CN106731806A - A kind of cross-current type ceramics film device and method of denitration for gas denitration - Google Patents
A kind of cross-current type ceramics film device and method of denitration for gas denitration Download PDFInfo
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- CN106731806A CN106731806A CN201611241297.6A CN201611241297A CN106731806A CN 106731806 A CN106731806 A CN 106731806A CN 201611241297 A CN201611241297 A CN 201611241297A CN 106731806 A CN106731806 A CN 106731806A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8625—Nitrogen oxides
- B01D53/8631—Processes characterised by a specific device
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/20—Reductants
- B01D2251/206—Ammonium compounds
- B01D2251/2062—Ammonia
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- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
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Abstract
The present invention relates to a kind of cross-current type ceramics film device and method of denitration for gas denitration, belong to gas purification technique field.Mainly using the ceramic membrane with double-deck or sandwich construction, in ceramic membrane inner surface supported catalyst, and nitrogen oxides and ammonia cross-current type are fed, prepare the cross-current type ceramics film device for gas denitration.Wherein nitrogen oxides also carries out " aeration type " air inlet using the porous of ceramic membrane, is fully reacted in the presence of catalyst with the ammonia in ceramic membrane channels, and denitration efficiency is higher compared with conventional method.
Description
Technical field
The present invention relates to a kind of cross-current type ceramics film device and method of denitration for gas denitration, belong to gas purification skill
Art field.
Background technology
Nitrogen oxides (NOx) it is one of Air Pollutant Discharge, serious harm ecological environment and human health.Current denitration
One of conventional technology is ammonia selective catalytic reduction, and conventional method is that catalyst is coated in into honeycomb or porous ceramics
Carrier surface, by carrier as closed container in, two gangs of flue gas (high temperature NOxWith NH3) be pooled to a pipeline after flow into container,
NOxWith NH3Reaction generation N2And vapor, reach the purpose of denitration.
But this method of denitration is existed, and reaction efficiency is low, catalyst easily by impurities in feed gas pollution and in
The problem of poison.
The content of the invention
The present invention proposes a kind of Benitration reactor of the tubular ceramic membrane of utilization inner surface supported catalyst, by NOxWith N2
Separately charging, using the narrow and easily-controllable advantage of ceramic membrane pore-size distribution, the reactor utilizes the inner passage reality of tubular ceramic membrane
Existing cross flow effects, then feed NO from supporting layer sidexUnstripped gas, NOxThrough ceramic film outer surface through supporter and film layer duct " aeration
Formula " enters ceramic membrane channels, realizes and gets rid of partial impurities by porous support layer, and realizes NO by porous supporting bodyx
The steady feed of unstripped gas, realizes interfacial reaction, while using cross flow effects on the inner surface catalyst layer of tubular ceramic membrane
Product is removed, catalytic reaction efficiency is improve.
Technical scheme is：
The first aspect of the invention：
A kind of tubular ceramic membrane of supported catalyst, it is configured as tubular membrane, and the outer wall of ceramic membrane is porous support layer, porous
Supporting layer inside is passage, and denitration catalyst oxidant layer is loaded with the inner surface of porous support layer.
The material of described denitration catalyst oxidant layer is selected from CeO2、V2O5、MnO2、Fe2O3、TiO2、WO3, one kind in MgO or
The catalyst that several mixing is constituted.
Porous support layer is made up of ceramic film support layer from outside to inside and ceramic membrane film layer；Described tubular membrane
Inner passage quantity be one or more.
, 15~60%, aperture is at 10~100 μm for ceramic film support layer porosity；Ceramic membrane film layer porosity 15~
60%, aperture is at 0.5~20 μm.
The second aspect of the invention：
A kind of cross-current type ceramics film device for gas denitration, includes Benitration reactor housing, is internally provided with load and urges
The tubular ceramic membrane of agent, cavity is formed between the outside of the tubular ceramic membrane of supported catalyst and Benitration reactor housing,
Benitration reactor enclosure interior is additionally provided with seal, and seal leads to cavity with the inside of the tubular ceramic membrane of supported catalyst
Road is isolated, and the shell air inlet being connected with cavity is provided with Benitration reactor housing, on Benitration reactor housing also
It is provided with ceramic membrane air inlet to be connected with ceramic membrane gas outlet, is connected to the tubular ceramic membrane channels of supported catalyst
Two ends.
The third aspect of the present invention：
A kind of method of denitration, comprises the following steps：
I) will contain NO using the tubular ceramic membrane of supported catalystxUnstripped gas from the press-in of the pipe of tubular ceramic membrane outside
In membrane tube, and infiltrate into denitration catalyst oxidant layer；
Ii) will contain NH3Unstripped gas sent into from the passage of the tubular ceramic membrane of supported catalyst, and formation contains NH3's
Unstripped gas makes NH from passage surface cross-flow passes3And NOxCatalytic reaction is carried out in denitrating catalyst layer surface.
