US20100251700A1 - HC-SCR System for Lean Burn Engines - Google Patents

HC-SCR System for Lean Burn Engines Download PDF

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Publication number
US20100251700A1
US20100251700A1 US12/732,634 US73263410A US2010251700A1 US 20100251700 A1 US20100251700 A1 US 20100251700A1 US 73263410 A US73263410 A US 73263410A US 2010251700 A1 US2010251700 A1 US 2010251700A1
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catalyst
conduit
treatment system
exhaust
exhaust stream
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Chung-Zong Wan
Patrick Burk
Xiaolai Zheng
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BASF Catalysts LLC
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BASF Catalysts LLC
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Publication of US20100251700A1 publication Critical patent/US20100251700A1/en
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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/18—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control
    • F01N3/20—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control specially adapted for catalytic conversion ; Methods of operation or control of catalytic converters
    • F01N3/2066—Selective catalytic reduction [SCR]
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/18—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control
    • F01N3/20—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control specially adapted for catalytic conversion ; Methods of operation or control of catalytic converters
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/46—Removing components of defined structure
    • B01D53/54—Nitrogen compounds
    • B01D53/56—Nitrogen oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N13/00—Exhaust or silencing apparatus characterised by constructional features ; Exhaust or silencing apparatus, or parts thereof, having pertinent characteristics not provided for in, or of interest apart from, groups F01N1/00 - F01N5/00, F01N9/00, F01N11/00
    • F01N13/009—Exhaust or silencing apparatus characterised by constructional features ; Exhaust or silencing apparatus, or parts thereof, having pertinent characteristics not provided for in, or of interest apart from, groups F01N1/00 - F01N5/00, F01N9/00, F01N11/00 having two or more separate purifying devices arranged in series
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
    • F01N3/023—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles
    • F01N3/0231—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles using special exhaust apparatus upstream of the filter for producing nitrogen dioxide, e.g. for continuous filter regeneration systems [CRT]
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/103—Oxidation catalysts for HC and CO only
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
    • F01N3/28—Construction of catalytic reactors
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2240/00—Combination or association of two or more different exhaust treating devices, or of at least one such device with an auxiliary device, not covered by indexing codes F01N2230/00 or F01N2250/00, one of the devices being
    • F01N2240/30—Combination or association of two or more different exhaust treating devices, or of at least one such device with an auxiliary device, not covered by indexing codes F01N2230/00 or F01N2250/00, one of the devices being a fuel reformer
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2410/00—By-passing, at least partially, exhaust from inlet to outlet of apparatus, to atmosphere or to other device
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2610/00—Adding substances to exhaust gases
    • F01N2610/03—Adding substances to exhaust gases the substance being hydrocarbons, e.g. engine fuel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/10—Internal combustion engine [ICE] based vehicles
    • Y02T10/12—Improving ICE efficiencies

Definitions

  • the present invention relates to emissions treatment systems and methods useful for reducing contaminants in exhaust gas streams.
  • embodiments of the invention are directed to emissions treatment systems, and methods of use, for reducing NOx, the systems including hydrocarbon conversion over a partial oxidation catalyst to generate hydrogen and exhaust gas stream partition.
  • lean burn engines e.g., diesel engines, lean burn gasoline engines and locomotive engines
  • Diesel engines in particular, also offer significant advantages over gasoline engines in terms of their durability, and their ability to generate high torque at low speed.
  • Effective abatement of NOx from lean burn engines is difficult to achieve because NOx conversion rates under fuel lean conditions is very low.
  • conversion of the NOx component of exhaust streams to innocuous components generally requires specialized NOx abatement strategies for operation under fuel lean conditions.
  • LNT catalysts contain NOx sorbent materials capable of adsorbing or “trapping” oxides of nitrogen under lean conditions and platinum group metal components to provide the catalyst with oxidation and reduction functions.
  • NSR NOx storage reduction
  • LNT catalysts contain NOx sorbent materials capable of adsorbing or “trapping” oxides of nitrogen under lean conditions and platinum group metal components to provide the catalyst with oxidation and reduction functions.
  • the LNT catalyst promotes a series of elementary steps which are depicted below in Equations 1-5.
  • NO 2 Equation 1
  • this reaction is typically catalyzed by a platinum group metal component, e.g., a platinum component.
