US2575014A - Production of aliphatic di-ketones - Google Patents

Production of aliphatic di-ketones Download PDF

Info

Publication number
US2575014A
US2575014A US85709A US8570949A US2575014A US 2575014 A US2575014 A US 2575014A US 85709 A US85709 A US 85709A US 8570949 A US8570949 A US 8570949A US 2575014 A US2575014 A US 2575014A
Authority
US
United States
Prior art keywords
ketones
ferrous
hydroperoxide
parts
solution
Prior art date
Legal status (The legal status 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 status listed.)
Expired - Lifetime
Application number
US85709A
Inventor
Hawkins Edwin George Edward
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Distillers Co Yeast Ltd
Distillers Co Ltd
Original Assignee
Distillers Co Yeast Ltd
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 Distillers Co Yeast Ltd filed Critical Distillers Co Yeast Ltd
Application granted granted Critical
Publication of US2575014A publication Critical patent/US2575014A/en
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

Links

Classifications

    • 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
    • C07C45/53Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by pyrolysis, rearrangement or decomposition of hydroperoxides

Definitions

  • the present invention is for a process for producing aliphatic di-ketones, in particular long chain di-ketones, and their derivatives bythe treatment of peroxidic compounds, and to compounds produced thereby.
  • the principal object of the invention is to produce a simple process for the production of such di-ketones and to produce useful products thereby.
  • the invention accordingly comprises the novel products as well as the novel processes and steps of processes according to which such products are manufactured, the specific. embodiments of which are described hereinafter by way of ex;- ample and in accordance, with which it is now preferred to practice the invention. 7
  • a suitable ferrous salt is, for instance, ferrous. sulphate, which is preferably used in aqueous solution.
  • Other ferrous salts are, for example, ferrous chloride, ferrous acetate, ferrous lactate.
  • cyclopentane isopropyl cyclopentane, methyl c'yclohexane, ethyl cyclohexane, isopropyl cyclohexane.
  • the proportion of the components of the reaction may vary.
  • the process according to this invention ma ,be carriedout by bringing the hydroperoxide of the said alicyclic hydrocarbons into intimate contact with for instance, ferrous sulphate, preferably in aqueous solution.
  • the reaction may be carried out with a solution of the hydroperoxide for instance in the unchanged 'alicyclic hydrocarbon which contains only a small percentage of the hydroperoxide.
  • solutions are obtained in the well known way for instance j when the alicyclic hydrocarbon is oxidised by means of molecular oxygen for the preparation "of its hydroperoxide without separating the latter from the unchanged hydrocarbon.
  • the process of this invention for c to the process of this invention is exothermic so the production of aliphatic di-ketones comprises carry out" the reaction in acid solution, preferably g acidified by mineral acid such as sulphuric acid.
  • the amount of acid is conveniently such as to prevent the iron from-being precipitated. 1
  • the di-ketone formed may be separated by, forinstance, decanting the organic solution from the aqueous phase and subsequently distilling the organic solution whereby unreacted hydrocarbon which served as a solvent, 'distils off.
  • hydrocarbon any alcohols and/or mono-ketones which are present in the reaction mixture distil From the residue the di-ketone over as well. Crystallises out or may be precipitated therefrom by the addition of a liquid for instance petrol ether in which the di-ketone is insoluble.
  • the di-ketones produced according to the process of this invention may be used for the preparation by oxidation of di-basic acids such as sebacic acid, suberic acid and the like.
  • Example 3 10 parts of methylcyclopetane hydroperoxide (87.2% pure) dissolved in 10 parts of ethanol were added slowly with stirring to a solution of 30 parts of crystalline ferrous sulphate, '7 parts of sulphuric acid, 32 parts of ethanol, and 70 parts of water. 4.4 parts of dodecanedione-Zzll were obtained which was isolated by filtration.
  • Example 4 10 parts of methylcyclopentane hydroperoxide (95.6% pure) was converted into its sodium salt by dissolution in the calculated quantity of 10% sodium hydroxide solution, and the aqueous solution soobtained was added slowly with stirring to a solution of 30 parts of crystalline ferrous sulphate made up to 100 parts with water. The precipitated iron hydroxide was dissolved by acidification, and the organic product was isolated by extraction with ether. 2.9 parts of dodecanedione-2:11 and 2.6 parts of a fraction consisting of alcohols and mono-ketones were thereby obtained.
  • a process which comprises reacting the oxidate solution resulting from reacting the alkyl substituted saturated alicyclic hydrocarbon ring "selected from the group consisting of cyclopentane and cyclohexane with molecular oxygen-to convert part of said hydrocarbon into the corresponding hydroperoxide so that unreacted hydro- ,carbon is present, with aqueous ferrous salt solu- "tion and recovering t di-ketone produced thereby from its solution in the unreacted hydrocarbon.

