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CN107081064A - Sintering flue gas SCR denitration technique based on dry method and semi-dry desulphurization - Google Patents

Sintering flue gas SCR denitration technique based on dry method and semi-dry desulphurization Download PDF

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Publication number
CN107081064A
CN107081064A CN201710482688.5A CN201710482688A CN107081064A CN 107081064 A CN107081064 A CN 107081064A CN 201710482688 A CN201710482688 A CN 201710482688A CN 107081064 A CN107081064 A CN 107081064A
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sintering
flue gas
sintering deposit
deposit
temperature
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陈旺生
秦林波
李泽
韩军
吴高明
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Wuhan University of Science and Engineering WUSE
Wuhan University of Science and Technology WHUST
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Wuhan University of Science and Engineering WUSE
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Priority to CN201710819135.4A priority patent/CN107551811B/en
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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
    • 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
    • B01D53/90—Injecting reactants
    • 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
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/207—Transition metals
    • B01D2255/20738—Iron
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
    • Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
    • Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters

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  • Engineering & Computer Science (AREA)
  • Environmental & Geological Engineering (AREA)
  • Chemical & Material Sciences (AREA)
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  • Biomedical Technology (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Exhaust Gas Treatment By Means Of Catalyst (AREA)

Abstract

The invention discloses the sintering flue gas SCR denitration technique based on dry method/semidry method desulphurization.Technical scheme includes the sintering flue gas for drawing sintering machine, the heat sinter direct heat transfer in annular cooling device drawn successively after removing dust, dry desulfurization with sintering machine, temperature is down to 350~400 DEG C of sintering deposit after heat exchange and temperature rises to 300~350 DEG C of sintering flue gas, into in portable denitrification apparatus, and selective catalytic reduction reaction is carried out under sintering deposit effect, by the NO in flue gasxIt is converted into N2, the flue gas drawn from portable denitrification apparatus 100 150 DEG C are cooled to through waste heat recovery after clean flue gas, then discharged by chimney, the sintering deposit drawn from portable denitrification apparatus is through secondary waste heat using sending into subsequent processing after being cooled to below 150 DEG C.The inventive method technique is simple, energy consumption is low, denitration desulfurized effect is good, catalyst poisoning can be avoided to inactivate；The denitrating catalyst source of use is wide, low of cost；Invention system floor space is small, cost of investment and operating cost are low, environmentally friendly.

Description

Sintering flue gas SCR denitration technique based on dry method and semi-dry desulphurization
Technical field
The present invention relates to a kind of flue gas purifying method and its system, the burning based on dry method and semi-dry desulphurization is specifically Tie flue gas SCR denitration technique.
Background technology
Steel industry SO2And NOxDischarge capacity is respectively 176.65 ten thousand tons and 93.10 ten thousand tons, occupies each industrial emission source Prostatitis, wherein more than 70% SO2, more than 50% NOxFrom stove sintering machine.National environmental protection portion is promulgated within 2012 《Steel sintering, pelletizing industrial air pollution thing discharge standard (GB 28662-2012)》, the standard is to sintering flue gas atmosphere pollution The discharge of thing proposes new requirement with control.Therefore, steel sintering flue gas desulfurization and denitrification will be steel and iron industry SO2And NOxDischarge The center of gravity of control.
Sintering flue gas has the big (4000~6000m of exhaust gas volumn3/ ton sintering deposit), temperature change big (120~180 DEG C), CO Concentration height (0.5~2.0%), SO2Big (1000~the 3000mg/Nm of change in concentration3)、NOxLow (300~the 500mg/Nm of concentration3)、 The features such as water capacity big (7~12%) and oxygen content high (15~18%).The characteristics of there is many itself compared with power-plant flue gas, Its smoke components is more complicated, and change fluctuation is bigger, handles more difficult.
China has gone into operation and has mainly had desulfurization by dry method (such as SDA methods, circulation in the sintering flue gas desulfurization process built at present Fluidized bed process and NID methods) and Wet Flue Gas Desulfurization Technique (such as ammonia-ammonium sulfate method).But these method purifying sintering flue gas respectively have excellent lack Point, such as ciculation fluidized bed process desulfuration efficiency are generally 80%, can not qualified discharge during processing high-concentration sulfur dioxide；Ammonia-ammonium sulfate Method desulfuration efficiency is up to more than 95%, but the escaping of ammonia is serious；NID methods desulfuration efficiency is 90% or so, but Desulphurization can not Effectively trapping, causes granular material discharged concentration severe overweight.Domestic and international iron and steel enterprise's experience is combined at present, it is believed that dry desulfurization skill Art such as SDA methods, ciculation fluidized bed process and NID methods are more protruded the clean-up effect for sintering flue gas, and dry method/semidry method desulphurization is used for The occupation rate of market of domestic sintering gas purifying is higher.
Compared to sintering flue gas desulfurization technology, China's sintering gas denitrifying technology research is started late, and there is presently no exploitation Go out the sintering gas denitrifying technology of maturation.But NH3SCR (NH3- SCR) method has been successfully applied to coal-fired flue-gas Denitration, and be most hopeful to be applied to steel sintering flue gas NOXPurification.SCR technology refers in the presence of a catalyst, to flue gas Middle penetrating NH3, make NH3Optionally with NOxReaction generation N2, without with O2Generation non-selective oxidation, so as to reach reduction NOx Reduction temperature, raising NOxThe purpose of removal efficiency.NH3The core of-SCR technology is SCR catalyst system；SCR catalyst is different, It reduces NOxOptimum temperature it is interval different.Catalyst (the V of SCR denitration is commercially used at present2O5-WO3(MoO3)/TiO2) There is excellent NO in 350~400 DEG C of temperature windowsxPurification efficiency, but exist catalyst cost it is higher, it is easy vulcanization lose Living the problems such as.
