WO2018225514A1 - エンジンの排気ガス処理装置及びその製造方法 - Google Patents

エンジンの排気ガス処理装置及びその製造方法 Download PDF

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Publication number
WO2018225514A1
WO2018225514A1 PCT/JP2018/019879 JP2018019879W WO2018225514A1 WO 2018225514 A1 WO2018225514 A1 WO 2018225514A1 JP 2018019879 W JP2018019879 W JP 2018019879W WO 2018225514 A1 WO2018225514 A1 WO 2018225514A1
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Prior art keywords
catalyst
filter
exhaust gas
supported
engine
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PCT/JP2018/019879
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English (en)
French (fr)
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栄治郎 田中
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マツダ株式会社
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Application filed by マツダ株式会社 filed Critical マツダ株式会社
Priority to US16/619,078 priority Critical patent/US10870082B2/en
Priority to EP18814241.8A priority patent/EP3617465B1/en
Priority to CN201880036612.2A priority patent/CN110709588B/zh
Publication of WO2018225514A1 publication Critical patent/WO2018225514A1/ja

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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
    • F01N3/033—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
    • 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
    • B01D53/944—Simultaneously removing carbon monoxide, hydrocarbons or carbon making use of oxidation catalysts
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D39/00—Filtering material for liquid or gaseous fluids
    • B01D39/14—Other self-supporting filtering material ; Other filtering material
    • B01D39/20—Other self-supporting filtering material ; Other filtering material of inorganic material, e.g. asbestos paper, metallic filtering material of non-woven wires
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D46/00—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D46/00—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours
    • B01D46/24—Particle separators, e.g. dust precipitators, using rigid hollow filter bodies
    • B01D46/2403—Particle separators, e.g. dust precipitators, using rigid hollow filter bodies characterised by the physical shape or structure of the filtering element
    • B01D46/2418—Honeycomb filters
    • 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
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    • B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
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    • 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
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    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/0215—Coating
    • B01J37/0228—Coating in several steps
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/0236—Drying, e.g. preparing a suspension, adding a soluble salt and drying
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/024—Multiple impregnation or coating
    • B01J37/0244—Coatings comprising several layers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J37/08—Heat treatment
    • 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
    • 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
    • F01N13/0093—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 the purifying devices are of the same type
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    • 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
    • F01N13/0097—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 the purifying devices are arranged in a single housing
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    • 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
    • F01N13/08—Other arrangements or adaptations of exhaust conduits
    • F01N13/10—Other arrangements or adaptations of exhaust conduits of exhaust manifolds
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    • F01N13/18—Construction facilitating manufacture, assembly, or disassembly
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    • 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
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    • 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
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
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    • 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
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    • 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
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    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
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    • F01N3/28—Construction of catalytic reactors
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    • F01N3/2842—Arrangements for mounting catalyst support in housing, e.g. with means for compensating thermal expansion or vibration specially adapted for monolithic supports, e.g. of honeycomb type
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    • 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
    • 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 engine exhaust gas treatment device and a method for manufacturing the same.
  • the exhaust gas discharged from the engine includes particulate matter (Particulate Matter, hereinafter referred to as “PM”). Is included.) Since this PM also causes air pollution, its emission regulations have been strengthened together with harmful gas components such as HC, CO, and NOx.
  • Patent Document 1 describes that in order to avoid an increase in the size of an exhaust gas treatment device, a catalyst is supported on a filter that collects PM, thereby collecting PM and purifying exhaust gas.
  • the filter is a honeycomb structure having open cells penetrating in the axial direction and closed cells whose upstream ends are closed, and is formed of porous ceramics.
  • the catalyst is supported on the cell wall in the downstream portion of the honeycomb structure in the exhaust gas flow direction, and the catalyst is not supported on the cell wall in the upstream portion of the honeycomb structure.
  • the exhaust gas flows from the open cell to the closed cell through the pores of the cell wall, whereby PM is collected in the pores, and the downstream side of the honeycomb structure.
  • the purification of the exhaust gas is promoted by the catalyst supported on the cell wall in the portion.
  • Patent Document 1 a catalyst is not supported on the cell wall on the upstream side of the honeycomb structure in order to avoid an increase in ventilation resistance. Therefore, the exhaust gas cannot be purified by the catalyst on the upstream side. If the amount of catalyst supported on the downstream side of the honeycomb structure is increased in order to improve the exhaust gas purification performance, the pores in the cell walls on the downstream side are blocked by the catalyst. Scavenging performance decreases.
  • an object of the present invention is to improve the exhaust gas purification performance while suppressing a decrease in scavenging performance of the engine.
  • the catalyst is supported on the surface of the porous filter that collects PM in the exhaust gas and is supported on the inner surface of the pore of the filter.
  • the engine exhaust gas treatment device disclosed herein is provided with a porous filter for collecting PM in the exhaust gas in the exhaust gas passage of the engine, An exhaust gas treatment device in which the exhaust gas is discharged from the surface of the filter through the pores of the filter, A catalyst for exhaust gas purification is supported on the filter surface and the inner surface of the pores, The catalyst is supported on the filter surface thicker than the inner surface of the pore.
  • this exhaust gas treatment device by carrying the catalyst thickly on the filter surface, the catalyst carrying thickness on the inner surface of the pore is reduced, so that the pore permeability is avoided by avoiding clogging of the pore by the catalyst. Easy to do. That is, it is avoided that the exhaust pressure loss due to the filter increases due to the catalyst being carried on the filter, in other words, that the scavenging efficiency in the exhaust stroke of the engine decreases.
  • the catalyst is thickly supported on the filter surface, exhaust gas purification is easy to proceed. Then, the exhaust gas whose temperature is increased by the heat of catalytic reaction on the filter surface passes through the pores. Therefore, although the catalyst is thinly supported on the inner surface of the pore, the exhaust gas purification through the catalyst efficiently proceeds due to the high exhaust gas temperature passing through the pore.
  • the supported amount of the catalyst per unit area of the filter surface is 50 times or more and 500 times or less of the supported amount of the catalyst per unit area of the pore inner surface. This is further advantageous in improving exhaust gas purification performance while suppressing a decrease in scavenging performance of the engine.
