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Issue 1, 2015
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Chelate-free metal ion binding and heat-induced radiolabeling of iron oxide nanoparticles

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Abstract

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 89Zr–Feraheme (89Zr–FH or 89Zr–ferumoxytol) can be isolated in 93 ± 3% radiochemical yield (RCY) and >98% radiochemical purity using size-exclusion chromatography. 89Zr–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 89Zr–FH can be employed with different radionuclides to yield 64Cu–FH (66 ± 6% RCY) and 111In–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.

Graphical abstract: Chelate-free metal ion binding and heat-induced radiolabeling of iron oxide nanoparticles

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Publication details

The article was received on 09 Sep 2014, accepted on 29 Sep 2014 and first published on 29 Sep 2014


Article type: Edge Article
DOI: 10.1039/C4SC02778G
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Chem. Sci., 2015,6, 225-236
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    Chelate-free metal ion binding and heat-induced radiolabeling of iron oxide nanoparticles

    E. Boros, A. M. Bowen, L. Josephson, N. Vasdev and J. P. Holland, Chem. Sci., 2015, 6, 225
    DOI: 10.1039/C4SC02778G

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