IP Library Granted Patent US 9,266,894
Granted Patent B2
US 9,266,894 · App. 14/346,006 · Granted Feb 23, 2016

Pyrrolobenzodiazepines as unsymmetrical dimeric PBD compounds for inclusion in targeted conjugates

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Quick Facts
Patent No.
US 9,266,894
App. No.
14/346,006
Granted
Feb 23, 2016
Kind
B2
Abstract

A compound with the formula I wherein: R 2 is of formula II where Q is selected from OH, SH and NR N , and R N is selected from H, methyl and ethyl, as well as drug-linkers and drug-conjugates made from this compound.

Claims (161)

1. A compound with the formula I:

wherein:

R 2 is of formula II:

where Q is selected from OH, SH and NHR N , and R N is selected from H, methyl and ethyl;

when there is a double bond present between C2′ and C3′, R 12 is selected from:

(ia) C 5-10 aryl group, optionally substituted by one or more substituents selected from the group comprising: halo, nitro, cyano, ether, C 1-7 alkyl, C 3-7 heterocyclyl and bis-oxy-C 1-3 alkylene;

(ib) C 1-5 saturated aliphatic alkyl;

(ic) C 3-6 saturated cycloalkyl;

 wherein each of R 21 , R 22 and R 23 are independently selected from H, C 1-3 saturated alkyl, C 2-3 alkenyl, C 2-3 alkynyl and cyclopropyl, where the total number of carbon atoms in the R 12 group is no more than 5;

 wherein one of R 25a and R 25b is H and the other is selected from: phenyl, which phenyl is optionally substituted by a group selected from halo, methyl, methoxy; pyridyl; and thiophenyl;and

 where R 24 is selected from: H; C 1-3 saturated alkyl; C 2-3 alkenyl; C 2-3 alkynyl; cyclopropyl; phenyl, which phenyl is optionally substituted by a group selected from halo, methyl, methoxy; pyridyl; and thiophenyl;

when there is a single bond present between C2′ and C3′,

R 12 is

 where R 26a and R 26b are independently selected from H, F, C 1-4 saturated alkyl, C 2-3 alkenyl, which alkyl and alkenyl groups are optionally substituted by a group selected from C 1-4 alkyl amido and C 1-4 alkyl ester; or, when one of R 26a and R 26b is H, the other is selected from nitrile and a C 1-4 alkyl ester;

R 6 and R 9 are independently selected from H, R, OH, OR, SH, SR, NH 2 , NHR, NRR′, nitro, Me 3 Sn and halo;

where R and R′ are independently selected from optionally substituted C 1-12 alkyl, C 3-20 heterocyclyl and C 5-20 aryl groups;

R 7 is selected from H, R, OH, OR, SH, SR, NH 2 , NHR, NHRR′, nitro, Me 3 Sn and halo;

either:

(a) R 10 is H, and R 11 is OH, OR A , where R A is C 1-4 alkyl;

(b) R 10 and R 11 form a nitrogen-carbon double bond between the nitrogen and carbon atoms to which they are bound; or

(c) R 10 is H and R 11 is SO Z M, where z is 2 or 3 and M is a monovalent pharmaceutically acceptable cation;

R″ is a C 3-12 alkylene group, which chain may be interrupted by one or more heteroatoms, and/or aromatic rings;

Y and Y′ are selected from O, S, or NH;

R 6′ , R 7′ , R 9′ are selected from the same groups as R 6 , R 7 and R 9 respectively and R 10′ and R 11′ are the same as R 10 and R 11 , wherein if R 11 and R 11′ are SO Z M, M may represent a divalent pharmaceutically acceptable cation.