Reaction temperature is 320~380 DEG C, containing NH3Unstripped gas 4~80Kpa of feed pressure, the unstripped gas containing NOx enters
5~100Kpa of material pressure.
Beneficial effect
Mainly using the ceramic membrane with double-deck or sandwich construction, in ceramic membrane inner surface supported catalyst, and by nitrogen oxygen
Compound feeds with ammonia cross-current type, prepares the cross-current type ceramics film device for gas denitration.Wherein nitrogen oxides is also using pottery
The porous of porcelain film carries out " aeration type " air inlet, is fully reacted in the presence of catalyst with the ammonia in ceramic membrane channels, takes off
Nitre efficiency is higher compared with conventional method.
Brief description of the drawings
Fig. 1 is the cross-current type ceramics film device front view schematic diagram provided by the present invention for denitration；
Fig. 2 is the cross-current type ceramics film device top view schematic diagram provided by the present invention for denitration；
Fig. 3 is the ceramic membrane schematic top plan view of supported catalyst.
Wherein, 1, cavity；2nd, the tubular ceramic membrane of supported catalyst；3rd, shell air inlet；4th, ceramic membrane air inlet；5th, make pottery
Porcelain film gas outlet；6th, ceramic film support layer；7th, ceramic membrane film layer；8th, denitration catalyst oxidant layer；9th, ceramic membrane channels；10th, denitration
Reactor shell；11st, seal.
Specific embodiment
The invention provides a kind of ceramic membrane of supported catalyst, it is tubular membrane, both can be single hose, or
Multi-channel type（It is i.e. internal to have a plurality of duct）, the structure of single hose ceramic membrane is as shown in figure 3, pipe outer wall is ceramic film support layer
6, the inwall side of ceramic film support layer 6 sets ceramic membrane film layer 7, and catalyst layer 8 is set in the inwall side of ceramic membrane film layer 7,
Wherein ceramic film support layer 6 and ceramic membrane film layer 7 in other embodiments, both may be used as generally porous support layer
Individually to use support body layer, it is also possible to individually use ceramic membrane film layer, it would however also be possible to employ the support of ecto-entad arrangement successively
Body layer and film layer, as long as outside is supporting layer internal load catalyst layer, can realize the purpose of the present invention.
As the material of catalyst layer 8, via disclosed in prior art, can use such as：CeO2、V2O5、MnO2、
Fe2O3、TiO2、WO3, the catalyst that constitutes of the mixing of one or more in MgO.
The supporter can increase the mechanical strength of ceramic membrane, require it is have larger aperture and porosity, with
Increase the permeability of gas, reduce gas transporting resistance.The porosity of supporter is in 15~60%, more preferably 20~40%.
The film layer is used for supported catalyst, prevents the coating of catalyst and immersion supporter duct in sintering process, when
Support body aperture exists, can the direct catalyst layer on supporter.The porosity of film layer 15~60%, more preferably 20%~
40%。
At 10~5000 μm, preferred scope is 500~800 μm to described support body aperture.
At 0.5~200 μm, preferred scope is 50~100 μm in described film layer aperture.
The supporter is loose structure with film layer, mechanical strength and supported catalyst catalyst except increasing ceramic membrane
Effect beyond, can be used for being uniformly distributed, into the NO inside membrane tubexGas, allows NOxGas " aeration type " enters ceramic membrane
Passage, NOxGas and NH3Reacted in the presence of catalyst more abundant.
NO in the present inventionxRefer to oxynitrides, for example：NO、NO2Deng.
The cross sectional shape of passage can make selected from square, hexagon, triangle or circle, and the outer wall of membrane tube institute shape
Into cross sectional shape can also similarly be selected from these shapes, and the shape in section that the section of passage is formed with the outer wall of membrane tube
Shape can be with identical, it is also possible to different.In some cases preferably, preferably two cross sectional shapes are all identical, because convenient life
Produce processing；In addition, cross sectional shape is preferably using circular, with larger guarantee membrane area, and production shaping can be adapted to.
Described supporter and/or the material of film layer be selected from carborundum, diatomite, mullite, aluminum oxide, zirconium oxide or
Titanium oxide, wherein be particularly well-suited to the supporter and/or film layer of aluminum oxide, zirconium oxide and titanium oxide material because its have compared with
Good stability.
