CN114042371A - Based on O3-NH3Modulated sintering flue gas desulfurization and denitrification purification process - Google Patents

Based on O3-NH3Modulated sintering flue gas desulfurization and denitrification purification process Download PDF

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CN114042371A
CN114042371A CN202111009393.9A CN202111009393A CN114042371A CN 114042371 A CN114042371 A CN 114042371A CN 202111009393 A CN202111009393 A CN 202111009393A CN 114042371 A CN114042371 A CN 114042371A
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flue gas
sintering flue
active coke
adsorption tower
active
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安忠义
李启超
段伦博
孙镇坤
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Huatian Engineering and Technology Corp MCC
Southeast University
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Huatian Engineering and Technology Corp MCC
Southeast University
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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
    • B01D53/75—Multi-step processes
    • 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
    • B01D53/02—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 by adsorption, e.g. preparative gas chromatography
    • B01D53/04—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 by adsorption, e.g. preparative gas chromatography with stationary adsorbents
    • 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
    • B01D53/76—Gas phase processes, e.g. by using aerosols
    • 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
    • B01D53/8621—Removing nitrogen compounds
    • B01D53/8625—Nitrogen oxides
    • B01D53/8628—Processes characterised by a specific catalyst
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/10—Oxidants
    • B01D2251/104—Ozone
    • 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
    • B01D2253/00—Adsorbents used in seperation treatment of gases and vapours
    • B01D2253/10—Inorganic adsorbents
    • B01D2253/102—Carbon
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/70—Non-metallic catalysts, additives or dopants
    • B01D2255/702—Carbon
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/30—Sulfur compounds
    • B01D2257/302—Sulfur oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/40—Nitrogen compounds
    • B01D2257/404—Nitrogen oxides other than dinitrogen oxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B01D2258/0283—Flue gases

Abstract

The invention discloses a method based on O3‑NH3The modulated sintering flue gas desulfurization denitration purification process. The method comprises the following steps: step one, introducing sintering flue gas into an active coke adsorption tower A to remove SO in the sintering flue gas2(ii) a Step two, utilizing O in the gas mixing tank A3NO in the desulfurized sintering flue gasxCarrying out oxidation; thirdly, the oxidized sintering flue gas enters a gas mixing tank B and NH from an ammonia gas storage tank3Mixing, feeding into active coke adsorption tower B, and reacting under the catalytic action of active cokeThe rapid selective catalytic reduction reaction (rapid SCR) is adopted, so that NO in the sintering flue gas is removedx. The invention utilizes the active coke to remove SO in the sintering flue gas2(ii) a Then the desulfurized sintering flue gas is mixed with O3Mixing, using O3The strong oxidizing property of the catalyst is to remove NO in the sintering flue gasxModulation to NO/NO2A mixture of 1 mol ratio and NH3After being mixed, the mixture is subjected to rapid selective catalytic reduction reaction under the catalytic action of the active coke, so that NO in the sintering flue gas is removedxFinally, the desulfurization and denitrification of the sintering flue gas are realized.

