Journal
INORGANIC CHEMISTRY
Volume 47, Issue 22, Pages 10788-10795Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ic801458u
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Funding
- National Institutes of Health/National Institute of Biomedical Imaging and Bioengineering [1 R01 EB005866-01]
- Nanomaterials for Cancer Diagnostics and Therapeutics [5 U54 CA1193 41-02]
- ARCS (Achievement Rewards for College Scientists) Foundation
- NSEC
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We report on the mechanism of a series of Zn-II-activated magnetic resonance contrast agents that modulate the access of water to a paramagnetic Gd-III ion to create an increase in relaxivity upon binding of Zn-II, In the absence and presence of Zn-II, the coordination at the Gd-III center is modulated by appended Zn-II binding groups. These groups were systematically varied to optimize the change in coordination upon Zn-II binding. We observe that at least one appended aminoacetate must be present as a coordinating group to bind Gd-III and effectively inhibit access of water. At least two binding groups are required to efficiently bind Zn-II, creating an unsaturated complex and allowing access of water. C-13 isotopic labeling of the acetate binding groups for NMR spectroscopy provides evidence of a change in the metal coordination of these groups upon the addition of Zn-II supporting our proposed mechanism of activation as presented.
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