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GB2190080A - Anthraquinones - Google Patents

Anthraquinones Download PDF

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Publication number
GB2190080A
GB2190080A GB08610765A GB8610765A GB2190080A GB 2190080 A GB2190080 A GB 2190080A GB 08610765 A GB08610765 A GB 08610765A GB 8610765 A GB8610765 A GB 8610765A GB 2190080 A GB2190080 A GB 2190080A
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GB
United Kingdom
Prior art keywords
process according
catalyst
reaction
butadiene
anthraquinone
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.)
Granted
Application number
GB08610765A
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GB2190080B (en
GB8610765D0 (en
Inventor
Yoshiyuki Okamoto
Raghavan Krishnan
Richard Vicari
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.)
Beazer East Inc
Original Assignee
Koppers Co Inc
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 Koppers Co Inc filed Critical Koppers Co Inc
Priority to GB8610765A priority Critical patent/GB2190080B/en
Priority to JP11043986A priority patent/JPS62267362A/en
Priority to DE19863616364 priority patent/DE3616364A1/en
Priority to FR8607429A priority patent/FR2599030B1/en
Publication of GB8610765D0 publication Critical patent/GB8610765D0/en
Publication of GB2190080A publication Critical patent/GB2190080A/en
Application granted granted Critical
Publication of GB2190080B publication Critical patent/GB2190080B/en
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C46/00Preparation of quinones

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

Abstract

Anthraquinone or a mono-substituted anthraquinone, wherein the substituent is selected from hydrogen, halogen, acyl, and alkyl, was prepared in a one step reaction which comprises reacting 1,4-naphthaquinone with a 1,3-butadiene compound which may be substituted as above, in the presence of a transition metal salt catalyst.

