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@INPROCEEDINGS{Holschbach:1027692,
author = {Holschbach, Marcus and Humpert, Swen and Schneider, Daniela
and Schulze, Annette and Bier, Dirk and Neumaier, Bernd},
title = {8-{B}icycloalkyl-{CPFPX} derivatives as potent and
selective tools for {PET} imaging of the {A}1 adenosine
receptor},
issn = {0969-8051},
reportid = {FZJ-2024-04004},
year = {2022},
abstract = {Objectives: The first successful in-house development [1]
ofa radiofluorinated A 1 adenosine receptor (A1AR)
antagonist withnanomolar affinity for the bovine A 1 AR for
in vivo PET studies was8-cyclopentyl-3-(3-[ 18
F]Fluoropropyl)-1-propyl-xanthine, [ 18 F]CPFPX. Although
this ligand proved to be useful in vivo in rodents,already
first preclinical studies revealed possible limitations for
PETimaging. At the beginning our efforts aimed at
synthesizing metabol-ically stabilized CPFPX derivatives,
but the recently published findingby Schneider et al. [2]
that affinity is the key pharmacokinetic deter-minant of
radiolabeled xanthines in the brain prompted us to focusour
efforts on the synthesis of A1AR ligands with high
affinity.Methods: In search of CPFPX-like A1AR ligands with
higher targetaffinity, we decided to replace the cyclopentyl
residue in the 8-posi-tion of the xanthine backbone with
sterically more demanding nor-bornyl residues [3]. The
target xanthines and the radiofluorinationprecursors
(sulfonates) were synthesized through multistep syn-theses
by a modified Traube protocol [4]. Binding experiments
wereperformed with membranes from CHO K1 cells stably
transfectedwith either the human A1 or A2AAR. Nucleophilic
radiofluorinationon the n.c.a level used the classical
Kryptofix™ 2.2.2/K 2 CO 3 method.For in vitro
autoradiography, frozen horizontal sections (20 μm) of
ratbrains were used.Results: From a series of newly
synthesized compounds 1-NBXhas emerged as the most potent
and selective candidate (Figure 1).The norbornyl group has
two surfaces, one being essentially a cyclo-pentyl ring
backed by a two-carbon bridge and the other being
acyclohexyl ring backed by a one-carbon bridge. The greater
potencyof 1-NBX relative to the 2- and 7-norbornyl isomers
probably occursbecause 1-NBX binds to the receptor with its
cyclopentyl surfacefacing the receptor, whereas the 2- and
7-isomers are forced to bindwith the less favorable
cyclohexyl ring facing the receptor.Cyclopentane exists
mainly in an “envelope” conformation, in whichfour of
the carbons form the corners of a flat envelope, and the
fifthcarbon represents the apex of a triangular flap, which
projects at anangle of about 120° from the body of the
envelope [5, 6]. Althoughany of the carbons can take the
out-of-plane position in cyclopen-tane, in norbornane the
bridging carbon is locked in this position.The greater
affinity of 1-NBX compared to that of CPFPX is mostlikely
due to the former being locked in the optimal conformation.
Asexpected from earlier studies, 1-propyl and
3-fluoropropylsubstitution at both 1- and 3-positions of the
xanthine scaffold wasoptimum to potent and selective A1AR
antagonism.#Conclusions: [ 18 F]1-NBX seems to be a
promising A1AR antagonisttracer suitable for PET. Future
preclinical studies will reveal weather1 NBX will have the
potential to serve as a substitute for [ 18
F]CPFPX.References:[1] Holschbach et al., J Med Chem. 2002,
45(23), 5150-5156.[2] Schneider et al., Nucl Med Biol. 2020,
82-83, 1-8.[3] Shimada et al., J Med Chem. 1992, 35,
924-930.[4] Holschbach et al., Org Lett. 2009, 11,
4266-4269.[5] Dragojlovic V., ChemTexts 2015, 1, 14.[6]
Trivedi et al., J Med Chem 1989, 32, 8-11},
month = {May},
date = {2022-05-29},
organization = {24th International Symposium on
Radiopharmaceutical Sciences, Nantes
(France), 29 May 2022 - 3 Jun 2022},
subtyp = {After Call},
cin = {INM-5},
ddc = {570},
cid = {I:(DE-Juel1)INM-5-20090406},
pnm = {5253 - Neuroimaging (POF4-525)},
pid = {G:(DE-HGF)POF4-5253},
typ = {PUB:(DE-HGF)6},
doi = {10.1016/S0969-8051(22)00096-8},
url = {https://juser.fz-juelich.de/record/1027692},
}