A modular system for the synthesis of multiplexed magnetic resonance probes

Daniel J. Mastarone, Victoria S.R. Harrison, Amanda L. Eckermann, Giacomo Parigi, Claudio Luchinat, Thomas J. Meade

Research output: Contribution to journalArticlepeer-review

95 Scopus citations

Abstract

We have developed a modular architecture for preparing high-relaxivity multiplexed probes utilizing click chemistry. Our system incorporates azide bearing Gd(III) chelates and a trialkyne scaffold with a functional group for subsequent modification. In optimizing the relaxivity of this new complex, we undertook a study of the linker length between a chelate and the scaffold to determine its effect on relaxivity. The results show a strong dependence on flexibility between the individual chelates and the scaffold with decreasing linker length leading to significant increases in relaxivity. Nuclear magnetic resonance dispersion (NMRD) spectra were obtained to confirm a 10-fold increase in the rotational correlation time from 0.049 to 0.60 ns at 310 K. We have additionally obtained a crystal structure demonstrating that modification with an azide does not impact the coordination of the lanthanide. The resulting multinuclear center has a 500% increase in per Gd (or ionic) relaxivity at 1.41 T versus small molecule contrast agents and a 170% increase in relaxivity at 9.4 T.(Figure Presented)

Original languageEnglish (US)
Pages (from-to)5329-5337
Number of pages9
JournalJournal of the American Chemical Society
Volume133
Issue number14
DOIs
StatePublished - Apr 13 2011

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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