WO2016060050A1 - 排ガス浄化用触媒 - Google Patents
排ガス浄化用触媒 Download PDFInfo
- Publication number
- WO2016060050A1 WO2016060050A1 PCT/JP2015/078551 JP2015078551W WO2016060050A1 WO 2016060050 A1 WO2016060050 A1 WO 2016060050A1 JP 2015078551 W JP2015078551 W JP 2015078551W WO 2016060050 A1 WO2016060050 A1 WO 2016060050A1
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- Prior art keywords
- exhaust gas
- region
- downstream
- catalyst
- partition wall
- Prior art date
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Images
Classifications
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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
- F01N3/24—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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
- B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
-
- 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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/42—Platinum
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/46—Ruthenium, rhodium, osmium or iridium
- B01J23/464—Rhodium
-
- 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
- F01N3/033—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 in combination with other devices
- F01N3/035—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 in combination with other devices with catalytic reactors, e.g. catalysed diesel particulate filters
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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
- F01N3/24—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
- F01N3/2803—Construction of catalytic reactors characterised by structure, by material or by manufacturing of catalyst support
- F01N3/2825—Ceramics
- F01N3/2828—Ceramic multi-channel monoliths, e.g. honeycombs
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2255/00—Catalysts
- B01D2255/90—Physical characteristics of catalysts
- B01D2255/915—Catalyst supported on particulate filters
- B01D2255/9155—Wall flow filters
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2255/00—Catalysts
- B01D2255/90—Physical characteristics of catalysts
- B01D2255/92—Dimensions
- B01D2255/9202—Linear dimensions
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/60—Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
-
- 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
- F01N2370/00—Selection of materials for exhaust purification
- F01N2370/02—Selection of materials for exhaust purification used in catalytic reactors
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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
- F01N2510/00—Surface coverings
- F01N2510/06—Surface coverings for exhaust purification, e.g. catalytic reaction
- F01N2510/068—Surface coverings for exhaust purification, e.g. catalytic reaction characterised by the distribution of the catalytic coatings
- F01N2510/0682—Surface coverings for exhaust purification, e.g. catalytic reaction characterised by the distribution of the catalytic coatings having a discontinuous, uneven or partially overlapping coating of catalytic material, e.g. higher amount of material upstream than downstream or vice versa
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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
- F01N3/02—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
- F01N3/022—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 characterised by specially adapted filtering structure, e.g. honeycomb, mesh or fibrous
- F01N3/0222—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 characterised by specially adapted filtering structure, e.g. honeycomb, mesh or fibrous the structure being monolithic, e.g. honeycombs
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- 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 an exhaust gas purifying catalyst provided in an exhaust system of an internal combustion engine. Specifically, the present invention relates to a wall flow type exhaust gas purification catalyst. Note that this international application claims priority based on Japanese Patent Application No. 2014-211381 filed on Oct. 16, 2014, the entire contents of which are incorporated herein by reference. Yes.
- Exhaust gas emitted from internal combustion engines such as automobile engines contains harmful components such as particulate matter (particulate matter; PM), hydrocarbons (HC), carbon monoxide (CO), and nitrogen oxides (NO x ). included.
- particulate matter particulate matter
- HC hydrocarbons
- CO carbon monoxide
- NO x nitrogen oxides
- the wall flow type exhaust gas purification catalyst has an inlet cell with an open end on the exhaust gas inflow side, an exit cell with an open end on the exhaust gas outflow side, and a porous partition wall (rib wall) that separates both cells. And.
- the exhaust gas-purifying catalyst includes a catalyst layer including a catalyst metal and a carrier that supports the catalyst metal particles.
- the exhaust gas discharged from the internal combustion engine flows into the inlet cell from the end on the exhaust gas inflow side, passes through the pores of the porous partition wall, and flows out from the end on the exhaust gas outflow side of the exit cell. To do.
- the exhaust gas component is purified (detoxified).
- Patent Documents 1 and 2 are cited as related art documents related to this.
- Patent Document 1 discloses an exhaust gas purifying catalyst including a two-layered catalyst layer. Specifically, a second catalyst layer including a first catalyst layer including Pd in the entire partition wall and including Rh on the surface of the partition wall in contact with the inlet cell so as to completely cover the first catalyst layer.
- An exhaust gas purifying catalyst having the above catalyst layer is disclosed.
- the first catalyst layer is provided on the entire inside of the partition wall, and the second catalyst layer is formed on the first catalyst layer.
- the pressure loss may increase excessively.
- eco-cars equipped with energy-saving mechanisms such as hybrid engines and idling stops have been spreading.
- the engine is repeatedly started and stopped during operation or during a temporary stop such as waiting for a signal.
- the temperature of exhaust gas repeatedly rises and falls.
- the present invention has been made in view of such circumstances, and an object thereof is to provide an exhaust gas purifying catalyst excellent in exhaust gas purifying performance while suppressing an increase in pressure loss.
- the exhaust gas purifying catalyst according to the present invention is a wall flow type exhaust gas purifying catalyst that is disposed in an exhaust pipe of an internal combustion engine such as an automobile engine and purifies exhaust gas discharged from the internal combustion engine.
- Such an exhaust gas purifying catalyst includes a base material having a wall flow structure, an upstream coat region, and a downstream coat region.
- the base material of the wall flow structure includes an entrance cell having an open end on the exhaust gas inflow side, an exit cell having an open end on the exhaust gas outflow side, and a porous partitioning the entrance cell and the exit cell. Quality partition walls.
- the upstream coat region is formed along the extending direction of the partition wall from the end portion on the exhaust gas inflow side in the partition wall in contact with the inlet side cell, and includes a catalyst metal and a carrier supporting the catalyst metal particles. It is out.
- the downstream coating region, in the partition wall in contact with the outlet side cells along the extending direction from an end portion of the exhaust gas outflow side is formed in a shorter than full length L w length of the partition, the catalytic metal and the catalyst metal And a carrier for supporting the particles.
- the catalyst metal is unevenly distributed in a surface layer portion that abuts on the outlet cell.
- the exhaust gas that has flowed into the inlet cell passes through the partition walls (in the pores of the partition walls). For this reason, the exhaust gas at the time of passing through the partition wall can be effectively purified by providing the upstream coat region inside the partition wall. Further, the exhaust gas after passing through the partition wall often flows straight toward the exhaust gas outflow side end of the exit side cell. For this reason, in the downstream coat region, the catalyst metal is unevenly distributed on the surface portion in contact with the exit cell, so that the exit cell can be brought into contact with exhaust gas that travels straight. As a result, purification performance can be improved.
