WO2005075800A1 - Reactor with heat exchange function - Google Patents

Reactor with heat exchange function Download PDF

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Publication number
WO2005075800A1
WO2005075800A1 PCT/JP2005/001416 JP2005001416W WO2005075800A1 WO 2005075800 A1 WO2005075800 A1 WO 2005075800A1 JP 2005001416 W JP2005001416 W JP 2005001416W WO 2005075800 A1 WO2005075800 A1 WO 2005075800A1
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WO
WIPO (PCT)
Prior art keywords
reactor
fluid
heat
heat transfer
temperature
Prior art date
Application number
PCT/JP2005/001416
Other languages
French (fr)
Japanese (ja)
Inventor
Akira Obuchi
Junko Uchisawa
Akihiko Ooi
Tetsuya Namba
Norio Nakayama
Atsushi Ogata
Original Assignee
National Institute Of Advanced Industrial Science And Technology
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Application filed by National Institute Of Advanced Industrial Science And Technology filed Critical National Institute Of Advanced Industrial Science And Technology
Priority to JP2005517681A priority Critical patent/JPWO2005075800A1/en
Publication of WO2005075800A1 publication Critical patent/WO2005075800A1/en

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Classifications

    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/021Exhaust 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
    • F01N3/023Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles
    • F01N3/0233Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles periodically cleaning filter by blowing a gas through the filter in a direction opposite to exhaust flow, e.g. exposing filter to engine air intake
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/021Exhaust 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
    • F01N3/023Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/021Exhaust 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
    • F01N3/023Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles
    • F01N3/0234Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles using heat exchange means in the exhaust line
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/021Exhaust 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
    • F01N3/023Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles
    • F01N3/027Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles using electric or magnetic heating means
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/021Exhaust 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
    • F01N3/033Exhaust 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
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2240/00Combination or association of two or more different exhaust treating devices, or of at least one such device with an auxiliary device, not covered by indexing codes F01N2230/00 or F01N2250/00, one of the devices being
    • F01N2240/02Combination or association of two or more different exhaust treating devices, or of at least one such device with an auxiliary device, not covered by indexing codes F01N2230/00 or F01N2250/00, one of the devices being a heat exchanger
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2510/00Surface coverings
    • F01N2510/06Surface coverings for exhaust purification, e.g. catalytic reaction
    • F01N2510/065Surface coverings for exhaust purification, e.g. catalytic reaction for reducing soot ignition temperature

