PL84224B1 - - Google Patents

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PL84224B1
PL84224B1 PL1971174907A PL17490771A PL84224B1 PL 84224 B1 PL84224 B1 PL 84224B1 PL 1971174907 A PL1971174907 A PL 1971174907A PL 17490771 A PL17490771 A PL 17490771A PL 84224 B1 PL84224 B1 PL 84224B1
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Poland
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carbon atoms
formula
group
hydroxy
alkyl
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PL1971174907A
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Polish (pl)
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D317/00Heterocyclic compounds containing five-membered rings having two oxygen atoms as the only ring hetero atoms
    • C07D317/08Heterocyclic compounds containing five-membered rings having two oxygen atoms as the only ring hetero atoms having the hetero atoms in positions 1 and 3
    • C07D317/44Heterocyclic compounds containing five-membered rings having two oxygen atoms as the only ring hetero atoms having the hetero atoms in positions 1 and 3 ortho- or peri-condensed with carbocyclic rings or ring systems
    • C07D317/46Heterocyclic compounds containing five-membered rings having two oxygen atoms as the only ring hetero atoms having the hetero atoms in positions 1 and 3 ortho- or peri-condensed with carbocyclic rings or ring systems condensed with one six-membered ring
    • C07D317/48Methylenedioxybenzenes or hydrogenated methylenedioxybenzenes, unsubstituted on the hetero ring
    • C07D317/62Methylenedioxybenzenes or hydrogenated methylenedioxybenzenes, unsubstituted on the hetero ring 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 atoms of the carbocyclic ring
    • C07D317/64Oxygen atoms
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00Technologies relating to chemical industry
    • Y02P20/50Improvements relating to the production of bulk chemicals
    • Y02P20/55Design of synthesis routes, e.g. reducing the use of auxiliary or protecting groups

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Acyclic And Carbocyclic Compounds In Medicinal Compositions (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)