- the providing the upstream coat area inside the partition wall by providing a length L D of the extending direction of the downstream coat area in total length L w shorter than the length of the partition wall, it is possible to suppress an increase in pressure loss . Therefore, according to the above configuration, exhaust gas purification performance can be improved while suppressing an increase in pressure loss.
- the phrase “the coating region is formed inside the partition wall” means that most of the coating region exists (is unevenly distributed) inside the partition wall.
- the total amount of catalyst metal in the range of a length of 0.1 Lw from the end on the exhaust gas inflow side toward the extending direction is 100% by mass.
- the catalyst metal present on the inner side of the partition wall at this time is typically 80% by mass or more, for example 90% by mass or more, preferably 95% by mass or more. Therefore, for example, when a coat region is formed outside the partition wall (typically on the surface), a part of the coat region unintentionally erodes into the partition wall. Are distinguished.
- “catalyst metal is unevenly distributed on the surface layer portion in contact with the exit side cell” means that a portion of the catalyst metal contained in the downstream coat region is in contact with the exit side cell. It exists in (is unevenly distributed).
- the total thickness of the downstream coating area when the T D within a depth from the surface of the exit-side cell side 0.5 T D, typically within 0.3 T D, for example, within 0.2T D, in particular refers to include in the region within 0.1 T D, more generally 80 wt% of the total amount of catalyst metal contained in the downstream coating zone.
- the downstream coat region is relatively close to the first downstream coat region that is relatively close to the entry-side cell in the thickness direction orthogonal to the stretching direction. It is divided into two areas, the second downstream coat area close to the exit cell.
- the first downstream coat region is substantially free of the catalyst metal.
- the second downstream coat region contains the catalyst metal.
- the downstream coating region is clearly divided into two regions according to the loading ratio of the catalytic metal, and the catalytic metal is concentrated on only the second downstream coating region that is in contact with the exit side cell, so that the capacity of the catalytic metal is not affected. It can be demonstrated. As a result, the contact frequency between the catalyst metal and the exhaust gas can be increased accurately, and the emission can be reduced at a higher level.
- substantially no catalyst metal means that the catalyst metal is not intentionally mixed in forming the first downstream coat region. Therefore, for example, in the formation of another coat region, or in the use stage of the exhaust gas purifying catalyst, it is allowed to mix an unintended catalyst metal from another coat region. Needless to say, inevitable mixing of trace components is allowed.
- the amount of catalyst metal in the first downstream coat region is approximately 5% by mass or less, for example, 1% by mass. Hereinafter, it means that the content is reduced to 0.1% by mass or less.
- the length L D of the extending direction of the downstream coating region is 10% to 50% of the L w.
- the length L U of the extending direction of the upstream coating region is 90% or less 60% of the L w. That is, the upstream coating region, the inside of the partition wall contacting the upper entry side cell, are formed in a shorter than full length L w length of the partition wall along the extending direction of the partition wall from the end portion of the exhaust gas inlet side Yes.
- L U and 60% or more of L w it is possible to increase the frequency of contact between exhaust gas and catalyst metal passes through the partition walls, it is possible to exert a higher exhaust gas purification performance.
- 90% or less of L w it is possible to suitably suppress the increase in the pressure loss.
- the L U and the L D satisfy the following formula: L w ⁇ (L U + L D ) ⁇ 2L w ;
- the upstream coat region and the downstream coat region are configured to partially overlap in the extending direction.
- exhaust gas components can be purified more accurately, and emission can be reduced at a higher level. . Therefore, it is possible to realize an exhaust gas purifying catalyst having further excellent exhaust gas purifying performance.
- Length and the upstream coating region and the downstream coating region overlap it is preferably 20% or less than 5% of the L w. Thereby, an even higher level of exhaust gas purification performance can be realized. It is also possible to suppress an excessive increase in pressure loss.
- the exhaust gas purifying catalyst disclosed herein in the thickness direction perpendicular to the stretching direction, the overall thickness of the partition wall when the T w, the downstream coat area not more than 30% of said T w It is formed in the partition wall in the thickness T D equivalent to.
- a catalyst metal can be utilized more effectively.
- the exhaust gas purifying catalyst disclosed herein in the thickness direction perpendicular to the stretching direction, the overall thickness of the partition wall when the T w, the upstream coating region at least 70% of said T w It is formed inside the partition wall in the corresponding thickness T U in.
- FIG. 1 is a perspective view schematically showing a base material of an exhaust gas purifying catalyst according to an embodiment of the present invention.
- FIG. 2 is a cross-sectional view schematically showing an end portion of the honeycomb substrate of FIG.
- FIG. 3 is an enlarged cross-sectional view schematically showing the configuration in the vicinity of the partition wall of the exhaust gas purifying catalyst according to one embodiment of the present invention.
- FIG. 4 is a graph comparing the exhaust gas purification performance at the time of temperature rise.
- FIG. 5 is a graph comparing the exhaust gas purification performance when the temperature is lowered.
- FIG. 6 is a graph comparing the rate of increase in pressure loss.
- FIG. 7 is an enlarged cross-sectional view schematically showing the configuration in the vicinity of the partition wall of the exhaust gas purifying catalyst according to the comparative example.
- the exhaust gas-purifying catalyst disclosed herein generally includes a base material having a wall flow structure and two coat regions (upstream coat region and downstream coat region) provided on the partition walls of the base material. ing.
- the exhaust gas-purifying catalyst disclosed herein is characterized in that, in the downstream coat region, the catalyst metal is unevenly distributed in the surface layer portion in contact with the outlet cell. Therefore, other configurations are not particularly limited.
- the exhaust gas-purifying catalyst of the present invention can be formed into a desired shape according to the intended use by appropriately selecting a base material, a carrier, a catalytic metal, and the like described later.
- FIG. 1 is a schematic diagram illustrating an example of a base material.
- the substrate shown in FIG. 1 is a honeycomb substrate (honeycomb structure) 1 having a cylindrical outer shape.
- the honeycomb substrate 1 has a plurality of cells regularly arranged along the extending direction (cylindrical cylinder axis direction) of the honeycomb substrate 1, and partition walls that partition the cells. Adjacent cells are alternately sealed with one open end in the extending direction and the other open end.
