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CH544775A - D-and l-isomers of 6h, 7h, cis-7-amino-3-aminomethyl cef -3 - Google Patents

D-and l-isomers of 6h, 7h, cis-7-amino-3-aminomethyl cef -3

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Publication number
CH544775A
CH544775A CH1334071A CH1334071A CH544775A CH 544775 A CH544775 A CH 544775A CH 1334071 A CH1334071 A CH 1334071A CH 1334071 A CH1334071 A CH 1334071A CH 544775 A CH544775 A CH 544775A
Authority
CH
Switzerland
Prior art keywords
lactam
aminomethyl
acid
carboxylic
thiazine
Prior art date
Application number
CH1334071A
Other languages
French (fr)
Inventor
Martel Jacques
Heymes Rene
Original Assignee
Roussel Uclaf
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
Priority claimed from FR7033898A external-priority patent/FR2120214A6/en
Application filed by Roussel Uclaf filed Critical Roussel Uclaf
Publication of CH544775A publication Critical patent/CH544775A/en

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    • C07D207/30Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having two double bonds between ring members or between ring members and non-ring members
    • C07D207/34Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having two double bonds between ring members or between ring members and non-ring members with hetero atoms or with carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals, directly attached to ring carbon atoms
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    • C07D207/30Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having two double bonds between ring members or between ring members and non-ring members
    • C07D207/34Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having two double bonds between ring members or between ring members and non-ring members with hetero atoms or with carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals, directly attached to ring carbon atoms
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    • C07D207/30Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having two double bonds between ring members or between ring members and non-ring members
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    • C07D501/02Preparation
    • C07D501/08Preparation by forming the ring or condensed ring systems
    • CCHEMISTRY; METALLURGY
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    • C07DHETEROCYCLIC COMPOUNDS
    • C07D501/00Heterocyclic compounds containing 5-thia-1-azabicyclo [4.2.0] octane ring systems, i.e. compounds containing a ring system of the formula:, e.g. cephalosporins; Such ring systems being further condensed, e.g. 2,3-condensed with an oxygen-, nitrogen- or sulfur-containing hetero ring
    • C07D501/14Compounds having a nitrogen atom directly attached in position 7
    • C07D501/16Compounds having a nitrogen atom directly attached in position 7 with a double bond between positions 2 and 3
    • C07D501/187-Aminocephalosporanic or substituted 7-aminocephalosporanic acids
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    • C07D501/14Compounds having a nitrogen atom directly attached in position 7
    • C07D501/16Compounds having a nitrogen atom directly attached in position 7 with a double bond between positions 2 and 3
    • C07D501/207-Acylaminocephalosporanic or substituted 7-acylaminocephalosporanic acids in which the acyl radicals are derived from carboxylic acids
    • C07D501/247-Acylaminocephalosporanic or substituted 7-acylaminocephalosporanic acids in which the acyl radicals are derived from carboxylic acids with hydrocarbon radicals, substituted by hetero atoms or hetero rings, attached in position 3
    • C07D501/38Methylene radicals, substituted by nitrogen atoms; Lactams thereof with the 2-carboxyl group; Methylene radicals substituted by nitrogen-containing hetero rings attached by the ring nitrogen atom; Quaternary compounds thereof
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    • C07D501/14Compounds having a nitrogen atom directly attached in position 7
    • C07D501/16Compounds having a nitrogen atom directly attached in position 7 with a double bond between positions 2 and 3
    • C07D501/207-Acylaminocephalosporanic or substituted 7-acylaminocephalosporanic acids in which the acyl radicals are derived from carboxylic acids
    • C07D501/247-Acylaminocephalosporanic or substituted 7-acylaminocephalosporanic acids in which the acyl radicals are derived from carboxylic acids with hydrocarbon radicals, substituted by hetero atoms or hetero rings, attached in position 3
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    • C07D513/02Heterocyclic compounds containing in the condensed system at least one hetero ring having nitrogen and sulfur atoms as the only ring hetero atoms, not provided for in groups C07D463/00, C07D477/00 or C07D499/00 - C07D507/00 in which the condensed system contains two hetero rings
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Abstract

Title cpds. of formula (I): (where R2 is H, alkyl or aryl) are prepd. from trityl derivs. of formula (II) by (i) resolution of the 1-sparteine diastereoisomers; (ii) ring closure with dicyclohexylcarbodiimide; (iii) detritylation with HCl gas in MeNO2.

Description

  

      On    a     décrit    dans le brevet     suisse    N  515276 un     procédé    de pré  paration de     dérivés    de la     céphalosporine,        racémiques    ou     optique-          ment    actifs, de formule     générale:

       
EMI0001.0010     
  
EMI0001.0011     
  
   
EMI0001.0012     
  
   
EMI0001.0013     
  
     dans     laquelle   <B>R'</B> et<B>R"</B>     représentent    des     radicaux        alcoyle    ou     aral-          coyle    ou forment     ensemble    le reste d'un     hétérocycle,        remplace     dans     ce        composé    le groupe     amine        substituée   
EMI0001.0027  
   par un  groupe     thioacyle,

       
EMI0001.0029     
  
   
EMI0001.0030     
  
     condense ce     dernier    avec une     énamine    de formule VII  
EMI0001.0033     
    dans laquelle R représente un radical alcoyle inférieur ou un radi  cal     aralcoyle    inférieur et  Y     représente    un groupe     imido    ou un groupe     acylamino    où le  terme     acyl    figure le reste d'un acide organique carboxylique infé  rieur, obtient un     y-lactame    de l'acide     2-(a-R-oxy        carbonyl        a-Y-          méthyl)

          5-aminométhyl        2,3-dihydro        1,3-thiazine        4-carboxylique,     de formule VIII:  
EMI0001.0048     
    qui se présente sous     forme    d'un mélange d'isomères     thréo    et       érythro,        ottsous        forme    de l'un des deux, scinde le groupe     imido     ou le groupe     acylamino,    Y, par un échange de fonction à l'aide de       l'hydrazine,    par une hydrolyse acide ou par une     hydrogénolyse,

       obtient le     y-lactame    correspondant de     formule    VIII':  
EMI0001.0060     
    pouvant exister sous     forme    d'isomères     thréo    et     érythro,    dont on  libère le groupe     carboxyle    par l'action d'un agent acide, obtient  un     y-lactame    de l'acide     2-(a-carboxy        a-aminométhyl)        5-aminomé-          thyl        2,3-dihydro        1,3-thiazine        4-carboxylique,    de formule IX:

