CN202237742U - Reactor for processing PAHs (polycyclic aromatic hydrocarbons) by filtering and electro-catalytic oxidation - Google Patents
Reactor for processing PAHs (polycyclic aromatic hydrocarbons) by filtering and electro-catalytic oxidation Download PDFInfo
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- CN202237742U CN202237742U CN201120276807XU CN201120276807U CN202237742U CN 202237742 U CN202237742 U CN 202237742U CN 201120276807X U CN201120276807X U CN 201120276807XU CN 201120276807 U CN201120276807 U CN 201120276807U CN 202237742 U CN202237742 U CN 202237742U
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Abstract
The utility model discloses a reactor for processing PAHs (polycyclic aromatic hydrocarbons) by filtering and electro-catalytic oxidation. The reactor comprises a shell, wherein one end of the shell is provided with an air inlet and the other end of the shell is provided with an air outlet; the outer wall surface of the shell is wrapped with a metal conductor; the metal conductor is grounded and serves as a dielectric barrier discharge external electrode; a porous metal reactant loaded with a metal oxide catalyst is exactly arranged at the center in the shell; the porous metal reactant is connected with an AC (alternating current) power supply and serves as a dielectric barrier discharge internal electrode; the end of the porous metal reactant, close to the air inlet, is closed, and the end of the porous metal reactant, close to the air outlet, is open and communicated with the air outlet; a certain gap is reserved between the shell and the porous metal reactant to form a dielectric barrier discharge air gap; and the dielectric barrier discharge air gap is communicated with the air inlet. The reactor disclosed by the utility model can be used for effectively degrading gas-phase and solid-phase PAHs.
Description
Technical field
The utility model relates to the reactor that a kind of organic pollution is administered, and relates in particular to a kind of reactor that filters composite electro catalytic oxidation processes PAHs.
Background technology
Polycyclic aromatic hydrocarbon (Polycyclic aromatic hydrocarbons is called for short PAHs) is meant the organic compound that two or more phenyl ring connect together, like naphthalene, anthracene, phenanthrene, pyrene etc.The toxicity of PAHs shows as very strong carcinogenic, mutagenesis and teratogenesis, and carcinogenic PAHs that finds at present and derivative thereof surpass 400 kinds, and distribute extensively.PAHs mainly is the imperfect combustion of fossil fuel (like coal, oil, natural gas etc.), timber, paper and rubbish in the atmosphere, and the annual anthropogenic discharge in the whole world reaches the hundreds of thousands ton to the PAHs in the atmosphere.Because the poorly water-soluble of PAHs and chemical property are stable, belong to persistence organic pollutant, in environment, are the trend of continuous accumulation, human health and ecological environment are produced very big potential hazard.Airborne PAHs mainly with gas phase and particle mutually two kinds of forms exist, wherein the small-molecular weight PAHs of 2～3 rings mainly exists with gas phase, the PAHs of 4 rings is basic identical in the distribution in mutually of gas phase and particle; There is (R.G.M.Lee in the macromolecule PAHs of 5～7 rings then overwhelming majority mutually with particle; P.Coleman, J.L.Jones, et al.EnvironmentalScience & Technology; 2005,39:1436-1447; Y.J.Chen, G.Y.Sheng, X.H.Bi, et al.Environmental Science & Technology, 2005,39:1861-1867).
