Compositions and processes for reducing NOemissions during fluid catalytic cracking
원문보기
IPC분류정보
국가/구분
United States(US) Patent
등록
국제특허분류(IPC7판)
B01J-029/80
B01J-029/00
B01J-029/06
출원번호
US-0824913
(2004-04-15)
등록번호
US-7304011
(2007-12-04)
발명자
/ 주소
Yaluris,George
Ziebarth,Michael Scott
Zhao,Xinjin
출원인 / 주소
W.R. Grace & Co. Conn.
인용정보
피인용 횟수 :
4인용 특허 :
142
초록▼
Compositions for reduction of NOx generated during a catalytic cracking process, preferably, a fluid catalytic cracking process, are disclosed. The compositions comprise a fluid catalytic cracking catalyst composition, preferably containing a Y-type zeolite, and a particulate NOx composition contain
Compositions for reduction of NOx generated during a catalytic cracking process, preferably, a fluid catalytic cracking process, are disclosed. The compositions comprise a fluid catalytic cracking catalyst composition, preferably containing a Y-type zeolite, and a particulate NOx composition containing particles of a zeolite having a pore size ranging from about 3 to about 7.2 Angstoms and a SiO2 to Al2O3 molar ratio of less than about 500. Preferably, the NOx reduction composition contains NOx reduction zeolite particles bound with an inorganic binder. In the alternative, the NOx reduction zeolite particles are incorporated into the cracking catalyst as an integral component of the catalyst. Compositions in accordance with the invention are very effective for the reduction of NOx emissions released from the regenerator of a fluid catalytic cracking unit operating under FCC process conditions without a substantial change in conversion or yield of cracked products, e.g., gasoline and light olefins. Processes for the use of the compositions are also disclosed.
대표청구항▼
What is claimed is: 1. A fluid cracking catalyst (FCC) composition, which composition comprises (a) a FCC cracking component suitable for catalyzing the cracking of hydrocarbons under FCC conditions, and (b) a particulate NOx reduction catalyst/additive composition having a mean particle size of gr
What is claimed is: 1. A fluid cracking catalyst (FCC) composition, which composition comprises (a) a FCC cracking component suitable for catalyzing the cracking of hydrocarbons under FCC conditions, and (b) a particulate NOx reduction catalyst/additive composition having a mean particle size of greater than 45 μm and comprising (i) at least 10 weight percent of NOx reduction zeolite component selected from the group consisting of ZSM-11, beta, MCM-49, mordenite, MCM-56, Zeolite-L, zeolite Rho, errionite, chabazite, clinoptilolite, MCM-22, MCM-35, MCM-61, Offretite, A, ZSM-12, ZSM-23, ZSM-18, ZSM-22, ZSM-57, ZSM-61, ZK-5, NaJ, Nu-87, Cit-1, SSZ-35, SSZ-48, SSZ-44, SSZ-23, Dachiardite, Merlinoite, Lovdarite, Levyne, Laumontite, Epistilbite, Gmelonite, Gismondine, Cancrinite, Brewsterite, Stilbite, Paulingite, Goosecreekite, Natrolite, omega or mixtures thereof, and (ii) about 5 to about 50 weight percent of an inorganic binder selected from the group consisting of alumina, silica, silica alumina, alumina phosphate, and mixtures thereof, wherein component (a) and component (b) are separate particles. 2. The catalyst of claim 1 wherein the FCC cracking component contains a Y-type zeolite. 3. The catalyst of claim 2 wherein the NOx reduction catalyst/additive composition is present in an amount sufficient to provide a ratio of NOx reduction zeolite component to Y-type zeolite of less than 2. 4. The catalyst of claim 1 wherein the amount of NOx reduction zeolite component present is at least 30 weight percent of the NOx reduction catalyst/additive composition. 5. The catalyst of claim 4 wherein the amount of NOx reduction zeolite component present is at least 40 weight percent of the NOx reduction catalyst/additive composition. 6. The catalyst of claim 5 wherein the amount of NOx reduction zeolite component present at least 50 weight percent of the NOx reduction catalyst/additive composition. 7. The catalyst of claim 1 wherein the amount of NOx reduction zeolite component present ranges from about 10 to about 85 weight percent of the NOx reduction catalyst/additive composition. 8. The catalyst of claim 7 wherein the amount of NOx reduction zeolite component present ranges from about 30 to about 80 weight percent of the NOx reduction catalyst/additive composition. 9. The catalyst of claim 8 wherein the amount of NOx reduction zeolite component present ranges from about 40 to about 75 weight percent of the NOx reduction catalyst/additive composition. 10. The catalyst of claim 1 wherein the NOx reduction zeolite component is exchanged with a cation selected from the group consisting of hydrogen, ammonium, alkali metal and combinations thereof. 