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CA1050995A - Process for the production of heterocyclic compounds and products obtained thereby - Google Patents

Process for the production of heterocyclic compounds and products obtained thereby

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Publication number
CA1050995A
CA1050995A CA205,349A CA205349A CA1050995A CA 1050995 A CA1050995 A CA 1050995A CA 205349 A CA205349 A CA 205349A CA 1050995 A CA1050995 A CA 1050995A
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CA
Canada
Prior art keywords
reaction
carried out
process according
formula
oxygen
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
Application number
CA205,349A
Other languages
French (fr)
Other versions
CA205349S (en
Inventor
Paolo Koch
Emilio Perrotti
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.)
Anic SpA
Original Assignee
Anic SpA
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Filing date
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Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D263/00Heterocyclic compounds containing 1,3-oxazole or hydrogenated 1,3-oxazole rings
    • C07D263/02Heterocyclic compounds containing 1,3-oxazole or hydrogenated 1,3-oxazole rings not condensed with other rings
    • C07D263/08Heterocyclic compounds containing 1,3-oxazole or hydrogenated 1,3-oxazole rings not condensed with other rings having one double bond between ring members or between a ring member and a non-ring member
    • C07D263/16Heterocyclic compounds containing 1,3-oxazole or hydrogenated 1,3-oxazole rings not condensed with other rings having one double bond between ring members or between a ring member and a non-ring member with hetero atoms or with carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals, directly attached to ring carbon atoms
    • C07D263/18Oxygen atoms
    • C07D263/20Oxygen atoms attached in position 2
    • C07D263/22Oxygen atoms attached in position 2 with only hydrogen atoms or radicals containing only hydrogen and carbon atoms, directly attached to other ring carbon atoms
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D263/00Heterocyclic compounds containing 1,3-oxazole or hydrogenated 1,3-oxazole rings
    • C07D263/02Heterocyclic compounds containing 1,3-oxazole or hydrogenated 1,3-oxazole rings not condensed with other rings
    • C07D263/08Heterocyclic compounds containing 1,3-oxazole or hydrogenated 1,3-oxazole rings not condensed with other rings having one double bond between ring members or between a ring member and a non-ring member
    • C07D263/16Heterocyclic compounds containing 1,3-oxazole or hydrogenated 1,3-oxazole rings not condensed with other rings having one double bond between ring members or between a ring member and a non-ring member with hetero atoms or with carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals, directly attached to ring carbon atoms
    • C07D263/18Oxygen atoms
    • C07D263/20Oxygen atoms attached in position 2
    • C07D263/24Oxygen atoms attached in position 2 with hydrocarbon radicals, substituted by oxygen atoms, attached to other ring carbon atoms
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D277/00Heterocyclic compounds containing 1,3-thiazole or hydrogenated 1,3-thiazole rings
    • C07D277/02Heterocyclic compounds containing 1,3-thiazole or hydrogenated 1,3-thiazole rings not condensed with other rings
    • C07D277/08Heterocyclic compounds containing 1,3-thiazole or hydrogenated 1,3-thiazole rings not condensed with other rings having one double bond between ring members or between a ring member and a non-ring member
    • C07D277/12Heterocyclic compounds containing 1,3-thiazole or hydrogenated 1,3-thiazole rings not condensed with other rings having one double bond between ring members or between a ring member and a non-ring member with hetero atoms or with carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals, directly attached to ring carbon atoms
    • C07D277/14Oxygen atoms
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D339/00Heterocyclic compounds containing rings having two sulfur atoms as the only ring hetero atoms
    • C07D339/02Five-membered rings
    • C07D339/06Five-membered rings having the hetero atoms in positions 1 and 3, e.g. cyclic dithiocarbonates
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D339/00Heterocyclic compounds containing rings having two sulfur atoms as the only ring hetero atoms
    • C07D339/08Six-membered rings

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Heterocyclic Carbon Compounds Containing A Hetero Ring Having Nitrogen And Oxygen As The Only Ring Hetero Atoms (AREA)
  • Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)
  • Heterocyclic Compounds Containing Sulfur Atoms (AREA)
  • Thiazole And Isothizaole Compounds (AREA)
  • Nitrogen And Oxygen Or Sulfur-Condensed Heterocyclic Ring Systems (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Catalysts (AREA)