Landscapes

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

Description

Patented Nov. 13, 1951 \PATEN T OFFICE I 1 PRODUCTION OF ALIPHATIC DI-KETVONEVSV Edwin George Edward Hawkins, Lower Kingswood, Tadworth, England, assignor to The Distillers Company Limited, Edinburgh, Scotland,
a British company No'Drawing. Application A ril5, 1949, Serial No. 85,709. In Great Britain April 29, 1948 The present invention is for a process for producing aliphatic di-ketones, in particular long chain di-ketones, and their derivatives bythe treatment of peroxidic compounds, and to compounds produced thereby.
It is known that hydroperoxides on reacting with ferrous sulphateyield ketones. Hook and Lang have described in Ber. 75 (1 942) 1 51 and Ber. '76 (1943) 1130 that the hydroperoxides of, indane and octa hydroanthracene react when heated with aqueous ferrous sulphate solution and are decomposed catalytically with the formation of ketones which possess the same number; of carbon atoms. The same applies to ethylbenzene hydroperoxide which yields acetophenone on being heated with an aqueous ferrous sol-- phate solution (ibidern 76 (1943) 172).
It has now been discovered in accordance with this invention that hydroperoxides of compounds wherein the peroxide group is attached to a tertiary carbon atom, which forms part ,ofthe saturated alicyclic hydrocarbon ring of cyclopentane or cyclohexane and at the same time. is
linked to an alkyl group attached to said ring,
react with ferrous compounds with the production of di-ketones. Fission of the linkage between the tertiary carbon atomand an adjacent carbon atom in the ring takes place and at the same time identical radicals link up together so' that di-ketones with double the. number of carbon atoms in the molecule are formed. The following formula for methyl cyclopentane hydro-- peroxide illustrates the reaction occurring:
0 onaaLqoHcr -cn.
The principal object of the invention is to produce a simple process for the production of such di-ketones and to produce useful products thereby. A I
The invention accordingly comprises the novel products as well as the novel processes and steps of processes according to which such products are manufactured, the specific. embodiments of which are described hereinafter by way of ex;- ample and in accordance, with which it is now preferred to practice the invention. 7
6 Claims. ((21.2'60-593) 2 reacting with a solution of a ferrous salt a hydroperoxide of an alkyl substituted alicyclic hydro-v carbon ringselected from the group consisting off cyclopentane and cyclohexane wherein the peroxide group is attachedto a tertiary carbon atom.
which forms part of said hydrocarbon ring andwhich is also attached to said alkyl group, the. di-ketones produced having twice as many car- Do bon atoms as the said ring compound.
A suitable ferrous salt is, for instance, ferrous. sulphate, which is preferably used in aqueous solution. Other ferrous salts are, for example, ferrous chloride, ferrous acetate, ferrous lactate.
,Alicyclic hydrocarbons, the hydroperoxides ;of{, -which may be subjected to the treatment of thei present invention and thereby yield di-k'etones, arefor instancebut without limitation thereto. methyl cyclopentane, ethyl cyclopentane, pr'opyl.
. cyclopentane, isopropyl cyclopentane, methyl c'yclohexane, ethyl cyclohexane, isopropyl cyclohexane. The proportion of the components of the reaction may vary.
The process according to this invention ma ,be carriedout by bringing the hydroperoxide of the said alicyclic hydrocarbons into intimate contact with for instance, ferrous sulphate, preferably in aqueous solution. Alternatively, the reaction may be carried out with a solution of the hydroperoxide for instance in the unchanged 'alicyclic hydrocarbon which contains only a small percentage of the hydroperoxide. Such solutions are obtained in the well known way for instance j when the alicyclic hydrocarbon is oxidised by means of molecular oxygen for the preparation "of its hydroperoxide without separating the latter from the unchanged hydrocarbon. In this case, it is preferred to treat the hydroperoxi'decontaining reaction mixture resulting from" the oxidation process with water or a solution of aqueous solution. It is preferred, however, to
Accordingly the process of this invention for c to the process of this invention is exothermic so the production of aliphatic di-ketones comprises carry out" the reaction in acid solution, preferably g acidified by mineral acid such as sulphuric acid. The amount of acid is conveniently such as to prevent the iron from-being precipitated. 1 The reaction of: the hydroperoxides according out and may be recovered directly by filtration.-
