IP Library Granted Patent US 11,028,105
Granted Patent B2
US 11,028,105 · App. 16/455,887 · Granted Jun 8, 2021

Difluoromethyl and difluoromethylene transfer reagents

Inventors: Nathaniel Szymczak (Ypsilanti, MI); Jacob Geri (Ann Arbor, MI)
Assignee: THE REGENTS OF THE UNIVERSITY OF MICHIGAN
C07F5/05C07F5/027C07F5/04
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Quick Facts
Patent No.
US 11,028,105
App. No.
16/455,887
Granted
Jun 8, 2021
Kind
B2
Abstract

Disclosed herein are borazine, borate, and azaborinine compounds and compositions, methods of making said compounds and compositions, and methods of forming aromatic difluorocarbon compounds and difluorocarbon compounds.

Claims (43)

1. A compound of Formula (I):

having a structure of:

wherein:

the dashed lines indicate optional double bonds;

R 1 is C 6-20 aryl or C 1-15 heteroaryl, and the heteroaryl comprises 1-5 ring heteroatoms selected from N, O, and S;

each R 2 and R 3 is independently OH, N(R 4 ) 2 , C 1-6 alkyl, C 3-8 cycloalkyl, OC 1-6 alkyl, or OC 3-8 cycloalkyl; or adjacent R 2 and R 3 , taken together with the atoms to which they are attached, form an optionally substituted 5-7 membered ring;

each R 4 is independently C 1-6 alkyl or C 3-8 cycloalkyl;

each R 5 is independently C 1-6 alkyl, C 3-8 cycloalkyl; or

each R 5 taken together with the atoms to which they are attached form an optionally substituted 5-7 membered ring;

each R 6 is independently C 1-6 alkyl, C 3-8 cycloalkyl, OC 1-6 alkyl, or OC 3-8 cycloalkyl; and

M comprises a counterion.

2. The compound of claim 1 , wherein R 1 is C 6-20 aryl.

3. The compound of claim 1 , wherein R 1 is C 1-15 heteroaryl.

4. The compound of claim 1 , wherein R 1 is selected from the group consisting of:

and

X is H, F, Cl, Br, I, CHs, OH, NH 2 , NO 2 , C 1-4 alkyl, OC 1-4 alkyl, CO 2 H, CHO, CF 3 , or CN.

5. The compound of claim 1 , wherein at least one R 2 or R 3 is methyl.

6. The compound of claim 1 having a structure selected from the group consisting of:

7. A composition comprising the compound of claim 1 and a crown ether.

8. A method for preparing the compound of claim 1 , comprising contacting H—CF 2 R 1 with a Lewis acid, a base, and optionally a crown ether under conditions sufficient to form the compound, wherein the Lewis acid has a structure:

9. The method of claim 8 , wherein the H—CF 2 R 1 is selected from the group consisting of:

and

X is H, F, Cl, Br, I, CHs, OH, NH 2 , NO 2 , C 1-4 alkyl, OC 1-4 alkyl, CO 2 H, CHO, CF 3 , or CN.

10. A method of forming an aromatic difluorocarbon compound comprising admixing the compound of claim 1 , with an electrophile under conditions sufficient to couple the electrophile and CF 2 R 1 to form the aromatic difluorocarbon compound.

11. A compound of Formula (III)

wherein:

the dashed lines indicate optional double bonds;

R 1 is H, C 6-20 aryl, or C 1-15 heteroaryl, and the heteroaryl comprises 1-5 ring heteroatoms selected from N, O, and S;

R 2 and R 3 are independently OH, N(R 4 ) 2 , C 1-6 alkyl, C 3-8 cycloalkyl, OC 1-6 alkyl, or OC 3-8 cycloalkyl, or R 2 and R 3 , taken together with the atoms to which they are attached, form an optionally substituted 5-7 membered ring;

each R 4 is independently C 1-5 alkyl or C 3-8 cycloalkyl;

each R 7 is independently H, C 1-6 alkyl, C 3-8 cycloalkyl, or at least one adjacent R 7 pair, taken together with the atoms to which they are attached, form an optionally substituted 5-7 membered ring; and

M comprises a counterion.

12. The compound of claim 11 , selected from the group consisting of:

13. The compound of claim 11 , wherein R 1 is H.

14. The compound of claim 11 , wherein R 1 is C 6-20 aryl.

15. The compound of claim 11 , wherein R 1 is C 1-15 heteroaryl.

16. The compound of claim 11 , wherein R 1 is selected from the group consisting of:

and

X is H, F, Cl, Br, I, CH 3 , OH, NH 2 , NO 2 , C 1-4 alkyl, OC 1-4 alkyl, CO 2 H, CHO, CF 3 , or CN.

17. The compound of claim 11 , wherein at least one of R 2 and R 3 is methyl.

18. A composition comprising the compound of claim 11 and a crown ether.

19. A method for preparing the compound of claim 11 , comprising contacting H—CF 2 R 1 with a Lewis acid, a base, and optionally a crown ether under conditions sufficient to form the compound, wherein the Lewis acid has a structure:

20. A method of forming a difluorocarbon compound comprising admixing the compound of, claim 11 , with an electrophile under conditions sufficient to couple the electrophile and CF 2 R 1 to form the aromatic difluorocarbon compound.

Assignments (3)
CONFIRMATORY LICENSE Recorded Mar 24, 2025
From: UNIVERSITY OF MICHIGAN
To: NATIONAL SCIENCE FOUNDATION
Reel/Frame 070602/0195 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jul 17, 2019
From: GERI, JACOB
To: THE REGENTS OF THE UNIVERSITY OF MICHIGAN
Reel/Frame 049774/0188 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jul 15, 2019
From: SZYMCZAK, NATHANIEL
To: THE REGENTS OF THE UNIVERSITY OF MICHIGAN
Reel/Frame 049755/0771 →
Continuity (2)
Provisional Application 62691735 · Jun 29, 2018
Related Publication 20200002362A1 · Jan 2, 2020