PL97275B1 - METHOD OF MAKING NEW DERIVATIVES OF THENOTRIIAZOLODUAZEPINE - Google Patents

METHOD OF MAKING NEW DERIVATIVES OF THENOTRIIAZOLODUAZEPINE Download PDF

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PL97275B1
PL97275B1 PL1974191789A PL19178974A PL97275B1 PL 97275 B1 PL97275 B1 PL 97275B1 PL 1974191789 A PL1974191789 A PL 1974191789A PL 19178974 A PL19178974 A PL 19178974A PL 97275 B1 PL97275 B1 PL 97275B1
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    • C07D333/04Heterocyclic compounds containing five-membered rings having one sulfur atom as the only ring hetero atom not condensed with other rings not substituted on the ring sulphur atom
    • C07D333/26Heterocyclic compounds containing five-membered rings having one sulfur atom as the only ring hetero atom not condensed with other rings not substituted on the ring sulphur atom 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 ring carbon atoms
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    • C07D495/12Heterocyclic compounds containing in the condensed system at least one hetero ring having sulfur atoms as the only ring hetero atoms in which the condensed system contains three hetero rings
    • C07D495/14Ortho-condensed systems

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Description

Przedmiotem wynalazku jest sposób wytwarzania nowych pochodnych tienotriazolodwuazepiny o ogólnym wzorze 1, w którym Ri oznacza atom chlorowca, R2 oznacza rodnik fenylowy, grupe o-trójfluorometylofenylo- wa, o-chlorowcofenylowa, o,o'-dwuchlorowcofenylowa, o-nitrofenylowa lub pirydylowa, R3 oznacza atom wodoru, rodnik alkilowy, grupe hydroksyalkilowa, al koksykarbonyIowa, chlorowcoalkilowa, alkoksyalkilowa, alkiiotioalkilowa, alkoksykarbonyloalkilowa lub grupe -alkil-Z, w której Z oznacza grupe o wzorze 3, zas R4 i R5 niezaleznie od siebie oznaczaja atom wodoru lub rodnik alkilowy, lub tez wspólnie razem z atomem azotu oznaczaja jednopierscieniowy, nasycony, 5-6-czlonowy pierscien heterocykliczny o najwyzej jednym dalszym atomie azotu lub tlenu, ewentualnie w postaci ich soli addycyjnych z kwasami.Stosowane w tym opisie wyrazenie „rodnik alkilowy", samo lub w polaczeniu jak w grupie hydroksyalkilo- wej, oznacza prostolancuchowy lub rozgaleziony rodnik weglowodorowy o 1-4 atomach wegla, jak np. rodnik metylowy, etylowy, propylowy, izopropylowy, trzeciorzedowy butylowy lub tym podobny.Wyrazenie „atom chlorowca" oznacza atom jednego z czterech pierwiastków bromu, chloru, fluoru lub jodu. Wyrazeme„grupa alkoksylowa" oznacza rodnik alkilowy z podstawionym tlenem funkcyjnym, jak np. grupa metoksylowa, etoksylowa, propoksylowa lub tym podobna.W wyróznionej klasie zwiazków o wzorze 1, Rt oznacza atom chlorowca, przy czym szczególnie korzystny jest atom chloru, R2 oznacza korzystnie grupe -o-chlorowcofenylowa, o,o-dwuchlorowcofenylowa lub 2-pirydylowa. Dla R2 w znaczeniu grupy o-chlorowcofenylowej, jako atomy chlorowca korzystne sa atomy fluoru lub chloru.W przypadku, gdy R2 wystepuje w znaczeniu grupy 0,0-dwuchlorowcofenylowej, chodzi tu korzystnie o dwa takie same atomy chlorowca, szczególnie zas o dwa atomy fluoru. Korzystne znaczenie R3 to rodnik alkilowy, grupa hydroksyalkilowa i aminoalkilowa.Jak wynika z powyzszego w zwiazkach o wzorze 1, Ri oznacza szczególnie korzystnie atom chloru, R2 grupe o-chlorofenylowa lub o-fluorofenylowa, a R3 grupe aminoalkilowa.Szczególnie korzystnym zwiazkiem jest 2-chloro-4-(o-chlorofenylo)-9-aminoetylo-6H- tieno[3,2-f]*s- tria- zolo[4,3-a]-f1,4]dwuazepinau Dalszymi reprezentatywnymi przedstawicielami zwiazków o wzorze 1 sa:2 97 275 tlenek 2-chforo-4-(o-chlorof8nylo)"9-metylo-6H- tieno[3,2-f]-s-triazolo[4,3-a][1,4] dwuazepiny, Ester