Site-specific labeling of cysteine-tagged camelid single-domain antibody-fragments for use in molecular imaging

Bioconjug Chem. 2014 May 21;25(5):979-88. doi: 10.1021/bc500111t. Epub 2014 May 9.

Abstract

Site-specific labeling of molecular imaging probes allows the development of a homogeneous tracer population. The resulting batch-to-batch reproducible pharmacokinetic and pharmacodynamic properties are of great importance for clinical translation. Camelid single-domain antibody-fragments (sdAbs)-the recombinantly produced antigen-binding domains of heavy-chain antibodies, also called Nanobodies-are proficient probes for molecular imaging. To safeguard their intrinsically high binding specificity and affinity and to ensure the tracer's homogeneity, we developed a generic strategy for the site-specific labeling of sdAbs via a thio-ether bond. The unpaired cysteine was introduced at the carboxyl-terminal end of the sdAb to eliminate the risk of antigen binding interference. The spontaneous dimerization and capping of the unpaired cysteine required a reduction step prior to conjugation. This was optimized with the mild reducing agent 2-mercaptoethylamine in order to preserve the domain's stability. As a proof-of-concept the reduced probe was subsequently conjugated to maleimide-DTPA, for labeling with indium-111. A single conjugated tracer was obtained and confirmed via mass spectrometry. The specificity and affinity of the new sdAb-based imaging probe was validated in a mouse xenograft tumor model using a modified clinical lead compound targeting the human epidermal growth factor receptor 2 (HER2) cancer biomarker. These data provide a versatile and standardized strategy for the site-specific labeling of sdAbs. The conjugation to the unpaired cysteine results in the production of a homogeneous group of tracers and is a multimodal alternative to the technetium-99m labeling of sdAbs.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Antigen-Antibody Reactions
  • Biomarkers, Tumor / analysis
  • Camelus / immunology*
  • Cysteine / chemistry*
  • Cysteine / immunology
  • Female
  • Humans
  • Mice
  • Mice, Nude
  • Models, Molecular
  • Molecular Imaging*
  • Molecular Probes / chemistry
  • Molecular Probes / immunology
  • Neoplasms, Experimental / diagnosis*
  • Protein Engineering
  • Receptor, ErbB-2 / analysis
  • Single-Domain Antibodies / chemistry*
  • Single-Domain Antibodies / immunology*
  • Tissue Distribution
  • Tumor Cells, Cultured

Substances

  • Biomarkers, Tumor
  • Molecular Probes
  • Single-Domain Antibodies
  • ERBB2 protein, human
  • Receptor, ErbB-2
  • Cysteine