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NO791576L - THIOL DERIVATIVES OF IMIDAZOLE - Google Patents

THIOL DERIVATIVES OF IMIDAZOLE

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Publication number
NO791576L
NO791576L NO791576A NO791576A NO791576L NO 791576 L NO791576 L NO 791576L NO 791576 A NO791576 A NO 791576A NO 791576 A NO791576 A NO 791576A NO 791576 L NO791576 L NO 791576L
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NO
Norway
Prior art keywords
imidazole
accordance
formula
methylenethiol
salts
Prior art date
Application number
NO791576A
Other languages
Norwegian (no)
Inventor
Franjo Kajfez
Original Assignee
Crc Ricerca Chim
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Crc Ricerca Chim filed Critical Crc Ricerca Chim
Publication of NO791576L publication Critical patent/NO791576L/en

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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D233/00Heterocyclic compounds containing 1,3-diazole or hydrogenated 1,3-diazole rings, not condensed with other rings
    • C07D233/54Heterocyclic compounds containing 1,3-diazole or hydrogenated 1,3-diazole rings, not condensed with other rings having two double bonds between ring members or between ring members and non-ring members
    • C07D233/64Heterocyclic compounds containing 1,3-diazole or hydrogenated 1,3-diazole rings, not condensed with other rings having two double bonds between ring members or between ring members and non-ring members with substituted hydrocarbon radicals attached to ring carbon atoms, e.g. histidine

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)
  • Plural Heterocyclic Compounds (AREA)
  • Nitrogen And Oxygen Or Sulfur-Condensed Heterocyclic Ring Systems (AREA)
  • Cephalosporin Compounds (AREA)
  • Nitrogen Condensed Heterocyclic Rings (AREA)

Description

Tiolderivater av imidazol samt frem-Thiol derivatives of imidazole as well as

gangsmåte til fremstilling av samme.procedure for manufacturing the same.

Den foreliggende oppfinnelse vedrører tiolderivater av imidazol, og deres salter med organiske og uorganiske syrer. The present invention relates to thiol derivatives of imidazole, and their salts with organic and inorganic acids.

Oppfinnelsen vedrører også en fremgangsmåte til fremstilling av samme. The invention also relates to a method for producing the same.

Derivatene kjennetegnes ved at de har formelenThe derivatives are characterized by having the formula

hvor R er en alkylrest med høyst 4 karbonatomer i kjeden. where R is an alkyl residue with no more than 4 carbon atoms in the chain.

Fremgangsmåten ifølge oppfinnelsen kjennetegnes ved at forbindelser med formelen hvor R har samme betydning som i formelen I og X er et halogen-atom, omsettes med et surt sulfid med den generelle formel MeHS, hvor Me er Na, K, Ca, Ba, Sr, Mg eller NH4- Det kan også anvendes andre sure sulfider, men disse er for tiden økonomisk ikke av interesse, noe som begrenser deres anvendelse. Idet praktisk talt alle sure sulfider er løselige i lavere alkoholer, som også forbindelsene med den generelle .formel II er løselige i, arbeides det fortrinnsvis i absolutt metanol, etanol eller propanol. Andre alkoholer, som f.eks. isopropanol, amylalkohol eller allylalkohol, kan også anvendes. Utbyttet er imidlertid generelt fra 10 til 15% lavere enn ved anvendelse av metanol eller etanol. Andre løsnings-midler, som f.eks. dimetylsulfoksyd (DMSO), er ikke gunstige idet disse enten virker oksydative eller løser betydelige mengder oksygen fra luften, noe som kan føre til dannelse av disulfider. The method according to the invention is characterized by the fact that compounds with the formula where R has the same meaning as in formula I and X is a halogen atom are reacted with an acidic sulphide of the general formula MeHS, where Me is Na, K, Ca, Ba, Sr, Mg or NH4- Other acid sulphides can also be used, but these are currently economically not of interest, which limits their use. As practically all acid sulphides are soluble in lower alcohols, in which the compounds of the general formula II are also soluble, the work is preferably carried out in absolute methanol, ethanol or propanol. Other alcohols, such as isopropanol, amyl alcohol or allyl alcohol can also be used. However, the yield is generally from 10 to 15% lower than when using methanol or ethanol. Other solvents, such as e.g. dimethylsulfoxide (DMSO), are not favorable as these either have an oxidative effect or dissolve significant amounts of oxygen from the air, which can lead to the formation of disulphides.

