MULTIFUNCTIONAL CATALYST FOR NAPHTHA CRACKING

Abstract

The addition of small amounts of alkaline earth metal oxides (CaO, MgO) as the isomerization function and transition metal oxides (such as MoO.sub.3, WO.sub.3) as the metathesis function significantly enhances the production of propylene using zeolites. Once the light olefins are formed by cracking on the acid sites of the zeolite, the 1-butene molecules undergo isomerization catalyzed by alkali earth metal oxides and then react with ethylene to produce more propylene.

Claims

1. A cracking catalyst suitable for the selective cracking of hydrocarbons to light olefins ethylene and propylene with a composition of the general formula (Zeolite)(IF)(MF), wherein: a) Zeolite represents zeolites from the family of Pentasils, Faujasites, Beta and Mordenite, or mixtures thereof wherein the Zeolite species makes up 1 to 75 wt % of the total weight of the cracking catalyst; b) Isomerization function (IF) represents oxides of Alkaline Earth metals selected from the group 2 elements or mixtures thereof wherein the Isomerization Function (IF) makes up 1 to 25 wt % of the total weight of the cracking catalyst; c) metathesis function (MF) represents oxides of Transition metals or mixtures thereof wherein Metathesis Function (MF) makes up 1 to 25 wt % of the total weight of the cracking catalyst; and characterizable by conversion ?85%, propylene selectivity ?30 wt % and a Propylene/Ethylene Ratio ?1 wt/wt using a test where the catalyst is loaded in a fixed-bed reactor such that the 50?d.sub.Tr/d.sub.P?10 (diameter of tube to diameter of catalyst particles) and 200?L/d.sub.P?50 (length of catalyst bed to diameter of catalyst particles) and 2?d.sub.P?0.5 mm (particle diameter) exposed to a feed stream of 1-hexene at a temperature of 625? C., atmospheric pressure and a feed rate of 60 hr.sup.?1 weight hourly space velocity.

2. The cracking catalyst according to claim 1 wherein the Zeolite species makes up 1 to 50 wt % of the total weight of the cracking catalyst.

3. The cracking catalyst according to claim 1 wherein the Zeolite species makes up 1 to 40 wt % of the total weight of the cracking catalyst.

4. The cracking catalyst according to claim 1 wherein the wherein the crystalline zeolite is selected from the group consisting of ZSM-5, Zeolite-Beta, Mordenite, Zeolite X and Zeolite Y and mixtures thereof.

5. The cracking catalyst according to claim 1 wherein the Silica-to-Alumina molar ratio of the Zeolite species varies from 2-1000.

6. The cracking catalyst according to claim 1 wherein the Silica-to-Alumina molar ratio of the Zeolite species varies from 2-400.

7. The cracking catalyst according to claim 1 wherein the Isomerization Function (IF) is selected from the group consisting of Beryllium (Be), Magnesium (Mg), Calcium (Ca), Strontium (Sr), Barium (Ba) and mixtures thereof.

8. The cracking catalyst according to claim 1 wherein the Isomerization Function (IF) makes up 1 to 15 wt % of the total weight of the cracking catalyst.

9. The cracking catalyst according to claim 1 wherein the Isomerization Function (IF) makes up 1 to 10 wt % of the total weight of the cracking catalyst.

10. The cracking catalyst according to claim 1 wherein Metathesis Function (MF) is selected from the group consisting of Titanium, Chromium, Manganese, Iron, Cobalt, Nickel, Copper, Zinc, Yttrium, Zirconium, Niobium, Molybdenum, Tungsten, Lanthanum, Cerium and mixtures thereof.

11. The cracking catalyst according to claim 1 wherein Metathesis Function (MF) makes up 1 to 15 wt % of the total weight of the cracking catalyst.

12. (canceled)

13. The cracking catalyst according to claim 1 wherein mass ratio of the Isomerization Function (IF) to the Metathesis Function (MF) varies from 10:1 to 1:1.

14. (canceled)

15. The cracking catalyst according to claim 1 wherein a support makes up 1 to 25 wt % of the total weight of the cracking catalyst.

16. The cracking catalyst according to claim 1 wherein a support comprises of silica, alumina, clays, kaolin, bentonite, attapulgite, or mixtures thereof.