  • a catalytic converter for purifying the exhaust gas is provided upstream of the filter in the exhaust gas passage.
  • the exhaust gas is also purified by the upstream catalytic converter, the amount of catalyst supported by the filter can be reduced, which is advantageous for suppressing an increase in exhaust pressure loss. Further, since the exhaust gas is purified by the upstream catalytic converter and the catalyst of the filter, the capacity of the catalytic converter can be kept low. That is, according to the embodiment, it is easy to ensure the desired exhaust gas purification performance while suppressing the increase in size and the increase in exhaust resistance as the entire exhaust gas processing apparatus.
  • the catalytic converter includes a catalyst that is active in an oxidation reaction of an unsaturated hydrocarbon having 6 to 9 carbon atoms (hereinafter referred to as “unsaturated high HC”),
  • the catalyst of the filter is active in the oxidation reaction of saturated hydrocarbons having 5 or less carbon atoms (hereinafter referred to as “saturated low HC”).
  • the unsaturated high HC in the exhaust gas is oxidized and purified by the catalyst of the upstream catalytic converter, and the exhaust gas temperature is raised by the catalytic reaction heat. Along with this, the temperature of the downstream filter rises. Therefore, although the saturated low HC in the exhaust gas is relatively incombustible, the temperature of the filter rises as described above, so that the catalyst supported on the filter is likely to work efficiently for the purification of the saturated low HC. Therefore, even when the exhaust gas temperature is relatively low, the unsaturated high HC and saturated low HC are efficiently purified.
  • the saturation low HC is generated by the cracking of the unsaturated high HC by the catalyst of the catalytic converter, and the saturation low HC flows to the filter on the downstream side of the catalytic converter. Since the catalyst supported on the filter is active in the purification of unsaturated low HC, the saturated low HC generated by the cracking is also efficiently purified by the catalyst of the filter.
  • the manufacturing method of the exhaust gas treatment device for an engine disclosed herein is A first step of immersing a porous filter having pores through which exhaust gas of an engine passes in a first catalyst slurry in which a catalyst for purifying exhaust gas is dispersed, and supporting the catalyst on the inner surface of the pores of the filter; The filter after the first step is immersed in a second catalyst slurry in which the catalyst is dispersed, and the catalyst is supported on the surface of the filter to be thicker than the thickness of the catalyst supported on the inner surface of the pore. A second step; And a third step of providing the filter having undergone the second step in an exhaust gas passage of the engine.
  • the catalyst is supported on the inner surface of the pore of the filter and the catalyst is supported on the surface of the filter in separate steps, and the catalyst is supported on the inner surface of the pore of the filter first. It becomes easy to carry a thicker on the filter surface than on the inner surface of the pores.
  • the components of the catalyst of the first catalyst slurry and the catalyst of the second catalyst slurry are the same.
  • the step of drying the catalyst supported on the pore inner surface of the filter Between the second step and the third step, there is provided a step of firing the catalyst supported on the surface of the filter and the catalyst supported on the inner surface of the pore.
  • the exhaust gas purifying catalyst is supported on the surface of the filter thicker than the inner surface of the filter pores.
  • the catalyst is supported thinner on the inner surface of the filter pores.
  • the top view which shows the principal part of the apparatus.
  • the front view which shows typically the filter with a catalyst of a GPF apparatus.
  • the longitudinal cross-sectional view which shows the same filter typically.
  • the cross-sectional view which shows a part of the filter.
  • the figure which shows the manufacturing process of the filter. The graph which shows the difference in the temperature which flows in into the pore of the filter with a catalyst of an Example and each comparative example.
  • 1 is a direct injection gasoline engine of an automobile
  • 2 is an exhaust manifold of the engine 1.
  • a catalytic converter 3 is coupled to a collective portion 2 a of the exhaust manifold 2 via a connecting pipe 4, and a GPF (gasoline particulate filter) device 5 is directly connected to the downstream side of the catalytic converter 3 in the exhaust flow direction.
  • An exhaust pipe 6 extends from the GPF device 5 toward the rear of the automobile.
  • the catalytic converter 3 is a two-bed type in which two honeycomb catalysts 7 and 8 at the front and rear stages are accommodated in a catalyst container in series.
  • the front stage honeycomb catalyst 7 is formed by supporting a first catalyst on a honeycomb carrier.
  • the latter honeycomb catalyst 8 is formed by supporting a second catalyst on a honeycomb carrier.
  • a honeycomb carrier having a capacity of about 0.5 to 1.5 L is preferably used.
  • the first catalyst exhibits activity in the oxidation reaction of unsaturated high HC such as toluene at a temperature lower than that of the second catalyst.
  • the second catalyst exhibits activity in the oxidation reaction of saturated low HC such as isopentane at a temperature lower than that of the first catalyst.
  • the GPF device 5 is configured by housing the filter with catalyst 10 in a filter container.
  • the filter with catalyst 10 is formed by supporting the second catalyst on a ceramic filter body made of an inorganic porous material such as cordierite, SiC, Si 3 N 4 , sialon, and AlTiO 3 .
  • the filter with catalyst 10 has a honeycomb structure and includes a large number of cells 12 and 13 extending in parallel to each other. Inflow side cells 12 whose downstream ends are closed by plugs 14 and outflow side cells 13 whose upstream ends are closed by plugs 14 are alternately provided.
  • the cell 12 and the cell 13 are separated by a thin partition wall (exhaust gas passage wall) 15.
  • reference numeral 11 denotes an exhaust gas passage.
  • the hatched portion in FIG. 4 shows the plug 14 at the upstream end of the exhaust gas outflow passage 13.
  • the filter body has a capacity of 1.0 to 2.0 L, a cell density of 200 to 300 cpsi, a partition wall thickness of 150 to 250 ⁇ m, a partition wall porosity of 40 to 60%, and a partition wall 15 pore volume. It is preferable to employ a material of about 70 to 400 cm 3 .
  • the exhaust gas flows into the inflow side cell 12 of the filter with catalyst 10, and flows out to the adjacent outflow side cell 13 through the partition wall 15 around the cell 12 as indicated by an arrow.
