CN111715057A - Method and process system for realizing multi-component recovery and resource utilization of flue gas - Google Patents
Method and process system for realizing multi-component recovery and resource utilization of flue gas Download PDFInfo
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- CN111715057A CN111715057A CN202010676097.3A CN202010676097A CN111715057A CN 111715057 A CN111715057 A CN 111715057A CN 202010676097 A CN202010676097 A CN 202010676097A CN 111715057 A CN111715057 A CN 111715057A
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- flue gas
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- 239000003546 flue gas Substances 0.000 title claims abstract description 141
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 124
- 238000000034 method Methods 0.000 title claims abstract description 51
- 238000011084 recovery Methods 0.000 title claims abstract description 20
- 150000003254 radicals Chemical class 0.000 claims abstract description 108
- 239000012528 membrane Substances 0.000 claims abstract description 63
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims abstract description 60
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 50
- 238000010521 absorption reaction Methods 0.000 claims abstract description 45
- 150000001875 compounds Chemical class 0.000 claims abstract description 37
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims abstract description 24
- 239000011593 sulfur Substances 0.000 claims abstract description 23
- 229910052815 sulfur oxide Inorganic materials 0.000 claims abstract description 17
- 239000006227 byproduct Substances 0.000 claims abstract description 15
- 238000004064 recycling Methods 0.000 claims abstract description 14
- 239000007787 solid Substances 0.000 claims abstract description 10
- 239000003054 catalyst Substances 0.000 claims abstract description 8
- 238000011065 in-situ storage Methods 0.000 claims abstract description 8
- 239000002245 particle Substances 0.000 claims abstract description 8
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims abstract description 7
- 230000001590 oxidative effect Effects 0.000 claims abstract description 7
- 150000003839 salts Chemical class 0.000 claims abstract description 7
- 229910052717 sulfur Inorganic materials 0.000 claims abstract description 6
- 239000002808 molecular sieve Substances 0.000 claims description 28
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 28
- 239000011248 coating agent Substances 0.000 claims description 27
- 238000000576 coating method Methods 0.000 claims description 27
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 21
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims description 18
- 239000000428 dust Substances 0.000 claims description 17
- 238000006477 desulfuration reaction Methods 0.000 claims description 16
- 230000023556 desulfurization Effects 0.000 claims description 16
- 229910021536 Zeolite Inorganic materials 0.000 claims description 11
- 239000007788 liquid Substances 0.000 claims description 11
- 239000010457 zeolite Substances 0.000 claims description 11
- 229910044991 metal oxide Inorganic materials 0.000 claims description 10
- 150000004706 metal oxides Chemical class 0.000 claims description 10
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 9
- 229910017604 nitric acid Inorganic materials 0.000 claims description 9
- 238000005507 spraying Methods 0.000 claims description 9
- 238000003860 storage Methods 0.000 claims description 9
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 8
- 239000012530 fluid Substances 0.000 claims description 8
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 7
- 239000012267 brine Substances 0.000 claims description 6
- 229910052878 cordierite Inorganic materials 0.000 claims description 6
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 claims description 6
- 239000013505 freshwater Substances 0.000 claims description 6
- 238000010438 heat treatment Methods 0.000 claims description 6
- HPALAKNZSZLMCH-UHFFFAOYSA-M sodium;chloride;hydrate Chemical compound O.[Na+].[Cl-] HPALAKNZSZLMCH-UHFFFAOYSA-M 0.000 claims description 6
- 230000003197 catalytic effect Effects 0.000 claims description 5
- 239000000919 ceramic Substances 0.000 claims description 5
- 238000000909 electrodialysis Methods 0.000 claims description 5
- 238000009292 forward osmosis Methods 0.000 claims description 5
- 239000012510 hollow fiber Substances 0.000 claims description 5
- 238000005373 pervaporation Methods 0.000 claims description 5
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims description 5
- 229910010271 silicon carbide Inorganic materials 0.000 claims description 5
- KZHJGOXRZJKJNY-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Si]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O KZHJGOXRZJKJNY-UHFFFAOYSA-N 0.000 claims description 4
- 229910052863 mullite Inorganic materials 0.000 claims description 4
- 239000003921 oil Substances 0.000 claims description 4
- 150000001298 alcohols Chemical class 0.000 claims description 3
- -1 alkane compounds Chemical class 0.000 claims description 3
- 229910052757 nitrogen Inorganic materials 0.000 claims description 3
- 238000012546 transfer Methods 0.000 claims description 3
- 239000002918 waste heat Substances 0.000 claims description 3
- 229910002651 NO3 Inorganic materials 0.000 claims description 2
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 2
- PFRUBEOIWWEFOL-UHFFFAOYSA-N [N].[S] Chemical compound [N].[S] PFRUBEOIWWEFOL-UHFFFAOYSA-N 0.000 claims description 2
- 239000012670 alkaline solution Substances 0.000 claims description 2
