US2005038058A1PendingUtilityA1

Novel compounds and methods for therapy

Assignee: ACAD OF SCIENCE CZECH REPUBLICPriority: Jun 29, 2001Filed: Sep 21, 2004Published: Feb 17, 2005
Est. expiryJun 29, 2021(expired)· nominal 20-yr term from priority
A61P 31/12A61P 35/00A61P 31/20A61P 31/18C07F 9/6512Y02P20/55
54
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Claims

Abstract

Novel compounds are provided having formula (I) where R 1 , R 2 , R 3 , R 4 , Z, X and * are defined herein. Also provided are antiviral methods for use and processes for synthesis of the compounds of formula (I).

Claims

exact text as granted — not AI-modified
1 . A compound of the formula (I)  
       
         
           
           
               
               
           
         
       
       where 
 R 1  is H, amino or methylsulfanyl;  
 R 2  is H, methyl, halo, —N(R 5 ) 2 , hydroxy, protected hydroxy or a group of the formula (Ia)  
                     
 R 3  is independently H, methyl, hydroxymethyl, halomethyl or protected hydroxymethyl;  
 R 4  is H or halo;  
 X independenly is oxygen, sulfur or a bond;  
 Z independently is hydroxy, an ester or amide;  
 R 5  is independently H, C 1 -C 8  alkyl or a protecting group; and  
 * designates a chiral carbon atom; and  
 salts and solvates thereof.  
 
     
     
         2 . The compound of  claim 1  wherein R 1 , and R 2  are amino, R 3  is hydrogen and X is oxygen.  
     
     
         3 . The compound of  claim 1  wherein R 1  and R 2  are simultaneously amino, R 3  is methyl, X is oxygen and the R 3  configuration is (R).  
     
     
         4 . The compound of  claim 1  wherein R 1  and R 2  are simultaneously amino, R 3  is hydroxymethyl, X is oxygen and the R 3  configuration is (R).  
     
     
         5 . The compound of  claim 1  wherein R 1  and R 2  are simultaneously amino, R 3  is hydrogen and X is sulfur.  
     
     
         6 . The compound of  claim 1  wherein R 1  is amino, R 2  is hydroxy, R 3  is hydrogen and X is oxygen.  
     
     
         7 . The compound of  claim 1  which is crystalline.  
     
     
         8 . The compound of  claim 1  which is a substantially pure enantiomer at the chiral carbon.  
     
     
         9 . The compound of  claim 8  which is in the (R) configuration.  
     
     
         10 . The compound of  claim 8  which is in the (S) configuration.  
     
     
         11 . 2,4-diamino-6-[2-(phosphonomethoxy)ethoxy]pyrimidine.  
     
     
         12 . 2,4-diamino-6-(R)-[2-(phosphonomethoxy)propoxy]pyrimidine.  
     
     
         13 . 2-amino-4-hydroxy-6-[2-(phosphonomethoxy)ethoxy]pyrimidine.  
     
     
         14 . 2,4-diamino-6-[(S)-3-hydroxy-2-(phosphonomethoxy)propoxy]pyrimidine.  
     
     
         15 . 2,4-diamino-6-[(RS)-3-hydroxy-2-(phosphonomethoxy)propoxy]pyrimidine.  
     
     
         16 . 2-amino-4-hydroxy-6-[(R)-2-(phosphonomethoxy)propoxy]pyrimidine.  
     
     
         17 . 2-amino-4-hydroxy-6-[(RS)-3-hydroxy-2 (phosphonomethoxy)propoxy]pyrimidine.  
     
     
         18 . 2-amino-4-hydroxy-6-[(S)-3-hydroxy-2-(phosphonomethoxy)propoxy]pyrimidine.  
     
     
         19 . 2,4-diamino-5-bromo-6-[2-(phosphonomethoxy)ethoxy]pyrimidine.  
     
     
         20 . 2-amino-5-bromo-4-hydroxy-6-[2-(phosphonomethoxy)ethoxy]pyrimidine.  
     
     
         21 . A composition comprising a pharmaceutically acceptable excipient and a compound of  claim 1 .  
     
     
         22 . A method of preparation of compounds of formula (I)  
       
         
           
           
               
               
           
         
       
       where 
 R 1  is H, amino or methylsulfanyl;  
 R 2  is H, methyl, halo, —N(R 5 ) 2 , hydroxy, protected hydroxy or a group of the formula (Ia)  
                     
 R 3  is independently H, methyl, hydroxymethyl, halomethyl or protected hydroxymethyl;  
 R 4  is H or halo;  
 X independently is oxygen, sulfur or a bond;  
 Z independently is hydroxy, an ester or amide;  
 R 5  is independently H, C 1 -C 8  alkyl or a protecting group; and  
 * designates a chiral carbon atom; and  
 comprising (a) reacting a compound of formula (II)  
                     
 where  
 R 2  is H, methyl, halo, —N(R 5 ) 2 , hydroxy or protected hydroxy; and  
 X is O or S;  
 with a compound of the formula (III) 
   Y—CH 2 CH(R 3 )—O—CH 2 P(O)(Z) 2   (III) 
 where  
 Z is an ester or an amide;  
 * designates a chiral carbon atom;  
 R 3  is H, methyl, halomethyl or protected hydroxymethyl; and  
 Y is a leaving group  
 in dipolar aprotic solvent in the presence of a base.  
 
     
     
         23 . The method of  claim 22  further comprising isolating the resulting compound of the formula (I).  
     
     
         24 . The method of  claim 22  wherein Z is ester or amide and additionally hydrolyzing one or both Z groups to produce the compound of formula (I) where at least one Z is hydroxy.  
     