- honeycomb substrate honeycomb structure
- FIG. 2 is a schematic diagram showing a cross section of the end portion 1a of the honeycomb substrate 1.
- the end 1a is substantially circular.
- the sealing part 2 and the opening part 4 are arranged in a checkered pattern.
- a porous partition wall 6 is disposed between the sealing portion 2 and the opening 4.
- the honeycomb substrate 1 can cope with, for example, the case where the internal combustion engine is exposed to high-temperature exhaust gas (for example, 400 ° C. or higher) generated when the internal combustion engine is operated under a high load condition, or the case where the PM component is burned and removed at a high temperature.
- high-temperature exhaust gas for example, 400 ° C. or higher
- the heat resistant material include ceramics such as cordierite, aluminum titanate, silicon carbide (SiC), and alloys such as stainless steel.
- the capacity of the honeycomb substrate 1 (total volume of cells) is usually 0.1 L or more, preferably 0.5 L or more, for example, 5 L or less, preferably 3 L or less, more preferably 2 L or less.
- the total length of the honeycomb substrate 1 in the extending direction (in other words, the total length L w of the partition walls 6 in the extending direction) is usually about 10 to 500 mm, for example, about 50 to 300 mm.
- the thickness of the partition wall 6 (the length in the direction perpendicular to the stretching direction) is preferably about 0.05 to 2 mm, for example, from the viewpoint of improving exhaust gas purification performance, mechanical strength, suppressing pressure loss, and the like.
- the porosity of the partition walls 6 is usually about 40 to 70% from the viewpoint of improving mechanical strength and suppressing pressure loss.
- the average pore diameter of the partition walls 6 is usually about 10 to 40 ⁇ m from the viewpoint of improving PM collection performance and suppressing pressure loss.
- the external shape of the whole honeycomb base material 1 can also be made into an elliptical cylinder shape, a polygonal cylinder shape, etc. instead of the cylindrical shape like FIG.
- FIG. 3 is an enlarged cross-sectional view schematically showing a configuration in the vicinity of the partition wall of the exhaust gas purifying catalyst 10 according to one embodiment of the present invention.
- the direction through which exhaust gas flows is drawn by the arrow direction. That is, the left side in FIG. 3 is upstream of the exhaust gas flow path (exhaust pipe), and the right side in FIG. 3 is downstream of the exhaust gas flow path.
- the exhaust gas-purifying catalyst 10 has a so-called wall flow structure.
- the exhaust gas purifying catalyst 10 has an inlet cell 24 having an open end 24a on the exhaust gas inflow side (a U-shape), and an end portion 25a on the exhaust gas outflow side adjacent to the input cell. It has an output side cell 25 and a porous partition wall 12 partitioning both cells.
- a sealing portion 22 is disposed and sealed at an end portion 25a on the exhaust gas outflow side of the inlet cell 24 and an end portion 24a on the exhaust gas inflow side of the outlet cell 25.
- the exhaust gas purifying catalyst 10 includes two coat regions, that is, an upstream coat region 26 and a downstream coat region 28 as a place for purifying exhaust gas.
- the upstream coat region 26 is formed inside (specifically, in the pores of the partition wall 12) in contact with the entry side cell 24 of the partition wall 12. Specifically, the upstream coat region 26 is formed with a predetermined length from the end portion 24a on the exhaust gas inflow side toward the extending direction of the partition wall 12.
- the downstream coat region 28 is formed inside (specifically, in the pores of the partition wall 12) in contact with the outlet side cell 25 of the partition wall 12. Specifically, the downstream coat region 28 is formed with a predetermined length from the end portion 25a on the exhaust gas outflow side toward the extending direction of the partition wall 12.
- Each of the upstream coat region 26 and the downstream coat region 28 includes catalyst metal particles that function as an oxidation and / or reduction catalyst, and a carrier that supports the catalyst metal particles.
- the exhaust gas discharged from the internal combustion engine flows into the inlet cell 24 from the end 24a on the exhaust gas inflow side and passes through the pores of the porous partition wall 12. Then, it flows out from the end portion 25a on the exhaust gas outflow side of the adjacent exit side cell 25. While passing through the exhaust gas purification catalyst 10, harmful components in the exhaust gas come into contact with the catalyst metal (catalyst metal contained in the upstream coat region 26 and / or the downstream coat region 28) and are purified (detoxified). .
- the HC component and CO component contained in the exhaust gas are oxidized by the catalytic function of the catalytic metal and converted (purified) into water (H 2 O), carbon dioxide (CO 2 ), and the like.
- the NO x component is reduced by the catalytic function of the catalytic metal and converted (purified) into nitrogen (N 2 ). Since the PM component hardly passes through the pores of the partition walls 12, it is generally deposited on the partition walls 12 in the entry-side cell 24. The deposited PM is decomposed and removed by the catalytic function of the catalytic metal or by burning at a predetermined temperature (for example, about 500 to 700 ° C.).
- the catalytic metal various kinds of metal species that can function as an oxidation catalyst or a reduction catalyst can be considered.
- noble metals such as rhodium (Rh), palladium (Pd), and platinum (Pt), which are platinum groups, can be used.
- ruthenium (Ru), osmium (Os), iridium (Ir), silver (Ag), gold (Au), or the like may be used.
- other metal species such as alkali metals, alkaline earth metals, and transition metals may be used.
- the catalyst metal is preferably used as fine particles having a sufficiently small particle diameter from the viewpoint of increasing the contact area with the exhaust gas.
- the average particle size of the catalyst metal particles (average value of particle sizes determined by observation with a transmission electron microscope; the same applies hereinafter) is usually about 1 to 15 nm, preferably 10 nm or less, 7 nm or less, and more preferably 5 nm or less. .
- an inorganic compound conventionally used in this type of exhaust gas purifying catalyst can be considered.
- a porous carrier having a relatively large specific surface area here, the specific surface area measured by the BET method; hereinafter the same
- Preferable examples include alumina (Al 2 O 3 ), ceria (CeO 2 ), zirconia (ZrO 2 ), silica (SiO 2 ), titania (TiO 2 ), and solid solutions thereof (for example, ceria-zirconia composite oxide ( CZ composite oxide)), or a combination thereof.
- Carrier particles may in view of heat resistance and structural stability, a specific surface area of 10 ⁇ 500m 2 / g, for example, is 200 ⁇ 400m 2 / g.
- the average particle size of the carrier particles is typically 1 to 500 nm, for example 10 to 200 nm.
