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Macrocyclic and Hydroxamate Ligands for 225Ac Radiopharmaceuticals: Evaluating SSTR2-Targeting Potential.

Satoru Tsushima1,2, Ayush Seal1,3, Sergey A Samsonov4

  • 1Institute of Resource Ecology, Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Dresden 01328, Germany.

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This study explored chelator structures for actinium-225 (225Ac) radiopharmaceuticals targeting somatostatin receptor 2 (SSTR2). Hydroxamate ligands and DOTP show promise, offering alternatives to DOTA for improved radiopharmaceutical design.

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Area of Science:

  • Radiopharmaceutical chemistry
  • Molecular interactions
  • Nuclear medicine

Background:

  • Effective radiopharmaceuticals depend on chelator properties influencing receptor binding.
  • Somatostatin receptor 2 (SSTR2) is a key target for targeted therapies.

Purpose of the Study:

  • To investigate molecular interactions between 225Ac radiopharmaceuticals with varying chelators and SSTR2.
  • To identify novel chelating agents for improved 225Ac radiopharmaceutical development.

Main Methods:

  • Comparative analysis of chelator structures (DOTP vs. DOTA) and linker effects (PEG4).
  • Density functional theory (DFT) calculations to explore hydroxamate ligands.
  • Synthesis and characterization of a siderophore ligand (DFO*) and its complexation with La3+.
  • NMR spectroscopy (1H and 139La) to confirm complexation.

Main Results:

  • 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetra(methylene)phosphonic acid (DOTP) is a viable alternative to DOTA due to higher negative charge.
  • Poly(ethylene glycol) linker (PEG4) enhanced receptor activation.
  • Hydroxamate ligands, like DFO*, show potential but exhibit flexibility issues.
  • The deoxy variant of 3,4,3-LI(1,2-HOPO) is a structurally suitable chelating agent for 225Ac.

Conclusions:

  • DOTP and PEG4 incorporation offer improved SSTR2 targeting for 225Ac radiopharmaceuticals.
  • Hydroxamate ligands require further structural optimization for stability.
  • The deoxy 3,4,3-LI(1,2-HOPO) ligand is a promising candidate for future 225Ac radiopharmaceutical development.