At present, also comparatively weak to the control of PAHs in the flue gas both at home and abroad.For the control of solid-state PAHs in the flue gas, generally solve through the mode of improving and improve dust removal performance, but since solid-state PAHs usually with PM
10Following fine particulate form exists, and conventional electrostatic precipitator is not good to the removal effect of this type of particle; And, do not have effective way at present for the control of gaseous state PAHs, and generally adopt adsorption technology, but the adsorbent after the absorption is often directly abandoned landfill, be easy to cause secondary pollution.Gas discharge under the low temperature plasma organic pollutant degradation techniques make use highfield produces materials such as having the active high energy electron of extensive chemical very, ion, free radical; These active particles all have very high efficient at aspects such as enhanced oxidation ability, promotion molecular dissociation and acceleration chemical reactions; Can carry out deep oxidation to the organic pollution of low concentration in the flue gas, generate harmless CO
2And H
2O.Dielectric barrier discharge makes plasma oxidation, catalytic oxidation performance synergy because technology such as ability and catalysis combine, the degradable organic pollutant of effective, harmless, thereby become one of optimal path of flue gas organic pollutant degradation gradually.Though existing research shows simple dielectric barrier discharge benzene, toluene, trichloro-ethylene etc. is had higher removal efficiency, has problems such as capacity usage ratio is low, carbonation rate is not high.People such as Magureanu (M.Magureanu; N.B.Mandache, et al.Applied Catalysis B-Environmental, 2007; Find when 74:270-277) the working medium barrier discharge is handled trichloro-ethylene; Though obtained 90% removal efficiency, energy density has reached 500J/L, in addition CO in the accessory substance
2Selection rate also have only 25%, generated more CO in the processing procedure.Recently, in order to overcome the shortcoming of simple dielectric barrier discharge, combining medium barrier discharge and chemical catalysis are handled organic pollution and are progressively grown up, removal efficiency, capacity usage ratio and CO
2Selection rate all increase (T Hammer, T.Kappes, et al.Catalysis Today, 2004,89:5-14; R.B.Sun, Z.G.Xi, et al.Atmospheric Environment, 2007,41:6853-6859).People such as Delagrange (S.Delagrange, L.Pinard, et al.AppliedCatalysis are B.2006:68:92-98) find that dielectric barrier discharge combines MnO
2/ γ-Al
2O
3When catalyst can make toluene conversion from independent discharge 36% brings up to 88%, CO
2The ratio of/CO brings up to 1.3, while MnO from 0.75
2Can effectively suppress O
3The generation of this accessory substance.
But, but rarely has report at present for the processing of PAHs.The concentration of PAHs in flue gas is lower, and existence form is more various, and structure is more stable, utilizes the dielectric impedance micro discharge to remove difficulty more.To really realize the effective elimination of PAHs in the dielectric impedance micro discharge flue gas, must capture at the absorption of gas phase PAHs, solid phase PAHs, the aspects such as reinforcement of plasma-catalytic oxidation performance have breakthrough.
Summary of the invention
The utility model is to present reluctant low concentration PAHs waste gas; A kind of reactor that filters composite electro catalytic oxidation processes PAHs waste gas is provided; This device integrates plasma oxidation, filtration and chemical catalytic oxidation, gives full play to each technological advantage and synergy, has increased the time of staying of PAHs in reactor greatly; Can realize the efficient degradation of the PAHs of gas phase and solid phase, simultaneously the effectively generation of control harmful side product.
A kind of reactor that filters composite electro catalytic oxidation processes PAHs comprises housing, and described housing one end is an air inlet, and the other end is the gas outlet; The outside wall surface coated metal conducting objects of housing, metallic conduction thing ground connection is as the external electrode of dielectric barrier discharge; The enclosure interior middle is provided with the porous metals reagent of metal oxide supporting catalyst, and the porous metals reagent connects the interior electrode of AC power as dielectric barrier discharge; The porous metals reagent is communicated with near an end opening of gas outlet and with the gas outlet near the end sealing of air inlet; Leave certain clearance between described housing and the porous metals reagent, form the dielectric barrier discharge air gap, said dielectric barrier discharge air gap is communicated with air inlet.
In order to produce in the discharge air-gap that guarantees dielectric barrier discharge evenly, to disperse and stable micro discharge; Gap between reactor middle shell and the porous metals reagent (being the spacing of dielectric barrier discharge air gap) is generally 1～4mm, and this moment, discharge voltage was greatly about 10kV～30kV.
In order to produce more uniform and stable micro discharge; The general preferred thickness of described metallic conduction thing is 0.5～1mm; Promptly adopt metal forming or metal coating; Metal forming or metal coating are wrapped in the quartz glass tube outer wall closely, reduce the discharge between reactor outside wall surface and the housing, improve energy efficiency.Be preferably silver, copper or aluminium as the material of described metal material conducting objects.
