CH307809A - Process for the production of a new coumarin derivative. - Google Patents

Process for the production of a new coumarin derivative.

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Publication number
CH307809A
CH307809A CH307809DA CH307809A CH 307809 A CH307809 A CH 307809A CH 307809D A CH307809D A CH 307809DA CH 307809 A CH307809 A CH 307809A
Authority
CH
Switzerland
Prior art keywords
production
oxy
parts
chloro
water
Prior art date
Application number
Other languages
German (de)
Inventor
F Hoffmann- Aktiengesellschaft
Original Assignee
Hoffmann La Roche
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 Hoffmann La Roche filed Critical Hoffmann La Roche
Publication of CH307809A publication Critical patent/CH307809A/en

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Classifications

    • 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
    • C07D311/42Benzo[b]pyrans, not hydrogenated in the carbocyclic ring with oxygen or sulfur atoms in positions 2 and 4
    • C07D311/44Benzo[b]pyrans, not hydrogenated in the carbocyclic ring with oxygen or sulfur atoms in positions 2 and 4 with one hydrogen atom in position 3
    • C07D311/46Benzo[b]pyrans, not hydrogenated in the carbocyclic ring with oxygen or sulfur atoms in positions 2 and 4 with one hydrogen atom in position 3 unsubstituted in the carbocyclic ring

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Pyrane Compounds (AREA)
  • Plural Heterocyclic Compounds (AREA)

Description

  

  Verfahren zur Herstellung eines neuen     Cumarinderivates.       Die vorliegende Erfindung betrifft ein  Verfahren zur Herstellung von     Cumarinderi-          vaten    der allgemeinen     Formel     
EMI0001.0005     
    worin R einen     Alkylrest    (vorzugsweise den       Äthylrest)    bedeutet.  



  Gemäss der vorliegenden Erfindung wer  den diese Verbindungen dadurch erhalten,  dass man auf ein     3-Acyl-4-oxy-cumarin    der  allgemeinen Formel  
EMI0001.0009     
    worin R einen     Alkylrest    bedeutet,     p-Chlor-          phenyl-magnesiumjodid    einwirken lässt, aus  der entstandenen Verbindung Wasser abspal  tet und das gebildete Reaktionsprodukt hy  driert.  



  Als Ausgangsmaterial dient, ein     3-Aeyl-          4-oxy-eumarin.    Es können beispielsweise 3  Acetyl-,     3-Propionyl-,        3-Butyroyl-4-oxy-euma-          rin    als Ausgangsmaterialien verwendet wer  den, die nach einer bereits beschriebenen Me  thode hergestellt werden. (J. Am.     Chem.        Soc.       72 [1950], Seite 5143; J.     Chem.        Soc.    London,  1950, Seite 903; Annalen 347 [1906], Seite<B>1).</B>  



  Man lässt auf die Ausgangsverbindung       p-Chlor-phenylmagnesiumjodid    einwirken, wo  bei zur Blockierung des aktiven Wasserstoff  atoms der vierständigen     Hydroxylgruppe    ein       Übersehuss    des     Chlorphenylderivates    verwen  det wird. Das hierbei entstehende tertiäre       Carbinol    der Formel  
EMI0001.0027     
    braucht nicht isoliert zu werden, sondern  kann sofort der     Dehydratisierung    unterwor  fen werden.

   Man bewerkstelligt diese     Dehy-          dratisierung    vorzugsweise durch Erhitzen des       Carbinols    mit geringen Mengen     p-Toluolsulfo-          säure    in     Toluol,    wobei das entstehende Was  ser durch     azeotrope    Destillation mit dem To  luol fortlaufend entfernt wird. Das für die  Wasserabspaltung     benötigte    Wasserstoffatom  wird von der ersten     CH2-Gruppe    des     Alkyl-          restes    R des tertiären     Carbinols    geliefert.  



  Die ungesättigte Verbindung kann isoliert  oder auch ohne Isolierung nach der Wasser  abspaltung direkt der Hydrierung unterwor  fen werden. Man. hydriert vorzugsweise in       Dioxan    oder     Äthylalkohol    in Gegenwart von       Palladium-Kohle    oder     Raney-Nickel.         Die .erfindungsgemäss hergestellten Ver  bindungen stellen weisse, kristallisierte Sub  stanzen dar.

   Sie sind schwer löslich in Was  ser und mässig löslich in den gebräuchlichen       organisehen    Lösungsmitteln.     Pharmakologiseh     zeichnen sie sich dadurch aus,     dass    sie den       Prothrombinspiegel    des Blutes in ganz gerin  gen Konzentrationen zu senken vermögen.  



