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US2510731A - Method of making alkyldihydrothebainones - Google Patents

Method of making alkyldihydrothebainones Download PDF

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US2510731A
US2510731A US667108A US66710846A US2510731A US 2510731 A US2510731 A US 2510731A US 667108 A US667108 A US 667108A US 66710846 A US66710846 A US 66710846A US 2510731 A US2510731 A US 2510731A
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methyldihydrothebainone
making
methyl magnesium
dihydrocodeinone
solution
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US667108A
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Frank C Whitmore
August H Homeyer
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Mallinckrodt Chemical Works
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Mallinckrodt Chemical Works
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D221/00Heterocyclic compounds containing six-membered rings having one nitrogen atom as the only ring hetero atom, not provided for by groups C07D211/00 - C07D219/00
    • C07D221/02Heterocyclic compounds containing six-membered rings having one nitrogen atom as the only ring hetero atom, not provided for by groups C07D211/00 - C07D219/00 condensed with carbocyclic rings or ring systems
    • C07D221/22Bridged ring systems
    • C07D221/28Morphinans

Definitions

  • This invention relates to the. manufacture. of narcotics and more articularly to. methodsior them-operation of intermediates for. the manu-. iacture of methyldihydromorphinone.
  • the invention accordingly comprises the steps and sequence of steps, and features ofsynthesis, analysis, or metathesis, which will; be. exemplifled. in the processes hereinafter described, and the. scope of the application of which. wilLbe-indicated in the following. claims.
  • methyldihydroinon. phinone In the manufacture of. methyldihydroinon. phinone. one of the, intermediates customarily, utilized; is. methyldihydrothebainone. This. in: termediate may be. prepared from thebaine by hydrogenation to dihydrothebaine, followed by reaction with a. Grignard reagent. to formin'ethe yldihydrothehainone It' has been found, hows ever, that on hydrogenation of thebaine, relatively small. quantities of dihydrothebaineiv are. obtained. together with larger quantities ofv dihydrothebainone.
  • Dihydrotheoainone has. been of'limited utility because to convert. ittothe desired methyldihy-- drothebainone ithasbeen necessary-toifirstform dihydrocodeinone, then the acetate or the enol' forinof dihydrocodeinone, and then to form the desired methyl derivative, methyldihydrothebainone.-
  • Example I Two molesof methyl magnesium iodide solution. (1310. cc. of. 1.53 N), was distilled in a 5 liter,
  • the'complex was decomposed by adding to the flask excess dilute hydrochloric acid (about 350 1 cc. concentrated hydrochloric acid diluted to 2 liters) and the benzene layer was separated and washed with dilute hydrochloric acid'whichwasadded-to the main aqueous phase.
  • the aqueous phase- was stirred with 1 liter of chloroform and ammonia-cal by adding a small excess of" 1 1.1 g, or"4:7-% of the theoreticalyield;
  • Example II itizruetherv solution. of-206cc. ofmethyl mag l cur 580 cc. portions of chloroform and the" inedextracts were distilled to dryness.
  • 270 cc. of dry benzene was added and the condenser was arranged for refluxing. After bringing to refluxing temperature, a warm solution of 40 grams of dihydrocodeinone in 700 cc. of dry benzene was added during 18 minutes. The solution was stirred and refluxed for one and one-half hours and then was refluxed without stirring for four and one half hours more.
  • methyl magnesium halides may be substituted for the methyl magnesium iodide and methyl magnesium bromide respectively described.
  • Example IV 72.5 grams of crude methyldihydrothebainone hydrochloride was dissolved in 300 cc. of hot water, decolorized with activated carbon and after filtering, 40 grams of sodium bromide was added. Methyldihydrothebainone hydrobromide crystallized rapidly. After cooling it was filtered off and washed with alcohol. The slightly moist hydrobromide weighed 71 grams.
  • the hydrobromide of methyldihydrothebainone can be prepared by reacting the alkaloid with hydrobromic acid or it can be formed by treating the hydrochloride of the alkaloid with a bromide salt.
  • the hydrobromide is of particular value. For example, it has more desirable solubility characteristics than the hydrochloride, and is accordingly of a special utility for purifying the alkaloid.
  • homologs of methyldihydrothebainone may be prepared in an analogous manner by using an appropriate Grignard reagent.
  • chloroform is not only an efiective solvent for this purpose, but it has certain advantages over the previously utilized solvents. For example, extraction with ether is hazardous and clumsy on account of the large volumes of solvent required. Extraction with benzene has a tendency to form stubborn emulsions. Chloroform as a solvent for this purpose is not subject to the foregoing disadvantages. Relatively small proportions of chloroform are effective to extract the methyldihydrothebainone efiiciently from its aqueous solution.
  • methyldihydrothebainone which comprises adding dihydrocodeinone in an aromatic solvent to a methyl Grignard reagent selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide in an aromatic solvent.
  • methyldihydrothebainone which comprises adding dihydrocodeinone to a methyl Grignard reagent selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide in benzene.
  • methyldihydrothebainone which comprises adding dihydrocodeinone in benzene to a methyl Grignard reagent selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide in benzene.
  • methyldihydrothebainone which comprises removing the major portion of the solvent ether from an ethereal solution of a methyl Grignard reagent selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide, adding an aromatic solvent to said Grignard reagent and then adding dihydrocodeinone.
  • a methyl Grignard reagent selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide
  • methyldihydrothebainone which comprises adding a benzene solution of dihydrocodeinone to a benzene solution of a methyl magnesium halide selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide, decomposing the complex formed by adding excess dilute hydrochloric acid, extracting the methyldihydrothebainone with chloroform, purifying the product by forming a hydroha-lide of the methyldihydrothebainone.
  • Fieser and Fieser Organic Chemistry (D. C. 2'364'833 Wemard 1 10 Heath'& Co., 1944; Boston); p. 39 and p.803.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)