    
EMI0001.0073     
      pouvant exister sous forme d'isomères     thréo    et     érythro    qu'on  traite par un agent de     tritylation,    obtient un     y-lactame    de l'acide       2-(a-carboxy        a-tritylaminométhyl)        5-aminométhyl        2,3-dihydro          1,3-thiazine        4-carboxylique    de formule IX':

    
EMI0002.0010     
  
EMI0002.0011     
  
     dans laquelle     Rl    a la signification précitée, et fait agir sur ces  composés un agent acide pour obtenir respectivement les iso  mères D et L du     y-lactame    de l'acide 6H, 7H     cis        7-amino        3-ami-          nométhyl        céph-3-ème        4-carboxylique    correspondants cherchés.  



  Le procédé, objet de la présente invention, possède sur celui  du brevet suisse N  515276 l'avantage d'opérer le dédoublement à  un stade moins avancé de la synthèse, ce qui est économiquement  plus avantageux.  



  Les indications données ci-après ont trait, pour des raisons de  simplifications, plus spécialement au cas où Ri = H.  



  Le réactif à l'aide duquel on effectue le dédoublement du dl     y-          lactame    de l'acide     2-(a-carboxy        a-tritylaminométhyl)        5-aminomé-          thyl        2,3-dihydro        1,3-thiazine        4-carboxylique    est, de préférence,

   la       1-spartéine.    On opère de .manière avantageuse au sein d'un mélan  ge d'eau et de méthanol et insolubilise le sel de     spartéine    du D     y-          lactame    de l'acide     2-(a-carboxy        oc-tritylaminométhyl)        5-aminomé-          thyl        2,3-dihydro        1,3-thiazine        4-carboxylique.    De ce sel, par     acidifi-          cation,

      on libère le D     y-lactame    de l'acide     2-(a-carboxy        oc-trityla-          minométhyl)        5-aminométhyl        2,3-dihydro        1,3-thiazine        4-carboxyli-          que.     



  Pour purifier ce     dernier,    on peut en former à nouveau le sel de       1-spartéine    que l'on cristallise dans un solvant convenable,     no-          tamment    dans un     mélange    d'eau et de méthanol, puis libère à  nouveau le composé désiré par action d'un agent acide sur le sel  de     spartéine    purifié.  



  Le sel de     spartéine    de l'isomère L du     y-lactame    de l'acide     2-(oc-          carboxy        oc-tritylaminométhyl)        5-aminométhyl        2,3-dihydro        1,3-          thiazine        4-carboxylique    se trouve dans les liqueurs mères de cris  tallisation du sel de     spartéine    de l'isomère D.  



  Par acidification de ces liqueurs mères, on insolubilise le L     y-          lactame    de l'acide     2-(at-carboxy        oc-tritylaminométhyl)        5-aminomé-          thyl        2,3-dihydro        1,3-thiazine        4-carboxylique.     



  Ce composé peut être purifié par transformation en sel     d'éphé-          drine,    cristallisation de ce sel     d'éphédrine    dans un-solvant ou un  mélange de solvants convenables tel qu'un mélange de méthanol  et de chlorure de méthylène, puis mise en     liberté    du composé dési  ré par acidification du sel     d'éphédrine    purifié.  



  La     1-spartéine    utilisée pour le dédoublement est récupérée  dans les liqueurs mères d'obtention du D     y-lactame    de for-    mule IX' et du L     y-lactame    de formule IX' par     alcalinisation    et  élimination du solvant par distillation sous pression réduite.  



  Par action d'un agent de cyclisation, tel que le     dicyclohexyl-          carbodiimide,    les     y-lactames    D et L de l'acide     2-(a-carboxy        oc-tri-          tylaminométhyl)        5-aminométhyl        2,3-dihydro        1,3-thiazine        4-car-          boxylique,    de formule IX', sont transformés respectivement en     y-          lactame    de l'acide D ou L 6H,

   7H     cis        7-tritylamino        3-aminomé-          thyl        céph-3-ème        4-carboxylique,    en opérant par exemple dans un  mélange de solvants constitué par le     nitrométhane,    la     pyridine    et  le chlorure de méthylène.

      La     détritylation    de ces     y-lactames    D et L est effectuée de pré  férence à l'aide de l'acide chlorhydrique gazeux, en opérant dans  le     nitrométhane    et l'on obtient respectivement les     y-lactames    D et  L de l'acide 6H, 7H     cis        7-amino        3-aminométhyl        céph-3-ème        4-car-          boxylique    de formule I.  



  L'exemple suivant illustre l'invention. Pour les premières  étapes du procédé, on se     reportera    au brevet principal mentionné  précédemment.         Exemple:        y-lactame   <I>de l'acide L (ou D) 6H, 7H</I>     cis        7-amino        3-ami-          nométhyl        céph-3-ème        4-carboxylique.     



       Stade   <I>A: Dédoublement du dl</I>     y-lactame   <I>de l'acide</I>     2-(a-carboxy   <I>a-</I>  <I>tritylaminométhyl)</I>     5-aminométhy12,3-dihydro        1,3-thiazine        4-car-          boxylique   <I>(isomère</I>     thréo).     



  <I>a) Obtention de l'isomère D</I>    A une solution de 3,75 g de     1-spartéine    dans 25     cm3    de métha  nol, on ajoute, sous agitation, 5 g de DL     y-lactame    de l'acide     2-(a-          carboxy        a-tritylaminométhyl)        5-aminométhyl        2,3-dihydro        1,3-          thiazine        4-carboxylique    (isomère     thréo),    ajoute 25     cm3    d'eau, ar  rête l'agitation,

   ajoute quelques     amorces    cristallines de sel de       spartéine    du D     y-lactame    de l'acide     2-(a-carboxy        a-tritylaminomé-          thyl)        5-aminométhyl        2,3-dihydro        1,3-thiazine        4-carboxylique    (iso  mère     thréo),    laisse au repos une heure à 20 C, isole le précipité de  sel de     spartéine,    par essorage, le lave, le sèche. On conserve les li  queurs mères de cristallisation (liqueurs mères A).

