NO790116L - INTERMEDIATE PRODUCTS FOR USE IN THE MANUFACTURE OF THERAPEUTIC ACTIVE COMPOUNDS - Google Patents

INTERMEDIATE PRODUCTS FOR USE IN THE MANUFACTURE OF THERAPEUTIC ACTIVE COMPOUNDS

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Publication number
NO790116L
NO790116L NO790116A NO790116A NO790116L NO 790116 L NO790116 L NO 790116L NO 790116 A NO790116 A NO 790116A NO 790116 A NO790116 A NO 790116A NO 790116 L NO790116 L NO 790116L
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Norway
Prior art keywords
compound
ethyl
formula
active compounds
manufacture
Prior art date
Application number
NO790116A
Other languages
Norwegian (no)
Inventor
Peter Bamberg
Thore Oskar Vaerner Rydh
Jan Urban Stenhede
Original Assignee
Astra Pharma Prod
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.)
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Publication date
Application filed by Astra Pharma Prod filed Critical Astra Pharma Prod
Publication of NO790116L publication Critical patent/NO790116L/en

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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C237/00Carboxylic acid amides, the carbon skeleton of the acid part being further substituted by amino groups
    • C07C237/02Carboxylic acid amides, the carbon skeleton of the acid part being further substituted by amino groups having the carbon atoms of the carboxamide groups bound to acyclic carbon atoms of the carbon skeleton
    • C07C237/04Carboxylic acid amides, the carbon skeleton of the acid part being further substituted by amino groups having the carbon atoms of the carboxamide groups bound to acyclic carbon atoms of the carbon skeleton the carbon skeleton being acyclic and saturated

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)
  • Acyclic And Carbocyclic Compounds In Medicinal Compositions (AREA)

Description

Mellomprodukter for bruk ved fremstilling av terapeutisk virksomme forbindelser. Intermediates for use in the manufacture of therapeutically active compounds.

Foreliggende oppfinnelse vedrører nye forbindelser,The present invention relates to new compounds,

en fremgangsmåte til fremstilling av disse og deres bruk som mellomprodukter ved fremstilling av terapeutisk virksomme forbindelser. a method for the production of these and their use as intermediates in the production of therapeutically active compounds.

Formålet med oppfinnelsen er å tilveiebringe et mellom-produkt som muliggjør fremstilling av terapeutisk virksomme forbindelser med forbedret økonomi og uten bruk i prosessen av forbindelser som er helsefarlige. Et annet formål med oppfinnelsen er å tilveiebringe en fremgangsmåte til fremstilling av terapeutisk virksomme forbindelser via en ny reaksjonsvei under anvendelse av nevnte nye mellomprodukter. The purpose of the invention is to provide an intermediate product that enables the production of therapeutically effective compounds with improved economy and without the use in the process of compounds that are hazardous to health. Another object of the invention is to provide a method for the production of therapeutically active compounds via a new reaction pathway using said new intermediates.

I norsk patent nr. 135.934 beskrives bl.a. en forbindelse med formelen: som er nyttig som et lengevirkende lokalanestetikum, samt en fremgangsmåte til fremstilling av denne forbindelse omfattende omsetting av en forbindelse med formelen: Norwegian patent no. 135,934 describes, among other things, a compound of the formula: which is useful as a long-acting local anesthetic, as well as a process for the preparation of this compound comprising reacting a compound of the formula:

med propylamin og omsetning av den således, oppnådde forbindelse med dietylsulfat. with propylamine and reaction of the thus obtained compound with diethyl sulfate.

En ulempe med denne kjente metode er at det bare oppnås et lite totalt utbytte. Hovedulempen er imidlertid toksisiteten av dietylsulfat som er en forbindelse som benyttes i prosessens siste trinn. Dietylsulfat antas å forårsake kreft, selv i lave konsentrasjoner. Utsettelse for dette stoff bør dermed hindres eller i det minste holdes ved et absolutt minimum. A disadvantage of this known method is that only a small total yield is achieved. The main disadvantage, however, is the toxicity of diethyl sulfate, which is a compound used in the last step of the process. Diethyl sulfate is thought to cause cancer, even in low concentrations. Exposure to this substance should therefore be prevented or at least kept to an absolute minimum.

