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