   Les 3,67 g de  précipité obtenus sont dissous dans 20 volumes de méthanol, on  acidifie par l'acide acétique, laisse cristalliser, essore, lave au mé  thanol puis à l'éther, sèche et obtient 2,15 g de D     y-lactame    de  l'acide     2-(oc-carboxy        oa-tritylaminométhyl)        5-aminométhyl        2,3-di-          hydro        1,3-thiazine        4-carboxylique    (isomère     thréo)    brut,  conserve les liqueurs mères de cristallisation (liqueurs mères B).

    
EMI0002.0168  
   (c=0,6%, méthanol à 1% de     triéthylamine).    On  <I>Purification:</I>  On opère sur 15 g d'isomère D brut provenant de plusieurs es  sais de dédoublement que l'on introduit dans une solution de  11,25 g de     I-spartéine    dans 100     cm3    de méthanol, chauffe à 40 C  pour obtenir la dissolution, refroidit à 20 C, ajoute 100     cm3    d'eau  distillée, laisse cristalliser, isole le précipité par essorage, le lave  par un mélange méthanol-eau (1,1) puis à l'éther, le reprend par  250     cm3    de méthanol, filtre, acidifie par l'acide acétique, laisse  cristalliser, isole par essorage le précipité formé, le lave au métha  nol, à l'éther, le sèche et obtient 12,

  1 g de D     y-lactame    de l'acide       2-(a-carboxy        a-tritylaminométhyl)        5-aminométhyl        2,3-dihydro          1,3-thiazine        4-carboxylique    (isomère     thréo)   
EMI0002.0182  
    (c=0,5%, méthanol à 1 % de     triéthylamine).     



  Pour autant que l'on sache, ce composé n'est pas décrit dans  la littérature.  



  Il en est de même du sel de     1-spartéine    du D     y-lactame    de  l'acide     2-(oc-carboxy        a-tritylaminométhyl)        5-aminométhyl        2,3-di-          hydro        1,3-thiazine        4-carboxylique.     



  <I>b)</I>     Obtention   <I>de l'isomère L</I>  Les liqueurs mères de cristallisation du sel de     1-spartéine    de  l'isomère D (liqueurs mères A) sont acidifiées par l'acide acétique,  on isole par essorage le précipité formé, le lave au méthanol, à  l'éther, le     sèche    et obtient 1,6 g de L     y-lactame    de l'acide     2-(at-car-          boxy        a-tritylaminométhyl)        5-aminométhyl        2,3-dihydro        1,3-thia-          zine        4-carboxylique    (isomère     thréo)

      brut
EMI0002.0206  
   (c=0,5%,      méthanol à I % de     triêthylamine).        On    conserve les liqueurs mères  de cristallisation (liqueurs     mères    C).  



  <I>Purification:</I>       On    opère sur 13,2 g     d'isomère    L     brut    provenant de divers es  sais de dédoublement, que l'on introduit dans une solution de  6,6 g de     1-éphédrine    dans 82     CM3    de méthanol. Dans la     solution     obtenue, on introduit lentement 164     cm3    d'éther éthylique,     laisse     cristalliser, isole par     essorage    le     précipité    formé; lave à l'éther, sè  che.

   Les 12,5 g de sel     d'éphédrine    brut obtenus sont dissous dans  400     CM3    d'un     mélange    de méthanol et de     chlorure    de méthylène  (1-1), on filtre, acidifie par     l'acide        acétique,    laisse     cristalliser,    isole  par essorage le     précipité        formé,    le lave au     méthanol,    à l'éther, le       sèche    et obtient 8,43 g de L     y-laetame    de     l'acide        2-(ix-carboxy    a  tritylaminométhyl)

       5-aminométhyl        2,3-dihydro        1,3-thiazine        4-car-          boxylique        (isomère        thréo@   
EMI0003.0034  
       (c=0,57%,    méthanol à  1 % de     triéthylamine):     Pour autant que l'on sache,     ce    composé n'est pas     décrit    dans  la littérature.  



  I l en est de     même    du sel de     1-éphédrine    du L     y-lactame    de  l'acide     2-(a-carboxy        a-tritylaminométhyl)        5-aminornéthyl        2,3-di-          hydro        1,3-thiazine        4-carboxylique.            Récupération   <I>de la</I>     l-spartéine     On réunit les liqueurs     mères    B et C, les     alcalinise    par la  soude 2N,     extrait    à l'éther,

   lave la     solution    éthérée à l'eau, sèche,  élimine le solvant par distillation     sous        pression    réduite, et     récu-          père    la     I-spartéine        avec    un     rendement        pratiquement    quantitatif.

           Stade   <I>B:</I>     y-lacrame   <I>de</I>     l'acide   <I>L 6H, 7H</I>     cis        7-tritylamino        3-amino-          méthyl        céph-3-ème        4-carboxylique     Dans 20     em3    de     pyridine,    on     introduit    2 g de L     y-lactame    de  l'acide     2-(a-carboxy        a-tritylaminométhyl)        5-aminométhyl        2,

  3-di-          hydro        1,3-thiazine        4-carboxylique        (isomère        thréo),    ajoute 1,5 g de       dicyclohexylcarbodiimide,        40        CM3    de     chlorure    de méthylène,  40     CM3    de     nitrométhane,        laisse    au     repos    à     20 C,    sous     atmosphère     d'azote, à     l'obscurité,        pendant    dix-huit     heures;

      élimine par filtra  tion la     dicyclohexyhrrée,        concentre    le     filtrat    à     sec    par     distillation     sous     pression        réduite,        ajouté'    de l'éther,     isole    par     essorage    le préci  pité formé, le     reprend    su     chlorure    de     méthylène,    ajoute du char  bon actif à la     solution        obtenue,        agite,

          élimine    le charbon actif par       filtration,        concentre    le     filtrat    à sec par     distillation    sous     pression     réduite, purifie le     résidu    par     chromatographie    sur gel de silice en       éluant    par un     mélange    de     chloroforme,        d'acétate    d'éthyle et  d'éthanol     (75-15-10),    obtient     2'g        d'un        produit    homogène,

   le dis  sout dans     le        chlorure    de     méthylène,    ajoute de l'éther éthylique,  isole par     essorage    le     précipité        formé    et obtient 1,22 g de     y-lactame     de     l'acide    L 6H, 7H     cis        7-trityiamino        3-aminornéthyl        céph-3-ème          4-carboxylique,   
EMI0003.0143  
       (c-0,5%,        chloroforme).     



