IP Library Granted Patent US 10,647,709
Granted Patent B2
US 10,647,709 · App. 15/192,113 · Granted May 12, 2020

Cysteine protease inhibitors and uses thereof

Inventors: Gregory R. J. Thatcher (Chicago, IL); Isaac Thomas Schiefer (Chicago, IL); Ottavio Arancio (New York, NY); Mauro Fa (New York, NY)
Assignees: THE TRUSTEES OF COLUMBIA UNIVERSITY IN THE CITY OF NEW YORK; THE BOARD OF TRUSTEES OF THE UNIVERSITY OF ILLINOIS
C07D417/12C07D303/48C07D403/12C07D405/12C07D409/12C07D417/14C07D495/04
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Quick Facts
Patent No.
US 10,647,709
App. No.
15/192,113
Granted
May 12, 2020
Kind
B2
Abstract

The invention provides for novel cysteine protease inhibitors and compositions comprising novel cysteine protease derivatives. The invention further provides for methods for treatment of neurodegenerative diseases comprising administration novel cysteine protease inhibitors or compositions comprising novel cysteine protease inhibitors. In some embodiments, the cysteine protease inhibitors are calpain inhibitors.

Claims (137)

1. A method of treating Alzheimer's disease in a subject in need thereof comprising administration of a therapeutically effective amount of a compound having a structure of formula (I-a):

wherein,

R 1 is CO 2 H or —CO 2 (C 1 -C 4 )-alkyl;

R 2 is hydrogen or —(C 1 -C 4 )-alkyl;

R 4 is —(CH 2 )-thiazolyl;

R 5 is —(C 1 -C 6 )-alkyl-R 6 , —(C 2 -C 5 )-alkenyl, —(C 2 -C 5 )-alkynyl, —(CH 2 ) n -aryl, or

—(CH 2 ) n -heteroaryl, wherein said aryl or heteroaryl are substituted with one or more R 7 groups;

R 6 is —N(R 10 )C(O)R 8 or —N(R 10 )S(O) 2 R 8 ;

R 7 is independently halogen, —(C 1 -C 3 )-alkyl, aryl, methylenedioxyphenyl, or —S(O) 2 N(R 10 ) 2 , wherein said aryl is optionally substituted with one or more R 9 groups;

R 8 is-(C 1 -C 6 )-alkyl-R 11 or aryl, wherein aryl is optionally substituted with one or more R 9 groups;

R 9 is independently hydrogen, halogen, —(C 1 -C 4 )-alkyl, —(C 1 -C 4 )-haloalkyl, —(C 2 -C 4 )-alkynyl, CN, NO 2 , —S(O) 2 N(R 10 ) 2 , or

R 10 is independently hydrogen or —(C 1 -C 4 )-alkyl;

R 11 is hydrogen of

n is an integer from 0-4; and

p is an integer from 0-3.

2. A method of increasing long-term potentiation in a subject comprising administration of a therapeutically effective amount of a compound having a structure of formula (I-a),

wherein,

R 1 is CO 2 H or —CO 2 (C 1 -C 4 )-alkyl;

R 2 is hydrogen or —(C 1 -C 4 )-alkyl;

R 4 is —(CH 2 )-thiazolyl;

R 5 is-(C 1 -C 6 )-alkyl-R 6 , —(C 2 -C 5 )-alkenyl, —(C 2 -C 5 )-alkynyl, —(CH 2 ) n -aryl, or

(CH 2 ) n -heteroaryl, wherein said aryl or heteroaryl are substituted with one or more R 7 groups;

R 6 is —N(R 10 )C(O)R 8 or —N(R 10 )S(O) 1 R 8 ;

R 7 is independently halogen, —(C 1 -C 3 )-alkyl, aryl, methylenedioxyphenyl, or —S(O) 2 N(R 10 ) 2 , wherein said aryl is optionally substituted with one or more R 9 groups;

R 8 is-(C 1 -C 6 )-alkyl-R 11 or aryl, wherein aryl is optionally substituted with one or more R 9 groups;

R 9 is independently hydrogen, halogen, —(C 1 -C 4 )-alkyl, —(C 1 -C 4 )-haloalkyl, —(C 2 -C 4 )-alkynyl, CN, NO 2 , —S(O) 2 N(R 10 ) 2 , or

R 10 is independently hydrogen or —(C 1 -C 4 )-alkyl;

R 11 is hydrogen or

n is an integer from 0-4; and

p is an integer from 0-3.