Definitions

  • the present invention relates to a reactor having a heat exchange function, and particularly to a suitable technology applicable to the field of thermal engineering for saving energy consumption and the field of environmental technology for purifying air and exhaust gas. Things.
  • a combination of a chemical reactor and heat exchange is widely used as a means for increasing energy efficiency in a chemical reaction process.
  • the chemical reactor and the heat exchange are separated, it is difficult to increase the heat recovery rate because the heat loss at these connecting portions is large and the overall shape is generally large. For this reason, a device that integrates heat exchange and a reactor is being used for the first time.
  • Such a conventional heat exchange reactor is of a self heat exchange type in which heat is exchanged between the upstream and downstream of the same fluid containing a reactant.
  • the downstream force with the increased temperature is designed to transfer heat to the upstream where preheating is required.
  • a self-heat-exchange type thermal reactor is provided with a heat transfer surface inside the heat exchanger, which is provided with an end on a partition wall, and in which the fluid containing the reactant is inverted.
  • a fluid inlet and a fluid inlet and a fluid inlet are provided at substantially the center in the longitudinal direction of a heat-transfer partition for heat exchange.
  • a reactor having a structure in which an outlet is provided and the fluid is reversed at both ends in the longitudinal direction of the partition wall has also been proposed (for example, see Patent Document 1).
  • a fluid containing a reactant is naturally divided into two inside a structure having a heat exchange function in a reactor, and flows toward each end. Therefore, compared to the case of FIG.
  • the heat recovery rate decreases due to the increase of the flow rate, and the temperature of the reaction zone decreases more and more.
  • such a method in which the flow path is divided inside the heat exchanger has the characteristic that the distribution ratio of the fluid and the difference between the maximum values of the temperatures in both reaction regions are widened. Having. If the fluid passes through the flow path on the low temperature side more, the required reaction rate may not be reached, and the desired reaction rate may not be obtained. Furthermore, since the temperature has two maximum values and the force spreads to the end of the reactor, it may be difficult to efficiently maintain a high temperature in the reaction zone where heat radiation is high.
  • Patent Document 1 Japanese Patent Application Laid-Open No. 2000-189757
  • Non-Patent Document 1 "Chemical Engineering”, edited by Kenji Hashimoto, Baifukan, 1997, p. 79, Disclosure of the invention
  • the present invention has been made in view of such a situation of the prior art, and is a compact heat exchanger in which a heat exchanger ⁇ and a chemical reactor are integrated, has a high heat recovery rate, and further has a low pressure loss.
  • the purpose is to provide a reactor equipped with Koura Noh.
  • a reactor having a two-fluid countercurrent type heat exchanger structure having two flow paths separated by a heat transfer surface, wherein a chemical reaction is promoted in at least a part of the flow path where heat exchange is performed.
  • a reactor provided with a heating means for moving the reactor.
  • a heating means in a streamline direction, and a filter for capturing combustible fine particles at the same position and / or in the vicinity of the heating means are arranged.
  • the heat generated by the chemical reaction and the heat added to continue the chemical reaction are recovered by the discharged fluid power, and re-supplied to the main part where the chemical reaction occurs.
  • a highly energy-saving reactor with little or no auxiliary heating is provided.
  • the reactor of the present invention can reduce both the flow rate and the flow path length of the portion having the heat exchange function by half compared with the conventional self-heat exchange type reactor in which only one continuous flow path is used, pressure loss is reduced. Can be significantly reduced, and the energy required for pumping can be saved in this respect as well.
  • the reactor of the present invention has a higher temperature in the main reaction region than a conventional self-heat exchange type reactor in which a fluid is naturally divided into two inside a structure having a heat exchange function in the reactor. Is less likely to be uneven, and heat loss due to heat radiation can be reduced.
  • the reactor of the present invention is a low-concentration organic component treatment device such as a deodorizing device or an automobile exhaust gas converter with high energy efficiency, or a particulate matter reduction device (DPF) that captures and removes particulate matter discharged from a diesel engine.
  • a low-concentration organic component treatment device such as a deodorizing device or an automobile exhaust gas converter with high energy efficiency
  • DPF particulate matter reduction device
  • FIG. 1 is a schematic configuration diagram of a conventionally known self-heat exchange type reactor having a flow path reversing part at one end.
  • FIG. 2 is a schematic configuration diagram of a conventionally known self-heat exchange type reactor having flow passage reversing portions at both ends.
  • FIG. 3 is a basic configuration diagram of the reactor of the present invention, and is a cross-sectional view of a main part of a reactor having a two-fluid countercurrent heat exchange function.
  • FIG. 3 (a) shows an example in which a catalytic reaction is used as a heating means.
  • FIG. 3 (b) shows a case where an electric heater is used as a heating means.
  • FIG. 4 is a configuration diagram of another reactor of the present invention, and has a two-fluid countercurrent type heat exchange function to which an introduction path for causing substantially equivalent fluids to flow in opposite directions is added. It is principal part sectional drawing of.
  • FIG. 4 (a) shows one fluid to be introduced after being divided into two.
  • Fig. 4 (b) shows a multi-cylinder engine in which half of the cylinder exhaust gas is introduced collectively.
  • FIG. 5 is a configuration diagram of still another reactor of the present invention, and is an oblique perspective view of a main part of a reactor having a two-fluid countercurrent heat exchange structure using a corrugated heat transfer body.
  • FIG. 5 (a) shows a corrugated heat transfer body and a catalyst layer installed thereon.
  • FIG. 5 (b) shows the main part of the reactor containing the structure of FIG. 5 (a) and the fluid flow path.
  • FIG. 6 is a configuration diagram of still another reactor of the present invention, which has a two-fluid countercurrent heat exchange structure having a particulate matter reduction function using a corrugated heat transfer material combined with a filter material. It is principal part sectional drawing of a vessel.
  • FIG. 6 (a) shows a case where a part of the gap of the corrugated heat transfer material is filled with a filter material.
  • Fig. 6 (b) shows a flat filter material sandwiched between two spacers to increase the geometric filtration area.
  • FIG. 6 (c) shows a combination of a flat filter material and a spacer having a form in which a fluid flow collides in one direction of the filter.
  • FIG. 3 is a schematic sectional view of a main part of a reactor having a two-fluid countercurrent heat exchanger function according to the first embodiment of the present invention.
  • FIG. 3 (a) shows an example of the reactor of the present invention based on the multi-tube cylindrical heat exchanger structure.
  • the inlet 2 and the outlet 3 respectively show the inside of the reaction vessel 1 from left to right in this figure.
  • the inlet 2 ′ and the outlet 3 ′ are separated from the flow path of the first fluid by the heat transfer surface, and are the entrances and exits of the second fluid flowing inside the vessel 1 to the right and left in this figure.
  • Reference numeral 5 denotes a catalyst layer provided in a portion near the center of the flow path of the first fluid, and is an example in which the catalyst layer is used as heating means for the reactor in the present invention.
  • a first fluid such as a mixture of hydrocarbon and air, having a composition capable of causing an exothermic reaction by the catalyst layer 5 enters the container 1 from the fluid inlet 2 and flows to the right.
  • a first fluid such as a mixture of hydrocarbon and air, having a composition capable of causing an exothermic reaction by the catalyst layer 5 enters the container 1 from the fluid inlet 2 and flows to the right.
  • heat is generated in this portion, whereby the catalyst layer 5 and the first fluid are heated. While this heated first fluid flows from the catalyst layer 5 to the fluid outlet 3 (section R in the figure), the first fluid force heat transfer surface, and furthermore, the heat transfer from the heat transfer surface to the second fluid, While the first fluid cools, it flows countercurrently The second fluid is heated.
  • the second fluid heated in the section flows between the catalyst layer 5 and the fluid outlet 3 ′ (section L in the drawing)
  • the second fluid is more than the first fluid separated by the heat transfer surface. It is hot. Therefore, heat transfer from the second fluid to the first fluid cools the second fluid while heating the first fluid.
  • the heat of reaction which is originally discharged to the outside together with the first fluid, is recovered inside the container 1, and as a result, the catalyst becomes more in comparison with the one-sided plug flow type reactor.
  • the reactor can keep the temperature of the layer 5 high by the reaction heat.
  • the type of catalyst used in the catalyst layer 5 is appropriately determined depending on the reaction components contained in the fluid, and the type of the catalyst is not limited.
  • the reaction components are hydrocarbons and oxygen in the air
  • catalysts in which noble metal fine particles such as Pt, Pd, Rh, and Ir are supported in the form of fine particles on a high surface area material such as alumina or zeolite, MnO, Co O, NiO, Cu
  • an oxide having high oxidation catalytic activity such as a metal oxide such as o and a composite oxide thereof.
  • the position of the catalyst layer 5 in the streamline direction is most effectively located near the center of the countercurrent.
  • the central force may also be shifted.
  • the thickness of the catalyst layer 5 in the flow channel direction is short in order to improve the heat recovery rate, and is more desirable, but long in order to improve the reaction rate, and is more desirable. May be determined based on a balance between the two conditions.
  • the catalyst layer 5 is filled in the flow channel, but may be coated on the heat transfer surface.
  • only the first fluid contains a reaction component, and the catalyst layer is disposed only in a part of the first fluid flow path. However, the same or different reaction components are also contained in the second fluid together with the first fluid.
  • a catalyst layer that contains and promotes the reaction may be disposed in a part of the second fluid flow path. In this case, it is most effective to arrange both catalyst layers at the center, but they may be intentionally shifted individually in the streamline direction.
  • other forms capable of countercurrent flow such as a force plate fin type using a multi-tube cylindrical type or a vortex type, may be used as the heat exchange structure.
  • FIG. 3 (b) shows the use of an electric heater 7 installed in a flow path without using the above-described catalytic reaction as a heating means.
  • the heating by the electric heater 7 and the heat recovery The temperature of the portion where the thermal heater 7 is installed can be effectively raised, thereby providing a reactor for promoting the thermal reaction.
  • the electric heater 7 is arranged only in the flow path of the first fluid, but may be arranged in a part of the second fluid in the same manner. In this case as well, it is most effective to arrange the electric heater in the vicinity of the center in the streamline direction in order to maximize the heat recovery rate. It is also possible to use other physical heating means such as microwaves, electromagnetic induction heating, etc., which can be used only with an electric heater. Good.
  • FIG. 4 is a schematic cross-sectional view of a reactor according to another embodiment of the present invention.
  • the reactor of this form is originally a single or substantially equivalent fluid divided into two, and used as first and second fluids which flow countercurrently. That is, in FIG. 4 (a), a piping structure is provided in which the reaction fluid entering from the fluid inlet 2 is divided into two at the three-way joint 8 and then guided to the two fluid inlets 2 ′ and 2 ′′ of the container 1.
  • the catalyst layer 5 is disposed in the middle of both flow paths of the first and second fluids in the heat exchange structure, whereby a heat recovery mechanism similar to that described in the first embodiment is provided. Thereby, the temperature near the catalyst layer 5 can be increased.
  • This structure has two main reaction areas where the temperature reaches a local maximum, compared to a conventional self-heat exchange type reactor in which the fluid naturally divides into two inside the structure having heat exchange capability inside the reactor. Since it is a common location in the flow path, the temperature is less likely to be uneven between the two flow paths. Further, since the maximum value of the temperature is limited to one location in the center of the reactor and it is easy to take a heat retaining means, the heat loss due to heat radiation can be further reduced.
  • a flow rate control valve 9 is appropriately provided in one or both of the flow paths divided by the three-way joint 8, so that the fluid inlets 2 'and 2 "
  • the distribution ratio of the input reaction fluid may be set to be equal or another intended ratio.
  • FIG. 4 (b) shows the exhaust gas of the engine 10 in which the reaction fluid has an even number of cylinders.
  • the exhaust gas from half the cylinders is the first fluid
  • the exhaust gas from the remaining half cylinders is the second fluid. It is equipped with a piping structure for flowing countercurrent to each other. The flow path of both fluids is the same as in Fig. 4 (a).
  • the catalyst layer 5 is provided inside.
  • the fluid in the reactor is Since there is no danger of a decrease in the heat recovery rate due to uneven flow rates between the two flow paths, it is possible to exhibit performance close to the maximum performance that can be expected.
  • FIG. 5 is a perspective view showing another embodiment of the reactor according to the present invention.
  • FIG. 5 (a) shows a rectangular heat conductor such as a stainless steel plate having heat resistance formed into a corrugated shape, and a catalyst layer 5 disposed near the center in the longitudinal direction. Most desirably, adjacent flat portions of the corrugations are formed so as to be parallel to each other at regular intervals. In order to achieve this, a material having heat resistance and air permeability, such as stainless steel wire mesh, may be interposed as a spacer in the whole or a part of the corrugated space.
  • FIG. 5 (b) shows a case where the corrugated heat transfer body 11 having the catalyst layer 5 is housed in a rectangular parallelepiped container 1.
  • the container 1 is provided with a first fluid inlet 2 'and an outlet 3' force near both ends in the longitudinal direction of the upper surface in FIG. 5 (b), and a lower surface is provided on the lower surface behind the outlet 3 'and the inlet 2', respectively.
  • Two fluid inlets 2 "and outlets 3" are provided.
  • the gap between the container 1 and the corrugated heat transfer body 11 is sealed with a suitable sealing material.
  • the first and second fluids entering from the fluid inlets 2 'and 2 "respectively form the ridges (or valleys) of the waveform in the voids on one side of the waveform and the opposite side across the waveform heat transfer body 11
  • both fluids contain a component that causes an exothermic reaction due to the action of the catalyst layer 5
  • the fluid flows from the fluid inlet 2 '(and the fluid outlet 3 ").
  • heat transfer occurs from the second fluid (the hatched arrow in the figure) to the first fluid (black arrow), and the section from the catalyst layer 5 to the fluid outlet 3 '(and the fluid inlet 2 ").
  • FIG. 6 is a cross-sectional view of a reactor according to another embodiment of the present invention, which is perpendicular to a plane portion of the corrugated heat transfer body 11.
  • FIG. 6 (a) shows a filter in which a combustible fine particle floating in a gas can be captured in a space near the center of the corrugated heat transfer body 11.
  • the filter 14 carries a catalyst having a function of promoting the heat generation by reacting the reaction components contained in the fluid, or in the same section where the filter is disposed, the corrugated heat transfer material 11
  • a physical heating means such as an electric heater capable of directly heating the filter is disposed on both sides of the filter.
  • the temperature of the filter 14 can be easily raised by the generated heat and the heat recovery action in the reactor. Thereby, the carbon fine particles are oxidized and removed, and the filter function can be maintained.
  • the filter 14 simply fills a part of the flow path, but may be as shown in FIG. 6 (b). That is, after a flexible flat filter material 15 is sandwiched between spacers 16 such as a stainless steel wire mesh having heat resistance and air permeability, it is stored in each gap of the corrugated heat transfer body 11.
  • spacers 16 such as a stainless steel wire mesh having heat resistance and air permeability
  • the downstream end of the flat filter material 15 is longer than the spacer 16 arranged on the upstream side in the longitudinal direction of the waveform, and the upstream end of the flat filter material 15 is arranged on the downstream side. Upstream end of flat filter material 15 longer than 16 And the downstream end are alternately brought into close contact with the heat transfer member surfaces on both sides of the gap.
  • the spacer 16 may also have a function as a catalyst support structure or an electric heater.
  • a heat-resistant and air-permeable switch having a periodic structure between the two flat filter members 15 that bends the flow of the fluid in the direction of colliding with the filter surface. It may be used with a spacer 17 in between. As such a spacer, a plain-woven stainless steel wire mesh, a corrugated metal plate having many small holes, or the like is used. With this structure, the flammable particulates are captured by the collision of the fluid on one surface of the filter, but the pressure loss can be reduced compared to the case of Fig. 6 (a) where the fluid penetrates the filter. it can.
  • the catalyst is supported on the filter material 15, the surface of the heat transfer body in contact with the filter material 15, or the surface of the spacer 17 having a function of bending the fluid flow, or a spacer having a function of bending the fluid flow. 17 can also be used as a heating means by also using an electric heater!
  • a fluid is provided with a pipe structure for dividing one fluid into two and flowing in countercurrent to each other, and has a corrugated stainless steel heat transfer body and flow path form as shown in Fig. 5. Then, a heat exchange reactor was prepared in which a heat-resistant fiber piece carrying an oxidation catalyst was disposed at a position corresponding to the filter material in FIG. 6 (c).
  • a heat transfer plate was fabricated by bending a strip of stainless steel thin plate having a thickness of 0.03 mm, a width of 300 mm, and a length of more than 1600 mm 39 times at right angles to the longitudinal direction at 40 mm intervals.
  • a 50-150 mm point from one end in the longitudinal direction of the corrugated structure is a platinum catalyst-carrying 0.25 mm thick, 80 mm long and 100 mm wide heat resistant at 1100 ° C.
  • Twenty pieces of plain woven fiber made of mullite having were placed between the corrugated peaks (20 pieces) of the heat transfer structure.
  • a stainless steel plain weave wire (0.45 mm in wire diameter, 8 mesh) (thickness: about lmm) was placed between the flat surfaces of the corrugated structure in places where there was no fiber piece as a spacer.
  • a stainless steel plain woven wire mesh with a wire diameter of 0.25 mm and 16 mesh (thickness of about 0.5 mm) was sandwiched between the fiber pieces.
  • the corrugated structure, the fiber piece supporting the platinum catalyst, and the wire mesh spacer are housed in a stainless steel container having a thickness of 0.6 mm and a rectangular parallelepiped (inner size of 40 mm x 47 mm x 300 mm), and a heat exchange type reactor is used. This was the No. 1 reactor.
  • the reactor was provided with rectangular openings of 10x47mm at four points where the longitudinal force at both ends was about 20mm, and a circular pipe with a diameter of 19mm was partially formed in each of these openings. It was cut into a shape and attached so that it could be covered, thereby providing a fluid entrance and exit.
  • the flow direction was such that the portion (catalyst layer) between the fiber pieces supporting the catalyst was closer to the outlet side than the center in the longitudinal direction of the reactor.
  • Ethylene removal rate and heat recovery performance were investigated when simulated contaminated air containing 0.13% ethylene was flowed at a flow rate of 30-180 L / min. Table 1 shows the obtained results.
  • the ethylene concentrations at which spontaneous catalytic combustion can be continued are 0.045, 0.056, 0.096, and 0.127%, respectively, all of which are low concentrations that cannot be realized with a normal catalyst layer without a heat recovery function.
  • the outlet temperature is much lower than the central temperature, and it is easily assumed that heat moves from downstream to upstream of the catalyst layer.
  • the reason why the difference between the outlet temperature and the inlet temperature is smaller than the theoretical rise temperature is that there is heat loss due to heat conduction to the reactor and convection to the air around the reactor other than the amount discharged together with the treated air. It is. Even taking these heat losses into account, the maximum heat recovery at each flow rate reached as high as 83, 82, 74 and 68%.
  • the differential pressure (pressure loss) before and after the reactor was as small as 19-28 mmAq at a flow rate of 30 L / min, and was only 281 mmAq at a flow rate of 176 L / min.
  • Heat recovery rate (central temperature-inlet temperature-theoretical boundary; 3 ⁇ 4degree) / (central temperature (Temperature-inlet conductivity): * 100
  • a second reactor was manufactured.
  • the piping structure of this second reactor and the configuration, shape, and dimensions of the reactor body are almost the same as those of the first reactor.
  • the width of the mullite fiber pieces on both sides of the corrugated structure was 40 mm (total weight used: 36 g), and Pt (total weight: 0.36 g) and MoO (0.36 g) were supported as catalysts there.
  • Heat recovery rate (Central part temperature-Inlet temperature-Theoretical rise temperature) / (Central part temperature-Inlet temperature ): * 100
  • the ⁇ trapping rate is obtained by measuring the ⁇ concentration before and after the reactor using an instantaneous fine particle mass measuring device ( ⁇ ) and also estimating the force. It is confirmed that it has the same high heat recovery as the first reactor and captures 50% of ⁇ .
  • the change over time of pressure loss which is an indicator of the accumulation status inside the device, is stable at an exhaust gas flow rate of 45 L / min at a central temperature of 456 ° C or higher, and when the hydrogen concentration is lowered, the temperature becomes 380 ° C. Only after reaching ° C did it show a remarkable upward trend.
  • the central part temperature is 456 ° C or higher, it can be assumed that PM oxidation proceeds at a sufficiently high rate and the amount of deposited PM does not increase, and continuous collection and removal of PM by oxidation are possible. You. Similarly, when the exhaust gas flow rate was 60 Lmin, it was confirmed that if the temperature in the central part was raised to 585 ° C, continuous collection and removal of the acid were possible.