  • the oxidation process does not stop here. Further oxidation of NO 2 to nitrate, with incorporation of atomic oxygen, is also a catalyzed reaction (Equation 2). There is little nitrate formation in the absence of the platinum group metal component even when NO 2 is used as the NOx source.
  • the platinum group metal component has the dual functions of oxidation and reduction. For its reduction role, the platinum group metal component first catalyzes the release of NOx upon introduction of a reductant, e.g., CO (carbon monoxide), H 2 (hydrogen) or HC (hydrocarbon) to the exhaust (Equation 3). This step may recover some NOx storage sites but contribute to limited reduction of NOx species.
  • a reductant e.g., CO (carbon monoxide), H 2 (hydrogen) or HC (hydrocarbon
  • NOx release is then further reduced to gaseous N 2 in a rich environment (Equations 4 and 5).
  • NOx release can be induced by fuel injection even in a net oxidizing environment.
  • H 2 , CO or HC requires overall net rich conditions.
  • a temperature surge can also trigger NOx release because metal nitrate is less stable at higher temperatures.
  • NOx trap catalysis is a cyclic operation. Metal compounds are believed to undergo a carbonate/nitrate conversion, as a dominant path, during lean/rich operations.
  • the system includes a diesel oxidation catalyst (DOC) upstream of the DPF and HC-SCR catalyst. In one or more embodiments, the system includes a diesel oxidation catalyst (DOC) upstream of the DPF and HC-SCR catalyst. In one or more embodiments, the system includes the diesel oxidation catalyst (DOC) is located downstream of the first junction in flow communication with the main exhaust conduit. In one or more embodiments, the system includes the diesel oxidation catalyst (DOC) is located downstream of the first junction in flow communication with the main exhaust conduit. In one or more embodiments, the system includes the diesel oxidation catalyst (DOC) is located downstream of the first junction in flow communication with the main exhaust conduit.
  • the system includes the diesel oxidation catalyst (DOC) is located downstream of the first junction and upstream of the DPF and in flow communication with the main exhaust conduit. In one or more embodiments, the system includes the DOC and DPF are integrated into a single component. In one or more embodiments, the system includes a NH3-SCR catalyst downstream of the HC-SCR catalyst. In one or more embodiments, the system includes an oxidation catalyst downstream of the HC-SCR catalyst.
  • DOC diesel oxidation catalyst
  • the amount of hydrocarbon injector into the slip exhaust stream conduit is controlled by a metering device.
  • the hydrocarbon is onboard fuel in one or more embodiments.
  • a first percentage of the exhaust stream passes through the main exhaust conduit and a second percentage of the exhaust stream passes through the slip exhaust stream conduit, where the first percentage is greater than the second percentage.
  • the second percentage of the exhaust stream is controlled by a metering device located within the slip exhaust stream conduit near the first junction.
  • One or more embodiments of the method further comprise passing the exhaust stream in the main exhaust conduit through a diesel particulate filter located upstream of the HC-SCR catalyst.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel particulate filter located downstream of the HC-SCR catalyst.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel particulate filter located downstream of the first junction and upstream of the second junction.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel oxidation catalyst located upstream of the diesel particulate filter.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel oxidation catalyst located upstream of the diesel particulate filter.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel oxidation catalyst located upstream of the diesel particulate filter.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel oxidation catalyst located downstream of the first junction.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel oxidation catalyst located downstream of the first junction.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel oxidation catalyst located downstream of the first junction.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel oxidation catalyst located downstream of the first junction and upstream of the diesel particulate filter.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel oxidation catalyst located downstream of the first junction and upstream of the diesel particulate filter.
  • One or more method embodiments may include passing the exhaust stream in the main exhaust conduit through a diesel oxidation catalyst located downstream of the first junction and upstream of the diesel particulate filter.
  • FIG. 1 is a schematic view showing an engine emission treatment system according to a detailed embodiment
  • FIG. 4 is an alternative emission treatment system according to one or more embodiments of the invention.
  • FIG. 6 is an alternative emission treatment system according to one or more embodiments of the invention.
  • FIG. 12 is an alternative emission treatment system according to one or more embodiments of the invention.
  • FIG. 13 is a perspective view of a wall flow filter substrate
  • Row periods refer to periods of exhaust treatment where the exhaust gas composition is rich, i.e., has a ⁇ 1.0.
