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DE1142350B - Process for the preparation of 1-halogen-3-hydroxy-alkanones- (2) - Google Patents

Process for the preparation of 1-halogen-3-hydroxy-alkanones- (2)

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Publication number
DE1142350B
DE1142350B DEC21743A DEC0021743A DE1142350B DE 1142350 B DE1142350 B DE 1142350B DE C21743 A DEC21743 A DE C21743A DE C0021743 A DEC0021743 A DE C0021743A DE 1142350 B DE1142350 B DE 1142350B
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Prior art keywords
halogen
hydroxy
ether
diol
bromo
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Pending
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DEC21743A
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German (de)
Inventor
Dr Herbert Meister
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Huels AG
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Chemische Werke Huels AG
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Priority to DEC21743A priority Critical patent/DE1142350B/en
Publication of DE1142350B publication Critical patent/DE1142350B/en
Pending legal-status Critical Current

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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C49/00Ketones; Ketenes; Dimeric ketenes; Ketonic chelates
    • C07C49/29Saturated compounds containing keto groups bound to rings
    • C07C49/337Saturated compounds containing keto groups bound to rings containing hydroxy groups
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C45/00Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds
    • C07C45/51Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by pyrolysis, rearrangement or decomposition
    • C07C45/511Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by pyrolysis, rearrangement or decomposition involving transformation of singly bound oxygen functional groups to >C = O groups
    • C07C45/513Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by pyrolysis, rearrangement or decomposition involving transformation of singly bound oxygen functional groups to >C = O groups the singly bound functional group being an etherified hydroxyl group
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C45/00Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds
    • C07C45/56Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds from heterocyclic compounds
    • C07C45/57Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds from heterocyclic compounds with oxygen as the only heteroatom
    • C07C45/59Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds from heterocyclic compounds with oxygen as the only heteroatom in five-membered rings

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Description

Verfahren zur Herstellung von 1-Halogen-3-hydroxy-alkanonen- (2) Für die Herstellung eines 1-Halogen-3-hydroxyalkanons- (2) sind bereits mehrere Darstellungsweisen bekanntgeworden. So wurde das I-Chlor-3-hydroxypropanon-2 durch Umsetzung von Methylacetylen mit unterchloriger Saure dargestellt (F. Smirnoff, C., 1904, 1, S. 576). Das I-Brom-3-methyl-butanol- (3)-on- (2) wurde durch Einwirkung von Brom auf Dimethylacetylen-carbinol-formiat erhalten (Nasarow, C. A., 1942, S. 746). Die ebenfalls zu dieser Verbindungsklasse führende Anlagerung von Wasser an die 3fache Bindung eines l-Halogen-alkin-(l)-ols-3 mit Hilfe von Quecksilbersalzen ergibt wider Erwarten nur minimale Ausbeuten : so wurde durch Anlagerung von Wasser an I-Brom-3-methyl-butin- (1)-ol- (3) das zu erwartende 1-Brom-3-methyl-butanol- (3)-on- (2) in einer Ausbeute von nur 4°/0 erhalten (Helv. chim. Acta, 34, S. 2424). Process for the preparation of 1-halo-3-hydroxy-alkanones- (2) For the production of a 1-halogen-3-hydroxyalkanone- (2) there are already several Modes of representation become known. So the I-chloro-3-hydroxypropanone-2 was through Reaction of methylacetylene with hypochlorous acid shown (F. Smirnoff, C., 1904, 1, p. 576). The I-bromo-3-methyl-butanol- (3) -one- (2) was by action obtained from bromine on dimethylacetylene carbinol formate (Nasarow, C. A., 1942, p. 746). The accumulation of water also leading to this class of compounds the 3-fold binding of a l-haloalkyne- (l) -ol-3 with the help of mercury salts yields only minimal yields, contrary to expectations: this was the case with the addition of water of I-bromo-3-methyl-butyn- (1) -ol- (3) the expected 1-bromo-3-methyl-butanol- (3) -on- (2) obtained in a yield of only 4% (Helv. Chim. Acta, 34, p. 2424).