China Patent No. CN201210533763.3 discloses a kind of sintering deposit UTILIZATION OF VESIDUAL HEAT IN based on sintering gas purifying Technique, the technique proposes, using heat sinter heat-agglomerating flue gas, to make sintering flue-gas temperature reach the window of SCR 350~400 DEG C of temperature of mouth, then carries out SCR denitration.It is low that the technique solves sintering flue-gas temperature, it is impossible to meets SCR denitration window The problem of mouth temperature, but follow-up sintering flue gas SCR denitration process still exists and sintering flue gas heating need to be increased energy consumption, is catalyzed The problem of agent cost height and catalyst are easily poisoned.
It is net that China Patent No. CN201310459262.X discloses a kind of sintering flue gas based on heat sinter catalytic action Change method.It this method propose sintering flue gas and the sintering deposit that sintering machine is drawn after the dedusting for drawing sintering machine cold in sintering deposit But direct heat transfer in equipment, and selective catalytic reduction reaction is carried out under sintering deposit effect, by the NO in flue gasxIt is converted into N2, the ammonia process of desulfurization is then carried out again and obtains clean flue gas, so that desulphurization denitration while realizing sintering flue gas.But in this method Temperature in the sintering deposit cooling device mentioned is extremely unstable (temperature is fluctuated in 300~600 DEG C), is burnt when ammonia is sprayed into Tie after ore deposit cooling device, most of ammonia may be oxidized to NOx in the environment of 450~600 DEG C, so that catalysis can not be played The purpose of reduction.It is oxidized to reduce ammonia as far as possible, by controlling NH in this method3/ NO is 0.4~0.5, but denitration Efficiency can be only sustained at 40% or so again.In addition, this method is using first SCR denitration, the then ammonia process of desulfurization again, the escaping of ammonia is very tight Weight.
China Patent No. CN201611216729.8 discloses a kind of moving bed heat sinter denitrification apparatus, in the device In, the sintering deposit catalyst temperature is 350~450 DEG C, NH3/ NO=0.5 and air speed ratio are 5000h-1O2Concentration is 15%, NO concentration is 400mg/Nm3, SO2Concentration is 50ppm, and humidity is 6.9%, CO2Concentration is the denitration effect in 5% mixed gas Rate is 39.46~42.62%.The problem of catalyst poisoning is inactivated, but NH can be solved using portable denitrification apparatus3And NOx Reacted under high temperature catalyst, the more difficult control of window temperature, easily by NH3It is oxidized to NOx, such as Fig. 1, heat sinter is from denitration reaction Continuously input is continuously exported the hopper 200 at the top of device 500 from the bottom of device for discharging 1000, and Benitration reactor passes through charge air flow point Cloth apparatus 810 and the connection air inlet pipe 100 of outlet airflow distribution device 820 and escape pipe 700, sintering flue gas and denitrification reducing agent NH3Benitration reactor 500 is entered by air inlet pipe 100, moving bed, sintering flue gas and denitrification reducing agent NH is formed3In denitration reaction NO in gas-solid contact, flue gas is carried out in the way of cross-flow between the sintering deposit of displacement in device 500XAnd NH3Reaction, it is raw Into N2With vapor as denitration flue gas is discharged by escape pipe 700.
First two scheme, which all exists to need to stop production after catalyst cost height, catalyst poisoning, to be changed, to sintering flue gas before denitration The problem of sulfur content is required is, it is necessary to which a kind of catalyst cost is low and continuously can prevent catalyst poisoning, window by more catalyst changeout Temperature stabilization, the escaping of ammonia is low, denitration efficiency it is higher and energy-conservation denitrating technique.
The content of the invention
The invention aims to solve above-mentioned technical problem, there is provided a kind of technique is simple, energy consumption is low, denitration desulfurization effect It is really good, catalyst poisoning inactivation can be avoided, catalyst source is wide and low of cost, small system footprint area, cost of investment and fortune Row cost is low, the environment amenable sintering flue gas SCR denitration technique based on dry method and semi-dry desulphurization.
The invention further relates to a kind of system for above-mentioned purification method.
The inventive method is including the 120-140 DEG C of sintering flue gas including being drawn from sintering machine successively removing dust device dedusting and takes off The 100-110 DEG C of desulfurization fume obtained after sulphur system desulfurization, it is characterised in that further comprising the steps of：
S01,800-900 DEG C of sintering deposit for drawing the desulfurization fume and sintering machine are direct in annular cooling device The sintering deposit after desulfurization fume and cooling after must being heated up after heat exchange；
S02, by into step S01 heat up after desulfurization fume in be passed through ammonia control flue gas in NH3/NOxVolume ratio =0.7~1.0；
Sintering deposit after cooling in S03, the desulfurization fume that will be mixed in step S02 with ammonia, and step S01, feeding movement Selective catalytic reduction reaction is carried out in formula denitrification apparatus；
S04, go out portable denitrification apparatus sintering flue gas be cooled to 100-150 DEG C through waste heat boiler after obtain clean cigarette Gas, then discharged by chimney, the sintering deposit for going out portable denitrification apparatus utilizes device to send into subsequent processing after exchanging heat through secondary waste heat.
It is preferred that, the feeding vibratory sieve screening of sintering deposit described in step S03, sieve takes the sintering deposit that particle diameter is 5~10mm, sieve Sintering deposit temperature after point is 350~400 DEG C, and the sintering deposit is sent into portable denitrification apparatus；It will be sintered after the heat exchange Flue gas cool-down is re-fed into portable denitrification apparatus and directly contacted with the sintering deposit to being mixed with ammonia after 300~350 DEG C Carry out selective catalytic reduction reaction.
It is preferred that, in order to reduce temperature drop of the sintering flue gas after desulphurization system desulfurization, reduction subsequent heat desulfurization fume Energy consumption, the desulphurization system is dry method or semi-dry desulphurization system, and the sintering flue-gas temperature after desulfurization is 100~110 DEG C.
