A self-assembled complex with a titanium(IV) catecholate core as a potential bimodal contrast agent |
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Authors: | Dehaen Geert Eliseeva Svetlana V Kimpe Kristof Laurent Sophie Vander Elst Luce Muller Robert N Dehaen Wim Binnemans Koen Parac-Vogt Tatjana N |
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Institution: | Katholieke Universiteit Leuven, Department of Chemistry, Celestijnenlaan 200F, P.O. Box 2404, 3001 Heverlee, Belgium. |
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Abstract: | A ditopic chelating ligand (H(6)4) that bears catechol and diethylenetriamine-N,N,N',N',N'-pentaacetate (DTPA) has been designed and shown to specifically bind lanthanide(III) ions at the DTPA core (Ln(H(2)4)(H(2)O)](-)) and further self-assemble with titanium(IV), thereby giving rise to the formation of a supramolecular metallostar complex with a lanthanide(III)-to-titanium(IV) ratio of 3:1, (Ln4)(3)Ti(H(2)O)(3)](5-) (Ln=La, Eu, Gd). The efficacy of the metallostar complex as a potential bimodal optical/magnetic resonance imaging (MRI) agent has been evaluated. Nuclear magnetic relaxation dispersion (NMRD) measurements for the (Gd4)(3)Ti(H(2)O)(3)](5-) complex have demonstrated an enhanced r(1) relaxivity that corresponds to 36.9 s(-1) mM(-1) per metallostar molecule at 20 MHz and 310 K, which is a result of a decreased tumbling rate. The ability of the complex to bind to human serum albumin (HSA) was also examined by relaxometric measurements. In addition, upon UV irradiation the (Gd4)(3)Ti(H(2)O)(3)](5-) complex exhibits broad-band green emission in the range 400-750 nm with a maximum at 490 nm. Taking into account the high relaxivity and luminescence properties, the (Gd4)(3)Ti(H(2)O)(3)](5-) complex is a good lead compound for the development of efficient bimodal contrast agents. |
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Keywords: | gadolinium lanthanides magnetic resonance imaging self‐assembly titanium |
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