IP Library Granted Patent US 8,883,119
Granted Patent B2
US 8,883,119 · App. 13/511,755 · Granted Nov 11, 2014

Process for the preparation of zeolites having CHA structure

Inventors: Ivor Bull (Hopewell Junction, NY); Ulrich Müller (Neustadt, DE)
Assignee: BASF SE
B01J29/7015B01D2257/404C01B39/46B01J35/04B01D2253/108C01B39/00B01D2255/20761B01D2251/2067B01J37/0246B01D2255/50B01D2258/012B01D2257/402C01B39/02C01B39/48B01D53/9418C01B39/04Y02C20/10B01J29/763
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Quick Facts
Patent No.
US 8,883,119
App. No.
13/511,755
Granted
Nov 11, 2014
Kind
B2
Abstract

A process for the preparation of zeolites having CHA framework structure and a composition comprising the molar ratio (n Si02):X203, wherein X is a trivalent element, and wherein n is at least 10, the process comprising (i) preparation of an aqueous solution containing at least one source for X203, wherein X is selected from Al, B, Ga, and a mixture of two or more, and at least one source for Si02, at least one organic structure directing agent (SDA) other than Tetramethylammonium hydroxide (TMAOH), acting as a template for the CHA structure, and Tetramethylammonium hydroxide (TMAOH), wherein the SDA or mixtures thereof are employed in such amounts that the aqueous solution in (i) exhibits a molar ratio of SDA:TMAOH of 0.01 to 5; (ii) hydrothermal crystallization of the aqueous solution according to (i); wherein the aqueous solution of (i) contains copper in an amount less than 0.005 Cu:((n O 2 ):X2O3) where n is in the range of 10 to 50.

Claims (31)

1. A process for the preparation of zeolites having CHA framework structure and a composition comprising the molar ratio (n SiO 2 ):X 2 O 3 , wherein X is a trivalent element, and wherein n is at least 10, the process comprising:

(i) preparation of an aqueous solution containing:

at least one source for X 2 O 3 , wherein X is selected from Al, B, Ga, and a mixture of two or more,

at least one source for SiO 2 ,

at least one organic structure directing agent (SDA) other than Tetramethylammonium hydroxide (TMAOH) as a template for the CHA structure, and

Tetramethylammonium hydroxide (TMAOH),

wherein the SDA or mixtures thereof are employed in such amounts that the aqueous solution in (i) exhibits a molar ratio of SDA:TMAOH in the range of 0.01 to 5;

(ii) hydrothermal crystallization of the aqueous solution according to (i);

wherein the aqueous solution of (i) contains copper in an amount less than 0.005 Cu:((n SiO 2 )+X 2 O 3 ) where n is at least 10.

2. The process of claim 1 , wherein the aqueous solution subjected to hydrothermal crystallization according to (ii) is free of alkali and/or earth alkali metals.

3. The process of claim 1 , wherein the structure directing agent comprises a 1-adamantyltrimethylammonium compound or a mixture of a 1-adamantyltrimethylammonium compound and a benzyltrimethylammonium compound.

4. The process of claim 1 , wherein the pH of the aqueous solution obtained in (i) is in the range of 10 to 14.

5. The process of claim 1 , wherein the ratio of SDA:TMAOH is in the range of 0.7 to 3.

6. The process of claim 1 , wherein the at least one source for SiO 2 and the at least one source for X 2 O 3 are employed in such amounts that the aqueous solution obtained according to (i) exhibits a molar ratio of water relative to the sum of (n X 2 O 3 ) and SiO 2 , relative to the structure directing agent (SDA), optionally the sum of SDAs, and TMAOH

( q H 2 O):[( n SiO 2 )+X 2 O 3 ]:( s SDA):( t TMAOH)

wherein q is at least 10, n is 10 to 1000, s is 0.025 to 0.1 and t is 0.01 to 0.1.

7. The process of claim 1 , wherein the aqueous solution obtained according to (i) has a OH−/Si ratio in the range of 0.1 to 0.5.

8. The process of claim 1 , additionally comprising

(iii) separating the zeolitic material from the suspension obtained according to (ii);

(iv) drying the zeolitic material, separated according to (iii), at a temperature in the range of from 100 to 150° C.;

(v) calcining the zeolitic material, dried according to (iv), at a temperature in the range of from 300 to 750° C.

9. A process for the preparation of zeolites having CHA framework structure and a composition comprising the molar ratio (n SiO 2 ):X 2 O 3 , wherein X is a trivalent element, and wherein n is at least 10, the process comprising:

(i) preparation of an aqueous solution containing:

at least one source for X 2 O 3 , wherein X is selected from Al, B, Ga, and a mixture of two or more,

at least one source for SiO 2 ,

at least one organic structure directing agent (SDA) other than Tetramethylammonium hydroxide (TMAOH) as a template for the CHA structure, and

Tetramethylammonium hydroxide (TMAOH),

wherein the SDA or mixtures thereof are employed in such amounts that the aqueous solution in (i) exhibits a molar ratio of SDA:TMAOH in the range of 0.01 to 5;

(ii) hydrothermal crystallization of the aqueous solution according to (i);

wherein the aqueous solution of (i) contains copper in an amount less than 0.005 Cu:((n SiO 2 )+X 2 O 3 ) where n is at least 10

wherein X comprises Al.

Assignments (3)
NUNC PRO TUNC ASSIGNMENT Recorded Jan 24, 2025
From: BASF SE
To: BASF CATALYSTS LLC
Reel/Frame 070001/0877 →
NUNC PRO TUNC ASSIGNMENT Recorded Jan 24, 2025
From: BASF CATALYSTS LLC
To: BASF MOBILE EMISSIONS CATALYSTS LLC
Reel/Frame 070002/0453 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 19, 2012
From: BULL, IVOR; MUELLER, ULRICH
To: BASF SE
Reel/Frame 028400/0799 →
Continuity (2)
Provisional Application 61263831 · Nov 24, 2009
Related Publication 20120244066A1 · Sep 27, 2012