Preparation of an Aminoxyl Analog of the Anticancer Agent Miltefosine
George Sosnovsky*, Jan Lukszo**, Robert C. Brasch
Department of Chemistry, University of Wisconsin-Milwaukee, Milwaukee. Wisconsin.
53201. USA. and Contrast Media Laboratory. Department of Radiology. School of Medicine.
University of California, San Francisco. CA 94143. USA
Z. Naturforsch. 51b, 888-890 (1996); received December 11, 1995
Anticancer Agents, Aminoxyl, Nitroxyl, Synthesis
The synthesis and a few properties of hexadecyl 2-[N,N-dimethyl-N-(2,2,6.6-tetramethyl-
l-oxyl-piperidin-4-yl)ammonio] ethyl phosphate are described. This compound is a spin la
beled analog of the antineoplastic drug hexadecylphosphocholine (Miltefosine).
Introduction
A decade ago in quest of developing new suit
able contrast agents for the clinical magnetic reso
nance imaging tomography (MRI), among a vari
ety of compounds [1-3] also were synthesized two
aminoxyls (nitroxyls, “nitroxides”) 1 and 3 con
taining quaternary ammonium moieties. While
compound 1 was used in a study [4] concerning
the membrane permeability of nitroxyl moieties
through human erythrocyte membranes, com
pound 3 was somewhat neglected and not
published.
Recently, it came to our attention [5] that hexa
decyl (cetyl) phosphocholine (Miltefosine, 2), and
related analogs were found [5] to have potent in
vitro and in vivo antineoplastic activities against
several cancer lines. These results prompted us to
disclose the synthesis and the available properties
of the nitroxyl labeled analog 3. It is believed that
this information would be of interest to the scien
tific community participating in the development
of anticancer drugs.
Results and Discussion
The key intermediate N-(2-hydroxyethyl)-N,N-
dimethyl-N-(2,2,6,6-tetramethyl-l-oxyl-piperidin-
4-yl)-tetraphenyl borate (7) was synthesized via
the known compound N-(2-hydroxyethyl)-N,N-di-
methyl-N-(2,2,6,6-tetramethyl-l-oxyl-piperidin-4-
yl) ammonium iodide (6) [6]. 6 was prepared from
4-oxo-2,2,6,6-tetramethyl-piperidin-l-oxyl (4) and
N-methylethanolamine by the reductive amination
reaction mediated by sodium cyanoborohydride.
followed by the methylation of the intermediate
N-(2-hydroxyethyl)-N-methyl-N-(2,2,6,6-tetra-
methyl-l-oxyl-piperidin-4-yl (5) with methyl
iodide to give 6. The reaction of 6 with sodium
tetraphenylborate gave the desired key intermedi
ate 7.
The other key intermediate hexadecylphosphate
(cetyl phosphate, 8) was obtained by using a
known method [7] from cetyl alcohol and phos
phorus oxychloride.
The condensation of 7 with 8 to give hexyl
2-[N,N-dimethyl-N-(2,2,6,6-tetramethyl-l-oxyl-pi-
* Reprint requests to George Sosnovsky.
** Present address: NIH. National Institute of Allergy and Infectious Diseases (NIAID), Laboratory of Molecular
Structure. 12441 Parklawn Drive, Rockville, MD 20852. U.S.A.
0932-0776/96/0600-0888 $06.00 © 1996 Verlag der Zeitschrift für Naturforschung. All rights reserved. n