Foreliggende oppfinnelse tilveiebringer nye forbindelser som benyttet som mellomprodukter ved fremstilling av den ovenfor angitte terapeutisk virksomme forbindelse med formel I, gir forbedret utbytte av nevnte forbindelse. Fremgangsmåten hvori man anvender de nye forbindelsene unngår videre bruk av det helsefarlige stoff dietylsulfat. Forbindelsene ifølge foreliggende oppfinnelse er forbindelser med strukturformelen: The present invention provides new compounds which, used as intermediates in the preparation of the above-mentioned therapeutically active compound of formula I, provide improved yield of said compound. The method in which the new compounds are used avoids further use of the hazardous substance diethyl sulphate. The compounds according to the present invention are compounds with the structural formula:

eller et salt derav, hvor R er metyl eller etyl. or a salt thereof, where R is methyl or ethyl.

Forbindelsene ifølge oppfinnelsen kan fremstilles ved omsetning av en ester av a-bromsmørsyre: The compounds according to the invention can be prepared by reacting an ester of α-bromobutyric acid:

hvor R er metyl eller etyl, med N-etyl-N-n-propylamin. where R is methyl or ethyl, with N-ethyl-N-n-propylamine.

Reaksjonen utføres hensiktsmessig ved å kombinere de to reaktantene i et organisk oppløsningsmiddel, slik som acetonitril, etanol, toluen, dimetylformamid eller xylen, fortrinns-vis acetonitril eller etanol, og underkaste blandingen for forsiktig tilbakeløpskoking. Valget av temperatur er ikke av-gjørende, men for å oppnå et optimalt utbytte, bør blandingen tilbakeløpskokes forsiktig. The reaction is conveniently carried out by combining the two reactants in an organic solvent, such as acetonitrile, ethanol, toluene, dimethylformamide or xylene, preferably acetonitrile or ethanol, and subjecting the mixture to gentle reflux. The choice of temperature is not decisive, but to achieve an optimal yield, the mixture should be carefully refluxed.

Fremstilling av den terapeutisk virksomme forbindelse Preparation of the therapeutically active compound

kan utføres på følgende måte.can be carried out in the following way.

Magnesiumspon behandles, med en forbindelse med formelen: Magnesium shavings are treated with a compound of the formula:

hvor R"*" er en alkylgruppe med 1-8 karbonatomer, slik som propyl eller oktyl, en cykloheksylgruppe eller en benzylgruppe og X where R"*" is an alkyl group with 1-8 carbon atoms, such as propyl or octyl, a cyclohexyl group or a benzyl group and X

er klorid, bromid eller jodid. Den oppnådde Grignard-reagens omsettes deretter med m-xylidin. Forbindelsen med formel III ifølge oppfinnelsen, oppløst i et organisk oppløsningsmiddel, slik som toluen, tetrahydrofuran, xylen eller eter, fortrinns-vis toluen, tilsettes deretter til blandingen og blandingen oppvarmes. Valget av temperatur er ikke avgjørende, men for å- oppnå et optimalt utbytte bør man velge en temperatur på omkring 105°C når toluen anvendes som oppløsningsmiddel, omkring 13 0°C'når xylen benyttes og omkring 65°C når tetrahydrofuran benyttes. Etter avkjøling kan sluttforbindelsen med formel I fra-separeres. is chloride, bromide or iodide. The Grignard reagent obtained is then reacted with m-xylidine. The compound of formula III according to the invention, dissolved in an organic solvent, such as toluene, tetrahydrofuran, xylene or ether, preferably toluene, is then added to the mixture and the mixture is heated. The choice of temperature is not decisive, but in order to achieve an optimal yield one should choose a temperature of around 105°C when toluene is used as solvent, around 130°C when xylene is used and around 65°C when tetrahydrofuran is used. After cooling, the final compound of formula I can be separated from.

Reaksjonsveien for fremstilling av den terapeutisk virksomme forbindelse illustreres ved nedenstående reaksjonsskjema: The reaction pathway for producing the therapeutically active compound is illustrated by the reaction scheme below:

hvor r\ X og R har de ovenfor angitte betydninger. where r\ X and R have the meanings indicated above.

