[go: up one dir, main page]

CH533105A - Pyrrolidine derivs hypotensive - Google Patents

Pyrrolidine derivs hypotensive

Info

Publication number
CH533105A
CH533105A CH499471A CH499471A CH533105A CH 533105 A CH533105 A CH 533105A CH 499471 A CH499471 A CH 499471A CH 499471 A CH499471 A CH 499471A CH 533105 A CH533105 A CH 533105A
Authority
CH
Switzerland
Prior art keywords
evapd
etoh
alkyl
formula
hrs
Prior art date
Application number
CH499471A
Other languages
German (de)
Inventor
Miller David
Sylvester Fake Charles
Original Assignee
Beecham Group Ltd
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 GB55708/67A external-priority patent/GB1185080A/en
Application filed by Beecham Group Ltd filed Critical Beecham Group Ltd
Publication of CH533105A publication Critical patent/CH533105A/en

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D207/00Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom
    • C07D207/02Heterocyclic 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
    • 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
    • C07D207/32Heterocyclic 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 only hydrogen atoms, hydrocarbon or substituted hydrocarbon radicals, directly attached to ring carbon atoms
    • C07D207/325Heterocyclic 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 only hydrogen atoms, hydrocarbon or substituted hydrocarbon radicals, directly attached to ring carbon atoms with substituted hydrocarbon radicals directly attached to the ring nitrogen atom
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D207/00Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom
    • C07D207/02Heterocyclic 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
    • C07D207/04Heterocyclic 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 no double bonds between ring members or between ring members and non-ring members
    • C07D207/06Heterocyclic 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 no double bonds between ring members or between ring members and non-ring members with radicals, containing only hydrogen and carbon atoms, attached to ring carbon atoms
    • 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
    • C07D295/12Heterocyclic 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 or doubly bound nitrogen atoms
    • C07D295/125Heterocyclic 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 or doubly bound nitrogen atoms with the ring nitrogen atoms and the substituent nitrogen atoms attached to the same carbon chain, which is not interrupted by carbocyclic rings
    • C07D295/13Heterocyclic 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 or doubly bound nitrogen atoms with the ring nitrogen atoms and the substituent nitrogen atoms attached to the same carbon chain, which is not interrupted by carbocyclic rings to an acyclic saturated chain
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D303/00Compounds containing three-membered rings having one oxygen atom as the only ring hetero atom
    • C07D303/02Compounds containing oxirane rings
    • C07D303/04Compounds containing oxirane rings containing only hydrogen and carbon atoms in addition to the ring oxygen atoms

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Pyrrole Compounds (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)

Abstract

(A) Method for cmpds. (I):- - and salts of (I), including all optical and geometrical stereoisomers. - (B) The cpds. (II) and some (III) - where R, R1 and R3 = H or (1-6C) alkyl - R2 = (1-6C) alkyl or cycloalkyl - R4 and R5 = H or (1-6C) alkyl, one of them may be NH2 or NO2 or - R4 + R5 together may be -CH2CH2- - n = 2-8 - Hypotensives with low side effects. - (a) 3-Chloromethylbut-1-yne-3-ol (11.85 g.), ethylenediamine hydrate (63.4 ml.), and EtOH (40 ml.), were refluxed 17 hrs., evapd. in vac., 40% NaOH (10 ml.) added, H2O removed by azeotropic distn. with PhH, evapd., and distilled, giving the pyrrol (III) (5.82 g.), b.p. 65.5-66 deg./2 mm. - (b) This (12.4 g.) was hydrog. at 25 deg. and 35 kg/cm2 in EtOH (250 ml.) and 5N-HCl (40 ml.), over a 5% Rh.-Al2O3 catalyst (5.0 g.), for 60 hrs. The mixture was filtered, evapd., basified (d.NaOH), extd. with Et2O, and distilled, giving the pyrrolidine (II) (8.72 g.), b.p. 66 deg./14 mm. - (c) This (3.84 g.), S-methylisothiouronium sulphate (4.17 g.), EtOH (40 ml.), and H2O (20 ml.), were refluxed 3.5 hrs., cooled, filtered, neutralised with 5N H2SO4 (6.0 ml.), evapd. in vac., and the residue refluxed with EtOH, giving (I) (7.31 g., 91%), m.p. 233-7 deg. (dec.).

Description

  

  Verfahren zur Herstellung von Pyrrolidinoguanidin-Verbindungen    Die vorliegende Erfindung     betrifft    ein Verfahren zur  Herstellung neuer Pyrrolidino-Guanidin-Verbindungen.  Es handelt sich dabei um Substanzen, welche gute blut  drucksenkende Eigenschaften mit geringen Nebenwir  kungen aufweisen.  