Description

SPECIFICATION Anthraquinones This invention relates to a process for preparing anthraquinones.
The anthraquinones probably comprise a greater number of dyes having outstanding fastness properties than anyothergroup of dyes, and anthraquinone is one of the mostvaluable intermediates in the manufacture of dyestuffs.
Conventionally, anthraquinone is manufactured from phthalic anhydride and dry benzene using a large amount of anhydrous aluminium chloride and an excess of benzenethat must be recovered. Other products ofthe process include hydrogen chloride and aluminium hydroxide.
German Offenlegungschrift No. 2,460,922 (Nippon Steel Chemical Co. Ltd.) describes a processor preparing pure anthraquinone by the reaction of 1 ,4-naphthaquinone with a small excess of 1 ,3-butadiene at 100-1 1 O"C in an autoclave followed by air oxidation of the resultanttetrahydroanthraquinone in the presence of a base. It is also known that anthraquinone can be prepared by the direct reaction of 1,3-butadiene with a mixture of naphthalene, phthalic anhydride and 1,4-naphthaquinone obtained by thevapoour phase oxidation of naphthalene (see U.S. Patent Specifications Nos. 2,652,408; 2,938,913; and 2,536,833).
According to the present invention there is provided a process for preparing a compound which can be represented by the general formula:
wherein X is hydrogen, halogen, an acyl group oran alkyl group, which process comprises reacting 1 ,4-naphthaquinonewith a 1,3-butadiene compound which can be represented by the general formula:
wherein Xis as previously defined, in the presence of a catalytic amount of a transition metal salt catalyst.
It has now been discovered that anthraquinones of the general formula (I) above can be obtained in good yield in a one step process by reacting 1 Anaphthaciuinone with a 1 ,3-butadiene, which may be substituted, in the presence of a transition metal salt catalyst and, preferably, phthalic acid. The 1 ,3-butadiene may be substituted, for example, with halogens such as chloro and bromo, acyl groups containing from 2 to 4carbon atoms, such as acetyl, propionyl and n-butyryl; alkyl groups containing from 1 to 3 carbon atoms, such as methyl, ethyl and isopropyl. The substitution can be in the 1 or 2 position.Representative examples of substituted 1 ,3-butadienes which can be used in the process of the invention include 1 -acetoxy-1 ,3-butadiene; 2-acetoxy-1 ,3-butadiene; 1 -ch loro-1 ,3-butadiene; 2-chloro-1 ,3-butadiene; 1 -methyl-1 ,3-butadiene; 2-methyl-1 ,3-butadiene; 1 -ethyl-1 ,3-butadiene; 2ethyl-l ,3-butadiene; 1-bromo-1,3-butadiene; and 2-bromo-1,3-butadiene.
Preferably,the catalyst is a salt of Cr, Mn, Fe, Co, Ni, Cu or Zn, although other transition metals may be used but are less preferred because of higher cost and limited availability. The anion used to form the salt may be selected from a number of inorganic and organic anions, including chloride, nitrate, carbonate, bicarbonate, sulphate, sulphide, oxide, phthalate, benzoate, naphthalate, toluate and phosphate. If desired, the salt may beformed in situ. Whilst it is preferred to use catalysts containing iron, the particular anion employed aswell as the cation employed (otherthan iron) is not particularly important.The amount of catalyst employed will depend upon the reactants butgenerallyfrom about 1% to about 20% by weight of the naphthaquinonewill be sufficient.
Depending upon the reactant employed, it may be necessary to use a solvent. Useful solvents are alcohols containing from 1 to 4 carbon atoms, such as methanol, ethanol, propanol and butanol; tetrahydrofuran and dioxane.
For best results, there should be used a slight excess of 1 ,3-butadiene compound to naphthaquinone.
Thus,whilesubstantially equimolaramounts may be used, it is preferred that the molar ratio of naphthaquinoneto butadiene should be in the range 1:1.1 to 1:1.4.
Preferably, the reaction is conducted at a temperature in the range of from about 80"C to about 130 C and at a pressure in the range of about3 to about 8 atmospheres over a period in the range of from about 4 hoursto about 10 hours. A preferred temperature range is from 90"C to 11 00C and a preferred pressure range is from 4 to 6 atmospheres.
Inthefollowing Examples, which will serveto illustratethe invention and preferred embodiments thereof, all parts and percentages (as elsewhere in the specification and claims) are by weight unless otherwise indicated.
Example 1 Chemically pure 1 ,4-naphthaquinone (2.0 g, 0.013 mole), 13-butadiene (1.0 g, 0.018 mole) and anhydrous FeCI3 (0.20 g, 0.0013 mole) were dissolved into 12 ml absolute alcohol and placed in a thick reaction tube (O.D.
1/2 to 5/8 inch, wall thickness 3/32 inch).
Chemically pure naphthaquinone was used as commercial grade naphthaquinone contains phthalic anhydride which causes the formation of anthraquinone. The tube was cooled to -70 C (dry ice-acetone) and evacuated by a high vacuum pump. Thetube was sealed in vacuum and heated at 90"-1 20"C for 17 hours, The pressure built up to 4-6 atmospheres during the reaction. Upon cooling the solution, the solid precipitated and was isolated by filtration and washed with dilute aqueous HCI and water. The solid was crystallized from 95% alcohol asyellow needles (m.p. 285-287"C) and identified as anthraquinone by l.R. and by mixed melting point. The yield was 2.30g (88%).
Example 2 (Comparative) The reaction was carried out under the same conditions as described in Example 1 except that a catalyst was not employed. The white solid produced was filtered and identified as 1,4-dihydro-9,10-anthraquinone (m.p. 105 -108 C). The yield was 2.29 g, (86%).
Example 3 The reaction was carried out under the same conditions as described in Example 1 except that equal molar amounts of FeCI3 and phthalic acid were used. Anthraquinone (m.p. 284 -286 C) was obtained. The yield was 2.33 g, (90%).
Example 4 The reaction was carried out under the same conditions as described in Example 1 except that equal molar amounts of NiCI2 and phthalic acid were used, Anthraquinone (m.p. 284 -286"C) was obtained. The yield was 1.49, (54%). In addition to anthraquinone, many side products were obtained and the structures were not identified.
Example 5 The reaction was carried out under the same conditions as described in Example 1 except that equal molar amounts of Ni(NO3)2 and phthalic acid were used. Anthraquinone (m.p. 284 -286 C) was obtained. The yield was 1.5 g, (56%). Other side products were also obtained.
Example 6 The reaction was carried out under the same conditions as described in Example 1 except that equal molar amounts ofCo(NO3)2 and phthalic acid were used. Anthraquinone (m.p. 284 -286"C) was isolated. The yield was 1 9, (54%). Other side products were also obtained.
Example 7 1 ,4-Naphthaquinone (7.9 g, 0.05 mole), 1,3-butadiene (3.5 g, 0.07 mole), Fe(NO3)3 (1.0 g, 0.0025 mole) and phthalic acid (0.4 g, 0.0025 mole) were dissolved into 60 ml absolute alcohol. The mixture was placed in an autoclave. This was then cooled in dry ice/acetone and degassed.
The autoclavewasthen heated at 1 1O"Cfor 6 hours. The pressure built upto 6 atmospheres duringthe reaction. Afterthe reaction, the container was cooled to room temperature. The volatile gases were analyzed by mass spectrum and found to be hydrogen and unreacted butadiene.
The solid produced was isolated and recrystallized from 95% alcohol (m.p. 285 -287 C). The solid was identified as anthraquinone by l.R. measurement and by mixed melting point measurement. The yield was 9.3 g, (89.5%).
Example 8 The reaction was carried out using the same conditions as described in Example 7 except that Co(NO3)2 (0.073 g, 0.0025 mole) instead of FeCI3 was used as the catalyst. Hydrogen and unreacted butadiene were detected and anthraquinone (m.p. 285 -287 C) was obtained. The yield was 8.5 g, (87.7%).

