US2005113398A1PendingUtilityA1

2,4-pyrimidinediamine compounds and uses as anti-proliferative agents

Priority: Aug 7, 2003Filed: Aug 6, 2004Published: May 26, 2005
Est. expiryAug 7, 2023(expired)· nominal 20-yr term from priority
A61K 31/506C07D 413/12C07D 417/12C07D 405/12C07D 403/12C07D 417/14C07D 498/04C07D 401/14A61K 31/4353A61P 35/04C07D 239/48C07D 413/14A61K 31/505C07D 401/12A61P 35/00A61P 43/00
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Claims

Abstract

The present invention provides 2,4-pyrimidinediamine compounds having antiproliferative activity, compositions comprising the compounds and methods of using the compounds to inhibit cellular proliferation and to treat proliferative diseases such as tumorigenic cancers.

Claims

exact text as granted — not AI-modified
1 . A method of inhibiting proliferation of a cancer cell, comprising contacting the cancer cell with an effective amount of a 2,4-pyrimidinediamine compound according to structural formula (I):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 L 1  and L 2  are each, independently of one another, selected from a lower alkyldiyl linker, a lower alkylene linker and a covalent bond;  
 R 2  is selected from the group consisting of lower alkyl optionally substituted with an R b  group,  
                     
  where Y is NH, O or CH 2 ;  
 R 2′  is hydrogen, methyl or lower alkyl;  
 R 4′  is hydrogen, methyl or lower alkyl;  
 R 4  is selected from the group consisting of lower alkyl optionally monosubstituted with an R a  or R b  group, lower cycloalkyl optionally monosubstituted with an R a  or R b  group, lower cycloheteroalkyl optionally substituted at one or more ring carbon and/or heteroatoms with an R a  or R b  group, —(CR a R a ) n —R b ,  
                     
  where D is ——(CR 7 R 7 ) m —,  
                     
  where Z 1  is N or CH and Z 2  is O, S, NH, S(O) 2 ;  
 R 5  is selected from the group consisting of halo, fluoro and —CF 3 ;  
 R 6  is hydrogen;  
 each R 7  is independently selected from the group consisting of hydrogen, methyl, lower alkyl and halo;  
 each R 8  is independently selected from the group consisting of hydrogen, lower alkyl, —(CH 2 ) n —OH, —OR a , —(CH 2 ) n —NR c R c , —O(CH 2 ) n —R a , —O(CH 2 ) n —R b , —C(O)OR a , —C(S)OR a , halo, —CF 3  and —OCF 3 ;  
 each R 9  is independently selected from the group consisting of hydrogen, lower alkyl, —OR a , —(CH 2 ) n —NR c R c , —O(CH 2 ) n —R a , —O(CH 2 ) n —R b , —C(O)—NR c R c , —C(S)—NR c R c , —S(O) 2 —NR c R c , —NHC(O)R a , —NHC(S)R a , —C(O)—NH—(CH 2 ) n —NR c R c , —C(S)—NH—(CH 2 ) n —NR c R c , halo, —CF 3 , —OCF 3 ,  
                     
 each R 10  is independently selected from the group consisting of hydrogen, lower alkyl, —(CH 2 ) n —OH, —(CH 2 ) n —NR c R c , —OR a , —O(CH 2 ) n —R a , —O(CH 2 ) n —R b , halo, —CF 3 , —OCF 3 ,  
                     
