CN108786788A - A kind of removing dioxin in flue gas and NOxCatalyst and preparation method and application - Google Patents
A kind of removing dioxin in flue gas and NOxCatalyst and preparation method and application Download PDFInfo
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- CN108786788A CN108786788A CN201810643448.3A CN201810643448A CN108786788A CN 108786788 A CN108786788 A CN 108786788A CN 201810643448 A CN201810643448 A CN 201810643448A CN 108786788 A CN108786788 A CN 108786788A
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- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/32—Manganese, technetium or rhenium
- B01J23/34—Manganese
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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
- B01D53/34—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
- B01D53/8628—Processes characterised by a specific catalyst
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- 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
- B01D53/8659—Removing halogens or halogen compounds
- B01D53/8662—Organic halogen compounds
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- 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
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- B01D53/90—Injecting reactants
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Abstract
The present invention provides a kind of removing dioxin in flue gas and NO x Catalyst, with TiO2For carrier, in the active component of the Dispersion on surface of carrier, the active component is by MnO x And CeO2Composition.The present invention also provides above-mentioned removing dioxin in flue gas and NO x Catalyst preparation method.The present invention also provides the methods using above-mentioned catalyst removal dioxin in flue gas and NOx, flue gas after dust-extraction unit dedusting is inputted from pipeline in a device containing above-mentioned catalyst, ozone is sprayed into from another pipeline in the device containing catalyst, another described pipeline is provided with multiple jet apertures, flue gas, ozone and catalyst are sufficiently mixed in a device, and the flue gas after removing bioxin and NOx is discharged.The present invention is coupled using ozone with containing Mn catalyst, can cooperation-removal bioxin and NO x 。
Description
Technical field
The invention belongs to chemical fields, are related to a kind of processing method of flue gas, specifically being a kind of removing Yan gas Zhong bis- Evil
English and NOxCatalyst and preparation method and application.
Background technology
Waste incinerator tail flue gas Zhong bioxin and nitrogen oxides (NOx) emission control, it is that current field of environment protection receives
Concern and two large problems urgently to be resolved hurrily.In recent years, incineration disposal is because can effectively realize rubbish " minimizing, innoxious, resource
Change ", it is rapidly developed in China, though alleviating the pressure of China's " garbage-surrounded city " to a certain extent, burning is not filled
The secondary pollutions such as bioxin caused by point, it has also become various circles of society's focus of attention.The newest promulgation in Environmental Protection in China portion《Life
Waste incinerator emission standard GB18485-2014》Jiang the emission limit of bioxin by 1.0ng I-TEQ/Nm3It lowers
To 0.1ng I-TEQ/Nm3.According to investigations, China still has more than 2/3rds domestic waste incineration and cannot be satisfied new discharge
Standard.Therefore, develop and improve advanced control method to realize that it is extremely urgent that dioxin in incineration smoke discharge meets new standard.
Currently, dioxin emission control method mainly has two major classes:Inhibit first, bioxin generates;Second is that having generated two
Evil English carries out tail portion removing.Bioxin, which generates, to be inhibited to include mainly burning process optimization and inhibitor addition.It is i.e. excellent to burn optimization
Change burning condition, be such as uniformly mixed fuel, control suitable ignition temperature, kept for the appropriate residence time etc., to reduce not
Completely burned product generates.Inhibitor adds, that is, some sulfenyls or nitrilo compound is added, and is reacted and is pressed down by inhibition " Deacon "
The generation of preparing chlorine gas, to inhibit bioxin to generate.However, only Tong Guo bioxin generates inhibition to control the effect of its discharge capacity
It is limited, therefore need to also realizes the efficient removal of dioxin by end-of-pipe control means.
In recent years, active carbon adsorption is widely used in the control of bioxin end because device structure is simple, removal efficiency is high
System.But active carbon adsorption can only realize that bioxin pollutes the transfer from gas phase to solid phase, but cannot achieve the thorough of bioxin
It degrades at bottom.And thorough mineralising of the catalytic degradation method because that can realize bioxin, form CO2、H2O, the inorganic molecules such as HCl are without making
At secondary pollution, it is considered to be a kind of bioxin end-of-pipe control technology of optimal potentiality.
