IP Library Granted Patent US 8,674,101
Granted Patent B2
US 8,674,101 · App. 13/054,458 · Granted Mar 18, 2014

Nucleophilic fluorination of aromatic compounds

Inventors: Nagichettiar Satyamurthy (Los Angeles, CA); Jorge R. Barrio (Agoura Hills, CA)
Assignee: The Regents of the University of California
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Quick Facts
Patent No.
US 8,674,101
App. No.
13/054,458
Granted
Mar 18, 2014
Kind
B2
Abstract

Iodylbenzene derivatives substituted with electron donating as well as electron withdrawing groups on the aromatic ring are used as precursors in aromatic nucleophilic substitution reactions. The iodyl group (IO 2 ) is regiospecifically substituted by nucleophilic fluoride to provide the corresponding fluoroaryl derivatives. No-carrier-added [F-18]fluoride ion derived from anhydrous [F-18](F/Kryptofix, [F-18]CsF or a quaternary ammonium fluoride (e.g., Me 4 NF, Et 4 NF, n-Bu 4 NF, (PhCH 2 ) 4 NF) exclusively substitutes the iodyl moiety in these derivatives and provides high specific activity F-18 labeled fluoroaryl analogs. Iodyl derivatives of a benzothiazole analog and 6-iodyl-L-dopa derivatives have been synthesized as precursors and have been used in the preparation of no-carrier-added [F-18]fluorobenzothiazole as well as 6-[F-18]fluoro-L-dopa.

Claims (21)

1. A procedure for preparing F-18 labeled compounds identified as product in the table below comprising:

providing a benzene derivative containing an iodyl group and an aqueous solution of [F-18] fluoride ion

replacing the iodyl group by said F-18 ion to produce an F-18 containing benzene derivative, the F-18 ion being free of a fluoride ion carrier

wherein the benzene derivative containing an iodyl group is selected from the group listed in the left hand column of the table below and the F-18 containing benzene derivative produced therefrom is listed in the corresponding right hand column of the table below:

Benzene Derivative

Containing Iodine

Product

.

2. The procedure of claim 1 wherein [O-18]water in a cyclotron target body is bombarded by photons to produce the aqueous solution of the [F-18]fluoride ion free of a fluoride ion carrier.

3. The procedure of claim 2 wherein each [F-18]fluoride ion is treated with potassium carbonate and a ligand, the aqueous solution is evaporated to dryness and reacted with the benzene derivatives containing and iodyl group to form a dry composition containing [F-18]fluoride ion labeled benzene derivative.

4. The procedure of claim 3 wherein the [F-18] fluorobenzene derivative is purified to produce a ≧95% radiochemically pure [F-18] fluorobenzene derivative.

5. The procedure of claim 3 wherein the [F-18] fluorobenzene derivative is purified to produce a ≧99% radiochemically and chemically pure product.

6. A method of producing the F-18 compounds of the formula

by subjecting an iodine containing compound of the formula

to dry/anhydrous no-carrier-added F-18 fluoride ion using conventional dry heating procedures or under microwave heating where the [F-18] fluoride ion is derived from [F-18]KF/Kryptofix complex, [F-18]CsF or [F-18] quaternary ammonium fluoride, the quaternary ammonium groups selected from tetramethyl, tetraethyl, tetra n-butyl, and tetrabenzyl

wherein:

R 1 ═H, OCH 3 , OCH 2 Ph, O-Boc, O-Methoxytrityl

wherein R 2 is bonded to the iodine containing compound at a C atom identified by *.

7. The method of claim 6 wherein one or more ketone groups in the F-18 compounds are oxidized using the Baeyer-Villiger reaction to form one or more ester groups.

8. The method of claim 6 further comprising producing F-18 labeled amino acids, F-18 labeled amines or F-18 labeled amino alcohols by hydrolyzing the F-18 compounds using conventional dry heating or microwave heating with mineral acids or organic acids.

9. The method of claim 8 wherein the mineral acids comprise HCl, HBr or HI and the organic acids comprise methanesulfonic acid, or trifluoromethane sulfonic acid.

Assignments (2)
CONFIRMATORY LICENSE Recorded Mar 30, 2020
From: UNIVERSITY OF CALIFORNIA LOS ANGELES
To: UNITED STATES DEPARTMENT OF ENERGY
Reel/Frame 052263/0368 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Apr 1, 2011
From: SATYAMURTHY, NAGICHETTIAR; BARRIO, JORGE R.
To: THE REGENTS OF THE UNIVERSITY OF CALIFORNIA
Reel/Frame 026063/0921 →
Continuity (2)
Provisional Application 61080524 · Jul 14, 2008
Related Publication 20110178302A1 · Jul 21, 2011