 each R 11  is independently selected from the group consisting of —OR a , —NR c R c  and —NR a R d ;  
 each R 12  is independently selected from the group consisting of lower alkyl, arylalkyl, —OR a , —NR c R c , —C(O)R a , —C(O)OR a  and —C(O)NR c R c ;  
 each R 13  is independently selected from the group consisting of lower alkyl, hydroxy, lower alkoxy, methoxy, —C(O)NR c R c  and —C(O)NH 2 ;  
 each R 15  is independently selected from the group consisting of hydrogen, lower alkyl, lower cycloakyl and phenyl;  
 each R 16  is independently selected from the group consisting of hydrogen, methyl, lower alkyl, lower cycloalkyl, lower branched alkyl and lower cycloalkylmethyl;  
 each R 17  is independently selected from the group consisting of hydrogen, lower alkyl, methyl and R d  or, alternatively, R 17  may be taken together with R 18  to form an oxo (═O) group;  
 each R 18  is independently selected from the group consisting of hydrogen, lower alkyl and methyl or, alternatively, R 18  may be taken together with R 17  to form an oxo (═O) group;  
 each R 19  is independently selected form the group consisting of hydrogen, lower alkyl, methyl and R d ;  
 each R 20  is independently selected from the group consisting of hydrogen, lower alkyl, methyl and R d ;  
 each m is independently an integer from 1 to 3;  
 each n is independently an integer from 1 to 3;  
 each R a  is independently selected from the group consisting of hydrogen, lower alkyl, lower cycloalkyl, lower cycloalkylalkyl, phenyl and benzyl;  
 each R b  is independently selected from the group consisting of —OR a , —CF 3 , —OCF 3 , —NR c R c , —C(O)R a , —C(S)R a , —C(O)OR a , —C(S)OR a , —C(O)NR c R c , —C(S)NR c R c , —S(O) 2 NR c R c , —C(O)NR a R d , —C(S)NR a R d  and —S(O) 2 NR a R d ;  
 each R c  is independently selected from the group consisting of hydrogen, lower alkyl and lower cycloalkyl, or, alternatively, two R c s may be taken together with the nitrogen atom to which they are bonded to form a 5-7 membered saturated ring which optionally includes 1-2 additional heteroatomic groups selected from O, NR a , NR a —C(O)R a , NR a —C(O)OR a  and NR a —C(O)NR a ; and  
 each R d  is independently selected from lower mono-hydroxyalkyl and lower di-hydroxyalkyl,  
 
         with the provisos that: 
 (i) when R 2  is  
                     
  then R 9  and R 10  are not both simultaneously lower alkoxy or methoxy, or when R 2  is 3,4,5-trimethoxyphenyl or 3,4,5-tri(loweralkoxy)phenyl, then R 4  is  
                     
 (ii) when R 2  is lower alkyl, then R 4  is  
                     
 (iii) when R 4  is  
                     
  and L 2  is lower alkylene, then R 2  is other than 3-(1,3-oxazolyl)phenyl;  
 (iv) when R 4  is  
                     
  where R 15  is t-butyl and R 2  is  
                     
  then at least two of R 8 , R 9  and R 10  or R 8 , R 9  and R 13  are other than hydrogen;  
 (v) when R 4  is  
                     
  where R 15  is t-butyl and R 2  is  
                     
  where R 8  and R 9  are each hydrogen, then R 10  is other than —(CH 2 ) n —OH or —O(CH 2 ) n —R b  where R b  is selected from —NR c R c , —C(O)R a , —C(O)NR c R c  and —C(O)NR a R d .  
 
       
     
     
         2 . The method of  claim 1  in which L 1  and L 2  are each a covalent bond.  
     
     
         3 . The method of  claim 2  in which R 5  is fluoro.  
     
     
         4 . The method of  claim 3  in which R 2′  and R 4′  are each hydrogen.  
     
     
         5 . The method of  claim 3  in which R 2′  is hydrogen and R 4′  is methyl.  
     
     
         6 . The method of  claim 3  in which R 2  is  
       
         
           
           
               
               
           
         
       
     
     
         7 . The method of  claim 6  in which R 4  is selected from unsubstituted cyclopropyl, unsubstituted cyclobutyl, unsubstituted cyclopentyl, unsubstituted cyclohexyl  
       
         
           
           
               
               
           
         
       
       where R e  and R f  are selected from (C1-C3) alkanyl and methyl and R g  is benzyl.  
     
