CN103768901B - Control the electric catalyst honeycomb of toxic emission - Google Patents
Control the electric catalyst honeycomb of toxic emission Download PDFInfo
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- CN103768901B CN103768901B CN201210393957.8A CN201210393957A CN103768901B CN 103768901 B CN103768901 B CN 103768901B CN 201210393957 A CN201210393957 A CN 201210393957A CN 103768901 B CN103768901 B CN 103768901B
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Abstract
The present invention has about a kind of electric catalyst honeycomb controlling toxic emission, in order to purify an oxygen-enriched combusting waste gas, includes a honey comb structure, a solid oxide nitride layer and a cathode layer.This honey comb structure comprises an anode, multiple gas channel and a shell, a skeleton of this this honey comb structure of anodic formation, and this gas channel is formed at for the circulation of this oxygen-enriched combusting waste gas in this skeleton, and this shell covers an outer surface of this anode; This solid oxide nitride layer is attached to an inner surface of this anode, engages and seal this anode with this shell, and has the tube wall of this gas channel faced by, this cathode layer is attached on this tube wall, wherein, this anode has a reproducibility environment, and this cathode layer has an oxidative environment.Accordingly, this reproducibility environment and this oxidative environment make between this anode and this cathode layer and produce an electromotive force, drive and promote that the nitrogen oxide in this oxygen-enriched combusting waste gas decomposes in this cathode layer.
Description
Technical field
The present invention, about a kind of electric catalyst honeycomb, espespecially a kind ofly controls toxic emission and the electric catalyst honeycomb of effectively decomposing nitrogen oxide and oxidizing carbon monoxide, hydrocarbon and shot-like particle.
Background technology
Pure and fresh is one of basic important document of human lives with the air of cleaning, breathes clean free of contamination air and can guarantee that the mankind are stable and survive healthily.The brilliance of science and technology promotes, though drive economic developing rapidly, but, come from the toxic emission of the vehicles and various factory of standing in great numbers, cause air to be polluted also, and very huge on the air quality impact of human lives.Wherein, heavy industry factory and motor vehicles are the main source of numerous polluter.
For motor vehicles, although motor vehicles discharge standard improves constantly, because vehicle fleet size constantly increases, the air pollution problems inherent that waste gas discharged by vehicles brings, still grows with each passing day.In general, multi-form fuel is discharged heat energy via cylinder internal combustion by operating as of motor vehicle engine, and produces transmission power; Only in combustion, the waste gas of generation comprises nitrogen oxide (NO usually
x), carbon monoxide (CO), hydrocarbon (hydrocarbons, HCs), shot-like particle (particulatematter, the noxious pollutant such as PM), these materials not only can form photochemical fog (photochemicalsmog), more can destroy ozone, aggravate the deterioration of greenhouse effects and cause acid rain etc., and then destruction ecological environment, be detrimental to health.
Wherein, carbon monoxide is from the imperfect combustion of engine, and the ability that itself and ferroheme are combined into Carbon monoxide haemoglobin (COHb) is that ferroheme and oxygen are combined into oxyhaemoglobin (HbO
2) 300 times, therefore during CO in Air excessive concentration, will the function of ferroheme delivering oxygen be affected; Nitrogen oxide then from the chemical combination of nitrogen and oxygen, mainly with nitric oxide (NO) or nitrogen dioxide (NO
2) form discharge, and react after Ultraviolet radiation with hydrocarbon and form poisonous photochemical fog, there is special odor, stimulate eyes, injure plant, and atmospheric visibility is reduced, and the water in nitrogen oxide and air reacts and forms nitric acid and nitrous acid, it is the composition of acid rain; Hydrocarbon can stimulate respiratory system when low concentration, if concentration improves, then can have an impact to the running function of central nervous system; And shot-like particle also can the health of harmful to human, causes even the generation of cancer.
Therefore, regardless of the advanced country such as China or European Union, Japan, the U.S., all stipulate the waste gas emission standard (as U.S. rule BIN5 and Europe rule EURO6) that benefit becomes strict, standard is stipulated in discharge for waste gas such as nitrogen oxide, carbon monoxide, hydrocarbon and shot-like particles, use and control and reduce the discharge of pernicious gas, encourage dealer to manufacture simultaneously, research and development, the anti-technology processed of the up-to-date pollution of introducing and employment product.