17. (canceled)

18. The cracking catalyst according to claim 1 wherein the BET surface area >100 m.sup.2/g.

19. The cracking catalyst according to claim 1 wherein the Transition metals are group 6 transition metals.

20. The cracking catalyst according to claim 1 characterizable by conversion >95%, propylene selectivity >40 wt % and a Propylene/Ethylene Ratio >2 wt/wt using a test where the catalyst is loaded in a fixed-bed reactor such that the 50?d.sub.T/d.sub.P?10 (diameter of tube to diameter of catalyst particles) and 200?L/d.sub.P?50 (length of catalyst bed to diameter of catalyst particles) and 2?d.sub.P?0.5 mm (particle diameter) exposed to a feed stream of 1-hexene at a temperature of 625? C., atmospheric pressure and a feed rate of 60 hr.sup.?1 weight hourly space velocity.

21. A method of making the catalyst of claim 1 comprising the steps of: i) dissolving appropriate salts of the Isomerization and Metathesis function or mixtures thereof in water; ii) impregnating the Zeolites with the salt solution; iii) drying the Zeolite impregnated with salt solutions iv) adding the desired binder to the impregnated Zeolite; and v) calcining the resultant mixture for 2-6 hrs in an oxygen containing atmosphere, preferably air, to produce the cracking catalyst particle.

22. The method according to claim 21, wherein the cracking catalyst and support are calcined at 300-1000? C., preferably at 350-800? C. and most preferably at 450-550? C. for 2-6 hrs in an oxygen containing atmosphere, preferably air.

25. A process for cracking hydrocarbons, comprising: passing a mixture of hydrocarbons comprising 4 to 100 carbon atoms into a reaction chamber, wherein the reaction chamber comprises the cracking catalyst according to claim 1; reacting the mixture of hydrocarbons over the cracking catalyst at a reaction temperature of 500-800? C., a weight hourly space velocity of 1-100 hr.sup.?1, and a pressure of 0.01-0.2 MPa; and converting, by wt %, at least 55% of the hydrocarbons in the mixture of hydrocarbons with a propylene selectivity of at least 30 wt %, and a propylene to ethylene mass ratio of at least 1.

24. (canceled)

25. (canceled)

Description

BRIEF DESCRIPTION OF THE DRAWINGS

[0075] FIG. 1 shows performance of various catalysts for naphtha cracking. Cat A is the as-is zeolite. Cat-B is the sample with the zeolite and binder. Cat-C is the zeolite+binder+isomerization function, while Cat D contains the zeolite+binder+isomerization function+metathesis function. The results provide quantifiable advantages of the cracking catalyst invention.

[0076] FIG. 2 shows the effect of SAR (Si/Al ratio) on performance of ZSM-5 based catalysts for naphtha cracking.

EXAMPLES

Example 1

[0077] The catalyst used was a commercial zeolite ZSM-5 from Zeolyst having a SiO.sub.2/Al.sub.2O.sub.3 molar ratio of 30 (Si/Al of 15) and a sodium content of 0.05% by weight. The zeolite was pelletized and sieved to 0.5-1.0 mm particles.

[0078] This catalyst is designated as Catalyst A

Example 2

[0079] The catalyst was prepared by dispersing alumina binder in the form of acidic Dispal (T25N4-80) from Sasol in DI water for 30 minutes, followed by mixing ZSM-5 zeolite having a SiO.sub.2/Al.sub.2O.sub.3 molar ratio of 30 (Si/Al of 15) to the dispersed Dispal for 30 minutes. The excess water was evaporated by heating to obtain paste form. The paste was dried overnight at 120? C., followed by calcination at 500? C. for 4 hours. The alumina binder content in the mixture was targeted to be 60 wt %.

[0080] This catalyst is designated as Catalyst B

Example 3

[0081] The catalyst was prepared by dispersing alumina binder in the form of acidic Dispal (T25N4-80) from Sasol in DI water for 30 minutes, followed by mixing ZSM-5 zeolite having a SiO.sub.2/Al.sub.2O.sub.3 molar ratio of 30 (Si/Al of 15) to the dispersed Dispal for 30 minutes. The excess water was evaporated by heating to obtain paste form. The paste was dried overnight at 120? C. After drying, the catalyst was ground and a solution of 4 wt % magnesium oxide in the form of Mg(NO.sub.3).sub.2*6H.sub.2O precursor in DI water was added to dried catalyst drop-wise via incipient wetness technique followed by drying and calcination at 500? C. for 4 hours.

[0082] This catalyst is designated as Catalyst C.