Forbindelsene med den generelle formel I er i basiske medier temmelig ubestandige, særlig ved høyere temperatur, idet de oksy-deres meget hurtig til disulfidforbindelser. For å hindre oksy-dasjonen utføres reaksjonen under gjennomstrømning av tørr i^S The compounds with the general formula I are rather unstable in basic media, particularly at higher temperatures, as they oxidize very quickly to disulphide compounds. In order to prevent the oxidation, the reaction is carried out under a flow of dry i^S

og ved temperaturer på mellom 0 og 20°C.and at temperatures between 0 and 20°C.

Det er kjent at sure metallsulfider er meget ubestandigeIt is known that acid metal sulphides are very unstable

og at de hydrolyseres lett med luftfuktighet og lar seg oksydere med oksygen i luften. Av den grunn er det fordelaktig å arbeide med friskt tilberedet kalium- eller natriumhydrogensulfid. Dette fremstiller man vanligvis av kalium- eller natriumalkoholater i absolutt alkohol med gassformet, tørt svovelvannstoff. Forbindelsene med den generelle formel I i form av de frie baser er meget ubestandige. Av den grunn isoleres de med fordel i form av salter med organiske eller uorganiske syrer. Disse salter oppnås f.eks. enkelt ved surgjøring av reaksjonsmediet med alkoholiske løsninger av de tilsvarende syrer. For isolering har gassformig HCl i isopropanol (35 prosentig løsning), 96 prosentig svovelsyre i isopropanol (40 prosentig løsning) og iseddik i butanol (50 prosentig løsning) vist seg best egnet. and that they are easily hydrolyzed by humidity and can be oxidized by oxygen in the air. For that reason, it is advantageous to work with freshly prepared potassium or sodium hydrogen sulphide. This is usually prepared from potassium or sodium alcoholates in absolute alcohol with gaseous, dry hydrogen sulphide. The compounds with the general formula I in the form of the free bases are very unstable. For that reason, they are advantageously isolated in the form of salts with organic or inorganic acids. These salts are obtained, e.g. simply by acidifying the reaction medium with alcoholic solutions of the corresponding acids. For isolation, gaseous HCl in isopropanol (35 percent solution), 96 percent sulfuric acid in isopropanol (40 percent solution) and glacial acetic acid in butanol (50 percent solution) have proven to be most suitable.

Ved fremgangsmåten ifølge oppfinnelsen er følgende nye forbindelser blitt fremstilt: 4(5)-metyl-5(4)-metylentiol-imidazol i form av hydroklorid. 4(5)-etyl-5(4)-metylentiol-imidazol i form av sulfat. 4(5)-butyl-5(4)-metylentiol-imidazol i form av acetat. By the method according to the invention, the following new compounds have been prepared: 4(5)-methyl-5(4)-methylenethiol-imidazole in the form of hydrochloride. 4(5)-ethyl-5(4)-methylenethiol-imidazole in the form of sulfate. 4(5)-butyl-5(4)-methylenethiol-imidazole in the form of acetate.

Fremgangsmåten ifølge oppfinnelsen er utledet av den kjente fremgangsmåte til fremstilling av tioalkoholer, som er beskrevet i Houben-Weyl "Methoden der organischen Chemie", bind IX, sider 7-11 (1955). Denne fremgangsmåte kan på grunn av den store ube-standighet til forbindelsene med formelen I ikke umiddelbart anvendes, idet den gir en blanding av forbindelsene med den generelle formel I og deres disulfider. Bare ved senkning av temperaturen til 0-5°C og under dråpevis tilsetning av løsningen av forbindelsene II samt under stadig gjennomstrømning av tørr H 2S gjennom reaksjonsblandingen kan forbindelsene med formel I oppnås med høye utbytter (over 90% av det teoretiske). The method according to the invention is derived from the known method for the preparation of thioalcohols, which is described in Houben-Weyl "Methoden der organischen Chemie", volume IX, pages 7-11 (1955). Due to the great instability of the compounds of the formula I, this method cannot be immediately used, as it gives a mixture of the compounds of the general formula I and their disulfides. Only by lowering the temperature to 0-5°C and during the dropwise addition of the solution of the compounds II as well as during constant flow of dry H 2S through the reaction mixture can the compounds of formula I be obtained with high yields (over 90% of the theoretical).