Further, 800-900 DEG C of the sintering deposit that the sintering flue gas is drawn with sintering machine is in annular cooling device Reverse direct heat transfer, makes the sintering flue gas utilization sintering deposit waste-heat after desulfurization heat up, it is also ensured that denitration reaction is in catalysis Under 300~400 DEG C of environment of agent window temperature carry out, it is to avoid cause because temperature distributing disproportionation is even ammonia be oxidized, denitration effect not It is good.
The desulfurization fume temperature gone out described in step S01 after being exchanged heat in annular cooling device is increased to 300~350 DEG C.Enter One step, it is described go out annular cooling device after sintering deposit temperature be down to 350~400 DEG C.
It is preferred that, O in the sintering flue gas after the heating2Concentration is percent by volume 12~18%, and NO concentration is 300- 600mg/Nm3, SO2Concentration be 0-100mg/Nm3。
NH3/ NO, which crosses conference, causes NH3Utilization rate is low, the escaping of ammonia is serious, NH3/ NO is too small to cause denitration rate too low, enter one Step, NH in the desulfurization fume after ammonia is mixed described in step S023/NOxVolume ratio=0.8~0.9.
In order to ensure its efficient catalytic effect, as the iron-based oxide of sintering catalyst for denitrating flue gas, step S01 or step Main component is in sintering deposit described in rapid S03：Fe contents are 50-70wt%, and FeO contents are 5.0-15.0wt%.
Further, in the portable denitrification apparatus, the sintering flue gas stops under 300~400 DEG C of environment of temperature It is 1.5~2.0s to stay the time.Residence time is long, and equipment size needed for handling identical flue gas is bigger, and investment is high, residence time mistake It is short to make NO and NH3Reaction is not abundant enough, causes denitration rate low.
It is preferred that, in the sintering flue gas SCR denitration technique based on dry method and semi-dry desulphurization, the annular cooling Equipment is made up of high temperature section and low-temperature zone, and sintering deposit is by the high temperature section of ring-like cooler enters, low-temperature zone is sent out, and desulfurization fume is first The low-temperature zone of ring-like cooler is sent into heat up with carrying out once heat exchange positioned at the sintering deposit of low-temperature zone, be then re-fed into high temperature section with Secondary heat exchange heating is carried out positioned at high temperature section sintering deposit, the annular cooling device exhanst gas outlet is sequentially connected portable denitration dress Put and waste heat boiler, the annular cooling device sintering deposit outlet is connected to portable denitrification apparatus sintering deposit through vibratory sieve successively Loading port.
Further, described portable denitrification apparatus includes vertical closed tank, and reaction zone is arranged on the top of tank body, Sintering deposit loading port is provided with the top of the tank body of the vertical closing, sintering deposit loading port connects vibratory sieve, and bottom is provided with burning Ore deposit outlet is tied, sintering deposit outlet is provided with rotary seal valve, and tank body top is connected by denitration exhanst gas outlet pipeline, waste heat boiler To chimney, reaction zone is additionally provided with sintering smoke air inlet, annular gas distribution flue and ammonia air inlet, and red-hot sintering deposit is loaded To reaction zone, the temperature of sintering deposit is 350 DEG C~400 DEG C；Then normal temperature ammonia, 300~350 DEG C of sintering are passed through from reaction zone Flue gas, sintering flue gas air speed is 1000~3000h-1, make red-hot sintering deposit in the tank body with mixing the sintering cigarette after ammonia Gas fully contacts carry out selective catalytic reduction reaction, and reacted sintering deposit is discharged by tank base, and is reacted with sintering deposit Denitration flue gas afterwards is then discharged from tank body top, and is passed through waste heat boiler temperature and is reduced to 100 DEG C~150 DEG C.
There is sintering deposit after whole grain high-specific surface area and uniform particle diameter to be easy to sintering flue gas uniformly to be contacted with sintering deposit, The efficiency of catalyst can be improved in sintering deposit after sintering deposit after whole grain is cooled down added to annular cooler.
The sintering flue gas and sintering deposit that the present invention draws sintering machine are moved after being exchanged heat in annular cooling device while sending into Denitration in dynamic formula denitrification apparatus.Its advantage includes：1) it is made to meet reaction temperature sintering flue gas heating using the high temperature of sintering deposit The requirement of degree, sintering flue gas and sintering deposit are then sent into portable denitrification apparatus simultaneously can ensure that denitration reaction section temperature is steady It is scheduled on the window temperature of catalyst choice catalysis reduction, it is to avoid ammonia is oxidized to NOx at a high temperature of higher than window temperature, Cause ammonia utilization rate low；2) substituting original SCR catalyst as catalyst in itself by the use of sintering deposit makes sintering flue gas in shifting Selective catalytic reduction reaction is carried out in dynamic formula denitrification apparatus, the purpose of denitration is reached；3) due to the catalysis of mobile denitrification apparatus Agent can avoid the problem of catalyst poisoning is inactivated in the sintering deposit catalyst constantly more renewed；4) mobile denitrification apparatus row The sintering deposit gone out can be reused for blast furnace ironmaking, and the zero cost of denitrating catalyst can be achieved；5) set before sintering denitrating flue gas Dry method or semi-dry desulphurization system, investment running cost are relatively low, and product is disposable, and avoids the temperature of desulfurization fume before denitration from dropping Low excessive, the energy consumption that desulfurization fume is warming up to window temperature is relatively low；6) make sintering flue gas under conditions of ammonia is not passed through with height Warm sintering deposit is directly contacted, and makes the Fe-NO compounds of sintering deposit NOx adsorption generation activation；7) sintering added after whole grain screening Ore deposit, specific surface area of catalyst is bigger, uniform particle sizes, in portable denitrification apparatus, and sintering flue gas can be with the uniform gas-solid of sintering deposit Contact, improves denitration conversion ratio；8) the sintering deposit temperature after being sieved through whole grain is reduced to window temperature, it is to avoid localized hyperthermia.
