CN105771652A - Flue gas denitration method by taking manganese oxide as cyclic absorption medium - Google Patents
Flue gas denitration method by taking manganese oxide as cyclic absorption medium Download PDFInfo
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- CN105771652A CN105771652A CN201610257217.XA CN201610257217A CN105771652A CN 105771652 A CN105771652 A CN 105771652A CN 201610257217 A CN201610257217 A CN 201610257217A CN 105771652 A CN105771652 A CN 105771652A
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- flue gas
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- 239000003546 flue gas Substances 0.000 title claims abstract description 83
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 70
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 title claims abstract description 52
- 238000010521 absorption reaction Methods 0.000 title claims abstract description 49
- 238000000034 method Methods 0.000 title claims abstract description 44
- 125000004122 cyclic group Chemical group 0.000 title claims abstract description 25
- 239000007789 gas Substances 0.000 claims abstract description 131
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 claims abstract description 107
- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(2+);dinitrate Chemical compound [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 claims abstract description 60
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 claims abstract description 52
- 239000007787 solid Substances 0.000 claims abstract description 46
- MGWGWNFMUOTEHG-UHFFFAOYSA-N 4-(3,5-dimethylphenyl)-1,3-thiazol-2-amine Chemical compound CC1=CC(C)=CC(C=2N=C(N)SC=2)=C1 MGWGWNFMUOTEHG-UHFFFAOYSA-N 0.000 claims abstract description 41
- 229910002089 NOx Inorganic materials 0.000 claims abstract description 24
- 239000002250 absorbent Substances 0.000 claims abstract description 20
- 230000002745 absorbent Effects 0.000 claims abstract description 20
- IOVCWXUNBOPUCH-UHFFFAOYSA-M Nitrite anion Chemical compound [O-]N=O IOVCWXUNBOPUCH-UHFFFAOYSA-M 0.000 claims abstract description 18
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims abstract description 5
- 238000010438 heat treatment Methods 0.000 claims abstract description 5
- -1 calcium nitrite Chemical compound 0.000 claims abstract description 4
- 239000011572 manganese Substances 0.000 claims description 23
- 238000000926 separation method Methods 0.000 claims description 23
- 238000000197 pyrolysis Methods 0.000 claims description 22
- 239000000243 solution Substances 0.000 claims description 22
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 17
- 229910052748 manganese Inorganic materials 0.000 claims description 17
- 238000006477 desulfuration reaction Methods 0.000 claims description 12
- 230000023556 desulfurization Effects 0.000 claims description 12
- 238000002156 mixing Methods 0.000 claims description 12
- 229910017604 nitric acid Inorganic materials 0.000 claims description 12
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 10
- 239000002253 acid Substances 0.000 claims description 10
- 239000003513 alkali Substances 0.000 claims description 10
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 9
- 238000001704 evaporation Methods 0.000 claims description 9
- 230000008020 evaporation Effects 0.000 claims description 9
- 239000007864 aqueous solution Substances 0.000 claims description 5
- FLTRNWIFKITPIO-UHFFFAOYSA-N iron;trihydrate Chemical compound O.O.O.[Fe] FLTRNWIFKITPIO-UHFFFAOYSA-N 0.000 claims description 3
- 239000007791 liquid phase Substances 0.000 claims description 3
- 239000011259 mixed solution Substances 0.000 claims description 3
- 239000007790 solid phase Substances 0.000 claims description 2
- RAFRTSDUWORDLA-UHFFFAOYSA-N phenyl 3-chloropropanoate Chemical compound ClCCC(=O)OC1=CC=CC=C1 RAFRTSDUWORDLA-UHFFFAOYSA-N 0.000 abstract description 16
- 239000006227 byproduct Substances 0.000 abstract description 8
- 230000008901 benefit Effects 0.000 abstract description 4
- 239000002341 toxic gas Substances 0.000 abstract description 3
- 239000002994 raw material Substances 0.000 abstract description 2
- 239000003929 acidic solution Substances 0.000 abstract 1
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 27
- 239000011575 calcium Substances 0.000 description 21
- 239000000047 product Substances 0.000 description 21
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 description 20
- OSGAYBCDTDRGGQ-UHFFFAOYSA-L calcium sulfate Chemical compound [Ca+2].[O-]S([O-])(=O)=O OSGAYBCDTDRGGQ-UHFFFAOYSA-L 0.000 description 16
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 12
- 229910052791 calcium Inorganic materials 0.000 description 12
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 11