  • Washcoat has its usual meaning in the art of a thin, adherent coating of a catalytic or other material applied to a refractory substrate, such as a honeycomb flow through monolith substrate or a filter substrate, which is sufficiently porous to permit the passage there through of the gas stream being treated.
  • ammonia-generating component means a part of the exhaust system that supplies ammonia (NH 3 ) as a result of its design and configuration driven by engine-out emissions and dosing of reductant (H 2 , CO and/or HC) via engine management or via injection into exhaust. Such a component excludes gas dosing or other externally supplied sources of NH 3 .
  • ammonia-generating components include NOx storage reduction (NSR) catalysts and lean NOx traps (LNT).
  • FIG. 1 shows an emissions treatment system 2 for NOx abatement in an exhaust stream from a lean burn engine 4 according to one embodiment.
  • An exhaust gas stream containing gaseous pollutants e.g., unburned hydrocarbons, carbon monoxide, nitrogen oxides
  • gaseous pollutants e.g., unburned hydrocarbons, carbon monoxide, nitrogen oxides
  • particulate matter is conveyed via a main exhaust conduit 6 in flow communication with a lean burn engine 4 .
  • the exhaust gas stream in the main exhaust conduit 6 is passed through a hydrocarbon selective catalytic reduction catalyst (HC-SCR) 8 in flow communication with the conduit 6 .
  • a slip exhaust stream conduit 10 branches off of the main exhaust conduit 6 .
  • Hydrocarbon feed can be introduced through the conduit 18 in the slip stream upstream of a CPO catalyst 14 .
  • the CPO 14 is effective to convert a portion of the hydrocarbons to carbon monoxide and hydrogen.
  • the CPO 14 according to one or more embodiments is designed to provide sufficient hydrogen to enhance the performance of the HC-SCR 8 .
  • the main exhaust conduit 6 includes an optional additional exhaust system component 22 downstream of the first junction 12 .
  • the additional exhaust system component 22 can be, for example, one or more of a diesel oxidation catalyst, a diesel particulate filter, a reductant injector and an air injector in flow communication with the main exhaust conduit.
  • the optional additional exhaust system component 22 for example, one or more of a diesel oxidation catalyst and a diesel particulate filter, can be placed upstream of the first junction 12 of the main exhaust conduit 6 .
  • the hydrocarbon injector 18 can include a metering device 24 adapted to control the amount of hydrocarbon injected into the slip exhaust stream conduit 10 .
  • the injected hydrocarbon is on-board fuel.
  • the portion of the exhaust gas diverted from the main exhaust conduit 6 is up to about 15%, 14%, 13%, 12% 11%, 10%, 9%, 8%, 7%, 6%, 5%, 4%, 3% or 2% of the total exhaust flow.
  • one or more of the CPO catalyst and the HC-SCR are disposed on a flow through monolith.
  • Additional embodiments of the invention are directed to methods of treating an exhaust stream from a lean burn engine.
  • the exhaust stream is passed through a main exhaust conduit 6 and a portion of the exhaust stream through a slip exhaust stream conduit 10 .
  • the main exhaust conduit 6 comprises a hydrocarbon selective catalytic reduction catalyst (HC-SCR) 8 .
  • the slip exhaust stream conduit 10 comprises a catalytic partial oxidation (CPO) catalyst 14 and hydrocarbons can be injected into the slip exhaust stream conduit 10 upstream of the CPO 14 using a hydrocarbon injector 18 .
  • the slip exhaust stream conduit 10 branches-off of the main exhaust conduit 6 at a first junction 12 and is in flow communication with the CPO 14 .
  • the slip exhaust stream conduit 10 rejoins the main exhaust conduit 6 at a second junction 16 .
  • the second junction 16 is located upstream of the HC-SCR 8 .
  • the CPO 14 is adapted to convert hydrocarbons in the slip exhaust stream conduit 10 to carbon monoxide and hydrogen.
  • Various embodiments of the invention further comprise passing the exhaust stream in the main exhaust conduit 6 through a diesel particulate filter 28 located downstream of the first junction 12 and upstream of the second junction 16 .
  • the exhaust stream in the main exhaust conduit 6 is passed through a diesel oxidation catalyst 30 located downstream of the first junction 12 and upstream of the diesel particulate filter 28 .
  • the diesel oxidation catalyst 30 and the diesel particulate filter 28 are integrated into a single component 32 .
