One-pot method for the synthesis of Cu-SSZ-13, the compound obtained by the method and use thereof

Patent metadata

Field	Value
Publication number	US-9878313-B2
Application number	US-201314442492-A
Country	US
Kind code	B2
Filing date	Dec 6, 2013
Priority date	Dec 12, 2012
Publication date	Jan 30, 2018
Grant date	Jan 30, 2018

Abstract

Process for the direct synthesis of Cu-SSZ-13 from a synthesis mixture comprising water, at least one silicon source, at least one Al source, at least one Cu source, at least one polyamine for complexing with Cu, and a single organic structure directing agent. A Cu containing molecular sieve having the framework structure of SSZ-13, obtainable by the process and use of the Cu containing molecular sieve.

First claim

The invention claimed is:

1. Process for the direct synthesis of Cu-SSZ-13 comprising the following steps:
(i) preparing a mixture containing water, at least one silicon source, at least one Al source, at least one Cu source, at least one polyamine for complexing with Cu and a single OSDA component selected from N,N,N-trimethyl-1-adamantammonium, or benzyl trimethylammonium cations, optionally one or more precursors including alkali cations [Alk] and fluoride anions [F] to obtain a final synthesis mixture having the following molar composition:
Si02: a A1203: b Cu: c Polyamine: d OSDA: e H20: f Alk: g F
wherein
a is in the range from 0.007 to 0.16;
b is in the range from 0.001 to 0.6;
c is in the range from 0.001 to 0.6;
d is in the range from 0.001 to 2;
e is in the range from 1 to 200;
f is in the range from 0 to 1; and
g is in the range from 0 to 1;
(ii) hydrothermal treating the final synthesis mixture at a temperature of 80-200° C. until formation of a crystalline material of Cu-SSZ-13; and
(iii) recovering the crystalline material of Cu-SSZ-13.

2. The process of claim 1 , wherein the at least one polyamine comprises primary, secondary and/or tertiary amines.

3. The process of claim 1 , wherein the at least one polyamine is selected from tetraethylenepentamine, triethylene-tetramine, 1,4,8,11-tetraazacyclotetradecane, 1,4,8,11-tetramethyl-1,4,8,11-tetraazacyclotetradecane.

4. The process according to claim 1 , wherein the final synthesis mixture has the following molar composition:
Si0 2 : a A1 2 0 3 : b Cu: c Polyamine: d OSDA: e H 2 0: f Alk: g F
wherein
a is in the range from 0.01 to 0.06; more preferably in the range from 0.015 to 0.05, and more preferably in the range from 0.02 to 0.05;
b is in the range from 0.01 to 0.4, and more preferably in the range from 0.02 to 0.2;
c is in the range from 0.01 to 0.4, and more preferably in the range from 0.02 to 0.2;
d is in the range from 0.05 to 1, and more preferably in the range from 0.1 to 0.7;
e is in the range from 2 to 100, and more preferably in the range from 2 to 50;
f is in the range from 0 to 0.6, and more preferably in the range from 0 to 0.5; and
g is in the range from 0 to 0.6, and more preferably in the range from 0 to 0.5.

5. The process according to claim 1 , wherein the hydrothermal treating in step (ii) is performed in an autoclave under static or dynamic conditions.

6. The process according to claim 1 , wherein the temperature for the hydrothermal treatment in step (ii) is between 100 and 200° C., more preferably between 130 and 175° C.

7. The process according to claim 1 , wherein crystals of SSZ-13 are added as seeds to the mixture or to the final synthesis mixture in amounts up to 25% by weight calculated on the total amount of oxides.

8. The process according to claim 1 , further comprising a step for removal of organic occluded inside the crystalline material of Cu-SSZ-13 by extraction and/or theimal treatment at temperatures over 25° C.

Assignees

• Haldor Topsoe As

Inventors

• Marin Manuel Moliner
• Franco Raquel Martinez
• Canós Avelino Corma
• Thøgersen Joakim Reimer

Classifications

• B01D2255/50

  Zeolites · CPC title

• B01J29/763

  CHA-type, e.g. Chabazite, LZ-218 · CPC title

• B01D53/04

  with stationary adsorbents {(B01D53/025 takes precedence)} · CPC title

• B01D53/8628

  Processes characterised by a specific catalyst · CPC title

• B01J29/76 Primary

  Iron group metals or copper · CPC title