DK154976B - Fremgangsmaade til fremstilling af 5-aroyl-1-laverealkylpyrrol-2-eddikesyrederivater - Google Patents
Fremgangsmaade til fremstilling af 5-aroyl-1-laverealkylpyrrol-2-eddikesyrederivater Download PDFInfo
- Publication number
- DK154976B DK154976B DK243676AA DK243676A DK154976B DK 154976 B DK154976 B DK 154976B DK 243676A A DK243676A A DK 243676AA DK 243676 A DK243676 A DK 243676A DK 154976 B DK154976 B DK 154976B
- Authority
- DK
- Denmark
- Prior art keywords
- pyrrole
- preparation
- lower alkyl
- ethyl
- acetate
- Prior art date
Links
- 238000000034 method Methods 0.000 title claims description 16
- GVUHUYQEAGMUNJ-UHFFFAOYSA-N 2-(1h-pyrrol-2-yl)acetic acid Chemical class OC(=O)CC1=CC=CN1 GVUHUYQEAGMUNJ-UHFFFAOYSA-N 0.000 title 1
- 238000006243 chemical reaction Methods 0.000 claims description 28
- -1 alkyl pyrrole-2-acetic acid derivatives Chemical class 0.000 claims description 26
- KAESVJOAVNADME-UHFFFAOYSA-N Pyrrole Chemical compound C=1C=CNC=1 KAESVJOAVNADME-UHFFFAOYSA-N 0.000 claims description 19
- 125000000217 alkyl group Chemical group 0.000 claims description 14
- 238000010992 reflux Methods 0.000 claims description 13
- ROSYAUHHRKAPHX-UHFFFAOYSA-N 2-(1-methylpyrrol-2-yl)acetonitrile Chemical compound CN1C=CC=C1CC#N ROSYAUHHRKAPHX-UHFFFAOYSA-N 0.000 claims description 10
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 9
- 239000003054 catalyst Substances 0.000 claims description 9
- 239000002904 solvent Substances 0.000 claims description 9
- NQUVCRCCRXRJCK-UHFFFAOYSA-N 4-methylbenzoyl chloride Chemical compound CC1=CC=C(C(Cl)=O)C=C1 NQUVCRCCRXRJCK-UHFFFAOYSA-N 0.000 claims description 8
- PISHKRUMARWBKY-UHFFFAOYSA-N ethyl 2-(1,4-dimethylpyrrol-2-yl)acetate Chemical compound CCOC(=O)CC1=CC(C)=CN1C PISHKRUMARWBKY-UHFFFAOYSA-N 0.000 claims description 6
- RKIDDEGICSMIJA-UHFFFAOYSA-N 4-chlorobenzoyl chloride Chemical compound ClC(=O)C1=CC=C(Cl)C=C1 RKIDDEGICSMIJA-UHFFFAOYSA-N 0.000 claims description 4
- 125000003545 alkoxy group Chemical group 0.000 claims description 4
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 claims description 4
- SKDHHIUENRGTHK-UHFFFAOYSA-N 4-nitrobenzoyl chloride Chemical compound [O-][N+](=O)C1=CC=C(C(Cl)=O)C=C1 SKDHHIUENRGTHK-UHFFFAOYSA-N 0.000 claims description 3
- PXRRXXGYCFSERC-UHFFFAOYSA-N ethyl 2-[1,4-dimethyl-5-(4-nitrobenzoyl)pyrrol-2-yl]acetate Chemical compound CN1C(CC(=O)OCC)=CC(C)=C1C(=O)C1=CC=C([N+]([O-])=O)C=C1 PXRRXXGYCFSERC-UHFFFAOYSA-N 0.000 claims description 3
- 229910052736 halogen Inorganic materials 0.000 claims description 3
- 150000002367 halogens Chemical class 0.000 claims description 3
- 125000001424 substituent group Chemical group 0.000 claims description 3
- 239000000010 aprotic solvent Substances 0.000 claims description 2
- 125000003118 aryl group Chemical group 0.000 claims description 2
- 125000006501 nitrophenyl group Chemical group 0.000 claims description 2
- 125000001544 thienyl group Chemical group 0.000 claims description 2
- 238000002360 preparation method Methods 0.000 claims 10
- CSCPPACGZOOCGX-UHFFFAOYSA-N acetone Substances CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims 2
- AGKFMUXEONTGAH-UHFFFAOYSA-N ethyl 2-[5-(4-chlorobenzoyl)-1,4-dimethylpyrrol-2-yl]acetate Chemical compound CN1C(CC(=O)OCC)=CC(C)=C1C(=O)C1=CC=C(Cl)C=C1 AGKFMUXEONTGAH-UHFFFAOYSA-N 0.000 claims 2
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims 1
- 101150046432 Tril gene Proteins 0.000 claims 1
- 150000004678 hydrides Chemical class 0.000 claims 1
- 239000000047 product Substances 0.000 description 10
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 9
- RFFLAFLAYFXFSW-UHFFFAOYSA-N 1,2-dichlorobenzene Chemical compound ClC1=CC=CC=C1Cl RFFLAFLAYFXFSW-UHFFFAOYSA-N 0.000 description 8
- YMWUJEATGCHHMB-UHFFFAOYSA-N Dichloromethane Chemical compound ClCCl YMWUJEATGCHHMB-UHFFFAOYSA-N 0.000 description 6
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 description 6
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 6
- 239000002243 precursor Substances 0.000 description 6
- 239000000243 solution Substances 0.000 description 6
- APSWAFZHMYVSMV-UHFFFAOYSA-N 2-[1-methyl-5-(4-methylbenzoyl)pyrrol-2-yl]acetonitrile Chemical compound C1=CC(C)=CC=C1C(=O)C1=CC=C(CC#N)N1C APSWAFZHMYVSMV-UHFFFAOYSA-N 0.000 description 5
- HEMHJVSKTPXQMS-UHFFFAOYSA-M sodium hydroxide Inorganic materials [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 5
- QPFMBZIOSGYJDE-UHFFFAOYSA-N 1,1,2,2-tetrachloroethane Chemical compound ClC(Cl)C(Cl)Cl QPFMBZIOSGYJDE-UHFFFAOYSA-N 0.000 description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- HEDRZPFGACZZDS-UHFFFAOYSA-N Chloroform Chemical compound ClC(Cl)Cl HEDRZPFGACZZDS-UHFFFAOYSA-N 0.000 description 4
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 4
