# US 11,298,656 B2 · Copper-promoted GMElinite and use thereof in the selective catalytic reduction of NOX

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- Number: US 11,298,656 B2
- Document ID: US11298656B2
- Status: Granted
- Kind: B2
- Application number: 16/304,511
- Filed: 2017-06-02
- Published: 2019-05-09
- Granted: 2022-04-12
- Earliest claimed: 2016-06-08
- Assignees: BASF SE
- Applicants: BASF Corporation
- Inventors: Mathias Feyen; Ulrich Mueller; Faruk Oezkirim; Stefan Dumser; Natalia Trukhan; Michaela Maltry; Stefan Maurer
- Web page: https://patentgrep.com/patent/US11298656B2

## CPC

- B01D 53/9418: {for removing nitrogen oxides by selective catalytic reduction [SCR] using a reducing agent in a lean exhaust gas}
- B01D 53/56: Nitrogen oxides (B01D53/60 takes precedence)
- B01D 53/60: Simultaneously removing sulfur oxides and nitrogen oxides
- B01D 53/9413: {Processes characterised by a specific catalyst}
- B01J 29/76: Iron group metals or copper
- B01J 29/763: {CHA-type, e.g. Chabazite, LZ-218}
- B01J 29/80: Mixtures of different zeolites
- B01J 35/33: Electric or magnetic properties
- B01J 37/30: Ion-exchange
- C01B 39/023: {Preparation of physical mixtures or intergrowth products of zeolites chosen from group C01B39/04 or two or more of groups C01B39/14 - C01B39/48}
- B01D 2251/2062: Ammonia
- B01D 2255/20738: Iron
- B01D 2255/20761: Copper
- B01D 2255/50: Zeolites
- B01D 2255/92: Dimensions
- B01D 2258/012: Diesel engines and lean burn gasoline engines
- B01J 2229/186: not in framework positions
- B01J 2229/62: in or on other molecular sieves
- B01D: SEPARATION (separating solids from solids by wet methods B03B, B03D; by pneumatic jigs or tables B03B; by other dry methods B07; magnetic or electrostatic separation of solid materials from solid materials or fluids, separation by high-voltage electric fields B03C; centrifuges, vortex apparatus B04; presses per se for squeezing-out liquid from liquid-containing material B30B9/02; treatment of water C02F, e.g. softening by ion-exchange C02F1/42; {arrangements of air intake cleaners in gas turbine plants F02C7/05} ; arrangements or mounting of filters in air-conditioning, air-humidification or ventilation F24F13/28)
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}

## 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.

## Claims

### Claim 1

A process for producing a catalyst comprising a zeolitic material, the process comprising:
crystallizing a mixture comprising a source of SiO2, a source of Al2O3, 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 SiO2 and Al2O3, and a CHA framework zeolite comprising SiO2 and Al2O3: and/or (B) a zeolite intergrowth phase comprising a GME framework zeolite comprising SiO2 and Al2O3 and a CHA framework zeolite comprising SiO2 and Al2O3, 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%.

### Claim 2 (depends on 1)

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

### Claim 3 (depends on 1)

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

### Claim 4

A catalyst, produced by the process comprising:
crystallizing a mixture comprising a source of SiO2, a source of Al2O3, 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 SiO2 and Al2O3 and a CHA framework zeolite comprising SiO2 and Al2O3: and/or (B) a zeolite intergrowth phase comprising a GME framework zeolite comprising SiO2 and Al2O3 and a CHA framework zeolite comprising SiO2 and Al2O3, 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%.

### Claim 5

A catalyst, comprising a zeolitic material comprising:
(A) a zeolite having a GME framework structure comprising SiO2 and Al2O3 and a zeolite having a CHA framework structure comprising SiO2 and Al2O3, and/or
(B) a zeolite intergrowth phase of one or more zeolites having a GME framework structure comprising SiO2 and Al2O3 and one or more zeolites having a CHA framework structure comprising SiO2 and Al2O3,
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 SiO2 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%.

### Claim 6 (depends on 5)

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

### Claim 7 (depends on 4)

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

### Claim 8 (depends on 4)

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

### Claim 9 (depends on 5)

The catalyst of claim 5, wherein the zeolitic material comprises (A) the zeolite having a GME framework structure comprising SiO2 and Al2O3 and the zeolite having a CHA framework structure comprising SiO2 and Al2O3.

### Claim 10 (depends on 5)

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 SiO2 and Al2O3 and the one or more zeolites having a CHA framework structure comprising SiO2 and Al2O3.

### Claim 11 (depends on 5)

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

### Claim 12 (depends on 5)

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

### Claim 13 (depends on 5)

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

### Claim 14 (depends on 5)

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

### Claim 15 (depends on 5)

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

### Claim 16 (depends on 5)

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

### Claim 17 (depends on 5)

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

### Claim 18 (depends on 5)

The catalyst of claim 5, wherein the zeolitic material comprises the SiO2 and the Al2O3 in an SiO2:Al2O3 molar ratio in a range of from 2 to 50.

### Claim 19 (depends on 5)

The catalyst of claim 5, wherein the zeolitic material comprises the SiO2 and the Al2O3 in an SiO2:Al2O3 molar ratio in a range of from 5 to 12.