Abstract

A reactor capable of providing a high energy-saving property comparable with a self-heat exchange type reactor and remarkably reducing pressure loss and suitably usable for easily heat-regenerable diesel particulate filter (DPF) by disposing a filter in a flow passage inside the reactor. The reactor moves heat from the downstream side of one fluid to the upstream side of the other fluid between two fluids by installing a heating means such as a catalytic layer and an electric heater in one or both of the flow passages of a two-fluid counter-current flow type heat exchange structure having two flow passages partitioned by a heat transfer surface, desirably a heat transfer surface formed of a waveform transmitting body, desirably at the center part thereof. Also, the filter may be installed in the flow passage of the reactor at the same position as the heating means and/or near the heating means.

Description

明 細 書  Specification
熱交換機能を備えた反応器  Reactor with heat exchange function
技術分野  Technical field
[0001] 本発明は、熱交換機能を備えた反応器に関し、特にエネルギー消費を節約するた めの熱工学分野、及び大気ゃ排ガス浄化を目的とする環境技術分野に適用し得る 好適な技術に関するものである。  The present invention relates to a reactor having a heat exchange function, and particularly to a suitable technology applicable to the field of thermal engineering for saving energy consumption and the field of environmental technology for purifying air and exhaust gas. Things.
背景技術  Background art
[0002] 化学反応器と熱交 を組み合わせることは、化学反応プロセスにおけるエネルギ 一効率を高めるための手段として広く行われている。しかし、化学反応器と熱交 が分離した装置である場合には、これらの接続部分での熱損失が大きいとともに全 体形状が概して大きくなるため、熱回収率を高めることが困難である。このため、熱交 翻と反応器を一体化させた装置も使われはじめて 、る。  [0002] A combination of a chemical reactor and heat exchange is widely used as a means for increasing energy efficiency in a chemical reaction process. However, in the case of a device in which the chemical reactor and the heat exchange are separated, it is difficult to increase the heat recovery rate because the heat loss at these connecting portions is large and the overall shape is generally large. For this reason, a device that integrates heat exchange and a reactor is being used for the first time.
[0003] このような従来の熱交換型反応器では、反応物を含む同一流体の上流と下流の間 で熱を交換する自己熱交換型となっている。通常の加熱反応器の場合には、温度が 高くなつた下流力 予備加熱が必要な上流へと熱を移動させるように設計されている 。さらに、自己熱交換型の熱反応器としては、図 1に示すように、熱交^^の内部に おいて伝熱面となる隔壁に端部を設けそこで反応物を含む流体を反転することにより 、該隔壁の互いに反対面を流体の上流と下流が逆方向に流れることにより、向流形 熱交棚能を付与したものが提案されている (例えば、非特許文献 1参照)。しかし、 このような流路構成では、狭隘な熱交翻内部の流路長が長くなるため、圧力損失 が極めて高くなるという問題点がある。  [0003] Such a conventional heat exchange reactor is of a self heat exchange type in which heat is exchanged between the upstream and downstream of the same fluid containing a reactant. In the case of a normal heating reactor, the downstream force with the increased temperature is designed to transfer heat to the upstream where preheating is required. In addition, as shown in Fig. 1, a self-heat-exchange type thermal reactor is provided with a heat transfer surface inside the heat exchanger, which is provided with an end on a partition wall, and in which the fluid containing the reactant is inverted. Thus, there has been proposed a configuration in which the upstream and downstream sides of the fluid flow in opposite directions on the mutually opposite surfaces of the partition wall to provide a counterflow heat exchange shelf function (for example, see Non-Patent Document 1). However, such a flow path configuration has a problem that the pressure loss becomes extremely high because the flow path length inside the narrow heat exchange becomes long.
[0004] また、このような欠点が解消されるものとして、図 2に示すように、熱交換を行う伝熱 体隔壁の長手方向ほぼ中央部に、該隔壁の互いに反対側に流体の入口及び出口 を設け、隔壁の長手方向両端部で流体を反転させる構造をとつた反応器も提案され ている(例えば、特許文献 1参照)。この方式では、反応物を含む流体が反応器内の 熱交換機能を持つ構造体の内部で自然に 2分割され、該両端部方向へそれぞれ流 れていく。このため、出入口を熱交換器構造体の端部に設けた図 1の場合と比べて、 流路長および各部分の流量が半減され、流体の圧力損失を小さくすることができる。 しかし、この方式では、温度が極大となる主反応領域が反応器両端部の 2箇所あるた め、両反応領域の温度を均等にすることが困難である。特に、流体が気体の場合、そ の粘性抵抗は温度の上昇とともに増すので、一方の反応領域が他方よりわずかでも 温度が高くなると、該領域に分割される流体の比率力 、さくなり、その結果、該流路 側の熱回収率が高まって益々該反応領域の温度が高くなつてしまう。一方、反対流 路側では、流量が増すため熱回収率が低くなり、益々その反応領域の温度が低くな つてしまう。つまり、このような、熱交換器内部で流路を分割する方式では、流体の分 配比および両反応領域における温度極大値の差が拡大する特性があり、反応器とし ては極めて重大な欠点を有する。低温側の流路をより多く通る流体では、必要とする 反応速度に達せず、所期の反応率が得られなくなるおそれがある。さらに、温度の極 大値が 2箇所し力も反応器の端部に広がっているので、放熱度も高ぐ反応領域を効 率よく高温に保つことが困難な場合もある。 [0004] In addition, as a solution to such a disadvantage, as shown in FIG. 2, a fluid inlet and a fluid inlet and a fluid inlet are provided at substantially the center in the longitudinal direction of a heat-transfer partition for heat exchange. A reactor having a structure in which an outlet is provided and the fluid is reversed at both ends in the longitudinal direction of the partition wall has also been proposed (for example, see Patent Document 1). In this method, a fluid containing a reactant is naturally divided into two inside a structure having a heat exchange function in a reactor, and flows toward each end. Therefore, compared to the case of FIG. 1 in which the entrance and exit are provided at the end of the heat exchanger structure, The flow path length and the flow rate of each part are halved, and the pressure loss of the fluid can be reduced. However, in this method, it is difficult to equalize the temperatures in both reaction zones because there are two main reaction zones where the temperature is maximized at both ends of the reactor. In particular, when the fluid is a gas, its viscous resistance increases as the temperature rises, so if one of the reaction areas becomes slightly higher in temperature than the other, the specific force of the fluid divided into the reaction area decreases, and as a result, As a result, the heat recovery rate on the flow path side is increased, and the temperature of the reaction region is further increased. On the other hand, on the opposite channel side, the heat recovery rate decreases due to the increase of the flow rate, and the temperature of the reaction zone decreases more and more. In other words, such a method in which the flow path is divided inside the heat exchanger has the characteristic that the distribution ratio of the fluid and the difference between the maximum values of the temperatures in both reaction regions are widened. Having. If the fluid passes through the flow path on the low temperature side more, the required reaction rate may not be reached, and the desired reaction rate may not be obtained. Furthermore, since the temperature has two maximum values and the force spreads to the end of the reactor, it may be difficult to efficiently maintain a high temperature in the reaction zone where heat radiation is high.
[0005] 特許文献 1:特開 2000-189757号公報 [0005] Patent Document 1: Japanese Patent Application Laid-Open No. 2000-189757
非特許文献 1 :橋本健治編「ケミカルエンジニアリング」、培風館、 1997発行、第 79頁 発明の開示  Non-Patent Document 1: "Chemical Engineering", edited by Kenji Hashimoto, Baifukan, 1997, p. 79, Disclosure of the invention
発明が解決しょうとする課題  Problems to be solved by the invention
[0006] 本発明は、このような従来技術の実情に鑑みてなされたもので、熱交^^と化学反 応器が一体化した、コンパクトで熱回収率が高ぐさらに圧力損失が低い熱交浦能 を備えた反応器を提供することを目的とする。 [0006] The present invention has been made in view of such a situation of the prior art, and is a compact heat exchanger in which a heat exchanger ^^ and a chemical reactor are integrated, has a high heat recovery rate, and further has a low pressure loss. The purpose is to provide a reactor equipped with Koura Noh.
課題を解決するための手段  Means for solving the problem
[0007] 本発明によれば、下記(1)一(5)の反応器が提供される。 According to the present invention, the following reactor (1)-(5) is provided.
(1)伝熱面によって隔てられた 2つの流路を有する 2流体向流型の熱交換器構造か らなる反応器であって、熱交換が行われる流路の少なくとも一部分に化学反応を促 進するための加熱手段を設けたことを特徴とする反応器。  (1) A reactor having a two-fluid countercurrent type heat exchanger structure having two flow paths separated by a heat transfer surface, wherein a chemical reaction is promoted in at least a part of the flow path where heat exchange is performed. A reactor provided with a heating means for moving the reactor.
(2)前記加熱手段が触媒層であることを特徴とする前記(1)に記載の反応器。  (2) The reactor according to (1), wherein the heating means is a catalyst layer.
(3) 1つの流体を 2分割した後、互いに向流させるものであることを特徴とする前記(1 )又は(2)に記載の反応器。 (4)前記熱交換器構造における伝熱面を構成する伝熱体が波形であり、かつ 2流体 を、主として該伝熱体の波形部分の一方およびその裏側の空隙部を波形の稜線方 向および Zまたは谷線方向に沿って向流させるものであることを特徴とする前記(1) 一 (3)の 、ずれかに記載の反応器。 (3) The reactor according to the above (1) or (2), wherein one fluid is divided into two and then flows countercurrent to each other. (4) In the heat exchanger structure, the heat transfer body constituting the heat transfer surface is corrugated, and the two fluids are mainly filled in one of the corrugated portions of the heat transfer body and the gap on the back side thereof in the direction of the corrugated ridge. The reactor according to any one of (1) to (3), wherein the reactor is caused to flow countercurrently along the Z or valley direction.
(5) 2流体の各流路内に、流線方向において加熱手段と、該加熱手段と同位置およ び/または近傍に燃焼性微粒子を補足するフィルターとを配置したことを特徴とする 前記(1)一(4)の 、ずれかに記載の反応器。  (5) In each flow path of the two fluids, a heating means in a streamline direction, and a filter for capturing combustible fine particles at the same position and / or in the vicinity of the heating means are arranged. (1) The reactor described in (4) above.
発明の効果  The invention's effect
[0008] 本発明によれば、化学反応によって発生する熱及び化学反応を継続するために加 える熱を、排出される流体力 回収して、化学反応が起こる主要部分に再供給するも のであるから、補助加熱の少ない、あるいはこれを全く必要としない省エネルギー性 の高い反応器が提供される。  [0008] According to the present invention, the heat generated by the chemical reaction and the heat added to continue the chemical reaction are recovered by the discharged fluid power, and re-supplied to the main part where the chemical reaction occurs. Thus, a highly energy-saving reactor with little or no auxiliary heating is provided.
本発明の反応器は、従来の連続した 1流路のみ力 なる自己熱交換型の反応器と 比べて、熱交換機能を持つ部分の流量および流路長を共に半分に短縮できるので 、圧力損失を著しく小さくすることができ、この点においても圧送に必要なエネルギー を節約できる。  Since the reactor of the present invention can reduce both the flow rate and the flow path length of the portion having the heat exchange function by half compared with the conventional self-heat exchange type reactor in which only one continuous flow path is used, pressure loss is reduced. Can be significantly reduced, and the energy required for pumping can be saved in this respect as well.