  • the CPO 14 , DOC 30 , DPF 28 as well as optional components 22 can be made of compositions well known in the art and may comprise base metals (e.g., ceria) and/or platinum group metals as catalytic agents.
  • the DOC and/or particulate filter provides several advantageous functions.
  • the catalyst serves to oxidize unburned gaseous and non-volatile hydrocarbons (i.e., the soluble organic fraction of the diesel particulate matter) and carbon monoxide to carbon dioxide and water. Removal of substantial portions of the SOF, in particular, assists in preventing too great a deposition of particulate matter on the HC-SCR 8 .
  • the platinum group metal is selected from the group consisting of platinum, palladium, rhodium and combinations thereof.
  • one or more of the DOC 30 , DPF 28 and optional components 22 are coated on a soot filter, for example, a wall flow filter to assist in the removal of the particulate material in the exhaust stream, and, especially the soot fraction (or carbonaceous fraction) of the particulate material.
  • a soot filter for example, a wall flow filter to assist in the removal of the particulate material in the exhaust stream, and, especially the soot fraction (or carbonaceous fraction) of the particulate material.
  • the DOC in addition to the other oxidation function mentioned above, lowers the temperature at which the soot fraction is oxidized to CO 2 and H 2 O. As soot accumulates on the filter, the catalyst coating assists in the regeneration of the filter.
  • a DPF 28 may be located downstream of the HC-SCR 8 to convert the CO and unconverted fuel species.
  • FIG. 11 shows an alternative embodiment of an emission treatment system comprising an ammonia oxidation (AMOX) catalyst 36 located downstream of the HC-SCR 8 catalyst.
  • AMOX ammonia oxidation
  • the ammonia oxidation catalyst 36 may be useful for removing or abating residual ammonia, which may be referred to as slipped ammonia through the system.
  • Optional components 22 for use with various embodiments of the invention can be, for example, one or more of a diesel oxidation catalyst, a diesel particulate filter, a reductant injector, an air injector, an ammonia oxidation catalyst, an ammonia selective catalytic reduction catalyst in flow communication with the main exhaust conduit. Additionally, the optional components 22 may be a combination of integrated components, including, but not limited to, those shown in FIG. 3 .
  • FIGS. 13 and 14 illustrate a wall flow filter substrate 50 which has a plurality of alternately blocked channels 52 and can serve as a particulate filter.
  • the passages are tubularly enclosed by the internal walls 53 of the filter substrate.
  • the substrate has an inlet end 54 and an outlet end 56 .
  • Alternate passages are plugged at the inlet end 54 with inlet plugs 58 and at the outlet end 56 with outlet plugs to form opposing checkerboard patterns at the inlet 54 and outlet 56 .
  • a gas stream enters through the unplugged channel inlet 60 , is stopped by outlet plug and diffuses through channel walls 53 (which are porous) to the outlet side. The gas cannot pass back to the inlet side of walls because of inlet plugs 58 . If such substrate is utilized, the resulting system will be able to remove particulate matters along with gaseous pollutants.
  • Wall flow filter substrates can be composed of ceramic-like materials such as cordierite, ⁇ -alumina, silicon carbide, aluminum titanate, silicon nitride, zirconia, mullite, spodumene, alumina-silica-magnesia or zirconium silicate, or of porous, refractory metal.
  • Wall flow substrates may also be formed of ceramic fiber composite materials. Specific wall flow substrates are formed from cordierite, silicon carbide, and aluminum titanate. Such materials are able to withstand the environment, particularly high temperatures, encountered in treating the exhaust streams.
  • Wall flow substrates for use in the inventive system can include thin porous walled honeycombs (monoliths) through which the fluid stream passes without causing too great an increase in back pressure or pressure across the article.
  • Ceramic wall flow substrates used in the system can be formed of a material having a porosity of at least 40% (e.g., from 40 to 75%) having a mean pore size of at least 10 microns (e.g., from 10 to 30 microns).
  • the substrates can have a porosity of at least 59% and have a mean pore size of between 10 and 20 microns.
  • DOC 30 , DPF 28 and optional components 22 the substrates can have a porosity of at least 59% and have a mean pore size of between 10 and 20 microns.
  • adequate levels of desired catalyst compositions can be loaded onto the substrates. These substrates are still able retain adequate exhaust flow characteristics, i.e., acceptable back pressures, despite the catalyst loading.