  Pour     autant    que l'on sache, ce     composé        n'est        pas        décrit        dans     la littérature.  



  De manière analogue à     celle        utilisée    dans. l'exemple, au départ  du D     y-lactame    de l'acide     2-(a-carboxy        a-tritylaminométhyl)        5-          aminométhyi        2,3-dihydro        1,3-thiazine        4-carboxylique,    on obtient  le     y-lactame    de     l'acide    D 6H,<B>7H</B>     cis        7-tritylamino        3-aminométhyl          oéph-3-ème4-caiboxylique,

     
EMI0003.0168  
       (c=0,5%,chloroforme).     



  Pour autant que l'on sache,     ce    composé     n'est        pas        décrit    dans       la    littérature.  



       Stade   <I>C:</I>     y-lacrame   <I>de</I>     l'acide   <I>L</I>     6H,   <I>7H</I>     cis        7-amino        3-aminométhyl          céph-3-ème        4-carboxylique     Dans 8     cm3    de     nitrornéthane,    on     dissout    1 g de     y-lactame    de  l'acide L<B>6H,

  </B> 7H     cis        7-tritylamiuo        3-aminométhyl        céph-3-ème        4-          carboxylique,        refroidit    la     solution    obtenue à + 10 C, y fait barbo  ter de     l'acide        chlorhydrique    gazeux     pendant        vingt        minutes,

          éli-          mine    1     cm3   <B>de</B>     nitrométhane    par     distillation    sous     pression        réduite,     ajoute 30     CM3        d'éther,    isole par     essorage    le     précipité        formé,    le lave  à l'éther, le reprend par de     l'éthanol,        ajoute    un     léger        excès    de trié-         thylamine,    laisse cristalliser,

   isole par essorage le précipité formé,  le lave à l'éthanol, à l'éther, le sèche et obtient 400 mg de     y-lac-          tame    de l'acide L 6H, 7H     cis        7-amino        3-aminométhyl        céph-3-ème          4-carboxylique,   
EMI0003.0225  
   (c=0,5%, eau).  



  Un échantillon de ce produit est     purifié    par dissolution dans  une solution aqueuse     normale    d'acide chlorhydrique, passage au  charbon actif et addition de     triéthylamine    (rendement de purifica  tion:     80%i   
EMI0003.0230  
   (c=0,5%, eau).  



  De la même façon, au départ du     y-lactame    de l'acide D 6H,  7H     cis        7-tritylamino        3-aminométhyl        céph-3-ème        4-carboxylique,     on obtient le     y-lactame    de l'acide D 6H, 7H     cis   RTI ID="0003.0239" WI="11" HE="4" LX="1683" LY="609">  7-amino        3-amino-          méthyl        céph-3-ème        4-carboxylique.     



  Les isomères D et L du     y-lactame    obtenus sont identiques à       ceux        décrits    dans le brevet suisse N  515276.



      Swiss Patent No. 515276 has described a process for the preparation of cephalosporin derivatives, racemic or optically active, of general formula:

       
EMI0001.0010
  
EMI0001.0011
  
   
EMI0001.0012
  
   
EMI0001.0013
  
     in which <B> R '</B> and <B> R "</B> represent alkyl or aralkyl radicals or together form the residue of a heterocycle, in this compound replaces the substituted amine group
EMI0001.0027
   by a thioacyl group,

       
EMI0001.0029
  
   
EMI0001.0030
  
     condenses the latter with an enamine of formula VII
EMI0001.0033
    in which R represents a lower alkyl radical or a radi cal aralkyl lower and Y represents an imido group or an acylamino group where the term acyl is the residue of a lower organic carboxylic acid, obtains a y-lactam of acid 2 - (aR-oxy carbonyl aY- methyl)

          4-carboxylic 5-aminomethyl 2,3-dihydro 1,3-thiazine, of formula VIII:
EMI0001.0048
    which is in the form of a mixture of threo and erythro isomers, otts in the form of one of the two, cleaves the imido group or the acylamino group, Y, by an exchange of functions using hydrazine, by acid hydrolysis or by hydrogenolysis,

       obtains the corresponding γ-lactam of formula VIII ':
EMI0001.0060
    which may exist as threo and erythro isomers, the carboxyl group of which is released by the action of an acidic agent, obtains a γ-lactam of 2- (a-carboxy a-aminomethyl) 5-aminomé acid thyl 2,3-dihydro 1,3-thiazine 4-carboxylic, of formula IX:

    
EMI0001.0073
      which may exist in the form of threo and erythro isomers which are treated with a tritylating agent, obtains a y-lactam of 2- (a-carboxy a-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3 -4-carboxylic thiazine of formula IX ':

    
EMI0002.0010
  
EMI0002.0011
  
     in which Rl has the aforementioned meaning, and causes an acidic agent to act on these compounds to obtain respectively the isomers D and L of the γ-lactam of 6H, 7H cis 7-amino 3-aminomethyl ceph-3- acid th 4-carboxylic correspondents sought.



  The process, which is the subject of the present invention, has the advantage over that of Swiss Patent No. 515276 of performing the resolution at a less advanced stage of the synthesis, which is economically more advantageous.



  The indications given below relate, for reasons of simplification, more especially to the case where Ri = H.



  The reagent with the aid of which the resolution of the dl y-lactam from 2- (a-carboxy a-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid is carried out is, preferably,

   1-sparteine. The procedure is advantageously carried out in a mixture of water and methanol and the sparteine salt of D y-lactam of 2- (a-carboxy oc-tritylaminomethyl) 5-aminomethyl acid is insolubilized. , 3-dihydro 1,3-thiazine 4-carboxylic. Of this salt, by acidification,

      the D y-lactam is freed from 2- (a-carboxy oc-tritylomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid.



  To purify the latter, it is possible to form again the salt of 1-sparteine which is crystallized in a suitable solvent, in particular in a mixture of water and methanol, then liberates again the desired compound by the action of an acidic agent on the purified spartein salt.