3. A method of improving memory in a subject comprising administration of a therapeutically effective amount of a compound having a structure of formula (I-a),

wherein,

R 1 is CO 2 H or —CO 2 (C 1 -C 4 )-alkyl;

R 2 is hydrogen or —(C 1 -C 4 )-alkyl;

R 4 is —(CH 2 )-thiazolyl;

R 5 is-(C 1 -C 6 )-alkyl-R 6 , —(C 2 -C 5 )-alkenyl, —(C 2 -C 5 )-alkynyl, —(CH 2 ) n -aryl, or

(CH 2 ) n -heteroaryl, wherein said aryl or heteroaryl are substituted with one or more R 7 groups;

R 6 is —N(R 10 )C(O)R 8 or)-N(R 10 )S(O) 2 R 8 ;

R 7 is independently halogen, —(C 1 -C 3 )-alkyl, aryl, methylenedioxyphenyl, or —S(O) 2 N(R 10 ) 2 , wherein said aryl is optionally substituted with one or more R 9 groups;

R 8 is-(C 1 -C 6 )-alkyl-R 11 or aryl, wherein aryl is optionally substituted with one or more R 9 groups;

R 9 is independently hydrogen, halogen, —(C 1 -C 4 )-alkyl, —(C 1 -C 4 )-haloalkyl, —(C 2 -C 4 )-alkynyl, CN, NO 2 ,—S(O) 2 N(R 10 ) 2 , or

R 10 is independently hydrogen or —(C 1 -C 4 )-alkyl;

R 11 is hydrogen or

n is an integer from 0-4; and

p is an integer from 0-3.

4. The method of claim 3 , wherein the subject has Alzheimer's Disease.

5. The method of claim 1 , wherein the compound is formulated as a pharmaceutical composition.

6. The method of claim 5 , wherein the pharmaceutical composition is formulated: as a sterile injectable solution or dispersion, for intravenous or oral administration, or for transmucosal or transdermal administration.

7. The method of claim 1 , wherein

(a) R 1 is —CO 2 H or —CO 1 (C 1 -C 2 )-alkyl;

R 2 is hydrogen or —(C 1 -C 2 )-alkyl;

R 5 is —(CH 2 ) n -phenyl, or —(CH 2 ) n -heteroaryl, wherein said phenyl or heteroaryl are substituted with one or more R 7 groups;

R 7 is independently halogen, —(C 1 -C 3 )-alkyl, phenyl, methylenedioxyphenyl, or —S(O) 2 N(R 10 ) 2 , wherein said phenyl is optionally substituted with one or more R 9 groups;

R 9 is independently hydrogen, halogen, —(C 1 -C 2 )-alkyl, —(C 1 -C 2 )-haloalkyl, —(C 2 -C 4 )-alkynyl, CN, NO 2 , —S(O) 2 N(R 10 ) 2 , or

R 10 is independently hydrogen or —(C 1 -C 2 )-alkyl;

n is an integer from 0-2; and

p is an integer from 0-1;

(b) R 1 is —CO 2 H or —CO 2 (C 1 -C 2 )-alkyl;

R 2 is hydrogen or —(C 1 -C 2 )-alkyl;

R 5 is —(CH 2 )-triazolyl, wherein said triazolyl is substituted with an R 7 group;

R 7 is phenyl optionally substituted with one or more R 9 groups;

R 9 is independently halogen, —(C 1 -C 2 )-alkyl, —(C 1 -C 2 )-haloalkyl, —(C 2 -C 4 )-alkynyl, CN, NO 2 , —S(O) 2 N(R 10 ) 2 , or

R 10 is independently hydrogen or —(C 1 -C 2 )-alkyl;

and

p is an integer from 0-1;

(c) R 1 is —CO 2 H or —CO 2 (C 1 -C 2 )-alkyl;

R 2 is hydrogen or —(C 1 -C 2 )-alkyl;

R 5 is —(CH 2 )-triazolyl, wherein said triazolyl is substituted with an R 7 group;