- 238000010612 desalination reaction Methods 0.000 claims description 2
- 239000007789 gas Substances 0.000 claims description 2
- 239000002608 ionic liquid Substances 0.000 claims description 2
- 238000007670 refining Methods 0.000 claims description 2
- 239000003344 environmental pollutant Substances 0.000 abstract description 8
- 231100000719 pollutant Toxicity 0.000 abstract description 8
- 239000000779 smoke Substances 0.000 abstract description 6
- 238000005516 engineering process Methods 0.000 description 18
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 12
- 239000000243 solution Substances 0.000 description 10
- 239000002250 absorbent Substances 0.000 description 6
- 230000002745 absorbent Effects 0.000 description 6
- 238000010586 diagram Methods 0.000 description 5
- 239000003999 initiator Substances 0.000 description 5
- 230000001502 supplementing effect Effects 0.000 description 5
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 4
- ZCCIPPOKBCJFDN-UHFFFAOYSA-N calcium nitrate Chemical compound [Ca+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ZCCIPPOKBCJFDN-UHFFFAOYSA-N 0.000 description 4
- OSGAYBCDTDRGGQ-UHFFFAOYSA-L calcium sulfate Chemical compound [Ca+2].[O-]S([O-])(=O)=O OSGAYBCDTDRGGQ-UHFFFAOYSA-L 0.000 description 4
- 238000011161 development Methods 0.000 description 4
- 229910000831 Steel Inorganic materials 0.000 description 3
- 239000000571 coke Substances 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 239000007800 oxidant agent Substances 0.000 description 3
- 230000003647 oxidation Effects 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- 238000005245 sintering Methods 0.000 description 3
- 239000010959 steel Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- AXCZMVOFGPJBDE-UHFFFAOYSA-L calcium dihydroxide Chemical compound [OH-].[OH-].[Ca+2] AXCZMVOFGPJBDE-UHFFFAOYSA-L 0.000 description 2
- 238000004939 coking Methods 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 239000004575 stone Substances 0.000 description 2
- 239000013589 supplement Substances 0.000 description 2
- PAWQVTBBRAZDMG-UHFFFAOYSA-N 2-(3-bromo-2-fluorophenyl)acetic acid Chemical compound OC(=O)CC1=CC=CC(Br)=C1F PAWQVTBBRAZDMG-UHFFFAOYSA-N 0.000 description 1
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 1
- 239000005864 Sulphur Substances 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 235000011114 ammonium hydroxide Nutrition 0.000 description 1
- BFNBIHQBYMNNAN-UHFFFAOYSA-N ammonium sulfate Chemical compound N.N.OS(O)(=O)=O BFNBIHQBYMNNAN-UHFFFAOYSA-N 0.000 description 1
- 229910052921 ammonium sulfate Inorganic materials 0.000 description 1
- 235000011130 ammonium sulphate Nutrition 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 238000011033 desalting Methods 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- CVQGBZGCMIYEGG-UHFFFAOYSA-N ethane-1,2-diamine;2-hydroxypropane-1,2,3-tricarboxylic acid Chemical compound NCCN.OC(=O)CC(O)(C(O)=O)CC(O)=O CVQGBZGCMIYEGG-UHFFFAOYSA-N 0.000 description 1
- 239000008187 granular material Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000001172 regenerating effect Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
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- 239000007921 spray Substances 0.000 description 1
- 230000026676 system process Effects 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
Images
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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
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/60—Simultaneously removing sulfur oxides and 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
-
- 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
- B01D53/77—Liquid phase processes
- B01D53/78—Liquid phase processes with gas-liquid contact
-
- 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
-
- 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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- Environmental & Geological Engineering (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Treating Waste Gases (AREA)
- Separation Using Semi-Permeable Membranes (AREA)
Abstract
The invention discloses a method and a process system for realizing multi-component recovery and resource utilization of flue gas, and belongs to the technical field of treatment of atmospheric pollutants. The method comprises the steps of catalyzing a free radical source compound to generate free radicals, oxidizing low-valence sulfur and nitrogen oxides in flue gas in situ, and obtaining sulfur and nitrogen containing byproducts through absorption and enrichment; the water is recovered and utilized by a membrane method, and solid particles and miscellaneous salts are separated at the same time. The invention also discloses a process system for realizing the method, which is characterized in that a free radical exciter with a built-in heat source and a catalyst coated on the outer surface is arranged in the flue to serve as a flue gas pretreatment system, and the generated free radicals are used for oxidizing sulfur and nitrogen oxides and then absorbing the oxidized sulfur and nitrogen oxides by absorption liquidAnd collecting, and recycling water through a membrane system to reach the standard and discharge. The invention is used for treating SO in flue gas2、NOx、H2And removing multiple components such as O, solid miscellaneous salt and the like to ensure that the smoke reaches the emission standard, and simultaneously, obtaining sulfur and nitrogen containing byproducts, recycling water and realizing the recovery and resource utilization of the multiple components in the smoke.