etylowy kwasu 2-chlaro-4-{o-chlorofenyio)-9-me£ylo-6H- tieno[3,2-f]-s-triazolo [4,3-a] [1,4]-dwuare- pino-6-karboksylowego, 2~ch!oro-9-metylo-4-(2pirydylo)-6H-tieno[3,2-f]-s-triazolo [4,3-a][1,4]dwuazepina, 2-chloro-9-metylo4-{o-nitrofeny1o)-6H-tseno[3,2-f]-s-triazolo[4/3-a][1/4]dwuazepina, 2-chloro-9-metylo4-f8nylo^H- tieno[3,2-f]-$-triazolo [4,3-a][M]dwuazepina, 2^hloro4-(o'fluorofenylo)-9-mety!o-6H-tieno[3,2-f]-s-triazolo[4,3-a][1,4]dwuazepina, 2-chloro-4-(o,o'-dwufiuoro)-9-metylo-6H- tleno[3,2-f]-s- triazoio[4,3-a][1,4] dwuazepina, 9-lil.rzed-butyio-2-chJoro4-(o-chlorofenylo)-6H-tieno[3,2-fjs-tnazolo [4,3-a][1,4j dwuazepina, 2-chloro-4-(o-chlorofeny!o)-9-metylotiometylo-6H-tieno [3,2-f]-s-triazolo[4,3-aj[1,4] dwuazepina, 2-cbioro*4-(o-chlorofeny!o)-9- morfolinometylo-6H-tieno[3,2-f]-s-triazolo [4,3-a][1 A] dwuazepina, 2"Chloro4-(o-chlorofenylo} 9*metoksymetylo-6H- tieno(3,2-f]-s-triazolo[4,3-a][1 A] dwuazepina, 2-chloro-4-(o-chlorofenylo)«9-hydroksymetylo-6H- tieno[3,2-fj-s-triazoio [4,3-a][1,4] dwuazepina, 2-chloro-4-tochiordfenylo)-9-dwumetyloaminometylo-6H- tieno[3,2-f]*-triazolo [4,3-a][1,4] dwuazepina, 2-chloro-9-chlorom8tylO"4-(o-chlorofenylo)-6H-tieno[3,2'f]-s-triazolo [4,3-a][1,4j dwuazepina, Octan [2*chloro-4-(o-chlorofenylo)-6H- tieno[3,2-f]-s-triazolo [4,3-f][1,4] dwuazepin-0-ylo]-metylowy, 2-€hloro-4*(o-chlorofenyio)-9-(1-hydroksyetylo)-6H-tieno[3,2-f]-f-triazolo [4,3-a][1,4j dwuazepina, 2-chloro-4-(o-chlorofenylo)-9-jodometyio-6H-tieno[3,2-f]-$-triazolo [4,3-a][M] dwuazepina, 2-chloro-9^etoksymetvlQ4-(nitrofenylo)*6H-tie^ Ester etylowy kwasu [2-chloro-4-(o-nitrofenylo)-6H-tieno [3,2-f]-s-triazolo [4,3-a][1,4] dwuasepin 9-yloj -karboksyiowego, 2~chlQro-9 2-chloro-9'metylo4-(o-trójfiuoromety!ofenylo)-6H-tieno [3,2-f]-s-triazoJo{4,3-a][1,4]- dwuazepina.Pochodne tienotriazolodwuazepiny o wzorze 1 i ich sole addycyjne z kwasami mozna wedlug wynalazku wytworzyc w ten sposób, ze cyklizuje sie zwiazek o wzorze ogólnym 2 w którym Rj, R2 i R3 maja wyzej podane znaczenie, Wedlug wynalazku cyklizacje prowadzi sie przez ogrzewanie zwiazków o wzorze 2 w srodowisku organicznym, przy czym jednak dla uzyskania zadowalajacych wydajnosci, w niektórych przypadkach pracuje sie korzystnie w obecnosci kwasu. Tak np. cyklizacje mozna przeprowadzic w ten sposób, ze zwiazek o wzorze 2 ogrzewa sie wciagu kilku godzin do temperatury wrzenia pod chlodnica zwrotna w roztworze alifatycznego kwasu karboksylowego, np. mrówkowego lub octowego, walkanolu, np, etanolu lub n-propanolu, lub wciagu stosunkowo krótkiego czasu, np. okolo 5 minut do 1/2 godziny, w alifatycznym kwasie karboksylowym, np, octowym, izomaslowym lub piwalinowym.Zwiazki o wzorze 2 nie musza i nie we wszystkich przypadkach moga byc stosowane w wyodrebnionej postaci, gdyz czesto w zastosowanych do ich wytwarzania warunkach ulegaja samorzutnej cyklizacji.Otrzymywanie zwiazków wyjsciowych o wzorze 2 przedstawiono na zalaczonym schemacie reakcji, ilustrujacym przypadek, gdy we wzorze 2 Ri oznacza atom wodoru, Ra oznacza rodnik fenylowy, zas R3 ma wyzej podane znaczenie. 2-amino-3-benzoi!otiofen o wzorze 4 przeprowadza sie przez traktowanie ortoestrem o wzorze R4 —C(0*alkil)3 w zwiazek o wzorze 5. Reakcje prowadzi sie celowo w obecnosci obojetnego rozpuszczalnika organicznego, jak benzen, toluen i tym podobne, i kwasnego katalizatora, jak kwas chlorowodorowy, siarkowy, octowy, propionowy, benzenosulfonowy, p-toluenosulfonowy i tym podobne. Temperatura nie jest Istotna, zwykle jednak pracuje sie w temperaturze okolo 50°C do I60°C, jednakze mozna równiez pracowac w temperaturach wyzszych i nizszych. Jako rozpuszczalniki nadaja sie weglowodory, jak benzen lub toluen i tym podobne, lub stosowany