US20140165380A1 - Method for fabricating exhaust gas decontamination reactor - Google Patents
Method for fabricating exhaust gas decontamination reactor Download PDFInfo
- Publication number
- US20140165380A1 US20140165380A1 US14/092,543 US201314092543A US2014165380A1 US 20140165380 A1 US20140165380 A1 US 20140165380A1 US 201314092543 A US201314092543 A US 201314092543A US 2014165380 A1 US2014165380 A1 US 2014165380A1
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- US
- United States
- Prior art keywords
- exhaust gas
- metal oxides
- fabricating
- reducing
- gas decontamination
- Prior art date
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- Abandoned
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- 238000000034 method Methods 0.000 title claims abstract description 58
- 238000005202 decontamination Methods 0.000 title claims abstract description 57
- 230000003588 decontaminative effect Effects 0.000 title claims abstract description 57
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- 239000011248 coating agent Substances 0.000 claims abstract description 10
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- 239000007789 gas Substances 0.000 description 60
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 17
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Images
Classifications
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
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- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
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- 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
- B01D53/32—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 by electrical effects other than those provided for in group B01D61/00
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
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- B01D53/8625—Nitrogen oxides
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- B01J23/894—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals also combined with metals, or metal oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with rare earths or actinides
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- B01J37/0244—Coatings comprising several layers
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- 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
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- F01N13/16—Selection of particular materials
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- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
- F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
- F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
- F01N3/28—Construction of catalytic reactors
- F01N3/2803—Construction of catalytic reactors characterised by structure, by material or by manufacturing of catalyst support
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Definitions
- the present invention relates to an electrochemical-catalytic converter, particularly to a method for fabricating an exhaust gas decontamination pipe and an exhaust gas decontamination honeycombed structure.
- the emission standard of motor vehicles has been advanced persistently. However, the continuously increasing motor vehicles still bring about more and more serious air pollution.
- the engine thereof burns fuel and converts chemical energy into mechanical energy.
- the burning process of fuel generates exhaust gases, including oxynitrides, carbon monoxide (CO), hydrocarbons (HC), and particulate matters, smoke, non-methane hydrocarbons (NMHC), and methane (CH 4 ), which would form photochemical smog, deplete ozone, enhance the greenhouse effect, cause acid rain, damage the ecological environment and endanger human health.
- the capability of carbon monoxide to combine with hemoglobin to form carboxyhemoglobin (COHb) is 300 times higher than the capability of oxygen to combine with hemoglobin to form oxyhemoglobin (HbO 2 ). Therefore, too high a concentration of carbon monoxide would degrade the capability of hemoglobin to transport oxygen.
- Oxynitrides are generated by the combination of nitrogen and oxygen and mainly in form of nitrogen monoxide (NO) and nitrogen dioxide (NO 2 ). Oxynitrides are also likely to combine with hemoglobin and would impair the breathing and circulating functions. Hydrocarbons can irritate the respiratory system even at a lower concentration and will affect the central nervous system at higher concentration.
- a catalytic oxidizing converter is installed in the exhaust pipe of a diesel engine vehicle to catalytically convert carbon monoxide (CO) and hydrocarbons (HCs), and an EGR (Exhaust Gas Recirculation) system or a cylinder water-spray apparatus is used to eliminate oxynitrides (NO x ).
- EGR Exhaust Gas Recirculation
- a cylinder water-spray apparatus is used to eliminate oxynitrides (NO x ).
- SCR Selective Catalytic Reduction
- ammonia (NH 3 ) gas or an aqueous urea (CO(NH 2 ) 2 ) solution is used as a reactant.
- the aqueous urea solution is sprayed into the exhaust pipe via nozzles and decomposed into ammonia gas. Then, the ammonia gas reacts with oxynitrides (NO x ) to generate products—nitrogen and water.
- NO x oxynitrides
- ammonia gas is poisonous, hard to store and likely to leak. Further, incomplete reaction of ammonia will cause secondary pollution.