Description
Technical Field
The invention belongs to the technical field of atmospheric pollutant treatment, and relates to a method and a process system for realizing multi-component recovery and resource utilization of flue gas.
Background
The flue gas contains SO2、NOx、H2O and SO on, with respect to SO in flue gas2And NOxEmission control of (b) has been the focus of environmental concern. Through the development of decades, the flue gas desulfurization technology, the flue gas denitration technology and other single pollutant control technologies are applied on a large scale, and the desulfurization and denitration integrated technology is relatively slow in development. At present, the traditional FGD + SCR combined desulfurization and denitrification technology has the defects of complex system, high equipment investment and operation cost and the like, and the FGD + SNCR combined desulfurization and denitrification technology has the problems of low denitrification efficiency, serious ammonia escape and the like. Under the situation that the environmental protection standard is continuously improved, the development of a novel and efficient integrated technology for flue gas desulfurization and denitration is a research hotspot in the field at present.
In the currently reported desulfurization and denitrification integrated technology, the oxidation-absorption technology can not only remove SO efficiently2And NOxAnd simultaneously, the recycling and utilization of the material can be realized. Due to NO in the flue gasxIs mainly insolubleThe oxidation of water-soluble NO to water-soluble higher nitrogen oxides is key to the oxidation-absorption technique. The German Linde company develops the LoTO using ozone to oxidize NO as the technical corexThe technology comprises the following technological processes: spraying ozone into the low-temperature flue gas at 100-150 ℃ to oxidize NO into high valence state, and absorbing with alkali liquor to obtain high-efficiency denitration efficiency. However, oxidant cost is a bottleneck for this technology. For example, 1 ton of NO is oxidized to NO2Theoretically, 1.6 tons of ozone needs to be consumed, and the high production cost of the ozone causes the high running cost of the technology, thereby seriously restricting the popularization and the application of the technology. Relevant studies show that free radicals generated from low-cost compounds can oxidize low-concentration NO into high-valence nitrogen oxides at proper temperature, and the free radicals are ideal oxidants. However, the current technology has very strict requirements on the working condition of the flue gas due to the difficulties of short existence time of free radicals and narrow active temperature window. Therefore, the development of the oxidation-absorption technology based on efficient free radicals is expected to greatly reduce the cost for removing the smoke pollutants. Meanwhile, the smoke after oxidation-absorption treatment contains a large amount of moisture, which not only causes the phenomenon of 'white smoke', but also causes a large amount of waste of water resources, and the recycling of the moisture in the smoke has attracted great attention of people.
In summary, the SO in the flue gas is aimed at2、NOx、H2And the components such as O and the like have important significance in developing an economical and efficient flue gas multi-component recycling and resource utilization technology.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention aims to provide a method and a process system for realizing multi-component recovery and resource utilization of flue gas. By using the method and utilizing the system process, SO in the multi-component components of the flue gas can be converted2And NOxThe in-situ oxidation-absorption is carried out to realize high-efficiency desulfurization and denitrification, simultaneously the water is recycled, and the recycling and resource utilization of multi-component substances in the flue gas are realized while the standard emission of the flue gas is realized.
In order to achieve the purpose, the invention adopts the following technical scheme to realize the purpose:
the invention discloses a method for realizing multi-component recovery and resource utilization of flue gas, which comprises the following steps:
step 1, preheating a free radical source compound, generating free radicals under the catalytic action of a catalyst coating on the surface of a built-in free radical exciter of a flue, contacting flue gas entering the flue with the free radicals, and oxidizing low-valence sulfur and nitrogen oxides contained in the flue gas in situ to obtain pretreated flue gas containing high-valence sulfur and nitrogen oxides;
step 2, removing solid particles in the pretreated flue gas obtained in the step 1, absorbing high-valence sulfur and nitrogen oxides in the pretreated flue gas, and enriching to obtain sulfur and nitrogen containing byproducts and desulfurization and denitrification flue gas;
step 3, collecting moisture in the desulfurization and denitrification flue gas obtained in the step 2 to obtain moisture and dischargeable flue gas; and one part of the collected water is used for absorbing water of high-valence sulfur and nitrogen oxides, and the other part of the collected water is subjected to desalting operation to obtain strong brine and fresh water, wherein the strong brine is evaporated by utilizing the waste heat of the flue gas to obtain miscellaneous salt solid particles, and the fresh water is used for preparing the free radical source compound.
Preferably, in step 1, the radical source compound comprises at least one of water, hydrogen peroxide, nitric acid, alcohols and alkane compounds; the preheating temperature of the free radical source compound is 50-100 ℃.