Abstract

ABSTRACT OF THE DISCLOSURE:
The present invention relates to a process for the production of five membered ketonic heterocyclic compounds of the general formula:

(l) wherein:
- R1, R2, R3, R4 and R6 are identical or different and each represent n hydrogen atom or an alkyl radical having from 1 to 3 carbon atoms, which may be substituted by an hydroxy group or a radical of the formula -COOR5 in which R5 represents an alkyl radical having from 1 to 3 carbon atoms;
- X is an oxygen or sulfur atom;
- Y is a sulfur or nitrogen atom; and - m is the valence of Y.
This process comprises reacting a difunctional compound of the formula:

(2) wherein R1, R2, R3, R4, R6, X, Y and m have the above meanings;
with carbon monoxyde and oxygen in the presence of a ctalyst selected among the soluble catalyst consisting of selenium or its derivatives, and the unsoluble catalyst consisting of a copper complex.

Description

9~5 The present invention relates to a process or the production of five membered ke-tonic heterocyclic compounds having two heteroatoms in the ring.
More especially the present invention relates to a process for the production of heterocyclic compounds of the general formula:

R - C C - R (1) X ~ 6)m-2 , ~ '.
wherein:
- Rl, R2j R3, R4 and R6 are identical or different and each represent a hydrogen atom or an alkyl radical having from 1 to 3 carbon atoms, wh.ich may be substituted by an hydroxy group or a radical of the formula - COOR5 in which R5 represents an alkyl radical having Erom 1 to 3 carbon atoms;
- X is an oxygen or sulfur atom;
- Y is a sulfur or nitrogen atom; and ~ m is the valence of Y, Up to now, the above products have been prepared through a reaction between a difunctional compound and phosgene or through a more complex syntheses. The use o phosgene involves several drawbacks because its toxicity and its reactivity with other functional groups present in the molecule.
It has now been found a simple and cheap process for :
obtaining these heterocyclic compounds at very high yields.
The process according to the invention comprises reacting a difunctional compound of the general ormula ~ 12 13 Rl - C . Y(R6)m_l (2) in which Rl, R2, R3, R4, R6, X, Y and m have the above meanings, with carbon monoxide and oxygen in presence ~

9~5 o~ a soluble or unsoluble catalyst, the former being selected between selenium and derivatives thereof, the la-tt.er being a copper complex.
The reaction may be carried out either in homogeneous phase by dissolving the reagents and the catalyst into a sui-table solvent or in heterogeneous phase by using an unsoluble catalyst. Unrestrictive examples of compounds according to the formula (2) may be ethanolamine, 2-aminopropano~ 3-aminopro-pano], diethanblamine, 1,2-ethandithiole, 1,3-propandithiole, 1,2-propandithiole, 2-aminoethanthiole, 2-aminopropanthiole, 3-aminopropanthiole. The reaction may be carried out under a pressure ranging from 1 to 100 atmospheres. For practical reasons, it is preferable to operate ~nder a pressu~e rang~g between l to 10 atmospheres.
As 2~resaid, the catalyst may be soluble into the reagents or in suitable solvents, or it may be unsoluble.
Among the soluble catalysts, it is possible to mention metallic selenium and the derivatives thereof whereas, as to the unso-luble catalysts, an advantageous use can be made of complexes containing Cu. The reaction may be carried out at temperatures ranging from 0 to 100C, preferably from the room temperature to 80C.
The Eollowing examples illustrate the invention, but are not limitative thereof.
Example 1:
23.8 mmoles of 1-2 dimercaptoethane,~l mmole of triethylamine and 0.5 mmole o Se were reacted ln 10 ml of T~F at 25C with a CO:O2 mixture in the molar ratio 10:1 at 3.5 atmos~heres.
After 40 hours, selenium was recovered and the solvent was 1~50~9'~
evaporated from the resulting suspension. The residual was distilled under vacuum. The IR analysis showed that the dis-tilled product was ethylenedithiocarbonate. Yield=90%.

