Enzyme-Responsive LipoCEST Agents: Assessment of MMP-2 Activity by Measuring the Intra-liposomal Water 1HNMR Shift

Mobile proton-containing solutes can be detected by MRI by the chemical exchange saturation transfer (CEST) method. CEST sensitivity is dramatically enhanced by using, as exchanging protons, the water molecules confined inside liposomes, shifted by a paramagnetic shift reagent. The chemical shift of...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2017-09, Vol.56 (40), p.12170
Main Authors: Ferrauto, Giuseppe, DiGregorio, Enza, Ruzza, Marta, Catanzaro, Valeria, Padovan, Sergio, Aime, Silvio
Format: Article
Language:English
Subjects:
Biotin
Enzymes
Exchanging
Gelatinase A
Liposomes
Magnetic resonance imaging
Phospholipids
Proteins
Protons
Saturation
Sensitivity enhancement
Solutes
Streptavidin
Water chemistry
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Summary:Mobile proton-containing solutes can be detected by MRI by the chemical exchange saturation transfer (CEST) method. CEST sensitivity is dramatically enhanced by using, as exchanging protons, the water molecules confined inside liposomes, shifted by a paramagnetic shift reagent. The chemical shift of the intraliposomal water resonance ([delta]IL) is affected by the overall shape of the supramolecular system. [delta]IL of a spherical LipoCEST acts as a sensitive reporter of the distribution of streptavidin proteins anchored at the liposome surface by biotinylated phospholipids. This finding prompted the design of a MMP-2 responsive LipoCEST agent as the streptavidin moieties can be released from the liposome surfaces when a properly tailored enzyme-cleavable peptide is inserted on the phospholipids before the terminal biotin residues. [delta]IL reports on the overall changes in the supramolecular architecture associated to the cleavage carried out by MMP-2.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201706271