In above-mentioned denitration reaction, the sintering deposit that the present invention is especially drawn using sintering machine substitutes existing SCR catalyst and made For denitrating catalyst, inventor's research finds that the main component that heat sinter SCR removings NO course of reaction plays catalytic action is Fe2O3.Its action principle is：NH3It is good for and ionic bond NH with being conjugated respectively4 +Form adsorb in Fe2O3The sour sites of the Lewis of iron Center andSour site center, such as formula (1) and (3)；The main absorption in the form of bridge-type nitro-nitrite of NO exists Catalyst surface, such as formula (5) and (6), Fe-O keys or Fe-N keys fracture the generation nitro compound of bridge-type nitro-nitrite and Monodentate type nitrite, while one Cation adsorption position of release carrys out adsorptive gaseous NO to generate Fe-NO compounds, as a result As in Figure 2-4.
NH3And NO/O2Catalyst surface adsorption reaction mechanism simultaneously follow Eley-Rideal mechanism formula (7) and Langmuir-Hinshelwood mechanism formula (8), its absorption-reaction equation is as follows：
NH3(a)+O(a)→NH2(a)+OH(a)(2)
O2(g)→2O(a)(4)
NH2(a)+NO(g)→N2(g)+H2O(g)(E-R mechanism)(7)
NH2(a)+NO2(a)→N2(g)+H2O(g)+O(a)(L-H mechanism)(8)
Also, inventor also found that carrying out denitration using the sintered ore of high temperature has multi-effect：1) itself is constituted Composition containing catalyst in composition, and from sintering machine, that is to say, that during processing sintering flue gas, it can effectively ensure that The continued synchronization supply of sintering deposit, it is ensured that the demand of catalyst；2) due to can be continuously in portable denitrification apparatus Heat sinter is supplied, even if the SO containing high concentration in flue gas2, do not exist as the sintering deposit generation poisoning and deactivation of catalyst yet The problem of, it is ensured that denitration is normally carried out, the problem of catalyst poisoning for solving denitrification process presence is inactivated, dry method flue gas Desulfurization technology, which is that gas is same, reacts, and for wet desulfurization system, equipment is simple, and floor space is small, invest and operating cost Relatively low, easy to operate, energy consumption is low, product is easy to disposal, without sewage disposal system etc..
Shortcoming：But reaction speed is slow, and desulfurization degree is low, advanced up to 95%, Wet Flue Gas Desulfurization Technology is gas liquid reaction, Reaction speed is fast, and desulfuration efficiency is high, advanced up to 99%, but product is liquid or sludge, it is more difficult to handle, equipment corrosion Seriously, flue gas needs reheating after washing, and high energy consumption, floor space is big, and investment and operating cost are high.System complex, equipment are huge, consumption Water is big, one-time investment is high.The desulfurization degree of semidry method is up to 95%.Its advantage：Desulfurization is under gas, liquid, solid three-phase state Carry out, process equipment is simple, product is CaSO, CaSO of dry state, disposable, without serious equipment corrosion and blocking feelings Condition, water consumption is also fewer.Shortcoming：Automation requires higher, and the consumption of absorbent is difficult to control to, and absorption efficiency is not very high； 3) the sintered ore temperature from sintering machine is high, is 800~900 DEG C, and this part heat is fully met needed for denitration catalyst reacts Reaction temperature requirement, it is not necessary to increase heating device in addition, make the waste heat of sintering deposit be fully used.
Beneficial effect：
1. the present invention substitutes existing SCR catalyst as denitrating catalyst completely using iron-based oxide (heat sinter), its Wide material sources, cost are relatively low, greatly reduce the operating cost of system, based on carrying out denitration reaction under E-L and L-H mechanism.
2. the present invention makes full use of sintering deposit waste heat to heat flue gas, it is not necessary to which the extra supplement energy makes to flue gas It reaches the window temperature of SCR denitration, while flue-gas temperature reaches 300~400 DEG C after heating, can be used；
3. present invention process is simple, floor space is smaller, and the catalytic reaction of denitration is completed in portable denitration device, energy Enough ensure that denitration reaction section temperature is maintained to carry out under the window temperature (300~400 DEG C) of catalyst, it is to avoid because of local temperature mistake Height causes ammonia to be oxidized, and also avoids, because of incomplete desulfurization, causing catalyst poisoning, the problem of denitration efficiency is reduced.
4. present invention process can realize sintering flue gas and desulfurizing and denitrifying, good purification, to NOxContent be up to 300-500mg/Nm3, sulphur is up to 1000-3000mg/Nm3Sintering flue gas be applicable, its bulk devulcanization efficiency >=95%, denitration Efficiency is 70-80%, and the flue gas after purification meets the sintering standard limit of smog release (GB 28662-2012) of national regulation.
5. the more former sintering deposit of sintering deposit specific surface area is higher after whole grain screening activation, and particle diameter distribution is uniform, is conducive to moving NH in dynamic formula denitrification apparatus3, NOx and sintering deposit fully contact, improve the conversion ratio of selective catalytic reduction reaction.
Brief description of the drawings
The structural representation of portable denitrification apparatus in Fig. 1 background of invention
The process chart of Fig. 2 embodiment of the present invention 1
The process chart of Fig. 3 embodiment of the present invention 2
Fig. 4 NH3In absorption-In situ FTIR spectrogram of agglomerate surface
Fig. 5 NO/O2In absorption-In situ FTIR spectrogram of agglomerate surface
Fig. 6 NH3, NO and O2In agglomerate surface eutectoid content-In situ FTIR spectrogram
Fig. 7 reaction temperatures and NH3Influences of/the NO to denitration efficiency.
Fig. 8 air speeds compare the influence of denitration efficiency.