Reaksjonene kan utføres i en oppløsning med eller uten isolering av mellomproduktene. The reactions can be carried out in a solution with or without isolation of the intermediate products.

Fremgangsmåten til fremstilling den terapeutisk virksomme forbindelse med formelen: The procedure for producing the therapeutically active compound with the formula:

eller et terapeutisk akseptabelt salt derav, kjennetegnet ved at en forbindelse med formelen: hvor R er metyl eller etyl, omsettes med en forbindelse med formelen: or a therapeutically acceptable salt thereof, characterized in that a compound of the formula: where R is methyl or ethyl, is reacted with a compound of the formula:

hvor X er klorid, bromid eller jodid, utgjør et ytterligere trekk ved oppfinnelsen. where X is chloride, bromide or iodide, constitutes a further feature of the invention.

Den terapeutisk virksomme sluttforbindelse I,samt forbindelsen med formel III ifølge oppfinnelsen, er optisk aktive forbindelser og de d- eller 1-optiske isomerer og blandinger derav inkludert racematet, omfattes således av oppfinnelsen. The therapeutically effective final compound I, as well as the compound with formula III according to the invention, are optically active compounds and the d- or 1-optical isomers and mixtures thereof including the racemate, are thus covered by the invention.

Oppfinnelsen illustreres ytterligere ved følgende eksempler. The invention is further illustrated by the following examples.

Eksempel 1Example 1

g-( N- etyl- N- n- propylamin)- smørsyremetylesterg-(N-ethyl-N-n-propylamine)-butyric acid methyl ester

En blanding av ct-bromsmørsyremetylester (26, 25 g, 0,145 mol) og N-etyl-N-n-propylamin (25,2 g, 0,29 mol) i acetonitril (130 ml), ble oppvarmet til svak tilbakeløpskoking natten over. Deretter ble oppløsningsmidlet inndampet og eter tilsatt til resten. Det utfelte etylpropylaminhydrobromid ble fjernet ved . filtrering, filtratet ble vasket méd vann og saltoppløsning, tørket og strippet. Det resterende oljeaktige råprodukt ble deretter fraksjonert og dette ga 19,2 g (Kp 85-90°C/13 mm Hg), 70,8%. A mixture of ct-bromobutyric acid methyl ester (26, 25 g, 0.145 mol) and N-ethyl-N-n-propylamine (25.2 g, 0.29 mol) in acetonitrile (130 mL) was heated to gentle reflux overnight. The solvent was then evaporated and ether added to the residue. The precipitated ethylpropylamine hydrobromide was removed at . filtration, the filtrate was washed with water and saline, dried and stripped. The remaining oily crude product was then fractionated and this gave 19.2 g (Kp 85-90°C/13 mm Hg), 70.8%.

Eksempel 2Example 2

a-( N- etyl- N- n- propylamin)- smørsyreetylesteren,a-(N-ethyl-N-n-propylamine)-butyric acid ethyl ester,

ble oppnådd på samme måte som beskrevet i eksempel 1 fra g-brom-smørsyreetylester (85,8 g, 0,44 mol) og N-etyl-N-n-propylamin (75,4 g, 86,6 mol) i .acetonitril (400 ml), utbytte 69 g, 78%, was obtained in the same manner as described in Example 1 from g-bromobutyric acid ethyl ester (85.8 g, 0.44 mol) and N-ethyl-N-n-propylamine (75.4 g, 86.6 mol) in acetonitrile ( 400 ml), yield 69 g, 78%,

Kp 83-85°C/ll mm Hg.Kp 83-85°C/ll mm Hg.

