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DE1229102B - Process for the preparation of monochloro-9-thiabicyclo-2-nonenes and their 9-oxides and 9,9-dioxides - Google Patents

Process for the preparation of monochloro-9-thiabicyclo-2-nonenes and their 9-oxides and 9,9-dioxides

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Publication number
DE1229102B
DE1229102B DEH51835A DEH0051835A DE1229102B DE 1229102 B DE1229102 B DE 1229102B DE H51835 A DEH51835 A DE H51835A DE H0051835 A DEH0051835 A DE H0051835A DE 1229102 B DE1229102 B DE 1229102B
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carbon atom
thiabicyclo
monochloro
nonenes
oxides
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Keith J Smith
Edward D Weil
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Hooker Chemical Corp
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Hooker Chemical Corp
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Description

Verfahren zur Herstellung von Monochlor-9-thiabicyclo-2-nonenen sowie deren 9-Oxyden und 9,9-Dioxyden Die Erfindung betrifft ein Verfahren zur Her. stellung von Monochlor-9-thiabicyclo-2-nonenen so. wie deren 9-Oxyden und 9,9-Dioxyden der allgemeinen Formel in der das Chlor an das Kohlenstoffatom 5 gebunden ist, wenn sich die Schwefelbrücke von dem Kohlenstoffatom 1 zu dem Kohlenstoffatom 6 erstreckt, dagegen an das Kohlenstoffatom 6 gebunden ist, wenn sich die Schwefelbrücke von dem Kohlenstoffatom 1 zu dem Kohlenstoffatom 5 erstreckt, und t = 0, 1 oder 2 bedeutet.Process for the production of monochloro-9-thiabicyclo-2-nonenes and their 9-oxides and 9,9-dioxydes. The invention relates to a process for the production of monochloro-9-thiabicyclo-2-nonenes. such as their 9-oxides and 9,9-dioxides of the general formula in which the chlorine is bonded to carbon atom 5 when the sulfur bridge extends from carbon atom 1 to carbon atom 6, whereas it is bonded to carbon atom 6 when the sulfur bridge extends from carbon atom 1 to carbon atom 5, and t = Means 0, 1 or 2.

Erfindungsgemäß wird dabei so vorgegangen, daß man Dichlor-9-thiabicyclononan so lange auf eine Temperatur von etwa 110 bis etwa 220"C erhitzt, bis 1 Moläquivalent Halogenwasserstoff freigesetzt ist, und gegebenenfalls das erhaltene Monochlor-9-thiabicyclononen in an sich bekannter Weise zum 9-Oxyd oder 9,9-Dioxyd oxydiert. According to the invention, the procedure is that dichloro-9-thiabicyclononane is used heated to a temperature of about 110 to about 220 "C until 1 molar equivalent Is released hydrogen halide, and optionally the resulting monochloro-9-thiabicyclononen oxidized in a manner known per se to 9-oxide or 9,9-dioxide.

Chlor-9-thiabicyclo-2-nonen verhält sich chemisch in vielen seiner Reaktionen so, als ob es ein Gleichgewichtsgemisch von [3,3,1]- und [4,2,1]-Strukturen, wahrscheinlich auch im Gleichgewicht mit einer ionischen Form X " S " S Cl Cl Cl [3,3,1] [ionisierte Form] [4,2,1] in der für andere ß-Chlorsulfide von F u 5 o n und Mitarbeitern, Journal of Organic Chemistry, Bd. 11, S. 476, beschriebenen Weise wäre.Chlor-9-thiabicyclo-2-nonene behaves chemically in many of its reactions as if it were an equilibrium mixture of [3,3,1] and [4,2,1] structures, probably also in equilibrium with an ionic one shape X "S" S Cl Cl Cl [3,3,1] [ionized form] [4,2,1] in the manner described for other β-chlorosulfides by F u 5 on and coworkers, Journal of Organic Chemistry, Vol. 11, p. 476.