2. A compound according to any claim 1 , wherein R 7 is selected from H, OH and OR.

3. A compound according to claim 2 , wherein R 7 is a C 1-4 alkyloxy group.

4. A compound according to claim 1 , wherein Y is O.

5. A compound according to claim 1 , wherein R″ is C 3-7 alkylene.

6. A compound according to claim 1 , wherein R 9 is H.

7. A compound according to claim 1 , wherein R 6 is selected from H and halo.

8. A compound according to claim 1 , wherein Q is NHR N .

9. A compound according to claim 8 , wherein R N is H or methyl.

10. A compound according to claim 1 , wherein Q is OH or SH.

11. A compound according to claim 1 , wherein there is a single bond between C2′ and C3′, R 12 is

and R 26a and R 26b are both H.

12. A compound according to claim 1 , wherein there is a single bond between C2′ and C3′, R 12 is

and R 26a and R 26b are both methyl.

13. A compound according to claim 1 , wherein there is a single bond between C2′ and C3′, R 12 is

one of R 26a and R 26b is H, and the other is selected from C 1-4 saturated alkyl, C 2-3 alkenyl, which alkyl and alkenyl groups are optionally substituted.

14. A compound according to claim 1 , wherein there is a double bond between C2′ and C3′, and R 12 is a C 5-7 aryl group.

15. A compound according to claim 14 , wherein R 12 is phenyl.

16. A compound according to claim 1 , wherein there is a double bond between C2′ and C3′, and R 12 is a C 8-10 aryl group.

17. A compound according to claim 1 , wherein R 12 bears one to three substituent groups.

18. A compound according to claim 1 , wherein there is a double bond between C2′ and C3′, and R 12 is a C 1-5 saturated aliphatic alkyl group.

19. A compound according to claim 18 , wherein R 12 is methyl, ethyl or propyl.

20. A compound according to claim 1 , wherein there is a double bond between C2′ and C3′, and R 12 is a C 3-6 saturated cycloalkyl group.

21. A compound according to claim 20 , wherein R 12 is cyclopropyl.

22. A compound according to claim 1 , wherein there is a double bond between C2′ and C3′, and R 12 is a group of formula:

23. A compound according to claim 22 , wherein the total number of carbon atoms in the R 12 group is no more than 4.

24. A compound according to claim 23 , wherein the total number of carbon atoms in the R 12 group is no more than 3.

25. A compound according to claim 22 , wherein one of R 21 , R 22 and R 23 is H, with the other two groups being selected from H, C 1-3 saturated alkyl, C 2-3 alkenyl, C 2-3 alkynyl and cyclopropyl.

26. A compound according to claim 22 , wherein two of R 21 , R 22 and R 23 are H, with the other group being selected from H, C 1-3 saturated alkyl, C 2-3 alkenyl, C 2-3 alkynyl and cyclopropyl.

27. A compound according to claim 1 , wherein there is a double bond between C2′ and C3′, and R 12 is a group of formula:

28. A compound according to claim 27 , wherein R 12 is the group:

29. A compound according to claim 1 , wherein there is a double bond between C2′ and C3′, and R 12 is a group of formula:

30. A compound according to claim 29 , wherein R 24 is selected from H, methyl, ethyl, ethenyl and ethynyl.

31. A compound according to claim 30 , wherein R 24 is selected from H and methyl.

32. A compound according to claim 1 , wherein R 10 and R 11 and form a nitrogen-carbon double bond.

33. A compound according to claim 1 wherein R 6′ , R 7′ , R 9′ , R 10′ , R 11′ and Y′ are the same as R 6 , R 7 , R 9 , R 10 , R 11 and y respectively.

34. The use of a compound according to claim 1 in the manufacture of a medicament for treating a proliferative disease.

35. A compound according to claim 1 for use in the treatment of a proliferative disease.

36. A compound of formula II:

wherein:

R 2 is of formula II:

where Q is selected from OH, SH and NHR N , and R N is selected from H, methyl and ethyl;

when there is a double bond present between C2′ and C3′, R 12 is selected from:

(ia) C 5-10 aryl group, optionally substituted by one or more substituents selected from the group comprising: halo, nitro, cyano, ether, C 1-7 alkyl, C 3-7 heterocyclyl and bis-oxy-C 1-3 alkylene;

