Copper-promoted GMElinite and use thereof in the selective catalytic reduction of NOX

Patent metadata

Field	Value
Publication number	US-11298656-B2
Application number	US-201716304511-A
Country	US
Kind code	B2
Filing date	Jun 2, 2017
Priority date	Jun 8, 2016
Publication date	Apr 12, 2022
Grant date	Apr 12, 2022

Abstract

A catalyst for the selective catalytic reduction of NOx comprises a zeolitic material which comprises (A) one or more zeolites having a GME framework structure containing YO2 and X2O3, and optionally further comprises one or more zeolites having a CHA framework structure containing YO2 and X2O3, and/or comprises, (B) one or more zeolite intergrowth phases of one or more zeolites having a GME framework structure containing YO2 and X2O3 and one or more zeolites having a CHA framework structure containing YO2 and X2O3, wherein Y is a tetravalent element, and X is a trivalent element, and the zeolitic material contains Cu and/or Fe as non-framework elements in an amount ranging from 0.1 to 15 wt. % calculated as the element and based on 100 wt. % of YO contained in the zeolitic material. Also provided are a process for its preparation, and a use in a method for the selective catalytic reduction of NOx.

First claim

The invention claimed is:

1. A process for producing a catalyst comprising a zeolitic material, the process comprising:
crystallizing a mixture comprising a source of SiO 2 , a source of Al 2 O 3 , and optionally comprising a seed crystal, to obtain a first zeolitic material comprising a GME framework zeolite and a CHA framework zeolite, and/or to obtain a second zeolitic material comprising a zeolite intergrowth phase comprising a GME framework zeolite and a CHA framework zeolite;
optionally isolating the first and/or second zeolitic material;
optionally washing the first and/or second zeolitic material;

and
optionally drying the first and/or second zeolitic material;
ion-exchanging the first and/or second zeolitic material with Cu and/or Fe; and

obtaining the catalyst which is suitable for selective catalytic reduction of NOx,
wherein the zeolitic material of the catalyst comprises:
Cu and/or Fe; and
(A) a GME framework zeolite comprising SiO 2 and Al 2 O 3 , and a CHA framework zeolite comprising SiO 2 and Al 2 O 3 : and/or (B) a zeolite intergrowth phase comprising a GME framework zeolite comprising SiO 2 and Al 2 O 3 and a CHA framework zeolite comprising SiO 2 and Al 2 O 3 , and
wherein a relative amount of the CHA framework zeolite in the zeolitic material, calculated from an X-ray powder diffraction pattern of the zeolitic material using a Relative Intensity Ratio method, and based on 100% of phases in the zeolitic material comprising the GME and CHA framework zeolite, is in a range of from 10 to 60%.

2. The process of claim 1 , wherein the mixture in the crystallizing further comprises a solvent system comprising a solvent.

3. The process of claim 1 , wherein the mixture in the crystallizing comprises substantially no phosphorous and/or phosphorous containing compounds.

4. A catalyst, produced by the process comprising:
crystallizing a mixture comprising a source of SiO 2 , a source of Al 2 O 3 , and optionally comprising a seed crystal, to obtain a first zeolitic material comprising a GME framework zeolite and a CHA framework zeolite, and/or to obtain a second zeolitic material comprising a zeolite intergrowth phase comprising a GME framework zeolite and a CHA framework zeolite;
ion-exchanging the first and/or second zeolitic material with Cu and/or Fe; and
obtaining the catalyst which is suitable for selective catalytic reduction of NOx,
wherein the first and/or second zeolitic material of the catalyst comprises:
Cu and/or Fe: and
(A) a GME framework zeolite comprising SiO 2 and Al 2 O 3 and a CHA framework zeolite comprising SiO 2 and Al 2 O 3 : and/or (B) a zeolite intergrowth phase comprising a GME framework zeolite comprising SiO 2 and Al 2 O 3 and a CHA framework zeolite comprising SiO 2 and Al 2 O 3 , and
wherein a relative amount of the CHA framework zeolite in the zeolitic material, calculated from an X-ray powder diffraction pattern of the zeolitic material using a Relative Intensity Ratio method, and based on 100% of phases in the zeolitic material comprising the GME and CHA framework zeolite, is in a range of from 10% to 60%; and
wherein the zeolite material has a degree of crystallinity greater than 50%.