- 238000005917 acylation reaction Methods 0.000 description 4
- 239000003795 chemical substances by application Substances 0.000 description 4
- 239000001257 hydrogen Substances 0.000 description 4
- 229910052739 hydrogen Inorganic materials 0.000 description 4
- 239000008096 xylene Substances 0.000 description 4
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 description 3
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- QGJOPFRUJISHPQ-UHFFFAOYSA-N Carbon disulfide Chemical compound S=C=S QGJOPFRUJISHPQ-UHFFFAOYSA-N 0.000 description 3
- 238000005727 Friedel-Crafts reaction Methods 0.000 description 3
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- 230000010933 acylation Effects 0.000 description 3
- 239000002585 base Substances 0.000 description 3
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- YLQBMQCUIZJEEH-UHFFFAOYSA-N Furan Chemical compound C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 2
- CSNNHWWHGAXBCP-UHFFFAOYSA-L Magnesium sulfate Chemical compound [Mg+2].[O-][S+2]([O-])([O-])[O-] CSNNHWWHGAXBCP-UHFFFAOYSA-L 0.000 description 2
- YTPLMLYBLZKORZ-UHFFFAOYSA-N Thiophene Chemical compound C=1C=CSC=1 YTPLMLYBLZKORZ-UHFFFAOYSA-N 0.000 description 2
- VSCWAEJMTAWNJL-UHFFFAOYSA-K aluminium trichloride Chemical compound Cl[Al](Cl)Cl VSCWAEJMTAWNJL-UHFFFAOYSA-K 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 150000004945 aromatic hydrocarbons Chemical class 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- MVPPADPHJFYWMZ-UHFFFAOYSA-N chlorobenzene Chemical compound ClC1=CC=CC=C1 MVPPADPHJFYWMZ-UHFFFAOYSA-N 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- JHIVVAPYMSGYDF-UHFFFAOYSA-N cyclohexanone Chemical compound O=C1CCCCC1 JHIVVAPYMSGYDF-UHFFFAOYSA-N 0.000 description 2
- SBZXBUIDTXKZTM-UHFFFAOYSA-N diglyme Chemical compound COCCOCCOC SBZXBUIDTXKZTM-UHFFFAOYSA-N 0.000 description 2
- 238000001914 filtration Methods 0.000 description 2
- 238000004817 gas chromatography Methods 0.000 description 2
- 125000001072 heteroaryl group Chemical group 0.000 description 2
- 239000011968 lewis acid catalyst Substances 0.000 description 2
- UAEPNZWRGJTJPN-UHFFFAOYSA-N methylcyclohexane Chemical compound CC1CCCCC1 UAEPNZWRGJTJPN-UHFFFAOYSA-N 0.000 description 2
- LQNUZADURLCDLV-UHFFFAOYSA-N nitrobenzene Chemical compound [O-][N+](=O)C1=CC=CC=C1 LQNUZADURLCDLV-UHFFFAOYSA-N 0.000 description 2
- 239000003960 organic solvent Substances 0.000 description 2
- HFPZCAJZSCWRBC-UHFFFAOYSA-N p-cymene Chemical compound CC(C)C1=CC=C(C)C=C1 HFPZCAJZSCWRBC-UHFFFAOYSA-N 0.000 description 2
- 150000003233 pyrroles Chemical class 0.000 description 2
- 230000009257 reactivity Effects 0.000 description 2
- OCJBOOLMMGQPQU-UHFFFAOYSA-N 1,4-dichlorobenzene Chemical compound ClC1=CC=C(Cl)C=C1 OCJBOOLMMGQPQU-UHFFFAOYSA-N 0.000 description 1
- HNAGHMKIPMKKBB-UHFFFAOYSA-N 1-benzylpyrrolidine-3-carboxamide Chemical compound C1C(C(=O)N)CCN1CC1=CC=CC=C1 HNAGHMKIPMKKBB-UHFFFAOYSA-N 0.000 description 1
- XCYJPXQACVEIOS-UHFFFAOYSA-N 1-isopropyl-3-methylbenzene Chemical compound CC(C)C1=CC=CC(C)=C1 XCYJPXQACVEIOS-UHFFFAOYSA-N 0.000 description 1
- JSZOAYXJRCEYSX-UHFFFAOYSA-N 1-nitropropane Chemical compound CCC[N+]([O-])=O JSZOAYXJRCEYSX-UHFFFAOYSA-N 0.000 description 1
- MKVATVUOVMCHJJ-UHFFFAOYSA-N 2-(1h-pyrrol-2-yl)acetonitrile Chemical compound N#CCC1=CC=CN1 MKVATVUOVMCHJJ-UHFFFAOYSA-N 0.000 description 1
- UMXKLXNZBXRMGD-UHFFFAOYSA-N 2-[4-(4-chlorobenzoyl)-1-methylpyrrol-2-yl]acetonitrile Chemical compound C1=C(CC#N)N(C)C=C1C(=O)C1=CC=C(Cl)C=C1 UMXKLXNZBXRMGD-UHFFFAOYSA-N 0.000 description 1
- GDRPXPPAYAOCIK-UHFFFAOYSA-N 2-[5-(4-chlorobenzoyl)-1-methylpyrrol-2-yl]acetonitrile Chemical compound CN1C(CC#N)=CC=C1C(=O)C1=CC=C(Cl)C=C1 GDRPXPPAYAOCIK-UHFFFAOYSA-N 0.000 description 1
- YHEAVHQIEBAMND-UHFFFAOYSA-N 2-methyl-2-(1h-pyrrol-2-yl)propanoic acid Chemical compound OC(=O)C(C)(C)C1=CC=CN1 YHEAVHQIEBAMND-UHFFFAOYSA-N 0.000 description 1
- VTXNOVCTHUBABW-UHFFFAOYSA-N 3,4-dichlorobenzoyl chloride Chemical compound ClC(=O)C1=CC=C(Cl)C(Cl)=C1 VTXNOVCTHUBABW-UHFFFAOYSA-N 0.000 description 1
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 description 1
- WKBOTKDWSSQWDR-UHFFFAOYSA-N Bromine atom Chemical compound [Br] WKBOTKDWSSQWDR-UHFFFAOYSA-N 0.000 description 1
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- 239000002841 Lewis acid Substances 0.000 description 1
- 238000005684 Liebig rearrangement reaction Methods 0.000 description 1
- 150000001422 N-substituted pyrroles Chemical class 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 229910003074 TiCl4 Inorganic materials 0.000 description 1
- 125000001931 aliphatic group Chemical group 0.000 description 1
- 150000001408 amides Chemical class 0.000 description 1
