IP Library Granted Patent US 8,748,625
Granted Patent B2
US 8,748,625 · App. 13/764,807 · Granted Jun 10, 2014

Crystalline forms of 3-[5-(2-fluorophenyl)-[1,2,4]oxadiazol-3-yl]-benzoic acid

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Quick Facts
Patent No.
US 8,748,625
App. No.
13/764,807
Granted
Jun 10, 2014
Kind
B2
Abstract

The present invention relates to crystalline forms of 3-[5-(2-fluorophenyl)-[1,2,4]oxadiazol-3-yl]-benzoic acid, pharmaceutical compositions and dosage forms comprising the crystalline forms, methods of making the crystalline forms and methods for their use for the treatment, prevention or management of diseases ameliorated by modulation of premature translation termination or nonsense-mediated mRNA decay.

Claims (842)

1. A process for preparing an anhydrous crystal form of 3-[5-(2-fluorophenyl)-[1,2,4]oxadiazol-3-yl]-benzoic acid comprising Form A crystals characterized by at least one of the following:

(a) unit cell parameters when measured at 150 K: a=24,220 Å; b=3,74640 Å; c=27,4678 Å; α=90°; β=92,9938°; γ=90°; V=2489,38(17) Å 3 ; Z=8; calculated density (d calc, g cm −3 ) is 1,517 g cm −3 ; and the space group is P2 1 /n (no. 14);

(b) an X-ray powder diffraction pattern comprising at least three peak positions (°2θ±0.2), when measured using Cu Kα radiation, selected from the group consisting of:

4.96

6.39

10.10

11.54

12.62

12.81

13.92

14.16

14.55

14.88

15.07

15.58

16.27

16.61

18.74

18.94

19.28

19.94

20.27

20.74

20.97

21.22

21.93

22.58

22.80

23.00

23.79

24.14

24.46

25.44

25.64

26.07

26.34

26.74

27.06

27.79

28.42

29.09

30.48

(c) a thermogravimetric analysis thermogram which has a mass loss of less than 1% of the total mass of the sample upon heating from 33° C. to 205° C.;

(d) a differential scanning calorimetry thermogram which has an endothermic event with a peak temperature at 244° C.; and

(e) fractional atomic coordinates equal to the following coordinates:

Átom

x

y

z

U(Å 2 )

F(122)

0.43198(12)

0.7655(8)

−0.17546(10)

0.0487(10)

F(222)

−0.20343(15)

0.7129(10)

0.06378(14)

0.0781(14)

O(13)

0.42977(13)

0.4875(8)

−0.08927(11)

0.0324(10)

O(23)

−0.12941(13)

0.4507(9)

0.12653(12)

0.0402(10)

O(151)

0.25519(13)

0.4795(9)

0.10765(12)

0.0382(10)

O(152)

0.29215(13)

0.2155(9)

0.17515(12)

0.0403(10)

O(251)

0.16226(13)

0.4813(9)

0.15012(12)

0.0385(10)

O(252)

0.19645(13)

0.1939(9)

0.21659(12)

0.0393(10)

N(11)

0.35817(15)

0.5856(9)

−0.04386(14)

0.0279(10)

N(14)

0.44373(16)

0.3409(10)

−0.04263(14)

0.0327(12)

N(21)

−0.04134(16)

0.5165(9)

0.11065(14)

0.0305(12)

N(24)

−0.09772(17)

0.3201(11)

0.16787(15)

0.0388(14)

C(12)

0.37827(18)

0.6256(11)

−0.08637(17)

0.0266(14)

C(15)

0.40019(19)

0.4091(11)

−0.01823(17)

0.0261(14)

C(22)

−0.0926(2)

0.5601(12)

0.09502(18)

0.0319(15)

C(25)

−0.0471(2)

0.3690(11)

0.15580(17)

0.0302(15)

C(121)

0.35225(19)

0.7961(11)

−0.12930(17)

0.0291(14)

C(122)

0.3784(2)

0.8567(12)

−0.17244(18)

0.0345(15)

C(123)

0.3519(2)

1.0117(12)

−0.21257(19)

0.0407(17)

C(124)

