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GB2036017A - Selective Process for the Preparation of 7-hydroxycoumarin Derivatives - Google Patents

Selective Process for the Preparation of 7-hydroxycoumarin Derivatives Download PDF

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Publication number
GB2036017A
GB2036017A GB7938197A GB7938197A GB2036017A GB 2036017 A GB2036017 A GB 2036017A GB 7938197 A GB7938197 A GB 7938197A GB 7938197 A GB7938197 A GB 7938197A GB 2036017 A GB2036017 A GB 2036017A
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formula
compound
reacting
produce
haloresorcinol
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GB7938197A
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GB2036017B (en
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Fidia SpA
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D311/00Heterocyclic compounds containing six-membered rings having one oxygen atom as the only hetero atom, condensed with other rings
    • C07D311/02Heterocyclic compounds containing six-membered rings having one oxygen atom as the only hetero atom, condensed with other rings ortho- or peri-condensed with carbocyclic rings or ring systems
    • C07D311/04Benzo[b]pyrans, not hydrogenated in the carbocyclic ring
    • C07D311/06Benzo[b]pyrans, not hydrogenated in the carbocyclic ring with oxygen or sulfur atoms directly attached in position 2
    • C07D311/08Benzo[b]pyrans, not hydrogenated in the carbocyclic ring with oxygen or sulfur atoms directly attached in position 2 not hydrogenated in the hetero ring
    • C07D311/16Benzo[b]pyrans, not hydrogenated in the carbocyclic ring with oxygen or sulfur atoms directly attached in position 2 not hydrogenated in the hetero ring substituted in position 7

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)
  • Pyrane Compounds (AREA)
  • Saccharide Compounds (AREA)

Abstract

A selective process for the preparation of substantially pure 8- halo-3-( beta -diethylaminoethyl)-4- methyl-7-ethoxycarbonylmethoxy coumarin comprises a) reacting a 2- haloresorcinol with alpha -acetyl- gamma - butyrolactone in the presence of KBr and acetic acid, b) reacting the resulting 3-( beta -bromoethyl)-4-methyl- 7-hydroxy-8-halocoumarin with ethyl chloroacetate and reacting the product with diethylamine in the presence of anhydrous K2CO3 to obtain the desired final product. Steps a) and b) may be reversed. Acid addition salts of the final product are disclosed.