- 230000003110 anti-inflammatory effect Effects 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- AAMATCKFMHVIDO-UHFFFAOYSA-N azane;1h-pyrrole Chemical compound N.C=1C=CNC=1 AAMATCKFMHVIDO-UHFFFAOYSA-N 0.000 description 1
- JFDZBHWFFUWGJE-UHFFFAOYSA-N benzonitrile Chemical compound N#CC1=CC=CC=C1 JFDZBHWFFUWGJE-UHFFFAOYSA-N 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 239000012267 brine Substances 0.000 description 1
- GDTBXPJZTBHREO-UHFFFAOYSA-N bromine Substances BrBr GDTBXPJZTBHREO-UHFFFAOYSA-N 0.000 description 1
- 229910052794 bromium Inorganic materials 0.000 description 1
- OBNCKNCVKJNDBV-UHFFFAOYSA-N butanoic acid ethyl ester Natural products CCCC(=O)OCC OBNCKNCVKJNDBV-UHFFFAOYSA-N 0.000 description 1
- 125000000484 butyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 125000004432 carbon atom Chemical group C* 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000003610 charcoal Substances 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 150000004985 diamines Chemical class 0.000 description 1
- 229940117389 dichlorobenzene Drugs 0.000 description 1
- 238000007336 electrophilic substitution reaction Methods 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- 150000002170 ethers Chemical class 0.000 description 1
- BRYGWFXDNVBTDF-UHFFFAOYSA-N ethyl 2-[5-(3,4-dichlorobenzoyl)-1,4-dimethylpyrrol-2-yl]acetate Chemical compound CN1C(CC(=O)OCC)=CC(C)=C1C(=O)C1=CC=C(Cl)C(Cl)=C1 BRYGWFXDNVBTDF-UHFFFAOYSA-N 0.000 description 1
- 230000007717 exclusion Effects 0.000 description 1
- 239000000706 filtrate Substances 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 125000005842 heteroatom Chemical group 0.000 description 1
- 150000002391 heterocyclic compounds Chemical class 0.000 description 1
- 150000002430 hydrocarbons Chemical group 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 239000011630 iodine Substances 0.000 description 1
- 229910052740 iodine Inorganic materials 0.000 description 1
- 125000001449 isopropyl group Chemical group [H]C([H])([H])C([H])(*)C([H])([H])[H] 0.000 description 1
- 150000002576 ketones Chemical class 0.000 description 1
- 150000007517 lewis acids Chemical class 0.000 description 1
- 229910052943 magnesium sulfate Inorganic materials 0.000 description 1
- 235000019341 magnesium sulphate Nutrition 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 125000000956 methoxy group Chemical group [H]C([H])([H])O* 0.000 description 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 1
- GYNNXHKOJHMOHS-UHFFFAOYSA-N methyl-cycloheptane Natural products CC1CCCCCC1 GYNNXHKOJHMOHS-UHFFFAOYSA-N 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 150000002825 nitriles Chemical class 0.000 description 1
- 125000004971 nitroalkyl group Chemical group 0.000 description 1
- 125000004433 nitrogen atom Chemical group N* 0.000 description 1
- TVMXDCGIABBOFY-UHFFFAOYSA-N octane Chemical compound CCCCCCCC TVMXDCGIABBOFY-UHFFFAOYSA-N 0.000 description 1
- 239000012044 organic layer Substances 0.000 description 1
- 125000005440 p-toluyl group Chemical group [H]C1=C([H])C(=C([H])C([H])=C1C(*)=O)C([H])([H])[H] 0.000 description 1
- 125000001147 pentyl group Chemical group C(CCCC)* 0.000 description 1
- 238000006116 polymerization reaction Methods 0.000 description 1
- TYJJADVDDVDEDZ-UHFFFAOYSA-M potassium hydrogencarbonate Chemical compound [K+].OC([O-])=O TYJJADVDDVDEDZ-UHFFFAOYSA-M 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 239000011541 reaction mixture Substances 0.000 description 1
- 239000012048 reactive intermediate Substances 0.000 description 1
- 238000001953 recrystallisation Methods 0.000 description 1
- 229930195734 saturated hydrocarbon Natural products 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- HPALAKNZSZLMCH-UHFFFAOYSA-M sodium;chloride;hydrate Chemical compound O.[Na+].[Cl-] HPALAKNZSZLMCH-UHFFFAOYSA-M 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 229930192474 thiophene Natural products 0.000 description 1
- XJDNKRIXUMDJCW-UHFFFAOYSA-J titanium tetrachloride Chemical compound Cl[Ti](Cl)(Cl)Cl XJDNKRIXUMDJCW-UHFFFAOYSA-J 0.000 description 1
- XFNJVJPLKCPIBV-UHFFFAOYSA-N trimethylenediamine Chemical compound NCCCN XFNJVJPLKCPIBV-UHFFFAOYSA-N 0.000 description 1
- 239000011592 zinc chloride Substances 0.000 description 1
- 235000005074 zinc chloride Nutrition 0.000 description 1
- JIAARYAFYJHUJI-UHFFFAOYSA-L zinc dichloride Chemical compound [Cl-].[Cl-].[Zn+2] JIAARYAFYJHUJI-UHFFFAOYSA-L 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07D—HETEROCYCLIC COMPOUNDS
- C07D207/00—Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom
- C07D207/02—Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom with only hydrogen or carbon atoms directly attached to the ring nitrogen atom
- C07D207/30—Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having two double bonds between ring members or between ring members and non-ring members