(ib) C 1-5 saturated aliphatic alkyl;

(ic) C 3-6 saturated cycloalkyl;

 wherein each of R 21 , R 22 and R 23 are independently selected from H, C 1-3 saturated alkyl, C 2-3 alkenyl, C 2-3 alkynyl and cyclopropyl, where the total number of carbon atoms in the R 12 group is no more than 5;

 wherein one of R 25a and R 25b is H and the other is selected from: phenyl, which phenyl is optionally substituted by a group selected from halo, methyl, methoxy; pyridyl; and thiophenyl;and

 where R 24 is selected from: H; C 1-3 saturated alkyl; C 2-3 alkenyl; C 2-3 alkynyl; cyclopropyl; phenyl, which phenyl is optionally substituted by a group selected from halo, methyl, methoxy; pyridyl; and thiophenyl;

when there is a single bond present between C2′ and C3′,

R 12 is

 where R 26a and R 26b are independently selected from H, F, C 1-4 saturated alkyl, C 2-3 alkenyl, which alkyl and alkenyl groups are optionally substituted by a group selected from C 1-4 alkyl amido and C 1-4 alkyl ester; or, when one of R 26a and R 26b is H, the other is selected from nitrile and a C 1-4 alkyl ester;

R 6 and R 9 are independently selected from H, R, OH, OR, SH, SR, NH 2 , NHR, NRR′, nitro, Me 3 Sn and halo;

where R and R′ are independently selected from optionally substituted C 1-12 alkyl, C 3-20 heterocyclyl and C 5-20 aryl groups;

R 7 is selected from H, R, OH, OR, SH, SR, NH 2 , NHR, NHRR′, nitro, Me 3 Sn and halo;

either:

(a) R 10 is carbamate nitrogen protecting group, and R 11 is O-Prot O , wherein Prot O is an oxygen protecting group;

(b) R 10 is a hemi-aminal nitrogen protecting group and R 11 is an oxo group;

R″ is a C 3-12 alkylene group, which chain may be interrupted by one or more heteroatoms, and/or aromatic rings;

Y and Y′ are selected from O, S, or NH;

R 6′ , R 7′ , R 9′ are selected from the same groups as R 6 , R 7 and R 9 respectively and R 10′ and R 11′ are the same as R 10 and R 11 .

37. A compound according to any claim 36 , wherein R 7 is selected from H, OH and OR.

38. A compound according to claim 37 , wherein R 7 is a C 1-4 alkyloxy group.

39. A compound according to claim 3 , wherein Y is O.

40. A compound according to claim 36 , wherein R″ is C 3-7 alkylene.

41. A compound according to claim 36 , wherein R 9 is H.

42. A compound according to claim 36 , wherein R 6 is selected from H and halo.

43. A compound according to claim 36 , wherein Q is NHR N .

44. A compound according to claim 43 , wherein R N is H or methyl.

45. A compound according to claim 36 , wherein Q is OH or SH.

46. A compound according to claim 36 , wherein there is a double bond between C2′ and C3′, and R 12 is a C 5-7 aryl group.

47. A compound according to claim 46 , wherein R 12 is phenyl.

48. A compound according to claim 36 , wherein there is a double bond between C2′ and C3′, and R 12 is a C 8-10 aryl group.

49. A compound according to claim 46 , wherein R 12 bears one to three substituent groups.

50. A compound according to claim 36 , wherein there is a single bond between C2′ and C3′, R 12 is

and R 26a and R 26b are both H.

51. A compound according to claim 36 , wherein there is a single bond between C2′ and C3′, R 12 is

and R 26a and R 26b are both methyl.

52. A compound according to claim 36 , wherein there is a single bond between C2′ and C3′, R 12 is

one of R 26a and R 26b is H, and the other is selected from C 1-4 saturated alkyl, C 2-3 alkenyl, which alkyl and alkenyl groups are optionally substituted.

53. A compound according to claim 36 , wherein there is a double bond between C2′ and C3′, and R 12 is a C 1-5 saturated aliphatic alkyl group.