Es wurde nun gefunden, daß man 1-Halogen-3-hydroxy-alkanone-2 der allgemeinen Formel XCHz-CO-COH (R, R,) wobei X ein Halogenatom und Ri und R2 Wasserstoffatome oder Alkylreste bedeuten, die auch zu einem cycloaliphatischen Rest verbunden sein können, in einfacher Weise dadurch herstellen kann, daß man 1-Halogenalken-(1)-diol-(2,3)-methylenäther-(2, 3) der allgemeinen Formel in saurem, wäßrigem Medium erhitzt.It has now been found that 1-halo-3-hydroxy-alkanones-2 of the general formula XCHz-CO-COH (R, R,) where X is a halogen atom and R 1 and R 2 are hydrogen atoms or alkyl radicals which also form a cycloaliphatic Remainder can be connected, can be produced in a simple manner by adding 1-haloalkene- (1) -diol- (2,3) -methylene ether- (2, 3) of the general formula heated in an acidic aqueous medium.

Als Ausgangsstoffe für die Umsetzung eignen sich die nach der deutschen Auslegeschrift C 21406 IVb/12q (deutsche Auslegeschrift 1 138 791) durch Umsetzung eines l-Halogen-alkin-(l)-ols-(3) mit Formaldehyd zugänglichen Methylenäther, wie z. B. I-Brompropen-(I)-diol-(2, 3)-methylenäther-(2, 3), I-Chlor-3-methylbuten-(l)-diol-(2, 3)-methylenäther-(2, 3), 1-Brom-3-methylpenten- (1)-diol (2, 3)-methylenather- (2, 3) sowie der Methylenäther des 1-Chlor-2-[cyclohexanol-1'-yl]-äthen- (1)-ols- (2). The starting materials for the implementation are those according to the German Auslegeschrift C 21406 IVb / 12q (German Auslegeschrift 1 138 791) through implementation of a l-haloalkyne- (l) -ols- (3) methylene ether accessible with formaldehyde, such as z. B. I-bromopropene- (I) -diol- (2, 3) -methylene ether- (2, 3), I-chloro-3-methylbutene- (l) -diol- (2, 3) -methylene ether- (2, 3), 1-bromo-3-methylpentene- (1) -diol (2, 3) -methylene ether- (2, 3) and the methylene ether of 1-chloro-2- [cyclohexanol-1'-yl] -ethen- (1) -ols- (2).

Die hydrolytische Abspaltung des Formaldehyds erfolgt in Gegenwart von mindestens der berechneten Menge Wasser, einer katalytischen Menge einer anorganischen oder organischen Säure, wie z. B. The hydrolytic cleavage of the formaldehyde takes place in the presence of at least the calculated amount of water, a catalytic amount of an inorganic one or organic acid, such as. B.

Salzsäure, Schwefelsäure, p-Toluolsulfonsäure oder Oxalsäure, oder sauer reagierenden Salzen, wie Zinc12, NaHSO4, und zweckmäßig in Gegenwart eines organischen Lösungsmittels, das in der 2-bis 4fachen Menge, bezogen auf den eingesetzten Methylenäther, dem Umsetzungsgemisch zugesetzt wird.Hydrochloric acid, sulfuric acid, p-toluenesulfonic acid or oxalic acid, or acidic salts such as Zinc12, NaHSO4, and expediently in the presence one organic solvent, in 2 to 4 times the amount, based on the amount used Methylene ether, is added to the reaction mixture.

Als Lösungsmittel kommen vor allem niedere Alkohole, wie z. B. Methanol, in Frage, welche mit dem abgespaltenen Formaldehyd unter Bildung von Dimethylformal reagieren. Infolge ihres niedrigen Siedepunktes lassen sich diese leicht aus dem Umsetzungsgemisch herausdestillieren. Aber auch Methylbutyläther, Dioxan, Tetrahydrofuran sind geeignete Lösungsmittel ; in diesem Falle kann der abgespaltene Formaldehyd mit Hilfe eines Stickstoffstromes aus dem Umsetzungsgemisch entfernt werden.Lower alcohols, such as. B. methanol, in question, which with the split off formaldehyde to form dimethyl formal react. Due to their low boiling point, these can be easily removed from the Distill out the reaction mixture. But also methyl butyl ether, dioxane, tetrahydrofuran are suitable solvents; in this case the split off formaldehyde can be removed from the reaction mixture with the aid of a stream of nitrogen.