Description

Przedmiotem wynalazku jest sposób wytwarza¬ nia nowych l-fenoksy-2-hydroksy-3-hydroksyalki- loaminopropanów w postaci racematów lub op¬ tycznych antypodów, ich estrów i soli addycyj¬ nych z kwasami.Nowym zwiazkom odpowiada wzór ogólny 1, w którym Rj oznacza wodór, chlorowiec, grupe al¬ kilowa lub alkoksylowa o 1—4 atomach wegla, grupe alkenylowa o 2—5 atomach wegla, grupe nitrylowa lub nitrowa, R2 oznacza wodór, chloro¬ wiec lub grupe alkilowa albo alkoksylowa o 1—4 atomach wegla i R3 oznacza prosta lub rozgalezio¬ na grupe hydroksyalkilowa o 3—6 atomach wegla.Wedlug wynalazku nowe zwiazki wytwarza sie przez zmydlenie zwiazku o wzorze ogólnym 2, w którym Ri—R3 maja wyzej podane znaczenie, a R4 oznacza grupe alkilowa.Stosowane jako produkty wyjsciowe zwiazki o wzorze 2 zawieraja juz gotowy szkielet 1-fenoksy- -2-hydroksy-3-hydroksyalkiloaminopropanu i moz¬ na je otrzymac z odpowiedniego fenolu przez re¬ akcje z epichlorohydryna i nastepnie poddanie wytworzonego l-fenoksy-2,3-epoksypropanu reakcji z hydroksyalkiloamina.Otrzymane sposobem wedlug wynalazku zwiazki posiadaja asymetryczny atom wegla w grupie CHOH i moga wskutek tego wystepowac w postaci zarówno racematu, jak i optycznych antypodów.Te ostatnie mozna otrzymac przez rozdzielenie ra¬ cematu za pomoca znanych kwasów pomocniczych, takich jak kwas dwubenzoilo- (wzglednie dwu-p- -toluilo)D-winowy lub kwas D-3-bromokamforo-8- -sulfonowy lub przez stosowanie optycznie czyn¬ nych zwiazków wyjsciowych.Otrzymane sposobem wedlug wynalazku 1-fe- noksy- 2-hydroksy- 3-hydroksyalkiloaminopropany o wzorze ogólnym 1, mozna przeprowadzic w zna¬ ny sposób w ich fizjologicznie dopuszczalne sole addycyjne z kwasami. Odpowiednimi kwasami sa np. kwas solny, bromowodorowy, siarkowy, meta- nosulfonowy, maleinowy, octowy, szczawiowy, mle¬ kowy, winowy lub 8-chloroteofilina. Równiez prze¬ prowadzenie tych zwiazków w ich estry zachodzi w znany sposób np. przez reakcje z halogenkiem lub bezwodnikiem acylu. Uzytecznymi estrami sa np. 2-octany lub 2-propioniany.Zwiazki o wzorze ogólnym 1 lub ich fizjologicz¬ nie dopuszczalne sole addycyjne z kwasami wy¬ kazuja w badaniach na swinkach morskich war¬ tosciowe wlasciwosci terapeutyczne, w szczególnos¬ ci dzialanie /?-adrenolityczne i mozna je wskutek tego stosowac w leczeniu i w profilaktyce scho¬ rzen wiencowych serca i arytmii serca, zwlaszcza w tychocardii, w medycynie. Równiez dzialanie obnizajace cisnienie krwi jest pod wzgledem tera¬ peutycznym interesujace. Zwiazki te w stosunku do znanych blokujacych /^-receptorów, takich jak np. l-(naftyloksy)- 2-hydroksy- 3-izopropyloamino- propan (propranolol), wykazuja znacznie mniejsza toksycznosc. 84 22484 224 3 Szczególnie wartosciowymi ^okazaly sie w szcze¬ gólnosci zwiazki o wzorze 1, w którym R4 oznacza rozgaleziona grupe hydroksyalkilowa, zwlaszcza l,l-dwumetylo-2-hydroksyetylowa.Dawka jednostkowa zwiazków otrzymanych spo¬ sobem wedlug wynalazku wynosi 1—300 mg, zwlaszcza 5—100 mg (doustnie) wzglednie 1—20 mg (pozajelitowo).Nowe substancje czynne mozna przeprowadzic w zwykle stosowane galenowe formy uzytkowe, takie jak tabletki, drazetki, roztwory, emulsje, proszki, kapsulki lub preparaty o przedluzonym dzialaniu, przy czym do wytwarzania ich stosuje sie znane farmaceutyczne srodki pomocnicze oraz znC^ej metody sporza4zania. Tabletki wytwarza sie nil. przez zmieszanie substancji czynnej ze znany¬ mi srodkami pomocniczymi, np. obojetnymi roz- ciaAi^miB iihiufti,*jak weglan lub fosforan wapnia lub^Tcwas ^Sitólwy,: srodkami rozkruszajacymi, jak skrobia kukurydziana lub kwas alginowy, srodkami wiazacymi, jak skrobia lub zelatyna, srodkiem poslizgowym, jak stearynian magnezu lub talk i/lub srodkami do wywolania efektu prze¬ dluzonego dzialania, jak karboksypolimetylen, kar- boksymetyloceluloza, ftalan acetylocelulozy lub po¬ lioctan winylu.Tabletki moga sie równiez skladac z kilku warstw. Drazetki otrzymuje sie przez powlekanie rdzeni, sporzadzonych analogicznie jak tabletki, zwykle stosowanymi do powlok srodkami, np. ko- lidonem lub szelakiem, guma arabska, talkiem, dwutlenkiem tytanu lub cukrem. Dla osiagniecia efektu przedluzonego dzialania lub unikniecia niezgodnosci, rdzenie moga sie skladac z kilku warstw. Podobnie, powloki drazetek moga skladac sie równiez z kilku warstw, przy czym stosuje sie wspomniane przy tabletkach srodki pomocnicze.Syropy z substancja czynna lub z polaczeniem substancji czynnych moga zawierac dodatkowo srodek slodzacy, taki jak sacharyna, cyklaminian, gliceryna