Preferably, the catalyst coating on the surface of the flue built-in free radical exciter is a coating surface containing a zeolite molecular sieve or a metal oxide modified zeolite molecular sieve, a built-in heat source is arranged in the flue built-in free radical exciter and used for keeping the surface temperature of the coating at 200-550 ℃.
Preferably, the flue gas contains SO2And NOxAny source off-gas of a component; the sulfur-and nitrogen-containing by-products comprise SO2Any one of sulfuric acid and sulfate, and NOxNitric acid, and nitrate.
The invention also discloses a process system for realizing the preparation method, which comprises a flue built-in free radical exciter, a dust remover, an absorption device, a primary membrane system, a secondary membrane system and a free radical source compound storage tank;
the free radical exciter arranged in the flue is arranged in the flue gas pipeline, the outlet end of the flue gas pipeline is connected to the inlet of the dust remover through a pipeline, the outlet of the dust remover is connected to the inlet of the absorption device through a pipeline, and the outlet of the absorption device is connected to the chimney through a primary membrane system; the free radical source compound storage tank extends into the flue gas pipeline through the spraying pipeline, and the tail end of the spraying pipeline faces the free radical exciter; leading-out pipelines of the first-stage membrane system are respectively connected into an absorption device and a second-stage membrane system, and leading-out pipelines of the second-stage membrane system are respectively connected into a pipeline at the inlet end of a dust remover and a free radical source compound storage tank;
the free radical exciter comprises an exciter channel with a built-in heat source, the outer surface of the exciter channel is coated with a coating containing a zeolite molecular sieve or a metal oxide modified zeolite molecular sieve, and the built-in heat source enables the temperature of the outer surface of the exciter channel to be maintained at 200-550 ℃.
Preferably, an absorption liquid is arranged in the absorption device, and the absorption liquid is composed of at least one of water, hydrogen peroxide, alkaline solution and ionic liquid.
Preferably, the primary membrane system is a ceramic membrane, a hollow fiber membrane or a molecular sieve membrane, and the secondary membrane system is a pervaporation membrane, an electrodialysis membrane or a forward osmosis membrane.
Preferably, the exciter passage is made of cordierite, silicon carbide or mullite.
Preferably, the built-in heat source of the energizer channel is a heating wire or a hot fluid.
Further preferably, the hot fluid comprises hot flue gas, hot air, hot nitrogen or heat transfer oil.
Compared with the prior art, the invention has the following beneficial effects:
the invention discloses a method for realizing multi-component recovery and resource utilization of flue gas, which is characterized in that a flue built-in free radical exciter is arranged in a matching manner, a catalyst coating is coated on the surface of the flue built-in free radical exciter, and a free radical source compound is catalyzedThe free radical is generated, in the process, reasonable catalysis temperature can be provided through the built-in free radical exciter of the flue, and the purpose of generating free radicals with controllable temperature is achieved, so that the free radical generating device is suitable for wide flue gas temperature window and can be applied to flue gas treatment under various working conditions; then, the obtained free radicals are utilized to oxidize low-valence sulfur and nitrogen oxides in the flue gas into high-valence sulfur and nitrogen containing byproducts in situ through absorption and enrichment, and meanwhile, the flue gas reaches the emission standard; the water in the desulfurization and denitrification flue gas is collected and recycled to the water replenishing of an absorption system and the preparation of a free radical source compound, so that the recycling of the water in the flue gas is realized; and removing solid dust in the flue gas and miscellaneous salt particles in the wastewater through separation. Therefore, the method can be used for treating SO in the flue gas2、NOx、H2And O and other multi-components are removed, so that the high-efficiency recovery and resource utilization of the flue gas can be realized while the flue gas is discharged up to the standard.
Furthermore, a coating containing a zeolite molecular sieve or a metal oxide modified zeolite molecular sieve is coated on a built-in free radical exciter in a flue, the catalytic temperature is controlled by a built-in heat source, a low-cost free radical source compound is used for catalyzing to generate free radicals, low-valence sulfur and nitrogen oxides in flue gas are efficiently oxidized into high-valence compounds in situ, the cost of an oxidant is greatly reduced, and the operation cost of the oxidation-absorption desulfurization and denitrification integrated technology is remarkably reduced.
The invention also discloses a process system for realizing the method for realizing the multi-component recovery and resource utilization of the flue gas. In the process system, a flue built-in free radical exciter is adopted, and a coating containing a zeolite molecular sieve or a metal oxide modified zeolite molecular sieve is coated on the surface of the flue built-in free radical exciter, SO that a free radical source compound can generate free radicals under the catalytic action of the coating on the surface of the free radical exciter, and further SO in flue gas is treated2、NOxCarrying out in-situ efficient oxidation; through setting up corresponding dust remover, absorbing device, one-level membrane system and second grade membrane system, can collect solid dust and miscellaneous salt granule in the flue gas, absorb the enrichment to high valence state sulphur, nitrogen oxide and getSulfur and nitrogen containing byproducts and water are recycled, so that multi-component recycling and resource utilization in the flue gas are realized.