As U.S. patent Nos announces the " ElectrochemicalcatalyticreductioncellforthereductionofNO of No. 5401372
xinanO
2-containingexhaustemission " disclose a kind of device of independent removal nitrogen oxide, for utilizing electrochemical catalyst reduction reaction, coordinate vanadic anhydride (vanadiumpentaoxide, V
2o
5) catalyst catalysis assists conversion of nitrogen oxides to be nitrogen.But this above-mentioned device must additionally add power source supply, cause the electrochemical cell running in this device, so not only expend the energy and the target simultaneously removing multiple pernicious gas in waste gas cannot be reached.
Therefore in " the ElectrocatalyticTubeofElectrochemical-CatalyticConverter forExhaustEmissionsControl " of No. 13362247th, U.S. patent Nos application, it discloses a kind of electric catalyst pipe controlling toxic emission, this electric catalyst pipe can be stacked into a honey comb structure, form the cellular electrochemical catalyst converter of an advanced person, and can in order to the nitrogen oxide in purifying exhaust air, carbon monoxide, hydrocarbon and shot-like particle, wherein this nitrogen oxide is broken down into nitrogen and oxygen, this carbon monoxide, this hydrocarbon and this shot-like particle are oxidized to carbon dioxide and water.Therefore, this electric catalyst pipe, not needing to expend under additional energy source and reducibility gas, can purify multiple pollutant.
But, this cellular electrochemical catalyst converter above-mentioned, the passage of its half must seal to form this electric catalyst pipe, so, compared with the cellular Cat Catalytic Converter of existing vehicle, not only conversion zone is reduced, also manufacturing cost is increased, therefore, its space be still improved.
Summary of the invention
Main purpose of the present invention, is to solve existing cellular electrochemical catalyst converter, has the problem of less conversion zone and higher manufacturing cost.
For reaching above-mentioned purpose, the invention provides a kind of electric catalyst honeycomb controlling toxic emission, in order to purify an oxygen-enriched combusting waste gas, this electric catalyst honeycomb includes a honey comb structure, a solid oxide nitride layer and a cathode layer.This honey comb structure comprises an anode, multiple gas channel and a shell, one skeleton of this this honey comb structure of anodic formation, be made up of one first porous material, and there is a reproducibility environment, this gas channel is formed in this skeleton for the circulation of this oxygen-enriched combusting waste gas, this shell covers an outer surface of this anode, and is one first dense microstructure; This solid oxide nitride layer is attached to an inner surface of this anode this outer surface relative, is one second dense microstructure, and has the tube wall of this gas channel faced by, and this solid oxide nitride layer engages with this shell and seals this anode; This cathode layer is attached on this tube wall, and this solid oxide nitride layer is between this anode and this cathode layer, and this cathode layer is then made up of one second porous material, and has an oxidative environment.
Wherein, this reproducibility environment and this oxidative environment make between this anode and this cathode layer and produce an electromotive force, drive and promote that the nitrogen oxide in this oxygen-enriched combusting waste gas carries out a decomposition reaction in this cathode layer and forms nitrogen and oxygen.
The electric catalyst honeycomb of described control toxic emission, wherein, this anode has the hole of multiple attachment one carbon species.
The electric catalyst honeycomb of described control toxic emission, wherein, the material of this anode selects the group that the Tao Jin of free metal and fluorite structure metal oxide composition, perovskite structure metal oxide, fluorite structure metal oxide, the perovskite structure metal oxide adding metal, the fluorite structure metal oxide adding metal and combination thereof form.
The electric catalyst honeycomb of described control toxic emission, wherein, the group that the material of this shell selects free metal, pottery, glass and combination thereof to form.
The electric catalyst honeycomb of described control toxic emission, wherein, the material of this solid oxide nitride layer is selected from the group be made up of fluorite structure metal oxide, perovskite structure metal oxide and combination thereof.
The electric catalyst honeycomb of described control toxic emission, wherein, the material of this cathode layer is selected from the group be made up of perovskite structure metal oxide, fluorite structure metal oxide, the perovskite structure metal oxide adding metal, the fluorite structure metal oxide adding metal and combination thereof.
