RO129982A2 - New 6,8-dichloroquinolones with antimicrobial activity and process for preparing the same - Google Patents

New 6,8-dichloroquinolones with antimicrobial activity and process for preparing the same Download PDF

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RO129982A2
RO129982A2 ROA201101345A RO201101345A RO129982A2 RO 129982 A2 RO129982 A2 RO 129982A2 RO A201101345 A ROA201101345 A RO A201101345A RO 201101345 A RO201101345 A RO 201101345A RO 129982 A2 RO129982 A2 RO 129982A2
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piperidinyl
chloro
methyl
quinoline
ethyl
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RO129982B1 (en
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Lucia Pintilie
Sultana Niţă
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Institutul Naţional De Cercetare-Dezvoltare Chimico-Farmaceutică - Iccf
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Abstract

The invention relates to quinolone derivatives with antimicrobial activity and to a process for preparing the same. The claimed quinolone derivatives have a formula wherein Ris 3-methyl-piperidinyl, 4-methyl-piperidinyl, piperidinyl, pyrrolidinyl or morpholinyl and Ris a hydrogen or a chlorine atom. The claimed process consists in the nucleophilic substitution of the hydrogen in the 8th position of the quinolone derivative wherein Ris 3-methyl-piperidinyl, 4-methyl-piperidinyl, piperidinyl, pyrrolidinyl, and Ris a hydrogen atom, while using sulphuryl chloride as chlorination agent in chloroform medium at the room temperature and at a quinolone derivative:sulphuryl chloride molar ratio of 1:3.

Description

Prezenta invenție se refera la derivați 6,8 diclorochinolonici cu activitate antimicrobiana si la procedee de preparare al lor.The present invention relates to 6.8 dichloroquinolone derivatives with antimicrobial activity and processes for their preparation.

Se cunosc dervatii substituiti ai acizilor chinolin-3-carboxilici definiți prin structura generala:Substituted dervishes of quinoline-3-carboxylic acids defined by the general structure are known:

in care substituentii au diferite semnificații, care prezintă activitate antibacteriana atat împotriva bacteriilor gram-pozitive cat si a celor gram-negative. [Koga H.; Itoh A.; Murayama S.; J.Med. Chem. ,1980,23, 1358-1363; Jose A.; J. Med. Chem. 1991, 34,78-81]wherein the substituents have different meanings, which exhibit antibacterial activity against both gram-positive and gram-negative bacteria. [Koga H.; Itoh A.; Murayama S.; J.Med. Chem. , 1980,23, 1358-1363; Jose A.; J. Med. Chem. 1991, 34.78-81]

Se cunosc de asemenea dervatii substituiti ai acizilor chinolin-3-carboxilici definiți prin structura generala :Substituted derves of quinoline-3-carboxylic acids defined by the general structure are also known:

in care substituentii au semnificații bine definite si prezintă activitate antibacteriana. [DE 2840910].wherein the substituents have well-defined meanings and exhibit antibacterial activity. [OF 2840910].

Se cunosc de asemenea dervatii substituiti ai acizilor chinolin-3-carboxilici definiți prin structura generala:Substituted derves of quinoline-3-carboxylic acids defined by the general structure are also known:

in care substituentii au semnificații bine definite si prezintă activitate antibacteriana. [Yun Xun Yang, Hui Yuan Guo; Chinese Chemical Letters, 2007,18, 1479-1482]wherein the substituents have well-defined meanings and exhibit antibacterial activity. [Yun Xun Yang, Hui Yuan Guo; Chinese Chemical Letters, 2007,18, 1479-1482]

Prezenta invenție lărgește gama derivatilor cu activitate antimicrobiana cu noi compuși care corespund formulei generale I:The present invention extends the range of derivatives with antimicrobial activity with new compounds corresponding to general formula I:

^2 0 1 1 ’ 0 1 3 4 5^ 2 0 1 1 '0 1 3 4 5

Ο 7 *12* 2011 intensa, timp de 45 de minute, la temperatura menționata mai sus, când are loc si îndepărtarea alcoolului etilic rezultat in urma reacției de condensare. Se răcește la 20°C si se filtrează precipitatul format, care se spala cu acetona si se usucă. Se obțin 105 g ester etilic al aciduluiΟ 7 * 12 * 2011 intense, for 45 minutes, at the temperature mentioned above, when the ethyl alcohol removal resulting from the condensation reaction also takes place. Cool to 20 ° C and filter the formed precipitate, which is washed with acetone and dried. 105 g of ethyl ester of the acid are obtained

6,7-dicloro-4-hidroxi-chinolin-3-carboxilic (p.t.° 310-315°C; randamentul global 87%).6,7-dichloro-4-hydroxy-quinoline-3-carboxylic acid (mp. 310-315 ° C; overall yield 87%).

*H-RMN(dmso-d6, δ ppm, JHz): 8.63(s, 1H, H-2); 8.23(s, 1H, H-5(8)); 7.88(s, 1H, H-8(5)); 4.22(q, 2H, H-12, 7.1); 1.28(t, 3H, H-13, 7.1).* H-NMR (dmso-d6, δ ppm, JHz): 8.63 (s, 1H, H-2); 8.23 (s, 1H, H-5 (8)); 7.88 (s, 1H, H-8 (5)); 4.22 (q, 2H, H-12, 7.1); 1.28 (t, 3H, H-13, 7.1).

FT-IR(solid in ATR, v cm1): 3142m;3088s; 1693vs; 1604s; 1546m; 1516s; 1447m; 1378m; 1359w; 1331w; 1294m; 1266w; 1187m; 1122m; 1108m; 1028w; 966w; 909w; 888w; 860w; 827w; 800m; 756w; 679w; 647w; 620w.FT-IR (solid in ATR, v cm 1 ): 3142m; 3088s; 1693vs; 1604s; 1546m; 1516s; 1447m; 1378m; 1359w; 1331w; 1294m; 1266w; 1187m; 1122m; 1108m; 1028w; 966w; 909w; 888w; 860w; 827w; 800m; 756w; 679w; 647w; 620w.