0.2973(2)

1.1101(13)

−0.21014(19)

0.0416(17)

C(125)

0.2694(2)

1.0543(12)

−0.1677(2)

0.0409(17)

C(126)

0.2966(2)

0.8996(12)

−0.12784(18)

0.0349(15)

C(151)

0.39702(19)

0.3013(11)

0.03319(16)

0.0260(14)

C(152)

0.34897(19)

0.3623(11)

0.05704(16)

0.0261(15)

C(153)

0.34631(18)

0.2594(11)

0.10554(16)

0.0253(14)

C(154)

0.39150(19)

0.0970(11)

0.13029(17)

0.0279(14)

C(155)

0.43977(19)

0.0412(11)

0.10614(17)

0.0291(15)

C(156)

0.44250(19)

0.1421(11)

0.05765(17)

0.0292(15)

C(157)

0.2955(2)

0.3188(12)

0.13209(18)

0.0312(15)

C(221)

−0.1109(2)

0.7083(12)

0.04727(19)

0.0388(17)

C(222)

−0.1643(3)

0.7823(15)

0.0331(2)

0.053(2)

C(223)

−0.1825(3)

0.9272(15)

−0.0122(3)

0.064(2)

C(224)

−0.1415(4)

0.9930(16)

−0.0433(3)

0.068(3)

C(225)

−0.0870(3)

0.9202(15)

−0.0316(2)

0.066(2)

C(226)

−0.0678(3)

0.7766(12)

0.01365(17)

0.0543(19)

C(251)

0.00110(19)

0.2695(11)

0.18877(17)

0.0300(15)

C(252)

0.05426(19)

0.3352(11)

0.17481(17)

0.0289(15)

C(253)

0.09949(19)

0.2449(11)

0.20524(17)

0.0277(15)

C(254)

0.0919(2)

0.0940(11)

0.25087(17)

0.0296(15)

C(255)

0.0389(2)

0.0335(11)

0.26491(17)

0.0300(15)

C(256)

−0.0064(2)

0.1185(12)

0.23430(17)

0.0322(15)

C(257)

0.1559(2)

0.3165(12)

0.18902(17)

0.0305(15)

H(123)

0.371

1.050

−0.241

0.048

H(124)

0.278

1.217

−0.238

0.050

H(125)

0.232

1.123

−0.166

0.049

H(126)

0.278

0.862

−0.099

0.042

H(151)

0.227

0.491

0.125

0.057

H(152)

0.318

0.473

0.041

0.031

H(154)

0.389

0.025

0.163

0.033

H(155)

0.471

−0.066

0.123

0.035

H(156)

0.475

0.103

0.041

0.035

H(223)

−0.220

0.975

−0.020

0.077

H(224)

−0.151

1.094

−0.074

0.082

H(225)

−0.061

0.969

−0.055

0.080

H(226)

−0.030

0.729

0.021

0.065

H(252)

0.226

0.213

0.202

0.059

H(254)

0.123

0.034

0.272

0.035

H(255)

0.033

−0.068

0.296

0.036

H(256)

−0.043

0.074

0.244

0.039

H(25A)

0.060

0.443

0.144

0.035

(f) an X-ray powder diffraction pattern comprising at least three peak positions (°2θ±0.2), when calculated from single crystal data, selected from the group consisting of:

4.74

4.99

6.44

7.30

10.15

10.51

11.27

11.59

12.90

14.25

14.50

14.64

15.17

15.69

16.31

16.37

16.74

18.44

18.78

19.04

19.07

19.40

20.03

20.06

20.30

20.39

21.11

21.20

22.03

22.64

23.16

23.86

23.95

24.21

24.27

24.61

24.84

24.86

24.94

25.00

25.02

25.13

25.61

25.79

25.87

26.02

26.20

26.48

26.87

26.87

27.08

27.10

27.16

27.26

27.45

27.92

28.05

28.20

28.28

28.53

28.83

28.93

28.96

29.05

29.18

29.24

29.42

29.52

29.57

29.94

30.00

30.43

30.58

30.79

30.93

31.07

31.18

31.42

31.97

32.46

32.65

32.88

33.13

33.17

33.40

33.64

33.90

34.25

34.74

35.18

35.59

35.96

36.64

wherein the process comprises:

(1) subliming or heating a Form A crystal or crystallizing Form A from a solvent; or

(2) exposing a Form B crystal to a relative humidity of 79% at 60° C. to convert Form B to Form A; or

(3) milling a Form B crystal at ambient or sub-ambient temperature to convert Form B to Form A; or

(4) slurrying a Form B crystal in methyl isobutyl ketone, or a 1:1 mixture of dioxane and water to convert Form B to Form A; or

(5) subliming or heating a Form B crystal to convert Form B to Form A,

wherein the Form B crystal is characterized by one or more X-ray powder diffraction patterns selected from an X-ray powder diffraction pattern comprising at least three peak positions (° 2±0.2), when measured using Cu Kα radiation, selected from the group consisting of:

6.14

6.39

6.96

7.92

10.78

12.44

12.61

12.88

13.52

13.78

13.97

14.30

15.46

15.68

15.89

16.33

16.76

17.03

20.10

21.03

23.34

23.86

24.18

24.42

24.64

26.62

26.96

27.29

27.64

27.96

28.81

31.05

32.38

32.58

36.23

37.81

38.28

38.44

39.16;

wherein the Form B crystal is characterized by an X-ray powder diffraction pattern comprising at least three peak positions (° 2θ±0.2), when measured using Cu Kα radiation, selected from the group consisting of:

6.42

7.00

7.89

10.85

12.61

12.92

13.47

13.97

15.81

16.45

17.12

20.05

21.05

23.92

24.28

27.00

27.39

27.84

28.04

28.94

31.10

32.58

36.11

37.71

38.15

38.61;

wherein the Form B crystal is characterized by an X-ray powder diffraction pattern comprising at least three peak positions (° 2θ±0.2), when measured using Cu Kα radiation, selected from the group consisting of:

6.10

6.38

6.54

7.10

8.02

10.91

12.71

13.50

13.62

13.86

14.10

15.56

15.70

15.91

16.55

16.96

17.22

17.50

19.82

20.08

20.34

21.15

23.78

23.93

24.38

24.56

26.88

27.16

27.48

27.88

28.04

28.78

29.02

32.71

36.01

38.10

38.56

39.38;

wherein the Form B crystal is characterized by an X-ray powder diffraction pattern comprising at least three peak positions (° 2θ±0.2), when measured using Cu Kα radiation, selected from the group consisting of:

1.79

2.30

2.57

2.78

3.29

3.59

3.89

4.07

4.34

4.49

4.76

5.06

6.47

6.91

7.96

10.89

12.87

13.58

13.99

15.97

16.48

17.10

20.00

20.36

21.04

23.40

24.29

24.89

26.87

27.49

27.80

28.07

29.08

38.61;

wherein the Form B crystal is characterized by an X-ray powder diffraction pattern comprising at least three peak positions (° 2θ±0.2), when measured using Cu Kα radiation, selected from the group consisting of:

 6.22

 6.51

 7.13

 8.17

10.91

12.87

13.80

14.12

14.28

15.78

16.23

16.54

17.15

20.33

21.22

21.36

23.94

24.30

27.30

27.58

28.00

28.74

28.96

32.70

36.74

38.18

38.38

38.52

39.31; or

wherein the Form B crystal is characterized by an X-ray powder diffraction pattern comprising at least three peak positions (° 2θ±0.2), when measured using Cu Kα radiation, selected from the group consisting of:

6.04

6.49

7.91

10.92

12.61

12.92

13.10

13.42

13.82

13.99

15.40

15.76

16.51

17.15

19.92

20.04

21.01

23.92

24.28

24.48

26.77

27.14

27.40

27.74

28.09

28.82

28.99

31.03

32.58

35.64

35.85

37.48

37.66

38.62.