- the SCR system is bulky and has to cooperate with precision sensors.
- a U.S. Pat. No. 5,401,372 disclosed an “Electrochemical Catalytic Reduction Cell for the Reduction of NO x in an O 2 -Containing Exhaust Emission”, which is dedicated to removing oxynitrides, wherein an electrocatalytic reducing reaction and a vanadium pentaoxide (V 2 O 5 ) catalyst convert oxynitrides into nitrogen.
- V 2 O 5 vanadium pentaoxide
- a U.S. patent application Ser. No. 13/037,693 disclosed an “Electrochemical-Catalytic Converter for Exhaust Emission Control”, which can eliminate oxynitrides (NO x ), carbon monoxide (CO), hydrocarbons (HC), and particulate matters (PM) in exhaust gas, and which comprises a battery module, wherein oxynitrides are electrocatalytically decomposed into nitrogen and oxygen, and wherein carbon monoxide, hydrocarbons, and particulate matters are converted into water and carbon dioxide by an oxidizing catalyst. Therefore, the prior art can eliminates multiple harmful gases simultaneously.
- Electrochemical-Catalytic Converter is hard to fabricate into a compact structure for vehicle application. Therefore, the prior art still has room to improve.
- the primary objective of the present invention is solve the problem that the conventional electrochemical-catalytic converter requires an additional reducing-gas system for generating electromotive force, which makes the fabrication cost increase, the structure likely to damage, and the volume hard to decrease.
- the present invention proposes a method for fabricating an exhaust gas decontamination reactor, which is an exhaust gas decontamination pipe or an exhaust gas decontamination honeycombed structure.
- the method for fabricating an exhaust gas decontamination pipe comprises the following steps:
- a pipe made of a solid-state oxide and including an internal channel, an inner wall surface surrounding the internal channel, and an outer wall surface far away from the inner wall surface;
- the method for fabricating a honeycombed structure comprises the following steps:
- honeycombed structure made of a solid-state oxide and including a plurality of tubes and a plurality of separation walls between the tubes;
- green cathode layers which contain a cathode material, on first inner wall surfaces of the first passages, and undertaking a first sintering process to convert the green cathode layers into cathode layers on the first inner wall surfaces;
- green anode layers which contain an anode material, on second inner wall surfaces of the second passages, and undertaking a second sintering process to convert the green anode layers into anode layers on the second inner wall surfaces, whereby the separation walls are between the anode layers and the cathode layers;
- the exhaust gas decontamination reactor fabricated according to the present invention can merely use the cathode layers to decontaminate exhaust gas without using any additional reducing-gas system. Therefore, the method of the present invention is able to reduce the fabrication cost, and the exhaust gas decontamination reactor fabricated by the present invention is less likely to be damaged.
- the present invention needn't arrange a reducing-gas system in the exhaust gas decontamination reactor and thus can obviously decrease the volume of the exhaust gas decontamination reactor. Therefore, the exhaust gas decontamination reactor fabricated according to the present invention can be arranged inside the exhaust pipe of a vehicle engine to decontaminate the harmful matters generated by oxygen-enriched combustion and reduce the air pollution.
- FIGS. 1A-1D are diagrams schematically showing the process of fabricating an exhaust gas decontamination pipe according to a first embodiment of the present invention.
- FIGS. 2A-2D are diagrams schematically showing the process of fabricating an exhaust gas decontamination honeycombed structure according to a second embodiment of the present invention.
- the present invention provides a method for fabricating an exhaust gas decontamination reactor, which is an exhaust gas decontamination pipe or an exhaust gas decontamination honeycombed structure.
- an exhaust gas decontamination reactor which is an exhaust gas decontamination pipe or an exhaust gas decontamination honeycombed structure.
- a first embodiment and a second embodiment are respectively used to demonstrate a method for fabricating an exhaust gas decontamination pipe and a method for fabricating an exhaust gas decontamination honeycombed structure.