Description

SPECIFICATION Selective Process for the Preparation of 7-hydroxycoumarin Derivatives The present invention relates to the preparation of derivatives of 7-hydroxycoumarin.
In ourcopending U.K. Patent Application No. 43690/78, (Publication No. 2008109 A) there is disclosed a new method for the preparation of basic coumarin derivatives of the general formula IA and of their acid addition salts with organic and inorganic acids:
where R1 is an alkyl group having thereon a basic substituent; R2 is H, alkyl or aryl; R3 is an alkyl group having thereon a basic substituent, or an alkenyl, carboxyalkyl or alkoxycarboxy-alkyl group; and X is halogen.
The compounds of formula IA may be considered as derivatives of carbochromene, i.e., 3-(p- diethylam inoethyl)-4-methyl-7-ethoxycarbonyl methoxycoumarin chlorohydrate, which is known in the literature and used as coronary dilator. Compared with carbochromane, the main characteristic of the compounds of formula IA is the presence of a halogen atom in the 8-position and a particular feature of the method disclosed in the previous application, is that the 8-halo derivatives are obtained in substantially pure state, i.e. without the presence of other halogen-derivated isomers or dihalogen derivatives or other impurities.
The present invention provides an alternative selective method for the preparation of 8-halo-3-(p- diethylaminoethyl)-4-methyl-7-ethoxycarbonylmethoxy coumarin and in particular the 8-chloro derivative, i.e. compounds of the formula IB
According to the present invention the compounds of formula IB, particularly the 8-chloro compound, and their acid addition salts, are prepared in isomerically pure form by a) reacting a 2-haloresorcinol of the formula II with cg-acetyl-y-butyrolactone in the presence of KBr and acetic acid to produce a compound of formula Ill;
where X is as defined above; b) reacting the compound of formula Ill with ethyl chloroacetate to produce a compound of the formula IV::
and, c) reacting the compound of formula IV with diethylamine to produce the compound of formula IB. Alternatively steps a) and b) can be reversed, i.e. the 2-halo-resorcinol may first be reacted with the ethylchloroacetate and then with the a-acetyl-y-butyrolactone. The characteristic step of the present invention is the reaction of the 8-halo-resorcinol, or its 1 -ethoxycarbonylmethoxy derivative, with the a-acetyl-y-butyrolactone in the presence of KBr and acetic acid.
The full reaction scheme is as follows:
Step a) is preferably carried out under reflux conditions.
Step b) is preferably carried out in the presence of a solvent, e.g. acetone and in the presence of KI and K2CO3, and is preferably followed by recrystallisation of the compound of formula IV, e.g. from aqueous acetone.
Step c) is preferably carried out in a suitable solvent such as benzene and a hydrogen bromide acceptor, preferably anhydrous K2CO3.
Following step c), the product compound may be converted into an acid addition salt in known manner, and preferably the hydrochloride by reaction in solution in CH2Cl2 with HCI.
The selective process according to the present invention will be better understood from the following working examples of the various phases of the process.
Example 1 3-(,B-bromoethyl)-4-methyl-7-hydroxy-8-chlorocoumarin (Ill) To a solution of 34 g of HBr in 116 ml of acetic acid there are added 9.2 g of 2-chlororesorcine and then, at 0 C, there are added dropwise 6.9 g of a-acetyl-y-butyrolactone. The reaction mixture is refluxed for 2 hours and then cooled to room temperature.
Upon addition, with stirring, of 350 ml of H2O an oily mass separates. The oily residue, on recrystal lisation from MetOH, gives the 3-(p-bromoethyl)-4-methyl-7-hydroxy-8-chlorocoumarin; m.p.
192-1 940C.
Example 2 3-(t\-brornoethyl)-4-rnethyl-7-ethoxycarbonyl-methoxy-8-chlorocoumarin ( IV) To a solution of 2.6 g of 3-(}ss-bromoethyl)-4-methyl-7-hydroxy-8-chlorocoumarin in 16 ml of acetone there are added 2.36 g of K2CO3 and the mixture is refluxed for 1 5 minutes. There are then added 4 mg of KI and 2 g of ethyl chloroacetate, keeping the mixture at the boiling point for an additional 1 5 minutes. After cooling to room temperature, there are added 70 ml of H2O and the mixture is stirred overnight. There precipitates therefrom a crystalline product which is removed by filtration and washed with water to a neutral pH.The residue, after recrystallization from acetonewater, gives the 3-(-bromoethyl)-4-methyl-7-ethoxycarbonyl methoxy-8-chlorocou marin; m.p. 1 61 - 1620C.
Example 3 3-(p-diethylaminoethyl)-4-methyl-7-ethoxy-carbonyl methoxy-8-chlorocoumarin Chlorohydrate (IB) To a solution of 1 g of 3-(A-bromoethyl)-4-methyl-7-ethoxywarbonylmethoxy-8-chloro-coumarin in 5 ml of benzene there are added 0.6 g of anhydrous K2CO3 and 0.45 g of diethylamine. The mixture is refiuxed for 5 hours and is then cooled to room temperature. The organic phase is washed with water and then dried over Na2SO4. After evaporation of the solvent, there is obtained a residue which is then dissolved in CH2CI2. The resulting solution is treated with HCI and then evaporated. The residue, after recrystallization from absolute EtOH, gives the 3-(,B-diethylaminoethyl)-4-methyl-7-ethoxywarbonyl- methoxy-8-chlorocoumarin chlorohydrate; m.p. 219--2200C.

Claims (10)

Claims
1. A method for the preparation of 8-halo-3-(p-diethylaminoethyl)-4-methyl-7- ethoxycarbonylmethoxy coumarin of the formula IB
where X is halogen, which comprises a) reacting a 2-haloresorcinol of the formula Il with a-acetyl-y-butyrolactone in the presence of KBr and acetic acid to produce a compound of the formula Ill;
where X is as defined above; b) reacting the compound of formula Ill with ethyl chloroacetate to produce a compound of the formula IV:
and c) reacting the compound of formula IV with diethylamine to produce the compound of formula IB.
-
2. A method according to claim 1, where X is chlorine.
3. A method according to claim 1 or 2, wherein step b) is carried out in the presence of K2CO3 and KI.
4. A method according to claim 1, 2 or 3, wherein step c) is carried out in the presence of anhydrous K2CO3.
5. A method according to any one of claims 1-4, wherein following step b) and before step c) the compound of formula IV is recrystallised from solution in aqueous acetone.
6. A method according to any one of the preceding claims, modified in that step a) comprises reacting the 2-haloresorcinol with ethyl chloracetate to produce a 1 -ethoxycarbonylmethoxy-2- haloresorcinol, and step b) comprises reacting the 1 -ethoxycarbonylmethoxy-2-haloresorcinol with said -acetyl-y-butyrolactone in the presence of said KBr and acetic acid to produce said compound of formula IV.
7. A method according to any one of claims 1-6, including the additional step of converting the product compound of formula IB to an acid addition salt.
8. A method according to claim 7, wherein said salt is the hydrochloride.
9. A method according to claim 1, substantially as hereinbefore described in Examples 1-3.
10. A compound of formula IB as defined in claim 1 when prepared by a method claimed in any one of claims 1-5, 8 or 9.
1 An acid addition salt of a compound of formula IB as defined in claim 1, when prepared by a method claimed in claim 6 or 7.
GB7938197A 1978-11-06 1979-11-05 Selective process for the preparation of 7-hydroxycoumarin derivatives Expired GB2036017B (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
IT29466/78A IT1100069B (en) 1978-11-06 1978-11-06 SELECTIVE PROCEDURE FOR THE PREPARATION OF DERIVATIVES OF 7-HYDROXICUMARINE