jako skladnik reakcji ortoester w nadmiarze. Tak otrzymany zwiazek o wzorze 5 poddaje sie w obojetnym rozpuszczalniku organicznym reakcji z hydrazyna, która korzystnie stosowac jest w postaci wodzianu.Jako rozpuszczalniki nadaja sie szczególnie aikanole jak metanol, etanol, 1-propanoi, 2-propanol i tym podobne. Reakcje prowadzi sie w temperaturze od okolo 0°C do temperatury wrzenia mieszaniny reakcyjnej pod chlodnica zwrotna, korzystnie od okolo 10°C do 30°C Reakcje mozna przyspieszyc przez dodanie katalizatora kwasnego, jak kwas chlorowodorowy/ bromawodorowy, siarkowy, fosforowy, octowy, propionowy, benzenosulfonowy, p-toluenosulfonowy i tym podobne. Tak otrzymany surowy produkt poddaje sie nastepnie reakcji z chlorobezwodnikiem alfa-chlorowcokwasu, jak chlorek chloroacetylu, bromek bromoacetylu i tym podobne, w obojetnym rozpuszczalniku organicznym, chlodzac lodem lub utrzymujac mieszanine reakcyjna ponizej temperatury wrzenia, z utworzeniem zwiazku o wzorze 6.97 275 3 Jako rozpuszczalniki nadaja sie chloroform, chlorek metylenu, eter^ pirydyna, kwas octowy, kwas jednochlorooctowy lub mieszaniny tego ^^ z woda. W przypadku stosowania rozpuszczalnika obojetnego reakcje prowadzi sie korzystnie w obecnosci akceptora kwasu, jak dwuweglan sodowy, weglan sodowy, dwuweglan potasowy, pirydyna/trójetyloamina, imidazol, 2-metyloimida- zol i tym podobne.Zwiazek o wzorze 6 zadaje sie nastepnie amoniakiem lub szesciometylenoczteroamina przy czym otrzymany zwiazek o wzorze 2 mozna bez wyodrebnienia zcyklizowac na odpowiedni zwiazek o wzorze 1.Zwózek o wzorze 3 nie wymaga wyodrebnienia przed cyklizacja, to znaczy ze zamkniecia pierscienia z utworzeniem zwiazku o wzorze 1 mozna dokonac w mieszaninie reakcyjnej, w której wytworzono zwiazek o wzorze 2, nie wyodrebniajac go, lub tez nie przerywajac toku reakcji. Mozna np. zwiazek o wzorze 6 dodac do alkoholowego, np. etanolowego lub metanolowego roztworu amoniaku lub tez zwiazek o wzorze 6 rozpuscic w obojetnym rozpuszczalniku organicznym i zadac cieklym amoniakiem lub szesciometylenoczteroamina, przy czym otrzymuje sie zwiazek o wzorze 2. Do reakcji tej nadaja sie jako rozpuszczalniki: chlorek metylenu, czterochlorek wegla, etery, jak tetrahydrofuran lub dioksan, dwumetylosulfotlenek, dwumetyloformamid, alkanole, jak metanol, etanole-propanol, 2~propanol, 1-butanol, 2-butanol i tym podobne. Otrzymany zwiazek o wzorze 2 czy to wstanie surowym, czy oczyszczonym mozna zcyklizowac w wyzej podany sposób z utworzeniem zwiazku o wzorze 1, W przypadku, gdy chce sie otrzymac zwiazki o wzorze 2, w którym Hx oznacza grupy inne niz atomy wodoru, a R2 oznacza grupe inna niz fenylowa, mozna zaleznie od rodzaju zadanego podstawnika wyjsc z odpowiednio podstawionych zwiazków o wzorze 4 lub wprowadzic ogólnie znanymi sposobami podstawniki lub przeksztalcic w inne podstawniki.Zwiazki o wzorach 5 i 6 sa to zwiazki nowe. Zwiazki o wzorze 1 i ich dajace sie farmaceutycznie stosowac sole addycyjne z kwasami sa wartosciowymi srodkami leczniczymi i moga byc stosowane jako srodki przeciwskurczowe, usmierzajace rozluzniajace miesnie, uspokajajace i przedwiekowe. Tak np. zwiazek 2-chlo- ro-4-fo-chlorofenylo-9-metylo- 6H*tieno[3,2-f]-s-triazolo[4l3-a][1,4]-dwuazepina w próbie antypentatetrazolowej ju myszy wykazuje wartosc wskaznika APR2#0 0,03-0,1 mg/kg doustnie. Wyzej podana próbe przeprowadza sie wedlug metody Orlaffa (Pros. Soc. Exp. Biol. Med. 70, 254-257,1949).Z niemieckiego opisu wylozeniowego nr 2221623 znane sa tienodwuazepiny o podobnym dzialaniu, ale test antypentatetrazolowy wykazal nieoczekiwana wyzszosc zwiazków otrzymywanych sposobem wedlug wynalazku.Nowe zwiazki o wzorze 1 wykazuja duzo lepsze wlasciwosci farmakologiczne