また、本発明の反応器は、流体が反応器内の熱交換機能を持つ構造体の内部で 自然に 2分割される従来の自己熱交換型の反応器と比べて、主反応領域における温 度の不均等化が生じ難ぐまた、放熱による熱損失も少なくすることができる。  In addition, the reactor of the present invention has a higher temperature in the main reaction region than a conventional self-heat exchange type reactor in which a fluid is naturally divided into two inside a structure having a heat exchange function in the reactor. Is less likely to be uneven, and heat loss due to heat radiation can be reduced.
本発明の反応器は、省エネルギー性の高い、脱臭装置や自動車排ガスコンバータ 一等の低濃度有機成分処理装置、あるいはディーゼルエンジン力 排出される粒子 状物質を捕捉'除去する粒子状物質減少装置 (DPF)等の用途に好適に用いられる 図面の簡単な説明  The reactor of the present invention is a low-concentration organic component treatment device such as a deodorizing device or an automobile exhaust gas converter with high energy efficiency, or a particulate matter reduction device (DPF) that captures and removes particulate matter discharged from a diesel engine. Brief description of drawings that are preferably used for applications such as
[0009] [図 1]図 1は、従来公知の一端に流路反転部を有する自己熱交換型の反応器の概略 構成図である。  FIG. 1 is a schematic configuration diagram of a conventionally known self-heat exchange type reactor having a flow path reversing part at one end.
[図 2]図 2は、従来公知の両端部に流路反転部を持つ自己熱交換型の反応器の概 略構成図である。 [図 3]図 3は、本発明の反応器の基本構成図であり、 2流体向流型熱交換機能を備え た反応器の主要部断面図である。 図 3 (a)は、触媒反応を加熱手段とするものを示 す。 図 3 (b)は、電熱ヒータを加熱手段とするものを示す。 [FIG. 2] FIG. 2 is a schematic configuration diagram of a conventionally known self-heat exchange type reactor having flow passage reversing portions at both ends. FIG. 3 is a basic configuration diagram of the reactor of the present invention, and is a cross-sectional view of a main part of a reactor having a two-fluid countercurrent heat exchange function. FIG. 3 (a) shows an example in which a catalytic reaction is used as a heating means. FIG. 3 (b) shows a case where an electric heater is used as a heating means.
[図 4]図 4は、本発明の他の反応器の構成図であり、実質的に同等な流体を互いに 向流させる導入経路を付加した 2流体向流型熱交換機能を備えた反応器の主要部 断面図である。 図 4 (a)は、 1つの流体を 2分割した後導入するものを示す。 図 4 (b )は、多気筒エンジンにおいて半数の気筒ずっ排ガスをまとめて導入するものを示す  [FIG. 4] FIG. 4 is a configuration diagram of another reactor of the present invention, and has a two-fluid countercurrent type heat exchange function to which an introduction path for causing substantially equivalent fluids to flow in opposite directions is added. It is principal part sectional drawing of. FIG. 4 (a) shows one fluid to be introduced after being divided into two. Fig. 4 (b) shows a multi-cylinder engine in which half of the cylinder exhaust gas is introduced collectively.
[図 5]本発明のさらに他の反応器の構成図であり、波形伝熱体を用いた 2流体向流型 熱交換構造を持つ反応器の主要部斜透視図である。 図 5 (a)は、波形伝熱体とこ れに設置した触媒層を示すものである。 図 5 (b)は、図 5 (a)の構造体を収納した反 応器主要部と流体の流路を示すものである。 FIG. 5 is a configuration diagram of still another reactor of the present invention, and is an oblique perspective view of a main part of a reactor having a two-fluid countercurrent heat exchange structure using a corrugated heat transfer body. FIG. 5 (a) shows a corrugated heat transfer body and a catalyst layer installed thereon. FIG. 5 (b) shows the main part of the reactor containing the structure of FIG. 5 (a) and the fluid flow path.
[図 6]本発明のさらに他の反応器の構成図であり、フィルター材と組み合わせた波形 伝熱体を用いた粒子状物質減少機能を具備する 2流体向流型熱交換構造を持つ反 応器の主要部断面図である。 図 6 (a)は、波形伝熱体空隙部の一部をフィルター材 で充填したものを示す。 図 6 (b)は、平板型フィルター材を 2枚のスぺーサ一で挟み 幾何学的ろ過面積を大きくしたものを示す。 図 6 (c)は、平板型フィルター材と流体 流れをフィルタ一面方向に衝突させる形態を持つスぺーサーを組み合わせたものを 示す。  FIG. 6 is a configuration diagram of still another reactor of the present invention, which has a two-fluid countercurrent heat exchange structure having a particulate matter reduction function using a corrugated heat transfer material combined with a filter material. It is principal part sectional drawing of a vessel. FIG. 6 (a) shows a case where a part of the gap of the corrugated heat transfer material is filled with a filter material. Fig. 6 (b) shows a flat filter material sandwiched between two spacers to increase the geometric filtration area. FIG. 6 (c) shows a combination of a flat filter material and a spacer having a form in which a fluid flow collides in one direction of the filter.
符号の説明 Explanation of symbols
1 容器  1 container
2、 2,、 2" 流体入口  2, 2, 2, 2 "fluid inlet
3、 3,、 3" 流体出口  3, 3, 3 ”fluid outlet
4、 4, 流体反転部  4, 4, fluid reversal part
5 触媒層  5 Catalyst layer
6 触媒を担持した伝熱体隔壁  6 Heat transfer partition supporting catalyst
7 電熱ヒータおよびその電源  7 Electric heater and its power supply
8 三方ジョイント 9 流量調節バルブ 8 Three-way joint 9 Flow control valve
10 エンジン  10 Engine
11 波形伝熱体  11 Corrugated heat transfer
12 波形伝熱体を収納した容器の正面  12 The front of the container containing the corrugated heat transfer
13 波形伝熱体を収納した容器の背面  13 The back of the container containing the corrugated heat conductor
14 フイノレター  14 Huino Letter
15 平板型フィルター材  15 Flat filter material
16 スぺーサー  16 Spacer
17 流体流れを曲げる機能を持つスぺーサ  17 Spacer with function to bend fluid flow
発明を実施するための最良の形態  BEST MODE FOR CARRYING OUT THE INVENTION
[0011] 以下、本発明における熱交換機能を備えた反応器について、幾つかの実施の形態 を図面を参照して詳細に説明するが、本発明は、これらの実施の形態に限定される ものではなぐ本発明の要旨を包含する限り様々な変更が可能である。  [0011] Hereinafter, several embodiments of a reactor having a heat exchange function according to the present invention will be described in detail with reference to the drawings, but the present invention is not limited to these embodiments. Various changes are possible as long as the gist of the present invention is included.
[0012] (第 1の実施の形態)  (First Embodiment)
図 3は、本発明の第 1の形態に係る 2流体向流型熱交換器機能を備えた反応器の 主要部の断面概略図である。  FIG. 3 is a schematic sectional view of a main part of a reactor having a two-fluid countercurrent heat exchanger function according to the first embodiment of the present invention.
図 3 (a)は、多管円筒型熱交換器構造をベースとした本発明の反応器の一例であり、 入口 2と出口 3は、それぞれ反応容器 1の内部をこの図で左から右へと流れる反応成 分を含む第 1流体の入口および出口である。一方、入口 2'と出口 3 'は、第 1流体の 流路と伝熱面で隔てられ、さらに容器 1の内部をこの図で右力 左へと流れる第 2流 体の出入口である。 5は、第 1流体の流路中央付近の一部分に設けた触媒層であり、 該触媒層を本発明における反応器の加熱手段とした例である。  FIG. 3 (a) shows an example of the reactor of the present invention based on the multi-tube cylindrical heat exchanger structure. The inlet 2 and the outlet 3 respectively show the inside of the reaction vessel 1 from left to right in this figure. And the inlet and outlet of the first fluid containing the reaction component flowing therethrough. On the other hand, the inlet 2 ′ and the outlet 3 ′ are separated from the flow path of the first fluid by the heat transfer surface, and are the entrances and exits of the second fluid flowing inside the vessel 1 to the right and left in this figure. Reference numeral 5 denotes a catalyst layer provided in a portion near the center of the flow path of the first fluid, and is an example in which the catalyst layer is used as heating means for the reactor in the present invention.
[0013] 次に、この装置の作用を説明する。炭化水素と空気の混合物など、触媒層 5によつ て発熱反応を起こしうる組成の第 1流体が、流体入口 2より容器 1に入り右方向へ流 れる。流路途中の触媒層 5において、該反応が引き起こされる結果、この部分で熱が 発生し、これによつて触媒層 5および第 1流体が加熱される。この加熱された第 1流体 が触媒層 5から流体出口 3へと流れる間(図中の区間 R)、第 1流体力 伝熱面、さら に伝熱面から第 2流体への熱伝導によって、第 1流体が冷却される一方、これと向流 する第 2流体は加熱される。次いで、前記区間で加熱された第 2流体が触媒層 5から 流体出口 3'の間(図中の区間 L)を流れる場合、第 2流体の方が伝熱面で隔てられ た第 1流体より高温になっている。このため、第 2流体から第 1流体へ熱移動すること により、第 2流体が冷却される一方、第 1流体が加熱される。以上の熱移動様態により 、本来、第 1流体とともに外部へと排出されてしまう反応熱が容器 1の内部へと回収さ れ、その結果として、一方的なプラグフロー型反応器と比べて、触媒層 5の温度を反 応熱により高く保つことができる反応器となる。 Next, the operation of this device will be described. A first fluid, such as a mixture of hydrocarbon and air, having a composition capable of causing an exothermic reaction by the catalyst layer 5 enters the container 1 from the fluid inlet 2 and flows to the right. As a result of the reaction being caused in the catalyst layer 5 in the middle of the flow path, heat is generated in this portion, whereby the catalyst layer 5 and the first fluid are heated. While this heated first fluid flows from the catalyst layer 5 to the fluid outlet 3 (section R in the figure), the first fluid force heat transfer surface, and furthermore, the heat transfer from the heat transfer surface to the second fluid, While the first fluid cools, it flows countercurrently The second fluid is heated. Next, when the second fluid heated in the section flows between the catalyst layer 5 and the fluid outlet 3 ′ (section L in the drawing), the second fluid is more than the first fluid separated by the heat transfer surface. It is hot. Therefore, heat transfer from the second fluid to the first fluid cools the second fluid while heating the first fluid. According to the above-described heat transfer mode, the heat of reaction, which is originally discharged to the outside together with the first fluid, is recovered inside the container 1, and as a result, the catalyst becomes more in comparison with the one-sided plug flow type reactor. The reactor can keep the temperature of the layer 5 high by the reaction heat.
[0014] 触媒層 5に用いる触媒の種類は、流体中に含まれる反応成分によって適宜決める ものであり、糸且成が限定されるものではない。例えば、反応成分が炭化水素と空気中 の酸素である場合は、 Pt、 Pd、 Rh、 Irなどの貴金属微粒子をアルミナまたはゼォライ トなどの高表面積材料に微粒子の形で担持した触媒や、 MnO、 Co O、 NiO、 Cu [0014] The type of catalyst used in the catalyst layer 5 is appropriately determined depending on the reaction components contained in the fluid, and the type of the catalyst is not limited. For example, when the reaction components are hydrocarbons and oxygen in the air, catalysts in which noble metal fine particles such as Pt, Pd, Rh, and Ir are supported in the form of fine particles on a high surface area material such as alumina or zeolite, MnO, Co O, NiO, Cu
2 3 4  2 3 4
oなどの金属酸化物やその複合酸化物など、酸化触媒活性の高いものを使用するこ とが好ましい。  It is preferable to use an oxide having high oxidation catalytic activity, such as a metal oxide such as o and a composite oxide thereof.
