Developing High Field MRI Contrast Agents by Tuning the Rotational Dynamics: Bisaqua GdAAZTA-based Dendrimers
Israel Journal of Chemistry, ISSN: 1869-5868, Vol: 57, Issue: 9, Page: 887-895
2017
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Article Description
Monomeric and dimeric AAZTA-based bifunctional chelators (AAZTA=6-amino-6-methylperhydro-1,4-diazepine tetraacetic acid) were attached to different generations (G0, G1 and G2) of ethylenediamine-cored PAMAM dendrimers (PAMAM=polyamidoamine) to obtain a series of six dendrimeric systems with 4 to 32 chelates at the periphery. These Gd-loaded dendrimers have molecular weight ranging from 3.5 to 25 kDa, thus allowing a systematic investigation on the changes in relaxivity (r) with the variation of the rotational dynamics following the increase in molecular size. Variable-temperature O NMR (on the dimeric building block GdL2) and H Nuclear Magnetic Relaxation Dispersion measurements at different temperatures indicate that the water exchange lifetime (τ∼90 ns) of the two inner sphere water molecules does not represent a limiting factor to the relaxivity of the systems. The r values at 1.5 T (60 MHz) and 298 K increases from 10.2 mM s for the monomer GdL1 to 31.4 mM s for the dendrimer GdG2-32 (+308 %). However, the relaxivity (per Gd) does not show a linear dependence on the molecular mass, but rather the enhancement tends to attenuate markedly for larger systems. This effect has been attributed to the growing decrease in correlation between local rotational motions and global molecular tumbling.
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