Forbindelsene med formel I tjener som mellomprodukter ved fremstillingen av forskjellige antihystaminika, som er kjent somH2-reseptor-blokkerere. The compounds of formula I serve as intermediates in the preparation of various antihistamines, which are known as H 2 -receptor blockers.

Oppfinnelsen vil bli illustrert ved hjelp av følgende eksem-pler.. The invention will be illustrated using the following examples.

Eksempel 1Example 1

4( 5)- metyl- 5( 4)- metylentio- imidazolhydroklorid4( 5)- methyl- 5( 4)- methylenethio-imidazole hydrochloride

5,86 g (0,15 mol) kalium ble løst i 100 ml absolutt metanol. Løsningen ble deretter mettet med H2S ved 0-5°C. Ved samme temperatur, i en strøm av f^S, ble det i løpet av to timer dråpevis tilsatt en løsning av 10,0 g (0,06 mol) 4(5)-klormetyl-5(4)-metylimidazolhydroklorid i 50 ml absolutt metanol. Etter til-setningen ble det omrørt i ytterligere 3 0 minutter, hvoretter det utskilte uorganiske salt ble avfiltrert. Den filtrerte løs-ning ble surgjort med 10 ml 34 prosentig HCl i isopropanol, hvoretter det ble tilsatt 0,5 g aktivkull og filtrert. Filtratet ble inndampet til et lite volum og i varme tynnet med 3 0-4 0 ml isopropyleter, hvoretter krystallisasjon' begynte. Det ble oppnådd 8,8-9,5 g produkt (dvs. 90-95% av det teoretiske), med et smeltepunkt på 226-227°C. IR (KBr): 3100-2600, 1630, 820 cm<-1>. NMR (DMSO-d6) 6 i ppm: 2,31 (s,3H), 3,86 (s,2H), 9,00 (s,lH), Rf: -0,50, på silikagelplate eluert med CH2Cl2/MeOH/HCOOH (8:2:0,5) og gjort synlig med joddamper. 5.86 g (0.15 mol) of potassium was dissolved in 100 ml of absolute methanol. The solution was then saturated with H2S at 0-5°C. At the same temperature, in a stream of f^S, a solution of 10.0 g (0.06 mol) 4(5)-chloromethyl-5(4)-methylimidazole hydrochloride in 50 ml was added dropwise over the course of two hours absolute methanol. After the addition, it was stirred for a further 30 minutes, after which the separated inorganic salt was filtered off. The filtered solution was acidified with 10 ml of 34% HCl in isopropanol, after which 0.5 g of activated carbon was added and filtered. The filtrate was evaporated to a small volume and diluted in heat with 30-40 ml of isopropyl ether, after which crystallization began. 8.8-9.5 g of product was obtained (ie 90-95% of the theoretical), with a melting point of 226-227°C. IR (KBr): 3100-2600, 1630, 820 cm<-1>. NMR (DMSO-d6) 6 in ppm: 2.31 (s,3H), 3.86 (s,2H), 9.00 (s,1H), Rf: -0.50, on silica gel plate eluted with CH2Cl2/ MeOH/HCOOH (8:2:0.5) and made visible with iodine vapors.