Die Reaktion dauert etwa 1 Stunde bei den höheren Temperaturen und bis zu mehreren Tagen bei den niedrigeren Temperaturen, bis Chlorwasserstoffent wicklung auftritt. Es ist nicht erforderlich, genau 1 Moläquivalent Chlorwasserstoff abzutrennen, doch ist dies nahezu das Optimum. Wenn mehr oder weniger Chlorwasserstoff abgetrennt wird, so kann das Endprodukt leicht durch fraktionierte Destilla tion von Nebenprodukten und/oder nicht umgesetztem Ausgangsmaterial isoliert werden. Harzartige Neben produkte können auf ein Minimum herabgesetzt werden, indem die Reaktion bis zu etwas weniger als der 1000/oigen Umwandlung durchgeführt wird. The reaction takes about 1 hour at the higher temperatures and up to several days at the lower temperatures until hydrogen chloride is found winding occurs. It is not necessary to use exactly 1 molar equivalent of hydrogen chloride to be separated, but this is almost the optimum. If more or less hydrogen chloride is separated, so the end product can easily tion by fractional distillation isolated from by-products and / or unreacted starting material. Resin-like by-products can be minimized by the Reaction to a little less than 1000% conversion is carried out.

Die Reaktion erfordert zwar kein Lösungsmittel, doch kann gegebenenfalls ein inertes Lösungsmittel verwendet werden, um die Wärmeüberführung oder Temperaturkontrolle zu erleichtetn oder die Austreibung des freigesetzten Chlorwasserstoffs zu unterstützen. Zu geeigneten Lösungsmitteln gehören aromatische oder aliphatische Kohlenwasserstoffe, wie beispielsweise Xylol, Cumol, Octan, Decahydronaphthalin oder Tetrahydronaphthalin; chlorierte Kohlenwasserstoffe, wie beispielsweise Tetrachloräthan, Dichlorbenzol, Trichlorbenzol; Anisol; Nitrobenzol; Diphenyläther und andere gegenüber Chlorwasserstoff beständige Lösungsmittel. Although the reaction does not require a solvent, it can optionally an inert solvent can be used for heat transfer or temperature control to facilitate or to support the expulsion of the released hydrogen chloride. Suitable solvents include aromatic or aliphatic hydrocarbons, such as xylene, cumene, octane, decahydronaphthalene or tetrahydronaphthalene; chlorinated hydrocarbons, such as tetrachloroethane, dichlorobenzene, Trichlorobenzene; Anisole; Nitrobenzene; Diphenyl ether and others against hydrogen chloride resistant solvents.

Bei dem erfindungsgemäßen Verfahren ist kein Katalysator erforderlich. Die Reaktion kann jedoch durch Lewis-Säuren (wie beispielsweise FeC, ZnCl2, SbCls, NiCl2, CoCl2 und andere bekannte Schwermetallsalze mit den Eigenschaften von Lewis-Säuren) und oberflächenaktive Festsubstanzen mit Eigenschaften von Lewis-Säuren, wie beispielsweise Aluminiumoxyd, Ton und Aktivkohle, beschleunigt werden. Zur Vermeidung einer Verharzung des Produktes ist es gut, nur kleinere Mengen derartiger Katalysatoren zu verwenden, wobei der übliche Mengenanteil etwa 1 Teil je Million bis zu etwa 50/0 beträgt. No catalyst is required in the process of the invention. However, the reaction can be triggered by Lewis acids (such as FeC, ZnCl2, SbCls, NiCl2, CoCl2 and other known heavy metal salts with the properties of Lewis acids) and surface-active solid substances with properties of Lewis acids, such as aluminum oxide, clay and activated carbon, can be accelerated. To avoid If the product becomes resinous, it is good to use only small amounts of such catalysts to use, the usual proportion of about 1 part per million up to about 50/0 is.

