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DE1001991B - Process for the preparation of new derivatives of theophylline - Google Patents

Process for the preparation of new derivatives of theophylline

Info

Publication number
DE1001991B
DE1001991B DESCH17824A DESC017824A DE1001991B DE 1001991 B DE1001991 B DE 1001991B DE SCH17824 A DESCH17824 A DE SCH17824A DE SC017824 A DESC017824 A DE SC017824A DE 1001991 B DE1001991 B DE 1001991B
Authority
DE
Germany
Prior art keywords
theophyllinyl
preparation
theophylline
new derivatives
acetone
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
DESCH17824A
Other languages
German (de)
Inventor
Dr Hans Priewe
Dr Alexander Poljak
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.)
Bayer Pharma AG
Original Assignee
Schering AG
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 Schering AG filed Critical Schering AG
Priority to DESCH17824A priority Critical patent/DE1001991B/en
Publication of DE1001991B publication Critical patent/DE1001991B/en
Pending legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D473/00Heterocyclic compounds containing purine ring systems
    • C07D473/02Heterocyclic compounds containing purine ring systems with oxygen, sulphur, or nitrogen atoms directly attached in positions 2 and 6
    • C07D473/04Heterocyclic compounds containing purine ring systems with oxygen, sulphur, or nitrogen atoms directly attached in positions 2 and 6 two oxygen atoms
    • C07D473/06Heterocyclic compounds containing purine ring systems with oxygen, sulphur, or nitrogen atoms directly attached in positions 2 and 6 two oxygen atoms with radicals containing only hydrogen and carbon atoms, attached in position 1 or 3
    • C07D473/08Heterocyclic compounds containing purine ring systems with oxygen, sulphur, or nitrogen atoms directly attached in positions 2 and 6 two oxygen atoms with radicals containing only hydrogen and carbon atoms, attached in position 1 or 3 with methyl radicals in positions 1 and 3, e.g. theophylline

Landscapes

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

Description

Verfahren zur Herstellung neuer Derivate des Theophyllins Die [Theophyllinyl-(7)]-acetone, insbesondere der Stammkörper dieser Reihe, besitzen wertvolle pharmakologische Eigenschaften. Ihre pharmazeutische Verwertbarkeit ist jedoch durch die geringe Wasserlöslichkeit erschwert. So ist z. B. schon das einfache unsubstituierte [Theophyllinyl-(7)]-aceton nur zu etwa 21/, °/o in Wasser löslich.Process for the preparation of new derivatives of theophylline Die [Theophyllinyl- (7)] - acetones, in particular the main body of this series have valuable pharmacological properties. However, their pharmaceutical usability is due to their low water solubility difficult. So is z. B. even the simple unsubstituted [Theophyllinyl- (7)] - acetone soluble in water to the extent of only about 21%.

Es wurde nun gefunden, daß man zu neuen Theophyllinderivaten gelangt, die dem Theophyllin entsprechende wertvolle pharmazeutische Eigenschaften, aber in Verbindung mit einer wesentlich erhöhten Wasserlöslichkeit, aufweisen, wenn man die obengenannten [Theophyllinyl-(7)]-acetone in ihre entsprechenden Diacetonalkohole überführt.It has now been found that new theophylline derivatives are obtained, the valuable pharmaceutical properties corresponding to theophylline, but in connection with a significantly increased water solubility, if one the above [theophyllinyl- (7)] acetones into their corresponding diacetone alcohols convicted.

Letzteren ist aus Analogiegründen die Formel zuzuschreiben, in der R, R' und R" ein Wasserstoffatom oder einen Kohlenwasserstoffrest bedeuten.The latter is the formula for reasons of analogy in which R, R 'and R "represent a hydrogen atom or a hydrocarbon radical.

