Claims
- 1. A process for the hydroxylation of a phenol or phenol ether having the general formula (I): ##STR4## in which R.sub.5 is a hydrogen atom, a methyl group, an ethyl group or a phenyl group, and R.sub.6 is a hydrogen atom, an alkyl radical having from 1 to 4 carbon atoms, an alkoxy radical having from 1 to 4 carbon atoms or a phenyl or cyclohexyl radical, comprising reacting such phenol or phenol ether with hydrogen peroxide in the presence of a catalytically effective amount of a titanozeosilite comprising an MFI zeolite based on titanium oxide and silicon oxide and having a monoclinic crystalline structure.
- 2. The process as defined by claim 1, said titanozeosilite comprising an MFI zeolite based on silicon oxide and titanium oxide and having, after calcination, the following formula (II):
- Si.sub.(96-x), Ti.sub.x O.sub.192 (II)
- in which x ranges from about 0.1 to 6.
- 3. The process as defined by claim 2, said titanozeosilite further comprising from 0.01 to 0.8% of fluorine by weight, after calcination.
- 4. The process as defined by claim 2, wherein formula (I), R.sub.5 is a hydrogen atom, a methyl group or an ethyl group, and R.sub.6 is a hydrogen atom, a methyl, ethyl or tert-butyl group, or a methoxy or ethoxy group.
- 5. The process as defined by claim 2, said phenol or phenol ether having the formula (I) comprising phenol, anisole, ortho-cresol, meta-cresol, para-cresol, 4-tert-butylphenol, 2-methoxyphenol or 4-methoxyphenol.
- 6. The process as defined by claim 1, wherein the mole ratio phenol/phenol ether to hydrogen peroxide ranges from 25:1 to 3:1.
- 7. The process as defined by claim 1, carried out discontinuously, and wherein the catalyst constitutes from 0.1% to 20% by weight of the weight of the compound of formula (I).
- 8. The process as defined by claim 1, carried out continuously on a fixed bed of catalyst.
- 9. The process as defined by claim 2, said titanozeosilite having been produced by:
- (i) first preparing a reaction mixture, in an aqueous medium, containing at least one source of silicon oxide, one source of titanium oxide, fluoride ions and a structuring agent, the pH of such reaction mixture ranging from approximately 1.5 to approximately 10.5;
- (ii) crystallizing such reaction mixture and recovering the crystalline precipitate therefrom; and
- (iii) calcining such precipitate at a temperature above 450.degree. C.
- 10. The process as defined by claim 9, wherein, during the preparation of the titanozeosilite, the mole ratio Ti/Si in the reaction mixture ranges from 1 to 0.01.
- 11. The process as defined by claim 9, wherein, during the preparation of the titanozeosilite, the mole ratio F/Si in the reaction mixture ranges from 6 to 0.06.
- 12. The process as defined by claim 9, wherein, during the preparation of the titanozeosilite, the mole ratio H.sub.2 O/Si in the reaction mixture ranges from 100 to 6.
- 13. The process as defined by claim 9, wherein, during the preparation of the titanozeosilite, the mole ratio structural agent/Si ranges from 1 to 0.04.
- 14. The process as defined by claim 1, said hydrogen peroxide comprising an aqueous solution thereof.
- 15. The process as defined by claim 1, said hydrogen peroxide comprising an organic solution thereof.
- 16. The process as defined by claim 1, carried out in a solvent for the compound of formula (I).
- 17. The process as defined by claim 16, said solvent comprising water, an alcohol, a ketone, a nitrile, a carboxylic acid, an ester, an ether, or a polar aprotic solvent.
- 18. The process as defined by claim 1, carried out at a temperature of from 45.degree. C. to 160.degree. C.
- 19. The process as defined by claim 1, said titanozeosilite having the x-ray diffraction pattern comprising:
- ______________________________________Extreme values Extreme valuesof d.sub.hkl (nm) I/I.sub.o of d.sub.hkl (nm) I/I.sub.o______________________________________1.110-1.128 S-SS 0.3785-0.3845 mS0.991-1.012 S-SS 0.3735-0.3795 m0.972-0.986 w 0.3715-0.3775 m0.895-0.906 ww 0.3705-0.3765 m0.803-0.813 ww 0.3645-0.3700 w0.741-0.753 ww (broad) 0.3610-0.3670 w0.704-0.715 ww (broad) 0.3470-0.3525 ww0.666-0.678 w 0.3430-0.3485 w (w)0.632-0.643 w 0.3415-0.3470 w (w)0.595-0.605 mw 0.3385-0.3439 ww0.589-0.598 w 0.3341-0.3394 w (w)0.568-0.577 mw 0.3290-0.3345 w (broad)0.565-0.574 w (shoulder) 0.3240-0.3292 w0.555-0.564 w 0.3045-0.3099 w (w)0.534-0.543 w (w) 0.3020-0.3068 w0.531-0.539 w (w) 0.2978-0.3025 w0.510-0.518 ww 0.2952-0.2999 ww (shoulder)0.502-0.508 ww 0.2944-0.2991 w0.496-0.504 mw 0.2914-0.2961 ww0.485-0.493 ww 0.2852-0.2898 ww (broad)0.468-0.476 ww 0.2774-0.2818 ww0.459-0.466 w 0.2722-0.2766 ww (broad)0.444-0.451 w 0.2676-0.2720 ww0.433-0.441 w 0.2606-0.2648 ww0.423-0.431 w 0.2586-0.2627 ww0.4055-0.4125 ww 0.2544- 0.2585 ww (broad)0.3985-0.4045 w 0.2508-0.2548 ww0.3835-0.3905 S 0.2478-0.2518 w0.3805-0.3865 mS.______________________________________
Priority Claims (1)
Number |
Date |
Country |
Kind |
62-15247 |
Oct 1987 |
FRX |
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Parent Case Info
This application is a continuation of application Ser. No. 07/261,590, filed Oct. 24, 1988, now abandoned.
US Referenced Citations (1)
Number |
Name |
Date |
Kind |
4229424 |
Kokotailo |
Oct 1980 |
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Foreign Referenced Citations (3)
Number |
Date |
Country |
2024790 |
Jan 1980 |
GBX |
2071071 |
Sep 1981 |
GBX |
2116974 |
Oct 1983 |
GBX |
Non-Patent Literature Citations (1)
Entry |
Chemical Reviews, vol. 88, No. 1, p. 152, 1988. |
Continuations (1)
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Number |
Date |
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Parent |
261590 |
Oct 1988 |
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