  • U.S. Pat. No. 4,329,162 is herein incorporated by reference with respect to the disclosure of suitable wall flow substrates.
  • Typical wall flow filters in commercial use are typically formed with lower wall porosities, e.g., from about 42% to 50%.
  • the pore size distribution of commercial wall flow filters is typically very broad with a mean pore size smaller than 25 microns.
  • the alloys may also contain small or trace amounts of one or more other metals such as manganese, copper, vanadium, titanium and the like.
  • the surface or the metal substrates may be oxidized at high temperatures, e.g., 1000° C. and higher, to improve the resistance to corrosion of the alloys by forming an oxide layer on the surfaces the substrates. Such high temperature-induced oxidation may enhance the adherence of the refractory metal oxide support and catalytically promoting metal components to the substrate.
  • one or all of the HC-SCR 8 , CPO 14 , DOC 30 , DPF 28 and optional components 22 may be deposited on an open cell foam substrate.
  • Such substrates are well known in the art, and are typically formed of refractory ceramic or metallic materials.
  • the principle of the CPO catalyst is the reaction of fuel with oxygen to yield carbon monoxide and hydrogen according to Equation 8.
  • the CPO comprises a suitable high surface area refractory metal oxide support layer is deposited on a substrate as described above to serve as a support upon which finely dispersed catalytic metal may be distended.
  • high surface area refractory metal oxide supports can be utilized, e.g., alumina support materials, also referred to as “gamma alumina” or “activated alumina,” typically exhibit a BET surface area in excess of 60 square meters per gram (“m 2 /g”), often up to about 200 m 2 /g or higher.
  • BET surface area has its usual meaning of referring to the Brunauer, Emmett, Teller method for determining surface area by N 2 adsorption. Pore diameter and pore volume can also be determined using BET-type N 2 adsorption or desorption experiments.
  • a specific support coating is alumina, for example, a stabilized, high-surface area transition alumina.
  • transition alumina includes gamma, chi, eta, kappa, theta and delta forms and mixtures thereof.
  • certain additives such as, e.g., one or more rare earth metal oxides and/or alkaline earth metal oxides may be included in the transition alumina (usually in amounts comprising from 2 to 10 weight percent of the stabilized coating) to stabilize it against the generally undesirable high temperature phase transition to alpha alumina, which is a relatively low surface area.
  • oxides of one or more of lanthanum, cerium, praseodymium, calcium, barium, strontium and magnesium may be used as a stabilizer.
  • platinum group metal catalytic component of the catalytic partial oxidation catalyst comprises palladium and platinum and, optionally, one or more other platinum group metals.
  • platinum group metals means platinum, palladium, rhodium, iridium, osmium and ruthenium. Suitable platinum group metal components are palladium and platinum and, optionally, rhodium. Desirable catalysts for partial oxidation should have at least one or more of the following properties. They should be able to operate effectively under conditions varying from oxidizing at the inlet to reducing at the exit; they should operate effectively and without significant temperature degradation over a temperature range of about 427° C.
  • the catalytic activity of platinum-palladium combination catalysts is not simply an arithmetic combination of their respective catalytic activities; the disclosed range of proportions of platinum and palladium have been found to provide efficient and effective catalytic activity in treating a rather wide range of hydrocarbon feeds with good resistance to high temperature operation and catalyst poisons.
  • Rhodium may optionally be included with the platinum and palladium. Under certain conditions, rhodium is an effective oxidation as well as a steam reforming catalyst, particularly for light olefins.
  • the combined platinum group metal catalysts can catalyze the autothermal reactions at quite low ratios of H 2 O to carbon (atoms of carbon in the feed) and oxygen to carbon, without significant carbon deposition on the catalyst. This feature provides flexibility in selecting H 2 O to C and O.sub.2 to C ratios in the inlet streams to be processed.
  • platinum group metals employed in the catalysts of embodiments of the present invention may be present in the catalyst composition in any suitable form, such as the elemental metals, as alloys or intermetallic compounds with the other platinum group metal or metals present, or as compounds such as an oxide of the platinum group metal.
  • palladium, platinum and/or rhodium “catalytic component” or “catalytic components” is intended to embrace the specified platinum group metal or metals present in any suitable form.