NOxFor one of another Air Pollutants that Refuse Incineration Process generates, easily cause photochemical fog, acid rain,
The series environmental problem such as greenhouse effects and depletion of the ozone layer, threatens environment for human survival and health.Ammonia (NH3) selectivity
Catalysis reduction (Selective Catalytic Reduction, SCR) method is currently widely used NO after burningxDischarge control
Method processed.Studies have shown that common NH3SCR denitration (main component V2O5-WO3/TiO2) it can also be used for catalysis drop
Xie bioxin.Such as utilize REMEDIA catalytic filtration systems (main component V2O5/WO3/TiO2) successfully taken off under the conditions of 260 DEG C
Except 99% bioxin in incineration flue gas, but by the system be applied to incinerator tail portion ammine selectivity catalytic reduction when, 220 DEG C of items
NOx removal efficiency under part is only 33%.Some researches show that by V2O5-WO3/TiO2Catalyst is heated to 300 DEG C, waste incineration
Stove tail flue gas Zhong bioxin and NOx catalytic eliminatings efficiency are respectively up to 97% and 90%;But when reaction temperature is reduced to 220 DEG C,
The two catalytic eliminating efficiency is reduced to 92% and 53% therewith.It is therefore seen that the existing NH of SCR catalyst3SCR denitration acts on, and energy
Effectively degradation bioxin.But traditional SCR catalyst activity is very sensitive to reaction temperature, and denitration activity temperature (300-400
DEG C) Yu bioxin catalytic degradation activity temperature (200-300 DEG C) is not or not same temperature area, therefore, is catalyzed currently with traditional SCR
Agent (V2O5/TiO2) it still cannot achieve efficient cooperation-removal under the conditions of the two low temperature (≤150 DEG C).Patent
CN201310751629.5 discloses a kind of Zheng bodies Shi bioxin Removal of catalyst and preparation method thereof, which is vanadium-tungsten-
Titanium system is tested under the conditions of 160~180 DEG C, and the conversion ratio for obtaining the degradation of bioxin reaches 95% or more, but the catalyst
To NO in tail gasxDegradation effect and do not specify.Patent 201510039629.1 discloses a kind of preparation of SCR denitration
The main component of method, the catalyst is Fe2O3, grain size is 35-65 mesh, and specific surface area reaches 93.76m2/ g, aperture 12nm,
Nitrogen oxides in effluent can be effectively removed, but the removal effect of dioxin in flue gas is not illustrated.Patent
201610865155.0 disclosing a kind of suitable for low temperature Synergistic degradation bioxin and NOxCatalyst and preparation method thereof, should
Catalyst carrier is TiO2Nano particle and titanium nanotube, main active component CeO2、V2O5And Pt, method for preparing catalyst
For infusion process, which is that , bioxin purification efficiencies reach 95% or more, NO within the scope of 140-300 DEG C in temperaturexPurification effect
Rate is only 80%, however the easy poisoning and deactivation of the catalyst.Patent 201510149492.5 disclose it is a kind of using ozone stage by stage
The method and device of exhaust gas is purified, the result shows that meeting GB18485-2014 standards by this method processing final vacuum, but simultaneously
The not yet explicitly removal efficiency of various vapor phase contaminants.
Invention content
For above-mentioned technical problem in the prior art, the present invention provides a kind of removing dioxin in flue gas and NOx's
Catalyst and preparation method and application, this removing dioxin in flue gas and NOxCatalyst and preparation method and answer
With solving to be unable to effective coordination removing dioxin in incineration smoke and NO in the prior artxThe technical issues of.
The present invention provides a kind of removing dioxin in flue gas and NOxCatalyst, with TiO2For carrier, in the table of carrier
Face is dispersed with active component, and the active component is by MnOx(x 2-4) and CeO2Composition, in the catalyst, Mn members
The mass percentage content of element is 1%-5%, and the mass percentage content of Ce elements is 5%-10%, the quality percentage of Ti elements
It is 40%-50% than content;Surplus is oxygen element.
