmaceuticals

Grants and funding

This research was funded by the Interdisciplinary Thematic Institute IMS, the drug discovery and development institute, as part of the ITI 2021–2028 program of the University of Strasbourg, CNRS, and Inserm, supported by IdEx Unistra (ANR-10-IDEX-0002) and SFRI-STRAT’US project (ANR-20-SFRI-0012). T.M. was supported by a fellowship from the ENS Paris-Saclay.