When a" solution of the hydroperoxide in unreacted hydrocarbon such as the crude oxidate, is
treated according to the present invention the di-ketone formed may be separated by, forinstance, decanting the organic solution from the aqueous phase and subsequently distilling the organic solution whereby unreacted hydrocarbon which served as a solvent, 'distils off. With the hydrocarbon any alcohols and/or mono-ketones which are present in the reaction mixture distil From the residue the di-ketone over as well. crystallises out or may be precipitated therefrom by the addition of a liquid for instance petrol ether in which the di-ketone is insoluble.
As by-products of the reaction with the ferrous salt according to the invention, alcohols and mono-ketones are produced. In the case of methyl cyclopentane hydroperoxide the ketone formed as such a by-product is mainly methylbutyl ketone. These alcohols and mono-ketones may be removed if desired by distillation. The ferric compounds produced during the reaction by oxidation of the ferrous compounds may be reconverted to ferrous compounds by reduction, for instance with sulphur dioxide.
The di-ketones produced according to the process of this invention may be used for the preparation by oxidation of di-basic acids such as sebacic acid, suberic acid and the like.
-The following examples illustrate the manner in which the process of the invention may be carried out in practice the quantities given being parts by weight.
Example 1 parts of methyl cyclopentane hydroperoxide were shaken at room temperature with 100 parts of water in which 62 parts of crystalline ferrous sulphate had been dissolved. The temperature of the reaction mixture rose considerably whilst a brown iron hydroxide deposit settled out. The reaction mixture after having been cooled was Example 2 '20 parts of methyl cyclohexane hydroperoxide were heated on a water bath for 3 hours with an aqueous solution containing parts of crystalline ferrous sulphate. The product was ether extracted and distilled. A fraction containing ketones and alcohols was obtained, weighing 15.0
parts,- whilst 1.7 parts of a fraction consisting 1 mainly of tetradecanedione-2213 was obtained. This di-ketone is insoluble in water, and soluble in most organic solvents. It crystallises in white shining leaflets with a M. P. of 76-77" C.
Example 3 10 parts of methylcyclopetane hydroperoxide (87.2% pure) dissolved in 10 parts of ethanol were added slowly with stirring to a solution of 30 parts of crystalline ferrous sulphate, '7 parts of sulphuric acid, 32 parts of ethanol, and 70 parts of water. 4.4 parts of dodecanedione-Zzll were obtained which was isolated by filtration.
A similar experiment in which the sulphuric acid was omitted yielded only 3.2 parts of dodecanedione.
. v Example 4 10 parts of methylcyclopentane hydroperoxide (95.6% pure) was converted into its sodium salt by dissolution in the calculated quantity of 10% sodium hydroxide solution, and the aqueous solution soobtained was added slowly with stirring to a solution of 30 parts of crystalline ferrous sulphate made up to 100 parts with water. The precipitated iron hydroxide was dissolved by acidification, and the organic product was isolated by extraction with ether. 2.9 parts of dodecanedione-2:11 and 2.6 parts of a fraction consisting of alcohols and mono-ketones were thereby obtained.
Equivalent quantities of ferrous chloride, ferrous acetate and ferrous lactate may be used in,
said ring compound.
2. A process according to claim 1 wherein the solution of the ferrous salt is an aqueous solution of ferrous sulphate.
3. A process according to claim 1 wherein the reaction is effected under acid conditions.
4. A process according to claim 1 wherein the hydroperoxide is methyl cyclopentane hydroperoxide.
5. A process according to claim 1 wherein the hydroperoxide is methyl cyclohexane hydroperoxide.
6. A process which comprises reacting the oxidate solution resulting from reacting the alkyl substituted saturated alicyclic hydrocarbon ring "selected from the group consisting of cyclopentane and cyclohexane with molecular oxygen-to convert part of said hydrocarbon into the corresponding hydroperoxide so that unreacted hydro- ,carbon is present, with aqueous ferrous salt solu- "tion and recovering t di-ketone produced thereby from its solution in the unreacted hydrocarbon.
I EDWIN GEORGE EDWARD HAWKINS.
REFERENCES CITED The following references are of record in the file of this patent:
Work, J. Chem. Soc., 1940 vol., pages 1307-1315.
fHock et al., Berichte, vol. 75, pages 1051-1054 (1942); vol. 76, pages 1130-1131 (1943); vol. 76, pages 169-172 (1943).