- 239000007788 liquid Substances 0.000 description 11
- 230000008569 process Effects 0.000 description 11
- 229910002651 NO3 Inorganic materials 0.000 description 10
- 239000000292 calcium oxide Substances 0.000 description 10
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 10
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 9
- AXCZMVOFGPJBDE-UHFFFAOYSA-L calcium dihydroxide Chemical compound [OH-].[OH-].[Ca+2] AXCZMVOFGPJBDE-UHFFFAOYSA-L 0.000 description 9
- 239000000920 calcium hydroxide Substances 0.000 description 9
- 229910001861 calcium hydroxide Inorganic materials 0.000 description 9
- 239000006200 vaporizer Substances 0.000 description 9
- 238000005728 strengthening Methods 0.000 description 7
- 229910021529 ammonia Inorganic materials 0.000 description 6
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 description 6
- 238000005979 thermal decomposition reaction Methods 0.000 description 6
- 230000007797 corrosion Effects 0.000 description 5
- 238000005260 corrosion Methods 0.000 description 5
- 239000011150 reinforced concrete Substances 0.000 description 5
- 239000000725 suspension Substances 0.000 description 5
- 239000003054 catalyst Substances 0.000 description 4
- 239000003638 chemical reducing agent Substances 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 229910052757 nitrogen Inorganic materials 0.000 description 4
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 3
- ZXTSZWBPUXLRFJ-UHFFFAOYSA-N [Ca].N(=O)O Chemical compound [Ca].N(=O)O ZXTSZWBPUXLRFJ-UHFFFAOYSA-N 0.000 description 3
- 230000002378 acidificating effect Effects 0.000 description 3
- GBAOBIBJACZTNA-UHFFFAOYSA-L calcium sulfite Chemical compound [Ca+2].[O-]S([O-])=O GBAOBIBJACZTNA-UHFFFAOYSA-L 0.000 description 3
- 235000010261 calcium sulphite Nutrition 0.000 description 3
- 239000002803 fossil fuel Substances 0.000 description 3
- 230000008929 regeneration Effects 0.000 description 3
- 238000011069 regeneration method Methods 0.000 description 3
- XTEGARKTQYYJKE-UHFFFAOYSA-M Chlorate Chemical compound [O-]Cl(=O)=O XTEGARKTQYYJKE-UHFFFAOYSA-M 0.000 description 2
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 2
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 2
- IOVCWXUNBOPUCH-UHFFFAOYSA-N Nitrous acid Chemical compound ON=O IOVCWXUNBOPUCH-UHFFFAOYSA-N 0.000 description 2
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 2
- GOPYZMJAIPBUGX-UHFFFAOYSA-N [O-2].[O-2].[Mn+4] Chemical compound [O-2].[O-2].[Mn+4] GOPYZMJAIPBUGX-UHFFFAOYSA-N 0.000 description 2
- 229910052925 anhydrite Inorganic materials 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 239000003245 coal Substances 0.000 description 2
- 238000002485 combustion reaction Methods 0.000 description 2
- 239000012141 concentrate Substances 0.000 description 2
- 229910001882 dioxygen Inorganic materials 0.000 description 2
- 239000011777 magnesium Substances 0.000 description 2
- 150000002697 manganese compounds Chemical class 0.000 description 2
- BYOBIQOEWYNTMM-UHFFFAOYSA-N manganese;nitric acid Chemical compound [Mn].O[N+]([O-])=O BYOBIQOEWYNTMM-UHFFFAOYSA-N 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000003345 natural gas Substances 0.000 description 2
- 239000003921 oil Substances 0.000 description 2
- 239000007800 oxidant agent Substances 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 238000004064 recycling Methods 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 238000003860 storage Methods 0.000 description 2
- 239000013589 supplement Substances 0.000 description 2
- 239000002351 wastewater Substances 0.000 description 2
- 230000036642 wellbeing Effects 0.000 description 2
- 235000019738 Limestone Nutrition 0.000 description 1
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000004202 carbamide Substances 0.000 description 1
- 235000013877 carbamide Nutrition 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 150000004696 coordination complex Chemical class 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 230000003009 desulfurizing effect Effects 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- 230000008676 import Effects 0.000 description 1
- 239000006028 limestone Substances 0.000 description 1
- 239000000395 magnesium oxide Substances 0.000 description 1
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 1
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 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
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 238000010926 purge Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000007634 remodeling Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000004088 simulation Methods 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000004083 survival effect Effects 0.000 description 1
