Through-Space Paramagnetic NMR Effects in Host-Guest Complexes: Potential Ruthenium(III) Metallodrugs with Macrocyclic Carriers

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Authors

CHYBA Jan NOVÁK Martin MUNZAROVÁ Petra NOVOTNÝ Jan MAREK Radek

Type Article in Periodical
Magazine / Source Inorganic Chemistry
MU Faculty or unit

Central European Institute of Technology

Citation
Web DOI: 10.1021/acs.inorgchem.7b03233
Doi http://dx.doi.org/10.1021/acs.inorgchem.7b03233
Keywords host-guest complex; paramagnetic NMR; x-ray diffraction; relativistic DFT; ruthenium(III); metallodrug; macrocyclic carrier; cyclodextrin; cucurbut[n]uril
Description The potential of paramagnetic ruthenium(III) compounds for use as anticancer metallodrugs has been investigated extensively during the past several decades. However, the means by which these ruthenium compounds are transported and distributed in living bodies remain relatively unexplored. In this work, we prepared several novel ruthenium(III) compounds with the general structure Na+[trans-RuIIICl4(DMSO)(L)]- (DMSO = dimethyl sulfoxide), where L stands for pyridine or imidazole linked with adamantane, a hydrophobic chemophore. The supramolecular interactions of these compounds with macrocyclic carriers of the cyclodextrin (CD) and cucurbit[n]uril (CB) families were investigated by NMR spectroscopy, X-ray diffraction analysis, isothermal titration calorimetry, and relativistic DFT methods. The long-range hyperfine NMR effects of the paramagnetic guest on the host macrocycle are related to the distance between them and their relative orientation in the host-guest complex. The CD and CB macrocyclic carriers being studied in this account can be attached to a vector that attracts the drug-carrier system to a specific biological target and our investigation thus introduces a new possibility in the field of targeted delivery of anticancer metallodrugs based on ruthenium(III) compounds.
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