MCM-56 manufacture

Patent metadata

Field	Value
Publication number	US-9446961-B2
Application number	US-201214238274-A
Country	US
Kind code	B2
Filing date	Aug 16, 2012
Priority date	Sep 16, 2011
Publication date	Sep 20, 2016
Grant date	Sep 20, 2016

Abstract

The present invention provides an improved method for manufacturing high quality porous crystalline MCM-56 material. It also relates to the MCM-56 material manufactured by the improved method, catalyst compositions comprising same and use thereof in a process for catalytic conversion of hydrocarbon compounds. One such conversion process involves production of monoalkylated aromatic compounds, particularly ethylbenzene and cumene, by the liquid or partial liquid phase alkylation of alkylatable aromatic compound, particularly benzene.

First claim

We claim:

1. A method for manufacturing synthetic porous crystalline MCM-56 material comprising the steps of:
a) preparing a first reaction mixture containing sources of alkali or alkaline earth metal (M) cation, an oxide of a trivalent element X, an oxide of a tetravalent element Y, zeolite seed crystals, and water, said first reaction mixture having a composition in terms of mole ratios of oxides within the following ranges:
YO 2 /X 2 O 3 =5 to 35;
H 2 O/YO 2 =10 to 70;
OH − /YO 2 =0.05 to 0.20;
M/YO 2 =0.05 to 3.0;

said first reaction mixture further comprising zeolite seed crystals in an amount from greater than or equal to 0.05 wt. % to less than or equal to 5 wt. %, based on the weight of said first reaction mixture;
b) adding directing agent R to the reaction mixture of step a) to form a second reaction mixture, having said directing agent R in terms of a mole ratio within the following range: R/YO 2 =0.08 to 0.3; and
c) crystallizing said second reaction mixture of step b) under conditions of temperature of from about 90° C. to about 175° C. and a time for less than 90 hours to form a resulting mixture comprising crystals of said MCM-56 material and less than 10 wt. % non-MCM-56 impurity crystals based on the total weight of said MCM-56 crystals in said second reaction mixture, as identified by X-ray diffraction,
wherein said crystals of said MCM-56 material have an X-ray diffraction pattern as shown in Table 1:

TABLE 1

Interplanar d-Spacing

(Angstroms)
Relative Intensity

12.4 ± 0.2 
vs

9.9 ± 0.3
m

6.9 ± 0.1
w

6.4 ± 0.3
w

6.2 ± 0.1
w

3.57 ± 0.07
m-s

3.44 ± 0.07
vs.

2. The method of claim 1 , wherein said amount of said zeolite seed crystals in said first reaction mixture is in the range of greater than or equal to 0.10 wt. % to less than or equal to 3 wt. %, based on the weight of the first reaction mixture.

3. The method of claim 1 , wherein said directing agent R is selected from the group consisting of cyclopentylamine, cyclohexylamine, cycloheptylamine, hexamethyleneimine (HMI), heptamethyleneimine, homopiperazine, and combinations thereof.

4. The method of claim 1 , wherein said directing agent R comprises hexamethyleneimine (HMI), X comprises aluminum and Y comprises silicon.

5. The method of claim 1 , wherein said resulting mixture of step c) comprises less than or equal to about 5 wt. % non-MCM-56 impurity crystals, based on the total weight of said MCM-56 crystals in said second reaction mixture, as identified by X-ray diffraction.

6. The method of claim 1 , wherein said first reaction mixture has a composition in terms of mole ratios of oxides within the following ranges:
YO 2 /X 2 O 3 =15 to 20;
H 2 O/YO 2 =15 to 20;
OH − /YO 2 =0.1 to 0.15;
M/YO 2 =0.11 to 0.15;
said first reaction mixture further comprising zeolite seed crystals in an amount from greater than or equal to 1 wt. % to less than or equal to 3 wt. %, based on the weight of said first reaction mixture; and step b) comprises adding hexamethyleneimine (HMI) as said directing agent R to said first reaction mixture to form a second reaction mixture having HMI in terms of a mole ratio within the range of: HMI/YO 2 =0.1 to 0.2.

7. The method of claim 1 , wherein said conditions of crystallizing step c) include crystallizing said second reaction mixture for less than 40 hours.

8. The method of claim 1 , wherein said conditions of crystallizing step c) include a temperature of from about 125° C. to about 175° C. for from about 20 to about 75 hours.

9. The method of claim 1 , wherein said second reaction mixture of step b) has a solids content of less than 30 wt. % based on the weight of said second reaction mixture.

10. The method of claim 1 , wherein said zeolite seed crystals exhibit the X-ray diffraction pattern for an MCM-22 family material.

11. The method of claim 1 , wherein said zeolite seed crystals exhibit said X-ray diffraction pattern for said MCM-56 crystals as set forth in Table 1.

12. The method of claim 1 , wherein said second reaction mixture of step b) is aged prior to crystallizing step c) for from about 0.5 to about 48 hours at a temperature of from about 25 to about 75° C.

13. The method of claim 1 , further comprising the step of:
d) separating and recovering at least a portion of said crystals of said MCM-56 material from said resulting mixture of step c),
wherein said crystals of MCM-56 from step d) are thermally treated by heating at a temperature of from about 370° C. to about 925° C. for a time of from 1 minute to about 20 hours to form calcined MCM-56 crystals, wherein said calcined MCM-56 crystals have an X-ray diffraction pattern as shown in Table 2:

TABLE 2

Interplanar d-Spacing

(Angstroms)
Relative Intensity

12.4 ± 0.2 
vs

9.9 ± 0.3
m

6.9 ± 0.1
w

6.2 ± 0.1
s

3.55 ± 0.07
m-s

3.42 ± 0.07
vs.

14. The method of claim 1 , wherein said non-MCM-56 impurity crystal is selected from the group consisting of MCM-22, MCM-49, ITQ-1, ITQ-2, PSH-3, SSZ-25, ERB-1, UZM-8 and UZM-8HS and mixtures thereof.

15. The method of claim 1 , wherein said non-MCM-56 impurity crystal is selected from the group consisting of ferrierite, kenyaite and mixtures thereof.

Assignees

• Johnson Ivy D
• Hrycenko Nadya A
• Roth Wieslaw J
• Helton Terry E
• Exxonmobil Chemical Patents Inc

Inventors

• Johnson Ivy D
• Hrycenko Nadya A
• Roth Wieslaw J
• Helton Terry E

Classifications

• Y02P20/52

  using catalysts, e.g. selective catalysts · CPC title

• C07C15/085

  Isopropylbenzene · CPC title

• B01J2229/42

  Addition of matrix or binder particles · CPC title

• B01J29/74

  Noble metals · CPC title

• C07C2529/70

  of types characterised by their specific structure not provided for in groups C07C2529/08 - C07C2529/65 · CPC title