Soll das 9-Oxyd oder 9,9-Dioxyd hergestellt werden, so wird das entsprechende Sulfid durch Behandlung mit 1 bzw. 2 Aquivalenten eines dafür geeigneten Oxydationsmittels oxydiert. Dafür geeignet sind Wasserstoffperoxyd, Peressigsäure, Perbenzoesäure, Perphthalsäure oder andere organische Peroxysäuren, Salpetersäure, Stickstoffdioxyd oder -tetroxyd, Permanganate, Chromsäure oder Dichromate, Bromsäuren oder Bromate, unterchlorige Säure. (oder Chlor + Wasser) oder Ozon. Molektilarer Sauerstoff kann ebenfalls verwendet werden, vorzugsweise unter Verwendung eines Katalysators, wie beispielsweise Vanadiumoxyd oder Stickstoffoxyd. If the 9-Oxide or 9,9-Dioxide is to be produced, then the corresponding is Sulphide by treatment with 1 or 2 equivalents of a suitable oxidizing agent oxidized. Suitable for this are hydrogen peroxide, peracetic acid, perbenzoic acid, Perphthalic acid or other organic peroxy acids, nitric acid, nitrogen dioxide or tetroxide, permanganate, chromic acid or dichromate, bromic acid or bromate, hypochlorous acid. (or chlorine + water) or ozone. Molectilar oxygen can can also be used, preferably using a catalyst such as for example vanadium oxide or nitrogen oxide.

Die erfindungsgemäß erhältlichen neuen Verbindungen sind als Zwischenprodukte, als Schädlingsbekämpfungsmittel, als Zusätze für Hochdruckschmieröle und Schneidöle und als Monomere und Comonomere für Harzsynthesen brauchbar. The novel compounds obtainable according to the invention are available as intermediates, as pesticides, as additives for high pressure lubricating oils and cutting oils and useful as monomers and comonomers for resin synthesis.

Im allgemeinen zeigen die erfindungsgemäß erhältlichen Verbindungen Wirksamkeit auf Mikroorganismen, d. h. Fungi, Bakterien, und in einigen Fällen Nematoden. In general, the compounds obtainable according to the invention show Effectiveness on microorganisms, d. H. Fungi, bacteria, and in some cases nematodes.

Die Verfahrensprodukte können auch mit anderen Wirkstoffen, beispielsweise anderen Fungiciden, z. B. The process products can also with other active ingredients, for example other fungicides, e.g. B.

Schwefel, Dithiocarbamaten, Dodecylguanidin, Nitropolychlorbenzolen und verschiedenen chlorierten Alkylthiogruppen enthaltenden Verbindungen, wie beispielsweise N - Trichlormethylmercapto - 4 - cyclohexen-1,2-dicarboximid, gemeinsam angewandt werden, auch mit Insekticiden, wie beispielsweise chlorierten Kohlenwasserstoff-Insekticiden, Phosphat-Insekticiden und Carbamat-Insekticiden, sowie mit Herbiciden, wie beispielsweise Natriumchlorid, Natriumborat, 2,4-Dichlorphenoxyessigsäure, herbiciden Triazinen, herbiciden Harnstoffen und herbiciden Urazilen.Sulfur, dithiocarbamates, dodecylguanidine, nitropolychlorobenzenes and various chlorinated alkylthio group-containing compounds such as N - trichloromethyl mercapto - 4 - cyclohexene-1,2-dicarboximide, used together also with insecticides, such as chlorinated hydrocarbon insecticides, Phosphate insecticides and carbamate insecticides, as well as with herbicides such as Sodium chloride, sodium borate, 2,4-dichlorophenoxyacetic acid, herbicidal triazines, herbicidal ureas and herbicidal uracilene.

Schließlich können die Verfahrensprodukte mit synergistischen Mitteln, die zur Erhöhung der Aktivität als Schädlingsbekämpfungsmittel dienen, beispielsweise Piperonylbutylat, gemeinsam eingesetzt werden. Finally, the process products can be used with synergistic agents, which serve as pesticides to increase the activity, for example Piperonyl butylate, can be used together.

Die folgenden Beispiele erläutern die Erfindung. The following examples illustrate the invention.