[0015] 流線方向における触媒層 5の位置は、熱回収率を最大化して触媒層 5における温 度を最高にするためには向流の中央付近とすることが最も効果的であるが、中央部 力もずらして配置してもよい。触媒層 5の流路方向厚さについては、熱回収率を向上 させるためには短!、ほど望ま 、が、反応率を向上させるためには長!、ほど望ま ヽ ので、必要とする総合性能に応じて両条件の兼ね合いから決定すればよい。また、 触媒層 5は、この形態では流路内に充填する様態としてあるが、伝熱面にコーティン グしてもよい。さらに、本形態では第 1流体のみが反応成分を含み、第 1流体流路の 一部分のみに触媒層を配置したものであるが、第 1流体とともに第 2流体も同様の、 あるいは異なる反応成分を含み、その反応を促進する触媒層を第 2流体流路の一部 分に配置してもよい。この場合、両触媒層とも中央部に配置することが最も効果的で あるが、流線方向において意図的に個別にずらして配置してもよい。また、熱交 構造としてここでは多管円筒型を用いた力 プレートフィン型やうずまき型など、向流 が可能な他の形態でもよ 、。  [0015] In order to maximize the heat recovery rate and maximize the temperature in the catalyst layer 5, the position of the catalyst layer 5 in the streamline direction is most effectively located near the center of the countercurrent. The central force may also be shifted. The thickness of the catalyst layer 5 in the flow channel direction is short in order to improve the heat recovery rate, and is more desirable, but long in order to improve the reaction rate, and is more desirable. May be determined based on a balance between the two conditions. In this embodiment, the catalyst layer 5 is filled in the flow channel, but may be coated on the heat transfer surface. Further, in the present embodiment, only the first fluid contains a reaction component, and the catalyst layer is disposed only in a part of the first fluid flow path. However, the same or different reaction components are also contained in the second fluid together with the first fluid. A catalyst layer that contains and promotes the reaction may be disposed in a part of the second fluid flow path. In this case, it is most effective to arrange both catalyst layers at the center, but they may be intentionally shifted individually in the streamline direction. In addition, other forms capable of countercurrent flow, such as a force plate fin type using a multi-tube cylindrical type or a vortex type, may be used as the heat exchange structure.
[0016] 図 3 (b)は、加熱手段として前記のような触媒反応を用いることなぐ流路内に設置 した電熱ヒータ 7を用いたものである。電熱ヒータ 7による加熱と熱回収作用により、電 熱ヒータ 7を設置した部分の温度を効果的に高くでき、これによつて熱反応を進行さ せる反応器となる。本形態では、第 1流体の流路内のみに電熱ヒータ 7を配置したが 、同様に第 2流体の一部分にも配置してもよい。この場合も電熱ヒータは流線方向に 対して中央付近に配置することが熱回収率を最大化する上で最も効果的であるが、 意図的に中央部力もずらして配置してもよい。また、電熱ヒータだけでなぐマイクロ 波、電磁誘導加熱をはじめとするその他の物理的加熱手段を用いることも可能である さらに、以上のような触媒反応と物理的加熱手段を組み合わせて使用してもよい。 FIG. 3 (b) shows the use of an electric heater 7 installed in a flow path without using the above-described catalytic reaction as a heating means. The heating by the electric heater 7 and the heat recovery The temperature of the portion where the thermal heater 7 is installed can be effectively raised, thereby providing a reactor for promoting the thermal reaction. In the present embodiment, the electric heater 7 is arranged only in the flow path of the first fluid, but may be arranged in a part of the second fluid in the same manner. In this case as well, it is most effective to arrange the electric heater in the vicinity of the center in the streamline direction in order to maximize the heat recovery rate. It is also possible to use other physical heating means such as microwaves, electromagnetic induction heating, etc., which can be used only with an electric heater. Good.
[0017] (第 2の実施の形態) (Second Embodiment)
図 4は、本発明における他の形態の反応器の断面概略図である。  FIG. 4 is a schematic cross-sectional view of a reactor according to another embodiment of the present invention.
この形態の反応器は、もともと一つの、あるいは、実質的に同等の流体を 2分割して 向流する第 1および第 2流体としたものである。すなわち、図 4 (a)では、流体入口 2か ら入った反応流体を三方ジョイント 8の部分で 2分割した後、容器 1の 2つの流体入口 2'および 2"に導く配管構造が備えられている。また、触媒層 5が熱交換構造内の第 1、第 2流体の両流路途中に配置されている。これにより、第 1の実施の形態で説明し たのと同様の熱回収機構により触媒層 5付近における温度を高くすることが可能にな る。  The reactor of this form is originally a single or substantially equivalent fluid divided into two, and used as first and second fluids which flow countercurrently. That is, in FIG. 4 (a), a piping structure is provided in which the reaction fluid entering from the fluid inlet 2 is divided into two at the three-way joint 8 and then guided to the two fluid inlets 2 ′ and 2 ″ of the container 1. In addition, the catalyst layer 5 is disposed in the middle of both flow paths of the first and second fluids in the heat exchange structure, whereby a heat recovery mechanism similar to that described in the first embodiment is provided. Thereby, the temperature near the catalyst layer 5 can be increased.
この構造は、流体が反応器内の熱交擁能を持つ構造体の内部で自然に 2分割 される従来の自己熱交換型の反応器と比べ、温度が極大値となる主反応領域が両 流路で共通な 1箇所となるため、両流路間で温度が不均等化することが少ない。また 、温度の極大値が反応器中央部の 1箇所に限定され、保温手段を講ずることも容易 であるため、放熱による熱損失をより小さくすることができる。なお、本発明では、図 4 (a)に示したように、三方ジョイント 8で分割した流路の一方あるいは両方の途中に流 量調節バルブ 9を適宜設けて、流体入口 2'と 2"から入る反応流体の分配比を等分 あるいは他の意図する割合に設定してもよ 、。  This structure has two main reaction areas where the temperature reaches a local maximum, compared to a conventional self-heat exchange type reactor in which the fluid naturally divides into two inside the structure having heat exchange capability inside the reactor. Since it is a common location in the flow path, the temperature is less likely to be uneven between the two flow paths. Further, since the maximum value of the temperature is limited to one location in the center of the reactor and it is easy to take a heat retaining means, the heat loss due to heat radiation can be further reduced. In the present invention, as shown in FIG. 4 (a), a flow rate control valve 9 is appropriately provided in one or both of the flow paths divided by the three-way joint 8, so that the fluid inlets 2 'and 2 " The distribution ratio of the input reaction fluid may be set to be equal or another intended ratio.
[0018] 図 4 (b)は、反応流体が偶数個の気筒を持つエンジン 10の排ガスであり、半数の気 筒からの排ガスを第 1流体、残りの半数の気筒からの排ガスを第 2流体として互いに 向流させる配管構造を備えたものである。図 4 (a)の場合と同じぐ両流体の流路途 中に触媒層 5を設けている。このようにすることにより、流量調節バルブ 9のような分配 比を調節する機構がなくても組成および流量がほぼ等しい第 1および第 2流体を互 いに向流させて反応器に導入することができる。その結果、 2分割された排ガスの上 流 下流間で互いに熱回収が実現され、反応器中央部分の温度を高くすることがで きる。 FIG. 4 (b) shows the exhaust gas of the engine 10 in which the reaction fluid has an even number of cylinders. The exhaust gas from half the cylinders is the first fluid, and the exhaust gas from the remaining half cylinders is the second fluid. It is equipped with a piping structure for flowing countercurrent to each other. The flow path of both fluids is the same as in Fig. 4 (a). The catalyst layer 5 is provided inside. By doing so, the first and second fluids having substantially the same composition and flow rate can be introduced into the reactor in countercurrent to each other without a mechanism for adjusting the distribution ratio such as the flow rate control valve 9. Can be. As a result, heat is mutually recovered between the upstream and downstream of the two divided exhaust gases, and the temperature of the central portion of the reactor can be increased.
このように、この構造によれば、流体が反応器内の熱交 能を持つ構造体の内 部で自然に 2分割される従来の自己熱交換型の反応器と異なり、反応器内の 2つの 流路間で流量が不均等化することによる熱回収率低下のおそれが全くないので、想 定し得る最高性能に近い性能を発揮することができる。  Thus, according to this structure, unlike the conventional self-heat exchange type reactor in which the fluid is naturally divided into two inside the structure having heat exchange in the reactor, the fluid in the reactor is Since there is no danger of a decrease in the heat recovery rate due to uneven flow rates between the two flow paths, it is possible to exhibit performance close to the maximum performance that can be expected.
[0019] (第 3の実施の形態) (Third Embodiment)
図 5は、本発明における他の形態の反応器を斜透視図で示したものである。  FIG. 5 is a perspective view showing another embodiment of the reactor according to the present invention.
図 5 (a)は、耐熱性を有するステンレス板などの長方形の伝熱体を波形に成形し、 さらにその長手方向の中央部付近に触媒層 5を配置したものである。波形の隣り合う 平面部分は、一定の間隔で互いに平行になるように成形することが最も望ましい。こ のようにするために、波形の空隙部全体あるいは一部にステンレス金網などの耐熱 性と通気性を有する材料をスぺーサ一として挟んでもよい。図 5 (b)は、この触媒層 5 を備えた波形伝熱体 11を、直方体の容器 1に収納したものである。容器 1は、図 5 (b )の上面の長手方向両端部近くに第 1流体の入口 2'と出口 3'力設けられ、下面にも 該出口 3'、入口 2'の裏側にそれぞれ、第 2流体の入口 2"および出口 3"が設けられ ている。また、図 5 (b)の正面および背面では容器 1と波形伝熱体 11のすき間は適当 なシール材により密封されて 、る。  FIG. 5 (a) shows a rectangular heat conductor such as a stainless steel plate having heat resistance formed into a corrugated shape, and a catalyst layer 5 disposed near the center in the longitudinal direction. Most desirably, adjacent flat portions of the corrugations are formed so as to be parallel to each other at regular intervals. In order to achieve this, a material having heat resistance and air permeability, such as stainless steel wire mesh, may be interposed as a spacer in the whole or a part of the corrugated space. FIG. 5 (b) shows a case where the corrugated heat transfer body 11 having the catalyst layer 5 is housed in a rectangular parallelepiped container 1. The container 1 is provided with a first fluid inlet 2 'and an outlet 3' force near both ends in the longitudinal direction of the upper surface in FIG. 5 (b), and a lower surface is provided on the lower surface behind the outlet 3 'and the inlet 2', respectively. Two fluid inlets 2 "and outlets 3" are provided. On the front and back surfaces of FIG. 5B, the gap between the container 1 and the corrugated heat transfer body 11 is sealed with a suitable sealing material.
[0020] 次に、この形態の反応器の作用を説明する。それぞれ流体入口 2'および 2"から入 つた第 1および第 2流体は、波形伝熱体 11を挟んで波形の一方の面の空隙部と反対 面の空隙部を波形の稜線 (あるいは谷線)方向に沿って互 、に向流し、熱交換を行う 。触媒層 5の作用で発熱反応を起こす成分が両流体中に含まれている場合、流体入 口 2' (および流体出口 3")から触媒層 5の区間では、第 2流体(図中の斜線矢印)か ら第 1流体 (黒矢印)へと熱移動が起こり、触媒層 5から流体出口 3' (および流体入口 2")の区間では、逆に第 1流体力 第 2流体へと熱移動が起こる。すなわち、両部分 とも、すでに触媒層 5を通過して反応が終わった流体力 触媒層 5へ流入しょうとする 流体へと熱が移動する。その結果、両流体とも予熱されることにより触媒層 5における 温度を高く保ち、反応を円滑に進行させることができる。本形態では加熱手段として 触媒反応を用いたが、前記形態 1と同様に、第 1および第 2両流体、あるいはいずれ かの流体の流路内に電熱ヒータあるいはその他の物理的加熱手段を配置して、熱反 応器としてもよ!/ヽし、触媒反応と物理的加熱手段を兼ね備えてもよ!ヽ。 Next, the operation of the reactor of this embodiment will be described. The first and second fluids entering from the fluid inlets 2 'and 2 "respectively form the ridges (or valleys) of the waveform in the voids on one side of the waveform and the opposite side across the waveform heat transfer body 11 In the case where both fluids contain a component that causes an exothermic reaction due to the action of the catalyst layer 5, the fluid flows from the fluid inlet 2 '(and the fluid outlet 3 "). In the section of the catalyst layer 5, heat transfer occurs from the second fluid (the hatched arrow in the figure) to the first fluid (black arrow), and the section from the catalyst layer 5 to the fluid outlet 3 '(and the fluid inlet 2 "). In the reverse, heat transfer occurs to the first fluid force and the second fluid, ie, both parts At the same time, the fluid force that has already passed through the catalyst layer 5 and reacted has transferred heat to the fluid that is about to flow into the catalyst layer 5. As a result, by preheating both fluids, the temperature in the catalyst layer 5 can be kept high, and the reaction can proceed smoothly. In this embodiment, a catalytic reaction was used as the heating means, but an electric heater or other physical heating means was arranged in the flow path of the first and second fluids or any of the fluids as in the first embodiment. It may also be used as a thermal reactor! / It may also have both catalytic reaction and physical heating means!