Puritate ~80%. Amestec cu 5,6-C12.Purity ~ 80%. Mixture with 5.6-C12.

Exemplul 2: Sinteza acidului l-etil-6,7-dicloro-l,4-dihidro-4-oxo-chinolin-3-carboxilic -6C1QAExample 2: Synthesis of l-ethyl-6,7-dichloro-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid-6C1QA

0,03 Moli de dietilsulfat(DES) se adauga la un amestec format din 5,72 g (0,02 moli) ester etilic al acidului 6,7-dicloro-4-hidroxi chinolin-3-carboxilic si 108 g 40% hidroxid de sodiu. Amestecul se agita la 20°C timp da 30 min. si apoi la 100°C timp de 30 min. Se mai adauga inca 0,03 moli de dietilsulfat (DES) si se agita in continuare inca o ora. Se răcește masa de reacție la 20°C, se filtrează si se spala cu apa . Se usucă si se purifica din Ν,Ν-dimetilformamida. Se obțin 3,49 g acid l-etil-6,7-dicloro-l,4-dihidro-4-oxo-chinolin-3-carboxilic (p.t. 294,8-296,7°C, randament reacție +purificare 61%).0.03 moles of diethylsulfate (DES) was added to a mixture of 5.72 g (0.02 moles) 6,7-dichloro-4-hydroxy quinoline-3-carboxylic acid ethyl ester and 108 g 40% hydroxide. of sodium. The mixture was stirred at 20 ° C for 30 min. and then at 100 ° C for 30 min. Another 0.03 moles of diethylsulfate (DES) was added and stirred for an additional hour. Cool the reaction to 20 ° C, filter and wash with water. It is dried and purified from Ν, Ν-dimethylformamide. 3.49 g of l-ethyl-6,7-dichloro-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid are obtained (mp 294.8-296.7 ° C, reaction yield + purification 61% ).

’H-NMR(dmso-d6, δ ppm, JHz): 9.06(s, 1H, H-2); 8.42(s, 1H, H-5); 8.41(s, 1H, H-8);H-NMR (dmso-d6, δ ppm, JHz): 9.06 (s, 1H, H-2); 8.42 (s, 1H, H-5); 8.41 (s, 1H, H-8);

4.59(q, 2H, H-17, 7.1); 1.39(t, 3H, H-18, 7.1).4.59 (q, 2H, H-17, 7.1); 1.39 (t, 3H, H-18, 7.1).

13C-NMR(dmso-d6, δ ppm): 176.31(019); 165.47(C-4); 150.33(02); 138.46(Cq); 137.51(Cq); 129.59(0}); 127.11(CH); 125.57(Cq); 120.55(CH); 108.6l(Cq); 49.36(017); 14.61(018). 13 C-NMR (dmso-d6, δ ppm): 176.31 (019); 165.47 (C-4); 150.33 (02); 138.46 (Cq); 137.51 (Cq); 129.59 (0}); 127.11 (CH); 125.57 (Cq); 120.55 (CH); 108.6l (Cq); 49.36 (017); 14.61 (018).

FT-IR(solid in ATR, vcm'1): 3094w; 3038w; 2990w; 1715s; 1599vs; 1547m; 1526m; 1486m; 1456vs; 1437vs; 1382s; 1300m; 1258m; 1219s; 1147m; 1122m; 1090m; 973m; 936s; 909m; 864m; 805m; 771w; 752w; 688w; 666m; 541w.FT-IR (solid in ATR, vcm ' 1 ): 3094w; 3038w; 2990w; 1715s; 1599vs; 1547m; 1526m; 1486m; 1456vs; 1437vs; 1382s; 1300m; 1258m; 1219s; 1147m; 1122m; 1090m; 973m; 936s; 909m; 864m; 805m; 771w; 752w; 688w; 666m; 541w.

Exemplul 3: Sinteza acidului l-etil-6-cloro-7-(4-metil-piperidinil)-l,4-dihidro4-oxo-chinolin-3-carboxilic - PQ 80Example 3: Synthesis of 1-ethyl-6-chloro-7- (4-methyl-piperidinyl) -1,4-dihydro4-oxo-quinoline-3-carboxylic acid - PQ 80

Λτ 2 Ο 1 1 - 0 ΐ 3 4 5 0 7,2‘ 2011Λτ 2 Ο 1 1 - 0 ΐ 3 4 5 0 7, 2 '2011

Un amestec format din acid l-etil-6,7-dicloro-l,4-dihidro-4-oxo-chinolin-3-carboxilic (6C1QA) (5,72 g, 0,02 moli), 4-metil-piperidina (9,9 g, 0,1 moli; 12,05 ml) si N,Ndimetilformamida (60 ml) se încălzește sub agitare energica timp de 8 ore la 110-120°C. Sfârșitul regimului de reacție este pus in evidenta prin cromatografie in strat subtirersistem de eluare: tetrahidrofuran :dioxan:amoniac conc. : 20:60:30 (v/v/v), suport Silica gel 60F 254(s-a urmărit dispariția spotului cracteristic acidului l-etil-6,7-dicloro-l,4-dihidro-4-oxo-chinolin-3-carboxilic. Masa de reacție este transvazata in instalația de distilare la vid pentru îndepărtarea solventului si a excesului de 4-metil-piperidina. Reziduu se dizolva intr-o soluție 2N de NaOH, prin încălzire la 60°C. Soluția rezultata se decolorează si se filtrează, si după răcire se aduce la pH 7 cu o soluție 10 % de acid actic. Precipitatul format se filtrează si se spala cu apa. După recristalizare din dimetilformamida se obțin 5 g produs pur (p.t. = 262,5-264,5°C; randament reacție + purificare 70 %).A mixture of l-ethyl-6,7-dichloro-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid (6C1QA) (5.72 g, 0.02 mol), 4-methyl-piperidine (9.9 g, 0.1 mol; 12.05 ml) and N, Ndimethylformamide (60 ml) was heated under vigorous stirring for 8 hours at 110-120 ° C. The end of the reaction regime is highlighted by chromatography in the elution sub-system: tetrahydrofuran: dioxane: ammonia conc. : 20:60:30 (v / v / v), support Silica gel 60F 254 (followed by the disappearance of the spot spot of the l-ethyl-6,7-dichloro-1, 4-dihydro-4-oxo-quinoline-3- acid bacterial spot). The reaction mass is transferred to the vacuum distillation facility to remove the solvent and the excess of 4-methyl-piperidine. The residue is dissolved in a 2N NaOH solution, heated to 60 ° C. The resulting solution is discolored and discolored. filter, and after cooling it is brought to pH 7 with a 10% solution of actic acid. The precipitate formed is filtered and washed with water. 5 g pure product is obtained after recrystallization from dimethylformamide (mp = 262.5-264.5 °). C; reaction yield + purification 70%).