Beispiel 1 6-Chlor-9-thiabicyclo-[3,3,1]-2-nonen 211 g 2,6 - Dichlor - 9 - thiabicyclo - [3,3,1] - nonan (1 Mol), erhalten gemäß Beispiel 1 der Patentanmeldung H 51 834 IV/12 q, wurden 20 Stunden auf 166 bis 184"C erhitzt, bis 36,5 Volumteile (1 Mol) Chlorwasserstoff (gemessen durch Auffangen in Wasser und Titration) abgegeben waren. Der Rückstand wurde im Vakuum destilliert, wobei man 148 g (850/0) farbloses Destillat vom Kp.o.i = 64 bis 69"C erhielt. N2D5= 1,5713. Example 1 6-chloro-9-thiabicyclo- [3,3,1] -2-nonene 211 g 2,6-dichloro - 9 - thiabicyclo - [3,3,1] - nonane (1 mol), obtained according to Example 1 of the patent application H 51 834 IV / 12 q, were heated to 166 to 184 "C for 20 hours, up to 36.5 parts by volume (1 mol) of hydrogen chloride (measured by collecting in water and titration) given off was. The residue was distilled in vacuo, giving 148 g (850/0) of colorless Distillate obtained from b.p.o.i = 64 to 69 "C. N2D5 = 1.5713.

Analyse: C8H11SCl. Analysis: C8H11SCl.

Berechnet ... Cl 20,3, S 18,35°/o; gefunden ... Cl 19,9, S 18,290/0. Calculated ... Cl 20.3, S 18.35%; found ... Cl 19.9, S 18.290 / 0.

Beispiel 2 6-Chlor-9-thiabicyclo- [3,3,1 ]-2-nonen-9-oxyd 17,5 Teile 6-Chlor-9- thiabicyclo- [3,3,1]-2-nonen wurden in 10() Volumteilen Eisessig gelöst. Zu dieser Lösung wurden allmählich 11,4Volumteile 300/obiges Wasserstoffperoxyd zugegeben. Man ließ die exotherme Reaktion bis -auf 76"C kommen. Nach dem Nachlassen der Wärmefreisetzung wurde das Reaktionsgemisch auf einem Wasserbad 15 Minuten auf 95"C erwärmt. Das Reaktionsgemisch wurde dann mit 1000 Teilen Wasser verdünnt und das organische Produkt mit Chloroform extrahiert. Der Extrakt wurde im Vakuum eingedampft, wobei man einen viskosen öligen Rückstand erhielt, der sich bei längerem Stehen verfestigte. Example 2 6-chloro-9-thiabicyclo- [3,3,1] -2-nonene-9-oxide 17.5 parts 6-chloro-9-thiabicyclo- [3,3,1] -2-nonene were dissolved in 10 () parts by volume of glacial acetic acid. 11.4 parts by volume of 300 / above hydrogen peroxide were gradually added to this solution admitted. The exothermic reaction was allowed to come to -76 "C. After subsiding To release heat, the reaction mixture was left on a water bath for 15 minutes 95 "C. The reaction mixture was then diluted with 1000 parts of water and the organic product extracted with chloroform. The extract was evaporated in vacuo, a viscous oily residue was obtained, which upon prolonged standing was obtained solidified.

Analyse: CsH11SOC1 Berechnet . . Cl l8,701o; gefunden . . Cl 16,7010.Analysis: CsH11SOC1 calculated. . Cl 18,701o; found . . Cl 16.7010.

Dieses Produkt ergab bei Anwendung auf zweigefleckte Milben bei 0,1 0/oiger Konzentration in wäßriger Dispersion in 24 Stunden eine praktisch vollständige Abtötung. This product when applied to two-spotted mites gave 0.1 0 / o concentration in aqueous dispersion practically complete in 24 hours Mortification.

Die Infrarotprüfung zeigte eine kleine Verunreinigung durch einen Acetatester, der für den etwas niedrigen Chlorgehalt verantwortlich ist. The infrared test showed a small amount of contamination from one Acetate ester, which is responsible for the somewhat low chlorine content.