5. A catalyst, comprising a zeolitic material comprising:
(A) a zeolite having a GME framework structure comprising SiO 2 and Al 2 O 3 and a zeolite having a CHA framework structure comprising SiO 2 and Al 2 O 3 , and/or
(B) a zeolite intergrowth phase of one or more zeolites having a GME framework structure comprising SiO 2 and Al 2 O 3 and one or more zeolites having a CHA framework structure comprising SiO 2 and Al 2 O 3 ,
wherein the zeolitic material comprises Cu and/or Fe as a non-framework element in a range of from 0.1 wt.-% to 15 wt.-% calculated as an element and based on 100 wt.-% of SiO 2 contained in the zeolitic material, and
wherein the catalyst is suitable for selective catalytic reduction of NOx, and wherein a relative amount of the CHA framework structure in the zeolitic material, calculated from an X-ray powder diffraction pattern of the zeolitic material using a Relative Intensity Ratio method, and based on 100% of phases in the zeolitic material comprising the GME and CHA framework structure, is in a range of from 10% to 60%; and
wherein the zeolite material has a degree of crystallinity greater than 50%.

6. The catalyst of claim 5 , wherein a framework of the zeolitic material comprises substantially no phosphorous.

7. A method for selective catalytic reduction of NOx, the method comprising contacting a gas stream comprising NOx with the catalyst of claim 4 .

8. A method, comprising:
contacting a gas stream comprising NOx with the catalyst according to claim 4 .

9. The catalyst of claim 5 , wherein the zeolitic material comprises (A) the zeolite having a GME framework structure comprising SiO 2 and Al 2 O 3 and the zeolite having a CHA framework structure comprising SiO 2 and Al 2 O 3 .

10. The catalyst of claim 5 , wherein the zeolitic material comprises (B) the zeolite intergrowth phase of one or more zeolites having a GME framework structure comprising SiO 2 and Al 2 O 3 and the one or more zeolites having a CHA framework structure comprising SiO 2 and Al 2 O 3 .

11. The catalyst of claim 5 , wherein the non-framework element comprises Cu.

12. The catalyst of claim 5 , wherein the non-framework element comprises Fe.

13. The catalyst of claim 5 , wherein the non-framework element comprises Cu and Fe.

14. The catalyst of claim 5 , wherein Cu and/or Fe are present in a range of from 0.5 wt.-% to 10 wt.-%.

15. The catalyst of claim 5 , wherein Cu and/or Fe are present in a range of from 2 wt.-% to 5 wt.-%.

16. The catalyst of claim 5 , wherein the relative amount is in a range of from 15 to 50%.

17. The catalyst of claim 5 , wherein the relative amount is in a range of from 20 to 45%.

18. The catalyst of claim 5 , wherein the zeolitic material comprises the SiO 2 and the Al 2 O 3 in an SiO 2 :Al 2 O 3 molar ratio in a range of from 2 to 50.

19. The catalyst of claim 5 , wherein the zeolitic material comprises the SiO 2 and the Al 2 O 3 in an SiO 2 :Al 2 O 3 molar ratio in a range of from 5 to 12.

Assignees

• Basf Corp

Inventors

• Feyen Mathias
• Mueller Ulrich
• Oezkirim Faruk
• Dumser Stefan
• Trukhan Natalia
• Maltry Michaela
• Maurer Stefan

Classifications

• B01J2229/62

  in or on other molecular sieves · CPC title

• B01J29/76

  Iron group metals or copper · CPC title

• B01D53/9413

  Processes characterised by a specific catalyst · CPC title

• B01D53/9418 Primary

  for removing nitrogen oxides by selective catalytic reduction [SCR] using a reducing agent in a lean exhaust gas · CPC title

• B01J37/30

  Ion-exchange · CPC title