lub cukier oraz srodek polepszajacy smak, np. srodek aromatyzujacy, jak wanilina lub ekstrakt pomaranczowy. Ponadto moga zawierac pomocnicze srodki zawieszajace lub zageszczajace, np. sól sodowa karboksymetylocelulozy, srodek zwilzajacy, np. produkt kondensacji alkoholi tlusz¬ czowych i tlenku etylenu lub srodek konserwuja¬ cy, jak p-hydroksybenzoesan.Roztwory iniekcyjne wytwarza sie w znany spo¬ sób, np. z dodatkiem srodka konserwujacego, jak p-hydroksybenzoesan lub stabilizatorów, jak kom- pleksony. Roztwór ten rozlewa sie do fiolek iniek- cyjnych lub ampulek.Kapsulki zawierajace substancje czynna lub po¬ laczenie substancji czynnych wytwarza sie np. przez zmieszanie substancji czynnej z obojet¬ nym nosnikiem, jak cukier mlekowy lub sorbit i ta mieszanina napelnia sie kapsulki zelatynowe i zamyka. 40 45 50 55 Czopki wytwarza sie np. przez zmieszanie sub¬ stancji czynnej lub substancji czynnych ze znany¬ mi nosnikami, takimi jak obojetne tluszcze lub po- liglikol etylenowy lub jego pochodne.Otrzymywane sposobem wedlug wynalazku zwiazki mozna laczyc z innymi farmakodynamicz- nie czynnymi sbustancjami, takimi jak srodki roz¬ szerzajace naczynia wiencowe serca, dzialajace po¬ budzajaco na uklad nerwowy wspólczulny, gliko¬ zydy nasercowe lub srodki uspokajajace.Nastepujace przyklady wyjasniaja blizej wyna¬ lazek, nie ograniczajac jego zakresu.Przyklad I. Chlorowodorek l-(4-hydroksykar- bonylofenoksy)- 2-hydroksy- 3-(l-metylo- 2-hydro- ksyetylo)-aminopropanu. 6 g (0,02 mola) l-(4-eto- ksykarbonylofenoksy)- 2-hydroksy- 3-(l-metylo- 2- -hydroksyetylo)-aminopropanu zadaje sie 80 mL stezonego kwasu solnego i ogrzewa do wrzenia pod chlodnica zwrotna przez 3 godziny. Po odde¬ stylowaniu kwasu solnego pozostalosc zadaje - sie 50 ml wody i alkalizuje 2n NaOH, po czym wy¬ trzasa z octanem etylu. Faze wodna zakwasza sie kwasem solnym i zateza. Pozostalosc zadaje sie 100 ml absolutnego alkoholu i ogrzewa do wrze¬ nia, a nastepnie odsacza nierozpuszczalna substan¬ cje. Po dodaniu eteru krystalizuje z alkoholu chlo¬ rowodorek, który przekrystalizowuje sie 2 razy z mieszaniny alkoholu/eteru. Wydajnosc: 3,7 g, temperatura topnienia: 168—169°C.Przyklad II. Chlorowodorek l-(4-hydroksy- karbonylofenoksy)- 2-hydroksy- 3-(l,l-dwumetylo- -2-hydroksyetylo)-aminopropanu. Chlorowodorek tytulowego zwiazku wytwarza sie analogicznie,, jak w przykladzie I z l-(4-etoksykarbonylofeno- ksy)- 2-hydroksy- 3-(l,l-dwumetylo- 2-hydroksy- etylo)-aminopropanu przez zmydlenie estru. Tem¬ peratura topnienia 168°C. PL PL PL PLThe subject of the invention is a process for the preparation of new 1-phenoxy-2-hydroxy-3-hydroxyalkylaminopropanes in the form of racemates or optical antipodes, their esters and acid addition salts. is hydrogen, halogen, alkyl or alkoxy with 1-4 carbon atoms, alkenyl group with 2-5 carbon atoms, nitrile or nitro group, R2 is hydrogen, halogen or alkyl or alkoxy group with 1-4 carbon atoms and R3 represents a straight or branched hydroxyalkyl group with 3 to 6 carbon atoms. According to the invention, the new compounds are prepared by saponification of a compound of formula II in which R 1 -R 3 have the meaning given above and R 4 is an alkyl group. the starting compounds of formula II already contain the finished 1-phenoxy-2-hydroxy-3-hydroxyalkylaminopropane skeleton and can be obtained from the corresponding phenol by reacting with epichlorohydrin and then subjecting the 1-phenoxy-2,3-epoxypropane formed to it. The compounds obtained by the process according to the invention have an asymmetric carbon atom in the CHOH group and can therefore be present in the form of both racemate and optical antipodes. The latter can be obtained by resolution of the racem with known auxiliary acids such as acid dibenzoyl- (or di-p-toluyl) D-tartaric acid or D-3-bromocamphoro-8-sulfonic acid or by using optically active starting compounds. 1-phenoxy-2-hydroxy- obtained according to the invention The 3-hydroxyalkylaminopropanes of general formula I can be converted into their physiologically acceptable acid addition salts in a known manner. Suitable acids are, for example, hydrochloric, hydrobromic, sulfuric, methanesulfonic, maleic, acetic, oxalic, lactic, tartaric or 8-chlorotheophylline. The conversion of these compounds into their esters also takes place in a known manner, for example by reaction with an acyl halide or anhydride. Useful esters are, for example, 2-acetates or 2-propionates. The compounds of general formula I or their physiologically acceptable acid addition salts have shown valuable therapeutic properties in a guinea pig study, in particular a therapeutic effect. they are adrenolytic and can therefore be used in the treatment and prophylaxis of coronary diseases and cardiac arrhythmias, especially in teocardia, in medicine. The blood pressure lowering effect is also therapeutically interesting. These compounds are much less toxic in relation to known β-blocking receptors, such as, for example, 1- (naphthyloxy) - 2-hydroxy-3-isopropylamino-propane (propranolol). 