Beispiel 3 6-Chlor-9-thiabicyclo- [3,3,1 ]-2-nonen-9,9-dioxyd Zu einer Lösung von 52,5 g (0,3 Mol) 6-Chlor-9-thiabicyclo-[3,3,1]-2-nonen in 300 ml Eisessig wurden 85,2 g (0,75 Mol) 300/obiges Wasserstoffperoxyd innerhalb von 20 Minuten unter Rühren zugesetzt, wobei die Temperatur bis zum Siedepunkt steigen gelassen wurde. Dann wurde das Gemisch 20 Minuten auf dem Dampfbad erhitzt, zu 3 1 Wasser gegeben und mit 400 ml Chloroform extrahiert. Die Extrakte wurden über Magnesiumsulfat getrocknet, filtriert, zur Entfernung des Chloroforms eingedampft und der Rückstand aus Essigsäure umkristallisiert, wobei 38 g farblose Kristalle vom F. 114 bis 115"C erhalten wurden. Umkristallisation aus Essigsäure lieferte 34 g (550/o) Ausbeute vom F. 119 bis 1200C, aus Methanol vom F. 120,5 bis 121,5"C. Das Infrarotspektrum (Nujol) zeigte eine C = C-Bande bei 1646 cm-1 und - SO2 --Banden bei 1119 und 1297 cm-l. Example 3 6-chloro-9-thiabicyclo- [3,3,1] -2-nonene-9,9-dioxide To a solution of 52.5 g (0.3 mol) of 6-chloro-9-thiabicyclo- [3,3,1] -2-nonene in 300 ml Glacial acetic acid was 85.2 g (0.75 mol) of 300 / above hydrogen peroxide within 20 Added minutes with stirring, the temperature rising to the boiling point was left. Then the mixture was heated on the steam bath for 20 minutes, to 3 1 added water and extracted with 400 ml of chloroform. The extracts were over Dried magnesium sulfate, filtered, evaporated to remove the chloroform and the residue was recrystallized from acetic acid, giving 38 g of colorless crystals with a melting point of 114 to 115 ° C. Recrystallization from acetic acid provided 34 g (550 / o) yield from 119 ° to 1200 ° C. from methanol from 120.5 ° to 121.5 ° C. The infrared spectrum (Nujol) showed a C = C band at 1646 cm-1 and - SO2 - bands at 1119 and 1297 cm-l.

Analyse: CsHllSO2Cl Berechnet C 46,48, H 5,36, Cl 17,16, S 15,510/0; gefunden C 46,52, H 5,33, Cl 17,20, S 15,470/0. Analysis: CsHIISO2Cl Calculated C 46.48, H 5.36, Cl 17.16, S 15.510 / 0; Found C 46.52, H 5.33, Cl 17.20, S 15.470 / 0.

Claims (1)

Patentanspruch: Verfahren zur Herstellung von Monochlor-9-thiabicyclo-2-nonenen sowie deren 9-Oxyden und 9,9-Dioxyden der allgemeinen Formel in der das Chlor an das Kohlenstoffatom 5 gebunden ist, wenn sich die Schwefelbrücke von dem Kohlenstoffatom 1 zu dem Kohlenstoffatom 6 erstreckt, dagegen an das Kohlenstoffatom 6 gebunden ist, wenn sich die Schwefelbrücke von dem Kohlenstoffatom 1 zu dem Kohlenstoffatom 5 erstreckt, und t = 0, 1 oder 2 bedeutet, d a -durch gekennzeichnet, daß man Di- chlor-9-thiabicyclononan so lange auf eine Temperatur von etwa 110 bis etwa 220"C erhitzt, bis 1 Moläquivalent Halogenwasserstoff freigesetzt ist, und gegebenenfalls das erhaltene Monochlor-9-thiabicyclononen in an sich bekannter Weise zum 9-Oxyd oder 9,9-Dioxyd oxydiert.Claim: Process for the preparation of monochloro-9-thiabicyclo-2-nonenes and their 9-oxides and 9,9-dioxides of the general formula in which the chlorine is bonded to carbon atom 5 when the sulfur bridge extends from carbon atom 1 to carbon atom 6, whereas it is bonded to carbon atom 6 when the sulfur bridge extends from carbon atom 1 to carbon atom 5, and t = 0, 1 or 2 means that dichloro-9-thiabicyclononane is heated to a temperature of about 110 to about 220 ° C. until 1 mol equivalent of hydrogen halide is released, and optionally the monochloro-9 obtained -thiabicyclononen oxidized in a manner known per se to the 9-oxide or 9,9-dioxide.
DEH51835A 1963-02-25 1964-11-25 Process for the preparation of monochloro-9-thiabicyclo-2-nonenes and their 9-oxides and 9,9-dioxides Pending DE1229102B (en)