  Bei den neuen Verbindungen handelt es sich um  solche der Formel (I), sowie um deren ungiftige Säure  additionssalze:  
EMI0001.0001     
         (HI)     In der Formel bedeuten R, R1 und R,3 Wasserstoff  oder niederes Alkyl. R2 ist niederes Alkyl oder     Cyclo-          alkyl.     



  n ist eine ganze Zahl von 2     bis    B.  



  Die neuen Verbindungen können. als Cis- und Trans  isomere vorkommen, wobei beide dieser     Formel    nach  dem erfindungsgemässen Verfahren herstellbar sind. Da  die Verbindungen ebenfalls     asymmetrische    Kohlenstoff  atome enthalten können sie auch in optisch aktiven  existieren, welche wiederum gleichfalls sich nach  dem     erfindungsgemässen    Verfahren herstellen lassen.  Der im vorstehenden benutzte Ausdruck  niederes  Alkyl  gilt für Alkylgruppen mit 1 bis 6 Kohlenstoffato  men.  



  Das erfindungsgemässe Verfahren zur Herstellung  der Verbindungen der Formel (1) ist dadurch gekenn  zeichnet, dass man ein Pyrrolidinoamin der Formel (II):  
EMI0001.0009     
    oder ein Salz davon mit einem gegebenenfalls alkylierten  1-Guanylpyrazol, insbesondere mit     1-Guanyl-3,5-dime-          thylpyrazol,    oder mit einem Salz davon umsetzt.  



  Vorzugsweise wird das guanylierende Agens mit dem  Amin oder dessen Salz in einem inerten Lösungsmittel  erwähnt, wobei die Verbindung der     Formel    (I) entsteht.  



  Die als Ausgangsprodukt verwendeten     Pyrrolidino-          alkylamine    können durch katalytische Hydrierung in  Lösung eines entsprechenden Fyrrols der Formel  hergestellt werden:  
EMI0001.0015     
    Hierbei kann man als Katalysator z.B. Rhodium auf  Aluminiumoxyd bzw. einen 5 oder 10% Palladium auf  Kohle enthaltenden Katalysator verwenden. Falls R oder  R1 andere Reste sind als ein Wasserstoffatom lassen sich  durch diese Reaktion Gemische von Cis-trans-Isomeren  herstellen.  



  Zar Herstellung der Pyrrolalkylamine der Formel  (III) können verschiedene Verfahren zur Anwendung ge  langen und insbesondere: (1) Umsetzung eines     acetyleni-          schen    Chlorcarbinols ClCHR - CR2(OH) - C-CR1  oder ClCHR - CR2(OH) - CH2 - C=CH mit einem  Amin NH2 - (CH2)n - NH2.  



  (2) Umsetzung eines     acetylenischen    Eiloxids der For  meln  
EMI0001.0019     
    oder    
EMI0002.0000     
    mit einem Amin NH2-(CH2)n-NH2.  



  (3) Überführung eines Pyrralalkanols der Formel  
EMI0002.0001     
    a  in ein reaktives Derivat der Formel  
EMI0002.0002     
    ,  worin in der letzteren Formel X ein     Halogenatom    oder  der Rest einer Sulfonsäure insbesondere     p-Toluolsulfon-          säure    ist und Umsetzung dieser Verbindung mit einem  Amin R3NH2.  



  Die Pyrrolidinoalkylamine der Formel (II) sind  gleichfalls neue Verbindungen, wie dies auch für eine  Anzahl der     anderen    im vorliegenden     beschriebenen    Zwi  schenprodukte zutrifft.  



  Die neuen Pyrrolidinoguanidine der Formel (I) las  sen sich in pharmazeutische Kompositionen einarbeiten  mit geeigneten     pharmazeutischen    Trägern. Geeignete  Trägerstoffe sind z.B. Excipientien, Füllstoffe, Binde  mittel und steriles Waser, woraus sich Zubereitungen  zur oralen parenteralen oder anderswie gearteten Ver  abreichung herstellen     lassen.     



  <I>Beispiel</I>  Eine Mischung von     1-Guanyl-3,5-dimethylpyrazol-          nitrat    u. 1-(&alpha;-Aminoäthyl)-2,4-dimethylpyrrolidin, wur  den 2¸ Stunden lang unter Rühren erwärmt. Der     Über-          schuss    an Amin wurde im Vakuum abgetrieben und der    Rückstand in Wasser gelöst. Es erfolgte Überführung in  das     1-(&alpha;-Guanidinoäthyl)-2,4-dimethylpyrrolidinsulfat-          hydrat    durch Behandlung mit einem starken Anionen  austauscherharz in Form des Sulfates. Die erhaltene Lö  sung wurde unter vermindertem Druck eingedampft und  der Rückstand aus wässrigem     Äthanol    kristallisiert. Das  erhaltene Produkt wurde aus Aceton/Wasser umkristal  lisiert.

