CH318326A - Process for preparing the levoisomers of 1-cyclohexyl-1-phenyl-3-pyrrolidinopropan-1-ol and 1-cyclohexyl-1-phenyl-3-piperidinopropan-1-ol - Google Patents

Process for preparing the levoisomers of 1-cyclohexyl-1-phenyl-3-pyrrolidinopropan-1-ol and 1-cyclohexyl-1-phenyl-3-piperidinopropan-1-ol

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Publication number
CH318326A
CH318326A CH318326DA CH318326A CH 318326 A CH318326 A CH 318326A CH 318326D A CH318326D A CH 318326DA CH 318326 A CH318326 A CH 318326A
Authority
CH
Switzerland
Prior art keywords
cyclohexyl
phenyl
piperidinopropan
pyrrolidinopropan
levo
Prior art date
Application number
Other languages
French (fr)
Inventor
Wallace Adamson Donald
Mark Duffin Walter
Original Assignee
Wellcome Found
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 Wellcome Found filed Critical Wellcome Found
Publication of CH318326A publication Critical patent/CH318326A/en

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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D295/00Heterocyclic compounds containing polymethylene-imine rings with at least five ring members, 3-azabicyclo [3.2.2] nonane, piperazine, morpholine or thiomorpholine rings, having only hydrogen atoms directly attached to the ring carbon atoms
    • C07D295/04Heterocyclic compounds containing polymethylene-imine rings with at least five ring members, 3-azabicyclo [3.2.2] nonane, piperazine, morpholine or thiomorpholine rings, having only hydrogen atoms directly attached to the ring carbon atoms with substituted hydrocarbon radicals attached to ring nitrogen atoms
    • C07D295/08Heterocyclic compounds containing polymethylene-imine rings with at least five ring members, 3-azabicyclo [3.2.2] nonane, piperazine, morpholine or thiomorpholine rings, having only hydrogen atoms directly attached to the ring carbon atoms with substituted hydrocarbon radicals attached to ring nitrogen atoms substituted by singly bound oxygen or sulfur atoms
    • C07D295/084Heterocyclic compounds containing polymethylene-imine rings with at least five ring members, 3-azabicyclo [3.2.2] nonane, piperazine, morpholine or thiomorpholine rings, having only hydrogen atoms directly attached to the ring carbon atoms with substituted hydrocarbon radicals attached to ring nitrogen atoms substituted by singly bound oxygen or sulfur atoms with the ring nitrogen atoms and the oxygen or sulfur atoms attached to the same carbon chain, which is not interrupted by carbocyclic rings
    • C07D295/092Heterocyclic compounds containing polymethylene-imine rings with at least five ring members, 3-azabicyclo [3.2.2] nonane, piperazine, morpholine or thiomorpholine rings, having only hydrogen atoms directly attached to the ring carbon atoms with substituted hydrocarbon radicals attached to ring nitrogen atoms substituted by singly bound oxygen or sulfur atoms with the ring nitrogen atoms and the oxygen or sulfur atoms attached to the same carbon chain, which is not interrupted by carbocyclic rings with aromatic radicals attached to the chain

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Hydrogenated Pyridines (AREA)

Description

  

  Procédé de     préparation    des     lévo-isomères    du       1-cyclohexyl-1-phényl-3-pyrrolidinopropane-1-ol    et du       1-cyclohexyl-1-phényl-3-pipéridinopropane-1-ol       La présente invention a pour objet un pro  cédé de préparation des     lévo-isomères    du     1-          cyclohexyl        -1-phényl-3-pyrrolidinopropane-1-ol     et du     1-cyclohexyl-1-phényl-3-pipéridinopro-          pane-1-ol,

      dans lequel on forme les sels d'addi  tion acides du     1-cyclohexyl-1-phényl-3-pyrro-          lidinopropane-1-ol    et du     1-cyclohexyl-1-phé-          nyl-3-pipéridinopropane-1-ol    avec l'acide     d-tar-          trique.     



  Les composés racémiques     1-cyclohexyl-1-          phényl-3-pyrrolidinopropane-1-oI    et     1-cyclo-          hexyl-1-phényl-3-pipéridinopropane-1-oI    et  leurs sels quaternaires     N-alcoyle    inférieur, par  exemple leurs sels quaternaires     N-méthyle    et       N-éthyle,    sont connus pour avoir des propriétés  spasmolytiques, et les deux premiers composés  mentionnés sont cliniquement employés pour le  traitement symptomatique du     parkinsonisme.     