54. A compound according to claim 53 , wherein R 12 is methyl, ethyl or propyl.

55. A compound according to claim 36 , wherein there is a double bond between C2′ and C3′, and R 12 is a C 3-6 saturated cycloalkyl group.

56. A compound according to claim 55 , wherein R 12 is cyclopropyl.

57. A compound according to claim 36 , wherein there is a double bond between C2′ and C3′, and R 12 is a group of formula:

58. A compound according to claim 57 , wherein the total number of carbon atoms in the R 12 group is no more than 4.

59. A compound according to claim 58 , wherein the total number of carbon atoms in the R 12 group is no more than 3.

60. A compound according to claim 57 , wherein one of R 21 , R 22 and R 23 is H, with the other two groups being selected from H, C 1-3 saturated alkyl, C 2-3 alkenyl, C 2-3 alkynyl and cyclopropyl.

61. A compound according to claim 57 , wherein two of R 21 , R 22 and R 23 are H, with the other group being selected from H, C 1-3 saturated alkyl, C 2-3 alkenyl, C 2-3 alkynyl and cyclopropyl.

62. A compound according to claim 36 , wherein there is a double bond between C2′ and C3′, and R 12 is a group of formula:

63. A compound according to claim 62 , wherein R 12 is the group:

64. A compound according to claim 36 , wherein there is a double bond between C2′ and C3′, and R 12 is a group of formula:

65. A compound according to claim 64 wherein R 24 is selected from H, methyl, ethyl, ethenyl and ethynyl.

66. A compound according to claim 65 , wherein R 24 is selected from H and methyl.

67. A compound according to claim 36 , wherein R 10 is Troc.

68. A compound according to claim 36 , wherein R 11 is OTBS.

69. A compound according to claim 36 , wherein R 11 is oxo and R 10 is SEM.

70. A compound according to claim 36 , wherein R6′, R7′, R9′, R 10′ , R 11′ and Y′ are the same as R 6 , R 7 , R 9 ,R 10 , R 11 and Y respectively.

71. A Conjugate having formula III:

L-(LU-D) p   (I)

wherein L is a Ligand unit which is a cell binding agent that specifically binds to a target molecule on the surface of a target cell, LU is a Linker unit of formula -A 1 -L 1 -, wherein L 1 is a dipeptide and A 1 is selected from:

where the asterisk indicates the point of attachment to L 1 , the wavy line indicates the point of attachment to the Ligand unit, and n is 0 to 6;

where the asterisk indicates the point of attachment to L 1 , the wavy line indicates the point of attachment to the Ligand unit, and n is 0 to 6;

where the asterisk indicates the point of attachment to L 1 , the wavy line indicates the point of attachment to the Ligand unit, n is 0 or 1 and m is 0 to 30; or

where the asterisk indicates the point of attachment to L 1 , the wavy line indicates the point of attachment to the Ligand unit, n is 0 or 1 and m is 0 to 30,

p is 1 to 20; and

D is a Drug unit which is a compound with the formula I:

wherein:

R 2 is of formula II:

where Q is selected from —O—, —S— and —NR N and R N is selected from H, methyl and ethyl;

when there is a double bond present between C2′ and C3′, R 12 is selected from:

(ia) C 5-10 aryl group optionally substituted by one or more substituents selected from the group comprising: halo, nitro, cyano, ether, C 1-7 alkyl C 3-7 heterocyclyl and bis-oxy-C 1-3 alkylene;

(ib) C 1-5 saturated aliphatic alkyl;

