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DE1008308B - Process for the preparation of ª[(ª-dialkylamino-alkyl)-alkyl-amino]-phenyl-acetic acid isoamyl and -n-nonyl esters - Google Patents

Process for the preparation of ª[(ª-dialkylamino-alkyl)-alkyl-amino]-phenyl-acetic acid isoamyl and -n-nonyl esters

Info

Publication number
DE1008308B
DE1008308B DEA17418A DEA0017418A DE1008308B DE 1008308 B DE1008308 B DE 1008308B DE A17418 A DEA17418 A DE A17418A DE A0017418 A DEA0017418 A DE A0017418A DE 1008308 B DE1008308 B DE 1008308B
Authority
DE
Germany
Prior art keywords
alkyl
amino
isoamyl
acetic acid
nonyl
Prior art date
Legal status (The legal status 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 status listed.)
Pending
Application number
DEA17418A
Other languages
German (de)
Inventor
Phil Nat Habil Herbert Arno Dr
Dr Phil Engelbert Kuehas
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Asta-Werke A-G Chemische Fabrik
Asta Medica GmbH
Original Assignee
Asta-Werke A-G Chemische Fabrik
Asta Werke AG Chemische Fabrik
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 Asta-Werke A-G Chemische Fabrik, Asta Werke AG Chemische Fabrik filed Critical Asta-Werke A-G Chemische Fabrik
Priority to DEA17418A priority Critical patent/DE1008308B/en
Publication of DE1008308B publication Critical patent/DE1008308B/en
Pending legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C231/00Preparation of carboxylic acid amides
    • C07C231/02Preparation of carboxylic acid amides from carboxylic acids or from esters, anhydrides, or halides thereof by reaction with ammonia or amines

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Description

DEUTSCHESGERMAN

Nach dem Verfahren der deutschen Patentschrift 842 206 sind a-[(jS-Dialkylamino-alkyl)-amino]-phenylessigsäureester bekannt, von denen sich der <z-[(/5-Diäthylaminoäthyl) - amino] - phenyl - essigsaure - isoamylester der FormelAccording to the method of German Patent 842 206, a - [(jS-Dialkylamino-alkyl) -amino] -phenylacetic acid esters are obtained known, of which the <z - [(/ 5-diethylaminoethyl) - amino] - phenyl - acetic acid - isoamyl ester of formula

>—CH-COO-C5H11 (i)> —CH-COO-C 5 H 11 (i)

NH-CH2-CH2N (C2H5)2 NH-CH 2 -CH 2 N (C 2 H 5 ) 2

insbesondere durch eine muskulotrope, papaverinähnliche « Wirkung auszeichnet. Diese Verbindungen werden auf dem Wege der N-Alkylierung von a-Amino-phenyl-essigsäureestern erhalten, wobei die Umsetzung in Abwesenheit von Lösungsmitteln und unter Anwendung von Dialkylamino-alkylhalogeniden in Form ihrer Hydrohalogenide durchgeführt wird.especially through a musculotropic, papaverine-like " Effect. These compounds are obtained by means of the N-alkylation of α-amino-phenylacetic acid esters obtained, the reaction in the absence of solvents and with the use of Dialkylamino-alkyl halides is carried out in the form of their hydrohalides.

Es hat sich nun überraschenderweise herausgestellt, daß diese Verbindungen in der muskulotropen, papaverinähnlichen Wirkung von Verbindungen der allgemeinen Formel 1:It has now surprisingly been found that these compounds are in the musculotropic, papaverine-like Effect of compounds of general formula 1:

— CH-COO —R,- CH-COO —R,

R1-N-CH-CH2-NR 1 -N-CH-CH 2 -N

worin R und R1 = Methyl oder Äthyl, R2 = Wasserstoff oder Methyl und R3 = iso-Amyl oder n-Nonyl bedeuten, um etwa das vier- bis fünffache übertroffen werden.where R and R 1 = methyl or ethyl, R 2 = hydrogen or methyl and R 3 = iso-amyl or n-nonyl, are exceeded by about four to five times.