  The sparteine salt of the L-isomer of 2- (oc-carboxy oc-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid isomer is found in mother liquors of crystallization of the spartein salt of the D isomer.



  By acidification of these mother liquors, the L y-lactam of 2- (at-carboxy α-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid is insolubilized.



  This compound can be purified by transformation into the ephedrine salt, crystallization of this ephedrine salt in a solvent or a mixture of suitable solvents such as a mixture of methanol and methylene chloride, and then setting free of the solvent. compound desired by acidifying the purified ephedrine salt.



  The 1-sparteine used for the resolution is recovered in the mother liquors for obtaining D y-lactam of formula IX 'and L y-lactam of formula IX' by basification and removal of the solvent by distillation under reduced pressure.



  By the action of a cyclizing agent, such as dicyclohexylcarbodiimide, γ-lactams D and L of 2- (α-carboxy α-tri-tylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3 -thiazine 4-carboxylic, of formula IX ', are transformed respectively into y-lactam of acid D or L 6H,

   7H cis 7-tritylamino 3-aminomethyl ceph-3-rd 4-carboxylic, for example by operating in a mixture of solvents consisting of nitromethane, pyridine and methylene chloride.

      The detritylation of these γ-lactams D and L is preferably carried out using gaseous hydrochloric acid, operating in nitromethane, and the γ-lactams D and L of the 6H acid are respectively obtained, 7H cis 7-amino 3-aminomethyl ceph-3-rd 4-carboxylic of formula I.



  The following example illustrates the invention. For the first steps of the process, reference is made to the main patent mentioned above. Example: L (or D) 6H, 7H </I> cis 7-amino 3-aminomethyl ceph-3-rd 4-carboxylic acid γ-lactam.



       Stage <I> A: Depletion of dl </I> y-lactam <I> from acid </I> 2- (a-carboxy <I> a- </I> <I> tritylaminomethyl) </ I > 5-aminomethy12,3-dihydro 1,3-thiazine 4-carboxylic <I> (isomer </I> threo).



  <I> a) Obtaining the D isomer </I> To a solution of 3.75 g of 1-sparteine in 25 cm3 of methanol, is added, with stirring, 5 g of DL y-lactam of the 2- (α-carboxy α-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid (threo isomer), add 25 cm3 of water, stop stirring,

   add some crystalline primers of 2- (a-carboxy a-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid (a-carboxy a-tritylaminomethyl) sparteine salt (thiazine isomer) 4-carboxylic (threo isomer) , left to stand for one hour at 20 C, isolate the precipitate of sparteine salt, by wringing, washing it and drying it. The mother liquors of crystallization (mother liquors A) are kept.

   The 3.67 g of precipitate obtained are dissolved in 20 volumes of methanol, acidified with acetic acid, allowed to crystallize, filtered off, washed with methanol and then with ether, dried and 2.15 g of D y- 2- (oc-carboxy oa-tritylaminomethyl) 5-aminomethyl 2,3-di-hydro 1,3-thiazine 4-carboxylic acid lactam (threo isomer) crude, preserves mother liquors of crystallization (mother liquors B) .

    
EMI0002.0168
   (c = 0.6%, methanol 1% triethylamine). It is <I> Purification: </I> The operation is carried out on 15 g of crude D isomer originating from several resolution tests which is introduced into a solution of 11.25 g of I-sparteine in 100 cm3 of methanol, heat to 40 ° C. to obtain the dissolution, cool to 20 ° C., add 100 cm3 of distilled water, allow to crystallize, isolate the precipitate by draining, wash it with a methanol-water mixture (1.1) then with ether, It is taken up in 250 cm3 of methanol, filtered, acidified with acetic acid, left to crystallize, isolate the precipitate formed by draining, wash it with methanol and ether, dry it and obtain 12,

  1 g of 2- (a-carboxy a-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid D y-lactam (threo isomer)
EMI0002.0182
    (c = 0.5%, methanol at 1% triethylamine).



  As far as we know, this compound is not described in the literature.



  The same is true of the 1-sparteine salt of D y-lactam of 2- (α-carboxy α-tritylaminomethyl) 5-aminomethyl 2,3-di-hydro 1,3-thiazine 4-carboxylic acid.



  <I> b) </I> Obtaining <I> of the L isomer </I> The mother liquors of crystallization of the 1-sparteine salt of the D isomer (mother liquors A) are acidified with acetic acid , the precipitate formed is isolated by suction, washed with methanol, with ether, dried and 1.6 g of L y-lactam of 2- (at-carboxyl a-tritylaminomethyl) 5- acid are obtained. aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic (threo isomer)

      gross
EMI0002.0206
   (c = 0.5%, methanol at 1% triethylamine). The mother liquors of crystallization (mother liquors C) are kept.



  <I> Purification: </I> The operation is carried out on 13.2 g of crude L isomer originating from various resolution tests, which is introduced into a solution of 6.6 g of 1-ephedrine in 82 cm3 of methanol. 164 cm3 of ethyl ether are slowly introduced into the solution obtained, allowed to crystallize and the precipitate formed is isolated by suction; washed with ether, dry.

   The 12.5 g of raw ephedrine salt obtained are dissolved in 400 cm3 of a mixture of methanol and methylene chloride (1-1), filtered, acidified with acetic acid, left to crystallize, isolated by draining the precipitate formed, washed with methanol and with ether, dried and obtained 8.43 g of L y-laetam of 2- (ix-carboxy a tritylaminomethyl) acid

       5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic (threo isomer @
EMI0003.0034
       (c = 0.57%, methanol at 1% triethylamine): As far as we know, this compound is not described in the literature.



  The same is true of the 1-ephedrine salt of 2- (α-carboxy α-tritylaminomethyl) 5-aminornethyl 2,3-di-hydro 1,3-thiazine 4-carboxylic acid L y-lactam. Recovery <I> of </I> l-sparteine The mother liquors B and C are combined, basified with 2N soda, extracted with ether,

   washing the ethereal solution with water, drying, removing the solvent by distillation under reduced pressure, and recovering the I-spartein in practically quantitative yield.