- the types of carriers contained in the two coat regions may be the same or different.
- the metal species contained in the upstream coat region 26 and the downstream coat region 28 may be the same or different.
- a metal species having a high reduction activity for example, rhodium
- a metal species having a high oxidation activity for example, palladium and / or platinum
- the upstream coat region 26 contains at least Rh or an alloy of Rh
- the downstream coat region 28 contains at least Rh, Pd, Pt, or an alloy containing these metal species.
- the catalytic metal purification activity can be exhibited at a higher level.
- the catalyst metal loading rate of the upstream coat region 26 and the downstream coat region 28 may be the same or different.
- the catalyst metal loading ratio in the upstream coat region 26 and the downstream coat region 28 (catalyst metal content when the carrier is 100% by mass) is not particularly limited because it may vary depending on, for example, the length and thickness of the coat region. Each may be approximately 1.5% by mass or less, preferably 0.05 to 1.5% by mass, and more preferably 0.2 to 1% by mass.
- the catalyst metal is unevenly distributed in the surface layer portion in contact with the outlet cell 25 in the downstream coat region 28.
- the catalyst metal loading rate is different in the thickness direction, and the loading rate is high in the vicinity of the outlet cell 25. That is, in the downstream coat region 28, there is a concentration of the catalyst metal loading rate in the thickness direction, and the catalyst metal loading rate in the region in contact with the outlet cell 25 is relatively high.
- the exhaust gas that has once passed through the partition wall 12 rarely flows backward and passes through the partition wall 12 again. That is, most of the exhaust gas that has passed through the partition wall 12 goes straight toward the end portion 25 a of the exit side cell 25. For this reason, by making catalyst metal unevenly distributed in the area
- a region relatively close to the entry cell 24 may or may not contain a catalyst metal. May be.
- the downstream coat region 25 is roughly divided into two regions in the thickness direction. For example, in the embodiment shown in FIG. 3, the downstream coat region 25 is relatively close to the exit cell 25 (contacts the exit cell 25) and the second downstream coat region 282 is relatively close to the entrance cell 24 ( And a first downstream coat region 281 far from the exit cell 25). The first downstream coat region 281 is substantially free of the catalyst metal.
- the second downstream coat region 282 contains a catalyst metal.
- the effect of the present invention can be exhibited at a higher level.
- a catalytic metal in an amount equivalent to that of the conventional product is intensively supported on the second downstream coat region 282
- relatively high purification performance can be exhibited.
- the catalyst metal loading rate in the second downstream coat region 282 is equal to that of the conventional product, the amount of catalyst metal used can be relatively reduced while maintaining the purification performance. This is preferable from the viewpoint of low cost and energy saving.
- the upstream coating region 26 has a relatively low loading rate
- the second The downstream coating region 282 has a relatively high loading rate. That is, in the upstream coat region 26, the catalyst metal is disposed in a wide range (with a low density) with a relatively low catalyst metal loading rate, and in the second downstream coat region 282, with a relatively high catalyst metal loading rate (with a high density) It is preferable to arrange a catalytic metal in Thereby, the pressure loss can be effectively reduced while maintaining the exhaust gas purification performance at a high level.
- the catalyst metal loading rate is preferably substantially uniform.
- the upstream coat region 26 is formed in a region in contact with the entry cell 24 inside the partition wall 12 with a predetermined length from the end 24a on the exhaust gas inflow side in the extending direction.
- the exhaust gas that has flowed into the entry side cell 24 passes through the partition wall 12.
- the upstream coat region 26 inside the partition wall 12 the exhaust gas purification performance when passing through the partition wall 12 can be effectively enhanced.
- such a configuration is particularly effective in reducing the pressure loss at the time of exhaust gas inflow.
- the length (average length) L U in the stretching direction of the upstream coat region 26 is not particularly limited, but is usually preferably shorter than the total length L w of the partition wall 12.
- 30% or more of the L w typically at least 50%, e.g., 60% or more, preferably a 70% or more, generally 99% or less, typically 95% or less, for example 90% or less, Speaking daringly, it should be 80% or less.
- the length L U of the upstream coat region 26 is approximately 70% of the L w .
- ash (ASH) made of incombustible components tends to be easily deposited in the vicinity of the sealing portion 22 of the entry side cell 24. Therefore, depending on the components of the exhaust gas, the pressure loss may increase at the portion where the ash is deposited, and the exhaust gas may not flow easily.
- L U equal to or less than a predetermined value (that is, by arranging the upstream coat region 26 in the vicinity of the vicinity of the sealing portion 22), an increase in pressure loss can be suitably suppressed.
- the L U equal to or higher than a predetermined value, it is possible to further suitably exhibit the exhaust gas purification performance.
- Thickness (average thickness) T U of the upstream coating region 26 are not particularly limited for obtaining depend upon a variety of factors, including the overall thickness T w and the stretching direction of the length L U of the partition wall 12.
- the Tw is generally 30% or more, typically 40% or more, such as 50% or more, preferably 60% or more, more preferably 70% or more, and more specifically 80% or more. It can also be formed in substantially the entire thickness direction (98% or more) of the partition wall 12.
- T 1 is less than 100% of said T w, for example, 90% or less.
- the thickness T U of the upstream coating region 26 is 80% approximately of the T w.
- Downstream coating region 28 the region in contact with the outlet side cells 25 of the partition wall 12, and is formed with a short length L D than the total length L w of the partition wall 12 toward the extending direction from the end portion 25a of the exhaust gas outlet side.
- the length of the first downstream coat region 281 is long. It is L 1, the above L w of approximately 10% or more, typically at least 15%, such as 20% or more, preferably a 30% or more, typically 50% or less, e.g., 40% or less Good.
- the length L 2 of the second downstream coating region 282 may be the same as the L 1, may be different.
- L 1 and L 2 are different, for example, the longer one can be regarded as the above L D.
- L 1 is approximately 35% of the L w
- L 2 is approximately 33% of the L w
- L 1 is slightly larger. Therefore, it can be regarded as L 1 ⁇ L D.
- Thickness (average thickness) T D of the downstream coating region 28 is not particularly limited for obtaining depend upon a variety of factors, including the length L D of the total thickness T w and the stretching direction, for example the partition wall 12. Normally, so as not to contact the inlet side cell 24, less than 100% of the T w, approximately 50% or less, typically 40% or less, for example, may is 30% or less. In the embodiment shown in FIG. 3, the thickness T D of the downstream coating region 28 is approximately 30% of the T w.