The structural representation of portable denitrification apparatus in Fig. 9 present invention
Embodiment
Embodiment 1：
As shown in Fig. 2 the sintering deposit outlet of sintering machine 1 is connected with the sintering deposit entrance of annular cooling device 4, the sintering The exhanst gas outlet of machine 1 and dust arrester 2, dry method/semidry method desulphurization device 3, annular cooling device 4, portable denitrification apparatus 5, Waste heat boiler 6 and chimney 8 are sequentially connected.The annular cooling device 4 is made up of high temperature section and low-temperature zone, and sintering deposit is by ring-like The high temperature section of cooler enters, low-temperature zone is sent out, and desulfurization fume first sends into the low-temperature zone of ring-like cooler with being located at low-temperature zone Sintering deposit carries out once heat exchange heating, is then re-fed into high temperature section with carrying out secondary heat exchange heating, institute positioned at high temperature section sintering deposit State annular cooling device exhanst gas outlet and be connected to portable denitrification apparatus gas approach, the annular cooling device sintering deposit outlet It is connected to portable denitrification apparatus sintering deposit air inlet.The sintering deposit outlet of the sintering machine 1 and the sintering of annular cooling device 4 Ore deposit entrance is connected, and the exhanst gas outlet removing dust device 2 and dry desulfurization device 3 of the sintering machine 1 are sintered with annular cooling device 4 Smoke inlet is connected.The annular cooling device 4 is preferably ring-like cooler, and the present embodiment includes 5 cooling sections.
Portable denitrification apparatus 5 as described in Figure 9 is vertical closed tank 11 (as disclosed in 200910187381.8 " tank body of vertical closing "), reaction zone 18 is arranged at the top of the top of tank body, the tank body of the vertical closing and is provided with sintering deposit Loading port 16, bottom is provided with sintering deposit outlet 13, and sintering deposit outlet is provided with rotary seal valve 10, and tank body top passes through denitration Exhanst gas outlet pipeline 12, waste heat boiler 7 are connected to chimney 8, and reaction zone is additionally provided with sintering smoke air inlet 14, annular gas distribution flue 19 and ammonia air inlet 17, red-hot sintering deposit is encased in reaction zone, the temperature of sintering deposit is 350 DEG C~400 DEG C；Then from Reaction zone is passed through normal temperature ammonia, and 300~350 DEG C of sintering flue gas, sintering flue gas air speed is 1000~3000h-1, make red-hot burning Tie ore deposit and fully contact carry out selective catalytic reduction reaction, reacted burning with the sintering flue gas after mixing ammonia in the tank body Knot ore deposit is discharged by tank base, and is then discharged with the reacted denitration flue gas of sintering deposit from tank body top, and is passed through waste heat boiler Temperature is reduced to 100 DEG C~150 DEG C.
Embodiment 2：
As shown in figure 3, the sintering deposit outlet of sintering machine 1 is connected with the sintering deposit entrance of annular cooling device 4, the sintering The exhanst gas outlet of machine 1 and dust arrester 2, dry method/semidry method desulphurization device 3, annular cooling device 4, vibratory sieve 41, movable type are de- Nitre device 5, waste heat boiler 6 and chimney 8 are sequentially connected.The annular cooling device 4 is made up of high temperature section and low-temperature zone, sintering Ore deposit is by the high temperature section of ring-like cooler enters, low-temperature zone is sent out, and desulfurization fume first sends into the low-temperature zone of ring-like cooler with being located at The sintering deposit of low-temperature zone carries out once heat exchange heating, is then re-fed into high temperature section with carrying out secondary heat exchange positioned at high temperature section sintering deposit Heating, the annular cooling device exhanst gas outlet is sequentially connected heat exchanger, portable denitrification apparatus, and the annular cooling device burns The outlet of knot ore deposit is connected to vibratory sieve 41.The sintering deposit outlet of the sintering machine 1 and the sintering deposit entrance of annular cooling device 4 connect Connect, the exhanst gas outlet removing dust device 2 and dry desulfurization device 3 of the sintering machine 1 and the annular sintering of cooling device 4 smoke inlet Connection.The annular cooling device 4 is preferably ring-like cooler, and the present embodiment includes 5 cooling sections.
Portable denitrification apparatus 5 as described in Figure 9 is vertical closed tank 11 (as disclosed in 200910187381.8 " tank body of vertical closing "), reaction zone 18 is arranged at the top of the top of tank body, the tank body of the vertical closing and is provided with sintering deposit Loading port 16, sintering deposit loading port connection vibratory sieve 41, bottom is provided with sintering deposit outlet 13, and sintering deposit outlet is provided with rotation Sealing valve 10, tank body top is connected to chimney 8 by denitration exhanst gas outlet pipeline 12, waste heat boiler 7, and reaction zone is additionally provided with sintering Smoke air inlet 14, annular gas distribution flue 19 and ammonia air inlet 17, reaction zone is encased in by red-hot sintering deposit, sintering deposit Temperature is 350 DEG C~400 DEG C；Then normal temperature ammonia is passed through from reaction zone, 300~350 DEG C of sintering flue gas sinters flue gas air speed For 1000~3000h-1, red-hot sintering deposit is fully contacted with the sintering flue gas after mixing ammonia in the tank body and selected Property catalytic reduction reaction, reacted sintering deposit is discharged by tank base, and with the reacted denitration flue gas of sintering deposit then from tank Body top is discharged, and is passed through waste heat boiler temperature and is reduced to 100 DEG C~150 DEG C.
