CN110152467A - A kind of flue gas deep treatment method of absorption process synchronized desulfuring and denitrifying - Google Patents
A kind of flue gas deep treatment method of absorption process synchronized desulfuring and denitrifying Download PDFInfo
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- CN110152467A CN110152467A CN201910524826.0A CN201910524826A CN110152467A CN 110152467 A CN110152467 A CN 110152467A CN 201910524826 A CN201910524826 A CN 201910524826A CN 110152467 A CN110152467 A CN 110152467A
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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
- B01D53/46—Removing components of defined structure
- B01D53/60—Simultaneously removing sulfur oxides and nitrogen oxides
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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
- B01D53/80—Semi-solid phase processes, i.e. by using slurries
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Abstract
It is Natural Manganese oxide ore to add surfactant or synthesis nano manganese oxide as NO the invention discloses a kind of flue gas deep treatment method of absorption process synchronized desulfuring and denitrifyingxAnd SO2Absorbing liquid, realize gas cleaning.The method of synchronized desulfuring and denitrifying of the present invention, SO2Removal efficiency maintains 95% or more, NO removal efficiency and maintains 80% or more, and reaction product is separable to be utilized, and operating cost is low, has good prospect.
Description
Technical field
The invention belongs to Air Pollution Control Engineering fields, and in particular to wet absorption method synchronized desulfuring and denitrifying fume treatment
Method.
Background technique
All kinds of boilers, kiln generate a large amount of SO during high-temp combustion2, NOx, cause the whole nation 81.6% city occur
Acid rain.Discharged nitrous oxides also result in the Regional Environmental Pollutions problem such as photochemical fog and depletion of the ozone layer.Advanced control nitrogen
The technology of emissions of oxides include selective catalytic oxidation (SCO), non-selective catalytic reduction (SNCR) and selective catalysis also
Former (SCR) etc..Sulfur removal technology is based on wet process, semidry method, wherein account for market proportion 85% is left again based on calcium method desulfurization
It is right.The widely used flue gas purifying technique in China is that " high temperature SCR denitration+dedusting+wet desulphurization " combination smoke handles work at present
On the one hand skill consumes a large amount of ammonia, there are the escaping of ammonia risk, on the other hand the desulfurization stone of a large amount of more difficult resource utilization of by-product again
Cream.Respectively separate, individual flue gas desulfurization and denitrification technology, one-time investment is big, operating cost is high, takes up a large area, and synchronizes
Desulphurization denitration technology is expected to overcome these difficulties.
China belongs to the main manganese in the world and contains state, Hunan, Hubei, Sichuan, Chongqing, Guangxi, Anhui, Yunnan, Gansu, Ningxia and
The central and west regions such as Qinghai Mn oxide ore reserve is abundant, and Di Kan department, country finds on Guizhou, Guangxi and other places again in recent years
Several ultra-large type manganese ores mineral deposit has verified manganese resource total amount and has reached 13.8 hundred million tons.Although China's pyrolusite is resourceful, manganese
Ore quality is generally poor, and most of is low-grade manganese mineral deposit, so that low-grade Mn oxide ore resource is in metallurgy, chemical industry
Field utilizes and is restricted.Using the exploratory development of low-grade Mn oxide ore resource exploitation Environmental Engineering Material to the dvimanganese
The application and environmental protection technology progress of ore resources have great importance.From the point of view of existing open source literature data, both at home and abroad
There is flue gas wet absorption synchronized desulfuring and denitrifying research work, and obtain certain achievement, such as: using chlorous acid in patent CN1843574A
As liquid absorbent, the additive is calcium hypochlorite, sodium bicarbonate, hydrogen peroxide, disodium hydrogen phosphate or hydrogen for sodium and additive
Under the catalysis of additive, oxidisability is greatly mentioned for one of calcium oxide or combinations thereof, chlorite and series of intermediate products
Height promotes SO2With the oxidation of NO, to greatly improve absorbing liquid to SO2、NOxAbsorption, and use jet bubbling
Reactor absorbs.Patent CN107744715A is using the primary product ammonium sulfite during the ammonia process of desulfurization as NO, SO2Absorption
Agent is added absorbefacient CuO using Bubbling method and in absorbing liquid, solves the problems, such as that NO is insoluble in water, but there are ammonia volatilizations etc.
