US2014200354A1PendingUtilityA1

Process for the Manufacture of Non-Steroidal Anti-Inflammatory Agents and Intermediates Thereof

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Assignee: INTENDIS GMBHPriority: Apr 18, 2007Filed: Mar 14, 2014Published: Jul 17, 2014
Est. expiryApr 18, 2027(~0.8 yrs left)· nominal 20-yr term from priority
C07D 333/72C07D 307/79C07D 209/44A61P 29/00C07D 333/54C07D 317/06C07D 209/08C07D 405/12C07D 307/78C07D 307/87C07D 405/08
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Claims

Abstract

The current invention describes novel chiral synthetic routes and intermediates for the manufacture of chiral anti-inflammatory agents of general formula VIII in which at least one of the groups X 1 , X 2 , X 3 is selected from fluoro, chloro, bromo, hydroxy, methoxy, ethoxy, trifluoromethyl, amino whereas the other groups X 1 , X 2 , X 3 have the meaning of a hydrogen atom, in which at least one of the groups Z 1 , Z 2 , Z 3 is selected from —O—, —S—, —N(—CH 3 )—, whereas the other groups Z 1 , Z 2 , Z 3 have the meaning of a —CH 2 — group, and in which Ar is an aromatic group.

Claims

exact text as granted — not AI-modified
1 .- 18 . (canceled) 
     
     
         19 . A process for producing a compound according to formula VIII 
       
         
           
           
               
               
           
         
         in which at least one of the groups X 1 , X 2 , X 3  is fluoro, chloro, bromo, hydroxy, methoxy, ethoxy, trifluoromethyl or amino 
         and the other groups X 1 , X 2 , X 3  are hydrogen, 
         and in which at least one of the groups Z 1 , Z 2 , Z 3  is —O—, —S—, —NH—, or —N(—CH 3 )—, and the other groups Z 1 , Z 2 , Z 3  are —CH 2 — groups 
         and in which Ar stands for an aromatic group comprising reducing an enantiomerically pure imine of formula VII 
       
       
         
           
           
               
               
           
         
         in which 
         at least one of the groups X 1 , X 2 , X 3  is fluoro, chloro, bromo, hydroxy, methoxy, ethoxy, trifluoromethyl or amino and the other groups X 1 , X 2 , X 3  are hydrogen, 
         and in which at least one of the groups Z 1 , Z 2 , Z 3  is —O—, —S—, —NH— or —N(—CH 3 )—, and the other groups Z 1 , Z 2 , Z 3  are —CH 2 — groups 
       
       and in which Ar stands for an aromatic group. 
     
     
         20 . The process of  claim 19 , wherein said compound of formula VII is obtained by reacting a compound according VI
   H 2 N—Ar  (VI)
   in which Ar is an aromatic group   
       with an enantiomerically pure aldehyde of formula V 
       
         
           
           
               
               
           
         
         in which X 1 , X 2 , X 3 , Z 1 , Z 2 , Z 3  have the above described meaning. 
       
     
     
         21 . The process according to  claim 20 , wherein said compound of formula V is obtained by oxidizing an enantiomerically pure compound according to formula I 
       
         
           
           
               
               
           
         
       
       in which at least one of the groups X 1 , X 2 , X 3  is fluoro, chloro, bromo, hydroxy, methoxy, ethoxy, trifluoromethyl or amino and the other groups X 1 , X 2 , X 3  are hydrogen, and in which at least one of the groups Z 1 , Z 2 , Z 3  is —O—, —S—, —NH—, or —N(—CH 3 )—, and the other groups Z 1 , Z 2 , Z 3  are —CH 2 —. 
     
     
         22 . A process according to  claim 21 , wherein the compound of formula I is reacted with SO 3 /pyridine complex to form the aldehyde of formula V. 
     
     
         23 . A process according to  claim 20 , wherein, in producing the compound of formula VII the compound of formula V is dissolved in acetic acid, the amine of formula VI is added at room temperature, toluene is added and the mixture is refluxed for 5-50 h to yield the imine of formula VII. 
     