11. The catalyst of claim 1 wherein the NOx reduction zeolite component further comprises at least one stabilizing metal. 12. The catalyst of claim 11 wherein the stabilizing metal is a metal selected from the group consisting of Groups 2A, 3B, 4B, 5B, 6B, 7B, 8B, 2B, 3A, 4A, 5A and the Lanthanide Series of the Periodic Table, Ag and mixtures thereof. 13. The catalyst of claim 12 wherein the stabilizing metal is selected from the group consisting of Groups 3B, 2A, 2B, 3A and the Lanthanide Series of the Periodic Table, and mixtures thereof. 14. The catalyst of claim 13 wherein the stabilizing metal is selected from the group consisting of lanthanum, aluminum, magnesium and zinc, and mixtures thereof. 15. The catalyst of claim 11 wherein the stabilizing metal is incorporated into the pores of the NOx reduction zeolite component. 16. The catalyst of claim 1 wherein the inorganic binder in the particulate NOx reduction catalyst/additive composition is selected from the group consisting of silica, alumina, silica alumina and mixtures thereof. 17. The catalyst of claim 16 wherein the inorganic binder is alumina. 18. The catalyst of claim 17 wherein the inorganic binder is aluminum chlorohydrol. 19. The catalyst of claim 17 wherein the alumina is an acid or base peptized alumina. 20. The catalyst of claim 1 wherein the amount of inorganic binder ranges from about 10 to about 30 weight percent of the NOx reduction catalyst/additive composition. 21. The catalyst of claim 20 wherein the amount of inorganic binder present ranges from about 15 to about 25 weight percent of the NOx reduction catalyst/additive composition. 22. The catalyst of claim 1 wherein the NOx reduction zeolite component is selected from the group consisting of beta, MCM-49, mordenite, MCM-56, Zeolite-L, zeolite Rho, errionite, chabazite, clinoptilolite, MCM-22, Offretite, A, ZSM-12, ZSM-23, omega and mixtures thereof. 23. The catalyst of claim 1 wherein the NOx reduction zeolite component has a SiO2 to Al2O3 molar ratio of less than 500. 24. The catalyst of claim 1 wherein the particulate NOx catalyst/additive composition further comprises a zeolite other than the NOx reduction zeolite component. 25. The catalyst of claim 24 wherein the other zeolite is a zeolite selected from the group consisting of ferrierite, ZSM-5, ZSM-35 and mixtures thereof. 26. The catalyst of claim 24 wherein the other zeolite is present in an amount ranging from about 1 to about 80 weight percent of the NOx reduction catalyst/additive composition. 27. The catalyst of claim 26 wherein the other zeolite is present in an amount ranging from about 10 to about 70 weight percent of the NOx reduction catalyst/additive composition. 28. The catalyst of claim 1 wherein the composition further comprises a matrix material selected from the group consisting of alumina, silica, silica alumina, titania, zirconia, yttria, lanthana, ceria, neodymia, samaria, europia, gadolinia, praseodymia and mixtures thereof. 29. The catalyst of claim 28 wherein the matrix material is present in an amount less than 70 weight percent of the NOx reduction catalyst/additive composition. 30. The catalyst of claim 1 further comprising at least one additional NOx reduction composition. 31. The catalyst of claim 30 wherein the additional NOx reduction composition is a non-zeolitic composition. 32. The catalyst of claim 31 wherein the additional NOx reduction composition comprises (a) an acidic metal oxide containing substantially no zeolite; (b) a metal component, measured as the oxide, selected from the group consisting of an alkali metal, an alkaline earth metal and mixtures thereof; (c) an oxygen storage metal oxide component; and, (d) at least one noble metal component. 33. The catalyst of claim 30 wherein the additional NOx reduction composition comprises (a) an acidic metal oxide support; (b) an alkali metal, alkaline earth metal or mixtures thereof; (c) a transition metal oxide having oxygen storage capability; and, (d) a transition metal selected from Groups IB and IIB of the Periodic Table, and mixtures thereof. 34. The catalyst of claim 30 wherein the additional NOx reduction composition is a low NOx CO combustion promoter composition which comprises (a) an acidic oxide support; (b) an alkali metal, an alkaline earth metal or mixtures thereof; (c) a transition metal oxide having oxygen storage capability; and (d) palladium. 