IP Library Granted Patent US 8,236,949
Granted Patent B2
US 8,236,949 · App. 12/174,913 · Granted Aug 7, 2012

Tetrazine-based bio-orthogonal coupling reagents and methods

Assignee: University of Delaware
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Quick Facts
Patent No.
US 8,236,949
App. No.
12/174,913
Granted
Aug 7, 2012
Kind
B2
Abstract

Coupling reactions, suitable for use in organic or aqueous media, are performed by contacting a 1,2,4,5-tetrazine with a dienophile. The dienophile may be covalently bonded to a protein, and the coupling reaction may be performed in biological media such as those containing cells or cell lysates. The reactions may be performed in the presence of primary amines, thiols, acetylenes, azides, phosphines, and products of Staudinger and/or Sharpless-Huisgen reactions Novel 3-substituted cyclopropene compounds and trans-cyclooctenes are exemplary dienophiles for these reactions.

Claims (25)

1. A method of performing a coupling reaction, comprising contacting a 1,2,4,5-tetrazine with a dienophile in an organic or aqueous medium comprising at least one species selected from the group consisting of primary amines, thiols, Staudinger reactants, Staudinger adducts, Sharpless-Huisgen reactants, and Sharpless-Huisgen adducts; said contacting performed under conditions sufficient to convert at least 50% of the 1,2,4,5-tetrazine or the dienophile to a Diels-Alder adduct of the 1,2,4,5-tetrazine with the dienophile; wherein the dienophile is selected from the group consisting of trans-cyclooctene, substituted trans-cyclooctenes and compounds according to formulas (7), (8) and (27)

2. The method of claim 1 , wherein the conversion is at least 90%.

3. The method of claim 1 , wherein the conditions comprise a temperature of at most 50° C. and a reaction time of at most 1 hour.

4. The method of claim 1 , wherein a concentration of the 1,2,4,5-tetrazine or the dienophile in the medium is at most 0.01M.

5. The method of claim 1 , wherein the medium is an aqueous medium.

6. The method of claim 1 , wherein the medium is a biological medium.

7. The method of claim 1 , wherein the 1,2,4,5-tetrazine is selected from the group consisting of compounds according to formulas (4), (22), (23), (30), (31), (32), (33) and (34)

8. The method of claim 1 , wherein the dienophile is selected from the group consisting of compounds according to formulas (7), (8) and (27)

9. The method of claim 1 , wherein the dienophile is trans-cyclooctene.

10. The method of claim 1 , wherein the dienophile is a substituted trans-cyclooctene.

11. The method of claim 1 , wherein the dienophile is a substituted trans-cyclooctene selected from the group consisting of the following compounds

12. The method of claim 1 , wherein the medium comprises a Staudinger reactant or a Sharpless-Huisgen reactant, the method further comprising subsequently contacting the Staudinger reactant or a Sharpless-Huisgen reactant with a complementary reactant under conditions sufficient to convert at least 50% of the Staudinger reactant, the Sharpless-Huisgen reactant, or the complementary reactant to a Staudinger adduct or a Sharpless-Huisgen adduct.

13. A method of performing a coupling reaction, comprising contacting a 1,2,4,5-tetrazine with a dienophile in an organic or aqueous medium; said contacting performed under conditions sufficient to convert at least 50% of the 1,2,4,5-tetrazine or the dienophile to a Diels-Alder adduct of the 1,2,4,5-tetrazine with the dienophile, wherein the dienophile is covalently bonded to a protein and wherein the dienophile is selected from the group consisting of trans-cyclooctene, substituted trans-cyclooctenes and compounds according to formulas (7), (8) and (27)

14. A method of performing a coupling reaction, comprising contacting a 1,2,4,5-tetrazine selected from the group consisting of compounds according to formulas (4), (22), (23), (30), (31), (32), (33) and (34)

with a substituted cyclopropene selected from the group consisting of compounds according to formulas (7), (8) and (27)

in an organic or aqueous medium under conditions sufficient to convert at least 50% of the 1,2,4,5-tetrazine or the substituted cyclopropene to a Diels-Alder adduct of the 1,2,4,5-tetrazine with the substituted cyclopropene.

15. The method of claim 14 , wherein the medium is an aqueous medium.

16. The method of claim 14 , wherein the medium is a biological medium.

17. A method of performing a coupling reaction, comprising contacting a 1,2,4,5-tetrazine selected from the group consisting of compounds according to formulas (4), (22), (23), (30), (31), (32), (33) and (34)

with trans-cyclooctene or a substituted trans-cyclooctene in an organic or aqueous medium under conditions sufficient to convert at least 50% of the 1,2,4,5-tetrazine, the trans-cyclooctene, or the substituted trans-cyclooctene to a Diels-Alder adduct of the 1,2,4,5-tetrazine with the trans-cyclooctene or the substituted trans-cyclooctene.

18. The method of claim 17 , wherein the contacting is performed with trans-cyclooctene.

19. The method of claim 17 , wherein the contacting is performed with a substituted trans-cyclooctene selected from the group consisting of the following compounds

20. A 1,2,4,5-tetrazine selected from the group consisting of compounds according to formulas (22), (23), (30), (31), (32), (33) and (34)

21. A method of quantitative analysis comprising the steps of exposing an adduct of a 1,2,4,5-tetrazine with a dienophile to UV radiation, and measuring either the fluorescent emission or UV absorption of the sample.

22. The method of claim 13 , wherein the dienophile comprises a trans-cyclooctene moiety.

Assignments (2)
CONFIRMATORY LICENSE Recorded May 26, 2017
From: UNIVERSITY OF DELAWARE
To: NATIONAL INSTITUTES OF HEALTH (NIH), U.S. DEPT. OF HEALTH AND HUMAN SERVICES (DHHS), U.S. GOVERNMENT
Reel/Frame 042589/0163 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Sep 11, 2008
From: FOX, JOSEPH MICHAEL; BLACKMAN, MELISSA; ROYZEN, MAKSIM; YAN, NI
To: UNIVERSITY OF DELAWARE
Reel/Frame 021515/0857 →
Continuity (2)
Provisional Application 60959803 · Jul 17, 2007
Related Publication 20090023916A1 · Jan 22, 2009