In embodiment 1 sintering machine 1 draw the dedusting of 120-140 DEG C of flue gas (also known as sintering flue gas) removing dust device 2 and The desulfurization of dry desulfurization device 3, the sintering flue-gas temperature after dedusting and desulfurization is 100-110 DEG C, wherein O in flue gas2Content be 14-18vol%, CO2Content be 3.0-7.0vol%, CO content is 0-2.0vol%, NOx, content be 300-500mg/ Nm3(wherein 90-95% NO), SO2, content be 0~100mg/Nm3；800-900 DEG C of the sintering deposit that sintering machine 1 is drawn (particle diameter is 1-100mm, wherein, at least containing Fe contents be 55-65wt%, FeO contents be 8.0-15.0wt%) and desulfurization set The sintering deposit entrance and the burning of annular cooling device 4 of standby 3 100~110 DEG C of sintering flue gases drawn respectively with annular cooling device 4 Tie smoke inlet connection, the flue gas and sintering deposit reverse direct heat transfer, the sintering deposit temperature after heat exchange in annular cooling device Spend for 350~400 DEG C, sintering flue-gas temperature is 300~350 DEG C.Then sintering of the described sintering deposit from annular cooling device 4 Ore deposit outlet is drawn, and is connected with the sintering deposit entrance of portable denitrification apparatus 5, and sintering deposit is drawn from annular cooler outlet and sent Enter in portable denitrification apparatus 5, described sintering flue gas is drawn from the sintering exhanst gas outlet of annular cooling device 4, to sintering cigarette Appropriate ammonia (control NH is supplemented in gas3After/NO=0.8~0.9), described sintering flue gas introduces portable denitrification apparatus 5 Sintering smoke inlet, in portable denitrification apparatus, heat sinter is used as catalyst, in the environment of 300~400 DEG C, cigarette NO in gasxWith NH3Selective catalytic reduction reaction is carried out under sintering deposit effect and carries out denitration, by the NO parts in flue gas Switch to N2And NO2.Temperature after denitration after the preheated boiler heat exchange of clean flue gas is down to 160 DEG C and directly discharged through chimney, in movement The sintering deposit that formula denitration device 5 is drawn sends into subsequent processing after being cooled down through air.
In embodiment 2 sintering machine 1 draw the dedusting of 120-140 DEG C of flue gas (also known as sintering flue gas) removing dust device 2 and The desulfurization of dry desulfurization device 3, the sintering flue-gas temperature after dedusting and desulfurization is 100-110 DEG C, wherein O in flue gas2Content be 14-18vol%, CO2Content be 3.0-7.0vol%, CO content is 0-2.0vol%, NOx, content be 300-500mg/ Nm3(wherein 90-95% NO), SO2, content be 0~100mg/Nm3；800-900 DEG C of the sintering deposit that sintering machine 1 is drawn (particle diameter is 1-100mm, wherein, at least containing Fe contents be 55-65wt%, FeO contents be 8.0-15.0wt%) and desulfurization set The sintering deposit entrance and the burning of annular cooling device 4 of standby 3 100~110 DEG C of sintering flue gases drawn respectively with annular cooling device 4 Tie smoke inlet connection, the flue gas and the sintering deposit reverse direct heat transfer in annular cooling device.Then described sintering deposit Export and draw from the sintering deposit of annular cooling device 4,5~10mm sintering deposit after being sieved through vibra feeder 41, sintering deposit warp Screening temperature is reduced to 350~400 DEG C, then draws in the portable denitrification apparatus 5 of feeding, and described sintering flue gas is set from annular cooling Standby 4 sintering exhanst gas outlet is drawn, and appropriate ammonia (control NH is supplemented into sintering flue gas3It is described after/NO=0.8~0.9) Sintering flue gas introduce the sintering smoke inlet of portable denitrification apparatus 5, the sintering flue-gas temperature is 300~350 DEG C, is being moved In dynamic formula denitrification apparatus, heat sinter is used as catalyst, in the environment of 300~400 DEG C, the NO in flue gasxWith NH3In sintering The lower catalytic reduction reaction for carrying out selectivity of ore deposit effect carries out denitration, and the NO parts in flue gas are switched into N2And NO2.It is clean after denitration Temperature after the preheated boiler heat exchange of neat stress is down to 160 DEG C and directly discharged through chimney, the burning drawn in portable denitration device 5 Knot ore deposit sends into subsequent processing after being cooled down through air.
The concentration through NOx in portable denitration process exiting flue gas is measured for 70-180mg/Nm3, SO2Concentration for 0~ 100mg/Nm3.Inventive desulfurization efficiency is 92-96.5%, and denitration efficiency is 70-80%.
According to the method described above, the flue gas for the different NOx concentrations drawn to sintering machine 1 is handled, using portable flue gas Analyzer (PG-350, Horiba company) determines the smoke components of import and export respectively, to ensure the authenticity of data, during it is each Data maintain 15min measure under stationary conditions.NOXDenitration efficiency by formula (10) calculate, i.e.,
In formula, C (NOX) in- imports NOXConcentration, ppm；
C(NOX) out- outlets NOXConcentration, ppm；
η-denitration efficiency, %.
It handles index and see the table below 1.
Table 1
The sintering deposit that embodiment is used comes from Wuhan City's sintering plant, takes 0.15mm~0.25mm (60 afterwards after crushing and screening ~100 mesh) it is used as research object.Under normal temperature, XRD surveys are carried out to sintering deposit catalyst with Cu-K alpha rays on XD-3A analyzers Examination；The main component of sintering deposit is analyzed using x-ray fluorescence analyzer (XRF), the Principle components analysis of sintering deposit is shown in Table 2；Adopt Specific surface area (BET), pore volume opening size test are carried out with Quantachrome QUADRASORB SI analyzers, adsorbing medium is liquid Nitrogen, adsorption temp is 77K, and sample deaerates 10 hours at 350 DEG C before test catalytic reaction；Using Fourier in-situ ft-ir (in situ DRIFTS) carries out original position DRIFTS phenetic analysis to sintering deposit, and wave-length coverage is 1000~4000cm-1, denitration Taken after reaction the discharge of portable Benitration reactor through NH3With the sintering deposit sample quality 50mg after NOx reduction reactions, and annular Cooling device or tower cooling device discharge adsorbed through NOx after sintering deposit sample 50mg, further study agglomerate surface Absorption-response characteristic.
The sintering deposit chemical constituent (%) of table 2
Table 3 is specific surface area, total pore volume and the average pore size before and after sintering deposit catalyst denitration.As shown in Table 2, before denitration The ratio surface of sintering deposit catalyst is 3.469m2/ g, total pore volume is 0.00583cm3/ g, average pore size is 6.714nm；And denitration The ratio surface of sintering deposit catalyst is 0.372m afterwards2/ g, total pore volume is 0.00131cm3/ g, average pore size is 14.074nm；Contrast The pore structure test result of sintering deposit is it may be speculated that the product during denitration reaction can enter in catalyst pores before and after denitration Or forming adsorption layer on its surface so that specific surface area of catalyst and total pore volume reduce, average pore size increase.