Secondary pollution problem.Patent CN101574617B is using the ore pulp that pyrolusite and metal-chelator are configured to as absorbent, to combustion
SO in flue-gas2、NOxSynchronous absorbing and removing, metal-chelator is for removing the multivalence such as calcium in pyrolusite pulp, magnesium, lead, zinc, iron
Metal ion, the problem of eliminating precipitation by metallic ion scale effect desulfurization interfacial reaction, sulphur can be utilized by being separated by solid-liquid separation post mother liquor
The poor solubility of both sour manganese and manganese nitrate at the same temperature is realized the recycling of sulphur, manganese, but is being inhaled there is no NO is improved
The dissolubility for receiving liquid, has that NO removal rate is low.
When forefathers' research is using strong oxidizers such as sodium chlorite, ozone, although NO, SO2Removal efficiency is higher, but oxidant
Mostly costly, investment cost and operating cost are higher, it is difficult to industrial applications;If using relatively inexpensive ammonium sulfite,
The absorbing liquids such as pyrolusite pulp, then NO removal rate is lower, generally 60-70%, it is difficult to reach industrial discharge standard.In view of above not
Foot, the scientific worker of environment protection field are badly in need of developing a kind of cheap, efficient wet flue gas synchronized desulfuring and denitrifying method.
Summary of the invention
To avoid above-mentioned existing deficiencies in the technology, the present invention provides a kind of absorption process synchronized desulfuring and denitrifyings
Flue gas deep treatment method, it is intended to can with lower cost realize NO, SO2Efficient removal.
The present invention is to realize goal of the invention, is adopted the following technical scheme that
A kind of flue gas deep treatment method of absorption process synchronized desulfuring and denitrifying, it is characterised in that:
(1) Mn oxide ore or commercial synthesis nano manganese oxide, grinding is selected to become the superfine powder of 325 meshes
Body;
(2) superfine powder is mixed with water according to mass ratio 1:10~40, is made into suspension;
(3) surfactant for accounting for the 1-5% of the suspension quality is added in the suspension of Xiang Suoshu, is then adjusted with acid
PH to 2~6 is saved, that is, obtains the absorbing liquid for being used for synchronized desulfuring and denitrifying;
(4) absorbing liquid is added in flue gas washing absorption plant, to remove the SO in flue gas2And NOx, after processing
SO2Removal efficiency maintains 95% or more, NOxRemoval efficiency maintains 80% or more;
(5) to SO2Removal efficiency is considered as absorbing liquid failure lower than 80%;Failure absorbing liquid is separated by solid-liquid separation, solids is discarded
Matter, remaining liq obtain manganese sulfate and manganese nitrate by-product through evaporative crystallization, or by remaining liq directly as liquid fertilizer
Raw material sale.
Further, the mass percent of manganese dioxide is greater than 25% in the Mn oxide ore, manganese oxygen therein
Compound mineral are at least one of cryptomelane, manganese calcium mine and birnessite.
Further, the Mn oxide ore is nano-mineral, and crystal diameter is less than 90 nanometers.
Further, the surfactant is polyethylene glycol.
Further, the flue gas washing absorption plant includes but is not limited to column plate type, material filling type, bubble type, is sprayed
Formula, fountain scrubbing tower.