Analyse for: C5HgClN2SAnalysis for: C5HgClN2S

beregnet: C: 36,47; H: 5,50; N: 17,01; S: 19,47% calcd: C: 36.47; H: 5.50; N: 17.01; S: 19.47%

funnet : C: 37,00; H: 5,66; N: 16,48; S: 20,02% found : C: 37.00; H: 5.66; N: 16.48; S: 20.02%

Eksempel 2Example 2

4( 5)- metyl- 5( 4)- metylentiol- imidazolhydroklorid4( 5)- methyl- 5( 4)- methylenethiol- imidazole hydrochloride

5,0 g (0,21 mol) natrium ble løst i 100 ml etanol. Løsningen ble mettet med H2S under kjøling (0-5°C). Til denne løsning ble 5.0 g (0.21 mol) of sodium was dissolved in 100 ml of ethanol. The solution was saturated with H2S under cooling (0-5°C). To this solution was

det i løpet av 2 timer under gjennomstrømning av I^S tilsatt 25,5 g (0,10 mol) 4(5)-brommetyl-5(4)-metylimidazol løst i 50 ml absolutt etanol. Deretter ble det omrørt i ytterligere 30 minutter, og det uorganiske salt ble avfiltrert. Filtratet ble 25.5 g (0.10 mol) of 4(5)-bromomethyl-5(4)-methylimidazole dissolved in 50 ml of absolute ethanol were added over the course of 2 hours while flowing through I^S. It was then stirred for a further 30 minutes and the inorganic salt was filtered off. The filtrate was

surgjort med 20 ml 34 prosentig HCl/isopropylalkohol, og det ble tilsatt 0,5 g aktivkull og filtrert. Filtratet ble inndampet til ca. 4 0 ml, og til den varme løsning ble det tilsatt diisopropyl-eter inntil begynnelse av krystallisasjon. Etter avkjøling til acidified with 20 ml of 34 percent HCl/isopropyl alcohol, and 0.5 g of activated carbon was added and filtered. The filtrate was evaporated to approx. 40 ml, and to the hot solution was added diisopropyl ether until the beginning of crystallization. After cooling to

0°C ble det avfiltrert, og bunnfallet ble spylt med eniblanding av metanol og isopropyleter (1:1). Produktet ble oppnådd med et smeltepunkt på 225-226°C (fra metanol) med et utbytte på 93-97%. IR (KBr): 3100-2600, 1630, 820 cm<-1>. NMR (DMSO-dg): 6 i ppm: 2,31 (s,3H), 3,86 (s,2H), 9,00 (s,lH). NMR (CD3OD): 2,33 (s,3H), 3,85 (s,2H), 8,80 (s,lH). 0°C, it was filtered off, and the precipitate was rinsed with a mixture of methanol and isopropyl ether (1:1). The product was obtained with a melting point of 225-226°C (from methanol) with a yield of 93-97%. IR (KBr): 3100-2600, 1630, 820 cm<-1>. NMR (DMSO-dg): 6 in ppm: 2.31 (s,3H), 3.86 (s,2H), 9.00 (s,1H). NMR (CD 3 OD): 2.33 (s,3H), 3.85 (s,2H), 8.80 (s,1H).

Analyse for C5HgClN2SAnalysis for C5HgClN2S

beregnet: C: 36,47; H: 5,50; N: 17,01; S: 19,47% calcd: C: 36.47; H: 5.50; N: 17.01; S: 19.47%

funnet : C: 36,90; H: 5,96; N: 16,68; S: 20,00% found : C: 36.90; H: 5.96; N: 16.68; S: 20.00%

Rf~0,5 med metylenklorid-metanol-maursyre (8,0:2,0:0,5). Rf~0.5 with methylene chloride-methanol-formic acid (8.0:2.0:0.5).

Eksempel 3Example 3

4( 5)- etyl- 5( 4)- metylentiol- imidazolsulfat4( 5)- ethyl- 5( 4)- methylenethiol- imidazole sulfate

Det ble arbeidet på samme måte som i eksempel 2, men det ble løst 6,5 g Ca(HS)2i 100 ml butanol, og 8,0 g 4(5)-etyl-5(4)-brommetylimidazol ble tilsatt. Surgjøring ble foretatt med 4 0 prosentig svovelsyre i isopropanol. Den ovenfor angitte forbindelse ble oppnådd i 88-90 prosentig utbytte og hadde smeltepunkt på 208-210°C. IR (KBr): 3200-2750, 1635, 915 og 820 cm<-1>. The procedure was the same as in example 2, but 6.5 g of Ca(HS) 2 were dissolved in 100 ml of butanol, and 8.0 g of 4(5)-ethyl-5(4)-bromomethylimidazole was added. Acidification was carried out with 40 percent sulfuric acid in isopropanol. The above compound was obtained in 88-90 percent yield and had a melting point of 208-210°C. IR (KBr): 3200-2750, 1635, 915 and 820 cm<-1>.