Specific surface area, total pore volume, average pore size before and after the catalyst denitration of table 2
Original position DRIFTS (infrared spectrum) researchs are carried out, the catalyst surface active under different adsorption conditionses is mainly studied The effect of position sour position and acidic site played in catalytic reduction process, to determine the molecular action of adsorbent and intermediate Mechanism.
Fig. 4 is that reaction temperature is NH under the conditions of 300 DEG C3In the DRIFT spectrograms of agglomerate surface absorption-reaction.Such as Fig. 3 institutes Show, when temperature is 300 DEG C, all absworption peaks (referring specifically to those absworption peaks) just can be detected in 10min. 3857cm-1And 3728cm-1The absworption peak at place is- OH groups on sour site；3189cm-1The absworption peak at place is The N-H symmetrical stretching vibrations in Lewis acid site；1600-1800cm-1And 1400-1600cm-1The strong absworption peak at place is with reaction The extension of time and gradually strengthen, 1600-1800cm-1The absworption peak at place is NH4 +Symmetric curvature vibration, i.e. Bronsted acid, 1400-1600cm-1The strong absworption peak at place belongs to Lewis acid site NH3Absorption；In 1000-1200cm-1The weak absorbing peak at place It is also Lewis acid site NH3Absorption.Therefore, NH3Except to be conjugated strong absorption on the center of Lewis sour sites, also with ion Strong NH4 +Absorption existsSour site center.
The DRIFT spectrograms that Fig. 5 reaction temperatures are adsorbed for NO under the conditions of 300 DEG C in agglomerate surface.As shown in figure 4,1600- 1800cm-1And 1400-1600cm-1The strong absworption peak at place can just be detected in 10min, and absworption peak intensity with The increase of time gradually increases；1143cm-1、3603cm-1And 3853cm-1The weak absorbing peak at place is just detected in 20min, and And the intensity of absworption peak is held essentially constant.1600-1800cm-1Place is probably 1629cm-1And 1668cm-1Resultant peak absworption peak, It is attributed to the NO of ADSORPTION STATE2With bridge-type nitrate；1400-1600cm-1Place is probably 1583,1547 and 1434cm-1Resultant peak, Bidentate type nitrate, monodentate type nitrate and nitro are attributed to respectively.In 1100-1200cm-1It is at the weak absorbing peak at place 1080cm-1And 1140cm-1Resultant peak, belongs to Gas Phase Adsorptions of the NO in catalyst surface.Understand that NO adsorbs initial stage, catalyst Surface cation is sufficient, and mainly absorption is in catalyst surface in the form of bridge-type nitro-nitrite by NO, with entering for absorption OK, adsorption product structure changes, Fe-O keys or Fe-N keys the fracture generation nitro compound of bridge-type nitro-nitrite Thing and monodentate type nitrite, while one Cation adsorption position of release carrys out adsorptive gaseous NO to generate Fe-NO compounds.
Fig. 6 is that reaction temperature is NH under the conditions of 300 DEG C3/Ar、NO/O2/ Ar and NH3/NO/O2/ Ar is successively in sintering deposit table The DRIFT spectrograms of face absorption-reaction.The specific order that is passed through is into portable Benitration reactor：First it is passed through 1000ppmNH3/Ar Middle 30min, is then passed through 1000ppmNO+15%O2/ Ar 30min, then it is passed through 1000ppmNH3+ 1000ppmNO+15%O2/Ar 30min, is finally passed through Ar 30min again.30min NH are passed through as shown in figure 5, working as3Afterwards, 1600-1800cm-1And 1400- 1600cm-1Place strong combination absworption peak be respectivelyThe NH at sour site center4 +Ion and Lewis acid site NH3Suction It is attached.Then 30min NO/O are passed through2Afterwards, 1600-1800cm-1And 1400-1600cm-1The strong absworption peak that combines of two of place is to high frequency Field offset, be part nitrate, Lewis acid site NH3 absorption andNH on sour site4 +The superposition of three； 1265cm-1And 1090cm-1Locate emerging absworption peak to be attributed toNH on sour site4 +With the NO of gas phase.And It is passed through 30min NH3/NO/O2Afterwards, 1600-1800cm-1And 1400-1600cm-1Two strong absworption peaks at place are displaced to originally again Position, and absorption peak strength substantially increases.Finally be passed through 30min Ar purging, find absworption peak intensity do not occur it is bright Aobvious change, the 3867cm occurred with whole process-1And 3735cm-1The absworption peak at place is- OH bases on sour site Group.
As shown in Figure 7, NH3The denitration efficiency of denitration reaction is at 300 DEG C when/NO mol ratios are respectively 0.8,0.9,1.0 All reach maximum, respectively 73.64%, 75.21%, 77.57%；When reaction temperature is more than 350 DEG C, different NH3/ NO rubs You start drastically to decline the denitration efficiency of ratio.This is due to the presence of denitration side reaction, at relatively high temperatures in flue gas Part NH3Can be by O2Oxidation is converted into NO, so that cause the concentration of NO in flue gas to raise, denitration efficiency reduction.
The influence result of comprehensive sintering deposit denitration efficiency is understood：Sintering deposit is 250 to the window temperature for sintering denitrating flue gas ~350 DEG C.
As shown in Figure 8, when air speed is from 1000h-1Increase to 2000h-1When, the denitration efficiency of three kinds of temperature reduces amplitude not Greatly, 300 DEG C when sintering deposit denitration efficiency be decreased to 72.92% from 76.50%, at 250 DEG C the denitration efficiency of sintering deposit from 73.75% is decreased to 65.62%, and the denitration efficiency of sintering deposit is decreased to 56.48% from 69.64% at 350 DEG C；When air speed from 2000h-1Increase to 2500h-1When, the denitration efficiency of three kinds of temperature is substantially reduced.

