Although several synthetic approaches to opicapone or
opicapone subunits have been disclosed, a synthetic approach
described by Bial was exemplified on a scale capable of
producing 14.4 kg of the active pharmaceutical ingredient
(API). Commercial 2,4-pentanedione (114) was condensed
with cyanoacetamide in warm methanol to give rise to
cyanopyridone 115 in excellent yield. Chlorination
with sulfuryl chloride in chilled acetonitrile followed by
treatment with phosphorus oxychloride resulted in dichloropyridine
117. Next, treatment with hydroxylamine in aqueous
methanol converted nitrile 117 to the corresponding Nhydroxyamidine
118, and this was followed by exposure to
pyridine and acid chloride 119. These operations facilitated a cyclization
reaction, which furnished the key oxadiazole 120 in good yield.
Subjection of 120 to urea hydrogen peroxide (UHP) in
dichloromethane to establish the pyridine N-oxide functionality
within opicapone preceded methyl ether cleavage through the
use of aluminum trichloride in warm pyridine to furnish
opicapone (X) in 53% yield for the two-step sequence.
The preparation of acid chloride 119 involved the nitration
of commercially available benzoic acid 121 followed by thionyl
chloride-mediated conversion of the resulting nitrobenzoic acid
122 to acid chloride 119. Interestingly, although
the nitration step is low-yielding and involves nitric acid, the
authors report an operationally simple isolation method that
has been exemplified on multiple kilogram scale. No yield was
reported for the conversion of 122 to 119.