Further, in the catalyst, the specific surface area ranging from 80-150m of catalyst2/g。
The present invention also provides above-mentioned removing dioxin in flue gas and NOxCatalyst preparation method, including walk as follows
Suddenly:
1) solution of tetrabutyl titanate, absolute ethyl alcohol and glacial acetic acid are weighed in proportion, at room temperature by solution of tetrabutyl titanate,
Absolute ethyl alcohol and glacial acetic acid are stirred to being uniformly mixed, and form solution A;
2) manganese nitrate, cerous nitrate, absolute ethyl alcohol and deionized water are weighed in proportion, by manganese nitrate, cerous nitrate, absolute ethyl alcohol
It is stirred at room temperature with deionized water to being uniformly mixed, forms solution B;
3) B solution is added dropwise in the solution A in high degree of agitation and forms solution C;Solution of tetrabutyl titanate, anhydrous second
Alcohol, glacial acetic acid, manganese nitrate, cerous nitrate, absolute ethyl alcohol and deionized water material ratio be 35ml:30ml:20ml:3ml:4.3g:
20ml:5-10ml;
4) by C solution stirring until solution be converted to vitreosol, then colloidal sol is placed under room temperature and forms gel for 24 hours,
Gel is placed in baking oven again, 105 DEG C of dryings 8 hours are subsequently placed in Muffle furnace and calcine;Muffle furnace is by room temperature with 10 DEG C/min
Heating rate rise to 300 DEG C stop 30min, be continuously heating to 550 DEG C stop 3h after be down to room temperature, by the catalyst after calcining
It is ground screening, obtains 40-60 mesh range catalyst particles.
The present invention also provides the methods using above-mentioned catalyst removal dioxin in flue gas and NOx, will be filled through dedusting
It sets the flue gas after dedusting to input in a device containing above-mentioned catalyst from pipeline, ozone is sprayed from another pipeline
Enter in the device containing catalyst, another described pipeline is provided with multiple jet apertures, flue gas, ozone and catalyst
It is sufficiently mixed in a device, the flue gas after removing bioxin and NOx is discharged.
Further, the temperature of the warm flue gas is 100-150 DEG C.
Further, ozone bioxin and NOxA concentration of 50-200ppm is added in gaseous mixture.
In the present invention, MnCeO is added as activator in ozonex/TiO2Composite catalyst, bioxin, NO and NH3Reaction
Catalyst low-temperature activity is improved in system and promotes bioxin and NO cooperation-removals.
It is originally used for NH3The SCR catalyst of SCR denitration design can also be used for bioxin catalytic degradation, but conventional scr is catalyzed
When agent is for the two cooperation-removal, there are problems that different under the conditions of low temperature (≤150 DEG C) while realizing the two efficient removal.
In consideration of it, the present invention selects MnOxAnd CeO2As catalyst main active component, TiO2As catalyst carrier, ozone conduct
Reacting movable agent, to realize bioxin and NOxEfficient (>=95%) cooperation-removal of low temperature (≤150 DEG C).
First, TiO2As catalyst carrier, is conducive to manganese cerium active component and disperses in its apparent height, help to improve
Catalyst low-temperature activity;
Secondly, MnOxIn a variety of oxidation state (such as Mn4+/Mn3+/Mn2+) mixing coexist, strengthen catalyst oxygen release ability:Mn
(II)-O keys are weak compared to Mn (III)-O and Mn (IV)-O, are more easy to release oxygen, and Mn2+(1.43) and Mn4+(1.95) electronegativity
Difference, the mobility of oxygen is strengthened because of electronics non-localized effect in Mn (II)-O-Mn (IV) structure;
Furthermore CeO2Because of Ce4+/Ce3+Between flexibly transformation have powerful oxygen storage capacity, the strong MnO with oxygen release abilityxKnot
Conjunction forms MnCeOxBinary catalyst can meet the double requirements for improving catalyst activity and enhancing anti-chlorine poisoning capability;
Finally, bioxin and NO is added as reacting movable agent in ozonexPromote the two cooperation-removal in gaseous mixture, it is main former
Because there is the following:
(1) ozone itself strong oxidation performance makes dioxin in flue gas and NOxMolecule pre-activate and it is readily removed;
(2) part NO can be aoxidized and be generated NO by ozone2, a small amount of NO is mixed in NO2Be conducive to NO and follow NO+NO2+2NH3→
2N2+3H2O equations carry out, and react (4NO+4NH compared to conventional scr3+O2→4N2+6H2O activation energy needed for) is lower;
(3) ozone is in MnCeOx/TiO2Composite catalyst surface, which is decomposed, generates stronger active group (such as O of oxidisability2 -、
O2 2-Deng), these active groups can reduce activation energy needed for bioxin degradation, promote bioxin Thermal degradation;
4) ozone and MnCeOx/TiO2There are synergistic effect, MnCeO between composite catalystx/TiO2Composite catalyst has
There is extremely strong ozone decomposed ability, therefore ozone utilization rate can be improved, ozone adds concentration down to 50-150ppm just to catalyst
Activity is obviously improved effect;Meanwhile ozone catalyst surface decomposition can increase catalyst surface active oxygen quantity and
Catalyst surface acidic site, to improve MnCeOx/TiO2Composite catalyst low temperature active.
