IP Library Granted Patent US 9,187,433
Granted Patent B2
US 9,187,433 · App. 14/629,046 · Granted Nov 17, 2015

Formation of N-protected 3,6-bis-(4-aminobutyl) -2, 5-diketopiperazine through a cyclic α-

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Quick Facts
Patent No.
US 9,187,433
App. No.
14/629,046
Granted
Nov 17, 2015
Kind
B2
Abstract

A method for the synthesis of N-protected 3,6-aminoalkyl-2,5-diketopiperazines is provided. The method includes obtaining a cyclic α-N protected active amino ester and adding it to a mixture of an amine catalyst in an organic solvent.

Claims (31)

1. A method for the synthesis of a N-protected-bis-3,6-aminoalkyl-2,5-diketopiperazine, the method comprising: adding a cyclic α-N protected active amino ester according to Formula II

wherein PG is selected from the group consisting of amide forming protecting groups and carbamate protecting groups; and

wherein n is from 1 to 8;

to a mixture of an amine catalyst in an organic solvent, wherein the amine catalyst is present in amount of 0.25 to 2.5 eq based on the amount of cyclic α-N protected active amino ester; and

heating the mixture after adding the cyclic α-N protected active amino ester.

2. The method of claim 1 , wherein PG is trifluoroacetyl.

3. The method of claim 1 , wherein n is 3.

4. The method of claim 1 , wherein the amine catalyst is aziridine.

5. The method of claim 1 , wherein the amine catalyst is an amidoxime.

6. The method of claim 1 , wherein the amine catalyst is benzamidoxime.

7. The method of claim 1 , wherein the amine catalyst is present in an amount of 1 to 2 eq based on the amount of cyclic α-N protected active amino ester.

8. The method of claim 1 , wherein the amine catalyst is present in an amount of 1.5 eq based on the amount of cyclic α-N protected active amino ester.

9. The method of claim 1 , wherein the mixture further comprises a second catalyst.

10. The method of claim 1 , wherein the organic solvent is ethanol and the amine catalyst is aziridine.

11. The method of claim 1 , wherein the organic solvent is THF and the amine catalyst is aziridine.

12. The method of claim 1 , wherein PG is acetyl.

13. The method of claim 1 , wherein PG is Boc.

14. The method of claim 1 , wherein PG is CBz.

15. A method for the synthesis of a N-protected-bis-3,6-aminoalkyl-2,5-diketopiperazine, the method comprising: adding a cyclic α-N protected active amino ester according to Formula II

wherein PG is trifluoroacetyl; and

wherein n is from 1 to 8;

to a mixture of an amine catalyst in an organic solvent, wherein the amine catalyst is present in amount of 1 to 2 eq based on the amount of cyclic α-N protected active amino ester and heating the mixture after adding the cyclic α-N protected active amino ester.

16. The method of claim 15 , wherein the organic solvent is selected from ethanol and THF and the amine catalyst is aziridine.

17. The method of claim 15 , wherein the organic solvent is selected from ethanol and THF and the amine catalyst is benzamidoxime.

18. The method of claim 15 , wherein n is 3.

19. The method of claim 15 , wherein the amine catalyst is present in amount of 1.5 eq based on the amount of cyclic α-N protected active amino ester.

20. A method for the synthesis of a N-protected-bis-3,6-aminoalkyl-2,5-diketopiperazine, the method comprising: adding a cyclic α-N protected active amino ester according to Formula II

wherein PG is selected from the group consisting of amide forming protecting groups and carbamate protecting groups; and

wherein n is from 1 to 8;

to a mixture of an amine catalyst and a second catalyst in an organic solvent,

wherein the amine catalyst is present in amount of 0.25 to 2.5 eq based on the amount of cyclic α-N protected active amino ester.

Assignments (5)
PATENT SECURITY AGREEMENT Recorded Aug 12, 2025
From: MANNKIND CORPORATION
To: WILMINGTON TRUST, NATIONAL ASSOCIATION, AS COLLATERAL AGENT
Reel/Frame 072444/0525 →
RELEASE OF SECURITY INTEREST Recorded Apr 5, 2024
From: MIDCAP FINANCIAL TRUST, AS AGENT
To: MANNKIND CORPORATION; MANNKIND LLC
Reel/Frame 067024/0082 →
RELEASE OF SECURITY INTEREST Recorded Aug 13, 2019
From: DEERFIELD PRIVATE DESIGN FUND II, L.P.; DEERFIELD PRIVATE DESIGN INTERNATIONAL II, L.P.; HORIZON SANTE FLML SARL
To: MANNKIND CORPORATION
Reel/Frame 050044/0138 →
SECURITY INTEREST Recorded Aug 13, 2019
From: MANNKIND CORPORATION; MANNKIND LLC
To: MIDCAP FINANCIAL TRUST, AS AGENT
Reel/Frame 050044/0181 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 11, 2015
From: FREEMAN, JOHN J.; PHANTSIEL, OTTO; BAY, WILLIAM ELLIOTT; KRAFT, KELLY SULLIVAN
To: MANNKIND, CORP.
Reel/Frame 035889/0093 →