Eksempel 3Example 3

et- ( N- etyl- N- n- propylamin) - smørsyreetylesteret-(N-ethyl-N-n-propylamine)-butyric acid ethyl ester

En blanding av a-bromsmørsyreetylester (63,2 g, 0,32 mol) og N-etyl—N-propylamin (55,9 g, 0,64 mol) i etanol (500 ml) A mixture of α-bromobutyric acid ethyl ester (63.2 g, 0.32 mol) and N-ethyl-N-propylamine (55.9 g, 0.64 mol) in ethanol (500 mL)

ble oppvarmet til svak tilbakeløpskoking i 22 timer. Oppløs-ningsmidlet ble inndampet, resten ble opptatt i eter (3 00 ml) was heated to gentle reflux for 22 hours. The solvent was evaporated, the residue was taken up in ether (300 ml).

og oppløsningen ble vasket med vann (2 x 50 ml) . Den organiske fasen ble ekstrahert med 2 N saltsyre (150 + 70 ml). Den sure fasen ble vasket med eter, nøytralisert med natriumbikarbonat og det oljeaktige produkt ble ekstrahert med eter (150 + 2 x 50 ml) . De kombinerte eter lag b.le vasket med vann og saltoppløsning, tørket og strippet. Resten ble destillert over en Vigreux-kolonne ved et trykk på 12 mm Hg og dette ga 39,5 g (60,7%) and the solution was washed with water (2 x 50 ml). The organic phase was extracted with 2 N hydrochloric acid (150 + 70 ml). The acid phase was washed with ether, neutralized with sodium bicarbonate and the oily product was extracted with ether (150 + 2 x 50 ml). The combined ether layers were washed with water and saline, dried and stripped. The residue was distilled over a Vigreux column at a pressure of 12 mm Hg and this gave 39.5 g (60.7%)

av produktet som kokte ved 88-9 0°C.of the product which boiled at 88-9 0°C.

Eksempel 4Example 4

ot- ( N- etyl- N- n- propylamino) - smørsyre 2, 6- dimetylanilid ot-( N- ethyl- N- n- propylamino) - butyric acid 2, 6- dimethylanilide

Magnesiumspon (0,61 g, 0,025 mol) i tetrahydrofuranMagnesium shavings (0.61 g, 0.025 mol) in tetrahydrofuran

(THF) (5 ml) ble behandlet i en nitrogenatmosfære med noen dråper av en oppløsning av n-propylbromid (2,3 ml, 0,0 25 mol) (THF) (5 mL) was treated under a nitrogen atmosphere with a few drops of a solution of n-propyl bromide (2.3 mL, 0.0 25 mol)

i THF (15 ml) for å starte en Grignard-reaksjon. Reaksjonen ble deretter holdt ved omkring tilbakeløpstemperatur ved tilsetning av propylbromidoppløsningen. Deretter ble m-xylidin (3,1 ml, 0,025 mol) i THF (10 ml) tilsatt dråpevis hvorved temperaturen steg til ca. 50°C. Etter at tilsetningen var ferdig, ble blandingen oppvarmet slik at en del av THF-materialet startet å destillere. Samtidig ble a-(N-etyl-N-n-propylamino)-smørsyre-etylester (2 g, 0,01 mol) i toluen (12 ml) tilsatt dråpevis. Etter ferdig tilsetning ble mer toluen (10 ml) tilsatt og blandingen ble oppvarmet inntil destillatets kokepunkt nådde 105°C. Deretter fikk blandingen avkjøles til 30°C og vann (20 ml) ble tilsatt. Oppløsningen over det dannede bunnfall ble frasepa-rert og resten ble triturert flere ganger med eter. Den kombinerte organiske fase ble dampdestillert. for å fjerne over-skudd, m-xylidin. Fra den resterende vannfase ble produktet ekstrahert med metylenklorid. Utbytte 2,4 gi form av gule' krystaller, 98,1% renhet (GLC), dvs. 85,2% av det teoretiske utbytte. in THF (15 mL) to initiate a Grignard reaction. The reaction was then maintained at about reflux temperature by addition of the propyl bromide solution. Then m-xylidine (3.1 ml, 0.025 mol) in THF (10 ml) was added dropwise whereby the temperature rose to approx. 50°C. After the addition was complete, the mixture was heated so that some of the THF material began to distill. At the same time, α-(N-ethyl-N-n-propylamino)-butyric acid ethyl ester (2 g, 0.01 mol) in toluene (12 ml) was added dropwise. After the addition was complete, more toluene (10 ml) was added and the mixture was heated until the boiling point of the distillate reached 105°C. The mixture was then allowed to cool to 30°C and water (20 ml) was added. The solution above the formed precipitate was separated and the residue was triturated several times with ether. The combined organic phase was steam distilled. to remove excess, m-xylidine. From the remaining aqueous phase, the product was extracted with methylene chloride. Yield 2.4 in the form of yellow crystals, 98.1% purity (GLC), i.e. 85.2% of the theoretical yield.

