CH521969A - Substd morphanthridene derivs - Google Patents

Substd morphanthridene derivs

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Publication number
CH521969A
CH521969A CH399772A CH399772A CH521969A CH 521969 A CH521969 A CH 521969A CH 399772 A CH399772 A CH 399772A CH 399772 A CH399772 A CH 399772A CH 521969 A CH521969 A CH 521969A
Authority
CH
Switzerland
Prior art keywords
formula
addition salts
acid addition
acid
methyl
Prior art date
Application number
CH399772A
Other languages
German (de)
Inventor
Alex Dr Berg
Klaus-Reinhold Dr Noll
Meyer Zu Reckendorf D Priv-Doz
Helmut Dr Franz
Original Assignee
Thomae Gmbh Dr K
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 Thomae Gmbh Dr K filed Critical Thomae Gmbh Dr K
Priority to CH399772A priority Critical patent/CH521969A/en
Publication of CH521969A publication Critical patent/CH521969A/en

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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D223/00Heterocyclic compounds containing seven-membered rings having one nitrogen atom as the only ring hetero atom
    • C07D223/14Heterocyclic compounds containing seven-membered rings having one nitrogen atom as the only ring hetero atom condensed with carbocyclic rings or ring systems
    • C07D223/18Dibenzazepines; Hydrogenated dibenzazepines
    • C07D223/20Dibenz [b, e] azepines; Hydrogenated dibenz [b, e] azepines
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D211/00Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings
    • C07D211/04Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings with only hydrogen or carbon atoms directly attached to the ring nitrogen atom
    • C07D211/06Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings 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
    • C07D211/08Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings 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 hydrocarbon or substituted hydrocarbon radicals directly attached to ring carbon atoms
    • C07D211/18Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings 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 hydrocarbon or substituted hydrocarbon radicals directly attached to ring carbon atoms with substituted hydrocarbon radicals attached to ring carbon atoms
    • C07D211/20Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings 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 hydrocarbon or substituted hydrocarbon radicals directly attached to ring carbon atoms with substituted hydrocarbon radicals attached to ring carbon atoms with hydrocarbon radicals, substituted by singly bound oxygen or sulphur atoms
    • C07D211/22Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings 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 hydrocarbon or substituted hydrocarbon radicals directly attached to ring carbon atoms with substituted hydrocarbon radicals attached to ring carbon atoms with hydrocarbon radicals, substituted by singly bound oxygen or sulphur atoms by oxygen atoms
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D211/00Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings
    • C07D211/04Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings with only hydrogen or carbon atoms directly attached to the ring nitrogen atom
    • C07D211/68Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having one double bond between ring members or between a ring member and a non-ring member
    • C07D211/70Heterocyclic compounds containing hydrogenated pyridine rings, not condensed with other rings with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having one double bond between ring members or between a ring member and a non-ring member with only hydrogen atoms, hydrocarbon or substituted hydrocarbon radicals, directly attached to ring carbon atoms

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

Abstract

Morphanthridenes of formula (I) (where R1= H or Me, R1=H or forms a piperidine ring by linkage to R3 or R4, R3 R4=Me or is linked to R2, X and Y,=H and/or hal). and their acid addition salts are anti-emetics histaminolytics, sedatives, spasmolytics, antiserotonics, pysychotropics. (I) may be prepd. by (a) ring closure of a 2-formyl-or 2-acety-lamino-diphenyl-methane analogue, e.g. with polyphosphoric acid or (b) dehydrogenation of the 5,6-dihydro analogne.

Description

  

  
 



  Verfahren zur Herstellung von neuen Morphanthridinen
Die Erfindung betrifft ein Verfahren zur Herstellung von neuen Morphanthridinen der Formel 1
EMI1.1     
 worin R1 ein Wasserstoffatom oder die Methylgruppe, R2 ein Wasserstoffatom oder zusammen mit   R    bzw.   R    und den dazwischenliegenden Kohlenstoffatomen und dem Stickstoffatom einen Piperidinring, R3 und/oder   Rw    Methylgruppen, X und Y, die gleich oder verschieden sein können,
Wasserstoff- oder Halogenatome bedeuten, sowie von deren Säureadditionssalzen mit anorganischen oder organischen Säuren.