w porównaniu ze znanymi zwiazkami o zblizonej budowie.W tablicy podaje sie dane porównawcze uzyskane w tescie metrazolowym, przy czym wyniki wskazuja na to, ze nowe zwiazki znacznie przewyzszaja zwiazki znane pod wzgledem dzialania farmakologicznego.Tablica Zwiazki o wzorze 1, w którym n = O, R3 = H, a znaczenia Ri, Ra i R4 podane sa w tablicy Ri Cl Cl Cl Cl Cl Cl Cl Cl Cl Cl a Cl Cl Cl Cl y z\a R2 o-nitrofenyl o,o'-dwufluoro- fenyl fenyl o-fluorofenyl o-nitrofenyl o-nitroferyl o-nitrofenyl o-chlorofenyl o-chlorofenyl o-nitrofenyl o-nitrofenyl o-chlorofenyl o-chlorofenyl o-chlorofenyl o-chlorofenyl nazek 0 wzorze 7 R4 -CH3 -CH3 -CHa -CHa -CHa-N(CH3)a -CO-O-CHa -CH3 -CHa-0-CH3 -CHa-OH -CHa -CH2-OH -CHa-N(CHi)a -CHa-N(CHi)a -CHa-NH-CH| -CHa-N(CaH|)a -CHa-NHa test metrazolowy (APR 2,0) 2,2 0,23 1,68 0,131 2,12 0,53 0,196 0,78 v 0,49 1,43 1,33 0,494 0,189 0,58 0,173 52,34 97 275 Zwiazki o wzorze 1, jak tez ich dajace sie farmaceutycznie stosowac sole addycyjne z kwasami mozna przerabiac na preparaty farmaceutyczne ogólnie znanymi metodami, np. na tabletki, drazetki, czopki, kapsulki, roztwory, zawiesiny, emulsje i tym podoba Obok powszechnie stosowanych farmakologicznie obojetnych nosników, jak np. cukier mlekowy, skrobia, talk, stearynian magnezu, woda, oleje roslinne, polietylenoglikole i tym podobne, preparaty te moga równiez zawierac srodki konserwujace, stabilizujace, zwilzajace iufo emulgujace, sole dla zmiany cisnienia osmotycznego, bufory lub jeszcze inne terapeutycznie wartosciowe substancje. l W razie koniecznosci mozna wspomniane preparaty sterylizowac lub tez^poddawac innym przyjetym w przemysle farmaceutycznym operacjom. Odpowiednia farmaceutyczna dawka jednostkowa moze zawierac od okolo 1 do 50 mg zwiazku wedlug wynalazku.Odpowiednie dawki dzienne do podawania doustnego dla ssaków mieszcza sie w granicach od okolo QJ mg do okolo 30 mg/kg; dla stosowania pozajelitowego dla ssaków odpowiednia dawka dzienna wynosi od okolc 0,1 mg/kg do okolo 10 mg/kg. Dawki te nalezy traktowac jedynie jako przykladowe; specyficzne dozowanie nalezy w kazdym przypadku dostosowywac do potrzeb indywidualnych.Przyklad. 500 mg nieoczyszczonegc dwuchlorowodorku 2-[(3,5 ylo]-5-ch1oro-3-tieny!o-o sodowego. Faze wodna ekstrahuje sie chlorkiem metylenu,, Po osuszeniu nad siarczanem sodu i odparowaniu fazy organicznej, pozostalosc ogrzewa sie do wrzenia pod chlodnica zwrotna w 5 mi absolutnego alkoholu w ciagu 30 min. Po odparowaniu surowa zasade chromatografuje sie na tlenku glinowym. Bluowana chloroformem i wykrystalizowana z octanu etylu 9(aminometylo)-2-chloro4-(o-chlorofenylo)-6H tienof3,2-fj Mriazolo [4,3-a]{1,4]-dvvuazepina ma temperature topnienia 167—168°C. Przekrystalzowana z octanu etylu i eteru naftowego próbka topi sie w temperaturze 170,5—171 °C. 2 Wzór 2 -n: \, Wzór 397 275 LX O -Alkii ó Wzor A Wzór 5 FL-C N ,S^M—C nr C=0 NH? FL-C N LX CH? Wzor 2 Wzór 6 Sch em a t 1 OL-C=Nx 3 I N DC ^C= NT WZOR 7 Prac. Poligraf. UP PRL naklaci 1/0+ !8 Cena 45 zl PLThe subject of the invention is a process for the preparation of new thienotriazole diazepine derivatives of the general formula I, in which Ri is a halogen atom, R2 is a phenyl radical, o-trifluoromethylphenyl, o-halophenyl, o, o'-dihalophenyl, o-nitrophenyl or pyridyl, R3 represents a hydrogen atom, an alkyl radical, a hydroxyalkyl group, an alkoxycarbonyl group, a haloalkyl group, an alkoxyalkyl group, an alkylthioalkyl group, an alkoxycarbonylalkyl group, or an e-alkyl-Z group, in which Z represents a group of formula 3, and R4 and R5 independently represent a hydrogen atom or an alkyl radical, or also taken together with the nitrogen atom to denote a monocircle saturated 5-6 membered heterocyclic