Analyse for C6H12<N>204S2Analysis for C6H12<N>204S2

beregnet: C: 29,99; H: 5,04; N: 11,55; S: 26,68% calculated: C: 29.99; H: 5.04; N: 11.55; S: 26.68%

funnet : C: 29,71; H: 5,26; N: 11,80; S: 26,35% found : C: 29.71; H: 5.26; N: 11.80; S: 26.35%

Eksempel 4Example 4

4( 5) - butyl- 5( 4)- metylentiol- imidazolacetat4(5)-butyl-5(4)-methylenethiol-imidazole acetate

Det ble arbeidet på samme måte som beskrevet i eksempel 2, men som utgangsmateriale ble det anvendt 6 g 4(5)-butyl-5(4)-brommetyl-imidazol og 10 g NH^SH, som begge var løst i isopropanol ved 15°C. Surgjøringen ble foretatt med 50 prosentig eddiksyre i butanol. Det ble oppnådd den ovenfor angitte forbindelse med smeltepunkt på 126-128°C og i utbytte på 85-90%. The work was carried out in the same way as described in example 2, but as starting material 6 g of 4(5)-butyl-5(4)-bromomethyl-imidazole and 10 g of NH^SH, both of which were dissolved in isopropanol at 15 °C. The acidification was carried out with 50 percent acetic acid in butanol. The above-mentioned compound was obtained with a melting point of 126-128°C and in a yield of 85-90%.

IR (KBr): 3150-2600, 1635, 910 og 820 cm"<1>. IR (KBr): 3150-2600, 1635, 910 and 820 cm"<1>.

Analyse for: ci0H18N2°2SAnalysis for: ci0H18N2°2S

beregnet: C: 52,15; H: 7,88; N: 12,16; S: 13,92% calcd: C: 52.15; H: 7.88; N: 12.16; S: 13.92%

funnet : C: 51,89; H: 7,99; N: 12,01; S: 13,65% found : C: 51.89; H: 7.99; N: 12.01; S: 13.65%

Claims (8)