2. The process of claim 1 , wherein crystallizing Form A from a solvent comprises:

(a) crystallizing Form A from methanol, t-butanol, 1-butanol, acetonitrile, isopropyl alcohol (IPA), isopropyl ether, dimethyl formamide, heptane, isopropyl acetate, toluene or water;

(b) crystallizing Form A by slow evaporation from acetonitrile; t-butanol; isopropyl alcohol; or isopropyl ether; or

(c) crystallizing Form A by fast evaporation from 1-butanol; dimethoxyether; t-butanol; a mixture of dimethyl formamide and water; isopropyl ether; or a mixture of t-butanol:water (in a 3:2 ratio), 1 molar equivalent methanol and 1 molar equivalent sodium chloride.

3. The Form A crystal form produced by the process of claim 1 , wherein said crystal form is physically stable: (1) when stored for six days at one or more of the following relative humidity conditions: 53% relative humidity at 40° C.; 75% relative humidity at 40° C.; 50% relative humidity at 60° C. or 79% relative humidity at 60° C., (2) when milled at ambient and at sub-ambient temperatures, or (3) when slurried at one or more of the following conditions: in 1-BuOH for four days at ambient temperature, in chloroform for two days at 50° C. or in dichloromethane for two days at 50° C.

4. The Form A crystal form produced by the process of claim 2 , wherein said crystal form is physically stable: (1) when stored for six days at one or more of the following relative humidity conditions: 53% relative humidity at 40° C.; 75% relative humidity at 40° C.; 50% relative humidity at 60° C. or 79% relative humidity at 60° C., (2) when milled at ambient and at sub-ambient temperatures, or (3) when slurried at one or more of the following conditions: in 1-BuOH for four days at ambient temperature, in chloroform for two days at 50° C. or in dichloromethane for two days at 50° C.

5. The process of claim 1 , further comprising a process for preparing a crystal form of 3-[5-(2-fluorophenyl)-[1,2,4]oxadiazol-3-yl]-benzoic acid comprising Form B crystals characterized by at least one of the following:

(a) an X-ray powder diffraction pattern comprising at least three peak positions (° 2θ±0.2), when measured using Cu Kα radiation, selected from the group consisting of:

6.14

6.39

6.96

7.92

10.78

12.44

12.61

12.88

13.52

13.78

13.97

14.30

15.46

15.68

15.89

16.33

16.76

17.03

20.10

21.03

23.34

23.86

24.18

24.42

24.64

26.62

26.96

27.29

27.64

27.96

28.81

31.05

32.38

32.58

36.23

37.81

38.28

38.44

39.16

(b) a thermogravimetric analysis thermogram which has a mass loss of less than 5% of the total mass of the sample upon heating from 25° C. to 165° C.; and

(c) a differential scanning calorimetry thermogram which has an endothermic event with a peak temperature at 243° C.,

wherein the process comprises heating Form A in 1-propanol to obtain the crystal Form B.

6. The crystal Form B produced by the process of claim 5 , wherein said crystal form is physically stable: (1) upon storage for six days at one or more of the following relative humidity conditions: 53% relative humidity at 40° C., 75% relative humidity at 40° C. or 50% relative humidity at 60° C., (2) when under compression alone, (3) when under compression in the presence of a 1:1 mixture of t-BuOH and water, or (4) when slurried for 1 day at ambient temperature in THF:heptane (1:1).

7. The process of claim 1 , further comprising a process for preparing a crystal form of 3-[5-(2-fluorophenyl)-[1,2,4]oxadiazol-3-yl]-benzoic acid comprising Form B crystals characterized by an X-ray powder diffraction pattern comprising at least three peak positions (° 2θ±0.2) (shifted 1), when measured using Cu Kα radiation, selected from the group consisting of:

6.42

7.00

7.89

10.85

12.61

12.92

13.47

13.97

15.81

16.45

17.12

20.05

21.05

23.92

24.28

27.00

27.39

27.84

28.04

28.94

31.10

32.58

36.11

37.71

38.15

38.61

wherein the process comprises slurrying Form A in 1-butyl acetate to obtain the crystal Form B.