     
         24 . A process according to  claim 20 , wherein the amine of formula VI is:
 1-amino-2-methyl-benzene   1-amino-4-methyl-benzene   2-amino-4-methylpyridine   2-amino-pyridine   2-amino-pyrimidine   3-amino-quinoline   4-amino-pyridine   4-amino-pyrimidine   5-amino-isoquinoline   5-amino-1-methyl-isoquinoline   5-amino-2,6-di-methylquinoline   5-amino-2-methyl-indole   5-amino-2-methyl-isoquinol-1(2H)-one   5-amino-2-methylquinoline   5-amino-6-chloro-2-methylquinoline   5-amino-6-fluoro-2-methylquinoline   5-amino-isoquinol-2(1H)-one   5-amino-quinoline   amino-benzene or   N-(4-aminophenyl)-piperidine   
     
     
         25 . A process according to  claim 24 , wherein the amine of formula VI is 5-amino-2-methylquinoline. 
     
     
         26 . A process according to  claim 19 , wherein the imine of formula VII is reacted with sodium borohydride in alcoholic solution to yield the compound according to formula VIII. 
     
     
         27 . A process according to  claim 19 , wherein the compound of formula VIII is:
 1,1,1 trifluoro-4-(5-fluoro-2,3-dihydrobenzofuran-7-yl)-4-methyl-2-{[(2-methyl-5-quinoline-5-ylimino]methyl}pentane-2-ol).   
     
     
         28 . A process according to  claim 19 , wherein the compound of formula VIII is:
 1,1,1 trifluoro-4-(5-fluoro-2,3-dihydrobenzofuran-7-yl)-4-methyl-2-{[(2-methyl-5-quinolinyl]methyl}pentane-2-ol).   
     
     
         29 . A process according to  claim 21 , wherein the enantiomerically pure compound of formula I is: 
       
         
           
                 
                 
                 
                 
                 
                 
                 
                 
               
                     
                 
                     
                   Z 1   
                   Z 2   
                   Z 3   
                   X 1   
                   X 2   
                   X 3   
                   enantiomer 
                 
                     
                 
                   a) 
                   O 
                     
                     
                   F 
                     
                     
                   R 
                 
                   b) 
                     
                   O 
                     
                     
                   F 
                     
                   R 
                 
                   c) 
                     
                     
                   O 
                     
                     
                   F 
                   R 
                 
                   d) 
                   NH 
                     
                     
                   F 
                     
                     
                   R 
                 
                   e) 
                     
                     
                   O 
                     
                   F 
                     
                   R 
                 
                   f) 
                   S 
                     
                     
                     
                     
                   F 
                   R 
                 
                   g) 
                     
                   NH 
                     
                   Cl 
                     
                     
                   R 
                 
                   h) 
                     
                     
                   NH 
                     
                   Cl 
                     
                   R 
                 
                   i) 
                     
                     
                   S 
                     
                     
                   Cl 
                   R 
                 
                   j) 
                     
                   S 
                     
                   CF 3   
                     
                     
                   R 
                 
                   k) 
                   S 
                     
                     
                     
                   CF 3   
                     
                   R 
                 
                   l) 
                   O 
                     
                     
                     
                     
                   CF 3   
                   R 
                 
                   m) 
                     
                   O 
                     
                   O—CH 3   
                     
                     
                   R 
                 
                   n) 
                     
                     
                   O 
                     
                   O—CH 3   
                     
                   R 
                 
                   o) 
                     
                   O 
                   O 
                     
                     
                   O—CH 3   
                   R 
                 
                   p) 
                   O 
                     
                     
                     
                   F 
                     
                   R 
                 
                   q) 
                   NH 
                     
                     
                     
                     
                   F 
                   R 
                 
                   r) 
                     
                   NH 
                     
                   NH 2   
                     
                     
                   R 
                 
                   s) 
                     
                     
                   NH 
                     
                   NH 2   
                     
                   R 
                 
                   t) 
                     
                     
                   O 
                     
                     
                   Br 
                   R 
                 
                   u) 
                   O 
                     
                     
                   F 
                     
                     
                   S 
                 
                   v) 
                     
                   O 
                     
                     
                   F 
                     
                   S 
                 
                   w) 
                     