'H-NMR CDCl3:5=l,02(3H,CH3 piperidina); 1,49 (3H, CH3 etil); 1,55-1,9 (5H, CH si CH2 din piperidina); 2,78 si 3,62 (fiecare 2H, CH2-piperidina) 4,35 (2H, Creții); 6,95 (1H, CH arom.); 8,39 (1H, CH arom.); 8,67 (1H,CH arom)H-NMR CDCl 3 : 5 = 1.02 (3H, CH 3 piperidine); 1.49 (3H, CH 3 ethyl); 1.55-1.9 (5H, CH and CH 2 from piperidine); 2.78 and 3.62 (each 2H, CH2-piperidine) 4.35 (2H, Cre); 6.95 (1H, aromatic CH); 8.39 (1H, CH arom.); 8.67 (1H, CH aroma)

Prin același procedeu au fost preparați următorii compuși:By the same process, the following compounds were prepared:

Exemplul 3a: acidul l-etil-6-cloro-7-(3-metil-piperidinil)-l,4-dihidro-4-oxo-chinolin-3carboxilic (6C1PQ-24) (raport molar acid chinolin carboxilic-heterociclu 1: 5,mediu de reacție •.dimetilformamida, temperatura de reacție 110°C, timp reacție 5,5 ore, p.t. = 216,2-218,4°C, randament reacție + purificare 58%)Example 3a: 1-ethyl-6-chloro-7- (3-methyl-piperidinyl) -1,4-dihydro-4-oxo-quinoline-3-carboxylic acid (6C1PQ-24) (quinoline carboxylic acid-heterocycle 1 molar ratio: 5, reaction medium • .dimethylformamide, reaction temperature 110 ° C, reaction time 5.5 hours, mp = 216.2-218.4 ° C, reaction yield + purification 58%)

'H-NMR(dmso-d6, δ ppm, 7 Hz): 9.00(s, 1H, H-2); 8.22(s, 1H, H-5); 7.30(s, 1H, H-8); 3.42(m, 4H, H-12-16); 2.83(m, 1H, H-15); 1.81(m, 3H, H-14-15); 1.47(t, 3H, H-18, 7.3); 1.17(q, 1H, H13, 6.4); 1.00(d, 3H, H-20, 6.4).H-NMR (dmso-d6, δ ppm, 7 Hz): 9.00 (s, 1H, H-2); 8.22 (s, 1H, H-5); 7.30 (s, 1H, H-8); 3.42 (m, 4H, H-12-16); 2.83 (m, 1H, H-15); 1.81 (m, 3H, H-14-15); 1.47 (t, 3H, H-18, 7.3); 1.17 (q, 1H, H13, 6.4); 1.00 (d, 3H, H-20, 6.4).

O 1 1-01345O 1 1-01345

7 -12- 2011 13ONMR(dmso-d6, δ ppm, JHz): 175.60(04); 166.11(C-21); 154.98(Cq); 149.31(02);7 -12- 2011 13 ONMR (dmso-d6, δ ppm, JHz): 175.60 (04); 166.11 (C-21); 154.98 (Cq); 149.31 (02);

139.85(Cq); 127.79(05); 127.16(Cq); 121.20(Cq); 108.51(Cq); 108.40(08); 59.00(012);139.85 (Cq); 127.79 (05); 127.16 (Cq); 121.20 (Cq); 108.51 (Cq); 108.40 (08); 59.00 (012);

51.98(017); 49.36(016); 32.58(015); 31.19(013); 25.25(014); 19.30(020); 14.61(018).51.98 (017); 49.36 (016); 32.58 (015); 31.19 (013); 25.25 (014); 19.30 (020); 14.61 (018).

FT-IR(solid in ATR, v cm'1): 3037; 2958; 2927; 2849; 2807; 2722; 1715; 1609; 1535; 1512; 1449; 1385; 1359; 1301; 1269; 1243; 1203; 1117; 1086; 1022; 976; 924; 897; 852; 806; 753; 714; 680; 620; 553;493;436.FT-IR (solid in ATR, v cm ' 1 ): 3037; 2958; 2927; 2849; 2807; 2722; 1715; 1609; 1535; 1512; 1449; 1385; 1359; 1301; 1269; 1243; 1203; 1117 1086; 1022; 976; 924; 897; 852; 806; 753; 714; 680; 620; 553; 493; 436.