  • the partition wall 15 has minute pores 16 communicating with the cells 12 and 13, and exhaust gas passes through the pores 16. PM in the exhaust gas is deposited mainly on the walls of the cells 12 and the pores 16.
  • the second catalyst 17 is supported on the surface (filter surface) of the partition wall 15 constituting the inflow side cell 12 and the inner surface of the pore 16.
  • the second catalyst 17 is supported on the surface of the partition wall 15 constituting the cell 12 thicker than the inner surface of the pore 16. It is preferable that the supported amount of the second catalyst per unit area of the surface of the partition wall 15 be 50 times or more and 500 times or less the supported amount of the second catalyst per unit area of the inner surface of the pore 16.
  • a majority of the total supported amount of the catalyst with respect to the filter body may be supported on the surface of the partition wall 15 constituting the inflow side cell 12. It is preferable that 65% or more and 85% or less of the total catalyst loading is supported on the surface of the partition wall 15 constituting the inflow side cell 12.
  • the amount of the second catalyst supported per 1 L of the filter body is preferably about 20 to 100 g / L in total including the surface of the partition wall 15 and the inner surface of the pores 16.
  • the amount of the second catalyst supported on the surface of the partition wall 15 constituting the inflow side cell 12 is, for example, 15 to 75 g per 1 L of the filter body, and the amount of the second catalyst supported on the inner surface of the pore 16 is, for example, a fine unit.
  • the amount may be 0.08 to 0.37 g per pore volume.
  • Second catalyst and second catalyst> As the first catalytic purification activity of unsaturated high HC is high, and containing Pd supported content of La 2 O 3 alumina made by supporting Pd on activated alumina containing La 2 O 3 4% by weight as essential components, further An OSC material (oxygen storage / release material) such as a CeZr-based composite oxide and an Rh catalyst obtained by supporting Rh on the OSC material are preferable.
  • the low HC purifying activity is higher second catalyst contains a Pt-supported content of La 2 O 3 alumina made by carrying Pt on activated alumina containing La 2 O 3 4% by weight as essential components, further, What contains the said OSC material is preferable.
  • the pre-honeycomb catalyst 7 of the catalytic converter 3 contains the first catalyst excellent in the purification of unsaturated high HC, so the unsaturated high HC in the exhaust gas is oxidized and purified by the first catalyst.
  • the exhaust gas temperature increases due to the heat of catalytic reaction that is sometimes generated.
  • the temperature of the latter-stage honeycomb catalyst 8 containing the second catalyst excellent in purification of saturated low HC rises. Therefore, the saturated low HC in the exhaust gas is efficiently purified by the second catalyst of the rear-stage honeycomb catalyst 8.
  • the exhaust gas rises in temperature due to the catalytic reaction heat accompanying the purification of HC in the honeycomb catalysts 7 and 8 and flows to the filter 10 with the catalyst on the downstream side. Therefore, purification of saturated low HC by the second catalyst of the filter with catalyst 10 proceeds efficiently.
  • saturated low HC is generated by cracking of unsaturated high HC by the upstream honeycomb catalyst 7 of the catalytic converter 3, and the saturated low HC flows to the downstream honeycomb catalyst 8 and the filter with catalyst 10. Since the second catalyst of the rear honeycomb catalyst 8 and the filter with catalyst 10 is excellent in the purification of unsaturated low HC, the saturated low HC generated by the cracking is also caused by the second catalyst of the latter honeycomb catalyst 8 and the filter with catalyst 10. It will be purified efficiently.
  • the second catalyst is supported thick on the surface of the partition wall 15 constituting the inflow side cell 12 and thin on the inner surface of the pore 16. Accordingly, since the exhaust gas purification becomes active on the surface of the partition wall 15, the exhaust gas whose temperature rises accordingly passes through the pores 16. Therefore, although the second catalyst is thinly supported on the inner surface of the pore 16, the exhaust gas purification through the second catalyst efficiently proceeds due to the high exhaust gas temperature passing through the pore 16.
  • ⁇ Manufacturing method of exhaust gas treatment device> Catalyst loading on the inner surface of the pores of the filter (first step)- As shown in FIG. 7, one end of the filter main body (catalyst unsupported) 21 is dipped in the catalyst slurry 23 related to the second catalyst stored in the first container 22 and pulled up.
  • This filter main body 21 is provided with the inflow side cells 12 and the outflow side cells 13 described above alternately.
  • the upstream end side of the filter main body 21 is immersed in the catalyst slurry 23 and pulled up. As a result, the catalyst slurry 23 adheres to the inner surface of the filter body 21 on the upstream end side of the inflow side cell 12.
  • a vacuum pump 24 is connected to the downstream end of the filter body 21, and the pump 24 is operated to make the outflow side 13 of the filter body 21 negative pressure. Due to the negative pressure in the outflow side cell 13, the catalyst slurry 23 attached to the upstream end side of the inflow side cell 12 is attracted to the downstream side of the cell 12 and soaks into the pores 16 of the partition wall 15. Go. As a result, the catalyst is supported on the inner surface of the pore 16 of the filter 21.
  • the catalyst slurry 23 stored in the first container 22 is adjusted to a viscosity that is easy to penetrate into the pores 16 of the partition walls 15.
  • the catalyst adhering to the inner surface of the pore 16 of the partition wall 15 is dried. This drying is performed, for example, by holding the filter body 21 at a temperature of 150 ° C. for 2 hours.
  • a vacuum pump 24 is connected to the downstream end of the filter body 21, and the pump 24 is operated to make the outflow side cell 13 of the filter body 21 have a negative pressure.
  • the outflow side cell 13 becomes negative pressure
  • the catalyst slurry 23 attached to the upstream end side of the inflow side cell 12 is drawn to the downstream side of the cell 12.
  • the catalyst is supported on the inner surface of the inflow side cell 12 of the filter 21, that is, on the surface of the partition wall 15.
  • the catalyst slurry 26 stored in the second container 25 is less than the catalyst slurry 23 in the first container 22 so as to be prevented from entering the pores 16 of the partition wall 15 during suction by the vacuum pump 24. Increase viscosity.