Further, the method referenced patent of manganese sulfate and manganese nitrate by-product is obtained through evaporative crystallization
CN101574617B。
The beneficial effects of the present invention are embodied in:
1, Mn oxide ore is natural nano-mineral material, from a wealth of sources, cheap, de- as wet process synchronized desulfuring
The active material of nitre, has the function of synchronized desulfuring and denitrifying.Mn oxide is natural oxidant, can be aoxidized in flue gas
SO2It is converted into sulfate (equation 1):
MnO2+SO2——Mn2++SO4 2-(1);
Manganese oxide particle is smaller, specific surface area is bigger, with SO2Reactivity is higher, and desulfurization effect is better.Mn oxide
Mn oxide is mainly nano whiskers particle in ore, is coated on clay mineral surface, or by needle-shaped manganese oxide particle shape
At pilotaxitic texture, mineral intergranular pore is flourishing, porosity is high, and reactivity is high.
2, the surfactant that the method for the present invention uses has the function of stablizing liquid film, when can extend microbubble stabilization
Between and gas in SO2、NOxWith the Mn oxide reaction time, accelerate SO in gas phase2、NOxMigration to liquid phase improves SO2、NOxIt goes
Except efficiency.
3, present invention warp experimental studies have found that, there are weak interactions by the surfactant that adds in absorbing liquid and NO, increase
The big solubility of NO in the liquid phase, the problem of accelerating NO rate of dissolution, overcome NO indissoluble in absorption process, this is this hair
One of the precondition of bright wet high-effective denitrating flue gas.
4, it is a discovery of the invention that nano manganese oxide has the function of autoxidation and catalytic oxidation NO (equation 2,3), oxidation is produced
Object is NO2, due to NO2Solubility is high, is extremely easily converted to stable nitrate, the oxidation of NO accelerates gas in turn
The dissolution of middle NO, improves denitration efficiency:
MnO2+NO——Mn2++NO3 - (2)
NO+O2——NO3 - (3)。
5, the method for the invention realizes synchronized desulfuring and denitrifyings, and are suitable for low temperature or containing toxic catalyst flue dust
Gas cleaning.As long as flue-gas temperature reaches 60 DEG C, SO295% or more removal rate, NO purification efficiency can reach 80% or more, gram
The shortcomings that having taken SCR denitration.
6, method of the invention can use Mn oxide ore, while realizing synchronized desulfuring and denitrifying, both recycle
Nitrogen oxides in flue gas becomes nitrate, and handles manganese ore and prepare manganese sulfate and manganese nitrate.Compared to SCR ammonia NO also
It originally was that useless nitrogen is more environmentally protective.
Detailed description of the invention
Fig. 1 is the SEM image of Mn oxide ore used in Examples 1 to 3, it will thus be seen that Mn oxide is in acicular morphology,
Interleaved arrangement, crystal diameter 50-90nm.
Fig. 2 is to absorb synchronized desulfuring and denitrifying experimental provision, figure label: 1-Ar gas cylinder, 2-O2/ Ar gas cylinder, 3-NO/Ar gas
Bottle, 4-SO2/ Ar gas cylinder, 5- mass flowmenter, 6- gas mixer, 7-pH/ temperature monitor, 8- absorbing reaction device, 9- gas
Release head, 10- heat magnetic stirring apparatus, 11- water-bath, 12- sulfuric acid drying bottle, 13- flue gas analyzer.
Fig. 3 is synchronized desulfuring and denitrifying effect versus time curve in embodiment 1, experiment condition are as follows: [NO]=[SO2]
=1000ppm;[O2]=9%;PEG mass concentration 3%;Flue gas flow 100mL/min;Initial pH=4;Solid-to-liquid ratio=1:10;T
=60 DEG C of
Fig. 4 is influence of the Polyethylene glycol to denitrification efficiency in embodiment 2, experiment condition are as follows: [NO]=[SO2]
=1000ppm;[O2]=9%;Flue gas flow 100mL/min;Initial pH=4;Solid-to-liquid ratio=1:20;T=60 DEG C.