Further, through adopting diversified heating methods such as heating wire or hot-fluid to heat the energizer passageway, can be applicable to under the multiple concrete operating mode condition.
Drawings
FIG. 1 is a technical route diagram of a method for realizing multi-component recycling and resource utilization of flue gas according to the present invention;
FIG. 2 is a schematic structural diagram of a built-in free radical exciter of a flue in the process system for realizing multi-component recovery and resource utilization of flue gas;
FIG. 3 is a schematic diagram of a process system for realizing multi-component recycling and resource utilization of flue gas.
Wherein: 1-flue gas; 2-flue built-in free radical exciter; 3-a dust remover; 4-an absorption device; 5-a first-stage membrane system; 6, a fan; 7-a chimney; 8-a secondary membrane system; 9-a reservoir of a compound of free radical origin; 10-a heater; 11-flue gas duct; 12-spraying a pipeline; 201-exciter channel; 202-coating.
Detailed Description
In order to make the technical solutions of the present invention better understood, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
It should be noted that the terms "first," "second," and the like in the description and claims of the present invention and in the drawings described above are used for distinguishing between similar elements and not necessarily for describing a particular sequential or chronological order. It is to be understood that the data so used is interchangeable under appropriate circumstances such that the embodiments of the invention described herein are capable of operation in sequences other than those illustrated or described herein. Furthermore, the terms "comprises," "comprising," and "having," and any variations thereof, are intended to cover a non-exclusive inclusion, such that a process, method, system, article, or apparatus that comprises a list of steps or elements is not necessarily limited to those steps or elements expressly listed, but may include other steps or elements not expressly listed or inherent to such process, method, article, or apparatus.
The invention is described in further detail below with reference to the accompanying drawings:
referring to fig. 1, a technical route of the method for realizing multi-component recycling and resource utilization of flue gas of the present invention includes the following steps:
step 1, heating and preheating a free radical source compound, generating free radicals under the catalytic action of a catalyst coating on the surface of a built-in free radical exciter of a flue, contacting flue gas entering the flue with the free radicals, and oxidizing low-valence sulfur and nitrogen oxides contained in the flue gas in situ to obtain pretreated flue gas containing high-valence sulfur and nitrogen oxides;
step 2, performing dust removal treatment on the pretreated flue gas obtained in the step 1, removing solid particles in the pretreated flue gas obtained in the step 1, absorbing high-valence sulfur and nitrogen oxides in the pretreated flue gas, and performing absorption enrichment to obtain sulfur and nitrogen containing byproducts and desulfurization and denitrification flue gas;
step 3, collecting moisture (catching water) of the desulfurization and denitrification flue gas obtained in the step 2 to obtain moisture and dischargeable flue gas (purified flue gas); and in the collected water, one part of the collected water is conveyed to an absorption device to be used for absorbing water of high-valence sulfur and nitrogen oxides, and the other part of the collected water is subjected to desalination operation through a refining process to obtain strong brine and fresh water, wherein the strong brine is evaporated by utilizing the waste heat of the flue gas to obtain miscellaneous salt solid particles, and the fresh water is used for preparing a free radical source compound.
Specifically, in step 1, the radical source compound comprises at least one of water, hydrogen peroxide, nitric acid, alcohols and alkane compounds; preheating the free radical source compound at 50-100 ℃; the flue gas contains SO2、NOxAnd the like, including but not limited to coal-fired power plant flue gas, steel sintering flue gas, coke oven flue gas and the like.
Referring to fig. 3, a schematic diagram of a process system for implementing multi-component recycling and resource utilization of flue gas of the present invention is shown, so that the process system specifically includes: the device comprises a free radical exciter 2, a dust remover 3, an absorption device 4, a primary membrane system 5, a secondary membrane system 8 and a free radical source compound storage tank 9 which are arranged in a flue;
the free radical exciter 2 arranged in the flue is arranged in a flue gas pipeline 11, the outlet end of the flue gas pipeline 11 is connected to the inlet of a dust remover 3 through a pipeline, the outlet of the dust remover 3 is connected to the inlet of an absorption device 4 through a pipeline, the outlet of the absorption device 4 is connected to a chimney 7 through a primary membrane system 5, and a fan 6 is arranged between the primary membrane system 5 and the chimney 7; the free radical source compound storage tank 9 extends into the flue gas pipeline 11 through the spraying pipeline 12, the tail end of the spraying pipeline 12 faces the free radical exciter 2, the spraying pipeline 12 is further provided with a heater 10, and the heater 10 is used for preheating the free radical source compound; leading-out pipelines of the first-stage membrane system 5 are respectively connected to the absorption device 4 and the second-stage membrane system 8, and leading-out pipelines of the second-stage membrane system 8 are respectively connected to a pipeline at the inlet end of the dust remover 3 and a free radical source compound storage tank 9;
the built-in free radical exciter 2 of the flue comprises an exciter channel 201 with a built-in heat source, a coating 202 containing a zeolite molecular sieve or a metal oxide modified zeolite molecular sieve is coated on the outer surface of the exciter channel 201, the built-in heat source enables the temperature of the outer surface of the exciter channel 201 to be maintained at 200-550 ℃ for enabling a free radical source compound to generate free radicals, and the flue gas 1 is introduced into the flue gas pipeline 11 and oxidized by the free radicals.