Description

Patented June 6, 1950 METHQD or. MAKING ALKYLDIHYDRO-- EBAINQNES.
Frank C. Whitmore, State College, Pa., and August H. Homeyer. Webster-Groves, Md, assigncrs to Mellinc rod h micat Works. St. Louis, Mo. a corporation of Missouri No Drawing. Application May 3, 1946, Serial No. 66?,108
V 9 Claims. (01.
This invention. relates to the. manufacture. of narcotics and more articularly to. methodsior them-operation of intermediates for. the manu-. iacture of methyldihydromorphinone.
Among the objects of this inventionaare the provision or methods, for the. utilization. of byproducts in the manufacture of derivativesof the morphine, series; the provision of .methods for improving the yield of desired products in the manufacture of derivatives of; the morphine series; and theprovision of methods. for more easily preparing intermediates for themanufacture of: methyldihydromorphinona.. Other ob-.- jects willbe in part apparent and inpart pointed out. hereinafter.
The invention accordingly comprises the steps and sequence of steps, and features ofsynthesis, analysis, or metathesis, which will; be. exemplifled. in the processes hereinafter described, and the. scope of the application of which. wilLbe-indicated in the following. claims.
In the manufacture of. methyldihydroinon. phinone. one of the, intermediates customarily, utilized; is. methyldihydrothebainone. This. in: termediate may be. prepared from thebaine by hydrogenation to dihydrothebaine, followed by reaction with a. Grignard reagent. to formin'ethe yldihydrothehainone It' has been found, hows ever, that on hydrogenation of thebaine, relatively small. quantities of dihydrothebaineiv are. obtained. together with larger quantities ofv dihydrothebainone.
Dihydrotheoainone has. been of'limited utility because to convert. ittothe desired methyldihy-- drothebainone ithasbeen necessary-toifirstform dihydrocodeinone, then the acetate or the enol' forinof dihydrocodeinone, and then to form the desired methyl derivative, methyldihydrothebainone.-
In accordance with the-present invention, however, it has been found that dihydrocodeinonecan be directly converted to methyldihydrothebainone without the intermediate formation,
to methyl-dihydrothebainoneby formation, for" example, of the acetyl derivative of'thezenol form:
of dihydrocodcinone, followed by reaction of this product with a Grignard reagent, are materially shortened and improved.
The following examples illustrate the invention:
Example I Two molesof methyl magnesium iodide solution. (1310. cc. of. 1.53 N), was distilled in a 5 liter,
three-necked flask fitted with amercury sealed stirrer, dropping funnel and condenser, until no more other came over with the bath at about C. One liter of. dry benzene was added to the residue, stirred, and heated to boiling, while a solution of 290 g. of dihydrocodeinone in 2 liters of dry benzene was added during 10 minutes. Distillation was continued by heating until 800 cc. of distillate were collected. Then the condenser was set for refluxing which was continued for 3 six hours. A voluminous white solid formed during the addition of the dihydrocodeinone to th'e Grignard reagent. At the end of the reaction, the'complex was decomposed by adding to the flask excess dilute hydrochloric acid (about 350 1 cc. concentrated hydrochloric acid diluted to 2 liters) and the benzene layer was separated and washed with dilute hydrochloric acid'whichwasadded-to the main aqueous phase. The aqueous phase-was stirred with 1 liter of chloroform and ammonia-cal by adding a small excess of" 1 1.1 g, or"4:7-% of the theoreticalyield;
Example II itizruetherv solution. of-206cc. ofmethyl mag l cur 580 cc. portions of chloroform and the" inedextracts were distilled to dryness. The methyldihydrothebainone' nesium bromide containing 0.4 mole was concentrated by distillation in a water bath until no more ether would distill. 270 cc. of dry benzene was added and the condenser was arranged for refluxing. After bringing to refluxing temperature, a warm solution of 40 grams of dihydrocodeinone in 700 cc. of dry benzene was added during 18 minutes. The solution was stirred and refluxed for one and one-half hours and then was refluxed without stirring for four and one half hours more. A test for the presence of a Grignard reagent was negative. The reaction mixture was decomposed by addition of excess dilute hydrochloric acid and then the solution was made alkaline with ammonia, and a little sodium hydrosulfite, NazSzOi, was added. The benzene layer was separated and the Water layer was extracted three times with chloroform. The benzene and chloroform extracts were combined, dried, and concentrated by distillation, the last traces of solvent being removed under reduced pressure. The residue, weighing 32.5 grams, was dissolved in 60 cc. of anhydrous alcohol and the solution was saturated with hydrogen chloride. A precipitate formed immediately and after storing in a refrigerator overnight, it was filtered off and washed with alcohol. The dry methyldihydrothebainone hydrochloride weighed 15.5 grams.
