# US 9,040,006 B1 · Catalyzed SCR filter and emission treatment method

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- Number: US 9,040,006 B1
- Document ID: US9040006B1
- Status: Granted
- Kind: B1
- Application number: 14/607,777
- Filed: 2015-01-28
- Published: 2015-06-04
- Granted: 2015-05-26
- Earliest claimed: 2003-08-05
- Assignees: BASF SE
- Applicants: BASF Corporation
- Inventors: Joseph A. Patchett; Joseph C. Dettling; Elizabeth A. Przybylski
- Web page: https://patentgrep.com/patent/US9040006B1

## CPC

- B01J 29/7615: {Zeolite Beta}
- B01D 5/0054: {General arrangements, e.g. flow sheets}
- B01D 5/009: {Collecting, removing and/or treatment of the condensate}
- B01D 19/0005: {with one or more auxiliary substances}
- B01D 19/0036: {Flash degasification (the other groups take precedence)}
- B01D 53/9413: {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}
- B01D 53/945: {characterised by a specific catalyst}
- B01D 53/9477: {with catalysts positioned on separate bricks, e.g. exhaust systems}
- B01J 29/76: Iron group metals or copper
- B01J 35/657: {larger than 1000 nm}
- B01J 37/0236: {Drying, e.g. preparing a suspension, adding a soluble salt and drying}
- B01J 37/024: {Multiple impregnation or coating}
- B01J 37/0246: {Coatings comprising a zeolite}
- B01J 37/08: Heat treatment {(B01J37/0009, B01J37/0018 take precedence)}
- F01N 3/0231: {using special exhaust apparatus upstream of the filter for producing nitrogen dioxide, e.g. for continuous filter regeneration systems [CRT]}
- F01N 3/10: by thermal or catalytic conversion of noxious components of exhaust
- F01N 3/106: {Auxiliary oxidation catalysts}
- F01N 3/2066: {Selective catalytic reduction [SCR]}
- F01N 3/2828: {Ceramic multi-channel monoliths, e.g. honeycombs}
- F01N 3/2892: {Exhaust flow directors or the like, e.g. upstream of catalytic device}
- F01N 13/009: {having two or more separate purifying devices arranged in series}
- B01D 53/944: {Simultaneously removing carbon monoxide, hydrocarbons or carbon making use of oxidation catalysts (three-way-catalysts [TWC] B01D53/9445)}
- B01D 2251/2062: Ammonia
- B01D 2251/2067: Urea
- B01D 2255/102: Platinum group metals
- B01D 2255/20715: Zirconium
- B01D 2255/20738: Iron
- B01D 2255/20761: Copper
- B01D 2255/50: Zeolites
- B01D 2255/502: Beta zeolites
- B01D 2255/9155: Wall flow filters
- B01D 2255/9202: Linear dimensions
- B01D 2255/9205: Porosity
- B01D 2257/404: Nitrogen oxides other than dinitrogen oxide
- B01D 2258/012: Diesel engines and lean burn gasoline engines
- B01J 35/56: Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional [3D] monoliths
- F01N 2330/06: Ceramic, e.g. monoliths
- F01N 2330/30: Honeycomb supports characterised by their structural details
- F01N 2370/04: Zeolitic material
- F01N 2510/063: zeolites
- F01N 2610/02: the substance being ammonia or urea
- F01N 2610/08: with prior mixing of the substances with a gas, e.g. air
- Y02T 10/12: Improving ICE efficiencies
- Y10S 55/10: Residue burned
- Y10S 55/30: Exhaust treatment
- Y10T 29/49345: Catalytic device making
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- 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)
- 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)
- Y02T: CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y10S: TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10T: TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION

## Abstract

Provided is a catalyst article for simultaneously remediating the nitrogen oxides (NOx), particulate matter, and gaseous hydrocarbons present in diesel engine exhaust streams. The catalyst article has a soot filter coated with a material effective in the Selective Catalytic Reduction (SCR) of NOx by a reductant, e.g., ammonia.