Zu dieser Überführung kann man sich der zur Ketolbildung aus Ketonen und insbesondere der zur Herstellung von Diacetonalkohol aus Aceton gebräuchlichen Arbeitsweisen bedienen (vgl. G. M. Schwab, Handbuch der Katalyse, Bd. VI, Die Katalyse in der organischen Chemie, 2. Hälfte, S. 372 bis 374, Wien, Springerverlag, 1943).For this conversion one can refer to the one for ketol formation from ketones and especially those commonly used to make diacetone alcohol from acetone Use working methods (cf. G. M. Schwab, Handbuch der Katalyse, Vol. VI, Die Katalyse in organic chemistry, 2nd half, pp. 372 to 374, Vienna, Springerverlag, 1943).

Beispiel 20 g [Theophyllinyl-(7)]-aceton werden in 100 ccm 1 n-Natronlauge über Nacht bei Zimmertemperatur geschüttelt. Man erhält so eine bräunliche Lösung, die mit Salzsäure auf einen pH-Wert von 7 neutralisiert und im Vakuum bei einer Badtemperatur von höchstens 50' zur Trockne eingedampft wird. Der trockne Rückstand wird zweimal mit je 250 ccm trocknem Tetrahydrofuran ausgekocht, vom ungelösten Natriumchlorid abgesaugt und das Filtrat auf ca. 50 ccm eingeengt. Über Nacht kristallisierte 6 g reines 1, S-Bis-[theophyllinyl-(7')]-2-methyl-2-oxy-pentanon-(4) vom F. 131 bis 132' (geringe Zersetzung) aus. Aus der Mutterlauge konnten weitere 12 g etwas unreineres Produkt mit Petroläther gefällt werden. Die Löslichkeit in Wasser übersteigt 600/,. Example 20 g of [theophyllinyl (7)] acetone are shaken in 100 cc of 1N sodium hydroxide solution overnight at room temperature. This gives a brownish solution which is neutralized with hydrochloric acid to a pH of 7 and evaporated to dryness in vacuo at a bath temperature of at most 50 '. The dry residue is boiled twice with 250 ccm of dry tetrahydrofuran each time, undissolved sodium chloride is filtered off with suction and the filtrate is concentrated to about 50 ccm. 6 g of pure 1, S-bis- [theophyllinyl- (7 ')] - 2-methyl-2-oxy-pentanone- (4) with a melting point of 131 to 132' (slight decomposition) crystallized out overnight. A further 12 g of somewhat impure product could be precipitated with petroleum ether from the mother liquor. The solubility in water exceeds 600 / ,.

Molekulargewicht Das Molekulargewicht wurde nach der kryoskopischen Methode in Wasser bestimmt. 0,9522 g Substanz in 15 ccm Wasser ergaben eine Gefrierpunktserniedrigung von 0,25°. Hieraus errechnet sich ein Molekulargewicht von 472,3 (± 5 °/o).Molecular Weight The molecular weight was determined according to the cryoscopic Method determined in water. 0.9522 g of substance in 15 ccm of water resulted in a lowering of the freezing point of 0.25 °. A molecular weight of 472.3 (± 5%) is calculated from this.

Mischschmelzpunkt mit 7-Acetonyltheophyllin 7-Acetonyltheophyllin F. 163 bis 164°. 1, 5-Bis-[theophyllinyl-(7')]-2-methyl-2-oxy-pentanon-(4) F.131 bis 132° (Zers.). Mischschmelzpunkt 120 bis 128°, nach vorausgehendem Sintern bei 110°.Mixed melting point with 7-acetonyltheophylline 7-acetonyltheophylline F. 163 to 164 °. 1,5-Bis- [theophyllinyl- (7 ')] - 2-methyl-2-oxy-pentanone- (4) F.131 up to 132 ° (decomp.). Mixed melting point 120 to 128 °, after previous sintering at 110 °.

Analyse des Oximderivates, F. 204 bis 205°: berechnet für C2oH"OBN9: C 49,3°/-,; H 5,10/0; N 25,90/0, gefunden C 49,10/,; H 5,10/,; N 25,4°/o.Analysis of the oxime derivative, m.p. 204-205 °: calculated for C2oH "OBN9: C 49.3 ° / -; H 5.10 / 0; N 25.90 / 0, found C 49.1% ; H 5.10%; N 25.4%.