[0021] (第 4の実施の形態) (Fourth Embodiment)
図 6は、本発明における他の形態の反応器を、波形伝熱体 11の平面部分に垂直 な断面図で示したものである。  FIG. 6 is a cross-sectional view of a reactor according to another embodiment of the present invention, which is perpendicular to a plane portion of the corrugated heat transfer body 11.
図 6 (a)は、気体中に浮遊する燃焼性微粒子を捕捉することが可能なフィルター 14 を、波形伝熱体 11の中央付近の空隙部に充填したものである。図示していないが、 このフィルター 14には、流体に含まれる反応成分を反応させて発熱を促す作用を持 つ触媒を担持するか、フィルターを配置したのと同じ区間において、波形伝熱体 11 の両面に同様の触媒を担持する力 ある 、はフィルターを直接加熱することができる 電熱ヒータ等の物理的加熱手段を配置する。  FIG. 6 (a) shows a filter in which a combustible fine particle floating in a gas can be captured in a space near the center of the corrugated heat transfer body 11. FIG. Although not shown, the filter 14 carries a catalyst having a function of promoting the heat generation by reacting the reaction components contained in the fluid, or in the same section where the filter is disposed, the corrugated heat transfer material 11 A physical heating means such as an electric heater capable of directly heating the filter is disposed on both sides of the filter.
[0022] 例えば、ディーゼルエンジン排ガスなどの炭素微粒子 (燃焼性微粒子の一例である )を含む気体をこの反応器の両流体入口 2'、 2"から導入すると、炭素微粒子がフィ ルター 14で捕捉される。酸素が含まれる処理気体にプロパンやエチレンなどの炭化 水素や Hをあら力じめ添加して触媒を作用させる力、あるいは電熱ヒータを用いるこ  [0022] For example, when a gas containing carbon fine particles (an example of combustible fine particles) such as diesel engine exhaust gas is introduced from both fluid inlets 2 'and 2 "of the reactor, the carbon fine particles are captured by the filter 14. It is necessary to add a hydrocarbon such as propane or ethylene or H to the process gas containing oxygen to make the catalyst work, or use an electric heater.
2  2
とによりフィルター 14を加熱すると、発生する熱およびこの反応器内での熱回収作用 により、フィルター 14の温度を容易に高温にすることができる。これにより、炭素微粒 子が酸化除去され、フィルター機能を維持することができる。  When the filter 14 is heated by the above, the temperature of the filter 14 can be easily raised by the generated heat and the heat recovery action in the reactor. Thereby, the carbon fine particles are oxidized and removed, and the filter function can be maintained.
[0023] 図 6 (a)の形態では、フィルター 14は単に流路の一部に充填するのみであるが、図 6 (b)のようにしてもよい。すなわち、耐熱性と通気性を有するステンレス金網等のス ぺーサ一 16で柔軟性を持つ平板型フィルター材 15を挟んだ後、波形伝熱体 11の 各空隙部に収納する。平板型フィルター材 15の下流側端部は、上流側に配置したス ぺーサ一 16よりも波形の長手方向に長ぐ平板型フィルター材 15の上流側端部は 下流側に配置したスぺーサー 16よりも長くして、平板型フィルター材 15の上流端部 と下流端部を空隙の両側の伝熱体面に互い違いに密着させる。このような構造を採 ることにより、各フィルター材の平板面を通過するような流路が形成され、図 6 (a)と比 ベて幾何学的なろ過面積を増カロさせ、ひいては、フィルターによる圧力損失を小さく することができる。なおスぺーサー 16は、触媒の支持構造体、あるいは電熱ヒータと しての機能を兼ね備えてもよ 、。 In the form of FIG. 6 (a), the filter 14 simply fills a part of the flow path, but may be as shown in FIG. 6 (b). That is, after a flexible flat filter material 15 is sandwiched between spacers 16 such as a stainless steel wire mesh having heat resistance and air permeability, it is stored in each gap of the corrugated heat transfer body 11. The downstream end of the flat filter material 15 is longer than the spacer 16 arranged on the upstream side in the longitudinal direction of the waveform, and the upstream end of the flat filter material 15 is arranged on the downstream side. Upstream end of flat filter material 15 longer than 16 And the downstream end are alternately brought into close contact with the heat transfer member surfaces on both sides of the gap. By adopting such a structure, a flow path that passes through the flat surface of each filter material is formed, increasing the geometrical filtration area as compared with Fig. 6 (a), and consequently the filter Pressure loss can be reduced. The spacer 16 may also have a function as a catalyst support structure or an electric heater.
[0024] さらに、図 6 (c)のように、 2つの平板型フィルター材 15の間に、流体の流れをフィル ター面に衝突させる方向に曲げる周期構造を有する耐熱性と通気性のあるスぺーサ 一 17を挟んで使用してもよい。このようなスぺーサ一としては、平織型ステンレス金網 や、多数の小穴を持つ波形の金属板などを用いる。このような構造とすることにより、 フィルタ一面への流体の衝突により燃焼性微粒子が捕捉される一方、フィルターの中 を流体が貫通する図 6 (a)の場合と比べて圧力損失を下げることができる。なお、この 場合も、フィルター材 15やそれに接する伝熱体表面、あるいは流体流れを曲げる機 能を持つスぺーサー 17表面に触媒を担持したり、流体の流れを曲げる機能を持つス ぺーサ一 17が電熱ヒータを兼用するなどして加熱手段としてもよ!/、。 Further, as shown in FIG. 6 (c), a heat-resistant and air-permeable switch having a periodic structure between the two flat filter members 15 that bends the flow of the fluid in the direction of colliding with the filter surface. It may be used with a spacer 17 in between. As such a spacer, a plain-woven stainless steel wire mesh, a corrugated metal plate having many small holes, or the like is used. With this structure, the flammable particulates are captured by the collision of the fluid on one surface of the filter, but the pressure loss can be reduced compared to the case of Fig. 6 (a) where the fluid penetrates the filter. it can. Also in this case, the catalyst is supported on the filter material 15, the surface of the heat transfer body in contact with the filter material 15, or the surface of the spacer 17 having a function of bending the fluid flow, or a spacer having a function of bending the fluid flow. 17 can also be used as a heating means by also using an electric heater!
<実施例 >  <Example>
以下、本発明を実施例によりさらに具体的に説明するが、本発明はこれらに実施例 によって何ら限定されるものではな 、。  Hereinafter, the present invention will be described more specifically with reference to examples, but the present invention is not limited to these examples.
実施例 1  Example 1
[0025] 図 4(a)に示すような一つの流体を 2分割させて互いに向流させる配管構造を備える とともに、図 5に示すような波形のステンレス製伝熱体および流路形態を有し、図 6(c) のフィルター材に相当する箇所に酸ィ匕触媒を担持させた耐熱性の繊維片を配置した 熱交換型反応器を作製した。  [0025] As shown in Fig. 4 (a), a fluid is provided with a pipe structure for dividing one fluid into two and flowing in countercurrent to each other, and has a corrugated stainless steel heat transfer body and flow path form as shown in Fig. 5. Then, a heat exchange reactor was prepared in which a heat-resistant fiber piece carrying an oxidation catalyst was disposed at a position corresponding to the filter material in FIG. 6 (c).
すなわち、厚さ 0.03mm、幅 300mm、長さ 1600mm余の帯状ステンレス薄板を長手方向 に対して直角に 40mm間隔で波形に 39回折り曲げた伝熱板を作った。この波形構造 体の一方の面において、波形構造体長手方向の一方の端部から 50— 150mmの箇所 に、白金触媒を担持した厚さ 0.25mm、縦 80mm、横 100mmの 1100°Cの耐熱性を持つ ムライト製平織繊維片 20枚を、伝熱構造体の各波形の山(20個)に被せるようにして 挟んだ。 これと同様に、同組成、同寸法の繊維片 19枚を、波形構造体の反対の面において 、先ほどとは反対の長手方向端部力 50— 150mmの箇所にも挟んだ。使用した白金 触媒は、 γ—アルミナに対し Pt微粒子を 10重量 %担持したものであり、これら各構成品 の総重量は、ムライト製繊維片 97g、 γ—アルミナ 7.2g、 Pt0.72gであった。 In other words, a heat transfer plate was fabricated by bending a strip of stainless steel thin plate having a thickness of 0.03 mm, a width of 300 mm, and a length of more than 1600 mm 39 times at right angles to the longitudinal direction at 40 mm intervals. On one side of this corrugated structure, a 50-150 mm point from one end in the longitudinal direction of the corrugated structure is a platinum catalyst-carrying 0.25 mm thick, 80 mm long and 100 mm wide heat resistant at 1100 ° C. Twenty pieces of plain woven fiber made of mullite having were placed between the corrugated peaks (20 pieces) of the heat transfer structure. Similarly, 19 pieces of fiber having the same composition and the same dimensions were sandwiched on the opposite surface of the corrugated structure at the opposite end force in the longitudinal direction of 50 to 150 mm. The platinum catalyst used supported 10% by weight of Pt fine particles with respect to γ-alumina.The total weight of these components was 97 g of mullite fiber pieces, 7.2 g of γ-alumina, and 0.72 g of Pt. .
[0026] 次に、波形構造体の平らな各面の隙間に、スぺーサ一として繊維片のないところに は線径 0.45mm、 8メッシュのステンレス製平織金網(厚さ約 lmm)を、また繊維片を挟 んであるところには線径 0.25mm、 16メッシュのステンレス製平織金網(厚さ約 0.5mm) を挟んだ。さらに、これらの波形構造体、白金触媒を担持した繊維片、金網スぺーサ 一を、肉厚 0.6mmで直方体(内寸 40mmx47mmx300mm)のステンレス製容器に収納し て熱交換型反応器からなる第 1号反応器とした。 Next, a stainless steel plain weave wire (0.45 mm in wire diameter, 8 mesh) (thickness: about lmm) was placed between the flat surfaces of the corrugated structure in places where there was no fiber piece as a spacer. In addition, a stainless steel plain woven wire mesh with a wire diameter of 0.25 mm and 16 mesh (thickness of about 0.5 mm) was sandwiched between the fiber pieces. Further, the corrugated structure, the fiber piece supporting the platinum catalyst, and the wire mesh spacer are housed in a stainless steel container having a thickness of 0.6 mm and a rectangular parallelepiped (inner size of 40 mm x 47 mm x 300 mm), and a heat exchange type reactor is used. This was the No. 1 reactor.
なお、当該反応器には、図 5に示すように長手方向の両端力 約 20mmのところ 4力 所に 10x47mmの長方形開口部を設け、これら各開口部に直径 19mmの円管を側面を 部分的に切り落とした形にして、被せるように取り付けることにより、流体の出入口とし た。  As shown in Fig. 5, the reactor was provided with rectangular openings of 10x47mm at four points where the longitudinal force at both ends was about 20mm, and a circular pipe with a diameter of 19mm was partially formed in each of these openings. It was cut into a shape and attached so that it could be covered, thereby providing a fluid entrance and exit.
この第 1号反応器を用いて、触媒を担持した繊維片が挟まれて ヽる箇所 (触媒層) が反応器の長手方向中央部よりも出口側に近くなるような流れ方向とし、濃度 0.02— 0.13%のエチレンを含む模擬汚染空気を流速 30— 180L/minで流した場合のェチレ ン除去率や熱回収性能などを調べた。得られた結果を表 1に示す。  Using the first reactor, the flow direction was such that the portion (catalyst layer) between the fiber pieces supporting the catalyst was closer to the outlet side than the center in the longitudinal direction of the reactor. — Ethylene removal rate and heat recovery performance were investigated when simulated contaminated air containing 0.13% ethylene was flowed at a flow rate of 30-180 L / min. Table 1 shows the obtained results.
[0027] [表 1] [Table 1]
処理空気 エチレン理論上昇入口温度出口温度 中央部 エチレン 熱回収率 圧力損失 流暈/し 1 /% 温度 */°c /°c /°c 温度 / 除去率 /% / /mmAqProcessed air Ethylene theoretical rise inlet temperature Outlet temperature Central part Ethylene heat recovery rate Pressure loss Runoff 1 /% Temperature * / ° c / ° c / ° c Temperature / removal rate /% / / mmAq
30 0.207 1 14 24 54 346 99.6 65 2830 0.207 1 14 24 54 346 99.6 65 28
