Synthesis of gadolinium-labeled shell-crosslinked nanoparticles for magnetic resonance imaging applications
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abstract
Shell-crosslinked knedel-like nanoparticles (SCKs; "knedel" is a Polish term for dumplings) were derivatized with gadolinium chelates and studied as robust magnetic-resonance-imaging-active structures with hydrodynamic diameters of 40 3 nm. SCKs possessing an amphiphilic core-shell morphology were produced front the aqueous assembly of diblock copolymers of poly(acrylic acid) (PAA) and poly(methyl acrylate) (PMA), PAA 52-b-PMA128, and subsequent covalent crosslinking by amidation upon reaction with 2,2-(ethylenedioxy)bis(ethylamine) throughout the shell layer. The properties of these materials, including non-toxicity towards mammalian cells, non-immunogenicity within mice, and capability for polyvalent targeting, make them ideal candidates for utilization within biological systems. The synthesis of SCKs derivatized with Gd III and designed for potential use as a unique nanometer-scale contrast agent for MRI applications is described herein. Utilization of an amino-functionalized diethylenetriaminepentaacetic acid-Gd analogue allowed for direct covalent conjugation throughout the hydrophilic shell layer of the SCKs and served to increase the rotational correlation lifetime of the Gd. In addition, the highly hydrated nature of the shell layer in which the Gd was located allowed for rapid water exchange; thus, the resulting material demonstrated large ionic relaxivities (39 s-1 mM-1) in an applied magnetic field of 0.47 T at 40C and, as a result of the large loading capacity of the material, also demonstrated high molecular relaxivities (20 000 s-1 mM-1). 2005 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