  • the catalyst slurry 26 when the catalyst slurry 26 is supported on the surface of the partition wall 15, some of the pores 16 are blocked. However, the catalyst slurry 26 supported on the surface of the partition wall 15 becomes a porous catalyst layer by subsequent firing. Therefore, the exhaust gas can pass through the catalyst layer and flow into the pores 16.
  • the catalyst adhering to the surface of the partition wall 15 of the filter main body 21 and the catalyst adhering to the inner surface of the pores 16 are baked. This firing is performed, for example, by holding the filter body 21 at a temperature of 500 ° C. for 2 hours. If necessary, a drying step (the filter main body 21 is maintained at a temperature of 150 ° C. for 2 hours) is added before the baking.
  • the catalyst-equipped filter 10 in which the second catalyst is supported on the surface of the partition wall 15 and the inner surface of the pore 16 in the inflow side cell 12 of the filter body 21 is obtained.
  • a cordierite filter having a capacity of 1.3 L was prepared as the filter body 21.
  • the cell density is 250 cpsi
  • the partition wall thickness is 200 ⁇ m
  • the partition wall porosity is 50%
  • the partition wall pore volume is about 100 cm 3 .
  • the second catalyst is 15 g / L (supported amount in the first step) on the pore inner surface of the filter body 21, and the second catalyst is 45 g / L (above) on the partition wall surface constituting the inflow side cell 12. (Supported amount in the second step) A filter with catalyst was obtained by supporting.
  • the total area of the partition walls constituting the inflow side cell 12 of the filter body 21 is 1.82 m 2 , and the total area of the pore inner surfaces of the filter body 21 calculated from the concept of hydraulic diameter is 258.009 m 2 .
  • catalyst loading per unit area of the catalyst loading is 24.73g / m 2
  • pore inner surface per unit area of the partition wall surface constituting the inlet cells 12 (filter surface) in 0.058 g / m 2 is there. Therefore, the catalyst carrying amount per unit area of the partition wall constituting the inflow side cell 12 is about 426 times the catalyst carrying amount per unit area of the pore inner surface.
  • a filter with catalyst was obtained by supporting 60 g / L of the second catalyst on the inner surface of the pores of the filter main body 21.
  • the amount of catalyst supported on the partition walls constituting the inflow side cell 12 was set to zero.
  • the amount of catalyst supported per unit area on the inner surface of the pore is 0.23 g / m 2 .
  • the total amount of CH 4 (0.06 mol) flowing into the filter was determined from the CH 4 concentration, the gas flow rate of 10 g / second, and the gas flow time of 60 seconds.