                     
                   O 
                     
                     
                   F 
                   S 
                 
                   x) 
                   NH 
                     
                     
                   F 
                     
                     
                   S 
                 
                   y) 
                     
                     
                   O 
                     
                   F 
                     
                   S 
                 
                   z) 
                   S 
                     
                     
                     
                     
                   F 
                   S 
                 
                   aa) 
                     
                   NH 
                     
                   Cl 
                     
                     
                   S 
                 
                   bb) 
                     
                     
                   NH 
                     
                   Cl 
                     
                   S 
                 
                   cc) 
                     
                     
                   S 
                     
                     
                   Cl 
                   S 
                 
                   dd) 
                     
                   S 
                     
                   CF 3   
                     
                     
                   S 
                 
                   ee) 
                   S 
                     
                     
                     
                   CF 3   
                     
                   S 
                 
                   ff) 
                   O 
                     
                     
                     
                     
                   CF 3   
                   S 
                 
                   gg) 
                     
                   O 
                     
                   O—CH 3   
                     
                     
                   S 
                 
                   hh) 
                     
                     
                   O 
                     
                   O—CH 3   
                     
                   S 
                 
                   ii) 
                     
                   O 
                   O 
                     
                     
                   O—CH 3   
                   S 
                 
                   jj) 
                   O 
                     
                     
                     
                   F 
                     
                   S 
                 
                   kk) 
                   NH 
                     
                     
                     
                     
                   F 
                   S 
                 
                   ll) 
                     
                   NH 
                     
                   NH 2   
                     
                     
                   S 
                 
                   mm) 
                     
                     
                   NH 
                     
                   NH 2   
                     
                   S 
                 
                   nn) 
                     
                     
                   O 
                     
                     
                   Br 
                    S. 
                 
                     
                 
             
                
                
                
               
               
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
               
            
           
         
       
     
     
         30 . A process according to  claim 19 , wherein one of the groups X 1 , X 2 , X 3  is fluoro and the other groups X 1 , X 2 , X 3  are hydrogen. 
     
     
         31 . A process according to  claim 19 , wherein one of the groups Z 1 , Z 2 , Z 3  is —O— and the others are —CH 2 — groups. 
     
     
         32 . A process according to  claim 19 , wherein Ar is 5-amino 2-methylquinoline. 
     
     
         33 . A process according to  claim 19 , wherein X 1  is H, X 2  is fluoro, X 3  is H, Z 1  is CH 2 , Z 2  is CH 2 , and Z 3  is O. 
     
     
         34 . A process according to  claim 19 , wherein said compound according to formula VIII is: 
       
         
           
           
               
               
           
         
       
     
     
         35 . A process according to  claim 29 , wherein said enantiomerically pure compound of formula I has an enantiomeric excess (ee)>80%. 
     
     
         36 . A process according to  claim 35 , wherein said enantiomerically pure compound of formula I has an enantiomeric excess (ee)>90%. 
     
     
         37 . A process according to  claim 36 , wherein said enantiomerically pure compound of formula I has an enantiomeric excess (ee)>95%. 
     
     
         38 . A process according to  claim 37 , wherein said enantiomerically pure compound of formula I has an enantiomeric excess (ee)>97%. 
     
     
         39 . An enantiomerically pure compound of formula I 
       
         
           
           
               
               
           
         
       
       wherein: 
       
         
           
                 
                 
                 
                 
                 
                 
                 
                 
               
                     
                 
                     
                   Z 1   
                   Z 2   
                   Z 3   
                   X 1   
                   X 2   
                   X 3   
                   enantiomer 
                 
                     
                 
                   a) 
                   O 
                     
                     
                   F 
                     
                     
                   R 
                 
                   b) 
                     
                   O 
                     
                     
                   F 
                     
                   R 
                 
                   c) 
                     
                     
                   O 
                     
                     
                   F 
                   R 
                 
                   d) 
                   NH 
                     
                     
                   F 
                     
                     
                   R 
                 
                   e) 
                   S 
                     
                     
                     
                     
                   F 
                   R 
                 
                   f) 
                     
                   NH 
                     
                   Cl 
                     
                     
                   R 
                 
                   g) 
                     