- 239000002912 waste gas Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- 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
- B01D53/96—Regeneration, reactivation or recycling of reactants
-
- 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
- B01D53/48—Sulfur compounds
- B01D53/50—Sulfur oxides
- B01D53/501—Sulfur oxides by treating the gases with a solution or a suspension of an alkali or earth-alkali or ammonium compound
- B01D53/504—Sulfur oxides by treating the gases with a solution or a suspension of an alkali or earth-alkali or ammonium compound characterised by a specific device
-
- 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
- B01D53/54—Nitrogen compounds
- B01D53/56—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
- B01D53/77—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
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/80—Semi-solid phase processes, i.e. by using slurries
-
- 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 flue gas denitration method by taking manganese oxide as a cyclic absorption medium. The flue gas denitration method comprises the following steps: heating manganese nitrate to generate nitrogen dioxide gas and a manganese dioxide solid; feeding the nitrogen dioxide gas into desulfurized flue gas, and absorbing SO2 and NOx in the desulfurized flue gas with an alkaline absorbent to generate sulfate and nitrite; absorbing NOx, which is artificially added together with the manganese dioxide solid, in the flue gas subjected to primary denitration with a manganese dioxide-containing acidic solution serving as an absorbent, so as to generate manganese nitrate. According to the flue gas denitration method, the alkaline absorbent which is readily available and cheap is used as a raw material, and a working medium (manganese oxide) is cyclically used, so that toxic gas such as NOx in the flue gas can be effectively removed; by absorption treatment, the content of SO2 in the flue gas is less than or equal to 1 PPM, the content of NOx is less than or equal to 50PPM, and nitrite, particularly calcium nitrite, which is a byproduct with low cost and high additional value can be obtained; an enterprise can protect the environment and earn economic benefits, and the heavy economic burden on relevant enterprises at the present is changed thoroughly.
Description
Technical field
The invention belongs to denitration technology field, all industries and the field of wherein nitrogen oxide NOx removed by the flue gas needs relating to producing after the Fossil fuels such as coal, oil, natural gas burn in fixed burner, is specifically related to a kind of flue gas method of denitration being cyclic absorption medium with manganese oxide.
Background technology
The Fossil fuels such as coal, oil, natural gas are after high-temp combustion, containing sulfur dioxide SO in flue gas2With the acidic materials such as nitrogen oxide NOx, air and environment for human survival are caused considerable damage for many years.Domestic and international prior art uses limestone, magnesium oxide as desulfurizing agent, can by the sulfur dioxide SO in flue gas2Take off to 100-200PPM；High-temperature flue gas adds the reducing agent such as ammonia, carbamide, when catalyst-free (being called for short SNCR) and strict control add quantity, can by the NOx removal 50-60% in flue gas.Though SNCR method small investment, operation temperature high (900-1200 DEG C), elasticity are little, and the escaping of ammonia rate height easily causes secondary pollution, and the management of storage liquefied ammonia or ammonia also has more trouble.The SCR method that large-scale power station is commonly used both at home and abroad at present, adopts the reducing agents such as ammonia equally, in 250-400 DEG C of temperature range, uses catalyst and have under oxygen existent condition, can be harmless nitrogen and water by NOx selective reduction.SCR method denitration rate is up to more than 90%, and shortcoming is to need the fluid velocity in catalytic bed, temperature and concentration are strictly controlled.Catalytic bed Structural Design Requirement is high, it is necessary to ammonia storage system, purging system and catalyst need from external import, expensive, easily aging, regeneration time easily cause secondary pollution, denitrification process product-free, without direct yield.Therefore, SCR method causes heavy financial burden to numerous domestic enterprise.There is achievement in research to add ozone in the gas phase, add hydrogen peroxide, chlorate, high-valency metal salt and metal complex in the liquid phase, it is possible to reach higher denitration effect, technically mostly not mature enough while increasing considerably operating cost.