- C07D207/32—Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having two double bonds between ring members or between ring members and non-ring members with only hydrogen atoms, hydrocarbon or substituted hydrocarbon radicals, directly attached to ring carbon atoms
- C07D207/33—Heterocyclic compounds containing five-membered rings not condensed with other rings, with one nitrogen atom as the only ring hetero atom with only hydrogen or carbon atoms directly attached to the ring nitrogen atom having two double bonds between ring members or between ring members and non-ring members with only hydrogen atoms, hydrocarbon or substituted hydrocarbon radicals, directly attached to ring carbon atoms with substituted hydrocarbon radicals, directly attached to ring carbon atoms
- C07D207/337—Radicals substituted by carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61P—SPECIFIC THERAPEUTIC ACTIVITY OF CHEMICAL COMPOUNDS OR MEDICINAL PREPARATIONS
- A61P29/00—Non-central analgesic, antipyretic or antiinflammatory agents, e.g. antirheumatic agents; Non-steroidal antiinflammatory drugs [NSAID]
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Life Sciences & Earth Sciences (AREA)
- General Chemical & Material Sciences (AREA)
- Medicinal Chemistry (AREA)
- Nuclear Medicine, Radiotherapy & Molecular Imaging (AREA)
- Pain & Pain Management (AREA)
- Pharmacology & Pharmacy (AREA)
- Rheumatology (AREA)
- Animal Behavior & Ethology (AREA)
- General Health & Medical Sciences (AREA)
- Public Health (AREA)
- Veterinary Medicine (AREA)
- Pyrrole Compounds (AREA)
- Plural Heterocyclic Compounds (AREA)
- Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)
Description
i
DK 154976 B
Ved forsøg på at aroylere N-substituerede pyrrol er i a-sti11 ingen stødes der på adskillige eksperimentelle problemer, som forhindrer, at h'øje udbytter opnås. Et sådant problem angår den resulterende a- og β-isomerfordeling af aroylerede produkter. Det er velkendt, at elektrofilt 5 angreb indtræffer mere ubesværet ved a- end ved ^-stillingen i hetero-aromatiske 5-ledede ringe med et heteroatom. Blandt sådanne hetero-cykliske forbindelser er pyrroler imidlertid blevet angivet som givende det ringeste forhold af or-isomer til β-isomer ved elektrofile substitutionsreaktioner (furan >thiophen »pyrrol) [se Int. J. Sulfur Chem., 10 C, 7, 64 (1972)].
Et andet problem angår anvendelsen af acyleringskatalysatorer. Koordinering af pyrrolnitrogenet med Lewis-syrer, som almindeligvis anvendes som katalysatorer ved en reaktion af Friedel-Crafts-typen, hæmmer reaktionen. Ydermere kan anvendelse af stærkere Lewis-syrekatalysatorer, 15 såsom aluminiumchlorid, inducere polymerisation af pyrroler. Mens eksempler på ukatalyserede acyleringer af N-substituerede pyrroler med alifatiske acyleringsmidler er kendte [se f.eks. Ber. 47, 2427 (1910);
Liebigs Ann. Chem., 721, 105 (1969)] er deres reaktion med aromatiske acyleringsmidler i fravær af katalysator ikke blevet rapporteret.
20 Aroylering af N-usubstituerede pyrroler er blevet gennemført under anvendelse af baser [se f.eks. Liebigs. Ann. Chem., 724, 137 (1969 og 733.
27 (1970)]. Basen virker ved at ekstrahere en proton fra ringnitrogenet, og ved sådanne reaktioner er pyrrolanionen det reaktive mellemprodukt.
Denne type af reaktivitet er imidlertid ikke mulig, når nitrogenatomet 25 bærer en substituent.
Aroyleringen af 1-al kyl pyrrol-2-eddikesyrederivater gennem en reaktion af Friedel-Crafts-typen med AlCl^-katalysator er blevet beskrevet i USA patentskrift nr. 3.752.826. Lave udbytter og dannelse af væsentlige mængder af den uønskede Ø-isomer er imidlertid typiske for denne 30 reaktion [se J. Med. Chem., 14» nr. 7. 647 (1971)].
Den ikke-katalyserede fremgangsmåde ifølge opfindelsen udgør en forbedring i forhold til de konventionelle katalyserede fremgangsmåder ved fremstilling af de a-aroylerede pyrroler med formel (I). Der opnås ikke blot økonomiske besparelser ved udeladelse af katalysatoren, men 35 der opnås også forbedrede udbytter af produkt (I), som i alt væsentligt er fri for de tilsvarende β-aroylisomere.
Den foreliggende opfindelse tilvejebringer en særlig fremgangsmåde til fremstilling af 5-aroyl-l-lavere al kyl pyrrol-2-eddikesyrederivater 2
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med den almene formel
5 TIL
ArCO-k (I) N £ I -
R
10 hvori R betegner lavere al kyl, R* betegner hydrogen eller lavere al kyl, Z betegner CN eller C00 (lavere al kyl), og Ar betegner phenyl, thienyl, 15 nitrophenyl, methylthiophenyl, trifluormethylphenyl eller phenyl substitueret med fra en til tre substituenter, som individuelt betegner lavere al kyl, lavere alkoxy eller halogen.
En del af forbindelserne er kendt fra USA patentskrift nr.
