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GB2239242A - Cyclohexanol derivative - Google Patents

Cyclohexanol derivative Download PDF

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Publication number
GB2239242A
GB2239242A GB9027816A GB9027816A GB2239242A GB 2239242 A GB2239242 A GB 2239242A GB 9027816 A GB9027816 A GB 9027816A GB 9027816 A GB9027816 A GB 9027816A GB 2239242 A GB2239242 A GB 2239242A
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United Kingdom
Prior art keywords
trans
cis
formula
carrying
acetone
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
GB9027816A
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GB2239242B (en
GB9027816D0 (en
Inventor
Ildiko Ratz
Pal Benko
Daniel Bozsing
Antal Tungler
Tibor Mathe
Gyoergy Kovanyi
Jozsef Petro
Ilona Sztruhar
Gyoergyi Vereczkey
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Egyt Gyogyszervegyeszeti Gyar
Egis Pharmaceuticals PLC
Original Assignee
Egyt Gyogyszervegyeszeti Gyar
Egis Pharmaceuticals PLC
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Egyt Gyogyszervegyeszeti Gyar, Egis Pharmaceuticals PLC filed Critical Egyt Gyogyszervegyeszeti Gyar
Publication of GB9027816D0 publication Critical patent/GB9027816D0/en
Publication of GB2239242A publication Critical patent/GB2239242A/en
Application granted granted Critical
Publication of GB2239242B publication Critical patent/GB2239242B/en
Anticipated expiration legal-status Critical
Expired - Fee Related legal-status Critical Current

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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C251/00Compounds containing nitrogen atoms doubly-bound to a carbon skeleton
    • C07C251/02Compounds containing nitrogen atoms doubly-bound to a carbon skeleton containing imino groups
    • C07C251/04Compounds containing nitrogen atoms doubly-bound to a carbon skeleton containing imino groups having carbon atoms of imino groups bound to hydrogen atoms or to acyclic carbon atoms
    • C07C251/06Compounds containing nitrogen atoms doubly-bound to a carbon skeleton containing imino groups having carbon atoms of imino groups bound to hydrogen atoms or to acyclic carbon atoms to carbon atoms of a saturated carbon skeleton
    • C07C251/08Compounds containing nitrogen atoms doubly-bound to a carbon skeleton containing imino groups having carbon atoms of imino groups bound to hydrogen atoms or to acyclic carbon atoms to carbon atoms of a saturated carbon skeleton being acyclic
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2601/00Systems containing only non-condensed rings
    • C07C2601/12Systems containing only non-condensed rings with a six-membered ring
    • C07C2601/14The ring being saturated

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Steroid Compounds (AREA)

Abstract

4-Trans-(N-isopropylidene-amino)-cyclohexanol of formula I <IMAGE> by hydrolizing 4-cis/trans-acetaminocyclohexanol of formula II, <IMAGE> and reacting the thus-obtained 4-cis/trans-aminocyclohexanol of formula III <IMAGE> with acetone, e.g. in situ. The above compound I is an important intermediate for the preparation of ambroxol, which is a bronchosecretolytic agent.