1. Tiolderivater av imidazol, og deres salter med organiske og uorganiske syrer, karakterisert ved at de har formelen 1. Thiol derivatives of imidazole, and their salts with organic and inorganic acids, characterized in that they have the formula hvor R er en alkylrest med høyst 4 karbonatomer i kjeden.where R is an alkyl residue with no more than 4 carbon atoms in the chain. 2. Tiolderivat i samsvar med krav 1, karakterisert ved at det er 4(5)-metyl-5(4)-metylentiol-imidazol.2. Thiol derivative in accordance with claim 1, characterized in that it is 4(5)-methyl-5(4)-methylenethiol-imidazole. 3. Tiolderivat i samsvar med krav 1, karakterisert ved at det er 4(5)-etyl-5(4)-metylentiol-imidazol.3. Thiol derivative in accordance with claim 1, characterized in that it is 4(5)-ethyl-5(4)-methylenethiol-imidazole. 4. Tiolderivat i samsvar med krav 1, karakterisert ved at det er 4(5)-butyl-5(4)-metylentiol-imidazol.4. Thiol derivative in accordance with claim 1, characterized in that it is 4(5)-butyl-5(4)-methylenethiol-imidazole. 5. Fremgangsmåte til fremstilling av tiolderivatene ifølge et av kravene 1-4, med formelen 5. Process for producing the thiol derivatives according to one of claims 1-4, with the formula og deres salter med uorganiske og organiske syrer, hvor R er et lavere alkylradikal med hø yst 4 karbonatomer i kjeden, karakterisert ved at forbindelser med formelen and their salts with inorganic and organic acids, where R is a lower alkyl radical with no more than 4 carbon atoms in the chain, characterized in that compounds with the formula hvor R har samme betydning som i formel I og X er et halogen-atom, omsettes med et surt metallsulfid MeHS, hvor Me er Na, K, Ca, :NH^, Ba eller Sr, i en lavere alkohol ved temperaturer på mellom 0 og 2 0°C og under gjennomstrømning med gassformig H2 S.where R has the same meaning as in formula I and X is a halogen atom, is reacted with an acidic metal sulphide MeHS, where Me is Na, K, Ca, :NH^, Ba or Sr, in a lower alcohol at temperatures between 0 and 2 0°C and under flow-through with gaseous H2 S. 6. Fremgangsmåte i samsvar med krav 1, karakterisert ved at det som MeHS anvendes friskt fremstilt KHS eller NaHS.6. Method in accordance with claim 1, characterized in that freshly prepared KHS or NaHS is used as MeHS. 7. Fremgangsmåte i samsvar med krav 5 eller 6, karakterisert ved at saltene av tittelforbindelsene, dvs. hydroklorider, sulfater eller acetater, fremstilles ved surgjøring med alkoholiske lø sninger av de tilsvarende syrer.7. Process in accordance with claim 5 or 6, characterized in that the salts of the title compounds, i.e. hydrochlorides, sulphates or acetates, are produced by acidification with alcoholic solutions of the corresponding acids. 8. Fremgangsmåte i samsvar med krav 5 eller 6, karakterisert ved at det som lavere alkoholer anvendes metanol, etanol eller isopropanol.8. Method in accordance with claim 5 or 6, characterized in that methanol, ethanol or isopropanol are used as lower alcohols.
NO791576A 1978-05-12 1979-05-11 THIOL DERIVATIVES OF IMIDAZOLE NO791576L (en)

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BE (1) BE875994A (en)
CS (1) CS213375B2 (en)
DE (1) DE2919147A1 (en)
DK (1) DK190379A (en)
FI (1) FI791405A7 (en)
FR (1) FR2425434A1 (en)
GB (1) GB2024206B (en)
GR (1) GR68392B (en)
HU (1) HU178707B (en)
IT (1) IT1166783B (en)
LU (1) LU81178A1 (en)
NL (1) NL7903731A (en)
NO (1) NO791576L (en)
PL (1) PL215534A1 (en)
SE (1) SE7904060L (en)
SU (1) SU784765A3 (en)
YU (1) YU110279A (en)

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CN113234018B (en) * 2021-05-11 2022-08-23 石家庄市普力制药有限公司 Production method of cimetidine

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JPS5440547A (en) * 1977-09-07 1979-03-30 Seikosha Kk Device for adjusting output frequency of frequency divider
IL56265A (en) * 1977-12-28 1982-08-31 Om Lab Sa Process for preparing imidazolyl methylthio guanidine derivatives and a novel intermediate therefor
GR65283B (en) * 1977-12-30 1980-08-01 Crc Ricerca Chim Method for the alkyliosis of 4(5)-merka ptomethyl-imidazoles with aziridin derivatives

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JPS57150666A (en) 1982-09-17
SU784765A3 (en) 1980-11-30
NL7903731A (en) 1979-11-14
IT1166783B (en) 1987-05-06
BE875994A (en) 1979-09-03
SE7904060L (en) 1979-11-13
GB2024206B (en) 1982-11-10
PL215534A1 (en) 1980-12-01
IT7922446A0 (en) 1979-05-08
GB2024206A (en) 1980-01-09
DK190379A (en) 1979-11-13
FI791405A7 (en) 1981-01-01
CS213375B2 (en) 1982-04-09
JPS5440548B1 (en) 1979-12-04
HU178707B (en) 1982-06-28
DE2919147A1 (en) 1979-11-15
FR2425434A1 (en) 1979-12-07
LU81178A1 (en) 1979-09-10
YU110279A (en) 1983-01-21
GR68392B (en) 1981-12-29

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