Therefore, ozone coupling MnCeOx/TiO2Composite catalyst can realize bioxin and NOxLow temperature (≤150 DEG C) is efficient
(>=95%) cooperation-removal provides a kind of economical and efficient for the solution for the air combined pollution problem that current waste incineration causes
Multiple pollutant Collaborative Control new approaches.
The present invention is compared with prior art, and technological progress is significant.Catalyst , bioxin using the present invention and
NOx efficient cryogenic cooperation-removals, " low temperature " refer to 100-150 DEG C;" efficient " refers to that both bioxin and NOx removal efficiency are all high
In 95%.The present invention is coupled using ozone with containing Mn catalyst, for removing bioxin and NOx, can be used for degrading it
Its organic pollution, such as chlorobenzene class organic pollution and NOx cooperation-removals.
Description of the drawings
Fig. 1 is the catalyst removal dioxin in flue gas and NO of the present inventionxFlow chart.
Specific implementation mode
Embodiment 1
MnCeO is prepared with sol-gel method in the present inventionx/TiO2Composite catalyst, preparation process are as follows:It takes according to the ratio
34ml solution of tetrabutyl titanate, 30ml absolute ethyl alcohols and 20ml glacial acetic acid are stirred at room temperature to uniformly mixed and form solution A;It presses
Proportioning takes 3ml manganese nitrates, 4.3g cerous nitrates, 20ml absolute ethyl alcohols and 5-10ml deionized waters to be stirred at room temperature to uniformly mixed
Form solution B;B solution is added dropwise in the solution A in high degree of agitation and forms solution C;C solution is kept stirring until molten
Liquid is converted to vitreosol, and then colloidal sol is placed under room temperature and forms gel for 24 hours, then gel is placed in 105 DEG C of dryings 8 in baking oven
Hour, which is placed in Muffle furnace, calcines;Muffle furnace rises to 300 DEG C of stop 30min by room temperature with the heating rate of 10 DEG C/min, after
Continue and be down to room temperature after being warming up to 550 DEG C of stop 3h, the catalyst after calcining is ground screening, 40-60 mesh ranges is obtained and urges
Catalyst particles.
Embodiment 2
As shown in Figure 1, the low dirt low-temperature flue gas after 1 dedusting of dust-extraction unit inputs one from pipeline 2 and contains MnCeOx/
TiO2In the device 3 of composite catalyst;Ozone sprays into MnCeO through pipe special (pipeline contains several jet apertures)x/TiO2
Inside composite catalyst, the two is sufficiently mixed (5min) and realizes ozone and MnCeOx/TiO2Composite catalyst couples;Flue gas is passed through
Ozone and MnCeOx/TiO2(flue gas stream is 1s in the catalyst surface residence time in the device that composite catalyst couples in advance;
Flue gas stream total residence time in catalytic unit is less than 5s), remove bioxin and NOx" cleaning " flue gas afterwards is discharged.
In above-mentioned flue gas, NO/NH3Molar ratio=0.8-1, NO initial concentrations be 300-1000ppm , bioxin at the beginning of
Begin a concentration of 2.0-12.6ng I-TEQ/m3。
Further, the temperature of the low-temperature flue gas is 100-150 DEG C.
Further, ozone bioxin and NOxA concentration of 50-200ppm is added in gaseous mixture.
Ozone is conducive to Huoization bioxin and NO as activator, its own strong oxidizing propertyxMolecule, Wei bioxin and NOx?
Catalyst surface cooperation-removal is prepared;MnCeOx/TiO2Composite catalyst energy efficient-decomposition ozone generates the stronger work of oxidisability
Free love base;MnCeOx/TiO2Composite catalyst has extremely strong ozone decomposed ability, improves ozone utilization rate;Ozone exists
MnCeOx/TiO2Composite catalyst surface increases catalyst surface active oxygen quantity and surface acidity bit quantity while decomposition,
Improve catalyst low-temperature activity;It is adsorbed to catalyst surface bioxin and NOxMolecule, in MnCeOx/TiO2Composite catalyzing
It is degraded by efficient cryogenic under the collective effect of living radical after agent, ozone and ozone decomposed.