Claims (1)

1. A PROCESS WHICH COMPRISES REACTING WITH A SOLUTION OF A FERROUS SALT IN THE PRESENCE OF SOME WATER, A HYDROPEROXIDE IN THE ALKYL SUBSTITUTED SATURATED ALICYCLIC HYDROCARBON RING SELECTED FROM THE GROUP CONSISTING OF CYCLOPENTANE AND CYCLOHEXANE WHEREIN THE PEROXIDE GROUP IS ATTACHED TO A TERTIARY CARBON ATOM WHICH FORMS PART OF SAID HYDROCARBON RIGN AND IS ALSO ATTACHED TO SAID ALKYL GROUP, THE DI-KETONE PRODUCED HAVING TWICE AS MANY CARBON ATOMS AS THE SAID RING COMPOUND.
US85709A 1948-04-29 1949-04-05 Production of aliphatic di-ketones Expired - Lifetime US2575014A (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
GB2575014X 1948-04-29

Publications (1)

Publication Number Publication Date
US2575014A true US2575014A (en) 1951-11-13

Family

ID=10910522

Family Applications (1)

Application Number Title Priority Date Filing Date
US85709A Expired - Lifetime US2575014A (en) 1948-04-29 1949-04-05 Production of aliphatic di-ketones

Country Status (1)

Country Link
US (1) US2575014A (en)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2671810A (en) * 1952-05-24 1954-03-09 Du Pont Long-chain diketones
US2700057A (en) * 1952-03-28 1955-01-18 Du Pont Process for preparing 2, 13-tetradecanedione from 1-methylcyclohexyl hydroperoxide
US2798096A (en) * 1954-02-17 1957-07-02 Exxon Research Engineering Co Production of cyclic hydroperoxides
US2822399A (en) * 1953-05-01 1958-02-04 Du Pont Manufacture of diketones

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
None *

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2700057A (en) * 1952-03-28 1955-01-18 Du Pont Process for preparing 2, 13-tetradecanedione from 1-methylcyclohexyl hydroperoxide
US2671810A (en) * 1952-05-24 1954-03-09 Du Pont Long-chain diketones
US2822399A (en) * 1953-05-01 1958-02-04 Du Pont Manufacture of diketones
US2798096A (en) * 1954-02-17 1957-07-02 Exxon Research Engineering Co Production of cyclic hydroperoxides

Similar Documents

Publication Publication Date Title
US3847993A (en) Allylic oxidation of bicyclic hydrocarbons to alcohols and ketones
US2859247A (en) Process for the preparation of bicyclic ketones
US1841768A (en) Chlorinated and brominated ethine carbinols
US2575014A (en) Production of aliphatic di-ketones
US2671809A (en) Controlled decomposition of aralkyl hydroperoxides
US2669588A (en) Production of bis (hydroxyaryl) substituted compounds
US3035091A (en) Carboxylated bisphenol compounds
US2870200A (en) Production of unsaturated polycarboxylic acids and esters
US2816913A (en) Preparation of substituted acids
Lambert et al. 9. Aliphatic nitro-compounds. Part XIX. Friedel–Crafts reactions with α-and β-nitro-olefins
US2594322A (en) Substituted oxacycloalkanes
US2677703A (en) Production of bibenzyl dicarboxylic acids
US2826600A (en) Preparation of thioethyl isophthalates
US2905712A (en) Acids and ketones prepared from peroxides and polyhalomethanes
US3187020A (en) Process for preparing diazides
US2633476A (en) Production of aromatic hydroperoxides
Walling et al. The Hydroperoxides from l-Bornyl Chloride Obtained by Oxidation of the Grignard Reagent1
US2547123A (en) Processes for preparing artificial oestrogenic compounds and products obtained thereby
US2967197A (en) Difunctional aliphatic compounds prepared from peroxides and halogens
US2635114A (en) Polyalkylbenzene carboxylic acid and process of preparing it
US2799703A (en) Manufacture of propiolic acid
US3026334A (en) Process for obtaining epsilon-substituted derivatives of caproic acid and its homologues, and the products thereof
EP0089586B1 (en) 2-alkyl-2,4-diacyloxy-3-butenals
US3177244A (en) Formation of high molecular weight compounds
US2781397A (en) Process for preparing polycyclic dibasic acid