3.752.826. Forbindelserne er i besiddelse af anti-inflammatorisk aktivi-20 tet.
Som anvendt heri kan "lavere al kyl" og "lavere alkoxy" være lige-kædede eller forgrenede mættede carbonhydridgrupper med fra 1 til 5 car-bonatomer, såsom f.eks. methyl, ethyl, propyl, isopropyl, butyl, pentyl og lignende alkylgrupper og de tilsvarende alkoxygrupper, såsom methoxy,.
25 ethoxy, isopropoxy, etc., og betegnelsen halogen er generisk for chlor, brom, fluor og iod.
Fremgangsmåden ifølge opfindelsen er ejendommelig ved det i krav l's kendetegnende del angivne.
Ifølge opfindelsen anvendes et aroylchlorid med formlen (II), hvori 30 Ar har den tidligere anførte betydning, som acyleringsmiddel ved omsætning med et 1-lavere alkylpyrrol-4-R*-2-eddikesyrederivat med formlen (III), hvori R, R* og Z har de tidligere anførte betydninger, i et aprot organisk opløsningsmiddel under fravær af katalysator ved en temperatur, som er tilstrækkelig til at få aroyleringen til at skride frem med en 35 bekvem hastighed.
3
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R1 R·?- 5 n Jn
ArCOCl + JJ-CH-Z -> ArCO-S^ >*"CH_-Z
Ψ 2 N 2 I i
R R
(II)· (III) (I) 10
Typiske anvendelige aprote opløsningsmidler er aromatiske carbon-hydrider, såsom benzen, toluen, xylen, p-cymen og lignende, substituere-15 de aromatiske carbonhydrider, såsom chlorbenzen, dichlorbenzen, nitrobenzen, benzoenitril, og lignende, paraffiner, såsom methylcyclohexan, octan og lignende, halogencarbonforbindel ser, såsom methylenchlorid, chloroform, tetrachlorethan, tetrachlorethyl en og lignende, ethere, såsom diethylether, diglyme og lignende, ketoner, såsom methylethylke-20 ton, cyclohexanon og lignende, estere, såsom ethylbutyrat og lignende, nitroalkaner, såsom nitropropan og lignende, carbondisulfid og lignende.
Reaktionstemperaturen afhænger af reaktiviteterne af aroylchloridet (II) og af den særlige pyrrolprækursor (III). For de pyrrolprækursorer, hvori R1 betegner lavere al kyl, og Z betegner C00(lavere al kyl), vil 25 aroyleringen f.eks. forløbe fyldestgørende ved omgivelsestemperatur (20-27°C), skønt forhøjede temperaturer op til opløsningsmidlets tilbagesvalingstemperatur kan anvendes til forøgelse af reaktionshastigheden. De pyrrolprækursorer, hvori R* betegner hydrogen, og Z betegner C00(lavere alkyl) kan aroyleres med en bekvem reaktionshastighed ved 30 temperaturer i området fra 50-250eC og for de pyrrolprækursorer, hvori R* betegner hydrogen, og Z betegner CN, vil en bekvem reaktionshastighed findes i området fra 80-300°C. α-aroyleringsreaktionerne ifølge opfindelsen gennemføres fortrinsvis ved en temperatur på mindst 50°C og op til højere tilbagesvalingstemperaturer i afhængighed af det særlige op-35 løsningsmiddel, der anvendes.
Reaktionen kan gennemføres under anvendelse af i det væsentlige ækvivalente mængder af reaktanter (II) og (III), skønt et overskud af acyleringsmidlet (II) kan anvendes til sikring af fuldførelse af reak- 4
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tionen. I sådanne tilfælde, hvor residualt aroylchlorid stadig er til stede ved afslutning af reaktionen kan standardreagenser anvendes, såsom f.eks. en base, såsom et al kalimetal hydroxid, f.eks. natrium- eller kaliumhydroxid eller en diamin, f.eks. Ν,Ν-dimethylaminopropylamin til 5 omsætning med det overskydende aroylchlorid og til lettelse af dets adskillelse fra det ønskede produkt (I).
Den ukatalyserede aroyleringsfremgangsmåde ifølge opfindelsen giver overraskende bedre udbytter af produktet, 4-R*-l-lavere alkyl-5-aroyl-pyrrol-2-eddikesyreester eller -nitril. Når betegner hydrogen, for-10 skydes det sædvanlige α til ^-forhold af produktet ved acyleringsreak-tioner, dvs. fordelingen af α-aroylerede og /}-aroylerede isomere desuden i meget høj grad til begunstigelse af det α-substituerede produkt.
F.eks. opnås der ved den AlClg-katalyserede Friedel-Crafts-reaktion af p-chlorbenzoylchlorid med l-methylpyrrol-2-acetonitril et udbytte på 21% 15 af tt-produktet, 5-(p-chlorbenzoyl)-l-methyl-pyrrol-2-acetonitril, og forholdet af denne α-isomer til den tilsvarende /Msomer, 4-(p-chlorben-zoyl)-1-methylpyrrol-2-acetonitril, er ca. 2,5:1, og i den på lignende måde katalyserede reaktion af p-toluoylchlorid med 1-methylpyrrol-2-ace-tonitril opnås et udbytte på 25% af α-produktet, 5-(p-toluoyl)-l-methyl-20 pyrrol-2-acetonitri 1, med et a- til /Msomerforhold på 3,7:1 [se Carson et al., Med. Chem., 14, 646 (1971)]. I modsætning hertil giver den ukatalyserede omsætning af p-chlorbenzoylchlorid med 1-methylpyrrol-2-acetonitril i til bagesval ende xylen i ca. 24 timer 46% af det tilsvarende α-produkt med et a/Ø-forhold på ca. 440:1, og den ukatalyserede om-25 sætning af p-toluoylchlorid med l-methylpyrrol-2-acetonitril i tilbagesval ende o-dichlorbenzen i ca. 4 timer giver 55% af det tilsvarende a-produkt med et a//J-forhold på ca. 180:1.