Utilize ozone coupling MnCeOx/TiO2Composite catalyzing agent method low temperature removes bioxin and NOxThe results are shown in Table 1.
1 ozone coupling MnCeO of tablex/TiO2Composite catalyst low temperature removes bioxin and NOx results
Claims (6)
1. a kind of removing dioxin in flue gas and NO x Catalyst, it is characterised in that:With TiO2For carrier, divide on the surface of carrier
Active component is dissipated, the active component is by MnO x And CeO2Composition, x 2-4, in the catalyst, the matter of Mn elements
Amount degree is 1%-5%, and the mass percentage content of Ce elements is 5%-10%, and the mass percentage content of Ti elements is
40%-50%;Surplus is oxygen element.
2. the catalyst of a kind of removing dioxin in flue gas and NOx according to claim 1, it is characterised in that described
In catalyst, the specific surface area ranging from 80-150 m of catalyst2/g。
3. the preparation method of the catalyst of a kind of removing dioxin in flue gas described in claim 1 and NOx, it is characterised in that packet
Include following steps:
1)Solution of tetrabutyl titanate, absolute ethyl alcohol and glacial acetic acid are weighed in proportion, at room temperature by solution of tetrabutyl titanate, anhydrous
Ethyl alcohol and glacial acetic acid are stirred to being uniformly mixed, and form solution A;
2)Manganese nitrate, cerous nitrate, absolute ethyl alcohol and deionized water are weighed in proportion, by manganese nitrate, cerous nitrate, absolute ethyl alcohol and are gone
Ionized water is stirred at room temperature to being uniformly mixed, and forms solution B;
3)B solution is added dropwise in the solution A in high degree of agitation and forms solution C;Solution of tetrabutyl titanate, absolute ethyl alcohol,
Glacial acetic acid, manganese nitrate, cerous nitrate, absolute ethyl alcohol and deionized water material ratio be 35 ml:30 ml:20ml:3ml:4.3g:20
ml:5-10ml;
4)By C solution stirring until solution is converted to vitreosol, then colloidal sol is placed under room temperature and forms gel for 24 hours, then will
Gel is placed in baking oven, and 105 DEG C of dryings 8 hours are subsequently placed in Muffle furnace and calcine;Muffle furnace is by room temperature with the liter of 10 DEG C/min
Warm rate rise to 300 DEG C stop 30 min, be continuously heating to 550 DEG C stop 3h after be down to room temperature, by the catalyst after calcining into
Row grinding screening, obtains 40-60 mesh range catalyst particles.
4. using the method for catalyst removal dioxin in flue gas and NOx described in claim 1, it is characterised in that:It will be through removing
Flue gas after dirt device dedusting is inputted from pipeline in a device containing catalyst described in claim 1, by ozone from
Another pipeline sprays into the device containing catalyst, another described pipeline is provided with multiple jet apertures, flue gas,
Ozone and catalyst are sufficiently mixed in a device, and the flue gas after removing bioxin and NOx is discharged.
5. the method for removing dioxin in flue gas and NOx according to claim 4, it is characterised in that:The warm flue gas
Temperature be 100-150 DEG C.
6. the method for removing dioxin in flue gas and NOx according to claim 4, it is characterised in that:Ozone bioxin
With a concentration of 50-200 ppm are added in NOx gaseous mixtures.
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Cited By (6)
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CN110368923A (en) * | 2019-07-23 | 2019-10-25 | 龙净科杰环保技术(上海)有限公司 | A kind of mesoporous denitration of middle low temperature takes off dioxin catalyst and preparation method thereof |
CN111841312A (en) * | 2020-07-27 | 2020-10-30 | 天津大学 | Method and device for removing chlorine-containing organic pollutants in flue gas by combining ozone catalysis with wet method |
CN111871070A (en) * | 2019-11-12 | 2020-11-03 | 南京工业大学 | Integrated filter material |
CN113466408A (en) * | 2021-06-23 | 2021-10-01 | 新疆生产建设兵团第八师生态环境监测站(石河子市生态环境监测站) | Mobile atmospheric ozone monitoring and processing device and method |
CN113499677A (en) * | 2021-07-26 | 2021-10-15 | 江苏百茂源环保科技有限公司 | Device for removing dioxin through catalytic oxidation for waste gas treatment and using method thereof |
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