Claims (17)

1. A process for preparing a compound which can be represented by the general formula:
wherein Xis hydrogen, halogen, an acyl group or an alkyl group which process comprises reacting 1,4-naphthaquinone with a 1 ,3-butadiene compound which can be represented by the general formula:
wherein Xis as previously defined, in the presence of a catalytic amount of a transition metal salt catalyst.
2. A process according to claim 1, wherein the catalyst is an iron salt.
3. A process according to claim 2, wherein the catalyst is FeCI3.
4. A process according to claim 2, wherein the catalyst is Fe(NO3)3.
5. A process according to claim 1 wherein the catalyst is a cobalt salt.
6. A process according to claim 5 wherein the catalyst is Co(NO3)2.
7. A process according to claim 1 wherein the catalyst is a nickel salt.
8. A process according to claim 7 wherein the catalyst is Ni(NO3).
9. A process according to claim 7 wherein the catalyst is Nick2.
10. A process according to any one of claims 1 to 9 wherein the reaction is conducted in the presence of phthalic acid.
11. A process according to any one of claims 1 to 10 wherein 1,4-naphthaquinone is reacted with 1,3-butadieneto produce anthraquinone.
12. A process according to any one of claims 1 to 11 wherein the reaction is carried out in a solvent.
13. A process according to claim 12 wherein an alcohol is employed as the solvent.
14. A process according to any one of claims 1 to 13 wherein the molar ratio of 1 ,4-naphthaquinoneto 1,3-butadiene compound is in the range offrom 1:1.1 to 1:1.4.
15. A process according to any one of claims 1 to 14, wherein the reaction is carried out at a temperature in the range of from 80"C to 130 C,
16. A process according to any one of claims 1 to 15, wherein the reaction is carried out at a pressure in the range offrom about 3 to about 8 atmospheres.
17. A process according to claim 1, substantially as described in the foregoing Examples.
GB8610765A 1986-05-02 1986-05-02 Anthraquinones Expired - Lifetime GB2190080B (en)

Priority Applications (4)

Application Number Priority Date Filing Date Title
GB8610765A GB2190080B (en) 1986-05-02 1986-05-02 Anthraquinones
JP11043986A JPS62267362A (en) 1986-05-02 1986-05-14 Production of anthraquinoes
DE19863616364 DE3616364A1 (en) 1986-05-02 1986-05-15 METHOD FOR PRODUCING ANTHRACHINONS
FR8607429A FR2599030B1 (en) 1986-05-02 1986-05-23 PROCESS FOR PRODUCING ANTHRAQUINONES.

