# US 8,541,331 B2 · Iron-containing aluminosilicate zeolites and methods of making and using same

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- Number: US 8,541,331 B2
- Document ID: US8541331B2
- Status: Granted
- Kind: B2
- Application number: 12/190,993
- Filed: 2008-08-13
- Published: 2009-02-19
- Granted: 2013-09-24
- Earliest claimed: 2007-08-13
- Assignees: PQ Corporation
- Applicants: Hong-Xin Li; William E. Cormier; Bjorn Moden
- Inventors: Hong-Xin Li; William E. Cormier; Bjorn Moden
- Web page: https://patentgrep.com/patent/US8541331B2

## CPC

- B01D 53/8628: {Processes characterised by a specific catalyst}
- B01D 53/9418: {for removing nitrogen oxides by selective catalytic reduction [SCR] using a reducing agent in a lean exhaust gas}
- B01J 29/146: {Y-type faujasite}
- B01J 29/166: {Y-type faujasite}
- B01J 29/24: Iron group metals or copper
- B01J 29/26: containing arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J 29/46: Iron group metals or copper
- B01J 29/48: containing arsenic, antimony, bismuth, vanadium, niobium tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J 29/68: Iron group metals or copper
- B01J 29/69: containing arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J 29/7215: {Zeolite Beta}
- B01J 29/7615: {Zeolite Beta}
- B01J 29/7815: {Zeolite Beta}
- B01J 29/88: Ferrosilicates; Ferroaluminosilicates {(B01J29/005 takes precedence)}
- B01J 35/56: Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional [3D] monoliths
- B01J 35/615: {100-500 m2/g}
- B01J 35/617: {500-1000 m2/g}
- B01J 35/633: {less than 0.5 ml/g}
- B01J 37/0246: {Coatings comprising a zeolite}
- F01N 3/0222: {the structure being monolithic, e.g. honeycombs}
- B01D 2255/20738: Iron
- B01D 2255/50: Zeolites
- B01D 2258/012: Diesel engines and lean burn gasoline engines
- Y02A 50/20: Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
- Y02T 10/12: Improving ICE efficiencies
- 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
- F01N: GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES (arrangements in connection with gas exhaust of propulsion units in vehicles B60K13/00; combustion-air intake silencers specially adapted for, or arranged on, internal-combustion engines F02M35/00; protecting against, or damping, noise in general G10K11/16)
- Y02A: TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02T: CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION

## Abstract

There is disclosed iron-containing aluminosilicate zeolites having both framework iron and iron cations on the ion-exchange sites. There is also disclosed a direct synthesis method of making an iron-containing aluminosilicate zeolite, which does not require the use of an intermediate step, such as ion-exchange or impregnation. In addition, there is disclosed a method of using the iron-containing aluminosilicate zeolite disclosed herein in a selective catalytic reduction reaction, typically in the presence of ammonia, to reduce or remove nitric oxides from exhaust emissions.

## Claims

### Claim 1

An iron-containing aluminosilicate zeolite, wherein the structure of said zeolite has both framework iron and iron cations on the ion-exchange sites, wherein said zeolite exhibits a selective catalytic reduction of nitrogen oxides with NH3 or urea of greater than 40% conversion at 250-300°C. in exhaust gases prior to aging or exposure to steam, and wherein said zeolite has a silica-to-alumina ratio (SAR) of less than 60, and is chosen from Beta and chabazite type zeolites.

### Claim 2 (depends on 1)

The iron-containing aluminosilicate zeolite of claim 1, wherein said iron comprises at least 1% by weight of said zeolite.

### Claim 3 (depends on 2)

The iron-containing aluminosilicate zeolite of claim 2, wherein said iron is present in an amount ranging from 1 to 5% by weight of said zeolite.

### Claim 4 (depends on 1)

The iron-containing aluminosilicate zeolite of claim 1, wherein said SAR ranges from 5 to 50.

### Claim 5 (depends on 1)

The iron-containing aluminosilicate zeolite of claim 1, further comprises at least one additional metal cation on the ion-exchange sites.

### Claim 6 (depends on 5)

The iron-containing aluminosilicate zeolite of claim 5, wherein said at least additional metal is chosen from copper, manganese, cobalt, and silver.

### Claim 7 (depends on 1)

The iron-containing aluminosilicate zeolite of claim 1, wherein said zeolite has both framework iron and iron cations on the ion-exchange sites, wherein said zeolite exhibits a selective catalytic reduction of nitrogen oxides with NH3 or urea of greater than 80% conversion at temperatures ranging from 300° C. to 500° C. in exhaust gases after hydrothermal aging or exposure to steam.

### Claim 8

A direct synthesis method of making an iron-containing aluminosilicate zeolite, said method comprising:
mixing a source of alumina, a source of silica, optionally a structural directing agent, (SDA) and with an iron constituent to form an iron containing synthesis mixture; and
performing at least one heating step on said iron containing synthesis mixture to form an iron-containing aluminosilicate zeolite wherein the structure of said zeolite has both framework iron and iron cations on the ion-exchange sites, wherein said zeolite exhibits a selective catalytic reduction of nitrogen oxides with NH3 or greater than 40% conversion at 250-300°C. in exhaust gases prior to aging or exposer to steam, wherein said iron-containing aluminosilicate zeolite has a silia to alumina ratio (SAR) of less than 60, and is chosen from Beta and chabazite type zeolites.

### Claim 9 (depends on 8)

The method of claim 8, wherein said iron comprises at least 1% by weight of said zeolite.

### Claim 10 (depends on 9)

The method of claim 9, wherein said iron is present in an amount ranging from 1 to 5% by weight of said zeolite.

### Claim 11 (depends on 8)

The method of claim 8, wherein said SAR ranges from 5 to 50.

### Claim 12 (depends on 8)

The method of claim 8, further comprising adding zeolite crystallization seeds to said iron containing synthesis mixture prior to said heating step.

### Claim 13 (depends on 8)

The method of claim 8, wherein said source of silica is chosen from silica sol, sodium silicate, sodium metalsilicate, precipitated silica, silica gel, and silica-alumina.

### Claim 14 (depends on 8)

The method of claim 8, wherein said source of alumina is chosen from sodium aluminate, aluminum nitrate, aluminum hydroxide, alumina, and aluminum sulfate.

### Claim 15 (depends on 8)

The method of claim 8, wherein said source of iron is an iron salt.

### Claim 16 (depends on 15)

The method of claim 15, wherein said iron salt is chosen from ferric nitrate, ferric chloride, ferrous chloride, and ferrous sulfate.

### Claim 17 (depends on 8)

The method of claim 8, wherein said at least one heating step is performed in an autoclave at a temperature ranging from 90° C. to 250° C.

### Claim 18 (depends on 8)

The method of claim 8, further comprising hydrothermal aging said product by exposing it to steam above 500° C.

### Claim 19 (depends on 8)

The method of claim 8, further comprising calcining said product up to 600° C. to produce a calcined product.

### Claim 20 (depends on 19)

The method of claim 19, wherein said calcined product is further subject to an ion-exchange and/or impregnation step to add more iron and/or at least one additional metal.

### Claim 21 (depends on 20)

The method of claim 20, wherein said at least additional metal is chosen from copper, manganese, cobalt, and silver.

### Claim 22 (depends on 1)

A monolith comprising an iron-containing aluminosilicate zeolite of claim 1.

### Claim 23 (depends on 1)

A diesel particulate filter comprising an iron-containing aluminosilicate zeolite of claim 1.