  • reference in the claims or herein to platinum group metal or metals catalytic component or components embraces one or more platinum group metals in any suitable catalytic form.
  • Suitable CPO catalysts are described in U.S. Pat. No. 4,522,894, the entire content of which is incorporated herein by reference.
  • a HC-SCR catalyst comprising silver on an alumina support is generally useful for the emissions treatment system of this invention.
  • the catalyst contains “well dispersed” silver species on the surface of an alumina.
  • the catalyst substantially free of silver metal and/or silver aluminate.
  • hydroxylated means that the surface of the alumina has a high concentration of surface hydroxyl groups in the alumina as it is obtained, for example boehmite, pseudoboehmite or gelatinous boehmite, diaspore, norstrandite, bayerite, gibbsite, alumina having hydroxyl groups added to the surface, and mixtures thereof.
  • Pseudoboehmite and gelatinous boehmite are generally classified as non-crystalline or gelatinous materials, whereas diaspore, norstrandite, bayerite, gibbsite, and boehmite are generally classified as crystalline.
  • aluminas are not subject to high temperature calcination, which would drive off many or most of the surface hydroxyl groups.
  • the alumina may be of a type subject to higher temperature calcinations to provide gamma, delta, theta and alpha-alumina and combinations thereof.
  • a temperature low enough to fix the silver and decompose the anion Typically for the nitrate salt this would be about 450-550 degrees centigrade to provide an alumina that has substantially no silver particles greater than about 20 nm in diameter.
  • the diameter of the silver is less than 10 nm, and in other embodiments, the silver is less than about 2 nm in diameter.
  • the processing is performed so that the silver is present in substantially ionic form and there is substantially no silver metal present as determined by UV spectroscopy. In one or more embodiments there is substantially no silver aluminate present. The absence of silver metal and silver aluminate can be confirmed by x-ray diffraction analysis. In the presence of small amount of hydrogen and adequate hydrocarbon fuel species, the catalyst can still perform well when it has been deposited with carbonaceous and sulfur species.
  • the oxidation catalyst can be formed from any composition that provides effective combustion of unburned gaseous and non-volatile hydrocarbons (i.e., the VOF) and carbon monoxide.
  • the oxidation catalyst should be effective to convert a substantial proportion of the NO of the NOx component to NO 2 .
  • substantially conversion of NO of the NOx component to NO 2 means at least 20%, and specifically between 30 and 60%.
  • Catalyst compositions having these properties are known in the art, and include platinum group metal- and base metal-based compositions.
  • the catalyst compositions can be coated onto honeycomb flow-through monolith substrates formed of refractory metallic or ceramic (e.g., cordierite) materials.
  • One specific oxidation catalyst composition that may be used in the emission treatment system contains a platinum group component (e.g., platinum, palladium or rhodium components) dispersed on a high surface area, refractory oxide support (e.g., ⁇ -alumina) which is combined with a zeolite component (e.g., a beta zeolite).
  • a specific platinum group metal component comprises platinum and palladium.
  • the concentration of platinum group metal is typically from about 10 to 150 g/ft 3 .
  • the platinum group metal is typically in the range of about 20 g/ft 3 to about 130 g/ft 3 , or about 30 g/ft 3 to about 120 g/ft 3 , or about 40 g/ft 3 to about 110 g/ft 3 or about 50 g/ft 3 to about 100 g/ft 3 .
  • Catalyst compositions suitable for the oxidation catalyst may also be formed using base metals as catalytic agents.
  • U.S. Pat. No. 5,491,120 discloses oxidation catalyst compositions that include a catalytic material having a BET surface area of at least about 10 m.sup.2/g and consist essentially of a bulk second metal oxide which may be one or more of titania, zirconia, ceria-zirconia, silica, alumina-silica, and ⁇ -alumina.
  • compositions that include a catalytic material containing ceria and alumina each having a surface area of at least about 10 m 2 /g, for example, ceria and activated alumina in a weight ratio of from about 1.5:1 to 1:1.5.
  • platinum may be included in the compositions described in the '907 patent in amounts effective to promote gas phase oxidation of CO and unburned hydrocarbons but which are limited to preclude excessive oxidation of SO 2 to SO 3 .
  • palladium in any desired amount may be included in the catalytic material.
  • the system may further comprise a NH 3 -SCR catalyst downstream of the HC-SCR catalyst.