84 22484 224 3 The compounds of formula I, in which R4 represents a branched hydroxyalkyl group, in particular 1,1-dimethyl-2-hydroxyethyl, have proved to be of particular value. The unit dose of the compounds obtained according to the invention is 1 to 300 mg, especially 5-100 mg (orally) or 1-20 mg (parenterally). New active substances can be converted into the usual galenic formulations, such as tablets, dragees, solutions, emulsions, powders, capsules or preparations with prolonged action, known pharmaceutical auxiliaries and the following preparation methods are used for their preparation. Tablets are made into liquid. by mixing the active ingredient with known adjuvants, for example, neutral dissolving agents such as calcium carbonate or phosphate, or sludge acid, a disintegrating agent such as corn starch or alginic acid, binding agents such as starch or gelatin, lubricants such as magnesium stearate or talc, and / or prolonging agents such as carboxypolymethylene, carboxymethyl cellulose, cellulose acetate phthalate or vinyl polyacetate. Tablets may also consist of several layers. Drazets are obtained by coating cores, prepared analogously to tablets, with the usual coating agents, for example colidone or shellac, gum arabic, talc, titanium dioxide or sugar. In order to achieve a prolonged effect or to avoid incompatibilities, the cores may consist of several layers. Likewise, dragee coatings may also consist of several layers, with the excipients mentioned for the tablets being used. Syrups with active ingredient or a combination of active ingredients may additionally contain a sweetening agent such as saccharin, cyclamate, glycerin or sugar, and a flavor enhancer. , e.g. a flavoring like vanillin or orange extract. In addition, they may contain suspending or thickening aids, for example sodium carboxymethyl cellulose, a wetting agent, for example a condensation product of fatty alcohols and ethylene oxide, or a preservative such as p-hydroxybenzoate. for example with the addition of a preservative such as p-hydroxybenzoate or stabilizers such as complexes. This solution is poured into injection vials or ampoules. Capsules containing the active ingredient or a combination of the active ingredients are prepared, for example, by mixing the active ingredient with an inert carrier such as milk sugar or sorbitol, and the mixture is filled into gelatine capsules and sealed. . 40 45 50 55 Suppositories are prepared, for example, by mixing the active ingredient or ingredients with known carriers, such as inert fats or polyethylene glycol or its derivatives. With substances such as dilating agents for the coronary arteries of the heart, inducing the sympathetic nervous system, cardiac glycosides, or sedatives. The following examples explain the invention closer without limiting its scope. -hydroxycarbonylphenoxy) - 2-hydroxy-3- (1-methyl-2-hydroxyethyl) -aminopropane. 6 g (0.02 mol) of 1- (4-ethoxycarbonylphenoxy) - 2-hydroxy-3- (1-methyl-2-hydroxyethyl) -aminopropane are mixed with 80 ml of concentrated hydrochloric acid and heated to reflux. for 3 hours. After distilling off the hydrochloric acid, the residue is taken up in 50 ml of water and made alkaline with 2N NaOH and then shaken with ethyl acetate. The aqueous phase is acidified with hydrochloric acid and concentrated. The residue is mixed with 100 ml of absolute alcohol and heated to boiling, and then the insoluble matter is filtered off. Upon addition of ether, the hydrochloride crystallizes from the alcohol, which recrystallizes twice from an alcohol / ether mixture. Yield: 3.7 g, mp: 168-169 ° C. Example II. 1- (4-Hydroxy-carbonylphenoxy) -2-hydroxy-3- (1,1-dimethyl--2-hydroxyethyl) -aminopropane hydrochloride. The hydrochloride of the title compound is prepared analogously to example 1 from 1- (4-ethoxycarbonylphenoxy) - 2-hydroxy-3- (1,1-dimethyl-2-hydroxyethyl) aminopropane by saponification of the ester. Melting point 168 ° C. PL PL PL PL