  Gegenstand des Patentes ist nun ein Ver  fahren zur Herstellung von     3-(1'-p-Chlor-          phenyl-propyl)-4-oxy-cumarin,    das dadurch  gekennzeichnet ist, dass man auf     3-Propionyl-          4-oxy-cumarin        p-Chlor-phenyl-magnesium-          jodid    einwirken lässt, die erhaltene     Organo-          metallv        erbindung    hydrolytisch zersetzt, aus  dem entstandenen     Carbinol    Wasser abspaltet  und das gebildete Reaktionsprodukt hydriert.

         Beispiel:     In einer aus 3,8 Gewichtsteilen Magne  sium und 36 Gewichtsteilen     p-Chlor-jodben-          zol    in etwa. 400 Raumteilen absolutem Äther  wie üblich zubereiteten     p-Chlor-pheriylmagne-          siumjodidlösung    werden unter Rühren 10,3  Gewichtsteile     3-Propionyl-4-oxy-cumarin    ein  ; getragen und 3 Stunden lang unter     Rüek-          fluss    gekocht.     1NTan    zersetzt mit einem Gemisch  von 15 Raumteilen konzentrierter Salzsäure  und 400 Raumteilen Wasser.

   Die Ätherschicht  wird mit. 200 Raumteilen     3n-Natronlauge        aus-          a    geschüttelt, die     wässerigalkalische    Schicht mit  50 Raumteilen     Toluol    gewaschen und hernach  mit konzentrierter Salzsäure vorsichtig ange  säuert. Das hierbei ausfallende Öl wird in 200       Raiunteilen        Toluol    aufgenommen, die     Toluol-          lösung    mit 100 mg     p-Toluolsulfosäure    versetzt    und am Wassersehender so lange am Rückfloss  gekocht, bis sich keine     Wassertröpfehen    mehr  abscheiden.

   Hierauf wird die     Toluollösung    im  Vakuum bei 40-50  C eingedampft und der  Rückstand in 200 Raumteilen Alkohol gelöst,.  wobei sich 0,3-0,4     Gewiehtsteile    unveränder  tes     3-Propionyl-4-oxy-cuniarin    absehenden, die  durch Filtration entfernt werden. Aus dem  Filtrat wird der Alkohol im Vakuum ver  dampft und das     zurüekbleibende    Harz mit .  Äther     angeteigt.    Hierbei erfolgt die     Abschei-          dungvon        3-[a-(4'-Chlor-pbenyl)-prop-l-enyl]-          4-oxy-cumarin.        Sehmelzpunkt    203-204  C.  



  3,7     Gewiehtsteile    dieser Verbindung wer  den in     .50    Raumteilen     Dioxan    gelöst und un  ter     Zusatz    von     Raney-Niekel    hydriert. Die  für die Hydrierung der     Doppelbindung    be  nötigte Wasserstoffmenge ist in etwa.     30-40     Minuten aufgenommen.

   Nach     Abfiltrieren    des  Katalysators, Abdampfen des     Dioxans    im Va  kuum und     Umkristallisieren    aus     Toluol    er  hält man das     3-(l.'-p-Chlor-phenyl-propyl)-4-          oxy-cumarin    in weissen Kristallen vom  Schmelzpunkt 186-188  C.



  Process for the production of a new coumarin derivative. The present invention relates to a process for the preparation of coumarin derivatives of the general formula
EMI0001.0005
    where R is an alkyl radical (preferably the ethyl radical).



  According to the present invention, these compounds are obtained by using a 3-acyl-4-oxy-coumarin of the general formula
EMI0001.0009
    where R is an alkyl radical, p-chlorophenylmagnesium iodide can act, water is split off from the compound formed and the reaction product formed is hydrogenated.



  The starting material is a 3-ayl-4-oxy-eumarin. For example, 3-acetyl, 3-propionyl, 3-butyroyl-4-oxy-eumarin can be used as starting materials, which are produced by a method already described. (J. Am. Chem. Soc. 72 [1950], page 5143; J. Chem. Soc. London, 1950, page 903; Annalen 347 [1906], page <B> 1). </B>



  The starting compound p-chlorophenylmagnesium iodide is allowed to act, where an excess of the chlorophenyl derivative is used to block the active hydrogen atom of the tetravalent hydroxyl group. The resulting tertiary carbinol of the formula
EMI0001.0027
    does not need to be isolated, but can be subjected to dehydration immediately.