   Smp. = 291 bis 292 C (Zers.). Es handelte sich  um     1-(&alpha;-Guanidinoäthyl)-2,4-dimethylpyrrolidin-sulfat-          -hydrat.  



  Process for the preparation of pyrrolidino-guanidine compounds The present invention relates to a process for the preparation of new pyrrolidino-guanidine compounds. These are substances that have good blood pressure-lowering properties with few side effects.



  The new compounds are those of the formula (I) and their non-toxic acid addition salts:
EMI0001.0001
         (HI) In the formula, R, R1 and R, 3 denote hydrogen or lower alkyl. R2 is lower alkyl or cycloalkyl.



  n is an integer from 2 to B.



  The new connections can. occur as cis and trans isomers, both of these formulas being producible by the process according to the invention. Since the compounds also contain asymmetric carbon atoms, they can also exist in optically active ones, which in turn can also be produced by the process according to the invention. The term lower alkyl used in the above applies to alkyl groups having 1 to 6 carbon atoms.



  The process according to the invention for the preparation of the compounds of the formula (1) is characterized in that a pyrrolidinoamine of the formula (II):
EMI0001.0009
    or a salt thereof is reacted with an optionally alkylated 1-guanylpyrazole, in particular with 1-guanyl-3,5-dimethylpyrazole, or with a salt thereof.



  Preferably the guanylating agent is mentioned with the amine or its salt in an inert solvent, whereby the compound of formula (I) is formed.



  The pyrrolidinoalkylamines used as the starting material can be prepared by catalytic hydrogenation in a solution of a corresponding fyrrole of the formula:
EMI0001.0015
    The catalyst here can be e.g. Use rhodium on aluminum oxide or a catalyst containing 5 or 10% palladium on carbon. If R or R1 are radicals other than a hydrogen atom, mixtures of cis-trans isomers can be produced by this reaction.



  To prepare the pyrrole alkylamines of the formula (III), various processes can be used, and in particular: (1) Reaction of an acetylenic chlorocarbinol ClCHR - CR2 (OH) - C-CR1 or ClCHR - CR2 (OH) - CH2 - C = CH with an amine NH2 - (CH2) n - NH2.



  (2) Implementation of an acetylenic oxide of the formula
EMI0001.0019
    or
EMI0002.0000
    with an amine NH2- (CH2) n-NH2.



  (3) Conversion of a pyrralalkanol of the formula
EMI0002.0001
    a into a reactive derivative of the formula
EMI0002.0002
    in which in the latter formula X is a halogen atom or the residue of a sulfonic acid, in particular p-toluenesulfonic acid, and reaction of this compound with an amine R3NH2.



  The pyrrolidinoalkylamines of the formula (II) are also new compounds, as is also the case for a number of the other intermediate products described herein.



  The new pyrrolidinoguanidines of the formula (I) can be incorporated into pharmaceutical compositions with suitable pharmaceutical carriers. Suitable carriers are e.g. Excipients, fillers, binders and sterile water, from which preparations for oral parenteral administration or other types of administration can be produced.



  <I> Example </I> A mixture of 1-guanyl-3,5-dimethylpyrazole nitrate u. 1 - (α-Aminoethyl) -2,4-dimethylpyrrolidine, was heated with stirring for 2¸ hours. The excess of amine was driven off in vacuo and the residue was dissolved in water. It was converted into 1 - (α-guanidinoethyl) -2,4-dimethylpyrrolidine sulfate hydrate by treatment with a strong anion exchange resin in the form of the sulfate. The solution obtained was evaporated under reduced pressure and the residue was crystallized from aqueous ethanol. The product obtained was recrystallized from acetone / water.

   M.p. = 291-292 C (dec). It was 1 - (α-guanidinoethyl) -2,4-dimethylpyrrolidine sulfate hydrate.