In prior art, Chinese patent CN101982419 discloses and leaches, with oxides of nitrogen gas, the method that manganese nitrate solution produced by pyrolusite under condition under elevated pressure.Due to pyrolusite resource-constrained, the method can be not applied directly to wider denitrating flue gas field.
Therefore, a kind of small investment of market in urgent need, operating cost are low, stable, can effectively remove the toxic gas such as nitrogen oxide NOx in flue gas and by-product has the new method of value-added product, help enterprise to have economic well-being of workers and staff while protection environment.
Summary of the invention
For the pyrolusite resource-constrained existed in prior art, the technical problem that denitration cost is high, it is an object of the invention to provide a kind of flue gas method of denitration being cyclic absorption medium with manganese oxide.
The technical scheme that the present invention takes is:
A kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, comprise the steps:
Pyrolysis manganese nitrate；Heating manganese nitrate generates nitrogen dioxide gas and manganese dioxide solid；
Denitration: pass into nitrogen dioxide gas in the flue gas after desulfurization, uses the SO in alkaline absorbent Absorption Desulfurization flue gas2And NOxGas, generates sulfate and nitrite；
Secondary denitration: use the acid solution containing manganese dioxide as absorbent, absorb NO that is in a denitration rear pass gas and that artificially add together with manganese dioxide solidxGas, generates manganese nitrate.
Further, the manganese nitrate in described pyrolysis manganese nitrate step adopts the manganese nitrate generated in secondary denitration.
Further, the nitrogen dioxide gas in a described denitrification step adopts the nitrogen dioxide gas that pyrolysis manganese nitrate obtains.
Further, the nitrogen dioxide gas passed in a described denitrification step is to make it mix the NO in gas before carrying out a denitration2/ NO mol ratio≤1.
Further, the sulfate generated in a described denitrification step and nitrite, filter out solid phase, evaporation liquid phase makes nitrite product.
Further, with the SO in calcium oxide or calcium hydroxide slurry Absorption Desulfurization flue in a described denitrification step2And NOxGas, generates calcium sulfate and calcium nitrite, filters out calcium sulfate, evaporation and concentration nitrous acid calcium solution, make calcium nitrite product, as reinforced concrete corrosion inhibiter；
Further, in described pyrolysis manganese nitrate step, manganese nitrate aqueous solution it is injected directly in side line temperature flue gas or adds in hot-air so that it is decomposing between 200-350 DEG C and produce nitrogen dioxide and manganese dioxide.
Further, the alkaline absorbent in a described denitrification step is set to NaOH, Mg (OH)2、Fe(OH)3, CaO or Ca (OH)2In any one.
Further, in described secondary denitrification step, the acid solution of manganese dioxide adopts the mixed solution containing manganese dioxide and nitric acid, and wherein, manganese dioxide concentration is 0.1%-5%, and concentration of nitric acid is 0-10%, and operation temperature is set to 15-60 DEG C.
Further, described operation temperature is set to 30-55 DEG C.
A kind of be cyclic absorption medium with manganese oxide the denitrification apparatus that adopts of flue gas method of denitration, including manganese nitrate pyrolysis apparatus, denitration one tower and denitration two tower:
Manganese nitrate pyrolysis apparatus: top passes into temperature flue gas in side line, and bottom connects gas solid separation assembly, and the portion gas of this gas solid separation assembly passes in denitration one tower by gas mixer, remaining gas and solid are entered in denitration two tower by gas solid separation module outlet；
Denitration one tower: top passes into the alkaline absorbent in alkali circulating slot, the SO in Absorption Desulfurization flue gas2With NOx gas, bottom passes into the mixing gas come in gas mixer, passes into the part nitrogen dioxide gas that gas solid separation components apart goes out in gas mixer, and the exit gas of denitration one tower is passed directly into denitration two tower bottom；
Denitration two tower: top passes into the acid solution in manganese circulating slot containing manganese dioxide, bottom passes into out remaining another part nitrogen dioxide gas and manganese dioxide solid in the flue gas of denitration one tower and gas-solid separation assembly, described manganese circulating slot and manganese nitrate pyrolysis apparatus and connects.