  • the embodiment filter it is assumed that 75% of the total amount of CH 4 is purified by the second catalyst supported on the partition wall surface of the inflow side cell 12, and the rising temperature of the gas at that time is set to the heat capacity of the filter 736 J / kg ⁇ It was determined from the following heat of combustion of K and weight 0.45kg and CH 4.
  • the CH 4 purification rate in the inflow side cell is zero. The results are shown in Table 1 and FIG.
  • the catalyst loading in each of the examples and comparative examples is also 60 g / L.
  • the entire amount of the catalyst is supported on the inner surface of the pores, whereas in the example, 3/4 of the total amount of the catalyst is supported on the partition walls constituting the inflow side cell 12 to the inner surface of the pores.
  • the amount of catalyst supported is 15 g / L. Therefore, in the example filter, the porosity of the partition wall is about 5.4% larger than that in the comparative example filter.
  • the exhaust pressure loss is about 93% compared to the comparative example. From this, it can be seen that when a part of the catalyst is carried on the partition wall constituting the inflow side cell as in the embodiment, the exhaust pressure loss is reduced, which is advantageous for improving the scavenging performance of the engine and hence improving the fuel consumption.

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Abstract

エンジンの排気ガス通路に排気ガス中のＰＭを捕集するハニカム状の多孔質フィルタが設けられている。排気ガスは、フィルタの流入側セル１２から該フィルタの隔壁１５の細孔１６を通過して流出側セル１３に流れる。フィルタの流入側セル１２を構成する隔壁１５の表面及び細孔１６の内面に触媒１７が担持されている。触媒１７は、細孔１６の内面よりも隔壁１５の表面に厚く担持されている。

Description

エンジンの排気ガス処理装置及びその製造方法
　本発明はエンジンの排気ガス処理装置及びその製造方法に関する。
　エンジンから排出される排気ガスには、ＨＣ（炭化水素）、ＣＯ（一酸化炭素）及びＮＯｘ（窒素酸化物）の他に、炭素を主成分とする粒子状物質（Particulate Matter、以下、「ＰＭ」という。）が含まれている。このＰＭも、大気汚染の原因となることから、ＨＣ、ＣＯ、ＮＯｘ等の有害ガス成分とともに、その排出規制が強化されてきている。
　特許文献１には、排気ガス処理装置の大型化を避けるべく、ＰＭを捕集するフィルタに触媒を担持することにより、ＰＭを捕集するとともに、排気ガスの浄化を図ることが記載されている。そのフィルタは、軸方向に貫通した開放セルと上流端が閉塞された閉塞セルとを有するハニカム構造体であり、多孔質のセラミックスによって形成されている。そのハニカム構造体の排気ガス流れ方向の下流側部分では、触媒がセル壁に担持され、ハニカム構造体の上流側部分では、触媒がセル壁に担持されていない。
　上記フィルタの場合、ハニカム構造体の上流側部分において、排気ガスが開放セルからセル壁の細孔を通って閉塞セルに流れることにより、ＰＭが細孔に捕集され、ハニカム構造体の下流側部分においてセル壁に担持された触媒により排気ガスの浄化が促進される。
特開２０１７－２０４４２号公報
　特許文献１の場合、通気抵抗の増大を避けるべく、ハニカム構造体の上流側のセル壁には触媒が担持されていない。そのため、この上流側では触媒による排気ガスの浄化が図れない。排気ガスの浄化性能を高めるべく、ハニカム構造体の下流側の触媒担持量を多くすると、下流側のセル壁の細孔が触媒によって塞がれるため、排気ガスの通気抵抗が増大し、エンジンの掃気性が低下する。
　そこで、本発明は、エンジンの掃気性の低下を抑えながら、排気ガスの浄化性能を向上させることを課題とする。
　本発明は、上記課題を解決するために、触媒を、排気ガス中のＰＭを捕集する多孔質フィルタの表面に厚く、該フィルタの細孔内面に薄く担持するようにした。
　ここに開示するエンジンの排気ガス処理装置は、エンジンの排気ガス通路に排気ガス中のＰＭを捕集する多孔質フィルタが設けられてなり、
　上記排気ガスが上記フィルタの表面から該フィルタの細孔を通過して排出される排気ガス処理装置であって、
　上記フィルタ表面及び上記細孔内面に排気ガス浄化用の触媒が担持されており、
　上記触媒は、上記細孔内面よりも上記フィルタ表面に厚く担持されていることを特徴とする。
　この排気ガス処理装置によれば、触媒をフィルタ表面に厚く担持することによって、細孔内面の触媒の担持厚さを薄くするから、触媒による細孔の閉塞を避けて細孔の通気性を確保することが容易になる。すなわち、フィルタへの触媒の担持によってフィルタによる排気圧損が大きくなること、換言すれば、エンジンの排気行程における掃気効率が低下することが避けられる。
　また、フィルタ表面では、触媒が厚く担持されているから、排気ガスの浄化が進み易い。そして、フィルタ表面での触媒反応熱によって温度が高くなった排気ガスが細孔を通過していく。よって、細孔内面には触媒が薄く担持されているものの、細孔を通る排気ガス温度が高いことによって、触媒による排気ガスの浄化が効率良く進む。