- FIGS. 1A-1D diagrams schematically showing the process of fabricating an exhaust gas decontamination pipe according to a first embodiment of the present invention.
- the method for fabricating an exhaust gas decontamination pipe comprises Steps 1 - 4 .
- Step 1 provide a pipe 10 made of a solid-state oxide, as shown in FIG. 1A .
- the solid-state oxide is a fluoride metal oxide or a perovskite metal oxide, such as a fluorite YSZ (yttria-stabilized zirconia), a stabilized zirconia, a fluorite GDC (gadolinia-doped ceria), a dopedceria, a perovskite LSGM (strontium/magnesium-doped lanthanum gallate), or a doped lanthanum gallate.
- the pipe 10 is made of zirconia.
- the pipe 10 includes an internal channel 11 , a first opening 14 , a second opening 15 , an inner wall surface 12 , and an outer wall surface 13 .
- the internal channel 11 is between the first opening 114 and the second opening 15 and interconnects the first opening 14 and the second opening 15 .
- the inner wall surface 12 surrounds the internal channel 11 .
- the outer wall surface 13 is far away from the inner wall surface 12 .
- Step 2 coat a green cathode layer, which contains a cathode material, on the outer wall surface 13 , and undertake a first sintering process to form a cathode layer 20 on the outer wall surface 13 , as shown in FIG. 1B .
- the cathode material is selected from a group consisting of perovskite metal oxides, fluorite metal oxides, metal-containing perovskite metal oxides, and metal-containing fluorite metal oxides.
- the cathode layer is made of a perovskite lanthanum strontium cobalt copper oxide, a lanthanum strontium manganese copper oxide, a combination of a lanthanum strontium cobalt copper oxide and a gadolinia-doped ceria; a combination of a lanthanum strontium manganese copper oxide and a gadolinia-doped ceria, a silver-containing lanthanum strontium cobalt copper oxide, a silver-containing lanthanum strontium manganese copper oxide, a combination of a silver-containing lanthanum strontium cobalt copper oxide and a gadolinia-doped ceria, or a combination of a silver-containing lanthanum strontium manganese copper oxide and a gadolinia-doped ceria.
- the first sintering process is to degrease the cathode material and sinter the cathode
- the green cathode layer is exemplified by one containing a combination of a lanthanum strontium manganese copper oxide and a gadolinia-doped ceria.
- a combination of a lanthanum strontium manganese copper oxide and a gadolinia-doped ceria Firstly, enclose the first opening 14 and the second opening 15 with adhesive tapes. Next, coat a fluorite gadolinia-doped ceria on the outer wall surface 12 with a dipping method. Next, take off the adhesive tapes, and dry the pipe 10 in an oven at a temperature of 50° C. for 6 hours. Next, heat the pipe 10 at a temperature rising speed of 5° C./min to a temperature of 600° C., and soak the pipe 10 at 600° C. for 2 hours.
- the following heating processes and cooling processes will be undertaken at the speed of 5° C./min also.
- heat the pipe 10 to a temperature of 900° C., and soak the pipe 10 at 900° C. for 2 hours.
- heat the pipe 10 to a temperature of 1200° C., and soak the pipe 10 at 1200° C. for 4 hours.
- take off the adhesive tapes and dry the pipe 10 in an oven at a temperature of 50° C. for 6 hours.
- Step 3 coat a green anode layer, which contains an anode material, on the inner wall surface 12 , and undertake a second sintering process to form an anode layer 30 on the inner wall surface 12 , as shown in FIG. 1C .
- the anode material is selected from a group consisting of fluorite metal oxides, perovskite metal oxides, metal-containing fluorite metal oxides, and metal-containing perovskite metal oxides.
- the anode material is a nickel-containing yttria-stabilized zirconia (Ni—YSZ cermet).
- the green anode layer is exemplified by one containing Ni—YSZ cermet.
- pour a slurry made of the anode material into the pipe 10 along the inner wall surface 12 and let the residual slurry slip away spontaneously, and then air-dry the slurry.