Das zum Vergleich herangezogene, dem 1, 5-Bis-[theophyllinyl-(7')]-2-methyl-2-oxy-pentanon-(4) der Zusammensetzung nach am nächsten kommende bekannte 1, 3-Bis-[theophyllinyl-(7')]-propanon-(2) (vgl. Comptes rendus hebdomadaises des seances de 1'academie des sciences, Bd. 236 [1953], S. 2520) weist nur eine geringe Wasserlöslichkeit auf (vgl. »Contribution ä 1'etude de la chimie des purines. Nouveaux derives de synthäse de la theophylline<<, Dissertation von Raymond Z e 1 n i k, Universität Paris, 1955, S. 76 und 77).The used for comparison, the 1, 5-bis [theophyllinyl- (7 ')] - 2-methyl-2-oxy-pentanone- (4) the composition of the closest known 1, 3-bis- [theophyllinyl- (7 ')] -propanone- (2) (cf. Comptes rendus hebdomadaises des seances de 1'academie des sciences, vol. 236 [1953], p. 2520) has only a low solubility in water (cf. »Contribution ä 1'etude de la chimie des purines. Nouveaux derives de synthäse de la theophylline <<, Dissertation by Raymond Z e 1 n i k, University of Paris, 1955, pp. 76 and 77).

Claims (2)

PATENTANSPRÜCHE: 1. Verfahren zur Herstellung neuer Derivate des Theophyllins, dadurch gekennzeichnet, daß man [Theophyllinyl-(7)]-acetone der allgemeinen Formel in der R, R' und R" ein Wasserstoffatom oder einen Kohlenwasserstoffrest bedeuten, nach den zur Ketolbildung aus Ketonen, insbesondere zur Herstellung von Diacetonalkohol aus Aceton bekannten Arbeitsweisen in die entsprechenden 1, 5-Bis-[theophyllinyl-(7')]-2-oxy-pentanone-(4) überführt. PATENT CLAIMS: 1. Process for the preparation of new derivatives of theophylline, characterized in that one [theophyllinyl- (7)] - acetones of the general formula in which R, R 'and R "denote a hydrogen atom or a hydrocarbon radical, according to the procedures known for ketol formation from ketones, in particular for the preparation of diacetone alcohol from acetone, in the corresponding 1, 5-bis [theophyllinyl- (7')] - 2-oxy-pentanone- (4) transferred. 2. Verfahren nach Anspruch 1, dadurch gekennzeichnet, daB man als Ausgangsstoff [Theophyllinyl-(7)]-aceton verwendet. In Betracht gezogene Druckschriften: K a rr e r, Lehrbuch der organischenChemie,1954, S. 179; Comptes rendus hebdomadaises des seances de 1'acad6mie des sciences, Bd.236 [1953], S. 2520.2. The method according to claim 1, characterized in that the starting material is used [Theophyllinyl- (7)] acetone was used. Publications considered: K a rr e r, Textbook of Organic Chemistry, 1954, p. 179; Comptes rendus hebdomadaises des seances de 1'acad6mie des sciences, Vol. 236 [1953], p. 2520.
DESCH17824A 1955-04-25 1955-04-25 Process for the preparation of new derivatives of theophylline Pending DE1001991B (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
DESCH17824A DE1001991B (en) 1955-04-25 1955-04-25 Process for the preparation of new derivatives of theophylline

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DESCH17824A DE1001991B (en) 1955-04-25 1955-04-25 Process for the preparation of new derivatives of theophylline

Publications (1)

Publication Number Publication Date
DE1001991B true DE1001991B (en) 1957-02-07

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Family Applications (1)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1238035B (en) * 1959-05-05 1967-04-06 Chemiewerk Homburg Process for the preparation of a new theophylline compound

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
None *

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1238035B (en) * 1959-05-05 1967-04-06 Chemiewerk Homburg Process for the preparation of a new theophylline compound

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