In der nachfolgenden Aufstellung werden die im Vergleich zu Papaverin, das gleich 1 gesetzt wurde, benötigten Mengen der neuen Verbindungen angegeben:In the following list, the required compared to papaverine, which was set equal to 1 Amounts of the new compounds indicated:

CHa CH a

N-CH9-CH9-NN-CH 9 -CH 9 -N

COO-C6H1 COO-C 6 H 1

-CH-CH

CH,CH,

N-CH2-CH2-NN-CH 2 -CH 2 -N

CH-COO-CH1 CH-COO-CH 1

C9H=C 9 H =

N- CH-CH9-NN-CH-CH 9 -N

-CH-COO-C9H19 -CH-COO-C 9 H 19

CH,CH,

CH,CH,

CH,CH,

CH5 CH 5

C9H5 C 9 H 5

C9H5 C 9 H 5

1 : 0,271: 0.27

1 : 0,191: 0.19

1 : 0,231: 0.23

Verfahren zur HerstellungMethod of manufacture

von α [(^Dialkylamino-alkyl)-alkyl-amino]-of α [(^ dialkylamino-alkyl) -alkyl-amino] -

phenyl-essigsäure-isoamyl- undphenylacetic acid isoamyl and

-n-nonylestern-n-nonyl esters

Anmelder:Applicant:

Asta-Werke A.-G.r Chemische Fabrik,
Brackwede (Westf.), Bielefelder Str. 83
Asta-Werke A.-G. r chemical factory,
Brackwede (Westphalia), Bielefelder Str. 83

Dr. phil. nat. habil. Herbert Arnold, Bielefeld,Dr. phil. nat. habil. Herbert Arnold, Bielefeld,

und Dr. phil. Engelbert Kühas, Gadderbaum,and Dr. phil. Engelbert Kühas, Gadderbaum,

sind als Erfinder genannt wordenhave been named as inventors

a5 Diese Verbindungen sind auf dem vorgenannten Verfahrensweg erhältlich, sie werden jedoch bevorzugt durch Erhitzen der entsprechenden a-Halogen-phenyl-cssigsäureester mit entsprechend substituierten aliphatischen Diaminen in Abwesenheit von Lösungsmitteln gemäß folgendem Reaktionsschema: a 5 These compounds can be obtained by the above-mentioned process route, but they are preferably obtained by heating the corresponding a-halophenyl acetic acid ester with appropriately substituted aliphatic diamines in the absence of solvents according to the following reaction scheme:

CH- CO — OR,CH- CO - OR,

HalHal

R1-NH-CH(R2)-CH2-N(R)2 >1 R 1 -NH-CH (R 2 ) -CH 2 -N (R) 2 > 1

worin R, R1, R2 und R3 die oben angegebene Bedeutung haben, hergestellt.in which R, R 1 , R 2 and R 3 have the meanings given above.

Daß die Umsetzung zwischen den a-Halogen-phenylessigsäureestern und den substituierten Diaminen ausschließlich in der angegebenen Richtung verläuft und zur Bildung der a-[(/?-Dialkylaminoalkyl)-alkyl-amino]-phenyl-essigsäure-n-nonylester bzw. -isoamylester führt, war keineswegs zu erwarten. Im Gegenteil, auf Grund der Tatsache, daß Halogenatome in ct-Halogen-phenylessigsäureestern außerordentlich leicht beweglich sind, war vielmehr anzunehmen, daß die Reaktionspartner zumindest teilweise unter Bildung quaternärer Verbindungen reagieren würden.That the reaction between the a-halophenylacetic acid esters and the substituted diamines runs exclusively in the direction indicated and to Formation of the a - [(/? - Dialkylaminoalkyl) -alkyl-amino] -phenyl-acetic acid-n-nonyl ester or isoamyl ester was by no means to be expected. On the contrary, due to the Fact that halogen atoms in ct-halo-phenylacetic acid esters are extraordinarily easy to move, it was rather to be assumed that the reactants at least would partially react to form quaternary compounds.