Fig. 5 is influence of the absorbing liquid temperature to denitrification efficiency in embodiment 3, experiment condition are as follows: [NO]=[SO2]=
1000ppm;[O2]=9%;PEG mass concentration 3%;Flue gas flow 100mL/min;Initial pH=3;Solid-to-liquid ratio=1:30.
Structural schematic diagram of the Fig. 6 for material filling type absorption tower in embodiment 5,1- shell, 2- air inlet, the gas outlet 3-, 4- are more
Dummy receptacle, 5- metal packing silk screen, 6- rotation spray shower pipe, 7- absorbing liquid circulation pipe.
Specific embodiment
In order to make the foregoing objectives, features and advantages of the present invention clearer and more comprehensible, below with reference to embodiment to this hair
Bright specific embodiment is described in detail.The following contents is only to design example of the invention and explanation, institute
Belong to those skilled in the art to make various modifications or additions to the described embodiments or using similar
Mode substitutes, and as long as it does not deviate from the concept of invention or beyond the scope defined by this claim, should belong to the present invention
Protection scope.
Embodiment 1
Select Anhui somewhere Mn oxide ore, ore chemistry composition are as follows: SiO2, 34.63%;MnO, 20.91%;
Fe2O3, 5.58%;Al2O3, 4.23%;CaO, 2.21%;ZnO, 1.64%;K2O, 1.04%;MgO, 0.65%;P2O5,
0.56%;Loss on ignition, 27.65%;Other, 0.9%.The content 26.4% of Mn oxide, Mn oxide microscopic feature therein
See Fig. 1.
Mn oxide ore, grinding 60min, screening obtained the powder of 325 mesh in the ball mill.Then according to manganese oxygen
Compound powder is mixed with water quality ratio 1:10, is made into suspension.Into suspension, addition accounts for the poly- second two of suspension quality 3%
Then alcohol is 4 with the pH of sulfuric acid adjustment suspension, that is, obtains the absorbing liquid for being used for synchronized desulfuring and denitrifying.
Absorbing liquid is put into imitative experimental appliance as shown in Figure 2, with NO/Ar, SO of NO percent by volume 0.1%2
The SO of percent by volume 0.1%2/Ar、O2The O of percent by volume 15%2/ Ar distribution carries out absorption experiment (Fig. 2), experiment condition
Are as follows: [NO]=[SO2]=1000ppm;[O2]=9%;PEG mass concentration 3%;Flue gas flow 100mL/min;Initial pH=4;
Solid-to-liquid ratio=1:10;T=60 DEG C.SO in tail gas after being absorbed with flue gas analyzer on-line checking2, NO concentration, calculate desulphurization denitration
Efficiency detects Mn in absorbing liquid2+、SO4 2-、NO3 -Concentration variation, understands reaction process.Through detecting, SO2Removal efficiency maintains 95%
Above, NO removal efficiency maintains 80% or more (Fig. 3).
Embodiment 2
Select Anhui somewhere Mn oxide ore, ore chemistry composition are as follows: SiO2, 34.63%;MnO, 20.91%;
Fe2O3, 5.58%;Al2O3, 4.23%;CaO, 2.21%;ZnO, 1.64%;K2O, 1.04%;MgO, 0.65%;P2O5,
0.56%;Loss on ignition, 27.65%;Other, 0.9%.The content 26.4% of Mn oxide, Mn oxide microscopic feature therein
See Fig. 1.
Mn oxide ore, grinding 30min, screening obtained the powder of 325 mesh in the ball mill.Then according to manganese oxygen
Compound ore powder is mixed with water quality ratio 1:20, is made into suspension.Into suspension addition account for suspension quality 0%,
0.2%, 0.6%, 1.0%, 1.4%, 1.8%, 2.2%, 2.6%, 3.0%, 3.4%, 3.8% polyethylene glycol, is then used
The pH that sulfuric acid adjusts suspension is 4, that is, obtains the absorbing liquid of the different Polyethylene glycols for synchronized desulfuring and denitrifying.