　一実施形態では、上記フィルタ表面の単位面積当たりの上記触媒の担持量は、上記細孔内面の単位面積当たりの上記触媒の担持量の５０倍以上５００倍以下である。これにより、エンジンの掃気性の低下を抑えながら、排気ガスの浄化性能を向上させる上でさらに有利になる。
　一実施形態では、上記排気ガス通路における上記フィルタよりも上流側に上記排気ガスを浄化する触媒コンバータが設けられている。
　これによれば、上流側の触媒コンバータによっても排気ガスが浄化されるから、上記フィルタの触媒担持量を少なめにすることができ、排気圧損の増大抑制に有利になる。また、上流側の触媒コンバータと上記フィルタの触媒によって排気ガスを浄化するから、触媒コンバータの容量も低く抑えることができる。すなわち、当該実施形態によれば、排気ガス処理装置全体として、大型化及び排気抵抗の増大を抑制しつつ、所期の排気ガス浄化性能を確保することが容易になる。
　一実施形態では、上記触媒コンバータは、炭素数が６～９である不飽和炭化水素（以下、「不飽和高ＨＣ」という。）の酸化反応に活性を示す触媒を備え、
　上記フィルタの上記触媒が炭素数が５以下である飽和炭化水素（以下、「飽和低ＨＣ」という。）の酸化反応に活性を示す。
　ここに、飽和炭化水素は不飽和炭化水素は比べて燃えにくい（酸化分解されにくい）ことが知られている。
　上記実施形態では、排気ガス中の不飽和高ＨＣが上流側の触媒コンバータの触媒によって酸化浄化され、その触媒反応熱によって排気ガス温度が高くなる。これに伴い、下流側のフィルタの温度が上昇する。そのため、排気ガス中の飽和低ＨＣは、比較的燃えにくいものの、フィルタの温度が上述の如く上昇するから、このフィルタに担持されている触媒が当該飽和低ＨＣの浄化に効率良く働きやすくなる。よって、排気ガス温度が比較的低い場合でも、上記不飽和高ＨＣ及び飽和低ＨＣが効率良く浄化される。
　また、触媒コンバータの触媒による不飽和高ＨＣのクラッキングによって飽和低ＨＣが生成し、該飽和低ＨＣが触媒コンバータよりも下流側のフィルタに流れる。このフィルタに担持されている触媒は不飽和低ＨＣの浄化に活性を示すから、上記クラッキングによって生成する飽和低ＨＣも当該フィルタの触媒によって効率良く浄化されることになる。
　ここに開示するエンジンの排気ガス処理装置の製造方法は、
　エンジンの排気ガスを通す細孔を有する多孔質フィルタを、排気ガス浄化用の触媒を分散させた第１触媒スラリーに浸漬し、該触媒を上記フィルタの細孔内面に担持する第１工程と、
　上記第１工程を経た上記フィルタを、上記触媒を分散させた第２触媒スラリーに浸漬し、該触媒を上記フィルタの表面に、上記細孔内面に担持された上記触媒の厚さよりも厚く担持する第２工程と、
　上記第２工程を経た上記フィルタを上記エンジンの排気ガス通路に設ける第３工程とを備えていることを特徴とする。
　この方法によれば、フィルタの細孔内面への触媒の担持とフィルタ表面への触媒の担持とを別工程で行ない、且つ先にフィルタの細孔内面に触媒を担持するようにしたから、触媒を細孔内面よりもフィルタ表面に厚く担持することが容易になる。
　一実施形態では、上記第１触媒スラリーの触媒と上記第２触媒スラリーの触媒とは、その成分が同じである。
　一実施形態では、上記第１工程と第２工程の間に、上記フィルタの細孔内面に担持した上記触媒を乾燥させる工程を備え、
　上記第２工程と上記第３工程の間に、上記フィルタの表面に担持された上記触媒及び上記細孔内面に担持された上記触媒を焼成する工程を備えている。
　フィルタの細孔内面に担持した触媒を乾燥させるから、第２工程において、フィルタの表面に触媒を担持するときに、細孔内面の触媒が流失することが避けられる。
　本発明によれば、排気ガス浄化用触媒がフィルタの細孔内面よりもフィルタの表面に厚く担持されているから、換言すれば、フィルタの細孔内面に触媒が薄く担持されているから、エンジンの掃気性の低下を抑えながら（エンジンの燃費を向上させながら）、排気ガスの浄化性能を向上させることができる。
エンジンの排気ガス処理装置を示す斜視図。 同装置の要部を示す平面図。 ＧＰＦ装置の模式的に示す図。 ＧＰＦ装置の触媒付フィルタを模式的に示す正面図。 同フィルタを模式的に示す縦断面図。 同フィルタの一部を示す横断面図。 同フィルタの製造工程を示す図。 実施例と比較例各々の触媒付フィルタの細孔に流入する温度の違いを示すグラフ図。 実施例の排気圧損の低下率を示すグラフ図。
　以下、本発明を実施するための形態を図面に基づいて説明する。以下の好ましい実施形態の説明は、本質的に例示に過ぎず、本発明、その適用物或いはその用途を制限することを意図するものではない。
　＜排気ガス処理装置＞
　図１において、１は自動車の直噴ガソリンエンジン、２はエンジン１の排気マニホールドである。排気マニホールド２の集合部２ａに触媒コンバータ３が連結管４を介して結合され、触媒コンバータ３における排気流れ方向の下流側にＧＰＦ（ガソリンパティキュレートフィルタ）装置５が直結されている。ＧＰＦ装置５から排気管６が自動車の後方へ向かって延びている。
　図２に示すように、触媒コンバータ３は、前段及び後段２つのハニカム触媒７，８を直列にして触媒容器に収容した２ベッド型である。前段のハニカム触媒７は、ハニカム担体に第１触媒を担持してなる。後段のハニカム触媒８は、ハニカム担体に第２触媒を担持してなる。ハニカム担体としては、容量０．５～１．５Ｌ程度のものを用いることが好ましい。
　第１触媒は、第２触媒よりも低い温度でトルエン等の不飽和高ＨＣの酸化反に活性を示す。一方、第２触媒は、第１触媒よりも低い温度でイソペンタン等の飽和低ＨＣの酸化反応に活性を示す。
　ＧＰＦ装置５は、触媒付フィルタ１０をフィルタ容器に収容してなる。触媒付フィルタ１０は、コージェライト、ＳｉＣ、Ｓｉ３Ｎ４、サイアロン、ＡｌＴｉＯ３等の無機多孔質材料よりなるセラミックス製フィルタ本体に上記第２触媒を担持させてなる。図３乃至図５に模式的に示すように、触媒付フィルタ１０は、ハニカム構造をなしており、互いに平行に延びる多数のセル１２、１３を備えている。下流端が栓１４により閉塞された流入側セル１２と、上流端が栓１４により閉塞された流出側セル１３とが交互に設けられている。セル１２とセル１３とは薄肉の隔壁（排気ガス通路壁）１５を介して隔てられている。図３において、符号１１は排気ガス通路を示す。図４おいてハッチングを付した部分は排気ガス流出路１３の上流端の栓１４を示している。
　フィルタ本体としては、容量が１．０～２．０Ｌ、セル密度が２００～３００cpsi、隔壁１５の厚さが１５０～２５０μｍ、隔壁１５の気孔率が４０～６０％、隔壁１５の細孔容積が７０～４００ｃｍ３程度のものを採用することが好ましい。
  図５に示すように、排気ガスは、触媒付フィルタ１０の流入側セル１２に流入し、矢印で示すように、セル１２の周囲の隔壁１５を通って隣接する流出側セル１３に流出する。