Die Hydrolyse der Methylenäther wird bei erhöhter Temperatur, am besten bei der Siedetemperatur des angewandten Lösungsmittels, durchgeführt. Zur Isolierung der Halogenhydroxyalkane wird zunächst das Lösungsmittel abdestilliert und dann der Rückstand zur Entfernung des im Überschuß zugesetzten Wassers in Äther oder einem anderen Lösungsmittel aufgenommen. Die Halogenhydroxyalkane erhält man dann durch Destillation der ätherischen Lösung. The hydrolysis of the methylene ethers is carried out at an elevated temperature, am best carried out at the boiling point of the solvent used. To the Isolation of the halohydroxyalkanes, the solvent is first distilled off and then the residue to remove the excess water in ether or another solvent. The halohydroxyalkanes are obtained then by distilling the essential solution.

Die Verbindungen stellen auf Grund ihrer funktionellen Gruppen wertvolle Zwischenprodukte für weitere Synthesen dar. The compounds are valuable because of their functional groups Are intermediates for further syntheses.

Beispiel 1 In einen Kolben, der mit gut wirkender Kolonne und einem Destillieraufsatz versehen ist, gibt man ein Gemisch von 50 g 1-Chlor-3-methylbuten- (1)-diol-(2, 3)-methylenäther-(2, 3), 125 ccm Methanol, 30 ccm Wasser und 5 ccm konzentrierter Salzsäure und kocht zunächst so lange unter Rückfluß, bis die Siedetemperatur am Kopf der Kolonne von 65 auf etwa 42°C gefallen ist. Bei dieser Temperatur beginnt man, bei einem Rücklaufverhältnis von etwa 1 : 10 das gebildete Dimethylformal abzudestillieren. Nach etwa 3 Stunden ist die Hydrolyse beendet und die Hauptmenge (31 ccm) des gebildeten Dimethylformals überdestilliert. Zur weiteren Aufarbeitung destilliert man unter leicht vermindertem Druck Methanol ab und nimmt den verbliebenen Rückstand nach Zugabe von konzentrierter Kochsalzlösung in Äther auf. Durch Destillation der Ätherlösung erhält man 35 g l-Chlor-3-methyl-butanol- (3)-on- (2) vom Siedepunkt Kpsls = 99 bis 100° C, entsprechend 77°/0 der Theorie, nt') 1, 459 ; D@20= 1, 179 ; Semicarbazon Schmp. 141 bis 142°C. Example 1 In a flask with a good working column and a Distillation attachment is provided, a mixture of 50 g of 1-chloro-3-methylbutene is (1) -diol- (2, 3) -methylene ether- (2, 3), 125 cc of methanol, 30 cc of water and 5 cc concentrated hydrochloric acid and refluxed until the boiling point at the head of the column from 65 to about 42 ° C has fallen. At this Temperature begins at a reflux ratio of about 1:10 the formed To distill off dimethyl formal. After about 3 hours, the hydrolysis is complete and the bulk (31 ccm) of the dimethyl formal formed distilled over. To further Working up, methanol is distilled off under slightly reduced pressure and taken the remaining residue after the addition of concentrated sodium chloride solution in ether on. By distilling the ethereal solution, 35 g of 1-chloro-3-methyl-butanol (3) -on- (2) from the boiling point Kpsls = 99 to 100 ° C, corresponding to 77 ° / 0 of theory, nt ') 1.459; D @ 20 = 1. 179; Semicarbazone m.p. 141 to 142 ° C.