Example 4

[0083] The catalyst was prepared by dispersing alumina binder in the form of acidic Dispal (T25N4-80) from Sasol in DI water for 30 minutes, followed by mixing ZSM-5 zeolite having a SiO.sub.2/Al.sub.2O.sub.3 molar ratio of 30 (Si/Al of 15) to the dispersed Dispal for 30 minutes. The excess water was evaporated by heating to obtain paste form. The paste was dried overnight at 120? C. After drying, the catalyst was ground and a mixed solution of 4 wt % magnesium oxide in the form of Mg(NO.sub.3).sub.2*6H.sub.2O precursor and 5 wt % tungsten oxide in the form of (NH.sub.4).sub.6W.sub.12O.sub.39*H.sub.2O in DI water was added to dried catalyst drop-wise via incipient wetness technique followed by drying and calcination at 500? C. for 4 hours.

[0084] This catalyst is designated as Catalyst D.

Example: Catalyst Tests

[0085] The above catalysts were tested as follows: a synthesized catalyst was loaded in a fixed-bed quartz reactor with a diameter of 10 mm such that d.sub.T/d.sub.p>10 and L/d.sub.p>50. The catalyst was activated and steamed at 725? C. for 16 hours. After steaming, the reactor temperature was lowered to reaction temperature of 625? C. The reaction was conducted at atmospheric pressure and 60/h WHSV. Product samples were withdrawn and analyzed using gas chromatographs equipped with Plot-Q 30 m columns. The results of naphtha cracking over the above catalysts are shown in FIG. 1.

Example 5

[0086] The catalyst was prepared by dispersing alumina binder in the form of acidic Dispal (T25N4-80) from Sasol in DI water for 30 minutes, followed by mixing ZSM-5 zeolite having a SiO.sub.2/Al.sub.2O.sub.3 molar ratio of 23 (Si/Al of 11.5) to the dispersed Dispal for 30 minutes. The excess water was evaporated by heating to obtain paste form. The paste was dried overnight at 120? C. After drying, the catalyst was ground and a mixed solution of 9 wt % magnesium oxide in the form of Mg(NO.sub.3).sub.2*6H.sub.2O precursor and 1 wt % tungsten oxide in the form of (NH.sub.4).sub.6W.sub.12O.sub.39*H.sub.2O in DI water was added to dried catalyst drop-wise via incipient wetness technique followed by drying and calcination at 500? C. for 4 hours. The alumina binder content in the mixture was targeted to be 60 wt %.

[0087] This catalyst is designated as Catalyst E.

Example 6

[0088] The catalyst used was as in Example 5, with the only difference being the SiO.sub.2/Al.sub.2O.sub.3 molar ratio was 30 (Si/Al of 15) instead of 23.

[0089] This catalyst is designated as Catalyst F.

Example 7

[0090] The catalyst used was as in Example 5, with the only difference being the SiO.sub.2/Al.sub.2O.sub.3 molar ratio was 80 (Si/Al of 40) instead of 23.

[0091] This catalyst is designated as Catalyst G.

Example 8

[0092] The catalyst used was as in Example 5, with the only difference being the SiO.sub.2/Al.sub.2O.sub.3 molar ratio was 280 (Si/Al of 140) instead of 23.

[0093] This catalyst is designated as Catalyst H.

Example 9

[0094] The catalyst used was as in Example 5, with the only difference being the SiO.sub.2/Al.sub.2O.sub.3 molar ratio was 371 (Si/Al of 185.5) instead of 23.

[0095] This catalyst is designated as Catalyst I.

Catalyst Tests

[0096] The above catalysts were tested as in Example Catalyst tests. The results of naphtha cracking over Catalysts E through I are shown in FIG. 2. Based on these results, ZSM-5 zeolites with higher SAR ratios produce higher amounts of propylene.

Example 10

[0097] The catalyst used was as in Example 5, with the only difference being the zeolite used was H-Y zeolite having a SiO.sub.2/Al.sub.2O.sub.3 molar ratio of 5.2 instead of ZSM5 zeolite.

[0098] This catalyst is designated as Catalyst J

Example 11

[0099] The catalyst used was as in Example 5, with the only difference being the zeolite used was H-Beta zeolite having a SiO.sub.2/Al.sub.2O.sub.3 molar ratio of 25 instead of ZSM5 zeolite.

[0100] This catalyst is designated as Catalyst K.

Catalyst Tests

[0101] The above catalysts were tested as in Example Catalyst tests. The results of naphtha cracking over the above catalysts are shown in Table 2.

TABLE-US-00002 TABLE 2 Performance of various catalysts for naphtha cracking Zeolite Used H-Y H-Beta 1-Hexene Conversion 100% 100% Propylene Selectivity 44% 55%

[0102] Results in Table 2 clearly show merits of the invention whereby adding an isomerization and metathesis function to conventional zeolites is able to enhance cracking rates and enhance selectivity to propylene production.

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