Diese Reaktion konnte auch beobachtet werden, wenn phenylsubstituierte Diamine als Reaktionspartner verwendet werden.This reaction could also be observed when using phenyl-substituted diamines as reactants will.

709 509/433709 509/433

Beispielexample

α-[ (/ϊ-Dimethylamino-äthyl) -methyl-amino] -α- [(/ ϊ-Dimethylamino-ethyl) -methyl-amino] -

phenylessigsäure-n-nonylesterphenylacetic acid n-nonyl ester

Ein Gemisch aus 100 g α-Chlor-phenyl-essigsäuren-nonylester und 60 g Trimethyläthylendiamm wird unter Rühren 4 Stunden am- Rückflußkühler auf 150° erhitzt. Das Reaktionsprodukt wird nach dem Erkalten in Wasser gelöst, mit Salzsäure angesäuert und zur Entfernung von unverändertem a - Chlor -phenyl - essigsäure - η - nonylester mit Äther ausgeschüttelt. Der wäßrige Anteil wird mit Natronlauge alkalisch gemacht, ausgeäthert und der Ätherauszug mit Natriumsulfat getrocknet. Nach Abdestillieren des Äthers wird der Rückstand im Vakuum destilliert.A mixture of 100 g of α-chloro-phenyl-acetic acid nonyl ester and 60 g of trimethylethylenediamine is heated to 150 ° for 4 hours in a reflux condenser with stirring. The reaction product is released after cooling in water, acidified with hydrochloric acid and for the removal of the natural a - chloro phenyl - acetic acid - η - nonyl extracted with ether. The aqueous portion is made alkaline with sodium hydroxide solution, extracted with ether and the ether extract is dried with sodium sulfate. After the ether has been distilled off, the residue is distilled in vacuo.

Kp.0>03 160 bis 165°.Kp. 0> 0 3 160 to 165 °.

In analoger Weise werden a-[(/?-Diäthylamino-isopropyl)-äthyl-amino]-phenyl-essigsäure-n-nonylester, Kp.0j05 178 bis 182°, und a-[(^-Dimethylamino-äthyl)-methylamino]-phenyl-essigsäure-isoamylester, Kp.OiC1 125 bis 130°, hergestellt.Kp -phenyl-acetic acid-n-nonyl, 0j05 178-182 °, and a in a manner analogous to a be - - [ethyl-amino (diethylamino-isopropyl /?)] -. [(^ - dimethylamino-ethyl) methylamino ] phenylacetic acid isoamyl ester, bp. OiC1 125 to 130 °.

-COO —R3 -COO -R 3

R1-N-CH-CH2-NR 1 -N-CH-CH 2 -N

Claims (1)