Further, described alkali circulating slot and sub-calcium vaporizer connect, and calcium sulfite is calcium sulfate by the dioxygen oxidation in flue gas and is filtered, and sub-calcium evaporator evaporation calcium nitrite becomes concentrated solution, makes calcium nitrite product further.
The invention have the benefit that
1, the present invention uses manganese oxide to be working media, and denitration product manganese nitrate produces nitrogen dioxide gas and manganese dioxide solid, self-produced nitrogen dioxide NO after thermal decomposition2Can strengthening the absorption of indissoluble gases NO, denitration product nitrite-oxidizing can be nitrate by manganese dioxide solid, it is ensured that nitrogen oxide gas NOXWhile constant absorption, generate reusable manganese nitrate.The present invention makes full use of nitrogen, the heat of manganese compound appraises at the current rate technology, only consumes the heat of manganese nitrate thermal decomposition, can be achieved with the high efficiente callback of nitrogen oxides and utilizes.
2, the present invention uses wide material sources and low-cost alkaline absorbent is raw material, recycles manganese oxide working media, can effectively remove nitrogen oxide NO in flue gasXToxic gas, obtains low cost by-product high value added product nitrite, it is not necessary to adding other reducing agent, catalyst or oxidant can SO in efficient removal flue gas2、NOxHarmful components, denitration liquid can concentrate and be processed into nitrite product.
3, artificial nitrogen dioxide gas being passed into denitration one tower and makes the NO in mixing gas in the present invention2/ NO (mol ratio)≤1, absorbent is preferably calcium oxide CaO or calcium hydroxide Ca (OH)2, calcium nitrite product is processed in the liquid that is absorbed after can making recycling concentration, and as reinforced concrete corrosion inhibiter, the market sales volume of side-product has a extensive future, and brings huge economic benefit.
4, the present invention supplements NO in processed gas2Gas, is conducive to the absorption of NO in flue gas；Denitration absorbing liquor introduces MnO2, the nitrite absorbed in liquid can be converted into the nitrate of correspondence in time, strengthening absorption process carries out.The NO of strengthening NO GAS ABSORPTION and Nitrite transformation2、MnO2, for side-product Mn (NO3)2Thermal decomposition product.Process through double absorption, sulfur dioxide in flue gas SO2≤ 1PPM, NOx≤50PPM, cyclic absorption process non-wastewater discharge, small investment, operating cost are low, stable.
5, the present invention produces nitrogen dioxide gas and the method for manganese dioxide solid, is by nitric acid Mn (NO3)2Concentrated solution is injected directly in the mixing gas of high-temperature flue gas and air, it is made to heat between 200-350 DEG C, decompose generation nitrogen dioxide gas and manganese dioxide solid circulation is used for strengthening flue gas denitrification process, make full use of the heat of high-temperature flue gas, only consume partial heat, denitrating flue gas cost can be greatly lowered.
6, this method is applicable to desulphurization denitration and the Treatment of Tail Gas from Nitric field of various fossil fuel combustion waste gas, enterprise can be helped to have economic well-being of workers and staff while protection environment, thoroughly change the financial burden that current each relevant enterprise is heavy.
Accompanying drawing explanation
Fig. 1 is the integrated artistic schematic flow sheet of denitrification apparatus in the present invention.
Wherein, 1, denitration one tower；2, alkali circulating slot；3, calcium circulating pump；4, sub-calcium vaporizer；5, gas mixer；6, manganese nitrate decomposer；7, gas solid separation assembly；8, denitration two tower；9, manganese circulating slot；10, manganese circulating pump；11, manganese nitrate vaporizer；12, dense manganese pump.