30 0.153 84 24 58 323 99.7 72 2730 0.153 84 24 58 323 99.7 72 27
30 0.099 55 25 59 280 99.6 78 2530 0.099 55 25 59 280 99.6 78 25
30 0.077 42 25 55 214 99.3 78 2330 0.077 42 25 55 214 99.3 78 23
30 0.056 31 25 51 204 98.8 83 2130 0.056 31 25 51 204 98.8 83 21
30 0.045 24 25 47 169 97 83 1930 0.045 24 25 47 169 97 83 19
61 0.098 53 24 48 245 97 76 5361 0.098 53 24 48 245 97 76 53
61 0.078 42 24 49 224 97 79 5161 0.078 42 24 49 224 97 79 51
60 0.056 29 25 46 183 95 82 4760 0.056 29 25 46 183 95 82 47
120 0.096 50 24 54 214 94 74 141120 0.096 50 24 54 214 94 74 141
176 0.127 67 25 68 236 95 68 281176 0.127 67 25 68 236 95 68 281
*当該濃度のエチレンが完全酸化した壜合に発生する熱量から予想される処理空気の上昇温度* Temperature rise of treated air expected from the amount of heat generated in bottles in which ethylene of the relevant concentration has been completely oxidized
** 熱回収率- (中央部温度-入口温度-理論上昇温度)/ (中央部温度-入口温度) *100 これらの反応では、反応開始時以外は外部から加熱することはなぐ当反応器の中 で進行する触媒酸化反応によって発生する反応熱のみで反応層の温度を維持し、 自発的な触媒反応を持続できた。表 1より、流速約30 (空間速度=320011—1)、60 (同 6400h— 、 120 (同 12800h— 、 176L/min (同 18800h— の条件において、エチレン除去 率は、それぞれ最高 99.7、 97、 94、 95%に達していた。 ** Heat recovery rate-(Central part temperature-Inlet temperature-Theoretical rise temperature) / (Central part temperature-Inlet temperature) * 100 In these reactions, the reactor cannot be externally heated except at the start of the reaction. The spontaneous catalytic reaction could be maintained by maintaining the temperature of the reaction layer only by the heat of reaction generated by the catalytic oxidation reaction progressing inside. From Table 1, a flow rate of about 30 (space velocity = 320011- 1), 60 (same 6400H-, 120 (same 12800h-, 176L / min (in terms of the 18800H-, ethylene removal rate, respectively up 99.7, 97, 94, 95%.
また、自発的な触媒燃焼を継続できるエチレン濃度は、それぞれ 0.045、 0.056、 0.096、 0.127%であり、いずれも熱回収機能を持たない通常の触媒層では到底実現 できない低濃度である。また、中央部温度に比べて出口温度は大幅に低ぐ熱が触 媒層の下流から上流へ移動して ヽることが容易に推測される。出口温度と入口温度 の差が理論上昇温度よりも小さいのは、処理された空気とともに排出される分以外に も反応器への熱伝導や反応器周囲の空気への対流による熱損失があるためである。 これらの熱損失を考慮に入れても、それぞれの流速における最高熱回収率は 83、 82 、 74、 68%という高い値に達していた。さらに反応器前後の差圧 (圧力損失)は、流速 30L/minでは 19一 28mmAqと小さく、また流速 176L/minでも 281mmAqに過ぎなかった 実施例 2 The ethylene concentrations at which spontaneous catalytic combustion can be continued are 0.045, 0.056, 0.096, and 0.127%, respectively, all of which are low concentrations that cannot be realized with a normal catalyst layer without a heat recovery function. In addition, the outlet temperature is much lower than the central temperature, and it is easily assumed that heat moves from downstream to upstream of the catalyst layer. The reason why the difference between the outlet temperature and the inlet temperature is smaller than the theoretical rise temperature is that there is heat loss due to heat conduction to the reactor and convection to the air around the reactor other than the amount discharged together with the treated air. It is. Even taking these heat losses into account, the maximum heat recovery at each flow rate reached as high as 83, 82, 74 and 68%. Furthermore, the differential pressure (pressure loss) before and after the reactor was as small as 19-28 mmAq at a flow rate of 30 L / min, and was only 281 mmAq at a flow rate of 176 L / min. Example 2
[0029] 前記の第 1号反応器を用いて、エチレンと同様な流れ方向とし、濃度 0.02— 0.06% のトルエンを含む模擬汚染空気を流速約 60ないし 122L/minで流した場合のトルエン 除去率や熱回収性能などを調べた。得られた結果を表 2に示す。  [0029] Toluene removal rate when simulated contaminated air containing 0.02-0.06% of toluene and flowing at a flow rate of about 60 to 122 L / min using the first reactor in the same flow direction as ethylene. And heat recovery performance. Table 2 shows the obtained results.
[0030] [表 2] 処理空気  [0030] [Table 2] Process air
トルエン 水素 理論上昇 入口温度出口温度 中央部 トルエン 熱回収率" 圧力損失 Toluene hydrogen Theoretical rise Inlet temperature Outlet temperature Central part Toluene Heat recovery rate "Pressure loss
¾m/L-min" ¾m / L-min "
1 A /% 温度 */°c /°c /¾ 温度 /°C 除去率 / / /mmAq 1 A /% temperature * / ° c / ° c / ¾ temperature / ° C removal rate /// mmAq
61 0.060 0.00 45 28 67 395 97 88 8461 0.060 0.00 45 28 67 395 97 88 84
61 0.050 0.00 74 28 64 348 96 77 7861 0.050 0.00 74 28 64 348 96 77 78
121 0.059 0.00 87 27 80 377 96 75 228121 0.059 0.00 87 27 80 377 96 75 228
122 0.060 0.50 137 27 88 496 98 71 267122 0.060 0.50 137 27 88 496 98 71 267
122 0.040 0.50 106 27 77 404 97 72 235122 0.040 0.50 106 27 77 404 97 72 235
122 0.021 0.50 77 27 74 333 96 75 213122 0.021 0.50 77 27 74 333 96 75 213
122 0.020 1.00 127 27 83 464 98 71 256122 0.020 1.00 127 27 83 464 98 71 256
*当該 a度のトルエンおよび水素が完全酸化した場合に発生する熱量から予想される空気の上昇温度 **熱回収率 = (中央部温度-入口温度-理論上界 ;¾度)/ (中央部温度-入口通度): *100 * The temperature rise of air expected from the amount of heat generated when toluene and hydrogen at the relevant a degree are completely oxidized ** Heat recovery rate = (central temperature-inlet temperature-theoretical boundary; ¾degree) / (central temperature (Temperature-inlet conductivity): * 100
[0031] この例では、補助加熱のために処理空気に水素を添加した結果も併せて示した。 In this example, the result of adding hydrogen to the processing air for auxiliary heating is also shown.
水素濃度がゼロの自発触媒酸化の結果から、トルエンについてもエチレンの場合と 同様に、高い除去率、低い自発触媒酸化濃度、高い熱回収率が達成されていること がわかった。さらに流速 122L/minにおいて、水素を 0.5%あるいは 1.0%添カ卩することに より、それぞれ 0.040%、 0.020%という低濃度でもトルエンを 97%以上除去できることを確 した ο  From the results of the spontaneous catalytic oxidation with zero hydrogen concentration, it was found that high removal rate, low spontaneous catalytic oxidation concentration, and high heat recovery were achieved for toluene as well as for ethylene. At a flow rate of 122 L / min, it was confirmed that 97% or more of toluene could be removed at low concentrations of 0.040% and 0.020%, respectively, by adding hydrogen at 0.5% or 1.0%.
実施例 3  Example 3
[0032] 図 6(c)に示す構造の反応器が、ディーゼルエンジン力 排出される粒子状物質( PM)を除去できることを検証するため、第 2号反応器を作製した。この第 2号反応器 の配管構造および反応器本体の構成、形状、寸法は、いずれも第 1号反応器とほぼ 同じである。ただし、波形構造体の両面ともにムライト質繊維片の横寸を 40mm (使用 総重量は 36g)とし、そこに触媒として Pt (総重量 0.36g)および MoO (同 0.36g)を担持  [0032] In order to verify that the reactor having the structure shown in Fig. 6 (c) can remove particulate matter (PM) discharged from the diesel engine, a second reactor was manufactured. The piping structure of this second reactor and the configuration, shape, and dimensions of the reactor body are almost the same as those of the first reactor. However, the width of the mullite fiber pieces on both sides of the corrugated structure was 40 mm (total weight used: 36 g), and Pt (total weight: 0.36 g) and MoO (0.36 g) were supported as catalysts there.
3  Three
し、これを波形構造体の長手方向端部より 130— 170mmの範囲、すなわち反応器中 央部に配置した。また、繊維片のある部分に配置した 16メッシュの各金網には γ—ァ ルミナ担持 Ptをコーティングした(Pt総重量 =0.17g、 γ—アルミナ総重量 =1.7g)。 この第 2号反応器を用いて、排気量 2180ccのディーゼルエンジンを搭載したディー ゼル車をシャーシダイナモメータ上で車速 60km/hに相当する条件で運転した際に発 生する排ガスの一部を導入し、さらに、水素を添加してその触媒燃焼により内部をカロ 熱した場合の PM捕集率や圧力損失の経時変化などを調べた。得られた結果を表 3 に示す。 This was placed in the range of 130 to 170 mm from the longitudinal end of the corrugated structure, that is, in the center of the reactor. In addition, each of the 16-mesh wire meshes arranged in a certain part of the fiber piece has γ- Lumina-supported Pt was coated (total Pt weight = 0.17 g, γ-alumina total weight = 1.7 g). Using this No. 2 reactor, a part of the exhaust gas generated when a diesel vehicle equipped with a 2180 cc diesel engine was driven on a chassis dynamometer at a vehicle speed of 60 km / h was introduced. In addition, the change in PM collection rate and pressure loss over time when hydrogen was added and the inside was heated by catalytic combustion was examined. Table 3 shows the obtained results.
[0033] [表 3] 排ガス流量 水素 理譫上昇 入口温度 出口温度 中央部 PM 熱回収率 圧力損失[Table 3] Exhaust gas flow rate Hydrogen Rise rise Inlet temperature Outlet temperature Center PM heat recovery rate Pressure loss
/L-min / 温度 c ,c /¾ 温度 /°c 除去率 /% /mmAq/ L-min / temperature c, c / ¾ temperature / ° c removal rate /% / mmAq
45 1.00 82 80 133 487 50 80 106 (安定)45 1.00 82 80 133 487 50 80 106 (stable)
45 0.90 74 82 141 493 48 82 108(安定)45 0.90 74 82 141 493 48 82 108 (stable)
45 0.80 66 84 137 456 50 82 110(安定)45 0.80 66 84 137 456 50 82 110 (stable)
45 0.59 49 84 126 380 51 84 1 14(上昇)45 0.59 49 84 126 380 51 84 1 14 (Up)
60 1.1 1 91 92 166 585 46 82 141 (安定)60 1.1 1 91 92 166 585 46 82 141 (stable)
*当 κ¾度の水素が完全酸化した場合に発生する熱量から予想される処理空気の上昇温度 **熱回収率 = (中央部温度-入口温度-理論上昇温度)/ (中央部温度-入口温度): *100 * Temperature rise temperature of process air expected from the amount of heat generated when this κ¾ degree of hydrogen is completely oxidized ** Heat recovery rate = (Central part temperature-Inlet temperature-Theoretical rise temperature) / (Central part temperature-Inlet temperature ): * 100
[0034] なお、 ΡΜ捕集率は、反応器前後の ΡΜ濃度を瞬時微粒子質量計測装置 (ΤΕΟΜ)に より測定した結果力も見積もったものである。第 1号反応器と同程度の高い熱回収率 を持つとともに、 ΡΜを 50%捕捉していることが確認される。また、本装置内部の ΡΜ堆 積状況を示す指標となる圧力損失の経時変化は、排ガス流量 45L/minでは中央部 温度 456°C以上では安定しており、水素濃度を下げて同温度が 380°Cとなって初めて 顕著に上昇傾向を見せた。すなわち、中央部温度を 456°C以上とすれば、 PM酸化が 十分な早さで進行し PM堆積量が増加することがなく、 PMの連続捕集 ·酸化除去が可 能なものと推察される。同様に、排ガス流量 60Lminの場合には、中央部温度を 585°C まで上昇させれば連続捕集 ·酸ィ匕除去が可能であることが確認された。 [0034] The ΡΜ trapping rate is obtained by measuring the 結果 concentration before and after the reactor using an instantaneous fine particle mass measuring device (ΤΕΟΜ) and also estimating the force. It is confirmed that it has the same high heat recovery as the first reactor and captures 50% of ΡΜ. In addition, the change over time of pressure loss, which is an indicator of the accumulation status inside the device, is stable at an exhaust gas flow rate of 45 L / min at a central temperature of 456 ° C or higher, and when the hydrogen concentration is lowered, the temperature becomes 380 ° C. Only after reaching ° C did it show a remarkable upward trend. In other words, if the central part temperature is 456 ° C or higher, it can be assumed that PM oxidation proceeds at a sufficiently high rate and the amount of deposited PM does not increase, and continuous collection and removal of PM by oxidation are possible. You. Similarly, when the exhaust gas flow rate was 60 Lmin, it was confirmed that if the temperature in the central part was raised to 585 ° C, continuous collection and removal of the acid were possible.