Description

PROCESS FOR THE PREPARATION OF A NOVEL INTERMEDIATE TECHNICAL FIELD The present invention relates to the preparation of novel 4-trans-(N-isopropylidene-amino)-cyclohexanol of formula I
The novel compound of the invention is a valuable intermediate for the preparation of N-(2-amino-3,5-dibromobenzyl)-trans-4aminocyclohexanol, commonly known as ambroxol.
Ambroxol is a very significant and wide-spread bronchosecretolytic agent for the treatment of the respiratory track and bronchial tubes.
SUMMARY OF THE INVENTION According to the invention 4-trans-(N-isopropylideneamino)-cyclohexanol of formula I is prepared by hydrolyzing 4cis/trans-acetamidocyclohexanol of formula II,
then reacting the 4-cis/trans-aminocyclohexanol of formula III thus obtained in situ with acetone, then recovering the product of formula I from the reaction mixture.
DETAILED DESCRIPTION OF THE INVENTION The hydrolysis of 4-cis/trans-acetamidocyclohexanol of formula II is carried out in the presence of a strong base in such a solvent which assures the homogeneity of the reaction mixture. Preferably alkaline metal hydroxide, more preferably sodium hydroxide, can be used as a base.
The reaction can be carried out within wide temperature ranges depending on the solvent or solvent mixture used. The preferred temperature range is 90 to 1200C. The reaction is completed within 6 to 18 hours, the 4-cis/transacetamidocyclohexanol of formula II is formed in almost quantitative yield within 8 hours. The product is led into a solvent-solvent extractor together with the reaction medium. The extraction can be carried out continuously with an inert apolar solvent, preferably with a chlorinated hydrocarbon.
The extraction time, depending on the quality and quantity of solvents, amounts to 8 to 16 hours, preferably (when chloroform is used) to 8 hours.
Then the solvent is distilled off, acetone is added to the 4-cis/trans-acetamidocyclohexanol and the mixture is heated at the boiling point of the reaction mixture. The rate of formation of the Schiff-base is relatively high at this temperature, under optimal conditions it is completed within 2 hours.
Upon cooling the reaction mixture, the desired trans-4 (N-isopropyliden-amino)-cyclohexanol selectively precipitates.
The solid product can be separated by filtration or centrifuging.
The 4-trans-(N-isopropylidene-amino)-cyclohexanol is obtained with good yield without any cis-isomer contamination.
This purity has great significance as the quality control standards of pharmaceutical ingredients allow -to a less and less extent the presence of contaminations derived from intermediates, starting materials, side-products, optionally from isomers.
The intermediate of ambroxol production is 4-transaminocyclohexanol which is separated from the cis/trans isomer mixture. Owing to the above quality requirements the formation of cis isomers and by-products is not desired, their complete removal is a very significant task.
The practical way of synthetizing ambroxol is to use a starting material which is free of cis-isomer at the earliest step of the multi-stage synthesis as the purification of the intermediates of the following synthesis steps requires much more work and time and results in higher losses.
The 4-acetamidocyclohexanol can be prepared from pacetamidophenol by catalytic hydrogenation (Ber. Dtsch. Chem.
Ges. 72, 995 /1939/; J. Am. Chem. Soc. 75, 1345 /1953/; Can. J.
Chem. 48, 2065 /1970/). 4-Acetamidocyclohexanol is present in the reaction mixture in the form of cis and trans isomers depending on the steric position of its amino and hydroxyl groups. The ratio of the formed cis/trans isomers is 1:4 to 1:1 depending on the mode of carrying out the reduction.
The separation of isomers is solved by fractional crystallization from different solvents (US patent specification No. 2,152,960). The most preferred solvents are diethyl ether and acetone.
According to J. Am. Chem. Soc. 75, 1345 (1953) the suitably pure trans isomer can be obtained with a yield of 31 % after 9-fold fractional recrystallization from acetone, while according to the method described in Can. J. Chem. 48, 2065 (1970) the product can be obtained with a yield of only 20-25 % after 4-fold recrystallization from acetone.
The 4-acetamidocyclohexanol prepared by the above methods comprises a significant amount of cis-isomer contamination, as was also proved by our experiments. This contamination results in the corresponding undesired cis-intermediates in the next steps of the synthesis.
The invention is further illustrated by the following, non-limiting examples.
Example 1 Preparation of 4-trans-(N-isopropylidene-amino)-cyclohexanol a) From 4-cis/trans-acetamidocyclohexanol 160 g (4 moles) of sodium hydroxide are dissolved in 640 ml of water then 100 g (0.64 mole) of 4-cis/transacetamidocyclohexanol (trans isomer content: 74 %) are added. The mixture is boiled for 8 hours, whereby a solution is obtained.
Then the solution is cooled to room temperature, led into a continuous solvent-solvent extractor and extracted with 1200 ml of chloroform for 8 hours. The phases are separated, the organic phase is dried over anhydrous magnesium sulfate, filtered with charcoal and the solvent is distilled off.
The thus-obtained crude 4-cis/trans-aminocyclohexanol are boiled for 2 hours in 650 ml (8.87 moles) of acetone. A solution is - obtained from which 4-trans-(N-isopropylidene-amino)cyclohexanol precipitates upon cooling in the form of white crystals.
Yield: 45 g (62 % calculated for the trans-isomer of the starting material) Melting point: 151 OC.
b) From 4-cis/trans-aminocyclohexanol 34.55 g (0.3 mole) of 4-cis/trans-aminocyclohexanol (trans-isomer content: 60 %) are boiled with 220 ml of acetone for 2 hours. The white 4-trans-(N-isopropylidene-amino)cyclohexanol precipitating from the solution is filtered off and dried. Thus 22.72 g (74 %) of pure trans-isomer are obtained.
Melting point: 151 OC.
Example 2 Preparation of the starting 4-cis/trans-acetamidocyclohexanol 4.5 g of palladium-on-charcoal catalyst wetted with 10 % by volume of water, 0.6 g (0.006 g mole) of potassium acetate dissolved in 10 ml of water and 150 g (0.99 mole) of pacetamidophenol are charged into an acid-resistant autoclave supplied with a turbo stirrer. The volume of the solution is supplemented to 450 ml. The reaction mixture is hydrogenated under a pressure of 5 bar at a temperature of 120-130 OC for about 6 hours. At the end of the reaction the catalyst is filtered off and the aqueous solution is evaporated to dryness.
Thus 155.2 g (99 %) of white, crystalline product are obtained whose trans-isomer content amounts to 74 %.
Melting point: 142 OC.
4-trans(N-isopropylidene-amino)-cyclohexanol may be reacted to form Amrboxol by a process described in a copending Application filed on 21st December, 1990 and claiming priority from Hungarian Patent Application No. 6745/89.