           Stage <I> B: </I> y-lacrame <I> of </I> acid <I> L 6H, 7H </I> cis 7-tritylamino 3-amino-methyl ceph-3-rd 4 -carboxylic In 20 em3 of pyridine, 2 g of L y-lactam of 2- (a-carboxy a-tritylaminomethyl) 5-aminomethyl 2 are introduced,

  3-dihydro 1,3-thiazine 4-carboxylic (threo isomer), add 1.5 g of dicyclohexylcarbodiimide, 40 CM3 of methylene chloride, 40 CM3 of nitromethane, leave to stand at 20 C, under a nitrogen atmosphere , in the dark, for eighteen hours;

      the dicyclohexyhrrea is filtered off, the filtrate is concentrated to dryness by distillation under reduced pressure, ether is added, the precipitate formed is isolated by filtering, it is taken up in methylene chloride, and activated charcoal is added to the solution obtained, shake,

          eliminates the activated carbon by filtration, concentrates the filtrate to dryness by distillation under reduced pressure, purifies the residue by chromatography on silica gel, eluting with a mixture of chloroform, ethyl acetate and ethanol (75-15- 10), obtains 2'g of a homogeneous product,

   dissolve it in methylene chloride, add ethyl ether, filter off the precipitate formed and obtain 1.22 g of y-lactam from L 6H, 7H cis 7-trityiamino 3-aminornethyl ceph-3 acid -th 4-carboxylic,
EMI0003.0143
       (c-0.5%, chloroform).



  As far as we know, this compound is not described in the literature.



  Analogously to that used in. Example, starting from D y-lactam of 2- (a-carboxy a-tritylaminomethyl) 5-aminomethyi 2,3-dihydro 1,3-thiazine 4-carboxylic acid, we obtain the y-lactam of l 'D 6H, <B> 7H </B> cis 7-tritylamino 3-aminomethyl oeph-3-rd4-caiboxylic acid,

     
EMI0003.0168
       (c = 0.5%, chloroform).



  As far as we know, this compound is not described in the literature.



       Stage <I> C: </I> y-lacrame <I> of </I> acid <I> L </I> 6H, <I> 7H </I> cis 7-amino 3-aminomethyl ceph -3-rd 4-carboxylic In 8 cm3 of nitrornethane, 1 g of γ-lactam of L <B> 6H acid is dissolved,

  </B> 7H cis 7-tritylamiuo 3-aminomethyl ceph-3-rd 4- carboxylic, cools the solution obtained to + 10 C, bubbling gaseous hydrochloric acid therein for twenty minutes,

          eliminates 1 cm3 <B> of </B> nitromethane by distillation under reduced pressure, adds 30 cm3 of ether, isolates the precipitate formed by draining, washing it with ether, taking it up in ethanol, adding a slight excess of triethylamine, allows to crystallize,

   isolates the precipitate formed by filtering, washing it with ethanol and ether, drying it and obtaining 400 mg of y-lactam from L 6H, 7H cis 7-amino 3-aminomethyl ceph-3- acid. th 4-carboxylic,
EMI0003.0225
   (c = 0.5%, water).



  A sample of this product is purified by dissolving in normal aqueous hydrochloric acid solution, passing through activated carbon and adding triethylamine (purification yield: 80% i
EMI0003.0230
   (c = 0.5%, water).



  In the same way, starting from the y-lactam of D 6H, 7H cis 7-tritylamino 3-aminomethyl ceph-3-rd 4-carboxylic acid, the y-lactam of D 6H, 7H cis acid is obtained RTI ID = "0003.0239" WI = "11" HE = "4" LX = "1683" LY = "609"> 7-amino 3-amino-methyl ceph-3-rd 4-carboxylic.



  The D and L isomers of the y-lactam obtained are identical to those described in Swiss Patent No. 515276.

 

Claims (1)