## Claims

### Claim 1

A method for treating emissions produced in an exhaust stream from a diesel engine comprising NOx and particulate matter, the method comprising:
adding ammonia or an ammonia precursor into the exhaust stream and passing the exhaust stream containing the ammonia through a wall flow monolith wherein particulate matter is filtered and a substantial portion of NOx is reduced to N2;
wherein the wall flow monolith has a plurality of longitudinally extending passages formed by longitudinally extending walls bounding and defining said passages, wherein the passages comprise inlet passages having an open inlet end and a closed outlet end, and outlet passages having a closed inlet end and an open outlet end, the wall flow monolith having a porosity of from 60% to 75% and an average pore size of from 10 to 30 microns;
wherein the wall flow monolith comprises a washcoat of SCR catalyst composition that permeates the walls, the SCR catalyst composition comprising a zeolite and base metal component selected from one or more of a copper and iron component, the washcoat permeating the walls at a loading up to 2.4 g/in3, the wall flow monolith providing integrated NOx and particulate removal efficiency when the exhaust stream comprising NOx and particulate matter passes through the wall flow monolith such that particulate matter is trapped on the wall flow monolith.

### Claim 2 (depends on 1)

The method of claim 1, wherein the method comprises, prior to passing the exhaust stream through the wall flow monolith: passing the exhaust stream through an oxidation catalyst wherein a substantial portion of NO is oxidized to NO2 to provide an NO2-enriched exhaust stream and then metering at periodic intervals ammonia or an ammonia precursor into the NO2-enriched exhaust stream.

### Claim 3 (depends on 2)

The method of claim 2, wherein the substantial portion of NO oxidized to NO2 is at least about 20%.

### Claim 4 (depends on 2)

The method of claim 2, wherein the substantial portion of NO oxidized to NO2 is between about 30% and about 60%.

### Claim 5 (depends on 1)

The method of claim 1, wherein the base metal component is a copper component.

### Claim 6 (depends on 5)

The method of claim 5, wherein the zeolite of the SCR catalyst composition has a silica to alumina ratio of at least about 10.

### Claim 7 (depends on 6)

The method of claim 6, wherein the zeolite of the SCR catalyst composition is a beta zeolite.

### Claim 8 (depends on 1)

The method of claim 1, wherein there is from 1.3 to 2.4 g/in3 of SCR catalyst composition disposed on the wall flow monolith.

### Claim 9 (depends on 1)

The method of claim 1, wherein there is from 1.6 to 2.4 g/in3 of SCR catalyst composition disposed on the wall flow monolith.

### Claim 10 (depends on 1)

The method of claim 1, wherein the base metal component is a copper component and the zeolite of the SCR catalyst composition has a silica to alumina ratio of at least about 10.

### Claim 11 (depends on 10)

The method of claim 10, wherein the zeolite of the SCR catalyst composition is selected from beta zeolite, USY and ZSM-20.

### Claim 12 (depends on 1)

The method of claim 1, wherein the particulate matter trapped on the wall flow monolith is burned to maintain an acceptable back pressure.

### Claim 13 (depends on 1)

The method of claim 1, wherein the SCR catalyst composition contains a copper promoter present in an amount of from about 0.1 to 30 percent by weight of the total weight of promoter plus zeolite.

### Claim 14 (depends on 1)

The method of claim 1, wherein the SCR catalyst composition contains a copper promoter present in an amount of from about 1 to 5 percent by weight of the total weight of promoter plus zeolite.

### Claim 15 (depends on 1)

The method of claim 1, wherein the longitudinally extending walls have an inlet side and an opposing outlet side and SCR catalyst is coated on both the inlet and outlet sides of the walls.

### Claim 16 (depends on 1)

The method of claim 1, wherein the exhaust gas exiting the wall flow monolith is passed through a subsequent SCR catalyst disposed on a honeycomb flow through monolith substrate.