- the thickness of the first downstream coat region 281 T 1 is approximately 50% of the T w or less, typically 40% or less, for example, may is 30% or less.
- the thickness T 2 of the second downstream coating region 282 is approximately 40% of the T w or less, typically below 30%, for example if is 20% or less.
- the thickness T 1 of the first downstream-coated region 281 is approximately 20% of the T w
- the thickness T 2 of the second downstream coating region 282 is 10% approximately of the T w.
- the T 2 and less than T 1 by concentrating the catalytic metal in the vicinity of the surface of the exit-side cell 25 (surface layer portion of the thickness direction), the purification performance of the catalyst metal is exhibited Ikan'naku.
- approximately 20% of the T 1 is the T w
- T 2 is 10% approximately of the T w
- the T D can be regarded as approximately 30% of the T w.
- the total length L w of the partition wall 12, the length L U of the upstream coat region 26, and the length L D of the downstream coat region 28 are expressed by the following formula: L w ⁇ (L U + L D ) ⁇ 2L w ;
- L w ⁇ (L U + L D ) ⁇ 2L w the length L of the upstream coat region 26 is determined. It is more preferable that U and the length L 2 of the second downstream coat region 282 satisfy the following formula: L w ⁇ (L U + L 2 ) ⁇ 2L w ;
- the length in which the upstream coat region 26 and the downstream coat region 28 (or the second downstream coat region 282) overlap in the extending direction can be different depending on the thickness of each coat region, for example, and is not particularly limited.
- the Lw is approximately 2% or more, typically 3% or more, and approximately 20% or less, typically 15% or less, for example, 12% or less.
- the length L U of the upstream coating region 26 to 70% approximately of the L w, a length L D of the downstream coating region 28 by 35% approximately of the L w, stretching direction Has an overlap of about 5%.
- the thickness T U of the upstream coat region 26 And the thickness T 2 of the second downstream coat region 282 preferably satisfy the following formula: (T U + T 2 ) ⁇ T w ;
- the upstream coating region 26 and the second downstream coating region 282 are spaced apart from each other so as not to contact in the thickness direction. That is, in the thickness direction, a region made of only the base material is interposed between the upstream coating region 26 and the second downstream coating region 282.
- the “gap” in the thickness direction between the upstream coating region 26 and the downstream coating region 28 (or the second downstream coating region 282) is, for example, 2% or more, typically 5% or more of the T w , It is generally good to be 20% or less, typically 15% or less.
- the exhaust gas-purifying catalyst 10 of the aspect shown in FIG. 3 may be formed as follows. First, a honeycomb substrate 1 as shown in FIGS. 1 and 2 is prepared, and an upstream coat region 26 is formed inside the partition walls of the honeycomb substrate 1. Specifically, a slurry for forming an upstream coat region containing a desired catalyst metal component (typically a solution containing a catalyst metal as ions) and a desired carrier powder is prepared.
- a desired catalyst metal component typically a solution containing a catalyst metal as ions
- a desired carrier powder is prepared.
- the properties (viscosity, solid content, etc.) of the slurry may be adjusted in consideration of the size of the honeycomb substrate 1 to be used, the porosity of the partition walls 12, and the like.
- This slurry is supplied into the inlet cell 24 from the end 24a of the honeycomb substrate 1 on the exhaust gas inflow side, and an upstream coat region 26 having a desired property is formed in the pores of the partition wall 12 by an internal coating method.
- the properties (for example, the thickness and the catalyst metal loading rate) of the upstream coat region 26 can be adjusted by, for example, the properties and supply amount of the slurry.
- the outlet cell 25 may be pressurized at the time of supplying the slurry to cause a pressure difference between the inlet cell 24 and the outlet cell 25 so that the slurry does not permeate the partition wall 12 excessively.
- the downstream coat region 28 is formed inside the partition walls of the honeycomb substrate 1.
- a first slurry containing a desired carrier powder is prepared. This slurry is supplied into the outlet cell 25 from the end 25a on the exhaust gas outflow side of the honeycomb substrate 1, and a carrier coat region having a desired property is formed in the pores of the partition wall 12.
- the property (for example, thickness) of the carrier coat region can be adjusted by, for example, the property of slurry and the supply amount.
- a second slurry containing a desired catalyst metal component typically a solution containing the catalyst metal as ions
- This slurry is immersed from the end 25a side of the honeycomb substrate 1 on the exhaust gas outflow side, and the catalyst metal is supported on a part of the carrier coat region by the impregnation supporting method.
- the arrangement and properties of the second downstream coat region 282 (for example, the thickness and the catalyst metal loading rate) can be adjusted by, for example, the catalyst metal concentration and viscosity of the slurry, the impregnation loading conditions, and the like. According to such a method, the catalyst metal can be unevenly distributed on the surface layer portion (portion in contact with the outlet cell 25) of the downstream coat region 28. Thereby, the second downstream coat region 282 can be formed. In this method, a region obtained by subtracting the second downstream coating region 282 from the carrier coating region becomes the first downstream coating region 281.
- the honeycomb substrate 1 after applying the slurry is dried and fired at a predetermined temperature and time. Thereby, the exhaust gas-purifying catalyst 10 as shown in FIG. 3 can be manufactured.
- the slurry can contain arbitrary additive components such as a conventionally known oxygen storage / release material, binder, and additive in addition to the catalyst metal and the carrier.
- oxygen storage / release material include CZ composite oxide as a carrier or a non-supported material.
- binder include alumina sol and silica sol.
- the exhaust gas purification catalyst disclosed herein can exhibit excellent exhaust gas purification performance while suppressing an increase in pressure loss. Therefore, it can arrange
- the application of the present invention is particularly effective in an eco-car equipped with an energy saving mechanism such as a hybrid engine or an idling stop.
- the number of cells is 300 cpsi (cells per square inch)
- the volume refers to the entire bulk volume including the volume of the cell passage
- the total length is 105 mm
- the outer diameter is 103 mm
- the partition wall thickness is 0.3 mm.