Specifically, referring to fig. 2, which is a schematic structural diagram of a flue built-in free radical exciter in the flue gas pretreatment system of the present invention, it can be known that the specific operation of generating free radicals by the free radical source compound is as follows: the free radical exciter 2 with the built-in flue is arranged in the flue gas pipeline 11, a free radical source compound is preheated and then sprayed on the surface of a coating 202 containing a zeolite molecular sieve or a metal oxide modified zeolite molecular sieve, and the surface temperature of the coating 202 is 200-550 ℃. When the internal heat source of the exciter channel 201 is a hot fluid, including but not limited to hot flue gas, hot air, hot nitrogen, heat transfer oil and other hot fluids, the flow direction of the hot fluid may be the same as or opposite to the flow direction of the flue gas 1; the cavity cross section of the exciter channel 201 is in any geometrical shape such as a circle, a rectangle, a hexagon and the like.
Specifically, the exciter channel 201 is made of a single material or a composite material such as cordierite, silicon carbide, mullite and the like, which can withstand a high temperature of more than 600 ℃; the first-stage membrane system 5 is a ceramic membrane, a hollow fiber membrane, a molecular sieve membrane and the like, and the second-stage membrane system 8 is a high-concentration-rate membrane such as a pervaporation membrane, an electrodialysis membrane, a forward osmosis membrane and the like.
Specifically, the preheated radical source compound is sprayed onto the surface catalyst coating 202 of the flue built-in radical initiator by using a spray gun.
The present invention will be described in detail with reference to the following specific examples:
example 1
Treating the flue gas of the coal-fired power plant, wherein the temperature of the flue gas is 300 ℃, and SO in the flue gas2The content is 2000mg/m3、NOxThe content is 350mg/m3. The free radical exciter is made of silicon carbide, the cross section of the cavity is circular, the surface of the cavity is provided with a zeolite molecular sieve coating, and hot flue gas is introduced to control the temperature of the outer surface of the cavity to be 500 ℃. The methanol solution is preheated to 50 ℃ and then sprayed on the outer surface of the free radical exciter to generate free radicals. Adopting calcium hydroxide solution as absorbent to wash flue gas, and treating SO in the flue gas2And NOxThe content is respectively lower than 35mg/m3And 50mg/m3The absorption liquid is evaporated and concentrated to obtain the by-products of calcium sulfate and calcium nitrate. And (3) recovering the water of the washed flue gas through a hollow fiber membrane, wherein the recovery rate is 46%, part of water is directly recycled for supplementing water to an absorption system, and the other part of water is treated by a pervaporation membrane and then is used for preparing a methanol solution.
Example 2
Treating the flue gas of the coal-fired power plant, wherein the temperature of the flue gas is 300 ℃, and SO in the flue gas2The content is 2000mg/m3、NOxThe content is 350mg/m3. Free radical exciterThe material of the hollow cavity is cordierite, the cross section of the cavity is rectangular, the surface is a zeolite molecular sieve coating, and hot air is introduced to control the temperature of the outer surface to be 360 ℃. The hydrogen peroxide solution is preheated to 80 ℃ and sprayed on the outer surface of the free radical initiator to generate free radicals. Adopting hydrogen peroxide solution as absorbent to wash flue gas, and treating SO in the flue gas2And NOxThe content is respectively lower than 35mg/m3And 50mg/m3The absorption liquid is evaporated and concentrated to obtain the by-products sulfuric acid and nitric acid. And (3) recovering the water of the washed flue gas through a ceramic membrane, wherein the recovery rate is 47%, part of water is directly recycled for supplementing water of an absorption system, and the other part of water is treated by a forward osmosis membrane and then is used for preparing a hydrogen peroxide solution.