ring of at most one further nitrogen or oxygen atoms, optionally in the form of their acid addition salts. The term "alkyl radical" as used in this specification, alone or in in combination as in a hydroxyalkyl group, means a straight-chained or branched hydrocarbon radical with 1-4 carbon atoms, such as, for example, methyl, ethyl, propyl, isopropyl, tertiary butyl or the like. The expression "halogen" denotes an atom of one of the four elements bromine, chlorine, fluorine or iodine. The expression "alkoxy" denotes an oxygen-functional alkyl radical, such as, for example, methoxy, ethoxy, propoxy or the like. In the class of compounds of formula I indicated, Rt is halogen, with chlorine being particularly preferred, R2 is preferably E-o-halophenyl, o, o-dihalophenyl or 2-pyridyl group. For R2 in the meaning of the o-halophenyl group, fluorine or chlorine atoms are preferred as halogen atoms. In the case where R2 is present in the meaning of the 0.0-dihalophenyl group, They are preferably two halogen atoms that are the same, in particular two fluorine atoms. A preferred meaning of R3 is an alkyl radical, a hydroxyalkyl group and an aminoalkyl group. As is apparent from the above in the compounds of formula I, Ri is particularly preferably a chlorine atom, R2 is a group o- chlorophenyl or o-fluorophenyl, and R3 is an aminoalkyl group. A particularly preferred compound is 2-chloro-4- (o-chlorophenyl) -9-aminoethyl-6H-thieno [3,2-f] * s-triazolo [4, 3 -a] -f1,4] diazepine Further representative compounds of formula I sa: 2 97 275 2-chforo-4- (o-chlorophyl) "9-methyl-6H-thieno [3,2-f] -s oxide -triazolo [4,3-a] [1,4] diazepine, 2-Chlaro-4- {o-chlorophenyio) -9-methyl-6H- thieno [3,2-f] -s- acid ethyl ester triazolo [4,3-a] [1,4] diarepinino-6-carboxylic, 2-ch-oro-9-methyl-4- (2-pyridyl) -6H-thieno [3,2-f] -s -triazolo [4,3-a] [1,4] diazepine, 2-chloro-9-methyl-4- {o-nitrophenyl-4- {o-nitrophenyl] -6H-teno [3,2-f] -s-triazolo [4/3-a ] [1/4] diazepine, 2-chloro-9-methyl-4-f8nyl, H -thieno [3,2-f] - α-triazolo [4,3-a] [M] diazepine, 2-chloro4- ( 'fluorophenyl) -9-methyl! o-6H-thieno [3,2-f] -s-triazolo [4,3-a] [1,4] diazepine, 2-chloro-4- (o, o'- difluoro) -9-methyl-6H-oxygen [3,2-f] -s-triazoio [4,3-a] [1,4] diazepine, 9-yl.pre-butyio-2-chJoro4- (o- chlorophenyl) -6H-thieno [3,2-tnazolo [4,3-a] [1,4] diazepine, 2-chloro-4- (o-chlorophenyl) -9-methylthiomethyl-6H-thieno [3 , 2-f] -s-triazolo [4,3-aj [1,4] diazepine, 2-collection * 4- (o-chlorophenes! O) -9-morpholinomethyl-6H-thieno [3,2-f] -s- triazolo [4,3-a] [1A] diazepine, 2 "Chloro4- (o-chlorophenyl} 9 * methoxymethyl-6H-thieno (3,2-f] -s-triazolo [4,3-a] [1 A] diazepine, 2-chloro-4- (o-chlorophenyl) -9-hydroxymethyl-6H-thieno [3,2-fj-s-triazo [4,3-a] [1,4] diazepine, 2-chloro -4-tochiordphenyl) -9-dimethylaminomethyl-6H-thieno [3,2-f] * - triazolo [4,3-a] [1,4] diazepine, 2-chloro-9-chlorom8tylO "4- (o- chlorophenyl) -6H-thieno [3,2'f] -s-triazolo [4,3-a] [1,4j diazepine, [2 * chloro-4- (o-chlorophenyl) -6H-thieno [3, 2-f] -s-triazolo [4,3-f] [1,4] diazepin-O-yl] -methyl, 2-chloro-4 * (o-chlorophenyio) -9- (1-hydroxyethyl) - 6H-thieno [3,2-f] -f-triazolo [4,3-a] [1,4-diazepine, 2-chloro-4- (o-chlorophenyl) -9-iodomethio-6H-thieno [3.2 -f] - α-triazolo [4,3-a] [M] diazepine, 2-chloro-9-ethoxymethyl Q4- (nitrophenyl) * 6H-thie4 [2-Chloro-4- (o-nitrophenyl) acid ethyl ester -6H-thieno [3,2-f] -s-triazolo [4,3-a] [1,4] 9-yl] -carboxy diasepin, 2-chloro-9 2-chloro-9'-methyl4- (o- trifluoromethics! -phenyl) -6H-thieno [3,2-f] -s-triazoJo {4,3-a] [1,4] - diazepine.Poc According to the invention, the cultivated thienotriazole-diazepines of the formula I and their acid addition salts can be