35. The catalyst of claim 30 wherein the additional NOx reduction composition comprises at least one metal-containing spinel which includes a first metal and a second metal having a valence higher than the valence of said first metal, at least one component of a third metal other than said first and second metals and at least one component of a fourth metal other than said first, second and third metals, wherein said third metal is selected from the group consisting of Group IB metals, Group IIB metals, Group VIA metals, the rare-earth metals, the Platinum Group metals and mixtures thereof, and said fourth metal is selected from the group consisting of iron, nickel, titanium, chromium, manganese, cobalt, germanium, tin, bismuth, molybdenum, antimony, vanadium and mixtures thereof. 36. The catalyst of claim 35 wherein the metal containing spinel comprises magnesium as said first metal and aluminum as said second metal. 37. The catalyst of claim 35 wherein the third metal component in the metal containing spinel is selected from the group consisting of a Platinum Group metal, the rare-earth metals and mixtures thereof. 38. The catalyst of claim 35 wherein the third metal component is present in an amount in the range of about 0.001 to about 20 weight percent, calculated as elemental third metal. 39. The catalyst of claim 35 wherein said fourth metal component is present in an amount in the range of about 0.001 to about 10 weight percent, calculated as elemental fourth metal. 40. The catalyst of claim 30 wherein the additional NOx reduction additive is a zinc based catalyst. 41. The catalyst of claim 30 wherein the additional NOx reduction additive is an antimony based NOx reduction additive. 42. The catalyst of claim 30 wherein the additional NOx reduction additive is a pervoskite-spinel NOx reduction additive. 43. The catalyst of claim 30 wherein the additional NOx reduction additive is a hydrotalcite containing composition. 44. The catalyst of claim 30 wherein the additional NOx reduction composition comprises (i) an acidic metal oxide, (ii) cerium oxide, (iii) a lanthanide oxide other than ceria, and (iv) optionally, at least one oxide of a transition metal selected from Groups IB and IIB of the Periodic Table, and mixtures thereof. 45. The catalyst of claim 1 wherein the particulate NOx reduction catalyst/additive composition has a mean particle size from about 50 to about 200 μm. 46. The catalyst of claim 45 wherein the particulate NOx reduction catalyst/additive composition has a mean particle size from about 55 to about 150 μm. 47. The catalyst of claim 1 wherein the particulate NOx reduction catalyst/additive composition has a Davison attrition index (DI) value of less than 50. 48. The catalyst of claim 47 wherein the particulate NOx reduction catalyst/additive composition has a DI value of less than 20. 49. The catalyst of claim 48 wherein the particulate NOx reduction catalyst/additive composition has a DI value of less than 15. 50. The catalyst of claim 3 wherein the ratio of NOx reduction zeolite component to Y-type zeolite in the total catalyst inventory is less than 1. 51. A fluid cracking catalyst comprising (a) a cracking component suitable for catalyzing the cracking of hydrocarbons and (b) at least 0.1 weight percent of a NOx reduction zeolite selected from the group consisting ZSM-11, beta, MCM-49, mordenite, MCM-56, Zeolite-L, zeolite Rho, errionite, chabazite, clinoptilolite, MCM-22, MCM-35, MCM-61, Offretite, A, ZSM-12, ZSM-23, ZSM-18, ZSM-22, ZSM-57, ZSM-61, ZK-5, NaJ, Nu-87, Cit-1, SSZ-35, SSZ-48, SSZ-44, SSZ-23, Dachiardite, Merlinoite, Lovdarite, Levyne, Laumontite, Epistilbite, Gmelonite, Gismondine, Cancrinite, Brewsterite, Stilbite, Paulingite, Goosecreekite, Natrolite, omega or mixtures thereof, wherein the NOx reduction zeolite comprises at least one stabilizing metal selected from the group consisting of Groups 3B, 2A, 2B, 3A and the Lanthanide Series of the Periodic Table, and mixtures thereof. 52. The cracking catalyst of claim 51 wherein said catalyst comprises integral particles which contain both components (a) and (b). 53. The cracking catalyst of claim 51 wherein component (b) comprises from about 0.1 to about 60 wt % of the cracking catalyst. 54. The cracking catalyst of claim 53 wherein component (b) comprises from about 1 to about 40 wt % of the cracking catalyst. 55. The catalyst of claim 51 further comprising at least one additional NOx reduction composition. 56. The catalyst of claim 55 wherein the additional NOx reduction composition is a non-zeolitic composition. 57. The catalyst of claim 56 wherein the additional NOx reduction composition comprises (a) an acidic metal oxide containing substantially no zeolite; (b) a metal component, measured as the oxide, selected from the group consisting of an alkali metal, an alkaline earth metal and mixtures thereof; (c) an oxygen storage metal oxide component; and (d) at least one noble metal component. 