Example 2 :
lO moles of 2,3-dimercaptopropanol-l, l mole of triethylamine and l mmole of Se were reacted in 10 ml of THF at 25C with a CO:O2 mixture in the molar ratio lO: l at 3.5 atmospheres.
After 16 hours, selenium was recovered from the resulting suspen5ion and the solvent was evaporated. The residual was distilled under vacuum. The distilled product, at IR and mass analysis, was 1-3 dithiolan-2-one-4-hydroxymethyl.
Yield = 90%.
20 mmoles of 2,3-dimercaptopropanol, l mmole of thiethylamine and O.S mmole o~ Se were reacted with C0 and 2 in condi-tions simllar to the precedi,ng ones. After 16 'hours the oolution was yellowish and homogeneous. The solverit was evaporated and the residual was distilled.
18 mmoles of 1-3 dithiolan-2-one-4-hydroxymethyl were obtained.
Yield = 90%~

Example 3:
14.8 mmoles of 2-mercaptoe-thylamine and 0.5 mmole of amorphous Se, in lO mI of THF, were reacted at 60C with a C0:02 mixture in the molar ratio lO:l at 3.5 atmospheres.
After 4 hours, the solution was filtered from selenium and the solvent was evaporated. The residual was again crystallized in CS2 (m.p.=50C). 1.4 g of 2-thiazolidinone were obtained, ' identified by IR and mass spectoscopy. Yield = 93%. ' ~ ' : .

.. . . . . . . . . . . . . . .. . .

105099~ -Example 4:
82 mmoles of ethanolamine and 1 mmole of amorphous selenium were reacted in 25 ml of THF with a CO:O2 mixture in the molar ratio 4:1 at 4 atmospheres. After 3 hours at 70 C selenium was filtered and the solvent was evaporated. The rèsidual was crystalIized from chloroform (m.p. 87 C).
6.8 g of product was o~tained. The IR ana:Lysis showed that it was 2-oxazolidone. Yield= 95%.
Example 5:
12.7 mmoles of 1-amino-2-propanol and 0.3 mmole of selenium were reacted at 60 C under conditions similar to the preceeding ones. After 3 hours selenium was filtered, the solvent was evaporated and the residual product was distilled under vacuum.
1.2 g of an oily product were obtained. The IR and mass analysis showed that it was 2-oxazolidone-5-methyl. Yield~ 95~.
Example 6:
10 mmoles of diethanolamine and 0.3 mmole of selenium were reacted at 60 C under conditions similar to the preceeding ones.
After 10 hours selenium was filtered, the solvent was evapora-ted and the residual was distilled under vacuum. 1.2 g of liquid product were obtained. The IR and mass analysis showed that it was 2-oxazolidone-3-hydroxyethyl~ Yield =91~.
Example 7:
: .
10.3 mmoles of trihydroxymethylaminomethane and 0.5 mmole of selentum were reacted in 20 ml of ethyl alcohol at 70C with a CO:O2 mixture in the molar ratio 4:1 at 4 atmospheres.
After 5 hours selenium was filtered and the solvent was eva-porated. The residual was crystallized from chloroform (m.p.=
104C). 1.5 g of product were obtained. The IR analysis showed that it was 2-oxazolidone-4, 4-bishydroxymethyl. Yield~ 99%.

, 4 _ L.~ , , , .. . . .: . . :. .. . ". .,. . .. ; , . . . . . . .. ..

Example_8:
16.~ mmoles of ethanolamine and 10 mmoles of CuCl in 10 ml of pyridine were treated, in autoclave at 70C, with a CO:O2 mixture in the molar ratio 4:1. After 16 hours the solution was filtered and the solvent evaporated under vacuum. The residual was crystallized from chloroform. 0.78 g of 2-oxazolidone was obtained. Yield = 55%.

.

' ~

.... . . . . . - . . . . . . .
. : . . .. . . . ... . . ..