　図６に示すように、隔壁１５はセル１２とセル１３とを連通する微小な細孔１６を有し、この細孔１６を排気ガスが通る。排気ガス中のＰＭは、主にセル１２及び細孔１６の壁部に付着して堆積する。
　第２触媒１７は、流入側セル１２を構成する隔壁１５の表面（フィルタ表面）と、細孔１６の内面に担持されている。第２触媒１７は、細孔１６の内面よりもセル１２を構成する隔壁１５の表面に厚く担持されている。上記隔壁１５の表面の単位面積当たりの第２触媒の担持量が、細孔１６の内面の単位面積当たりの第２触媒の担持量の５０倍以上５００倍以下になるようにすることが好ましい。
　そのためには、フィルタ本体に対する触媒総担持量の過半量を、流入側セル１２を構成する隔壁１５の表面に担持するようにすればよい。触媒総担持量の６５％以上８５％以下を、流入側セル１２を構成する隔壁１５の表面に担持することが好ましい。
　上記フィルタ本体１Ｌ当たりの第２触媒の担持量は隔壁１５の表面及び細孔１６の内面合わせて２０～１００ｇ／Ｌ程度とすることが好ましい。流入側セル１２を構成する隔壁１５の表面への第２触媒の担持量は、例えば、フィルタ本体１Ｌ当たり１５～７５ｇ、細孔１６の内面への第２触媒の担持量は、例えば、単位細孔容積当たり０．０８～０．３７ｇとすればよい。
　＜第１触媒及び第２触媒＞
　不飽和高ＨＣの浄化活性が高い第１触媒としては、Ｌａ２Ｏ３を４質量％含有する活性アルミナにＰｄを担持させてなるＰｄ担持Ｌａ２Ｏ３含有アルミナを必須成分として含有し、さらに、ＣｅＺｒ系複合酸化物等のＯＳＣ材（酸素吸蔵放出材）、及び該ＯＳＣ材にＲｈを担持させてなるＲｈ触媒を含有するものが好ましい。
　飽和低ＨＣの浄化活性が高い第２触媒としては、Ｌａ２Ｏ３を４質量％含有する活性アルミナにＰｔを担持させてなるＰｔ担持Ｌａ２Ｏ３含有アルミナを必須成分として含有し、さらに、上記ＯＳＣ材を含有するものが好ましい。
　上述の如く、触媒コンバータ３の前段ハニカム触媒７は、不飽和高ＨＣの浄化に優れた第１触媒を含有するから、排気ガス中の不飽和高ＨＣが当該第１触媒によって酸化浄化され、そのときに発生する触媒反応熱によって排気ガス温度が高くなる。これに伴い、飽和低ＨＣの浄化に優れた第２触媒を含有する後段ハニカム触媒８の温度が上昇する。従って、排気ガス中の飽和低ＨＣが、後段ハニカム触媒８の第２触媒によって効率良く浄化されることになる。
　さらに、排気ガスは、ハニカム触媒７，８でのＨＣの浄化に伴う触媒反応熱によって温度が上昇して下流側の触媒付フィルタ１０に流れる。そのため、触媒付フィルタ１０の第２触媒による飽和低ＨＣの浄化が効率良く進むことになる。
　また、触媒コンバータ３の前段ハニカム触媒７による不飽和高ＨＣのクラッキングによって飽和低ＨＣが生成し、該飽和低ＨＣが後段ハニカム触媒８及び触媒付きフィルタ１０に流れる。後段ハニカム触媒８及び触媒付きフィルタ１０の第２触媒は不飽和低ＨＣの浄化に優れているから、上記クラッキングによって生成する飽和低ＨＣも当該後段ハニカム触媒８及び触媒付きフィルタ１０の第２触媒によって効率良く浄化されることになる。
　触媒付フィルタ１０では、第２触媒が、流入側セル１２を構成する隔壁１５の表面において厚く、細孔１６の内面において薄く担持されている。従って、当該隔壁１５の表面において排気ガスの浄化が活発になるから、それに伴って温度が上昇した排気ガスが細孔１６を通過していく。そのため、細孔１６の内面には第２触媒が薄く担持されているものの、細孔１６を通る排気ガス温度が高いことによって、当該第２触媒による排気ガスの浄化が効率良く進む。
　＜排気ガス処理装置の製造方法＞
　－フィルタの細孔内面への触媒の担持（第１工程）－
　図７に示すように、フィルタ本体（触媒未担持）２１の一端部を、第１容器２２に貯留した上記第２触媒に係る触媒スラリー２３に浸漬して引き上げる。このフィルタ本体２１は、上述の流入側セル１２と流出側セル１３とが交互に設けられものである。
　触媒スラリー２３に対してはフィルタ本体２１の上流端側を浸漬して引き上げる。これにより、フィルタ本体２１の流入側セル１２の上流端側の内面に触媒スラリー２３が付着する。
　次いで、フィルタ本体２１の下流端に真空引きポンプ２４を接続し、該ポンプ２４を作動させてフィルタ本体２１の流出側１３を負圧にする。この流出側セル１３が負圧になることにより、流入側セル１２の上流端側に付着した触媒スラリー２３が、当該セル１２の下流側に引き寄せられるとともに、隔壁１５の細孔１６に浸み込んでいく。これにより、フィルタ２１の細孔１６の内面に触媒が担持される。
　ここに、第１容器２２に貯留する触媒スラリー２３は、隔壁１５の細孔１６に浸み込みやすい粘度に調整する。
　－乾燥－
　フィルタ本体２１を加熱することにより、隔壁１５の細孔１６の内面に付着した触媒を乾燥させる。この乾燥は、例えば、フィルタ本体２１を１５０℃の温度に２時間保持することにより行なう。
　－フィルタ隔壁表面への触媒の担持（第２工程）－
　上記乾燥後のフィルタ本体２１の上流端側の端部を第２容器２５に貯留した上記第２触媒に係る触媒スラリー２６に浸漬して引き上げる。これにより、フィルタ本体２１の流入側セル１２の上流端側の内面に触媒スラリー２６が付着する。
　次いで、フィルタ本体２１の下流端に真空引きポンプ２４を接続し、該ポンプ２４を作動させてフィルタ本体２１の流出側セル１３を負圧にする。この流出側セル１３が負圧になることにより、流入側セル１２の上流端側に付着した触媒スラリー２３が、当該セル１２の下流側に引き寄せられる。これにより、フィルタ２１の流入側セル１２の内面に、すなわち、隔壁１５の表面に触媒が担持される。
　ここに、第２容器２５に貯留する触媒スラリー２６は、真空引きポンプ２４による吸引時に隔壁１５の細孔１６に浸入することを抑制されるように、第１容器２２の触媒スラリー２３よりも、粘度を高くする。
　なお、触媒スラリー２６を隔壁１５の表面に担持したとき、一部の細孔１６が塞がれるが、隔壁１５の表面に担持された触媒スラリー２６は、その後の焼成によって多孔質の触媒層になるから、排気ガスはその触媒層を通過して細孔１６に流入することができる。
　－焼成－
　上記第２工程を経たフィルタ本体２１加熱することにより、フィルタ本体２１の隔壁１５の表面に付着した触媒及び細孔１６の内面に付着した触媒を焼成する。この焼成は、例えば、フィルタ本体２１を５００℃の温度に２時間保持することにより行なう。必要に応じて、当該焼成前に、乾燥工程（フィルタ本体２１を１５０℃の温度に２時間保持）を入れる。
　以上により、フィルタ本体２１の流入側セル１２における隔壁１５の表面と細孔１６の内面に第２触媒が担持された触媒付フィルタ１０が得られる。
