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Process for the preparation of 4'-epidaunorubicin, 3',4'-diepidaunorubicin, their doxorubicin analogs, and intermediates used in said process

Assignee: Pfizer Italia SRL
•
Filing: 1980-06-30
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Granted: 1982-08-17
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Expires: 2000-06-30
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Abstract

Abstract Disclosed is a process for preparing the known antitumor glycosides: 4'-epidaunorubicin, 3',4'-diepidaunorubicin, and their doxorubicin analogs by oxidizing the C-4' hydroxyl group of N-protected daunorubicin to form certain novel intermediates having a 4'-keto configuration, followed by reduction of the keto group with NaBH 4 and mild alkaline hydrolysis to remove the N-protecting acyl groups.

Inventors

  • 👤 Antonio Suarato
  • 👤 Sergio Penco
  • 👤 Federico Arcamone

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-11-08 14:28
CPC Classifications
C; C07; C07H; C07H15/00; C07H15/20; C07H15/24; C07H15/252

Claims Analysis

Total Claims: 9
Claim 1
Independent Claim 217 words
A process for preparing 4'-epi-daunorubicin.HCl (VII) and 3',4'-di-epidaunorubicin.HCl (VIII): ##STR3## said process comprising subjecting N-trifluoroacetyl daunrorubicin (I): ##STR4## by treatment with dimethylsulfoxide activated by trifluoroacetic anhydride, to oxidation at the C-4' hydroxyl group at a temperature of about -65° to -60° C., followed by basification thereof with 1,5-diazobicyclo (4.3.0)-non-5-ene to form 4'-keto-N-trifluoroacetyl daunorubicin (III a): ##STR5## subjecting said 4'-keto-N-trifluoroacetyl daunorubicin (IIIa) to selective stereospecific reduction with sodium borohydride at a temperature of about -10° C. to obtain 4'-epi-N-trifluoroacetyl daunorubicin Va: ##STR6## converting said 4'-epi-N-trifluoroacetyl daunorubicin (Va) to 4'-epi-daunorubicin base (VII) by treatment with a mild alkali to remove the N-trifluoroacetyl group and isolating said 4'-epi-daunorubicin as its hydrochloride or alternatively, subjecting said 4'-keto-N-trifluoroacetyl daunorubicin (IIIa) to epimerization by filtering a solution thereof through a column of silica gel buffered at pH 7 with M/15 phosphate buffer to give a 1:1 epimeric mixture of said (IIIa) and 3'-epi-4'-keto-N-trifluoroacetyl daunorubicin (IV a): ##STR7## stereospecifically reducing said epimeric mixture with sodium borohydride as hereinabove described to obtain a 1:1 mixture of 4'-epi-N-trifluoroacetyl daunorubicin (Va) and 3'-4'-diepi-N trifluoroacetyl daunorubicin VI a: ##STR8## separating pure (VIa) from said mixture by chromatography on a column of silica gel buffered at pH 7 with M/15 phosphate buffer, removing the N-trifluoroacetyl group therefrom to obtain free 3',4'-diepi-daunorubicin base (VIII) and isolating same as the hydrochloride.
Claim 2
Dependent Claim 217 words
A process for preparing 4'-epi-daunorubicin.HCl (VII) and 3',4'-di-epidaunorubicin.HCl (VIII): ##STR3## said process comprising subjecting N-trifluoroacetyl daunrorubicin (I): ##STR4## by treatment with dimethylsulfoxide activated by trifluoroacetic anhydride, to oxidation at the C-4' hydroxyl group at a temperature of about -65° to -60° C., followed by basification thereof with 1,5-diazobicyclo (4.3.0)-non-5-ene to form 4'-keto-N-trifluoroacetyl daunorubicin (III a): ##STR5## subjecting said 4'-keto-N-trifluoroacetyl daunorubicin (IIIa) to selective stereospecific reduction with sodium borohydride at a temperature of about -10° C. to obtain 4'-epi-N-trifluoroacetyl daunorubicin Va: ##STR6## converting said 4'-epi-N-trifluoroacetyl daunorubicin (Va) to 4'-epi-daunorubicin base (VII) by treatment with a mild alkali to remove the N-trifluoroacetyl group and isolating said 4'-epi-daunorubicin as its hydrochloride or alternatively, subjecting said 4'-keto-N-trifluoroacetyl daunorubicin (IIIa) to epimerization by filtering a solution thereof through a column of silica gel buffered at pH 7 with M/15 phosphate buffer to give a 1:1 epimeric mixture of said (IIIa) and 3'-epi-4'-keto-N-trifluoroacetyl daunorubicin (IV a): ##STR7## stereospecifically reducing said epimeric mixture with sodium borohydride as hereinabove described to obtain a 1:1 mixture of 4'-epi-N-trifluoroacetyl daunorubicin (Va) and 3'-4'-diepi-N trifluoroacetyl daunorubicin VI a: ##STR8## separating pure (VIa) from said mixture by chromatography on a column of silica gel buffered at pH 7 with M/15 phosphate buffer, removing the N-trifluoroacetyl group therefrom to obtain free 3',4'-diepi-daunorubicin base (VIII) and isolating same as the hydrochloride.
Claim 3
Dependent Claim 20 words
A process according to claim 1 wherein the N-trifluoroacetyl protecting groups are removed by hydrolysis with dilute aqueous sodium hydroxide.
Claim 4
Dependent Claim 27 words
A process according to claim 1 wherein the free bases of 4'-epi-daunorubicin (VII) and 3',4'-diepi-daunorubicin (VIII) are converted to their hydrochlorides by treatment with methanolic hydrogen chloride.
Claim 5
Dependent Claim 15 words
A process according to claim 1 wherein the selective stereospecific reduction is effected in methanol.
Claim 6
Dependent Claim 16 words
A compound of the formulae: ##STR9## wherein R is--COCF 3 or --COOCH 2 CCl 3 .
Claim 7
Dependent Claim 16 words
A compound of the formulae: ##STR9## wherein R is--COCF 3 or --COOCH 2 CCl 3 .
Claim 8
Dependent Claim 10 words
A compound according to claim 5 which is 4'-keto-N-trifluoroacetyl daunorubicin.
Claim 9
Dependent Claim 10 words
A compound according to claim 5 which is 3'-epi-4'-keto-N-trifluoroacetyl daunorubicin.

References Cited (Backward Citations)

US4039663A Cited
US4112076A Cited

USPTO Annuity & Maintenance Windows

Annuity Stage Window Opens Payment Deadline Surcharge Period Until Estimated Fee Status
3.5 Years (Year 4) 1985-08-16 1986-02-15 1986-08-17 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1989-08-16 1990-02-15 1990-08-17 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 1993-08-16 1994-02-15 1994-08-17 $7700.00 Window Closed / Lapsed

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