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1. WO1993016972 - PROCEDE PERFECTIONNE ET CATALYSEUR LAVE PERMETTANT D'HYDROGENER PARTIELLEMENT DES COMPOSES AROMATIQUES ET PRODUIRE DES CYCLO-OLEFINES

Note: Texte fondé sur des processus automatiques de reconnaissance optique de caractères. Seule la version PDF a une valeur juridique

[ EN ]

CLAIMS

WE CLAIM AS OUR INVENTION:

1. A process for producing cycloolefins from aromatic feedstocks comprising the steps of:
contacting hydrogen and an aromatic feedstock
comprising one or more monocyclic or polycyclic aromatic hydrocarbons with a partial
hydrogenation catalyst system of:
a. a hydrogenation catalyst comprising at least an effective amount of ruthenium, a metallic selectivity promoter, a composite catalyst support material, and
b. a water solution at pH 3-7 containing no dissolved salts
to hydrogenate partially the aromatic feedstock and produce a corresponding cycloolefin, and
separating the cycloolefin from the
hydrogenation catalyst.

2. The process of claim 1 where the aromatic feedstock comprises at least one of benzene and
alkylbenzenes .

3. The process of claim 2 where the aromatic feedstock comprises benzene.

4. The process of claim 2 where the aromatic feedstock comprises at least one alkylbenzene selected from the group consisting of toluene, o-xylene, m-xylene, p-xylene, ethylbenzene, propylbenzene, isopropylbenzene, butylbenzene, t-butylbenzene, and isobutylbenzene.

5. The process of claim 1 where the aromatic feedstock comprises one or more fused or non-fused polycyclic aromatic compounds.

6. The process of claim 5 where the polycyclic aromatic compound is selected from naphthalenes and biphenyls .

7. The process of claim 1 where the catalyst support material comprises a major amount of a first relatively high specific surface area oxidic core
material which is at least partially surrounded by a minor amount of a second relatively low inherent surface area oxidic material.

8. The process of claim 7 where the first relatively high specific surface area oxidic core
material is selected from the group consisting of silica, alumina, and silica-alumina.

9. The process of claim 7 where the second relatively low inherent surface area oxidic material is selected from metal or semimetal oxides or lanthanum-containing material of the formula:

x(LaON03) + y(La203) + z(La(N03)3)

where x<l, z<l and x+y+z=l.

10. The process of claim 7 where the second relatively low inherent surface area oxidic material is selected from one or more metal or semimetal oxides of lanthanum oxide, zinc oxide, boria, ceria, zirconia, or titania.

11. The process of claim 1 where the catalyst support material comprises a major amount of a relatively high specific surface area oxidic material selected from the group consisting of silica, alumina, and silica-alumina.

12. The process of claim 1 where the ruthenium in the hydrogenation catalyst was introduced into the catalyst support material by a heat soaked acidic RuCl3 solution.

13. The process of claim 9 where the ruthenium in the hydrogenation catalyst was introduced into the catalyst support material by a heat soaked acidic RuCl3 solution.

14. The process of claim 1 where the selectivity promoter metal cation is selected from the group consisting of Fe, Co, Ni, Zn, Cu, Ag, Au, Pd and Pt.

15. The process of claim 14 where the selectivity promoter metal cation is Co.

16. The process of claim 14 where the weight ratio of selectivity promoter to ruthenium is between 0.05:1 and 5:1.

17. The process of claim 14 where the pH of the water solution is between 3 and 7.

18. The process of claim 1 where the volume ratio of the water solution to the aromatic feedstock and cycloolefins is 1:1 or less.

19. The process of claim 18 where the volume ratio is 0.1:1 to 1:1 and the process is operated in stirred tank reactors in series or in a single stirred tank reactor.

20. The process of claim 1 where the volume ratio of the water solution to the aromatic feedstock and cycloolefin is greater than 5:1.

21. The process of claim 20 where the process is operated in a trickle bed reactor.

22. A process for producing cycloolefins from aromatic feedstocks comprising the steps of:
contacting hydrogen and the aromatic feedstock with a partial hydrogenation catalyst system of:
a. a hydrogenation catalyst comprising at
least an effective amount of and up to
about 20 % by weight of ruthenium, a
selectivity promoter, and a composite
catalyst support material comprising a
major amount of a first relatively high
specific surface area oxidic core material
which is at least partially surrounded by a
minor amount of a second relatively low
inherent surface area oxidic material, and b. an aqueous solution containing
substantially no dissolved salts,

to hydrogenate partially the aromatic feedstock and produce the corresponding cycloolefin, and separating the cycloolefin from the hydrogenation catalyst.