Claims (1)

1. Zastrzezenie patentowe Sposób wytwarzania nowych l-fenoksy-2-hydro- ksy-3-hydroksyalkiloaminopropanów o wzorze ogól¬ nym 1, w którym R± oznacza wodór, chlorowiec, grupe alkilowa lub alkoksylowa o 1—4 atomach wegla, grupe alkenylowa o 2—5 atomach wegla, grupe nitrylowa lub nitrowa, Rg oznacza wodór, chlorowiec lub grupe alkilowa albo alkoksylowa o 1—4 atomach wegla i Rs oznacza prosta lub roz¬ galeziona grupe hydroksyalkilowa o 3—6 atomach wegla w postaci racematów i optycznych antypo¬ dów, znamienny tym, ze zwiazek o wzorze ogól¬ nym 2, w którym Ri—Rg maja wyzej podane zna¬ czenie, a R4 oznacza grupe alkilowa, zmydla sie i otrzymany racemat ewentualnie rozszczepia sie na optyczne antypody i/lub otrzymany zwiazek o wzorze 1, przeprowadza w sól addycyjna z kwa¬ sem lub w ester.84 224 COOH jf3~ 0CH2" CHOH-CH2-NH-R3 R2 Wzór 1 COOR^ /7V0CH2"CH0H^CH2"NHR3 1 R2 Wzór 2 PL PL PL PL1. Claim 1. Process for the preparation of new 1-phenoxy-2-hydroxy-3-hydroxyalkylaminopropanes of the general formula I, in which R ± is hydrogen, halogen, alkyl or alkoxy with 1-4 carbon atoms, alkenyl group 2-5 carbon atoms, nitrile or nitro group, Rg is hydrogen, halogen or alkyl or alkoxy group with 1-4 carbon atoms, and Rs is straight or branched hydroxyalkyl group with 3-6 carbon atoms in the form of racemates and optical antipopes is saponified and the resulting racemate is optionally split into optical antipodes and / or the resulting compound of formula 1, converts to an acid addition salt or ester. 84 224 COOH? F3 ~ OCH2 "CHOH-CH2-NH-R3 R2 Formula 1 COOR ^ / 7V0CH2" CHOH ^ CH2 "NHR3 1 R2 Formula 2 PL PL PL PL
PL1971174907A 1970-10-05 1971-10-04 PL84224B1 (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE19702048838 DE2048838A1 (en) 1970-10-05 1970-10-05 New 1 phenoxy 2 hydroxy 3 hydroxyal kylaminopropane and process for their manufacture