     
         8 . The method of  claim 7  in which R 8  is hydrogen; R 9  is selected from  
       
         
           
           
               
               
           
         
       
       and R 10  is other than  
       
         
           
           
               
               
           
         
       
     
     
         9 . The method of  claim 8  in which R 10  is selected from hydrogen, methyl, methoxy, hydroxymethyl, trifluoromethyl and chloro.  
     
     
         10 . The method of  claim 8  in which R 12  is selected from methyl, —C(O)CH 3 , —C(O)OCH 3  and —C(O)OCH 2 CH 3 .  
     
     
         11 . The method of  claim 8  in which R 8  is hydrogen; R 9  is other than  
       
         
           
           
               
               
           
         
       
       and R 10  is selected from  
       
         
           
           
               
               
           
         
       
     
     
         12 . The method of  claim 11  in which R 9  is selected from hydrogen, methyl, methoxy, hydroxymethyl, trifluoromethyl and chloro.  
     
     
         13 . The method of  claim 11  in which R 12  is selected from methyl, —C(O)CH 3 , —C(O)OCH 3  and —C(O)CH 2 CH 3 .  
     
     
         14 . The method of  claim 8  in which R 9  is other than  
       
         
           
           
               
               
           
         
       
       and R 10  is other than  
       
         
           
           
               
               
           
         
       
     
     
         15 . The method of  claim 14  in which R 8  and R 9  are each hydrogen and R 10  is —OCH 2 NHR a .  
     
     
         16 . The method of  claim 14  in which R 8 , R 9  and R 10  are each, independently of one another, selected from hydrogen, methyl, methoxy, hydroxymethyl, trifluoromethyl and chloro, with the proviso that at least two of R 8 , R 9  and R 10  are other than hydrogen.  
     
     
         17 . The method of  claim 7  in which the 2,4-pyrimidinediamine compound is selected from any compound in any one of TABLEs 1A-1D having an IC 50  of <20 μM against at least one tumor cell line in an in vitro antiproliferation assay.  
     
     
         18 . The method of  claim 3  in which R 4  is  
       
         
           
           
               
               
           
         
       
     
     
         19 . The method of  claim 18  in which R a  is hydrogen and R 15  is selected from lower branched alkyl and lower cycloalkyl.  
     
     
         20 . The method of  claim 18  in which R 15  is t-butyl or cyclopropyl.  
     
     
         21 . The method of  claim 18  in which R 2  is  
       
         
           
           
               
               
           
         
       
     
     
         22 . The method of  claim 21  in which R 8  is hydrogen; R 9  is selected from  
       
         
           
           
               
               
           
         
       
       and R 10  is other than  
       
         
           
           
               
               
           
         
       
     
     
         23 . The method of  claim 22  in which R 10  is selected from methyl, trifluoromethyl and chloro.  
     
     
         24 . The method of  claim 22  in which R 12  of R 9  is selected from methyl, —C(O)CH 3 , —C(O)OCH 3  and —C(O)CH 2 CH 3 .  
     
     
         25 . The method of  claim 21  in which R 8  is hydrogen; R 9  is other than  
       
         
           
           
               
               
           
         
       
       and R 10  is selected from  
       
         
           
           
               
               
           
         
       
     
     
         26 . The method of  claim 25  in which R 9  is selected from hydrogen, methyl, trifluoromethyl and chloro.  
     
     
         27 . The method of  claim 25  in which R 12  of R 10  is selected from methyl, —C(O)CH 3 , —C(O)OCH 3  and —C(O)CH 2 CH 3 .  
     
     
         28 . The method of  claim 18  in which the 2,4-pyrimidinediamine compound is selected from any compound in TABLE 2 having an IC 50  of <20 μM against at least one tumor cell line in an in vitro antiproliferation assay.  
     
     
         29 . The method of  claim 3  in which R 4  is lower alkyl.  
     
     
         30 . The method of  claim 29  in which the lower alkyl is branched.  
     