Dette materiale ble oppløst i aceton (10 ml) og konsen-trert saltsyre (1 ml) ble tilsatt.. Hydrokloridet utkrystalli- serte seg etter avkjøling ved 0-5°C natten over, i form av hvite krystaller i en mengde på 1,8 g og med smeltepunkt 199-200°C. Den ovenfor angitte ønskede forbindelse ble oppnådd på s-amme måte som beskrevet ovenfor under anvendelse av oktylbromid eller benzylklorid som reagens for Gr,ignard-reaksjonen. This material was dissolved in acetone (10 ml) and concentrated hydrochloric acid (1 ml) was added. The hydrochloride crystallized after cooling at 0-5°C overnight, in the form of white crystals in an amount of 1, 8 g and with a melting point of 199-200°C. The desired compound indicated above was obtained in the same manner as described above using octyl bromide or benzyl chloride as reagent for the Grignard reaction.

Claims (3)

1. Forbindelse, karakterisert ved den ■ strukturelle formel:1. Compound, characterized by the ■ structural formula: eller et salt derav, hvor R er metyl eller etyl. or a salt thereof, where R is methyl or ethyl. 2. Fremgangsmåte til fremstilling av en forbindelse som definert i krav 1, karakterisert ved at en ester av a-bromsmørsyre.med formelen: 2. Process for producing a compound as defined in claim 1, characterized in that an ester of α-bromobutyric acid with the formula: hvor R er metyl eller etyl, omsettes med N-etyl-N-propylamin.where R is methyl or ethyl, is reacted with N-ethyl-N-propylamine. 3. Fremgangsmåte til fremstilling av en terapeutisk virksom forbindelse med formelen: 3. Method for producing a therapeutically active compound with the formula: eller et terapeutisk akseptabelt salt derav, karakterisert ved at en forbindelse med formelen: or a therapeutically acceptable salt thereof, characterized in that a compound of the formula: hvor R er metyl eller etyl, omsettes med en forbindelse med formelen: where R is methyl or ethyl, is reacted with a compound of the formula: hvor X er klorid, bromid eller jodid.where X is chloride, bromide or iodide.
NO790116A 1978-01-30 1979-01-15 INTERMEDIATE PRODUCTS FOR USE IN THE MANUFACTURE OF THERAPEUTIC ACTIVE COMPOUNDS NO790116L (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
SE7801062A SE424442B (en) 1978-01-30 1978-01-30 ESTARS OF ALFA (N-ETHYL-N-N-PROPYLAMIN) -BUTY ACID FOR USE AS INTERMEDIATES IN THE PREPARATION OF THERAPEUTICALLY ACTIVE COMPOUNDS

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NO790116L true NO790116L (en) 1979-07-31

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JP (1) JPS54112821A (en)
AT (1) AT367393B (en)
DK (1) DK20879A (en)
ES (1) ES477051A1 (en)
FI (1) FI790229A7 (en)
IT (1) IT1116533B (en)
NL (1) NL7900643A (en)
NO (1) NO790116L (en)
SE (1) SE424442B (en)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3401969A (en) * 1966-10-28 1968-09-17 Forest J. Neel Safety chain locking device
US3544154A (en) * 1968-07-26 1970-12-01 Gailerd B Ford Dump truck spreader chain mounting

Also Published As

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FI790229A7 (en) 1979-07-31
SE424442B (en) 1982-07-19
NL7900643A (en) 1979-08-01
AT367393B (en) 1982-06-25
IT7947765A0 (en) 1979-01-24
IT1116533B (en) 1986-02-10
SE7801062L (en) 1979-07-31
ATA59279A (en) 1981-11-15
DK20879A (en) 1979-07-31
ES477051A1 (en) 1979-06-16
JPS54112821A (en) 1979-09-04

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