US2012130097A1PendingUtilityA1

Process for the preparation of cyclopropyl carboxylic acid esters and derivatives

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Assignee: CLARK ADRIANPriority: Jun 2, 2000Filed: Jan 30, 2012Published: May 24, 2012
Est. expiryJun 2, 2020(expired)· nominal 20-yr term from priority
C07C 51/60C07C 2601/02C07C 247/22C07C 211/40C07B 2200/07C07C 67/347C07C 51/38C07C 69/753C07C 51/09C07C 57/60C07C 57/66C07C 61/40C07C 2601/14C07D 487/04
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Claims

Abstract

The invention relates to a novel process for the preparation of certain cyclopropyl carboxylic acid esters and other cyclopropyl carboxylic acid derivatives; a novel process for the preparation of dimethylsulfoxonium methylide and dimethylsulfonium methylide; to the use of certain cyclopropyl carboxylic acid esters in a process for the preparation of intermediates that can be used in the synthesis of pharmaceutically active entities; and to certain intermediates provided by these processes.

Claims

exact text as granted — not AI-modified
1 . A process for the preparation of a compound of formula (I): 
       
         
           
           
               
               
           
         
         wherein: 
         R is phenyl substituted with one or more halogen; 
         Y is OR 1 , where R 1  is a straight chain alkyl, branched alkyl, cycloalkyl, or a substituted bicycloheptyl group; 
         which comprises contacting a compound of formula (II): 
       
       
         
           
           
               
               
           
         
         where R and Y are as defined above, with dimethylsulfoxonium methylide in the presence of a solvent at a temperature of −10° C.-90° C. 
       
     
     
         2 . A process for the preparation of a compound of formula (I) as claimed in  claim 1  comprising the steps of;
 i) reacting a trimethylsufoxonium salt with a solid metal hydroxide in dimethyl sulfoxide at ambient or an elevated temperature to produce dimethylsulfoxonium methylide; and 
 ii) contacting compound of formula (II) with dimethylsulfoxonium methylide in the presence of a solvent at a temperature of −10° C.-90° C. 
 
     
     
         3 . A process according to  claim 2  in which the metal hydroxide is sodium hydroxide. 
     
     
         4 . A process according to  claim 1  in which the compound of formula (II) is prepared from a compound of formula (III): 
       
         
           
           
               
               
           
         
         where R is as defined in  claim 1 , by reaction with a chlorinating agent in the presence of an inert solvent and a catalyst at a temperature of 0-200° C., and than reacting the resulting solution with YH or Y, where Y is as defined in  claim 1 , at an elevated temperature. 
       
     
     
         5 . A process according to  claim 4  in which a compound of formula (III) is reacted with thionyl chloride in the presence of an inert solvent and pyridine at a temperature of 0-200° C., and the resulting solution is then reacted with YH or Y, where Y is as defined above at an elevated temperature. 
     
     
         6 . A process according to  claim 1  in which YH represents L-menthol. 
     
     
         7 . A process according to  claim 4  in which a compound of formula (III) is prepared by contacting a compound of formula (IV): 
       
         
           
           
               
               
           
         
         where R is as defined above, with malonic acid in the presence of pyridine and piperidne at elevated temperatures. 
       
     
     
         8 . A process for the preparation of a compound of formula (V): 
       
         
           
           
               
               
           
         
         where R is as defined in  claim 1 , comprising base hydrolysis of a compound of formula (I). 
       
     
     
         9 . A process according to  claim 8  wherein base hydrolysis is achieved using an alkali metal hydroxide and solvent at 10-100° C. 
     
     
         10 . A process for the preparation of a compound of formula (VI): 
       
         
           
           
               
               
           
         
         where R is as defined in  claim 1 , from a compound of formula (V) by reaction with thionyl chloride in the presence of solvent and a catalyst at 0-200° C. 
       
     
     
         11 . A process for the preparation of a compound of formula (VII): 
       
         
           
           
               
               
           
         
         where R is as defined in  claim 1 , from a compound of formula (VI), by reaction with an alkali metal azide in the presence of a phase transfer catalyst, aqueous potassium carbonate and an inert solvent. 
       
     
     
         12 . A process for the preparation of a compound of formula (VIII): 
       
         
           
           
               
               
           
         
         where R is as defined in  claim 1 , from a compound of formula (VII), by rearrangement in toluene at elevated temperatures, and subsequent reaction with hydrochloric acid at elevated temperatures. 
       
     
     
         13 . A process for the preparation of a compound of formula (IX): 
       
         
           
           
               
               
           
         
         where R is as defined in  claim 1 , by adjusting to pH 10 or more an aqueous solution of the salt of a compound of formula (VIII). 
       
     
     
         14 . A process for the preparation of a compound the mandelic acid salt of a compound of formula (IX) by addition of R-(−)-mandelic acid to the compound of formula (IX) as made in  claim 13 , at ambient or an elevated temperature. 
     
     
         15 . A process according to  claim 1  in which R is phenyl substituted by one or more fluorine atoms. 
     
     
         16 . A process according to  claim 15  in which R is 3,4-difluorophenyl. 
     
     
         17 . A process according to  claim 1  in which Y is chiral. 
     
     
         18 . A process according to  claim 17  in which Y is L-menthoxy. 
     
     
         19 . A process according to  claim 1  in which a compound of formula (I) is resolved to yield a compound of formula (Ia): 
       
         
           
           
               
               
           
         
         where R and Y are as defined in  claim 1 , by crystallisation or by chromatrographic methods. 
       
     
     
         20 . A process according to  claim 19  in which the resolution is carried out by extracting a compound of formula (I) into heptane and then effecting crystallisation from the heptane extracts. 
     
     
         21 . The intermediate compounds of formulae (I), (Ia), (II), (III), (V), (Va), (VI), (VIa), (VII), (VIIa), (VIII), (VIIIa), (IX) and (IXa) above. 
     
     
         22 . The intermediate compounds;
 (1R, 2S, 5R)-2-isopropyl-5-methylcyclohexyl trans-2-(3,4-difluorophenyl)cyclopropanecarboxylate;   (1R,2S,5R)-2-isopropyl-5-methylcyclohexyl trans- (1R, 2R)-2-(3,4-difluorophenyl)cyclopropanecarboxylate;   (1R,2S,5R)-2-isopropyl-5-methylcyclohexyl(E)-3-(3,4-difluorophenyl)-2-propenoate;   (E)-3-(3,4-difluorophenyl)-2-propenoic acid;   (E)-3-(3,4-difluorophenyl)-2-propenoyl chloride;   trans-(1R, 2R)-2-(3,4-difluorophenyl)cyclopropanecarboxylic acid;   trans-(1R, 2R)-2-(3,4-difluorophenyl)cyclopropanecarbonyl chloride;   trans-(1R, 2R)-2-(3,4-difluorophenyl)cyclopropanecarbonyl azide;   trans-(1R,2S)-2-(3,4-difluorophenyl)cyclopropyl amine;   and trans-(1 R,2S)-2-(3,4-difluorophenyl)cyclopropanaminium (2R)-2-hydroxy-2-phenylethanoate.

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