Claims (12)

1. a kind of sintering flue gas SCR denitration technique based on dry method and semi-dry desulphurization, including the 120-140 drawn from sintering machine The 100-110 DEG C of desulfurization fume that DEG C sintering flue gas is obtained after the dedusting of removing dust device and desulphurization system desulfurization successively, it is characterised in that It is further comprising the steps of：
S01,800-900 DEG C of the sintering deposit direct heat transfer in annular cooling device for drawing the desulfurization fume and sintering machine Sintering deposit after sintering flue gas and cooling after must heating up afterwards；
S02, by into step S01 heat up after sintering flue gas in be passed through ammonia control flue gas in NH3/NOxVolume ratio= 0.7~1.0；
S03, by the sintering flue gas mixed in step S02 with ammonia, and sintering deposit, the portable denitration of feeding after cooling in step S01 Selective catalytic reduction reaction is carried out in device；
S04, go out portable denitrification apparatus sintering flue gas be cooled to 100-150 DEG C through waste heat boiler after obtain clean flue gas, then Discharged by chimney, go out the sintering deposit in portable denitrification apparatus or step S03 through secondary waste heat using under feeding after device heat exchange One process.
2. the sintering flue gas SCR denitration technique according to claim 1 based on dry method and semi-dry desulphurization, its feature exists In the feeding vibratory sieve screening of sintering deposit described in step S03, sieve takes the sintering deposit that particle diameter is 5~10mm, the sintering deposit after screening Temperature is 350~400 DEG C, and the sintering deposit is sent into portable denitrification apparatus；The sintering flue gas is mixed with ammonia, then sent Enter portable denitrification apparatus and directly contact carry out selective catalytic reduction reaction with the sintering deposit.
3. the sintering flue gas SCR denitration technique according to claim 1 based on dry method and semi-dry desulphurization, its feature exists In the desulphurization system is dry method or semi-dry desulphurization system.
4. the sintering flue gas SCR denitration technique according to claim 1 based on dry method and semi-dry desulphurization, its feature exists In 800-900 DEG C of sintering deposit reverse direct heat transfer in annular cooling device that the sintering flue gas is drawn with sintering machine.
5. the sintering flue gas SCR denitration technique according to claim 1 based on dry method and semi-dry desulphurization, its feature exists In the sintering flue-gas temperature gone out described in step S01 after being exchanged heat in annular cooling device is increased to 300~350 DEG C.
6. the sintering flue gas SCR denitration technique according to claim 1 based on dry method and semi-dry desulphurization, its feature exists In the sintering deposit temperature gone out described in step S01 after annular cooling device is down to 350~400 DEG C.
7. the sintering flue gas SCR denitration technique according to claim 1 based on dry method and semi-dry desulphurization, its feature exists In O in the sintering flue gas after being heated up described in step S012Concentration is percent by volume 12~18%, and NO concentration is 300- 600mg/Nm3, SO2Concentration be 0-100mg/Nm3。
8. the sintering flue gas SCR denitration technique according to claim 1 based on dry method and semi-dry desulphurization, its feature exists In NH in the desulfurization fume after mixing ammonia described in step S023/NOxVolume ratio=0.8~0.9.
9. the sintering flue gas SCR denitration technique according to claim 1 based on dry method and semi-dry desulphurization, its feature exists In main component is in step S01 or in sintering deposit described in step S03：Fe contents are 50-70wt%, and FeO contents are 5.0- 15.0wt%.
10. the sintering flue gas SCR denitration technique according to claim 1 or 2 based on dry method and semi-dry desulphurization, its feature Be, in the portable denitrification apparatus, it is described sintering flue gas under 300~400 DEG C of environment of temperature the residence time be 1.5~ 2.0s。
11. the sintering flue gas SCR denitration technique according to claim 2 based on dry method and semi-dry desulphurization, its feature exists In the annular cooling device is made up of high temperature section and low-temperature zone, and sintering deposit is entered by the high temperature section of ring-like cooling device, low temperature Section is sent out, and the low-temperature zone that desulfurization fume first sends into ring-like cooling device rises with carrying out once heat exchange positioned at the sintering deposit of low-temperature zone Temperature, is then re-fed into high temperature section with carrying out secondary heat exchange heating positioned at high temperature section sintering deposit, the annular cooling device flue gas goes out Mouth is sequentially connected portable denitrification apparatus and waste heat boiler, and the annular cooling device sintering deposit outlet is connected through vibratory sieve successively To portable denitrification apparatus sintering deposit loading port.
12. the sintering flue gas SCR denitration technique as claimed in claim 11 based on dry method and semi-dry desulphurization, its feature exists In described portable denitrification apparatus includes vertical closed tank, and reaction zone is arranged on the top of tank body, the vertical closing Sintering deposit loading port is provided with the top of tank body, sintering deposit loading port connection vibratory sieve, bottom is provided with sintering deposit and exported, sintering deposit Outlet is provided with rotary seal valve, and tank body top is connected to chimney by denitration exhanst gas outlet pipeline, waste heat boiler, and reaction zone is also Provided with sintering smoke air inlet, annular gas distribution flue and ammonia air inlet, red-hot sintering deposit is encased in reaction zone, sintering deposit Temperature be 350 DEG C~400 DEG C；Then normal temperature ammonia is passed through from reaction zone, 300~350 DEG C of sintering flue gas, sintering flue gas is empty Speed is 1000~3000h-1, red-hot sintering deposit is fully contacted with the sintering flue gas after mixing ammonia in the tank body and selected Selecting property catalytic reduction reaction, reacted sintering deposit row is discharged by tank base, and with the reacted denitration flue gas of sintering deposit then Discharged from tank body top, and be passed through waste heat boiler temperature and be reduced to 100 DEG C~150 DEG C.
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Application publication date: 20170822