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Polyfunctionalised Nanoparticles Bearing Robust Gadolinium Surface Units for High Relaxivity Performance in MRI

Research output: Contribution to journalArticle

Nicolas G. Chabloz, Margot N. Wenzel, Hannah L. Perry, Il Chul Yoon, Susannah Molisso, Graeme J. Stasiuk, Daniel S. Elson, Anthony E.G. Cass, James D.E.T. Wilton-Ely

Original languageEnglish
Pages (from-to)10895-10906
Number of pages12
JournalChemistry - A European Journal
Volume25
Issue number46
DOIs
Accepted/In press16 May 2019
Published14 Aug 2019

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Abstract

The first example of an octadentate gadolinium unit based on DO3A (hydration number q=1) with a dithiocarbamate tether has been designed and attached to the surface of gold nanoparticles (around 4.4 nm in diameter). In addition to the superior robustness of this attachment, the restricted rotation of the Gd complex on the nanoparticle surface leads to a dramatic increase in relaxivity (r1) from 4.0 mm−1 s−1 in unbound form to 34.3 mm−1 s−1 (at 10 MHz, 37 °C) and 22±2 mm−1 s−1 (at 63.87 MHz, 25 °C) when immobilised on the surface. The one-pot synthetic route provides a straightforward and versatile way of preparing a range of multifunctional gold nanoparticles. The incorporation of additional surface units for biocompatibility (PEG and thioglucose units) and targeting (folic acid) leads to little detrimental effect on the high relaxivity observed for these non-toxic multifunctional materials. In addition to the passive targeting attributed to gold nanoparticles, the inclusion of a unit capable of targeting the folate receptors overexpressed by cancer cells, such as HeLa cells, illustrates the potential of these assemblies.

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