Described porous metals reagent is the porous material with rigid structure that is made through compression moulding and high temperature sintering by spherical or erose powder of stainless steel, and metal oxide supporting catalyst.The metal oxide catalyst of load is preferably the oxide (TiO of titanium, cobalt or manganese
x, CoO
xOr MnO
x), adopt the oxide of titanium, cobalt, manganese can under lower temperature, (100～300 ℃) react as catalyst, avoid the condition of high temperature of PAHs degraded, help oxidative free radical and catalyst generation concerted reaction simultaneously, improve the degradation effect of PAHs.Supported catalyst dosage accounts for 3%～5% of porous metals reagent gross mass.
Described metal oxide catalyst adopts the dipping method load; At first the nitrate solution with the Ti, Co or the Mn that prepare floods the stainless steel metal reagent; Afterwards at air drying, and then under 400～500 ℃ temperature, carry out the calcining of 5h, cooling is at last weighed.This porous metals reagent has characteristics such as density is little, porosity is high, specific area is big.The porous metals reagent also is the carrier of catalyst not only as sparking electrode, simultaneously solid phase PAHs is had good filtration crown_interception.
In order to obtain bigger reaction specific area, the less resistance that passes through has filter effect preferably to fine PAHs particle simultaneously, and the porosity of general porous metals reagent is greater than 60%, and the aperture is less than 0.1mm.
Preferably, said AC supply voltage is 10～30kV.
Described reactor can be processed into tubular type or plank frame.In order to guarantee that reacting gas can be with less resistance through the porous metals reagent, require the circulation area of circulation area and porous metals reagent of dielectric barrier discharge basic identical.
For tubular structure, a kind of housing of preferred reactor and porous metals reagent are tubulose, and the external diameter of porous metals reagent is 7～13mm, and wall thickness is 2～3mm.
For plank frame; A kind of housing of preferred reactor and porous metals reagent cross section are rectangle; One relative wall of porous metals reagent is close to the inwall of housing, and isolates with insulating materials, leaves discharge air-gap between wall that another is relative and the inner walls.The relative distance that leaves between the described and inner walls between the wall of discharge air-gap is 4～10mm, and wall thickness is 3～5mm.
Pending PAHs waste gas gets into from the reactor air inlet, at first passes through the dielectric barrier discharge air gap.In the dielectric barrier discharge process, form a lot of micro discharge channels in the discharge air-gap, produce a large amount of high energy electron and living radical, these active materials and PAHs react, and realize tentatively degraded.After preliminary degraded, be filtered the time for the PAHs of solid phase and be retained in its surface, thereby prolonged the time of staying in reactor greatly through the porous metals reagent.Be not able to do in time reactive activity material and the gas phase PAHs that in discharge process, produces simultaneously on porous metals reagent surface and inner and metal oxide catalyst act synergistically, the active material of generation longer life has improved catalytic oxidation performance.And be filtered the PAHs that is retained in the surface deep oxidation reaction taking place under the effect of catalyst, finally changes into harmless CO
2And H
2O.
The filtration composite electro catalytic oxidation processes PAHs reactor of the utility model; The reagent that the porous metal material that will form with metal oxide catalyst and powder of stainless steel mixed sintering is made is as interior electrode; It is not only sparking electrode, also is the carrier of catalyst.Porous metal bodies has the advantages that the aperture is little, porosity is high and specific area is big, and the PAHs of gas phase is had good handling capacity, has good filter capacity for the PAHs of solid phase.For the PAHs of gaseous state, at first in the dielectric barrier discharge gap, accomplish preliminary oxidation, next can fully contact with its inner metal oxide catalyst during through the porous metals reagent at it, further accomplish the catalytic oxidation of the degree of depth; For some small solid-state PAHs, when its process porous metals reagent, can be retained down on porous metals reagent surface, prolong its reaction time greatly, and under catalysed oxidn, finally change into harmless CO
2And H
2O.
The beneficial effect that the utility model compared with prior art has:
1,, can make it uniformly through interior electrode for the PAHs of gaseous state.Because the porous metals reagent is to be formed by the powder of stainless steel sintering, and supported catalyst, it is big to have specific area, and porosity is high, and catalytic reaction waits characteristics fully, can realize the degree of depth degraded of gaseous state PAHs.
2, for solid-state PAHs, it at first is retained down at interior electrode surface, prolong the time of staying of reaction greatly, can make it finally be oxidized to harmless CO through electrocatalysis afterwards
2And H
2O.