prepared in such a way that a compound of the general formula II is cyclized in which R1, R2 and R3 have the above meaning. According to the invention, the cyclization is carried out by heating the compounds of the formula II in an organic environment, but in order to obtain satisfactory yields, in some cases it is advantageously operated in the presence of acid. For example, the cyclization can be carried out by heating the compound of formula II within a few hours to the reflux temperature in a solution of an aliphatic carboxylic acid, e.g. formic or acetic acid, walkanol, e.g. ethanol or n-propanol, or for a relatively short time, e.g. about 5 minutes to 1/2 hour, in an aliphatic carboxylic acid, e.g. acetic, isobutyric or pivalic. The compounds of formula 2 need not and may not be used in their isolated form in all cases, as they are often used in the conditions for their preparation undergo spontaneous cyclization. The preparation of starting compounds of formula 2 is shown in the attached reaction scheme, which shows the case where in formula 2, Ri is hydrogen, Ra is phenyl and R3 is as defined above. The 2-amino-3-benzothiophene of formula 4 is converted by treatment with an orthoester of formula R4-C (O * alkyl) 3 to the compound of formula 5. The reactions are expediently carried out in the presence of an inert organic solvent such as benzene, toluene, etc. the like, and acid catalyst, such as hydrochloric, sulfuric, acetic, propionic, benzenesulfonic, p-toluenesulfonic acid and the like. Temperature is not critical, however you usually work around 50 ° C to 60 ° C, but you can also work at warmer and cooler temperatures. Suitable solvents are hydrocarbons such as benzene or toluene and the like, or the excess orthoester used as a reaction component. The compound of the formula V thus obtained is reacted in an inert organic solvent with hydrazine, which is preferably used in the form of its hydrate. Aicanols such as methanol, ethanol, 1-propanol, 2-propanol and the like are particularly suitable as solvents. The reactions are carried out at a temperature from about 0 ° C to the reflux temperature of the reaction mixture, preferably from about 10 ° C to 30 ° C. The reactions can be accelerated by adding an acid catalyst, such as hydrochloric / hydrobromic acid, sulfuric acid, phosphoric acid, acetic acid, propionic acid. , benzenesulfonic, p-toluenesulfonic and the like. The thus-obtained crude product is then reacted with an alpha-halogen acid chloranhydride such as chloroacetyl chloride, bromoacetyl bromide and the like in an inert organic solvent with ice cooling or keeping the reaction mixture below the boiling point to form the compound of formula 6.97 275 3. chloroform, methylene chloride, ether, pyridine, acetic acid, mono-chloroacetic acid, or mixtures thereof with water. When an inert solvent is used, the reactions are preferably carried out in the presence of an acid acceptor such as sodium bicarbonate, sodium carbonate, potassium bicarbonate, pyridine / triethylamine, imidazole, 2-methylimidazole and the like. The compound of formula 6 is then treated with ammonia or hexamine hexamethylene tetra whereby the obtained compound of formula 2 can be cyclized into the corresponding compound of formula 1 without isolation. The cart of formula 3 does not require isolation before cyclization, that is, the closure of the ring to form the compound of formula 1 can be performed in the reaction mixture in which the compound of formula 1 was prepared 2, without isolating it, or without interrupting the course of the reaction. For example, a compound of formula VI can be added to an alcoholic, e.g. ethanolic or methanolic ammonia solution, or