58. The catalyst of claim 55 wherein the additional NOx reduction composition comprises (a) an acidic metal oxide support; (b) an alkali metal, alkaline earth metal or mixtures thereof (c) a transition metal oxide having oxygen storage capability; and, (d) a transition metal selected from Groups IB and IIB of the Periodic Table, and mixtures thereof. 59. The catalyst of claim 55 wherein the additional NOx reduction composition is a low NOx CO combustion promoter composition which comprises (a) an acidic oxide support; (b) an alkali metal, an alkaline earth metal or mixtures thereof (c) a transition metal oxide having oxygen storage capability; and (d) palladium. 60. The catalyst of claim 55 wherein the additional NOx reduction composition comprises at least one metal-containing spinel which includes a first metal and a second metal having a valence higher than the valence of said first metal, at least one component of a third metal other than said first and second metals and at least one component of a fourth metal other than said first, second and third metals, wherein said third metal is selected from the group consisting of Group IB metals, Group IIB metals, Group VIA metals, the rare-earth metals, the Platinum Group metals and mixtures thereof, and said fourth metal is selected from the group consisting of iron, nickel, titanium, chromium, manganese, cobalt, germanium, tin, bismuth, molybdenum, antimony, vanadium and mixtures thereof. 61. The catalyst of claim 60 wherein the metal containing spinel comprises magnesium as said first metal and aluminum as said second metal. 62. The catalyst of claim 60 wherein the third metal component in the metal containing spinel is selected from the group consisting of a Platinum Group metal, the rare-earth metals and mixtures thereof. 63. The catalyst of claim 60 wherein the third metal component is present in an amount in the range of about 0.001 to about 20 weight percent, calculated as elemental third metal. 64. The catalyst of claim 60 wherein said fourth metal component is present in an amount in the range of about 0.001 to about 10 weight percent, calculated as elemental fourth metal. 65. The catalyst of claim 55 wherein the additional NOx reduction additive is a zinc based catalyst. 66. The catalyst of claim 55 wherein the additional NOx reduction additive is an antimony based NOx reduction additive. 67. The catalyst of claim 55 wherein the additional NOx reduction additive is a pervoskite-spinel NOx reduction additive. 68. The catalyst of claim 55 wherein the additional NOx reduction additive is a hydrotalcite containing composition. 69. The catalyst of claim 55 wherein the additional NOx reduction composition comprises (i) an acidic metal oxide, (ii) cerium oxide, (iii) a lanthanide oxide other than ceria, and (iv) optionally, at least one oxide of a transition metal selected from Groups IB and IIB of the Periodic Table, and mixtures thereof. 70. The catalyst of claim 51 wherein component (a) comprises a Y-type zeolite and component (b) is present in an amount sufficient to provide a ratio of NOx reduction zeolite to Y-type zeolite of less than 2 in the total catalyst. 71. The catalyst of claim 70 wherein component (b) is present in an amount sufficient to provide a ratio of NOx reduction zeolite to Y-type zeolite of less than 1 in the total catalyst. 72. The catalyst of claim 51 wherein the stabilizing metal is selected from the group consisting of lanthanum, aluminum, magnesium and zinc, and mixtures thereof. 73. The catalyst of claim 51 wherein the stabilizing metal is incorporated into the pores of component (b). 74. The catalyst of claim 51 wherein the NOx reduction zeolite is selected from the group consisting of beta, MCM-49, mordenite, MCM-56, Zeolite-L, zeolite Rho, errionite, chabazite, clinoptilolite, MCM-22, Offretite, A, ZSM-12, ZSM-23, omega and mixtures thereof. 75. The catalyst of claim 51 wherein the NOx reduction zeolite has a SiO2 to Al2O3 molar ratio of less than 500. 76. The catalyst of claim 51 further comprising a zeolite other than the NOx reduction zeolite. 77. The catalyst of claim 76 wherein the other zeolite is selected from the group consisting of ferrierite, ZSM-5, ZSM-35 and mixtures thereof. 78. The catalyst of claim 76 or 77 wherein the other zeolite is present in an amount ranging from about 1 to about 80 weight percent of the composition. 79. The catalyst of claim 78 wherein the other zeolite is present in an amount ranging from about 10 to about 70 weight percent of the composition. 80. The catalyst of claim 51 wherein the NOx reduction zeolite is exchanged with a cation selected from the group consisting of hydrogen, ammonium, alkali metal and combinations thereof.
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