Beispiel 2 In der im Beispiel I beschriebenen Weise erhitzt man ein Gemisch von 96, 5 g 1-Brom-3-methylbuten-(l)-diol- (2, 3)-methylenäther- (2, 3), 200 ccm Methanol, 50 ccm Wasser und 8 ccm konzentrierter Salzsäure zum Sieden und destilliert laufend das gebildete Dimethylformal ab. Nach 3 Stunden sind insgesamt 41 ccm Dimethylformal überdestilliert. Die Aufarbeitung erfolgt in der im Beispiel I angegebenen Weise mittels Äther und Kochsalzlösung. Durch Destillation des Ätherauszuges erhält man als Hauptfraktion 68, 5 g 1-Brom-3-methyl-butanol- (3)-on- (2) vom Siedepunkt Kp.13 = 99 bis 103°C ; Ausbeute 75, 7°/0 der Theorie ; nD20 = 1, 484 ; D. 1, 494 ; Semicarbazon F. = 122 bis 123°C. Example 2 The mixture is heated in the manner described in Example I Mixture of 96.5 g of 1-bromo-3-methylbutene- (l) -diol- (2, 3) -methylene ether- (2, 3), 200 cc of methanol, 50 cc of water and 8 cc of concentrated hydrochloric acid for boiling and the dimethyl formal formed is continuously distilled off. After 3 hours are in total 41 cc of dimethyl formal distilled over. The work-up is carried out in the example I indicated way by means of ether and saline solution. By distilling the ether extract the main fraction obtained is 68.5 g of 1-bromo-3-methyl-butanol- (3) -one- (2) with a boiling point Bp 13 = 99 to 103 ° C; Yield 75.7% of theory; nD20 = 1.484; D. 1,494 ; Semicarbazone F. = 122 to 123 ° C.

Beispiel 3 Entsprechend den Beispielen 1 und 2 wird ein Gemisch von 50g g 1-Chlor-3-methylpenten- (I)-diol-(2, 3)-methylenäther- (2, 3), 125 ccm Methanol, 30 ccm Wasser und 5 ccm konzentrierter Salzsäure 3 Stunden zum Sieden erhitzt und das gebildete Dimethylformal abdestilliert. Durch Aufarbeitung in der oben beschriebenen Weise erhält man 40, 8 g 1-Chlor-3-methyl-pentanol- (3)-on- (2), entsprechend einer Ausbeute von 88% der Theorie, Kip. je = 101 bis 103°C ; nD20 = 1, 460 ; D.'« = 1, 143 ; Semicarbazon F.-124 bis 126°C. Example 3 According to Examples 1 and 2, a mixture of 50g g of 1-chloro-3-methylpentene- (I) -diol- (2, 3) -methylene ether- (2, 3), 125 ccm of methanol, 30 cc of water and 5 cc of concentrated hydrochloric acid heated to boiling for 3 hours and the dimethyl formal formed is distilled off. By working up in the manner described above 40.8 g of 1-chloro-3-methyl-pentanol- (3) -one- (2) are obtained, corresponding to one Yield of 88% of theory, Kip. each = 101 to 103 ° C; nD20 = 1,460; D. '«= 1, 143; Semicarbazone m.p.-124 to 126 ° C.

In der gleichen Weise wurden durch Hydrolyse von 70 g I-Brom-3-methylpenten- (])-diol- (2, 3)-methylenäther-(2, 3) 51, 2g (= 77, 5°/o der Theorie) l-Brom-3-methyl-pentanol- (3)-on- (2) erhalten : Kp. 15 = 110 bis 113°C, nD20 = 1,479; D.D20 = 1,373; Semicarbazon F. 117 bis 1 18 y C. In the same way, by hydrolysis of 70 g of I-bromo-3-methylpentene (]) - diol- (2, 3) -methylene ether- (2, 3) 51.2g (= 77.5% of theory) l-bromo-3-methylpentanol- (3) -on- (2) obtained: bp 15 = 110 to 113 ° C, nD20 = 1.479; D.D20 = 1.373; Semicarbazone F. 117 to 1 18 y C.