a compound of formula VI can be dissolved in an inert organic solvent and mixed with liquid ammonia or hexamethylene tetraamine, to obtain the compound of formula 2. Suitable for this reaction are as solvents: methylene chloride, carbon tetrachloride, ethers like tetrahydrofuran or dioxane, dimethylsulfoxide, dimethylformamide, alkanols like methanol, ethanol-propanol, 2-propanol, 1-butanol, 2-butanol and the like. The obtained compound of formula II, whether in a crude or purified state, can be cyclized in the above-mentioned manner to form a compound of formula 1. In the event that compounds of formula II are to be obtained, where Hx represents groups other than hydrogen atoms and R2 is a group other than a phenyl group, depending on the kind of the desired substituent, it is possible to start with the appropriately substituted compounds of the formula IV or introduce substituents by generally known methods or transform them into other substituents. Compounds of the formula 5 and 6 are new compounds. The compounds of formula I and their pharmaceutically usable acid addition salts are valuable medicaments and can be used as antispasmodics, calming, relaxing and anxiolytic agents. For example, the compound 2-chloro-4-fo-chlorophenyl-9-methyl-6H * thieno [3,2-f] -s-triazolo [413-a] [1,4] -diazepine in the antipentatetrazole test already mice exhibit an APR2 # 0 value of 0.03-0.1 mg / kg orally. The above-mentioned test is carried out according to the Orlaff method (Pros. Soc. Exp. Biol. Med. 70, 254-257, 1949). Thienodiazepines are known to have a similar effect from the German publication No. 2221623, but the antipentatetrazole test showed an unexpected superiority of the compounds obtained by this method. According to the invention, the new compounds of formula 1 exhibit much better pharmacological properties compared to known compounds of similar structure. The table gives comparative data obtained in the metrazol test, the results showing that the new compounds significantly exceed the known compounds for their activity. Table Compounds of formula 1, where n = O, R3 = H, and the meanings of Ri, Ra and R4 are given in the table Ri Cl Cl Cl Cl Cl Cl Cl Cl Cl Cl Cl a Cl Cl Cl Cl yz \ a R2 o -nitrophenyl o, o'-difluorophenyl phenyl o-fluorophenyl o-nitrophenyl o-nitrophenyl o-nitrophenyl o-chlorophenyl o-chlorophenyl o-nitrophenyl o-nitrophenyl o-chlorophenyl o-chlorophenyl o-chlorophenyl o-chlorophenyl o-chlorophenyl o-chlorophenyl 7 R4 -CH3 -CH3 -CHa -CHa -CHa-N (CH3) a -CO-O-CHa -CH3 -CHa-O-CH3 -CHa-OH -CHa -CH2-OH -CHa-N (CHi) a -CHa-N (CHi) a -CHa-NH-CH | -CHa-N (CaH |) a -CHa-NHa metrazol test (APR 2.0) 2.2 0.23 1.68 0.131 2.12 0.53 0.196 0.78 v 0.49 1.43 1, 33 0.494 0.189 0.58 0.173 52.34 97 275 The compounds of formula I as well as their pharmaceutically usable acid addition salts can be converted into pharmaceutical preparations by generally known methods, e.g. into tablets, dragees, suppositories, capsules, solutions, suspensions, emulsions and the like In addition to commonly used pharmacologically inert carriers, such as, for example, milk sugar, starch, talc, magnesium stearate, water, vegetable oils, polyethylene glycols and the like, these preparations may also contain preservatives, stabilizers, wetting agents and emulsifying agents, salts for changing the osmotic pressure, buffers or still other therapeutically valuable substances. If necessary, the mentioned preparations can be sterilized or also subjected to other operations accepted in the pharmaceutical industry. A suitable pharmaceutical dosage unit may contain from about 1 to 50 mg of a compound of the invention. Suitable daily doses for oral administration for