Description of drawings
Fig. 1 is the utility model cartridge reactor structural representation;
Fig. 2 is Fig. 1 reactor A-A cross-sectional view;
Fig. 3 is the utility model plate-type reactor structural representation;
Fig. 4 is Fig. 3 reactor B-B cross-sectional view.
Wherein:
1-housing 2-metallic conduction thing 3-porous metals reagent 4-air inlet
5-gas outlet 6-ac high voltage source 7-discharge air-gap
The specific embodiment
The reactor of a kind of barrel type filtering composite electro catalytic oxidation processes PAHs as depicted in figs. 1 and 2 comprises that cross section is circular housing 1 (urceolus) and porous metals reagent 3 (inner core).Urceolus is quartz glass tube or pottery, the outside wall surface coated metal conducting objects 2 of quartz glass tube or pottery, and metallic conduction thing 2 ground connection are as the external electrode of dielectric barrier discharge.Metallic conduction thing 2 is thickness 0.5～1mm metal forming or metal coating, and material is silver, copper or aluminium.Inner core connects ac high voltage source 6 (10～30kV) the interior electrodes as dielectric barrier discharge.Porous metals reagent 3 is to make the porous material with rigid structure by spherical or erose powder of stainless steel through compression moulding and high temperature sintering, and metal oxide supporting catalyst.The catalyst of load is preferably TiO
x, CoO
xOr MnO
x, load capacity generally accounts for 3%～5% of porous metals reagent gross mass.Metal oxide catalyst adopts the dipping method load, at first with the Ti, Co or the Mn nitrate solution that prepare metal reaction body 3 is flooded, and afterwards at air drying, under 400～500 ℃ temperature, carries out the calcining of 5h then, and cooling is at last weighed.The external diameter of porous metals reagent 3 is 7～13mm, and wall thickness is 2～3mm, and porosity is greater than 60%, and the aperture is not more than 0.1mm.Inner core is communicated with near perforate in the middle of the end of gas outlet 5 and with gas outlet 5 near the end sealing of air inlet 4.Form the discharge air-gap 7 of dielectric impedance between urceolus and the inner core, in order to produce uniform and stable discharge, the spacing of general discharge air-gap 7 is 1～4mm.
Like the reactor of Fig. 3 and a kind of board-like filtration composite electro catalytic oxidation processes PAHs shown in Figure 4, comprise the housing 1 of quartz glass or pottery, housing 1 one ends are air inlet 4, the other end is gas outlet 5; The outer coated metal conducting objects 2 of housing 1, metallic conduction thing 2 ground connection are as the external electrode of dielectric barrier discharge; Metallic conduction thing 2 is thickness 0.5～1mm metal forming or metal coating, and material is silver, copper or aluminium.One porous metals reagent 3 is arranged in the housing 1, porous metals reagent 3 connect ac high voltage source 6 (10～30kV), as the interior electrode of dielectric barrier discharge.The cross section of housing 1 and porous metals reagent 3 is rectangle, and a relative wall of reagent 3 is close to the inwall of housing 1, and isolates with insulating materials; Another relative wall is an expanded metal, and expanded metal is to be formed by the powder of stainless steel sintering, and metal oxide supporting catalyst.The catalyst of load is preferably TiO
x, CoO
xOr MnO
x, load capacity generally accounts for 3%～5% of porous metals reagent gross mass.Metal oxide catalyst adopts the dipping method load, at first with the Ti, Co or the Mn nitrate solution that prepare metal reaction body 3 is flooded, and afterwards at air drying, under 400～500 ℃ temperature, carries out the calcining of 5h then, and cooling is at last weighed.The porous metals thickness of slab is 3～5mm, and the spacing of expanded metal is 4～10mm relatively; The porosity of expanded metal is greater than 60%, and the aperture is not more than 0.1mm.Leave discharge air-gap 7 between expanded metal and the inner walls, the spacing of discharge air-gap 7 is 1～4mm.
Pending PAHs waste gas gets into reactor from air inlet 4, at first through 1～4mm dielectric barrier discharge air gap 7.In the dielectric barrier discharge process, can form a lot of micro discharge channels in the discharge air-gap 7, produce a large amount of high energy electron and living radical, electron collision reaction or chain type chemical reaction take place in these active materials and PAHs, can realize the preliminary degraded of PAHs.The PAHs of preliminary afterwards degraded realizes through porous metals reagent 3 being discharged by gas outlet 5 after the degraded of the degree of depth.