- an upstream coat region was formed. Specifically, 40 g of Al 2 O 3 powder ( ⁇ -Al 2 O 3 , average particle size 1 ⁇ m) as a carrier, an appropriate amount of rhodium aqueous solution having an Rh content of 0.5 g, and an appropriate amount of pure water Mixed. After stirring and mixing the obtained liquid mixture, it dried and baked (500 degreeC, 1 hour), and Rh carrying
- the slurry is supplied into the inlet cell from the end of the honeycomb substrate on the exhaust gas inflow side so that the Rh loading after firing is 0.275 g per 100% by mass of the carrier, and the partition wall in contact with the inlet cell is supplied.
- An upstream coat region (length L U in the stretching direction: 70% of the total length of the partition walls, thickness T U : 80% of the total thickness of the partition walls) was formed in the pores.
- a downstream coat region was formed. Specifically, 40 g of Al 2 O 3 powder ( ⁇ -Al 2 O 3 , average particle size 1 ⁇ m) was first mixed with an appropriate amount of pure water to prepare a carrier slurry. This slurry is supplied into the outlet cell from the end of the honeycomb substrate on the exhaust gas outflow side, and in the pores of the partition contacting the outlet cell, the coating region (length L D in the stretching direction: 35% of the total length of the partition walls and thickness T D : 30% of the total thickness of the partition walls).
- Exhaust gas purifying catalysts according to a comparative example as shown in FIG. 7 were prepared in the same manner as in Example 1 except that the catalyst metal was supported over the entire downstream coat region.
- the reference numerals in FIG. 7 are the same as those in FIG. That is, first, an upstream coat region (length L U in the stretching direction: 70% of the total length of the partition walls, thickness T U : 80% of the total thickness of the partition walls) was formed in the same manner as in the above example. Next, a downstream coat region was formed.
- the purification performance of the obtained exhaust gas purification catalysts was compared. Specifically, first, the purification performance at the time of temperature increase was compared. That is, an exhaust gas purifying catalyst is installed in a rig apparatus, and the gas temperature of the catalyst is changed from 150 ° C. to a temperature rising rate of 50 ° C./min. The simulated exhaust gas was allowed to flow in while raising the NO, and the NOx concentration, HC (here propylene) concentration, and CO concentration on the outlet side of the catalyst were measured. And the temperature (50% purification rate attainment temperature) when the gas concentration on the outlet side reached 50 mol% with respect to the concentration of the inflowing gas was evaluated.
- the results are shown in FIG.
- the 50% purification rate reaching temperature indicates that the lower the temperature, the better the purification performance.
- the purification performance when the temperature was lowered was compared. That is, using a heat exchanger, the gas temperature of the catalyst is changed from 500 ° C. to a heating rate of 50 ° C./min.
- the simulated exhaust gas was allowed to flow in while lowering the pressure, and the NOx concentration, HC (here propylene) concentration, and CO concentration on the outlet side of the catalyst were measured. And the temperature which can hold
- the results are shown in FIG. The lower the temperature, the better the purification performance.
- the example showed better pressure loss performance than the comparative example. That is, according to the technology disclosed herein, it has been found that the exhaust gas purification performance can be improved while suppressing an increase in pressure loss. This result shows the technical significance of the present invention.