Claims

請求の範囲 The scope of the claims
[1] 伝熱面によって隔てられた 2つの流路を有する 2流体向流型の熱交 構造から なる反応器であって、熱交換が行われる流路の少なくとも一部分に化学反応を促進 するための加熱手段を設けたことを特徴とする反応器。  [1] A reactor having a two-fluid counter-current heat exchange structure having two flow paths separated by a heat transfer surface, for promoting a chemical reaction in at least a part of the flow path where heat exchange is performed A reactor provided with a heating means.
[2] 前記加熱手段が触媒層であることを特徴とする請求項 1に記載の反応器。 [2] The reactor according to claim 1, wherein the heating means is a catalyst layer.
[3] 1つの流体を 2分割した後、互いに向流させるものであることを特徴とする請求項 1 又は 2に記載の反応器。 [3] The reactor according to claim 1 or 2, wherein a single fluid is divided into two and then flows countercurrent to each other.
[4] 前記熱交換器構造における伝熱面を構成する伝熱体が波形であり、かつ 2流体を[4] The heat transfer body constituting the heat transfer surface in the heat exchanger structure has a waveform, and the two fluids
、主として該伝熱体の波形部分の一方およびその裏側の空隙部を波形の稜線方向 および Zまたは谷線方向に沿って向流させるものであることを特徴とする請求項 1一11. The method according to claim 11, wherein one of the corrugated portions of the heat transfer body and a void portion on the back side thereof are countercurrently flown along the ridge direction and the Z or valley direction of the waveform.
3の 、ずれか 1項に記載の反応器。 3. The reactor according to item 1 or 3.
[5] 2流体の各流路内に、流線方向において加熱手段と、該加熱手段と同位置および[5] In each flow path of the two fluids, a heating means in a streamline direction, and the same position and
Zまたは近傍に燃焼性微粒子を補足するフィルターとを配置したことを特徴とする請 求項 1一 4のいずれか 1項に記載の反応器。 5. The reactor according to claim 1, wherein a filter for capturing combustible fine particles is arranged at or near Z.
PCT/JP2005/001416 2004-02-05 2005-02-01 Reactor with heat exchange function WO2005075800A1 (en)

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JP2007170323A (en) * 2005-12-26 2007-07-05 National Institute Of Advanced Industrial & Technology Exhaust emission control device
JP2007198706A (en) * 2006-01-30 2007-08-09 National Institute Of Advanced Industrial & Technology Internal heating type heat exchange structure having intersecting passage directions
JP2007196180A (en) * 2006-01-30 2007-08-09 National Institute Of Advanced Industrial & Technology Inner heat generating type heat exchange structure

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JPH05296410A (en) * 1992-04-21 1993-11-09 Matsushita Electric Ind Co Ltd Catalyst reactor
JPH07139343A (en) * 1993-11-19 1995-05-30 Honda Motor Co Ltd Exhaust emission control device for engine
JPH07506884A (en) * 1992-04-30 1995-07-27 ガイザー ゲルト Reactor for catalytic treatment of gaseous fluids
JP2000189757A (en) * 1998-12-30 2000-07-11 Volvo Ab Catalytic purification device

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JPH05228320A (en) * 1991-03-21 1993-09-07 Schwaebische Huettenwerke Gmbh Exhaust gas filter or catalyst
JPH05137959A (en) * 1991-05-02 1993-06-01 Scambia Ind Dev Ag Catalytic converter for catalytic treatment of exhaust gas
JPH05296410A (en) * 1992-04-21 1993-11-09 Matsushita Electric Ind Co Ltd Catalyst reactor
JPH07506884A (en) * 1992-04-30 1995-07-27 ガイザー ゲルト Reactor for catalytic treatment of gaseous fluids
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JP2000189757A (en) * 1998-12-30 2000-07-11 Volvo Ab Catalytic purification device

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JP2007170323A (en) * 2005-12-26 2007-07-05 National Institute Of Advanced Industrial & Technology Exhaust emission control device
JP4639381B2 (en) * 2005-12-26 2011-02-23 独立行政法人産業技術総合研究所 Exhaust gas purification device
JP2007198706A (en) * 2006-01-30 2007-08-09 National Institute Of Advanced Industrial & Technology Internal heating type heat exchange structure having intersecting passage directions
JP2007196180A (en) * 2006-01-30 2007-08-09 National Institute Of Advanced Industrial & Technology Inner heat generating type heat exchange structure
JP4521513B2 (en) * 2006-01-30 2010-08-11 独立行政法人産業技術総合研究所 Internal heating type heat exchange structure

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