I modsætning til rapporterede acyleringer af visse andre heteroaro-matiske substrater under anvendelse af Lewis-syrekatalysatorer [se 30 f.eks. Synthesis, Oct., 1972, s. 533; og J. Am. Chem. Soc., 69, 1012 (1947)] formindsker tilsætningen af små mængder af sådanne katalysatorer ligefrem aroyleringshastigheden for de omhandlede pyrrolprækursorer (III), som vist i eksempel 3.
Opfindelsen illustreres nærmere i de efterfølgende eksempler. Med 35 mindre andet er anført er alle dele på vægtbasis.
5
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Eksempel 1 1-methyl-5-fi-toluoylpyrrol-2-acetonitri 1.
En opløsning af 11,5 g (0,075 mol) p-toluoylchlorid og 6,0 g (0,05 5 mol) 1-methylpyrrol-2-acetonitril i 30 ml toluen opvarmes under tilbagesvaling i 68 timer. Reaktionsblandingen køles dernæst, hældes i en vandig opløsning af Ν,Ν-dimethylaminopropylamin og fortyndes med chloroform. Det organiske lag fraskilles, vaskes successivt med fortyndet saltsyre og saltvand, tørres (MgSO^), behandles med trækul, og opløs-10 ningsmidlet afdampes i vakuum. Remanensen omkrystalliseres med methanol til frembringelse af 5,8 g (49% udbytte) af et brunligt faststof, 1-methyl-5-p-toluoylpyrrol-2-acetonitril, smeltepunkt 103-105eC. Der fremstilles ingen betydende mængde af den tilsvarende 4-isomer.
15 Eksempel 2
Opløsninger af 7,0 g (0,045 mol) p-toluoylchlorid og 3,6 g (0,029 mol) N-methylpyrrol-2-acetonitril opvarmes under tilbagesvaling i 20 ml af hvert af de nedenfor angivne opløsningsmidler. De indledende omsætningshastigheder påvises efter 6 timer ved hjælp af gaskromatografi. De 20 procentuelle omdannelser til l-methyl-5-p-toluoylpyrrol-2-acetonitril vises i tabellen.
Opløsningsmiddel Omdannelse. % 25 o-dichlorbenzen, kogepunkt 180®C 54 1,1,2,2-tetrachlorethan, kgp. 146°C 37 p-cymen, kgp. 177°C 32 xylen, - 140°C 16 diglyme, - 161eC 30 30
Eksempel 3
Opløsninger af 7,0 g (0,045 mol) p-toluoylchlorid og 3,6 g (0,029 mol) N-methylpyrrol-2-acetonitril i 20 ml o-dichlorbenzen opvarmes under tilbagesvaling med 1% af hver af de nedenfor anførte katalysatorer.
35 Efter 6 timer påvises de indledende omsætningshastigheder ved hjælp af gaskromatografi. Den procentuelle omdannelse til l-methyl-5-p-toluoyl-pyrrol-2-acetonitril vises i tabellen.
6
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Katal vsator Omdannelse, % ingen 54
FeCL 35 5 I2 16
ZnCl2 20
TiCl4 20
SnCl4 25 10 Eksempel 4
En opløsning af 30 g l-methylpyrrol-2-acetonitril og 60 g p-toluoylchlorid i 200 ml o-dichlorbenzen tilbagesvales under nitrogen i 4=' timer. Blandingen koncentreres til næsten tørhed, fortyndes med 250 ml methylenchlorid, vaskes successivt med en vandig opløsning af dimethyl -15 aminopropylamin, fortyndet saltsyre og kaliumcarbonatopløsning.
Fjernelse af det organiske opløsningsmiddel efterlader en olieagtig remanens, som omkrystalliseres i 80 ml methanol til frembringelse af 22,2’ , g (39%) 1-methyl-5-(p-toluoyl)-pyrrol-2-acetonitri1. Methanol filtratet koncentreres, og den tiloversblevne olie hydrolyseres til amidet ved 20 kortvarig tilbagesvaling med vandig ethanolisk NaOH (10%). Det udskilte faste stof opsamles og giver 10,1 g (16,4%) 1-methyl-5-(p-toluoyl)-pyrrol -2-acetamid. Totalt udbytte = 55,4%.
Eksempel 5 25 Ethvl-1.4-dimethvl-5-fp-nitrobenzovlIpvrrol-2-acetat:
En opløsning af 7,24 g (0,04 mol) ethyl-1,4-dimethylpyrrol-2-acetat og 11,1 g (0,06 mol) p-nitrobenzoylchlorid i 30 ml ether under argon omrøres ved stuetemperatur og i mørke i 2 dage. Bundfaldet opsamles ved filtrering. Omkrystallisering fra isopropanol giver 11,2 g (85% udbytte) , 30 ethyl-1,4-dimethyl-5-(p-nitrobenzoyl)pyrrol-2-acetat som gule krystaller, smeltepunkt 148-149eC.
Eksempel 6
Ethvl-5-(3.4-di chlorbenzovl1-1,4-di methvlpyrrol-2-acetat: 35 En opløsning af 3,6 g ethyl-1,4-dimethylpyrrol-2-acetat og 8,3 g 3,4-dichlorbenzoylchlorid i 20 ml xylen tilbagesvales i 40 minutter og afkøles dernæst. Det udskilte faste stof opsamles ved filtrering og tørres til frembringelse af 5,6 g (80%) ethyl-5-(3,4-dichlorbenzoyl)-l,4- 7
DK 154976 B
dimethylpyrrol-2-acetat som hvide krystaller, smeltepunkt 92-93,5°C.
Eksempel 7
En sammenligning af katalyserede og ikke-katalyserede aroyleringer 5 under anvendelse af de angivne forhold mellem aroylchlorider (II) og pyrrolprækursorer (III) under de viste betingelser anføres i tabel I nedenfor.