Exemplul 3b : acid l-etil-6-cloro-7-morfolinil-l,4-dihidro-4-oxo-chinolin-3-carboxilic (6C1PQ25) (raport molar acid chinolin carboxilic-heterociclu 1:5, temperatura de reacție 110°C,mediu de reacție : dimetilsulfoxid, timp reacție 6 ore, p.t. - 267,1-269,2°C, randament reacție + purificare 80%)Example 3b: 1-ethyl-6-chloro-7-morpholinyl-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid (6C1PQ25) (quinoline carboxylic acid-heterocycle 1: 5 molar ratio, reaction temperature 110 ° C, reaction medium: dimethylsulfoxide, reaction time 6 hours, mp - 267.1-269.2 ° C, reaction yield + purification 80%)

1 H-NMR(dmso-d6, δ ppm, JHz): 9.02(s, 1H, H-2); 8.27(s, 1H, H-5); 7.36(s, 1H, H-8); 4.64(q, 2H, H-17, 7.1); 3.85(m, sist. A2B2, 4H, H-13-15); 3.28(m, sist. A2B2, 4H, H-12-16); 1.46(t, 3H, H-18, 7.1). 1 H-NMR (dmso-d6, δ ppm, JHz): 9.02 (s, 1H, H-2); 8.27 (s, 1H, H-5); 7.36 (s, 1H, H-8); 4.64 (q, 2H, H-17, 7.1); 3.85 (m, sist. A 2 B 2 , 4H, H-13-15); 3.28 (m, sist. A 2 B 2 , 4H, H-12-16); 1.46 (t, 3H, H-18, 7.1).

13ONMR(dmso-d6, δ ppm): 175.61(04); 165.34(021); 153.01(Cq); 148.89(CH-2); 13 ONMR (dmso-d6, δ ppm): 175.61 (04); 165.34 (021); 153.01 (Cq); 148.89 (CH-2);

138.72(Cq); 126.90(05); 125.91(Cq); 120.66(Cq); 107.86(C-8); 65.67(013-15); 50.53(012-138.72 (Cq); 126.90 (05); 125.91 (Cq); 120.66 (Cq); 107.86 (C-8); 65.67 (013-15); 50.53 (012-

16); 48.55(017); 13.89(018).16); 48.55 (017); 13.89 (018).

FT-IR(solid in ATR, v cm’1): 3035; 2971; 2947; 2904; 2865; 1724; 1609; 1514; 1466; 1438; 1384; 1337; 1294; 1237; 1191; 1111; 1062; 995; 950; 912; 865; 842; 805; 750; 713; 686; 625; 552; 490; 453; 426.FT-IR (solid in ATR, v cm ' 1 ): 3035; 2971; 2947; 2904; 2865; 1724; 1609; 1514; 1466; 1438; 1384; 1337; 1294; 1237; 1191; 1111; 1062; 995; 950; 912; 865; 842; 805; 750; 713; 686; 625; 552; 490; 453; 426.

Exemplul 3c : acid l-etil-6-cloro-7-piperidinil-l,4-dihidro-4-oxo-chinolin-3-carboxilic (6C1PQ32) (raport molar acid chinolin carboxilic-heterociclu 1:5, temperatura de reacție 110°C, mediu de reacție dimetilformamida, timp reacție 8 ore, p.t. = 234,4-236,4 randament reacție + purificare 53%)Example 3c: l-ethyl-6-chloro-7-piperidinyl-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid (6C1PQ32) (quinoline carboxylic acid-heterocycle molar ratio 1: 5, reaction temperature 110 ° C, dimethylformamide reaction medium, reaction time 8 hours, mp = 234.4-236.4 reaction yield + purification 53%)

‘H-NMRidmso-dâ, δ ppm, JHz): 8.97(s, 1H, H-2); 8.20(s, 1H, H-5); 7.28(s, 1H, H-8); 4.58(q, 2H, H-17, 7.1); 3.18(m, 4H, 2H-20, 2H-24); 1.72(bs, 4H, 2H-21, 2H-23); 1.62(bs, 2H, H-22); 1.42(t, 3H, H-18, 7.1).H-NMRidmso-dâ, δ ppm, JHz): 8.97 (s, 1H, H-2); 8.20 (s, 1H, H-5); 7.28 (s, 1H, H-8); 4.58 (q, 2H, H-17, 7.1); 3.18 (m, 4H, 2H-20, 2H-24); 1.72 (bs, 4H, 2H-21, 2H-23); 1.62 (bs, 2H, H-22); 1.42 (t, 3H, H-18, 7.1).

(λ“2 Ο 1 1 - Ο 1 3 4 5(λ “2 Ο 1 1 - Ο 1 3 4 5

O 7 -12- 2011 13C-NMR(dmso-d6, δ ppm): 176.01(C-4); 165.75(019); 154.61(09); 148.99(02); 139.16(0O 7 -12- 2011 13 C-NMR (dmso-d6, δ ppm): 176.01 (C-4); 165.75 (019); 154.61 (09); 148.99 (02); 139.16 (0

9);9);

127.04(05); 120.41(03); 107.90(08); 107.73(010); 51.84(020, 024); 48.86(017); 25.44(021, 023); 23.49(022); 14.17(018).127.04 (05); 120.41 (03); 107.90 (08); 107.73 (010); 51.84 (020, 024); 48.86 (017); 25.44 (021, 023); 23.49 (022); 14.17 (018).

FT-IR(solid in ATR, v cm’1): 3O35w; 2990w; 295 lm; 2937m; 2917m; 2842w; 1722vs; 1608s; 1513s; 1486m; 1462vs; 1443vs; 1388m; 1373s; 1340m; 1297m; 1256m; 1240vs; 1197sm; 1091m; 1061m; 1032m; 985m; 949m; 914w; 899m; 863m; 843w; 823w; 805m; 750w; 687m; 528w.FT-IR (solid in ATR, v cm ' 1 ): 3O35w; 2990w; 295 lm; 2937m; 2917m; 2842w; 1722vs; 1608s; 1513s; 1486m; 1462vs; 1443vs; 1388m; 1373s; 1340m; 1297m; 1256m; 1240vs; 1197sm; 1091m; 1061m; 1032m; 985m; 949m; 914w; 899m; 863m; 843w; 823w; 805m; 750w; 687m; 528w.