  • the NH 3 -SCR catalyst can prevent any NH 3 generated in the system from releasing to the environment.
  • Suitable NH 3 -SCR catalysts can be any of the known SCR catalysts useful in the Urea-SCR application. It is advantageous that NH 3 -SCR catalyst comprising molecular sieves with CHA X-ray crystal structures (e.g. Cu-CHA, Cu-SAPO) are employed. These molecular sieves with CHA structure exhibiting superior hydrothermal stability and durability are particularly useful in this invention.
  • an exemplary system would include a system of the type shown in FIG. 1 , wherein exhaust from a lean burn engine is in flow communication with component 22 , which may be a suitable catalyst for oxidizing carbon monoxides and hydrocarbons.
  • component 22 which may be a suitable catalyst for oxidizing carbon monoxides and hydrocarbons.
  • a suitable catalyst for a gasoline engine is a three-way catalyst (TWC).
  • Electrolyzers such as proton exchange membranes (PEM) can be used to produce hydrogen on board the a vehicle.
  • PEM proton exchange membranes
  • the PEM splits water into hydrogen and oxygen molecules which can then be compressed and injected into the exhaust.
  • PEM systems require only small amounts of water maintained in the system.
  • Plasma reformers convert gaseous hydrocarbons, like gasoline, diesel fuel, methane, ethane, etc., to hydrogen.
  • a reaction chamber is charged with sufficient fuel and air and a plasma is ignited.
  • the plasma based reaction results in hydrogen evolution.
  • the hydrogen evolution can be optimized with catalytic components.
  • Thermal decomposition devices can crack, or pyrolyze, fuel to yield hydrogen and carbon oxide species. Thermal decomposition generally requires high temperatures for efficient conversion.
  • Steam reformers can generate hydrogen by reacting fuel with water. The reaction is exothermic, resulting in an increased reaction rate. Like electrolysis, a small onboard water source is required for this type of hydrogen injector.
  • the available pore volume of the various supports was determined by titrating the bare support with water while mixing until incipient wetness was achieved. This resulted in a liquid volume per gram of support. Using the final target Ag 2 O level and the available volume per gram of support, the amount of 1M AgNO 3 solution needed was calculated. DI water was added to the silver solution, if needed, so that the total volume of liquid was equal to amount needed to impregnate the support sample to incipient wetness. If the amount of AgNO 3 solution needed exceeds the pore volume of the support, then multiple impregnations were done.
  • the appropriate AgNO 3 solution was added slowly to the support with mixing. After incipient wetness is achieved, the resulting solid was dried at 90° C. for 16 h, then calcined at 540° C. for 2 hours.
  • the catalyst was also optionally subjected to a flowing stream of about 10% steam in air for at least about, typically about 16 hours at 650° C.
  • Catalysts were prepared as described above using commercially available pseudoboehmite (Catapal® C1, 270 m 2 /g, 0.41 cc/g pore volume, 6.1 nm average pore diameter, produced by Sasol, North America) and boehmite (P200 (from Sasol), 100 m 2 /g, 0.47 cc/g pore volume, 17.9 nm average pore diameter) alumina supports. Each alumina was processed until the silver content of the finished catalyst was about 3% by weight on an Ag 2 O basis. A monolith having about 300 cells per square inch was washcoated with the alumina, resulting in a loading of about 2 g/in 3 .
  • the HC-SCR catalyst was placed in front of a DOC/DPF in a configuration in an engine exhaust system and aged on an engine for 50 hours. During the aging, a number of fuel burning cycles to simulate the regeneration of DOC/DPF were employed.
  • the NOx conversion results are shown in FIG. 13 .
  • the engine aged sample as received without any treatment shows about 20% NOx conversion in the entire temperature range evaluated.
  • the catalyst exhibits 10% better NOx conversion at 500° C., 20% better NOx conversion at 400° C., and 50% better NOx conversion at 300° C. when 1000 ppm H 2 is introduced into the simulated exhaust.
  • the presence of hydrogen in the exhaust drastically enhances the NOx performance of the severely deactivated catalyst.

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JP2012522930A (ja) 2012-09-27
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EP2419612A4 (en) 2015-05-27
CN102388207A (zh) 2012-03-21
BRPI1015090A2 (pt) 2016-04-26
KR20120041162A (ko) 2012-04-30

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