Application examples 1
Adopt the barrel type filtering composite electro catalytic oxidation reactor of embodiment 1 to carry out the processing of naphthalene, exhaust gas flow 50mL/min, naphthalene concentration 48mg/m
3, quartz glass outerwrap 0.5～1mm silver coating, porous metals reagent porosity 80%, aperture 20um, load 3%MnO
2Catalyst, the discharge air-gap of dielectric barrier discharge are 4mm, and behind the ac high-voltage of input 24kV, the degradation efficiency of naphthalene reaches as high as more than 95%.
Claims (5)
1. a reactor that filters composite electro catalytic oxidation processes PAHs comprises housing, it is characterized in that: described housing one end is an air inlet, and the other end is the gas outlet; The outside wall surface coated metal conducting objects of housing, metallic conduction thing ground connection is as the external electrode of dielectric barrier discharge; The enclosure interior middle is provided with the porous metals reagent of metal oxide supporting catalyst, and the porous metals reagent connects the interior electrode of AC power as dielectric barrier discharge; The porous metals reagent is communicated with near an end opening of gas outlet and with the gas outlet near the end sealing of air inlet; Leave certain clearance between described housing and the porous metals reagent, form the dielectric barrier discharge air gap, said dielectric barrier discharge air gap is communicated with air inlet.
2. reactor as claimed in claim 1 is characterized in that: the gap between described housing and the porous metals reagent is 1～4mm.
3. reactor as claimed in claim 1 is characterized in that: the thickness of described metallic conduction thing is 0.5～1mm.
4. reactor as claimed in claim 1 is characterized in that: described housing and porous metals reagent are tubulose; The external diameter of porous metals reagent is 7～13mm, and wall thickness is 2～3mm, and porosity is greater than 60%, and the aperture is not more than 0.1mm.
5. reactor as claimed in claim 1; It is characterized in that: described housing and porous metals reagent cross section are rectangle; One relative wall of reagent is close to the inwall of housing, and isolates with insulating materials, leaves discharge air-gap between wall that another is relative and the inner walls; The relative distance that leaves between the described and inner walls between the wall of discharge air-gap is 4～10mm, and wall thickness is 3～5mm.
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201120276807XU CN202237742U (en) | 2011-08-02 | 2011-08-02 | Reactor for processing PAHs (polycyclic aromatic hydrocarbons) by filtering and electro-catalytic oxidation |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201120276807XU CN202237742U (en) | 2011-08-02 | 2011-08-02 | Reactor for processing PAHs (polycyclic aromatic hydrocarbons) by filtering and electro-catalytic oxidation |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103877842A (en) * | 2012-12-21 | 2014-06-25 | 陈晓波 | Efficient plasma waste gas treatment device |
| CN105013301A (en) * | 2015-07-13 | 2015-11-04 | 江苏保丽洁环境科技股份有限公司 | Tubular exhaust gas treating device based on dielectric barrier discharge plasmas |
| CN105056858A (en) * | 2015-07-20 | 2015-11-18 | 浙江工商大学 | Reactor and method for preparing synthesis gases through reforming greenhouse gases |
-
2011
- 2011-08-02 CN CN201120276807XU patent/CN202237742U/en not_active Expired - Fee Related
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103877842A (en) * | 2012-12-21 | 2014-06-25 | 陈晓波 | Efficient plasma waste gas treatment device |
| CN105013301A (en) * | 2015-07-13 | 2015-11-04 | 江苏保丽洁环境科技股份有限公司 | Tubular exhaust gas treating device based on dielectric barrier discharge plasmas |
| CN105013301B (en) * | 2015-07-13 | 2017-07-21 | 江苏保丽洁环境科技股份有限公司 | Tubular type dielectric barrier discharge plasma emission-control equipment |
| CN105056858A (en) * | 2015-07-20 | 2015-11-18 | 浙江工商大学 | Reactor and method for preparing synthesis gases through reforming greenhouse gases |
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| CF01 | Termination of patent right due to non-payment of annual fee |
Granted publication date: 20120530 Termination date: 20140802 |
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