REVENDICATION Procédé de préparation des isomères D et L du y-lactame de l'acide 6H, 7H cis 7-amino 3-aminométhyl céph-3-éme 4-carboxy- lique de formule générale: EMI0003.0255 dans laquelle RI représente de l'hydrogène, un radical alcoyle substitué ou non substitué ou un radical aryle substitué ou non substitué; caractérisé en ce que l'on soumet un acide 2,3-dioxo pyrrolidine 4-carboxylique de formule IV': CLAIM Process for preparing the D and L isomers of the γ-lactam of 6H, 7H cis 7-amino 3-aminomethyl ceph-3-th 4-carboxylic acid of general formula: EMI0003.0255 in which RI represents hydrogen, a substituted or unsubstituted alkyl radical or a substituted or unsubstituted aryl radical; characterized in that a 2,3-dioxo pyrrolidine 4-carboxylic acid of formula IV 'is subjected: EMI0003.0259 à une aminométhylation par action d'une dialcoylamine en pré- sence de formol, obtient une 2,3-dioxo 4-(R', R")-aminométhyl pyrrolidine, de formule V EMI0003.0269 dans laquelle R' et R" représentent des radicaux alcoyle ou aral- coyle ou forment ensemble le reste d'un hétérocycle, EMI0003.0259 to an aminomethylation by the action of a dialkoylamine in the presence of formalin, obtains a 2,3-dioxo 4- (R ', R ") - aminomethyl pyrrolidine, of formula V EMI0003.0269 in which R 'and R "represent alkyl or aralkyl radicals or together form the residue of a heterocycle, remplace dans ce composé le groupe amine substituée EMI0003.0276 par un groupe thioacyle, obtient une 2,3-dioxo 4-acyl thiométhyl pyrrolidine de for mule VI: in this compound replaces the substituted amine group EMI0003.0276 by a thioacyl group, obtains a 2,3-dioxo 4-acyl thiomethyl pyrrolidine of formula VI: EMI0004.0000 dans laquelle Ac représente le radical acyle, libère la fonction thiol par une alcoolyse acide, obtient un mer- EMI0004.0003 condense ce dernier avec une énamine de formule VII EMI0004.0007 dans laquelle R représente un radical alcoyle inférieur ou un radi cal aralcoyle inférieur et Y représente un groupe imido ou un groupe acylamino où le terme acyl figure le reste d'un acide organique carboxylique infé rieur, EMI0004.0000 in which Ac represents the acyl radical, releases the thiol function by an acid alcoholysis, obtains a mer- EMI0004.0003 condenses the latter with an enamine of formula VII EMI0004.0007 in which R represents a lower alkyl radical or a radi cal aralkyl lower and Y represents an imido group or an acylamino group where the term acyl represents the residue of a lower organic carboxylic acid, obtient un y-lactame de l'acide 2-(a-R-oxy carbonyl a-Y-méthyl) 5-aminométhyl 2,3-dihydro 1,3-thiazine 4-carboxylique, de for- EMI0004.0020 qui se présente sous forme d'un mélange d'isomères thréo et érythro, ou sous forme de l'un des deux, scinde le groupe imido ou le groupe acylamino, Y, par un échange de fonction à l'aide de l'hydrazine, obtains a y-lactam of 2- (a-R-oxy carbonyl a-Y-methyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid, of for- EMI0004.0020 which is in the form of a mixture of threo and erythro isomers, or as one of the two, cleaves the imido group or the acylamino group, Y, by an exchange of functions using hydrazine , par une hydrolyse acide ou par une hydrogénolyse, obtient le y-lactame correspondant de formule VIII': EMI0004.0028 pouvant exister sous forme d'isomères thréo et érythro, dont on libère le groupe carboxyle par l'action d'un agent acide, obtient un y-lactame de l'acide 2-(a-carboxy a-aminométhyl) 5-aminomé- thyl 2,3-dihydro 1,3-thiazine 4-carboxylique, de formule IX: by acid hydrolysis or by hydrogenolysis, the corresponding γ-lactam of formula VIII 'is obtained: EMI0004.0028 which may exist as threo and erythro isomers, the carboxyl group of which is released by the action of an acidic agent, obtains a γ-lactam of 2- (a-carboxy a-aminomethyl) 5-aminomé acid thyl 2,3-dihydro 1,3-thiazine 4-carboxylic, of formula IX: EMI0004.0039 pouvant exister sous forme d'isomères thréo et érythro qu'on traite par un agent de tritylation, obtient un y-lactame de l'acide 2-(x-carboxy a-tritylaminométhyl) 5-aminométhyl 2,3-dihydro 1,3-thiazine 4-carboxylique de formule IX': EMI0004.0039 which may exist in the form of threo and erythro isomers which are treated with a tritylation agent, obtains a y-lactam of 2- (x-carboxy a-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3 -4-carboxylic thiazine of formula IX ': EMI0004.0050 pouvant exister sous forme d'isomères thréo et érythro, que l'on soumet à l'action d'un réactif de dédoublement, sépare ainsi les isomères D et L correspondants, que l'on soumet à l'action d'un réactif de cyclisation pour obtenir respectivement les isomères D et L du y-lactame de l'acide 6H, 7H cis 7-tritylamino 3-aminomé- thyl céph-3-ème 4-carboxylique correspondants de formule géné rale EMI0004.0061 dans laquelle RI a la signification précitée, EMI0004.0050 which may exist in the form of threo and erythro isomers, which are subjected to the action of a resolution reagent, thus separates the corresponding D and L isomers, which are subjected to the action of a cyclization to obtain respectively the D and L isomers of the γ-lactam of 6H, 7H cis 7-tritylamino 3-aminomethyl ceph-3-rd 4-carboxylic acid corresponding of general formula EMI0004.0061 in which RI has the above meaning, et fait agir sur ces composés un agent acide pour obtenir respectivement les iso mères D et L du y-lactame de l'acide 6H, 7H cis 7-amino 3-ami- nométhyl céph-3-ème 4-carboxylique correspondants cherchés. SOUS-REVENDICATIONS 1. and causes an acidic agent to act on these compounds to obtain respectively the D and L isomers of the γ-lactam of the 6H, 7H cis 7-amino 3-aminomethyl ceph-3-rd 4-carboxylic acid desired. SUB-CLAIMS 1. Procédé selon la revendication, caractérisé en ce que l'on fait réagir la 1-spartéine, au sein d'un mélange d'eau et de métha nol, sur le DL y-lactame de l'acide 2-(a-carboxy a-tritylaminomé- thyl) 5-aminométhyl 2,3-dihydro 1,3-thiazine 4-carboxylique, in solubilise le sel de spartéine du D y-lactame de l'acide 2-(a-car- boxy a-tritylaminométhyl) Process according to claim, characterized in that the 1-sparteine, in a mixture of water and methanol, is reacted with the DL y-lactam of 2- (a-carboxy a -tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic, in solubilizes the D y-lactam sparteine salt of 2- (a-carboxy a-tritylaminomethyl) acid 5-aminométhyl 2,3-dihydro 1,3-thia- zine 4-carboxylique, fait agir sur ce sel l'acide acétique pour obte nir le D y-lactame de l'acide 2-(a-carboxy a-tritylaminométhyl) 5- aminométhyl 2,3-dihydro 1,3-thiazine 4-carboxylique brut, que l'on purifie, acidifie