Description

Based on O3-NH3Modulated sintering flue gas desulfurization and denitrification purification process
Technical Field
The invention utilizes the active coke to adsorb SO in the sintering flue gas2And is in H2O and O2Is oxidized to H under an atmosphere of2SO4Thereby removing SO in the sintering flue gas2(ii) a Then the desulfurized sintering flue gas is mixed with O3Mixing, using O3The strong oxidizing property of the catalyst is to remove NO in the sintering flue gasxModulation to NO/NO2A mixture of 1 mol ratio and NH3After being mixed, the mixture is subjected to rapid selective catalytic reduction reaction under the catalytic action of active coke, so that NO in the sintering flue gas is removedxBelonging to the technical field of environmental protection.
Background
China is the first steel producing country in the world, and the steel industry is the prop industry of national economy in China. According to the data of the world iron and steel association, the output of pig iron, crude steel and steel in 2019 in China respectively reaches 8.09 hundred million tons, 9.96 million tons and 12.05 hundred million tons, wherein the output of crude steel accounts for 53.3 percent of the whole world. Sintering flue gas is waste gas discharged in the steel production process, and contains a large amount of Nitrogen Oxides (NO)x) Sulfur dioxide (SO)2) Pollutants such as dioxin, dust and the like can destroy the ozone layer to aggravate the greenhouse effect, form photochemical smog and attractCausing respiratory diseases and the like, and causing great harm to the production, life and ecological environment of people. The departments in the center and all the places continuously issue policies to promote the steel industry to carry out ultralow emission modification.
The mainstream technologies for removing the pollutants in the current sintering flue gas include an active coke desulfurization and denitrification technology and an O3Oxidation absorption techniques, and the like. The desulfurization and denitrification technology of the active coke utilizes the advantages of large specific surface area, rich surface functional groups and the like of the active coke to realize the simultaneous desulfurization and denitrification through adsorption and catalysis mechanisms. In the actual process, two-stage adsorption towers are usually adopted for desulfurization and denitration in sequence, and in the desulfurization section, SO is adsorbed by activated coke2After at O2And H2Oxidizing it to H under O condition2SO4And storing, desulphurizing the flue gas and the introduced NH3And entering a denitration section together to perform Selective Catalytic Reduction (SCR) denitration reaction. The desulfurization rate of the activated coke desulfurization and denitrification technology is high (about more than 95%), the desulfurized and denitrified activated coke can be recycled through thermal regeneration, and the desorbed SO in the thermal regeneration process2Can prepare by-product sulfuric acid so as to reduce the cost, thereby having good development prospect. However, for the actual process operation, the denitration rate of the technology is low (about 75%), and with the gradual advance of the ultra-low emission policy and the increasingly deep social environmental awareness, the technology is gradually difficult to meet the ultra-low emission requirement in the aspect of denitration effect.
O3Oxidation absorption technique using O3Has the advantages of strong oxidizing property, no secondary pollution after oxidation and the like, and adopts O3Oxidizing NO in flue gas into NO with better solubility2And N2O5Followed by the use of Na2S, ammonia, Mg (OH)2The alkali liquor is used for removing NO in a wet desulphurization towerxAnd SO2And simultaneously absorbing to generate corresponding nitrate and sulfate. The desulfurization and denitrification rate of the technology can reach more than 90 percent, but the alkali liquor absorption provides more strict corrosion resistance requirements for the corrosion resistance of equipment and pipelines, and the NO is ensured in the actual processxCan be fully oxidized, and generally needs to be O3O is introduced in an amount of more than 2/NO molar ratio3And the operation cost is greatly improved.
Therefore, the existing mainstream sintering flue gas desulfurization and denitration technology is difficult to realize both high removal rate and low economic cost, so that the optimization and improvement of the existing sintering flue gas desulfurization and denitration technology are necessary.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides a catalyst based on O3-NH3The modulated sintering flue gas desulfurization and denitrification purification process utilizes active coke to adsorb SO in the sintering flue gas2And is in H2O and O2Is oxidized to H under an atmosphere of2SO4Thereby removing SO in the sintering flue gas2(ii) a Then the desulfurized sintering flue gas is mixed with O3Mixing, using O3The strong oxidizing property of the catalyst is to remove NO in the sintering flue gasxModulation to NO/NO2A mixture of 1 mol ratio and NH3After being mixed, the mixture is subjected to rapid selective catalytic reduction under the catalytic action of active coke, so that NO in the sintering flue gas is removedxFinally realizing the desulfurization and denitrification of the sintering flue gas and simultaneously obtaining high-concentration SO2By-products.