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
GB8610765A GB2190080B (en) 1986-05-02 1986-05-02 Anthraquinones

Publications (3)

Publication Number Publication Date
GB8610765D0 GB8610765D0 (en) 1986-06-11
GB2190080A true GB2190080A (en) 1987-11-11
GB2190080B GB2190080B (en) 1990-03-21

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GB8610765A Expired - Lifetime GB2190080B (en) 1986-05-02 1986-05-02 Anthraquinones

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JP (1) JPS62267362A (en)
DE (1) DE3616364A1 (en)
FR (1) FR2599030B1 (en)
GB (1) GB2190080B (en)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0597287A1 (en) * 1992-11-11 1994-05-18 BASF Aktiengesellschaft Process for the preparation of anthraquinones
WO1998033757A1 (en) * 1997-02-03 1998-08-06 Girex Method for preparing substituted anthraquinone and application to the preparation of rheins

Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB320375A (en) * 1928-07-06 1929-10-07 Ig Farbenindustrie Ag Improvements in the manufacture and production of anthraquinone and its derivatives

Family Cites Families (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR39333E (en) * 1930-06-19 1931-10-12 Ig Farbenindustrie Ag Process for the production of anthraquinone and its derivatives
US2652408A (en) * 1951-07-14 1953-09-15 American Cyanamid Co Preparation of anthraquinone compounds
BE573902A (en) * 1957-12-16
DE2437220C3 (en) * 1974-08-02 1979-06-13 Bayer Ag, 5090 Leverkusen Process for the production of anthraquinone
US4308211A (en) * 1980-12-29 1981-12-29 The Goodyear Tire & Rubber Company Process for the preparation of anthraquinone
JPS57203027A (en) * 1981-06-09 1982-12-13 Kawasaki Kasei Chem Ltd Purification of anthraquinone
JPS57206633A (en) * 1981-06-12 1982-12-18 Kawasaki Kasei Chem Ltd Purifying method of anthraquinone

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB320375A (en) * 1928-07-06 1929-10-07 Ig Farbenindustrie Ag Improvements in the manufacture and production of anthraquinone and its derivatives

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0597287A1 (en) * 1992-11-11 1994-05-18 BASF Aktiengesellschaft Process for the preparation of anthraquinones
US5387704A (en) * 1992-11-11 1995-02-07 Basf Aktiengesellschaft Preparation of anthraquinones
WO1998033757A1 (en) * 1997-02-03 1998-08-06 Girex Method for preparing substituted anthraquinone and application to the preparation of rheins
FR2759079A1 (en) * 1997-02-03 1998-08-07 Girex PROCESS FOR THE PREPARATION OF SUBSTITUTED ANTHRAQUINONES AND APPLICATION TO THE PREPARATION OF RHEINES
US6057461A (en) * 1997-02-03 2000-05-02 Girex Method for preparing substituted anthraquinone and application to the preparation of rheins

Also Published As

Publication number Publication date
DE3616364A1 (en) 1987-11-19
GB2190080B (en) 1990-03-21
FR2599030B1 (en) 1988-12-02
GB8610765D0 (en) 1986-06-11
JPS62267362A (en) 1987-11-20
FR2599030A1 (en) 1987-11-27

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Legal Events

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732 Registration of transactions, instruments or events in the register (sect. 32/1977)
PCNP Patent ceased through non-payment of renewal fee

Effective date: 19930502