Method of synthesizing an aluminosilicate molecular sieve by a crystal seed-assisted method

Patent metadata

Field	Value
Publication number	US-11634334-B2
Application number	US-202017037409-A
Country	US
Kind code	B2
Filing date	Sep 29, 2020
Priority date	Sep 30, 2019
Publication date	Apr 25, 2023
Grant date	Apr 25, 2023

Abstract

The present disclosure provides a method of synthesizing an aluminosilicate molecular sieve by a crystal seed-assisted method, a natural aluminosilicate clay mineral treated and activated by an alkali is used as a crystal seed for synthesis of the aluminosilicate molecular sieve, and the target molecular sieve product is synthesized by hydrothermal crystallization, wherein the synthesis process does not require addition of conventional crystal seeds of a molecular sieve or use of any organic template agent, thus the synthesized product does not require a calcination process to remove the template agent. The method of synthesizing an aluminosilicate molecular sieve by a crystal seed-assisted method can meet the requirements of both crystallinity and nucleation time, and greatly reduce costs of synthesizing the aluminosilicate molecular sieve, and reduce the environmental pollution caused by removal of the template agent by calcinating.

First claim

What is claimed is:

1. A method of synthesizing an aluminosilicate molecular sieve by a crystal seed-assisted method, comprising:
performing activating treatment of a natural aluminosilicate clay mineral raw material with an alkali source, so as to prepare an activated crystal seed;
mixing an alkali source aqueous solution with an aluminum source until a clear and transparent mixture is obtained, adding a silica sol dropwise into the mixture and stirring constantly, so as to prepare a reactant gel with an element composition controlled to be consistent with a composition of a target molecular sieve product;
adding the activated crystal seed to the reactant gel and mixing to form a reactant precursor;
putting the reactant precursor into a reactor for crystallization, wherein a crystallization temperature is 150-190° C., and a crystallization time is 36-72 h; and
filtering a crystallization product, and washing to be neutral, then drying, so as to obtain the aluminosilicate molecular sieve;
wherein the aluminosilicate molecular sieve is a ZSM-35 molecular sieve, a molar ratio of each component in the reactant gel is controlled as Na 2 O:K 2 O:SiO 2 :Al 2 O 3 :H 2 O=1.5:2.0-3.0:20-30:1:400-1200.

2. The method of synthesizing an aluminosilicate molecular sieve by a crystal seed-assisted method according to claim 1 , wherein an additive amount of the activated crystal seed is 5.0-8.0% with respect to a total mass of a silicon source calculated in terms of silica in the reactant gel.

3. The method of synthesizing an aluminosilicate molecular sieve by a crystal seed-assisted method according to claim 1 , wherein the natural aluminosilicate clay mineral raw material used for preparing the activated crystal seed is at least one selected from kaolin, rectorite, bentonite, illite, montmorillonite, mullite and diatomite.

4. The method of synthesizing an aluminosilicate molecular sieve by a crystal seed-assisted method according to claim 1 , wherein the activating treatment comprises thermal activation, alkali fusion activation, sub-molten salt activation or quasi-solid-phase activation.

5. The method of synthesizing an aluminosilicate molecular sieve by a crystal seed-assisted method according to claim 1 , wherein the crystallization comprises dynamic crystallization or static crystallization.

6. The method of synthesizing an aluminosilicate molecular sieve by a crystal seed-assisted method according to claim 1 , wherein the alkali source used for preparing the activated crystal seed and the reactant gel is sodium hydroxide, potassium hydroxide or mixture thereof; the aluminum source comprises one or more selected from sodium aluminate, aluminum sulfate, aluminum nitrate, aluminum chloride and aluminum hydroxide.

Assignees

• Univ China Petroleum Beijing

Inventors

• Zheng Tao
• Liu Haiyan
• Liu Zhichang
• Meng Xianghai
• Zhang Rui
• Xu Chunming

Classifications

• C01B39/44 Primary

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

• C01B39/26 Primary

  Mordenite type {(C01B39/023, C01B39/026, C01B39/06 take precedence)} · CPC title

• C01P2002/72

  by d-values or two theta-values, e.g. as X-ray diagram · CPC title

• C01P2006/14

  Pore volume · CPC title

• C01P2004/03

  obtained by SEM · CPC title