     
         31 . The method of  claim 30  in which R 4  is i-propyl or t-butyl.  
     
     
         32 . The method of  claim 30  in which R 2  is  
       
         
           
           
               
               
           
         
       
     
     
         33 . The method of  claim 32  in which R 8  is hydrogen; R 9  is selected from  
       
         
           
           
               
               
           
         
       
       and R 10  is other than  
       
         
           
           
               
               
           
         
       
     
     
         34 . The method of  claim 33  in which R 10  is selected from hydrogen, methyl, trifluoromethyl and chloro.  
     
     
         35 . The method of  claim 33  in which R 12  of R 9  is methyl.  
     
     
         36 . The method of  claim 32  in which R 8  is hydrogen; R 9  is hydrogen and R 10  is selected from  
       
         
           
           
               
               
           
         
       
     
     
         37 . The method of  claim 36  in which R 12  is methyl.  
     
     
         38 . The method of  claim 18  in which the 2,4-pyrimidinediamine compound is selected from any compound in TABLE 3 having an IC 50  of <20 μM against at least one tumor cell line in an in vitro antiproliferation assay.  
     
     
         39 . The method of  claim 3  in which R 4  is selected from  
       
         
           
           
               
               
           
         
       
     
     
         40 . The method of  claim 39  in which R 19  and R 20  are different from one another such that the carbon atom to which they are bonded is chiral.  
     
     
         41 . The method of  claim 40  in which the 2,4-pyrimidinediamine compound is a racemate of R and S enantiomers.  
     
     
         42 . The method of  claim 40  which the 2,4-pyrimidinediamine compound is enriched in the R enantiomer.  
     
     
         43 . The method of  claim 42  in which the 2,4-pyrimidinediamine compound is substantially free of the S enantiomer.  
     
     
         44 . The method of  claim 40  in which the 2,4-pyrimidinediamine compound is enriched in the S enantiomer.  
     
     
         45 . The method of  claim 44  in which the 2,4-pyrimidinediamine compound is substantially free of the R enantiomer.  
     
     
         46 . The method of  claim 39  in which R 2  is  
       
         
           
           
               
               
           
         
       
     
     
         47 . The method of  claim 46  in which R 8 , R 9  and R 10  are each, independently of one another, selected from hydrogen, lower alkyl, methyl, lower alkoxy, methoxy, halo, chloro and —OCH 2 C(O)NHR a , with the proviso that at least one of R 8 , R 9  or R 10  is other than hydrogen.  
     
     
         48 . The method of  claim 46  in which R 8  is hydrogen; R 9  is selected from  
       
         
           
           
               
               
           
         
       
       and R 10  is selected from hydrogen, methyl and chloro.  
     
     
         49 . The method of  claim 48  in which R 12  is selected from methyl, —C(O)CH 3 , —C(O)OCH 3  and —C(O)OCH 2 CH 3 .  
     
     
         50 . The method of  claim 46  in which R 8  is hydrogen, R 9  is selected from hydrogen, methyl and chloro; and R 10  is selected from  
       
         
           
           
               
               
           
         
       
     
     
         51 . The method of  claim 50  in which R 12  is selected from methyl, —C(O)CH 3 , —C(O)OCH 3  and —C(O)OCH 2 CH 3 .  
     
     
         52 . The method of  claim 46  in which the substituents on the R 4  and R 2  groups are independently selected from any combinations described in TABLE 4 or TABLE 6.  
     
     
         53 . The method of  claim 46  in which the 2,4-pyrimidinediamine compound is selected from any compound in TABLE 4 or TABLE 6 having an IC 50  of <20 μM against at least one tumor cell line in an in vitro antiproliferation assay.  
     
     
         54 . The method of  claim 3  in which R 4  is  
       
         
           
           
               
               
           
         
       
     
     
         55 . The method of  claim 54  in which D is selected from —CH 2 —CH 2 —, —CF 2 —CF 2 , —CH 2 — and —CF 2 —.  
     