To achieve the above object, the present invention is based on O3-NH3The modulated sintering flue gas desulfurization, denitrification and purification process comprises the following steps:
step one, introducing sintering flue gas into an active coke adsorption tower A to remove SO in the sintering flue gas2；
Step two, utilizing O in the gas mixing tank A3NO in the desulfurized sintering flue gasxCarrying out oxidation;
thirdly, the oxidized sintering flue gas enters a gas mixing tank B and NH from an ammonia gas storage tank3Mixing, feeding into active coke adsorption tower B, and performing rapid selective catalytic reduction (rapid SCR) under the catalytic action of active coke to remove NO in the sintering flue gasx。
And further, the step four is included, desorption and regeneration are carried out on the active coke in the active coke adsorption tower A and/or the active coke adsorption tower B at preset time intervals.
Further, the fourth step is specifically: feeding the activated coke in the activated coke adsorption tower A and/or the activated coke adsorption tower B into an activated coke desorption system at intervals of preset time, desorbing and regenerating the activated coke under heating condition, and releasing SO2And the regenerated active coke enters an active coke screening system, the inactivated active coke is screened and discharged, and the rest active coke and the active coke from the active coke storage bin (10) are sent to an active coke adsorption tower B or an active coke adsorption tower A (1) together.
Further, the temperature in the active coke adsorption tower A in the step one is 80-130 ℃, and the pressure is 1000-3000 Pa.
Further, the particle size distribution of the active coke in the step one is 2-12 mm, and the specific surface area is more than 300m2The average pore diameter is more than 2nm, the content of C element is more than 70 percent, and the content of O element is more than 20 percent.
Further, O in the gas mixing tank A is introduced in the step two3Is determined by the mole number of NO in the sintering flue gas, O3The input amount of the catalyst is half of the mole number of NO in the sintering flue gas, and the NO in the sintering flue gas is introducedxTo adjust NO and NO at a molar ratio of 12A mixture of (a).
Further, NH in the gas mixing tank B in the third step3With NOx(specifically, NO and NO in the sintering flue gas)2The sum of the moles) is 1: 1.
And further, in the fourth step, the active coke screening system is used for physically screening according to the difference of the particle sizes of the active coke, active coke powder with the particle size smaller than 2mm is screened out as the inactivated active coke, and the active coke with the particle size distributed within 2-12 mm is re-introduced into the active coke adsorption tower B as a qualified product for regeneration.
To achieve the above object, the present invention is based on O3-NH3The sintering flue gas desulfurization denitration clean system of modulation, the system include:
an air inlet pipe of the active coke adsorption tower A is connected with sintering flue gas, and the sintering flue gas is introduced into the active coke adsorption tower A to remove SO in the sintering flue gas2；
The air outlet pipe of the active coke adsorption tower A and the air outlet pipe of the ozone generator are communicated with the gas mixing tank A so as to utilize O3Oxidizing the desulfurized sintering flue gas;
the gas outlet pipe of the gas mixing tank A and the gas outlet pipe of the ammonia gas storage tank are communicated with the gas mixing tank B;
the gas outlet pipe of the gas mixing tank B is communicated with the gas inlet pipe of the active coke adsorption tower B so as to carry out rapid selective catalytic reduction under the catalytic action of the active coke to remove NO in the sintering flue gasx。
Compared with the prior art, the invention has the following advantages:
1. according to the invention, O3O is introduced in an amount such that the molar ratio of NO/O is 0.53Regulating NO/NO in sintering flue gas2The molar ratio is 1:1, compared with the conventional O3The oxidation absorption process greatly reduces O3The amount of introduction;
2. the active coke has reducibility, and the C-containing functional group on the surface can convert nitrogen oxide NO in high valence state2And N2O5Reducing to NO and simultaneously separating out CO gas. The invention avoids O by arranging the gas mixer A behind the active coke adsorption tower A3NO in oxidized sintering flue gas2Is reduced by active coke; at the same time, in O3Introducing reducing gas NH after oxidation pre-modulation3Significantly reduce NO2The consumption of the active coke prolongs the life cycle of the active coke;
3. the invention absorbs the smoke through the active coke, and does not need to use alkali liquor to absorb NO2Etc. are recycled, avoiding the traditional O3The common problems of alkali liquor corrosion on pipelines and equipment in the oxidation absorption denitration process are solved;
4. by the use of O in the invention3Modulation of NOxMedium NO/NO2In a 1:1 molar ratio, followed by NO under the catalysis of active cokexAnd NH3The rapid SCR reaction is generated, the standard SCR reaction is replaced, and the denitration efficiency is obviously improved.
