期刊
CHEMICAL SCIENCE
卷 6, 期 1, 页码 225-236出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4sc02778g
关键词
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资金
- Australian National Science and Technology Organisation (ANSTO, Sydney, Australia)
- Swiss National Science Foundation
- Goethe International Postdoc Programme Fellowship (EU project GO-IN) [291776]
A novel reaction for chelate-free, heat-induced metal ion binding and radiolabeling of ultra-small paramagnetic iron oxide nanoparticles (USPIOs) has been established. Radiochemical and non-radioactive labeling studies demonstrated that the reaction has a wide chemical scope and is applicable to p-, d- and f-block metal ions with varying ionic sizes and formal oxidation states from 2+ to 4+. Radiolabeling studies found that Zr-89-Feraheme (Zr-89-FH or Zr-89-ferumoxytol) can be isolated in 93 +/- 3% radiochemical yield (RCY) and >98% radiochemical purity using size-exclusion chromatography. Zr-89-FH was found to be thermodynamically and kinetically stable in vitro using a series of ligand challenge and plasma stability tests, and in vivo using PET/CT imaging and biodistribution studies in mice. Remarkably, ICP-MS and radiochemistry experiments showed that the same reaction conditions used to produce Zr-89-FH can be employed with different radionuclides to yield Cu-64-FH (66 +/- 6% RCY) and In-111-FH (91 +/- 2% RCY). Electron magnetic resonance studies support a mechanism of binding involving metal ion association with the surface of the magnetite crystal core. Collectively, these data suggest that chelate-free labeling methods can be employed to facilitate clinical translation of a new class of multimodality PET/MRI radiotracers derived from metal-based nanoparticles. Further, this discovery is likely to have broader implications in drug delivery, metal separation science, ecotoxicology of nanoparticles and beyond.
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