The structure of the reactor as depicted in figs. 1 and 2, includes Benitration reactor housing 10, is internally provided with load and urges
The tubular ceramic membrane 2 of agent, cavity is formed between the outside of the tubular ceramic membrane 2 of supported catalyst and Benitration reactor housing 10
1, seal 11 is additionally provided with inside Benitration reactor housing 10, seal 11 makes pottery the tubular type of cavity 1 and supported catalyst
The inner passage of porcelain film 2 is isolated, and the shell air inlet 3 being connected with cavity 1 is provided with Benitration reactor housing 10, is taken off
Ceramic membrane air inlet 4 is additionally provided with nitre reactor shell 10 to be connected with ceramic membrane gas outlet 5, is connected to supported catalyst
The two ends of the passage of tubular ceramic membrane 2 of agent.
During plant running, NOxWith NH3Separately charging, NOxEnter reactor from shell air inlet 3, and NH3From ceramics
Film air inlet 4 is fed, and reaction is produced and left from the ceramic membrane gas outlet 5 of the other end.It is narrow and easily-controllable using ceramic membrane pore-size distribution
Advantage, on ceramic film support or film layer load one layer of catalyst, NOxThrough ceramic film outer surface through supporter and film layer hole
Road " aeration type " enters ceramic membrane channels and NH3Mixing, and fully reacted in the presence of catalyst, generate N2With vapor.
Ceramic membrane denitration operation test
The ceramic membrane denitrification test apparatus structure that the present invention is used by many ceramic-film tubes as shown in figure 1, be mounted vertically in device
In, the cavity that device is internally formed is NOx(gas) shell side, the passage of ceramic-film tube is NH3(gas) tube side, NOxThrough membrane tube support
Body layer, film layer, catalyst layer enter the NH with slow flowing inside ceramic-film tube3Fully reacted in the presence of catalyst, it is raw
Into N2And vapor.
Embodiment 1
Test it is different it is following under the conditions of be all tested：
9 ceramic-film tubes are installed altogether in component, 3*3 arrangements are seen as from section, membrane tube length is 1m.Membrane tube is single tube, chi
Very little profile：Circle, external diameter 12mm, internal diameter 8mm.
Containing NO2Air from reactor shell side enter, NOxConcentration 1000mg/Nm3, 350 DEG C of temperature, pressure is 15KPa, stream
Amount 0.3m3/min。
Lead to NH in membrane tube passage3Pure ammonia after pure ammonia pyrolysis, enters film flow 0.3m3/ min, 310 DEG C of temperature, pressure is
10Kpa。
Using supporter and the porosity 45% of film layer, material is all the membrane tube of aluminum oxide, and the average pore size of supporter is 50
μm, 10 μm of film layer average pore size, 20 μm of catalyst layer thickness, is V2O5Catalyst, by after reaction, device exports NOxUnder concentration
It is down to 95mg/Nm3, denitration efficiency is 90.5%.
Embodiment 2
Test it is different it is following under the conditions of be all tested：
16 ceramic-film tubes are installed altogether in component, 4*4 arrangements are seen as from section, membrane tube length is 1.2m.Membrane tube is single tube,
Form factor：Circle, external diameter 20mm, internal diameter 14mm.
Containing NO2Air from reactor shell side enter, NOxConcentration 1000mg/Nm3, 320 DEG C of temperature, pressure is 18KPa, stream
Amount 0.5m3/min。
Lead to NH in membrane tube passage3Pure ammonia after pure ammonia pyrolysis, enters film flow 0.2m3/ min, 340 DEG C of temperature, pressure is
12Kpa。
Using supporter and the porosity 35% of film layer, material is all the membrane tube of zirconium oxide, and the average pore size of supporter is
1000 μm, film layer average pore size is respectively adopted 20,50,100,200 μm, and 20 μm of catalyst layer thickness, is V2O5Catalyst, passes through
After reaction, NO is exported under the conditions of different pore sizexConcentration and denitration efficiency are as follows
Embodiment 3
Test it is different it is following under the conditions of be all tested：
9 ceramic-film tubes are installed altogether in component, 3*3 arrangements are seen as from section, membrane tube length is 1.0m.Membrane tube is single tube,
Form factor：Circle, external diameter 10mm, internal diameter 5mm.
Containing NO2Air from reactor shell side enter, NOxConcentration 1500mg/Nm3, 360 DEG C of temperature, pressure is 12KPa, stream
Amount 0.4m3/min。
Lead to NH in membrane tube passage3Pure ammonia after pure ammonia pyrolysis, enters film flow 0.5m3/ min, 320 DEG C of temperature, pressure is
11Kpa。
Using supporter and the porosity 40% of film layer, material is all the membrane tube of zirconium oxide, the average pore size difference of supporter
Using 200,500,800,1000,2000 μm, film layer average pore size is respectively adopted 50 μm, and 15 μm of catalyst layer thickness, is V2O5Urge
Agent.