The absorbing liquid of different Polyethylene glycols is respectively put into imitative experimental appliance as shown in Figure 2, with NO volume
NO/Ar, SO of percentage 0.1%2The SO of percent by volume 0.1%2/Ar、O2The O of percent by volume 15%2/ Ar distribution carries out
Absorption experiment (Fig. 2), experiment condition are as follows: [NO]=[SO2]=1000ppm;[O2]=9%;Flue gas flow 100mL/min;Initially
PH=4;Solid-to-liquid ratio=1:20;T=60 DEG C.SO in tail gas after being absorbed with flue gas analyzer on-line checking2, NO concentration, calculate de-
Sulphur denitration efficiency.Through detecting, SO2Removal efficiency maintains 95% or more, the NO removal efficiency when polyethylene glycol joined 3.0% or more
Maintain 80% or more (Fig. 4).
Embodiment 3
Select Anhui somewhere Mn oxide ore, ore chemistry composition are as follows: SiO2, 34.63%;MnO, 20.91%;
Fe2O3, 5.58%;Al2O3, 4.23%;CaO, 2.21%;ZnO, 1.64%;K2O, 1.04%;MgO, 0.65%;P2O5,
0.56%;Loss on ignition, 27.65%;Other, 0.9%.The content 26.4% of Mn oxide, Mn oxide microscopic feature therein
See Fig. 1.
Mn oxide ore, grinding 30min, screening obtained the powder of 325 mesh in the ball mill.Then according to soft manganese
Miberal powder body is mixed with water quality ratio 1:30, is made into suspension.Into suspension, addition accounts for the poly- second two of suspension quality 3.0%
Then alcohol is 3 with the pH of sulfuric acid adjustment suspension, that is, obtains the absorbing liquid for being used for synchronized desulfuring and denitrifying.
Absorbing liquid is put into imitative experimental appliance as shown in Figure 2, with NO/Ar, SO of NO percent by volume 0.1%2
The SO of percent by volume 0.1%2/Ar、O2The O of percent by volume 15%2/ Ar distribution carries out absorption experiment (Fig. 2), experiment condition
Are as follows: [NO]=[SO2]=1000ppm;[O2]=9%;PEG mass concentration 3.0%;Flue gas flow 100mL/min;Initial pH=
3;Solid-to-liquid ratio=1:30;T=40,50,60,70,80 DEG C.SO in tail gas after being absorbed with flue gas analyzer on-line checking2, NO it is dense
Degree calculates denitrification efficiency.Through detecting, SO2Removal efficiency maintains 95% or more, the NO removal efficiency when temperature is at 60 DEG C or more
80% or more (Fig. 5) can be maintained.
Embodiment 4
By MnSO4.H2O、KMnO4, water according to mass ratio 1:2:2 mixed dissolution, magnetic agitation reacts 60min, centrifugal dehydration
Obtain synthesis Mn oxide.
Synthesis Mn oxide, grinding 30min, screening obtained the powder of 325 mesh in the ball mill.Then according to synthesis
Mn oxide is mixed with water quality ratio 1:40, is made into suspension.Into suspension, addition accounts for the poly- second two of suspension quality 3%
Then alcohol is 5 with the pH of sulfuric acid adjustment suspension, that is, obtains the absorbing liquid for being used for synchronized desulfuring and denitrifying.
Suspension is put into imitative experimental appliance as shown in Figure 2, with NO/Ar, SO of NO percent by volume 0.1%2
The SO of percent by volume 0.1%2/Ar、O2The O of percent by volume 15%2/ Ar distribution carries out absorption experiment (Fig. 2), experiment condition
Are as follows: [NO]=[SO2]=1000ppm;[O2]=9%;PEG mass concentration 3.0%;Flue gas flow 100mL/min;Initial pH=
5;Solid-to-liquid ratio=1:40;Absorbing liquid temperature maintains between 60-80 DEG C.After being absorbed with flue gas analyzer on-line checking in tail gas
SO2, NO concentration, calculate denitrification efficiency.Through detecting, SO2Removal efficiency maintains 95% or more, NO removal efficiency and maintains 80%
More than.