Detailed description of the invention
For making the denitration to the present invention, calcium nitrite manufacture and manganese oxide regeneration and producing nitrogen dioxide NO2The principles of chemistry of gas and implementation have further understanding, and special explanation is as follows:
Embodiment 1
A kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, comprise the steps:
Pyrolysis manganese nitrate；Heating manganese nitrate generates nitrogen dioxide gas and manganese dioxide solid；
Denitration: pass into nitrogen dioxide gas in the flue gas after desulfurization, using calcium oxide or calcium hydroxide is the SO in absorbent Absorption Desulfurization flue gas2And NOxGas, generates calcium sulfate and calcium nitrite；
Secondary denitration: use the acid solution containing manganese dioxide as absorbent, absorb NO that is in a denitration rear pass gas and that artificially add together with manganese dioxide solidxGas, generates manganese nitrate.
Further, the manganese nitrate in described pyrolysis manganese nitrate step adopts the manganese nitrate generated in secondary denitration.
Further, the nitrogen dioxide gas in a described denitrification step adopts the nitrogen dioxide gas that pyrolysis manganese nitrate obtains.
Further, the nitrogen dioxide gas passed in a described denitrification step is to make it mix the mol ratio NO in gas before carrying out a denitration2/NO≤1。
Use manganese oxide is working media, and denitration product manganese nitrate produces nitrogen dioxide gas and manganese dioxide solid, self-produced nitrogen dioxide NO after thermal decomposition2The absorption of indissoluble gases NO can be strengthened, denitration product nitrite-oxidizing can be nitrate by manganese dioxide solid, while ensureing nitrogen oxide gas constant absorption, generate reusable manganese nitrate, make full use of nitrogen, the heat of manganese compound appraises at the current rate technology, only consume the heat of manganese nitrate thermal decomposition, can be achieved with the high efficiente callback of nitrogen oxides and utilize.
Further, filtering out calcium sulfate in a described denitrification step, evaporation calcium nitrite makes calcium nitrite product, as reinforced concrete corrosion inhibiter.
Further, in described pyrolysis manganese nitrate step, manganese nitrate aqueous solution is injected directly in side line temperature flue gas or adds in hot-air, it is made to decompose generation nitrogen dioxide and manganese dioxide between 200-350 DEG C, decompose generation nitrogen dioxide gas and manganese dioxide solid circulation is used for strengthening flue gas denitrification process, make full use of the heat of high-temperature flue gas, only consume partial heat, denitrating flue gas cost can be greatly lowered.
Further, the alkaline absorbent in a described denitrification step is set to NaOH, Mg (OH)2、Fe(OH)3, CaO or Ca (OH)2In any one, obtain low cost by-product high value added product nitrite, it is not necessary to adding other reducing agent, catalyst or oxidant can SO in efficient removal flue gas2、NOxHarmful components, denitration liquid can concentrate and be processed into nitrite product.
Further, described alkaline absorbent is preferably calcium oxide CaO or calcium hydroxide Ca (OH)2, calcium nitrite product is processed in the liquid that is absorbed after can making recycling concentration, and as reinforced concrete corrosion inhibiter, the market sales volume of side-product has a extensive future, and brings huge economic benefit.
Further, in described secondary denitrification step, the acid solution of manganese dioxide adopts the mixed solution containing manganese dioxide and nitric acid, wherein, manganese dioxide concentration is 0.1%-5%, concentration of nitric acid is 0-10%, and operation temperature is set to 15-60 DEG C, introduces MnO in denitration absorbing liquor2, the nitrite absorbed in liquid can be converted into the nitrate of correspondence in time, strengthening absorption process carries out.The NO of strengthening NO GAS ABSORPTION and Nitrite transformation2、MnO2, for side-product Mn (NO3)2Thermal decomposition product.Process through double absorption, sulfur dioxide in flue gas SO2≤ 1PPM, NOx≤50PPM, cyclic absorption process non-wastewater discharge, small investment, operating cost are low, stable.
Further, described operation temperature is set to 30-55 DEG C.
