Stabilization Strategies for Linear Minigastrin Analogues: Further Improvements via the Inclusion of Proline into the Peptide Sequence

J Med Chem. 2020 Dec 10;63(23):14668-14679. doi: 10.1021/acs.jmedchem.0c01233. Epub 2020 Nov 23.

Abstract

Minigastrin (MG) analogues, known for their high potential to target cholecystokinin-2 receptor (CCK2R) expressing tumors, have limited clinical applicability due to low enzymatic stability. By introducing site-specific substitutions within the C-terminal receptor-binding sequence, reduced metabolization and improved tumor targeting can be achieved. In this work, the influence of additional modification within the N-terminal sequence has been explored. Three novel 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA)-conjugated CCK2R ligands with proline substitution at different positions were synthesized. Substitution did not affect CCK2R affinity, and the conjugates labeled with indium-111 and lutetium-177 showed a high enzymatic stability in different incubation media as well as in vivo (57-79% intact radiopeptide in blood of BALB/c mice at 1 h p.i.) combined with enhanced tumor uptake (29-46% IA/g at 4 h in xenografted BALB/c nude mice). The inclusion of Pro contributes significantly to the development of CCK2R ligands with optimal targeting properties for application in targeted radiotherapy.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Amino Acid Sequence
  • Animals
  • Cell Line, Tumor
  • Drug Stability
  • Female
  • Gastrins / chemical synthesis
  • Gastrins / metabolism*
  • Gastrins / pharmacokinetics
  • Heterocyclic Compounds, 1-Ring / chemical synthesis
  • Heterocyclic Compounds, 1-Ring / metabolism*
  • Heterocyclic Compounds, 1-Ring / pharmacokinetics
  • Humans
  • Indium Radioisotopes / chemistry
  • Lutetium / chemistry
  • Mice, Inbred BALB C
  • Proline / chemistry*
  • Protein Binding
  • Radioisotopes / chemistry
  • Radiopharmaceuticals / chemical synthesis
  • Radiopharmaceuticals / metabolism*
  • Radiopharmaceuticals / pharmacokinetics
  • Rats
  • Receptor, Cholecystokinin B / metabolism

Substances

  • Gastrins
  • Heterocyclic Compounds, 1-Ring
  • Indium Radioisotopes
  • Radioisotopes
  • Radiopharmaceuticals
  • Receptor, Cholecystokinin B
  • 1,4,7,10-tetraazacyclododecane- 1,4,7,10-tetraacetic acid
  • minigastrin
  • Lutetium
  • Proline
  • Lutetium-177
  • Indium-111