### Claim 17 (depends on 1)

The method of claim 1, wherein greater than about 80% of the particulate matter is removed by the wall flow monolith.

### Claim 18 (depends on 1)

The method of claim 1, wherein the wall flow monolith is comprised of one or more of cordierite, a-alumina, silicon carbide, silicon nitride, zirconia, mullite, spodumene, alumina-silica-magnesia, zirconium silicate, a porous refractory metal or ceramic fiber composite materials.

### Claim 19 (depends on 1)

The method of claim 1, further comprising passing the exhaust stream through a slip oxidation catalyst located downstream of the wall flow monolith, the slip oxidation catalyst oxidizing residual reductant.

### Claim 20 (depends on 1)

The method of claim 1, wherein the average pore size of the wall flow monolith is of from 10 to 25 microns.

### Claim 21

A method for treating emissions produced in an exhaust stream from a diesel engine comprising NOx and particulate matter, the method comprising:
adding ammonia or an ammonia precursor into the exhaust stream and passing the exhaust stream containing the ammonia through a wall flow monolith wherein particulate matter is filtered and a substantial portion of NOx is reduced to N2;
wherein the wall flow monolith has a plurality of longitudinally extending passages formed by longitudinally extending walls bounding and defining said passages, wherein the passages comprise inlet passages having an open inlet end and a closed outlet end, and outlet passages having a closed inlet end and an open outlet end, the wall flow monolith having a porosity of from 60% to 75% and an average pore size of from 10 to 30 microns;
wherein the wall flow monolith comprises a washcoat of SCR catalyst composition that permeates the walls, the SCR catalyst composition comprising a zeolite and base metal component selected from one or more of a copper and iron component, the washcoat permeating the walls at a loading of at least 1.3 g/in3, the wall flow monolith providing integrated NOx and particulate removal efficiency when the exhaust stream comprising NOx and particulate matter passes through the wall flow monolith such that particulate matter is trapped on the filter.

### Claim 22 (depends on 21)

The method of claim 21, wherein the zeolite of the SCR catalyst composition has a silica to alumina ratio of at least 10 and the base metal component is a copper component present in an amount of from about 0.1 to 30 percent by weight of the total weight of promoter plus zeolite.

### Claim 23 (depends on 21)

The method of claim 21, wherein the particulate matter trapped on the wall flow monolith is burned to maintain an acceptable back pressure.

### Claim 24 (depends on 21)

The method of claim 21, wherein the SCR catalyst composition contains a copper promoter present in an amount of from about 1 to 5 percent by weight of the total weight of promoter plus zeolite.

### Claim 25 (depends on 21)

The method of claim 21, wherein the longitudinally extending walls have an inlet side and an opposing outlet side and SCR catalyst is coated on both the inlet and outlet sides of the walls.

### Claim 26 (depends on 21)

The method of claim 21, wherein the exhaust gas exiting the wall flow monolith is passed through a subsequent SCR catalyst disposed on a honeycomb flow through monolith substrate.

### Claim 27 (depends on 21)

The method of claim 21, wherein greater than about 80% of the particulate matter is removed by the wall flow monolith.

### Claim 28 (depends on 21)

The method of claim 21, wherein the wall flow monolith is comprised of one or more of cordierite, a-alumina, silicon carbide, silicon nitride, zirconia, mullite, spodumene, alumina-silica-magnesia, zirconium silicate, a porous refractory metal or ceramic fiber composite materials.

### Claim 29 (depends on 21)

The method of claim 21, wherein the method comprises, prior to passing the exhaust stream through the wall flow monolith: passing the exhaust stream through an oxidation catalyst wherein between about 30% and 60% of NO is oxidized to NO2 to provide an NO2-enriched exhaust stream and then metering at periodic intervals ammonia or an ammonia precursor into the NO2-enriched exhaust stream.

### Claim 30 (depends on 21)

The method of claim 21, wherein the average pore size of the wall flow monolith is of from 10 to 25 microns.