- undertake a second sintering process Beforehand, dry the pipe 10 in an oven at a temperature of 50° C. for 6 hours. Then, undertake heat treatments at a temperate rising speed of 5° C./min. Heat the pipe 10 to a temperature of 300° C., and soak the pipe 10 at 300° C. for 2 hours. Next, heat the pipe 10 to a temperature of 600° C., and soak the pipe 10 at 600° C.
- the second sintering process is the same as that of the first sintering process and will not repeat herein.
- the second sintering process is different from the first sintering process in that nickel oxide needs to be reduced into nickel metal. Therefore, the green anode layer together with the pipe 10 is placed in a quartz tube for a reducing heat treatment.
- the quartz tube is filled with hydrogen, heated at a temperature-rising speed of 5° C./min to a temperature of 400° C., and soaked at the temperature of 400° C. for 8 hours to reduce the combination of nickel oxide and the Ni—YSZ cermet into nickel metal and the Ni—YSZ cermet. Thereby is completed the anode layer 30 .
- Step 4 provide a reducing environment 111 for the internal channel 11 , and seal the pipe 10 to enclose the reducing environment 111 and complete the exhaust gas decontamination pipe, as shown in FIG. 1D .
- a reducing agent 112 is filled into the internal channel 11 to form the reducing environment 111 .
- the reducing agent 112 may be a solid-state reducing agent (such as graphite powder or carbon black), a liquid reducing agent (such as aqueous ammonia solution), or a gaseous reducing agent (such as methane or hydrogen).
- the reducing agent 112 is enclosed inside the internal channel 11 by sealing elements 113 to form the reducing environment 111 .
- the sealing elements 113 are made of a heat-resistant ceramic putty having a thermal expansion coefficient near that of the pipe 10 .
- the sealing element 113 normally contains aluminum oxides and silicon oxides.
- the internal channel 11 is not filled with the reducing agent 112 but directly sealed by the sealing elements 113 , and the air pressure inside the internal 11 is lowered to below 1 atm, e.g. a vacuum state, whereby is also formed the reducing environment 111 .
- FIGS. 2A-2D diagrams schematically showing the process of fabricating an exhaust gas decontamination honeycombed structure according to a second embodiment of the present invention.
- the method for fabricating an exhaust gas decontamination honeycombed structure comprises Steps A-E.
- the honeycombed structure 50 includes a plurality of tubes 51 and a plurality of separation walls 52 between each two tubes 51 , as shown in FIG. 2A .
- the tubes 51 are separated by the separation walls 52 and arranged together.
- the tubes 51 have square sections.
- the present invention does not constrain that the sections of the tubes 51 must be square.
- the tubes 51 may have circular or hexagonal sections, which are closely arranged to form a compact structure.
- Step B define in the tubes 51 a plurality of first passages 511 allowing an exhaust gas 80 (shown in FIG. 2D ) to pass and a plurality of second passages 513 to be sealed later.
- Each first passage 511 is adjacent to several second passages 513 .
- the first passages 511 and the second passages 513 are alternately arranged to make each first passage 511 surrounded by four second passages 513 .
- the present invention is not limited by the second embodiment.
- Step C coat a green cathode layer containing a cathode material on a first inner wall surface 512 of each first passage 511 , and undertake a first sintering process to convert the green cathode layer into a cathode layer 60 on the first inner wall surface 512 , as shown in FIG. 2B .
- Step C of the second embodiment is characterized in that the second passages 513 are sealed with silicone pads before the green cathode layers are coated on the first inner wall surfaces 512 .
- the method to coat the green cathode layer and the first sintering process are the same as those in Step 2 and will not repeat herein. Thereby is obtained the cathode layer 60 in Step C.
- Step D coat a green anode layer containing an anode material on a second inner wall surface 514 of the second passage 513 , and undertake a second sintering process to convert the green anode layer into an anode layer 70 on the second inner wall surface 514 , as shown in FIG. 2C .
