Open AccessNanoparticle‐based PARACEST agents: the quenching effect of silica nanoparticles on the CEST signal from surface‐conjugated chelates
Author(s) -
Evbuomwan Osasere M.,
Merritt Matthew E.,
Kiefer Garry E.,
Dean Sherry A.
Publication year - 2012
Publication title -
contrast media & molecular imaging
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.714
H-Index - 50
eISSN - 1555-4317
pISSN - 1555-4309
DOI - 10.1002/cmmi.459
Subject(s) - chemistry , nanoparticle , protonation , conjugated system , quenching (fluorescence) , molecule , fluorescence , catalysis , chelation , microemulsion , photochemistry , inorganic chemistry , organic chemistry , nanotechnology , materials science , ion , polymer , pulmonary surfactant , biochemistry , physics , quantum mechanics
Silica nanoparticles of average diameter 53 ± 3 nm were prepared using standard water‐in‐oil microemulsion methods. After conversion of the surface Si–OH groups to amino groups for further conjugation, the PARACEST agent, EuDOTA–(gly) 4 − was coupled to the amines via one or more side‐chain carboxyl groups in an attempt to trap water molecules in the inner‐sphere of the complex. Fluorescence and ICP analyses showed that ~1200 Eu 3+ complexes were attached to each silica nanoparticle, leaving behind excess protonated amino groups. CEST spectra of the modified silica nanoparticles showed that attachment of the EuDOTA–(gly) 4 − to the surface of the nanoparticles did not result in a decrease in water exchange kinetics as anticipated, but rather resulted in a complete elimination of the normal Eu 3+ ‐bound water exchange peak and broadening of the bulk water signal. This observation was traced to catalysis of proton exchange from the Eu 3+ ‐bound water molecule by excess positively charged amino groups on the surface of the nanoparticles. Copyright © 2012 John Wiley & Sons, Ltd.