Publications (1)

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PL84224B1 true PL84224B1 (en) 1976-03-31

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PL1971174906A PL84225B1 (en) 1970-10-05 1971-10-04
PL1971174910A PL84396B1 (en) 1970-10-05 1971-10-04
PL1971174905A PL84226B1 (en) 1970-10-05 1971-10-04
PL1971174909A PL84267B1 (en) 1970-10-05 1971-10-04
PL1971150902A PL82037B1 (en) 1970-10-05 1971-10-04
PL1971174907A PL84224B1 (en) 1970-10-05 1971-10-04
PL1971174908A PL84223B1 (en) 1970-10-05 1971-10-04
PL1971174911A PL84227B1 (en) 1970-10-05 1971-10-04
PL1971174903A PL84212B1 (en) 1970-10-05 1971-10-04
PL1971174912A PL84276B1 (en) 1970-10-05 1971-10-04

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PL1971174906A PL84225B1 (en) 1970-10-05 1971-10-04
PL1971174910A PL84396B1 (en) 1970-10-05 1971-10-04
PL1971174905A PL84226B1 (en) 1970-10-05 1971-10-04
PL1971174909A PL84267B1 (en) 1970-10-05 1971-10-04
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PL1971174911A PL84227B1 (en) 1970-10-05 1971-10-04
PL1971174903A PL84212B1 (en) 1970-10-05 1971-10-04
PL1971174912A PL84276B1 (en) 1970-10-05 1971-10-04

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JP (1) JPS5710097B1 (en)
AT (10) AT318564B (en)
AU (1) AU469119B2 (en)
BE (1) BE773472A (en)
BG (8) BG20100A3 (en)
CA (1) CA1008866A (en)
CH (11) CH583685A5 (en)
CS (2) CS172932B2 (en)
DE (1) DE2048838A1 (en)
DK (1) DK130958B (en)
ES (8) ES395671A1 (en)
FI (1) FI55491C (en)
FR (1) FR2110230B1 (en)
GB (1) GB1364280A (en)
HU (1) HU163226B (en)
IE (1) IE35693B1 (en)
IL (1) IL37830A (en)
NL (1) NL174249C (en)
NO (1) NO132835C (en)
PH (1) PH9959A (en)
PL (10) PL84225B1 (en)
RO (8) RO62357A (en)
SE (1) SE383631B (en)
SU (2) SU419024A3 (en)
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US4055658A (en) * 1976-05-17 1977-10-25 Mead Johnson & Company Cyanomethylphenethanolamines
US4454154A (en) * 1981-06-23 1984-06-12 American Hospital Supply Corporation Method for treating glaucoma by the topical administration of selectively metabolized beta-blocking agents
DE3248835A1 (en) * 1981-06-23 1983-06-30 American Hospital Supply Corp COMPOSITIONS FOR TREATING GLAUCOMA
US4652584A (en) * 1984-07-13 1987-03-24 Mcneilab, Inc. Acetylenic phenoxypropanol derivatives and pharmaceutical compositions for the treatment of hypertension
DE4422707A1 (en) * 1994-06-29 1996-01-04 Hoechst Ag Process for dyeing aminated cellulose / polyester blends with fiber-reactive disperse dyes
JP4934287B2 (en) * 2005-04-05 2012-05-16 花王株式会社 Whitening agent