　－アセンブリー（第３工程）－
　触媒付フィルタ１０をフィルタ容器に収容したＧＰＦ装置５を、ハニカム触媒７，８を触媒容器に収容した触媒コンバータ３と結合し、触媒コンバータ３を排気マニホールド２に連結管４を介して接続し、ＧＰＦ装置５と排気管６を接合する。これにより、エンジンの排気ガス処理装置が得られる。
　＜実施例及び比較例＞
　フィルタ本体２１として、容量１．３Ｌのコージェライト製フィルタを準備した。そのセル密度は２５０cpsi、隔壁厚は２００μｍ、隔壁の気孔率は５０％、隔壁の細孔容積は約１００ｃｍ３である。
　実施例では、当該フィルタ本体２１の細孔内面に第２触媒を１５ｇ／Ｌ（上記第１工程での担持量）、流入側セル１２を構成する隔壁面に第２触媒を４５ｇ／Ｌ（上記第２工程での担持量）担持させることによって触媒付フィルタを得た。
　フィルタ本体２１の流入側セル１２を構成する隔壁面の総面積は１．８２ｍ２、水力直径の概念から計算したフィルタ本体２１の細孔内面の総面積は２５８．０９ｍ２である。従って、流入側セル１２を構成する隔壁面（フィルタ表面）の単位面積当たりの触媒担持量は２４．７３ｇ／ｍ２、細孔内面の単位面積当たりの触媒担持量は０．０５８ｇ／ｍ２である。よって、流入側セル１２を構成する隔壁面の単位面積当たりの触媒担持量は、細孔内面の単位面積当たりの触媒担持量の約４２６倍である。
　比較例では、当該フィルタ本体２１の細孔内面に第２触媒を６０ｇ／Ｌ担持させることによって触媒付フィルタを得た。流入側セル１２を構成する隔壁面への触媒担持量は零とした。細孔内面の単位面積当たりの触媒担持量は０．２３ｇ／ｍ２である。
　[昇温特性]
　実施例及び比較例各々の触媒付フィルタに模擬排気ガスとしてのメタンガス（フィルタ入口でのガス温度３００℃，ＣＨ４濃度１６０ｐｐｍＣ）を流したときの、細孔に流入するガス温度を試算した。
　ＣＨ４濃度、ガス流量１０ｇ／秒及びガス流通時間６０秒からフィルタに流入するＣＨ４総量（０．０６mol）を求めた。実施例フィルタでは、ＣＨ４総量の７５％が流入側セル１２の隔壁面に担持されている第２触媒で浄化されると仮定し、そのときのガスの上昇温度をフィルタの熱容量７３６Ｊ／ｋｇ・Ｋ及び重量０．４５ｋｇとＣＨ４の下記燃焼熱から求めた。比較例フィルタでは流入側セルでのＣＨ４浄化率は零である。結果を表１及び図８に示す。
　　ＣＨ４ ＋ ２Ｏ２ → ＣＯ２ ＋ ２Ｈ２Ｏ ＋ ８９１ｋＪ／mol
Figure JPOXMLDOC01-appb-T000001
　実施例のように、流入側セル１２を構成する隔壁面に触媒を担持すると、触媒反応熱によって細孔に流入する排気ガス温度が上昇し、細孔内面に担持されている触媒による排気ガスの浄化に有利になることがわかる。
　[排気圧損］
　実施例及び比較例各々の触媒担持量は同じく６０ｇ／Ｌである。比較例ではその触媒全量を細孔内面に担持しているのに対して、実施例では、触媒全量の３／４を流入側セル１２を構成する隔壁面に担持することにより、細孔内面への触媒担持量を１５ｇ／Ｌとしている。そのため、実施例フィルタでは、比較例フィルタに比べて、隔壁の気孔率が５．４％程度大きくなっている。
　触媒付フィルタによるエンジンの排気圧損は気孔率のみに依存すると仮定して、比較例を基準（１００％）とする実施例の排気圧損の低下率を算出した。その算出において、排気ガス流量は０．１５ｇ／ｓとし、排気ガス温度は５５０℃とした。結果を図９に示す。
　実施例では、排気圧損が比較例比で９３％程度になっている。これから、実施例のように、触媒の一部を流入側セルを構成する隔壁面に担持すると、排気圧損が小さくなり、エンジンの掃気性の向上、ひいては燃費の向上に有利になることがわかる。
　　１　　ガソリンエンジン
　　２　　排気マニホールド
　　３　　触媒コンバータ
　　５　　ＧＰＦ装置
　　７　　前段ハニカム触媒
　　８　　後段ハニカム触媒
　１０　　触媒付フィルタ
　１２　　流入側セル
　１３　　流出側セル
　１４　　栓
　１５　　隔壁
　１６　　細孔
　１７　　第２触媒

Claims (6)

  1. 　エンジンの排気ガス通路に排気ガス中の粒子状物質を捕集する多孔質フィルタが設けられてなり、
    　上記排気ガスが上記フィルタの表面から該フィルタの細孔を通過して排出される排気ガス処理装置であって、
    　上記フィルタ表面及び上記細孔内面に排気ガス浄化用の触媒が担持されており、
    　上記触媒は、上記細孔内面よりも上記フィルタ表面に厚く担持されていることを特徴とするエンジンの排気ガス処理装置。
  2. 　請求項１において、
    　上記フィルタ表面の単位面積当たりの上記触媒の担持量は、上記細孔内面の単位面積当たりの上記触媒の担持量の５０倍以上５００倍以下であることを特徴とするエンジンの排気ガス処理装置。
  3. 　請求項１又は請求項２において、
    　上記排気ガス通路における上記フィルタよりも上流側に上記排気ガスを浄化する触媒コンバータが設けられていて、
    　上記触媒コンバータは、炭素数が６～９である不飽和炭化水素の酸化反応に活性を示す触媒を備え、
    　上記フィルタの上記触媒が炭素数が５以下である飽和炭化水素の酸化反応に活性を示すことを特徴とするエンジンの排気ガス処理装置。
  4. 　エンジンの排気ガスを通す細孔を有する多孔質フィルタを、排気ガス浄化用の触媒を分散させた第１触媒スラリーに浸漬し、該触媒を上記フィルタの細孔内面に担持する第１工程と、
    　上記第１工程を経た上記フィルタを、上記触媒を分散させた第２触媒スラリーに浸漬し、該触媒を上記フィルタの表面に、上記細孔内面に担持された上記触媒の厚さよりも厚く担持する第２工程と、
    　上記第２工程を経た上記フィルタを上記エンジンの排気ガス通路に設ける第３工程とを備えていることを特徴とするエンジンの排気ガス処理装置の製造方法。
  5. 　請求項４において、
    　上記第１触媒スラリーの触媒と上記第２触媒スラリーの触媒とは、その成分が同じであることを特徴とするに分散させたエンジンの排気ガス処理装置の製造方法。
  6. 　請求項４又は請求項５において、
    　上記第１工程と上記第２工程の間に、上記フィルタの細孔内面に担持した上記触媒を乾燥させる工程を備え、
    　上記第２工程と上記第３工程の間に、上記フィルタの表面に担持された上記触媒及び上記細孔内面に担持された上記触媒を焼成する工程を備えていることを特徴とするエンジンの排気ガス処理装置の製造方法。
PCT/JP2018/019879 2017-06-05 2018-05-23 エンジンの排気ガス処理装置及びその製造方法 WO2018225514A1 (ja)

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