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@INPROCEEDINGS{Cavani:825301,
author = {Cavani, Melanie and Bier, Dirk and Coenen, Heinrich Hubert},
title = {{N}ew strategy of a two-step radiosynthesis of
[{F}-18]fluoropyridine-based maleimide-containing prosthetic
groups for labelling of peptides and proteins},
reportid = {FZJ-2016-07765},
year = {2015},
abstract = {Objectives The use of thiol-reactive groups allows the
introduction of fluorine-18 in a peptide or protein with
cysteine residues, and different radiofluorinated
maleimide-containing prosthetic groups have been described
in the literature. All compounds were, however, prepared by
a two- or three-step synthesis with an overall reaction time
of at least 70 minutes. The aim of this work was to improve
the radiosynthesis of maleimide-containing compounds with
reduced reaction steps by using a new synthetic route via
protection of the maleimide function. This was first done
here with the example of
1-[3-(2-[18F]fluoropyridin-3-oxy)propyl]pyrrol-2,5-dione
([18F]FPyME) which is usually prepared in three steps [1].
Methods The first step for the preparation of the precursor
was a Williamson reaction to form the ether from
3-hydroxy-2-nitropyridine with 1,3-dibromopropane. In a
parallel process maleimide was protected with
2,5-dimethylfurane via a Diels-Alder-reaction. These two
products were combined by N-alkylation to form the
precursor. The radiosynthesis includes the introduction of
fluorine-18 by nucleophilic substitution of the nitro group
followed by deprotection of the maleimide function (see fig.
1). The reaction steps were optimized with regard to
temperature, time and solvents. Results The optimal
conditions for the n.c.a. radiofluorination were identified
at a temperature of 80 °C in DMSO and a reaction time of 5
minutes, resulting in a radiochemical yield of about 29 ± 3
$\%.$ At higher temperatures the deprotection of the
precursor and the labelled compound come to the fore and
thereby the decomposition of the unprotected maleimide
occurs due to the basic reaction conditions. The
deprotection step was quantitatively carried out within 15
minutes. [18F]FPyME was isolated by HPLC to provide the pure
prosthetic group which was directly used for effective
peptide labelling. The overall synthesis time was about 60
minutes and the overall radiochemical yield was about 20
$\%.$ Conclusions The described synthetic route provides the
possibility to gain a variety of further
[18F]fluoropyridine-based maleimide-containing compounds in
two steps only. In addition, this method offers to be
performed as one-pot synthesis. Acknowledgements References
[1] de Bruin B. et al. (2006) Bioconjugate Chem., 16,
406-420.},
month = {May},
date = {2015-05-26},
organization = {21st International Symposium on
Radiopharmaceutical Sciences, Columbia
(USA), 26 May 2015 - 31 May 2015},
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/825301},
}