Example 3
Treating coke oven flue gas at 260 deg.C and SO2The content is 300mg/m3、NOxThe content is 1100mg/m3. The free radical exciter is made of silicon carbide, the cross section of the cavity is circular, the surface of the cavity is provided with a zeolite molecular sieve coating, and hot flue gas is introduced to control the temperature of the outer surface of the cavity to be 500 ℃. The methanol solution was preheated to 50 ℃ and sprayed on the outer surface of the radical initiator to generate radicals. Adopting ethylenediamine citric acid solution as absorbent to wash flue gas, and treating SO in the flue gas2And NOxThe content is respectively lower than 30mg/m3And 150mg/m3Reaching the special emission limit of atmospheric pollutants in the emission Standard of pollutants for coking chemical industry (GB 16171-2012), and heating and regenerating the absorption liquid to obtain a byproduct high-concentration SO2And NOx. And (3) recovering the water of the washed flue gas through a molecular sieve membrane, wherein the recovery rate is 42%, part of water is directly recycled for supplementing water of an absorption system, and the other part of water is treated by an electrodialysis membrane and then is used for preparing a methanol solution.
Example 4
Treating coke oven flue gas at 260 deg.C and SO2The content is 300mg/m3、NOxThe content is 1100mg/m3. The free radical exciter is made of cordierite, the cross section of the cavity is rectangular, and the surface of the cavity is modified by metal oxideAnd (3) coating the stone molecular sieve, and introducing hot air of heat-conducting oil to control the temperature of the outer surface of the stone molecular sieve to be 360 ℃. The hydrogen peroxide solution is preheated to 80 ℃ and sprayed on the outer surface of the free radical initiator to generate free radicals. Ammonia water solution is used as absorbent to wash flue gas, and SO in the treated flue gas2And NOxThe content is respectively lower than 30mg/m3And 150mg/m3And the special emission limit of atmospheric pollutants reaches the emission standard of pollutants for the coking chemical industry (GB 16171-2012), and the absorption liquid is evaporated and concentrated to obtain byproducts of ammonium sulfate and ammonium nitrate. And (3) recovering the water of the washed flue gas through a hollow fiber membrane, wherein the recovery rate is 45%, part of water is directly recycled for water supplement of an absorption system, and the other part of water is treated by a pervaporation membrane and then is used for preparing a hydrogen peroxide solution.
Example 5
Treating the steel sintering flue gas with the temperature of 150 ℃ and SO in the flue gas2The content is 800mg/m3、NOxThe content is 320mg/m3. The free radical exciter is made of mullite, the cross section of the cavity is hexagonal, the surface of the cavity is a metal oxide modified zeolite molecular sieve coating, and hot flue gas is introduced to control the temperature of the outer surface of the cavity to be 400 ℃. The nitric acid solution is preheated to 100 ℃ and sprayed on the outer surface of the free radical exciter to generate free radicals. Adopting calcium hydroxide solution as absorbent to wash flue gas, and treating SO in the flue gas2And NOxThe content is respectively lower than 35mg/m3And 50mg/m3And the absorption liquid is evaporated and concentrated to obtain byproducts calcium sulfate and calcium nitrate. And (3) recovering the water of the washed flue gas through a ceramic membrane, wherein the recovery rate is 43%, part of water is directly recycled for supplementing water of an absorption system, and the other part of water is treated by a forward osmosis membrane and then is used for preparing a nitric acid solution.
Example 6
Treating the steel sintering flue gas with the temperature of 150 ℃ and SO in the flue gas2The content is 800mg/m3、NOxThe content is 320mg/m3. The free radical exciter is made of cordierite, the cross section of the cavity is rectangular, the surface of the cavity is provided with a metal oxide modified zeolite molecular sieve coating, and heat is introducedThe external surface temperature of the nitrogen gas was controlled to 360 ℃. The hydrogen peroxide solution is preheated to 80 ℃ and sprayed on the outer surface of the free radical initiator to generate free radicals. Adopting hydrogen peroxide solution as absorbent to wash flue gas, and treating SO in the flue gas2And NOxThe content is respectively lower than 35mg/m3And 50mg/m3The absorption liquid is evaporated and concentrated to obtain the by-products sulfuric acid and nitric acid. And (3) recovering the water of the washed flue gas through a molecular sieve membrane, wherein the recovery rate is 45%, part of water is directly recycled for supplementing water to an absorption system, and the other part of water is treated by an electrodialysis membrane and then is used for preparing a hydrogen peroxide solution.
In conclusion, the invention discloses a method for realizing multi-component recovery and resource utilization of flue gas and a process system thereof. A free radical exciter containing a built-in heat source and an outer surface coating is arranged in a flue to serve as a flue gas pretreatment system, and free radicals generated by a low-cost free radical source compound are used for converting SO in flue gas2、NOxThe oxidation method is suitable for wide temperature window of the flue gas, can be applied to various working conditions, enables free radicals to be easily generated, and is further applied to the subsequent pretreatment of the flue gas. The formed high-valence compounds are absorbed by absorption liquid to realize high-efficiency desulfurization and denitrification of the flue gas, the purified flue gas is discharged after reaching the standard after moisture is recovered by a membrane system, and the trapped moisture can be respectively recycled for water supplement of an absorption system and preparation of a free radical source compound. Compared with the prior art, the technology has obvious advancement and economy.