5. The active coke after catalytic denitration is subjected to adsorption desulfurization reaction, and the desulfurized active coke enters a desorption system for thermal regeneration, so that the efficient utilization of active coke resources is realized.
Drawings
FIG. 1 is a diagram based on O3-NH3Schematic diagram of the modulated sintering flue gas desulfurization and denitrification purification process.
The figure shows that: the device comprises an active coke adsorption tower A (1), a gas mixing tank A (2), a gas mixing tank B (3), an active coke adsorption tower B (4), an oxygen storage tank (5), an ozone generator (6), an ammonia storage tank (7), an active coke desorption system (8), an active coke screening system (9) and an active coke storage bin (10).
Detailed Description
The invention is explained in more detail below with reference to exemplary embodiments and the accompanying drawings. The following examples are not intended to limit the present invention in any way, and all technical solutions obtained by means of equivalent substitution or equivalent transformation are within the scope of the present invention.
Examples
Based on O3-NH3The schematic diagram of the modulated sintering flue gas desulfurization and denitrification purification process is shown in fig. 1, and comprises the following steps:
step one, the sintering flue gas enters an active coke adsorption tower A, and SO in the sintering flue gas is adsorbed by the active coke2And is in H2O and O2Is oxidized to H under an atmosphere of2SO4Thereby removing SO in the sintering flue gas2. In this example, the temperature in the activated coke adsorption column A was 100 ℃ and the pressure was 3000 Pa.
Step two, O in the oxygen storage tank2Entering an ozone generator to react to generate O3Entering a gas mixing tank A to be mixed with the desulfurized sintering flue gas, wherein part of NO in the sintering flue gas is replaced by O3By oxidation to NO2. In this example, the temperature in the gas mixing tank A was 100 ℃ and O3The amount of the oxygen is half of the mole number of NO in the sintering flue gas, and the oxygen is in the range of O3Under the action of strong oxidizing property of the oxygen, NO in the sintering flue gasxTo adjust NO and NO at a molar ratio of 12A mixture of (a).
Thirdly, the oxidized sintering flue gas enters a gas mixing tank B and NH from an ammonia gas storage tank3The components are mixed and then are mixed,the mixture enters an active coke adsorption tower B to generate rapid SCR under the catalytic action of active coke, thereby removing NO in the sintering flue gasx. In this example, the temperature in the gas mixing tank B was 100 ℃ and NH3Is equal to O3NO and NO in oxidized sintering flue gas2The temperature in the active coke-adsorbing tower B was 100 ℃ and the pressure was 3000 Pa.
Sending the active coke in the active coke adsorption tower A into an active coke desorption system at intervals, desorbing and regenerating the active coke under the heating condition, and releasing SO2And the regenerated active coke enters an active coke screening system, the inactivated active coke is screened and discharged, the rest active coke and the active coke from the active coke storage bin are sent to an active coke adsorption tower B together, and redundant active coke in the active coke adsorption tower B is supplemented to an active coke adsorption tower A. The temperature in the active coke desorption system in this example was 300 ℃ and the pressure was-50 Pa.
The temperature in the active coke adsorption tower A in the step one is 80-130 ℃, and the pressure is 1000-3000 Pa. The particle size distribution of the active coke in the step one is 2-12 mm, and the specific surface area is more than 300m2The average pore diameter is more than 2nm, the content of C element is more than 70 percent, and the content of O element is more than 20 percent.
The temperature in the gas mixing tank A in the second step is 80-130 ℃. O introduced into the gas mixing tank A in the second step3Is determined by the mole number of NO in the sintering flue gas, O3The input amount of the catalyst is half of the mole number of NO in the sintering flue gas, and the NO in the sintering flue gas is introducedxTo adjust NO and NO at a molar ratio of 12A mixture of (a).
The temperature in the gas mixing tank B in the third step is 80-130 ℃. NH in gas mixing tank B in step three3With NOx(specifically, NO and NO in the sintering flue gas)2The sum of the moles) is 1: 1. The temperature in the active coke adsorption tower B in the third step is 80-130 ℃, and the pressure is 1000-3000 Pa.
The active coke screening system in the fourth step is used for physically screening active coke with the particle size smaller than 2 according to the difference of the particle sizes of the active cokeAnd (3) screening out mm active coke powder as deactivated active coke, and feeding the active coke with the particle size distributed within 2-12 mm as a regenerated qualified product into an active coke adsorption tower B again. The temperature in the active coke desorption system in the fourth step is 250-350 ℃, and the pressure is-300-50 Pa. In the fourth step, high-concentration SO can be obtained at the outlet of the active coke desorption system2By-products.