  On a maintenant trouvé que les     lévo-iso-          mères    de ces composés possèdent des proprié  tés qui les rendent plus précieux comme agents  thérapeutiques que leurs formes racémiques  correspondantes. On a     trouvé'que    les propriétés  semblables à     celles    de l'atropine sont limitées       dans    chacun des cas presque entièrement à ces       lévo-isomères,    les     dextro-isomères        étant    pres  que inactifs et, de plus, ce qui était inattendu,    que le     lévo    isomère, dans chaque cas, n'est pas  plus toxique, en injection intraveineuse chez la  souris,

   que la forme racémique ou la forme  dextrogyre. Les     lévo-isomères    de ces composés  présentent donc un avantage précieux et inat  tendu sur leurs formes racémiques, pour l'em  ploi comme agents d'action semblable à l'atro  pine.  



  Les     1-cyclohexyl-1-phényl-3-pyrrolidino-          propane-1-ol    et     1-cyclohexyl        1-phényl43-pipé-          ridinopropane-1-ol    racémiques (préparés, par  exemple, de la manière décrite par     Adamson,     Journal, of the     Chemical    Society, Londres,  1951, page 52) peuvent être dédoublés:

   en leurs  isomères optiques par toute méthode connue  pouvant être employée pour le dédoublement  d'une base organique ou d'un alcool, par exem  ple en     foimant    le sel avec l'acide     d-tartrique     et séparant les deux sels par     cristallisation    frac  tionnée dans l'alcool éthylique ou     un    mélange  d'alcool     éthylique    et d'acétate d'éthyle. Le     lévo-          isomère    peut être utilisé sous forme de     chlor-          hydrate    ou de- sel de tout acide non toxique  aux doses auxquelles il doit être administré.  



  Les sels quaternaires     N-alcoyle    peuvent  être préparés à partir du     lévo-isomère    selon les  méthodes ordinaires pour former les sels qua-      ternaires à partir des amines tertiaires. Ainsi,  le     méthiodure    ou     l'éthiodure    peuvent être pré  parés en faisant réagir la base     optiquement    ac  tive avec de l'iodure de méthyle ou     die    l'iodure  d'éthyle, respectivement ; les composés quater  naires peuvent avoir comme anion tout radical  acide désiré.  



  Le procédé faisant l'objet de la présente  invention est caractérisé en ce qu'on soumet le  sel d'addition acide correspondant à un procédé  de     cristallisation    fractionnée pour effectuer la  séparation partielle des formes dextrogyre et  lévogyre, on     alcalinise    les liqueurs mères com  binées desdites cristallisations fractionnées qui       contiennent    la forme lévogyre,

   on soumet ces  liqueurs mères     alcalinisées    à     _    un     procédé    de       cristallisation    fractionnée pour isoler la     lévo-          base    et l'obtenir sous une forme pratiquement  exempte de     dextro-isomère.     



  Des exemples de mise en     aeuvre    du procédé  selon l'invention sont donnés ci-après, dans les  quels toutes les températures sont données en  degrés centigrades.  



  <I>Exemple 1</I>  <I>Dédoublement du</I>     1-cyclohexyl-1-phényl-3-          pyrrolidinopropane-1-ol     On a ajouté du     1-cyclohexyl-1-phényl-3-          pyrrolidinopropane-1-ol    (60 g) en solution  dans de l'alcool éthylique chaud (120 cc) à une  solution d'acide     d-tartrique    (30 g) dans de l'al  cool éthylique (100 cc) et laissé cristalliser ;  des enlèvements successifs du corps solide ont  été faits jusqu'à ce qu'il ne se sépare plus  qu'une substance huileuse.

   On peut ajouter gra  duellement de l'éther pour faciliter la     cristalli-          .        sation.    L'huile et la liqueur mère ont été com  binées,     basifiées    avec de l'ammoniaque puis ex  traites avec de l'éther, et la base a été cristalli  sée d'ans de l'alcool éthylique. Les premières  récoltes consistaient en     lévo-base    pure, les sui  vantes en la forme racémique.

   La base     optique-          ment    active     lévo-1-cyclohexyl-1-phényl-3-pyr-          rolidinopropane-1-ol    a un point de fusion de       105-106-    ; [ a ]
EMI0002.0031  
   (C = 0,4 dans  de l'alcool éthylique). Le chlorhydrate, obtenu    par les méthodes     usuelles,    cristallise dans l'al  cool     éthylique-acétate    d'éthyle et a un point de  fusion de 2460 ; [ a ] (C = 0,4  dans du chloroforme).
EMI0002.0034  
    



  <I>Exemple 2</I>  <I>Dédoublement du</I>     1-cyclohexyl-1-phényl-3-          pipéridinopropane-1-ol     Du     1-cyclohexyl-1-phényl-3        -pipéridino-          propane-1-ol    (20 g) a été dissous dans une so  lution d'acide     d-tartrique    (10 g) dans de l'al  cool éthylique (80 cc) et on a laissé     cristalliser    ;  on a fait des     enlèvements    successifs du corps  solide jusqu'à ce     qu'il    ne se sépare plus qu'une  substance huileuse. On peut ajouter graduelle  ment de l'éther pour faciliter la cristallisation.