     
         25 . The method of  claim 22  where Z is (OR 4 ) 2  and R 4  is isopropyl.  
     
     
         26 . The method of  claim 22  where R 3  is methyl and Y is p-toluenesulfonyloxy.  
     
     
         27 . A method for the preparation of compounds of formula (I)  
       
         
           
           
               
               
           
         
       
       where 
 R 1  is H, amino or methylsulfanyl;  
 R 2  is —N(R 5 ) 2 ;  
 R 3  is independently H, methyl, hydroxymethyl, halomethyl or protected hydroxymethyl;  
 R 4  is H or halo;  
 X is oxygen or sulfur;  
 Z independently is hydroxy, ester or amide;  
 R 5  is independently H, C 1 -C 8  alkyl or a protecting group; and  
 * designates a chiral carbon atom  
 comprising reacting a compound (IV)  
                     
 where  
 R 3  is H, methyl, halomethyl or protected hydroxymethyl;  
 X is O or S; and  
 Z is amidate or ester;  
 with N(R 5 ) 2 .  
 
     
     
         28 . The method of  claim 27  further comprising hydrolyzing one or both Z groups to produce the compound of formula (I) where one or both of Z are hydroxyl.  
     
     
         29 . A method for preparation of compounds of formula (V)  
       
         
           
           
               
               
           
         
       
       where 
 R 3  is H, methyl, hydroxymethyl, halomethyl or protected hydroxymethyl;  
 R 5  independently is H, C 1 -C 8  alkyl or a protecting group;  
 X is oxygen or sulfur;  
 Z independently is hydroxy, an ester or amide; and  
 * designates a chiral carbon atom;  
 comprising reacting compound (IVa)  
                     
 with N(R 5 ) 2  in anhydrous solvent, alkali hydroxide or alkali carbonate in aqueous solution.  
 
     
     
         30 . A method of preparation of the compounds of formula (VI)  
       
         
           
           
               
               
           
         
       
       where 
 R 1  is H, amino or methylsulfanyl;  
 R 3  is H, methyl, hydroxymethyl, halomethyl or protected hydroxymethyl;  
 Z independently is hydroxy, an ester or amide; and  
 * designates a chiral carbon atom;  
 comprising (a) reacting a compound of formula (VII)  
                     
 where  
 R 1  is H, amino or methylsulfanyl  
 with a compound of the formula (VIII) 
   
   
 *  
   HOCH 2 CH 2 (R 3 )OCH 2 P(O)(Z) 2   (VIII) 
 where  
 Z is amide or ester  
 in the presence of a base.  
 
     
     
         31 . The method of  claim 30  further comprising hydrolyzing Z group to produce a compound of formula (VI) where 1 or 2 Z groups are hydroxy.  
     
     
         32 . A method of preparation of compounds of formula (XIII)  
       
         
           
           
               
               
           
         
       
       where 
 R 1  is H, amino or methylsulfanyl;  
 * is a chiral carbon atom;  
 R 2  is H, chloro, hydroxy or amino;  
 R 3  is H, methyl, halomethyl or hydroxymethyl;  
 Z is amide or ester  
 comprising (a) reacting a compound of the formula (IX)  
                     
 where  
 R 1  is H, amino or methylsulfanyl;  
 R 2  is H, chloro or amino;  
 with a compound of the formula (X)  
                     
 where  
 R 3  is H, methyl, hydroxymethyl, halomethyl or protected hydroxymethyl;  
 * is a chiral carbon atom;  
 R 6  is hydroxy or protected hydroxy;  
 or R 3  and R 6  are joined by a cyclic acetal or ketal protecting group; in the presence of a base without solvent or in the presence of an aprotic solvent, to produce a compound of formula (XI)  
                     
 where  
 R 1  is H, amino or methylsulfanyl;  
 * is a chiral carbon atom;  
 R 2  is H, chloro or amino; and  
 R 3  is H, methyl, halomethyl or protected hydroxymethyl; and  
 (b) reacting compound (XI) with a compound of the formula (XII) 
   Y—CH 2 P(O)(OZ) 2   (XII) 
 where  
 Y is a leaving group;  
 Z is amide or ester  
 in the presence of a base in dimethylformamide or tetrahydrofurane to produce a compound of formula (XIII).  
 
     
     
         33 . The method of  claim 32  further comprising hydrolyzing Z group to produce a compound of formula (XIII) where 1 or 2 Z groups are hydroxyl.  
     
     
         34 . A method of preparation of a compound of formula (I)  
       
         
           
           
               
               
           
         
       
       where 
 R 1  is H, amino or methylsulfanyl;  
 R 3  is H, methyl, hydroxymethyl, halomethyl or protected hydroxymethyl;  
 R 4  is halo;  
 X is oxygen;  
 Z independently is hydroxy, an ester or amide; and  
 * designates a chiral carbon atom;  
 comprising (a) reacting a compound of the formula (VI)  
                     
 where  
 R 1  is H, amino or methylsulfanyl;  
 R 3  is H, methyl, hydroxymethyl, halomethyl or protected hydroxymethyl;  
 Z independently is an ester; and  
 * designates a chiral carbon atom;  
 with elemental halogen in an inert solvent to produce a compound of formula (I).  
 
     
     
         35 . The method of  claim 34  further comprising hydrolyzing Z group to produce a compound of formula (I) where 1 or 2 Z groups are hydroxyl.  
     
     
         36 . A method for the treatment of a viral infection comprising administering a therapeutically effective amount of a compound of  claim 1  to a patient in need of such treatment.  
     
     
         37 . The method of  claim 36  where the virus is a DNA virus.  
     
     
         38 . The method of  claim 37  where the virus is a retrovirus or hepadnavirus.

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