Exemplul 3d : acid l-etil-6-cloro-7-pirolidinil-l,4-dihidro-4-oxo-chinolin-3-carboxilic (6C1PQ35) (raport molar acid chinolin carboxilic-heterociclu 1:5, temperatura de reacție 80-90°C, mediu de reacție: dimetilformamida, timp reacție 5 ore, p.t. = 312,3-315,5°C, randament reacție + purificare 75%)Example 3d: l-ethyl-6-chloro-7-pyrrolidinyl-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid (6C1PQ35) (quinoline carboxylic acid-heterocycle molar ratio 1: 5, reaction temperature 80 -90 ° C, reaction medium: dimethylformamide, reaction time 5 hours, mp = 312.3-315.5 ° C, reaction yield + purification 75%)

’H-NMR(dmso-d6, δ ppm, JHz): 8.89(s, IH, H-2); 8.14(s, IH, H-5); 6.83(s, IH, H-8); 4.52(q, 2H, H-17, 7.1); 3.66(m, 4H, H-20, H-23); 1.97(m, 4H, H-21, H-22); 1.42(t, 3H, H-18, 7.1).H-NMR (dmso-d6, δ ppm, JHz): 8.89 (s, IH, H-2); 8.14 (s, IH, H-5); 6.83 (s, IH, H-8); 4.52 (q, 2H, H-17, 7.1); 3.66 (m, 4H, H-20, H-23); 1.97 (m, 4H, H-21, H-22); 1.42 (t, 3H, H-18, 7.1).

FT-IR(solid in ATR, v cm'1): 3057m; 2929s; 2846m; 1708s; 1614vs; 1558m; 1530m; 1510s; 1467vs; 1442s; 1402s; 1344sm; 1273m; 1252m; 1217m; 1177m; 111 lm; 1095m; 1027m;995m; 933w; 873w; 809m; 748w; 649m.FT-IR (solid in ATR, v cm ' 1 ): 3057m; 2929s; 2846m; 1708s; 1614vs; 1558m; 1530m; 1510s; 1467vs; 1442s; 1402s; 1344sm; 1273m; 1252m; 1217m; 1177m; 111 lm; 1095m; 1027m, 995m; 933w; 873w; 809m; 748w; 649m.

Exemplul 4: acid l-etil-6-cloro-7-morfolinil-8-cloro—4-oxo-l,4-dihidro-chinolin-3-carboxilic 6C1PQ-28Example 4: 1-ethyl-6-chloro-7-morpholinyl-8-chloro-4-oxo-1,4-dihydro-quinoline-3-carboxylic acid 6C1PQ-28

Peste o soluție de acid l-etil-6-cloro-7-morfolinil-l,4-dihidro-4-oxo-chinolin-3-carboxilic (6C1PQ-25) (1,68 g; 0,005 moli) in cloroform (150 ml), se picura, sub agitare la temperatura camerei, clorura de sulfuril (2,07 g; 0,015 moli; 1,14 ml), după care, se mai agita masa de reacție inca 30 minute la aceeași temperatura. Soluția cloroformica de acid l-etil-6-cloro-7-morfolinil-8cloro-l,4-dihidro-4-oxo-chinolin-3-carboxilic se spala cu 2x200 ml apa, se usucă pe sulfat de sodiu anhidru, si se concentrează. Peste reziduu se adauga 50 ml metanol pentru precipitarea produsului .Se obțin 1,52 g produs pur (spot cromatografic unitar; p.t.0 213,9-216,7°C; randament -81,9%).Over a solution of l-ethyl-6-chloro-7-morpholinyl-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid (6C1PQ-25) (1.68 g; 0.005 mol) in chloroform (150 ml), sulfuryl chloride (2.07 g; 0.015 mol; 1.14 ml) is dripped at room temperature, followed by stirring for another 30 minutes at the same temperature. The chloroform solution of l-ethyl-6-chloro-7-morpholinyl-8-chloro-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid was washed with 2x200 ml of water, dried over anhydrous sodium sulfate, and dried. concentrated. To the residue was added 50 ml of methanol to precipitate the product .It is obtained 1.52 g of pure product (single spot by chromatography, for 0 213.9 to 216.7 ° C; yield -81.9%).

^-2011-01345^ -2011 to 01,345

7 -12- 20117-12 December 2011

’H-NMRCdmso-dâ, δ ppm, JHz): 8.92(s, 1H, H-2); 8.22(s, 1H, H-5); 4.80(m, 2H, H-17, 7.1); 3.78(m, 4H, H-21, H-23); 3.33(m, 4H, H-20, H-24); 1.40(t, 3H, H-18, 7.1).'H-NMRCdmso-dâ, δ ppm, JHz): 8.92 (s, 1H, H-2); 8.22 (s, 1H, H-5); 4.80 (m, 2H, H-17, 7.1); 3.78 (m, 4H, H-21, H-23); 3.33 (m, 4H, H-20, H-24); 1.40 (t, 3H, H-18, 7.1).

13ONMR(dmso-d6, δ ppm): 175.70(04); 165.00(019); 152.98(02); 150.40(09); 138.54(0 7); 130.76(06); 125.81 (C-5); 124.60(010); 108.61(03); 66.64(021, 023); 52.97(017); 50.19(020, 024); 15.47(018). 13 ONMR (dmso-d6, δ ppm): 175.70 (04); 165.00 (019); 152.98 (02); 150.40 (09); 138.54 (0 7); 130.76 (06); 125.81 (C-5); 124.60 (010); 108.61 (03); 66.64 (021, 023); 52.97 (017); 50.19 (020, 024); 15.47 (018).

FT-IR(solid in ATR, v cm’1): 3046w; 2981m; 2948w; 2913w; 2834m; 1716vs; 1610vs; 1547m; 1491vs; 1430vs; 1367m; 1290w; 1258m; 1236m; 1113s; lOOOm; 928s; 860w; 835m; 803m; 761m; 607w.FT-IR (solid in ATR, v cm ' 1 ): 3046w; 2981m; 2948w; 2913w; 2834m; 1716vs; 1610vs; 1547m; 1491vs; 1430vs; 1367m; 1290w; 1258m; 1236m; 1113s; lOOOm; 928S; 860w; 835m; 803m; 761m; 607w.