The technical scheme in the present invention is further illustrated below in conjunction with chemical equation:
A kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, specifically include following steps:
(1) supplement in the flue gas after desulfurization after part nitrogen dioxide gas, enter denitration one tower, with the SO in calcium oxide or calcium hydroxide slip Absorption Desulfurization flue gas2With NOx gas, generation calcium sulfite Ca (SO3)2With calcium nitrite Ca (NO2)2Aqueous solution:
Ca(OH)2+SO2→CaSO3+H2O
CaSO3+1/2O2→CaSO4↓
Ca(OH)2+NO+NO2→Ca(NO2)2+H2O
Filter out calcium sulfate CaSO4, evaporation and concentration nitrous acid calcium solution, make calcium nitrite product, as reinforced concrete corrosion inhibiter；
(2) enter denitration two tower together with going out part nitrogen dioxide gas that the flue gas of denitration one tower produces with pyrolysis manganese nitrate, manganese dioxide solid, absorbed by the acidic suspension containing manganese dioxide:
NO+NO2+H2O→2HNO2
HNO2+HNO3+MnO2→Mn(NO3)2+H2O
2NO2+H2O→HNO2+HNO3
(3) go out the flue gas after denitration two tower directly or to discharge after heating, Mn (NO in circulating absorption solution3)2After 10%, take out the concentrated solution being condensed into 30-55%；Manganese nitrate concentrated solution is introduced heat resolve in 200-350 DEG C of high temperature gas flow, and the chemical reaction of described cyclic absorption medium circulation regeneration is as follows:
Mn(NO3)2=MnO2+2NO2↑
By gas solid separation unit equipment, the part NO without manganese dioxide2Mixing gas enters denitration one tower, the NO containing manganese dioxide together with processed gas2Part mixing gas enters denitration two tower.
Embodiment 2
A kind of be cyclic absorption medium with manganese oxide the denitrification apparatus that adopts of flue gas method of denitration, including manganese nitrate pyrolysis apparatus, denitration one tower and denitration two tower:
Manganese nitrate pyrolysis apparatus: top passes into temperature flue gas in side line, bottom connects gas solid separation assembly, a part of gas outlet of this gas solid separation assembly passes in denitration one tower by gas mixer, and another part gas of gas solid separation assembly and solid outlet pass in denitration two tower；
Denitration one tower: top passes into the alkaline absorbent in alkali circulating slot, the SO in Absorption Desulfurization flue gas2With NOx gas, bottom passes into the mixing gas come in gas mixer, passes into the part nitrogen dioxide gas that gas solid separation components apart goes out in gas mixer, and the exit gas of denitration one tower is passed directly into denitration two tower bottom；
Denitration two tower: top passes into the acid solution in manganese circulating slot containing manganese dioxide, bottom passes into out remaining another part nitrogen dioxide gas and manganese dioxide solid in the flue gas of denitration one tower and gas-solid separation assembly, described manganese circulating slot and manganese nitrate pyrolysis apparatus and connects.
Further, described alkali circulating slot and sub-calcium vaporizer connect, and calcium sulfite is calcium sulfate by the dioxygen oxidation in flue gas and is filtered, sub-calcium evaporator evaporation concentration nitrous acid calcium solution, make calcium nitrite product further.
The denitrating system that in the present invention, denitrification apparatus is formed is further illustrated below by the annexation between all parts.
A kind of be cyclic absorption medium with manganese oxide flue gas denitrification apparatus, including denitration one tower, alkali circulating slot, calcium circulating pump, sub-calcium vaporizer, gas mixer, manganese nitrate decomposer, gas solid separation assembly, denitration two tower, manganese circulating slot, manganese circulating pump, manganese nitrate vaporizer and dense manganese pump, described denitration one tower top end is connected by flue and denitration two tower, the bottom of denitration one tower and denitration two tower is respectively arranged with alkali circulating slot and manganese circulating slot, alkali circulating slot one end is connected by calcium circulating pump and denitration one tower upper end, the alkali circulating slot other end connects sub-calcium vaporizer by pipeline；Manganese circulating slot one end is connected by manganese circulating pump and denitration two tower upper end, the manganese circulating slot other end connects manganese nitrate vaporizer, manganese nitrate vaporizer is connected by dense manganese pump and manganese nitrate decomposer, the top of manganese nitrate decomposer passes into temperature flue gas in side line, the bottom of manganese nitrate decomposer connects gas solid separation assembly, gas solid separation assembly one end and denitration two tower lower end connect, the gas solid separation assembly other end connects gas mixer, gas mixer one end passes into flue gas, the gas mixer other end and denitration one tower lower end and connects.