   Die neuen Verbindungen werden erfindungsgemäss hergestellt, indem man eine Verbindung der Formel 2
EMI1.2     
 durch ein Oxydationsmittel dehydriert.



   Die Dehydrierung wird zweckmässig bei erhöhten Temperaturen, vorzugsweise bei Temperaturen zwischen 60 und   12()0C,    zweckmässig in einem organischen Lösungsmittel oder in Wasser bzw. in einer verdünnten   Mi-    neralsäure durchgeführt. Es können alle üblichen Oxydationsmittel, beispielsweise Chinone, Wasserstoffperoxyd, Jod, Chromsäure, Kaliumpermanganat, Eisen-IIIchlorid, oder nitrose Gase verwendet werden. Die Oxydation erfolgt jedoch auch bereits bei mehrstündigem Durchblasen von Luft bei erhöhten Temperaturen. Sie lässt sich auch mit allen angeführten Oxydationsmitteln bei Zimmertemperatur durchführen, die Reaktionsdauer beträgt dann jedoch mehrere Tage.



   Die nach dem Verfahren erhaltenen Verbindungen der Formel 1 können gewünschtenfalls nach üblichen Methoden in ihre Säureadditionssalze überführt werden.



  Als Säuren kommen physiologisch verträgliche anorganische oder organische Säuren wie Salzsäure, Schwefelsäure, Phosphorsäure, Zitronensäure, Maleinsäure, Fumarsäure oder Weinsäure in Betracht.



   Die als Ausgangsstoffe verwendeten Verbindungen der Formel 2 sind im belgischen Patent Nr. 652 938 [siehe C.A. 64, 19 575 h (1966)] beschrieben oder können analog dem beschriebenen Verfahren hergestellt werden.



   Die neuen Verbindungen sowie ihre Säureadditionssalze besitzen wertvolle therapeutische Eigenschaften, insbesondere weisen sie eine histaminolytische, sedative, spasmolytische, eine Antiserotoninwirkung, psychotrope und antiemetische Wirkung auf.



   Die pharmakologische Wirksamkeit von A   11 -(1 -Methyl-4-piperidyliden)-morphanthridin    wurde im Vergleich zu B =   SH-Dibenzo[a,d]-5-(1-methyl-4-piperidyliden)-cy-       cloheptenhydrochloridmonohydrat,    die von C =   3-Chlor- 11 -(3-dimethylaminopropyliden)-mor-    phanthridin im Vergleich zu D = 2-Methyl-3-o-tolyl-4(3H)-chinazolon getestet.  



  1)   Histamiaantagonistische    Wirkung am intakten Meer   schtveinchen:   
Nach der Methode von Konzett-Rössler [Arch. exp.



  Path. Pharmakol. 195, 71 (1940)] wurde die histaminantagonistische Wirkung vergleichend als eine den Histamin-bedingten Bronchospasmus des Meerschweinchens abschwächende Wirkung geprüft.



   Durch graphische Extrapolation wurde für jede Substanz die Dosis bestimmt, die zu einer 50%igen Abschwächung des mit der Standarddosis des Histamins erzielten Effektes führte:    Dosis Dosis Zahl der gemittelte Hemmeffekte y/kg i.v. Tiere i.v. in SO des Ausgangswertes   
A 5,0 5 38,6
A 10,0 4 54,0
A 20,0 4 64,9
B 5.0 10 10,0
B   10.0    7 42,4
B 20,0 6 54,5
B 40,0 4 68,9
Die nachfolgende Tabelle gibt die relative Wirksamkeit der Substanz A im Vergleich zu der Substanz B in der Versuchsanordnung nach Konzett-Rössler wieder:   
Substanz EDsp relative Wirksamkeit ylkg ylkg i.v.   



   A 8,6 1,92
B 16,5 1,00 2)   Sedierende    Wirkung:
Die sedierende Wirkung wurde an der Maus nach der Methode von Dews [Brit. J. Pharmacol. 8, 46 (1953)] bestimmt.