Embodiment 5
Select somewhere Mn oxide ore, the content 47.3% of Mn oxide.
Mn oxide ore, grinding 30min, screening obtained the powder of 325 mesh in the ball mill.Then according to soft manganese
Miberal powder body is mixed with water quality ratio 1:20, is made into suspension.Into suspension, addition accounts for the poly- second two of suspension quality 3.0%
Then alcohol is 3 with the pH of sulfuric acid adjustment suspension, that is, obtains the absorbing liquid for being used for synchronized desulfuring and denitrifying.
Prepared absorbing liquid, circulated sprinkling, wire mesh are waveform, wave height in the packed tower absorption plant of Fig. 6
20mm, wavelength 100mm, the diameter 0.4mm of wire, aperture 2mm.It is process object, flue gas air inlet temperature with glass furnace fume
Between 120-180 DEG C of degree, SO in tail gas after being absorbed with flue gas analyzer on-line checking2, NO concentration, calculate denitrification efficiency.
Through detecting, SO2Removal efficiency maintains 98%, NO removal efficiency and maintains 80% or more.
Claims (5)
1. a kind of flue gas deep treatment method of absorption process synchronized desulfuring and denitrifying, it is characterised in that:
(1) Mn oxide ore or commercial synthesis nano manganese oxide, grinding is selected to become the superfine powder of 325 meshes;
(2) superfine powder is mixed with water according to mass ratio 1:10~40, is made into suspension;
(3) surfactant for accounting for the 1-5% of the suspension quality is added in the suspension of Xiang Suoshu, is then adjusted with acid pH
To 2~6, that is, obtain the absorbing liquid for being used for synchronized desulfuring and denitrifying;
(4) absorbing liquid is added in flue gas washing absorption plant, to remove the SO in flue gas2And NOx, SO after processing2It is de-
Except rate maintains 95% or more, NOxRemoval efficiency maintains 80% or more;
(5) to SO2Removal efficiency is considered as absorbing liquid failure lower than 80%;Failure absorbing liquid is separated by solid-liquid separation, solid matter is discarded, remains
Extraction raffinate body obtains manganese sulfate and manganese nitrate by-product through evaporative crystallization, or by remaining liq directly as the raw material of liquid fertilizer
Sale.
2. a kind of flue gas deep treatment method of absorption process synchronized desulfuring and denitrifying according to claim 1, it is characterised in that:
In the Mn oxide ore mass percent of manganese dioxide be greater than 25%, manganites film therein be cryptomelane,
At least one of manganese calcium mine and birnessite.
3. a kind of flue gas deep treatment method of absorption process synchronized desulfuring and denitrifying according to claim 1, it is characterised in that:
The Mn oxide ore is nano-mineral, and crystal diameter is less than 90 nanometers.
4. a kind of flue gas deep treatment method of absorption process synchronized desulfuring and denitrifying according to claim 1, it is characterised in that:
The surfactant is polyethylene glycol.
5. a kind of flue gas deep treatment method of absorption process synchronized desulfuring and denitrifying according to claim 1, it is characterised in that:
The flue gas washing absorption plant includes column plate type, material filling type, bubble type, atomizing, fountain scrubbing tower.
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CN110917829A (en) * | 2019-12-13 | 2020-03-27 | 西安润川环保科技有限公司 | Desulfurization and denitrification flue gas advanced treatment method |
CN111272946A (en) * | 2020-03-30 | 2020-06-12 | 合肥工业大学 | Device and method for measuring content of organic carbon in industrial waste salt |
CN111650972A (en) * | 2020-06-12 | 2020-09-11 | 重庆科技学院 | Multi-component dynamic gas distribution test system with mixer |
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