Claims (8)

1. Based on O3-NH3The modulated sintering flue gas desulfurization, denitrification and purification process is characterized by comprising the following steps:
step one, introducing sintering flue gas into an active coke adsorption tower A to remove SO in the sintering flue gas2；
Step two, utilizing O in the gas mixing tank A3NO in the desulfurized sintering flue gasxCarrying out oxidation;
thirdly, the oxidized sintering flue gas enters a gas mixing tank B and NH from an ammonia gas storage tank3Mixing, feeding into active coke adsorption tower B, and performing rapid selective catalytic reduction (rapid SCR) under the catalytic action of active coke to remove NO in the sintering flue gasx。
2. An O-based alloy as claimed in claim 13-NH3The modulated sintering flue gas desulfurization, denitrification and purification process is characterized by further comprising a fourth step of desorbing and regenerating the active coke in the active coke adsorption tower A and/or the active coke adsorption tower B at preset time intervals.
3. An O-based alloy as claimed in claim 13-NH3The modulated sintering flue gas desulfurization, denitrification and purification process is characterized by comprising the following steps: feeding the activated coke in the activated coke adsorption tower A and/or the activated coke adsorption tower B into an activated coke desorption system at intervals of preset time, desorbing and regenerating the activated coke under heating condition, and releasing SO2The regenerated active coke enters an active coke screening system, the inactive active coke is screened and discharged, and the rest active coke is mixed with the coming active cokeThe active coke from the active coke storage bin (10) is sent to an active coke adsorption tower B or an active coke adsorption tower A (1).
4. An O-based composition according to claim 13-NH3The modulated sintering flue gas desulfurization and denitrification purification process is characterized in that in the first step, the temperature in the active coke adsorption tower A is 80-130 ℃, and the pressure is 1000-3000 Pa.
5. An O-based composition according to claim 13-NH3The modulated sintering flue gas desulfurization, denitrification and purification process is characterized in that the particle size distribution of the active coke in the step one is 2-12 mm, and the specific surface area is more than 300m2The average pore diameter is more than 2nm, the content of C element is more than 70 percent, and the content of O element is more than 20 percent.
6. An O-based composition according to claim 13-NH3The modulated sintering flue gas desulfurization and denitration purification process is characterized in that O introduced into the gas mixing tank A in the step two3Is determined by the mole number of NO in the sintering flue gas, O3The input amount of the catalyst is half of the mole number of NO in the sintering flue gas, and the NO in the sintering flue gas is introducedxTo adjust NO and NO at a molar ratio of 12A mixture of (a).
7. An O-based composition according to claim 13-NH3The modulated sintering flue gas desulfurization and denitration purification process is characterized in that NH in a gas mixing tank B in the third step3With NOx(specifically, NO and NO in the sintering flue gas)2The sum of the moles) is 1: 1.
8. An O-based composition according to claim 13-NH3The modulated sintering flue gas desulfurization, denitrification and purification process is characterized in that in the fourth step, an active coke screening system screens out active coke powder with the particle size of less than 2mm as inactive active coke, and the active coke with the particle size distributed within 2-12 mm is used as a regenerated qualified productAnd newly enters an active coke adsorption tower B.
CN202111009393.9A 2021-08-31 2021-08-31 Based on O3-NH3Modulated sintering flue gas desulfurization and denitrification purification process Pending CN114042371A (en)

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