   Durch graphische Extrapolation wurde für jede Substanz die Dosis bestimmt, bei der die Motilität der Versuchstiere auf 50% herabgesetzt wird:   
Dosis Zahl der Motilität in %
Substanz mg/kg p.o. Tiere gegenüber Kontrollen   
C 3,125 5 99
C 6,25 5 96
C 12,5 5 47
C 25,0 5 18
C 50,0 5 9
C 100,0 5 1
D 25,0 10 70,3
D 50,0 10 50,5
D 100,0 10 27,6
Die nachfolgende Tabelle gibt die relative Wirksamkeit der Substanz C im Vergleich zu der Substanz D in der Versuchsanordnung nach Dews wieder:
Substanz   ED55    mg/kg p.o. relative Wirksamkeit
C 14 3,4
D 48 1 3) Akute Toxizität:
Die perorale akute Toxizität an der Maus wurde nach der Methode von Litchfield und Wilcoxon [J.



  Pharmacol. exp. Therap. 94, 99 (1949)] berechnet:
Substanz DL5o mg/kg relative Toxizität
A 176 1
B 106 1,66
Die nachstehenden Beispiele sollen die Erfindung näher erläutern:
Beispiel I
11-(1-Methyl-4piperidyliden)-morphanthridin
288 mg   5,6 - Dihydro- 11-    (1-methyl-4-piperidyliden) -morphanthridin werden in 15 ml Toluol mit 245 mg Chloranil 3 Stunden gekocht. Die Reaktionslösung wird nach Abkühlen filtriert und mit Salzsäure extrahiert.



  Aus der salzsäuren Lösung wird mit Ammoniak die Base in Freiheit gesetzt und in Äther aufgenommen. Nach dem Trocknen über Natriumsulfat und Einengen der Ätherlösung erhält man 150 mg   1 1-(1-Methyl-4-piperi-    dyliden)-morphanthridin vom Schmelzpunkt   1030C.   



   Die gleiche Verbindung wird auch erhalten, wenn man 288 mg   5,6-Dihydro-1 1-(l-methyl-4-piperidyliden)-    -morphanthridin in 30 ml verdünnter Salzsäure löst und unter Erhitzen auf 1000C 8 Stunden lang Luft durchleitet.



   Ausbeute:   170mg,    Schmelzpunkt: 100 bis   102oC.   



   Beispiel 2
11-(3-Dimethylaminopropyliden)-morphanthridin
Aus 5,6 - Dihydro - 11 - (3-dimethylaminopropyliden) -morphanthridin analog Beispiel 1. Das erhaltene Produkt ist sirupartig, aber dünnschichtchromatographisch einheitlich.



   Schmelzpunkt des Produktes: 175 bis 1760C.



   Beispiel 3    3-Chlar-11-(3-dimethylaminopropyliden)-mmrphanthridin   
Aus   3 -Chlor-5,6-dihydro- 1 1-(3-dimethylaminopropy-    liden)-morphanthridin analog Beispiel 1.



   Schmelzpunkt: 119 bis 1200C.



   Die Verbindungen der Formel 1 können zur pharmazeutischen Anwendung in die üblichen pharmazeutischen Präparate eingearbeitet werden gegebenenfalls in Kombination mit anderen Wirksubstanzen. Die Einzeldosis beträgt für Erwachsene bei innerer Anwendung 0,25 bis 8,0 mg, vorzugsweise 2,0 bis 4,0 mg, die Tages  dosis 5 bis 50 mg, für Kinder die Hälfte bis ein Viertel dieser Dosis. Bei lokaler Anwendung beträgt die Konzentration 0,1 bis 0,5%, vorzugsweise 0,2%. 



  
 



  Process for the preparation of new morphanthridines
The invention relates to a process for the preparation of new morphanthridines of the formula 1
EMI1.1
 in which R1 is a hydrogen atom or the methyl group, R2 is a hydrogen atom or together with R or R and the carbon atoms in between and the nitrogen atom a piperidine ring, R3 and / or Rw are methyl groups, X and Y, which can be identical or different,
Mean hydrogen or halogen atoms, as well as their acid addition salts with inorganic or organic acids.