   This dehydration is preferably accomplished by heating the carbinol with small amounts of p-toluenesulfonic acid in toluene, the resulting water being continuously removed by azeotropic distillation with the toluene. The hydrogen atom required for dehydration is supplied by the first CH2 group of the alkyl radical R of the tertiary carbinol.



  The unsaturated compound can be subjected to the hydrogenation directly after the water has been split off, either isolated or without isolation. Man. hydrogenated preferably in dioxane or ethyl alcohol in the presence of palladium-carbon or Raney nickel. The compounds produced in accordance with the invention are white, crystallized substances.

   They are sparingly soluble in water and moderately soluble in common organic solvents. Pharmacologically, they are distinguished by the fact that they are able to lower the prothrombin level in the blood in very low concentrations.



  The subject of the patent is now a process for the production of 3- (1'-p-chlorophenyl-propyl) -4-oxy-coumarin, which is characterized in that 3-propionyl-4-oxy-coumarin p -Chlor-phenyl-magnesium iodide to act, the resulting organometallic compound is hydrolytically decomposed, water is split off from the resulting carbinol and the reaction product formed is hydrogenated.

         Example: In one made of 3.8 parts by weight of magnesium and 36 parts by weight of p-chloro-iodobenzene, roughly. 400 parts by volume of absolute ether, p-chloro-pheriylmagnesium iodide solution prepared as usual, are mixed in with 10.3 parts by weight of 3-propionyl-4-oxycoumarin; worn and cooked under reflux for 3 hours. 1NTan decomposes with a mixture of 15 parts by volume of concentrated hydrochloric acid and 400 parts by volume of water.

   The ether layer is with. 200 parts by volume of 3N sodium hydroxide solution are shaken out, the aqueous-alkaline layer is washed with 50 parts by volume of toluene and then carefully acidified with concentrated hydrochloric acid. The oil which precipitates out is taken up in 200 raiunteile of toluene, 100 mg of p-toluenesulfonic acid are added to the toluene solution and refluxed on the water-seizing unit until no more water droplets separate.

   The toluene solution is then evaporated in vacuo at 40-50 ° C. and the residue is dissolved in 200 parts by volume of alcohol. 0.3-0.4 parts by weight of unchanged 3-propionyl-4-oxy-cuniarin, which are removed by filtration. The alcohol is evaporated from the filtrate in vacuo and the resin that remains with it. Ether made into a paste. This results in the separation of 3- [a- (4'-chloro-pbenyl) -prop-1-enyl] -4-oxycoumarin. Sea melting point 203-204 C.



  3.7 parts by weight of this compound are dissolved in .50 parts by volume of dioxane and hydrogenated under the addition of Raney-Niekel. The amount of hydrogen required for the hydrogenation of the double bond is approximately. Recorded for 30-40 minutes.

   After filtering off the catalyst, evaporating the dioxane in vacuo and recrystallizing it from toluene, the 3- (l'- p-chloro-phenyl-propyl) -4-oxy-coumarin is obtained in white crystals with a melting point of 186-188 C.

 

Claims (1)

.Verfahren PATENTANSPRUCH: zur Herstellung von 3-(1'-p- Chlor-phenyl-propyl)-4-oxy-eitmarin, dadurch gekennzeichnet, dass man auf 3-Propionyl-4- oxy-eumarin p-Chlor-phenyl-magnesiumjodid einwirken lässt, die erhaltene Organometall- verbindung hydrolytisch zersetzt, aus dem entstandenen Carbinol Wasser abspaltet und das gebildete Reaktionsprodukt hydriert. .Process PATENT CLAIM: for the production of 3- (1'-p-chloro-phenyl-propyl) -4-oxy-eitmarin, characterized in that p-chloro-phenyl-magnesium iodide is used on 3-propionyl-4-oxy-eumarin lets act, the resulting organometallic compound is hydrolytically decomposed, water is split off from the resulting carbinol and the reaction product formed is hydrogenated. Die neue Verbindung bildet weisse Kri stalle, die bei 186-188 C schmelzen. The new compound forms white crystals that melt at 186-188 C.
CH307809D 1952-08-25 1952-08-25 Process for the production of a new coumarin derivative. CH307809A (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CH307809T 1952-08-25

Publications (1)

Publication Number Publication Date
CH307809A true CH307809A (en) 1955-06-15

Family

ID=4493285

Family Applications (1)

Application Number Title Priority Date Filing Date
CH307809D CH307809A (en) 1952-08-25 1952-08-25 Process for the production of a new coumarin derivative.

Country Status (1)

Country Link
CH (1) CH307809A (en)

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