Process for preparing zeolite beta and use thereof

Patent metadata

Field	Value
Publication number	US-9555402-B2
Application number	US-201314650692-A
Country	US
Kind code	B2
Filing date	Dec 10, 2013
Priority date	Dec 10, 2012
Publication date	Jan 31, 2017
Grant date	Jan 31, 2017

Abstract

Method for preparing zeolite beta which method comprises crystallization of zeolite beta from a solution comprising a template, a silicon source and an aluminum source in which the template is polymeric compound comprising ionizable polydiallyldimethylammonium (PDADMA) cationcrystallization. Furthermore, the present invention provides the use of thus prepared zeolite beta in catalysts for hydrocarbon conversions.

First claim

That which is claimed is:

1. A method for preparing zeolite beta which method comprises crystallization of zeolite beta from a solution consisting essentially of a template, a silicon source and an aluminum source in which the template is a polymeric compound comprising a ionizable polydiallyldimethylammonium (PDADMA) cation.

2. A method according to claim 1 , wherein the zeolite beta is prepared by hydrothermal crystallization of a solution comprising PDADMA and a silicon source which are present in a molar ratio SiO 2 /PDADMA between the silicon source calculated as SiO 2 and the polymeric compound calculated as the cationic PDADMA monomer is 1-10, the molar ratio SiO 2 /M 2 O between the silicon source calculated as SiO 2 and the base source calculated as alkali metal oxide M 2 O is of 1-10.

3. A method according to claim 1 , wherein the hydrothermal crystallization is carried out at a temperature of 150-230° C.

4. The method according to claim 1 , wherein the molar ratio SiO 2 /Al 2 O 3 between the silicon source calculated as SiO 2 and the aluminum source calculated as Al 2 O 3 is of 20-100.

5. The method of claim 1 , comprising dissolving the aluminum source and the base source in the water, adding the polymeric PDADMA compound and stirring for a time period of 0.2-1.5 h.

6. The method of claim 1 , wherein the product obtained by crystallization is filtered, dried and calcined sequentially to obtain a final zeolite beta with a composite pore structure.

7. The method of claim 1 , wherein the templating polymeric PDADMA compound has a molecular weight of 1×10 5 -5×10 5 .

8. The method of claim 1 , wherein the templating polymeric PDADMA compound is PDADMA salt.

9. The method of claim 8 , wherein the templating PDADMA salt is added to the preparation solution in the form of an aqueous solution with a solid content of 10-60 wt %.

10. A hydroconversion catalyst, comprising from 5 to 95 wt % zeolite beta prepared by crystallization of zeolite beta from a solution comprising a template, a silicon source and an aluminum source in which the template is polymeric compound comprising ionizable polydiallyldimethylammonium (PDADMA) cation; from 5 to 95 wt % refractory oxide binder; and from 0.01 to 30 wt % catalytically active metal, wherein the percentages are based on the total dry weight of the catalyst.

11. A hydrocarbon conversion process, which comprises contacting hydrocarbon compounds with the hydroconversion catalyst of claim 10 and hydrogen at a reaction temperature in the range of from 250 to 500° C. and reactor inlet pressure in the range of from 3×10 6 to 3×10 7 Pa.

12. The process of claim 11 , wherein the hydrocarbon conversion process is chosen from the group consisting of pyrolysis of polyethylene, alkylation of benzene with benzyl alcohol (ABB), condensation of benzaldehyde with hydroxyacetophenone (CBH), and alkylation of phenol with tert-butyl alcohol (APT).

13. The hydroconversion catalyst according to claim 10 , wherein the zeolite beta is prepared by hydrothermal crystallization of a solution comprising PDADMA and a silicon source which are present in a molar ratio SiO 2 /PDADMA between the silicon source calculated as SiO 2 and the polymeric compound calculated as the cationic PDADMA monomer is 1-10, the molar ratio SiO 2 /M 2 O between the silicon source calculated as SiO 2 and the base source calculated as alkali metal oxide M 2 O is of 1-10.

14. The hydroconversion catalyst according to claim 10 , wherein the hydrothermal crystallization is carried out at a temperature of 150-230° C.

15. The hydroconversion catalyst according to claim 10 , wherein the molar ratio SiO 2 /Al 2 O 3 between the silicon source calculated as SiO 2 and the aluminum source calculated as Al 2 O 3 is of 20-100.

16. The hydroconversion catalyst according to claim 10 , comprising dissolving the aluminum source and the base source in the water, adding the polymeric PDADMA compound and stirring for a time period of 0.2-1.5 h.

17. The hydroconversion catalyst according to claim 10 , wherein the product obtained by crystallization is filtered, dried and calcined sequentially to obtain a final zeolite beta with a composite pore structure.

18. The hydroconversion catalyst according to claim 10 , wherein the templating polymeric PDADMA compound has a molecular weight of 1×10 5 -5×10 5 .

19. The hydroconversion catalyst according to claim 10 , wherein the templating polymeric PDADMA compound is PDADMA salt.

20. The hydroconversion catalyst according to claim 19 , wherein the templating PDADMA salt is added to the preparation solution in the form of an aqueous solution with a solid content of 10-60 wt %.

Assignees

• Shell Oil Co

Inventors

• Xiao Fengshou
• Meng Xiangju
• Zhu Jie

Classifications

• B01J2235/00

  Indexing scheme associated with group B01J35/00, related to the analysis techniques used to determine the catalysts form or properties · CPC title

• B01J2235/15

  X-ray diffraction · CPC title

• B01J2235/30

  Scanning electron microscopy; Transmission electron microscopy · CPC title

• B01J35/70

  characterised by their crystalline properties, e.g. semi-crystalline (catalysts comprising carbon B01J21/18; molecular sieves B01J29/00) · CPC title

• B01J35/30

  characterised by their physical properties · CPC title