IP Library Granted Patent US 9,593,061
Granted Patent B2
US 9,593,061 · App. 14/887,298 · Granted Mar 14, 2017

Synthesis of intermediates for producing prostacyclin derivatives

Inventors: Hitesh Batra (Herndon, VA); Sudersan M. Tuladhar (Silver Spring, MD); David A. Walsh (Spotsylvania, VA)
Assignee: United Therapeutics Corporation
C07C45/67C07C45/64C07C45/81C07C67/31C07C67/333
View Patent ↗
Loading inventors, assignments & file history…
Monitor This Case
Get email alerts when status or documents change.
Order Certified Copies
Most orders are placed with the USPTO same day — all within 24 business hours.
Order via The Patent Place →
Pre-filled with this patent's details
Quick Facts
Patent No.
US 9,593,061
App. No.
14/887,298
Granted
Mar 14, 2017
Kind
B2
Abstract

The present disclosure provides regioselective methods for synthesizing intermediates useful in making prostacyclin derivatives, such as treprostinil.

Claims (29)

1. A method of producing a compound of formula 3:

comprising heating a solution comprising a compound of formula 2:

and an organic solvent, wherein said heating comprises irradiating said solution with microwave radiation and wherein X is hydrogen, an alkoxy group, or OR 2 , unsubstituted or substituted aryl, or unsubstituted or substituted benzyl, wherein R 2 is C 1-4 alkyl; unsubstituted or substituted aryl; or unsubstituted or substituted benzyl, and wherein the organic solvent comprises at least one of triglyme, N-methylpyrrolidinone, tetradecane, tetrahydronaphthalene, p-chlorophenol, 1,2-dichlorobenzene, diphenyl ether, and a mixture of 26.5% diphenyl and 73.5% diphenyl oxide.

2. The method of claim 1 , wherein said solution is heated at a temperature ranging from 175° C. to 195° C.

3. The method of claim 1 , wherein X is hydrogen or an alkoxy group.

4. The method of claim 3 , wherein said heating results in separating the compound of formula 3 from a compound of formula 4:

5. The method of claim 3 , further comprising O-alkylating the compound of formula 3 to form a compound of formula 5

wherein R 1 is selected from (a) unsubstituted or substituted benzyl and (b) CH 2 COOR 4 , wherein R 4 is C 1-4 alkyl.

6. The method of claim 5 , further comprising forming from the compound of formula 5 treprostinil using a process comprising Pauson-Khand cyclization.

7. The method of claim 5 , wherein R 1 is benzyl or substituted benzyl.

8. The method of claim 5 , wherein R 1 is CH 2 COOR 4 , wherein R 4 is C 1-4 alkyl.

9. The method of claim 1 , wherein X is OR 2 , where R 2 is C 1-4 alkyl; unsubstituted or substituted aryl; or unsubstituted or substituted benzyl.

10. The method of claim 9 , wherein R 2 is methyl.

11. The method of claim 9 , wherein R 2 is ethyl.

12. The method of claim 9 , further comprising separating the compound of formula 3 from a compound of formula 4:

by a selective base hydrolysis.

13. The method of claim 9 , further comprising O-alkylating the compound of formula 3 to form a compound of formula 5

wherein R 1 is selected from a) benzyl or substituted benzyl; and b) CH 2 COOR 4 , wherein R 4 is C 1-4 alkyl.

14. The method of claim 13 , further comprising forming from the compound of formula 5 treprostinil using a process comprising Pauson-Khand cyclization.

15. The method of claim 13 , wherein R 1 is benzyl or substituted benzyl.

16. The method of claim 13 , wherein R 1 is CH 2 COOR 4 .

17. The method of claim 9 , further comprising O-alkylating and hydrolyzing the compound of formula 3 to form a compound of formula 11

wherein R 3 is C 1-4 alkyl or a phenolic protecting group.

18. The method of claim 17 , further comprising forming from the compound of formula 11 treprostinil using a process comprising Pauson-Khand cyclization.

19. The method of claim 17 , wherein R 3 is C 1-4 alkyl.

20. The method of claim 17 , wherein R 3 is a phenolic protecting group.

21. The method of claim 20 , wherein R 3 is benzyl.

22. The method of claim 1 , further comprising allylating a compound of formula 1

to produce the compound of formula 2.

Assignments (1)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Apr 14, 2016
From: BATRA, HITESH; TULADHAR, SUDERSAN M.; WALSH, DAVID A.
To: UNITED THERAPEUTICS CORPORATION
Reel/Frame 038286/0114 →
Continuity (2)
Provisional Application 62066009 · Oct 20, 2014
Related Publication 20160107973A1 · Apr 21, 2016