The electric catalyst honeycomb of described control toxic emission, wherein, also comprises one and is arranged between this cathode layer with this solid oxide nitride layer to promote the boundary layer that this cathode layer is connected with this solid oxide nitride layer.
The electric catalyst honeycomb of described control toxic emission, wherein, the material of this boundary layer is selected from the group be made up of fluorite structure metal oxide, perovskite structure metal oxide and combination thereof.
The electric catalyst honeycomb of described control toxic emission, wherein, also comprises one and is attached to oxidation catalyst layer on this cathode layer.
The electric catalyst honeycomb of described control toxic emission, wherein, the group that the material of this oxidation catalyst layer selects free metal, alloy, fluorite structure metal oxide, perovskite structure metal oxide and combination thereof to form.
In sum, in the present invention, by these gas channels all of this electric catalyst honeycomb all for reacting with this oxygen-enriched combusting waste gas, and this electric catalyst honeycomb is compared existing cellular electrochemical catalyst converter and is more easily made, accordingly, the present invention, compared with existing cellular electrochemical catalyst converter, has:
1. larger conversion zone.
2. lower manufacturing cost.
Accompanying drawing explanation
Fig. 1 is the stereoscopic schematic diagram of first embodiment of the invention;
Fig. 2 is the generalized section of first embodiment of the invention;
Fig. 3 is the section close-up schematic view of first embodiment of the invention;
Fig. 4 is the section close-up schematic view of second embodiment of the invention;
Fig. 5 is the schematic front view of third embodiment of the invention.
Detailed description of the invention
Detailed description for the present invention and technology contents, now just coordinate graphic being described as follows:
Please arrange in pairs or groups and consult shown in Fig. 1 to Fig. 3, Fig. 1 is the stereoscopic schematic diagram of first embodiment of the invention, Fig. 2 is the generalized section of first embodiment of the invention, Fig. 3 is the section close-up schematic view of first embodiment of the invention, the present invention is a kind of electric catalyst honeycomb controlling toxic emission, in order to purify an oxygen-enriched combusting waste gas, this oxygen-enriched combusting waste gas can comprise nitrogen oxide (NO
x), carbon monoxide (CO), hydrocarbon (hydrocarbons, and shot-like particle (particulatematter HCs), PM), this electric catalyst honeycomb includes honey comb structure 10, solid oxide nitride layer 20 and a cathode layer 30.This honey comb structure 10 includes an anode 11, multiple gas channel 12 and a shell 13, this anode 11 forms a skeleton of this honey comb structure 10, in this embodiment, this anode 11 is made up of one first porous material, and there is a large amount of holes, the material of this anode 11 can be the Tao Jin (cermet) of metal and fluorite structure metal oxide composition, fluorite structure metal oxide (f1uoritemetaloxides), perovskite structure metal oxide (perovskitemetaloxides), add the fluorite structure metal oxide of metal or add the perovskite structure metal oxide of metal, such as: nickel (Ni) and yttria stabilized zirconia (yttria-stabilizedzirconia, YSZ) Tao Jin (Ni-YSZcermet), this gas channel 12 is formed in this skeleton, runs through the two ends that this honey comb structure 10 is relative, for the circulation of this oxygen-enriched combusting waste gas, 13, this shell covers an outer surface 111 of this anode 11, and is one first dense microstructure, and its material can be metal, pottery (ceramics) or glass, such as, be stainless steel, aluminium oxide, quartz glass etc.
This solid oxide nitride layer 20 is attached to an inner surface 112 of this anode 11 this outer surface 111 relative, and the two ends relative on this anode 11 with this shell 13 engage, and seal this anode 11 completely, make in this anode 11 and can be a reproducibility environment, this solid oxide nitride layer 20 also has one in the face of the tube wall 21 of this gas channel 12, and the structure of this solid oxide nitride layer 20 is one second dense microstructure, and can oxygen-ion conductive be had, its material can be fluorite structure metal oxide or perovskite structure metal oxide; Such as: the gadolinia-doped ceria (gadolinia-dopedceria of the yttria stabilized zirconia of fluorite structure, stabilized zirconia, fluorite structure, GDC), the strontium of doped cerium oxide, perovskite structure and magnesium doped lanthanum gallate (strontium/magnesium-dopedlanthanumgallate, LSGM), doped lanthanum gallate.