8
DK 154976 B
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Claims (11)
1. Fremgangsmåde til fremstilling af 5-aroyl-l-lavere al kyl pyrrol -2-eddikesyrederivater med den almene formel 5 R1 ΓΊ ArCO-'x CH2-Z 10 i- R hvori R betegner lavere al kyl, R1 betegner hydrogen eller lavere al kyl, 15. betegner CN eller C00(lavere al kyl), og Ar betegner phenyl, thienyl, nitrophenyl, methyl thiophenyl, trifluormethylphenyl eller phenyl substitueret med fra 1 til 3 substitutenter, som individuelt betegner lavere al kyl, lavere alkoxy eller halogen ved hvilken et aroylchlorid med formlen: 20 ArCOCl hvori Ar har den ovenfor anførte betydning, omsættes med en pyrrol med formi en: 25 Ri Γ71 ^ >*-CH -Z • N *
30 R hvori R, R* og Z har den ovenfor anførte betydning, i et aprot opløsningsmiddel, kendetegnet ved, at omsætningen foretages i fravær af katalysator.
2. Fremgangsmåde ifølge krav 1 k e n d e t e g n e t ved, at om sætningen foretages ved en temperatur fra 50°C til opløsningsmidlets ti 1 bagesval i ngstemperatur.
3. Fremgangsmåde ifølge krav 1 til fremstilling af 5-aroyl-l- DK 154976 B lavere al kylpyrrol-2-eddi kesyreestre med den almene formel: (lavere al kyl) 5 _ Arco ^J— ch2coo (] avere al kyl) 10 (lavere al kyl) hvori Ar har den ovenfor anførte betydning kendetegnet ved, at omsætningen foretages ved en temperatur fra omgi vel sestemperatur til opløsn i ngsmi dlets til bagesval i ngstemperatur.
4. Fremgangsmåde ifølge krav 1 til fremstilling af 5-aroyl-l- lavere al kyl pyrrol-2-eddikesyreestre med den almene formel: 20 rn ArCO-^ y)— ch~-coo (lavere al kyl) N * (lavere al kyl) 25 hvori Ar har den ovenfor anførte betydning, kendetegnet ved, at omsætningen foretages ved 50-250T.
5. Fremgangsmåde ifølge krav 1 til fremstilling af 5-aroyl-l-lavere al kyl pyrrol-2-eddikesyrenitri ler med den almene formel: 30 JTT ArCO*^ n/l-· ch -CN 35 I (lavere al kyl) DK 154976 B hvori Ar har den ovenfor anførte betydning, kendetegnet ved, at omsætningen foretages ved 80-300eC.
6. Fremgangsmåde ifølge krav 1 til fremstilling af 1-methyl-5-p-tol uoyl pyrrol-2-acetoni tril, kendetegnet ved, at p-toluoyl- 5 chlorid omsættes med 1-methylpyrrol-2-acetonitril ved 80-300eC.
7. Fremgangsmåde ifølge krav 1 til fremstilling af 1-methyl-5-p-tol uoyl pyrrol-2-acetoni tri 1, kendetegnet ved, at p-toluoyl-chlorid omsættes med 1-methylpyrrol-2-acetonitril i et aromatisk carbon-hydridopløsningsmiddel under tilbagesvaling.
8. Fremgangsmåde ifølge krav 1 til fremstilling af ethyl-l,4-di- methyl-5-(p-nitrobenzoyl) pyrrol-2-acetat, kendetegnet ved, at p-nitrobenzoylchlorid omsættes med ethyl-1,4-dimethylpyrrol-2-acetat ved en temperatur fra omgivelsestemperatur til opløsningsmidlets ti 1 bagesval i ngstemperatur.
9. Fremgangsmåde ifølge krav 1 til fremstilling af ethyl-1,4-di- methyl-5-(p-nitrobenzoyl)pyrrol-2-acetat, kendetegnet ved, at p-nitrobenzoylchlorid omsættes med ethyl-1,4-dimethylpyrrol-2-acetat i ether ved omgivelsestemperatur.
10. Fremgangsmåde ifølge krav 1 til fremstilling af ethyl-5-p- 20 chlorbenzoyl-l,4-dimethylpyrrol-2-acetat, kendetegnet ved, at p-chlorbenzoylchlorid omsættes med ethyl-l,4-dimethylpyrrol-2-acetat ved en temperatur fra omgivelsestemperatur til opløsningsmidlets tilbagesvalingstemperatur.
11. Fremgangsmåde ifølge krav 1 til fremstilling af ethyl-5-p- 25 chlorbenzoyl-l,4-dimethylpyrrol-2-acetat, kendetegnet ved, at p-chlorbenzoylchlorid omsættes med ethyl-1,4-dimethylpyrrol-2-acetat i ether ved omgivelsestemperatur. 30 35
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| US58306575 | 1975-06-02 | ||
| US05/583,065 US3998844A (en) | 1975-06-02 | 1975-06-02 | Uncatalyzed aroylation of 1-alkylpyrrole-2-acetic acid derivatives |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4048191A (en) * | 1975-06-27 | 1977-09-13 | Mcneil Laboratories, Incorporated | Halo-substituted 1-loweralkyl-5-aroylpyrrole-2-acetic acid compounds |
| US4207237A (en) * | 1977-04-20 | 1980-06-10 | Mcneilab, Inc. | Preparation of pyrrole-2-acetates |
| US4200645A (en) * | 1977-05-10 | 1980-04-29 | Beecham Group Limited | Pyrrole derivatives |
| US4119639A (en) * | 1977-06-27 | 1978-10-10 | Mcneil Laboratories, Incorporated | Preparation of 5-aroylpyrrole-2-acetic acid derivatives |
| GB1592996A (en) * | 1977-10-10 | 1981-07-15 | Rolland Sa A | Acylated pyrrole carboxylic acids and derivatives thereof |
| JPS5481264A (en) * | 1977-12-08 | 1979-06-28 | Sagami Chem Res Center | Preparation of 1-methyl-5-aroylpryrrole-2-acetic acid |