    L'huile et la liqueur mère ont été combinées,       basifiées    avec de l'ammoniaque, et la base a été  cristallisée dans de l'alcool éthylique. La base       lévo-1-cyclohexyl-1-phényl-3        -pipéridinopro-          pane-1-ol,        optiquement    active, a un point de  fusion de     112-113o    ;

   [a]
EMI0002.0050  
    (C = 0,4 dans de l'alcool     éthylique).    Son     chlor-          hydrate,    obtenu par les méthodes usuelles, cris  tallise dans l'alcool     isopropylique    et a un point       de    fusion de 2640 ;<B>[</B>a<B>]
EMI0002.0056  
  </B>  (C = 0,4 dans du chloroforme).



  Process for preparing the levo-isomers of 1-cyclohexyl-1-phenyl-3-pyrrolidinopropan-1-ol and of 1-cyclohexyl-1-phenyl-3-piperidinopropan-1-ol The present invention relates to a process of preparation of the levo-isomers of 1-cyclohexyl -1-phenyl-3-pyrrolidinopropan-1-ol and 1-cyclohexyl-1-phenyl-3-piperidinopropan-1-ol,

      in which the acid addition salts of 1-cyclohexyl-1-phenyl-3-pyrrolidinopropan-1-ol and 1-cyclohexyl-1-phenyl-3-piperidinopropan-1-ol are formed with d-tartaric acid.



  The racemic compounds 1-cyclohexyl-1-phenyl-3-pyrrolidinopropane-1-oI and 1-cyclohexyl-1-phenyl-3-piperidinopropane-1-oI and their N-lower alkyl quaternary salts, for example their quaternary salts N-methyl and N-ethyl, are known to have spasmolytic properties, and the first two compounds mentioned are clinically used for the symptomatic treatment of parkinsonism.



  It has now been found that the levo-isomers of these compounds possess properties which make them more valuable as therapeutic agents than their corresponding racemic forms. It was found that the atropine-like properties are in each case limited almost entirely to these levoisomers, the dextro-isomers being almost inactive and, moreover, unexpectedly, the levoisomer , in each case, is not more toxic, by intravenous injection in mice,

   than the racemic form or the dextrorotatory form. The levoisomers of these compounds therefore exhibit a valuable and unexpected advantage over their racemic forms, for use as agents of atropine-like action.



  Racemic 1-cyclohexyl-1-phenyl-3-pyrrolidino-propan-1-ol and 1-cyclohexyl 1-phenyl43-piperidinopropan-1-ol (prepared, for example, as described in Adamson, Journal, of the Chemical Society, London, 1951, page 52) can be split:

   into their optical isomers by any known method which can be used for the resolution of an organic base or of an alcohol, for example by forming the salt with d-tartaric acid and separating the two salts by fractional crystallization in the ethyl alcohol or a mixture of ethyl alcohol and ethyl acetate. The levoisomer can be used as the hydrochloride or salt of any non-toxic acid at the doses at which it is to be administered.



  The N-alkyl quaternary salts can be prepared from the levoisomer according to ordinary methods to form the quaternary salts from the tertiary amines. Thus, methiodide or ethiodide can be prepared by reacting the optically active base with methyl iodide or ethyl iodide, respectively; the quaternary compounds can have any desired acid radical as an anion.



  The process forming the subject of the present invention is characterized in that subjecting the acid addition salt corresponding to a fractional crystallization process in order to effect the partial separation of the dextrorotatory and levorotatory forms, the combined mother liquors of said said liquors are basified. fractional crystallizations which contain the levorotatory form,

   These alkalized mother liquors are subjected to a fractional crystallization process to isolate the levobase and obtain it in a form substantially free of dextro-isomer.



  Examples of implementation of the process according to the invention are given below, in which all the temperatures are given in degrees centigrade.



  <I> Example 1 </I> <I> Duplication of </I> 1-cyclohexyl-1-phenyl-3- pyrrolidinopropan-1-ol 1-cyclohexyl-1-phenyl-3- pyrrolidinopropane-1 was added -ol (60 g) dissolved in hot ethyl alcohol (120 cc) in a solution of d-tartaric acid (30 g) in ethyl alcohol (100 cc) and allowed to crystallize; successive removals of the solid body were made until only an oily substance separated.