   According to the invention, the new compounds are prepared by adding a compound of the formula 2
EMI1.2
 dehydrated by an oxidizing agent.



   The dehydrogenation is expediently carried out at elevated temperatures, preferably at temperatures between 60 and 12 ° C., expediently in an organic solvent or in water or in a dilute mineral acid. All the usual oxidizing agents, for example quinones, hydrogen peroxide, iodine, chromic acid, potassium permanganate, ferric chloride, or nitrous gases can be used. However, the oxidation also takes place when air is blown through for several hours at elevated temperatures. It can also be carried out with all the oxidizing agents mentioned at room temperature, but the reaction time is then several days.



   The compounds of formula 1 obtained by the process can, if desired, be converted into their acid addition salts by customary methods.



  Suitable acids are physiologically compatible inorganic or organic acids such as hydrochloric acid, sulfuric acid, phosphoric acid, citric acid, maleic acid, fumaric acid or tartaric acid.



   The compounds of formula 2 used as starting materials are described in Belgian Patent No. 652 938 [see C.A. 64, 19 575 h (1966)] or can be prepared analogously to the process described.



   The new compounds and their acid addition salts have valuable therapeutic properties, in particular they have a histaminolytic, sedative, spasmolytic, antiserotonin, psychotropic and antiemetic effect.



   The pharmacological effectiveness of A 11 - (1-methyl-4-piperidylidene) -morphanthridine was compared to B = SH-dibenzo [a, d] -5- (1-methyl-4-piperidylidene) -cycloheptene hydrochloride monohydrate, the of C = 3-chloro-11 - (3-dimethylaminopropylidene) -morphanthridine compared to D = 2-methyl-3-o-tolyl-4 (3H) -quinazolone tested.



  1) Histamia antagonistic effect on the intact sea schtveinchen:
According to the method of Konzett-Rössler [Arch. exp.



  Path. Pharmacol. 195, 71 (1940)], the histamine-antagonistic effect was tested comparatively as an effect that attenuated the histamine-induced bronchospasm in guinea pigs.



   The dose that led to a 50% weakening of the effect achieved with the standard dose of histamine was determined by graphical extrapolation for each substance: dose dose number of averaged inhibitory effects y / kg i.v. Animals i.v. in SO of the initial value
A 5.0 5 38.6
A 10.0 4 54.0
A 20.0 4 64.9
B 5.0 10 10.0
B 10.0 7 42.4
B 20.0 6 54.5
B 40.0 4 68.9
The following table shows the relative effectiveness of substance A in comparison to substance B in the experimental setup according to Konzett-Rössler:
Substance EDsp relative effectiveness ylkg ylkg i.v.



   A 8.6 1.92
B 16.5 1.00 2) Sedative effect:
The sedative effect was determined on the mouse by the method of Dews [Brit. J. Pharmacol. 8, 46 (1953)].



   The dose at which the motility of the test animals is reduced to 50% for each substance was determined by graphical extrapolation:
Dose number of motility in%
Substance mg / kg p.o. Animals versus controls
C 3.125 5 99
C 6.25 5 96
C 12.5 5 47
C 25.0 5 18
C 50.0 5 9
C 100.0 5 1
D 25.0 10 70.3
D 50.0 10 50.5
D 100.0 10 27.6
The following table shows the relative effectiveness of substance C in comparison to substance D in the test arrangement according to Dews:
Substance ED55 mg / kg p.o. relative effectiveness
C 14 3.4
D 48 1 3) Acute toxicity:
The acute peroral toxicity in the mouse was determined by the method of Litchfield and Wilcoxon [J.



  Pharmacol. exp. Therap. 94, 99 (1949)] calculated:
Substance DL50 mg / kg relative toxicity
A 176 1
B 106 1.66
The following examples are intended to explain the invention in more detail:
Example I.
11- (1-methyl-4piperidylidene) -morphanthridine
288 mg of 5,6-dihydro-11- (1-methyl-4-piperidylidene) -morphanthridine are boiled in 15 ml of toluene with 245 mg of chloranil for 3 hours. After cooling, the reaction solution is filtered and extracted with hydrochloric acid.