mammals range from about QJ mg to about 30 mg / kg; for parenteral administration to mammals, a suitable daily dose is from about 0.1 mg / kg to about 10 mg / kg. These doses should only be taken as examples; the specific dosage must be adapted to individual needs in each case. 500 mg of crude sodium 2 - [(3.5 yl] -5-chloro-3-thiene dihydrochloride). The aqueous phase is extracted with methylene chloride. After drying over sodium sulphate and evaporating the organic phase, the residue is heated to the boiling point under a chiller. reflux in 5 ml of absolute alcohol for 30 minutes After evaporation, the crude base is chromatographed on alumina, bleached with chloroform and crystallized from ethyl acetate 9 (aminomethyl) -2-chloro-4- (o-chlorophenyl) -6H-thienoph-3,2-fj Mriazolo [4,3-a] {1,4] -dvuazepine has a melting point of 167-168 ° C. Recrystallized from ethyl acetate and petroleum ether, the sample melts at 170.5-171 ° C. 2 Formula 2 -n: \ , Formula 397 275 LX O -Alkii ó Formula A Formula 5 FL-C N, S ^ M — C No. C = 0 NH? FL-C N LX CH? Formula 2 Formula 6 Schem at 1 OL-C = Nx 3 IN DC ^ C = NT WZOR 7 Printing work UP PRL print 1/0 +! 8 Price PLN 45 PL

Claims (1)

1. Zastrzezenie patentowe Sposób wytwarzania nowych pochodnych tienotriazolodwuazepiny o ogólnym wzorze 1, w którym Rj oznacza atom chlorowca, R2 oznacza rodnik fenylowy, grupe o-trójfluorometyiofenylowa, o-chlorowcofenylo- wa, o,o'-dwuchlorowcofenylowa, o-nitrofenylowa lub grupe pirydylowa, Rj oznacza atom wodoru, rodnik alkilowy, grupe hydroksyalkilowa, al koksykarbony Iowa, chlorowcoal kilowa, alkoksyalkilowa, al kilotioalkilowa, alkoksykarbonyloalkilowa, lub grupe -alkil-Z, w której Z oznacza grupe o wzorze 3, zas R4 i R5 niezaleznie od siebie oznaczaja atom wodoru lub rodnik alkilowy, lub tez razem z atomem azotu oznaczaja jednopierscieniowy, nasycony, 5-6-czlonowy pierscien heterocykliczny o najwyzej jednym dalszym atomie azotu lub tlenu, ewentualnie w postaci soli addycyjnych z kwasami, znamienny tym, ze cyklizuje sie zwiazek o ogólnym wzorze 2, w którym Rt, R2 i R3 maja wyzej podane znaczenie i otrzymany zwiazek ewentualnie przeprowadza w sól addycyjna z kwasem. '97 275 R--C9 ;n .3 \ // 1 ^C 5CH2 *2 Wzór 1 N N CHn C=0 NhL' I 2 * PLClaim 1. Process for the preparation of new thienotriazole diazepine derivatives of general formula I, in which Rj is a halogen atom, R2 is a phenyl radical, o-trifluoromethylphenyl, o-halophenyl, o, o'-dihalophenyl, o-nitrophenyl or pyridyl group , Rj represents a hydrogen atom, an alkyl radical, a hydroxyalkyl group, Iowa alkoxycarbones, halogen halogen, alkoxyalkyl, alkylthioalkyl, alkoxycarbonylalkyl, or an e-alkyl-Z group, in which Z is a group of formula 3, and R4 and R5 independently of each other are a hydrogen atom or an alkyl radical, or also together with the nitrogen atom, represent a single ring, saturated 5-6-membered heterocyclic ring with at most one further nitrogen or oxygen atom, optionally in the form of acid addition salts, characterized in that a compound with the general general Formula 2, wherein Rt, R2 and R3 are as defined above and the resulting compound is optionally converted into an acid addition salt. '97 275 R - C9; n. 3 \ // 1 ^ C 5CH2 * 2 Formula 1 N N CHn C = 0 NhL 'I 2 * PL
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DE2533924C3 (en) * 1975-07-30 1979-05-03 C.H. Boehringer Sohn, 6507 Ingelheim Process for the preparation of 6-aryl-4H-striazolo [3,4-c] thieno [2,3-e] 1,4-diazepines
DE2531678C3 (en) * 1975-07-16 1979-06-28 C.H. Boehringer Sohn, 6507 Ingelheim Thieno [2,3e] triazole [3,4c] 5,6-dihydro-1,4-diazepines and processes for their preparation
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