(ic) C 3-6 saturated cycloalkyl;

 wherein each of R 21 , R 22 and R 23 are independently selected from H, C 1-3 saturated alkyl C 2-3 alkenyl and cyclopropyl, where the total number of carbon atoms in the R 12 group is no more than 5;

 wherein one of R 25a and R 25b is H and the other is selected from: phenyl; which phenyl is optionally substituted by a group selected from halo, methyl, methoxy; pyridyl; and thiophenyl; and

 where R 24 is selected from: H; C 1-3 saturated alkyl; C 2-3 alkenyl; C 2-3 alkynyl; cyclopropyl; phenyl, which phenyl is optionally substituted by a group selected from halo, methyl, methoxy; pyridyl; and thiophenyl;

when there is a single bond present between C2′ and C3′,

R 12 is

 where R 26a and R 26b are independently selected from H, F, C 1-4 saturated alkyl, C 2-3 alkenyl, which alkyl and alkenyl groups are optionally substituted by a group selected from C 1-4 alkyl amido and C 1-4 alkyl ester; or, when one of R 26a and R 26b is H, the other is selected from nitrile and a C 1-4 alkyl ester;

R 6 and R 9 are independently selected from H, R, OH ,OR SH, SR, NH 2 NHR, NRR′ nitro, Me 3 Sn and halo;

where R and R′ are independently selected from optionally substituted C 1-12 alkyl, C 3-20 heterocyclyl and C 5-20 aryl groups;

R 7 is selected from H, R, OH, OR, SH, SR, NH 2 , NHR, NHRR′, nitro, Me 3 Sn and halo;

either:

(a) R 10 is H, and R 11 is OH, OR A , where R A is C 1-4 alkyl;

(b) R 10 and R 11 form a nitrogen-carbon double bond between the nitrogen and carbon atoms to which they are bound; or

(c) R 10 is H and R 11 is SO z M, where z is 2 or 3 and M is a monovalent pharmaceutically acceptable cation;

R″ is a C 3-12 alkylene group which chain may be interrupted by one or more heteroatoms and/or aromatic rings;

Y and Y′ are selected from O, S, or NH;

R 6′ , R 7′ , R 9′ are selected from the same groups as R 6 , R 7 and R 9 respectively and R 10′ and R 11′ are the same as R 10 and R 11 wherein if R 11 and R 11′ are SO z M, M may represent a divalent pharmaceutically acceptable cation,

wherein LU is connected to D via the Q substituent of R 2 .

72. The Conjugate of claim 71 , wherein A 1 is

where the asterisk indicates the point of attachment to L 1 , the wavy line indicates the point of attachment to the Ligand unit, n is 0 or 1 and m is 0 to 30.

73. The Conjugate of claim 71 , wherein A 1 is:

where the asterisk indicates the point of attachment to L 1 , the wavy line indicates the point of attachment to the Ligand unit, and n is 0 to 6.

74. The Conjugate of claim 73 , wherein n is 5.

75. The Conjugate of claim 71 , wherein L 1 is selected from the group consisting of valine-alanine, valine-citrulline and phenyalanine-lysine.

76. A method of treating a mammal having a proliferative disease or an autoimmune disease, comprising administering an effective amount of the Conjugate of claim 71 .

Assignments (5)
CORRECTIVE ASSIGNMENT TO CORRECT THE POSTAL CODE OF THE ASSIGNEE PREVIOUSLY RECORDED AT REEL: 036932 FRAME: 0278. ASSIGNOR(S) HEREBY CONFIRMS THE ASSIGNMENT . Recorded Apr 11, 2017
From: SPIROGEN SÀRL
To: MEDIMMUNE LIMITED
Reel/Frame 042242/0389 →
CONFIRMATORY ASSIGNMENT Recorded Oct 23, 2015
From: SPIROGEN SÀRL
To: MEDIMMUNE LIMITED
Reel/Frame 036932/0278 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Apr 23, 2014
From: HOWARD, PHILIP WILSON
To: SPIROGEN LIMITED
Reel/Frame 032737/0317 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Apr 23, 2014
From: SPIROGEN LIMITED
To: SPIROGEN DEVELOPMENTS SARL
Reel/Frame 032737/0433 →
MERGER Recorded Apr 23, 2014
From: SPIROGEN DEVELOPMENTS SARL
To: SPIROGEN SARL
Reel/Frame 032743/0340 →