Prin același procedeu au fost preparați următorii compuși:By the same process, the following compounds were prepared:

Exemplul 4a : acid l-etil-6-cloro-7-(3-metil-piperidinil)-8-cloro-4-oxo-l,4-dihidro-chinolin-3carboxilic 6C1PQ-30 (p.t. = 190,3-192,2°C, randament 60%)Example 4a: 1-ethyl-6-chloro-7- (3-methyl-piperidinyl) -8-chloro-4-oxo-1,4-dihydro-quinoline-3-carboxylic acid 6C1PQ-30 (pt = 190.3-192 , 2 ° C, 60% yield)

’H-NMR(CDCI3+tfa, δ ppm, JHz): 8.59(s, 1H, H-2); 8.32(s, 1H, H-5); 4.62(q, 2H, H-17, 7.1); 3.20-2.80(m, 4H, H-20, H-24); 1.95-1.80(m, 3H, H-22, H-23); 1.48(t, 3H, H-18, 7.1); 0.85(d, 3H, H-25, 6.3).H-NMR (CDCl 3 + tfa, δ ppm, JHz): 8.59 (s, 1H, H-2); 8.32 (s, 1H, H-5); 4.62 (q, 2H, H-17, 7.1); 3.20-2.80 (m, 4H, H-20, H-24); 1.95-1.80 (m, 3H, H-22, H-23); 1.48 (t, 3H, H-18, 7.1); 0.85 (d, 3H, H-25, 6.3).

13ONMR(CDCl3+tfa, δ ppm): 176.65(04); 165.43(019); 152.92(07); 151.41(02); 139.24(0 6); 132.46(08); 127.12(Cq); 126.87(05); 125.24(Cq); 109.52(Cq); 59.13(020); 53.51 (017); 51.59(024); 32.79(022); 31.69(023); 26.14(021); 19.20(025); 15.86(018). 13 ONMR (CDCl 3 + tfa, δ ppm): 176.65 (04); 165.43 (019); 152.92 (07); 151.41 (02); 139.24 (0 6); 132.46 (08); 127.12 (Cq); 126.87 (05); 125.24 (Cq); 109.52 (Cq); 59.13 (020); 53.51 (017); 51.59 (024); 32.79 (022); 31.69 (023); 26.14 (021); 19.20 (025); 15.86 (018).

FT-IR(solid in ATR, v cm'1): 3050m; 2925s; 2840m; 1717vs; 1610vs; 1547s; 1492vs; 1433vs; 1404vs; 1381s; 1357s; 1281m; 1263m; 1240m; 1210m; 1192m; 1144w; 1119w; 1090m; 1068w; 1022w; 973w; 923m; 85 lw; 834w; 801m; 714m.FT-IR (solid in ATR, v cm ' 1 ): 3050m; 2925s; 2840m; 1717vs; 1610vs; 1547s; 1492vs; 1433vs; 1404vs; 1381s; 1357s; 1281m; 1263m; 1240m; 1210m; 1192m; 1144w; 1119w; 1090m; 1068w; 1022w; 973w; 923m; 85 lw; 834w; 801m; 714m.

Exemplul 4b : acid l-etil-6-cloro-7-(4-metil-piperidinil)-8-cloro-4-oxo-l,4-dihidro-chinolin-3carboxilic Q-87 (p.t. = 152,3-154,9°C, randament 78%)Example 4b: 1-ethyl-6-chloro-7- (4-methyl-piperidinyl) -8-chloro-4-oxo-1,4-dihydro-quinoline-3-carboxylic acid Q-87 (pt = 152.3-154 , 9 ° C, yield 78%)

(^-20 11-0 1345 0 1 -12’ 2011(^ -20 11-0 1345 0 1 -12 '2011

’H-NMR(DMSO-d6„ δ ppm, JHz): 8.97(s, 1H, H-2); 8.31(s, 1H, H-5); 5,l(q, 2H, H-17, 7.1); 3.62 (2H, H-20, H-24); 3.48 (m, 1H, H-20); 3.39 (m, 1H, H-24); 2,48-2,52(m,4H,H-21,H-22), l,43(m, 3H, H-23); 1.4l(t, 3H, H-18, 7.1); l,24(d, 3H, H-25, 6.5).H-NMR (DMSO-d6 "δ ppm, JHz): 8.97 (s, 1H, H-2); 8.31 (s, 1H, H-5); 5, l (q, 2H, H-17, 7.1); 3.62 (2H, H-20, H-24); 3.48 (m, 1H, H-20); 3.39 (m, 1H, H-24); 2.48-2.52 (m, 4H, H-21, H-22), l, 43 (m, 3H, H-23); 1.4l (t, 3H, H-18, 7.1); l, 24 (d, 3H, H-25, 6.5).

FT-IR(solid in ATR, v cm’1): 3059; 2948; 1728; 1612; 1554; 1489; 1456; 1417; 1388; 1339;1293; 1255; 1236; 1211; 1172; 1149; 1116; 1085; 1044; 927; 838; 807; 771; 721.FT-IR (solid in ATR, v cm ' 1 ): 3059; 2948; 1728; 1612; 1554; 1489; 1456; 1417 1388; 1339, 1293; 1255; 1236; 1211; 1172; 1149; 1116; 1085; 1044; 927; 838; 807; 771; 721.