   Ether can be added gradually to facilitate crystallization. sation. The oil and the mother liquor were combined, basified with ammonia then extracted with ether, and the base was crystallized from ethyl alcohol. The first harvests consisted of pure levo-base, the following ones in the racemic form.

   The optically active base levo-1-cyclohexyl-1-phenyl-3-pyrrolidinopropan-1-ol has a melting point of 105-106-; [ at ]
EMI0002.0031
   (C = 0.4 in ethyl alcohol). The hydrochloride, obtained by the usual methods, crystallizes from ethyl alcohol-ethyl acetate and has a melting point of 2460; [a] (C = 0.4 in chloroform).
EMI0002.0034
    



  <I> Example 2 </I> <I> Depletion of </I> 1-cyclohexyl-1-phenyl-3- piperidinopropan-1-ol 1-cyclohexyl-1-phenyl-3 -piperidino-propane-1- ol (20 g) was dissolved in a solution of d-tartaric acid (10 g) in ethyl alcohol (80 cc) and allowed to crystallize; successive removals of the solid body were made until only an oily substance separated. Ether can be added gradually to facilitate crystallization.

    The oil and mother liquor were combined, basified with ammonia, and the base was crystallized from ethyl alcohol. The optically active levo-1-cyclohexyl-1-phenyl-3 -piperidinopropan-1-ol base has a melting point of 112-113o;

   [at]
EMI0002.0050
    (C = 0.4 in ethyl alcohol). Its hydrochloride, obtained by the usual methods, crystallizes in isopropyl alcohol and has a melting point of 2640; <B> [</B> a <B>]
EMI0002.0056
  </B> (C = 0.4 in chloroform).

 

Claims (1)

REVENDICATION Procédé de préparation des lévo-isomères du 1-cyclohexyl-1-phényl- 3 -pyrrolidinopro- pane-1-ol et du 1-cyclohexyl-1-phényl-3-pipé- ridinopropane-1-ol, dans lequel on forme les sels d'addition acides du 1-cyclohexyl@-1-phényl- 3-pyrrolidinopropane-1-ol et du 1-cyclohexyl- 1-phényl-3-pipéridinopropane-1-ol avec l'acide d-tartrique, CLAIM Process for preparing the levo-isomers of 1-cyclohexyl-1-phenyl-3 -pyrrolidinopropan-1-ol and of 1-cyclohexyl-1-phenyl-3-piperidinopropan-1-ol, in which one forms the acid addition salts of 1-cyclohexyl @ -1-phenyl-3-pyrrolidinopropan-1-ol and of 1-cyclohexyl-1-phenyl-3-piperidinopropan-1-ol with d-tartaric acid, caractérisé en ce qu'on soumet le sel d'addition acide correspondant à un pro cédé- de cristallisation fractionnée pour effec tuer la séparation partielle des formes dextro gyre et lévogyre, on alcalinise les liqueurs mères combinées desdites cristallisations frac tionnées qui contiennent la forme lévogyre, on soumet ces liqueurs mères alcalinisées à un pro- cédé de cristallisation fractionnée pour isoler la lévo-base et l'obtenir sous une forme prati quement exempte de dextro-isomère. SOUS-REVENDICATIONS 1. characterized in that the corresponding acid addition salt is subjected to a fractional crystallization process to effect the partial separation of the dextro gyre and the levorotatory forms, the combined mother liquors of said fractional crystallizations which contain the levorotatory form are alkalized. , these alkalized mother liquors are subjected to a fractional crystallization process to isolate the levo-base and obtain it in a form substantially free of dextro-isomer. SUB-CLAIMS 1. Procédé selon la revendication, caracté risé en ce qu'on effectue lesdites cristallisations fractionnées dans de l'alcool éthylique. 2. Procédé selon la revendication, caracté risé en ce qu'on alcalinise lesdites liqueurs mères avec de l'ammoniaque. Process according to claim, characterized in that said fractional crystallizations are carried out in ethyl alcohol. 2. Method according to claim, characterized in that said mother liquors are basified with ammonia.
CH318326D 1953-03-23 1954-03-23 Process for preparing the levoisomers of 1-cyclohexyl-1-phenyl-3-pyrrolidinopropan-1-ol and 1-cyclohexyl-1-phenyl-3-piperidinopropan-1-ol CH318326A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB318326X 1953-03-23
GB100853X 1953-08-10

Publications (1)

Publication Number Publication Date
CH318326A true CH318326A (en) 1956-12-31

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CH318326D CH318326A (en) 1953-03-23 1954-03-23 Process for preparing the levoisomers of 1-cyclohexyl-1-phenyl-3-pyrrolidinopropan-1-ol and 1-cyclohexyl-1-phenyl-3-piperidinopropan-1-ol

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Country Link
CH (1) CH318326A (en)

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