This cathode layer 30 is attached on this tube wall 21, make this solid oxide nitride layer 20 between this anode 11 and this cathode layer 30, in this embodiment, this cathode layer 30 is made up of one second porous material, and there is a large amount of holes, such as can be perovskite structure metal oxide, fluorite structure metal oxide, add the perovskite structure metal oxide of metal or add the fluorite structure metal oxide of metal, such as: the lanthanum strontium cobalt Cu oxide of perovskite structure, lanthanum strontium copper-manganese oxide, the combination of lanthanum strontium cobalt Cu oxide and gadolinia-doped ceria, the combination of lanthanum strontium copper-manganese oxide and gadolinia-doped ceria, add the lanthanum strontium cobalt Cu oxide of silver, add the lanthanum strontium copper-manganese oxide of silver, add the lanthanum strontium cobalt Cu oxide of silver and the combination of gadolinia-doped ceria, add the lanthanum strontium copper-manganese oxide of silver and the combination of gadolinia-doped ceria.
In the present invention, this anode 11 comprises a metal oxide when preliminary making, and this metal oxide, in time making this anode 11, first uses the process of a reducibility gas through one and is reduced to a metal, such as, be reduced to nickel by nickel oxide; Or, also can be the metal oxide (oxygen-deficientmetaloxide) of an anoxic by this metal oxide back, to form this reproducibility environment of this anode 11.In addition, before this solid oxide nitride layer 20 engages this shell 13 and seals this anode 11 completely, first carbon monoxide or hydrocarbon can be made an addition to this anode 11, as passed into methane, ethane, the third rare or propane etc. in this anode 11 via hole diffusion (porediffusion), to form the carbon species being attached to the hole of this anode 11, to strengthen this reproducibility environment forming this anode 11.Again in addition, before sealing this anode 11 completely, the gas that can extract in the hole of this anode 11 is down to a below atmospheric pressure to make its gas pressure or is down to vacuum, accordingly, and can reduce this honey comb structure 10 in the exhaust-gas treatment operation above issuable structure damage because expanding with heat and contract with cold.
Please arrange in pairs or groups and consult shown in Fig. 4, for the section close-up schematic view of second embodiment of the invention, in second embodiment, with the first embodiment in comparison, it is characterized in that, this electric catalyst honeycomb also can comprise a boundary layer 40, this boundary layer 40 is arranged between this cathode layer 30 and this solid oxide nitride layer 20, to promote that this cathode layer 30 is connected with this solid oxide nitride layer 20, at this, the material of this boundary layer 40 can be fluorite structure metal oxide, or perovskite structure metal oxide, such as, be the gadolinia-doped ceria of fluorite structure.
Moreover, in a second embodiment, this electric catalyst honeycomb also can comprise an oxidation catalyst layer 50 further, to impel a composition oxidation of this oxygen-enriched combusting waste gas being not easy to the oxidation of this cathode layer 30, this oxidation catalyst layer 50 is connected with this cathode layer 30, and be attached on this cathode layer 30, the material of this oxidation catalyst layer 50 can be metal, alloy, metal oxide, fluorite structure metal oxide, perovskite structure metal oxide, such as: palladium, the gadolinia-doped ceria of fluorite structure and lanthanum-strontium-manganese oxide (lanthanum – strontium – manganeseoxide) etc.
The mechanism continued purifying exhaust air of the present invention is described, first this electric catalyst honeycomb is positioned in an exhaust environment, this waste gas has an oxidative environment for this oxygen-enriched combusting waste gas, maybe can add auxiliary air and make its oxygen enrichment more, the operating temperature of this electric catalyst honeycomb is by normal temperature to 800 ° C, this oxygen-enriched combusting waste gas mainly comprises nitrogen oxide, carbon monoxide, hydrocarbon and shot-like particle composition, the present invention is for the purification aspect of this oxygen-enriched combusting waste gas, mainly can be divided into removal and the carbon monoxide of nitrogen oxide, hydrocarbon, removal two parts of shot-like particle are carried out.