                     
                   NH 
                     
                   Cl 
                     
                   R 
                 
                   h) 
                     
                     
                   S 
                     
                     
                   Cl 
                   R 
                 
                   i) 
                     
                   S 
                     
                   CF 3   
                     
                     
                   R 
                 
                   j) 
                   S 
                     
                     
                     
                   CF 3   
                     
                   R 
                 
                   k) 
                   O 
                     
                     
                     
                     
                   CF 3   
                   R 
                 
                   l) 
                     
                   O 
                     
                   O—CH 3   
                     
                     
                   R 
                 
                   m) 
                     
                     
                   O 
                     
                   O—CH 3   
                     
                   R 
                 
                   n) 
                     
                   O 
                   O 
                     
                     
                   O—CH 3   
                   R 
                 
                   o) 
                   O 
                     
                     
                     
                   F 
                     
                   R 
                 
                   p) 
                   NH 
                     
                     
                     
                     
                   F 
                   R 
                 
                   q) 
                     
                   NH 
                     
                   NH 2   
                     
                     
                   R 
                 
                   r) 
                     
                     
                   NH 
                     
                   NH 2   
                     
                   R 
                 
                   s) 
                     
                     
                   O 
                     
                     
                   Br 
                   R 
                 
                   t) 
                   O 
                     
                     
                   F 
                     
                     
                   S 
                 
                   u) 
                     
                   O 
                     
                     
                   F 
                     
                   S 
                 
                   v) 
                     
                     
                   O 
                     
                     
                   F 
                   S 
                 
                   w) 
                   NH 
                     
                     
                   F 
                     
                     
                   S 
                 
                   x) 
                   S 
                     
                     
                     
                     
                   F 
                   S 
                 
                   y) 
                     
                   NH 
                     
                   Cl 
                     
                     
                   S 
                 
                   z) 
                     
                     
                   NH 
                     
                   Cl 
                     
                   S 
                 
                   aa) 
                     
                     
                   S 
                     
                     
                   Cl 
                   S 
                 
                   bb) 
                     
                   S 
                     
                   CF 3   
                     
                     
                   S 
                 
                   cc) 
                   S 
                     
                     
                     
                   CF 3   
                     
                   S 
                 
                   dd) 
                   O 
                     
                     
                     
                     
                   CF 3   
                   S 
                 
                   ee) 
                     
                   O 
                     
                   O—CH 3   
                     
                     
                   S 
                 
                   ff) 
                     
                     
                   O 
                     
                   O—CH 3   
                     
                   S 
                 
                   gg) 
                     
                   O 
                   O 
                     
                     
                   O—CH 3   
                   S 
                 
                   hh) 
                   O 
                     
                     
                     
                   F 
                     
                   S 
                 
                   ii) 
                   NH 
                     
                     
                     
                     
                   F 
                   S 
                 
                   jj) 
                     
                   NH 
                     
                   NH 2   
                     
                     
                   S 
                 
                   kk) 
                     
                     
                   NH 
                     
                   NH 2   
                     
                   S 
                 
                   ll) 
                     
                     
                   O 
                     
                     
                   Br 
                    S. 
                 
                     
                 
             
                
                
                
               
               
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
                
               
            
           
         
       
     
     
         40 . A compound according to  claim 39 , wherein said enantiomerically pure compound of formula I has an enantiomeric excess (ee)>80%. 
     
     
         41 . A compound according to  claim 39 , wherein said enantiomerically pure compound of formula I has an enantiomeric excess (ee)>90%. 
     
     
         42 . A compound according to  claim 39 , wherein said enantiomerically pure compound of formula I has an enantiomeric excess (ee)>95%. 
     
     
         43 . A compound according to  claim 39 , wherein said enantiomerically pure compound of formula I has an enantiomeric excess (ee)>97%. 
     
     
         44 . A process according to  claim 29 , wherein 
       one of the groups X 1 , X 2 , X 3  is F, Cl, CF 3 , OCH 3 , NH 2  or Br and the other groups X 1 , X 2 , X 3  are each H; 
       and 
       one of the groups Z 1 , Z 2 , Z 3  is O, S or NH and the other groups Z 1 , Z 2 , Z 3  are each —CH 2 —.

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