Publications (2)

Publication Number Publication Date
GB2036017A true GB2036017A (en) 1980-06-25
GB2036017B GB2036017B (en) 1983-03-23

Family

ID=11227039

Family Applications (1)

Application Number Title Priority Date Filing Date
GB7938197A Expired GB2036017B (en) 1978-11-06 1979-11-05 Selective process for the preparation of 7-hydroxycoumarin derivatives

Country Status (16)

Country Link
JP (1) JPS5569575A (en)
AT (1) AT372380B (en)
BE (1) BE879821A (en)
CA (1) CA1113948A (en)
CH (1) CH641796A5 (en)
DE (1) DE2944376A1 (en)
ES (1) ES485745A1 (en)
FI (1) FI793400A7 (en)
FR (1) FR2440948A1 (en)
GB (1) GB2036017B (en)
GR (1) GR68055B (en)
IT (1) IT1100069B (en)
NL (1) NL7907983A (en)
PT (1) PT70412A (en)
YU (1) YU40580B (en)
ZA (1) ZA795805B (en)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5482975A (en) * 1991-10-22 1996-01-09 Octamer, Inc. Adenosine diphosphoribose polymerase binding nitroso aromatic compounds useful as retroviral inactivating agents, anti-retroviral agents and anti-tumor agents
US5484951A (en) * 1990-10-19 1996-01-16 Octamer, Incorporated 5-iodo-6-amino-6-nitroso-1,2-benzopyrones useful as cytostatic and antiviral agents
US5783599A (en) * 1993-02-24 1998-07-21 Octamer Inc Methods of treating cancer and viral infections with 5-iodo-6-amino-and 5-iodo-6-nitroso-1 2-benzopyrones
US5877185A (en) * 1991-10-22 1999-03-02 Octamer, Inc. Synergistic compositions useful as anti-tumor agents

Family Cites Families (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2361M (en) * 1961-08-12 1964-02-24 Cassella Farbwerke Mainkur Ag Coronary dilator drug containing a derivative of 7-hydroxy-coumarin.
DE2039867A1 (en) * 1970-08-11 1972-02-17 Troponwerke Dinklage & Co Amino-hydroxypropyl-coumarins - with coronary dilating activity
IT1088554B (en) * 1977-11-17 1985-06-10 F I D I A Spa SELLECTIVE PROCEDURE FOR THE PREPARATION OF DERIVATIVES OF 7-INDROSSI CUMARINA

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5484951A (en) * 1990-10-19 1996-01-16 Octamer, Incorporated 5-iodo-6-amino-6-nitroso-1,2-benzopyrones useful as cytostatic and antiviral agents
US5519053A (en) * 1990-10-19 1996-05-21 Octamer, Inc. 5-Iodo-6-amino-1,2-Benzopyrones and their metabolites useful as cytostatic agents
US5482975A (en) * 1991-10-22 1996-01-09 Octamer, Inc. Adenosine diphosphoribose polymerase binding nitroso aromatic compounds useful as retroviral inactivating agents, anti-retroviral agents and anti-tumor agents
US5877185A (en) * 1991-10-22 1999-03-02 Octamer, Inc. Synergistic compositions useful as anti-tumor agents
US5783599A (en) * 1993-02-24 1998-07-21 Octamer Inc Methods of treating cancer and viral infections with 5-iodo-6-amino-and 5-iodo-6-nitroso-1 2-benzopyrones

Also Published As

Publication number Publication date
FR2440948A1 (en) 1980-06-06
NL7907983A (en) 1980-05-08
GR68055B (en) 1981-10-29
ATA712979A (en) 1983-02-15
CA1113948A (en) 1981-12-08
YU40580B (en) 1986-02-28
DE2944376A1 (en) 1980-05-14
AT372380B (en) 1983-09-26
PT70412A (en) 1979-12-01
GB2036017B (en) 1983-03-23
ES485745A1 (en) 1980-07-01
BE879821A (en) 1980-03-03
CH641796A5 (en) 1984-03-15
IT7829466A0 (en) 1978-11-06
IT1100069B (en) 1985-09-28
ZA795805B (en) 1980-10-29
JPS5569575A (en) 1980-05-26
FI793400A7 (en) 1981-01-01
YU269679A (en) 1983-01-21
FR2440948B1 (en) 1983-06-24

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PCNP Patent ceased through non-payment of renewal fee

Effective date: 19941105