par ailleurs les liqueurs mères de cristallisa tion du sel de spartéine de l'isomère D par l'acide acétique, 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic, causes acetic acid to act on this salt to obtain the D y-lactam of 2- (a-carboxy a-tritylaminomethyl) acid Crude 5- aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid, which is purified, moreover acidifies the mother liquors of crystallization of the sparteine salt of isomer D by acetic acid, pour obtenir le L y-lactame de l'acide 2-(a-carboxy a-tritylaminomé- thyl) 5-aminométhyl 2,3-dihydro 1,3-thiazine 4-carboxylique brut que l'on purifie, récupère la 1-spartéine, utilisée dans le dédouble ment, dans les liqueurs mères des D et L y-lactame de l'acide 2-(a- carboxy a-tritylaminométhyl) 5-aminométhyl 2, to obtain the L y-lactam of the crude 2- (a-carboxy a-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid which is purified, the 1- sparteine, used in the resolution, in the mother liquors of the D and L y-lactam of 2- (a-carboxy a-tritylaminomethyl) 5-aminomethyl 2 acid, 3-dihydro 1,3- thiazine 4-carboxylique, fait réagir, au sein d'un mélange de chlo rure de méthylène et de nitrométhane, la dicyclohexylcarbodii- mide sur le L y-lactame de l'acide 2-(a-carboxy a-trity1aminomé- thyl) 5-aminométhyl 2,3-dihydro 1,3-thiazine 4-carboxylique, pour obtenir le y-lactame de l'acide L 6H, 3-dihydro 1,3-thiazine 4-carboxylic, reacts, in a mixture of methylene chloride and nitromethane, the dicyclohexylcarbodiimide with the L y-lactam of 2- (a-carboxy acid a-trity1aminomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic, to obtain the γ-lactam of L 6H acid, 7H cis 7-tritylamino 3 aminométhyl céph-3-ème 4-carboxylique, obtient, par ailleurs de la même façon, en faisant réagir la dicyclohexylcarbodiimide sur le D y-lactame de l'acide 2-(a-carboxy a-tritylaminométhyl) 5- aminométhyl 2,3-dihydro 1,3-thiazine 4-carboxylique, le y-lac- tame de l'acide D 6H, 7H cis 7-tritylamino 3 aminomethyl ceph-3-rd 4-carboxylic, obtained, moreover in the same way, by reacting dicyclohexylcarbodiimide on the D y-lactam of 2- (a-carboxy a-tritylaminomethyl) acid 5- aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid, γ-lactam of D 6H acid, 7H cis 7-tritylamino 3-aminométhyl céph- 3-ème 4-carboxylique, fait réagir sur le y-lactame de l'acide L 6H, 7H cis 7-tritylamino 3-aminométhyl céph-3-ème 4-carboxylique l'acide chlorhydrique gazeux au sein du nitrométhane, alcalinise par la triéthylamine pour obtenir le y-lactame de l'acide L 6H, 7H cis 7-tritylamino 3-aminomethyl ceph-3-rd 4-carboxylic acid, reacts with the y-lactam of L 6H, 7H cis 7-tritylamino 3-aminomethyl ceph-3-rd 4-carboxylic acid gaseous hydrochloric acid within nitromethane, alkalinized by triethylamine to obtain the y-lactam of L 6H acid, 7H cis 7-amino 3-aminométhyl céph-3-ème 4-carboxylique, obtient, par ailleurs de la même façon, par action de l'acide chlorhydrique gazeux sur le y-lactame de l'acide D 6H, 7H cis 7-tritylamino 3- aminométhyl céph-3-ème 4-carboxylique, 7H cis 7-amino 3-aminomethyl ceph-3-rd 4-carboxylic, obtained, moreover in the same way, by the action of hydrochloric acid gas on the y-lactam of the acid D 6H, 7H cis 7- tritylamino 3- aminomethyl ceph-3-rd 4-carboxylic, le y-lactame de l'acide D 6H, 7H cis 7-amino 3-aminométhyl céph-3-ème 4-carboxylique. 2. Procédé selon la 1, pour la purification du D y-lactame de l'acide 2-(a-carboxy (x-tritylaminométhyl) 5- aminométhyl 2,3-dihydro 1, the γ-lactam of D 6H, 7H cis 7-amino 3-aminomethyl ceph-3-rd 4-carboxylic acid. 2. Method according to 1, for the purification of D y-lactam from 2- (a-carboxy (x-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1 acid, 3-thiazine 4-carboxylique brut, carac térisé en ce que l'on transforme ce D y-lactante en sel de 1-spar- téine, cristallise le sel de spartéine dans un mélange d'eau et de méthanol, Crude 3-thiazine 4-carboxylic, charac terized in that this D y-lactant is converted into 1-sparteine salt, crystallizes the sparteine salt in a mixture of water and methanol, acidifie en milieu méthanolique par l'acide acétique pour obtenir le<B>D</B> y-lactame de l'acide 2-(a-carboxy a-tritylamino- méthyl) 5-aminométhyl 2,3-dihydro 1,3-thiazine 4-carboxylique pur. acidifies in methanolic medium with acetic acid to obtain the <B> D </B> y-lactam of 2- (a-carboxy a-tritylamino-methyl) 5-aminomethyl 2,3-dihydro 1,3 - pure 4-carboxylic thiazine. 3. Procédé selon la sous-revendication 1, pour la purification du L y-lactame de l'acide 2-(a-carboxy a-tritylaminométhyl) 5- aminométhyl 2,3-dihydro 1,3-thiazine 4-carboxylique brut, carac térisé en ce que l'on transforme le L y-lactame en sel de 1-éphé- drine, 3. Process according to sub-claim 1, for the purification of L y-lactam from crude 2- (a-carboxy a-tritylaminomethyl) 5-aminomethyl 2,3-dihydro 1,3-thiazine 4-carboxylic acid, charac terized in that the L y-lactam is converted into 1-ephedrine salt, cristallise le sel de 1-éphédrine formé dans un mélange de méthanol et d'éther éthylique, acidifie en milieu méthanolique par l'acide acétique le sel purifié, pour obtenir le L y-lactame de l'acide 2-(a-carboxy a-tritylaminométhyl) 5-aminométhyl 2,3-di- hydro 1,3-thiazine 4-carboxylique pur. crystallizes the salt of 1-ephedrine formed in a mixture of methanol and ethyl ether, acidifies in methanolic medium with acetic acid the purified salt, to obtain the L y-lactam of 2- (a-carboxy a -tritylaminomethyl) 5-aminomethyl 2,3-di-hydro 1,3-thiazine 4-carboxylic pure. 4. Procédé selon la sous-revendication 1, caractérisé en ce que l'on alcalinise les liqueurs mères de cristallisation des D et L y-lac- tames de l'acide 2-(a-carboxy a-tritylaminométhyl) 5-aminomé- thyl 2,3-dihydro 1,3-thiazine 4-carboxylique, puis élimine le mé thanol par distillation sous pression réduite et récupère ainsi la 1- spartéine utilisée dans le dédoublement. 4. Method according to sub-claim 1, characterized in that the mother liquors of crystallization of D and L y-lactam acid 2- (a-carboxy a-tritylaminomethyl) 5-aminomé are basified. thyl 2,3-dihydro 1,3-thiazine 4-carboxylique, then eliminates the methanol by distillation under reduced pressure and thus recovers the 1-sparteine used in the resolution.
CH1334071A 1968-06-27 1971-09-10 D-and l-isomers of 6h, 7h, cis-7-amino-3-aminomethyl cef -3 CH544775A (en)

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FR156898 1968-06-27
FR7033898A FR2120214A6 (en) 1970-09-18 1970-09-18 D-and l-isomers of 6h, 7h, cis-7-amino-3-aminomethyl cef -3 - em-4-car acid-gamma- lactams

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