IP Library Granted Patent US 10,906,911
Granted Patent B2
US 10,906,911 · App. 16/457,788 · Granted Feb 2, 2021

Synthesis of coelenterazine

Inventors: Rajagopala Reddy Duvvuru (Hyderabad, IN); Rama Bhatt (Newcastle, WA); Anil Kumar (Puyallup, WA)
Assignee: International Paper Company
C07D487/04B01J20/22B01J31/2404B01J2531/824C07B51/00
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Quick Facts
Patent No.
US 10,906,911
App. No.
16/457,788
Granted
Feb 2, 2021
Kind
B2
Abstract

Disclosed herein are synthesis methods for coelenterazine. Also disclosed are articles including the coelenterazine and coelenterazine derivatives. Representative absorbent articles include disposable diapers and adult incontinence products.

Claims (14)

1. A method of making coelenterazine, comprising:

coupling 4-(5-amino-6-benzylpyrazin-2-yl)phenol (7) with 1,1-diethoxy-3-(4-hydroxyphenyl)propan-2-one (14) to provide coelenterazine, or a salt thereof.

2. The method of claim 1 , wherein the 4-(5-amino-6-benzylpyrazin-2-yl)phenol (7) is prepared by (a) reacting 3,5-dibromopyrazin-2-amine and (bromomethyl)benzene in the presence of zinc, iodine, and a first palladium catalyst to provide 3-benzyl-5-bromopyrazin-2-amine (2), or a salt thereof; and (b) reacting 3-benzyl-5-bromopyrazin-2-amine (2) in two sequential steps to provide the 4-(5-amino-6-benzylpyrazin-2-yl)phenol (7).

3. The method of any one of claim 2 , wherein (b) comprises a first step of reacting the 3-benzyl-5-bromopyrazin-2-amine (2) with (4-methoxyphenyl)boronic acid in the presence of a second palladium catalyst to provide 3-benzyl-5-(4-methoxyphenyl)pyrazin-2-amine (5) (coelenteramine), or a salt thereof.

4. The method of claim 3 , wherein (b) further comprises isolating the 3-benzyl-5-(4-methoxyphenyl)pyrazin-2-amine (5) (coelenteramine) by precipitation of the 3-benzyl-5-(4-methoxyphenyl)pyrazin-2-amine (5) as a hydrochloride salt, and wherein isolating the 3-benzyl-5-(4-methoxyphenyl)pyrazin-2-amine (5) does not include chromatography (e.g., liquid chromatography), does not include recrystallization, or does not include chromatography and recrystallization.

5. The method of any one of claim 3 , wherein (b) further comprises a second step of deprotecting the 3-benzyl-5-(4-methoxyphenyl)pyrazin-2-amine (5) to provide 4-(5-amino-6-benzylpyrazin-2-yl)phenol (7).

6. The method of any one of claim 1 , wherein coupling of the 4-(5-amino-6-benzylpyrazin-2-yl)phenol (7) with the 1,1-diethoxy-3-(4-hydroxyphenyl)propan-2-one (14) is conducted in a solvent mixture comprising dioxane, water, and HCl; or in a solvent mixture comprising dioxane, methanol, and isopropyl alcohol.

7. The method of any one of claim 1 , wherein the coupling reaction of 4-(5-amino-6-benzylpyrazin-2-yl)phenol (7) with 1,1-diethoxy-3-(4-hydroxyphenyl)propan-2-one (14) is monitored by reverse phase HPLC and is quenched when 4-(5-amino-6-benzylpyrazin-2-yl)phenol (7) stops depleting or when coelenterazine starts to decompose.

8. The method of claim 7 , further comprising triturating the reaction mixture after coupling the 4-(5-amino-6-benzylpyrazin-2-yl)phenol (7) with the 1,1-diethoxy-3-(4-hydroxyphenyl)propan-2-one (14).

9. An absorbent article, comprising the coelenterazine, or a salt thereof, synthesized by the methods of any one of claim 1 .

10. A method of making coelenterazine, comprising:

(a) reacting 3,5-dibromopyrazin-2-amine and (bromomethyl)benzene in the presence of zinc, iodine, and a first palladium catalyst to provide 3-benzyl-5-bromopyrazin-2-amine (2);

(b) reacting 3-benzyl-5-bromopyrazin-2-amine (2) in a first step to provide a hydrochloride salt of 3-benzyl-5-(4-methoxyphenyl)pyrazin-2-amine (5), and reacting the hydrochloride salt of 3-benzyl-5-(4-methoxyphenyl)pyrazin-2-amine (5) in a second step to provide 4-(5-amino-6-benzylpyrazin-2-yl)phenol (7); and

(c) coupling 4-(5-amino-6-benzylpyrazin-2-yl)phenol (7) with 1,1-diethoxy-3-(4-hydroxyphenyl)propan-2-one (14) to provide coelenterazine, or a salt thereof.

Assignments (2)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 14, 2025
From: INTERNATIONAL PAPER COMPANY
To: GCF US HOLDINGS LLC
Reel/Frame 073563/0717 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 10, 2020
From: DUVVURU, RAJAGOPALA REDDY; BHATT, RAMA; KUMAR, ANIL
To: INTERNATIONAL PAPER COMPANY
Reel/Frame 054328/0099 →