In the foregoing examples other methyl magnesium halides may be substituted for the methyl magnesium iodide and methyl magnesium bromide respectively described.
ExampZe III 12 grams of impure methyldihydrothebainone was suspended in 100 cc. of Water and dissolved by adding hydrobromic acid until all the solid was in solution and the solution was acid to Congo. The solution was decolorized with activated carbon and allowed to crystallize. The crystals of methyldihydrothebainone hydrobromide after drying weighed 12.6 grams.
Example IV 72.5 grams of crude methyldihydrothebainone hydrochloride was dissolved in 300 cc. of hot water, decolorized with activated carbon and after filtering, 40 grams of sodium bromide was added. Methyldihydrothebainone hydrobromide crystallized rapidly. After cooling it was filtered off and washed with alcohol. The slightly moist hydrobromide weighed 71 grams.
As shown in these examples the hydrobromide of methyldihydrothebainone can be prepared by reacting the alkaloid with hydrobromic acid or it can be formed by treating the hydrochloride of the alkaloid with a bromide salt. The hydrobromide is of particular value. For example, it has more desirable solubility characteristics than the hydrochloride, and is accordingly of a special utility for purifying the alkaloid.
It will be understood, of course, that homologs of methyldihydrothebainone may be prepared in an analogous manner by using an appropriate Grignard reagent.
The extraction of the crude methyldihydrothebainone is advantageously carried out by the use of chloroform as indicated in the foregoing examples. chloroform is not only an efiective solvent for this purpose, but it has certain advantages over the previously utilized solvents. For example, extraction with ether is hazardous and clumsy on account of the large volumes of solvent required. Extraction with benzene has a tendency to form stubborn emulsions. Chloroform as a solvent for this purpose is not subject to the foregoing disadvantages. Relatively small proportions of chloroform are effective to extract the methyldihydrothebainone efiiciently from its aqueous solution.
In view of the above, it will be seen that the several objects of the invention are achieved and other advantageous results attained.
As many changes could be made in the above processes without departing from the scope of the invention, it is intended that all matter contained in the above description shall be interpreted as illustrative and not in a limiting sense.
We claim:
1. The method of making an alkyldihydrothebainone which comprises adding dihydrocodeinone to a Grignard reagent selected from the group consisting of an alkyl magnesium bromide and an alkyl magnesium iodide in an aromatic solvent.
2. The method of making methyldihydrothebainone which comprises adding dihydrocodeinone in an aromatic solvent to a methyl Grignard reagent selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide in an aromatic solvent.
3. The method of making methyldihydrothebainone which comprises adding dihydrocodeinone to a methyl Grignard reagent selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide in benzene.
4. The method of making methyldihydrothebainone which comprises adding dihydrocodeinone in benzene to a methyl Grignard reagent selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide in benzene.
5. The method of making methyldihydrothebainone which comprises removing the major portion of the solvent ether from an ethereal solution of a methyl Grignard reagent selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide, adding an aromatic solvent to said Grignard reagent and then adding dihydrocodeinone.
6. The method of making methyldihydrothebainone which comprises adding a benzene solution of dihydrocodeinone to a benzene solution of a methyl magnesium halide selected from the group consisting of a methyl magnesium bromide and a methyl magnesium iodide, decomposing the complex formed by adding excess dilute hydrochloric acid, extracting the methyldihydrothebainone with chloroform, purifying the product by forming a hydroha-lide of the methyldihydrothebainone.
7. The method of making an alkyldihydrothebainone which comprises reacting dihydrocodeinone with a Grignard reagent selected from the group consisting of an alkyl magnesium bromide and an alkyl magnesium iodide in an aromatic solvent.
8. The. method of making an alkyldihydrothebainone which comprises reacting dihydrocodeinone with an alkyl magnesium bromide and an aromatic solvent.
9. The method of making an alkyldihydrothebainone which comprises reacting dihydrocodeinone with alkyl magnesium iodide and an aromatic solvent.
FRANK C. WHITMO-RE. AUGUST H. HOMEYER.
(References on following page) REFERENCES ormn OTfiER REFERENCES The following references are of record in the vLutz at ,1,: J. Am. Chem. Soc., vol. 57, pp. 265ifile of this patent: 2656 (1935).
' Sm 11 t 1.: J. .Ch .SOc., 1.58, .1457- UNITED STATES PATENTS 5 14 3 Au g. 1936) em v0 pp Gilman: Organic Chemistry (John Wiley New Number Name Date 2,178,010 Small et a1 Oct 31. 1939 York, 1938), vol. I, pp. 109, 110 and 556.
Fieser and Fieser: Organic Chemistry (D. C. 2'364'833 Wemard 1 10 Heath'& Co., 1944; Boston); p. 39 and p.803.