- the downstream coat region 28 is composed of two layers, that is, a first downstream coat region 281 that does not contain a catalyst metal and a second downstream coat region 282 that contains a catalyst metal.
- the downstream coat region 28 may be formed in a gradation in which the catalyst metal loading is gradually changed so that the catalyst metal increases as the surface layer portion is approached.
- the downstream coat region 28 may be composed of three or more layers having different catalyst metal loadings in stages.
- the downstream coating region 28 is formed inside the partition wall 12. However, it is not limited to this.
- the downstream coat region 28 can be formed on the surface of the partition wall 12 or can be formed continuously over the surface and the inside of the partition wall 12.
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Abstract
Description
なお、本国際出願は2014年10月16日に出願された日本国特許出願2014-211381号に基づく優先権を主張しており、その出願の全内容は本明細書中に参照として組み入れられている。
これに関連する従来技術文献として、特許文献1,2が挙げられる。例えば特許文献1には、2層構造の触媒層を備えた排ガス浄化用触媒が開示されている。具体的には、隔壁の内部全体にPdを含む第1の触媒層を備え、且つ上記第1の触媒層を完全に覆うように入側セルと接する側の隔壁の表面にRhを含む第2の触媒層を備えた排ガス浄化用触媒が開示されている。
本発明はかかる事情を鑑みてなされたものであり、その目的は、圧損の上昇を抑制しつつ、排ガス浄化性能に優れた排ガス浄化用触媒を提供することにある。
本発明に係る排ガス浄化用触媒は、自動車エンジンなどの内燃機関の排気管に配置されて該内燃機関から排出される排ガスの浄化を行うウォールフロー型の排ガス浄化用触媒である。かかる排ガス浄化用触媒は、ウォールフロー構造の基材と上流コート領域と下流コート領域とを備えている。上記ウォールフロー構造の基材は、排ガス流入側の端部が開口した入側セルと、排ガス流出側の端部が開口した出側セルと、上記入側セルと上記出側セルとを仕切る多孔質な隔壁と、を備えている。上記上流コート領域は、上記入側セルに接する上記隔壁の内部において上記排ガス流入側の端部から上記隔壁の延伸方向に沿って形成され、触媒金属と該触媒金属粒子を担持する担体とを含んでいる。上記下流コート領域は、上記出側セルに接する上記隔壁において上記排ガス流出側の端部から上記延伸方向に沿って上記隔壁の全長Lwよりも短い長さで形成され、触媒金属と該触媒金属粒子を担持する担体とを含んでいる。そして、上記下流コート領域では、上記触媒金属が上記出側セルに当接する表層部分に偏在している。
したがって、上記構成によれば、圧損の上昇を抑制しつつ排ガス浄化性能を向上することができる。
上記上流コート領域と上記下流コート領域とが重なり合う長さは、上記Lwの5%以上20%以下であることが好ましい。これにより、更に高いレベルの排ガス浄化性能を実現することができる。また、圧損が過度に増大することを抑制することもできる。
図3は、本発明の一実施形態に係る排ガス浄化用触媒10の隔壁近傍の構成を模式的に示す拡大断面図である。なお、この図では、排ガスが流れる向きを矢印方向で描いている。すなわち、図3の向かって左側が排ガス流路(排気管)の上流であり、図3の向かって右側が排ガス流路の下流である。排ガス浄化用触媒10は、いわゆるウォールフロー構造である。排ガス浄化用触媒10は、排ガス流入側の端部24aが開口した(コの字状の)入側セル24と、該入側セルに隣接し排ガス流出側の端部25aが開口した(コの字状の)出側セル25と、両セルを仕切る多孔質な隔壁12とを備えている。入側セル24の排ガス流出側の端部25aと、出側セル25の排ガス流入側の端部24aとには封止部22が配置され、目封じされている。
好適な一態様では、厚み方向において下流コート領域25が大まかに2つの領域に区分されている。例えば図3に示す態様では、下流コート領域25が、相対的に出側セル25に近い(出側セル25に当接する)第2下流コート領域282と、相対的に入側セル24に近い(出側セル25から遠い)第1下流コート領域281とで構成されている。第1下流コート領域281は、実質的に上記触媒金属を含まない。第2下流コート領域282は、触媒金属を含んでいる。出側セル25と接する第2下流コート領域282に触媒金属を集中的に(高い担持率で)配置することにより、本発明の効果をより高いレベルで発揮することができる。例えば、従来品と同等の量の触媒金属を第2下流コート領域282に集中的に担持する場合には、相対的に高い浄化性能を発揮することができる。或いは、第2下流コート領域282における触媒金属担持率を従来品と同等とする場合には、浄化性能を維持したままで相対的に触媒金属の使用量を低減することができる。このことは、低コストや省エネの観点から好ましい。
上流コート領域26の厚み方向において、触媒金属担持率は概ね均質であるとよい。
下流コート領域28が、触媒金属を含まない領域(第1下流コート領域281)と、触媒金属を含む領域(第2下流コート領域282)とから構成される場合、上流コート領域26の長さLUと第2下流コート領域282の長さL2とは、次式:Lw<(LU+L2)<2Lw;を満たすことがなお好ましい。
例えば図3に示す態様の排ガス浄化用触媒10は、以下のように形成するとよい。
先ず、図1,2に示すようなハニカム基材1を用意し、ハニカム基材1の隔壁内部に上流コート領域26を形成する。具体的には、所望の触媒金属成分(典型的には触媒金属をイオンとして含む溶液)と、所望の担体粉末とを含む上流コート領域形成用スラリーを調製する。スラリーの性状(粘度や固形分率など)は、使用するハニカム基材1のサイズや隔壁12の気孔率などを考慮して調整するとよい。このスラリーをハニカム基材1の排ガス流入側の端部24aから入側セル24内に供給し、内部コート法によって隔壁12の細孔内に所望の性状の上流コート領域26を形成する。上流コート領域26の性状(例えば厚みや触媒金属担持率)は、例えばスラリーの性状や供給量などによって調整することができる。或いは、上記スラリーの供給時に出側セル25を加圧して、入側セル24と出側セル25に圧力差を生じさせ、上記スラリーが隔壁12内に浸透しすぎないよう調整するのもよい。
具体的には、所望の担体粉末を含む第1のスラリーを調製する。このスラリーをハニカム基材1の排ガス流出側の端部25aから出側セル25内に供給し、隔壁12の細孔内に所望の性状の担体コート領域を形成する。担体コート領域の性状(例えば厚み)は、例えばスラリーの性状や供給量などによって調整することができる。
次に、所望の触媒金属成分(典型的には触媒金属をイオンとして含む溶液)を含む第2のスラリーを調製する。このスラリーをハニカム基材1の排ガス流出側の端部25a側から浸漬させ、含浸担持法によって担体コート領域の一部に触媒金属を担持する。第2下流コート領域282の配置や性状(例えば厚みや触媒金属担持率)は、例えばスラリーの触媒金属濃度や粘度、含浸担持の条件などで調整することができる。かかる手法によれば、下流コート領域28の表層部分(出側セル25に当接する部分)に触媒金属を偏在させることができる。これにより、第2下流コート領域282を形成することができる。
なお、かかる手法では、上記担体コート領域から第2下流コート領域282を差し引いた領域が、第1下流コート領域281となる。
基材として、セル数300cpsi(cells per square inch)、容積(セル通路の容積も含めた全体の嵩容積をいう)0.9L、全長105mm、外径103mm、隔壁の厚み0.3mmであり、平均細孔径15μm、気孔率が59%のコーディエライト製のハニカム基材を準備した。