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DE19641543648 Pending DE1543648B1 (en) 1963-02-25 1964-02-25 Process for the preparation of chlorination products of dichloro-9-thiabicyclononanes
DEH51834A Pending DE1232976B (en) 1963-02-25 1964-02-25 Process for the preparation of beta, beta'-dichloro-9-thiabicyclononanes or their 9-oxides or 9, 9-dioxides
DEH58112A Pending DE1297111B (en) 1963-02-25 1964-02-25 Thiabicyclo-2-nonene compounds
DEH58369A Pending DE1295567B (en) 1963-02-25 1964-02-25 Process for the preparation of 9-thiabicyclononane derivatives
DEH51835A Pending DE1229102B (en) 1963-02-25 1964-11-25 Process for the preparation of monochloro-9-thiabicyclo-2-nonenes and their 9-oxides and 9,9-dioxides

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DEH51834A Pending DE1232976B (en) 1963-02-25 1964-02-25 Process for the preparation of beta, beta'-dichloro-9-thiabicyclononanes or their 9-oxides or 9, 9-dioxides
DEH58112A Pending DE1297111B (en) 1963-02-25 1964-02-25 Thiabicyclo-2-nonene compounds
DEH58369A Pending DE1295567B (en) 1963-02-25 1964-02-25 Process for the preparation of 9-thiabicyclononane derivatives

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US4458061A (en) * 1982-09-29 1984-07-03 The Dow Chemical Company 9-Thiabicyclononanediisocyanates and polymers made therefrom
US4581435A (en) * 1982-12-29 1986-04-08 The Dow Chemical Company Alkyl-substituted thiapolycyclic polyahl and polyurethanes, polyamides and polyureas based thereon
JPS61500965A (en) * 1984-06-29 1986-05-15 ザ・ダウ・ケミカル・カンパニ− Alkyl-substituted thia polycyclic polyal and polymers produced therefrom
AU571553B2 (en) * 1984-06-29 1988-04-21 Dow Chemical Company, The 9-thiabicyclononanediisocyanates and polymers prepared therefrom
GB9510459D0 (en) 1995-05-24 1995-07-19 Zeneca Ltd Bicyclic amines
DE69728531T2 (en) * 1996-05-13 2004-09-30 Syngenta Ltd., Guildford BICYCLIC AMINES AS INSECTICIDES
GB9623944D0 (en) * 1996-11-15 1997-01-08 Zeneca Ltd Bicyclic amine derivatives
GB9624114D0 (en) * 1996-11-20 1997-01-08 Zeneca Ltd Pesticidal bicyclic amine derivatives
GB9624611D0 (en) * 1996-11-26 1997-01-15 Zeneca Ltd Bicyclic amine compounds
ES2216131T3 (en) * 1996-11-26 2004-10-16 Syngenta Limited DERIVATIVES OF 8-AZABICICLO 3,2,1) OCTANO-, 8- AZABICICLO 3,2.1) OCT-6- ENO- 9-AZABICICLO 3.3.1) NONANO-, 9-AZA -3- OXABICICLO 3.3.1) NONANO - AND 9 -AZA-3- THIABICICLE 3.3.1) NONANO, ITS PREPARATION AND ITS USE AS INSECTICIDES.

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DE1543648B1 (en) 1970-04-02
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NL129205C (en)

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