PATENTANSPRUCH:PATENT CLAIM: Verfahren zur Herstellung von a-[(/?-Dialkylaminoalkyl)-alkyl -amino] -phenyl -essigsäure -isoamyl- und -n-nonylestern der allgemeinen FormelProcess for the preparation of α - [(/? - dialkylaminoalkyl) alkyl -amino] -phenyl-acetic acid -isoamyl- and -n-nonyl esters of the general formula worin R und R1 = Methyl oder Äthyl, R2 = Wasserstoff oder Methyl und R3 = Isoamyl oder n-Nonyl bedeuten, dadurch gekennzeichnet, daß man entweder am N-Atom alkylierte a-Amino-phenyl-essigsäure-isoamyl- oder -n-nonylester mit einem jß-Dialkylamino-alkyl-halogenid in Salzform oder a-Halogenphenyl-essigsäure-isoamylester oder -n-nonylester mit der äquivalenten Menge eines (/9-Dialkylamino-alkyl)-alkyl-amins in Abwesenheit eines Lösungsmittels bei erhöhter Temperatur miteinander umsetzt und gegebenenfalls die dabei gebildeten a-[(/3-Dialkylaminoalkyl) -alkyl-amino] -phenyl-essigsäure-isoamyl- bzw. -n-nonylester mit Mineralsäuren, vorzugsweise Salzsäure, in die entsprechenden wasserlöslichen Salze überführt.where R and R 1 = methyl or ethyl, R 2 = hydrogen or methyl and R 3 = isoamyl or n-nonyl, characterized in that either a-amino-phenylacetic acid-isoamyl- or - n-nonyl ester with a β-dialkylamino-alkyl halide in salt form or α-halophenyl-acetic acid-isoamyl ester or -n-nonyl ester with the equivalent amount of a (/ 9-dialkylamino-alkyl) -alkyl-amine in the absence of a solvent at increased Reacts temperature with each other and optionally the a - [(/ 3-dialkylaminoalkyl) -alkyl-amino] -phenyl-acetic acid-isoamyl- or -n-nonyl ester with mineral acids, preferably hydrochloric acid, converted into the corresponding water-soluble salts. In Betracht gezogene Druckschriften:Considered publications: Berichte der Deutschen Chemischen Gesellschaft, 30, 2305;Reports of the German Chemical Society, 30, 2305; Beilstein, Handbuch der organischen Chemie, 4. Auflage, Hptw. Bd. 14, S. 463, 466, 467, 468; Ergw. I, Bd. 14, S. 592;Beilstein, Handbook of Organic Chemistry, 4th Edition, Hptw. Vol. 14, pp. 463, 466, 467, 468; Ergw. I, Vol. 14, p. 592; deutsche Patentschrift Nr. 842206;German Patent No. 842206; Bulletin de la Soc. Chim. de France Γ4] 9, 985.Bulletin de la Soc. Chim. de France Γ4] 9, 985. © 709 50W433 5.57© 709 50W433 5.57
DEA17418A 1953-02-09 1953-02-09 Process for the preparation of ª[(ª-dialkylamino-alkyl)-alkyl-amino]-phenyl-acetic acid isoamyl and -n-nonyl esters Pending DE1008308B (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
DEA17418A DE1008308B (en) 1953-02-09 1953-02-09 Process for the preparation of ª[(ª-dialkylamino-alkyl)-alkyl-amino]-phenyl-acetic acid isoamyl and -n-nonyl esters

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DEA17418A DE1008308B (en) 1953-02-09 1953-02-09 Process for the preparation of ª[(ª-dialkylamino-alkyl)-alkyl-amino]-phenyl-acetic acid isoamyl and -n-nonyl esters

Publications (1)

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DE1008308B true DE1008308B (en) 1957-05-16

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0058373A1 (en) * 1981-02-12 1982-08-25 Ciba-Geigy Ag Substituted aliphatic secondary amines and their salts, pharmaceutical compositions containing them and their use
US4723031A (en) * 1984-08-27 1988-02-02 Chevron Research Company Processes for synthesizing substituted and unsubstituted aminoacetate esters

Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE842206C (en) * 1950-01-28 1952-06-23 Asta Werke Ag Chem Fab Process for the N-alkylation of ª ‡ -aminophenyl acetic acid esters

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE842206C (en) * 1950-01-28 1952-06-23 Asta Werke Ag Chem Fab Process for the N-alkylation of ª ‡ -aminophenyl acetic acid esters

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0058373A1 (en) * 1981-02-12 1982-08-25 Ciba-Geigy Ag Substituted aliphatic secondary amines and their salts, pharmaceutical compositions containing them and their use
US4723031A (en) * 1984-08-27 1988-02-02 Chevron Research Company Processes for synthesizing substituted and unsubstituted aminoacetate esters

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