     
         56 . The method of  claim 54  in which R 2  is  
       
         
           
           
               
               
           
         
       
     
     
         57 . The method of  claim 56  in which R 8 , R 9  and R 10  are each, independently of one another, selected from hydrogen, lower alkyl, methyl, hydroxy, lower alkoxy, methoxy, halo, chloro, fluoro, —OCH 2 C(O)NHR a , —OCH 2 C(O)NR c R c , —OCH 2 C(O)OR a , trifluoromethyl and —O(CH 2 ) n OH, with the proviso that at least one of R 8 , R 9  or R 10  is other than hydrogen.  
     
     
         58 . The method of  claim 54  which is selected from any compound in TABLE 5 having an IC 50  of <20 μM against at least one tumor cell line in an in vitro antiproliferation assay.  
     
     
         59 . The method of  claim 3  in which R 2  is  
       
         
           
           
               
               
           
         
       
     
     
         60 . The method of  claim 59  in which R 11  is selected from any R 11  group listed in TABLE 7.  
     
     
         61 . The method of  claim 59  in which the 2,4-pyrimidinediamine compound is selected from any compound in TABLE 7 having an IC 50  of <20 μM against at least one tumor cell line in an in vitro antiproliferation assay.  
     
     
         62 . The method of  claim 3  in which R 4  is  
       
         
           
           
               
               
           
         
       
     
     
         63 . The method of  claim 62  in which R 2  is  
       
         
           
           
               
               
           
         
       
     
     
         64 . The method of  claim 63  in which each R 8 , R 9  and R 10  is selected such that the compound is not an N2,N4-bis(substituted phenyl)-2,4-pyrimidinediamine.  
     
     
         65 . The method of  claim 63  in which each R 8 , R 9  and R 10  is, independently of the others, selected from hydrogen, lower alkyl, methyl, hydroxy, trifluoromethoxy, lower linear alkoxy, halo, —O(CH 2 ) n NR c R c , —OCH 2 C(O)NHR a , —OCH 2 C(O)NR c R c  and —OCH 2 C(O)OR a .  
     
     
         66 . The method of  claim 65  in which R 8 , R 9  and R 10  are each, independently of one another, selected from hydrogen, methyl, trifluoromethyl, methoxy, trifluoromethoxy, and chloro, with the proviso that at least one of R 8 , R 9  and R 10  on both of R 2  and R 4  is other than hydrogen.  
     
     
         67 . The method of  claim 66  in which at least two of R 8 , R 9  and R 10  on both of R 2  and R 4  are other than hydrogen.  
     
     
         68 . The method of  claim 63  in which R 8  and R 9  of R 2  are each hydrogen; R 10  of R 2  is —OCH 2 C(O)NR c R c  or —OCH 2 C(O)NHR a ; R 8  and R 10  of R 4  are, independently of one another, selected from hydrogen, methyl and chloro; and R 9  of R 4  is selected from hydroxy,  
       
         
           
           
               
               
           
         
       
     
     
         69 . The method of  claim 63  in which the 2,4-pyrimidinediamine compound is selected from any compound in TABLE 8 having an IC 50  of <20 μM against at least one tumor cell line in an in vitro antiproliferation assay.  
     
     
         70 . The method of  claim 3  in which R 2  is  
       
         
           
           
               
               
           
         
       
     
     
         71 . The method of  claim 70  in which R 4  is  
       
         
           
           
               
               
           
         
       
       where D is —CH 2 CH 2 —.  
     
     
         72 . The method of  claim 71  in which R 8 , R 9  and R 10  are each, independently of one another, selected from hydrogen, methyl, methoxy, fluoro and chloro.  
     
     
         73 . The method of  claim 71  which is selected from any compound in TABLE 10 having an IC 50  of <20 μM against at least one tumor cell line in an in vitro antiproliferation assay.  
     