R 7 is phenyl optionally substituted with one or more R 9 groups;

R 9 is independently halogen, —(C 1 -C 2 )-alkyl, —(C 1 -C 2 )-haloalkyl, —(C 2 -C 4 )-alkynyl, CN, NO 2 , —S(O) 2 N(R 10 ) 2 , or

R 10 is independently hydrogen or methyl; and

p is an integer from 0-1; or

(d) R 1 is —CO 2 H or —CO 2 (C 1 -C 2 )-alkyl;

R 2 is hydrogen;

R 5 is

R 7 is phenyl optionally substituted with one or more R 9 groups;

R 9 is independently halogen, —(C 1 -C 2 )-alkyl, —(C 1 -C 2 )-haloalkyl, —(C 2 -C 3 )-alkynyl, NO 2 , —S(O) 2 NH 2 , or

and

p is an integer from 0-1.

8. The method of claim 1 , wherein the compound is:

(2S,3S)-3-((S)-1-(4-(4-fluorophenyl)thiazol-2-ylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid;

(2S,3S)-3-((S)-1-(4-(4-ethynylphenyl)thiazol-2-ylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid;

(2S,3S)-3-((S)-1-((1-(4-fluorophenyl)-1H-1,2,3-triazol-4-yl)methylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid; or

(2S,3S)-3-((S)-1-((1-(4-bromophenyl)-1H-1,2,3-triazol-4-yl)methylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid.

9. The method of claim 2 , wherein the compound is:

(2S,3S)-3-((S)-1-(4-(4-fluorophenyl)thiazol-2-ylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid;

(2S,3S)-3-((S)-1-(4-(4-ethynylphenyl)thiazol-2-ylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid;

(2S,3S)-3-((S)-1-((1-(4-fluorophenyl)-1H-1,2,3-triazol-4-yl)methylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid; or

(2S,3S)-3-((S)-1-((1-(4-bromophenyl)-1H-1,2,3-triazol-4-yl)methylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid.

10. The method of claim 3 , wherein the compound is:

(2S,3S)-3-((S)-1-(4-(4-fluorophenyl)thiazol-2-ylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid;

(2S,3S)-3-((S)-1-(4-(4-ethynylphenyl)thiazol-2-ylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid;

(2S,3S)-3-((S)-1-((1-(4-fluorophenyl)-1H-1,2,3-triazol-4-yl)methylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid; or

(2S,3S)-3-((S)-1-((1-(4-bromophenyl)-1H-1,2,3-triazol-4-yl)methylamino)-1-oxo-3-(thiazol-4-yl)propan-2-ylcarbamoyl)oxirane-2-carboxylic acid.

11. The method of claim 2 , wherein the compound is formulated as a pharmaceutical composition.

12. The method of claim 11 , wherein the pharmaceutical composition is formulated: as a sterile injectable solution or dispersion, for intravenous or oral administration, or for transmucosal or transdermal administration.

13. The method of claim 3 , wherein the compound is formulated as a pharmaceutical composition.

14. The method of claim 13 , wherein the pharmaceutical composition is formulated: as a sterile injectable solution or dispersion, for intravenous or oral administration, or for transmucosal or transdermal administration.

15. The method of claim 1 , wherein

R 1 is —CO 2 H or —CO 2 (C 1 -C 4 )-alkyl;

R 2 is hydrogen or —(C 1 -C 4 )-alkyl;

R 4 is

R 5 is-(C 1 -C 4 )-alkyl-R 6 , —(CH 2 ) n -aryl, or —(CH 2 ) n -heteroaryl, wherein said aryl or heteroaryl are substituted with one or more R 7 groups;

R 6 is —N(R 10 )C(O)R 8 or —N(R 10 )S(O) 2 R 8 ;

R 7 is independently halogen, —(C 1 -C 3 )-alkyl, aryl, methylenedioxyphenyl, or —S(O) 2 N(R 10 ) 2 , wherein said aryl is optionally substituted with one or more R 9 groups;

R 8 is-(C 1 -C 6 )-alkyl-R 11 or aryl, wherein aryl is optionally substituted with one or more R 9 groups;

R 9 is independently hydrogen, halogen, —(C 1 -C 2 )-alkyl, —(C 1 -C 2 )-haloalkyl, —(C 2 -C 4 )-alkynyl, CN, NO 2 , —S(O) 2 N(R 10 ) 2 , or

R 10 is independently hydrogen or —(C 1 -C 4 )-alkyl;

R 11 is hydrogen or

n is an integer from 0-2; and

p is an integer from 0-1.

