Method for synthesizing a FER/MOR composite molecular sieve

Patent metadata

Field	Value
Publication number	US-11260377-B2
Application number	US-201515541092-A
Country	US
Kind code	B2
Filing date	Dec 28, 2015
Priority date	Jan 4, 2015
Publication date	Mar 1, 2022
Grant date	Mar 1, 2022

Abstract

This application consists of a method for the synthesis of a type of FER/MOR composite molecular sieve. That method consisting of mixing FER seed crystals, MOR seed crystals, a silicon source, water and an acid or alkali, thus yielding a reaction mixture; by adjusting the proportions of the seed crystals added, the silicon-aluminium proportion, acidity/alkalinity and other reaction conditions, it is possible to obtain a dual phase composite molecular sieve within which the proportions of the crystal phases may be adjusted. In the synthesis process to which the method of this application relates, there is no need to add any organic template, thus reducing the cost of the reaction, in addition to reducing likely environmental pollution, thus having major potential applications.

First claim

The invention claimed is:

1. A method for the synthesis of a type of FER/MOR composite molecular sieve, wherein that method includes the following steps:
(a) mixing FER seed crystals, MOR seed crystals, a silicon source, an aluminium source, water and an acid or alkali to obtain a reaction mixture;
(b) subjecting the reaction mixture to a crystallization reaction to obtain FER/MOR composite molecular sieve under conditions where there is no organic template present.

2. The method according to claim 1 , wherein the silicon source is solid silica gel, colloidal silica, sodium silicate, silicon dioxide, tetraethoxysilane, silicic acid, or any mixture of these.

3. The method according to claim 2 , wherein the silicon source is SiO 2 .

4. The method according to claim 1 , wherein the aluminium source is sodium metaaluminate, aluminium hydroxide, aluminium sulphate, boehmite, or any mixture of these.

5. The method according to claim 4 , wherein the aluminium source is Al 2 O 3 .

6. The method according to claim 1 , wherein the FER seed crystals are present at 5-95% by mass, based on the total mass of the FER seed crystals and the MOR seed crystals.

7. The method according to claim 1 , wherein the MOR seed crystals are present at 5-95% by mass, based on the total mass of the FER seed crystals and the MOR seed crystals.

8. The method according to claim 1 , wherein the FER crystals are present at not less than 33% by mass, based on the total mass of the FER seed crystals and the MOR seed crystals.

9. The method according to claim 1 , wherein the alkali is used to obtain the reaction mixture, and the alkali is an inorganic alkali.

10. The method according to claim 9 , wherein the inorganic alkali is sodium hydroxide, potassium hydroxide, ammonium hydroxide, or any mixture of these.

11. The method according to claim 1 , wherein the acid is used to obtain the reaction mixture, and the acid is an inorganic acid.

12. The method according to claim 11 , wherein the inorganic acid is sulphuric acid, hydrochloric acid, nitric acid, or any mixture of these.

13. The method according to claim 1 , wherein the reaction mixture has a pH of 9 or above.

14. The method according to claim 1 , wherein water and the aluminium source are present in the reaction mixture such that mole ratio between the alkali, measured as OH − , and the aluminium source, measured as Al 3+ is between 1.25:1 and 15:1.

15. The method according to claim 1 , wherein water, the silicon source and the aluminium source are present in the reaction mixture such that mole ratio between the silicon source, measures as Si 4+ , and the aluminium source, measured as Al 3+ , is between 2.5:1 and 25:1.

16. The method according to claim 1 , wherein water and the aluminium source are present in the reaction mixture such that mole ratio between water and the aluminium source, measured as Al 3+ , is between 100:1 and 1000:1.

17. The method of claim 1 , wherein step (b) comprises subjecting the reaction mixture of step (a) to a reaction under conditions of self-generated pressure and a temperature of between 140-220° C. for between 20-120 hours.

18. The method of claim 1 , wherein the crystallization reaction takes place in a reactor which includes a rotating oven, the rate of rotation of the rotating oven being between 30-100 rpm.

19. The method according to claim 1 , further comprising a step of pre-crystallization of the reaction mixture takes place under conditions of 80-120° C. for between 4-24 hours between step (a) and step (b).

20. The method according to claim 19 , wherein the pre-crystallization takes place in a reactor with a rotating oven, the speed of rotation of that rotating oven being between 30-100 rpm.

21. The method according to claim 1 , further comprising the step of separating the FER/MOR composite molecular sieve after step (b).

22. The method of claim 1 , wherein the FER seed crystals and MOR seed crystals are processed by calcination prior to the mixing step.

23. The method of claim 1 , wherein the FER seed crystals or MOR seed crystals are ammonium type molecular sieve, nitrogen type molecular sieve or sodium type molecular sieve.

24. The method according to claim 1 , wherein the FER seed crystals are present at 5-80% by mass, based on the total mass of the FER seed crystals and the MOR seed crystals.

25. The method according to claim 1 , wherein the FER seed crystals are present at 30-80% by mass, based on the total mass of the FER seed crystals and the MOR seed crystals.

Assignees

• Dalian Inst Chem & Physics Cas
• Bp China Holdings Ltd

Inventors

• Li Xiujie
• Liu Shenglin
• Zhu Xiangxue
• Xie Sujuan
• Xu Longya
• Yang Zhiqiang
• Liu Xuebin

Classifications

• C07C2529/18

  of the mordenite type · CPC title

• B01J29/80 Primary

  Mixtures of different zeolites · CPC title

• B01J2229/62

  in or on other molecular sieves · CPC title

• C01B39/44

  Ferrierite type, e.g. types ZSM-21, ZSM-35 or ZSM-38 · CPC title

• C07C2529/80

  Mixtures of different zeolites · CPC title