8. The process of claim 1 , further comprising a process for preparing a crystal form of 3-[5-(2-fluorophenyl)-[1,2,4]oxadiazol-3-yl]-benzoic acid comprising Form B crystals characterized by an X-ray powder diffraction pattern comprising at least three peak positions (° 2θ±0.2) (shifted 2), when measured using Cu Kα radiation, selected from the group consisting of:

6.10

6.38

6.54

7.10

8.02

10.91

12.71

13.50

13.62

13.86

14.10

15.56

15.70

15.91

16.55

16.96

17.22

17.50

19.82

20.08

20.34

21.15

23.78

23.93

24.38

24.56

26.88

27.16

27.48

27.88

28.04

28.78

29.02

32.71

36.01

38.10

38.56

39.38

wherein the process comprises slurrying a mixture of the crystal Form B and Form A in a 1:1 mixture of tetrahydrofuran:heptanes with heating to obtain the crystal Form B.

9. The process of claim 1 , further comprising a process for preparing a crystal form of 3-[5-(2-fluorophenyl)-[1,2,4]oxadiazol-3-yl]-benzoic acid comprising Form B crystals characterized by an X-ray powder diffraction pattern comprising at least three peak positions (° 2θ±0.2) (shifted 3), when measured using Cu Kα radiation, selected from the group consisting of:

1.79

2.30

2.57

2.78

3.29

3.59

3.89

4.07

4.34

4.49

4.76

5.06

6.47

6.91

7.96

10.89

12.87

13.58

13.99

15.97

16.48

17.10

20.00

20.36

21.04

23.40

24.29

24.89

26.87

27.49

27.80

28.07

29.08

38.61

wherein the process comprises storing the crystal Form B in 75% relative humidity at 40° C.

10. The process of claim 1 , further comprising a process for preparing a crystal form of 3-[5-(2-fluorophenyl)-[1,2,4]oxadiazol-3-yl]-benzoic acid comprising Form B crystals characterized by an X-ray powder diffraction pattern comprising at least three peak positions (° 2θ±0.2) (shifted 3), when measured using Cu Kα radiation, selected from the group consisting of:

6.22

6.51

7.13

8.17

10.91

12.87

13.80

14.12

14.28

15.78

16.23

16.54

17.15

20.33

21.22

21.36

23.94

24.30

27.30

27.58

28.00

28.74

28.96

32.70

36.74

38.18

38.38

38.52

39.31

wherein the process comprises crystallizing the crystal form by slow evaporation from dimethoxyether to obtain the crystal Form B.

Assignments (6)
TERMINATION AND RELEASE OF PATENT SECURITY AGREEMENT @ REEL 061803 AND FRAME 0878 Recorded Oct 20, 2023
From: WILMINGTON TRUST, NATIONAL ASSOCIATION, AS ADMINISTRATIVE AGENT
To: PTC THERAPEUTICS, INC.
Reel/Frame 065303/0163 →
SECURITY INTEREST Recorded Oct 28, 2022
From: PTC THERAPEUTICS, INC.
To: WILMINGTON TRUST, NATIONAL ASSOCIATION
Reel/Frame 061803/0878 →
RELEASE OF SECURITY INTEREST Recorded Jul 14, 2020
From: MIDCAP FINANCIAL TRUST, AS AGENT
To: PTC THERAPEUTICS, INC.
Reel/Frame 053209/0872 →
CORRECTIVE ASSIGNMENT TO CORRECT THE INCLUSION OF 6420591,6583309,6503713, 5843995,7029846,7056656, 6468969,6486305,6630294, 6989256,6627398,8247167, 9017935 PREVIOUSLY RECORDED ON REEL 042418 FRAME 0774. ASSIGNOR(S) HEREBY CONFIRMS THE SECURITY INTEREST. Recorded Aug 24, 2017
From: PTC THERAPEUTICS, INC.
To: MIDCAP FINANCIAL TRUST, AS AGENT
Reel/Frame 043672/0096 →
SECURITY INTEREST Recorded May 8, 2017
From: PTC THERAPEUTICS, INC.
To: MIDCAP FINANCIAL TRUST, AS AGENT
Reel/Frame 042418/0774 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded May 3, 2013
From: ALMSTEAD, NEIL G.; HWANG, PETER SEONGWOO; MOON, YOUNG-CHOON
To: PTC THERAPEUTICS, INC.
Reel/Frame 030347/0391 →