 

Claims (1)

PATENTANSPRUCH Verfahren zur Herstellung von Pyrrolidinoguanidin- verbindungen der Formel EMI0002.0021 und ihrer ungiftigen Säureadditionssalze, wobei R, R1 und R3 Wasserstoff oder Niederalkyl, R= Niederalkyl oder Cycloalkyl und n eine ganze Zahl von 2 bis 8 ist, dadurch gekennzeichnet dass ein Pyrrolidinoamin der Formel EMI0002.0022 oder ein Salz davon mit einem gegebenenfalls alkylsub stituierten 1-Guanylpyrazol oder einem Salz davon um gesetzt wird. UNTERANSPRUCH Verfahren nach Patentanspruch, dadurch gekenn zeichnet, dass man mit 1-Guanyl-3,5-dimethylpyrazol oder einem Salz davon arbeitet. PATENT CLAIM Process for the production of pyrrolidinoguanidine compounds of the formula EMI0002.0021 and their non-toxic acid addition salts, where R, R1 and R3 are hydrogen or lower alkyl, R = lower alkyl or cycloalkyl and n is an integer from 2 to 8, characterized in that a pyrrolidinoamine of the formula EMI0002.0022 or a salt thereof is reacted with an optionally alkyl-substituted 1-guanylpyrazole or a salt thereof. SUBClaimed method according to claim, characterized in that 1-guanyl-3,5-dimethylpyrazole or a salt thereof is used.
CH499471A 1967-12-07 1968-12-09 Pyrrolidine derivs hypotensive CH533105A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB55708/67A GB1185080A (en) 1967-12-07 1967-12-07 Pyrrolidines
CH1833468A CH534679A (en) 1967-12-07 1968-12-09 Process for the preparation of pyrrolidino compounds

Publications (1)

Publication Number Publication Date
CH533105A true CH533105A (en) 1973-01-31

Family

ID=25720857

Family Applications (1)

Application Number Title Priority Date Filing Date
CH499471A CH533105A (en) 1967-12-07 1968-12-09 Pyrrolidine derivs hypotensive

Country Status (1)

Country Link
CH (1) CH533105A (en)

Similar Documents

Publication Publication Date Title
DE965036C (en) Process for the preparation of p-(bis-2-chloroethylamino)-ª‰-phenyl-alanine
DE2527914C3 (en) Vincamine derivatives, processes for their preparation and pharmaceutical agents
DE2929517A1 (en) PINE DERIVATIVES, METHOD FOR THEIR PRODUCTION AND PHARMACEUTICAL PREPARATIONS CONTAINING THE SAME
DE69102762T2 (en) BETA-PHENYLISOSER DERIVATIVES, THEIR PRODUCTION AND THEIR USE.
CH533105A (en) Pyrrolidine derivs hypotensive
DE2454950C2 (en) Process for the preparation of 2-aminobutan-1-ol and its acid addition salts
DE2303176A1 (en) SUBSTITUTED 5-CHROMANOLS, METHOD FOR THEIR MANUFACTURING AND MEDICINAL PREPARATIONS CONTAINING THESE COMPOUNDS
DE69014434T2 (en) Crystalline aluminophosphates and related compounds.
DE1693032B1 (en) Process for the preparation of 1,2-disubstituted adamantane compounds
DE2718533C3 (en) Catalyst system and its use for asymmetric hydrogenation
AT208872B (en) Process for the preparation of new 1,4-diazacycloheptanes
AT317209B (en) Process for the preparation of new phenylimidazolidinone derivatives and their salts
DE948687C (en) Process for the production of dialkylxanthine capsules
AT334874B (en) PROCESS FOR THE PREPARATION OF NEW 2,2,3-TRIMETHYL-7-AMINONORBORNANES AND THEIR ACID ADDITION SALTS
DE1199753B (en) Process for the preparation of glucuronic acid amides and their N-alkyl substitution products
DE842345C (en) Process for the preparation of heterocyclic nitrogen compounds
DE2511576A1 (en) METFORMIN-CLOFIBRATE, THE METHOD FOR MANUFACTURING IT AND THE MEDICINAL PRODUCT CONTAINING IT
DE1811832A1 (en) Pyrrolidine derivs hypotensive
DE2628042B2 (en) 3-Amino-tricyclo [53.1.0.3A1 -undecane, its acid addition salts and process for the preparation of these compounds
AT266080B (en) Process for the preparation of the new 1-isopropylamino-2-hydroxy-3- (o-lower alkoxymethyl-phenoxy) -propanes and their salts
DE859892C (en) Process for the preparation of substituted piperidinoacetic acid esters
AT282594B (en) PROCESS FOR THE PREPARATION OF NEW RACEMIC OR OPTICALLY ACTIVE (1-2&#39;-NITRILOPHENOXY) -2-HYDROXY-3-ISOPROPYLAMINOPROPANE AND ITS SALTS
DE2263093A1 (en) 7-METHOXY-2,3-DIHYDROBENZOFURA DERIVATIVES AND THE PROCESS FOR THEIR PRODUCTION
DE2027433C3 (en) Basic ß-thienyl derivatives, processes for their preparation and pharmaceuticals containing them
AT309395B (en) Process for the preparation of (+) - 2,2 &#39;- (ethylenediimino) -di-1-butanol-dihydrochloride

Legal Events

Date Code Title Description
PL Patent ceased