NO is exported under the conditions of different support body aperturesxConcentration and denitration efficiency are as follows：
Comparative example 1
Difference with embodiment 1 is：By NOxWith NH3Enter reactor, NO from charging aperture 42Gas and NH3Gas flow all phases
Together, reaction condition is identical, device outlet NOxConcentration drops to 540 mg/Nm3, denitration efficiency is 46%.
Claims (8)
1. a kind of tubular ceramic membrane of supported catalyst, it is characterised in that it is configured as tubular membrane, and the outer wall of ceramic membrane is porous
Supporting layer, is ceramic membrane channels inside porous support layer（9）, denitrating catalyst is loaded with the inner surface of porous support layer
Layer（8）.
2. the tubular ceramic membrane of supported catalyst according to claim 1, it is characterised in that described denitration catalyst oxidant layer
（8）Material be selected from CeO2、V2O5、MnO2、Fe2O3、TiO2、WO3, the catalyst that constitutes of the mixing of one or more in MgO.
3. the tubular ceramic membrane of supported catalyst according to claim 1, it is characterised in that porous support layer is by from outer
Ceramic film support layer in（6）With ceramic membrane film layer（7）Constituted；The ceramic membrane channels of the inside of described tubular membrane
（9）Quantity is one or more.
4. the tubular ceramic membrane of supported catalyst according to claim 1, it is characterised in that ceramic film support layer（6）
, 15~60%, aperture is at 10~100 μm for porosity；Ceramic membrane film layer（7）, 15~60%, aperture is at 0.5~20 μm for porosity.
5. a kind of cross-current type ceramics film device for gas denitration, it is characterised in that include Benitration reactor housing（10）,
The tubular ceramic membrane of the supported catalyst being internally provided with described in any one of Claims 1 to 4（2）, the tubular type of supported catalyst
Ceramic membrane（2）Outside and Benitration reactor housing（10）Between form cavity（1）, in Benitration reactor housing（10）Inside is also
It is provided with seal（11）, seal（11）By cavity（1）With the tubular ceramic membrane of supported catalyst（2）Inner passage be separated by
From in Benitration reactor housing（10）On be provided with and cavity（1）The shell air inlet being connected（3）, Benitration reactor housing
（10）On be additionally provided with ceramic membrane air inlet（4）With ceramic membrane gas outlet（5）It is connected, is connected to the pipe of supported catalyst
Formula ceramic membrane（2）The two ends of passage.
6. a kind of method of denitration, it is characterised in that comprise the following steps：
I) uses the tubular ceramic membrane of the supported catalyst described in any one of Claims 1 to 4（2）, NO will be containedxRaw material
Gas is from tubular ceramic membrane（2）Pipe outside press-in membrane tube in, and infiltrate into denitration catalyst oxidant layer；
Ii) will contain NH3Unstripped gas from the tubular ceramic membrane of supported catalyst（2）Passage feeding, and formation contain NH3
Unstripped gas from passage surface cross-flow passes, make NH3And NOxCatalytic reaction is carried out in denitrating catalyst layer surface.
7. method of denitration according to claim 6, it is characterised in that comprise the following steps：
I) uses the tubular ceramic membrane of supported catalyst（2）, NO will be containedxUnstripped gas from tubular ceramic membrane（2）Pipe outside
In press-in membrane tube, and infiltrate into denitration catalyst oxidant layer；
Ii) will contain NH3Unstripped gas from the tubular ceramic membrane of supported catalyst（2）Passage feeding, and formation contain NH3
Unstripped gas from passage surface cross-flow passes, make NH3And NOxCatalytic reaction is carried out in denitrating catalyst layer surface.
8. method of denitration according to claim 7, it is characterised in that reaction temperature is 320~380 DEG C, containing NH3Raw material
Gas 4~80Kpa of feed pressure, the 5~100Kpa of feed pressure of the unstripped gas containing Nox.
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| Application Number | Priority Date | Filing Date | Title |
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| CN201611241297.6A CN106731806B (en) | 2016-12-29 | 2016-12-29 | Cross-flow ceramic membrane device for gas denitration and denitration method |
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| CN201611241297.6A CN106731806B (en) | 2016-12-29 | 2016-12-29 | Cross-flow ceramic membrane device for gas denitration and denitration method |
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| CN108404658A (en) * | 2018-03-27 | 2018-08-17 | 华中科技大学 | A kind of anti-SO of raising honeycomb-shaped SCR catalyst2The method and product of performance |
| CN113877346A (en) * | 2021-10-27 | 2022-01-04 | 盐城工学院 | Flue gas filtering pipeline for industrial denitration |
| CN114563310A (en) * | 2021-05-08 | 2022-05-31 | 南京工业大学 | CO (carbon monoxide)2/N2Method for predicting diffusion process of binary mixture through multilayer ceramic membrane |
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| CN106731806B (en) | 2022-12-23 |
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