  The base is set free from the hydrochloric acid solution with ammonia and taken up in ether. After drying over sodium sulfate and concentrating the ether solution, 150 mg of 1 1- (1-methyl-4-piperidylidene) -morphanthridine with a melting point of 1030 ° C. are obtained.



   The same compound is also obtained when 288 mg of 5,6-dihydro-1 1- (l-methyl-4-piperidylidene) - -morphanthridine is dissolved in 30 ml of dilute hydrochloric acid and air is passed through it for 8 hours while heating to 1000 ° C.



   Yield: 170mg, melting point: 100 to 102oC.



   Example 2
11- (3-dimethylaminopropylidene) morphanthridine
From 5,6-dihydro-11- (3-dimethylaminopropylidene) -morphanthridine analogously to Example 1. The product obtained is syrupy, but uniform according to thin-layer chromatography.



   Melting point of the product: 175 to 1760C.



   Example 3 3-Chlar-11- (3-dimethylaminopropylidene) -mmrphanthridine
From 3-chloro-5,6-dihydro-1 1- (3-dimethylaminopropylidene) -morphanthridine analogously to Example 1.



   Melting point: 119 to 1200C.



   For pharmaceutical use, the compounds of formula 1 can be incorporated into the customary pharmaceutical preparations, if appropriate in combination with other active substances. The single dose for adults for internal use is 0.25 to 8.0 mg, preferably 2.0 to 4.0 mg, the daily dose is 5 to 50 mg, and for children, half to a quarter of this dose. When applied locally, the concentration is 0.1 to 0.5%, preferably 0.2%.

 

Claims (1)

PATENTANSPRUCH PATENT CLAIM Verfahren zur Herstellung von neuen Morphanthridinen der Formel 1 EMI3.1 worin Rl ein Wasserstoffatom oder die Methylgruppe, R ein Wasserstoffatom oder zusammen mit R3 bzw. Rg und den dazwischenliegenden Kohlenstoffatomen und dem Stickstoffatom einen Piperidinring, R3 und/oder R4 Methylgruppen, X und Y, die gleich oder verschieden sein können, Wasserstoff- oder Halogenatome bedeuten, sowie von ihren Säureadditionssalzen mit physiologisch verträglichen anorganischen oder organischen Säuren, dadurch gekennzeichnet, dass man eine Verbindung der Formel 2 EMI3.2 durch ein Oxydationsmittel dehydriert. Process for the preparation of new morphanthridines of formula 1 EMI3.1 wherein Rl is a hydrogen atom or the methyl group, R is a hydrogen atom or together with R3 or Rg and the carbon atoms in between and the nitrogen atom a piperidine ring, R3 and / or R4 are methyl groups, X and Y, which can be identical or different, Denotes hydrogen or halogen atoms, as well as their acid addition salts with physiologically compatible inorganic or organic acids, characterized in that a compound of the formula 2 EMI3.2 dehydrated by an oxidizing agent. UNTERANSPRÜCHE 1. Verfahren nach Patentanspruch, dadurch gekennzeichnet, dass man die Dehydrierung in einem organischen oder wässrigen Lösungsmittel durchführt. SUBCLAIMS 1. The method according to claim, characterized in that the dehydrogenation is carried out in an organic or aqueous solvent. 2. Verfahren nach Patentanspruch, dadurch gekennzeichnet, dass man die erhaltenen Verbindungen in ihre Säureadditionssalze mit physiologisch verträglichen anorganischen oder organischen Säuren überführt. 2. The method according to claim, characterized in that the compounds obtained are converted into their acid addition salts with physiologically compatible inorganic or organic acids.
CH399772A 1969-04-28 1969-04-28 Substd morphanthridene derivs CH521969A (en)

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Application Number Priority Date Filing Date Title
CH645169A CH521974A (en) 1969-04-28 1969-04-28 Substd morphanthridene derivs
CH399772A CH521969A (en) 1969-04-28 1969-04-28 Substd morphanthridene derivs

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