Claims (7)

The embodiments of the invention in which an exclusive property or privilege is claimed are defined as follows:
1. Process for the production of five membered ketonic heterocyclic compounds of the general formula:

(1) wherein:
- R1, R2, R3, R4 and R6 are identical or different and each represent a hydrogen atom or an alkyl radical having from 1 to 3 carbon atoms, which may be substituted by an hydroxy group or a radical of the formula - COOR5 in which R5 represents an alkyl radical having from 1 to 3 carbon atoms;
- X is an oxygen or sulfur atom;
- Y is a sulfur or nitrogen atom; and - m is the valence of Y, said process comprising reacting a difunctional compound of the formula:

(2) wherein R1, R2, R3, R4 R6, X, Y and m have the above meanings with carbon monoxyde and oxygen in the presence of a catalyst selected among the soluble catalyst consisting of selenium or its derivatives, and the unsoluble catalyst consisting of a copper complex.
2. Process according to claim 1, characterized in that the reaction is carried out in homogeneous phase, the catalyst and the reagents being dissolved in a solvent.
3. Process according to claim 1, characterized in that the reaction is carried out in heterogeneous phase.
4. Process according to claim 1, characterized in that the reaction is carried out under a pressure ranging from 1 to 100 atmospheres.
5. Process according to claim 4, characterized in that the reaction is carried out under a pressure ranging from 1 to 10 atmospheres.
6. Process according to claim 1, characterized in that the reaction is carried out at a temperature ranging from 0 to 100°C.
7. Process according to claim 6, characterized in that the reaction is carried out at a temperature ranging from the room temperature to 80°C.
CA205,349A 1973-08-01 1974-07-22 Process for the production of heterocyclic compounds and products obtained thereby Expired CA1050995A (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
IT27389/73A IT995110B (en) 1973-08-01 1973-08-01 PROCEDURE FOR THE PRODUCTION OF HETEROCYCLIC COMPOUNDS AND OBTAINED PRODUCTS

Publications (1)

Publication Number Publication Date
CA1050995A true CA1050995A (en) 1979-03-20

Family

ID=11221549

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Application Number Title Priority Date Filing Date
CA205,349A Expired CA1050995A (en) 1973-08-01 1974-07-22 Process for the production of heterocyclic compounds and products obtained thereby

Country Status (16)

Country Link
JP (1) JPS5616790B2 (en)
BE (1) BE818139A (en)
CA (1) CA1050995A (en)
CH (1) CH606025A5 (en)
DE (1) DE2437132C3 (en)
DK (1) DK409174A (en)
ES (1) ES429501A1 (en)
FR (1) FR2239469B1 (en)
GB (1) GB1471007A (en)
IE (1) IE40506B1 (en)
IT (1) IT995110B (en)
LU (1) LU70600A1 (en)
NL (1) NL160560C (en)
NO (1) NO144018C (en)
SU (1) SU654169A3 (en)
ZA (1) ZA744929B (en)

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2655369A1 (en) * 1976-12-03 1978-06-08 Schering Ag 5- (SUBST. PHENYL) -OXAZOLIDINONE AND THEIR SULFUR ANALOGS AND PROCESS FOR THEIR PRODUCTION
SE8605573D0 (en) * 1986-12-29 1986-12-29 Haessle Ab NOVEL COMPOUNDS
ATE156823T1 (en) * 1990-06-07 1997-08-15 Zeneca Ltd THERAPEUTIC HETEROCYCLIC COMPOUNDS
EP2736890A4 (en) * 2011-07-28 2015-07-15 Promentis Pharm Inc Cysteine prodrugs

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2868801A (en) * 1959-01-13 Preparation of substituted

Also Published As

Publication number Publication date
NL160560B (en) 1979-06-15
FR2239469B1 (en) 1978-01-20
IT995110B (en) 1975-11-10
ES429501A1 (en) 1976-09-01
JPS5047984A (en) 1975-04-28
DK409174A (en) 1975-03-24
NO144018C (en) 1981-06-10
SU654169A3 (en) 1979-03-25
BE818139A (en) 1974-11-18
DE2437132C3 (en) 1981-09-10
LU70600A1 (en) 1974-11-28
GB1471007A (en) 1977-04-21
NL160560C (en) 1979-11-15
CH606025A5 (en) 1978-10-13
ZA744929B (en) 1975-08-27
NO742773L (en) 1975-03-03
NO144018B (en) 1981-02-23
IE40506B1 (en) 1979-06-20
IE40506L (en) 1975-02-01
DE2437132B2 (en) 1980-10-16
DE2437132A1 (en) 1975-02-27
FR2239469A1 (en) 1975-02-28
JPS5616790B2 (en) 1981-04-18
NL7410385A (en) 1975-02-04
AU7162474A (en) 1976-01-29

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