- the separation walls 52 are between the anode layers 70 and the cathode layers 60 .
- Step D of the second embodiment is characterized in that the silicone pads sealing the second passages 513 are removed, and that the first passages 511 are sealed with silicone pads before the anode material is coated on the second inner wall surface 514 with a dipping method. Then, take off the silicone pads from the first passages 511 , and undertake the same second sintering process and reducing process as that used in Step 3 to convert the green anode layer into the anode layer 70 on the second inner wall surface 514 .
- Step E provide reducing environments 515 for the second passages 513 , and seal the second passages 513 to enclose the reducing environments 515 and complete the exhaust gas decontamination honeycombed structure.
- the reducing agents 516 , the sealing elements 517 and the method to form the reducing environments 515 are similar to those used in Step 4 .
- Step E is different from Step 4 in that the reducing environments 515 are formed in the second passages 513 , and that the exhaust gas 80 flows through the first passages 511 , and that the separation walls 512 are formed between the first passages 511 and the second passages 513 .
- the reducing environment 515 , the anode layer 70 , the separation wall 52 and the cathode layer 60 are sequentially formed from the second passage 513 to the first passage 511 . Then, the surfaces of the cathode layers 60 function as reaction sites to undertake a catalytic decomposition reaction of oxynitrides and decontaminate the exhaust gas 80 .
- the exhaust gas decontamination pipe and honeycombed structure fabricated according to the present invention can merely use the cathode layers to decontaminate exhaust gas without using any additional reducing-gas system. Therefore, the method of the present invention is able to reduce the fabrication cost, and the exhaust gas decontamination reactor fabricated by the present invention is less likely to be damaged. As the present invention needn't arrange a reducing-gas system in the exhaust gas decontamination reactor, the present invention can obviously decrease the volume of the exhaust gas decontamination reactor. Therefore, the exhaust gas decontamination reactor fabricated according to the present invention can be arranged inside the exhaust pipe of a vehicle engine to decontaminate the harmful matters generated by oxygen-enriched combustion and reduce the air pollution.
- the present invention possesses utility, novelty and non-obviousness and meets the condition for a patent.
- the Inventors file the application for a patent. It is appreciated if the patent is approved fast.
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TW101148109 | 2012-12-18 | ||
TW101148109A TWI491436B (zh) | 2012-12-18 | 2012-12-18 | Production method of exhaust gas purifying reactor |
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US20140165380A1 true US20140165380A1 (en) | 2014-06-19 |
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US14/092,543 Abandoned US20140165380A1 (en) | 2012-12-18 | 2013-11-27 | Method for fabricating exhaust gas decontamination reactor |
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CN114570172A (zh) * | 2022-03-03 | 2022-06-03 | 张震渝 | 一种火电厂废气处理设备及处理工艺 |
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CN109772165B (zh) * | 2018-12-14 | 2021-09-14 | 深圳大学 | 一种尾气净化反应器及其制备方法与尾气净化反应电堆 |
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CN1145588C (zh) * | 1999-05-06 | 2004-04-14 | 科学技术振兴事业团 | 微量有害物质的氧化分解装置 |
GB0502227D0 (en) * | 2005-02-03 | 2005-03-09 | Thermal Energy Systems Ltd | Gas separation and compresssion device |
JP2009125622A (ja) * | 2007-11-20 | 2009-06-11 | Toyota Industries Corp | 排気ガスの浄化装置 |
JP4803400B2 (ja) * | 2008-03-27 | 2011-10-26 | 三菱自動車工業株式会社 | 内燃機関の排気浄化装置 |
TWI414343B (zh) * | 2010-10-29 | 2013-11-11 | Nat Univ Tsing Hua | An electrochemical catalyst converter for controlling exhaust emissions |
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2012
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2013
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TWI491436B (zh) | 2015-07-11 |
TW201424827A (zh) | 2014-07-01 |
CN103861453A (zh) | 2014-06-18 |
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