     
         74 . The method of  claim 3  in which R 2  is  
       
         
           
           
               
               
           
         
       
     
     
         75 . The method of  claim 74  in which R 4  is  
       
         
           
           
               
               
           
         
       
     
     
         76 . The method of  claim 75  in which R 16  is selected from hydrogen, lower linear alkanyl, lower branched alkanyl, lower cyclic alkanyl and lower cyclicalkanylmethyl.  
     
     
         77 . The method of  claim 75  in which the 2,4-pyrimidinediamine compound is selected from any compound in TABLE 13 having an IC 50  of ≦20 μM against at least one tumor cell line in an in vitro antiproliferation assay.  
     
     
         78 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is selected from any compound illustrated in TABLES 1-14 having an IC 50  of ≦20 μM against at least one tumor cell line in an in vitro antiproliferation assay.  
     
     
         79 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (Ia):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 m is as integer ranging from 1 to 3;  
 R 21  is selected from hydrogen, lower alkyl, methyl, lower alkoxy, methoxy, halogen and chloro;  
 R 22  is selected from hydrogen, lower alkoxy, methoxy, halogen, chloro,  
                     
 R 23  is selected from hydrogen, methyl, lower alkyl, lower alkoxy, methoxy, halogen, chloro, trifluomethyl, —OCH 2 C(O)NHR a ,  
                     
  and  
 R 24  is selected from hydrogen and methyl,  
 with the provisos that (i) when R 22  is  
                     
  then R 23  is other than  
                     
  and (ii) when R 23  is  
                     
  then R 22  is other than  
                     
 
       
     
     
         80 . The method of  claim 79  in which R 21  and R 22  are each hydrogen and R 23  is selected from —OCH 2 C(O)NHR a ,  
       
         
           
           
               
               
           
         
       
     
     
         81 . The method of  claim 79  in which R 22  is selected from hydrogen methoxy, chloro,  
       
         
           
           
               
               
           
         
       
     
     
         82 . The method of  claim 81  in which R 12  is methyl.  
     
     
         83 . The method of  claim 79  in which R 21  is hydrogen and R 22  is  
       
         
           
           
               
               
           
         
       
       where R 12  is methyl.  
     
     
         84 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (Ib):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 R 15  is selected from t-butyl and cyclopropyl;  
 R 21 , R 22  and R 23  are as defined in  claim 79 .  
 
       
     
     
         85 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (Ic):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 R 14  is selected from i-propyl and t-butyl; and  
 R 21 , R 22  and R 23  are as defined in  claim 79 .  
 
       
     
     
         86 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (Id):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 Z 1  is selected from N and CH;  
 Z 2  is selected from NH, O, S and S(O) 2 ;  
 R 16  is selected from hydrogen and methyl;  
 R 19  is as defined in  claim 1;   
 R 20  is as defined in  claim 1;   
 R 24  is as defined in  claim 79;   
 R 41  is selected from hydrogen, lower alkyl, methyl; hydroxy, lower alkoxy, methoxy, halo, chloro, trifluoromethyl and —CH 2 OH;  
 R 42  is selected from hydrogen, lower alkyl, methyl, hydroxy, lower alkoxy, methoxy, halo, chloro, trifluoromethyl, trifluoromethoxy, —OCH 2 C(O)NHR a ,  
                     
  where R 12  is as defined in  claim 1;  and  
 R 43  is selected from hydrogen, lower alkyl, methyl, hydroxy, lower alkoxy, methoxy, halo, chloro, trifluoromethyl, trifluoromethoxy, —OCH 2 C(O)NHR a , —OCH 2 C(O)OR a ,  
                     
  where R 12  is as defined in  claim 1 ,  
 
         with the provisos that: 
 (i) when R 42  is  
                     
  then R 43  is other than  
                     
  and  
 (ii) when R 43  is  
                     
  then R 42  is other than  
                     
 
       
     
     
         87 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (Ie):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein Z 1 , Z 2 , R 16 , R 19 , R 20 , R 24 , R 41 , R 42  and R 43  are as defined in  claim 86 .  
       
