Aluminum-substituted molecular sieve CIT-13

Patent metadata

Field	Value
Publication number	US-10155666-B2
Application number	US-201715720046-A
Country	US
Kind code	B2
Filing date	Sep 29, 2017
Priority date	Nov 17, 2016
Publication date	Dec 18, 2018
Grant date	Dec 18, 2018

Abstract

Methods are provided for the synthesis of molecular sieve CIT-13 having aluminum incorporated into the framework structure and use of such materials in organic compound conversion and/or sorptive processes.

First claim

The invention claimed is:

1. A method of synthesizing an aluminogermanosilicate molecular sieve having the structure of CIT-13, the method comprising:
(a) providing a reaction mixture comprising:
(1) an aluminosilicate FAU framework type zeolite;
(2) a source of germanium;
(3) a structure directing agent (Q) comprising one or more of 1-methyl-3-(3-methylbenzyl)imidazolium cations, 1-methyl-3-(3,5-dimethylbenzyl)imidazolium cations, 1,2-dimethyl-3-(3-methylbenzyl)imidazolium cations, and 1,2-dimethyl-3-(3,5-dimethylbenzyl)imidazolium cations;
(4) a source of fluoride ions;
(5) water; and

(b) subjecting the reaction mixture to crystallization conditions sufficient to form crystals of the aluminogermanosilicate molecular sieve.

2. The method of claim 1 , wherein the reaction mixture has a composition, in terms of molar ratios, as follows:

(SiO 2 + GeO 2 )/Al 2 O 3
35 to 500

Q/(SiO 2 + GeO 2 )
0.20 to 0.75

F/(SiO 2 + GeO 2 )
0.20 to 0.75

H 2 O/(SiO 2 + GeO 2 )
5 to 20.

3. The method of claim 1 , wherein the reaction mixture has a composition, in terms of molar ratios, as follows:

(SiO 2 + GeO 2 )/Al 2 O 3
50 to 150

Q/(SiO 2 + GeO 2 )
0.25 to 0.65

F/(SiO 2 + GeO 2 )
0.25 to 0.65

H 2 O/(SiO 2 + GeO 2 )
5 to 15.

4. The method of claim 1 , wherein the reaction mixture also contains seeds of a molecular sieve material having the structure of CIT-13.

5. The method of claim 4 , wherein the reaction mixture comprises from 0.01 ppm by weight to 10,000 ppm by weight of seeds.

6. The method of claim 1 , wherein the crystallization conditions include a temperature of from 125° C. to 200° C.

7. An aluminogermanosilicate molecular sieve having a framework structure of CIT-13 and, in its as-synthesized form, comprising one or more of 1-methyl-3-(3-methylbenzyl)imidazolium cations, 1-methyl-3-(3,5-dimethylbenzyl)imidazolium cations, 1,2-dimethyl-3-(3-methylbenzyl)imidazolium cations, and 1,2-dimethyl-3-(3,5-dimethylbenzyl)imidazolium cations in its pores.

8. An aluminogermanosilicate molecular sieve synthesized by the method of claim 1 .

9. The crystalline molecular sieve of claim 7 , having a composition, in terms of molar ratios, as follows:

(SiO 2 + GeO 2 )/Al 2 O 3
50 to 150

Q/(SiO 2 + GeO 2 )
>0 to 0.1

F/(SiO 2 + GeO 2 )
>0 to 0.1

wherein Q is selected from one or more of 1-methyl-3-(3-methylbenzyl)imidazolium cations, 1-methyl-3-(3,5-dimethylbenzyl)imidazolium cations, 1,2-dimethyl-3-(3-methylbenzyl)imidazolium cations, and 1,2-dimethyl-3-(3,5-dimethylbenzyl)imidazolium cations.

10. The aluminogermanosilicate molecular sieve of claim 7 , having a composition, in terms of mole ratios, as follows:

(SiO 2 + GeO 2 )/Al 2 O 3
35 to 500

Q/(SiO 2 + GeO 2 )
>0 to 0.1

F/(SiO 2 + GeO 2 )
>0 to 0.1

wherein Q is selected from one or more of 1-methyl-3-(3-methylbenzyl)imidazolium cations, 1-methyl-3-(3,5-dimethylbenzyl)imidazolium cations, 1,2-dimethyl-3-(3-methylbenzyl)imidazolium cations, and 1,2-dimethyl-3-(3,5-dimethylbenzyl)imidazolium cations.

11. A process for converting a feedstock comprising an organic compound to a conversion product, the process comprising contacting the feedstock with a catalyst at organic compound conversion conditions, the catalyst comprising an active form of the crystalline molecular sieve of claim 8 .

Assignees

• Chevron Usa Inc

Inventors

• Zones Stacey Ian

Classifications

• B01J29/047

  Germanosilicates; Aluminogermanosilicates (B01J29/005 takes precedence) · CPC title

• B01J29/70

  of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 · CPC title

• C01B39/065

  Galloaluminosilicates; Group IVB- metalloaluminosilicates; Ferroaluminosilicates · CPC title

• C01B39/026

  After-treatment · CPC title

• C01B39/48 Primary

  using at least one organic template directing agent · CPC title