In nitrogen oxide removal, nitrogen oxide is mainly nitric oxide (NO) and nitrogen dioxide (NO
2), can there is decomposition reaction in cathode layer 30 and produce nitrogen and oxygen in nitric oxide, its reaction equation is following formula (1).
2NO→N
2+O
2(1)
Can there is decomposition reaction in cathode layer 30 and produce nitric oxide in nitrogen dioxide, its reaction equation is following formula (2).
2NO
2→2NO+O
2(2)
Can decomposition reaction be there is in cathode layer 30 again and produce nitrogen and oxygen in its nitric oxide.
Different partials pressure of oxygen is produced in this anode 11 from this cathode layer 30 by this reproducibility environment of this anode 11 and this oxidative environment of this cathode layer 30, can impel between this cathode layer 30 and this anode 11 and produce electromotive force (electromotiveforce, emf), and drive and promote that the nitrogen oxide in this oxygen-enriched combusting waste gas carries out decomposition reaction in this cathode layer 30 and forms nitrogen and oxygen, this electromotive force be produced as according to following principle:
emf＝[(RT)/(4F)]·ln[(P
O2|Cathode)/(P
O2|Anode)](3)
Wherein, R is gas constant (gasconstant), T is absolute temperature, and F is Faraday constant (Faradicconstant), P
o2for partial pressure of oxygen.Due to this anode 11 that this metal or the metal oxide of this anoxic are formed, or by being attached with this anode 11 of this carbon species, it is reproducibility compound, to one be caused to have the environment of quite low partial pressure of oxygen in anode (Anode) side, thus produce a larger electromotive force.Different reproducibility compounds will cause different partials pressure of oxygen in anode-side, and can produce different electromotive force; The oxygen concentration also corresponding different oxygen partial pressure value that negative electrode (Cathode) side is different, also different electromotive force can be produced, namely the higher then electromotive force of oxygen content in this oxygen-enriched combusting waste gas of cathode side is larger, electromotive force is larger, through electrochemistry, nitrogen oxide of the present invention promotes that the reaction rate that (electrochemicalpromotion) decomposes is larger, accordingly, although this oxygen-enriched combusting waste gas is for can produce an electromotive force at an oxidative environment, then adds this auxiliary air and enter this oxygen-enriched combusting waste gas and can cause a larger electromotive force.And in certain temperature range, decomposition reaction speed can be lower and larger with operating temperature, can be the same with during at higher temperature effective in the decomposition reaction of normal temperature.
In the reaction of removing carbon monoxide, hydrocarbon and shot-like particle in this oxygen-enriched combusting waste gas, because this oxygen-enriched combusting waste gas is oxygen enrichment state, or add auxiliary air and make its oxygen enrichment more, it this cathode layer 30 of mat and this oxidation catalyst layer 50 catalytic oxidation can form innocuous gas, carbon monoxide wherein in this oxygen-enriched combusting waste gas is oxidable is carbon dioxide, hydrocarbon and shot-like particle (carbon containing (C) material) oxidable be carbon dioxide and water, its reaction equation respectively as shown in the formula (4) to (6):
2CO+O
2→2CO
2(4)
HCs+O
2→H
2O+CO
2(5)
C+O
2→CO
2(6)
Therefore, for the first embodiment of the present invention, be mainly and promote that the removal of nitrogen oxide is carried out in decomposition reaction by electrochemistry, and remove carbon monoxide, hydrocarbon and shot-like particle by oxidation reaction, and effectively remove the harmful components in this oxygen-enriched combusting waste gas.
Refer to shown in Fig. 5, for the schematic front view of third embodiment of the invention, in this embodiment, the crosssections in appearance of this honey comb structure 10 forms hexagon, the crosssections in appearance of this gas channel 12 then forms circle, but not as restriction, this honey comb structure 10 and the cross-sectional shape of this gas channel 12, can change according to the demand used and form.