     
     
         88 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (If):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 Z 3  is selected from N and CH;  
 p is 0 or 1;  
 R 7  is selected from hydrogen and fluoro;  
 R 24  is as defined in  claim 79;   
 R 51  is selected from hydrogen, lower alkyl, methyl, lower alkoxy, methoxy, halo, trifluoromethyl, CH 2 OH and —C(O)OCH 3 ;  
 R 52  is selected from hydrogen, lower alkyl, methyl, hydroxy, lower alkoxy, methoxy, halo, trifluoromethyl, CH 2 OH and —OCH 2 C(O)NR a R a  where R a  is as defined in  claim 1;  and  
 R 53  is selected from hydrogen, lower alkyl, methyl, lower alkoxy, methoxy, halo, trifluoromethyl, CH 2 OH, —OCH 2 C(O)OR a  and —OCH 2 C(O)NHR a  where R a  is as defined in  claim 1 .  
 
       
     
     
         89 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (Ig):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 R 28  is hydrogen or methyl;  
 R 16  is as defined in  claim 86;  and  
 R 21 , R 22 , R 23  and R 24  are as defined in  claim 79 .  
 
       
     
     
         90 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (Ih):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 R 24  is as defined in  claim 79;   
 R 61  is selected from H and Cl;  
 R 62  is selected from —CH 2 NHBoc, —CH 2 NH 2 , —C(O)NH 2 , —C(O)NH—CH 2 —C(O)OH, —C(O)NH—CH 2 —C(O)OMe and —C(O)NH—CH 2 CH 2 —N(Et) 2 ;  
 R 63  is selected from H and Cl;  
 R 71  is H;  
 R 72  is selected from H, OMe, Cl and —C(O)NH 2 ; and  
 R 73  is selected from H, OMe and Cl.  
 
       
     
     
         91 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (Ii):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 each R 24  is independently as defined in  claim 79;  and  
 R 30  is selected from alkanyl and alkenyl.  
 
       
     
     
         92 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (Ij):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 R 24  is as defined in  claim 79;   
 R 81  is selected from hydrogen, methyl and methoxy;  
 R 82  is selected from hydrogen, methoxy and chloro; and  
 R 83  is selected from methyl, methoxy, halo and fluoro.  
 
       
     
     
         93 . The method of  claim 1  in which the 2,4-pyrimidinediamine compound is a compound according to structural formula (Ik), (Il), (Im) or (In):  
       
         
           
           
               
               
           
         
         including prodrugs, salts, hydrates, solvates and N-oxides thereof, wherein: 
 R 91 , if present, is hydrogen;  
 R 92 , if present, is selected from lower alkoxy, methoxy, halo, chloro and fluoro;  
 R 93 , if present, is selected from lower alkoxy, methoxy, halo and chloro; and  
 R 96  is selected from hydrogen, lower linear alkanyl, lower branched alkanyl, lower cycloalkanyl and lower cycloalkanylmethyl.  
 
       
     
     
         94 . The method of  claim 1  in which the cancer cell is a tumor cell.  
     
     
         95 . The method of  claim 94  in which the tumor cell is a bladder, lung, colon, breast, prostate, pancreatic, ovarian or hepatic tumor cell.  
     
     
         96 . The method of  claim 1  which is practiced in vivo as a therapeteutic approach towards the treatment of cancer.  
     
     
         97 . The method of  claim 96  in which the cancer is a metastatic tumor.  
     
     
         98 . The method of  claim 97  in which the cancer is selected from the group consisting of breast, colon, pancreatic, lung, neural, esophageal, gastric, and melanoma.  
     
     
         99 . The method of  claim 96  in which the compound is administered in the form of a pharmaceutical composition.  
     
     
         100 . The method of  claim 99  in which the compound is administered orally or intravenously.  
     
     
         101 . The method of  claim 100  in which the subject is a human.

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