The above-mentioned contents are only for illustrating the technical idea of the present invention, and the protection scope of the present invention is not limited thereby, and any modification made on the basis of the technical idea of the present invention falls within the protection scope of the claims of the present invention.
Claims (10)
1. A method for realizing multi-component recovery and resource utilization of flue gas is characterized by comprising the following steps:
step 1, preheating a free radical source compound, generating free radicals under the catalytic action of a catalyst coating on the surface of a built-in free radical exciter of a flue, contacting flue gas entering the flue with the free radicals, and oxidizing low-valence sulfur and nitrogen oxides contained in the flue gas in situ to obtain pretreated flue gas containing high-valence sulfur and nitrogen oxides;
step 2, removing solid particles in the pretreated flue gas obtained in the step 1, absorbing high-valence sulfur and nitrogen oxides in the pretreated flue gas, and enriching to obtain sulfur and nitrogen containing byproducts and desulfurization and denitrification flue gas;
step 3, collecting moisture of the desulfurization and denitrification flue gas obtained in the step 2 to obtain moisture and dischargeable flue gas; and one part of the collected water is used for absorbing water of high-valence sulfur and nitrogen oxides, and the other part of the collected water is subjected to desalination refining operation to obtain strong brine and fresh water, wherein the strong brine is evaporated by utilizing the waste heat of the flue gas to obtain miscellaneous salt solid particles, and the fresh water is used for preparing the free radical source compound.
2. The method for realizing multi-component recycling and resource utilization of flue gas according to claim 1, wherein in the step 1, the radical source compound comprises at least one of water, hydrogen peroxide, nitric acid, alcohols and alkane compounds; the preheating temperature of the free radical source compound is 50-100 ℃.
3. The method for realizing multi-component recovery and resource utilization of flue gas according to claim 1, wherein the surface catalyst coating of the built-in flue free radical exciter is the surface of a coating containing a zeolite molecular sieve or a metal oxide modified zeolite molecular sieve, a built-in heat source is arranged in the built-in flue free radical exciter and is used for keeping the surface temperature of the coating at 200-550 ℃.
4. The method for realizing multi-component recycling and resource utilization of flue gas as claimed in claim 1, wherein the flue gas contains SO2And NOxAny source off-gas of a component;
the sulfur-and nitrogen-containing by-products comprise SO2Any one of sulfuric acid and sulfate, and NOxNitric acid, and nitrate.
5. A process system for implementing the method according to any one of claims 1 to 4, characterized by comprising a flue built-in free radical exciter (2), a dust remover (3), an absorption device (4), a primary membrane system (5), a secondary membrane system (8) and a free radical source compound storage tank (9);
the free radical exciter (2) arranged in the flue is arranged in a flue gas pipeline (11), the outlet end of the flue gas pipeline (11) is connected to the inlet of the dust remover (3) through a pipeline, the outlet of the dust remover (3) is connected to the inlet of the absorption device (4) through a pipeline, and the outlet of the absorption device (4) is connected to a chimney (7) through a primary membrane system (5); the free radical source compound storage tank (9) extends into the flue gas pipeline (11) through the spraying pipeline (12), and the tail end of the spraying pipeline (12) faces the free radical exciter (2); leading-out pipelines of the first-stage membrane system (5) are respectively connected into the absorption device (4) and the second-stage membrane system (8), and leading-out pipelines of the second-stage membrane system (8) are respectively connected into a pipeline at the inlet end of the dust remover (3) and a free radical source compound storage tank (9);
the free radical exciter (2) comprises an exciter channel (201) with a built-in heat source, a coating (202) containing a zeolite molecular sieve or a metal oxide modified zeolite molecular sieve is coated on the outer surface of the exciter channel (201), and the built-in heat source enables the temperature of the outer surface of the exciter channel (201) to be maintained at 200-550 ℃.
6. The process system according to claim 5, wherein an absorption liquid is provided in the absorption device (4), and the absorption liquid is at least one of water, hydrogen peroxide, alkaline solution and ionic liquid.
7. The process system according to claim 5, wherein the primary membrane system (5) is a ceramic membrane, a hollow fiber membrane or a molecular sieve membrane and the secondary membrane system (8) is a pervaporation membrane, an electrodialysis membrane or a forward osmosis membrane.
8. The process system of claim 5, wherein the exciter passage (201) is cordierite, silicon carbide, or mullite.
9. The process system according to claim 5, wherein the built-in heat source of the energizer channel (201) is a heating wire or a hot fluid.
10. The process system of claim 9, wherein the hot fluid is hot flue gas, hot air, hot nitrogen, or heat transfer oil.
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