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@INPROCEEDINGS{Vanasschen:824537,
author = {Vanasschen, Christian and Tircsó, Gyula and Monár, Enikő
and Brandt, Marie and Ermert, Johannes and Coenen, Heinrich
Hubert and Neumaier, Bernd},
title = {{A} novel {CDTA}-based bifunctional chelator for
52g/55{M}n({II})-labeled bimodal {PET}/{MR} tracers},
reportid = {FZJ-2016-07109},
year = {2016},
abstract = {Research on contrast agents for MRI increasingly
concentrates on paramagnetic MnII complexes as alternative
to GdIII chelates commonly used in the clinical setting.
Besides being an essential metal in vivo and possessing
excellent physical properties for T1-weighted MR
applications, an additional feature of MnII is the
availability of the positron-emitting isotope 52gMn, a
promising candidate for PET imaging. We have recently shown
that radiolabeling CDTA
(trans-1,2-diaminocyclohexane-N,N,N´,N´-tetraacetic acid)
with an isotopic 52g/55Mn mixture gives direct access to the
corresponding bimodal PET/MR tracer.[1] This technique
ensures that both the PET and MR reporter molecules are
present in the required concentrations for each imaging
modality (PET is >106 times more sensitive than MRI) as well
as chemically identical, thus exhibiting the same in vivo
behavior.In order to fully benefit from the synergistic
combination of PET and MR imaging, a dual modal manganese
tracer should either (i) be specific to a tissue/disease,
(ii) have a high relaxivity or (iii) be biomarker
responsive. As the design of such optimized probes requires
the use of a bifunctional MnII chelator (BFMnC), the
CuAAC-reactive compound 1 was synthesized in 6 steps with an
overall yield of $25\%$ (CuAAC = CuI-catalyzed azide-alkyne
cycloaddition). The model chelator 4-HET-CDTA (2), which was
obtained by clicking 1 with 2-azidoethanol followed by
deprotection, was used to assess the equilibrium and kinetic
properties of the corresponding MnII chelate. The stability
constant (log KMnL) and the kinetic inertness (characterized
by the dissociation half-life, t1/2) obtained for
[Mn(4-HET-CDTA)]2- appeared to be equivalent or $35\%$
higher, respectively, than for [Mn(CDTA)]2- (see Table).
Additionally, the $27\%$ relaxivity increase observed for
[Mn(4-HET-CDTA)]2- compared to [Mn(CDTA)]2- indicates that
the novel complex is monoaquated (q = 1). Parameter
[Mn(4-HET-CDTA)]2- [Mn(CDTA)]2- [2]Stability constant –
log KMnL a 13.80 14.32Dissociation half-life – t1/2 (h) b
16.23 12.00Relaxivity – r1 (mM-1s-1) c 4.56 3.6Conditions:
a = 0.15 M NaCl, 25°C; b pH = 7.4, [Cu2+] = 10-5 M, 25°C;
c 20 MHz, 25°C.Current efforts focus on the design of
PSMA-targeted 52g/55Mn-tracers for hybrid PET/MR imaging of
prostate cancer (PSMA = prostate-specific membrane antigen).
Notably, an azide-containing, tert-butyl-protected
PSMA-binding motif was prepared and efficiently coupled to
BFMnC 1 by CuAAC in $>70\%$ yield. Radiolabeling of the
obtained conjugate with isotopic 52g/55Mn upon deprotection
is under progress, aiming at the first evaluation of
manganese-based PET/MR probes in animal models.},
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},
cid = {I:(DE-Juel1)INM-5-20090406},
pnm = {573 - Neuroimaging (POF3-573)},
pid = {G:(DE-HGF)POF3-573},
typ = {PUB:(DE-HGF)24},
url = {https://juser.fz-juelich.de/record/824537},
}