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@INPROCEEDINGS{Petina:824536,
author = {Petina, Olga and Ermert, Johannes and Coenen, Heinrich
Hubert and Neumaier, Bernd},
title = {{NOTA}- and {DOTA}-coated gold nanoparticles for bimodal
{PET}-{MR} molecular imaging},
reportid = {FZJ-2016-07108},
year = {2016},
abstract = {Bimodal hybrid PET-MR imaging offers as valuable and
promising tool for non-invasive diagnosis ofvarious diseases
as it benefits from the advantages of both individual
imaging modalities, i.e. thesuperb soft tissue contrast of
MRI combined with the excellent sensitivity and ability of
quantificationof PET. With hybrid PET-MR scanners already
available, the development of suitable bimodal PET-MRimaging
agents is essential. Those molecular probes will provide
better morphological correlation ofmolecular function,
biomarker-responsive imaging and time-saving
“PET-guided” high-resolutionMRI.For this purpose, gold
nanoparticle (Au-NP) based bimodal contrast agents were
designed. Incontrast to small organic molecules with a
limited number of attachment points, nanoparticles (NPs)can
be loaded with various ligands in the required ratio. This
allows to overcome the mismatch ofconcentrations of the
imaging probes which are required for PET and MRT
measurements,respectively. The GdDOTA complex was chosen as
MRI-reporting moiety due to its highthermodynamic stability
and kinetic inertness which are very important properties
for the in vivoapplication of Gd-loaded NPs with an enhanced
time of circulation in the body.The very challenging
synthesis of a DOTA-like chelator with a thiol anchoring
group for the directcovalent immobilization on the gold
surface was carried out using the “bisaminal route”.
Startingfrom triethylenetetramine, a $DOTA_OH-tBu4$ ester
was obtained, according to some optimization of adescribed
procedure1. The O-alkylation of $DOTA_OH-tBu4$ ester with
thiol-bearing electrophiles,which was followed by
deprotection, led to the DOTA derivatives L1 and L2 with the
thiol handlebeing directly attached to the macrocyclic
backbone. The thiol-containing NOTA L3 for radiolabelingof
Au-NPs with the PET radionuclide 68Ga was directly obtained
from a commercially available NODAGA-NHS ester through
reaction with cysteamine.Citrate-stabilized Au-NPs with d
≈ 13 nm were prepared by citrate reduction of HAuCl4 and
thenfunctionalized with thiol-ending chelators by a ligand
place exchange reaction. The DOTAfunctionalizedAu-NPs formed
the corresponding complexes Au@GdL1 and Au@GdL2 with Gd
ionswhich were tested for their potential as contrast
agents. As expected, the paramagnetic Au-NPsshowed an
increased relaxivity (36-39 mM-1s-1, 25°C, 20 MHz) compared
with their small molecularanalogues GdL1/Gd2L22 (4-12
mM-1s-1, 25°C, 20 MHz). After that the mixture of DOTA and
NOTAchelating agents were grafted to the gold surface. The
difference in cavity size of NOTA and DOTAshould lead to a
selective complex formation of Au@DOTA-NOTA first with
paramagnetic Gd andthen with radioactive 68Ga,2 forming
thereby a bimodal PET-MR imaging agent.},
month = {Sep},
date = {2016-09-26},
organization = {Being Smart In Coordination Chemistry:
Medical Applications, Orleans (France),
26 Sep 2016 - 28 Sep 2016},
subtyp = {Plenary/Keynote},
cin = {INM-5 / INM-4},
cid = {I:(DE-Juel1)INM-5-20090406 / I:(DE-Juel1)INM-4-20090406},
pnm = {573 - Neuroimaging (POF3-573)},
pid = {G:(DE-HGF)POF3-573},
typ = {PUB:(DE-HGF)24},
url = {https://juser.fz-juelich.de/record/824536},
}