Claims (11)

1. A process for the preparation of 4-trans-(Nisopropylidene-amino)-cyclohexanol of formula I
w h i c h c o m p r i s e s hydrolizing 4-cis/transacetamidocyclohexanol of formula II,
reacting the thus-obtained 4-cis/trans-aminocyclohexanol of formula III
with acetone (preferably in situ), then recovering the product of formula I thus obtained.
2. A process as claimed in claim 1, w h i c h c o m p r i s e s carrying out the hydrolysis of 4-cis/transacetamidocyclohexanol of formula II with the aid of an alkaline metal hydroxide, preferably sodium hydroxide.
3. A process as claimed in claim 2, w h i c h c o m p r i s e s carrying out the hydrolysis in a solvent ensuring a homogeneous reaction mixture.
4. A process as claimed in claim 3, w h i c h c o m p r i s e s carrying out the hydrolysis in an aqueous medium.
5. A process as claimed in any of claims 2 to 4, w h i c h c o m p r i s e s carrying out the reaction at a temperature of 90 to 120 OC.
6. A process as claimed in any of claims 2 to 5, w h i c h c o m p r i s e s extracting the 4-cis/transaminocyclohexanol of formula III with an inert apolar solvent.
7. A process as claimed in claim 6, w h i c h c o m p r i s e s using a chlorinated hydrocarbon, preferably chloroform, as inert apolar solvent.
8. A process as claimed in claim 1, w h i c h c o m p r i s e s carrying out the reaction of 4-cis/transaminocyclohexanol of formula III with acetone in situ at the boiling point of the reaction mixture.
9. 4-Trans-(N-isopropylidene-amino)-cyclohexanol of formula I.
10. A process of making a compound of the general formula I substantially as hereinbefore described in Example 1.
11. A process of making a compound of the general Formula I which comprises reacting 4-cis/trans-aminocyclohexanol of the general Formula III with acetone and recovering the compound of the general Formula I thus obtained.
GB9027816A 1989-12-22 1990-12-21 Process and the preparation of cyclohexanol derivatives Expired - Fee Related GB2239242B (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
HU896744A HU208949B (en) 1989-12-22 1989-12-22 Process for producing 4-trans-/4-isopropyliden-amino/-cyclohexanol

Publications (3)

Publication Number Publication Date
GB9027816D0 GB9027816D0 (en) 1991-02-13
GB2239242A true GB2239242A (en) 1991-06-26
GB2239242B GB2239242B (en) 1993-07-21

Family

ID=10971987

Family Applications (1)

Application Number Title Priority Date Filing Date
GB9027816A Expired - Fee Related GB2239242B (en) 1989-12-22 1990-12-21 Process and the preparation of cyclohexanol derivatives

Country Status (5)

Country Link
JP (1) JPH0592945A (en)
AT (1) AT398969B (en)
GB (1) GB2239242B (en)
HU (1) HU208949B (en)
IT (1) IT1246048B (en)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE19745529C1 (en) * 1997-10-15 1999-03-18 Great Lakes Chem Konstanz Gmbh Production of trans-4-amino-cyclohexanol from paracetamol
US7531567B2 (en) 2001-05-28 2009-05-12 Serumwerk Bernburg Ag Use of a medicament containing an effector of the glutathione metabolism together with α-lipoic acid in kidney replacement therapy
CN113402402A (en) * 2021-06-29 2021-09-17 江西荣兴药业有限公司 Method for recovering trans-p-aminocyclohexanol from low-concentration waste liquid

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE19745529C1 (en) * 1997-10-15 1999-03-18 Great Lakes Chem Konstanz Gmbh Production of trans-4-amino-cyclohexanol from paracetamol
EP0909753A3 (en) * 1997-10-15 2000-10-25 Great Lakes Chemical Konstanz GmbH Process for the preparation of trans-4-aminocyclohexanol
US7531567B2 (en) 2001-05-28 2009-05-12 Serumwerk Bernburg Ag Use of a medicament containing an effector of the glutathione metabolism together with α-lipoic acid in kidney replacement therapy
CN113402402A (en) * 2021-06-29 2021-09-17 江西荣兴药业有限公司 Method for recovering trans-p-aminocyclohexanol from low-concentration waste liquid
CN113402402B (en) * 2021-06-29 2023-08-18 江西荣兴药业有限公司 Method for recycling trans-p-aminocyclohexanol from low-concentration waste liquid

Also Published As

Publication number Publication date
IT9022506A0 (en) 1990-12-21
ATA261890A (en) 1994-07-15
AT398969B (en) 1995-02-27
JPH0592945A (en) 1993-04-16
HUT58281A (en) 1992-02-28
IT1246048B (en) 1994-11-07
GB2239242B (en) 1993-07-21
GB9027816D0 (en) 1991-02-13
HU208949B (en) 1994-02-28
IT9022506A1 (en) 1992-06-21
HU896744D0 (en) 1990-03-28

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PCNP Patent ceased through non-payment of renewal fee

Effective date: 19961221