Exemplul 4c : acid l-etil-6-cloro-7-piperidinil-8-cloro-4-oxo-l,4-dihidro-chinolin-3-carboxilicExample 4c: 1-ethyl-6-chloro-7-piperidinyl-8-chloro-4-oxo-1,4-dihydro-quinoline-3-carboxylic acid

6C1PQ-33 (p.t. = 214,6-216,3°C, randament 76%)6C1PQ-33 (mp = 214.6-216.3 ° C, 76% yield)

6CIPQ 33 ‘H-NMR(DMSO-d6„ δ ppm, JHz): 8.89(s, 1H, H-2); 8.19(s, 1H, H-5); 4,77(q, 2H, H-17, 7.1);6CIPQ 33 'H-NMR (DMSO-d6' δ ppm, JHz): 8.89 (s, 1H, H-2); 8.19 (s, 1H, H-5); 4.77 (q, 2H, H-17, 7.1);

3.6 (m,4H, H-20, H-24); 2,53(bs,4H, H-21,; 2,5 (bs,2H,H-22); l,4(t,3H,H-18)3.6 (m, 4H, H-20, H-24); 2.53 (bs, 4H, H-21,; 2.5 (bs, 2H, H-22); l, 4 (t, 3H, H-18)

FT-IR(solid in ATR, v cm’1): 3057; 2933; 2848; 1723; 1612; 1552; 1489; 1454; 1424; 1346; 1301;1252; 1234; 1158; 1117; 1094; 1023; 992; 928; 860; 801; 768.FT-IR (solid in ATR, v cm -1 ): 3057; 2933; 2848; 1723; 1612; 1552; 1489; 1454; 1424; 1346; 1301, 1252; 1234; 1158; 1117 1094; 1023; 992; 928; 860; 801; 768.

Exemplul 4d : acid l-etil-6-cloro-7-pirolidinil-8-cloro-4-oxo-l,4-dihidro-chinolin-3-carboxilic 6C1PQ-30 (p.t. = 200-203,3°C, randament 67%)Example 4d: 1-ethyl-6-chloro-7-pyrrolidinyl-8-chloro-4-oxo-1,4-dihydro-quinoline-3-carboxylic acid 6C1PQ-30 (mp = 200-203.3 ° C, yield 67%)

6CIPQ-36 c\- 2 O 1 1 O 1 3 4 56CIPQ-36 c \ - 2 O 1 1 O 1 3 4 5

O 7 -12- 2011 'H-NMR(CDCl3+tfa, δ ppm, JHz): 9.07(s, 1H, H-2); 8.62(s, 1H, H-5); 5.02(q, 2H, H-17, 7.1);O 7 -12- 2011 'H-NMR (CDCl 3 + tfa, δ ppm, JHz): 9.07 (s, 1H, H-2); 8.62 (s, 1H, H-5); 5.02 (q, 2H, H-17, 7.1);

3.58(m, 4H, H-20, H-23); 2.99(m, 4H, H-21, H-22); 1.66(t, 3H, H-18, 7.1).3.58 (m, 4H, H-20, H-23); 2.99 (m, 4H, H-21, H-22); 1.66 (t, 3H, H-18, 7.1).

l3C-NMR(CDCl3+tfa, δ ppm): 175.94(04); 169.81(019); 153.64(02); 144.21(Cq); 137.98(0 7); 136.09(09); 127.29(05); 126.96(03); 108.08(010); 95.22(08); 55.82(020, 023); 48.13(017); 42.76(021, 022); 16.37(018). l3 C-NMR (CDCl 3 + tfa, δ ppm): 175.94 (04); 169.81 (019); 153.64 (02); 144.21 (Cq); 137.98 (0 7); 136.09 (09); 127.29 (05); 126.96 (03); 108.08 (010); 95.22 (08); 55.82 (020, 023); 48.13 (017); 42.76 (021, 022); 16.37 (018).

FT-IR(solid in ATR, v cm1): 3063w; 3000w; 2938w; 2890w; 2843w; 1716vs; 1606s; 1553m; 1492m; 1481m;1461s; 1429vs; 1382m; 1366m; 1350m; 1329m; 1257m; 1204m; 1173m; 1118m; 1065s; 1035m; 926m; 842m; 806m; 710w; 670m..FT-IR (solid in ATR, v cm 1 ): 3063w; 3000W; 2938w; 2890w; 2843w; 1716vs; 1606s; 1553m; 1492m; 1481m; 1461s; 1429vs; 1382m; 1366m; 1350m; 1329m; 1257m; 1204m; 1173m; 1118m; 1065s; 1035m; 926m; 842m; 806m; 710W; 670m ..

In scopul determinării proprietății antimicrobiene pe care o pot avea clorochinolonele , s-a recurs la metoda dilutiilor seriate in vederea stabilirii unei concentrații minime inhibitorii (CMI) si a tipului de de acțiune pe care acestea le au fata de tulpini bacteriene test, frecvent întâlnite in tehnologiile farmaceutice (activitate bactericida-CMB).S-a determinat CMI în bulion MuellerHinton, utilizandu-se metoda microdiluțiilor. Tulpinile test față de care s-a făcut testarea sunt Escherichia coli ATCC 25922, Staphylococcus aureus ATCC 25923 si Pseudomonas aeruginosa ATCC 9027.In order to determine the antimicrobial properties that chloroquinolones can have, the dilution method was used in order to establish a minimum inhibitory concentration (CMI) and the type of action that they have against the test bacterial strains, commonly encountered in pharmaceutical technologies. (bactericidal activity-CMB). CMI was determined in MuellerHinton broth, using the microdilution method. The test strains tested were Escherichia coli ATCC 25922, Staphylococcus aureus ATCC 25923 and Pseudomonas aeruginosa ATCC 9027.