In sum, because the present invention forms different partials pressure of oxygen by respectively between this anode-side from this cathode side, and produce this electromotive force to promote this catalyst decomposition reaction, not only structure is simplified, reduce production cost, moreover, the present invention is used minimum volume to reach the effect of purification, such as be arranged in car engine blast pipe, eliminate the harmful substance in this oxygen-enriched combusting waste gas of engine emissions, reduce air pollution, finally, the present invention and existing cellular electrochemical catalyst converter are compared, this gas channels all are all for reacting with this oxygen-enriched combusting waste gas, and there is larger conversion zone and preferably reaction efficiency, therefore the present invention has progressive and meets the important document of application patent of invention, file an application in whence in accordance with the law, pray an ancient unit of weight office and grant quasi patent early, true feeling moral just.
Below the present invention be described in detail, only as described above, be only a preferred embodiment of the present invention, when not limiting scope of the invention process.Namely all equalizations done according to the present patent application scope change and modify, and all should still belong in patent covering scope of the present invention.
Claims (10)
1. control an electric catalyst honeycomb for toxic emission, in order to purify an oxygen-enriched combusting waste gas, it is characterized in that this electric catalyst honeycomb includes:
One honey comb structure, comprise the anode of a skeleton of this honey comb structure of formation, multiple shell being formed in this skeleton an outer surface of gas channel and this anode of covering supplying the circulation of this oxygen-enriched combusting waste gas, this anode is made up of one first porous material, and there is a reproducibility environment, this shell is one first dense microstructure, each the plurality of gas channel has a caliber width, and the distance between any two neighboring gas flow path is less than this caliber width;
The one solid oxide nitride layer being attached to the relative inner surface of this outer surface of this anode, this solid oxide nitride layer is one second dense microstructure, and has one in the face of the tube wall of this gas channel, and this solid oxide nitride layer engages with this shell and seals this anode; And
One is attached to the cathode layer on this tube wall, and this solid oxide nitride layer is between this anode and this cathode layer, and this cathode layer is then made up of one second porous material, and has an oxidative environment;
Wherein, this reproducibility environment and this oxidative environment make between this anode and this cathode layer and produce an electromotive force, drive and promote that the nitrogen oxide in this oxygen-enriched combusting waste gas carries out a decomposition reaction in this cathode layer and forms nitrogen and oxygen.
2. the electric catalyst honeycomb of control toxic emission according to claim 1, is characterized in that, this anode has the hole of multiple attachment one carbon species.
3. the electric catalyst honeycomb of control toxic emission according to claim 1, it is characterized in that, the group that the material of this anode selects the Tao Jin of free metal and fluorite structure metal oxide composition, perovskite structure metal oxide, fluorite structure metal oxide, the perovskite structure metal oxide adding metal, the fluorite structure metal oxide adding metal and combination thereof to form.
4. the electric catalyst honeycomb of control toxic emission according to claim 1, is characterized in that, the group that the material of this shell selects free metal, pottery, glass and combination thereof to form.
5. the electric catalyst honeycomb of control toxic emission according to claim 1, is characterized in that, the material of this solid oxide nitride layer is selected from the group be made up of fluorite structure metal oxide, perovskite structure metal oxide and combination thereof.
6. the electric catalyst honeycomb of control toxic emission according to claim 1, it is characterized in that, the material of this cathode layer is selected from the group be made up of perovskite structure metal oxide, fluorite structure metal oxide, the perovskite structure metal oxide adding metal, the fluorite structure metal oxide adding metal and combination thereof.
7. the electric catalyst honeycomb of control toxic emission according to claim 1, is characterized in that, also comprises one and is arranged between this cathode layer with this solid oxide nitride layer to promote the boundary layer that this cathode layer is connected with this solid oxide nitride layer.
8. the electric catalyst honeycomb of control toxic emission according to claim 7, is characterized in that, the material of this boundary layer is selected from the group be made up of fluorite structure metal oxide, perovskite structure metal oxide and combination thereof.
9. the electric catalyst honeycomb of control toxic emission according to claim 1, is characterized in that, also comprises one and is attached to oxidation catalyst layer on this cathode layer.
10. the electric catalyst honeycomb of control toxic emission according to claim 9, is characterized in that, the group that the material of this oxidation catalyst layer selects free metal, alloy, fluorite structure metal oxide, perovskite structure metal oxide and combination thereof to form.
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