Beispiel 4 Man kocht ein Gemisch von 94, 25 g des Methylenäthers von 1-Chlor-2-[cyclohexanol-(1')-yl]-äthen-(1)-ol-(2) mit 150 ccm Methanol, 30 ccm Wasser und 5 ccm konzentrierter Salzsäure 3 Stunden unter Rückfluß und destilliert das gebildete Dimethylformal laufend ab. Durch Aufarbeitung des Reaktionsgemisches in der im Beispiel I beschriebenen Weise erhält man 74, 8 g (= 84, 8 0/, der Theorie) I-Chlor-2-[cyclohexanol- (l')-yl]-äthanon- (2) ; Kp. o, s = 77 bis 81°C ; Schmp. 67 bis 69 (aus Cyclohexan). Example 4 A mixture of 94.25 g of the methylene ether is boiled of 1-chloro-2- [cyclohexanol- (1 ') - yl] -ethen- (1) -ol- (2) with 150 cc of methanol, 30 cc Water and 5 cc of concentrated hydrochloric acid under reflux and distilled for 3 hours the dimethyl formal formed continuously. By working up the reaction mixture in the manner described in Example I, 74.8 g (= 84.8 0 /, of theory) are obtained I-chloro-2- [cyclohexanol- (1 ') - yl] -ethanone- (2); B.p. o, s = 77 to 81 ° C; M.p. 67 to 69 (from cyclohexane).

Durch Hydrolyse von 116, 5 g des Methylenäthers von I-Brom-2-[cyclohexanol-(1')-yl]-äthen-(1)-ol-(2) wurden in gleicher Weise 82g (= 74°10 der Theorie) I-Brom-2-[cyclohexanol-(1')-yl]-äthanon-(2) erhalten. By hydrolysis of 116.5 g of the methylene ether of I-bromo-2- [cyclohexanol- (1 ') - yl] -ethen- (1) -ol- (2) were in the same way 82g (= 74 ° 10 of theory) I-bromo-2- [cyclohexanol- (1 ') - yl] -ethanone- (2) obtain.

Claims (1)

Kip. 2= 108 bis 109°C : Schmp. 30 bis 31°C; nD20 -1, 5162 ; D.420-1, 430 (unterkühlt.) PATENTANSPRUCH : Verfahren zur Herstellung von l-Halogen-3-hydroxy-alkanonen- (2) der allgemeinen Formel XCH2-CO COH(R1R2) wobei X ein Halogenatom und Rl und R2 Wasserstoffatome oder Alkylreste bedeuten, die auch zu einem cycloaliphatischen Rest verbunden sein können, dadurch gekennzeichnet, daß man 1-Halogenalken- (I)-diol- (2, 3)-niethylen5ther- (2, 3) der allgemeinen Formel R1 XCH=C C R2 O 0 CH2 in saurem, wäßrigem Medium erhitzt.Kip. 2 = 108 to 109 ° C: m.p. 30 to 31 ° C; nD20 -1,5162; D.420-1, 430 (supercooled.) PATENT CLAIM: Process for the production of l-halogen-3-hydroxy-alkanone- (2) of the general formula XCH2-CO COH (R1R2) where X is a halogen atom and Rl and R2 denotes hydrogen atoms or alkyl radicals which also form a cycloaliphatic Rest can be connected, characterized in that 1-haloalkene (I) -diol- (2, 3) -niethylen5ther- (2, 3) of the general formula R1 XCH = C C R2 O 0 CH2 in acidic, heated aqueous medium.
DEC21743A 1960-06-22 1960-06-22 Process for the preparation of 1-halogen-3-hydroxy-alkanones- (2) Pending DE1142350B (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0296488A3 (en) * 1987-06-24 1989-05-03 Basf Aktiengesellschaft Method for the production of unsaturated and saturated ketones

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0296488A3 (en) * 1987-06-24 1989-05-03 Basf Aktiengesellschaft Method for the production of unsaturated and saturated ketones

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