Tabel : Activitatea antimicrobiana „in vitro” a clorochinolonelorTable: "In vitro" antimicrobial activity of chloroquinolones

Denumire compus Name compound Concentrație minima inhibitorie ( pg/ml) Minimum inhibitory concentration (pg / ml) Escherichia coli ATCC 25922 Escherichia coli ATCC 25922 Staphylococcus aureus ATCC 25923 Staphylococcus aureus ATCC 25923 Pseudomonas aeruginosa ATCC 9027 Pseudomonas aeruginosa ATCC 9027 Q-87 Q-87 3,12 3.12 6,25 6.25 6,25 6.25 6C1PQ-28 6C1PQ-28 1,28 1.28 1,28 1.28 64 64 6C1PQ-30 6C1PQ-30 8 8 2,56 2.56 2,56 2.56 6C1PQ-33 6C1PQ-33 2,56 2.56 2,56 2.56 2,56 2.56 6C1PQ-36 6C1PQ-36 2,56 2.56 2,56 2.56 2,56 2.56

Dintre compușii testați, compusul 6C1PQ 28 prezintă activitate antibacteriană mai intensa față de E. Coli ATCC 25922 (CMI 1,28 pg/mL), si fata de S.aureus ATCC29223 (CMI 1,28 pg/mL).Of the compounds tested, compound 6C1PQ 28 exhibits more antibacterial activity compared to E. coli ATCC 25922 (CMI 1.28 pg / mL), and to S.aureus ATCC29223 (CMI 1.28 pg / mL).

(>‘20 11-0 1345(> '20 11-0 1345

Claims (8)

REVENDICĂRI 8 1 ·®“ 2811Claims 8 1 · ® “2811 1.Derivații chinolonici, cu formula generala I 1. Chinolinic derivatives, of general formula I O A | | Re Re C2H5 C 2 H 5
caracterizați prin aceea ca in care : R7 este 3-metil-piperidinil, 4-metil-piperidinil, piperidinil, pirolidinil sau morfolinil iar Rg este un atom de hidrogen sau clor.characterized in that: R7 is 3-methyl-piperidinyl, 4-methyl-piperidinyl, piperidinyl, pyrrolidinyl or morpholinyl and Rg is a hydrogen or chlorine atom.
2. Derivat chinolonic, conform revendicării 1, caracterizat prin aceea ca, este acidul 1-etil6-cloro-7-(4-metil-piperidinil)-l,4-dihidro-4-oxo-chinolin-3-carboxilic.A quinolone derivative according to claim 1, characterized in that it is 1-ethyl 6-chloro-7- (4-methyl-piperidinyl) -1,4-dihydro-4-oxo-quinoline-3-carboxylic acid. 3. Derivat chinolonic, conform revendicării 1, caracterizat prin aceea ca, este acidul 1-etil6-cloro-7-(4-metil-piperidinil)-8-cloro-l,4-dihidro-4-oxo-chinolin-3-carboxilic.A quinolone derivative according to claim 1, characterized in that it is 1-ethyl 6-chloro-7- (4-methyl-piperidinyl) -8-chloro-1,4-dihydro-4-oxo-quinoline-3-. acid. 4. Derivat chinolonic, conform revendicării 1, caracterizat prin aceea ca, este acidul 1-etil6-cloro-7-(3-metil-piperidinil)-8-cloro-l,4-dihidro-4-oxo-chinolin-3-carboxilic.A quinolone derivative according to claim 1, characterized in that it is 1-ethyl 6-chloro-7- (3-methyl-piperidinyl) -8-chloro-1,4-dihydro-4-oxo-quinoline-3-. acid. 5. Derivat chinolonic, conform revendicării 1, caracterizat prin aceea ca, este acidul 1-etil6-cloro-7-piperidinil-8-cloro-l,4-dihidro-4-oxo-chinolin-3-carboxilic.A quinolone derivative according to claim 1, characterized in that it is 1-ethyl-6-chloro-7-piperidinyl-8-chloro-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid. 6. Derivat chinolonic, conform revendicării 1, caracterizat prin aceea ca, este acidul 1-etil6-cloro-7-pirolidinil-8-cloro-l,4-dihidro-4-oxo-chinolin-3-carboxilic.A quinolone derivative according to claim 1, characterized in that it is 1-ethyl 6-chloro-7-pyrrolidinyl-8-chloro-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid. 7. Derivat chinolonic, conform revendicării 1, caracterizat prin aceea ca, este acidul 1-etil6-cloro-7-morfolinil-8-cloro-l,4-dihidro-4-oxo-chinolin-3-carboxilic.The quinolone derivative according to claim 1, characterized in that it is 1-ethyl 6-chloro-7-morpholinyl-8-chloro-1,4-dihydro-4-oxo-quinoline-3-carboxylic acid. 8. Procedeu de preparare a derivatilor chinolonici, definiți in revendicarea 1, in care R7 este 3-metil-piperidinil, 4-metil-piperidinil, piperidinil, pirolidinil sau morfolinil iar Rg este un atom de clor, caracterizat prin aceea ca, are loc printr-o reacție de substituție nucleofila a hidrogenului din poziția 8 a derivatului chinolonic definit in revendicarea 1, in care R7 este 3-metil-piperidinil, 4-metil-piperidinil, piperidinil, pirolidinil iar Rg este un atom de hidrogen, utilizând drept agent de clorurare, clorură de sulfuril, in mediu de cloroform, la temperatura camerei si la un raport molar intre derivatul chinolonic si clorură de sulfuril de 1 la 3.A process for preparing quinolone derivatives, as defined in claim 1, wherein R 7 is 3-methyl-piperidinyl, 4-methyl-piperidinyl, piperidinyl, pyrrolidinyl or morpholinyl and Rg is a chlorine atom, characterized in that by a nucleophile substitution reaction of hydrogen at position 8 of the quinolone derivative as defined in claim 1, wherein R7 is 3-methyl-piperidinyl, 4-methyl-piperidinyl, piperidinyl, pyrrolidinyl and Rg is a hydrogen atom, using as the agent of chloride, sulfuryl chloride, in chloroform medium, at room temperature and at a molar ratio between quinolone derivative and sulfuryl chloride 1 to 3.
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CN114456110A (en) * 2022-03-02 2022-05-10 重庆南松凯博生物制药有限公司 Synthesis method of 7-chloro-4-hydroxyquinoline-3-carboxylic acid

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114456110A (en) * 2022-03-02 2022-05-10 重庆南松凯博生物制药有限公司 Synthesis method of 7-chloro-4-hydroxyquinoline-3-carboxylic acid

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