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CA945172A (en) * 1969-02-21 1974-04-09 Imperial Chemical Industries Limited Alkanolamine derivatives

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ES399868A1 (en) 1975-06-16
DK130958B (en) 1975-05-12
SU419024A3 (en) 1974-03-05
AT318569B (en) 1974-10-25
FI55491C (en) 1979-08-10
AT318567B (en) 1974-10-25
JPS5710097B1 (en) 1982-02-24
CH564515A5 (en) 1975-07-31
ES399870A1 (en) 1975-07-16
IE35693L (en) 1972-04-05
ES399872A1 (en) 1975-07-01
RO62313A (en) 1977-08-15
AT318566B (en) 1974-10-25
NO132835C (en) 1976-01-14
FR2110230A1 (en) 1972-06-02
FR2110230B1 (en) 1975-03-14
CH564516A5 (en) 1975-07-31
RO62355A (en) 1977-10-15
BG18857A3 (en) 1975-03-20
ES399869A1 (en) 1975-06-16
PH9959A (en) 1976-06-14
PL84212B1 (en) 1976-03-31
BG18858A3 (en) 1975-03-20
CH563342A5 (en) 1975-06-30
IE35693B1 (en) 1976-04-28
BG19134A3 (en) 1975-04-30
RO62267A (en) 1978-01-15
RO62359A (en) 1977-11-15
AU3418271A (en) 1973-04-12
CH587227A5 (en) 1977-04-29
NL174249C (en) 1984-05-16
SU677649A3 (en) 1979-07-30
BG19133A3 (en) 1975-04-30
PL82037B1 (en) 1975-10-31
RO61540A (en) 1977-02-15
DK130958C (en) 1975-10-13
AT318571B (en) 1974-10-25
PL84276B1 (en) 1976-03-31
BE773472A (en) 1972-04-04
ES395671A1 (en) 1974-10-16
PL84225B1 (en) 1976-03-31
PL84267B1 (en) 1976-03-31
ES399873A1 (en) 1975-07-01
BG20100A3 (en) 1975-10-30
FI55491B (en) 1979-04-30
IL37830A (en) 1975-03-13
CH584185A5 (en) 1977-01-31
HU163226B (en) 1973-07-28
AT318572B (en) 1974-10-25
BG20338A3 (en) 1975-11-05
SE383631B (en) 1976-03-22
RO62357A (en) 1977-10-15
AT318565B (en) 1974-10-25
CH564507A5 (en) 1975-07-31
DE2048838A1 (en) 1972-04-06
YU23679A (en) 1980-10-31
IL37830A0 (en) 1971-12-29
YU35577B (en) 1981-04-30
YU250571A (en) 1980-10-31
BG18859A3 (en) 1975-03-20
CH583685A5 (en) 1977-01-14
AT318561B (en) 1974-10-25
PL84227B1 (en) 1976-03-31
GB1364280A (en) 1974-08-21
AT318568B (en) 1974-10-25
CA1008866A (en) 1977-04-19
YU35576B (en) 1981-04-30
ES399871A1 (en) 1975-06-16
CH583686A5 (en) 1977-01-14
RO62358A (en) 1978-04-15
CH563341A5 (en) 1975-06-30
NL174249B (en) 1983-12-16
PL84226B1 (en) 1976-03-31
CS172950B2 (en) 1977-01-28
PL84223B1 (en) 1976-03-31
AU469119B2 (en) 1976-02-05
CS172932B2 (en) 1977-01-28
AT318570B (en) 1974-10-25
CH583687A5 (en) 1977-01-14
NL7113581A (en) 1972-04-07
NO132835B (en) 1975-10-06
ES399874A1 (en) 1975-07-01
RO62356A (en) 1977-08-15
PL84396B1 (en) 1976-03-31
AT318564B (en) 1974-10-25
BG19793A3 (en) 1975-10-10
CH587223A5 (en) 1977-04-29
ZA716643B (en) 1973-06-27

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