Claims (1)

  1. 6. THE METHOD OF MAKING METHYLDIHYDROTHEBAINONE WHICH COMPRISES ADDING A BENZENE SOLUTION OF DIHYDROCODEINONE TO A BENZENE SOLUTION OF A METHYL MAGNESIUM HALIDE SELECTED FROM THE GROUP CONSISTING OF A METHYL MAGNESIUM BROMIDE AND A METHYL MAGNESIUM IODIDE, DECOMPOSING THE COMPLEX FORMED BY ADDING EXCESS DILUTE HYDROCHLORIC ACID, EXTRACTING THE METHYLDIHYDROTHEBAINONE WITH CHLOROFORM, PURIFYING THE PRODUCT BY FORMING A HYDROHALIDE OF THE METHYLDIHYDROTHEBAINONE.
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Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2178010A (en) * 1937-02-03 1939-10-31 Small Lyndon Frederick Nuclear substituted derivatives of the morphine series and methods for their preparation
US2364833A (en) * 1941-12-06 1944-12-12 Merck & Co Inc N-allylnormorphine and processes for its production

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2178010A (en) * 1937-02-03 1939-10-31 Small Lyndon Frederick Nuclear substituted derivatives of the morphine series and methods for their preparation
US2364833A (en) * 1941-12-06 1944-12-12 Merck & Co Inc N-allylnormorphine and processes for its production

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