16. The method of claim 2 , wherein

R 1 is —CO 2 H or —CO 2 (C 1 -C 4 )-alkyl;

R 2 is hydrogen or —(C 1 -C 4 )-alkyl;

R 4 is

R 5 is-(C 1 -C 4 )-alkyl-R 6 , —(CH 2 ) n -aryl, or —(CH 2 ) n -heteroaryl, wherein said aryl or heteroaryl are substituted with one or more R 7 groups;

R 6 is —N(R 10 )C(O)R 8 or —N(R 10 )S(O) 2 R 8 ;

R 7 is independently halogen, —(C 1 -C 3 )-alkyl, aryl, methylenedioxyphenyl, or —S(O) 2 N(R 10 ) 2 , wherein said aryl is optionally substituted with one or more R 9 groups;

R 8 is-(C 1 -C 6 )-alkyl-R 11 or aryl, wherein aryl is optionally substituted with one or more R 9 groups;

R 9 is independently hydrogen, halogen, —(C 1 -C 2 )-alkyl, —(C 1 -C 2 )-haloalkyl, —(C 2 -C 4 )-alkynyl, CN, NO 2 , —S(O) 2 N(R 10 ) 2 , or

R 10 is independently hydrogen or —(C 1 -C 4 )-alkyl;

R 11 is hydrogen or

n is an integer from 0-2; and

p is an integer from 0-1.

17. The method of claim 3 , wherein

R 1 is —CO 2 H or —CO 2 (C 1 -C 4 )-alkyl;

R 2 is hydrogen or —(C 1 -C 4 )-alkyl;

R 4 is

R 5 is-(C 1 -C 4 )-alkyl-R 6 , —(CH 2 ) n -aryl, or —(CH 2 ) n -heteroaryl, wherein said aryl or heteroaryl are substituted with one or more R 7 groups;

R 6 is —N(R 10 )C(O)R 8 or —N(R 10 )S(O) 2 R 8 ;

R 7 is independently halogen, —(C 1 -C 3 )-alkyl, aryl, methylenedioxyphenyl, or —S(O) 2 N(R 10 ) 2 , wherein said aryl is optionally substituted with one or more R 9 groups;

R 8 is-(C 1 -C 6 )-alkyl-R 11 or aryl, wherein aryl is optionally substituted with one or more R 9 groups;

R 9 is independently hydrogen, halogen, —(C 1 -C 2 )-alkyl, —(C 1 -C 2 )-haloalkyl, —(C 2 -C 4 )-alkynyl, CN, NO 2 , —S(O) 2 N(R 10 ) 2 , or

R 10 is independently hydrogen or —(C 1 -C 4 )-alkyl;

R 11 is hydrogen or

n is an integer from 0-2; and

p is an integer from 0-1.

Assignments (3)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Sep 22, 2016
From: ARANCIO, OTTAVIO; FA, MAURO
To: THE TRUSTEES OF COLUMBIA UNIVERSITY IN THE CITY OF NEW YORK
Reel/Frame 039830/0852 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Sep 22, 2016
From: SCHIEFER, ISAAC THOMAS; THATCHER, GREGORY R.J.
To: THE BOARD OF TRUSTEES OF THE UNIVERSITY OF ILLINOIS
Reel/Frame 039831/0422 →
CONFIRMATORY LICENSE Recorded Aug 13, 2016
From: COLUMBIA UNIV NEW YORK MORNINGSIDE
To: NATIONAL INSTITUTES OF HEALTH (NIH), U.S. DEPT. OF HEALTH AND HUMAN SERVICES (DHHS), U.S. GOVERNMENT
Reel/Frame 039671/0880 →
Continuity (3)
Continuation 14376361
Provisional Application 61593664 · Feb 1, 2012
Related Publication 20170008884A1 · Jan 12, 2017