| SE435278B (sv) * | 1977-12-08 | 1984-09-17 | Sagami Chem Res | 5-cyano-1-legre(c?711?71-?714)alkyl-pyrrol-2-ettiksyra, framstellning derav och anvendningen som mellanprodukt vid framstellning av terapeutiskt verksamma pyrrolderivat |
| US4216150A (en) * | 1978-10-16 | 1980-08-05 | Mcneil Lab, Inc. | Preparation of pyrrole-2-acetates |
| US4213905A (en) * | 1979-06-25 | 1980-07-22 | Mcneilab, Inc. | Preparation of 5-aroyl-1-loweralkylpyrrole-2-acetic acid salts |
| US4284562A (en) * | 1979-11-27 | 1981-08-18 | Mcneilab, Inc. | Process for preparing pyrrole-2-acetic acids |
| US4255335A (en) * | 1980-04-03 | 1981-03-10 | Mcneilab, Inc. | Preparation of 5-aroyl-1-loweralkylpyrrole-2-acetic acid derivatives |
| US4299770A (en) * | 1980-05-29 | 1981-11-10 | Mallinckrodt, Inc. | Recovery of substituted pyrrole acetate |
| FI77022C (fi) * | 1981-08-10 | 1989-01-10 | Merck & Co Inc | Foerfarande foer framstaellning av nya terapeutiskt anvaendbara pyrrolaettiksyraderivat. |
| US5418236A (en) * | 1993-12-23 | 1995-05-23 | Ortho Pharmaceutical Corporation | Anxiolytic aroyl piperidinyl and piperazinylacyl pyrroles |
| US6441194B1 (en) | 1999-10-21 | 2002-08-27 | Emory University | Synthesis of 4-substituted pyrrole-2-carbaldehyde compounds |
Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3752826A (en) * | 1970-01-26 | 1973-08-14 | Mcneilab Inc | Aroyl substituted pyrroles |
| US3846447A (en) * | 1972-08-03 | 1974-11-05 | Mcneilab Inc | Preparation of 5-aroyl-pyrroles and intermediates therefor |
-
1975
- 1975-06-02 US US05/583,065 patent/US3998844A/en not_active Expired - Lifetime
-
1976
- 1976-05-05 NZ NZ180785A patent/NZ180785A/xx unknown
- 1976-05-05 IN IN783/CAL/76A patent/IN141746B/en unknown
- 1976-05-10 GB GB1907276A patent/GB1477998A/en not_active Expired
- 1976-05-14 FR FR7614686A patent/FR2313364A1/fr active Granted
- 1976-05-28 AU AU14405/76A patent/AU497557B2/en not_active Expired
- 1976-05-31 CA CA253,677A patent/CA1066297A/en not_active Expired
- 1976-05-31 RO RO7686309A patent/RO69252A/ro unknown
- 1976-05-31 PT PT65161A patent/PT65161B/pt unknown
- 1976-05-31 ES ES448408A patent/ES448408A1/es not_active Expired
- 1976-05-31 JP JP51062478A patent/JPS5919536B2/ja not_active Expired
- 1976-05-31 IL IL49687A patent/IL49687A/xx unknown
- 1976-06-01 AT AT401476A patent/AT358572B/de not_active IP Right Cessation
- 1976-06-01 CH CH689476A patent/CH603578A5/xx not_active IP Right Cessation
- 1976-06-01 SE SE7606165A patent/SE414765B/xx unknown
- 1976-06-01 DE DE2624557A patent/DE2624557C2/de not_active Expired
- 1976-06-01 DE DE19762624558 patent/DE2624558A1/de not_active Withdrawn
- 1976-06-01 BE BE167534A patent/BE842458A/xx not_active IP Right Cessation
- 1976-06-01 ZA ZA00763191A patent/ZA763191B/xx unknown
- 1976-06-02 YU YU1360/76A patent/YU40648B/xx unknown
- 1976-06-02 CS CS763662A patent/CS220310B2/cs unknown
- 1976-06-02 NL NL7605958A patent/NL7605958A/xx not_active Application Discontinuation
- 1976-06-02 DK DK243676A patent/DK154976C/da active
- 1976-06-02 PL PL1976190059A patent/PL101700B1/pl unknown
- 1976-06-02 HU HU76ME00001986A patent/HU172047B/hu unknown
Also Published As
| Publication number | Publication date |
|---|---|
| BE842458A (fr) | 1976-12-01 |
| YU40648B (en) | 1986-04-30 |
| JPS5919536B2 (ja) | 1984-05-07 |
| FR2313364B1 (da) | 1980-09-12 |
| US3998844A (en) | 1976-12-27 |
| HU172047B (hu) | 1978-05-28 |
| CH603578A5 (da) | 1978-08-31 |
| ATA401476A (de) | 1980-02-15 |
| ES448408A1 (es) | 1977-11-16 |
| AU1440576A (en) | 1977-12-01 |
| PL101700B1 (pl) | 1979-01-31 |
| ZA763191B (en) | 1978-01-25 |
| GB1477998A (en) | 1977-06-29 |
| PT65161B (en) | 1978-07-03 |
| AT358572B (de) | 1980-09-25 |
| NZ180785A (en) | 1978-03-06 |
| NL7605958A (nl) | 1976-12-06 |
| JPS51143664A (en) | 1976-12-10 |
| PT65161A (en) | 1976-06-01 |
| RO69252A (ro) | 1981-08-30 |
| IN141746B (da) | 1977-04-09 |
| YU136076A (en) | 1982-05-31 |
| CS220310B2 (en) | 1983-03-25 |
| DE2624557A1 (de) | 1976-12-23 |
| DE2624557C2 (de) | 1984-04-05 |
| AU497557B2 (en) | 1978-12-14 |
| FR2313364A1 (fr) | 1976-12-31 |
| IL49687A0 (en) | 1976-07-30 |
| DK243676A (da) | 1976-12-03 |
| CA1066297A (en) | 1979-11-13 |
| SE414765B (sv) | 1980-08-18 |
| DK154976C (da) | 1989-06-05 |
| SE7606165L (sv) | 1976-12-03 |
| DE2624558A1 (de) | 1976-12-23 |
| IL49687A (en) | 1978-10-31 |
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