具体的には、担体であるAl2O3粉末(γ-Al2O3、平均粒径1μm)40gと、Rh含有量が0.5gである適量のロジウム水溶液と、適量の純水とを混合した。得られた混合液を撹拌混合した後、乾燥、焼成(500℃、1時間)することにより、Rh担持粉末を得た。かかるRh担持粉末と、焼成後のCZ複合酸化物量が60gとなるセリア-ジルコニア複合酸化物溶液と、適量の純水とを混合し、上流コート領域形成用スラリーを調製した。このスラリーを、焼成後のRh担持率が担体100質量%当たり0.275gとなるようにハニカム基材の排ガス流入側の端部から入側セル内に供給し、該入側セルと接する隔壁の細孔内に上流コート領域(延伸方向の長さLU:隔壁の全長の70%、厚みTU:隔壁の全体厚みの80%)を形成した。
具体的には、先ず、Al2O3粉末(γ-Al2O3、平均粒径1μm)40gを適量の純水に混合し、担体スラリーを調製した。このスラリーを、ハニカム基材の排ガス流出側の端部から出側セル内に供給し、該出側セルと接する隔壁の細孔内に、担体のみのコート領域(延伸方向の長さLD:隔壁の全長の35%、厚みTD:隔壁の全体厚みの30%)を形成した。
そして、150℃で1時間乾燥した後、500℃で1時間の焼成を行うことにより、実施例に係る排ガス浄化用触媒を得た。
下流コート領域の全体に亘って触媒金属を担持させたこと以外は上記例1と同様に、図7に示すような比較例に係る排ガス浄化用触媒を作製した。なお、図7における符号は、図3と同様である。
即ち、先ず上記実施例と同様にして上流コート領域(延伸方向の長さLU:隔壁の全長の70%、厚みTU:隔壁の全体厚みの80%)を形成した。次に、下流コート領域を形成した。具体的には、担体であるAl2O3粉末(γ-Al2O3、平均粒径1μm)40gと、Pt含有量が1.2gである適量の白金水溶液と、適量の純水とを混合した。得られた混合液を撹拌混合した後、乾燥、焼成(500℃、1時間)することにより、Pt担持粉末を得た。かかるPt担持粉末を適量の純水に混合し、下流コート領域形成用スラリーを調製した。このスラリーを焼成後のPt担持率が担体100質量%当たり0.66gとなるようにハニカム基材の排ガス流出側の端部から出側セル内に供給し、該出側セルと接する隔壁の細孔内に、下流コート領域(延伸方向の長さLD:隔壁の全長の35%、厚みTD:隔壁の全体厚みの30%)を形成した。
上記得られた排ガス浄化用触媒(実施例,比較例)の浄化性能を比較した。具体的には先ず、昇温時の浄化性能を比較した。即ち、排ガス浄化用触媒をリグ装置に設置し、熱交換器を用いて触媒の入りガス温度を150℃から昇温速度50℃/min.で上昇させながら模擬排ガスを流入させ、触媒の出側におけるNOx濃度、HC(ここではプロピレン)濃度、CO濃度を測定した。そして、流入ガスの濃度に対して出側のガス濃度が50mol%に到達したときの温度(50%浄化率到達温度)を評価した。結果を図4に示す。なお、50%浄化率到達温度は低温であるほど浄化性能が優れていることを表している。
次に、降温時の浄化性能を比較した。即ち、熱交換器を用いて触媒の入りガス温度を500℃から昇温速度50℃/min.で降下させながら模擬排ガスを流入させ、触媒の出側におけるNOx濃度、HC(ここではプロピレン)濃度、CO濃度を測定した。そして、流入ガスの濃度に対して出側のガス濃度が50mol%以上を保持できる温度を評価した。結果を図5に示す。なお、この温度も低温であるほど浄化性能が優れていることを表している。
一方、図5に示すように、降温時は比較例よりも実施例のほうが高い浄化性能を示していた。この理由としては、降温時は触媒の上流側から冷却されるために、触媒の下流側の反応寄与が大きく、触媒金属を出側セルに当接する表層部分に偏在化させた効果が顕著に表れたことが考えられる。
次に、上記得られた排ガス浄化用触媒(実施例,比較例)をガソリンエンジンの排気管に装着し、圧損を比較した。具体的には、エンジンベンチの排気系に排ガス浄化用触媒をそれぞれ設置し、触媒温度750℃で50時間の耐久試験を行った。次に、耐久試験後の排ガス浄化用触媒の圧損(kPa)を測定した。また、基準として基材のみの圧損(kPa)も測定した。結果を図6に示す。なお、図6では基材のみの圧損を基準とし、これに対する圧損の上昇率を表している。
即ち、ここに開示される技術によれば、圧損の上昇を抑制しつつ排ガス浄化性能を向上することができるとわかった。かかる結果は、本発明の技術的意義を示すものである。
例えば上記実施例では、下流コート領域28が、触媒金属を含まない第1下流コート領域281と、触媒金属を含む第2下流コート領域282の2つの層で構成されていた。しかし、これには限定されない。下流コート領域28は、例えば表層部分に近づくほど触媒金属が多くなるように触媒金属担持率を漸次的に変化させたグラデーション状に構成してもよい。或いは、下流コート領域28は、触媒金属担持率が段階的に異なる3層以上で構成してもよい。また、上記実施例では、下流コート領域28が、隔壁12の内部に形成されていた。しかし、これには限定されない。下流コート領域28は、隔壁12の表面に形成することもできるし、隔壁12の表面と内部とに亘って連続的に形成することもできる。
1a 端部
2 封止部
4 開口部
6、12 隔壁
10 排ガス浄化用触媒
22 封止部
24 入側セル
24a 排ガス流入側の端部
25 出側セル
25a 排ガス流出側の端部
26 上流コート領域
28 下流コート領域
281 第1下流コート領域
282 第2下流コート領域
Claims (8)
- 内燃機関の排気管に配置されて該内燃機関から排出される排ガスの浄化を行うウォールフロー型の排ガス浄化用触媒であって、
排ガス流入側の端部が開口した入側セルと、排ガス流出側の端部が開口した出側セルとが、多孔質な隔壁によって仕切られているウォールフロー構造の基材と、
前記隔壁の内部であって前記入側セルと接する領域に、前記排ガス流入側の端部から前記隔壁の延伸方向に沿って形成されている上流コート領域と、
前記隔壁の前記出側セルと接する領域に、前記排ガス流出側の端部から前記延伸方向に沿って前記隔壁の全長Lwよりも短い長さで形成されている下流コート領域と、
を備え、
前記上流コート領域および前記下流コート領域は、それぞれ、触媒金属と該触媒金属粒子を担持する担体とを含み、
前記下流コート領域では、前記触媒金属が前記出側セルと当接する表層部分に偏在している、ウォールフロー型の排ガス浄化用触媒。 - 前記下流コート領域は、前記延伸方向と直交する厚み方向において、相対的に前記入側セルに近い第1下流コート領域と、相対的に前記出側セルに近い第2下流コート領域と、の2つの領域に区分され、
前記第1下流コート領域は実質的に前記触媒金属を含まず、
前記第2下流コート領域は前記触媒金属を含む、請求項1に記載の排ガス浄化用触媒。 - 前記下流コート領域の前記延伸方向の長さLDが、前記Lwの10%以上50%以下である、請求項1又は2に記載の排ガス浄化用触媒。
- 前記上流コート領域の前記延伸方向の長さLUが、前記Lwの60%以上90%以下である、請求項1~3のいずれか一項に記載の排ガス浄化用触媒。
- 前記延伸方向において、前記Lwと前記LUと前記LDとが、次式:Lw<(LU+LD)<2Lw;を満たし、前記上流コート領域と前記下流コート領域とが前記延伸方向に一部重なり合っている、請求項1~4のいずれか一項に記載の排ガス浄化用触媒。
- 前記上流コート領域と前記下流コート領域とが前記延伸方向に重なり合う長さは、前記Lwの5%以上20%以下である、請求項5に記載の排ガス浄化用触媒。
- 前記延伸方向と直交する厚み方向において、前記隔壁の全体厚みをTwとしたときに、前記下流コート領域が前記Twの30%以下である、請求項1~6のいずれか一項に記載の排ガス浄化用触媒。
- 前記延伸方向と直交する厚み方向において、前記隔壁の全体厚みをTwとしたときに、前記上流コート領域が前記Twの70%以上である、請求項1~7のいずれか一項に記載の排ガス浄化用触媒。
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US20170298797A1 (en) | 2017-10-19 |
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JPWO2016060050A1 (ja) | 2017-08-31 |
US10344655B2 (en) | 2019-07-09 |
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