23. The process of claim 22 where the aromatic feedstock comprises at least one of benzene and alkylbenzenes .

24. The process of claim 23 where the aromatic feedstock comprises benzene.

25. The process of claim 23 where the aromatic feedstock comprises at least one alkylbenzene selected from the group consisting of toluene, o-xylene, m-xylene, p-xylene, ethylbenzene, propylbenzene, isopropylbenzene, butylbenzene, t-butylbenzene, and isobutylbenzene.

26. The process of claim 25 where the aromatic feedstock comprises one or more fused or non-fused polycyclic aromatic compounds.

27. The process of claim 26 where the polycyclic aromatic compound is selected from naphthalenes and biphenyls .

28. The process of claim 27 where the first relatively high specific surface area oxidic core material is selected from the group consisting of silica, alumina, and silica-alumina.

29. The process of claim 28 where the first relatively high specific surface area oxidic core material is silica and the second relatively low inherent surface area oxidic material is a lanthanum-containing material of the formula: x (LaON03 ) + y (La203 ) + z (La (N03 ) 3 )
where x<l , z<l and x+y+z=l .

30. The process of claim 29 where the ruthenium in the hydrogenation catalyst was introduced into the catalyst support material by a heat soaked acidic RuCl3 solution.

31. The process of claim 28 where the selectivity promoter is selected from the group consisting of Fe, Co, Ni, Zn, Cu, Ag, Au, Pd and Pt.

32. The process of claim 31 where the promoter metal cation is Co.

33. The process of claim 31 where the weight ratio of selectivity promoter to ruthenium is between 0.05:1 and 5:1.

34. The process of claim 32 where the pH of the aqueous solution is between 3 and 7.

35. The process of claim 22 where the volume ratio of the aqueous solution to the aromatic feedstock and cycloolefins is 1:1 or less.

36. The process of claim 35 where the volume ratio is 0.1:1 to 1:1 and the process is operated in stirred tank reactor in series or in a single stirred tank reactor.

37. The process of claim 22 where the volume ratio of the aqueous solution to the aromatic feedstock and cycloolefin is greater than 5:1.

38. The process of claim 37 where the process is operated in a trickle bed reactor.

39. A hydrogenation catalyst composition comprising metallic ruthenium, a selectivity promoter, and a composite catalyst support material comprising a major amount of a first relatively high specific surface area oxidic core material which is at least partially surrounded by a minor amount of a second relatively low inherent surface area oxidic material.

40. The hydrogenation catalyst of claim 39 where the first relatively high specific surface area oxidic core material is selected from the group consisting of silica, alumina, and silica-alumina.

41. The hydrogenation catalyst of claim 39 where the second relatively low inherent surface area oxidic material is selected from metal or semimetal oxides or lanthanum-containing material of the formula:

x(LaON03) + y(La203) + z(La(N03)3)

where x<l, z l and x+y+z=l.

42. The hydrogenation catalyst of claim 40 where the second relatively low inherent surface area oxidic material is a lanthanum-containing material of the formula:

x(LaON03) + y(La203) + z(La(N03)3)

where x<l, z<l and x+y+z»l.

43. The hydrogenation catalyst of claim 42 where the ruthenium in the hydrogenation catalyst was introduced into the catalyst support material by a heat soaked acidic RuCl3 solution.

44. The hydrogenation catalyst of claim 39 where the selectivity promoter is selected from the group consisting of Fe, Co, Ni, Zn, Cu, Ag, Au, Pd, and Pt.

45. The hydrogenation catalyst of claim 44 where the selectivity promoter is Co.

46. The hydrogenation catalyst of claim 45 where the ratio of Co:Ru is between 0.05:1 and 5:1.

47. A hydrogenation catalyst composition comprising metallic ruthenium, a selectivity promoter, and a composite catalyst support material comprising a major amount of a first relatively high specific surface area oxidic core material selected from the group consisting of silica, alumina, and silica-alumina and which is at least partially surrounded by a minor amount of a second relatively low inherent surface area oxidic material of a lanthanum-containing material of the formula:

x(LaON03) + y(La203) + z(La(N03)3)

where x<l, z<l and x+y+z=l.

48. The hydrogenation catalyst of claim 47 where the first relatively high specific surface area oxidic core material is silica.

49. The hydrogenation catalyst of claim 48 where the ruthenium in the hydrogenation catalyst was introduced into the catalyst support material by a heat soaked acidic RuCl solution.

50. The hydrogenation catalyst of claim 47 in which the selectivity promoter is selected from the group consisting of Fe, Co, Ni, Zn, Cu, Ag, Au, Pd, and Pt.

51. The hydrogenation catalyst of claim 50 in which the selectivity promoter is Co.

52. The hydrogenation catalyst of claim 48 in which the selectivity promoter is Co.

53. The hydrogenation catalyst of claim 51 where the ratio of Co:Ru is between 0.05:1 and 5:1.