The present invention passes through gas solid separation unit equipment, the part NO without manganese dioxide2Mixing gas enters denitration one tower, the NO containing manganese dioxide together with processed gas2Part mixing gas enters denitration two tower, the flue gas containing nitrogen oxide NOx and self-produced part nitrogen dioxide NO2Pass into denitration one tower together, react generation nitrite (when being chosen as calcium oxide or calcium hydroxide slurry when alkaline absorbent, generating calcium nitrite with the calcium hydroxide reaction absorbed in liquid) with the alkaline absorbent absorbed in liquid；The flue gas going out denitration one tower still contains small amounts nitrogen NOx, again it is mixed into self-produced nitrogen dioxide and enters denitration two tower together with manganese dioxide, circulating absorption solution in denitration two tower is the acidic aqueous solution being mixed with manganese dioxide, in acid condition, nitrite-oxidizing for denitration product one-tenth nitric acid is simultaneously generated manganese nitrate by manganese dioxide.Evaporation and concentration obtains concentrated nitric acid manganese solution；Being sprayed into by concentrated nitric acid manganese solution in 200-350 DEG C of side line flue gas, generate self-produced nitrogen dioxide gas and manganese dioxide solid, circulation passes into denitration one, two tower.Process through double absorption, sulfur dioxide in flue gas SO2≤ 1PPM, NOx≤50PPM.
Embodiment 3
The denitrating system adopting upper and lower laid out in parallel mode to form for denitration one tower (lower tower) and denitration two tower (upper tower) below, further illustrates the flue gas method of denitration in the present invention.
Denitration packed tower height overall 2000mm, upper and lower each 1000mm, diameter 50mm；Operation temperature 35 DEG C, under denitration, tower bottom passes into containing NO350ppm, NO2450ppm、O2The simulation mixing gas 5L/min of 6.2%, is spilled into 2%Ca (OH) in the middle part of tower2Suspension, liquid-gas ratio (L/G)=6.5.Measure NO87ppm, NO in lower tower exit gas262ppm.Lower tower exit gas is passed directly into upper tower bottom, and tower top is spilled into 1 ‰ MnO2, 3%HNO3Suspension, liquid-gas ratio (L/G)=10, NO28ppm, NO in tower exit gas in measurement221ppm。
Embodiment 4
The denitrating system formed for denitration one tower and denitration two tower employing left and right parallel arrangement mode below, further illustrates the flue gas method of denitration in the present invention.
As it is shown in figure 1, denitration one tower, each height of denitration two tower are the packed tower of 5000mm, diameter 1000mm, enters denitrating tower flue gas flow 12000NM3/ h, temperature 55 DEG C, the nitrogen dioxide gas come with manganese nitrate decomposition process mixes, and passes into denitration one tower bottom together, and recording gas group becomes SO272ppm、NO378ppm、NO2502ppm, a top of tower is spilled into 2%Ca (OH)2Suspension, liquid-gas ratio (L/G)=3.5.Measure NO71ppm, NO in a tower exit gas242ppm.Denitration one tower exit gas is passed directly into denitration two tower bottom, and tower top is spilled into 1 ‰ MnO2, 2%HNO3Suspension, liquid-gas ratio (L/G)=6, NO21ppm, NO in tower exit gas in measurement216ppm, SO22ppm。
It is continuously replenished Ca (OH)2After running 48 hours continuously, the denitration liquid of denitration one tower is containing Ca (NO3)26.8%, evaporation and concentration is the calcium nitrite product of content 95%.
Take after running 96 hours continuously the denitration liquid of denitration two tower containing Mn (NO3)25.3%, flash to 50% concentrated solution, spray in 320 DEG C of side line flue gases, record Mn (NO3)2Resolution ratio 89%, newly-generated NO2Gas introduces denitration one tower, denitration two tower, NO in cyclic hardening flue gas respectively with side line mixing gas after gas solid separationXGAS ABSORPTION and absorption liquid Nitrite are converted into nitrate anion.
The above is not limitation of the present invention; it is noted that, for those skilled in the art; under the premise without departing from essential scope of the present invention, it is also possible to make some changes, remodeling, interpolation or replacement, these improve and change also should be regarded as protection scope of the present invention.
Claims (10)
1. the flue gas method of denitration that a kind is cyclic absorption medium with manganese oxide, it is characterised in that comprise the steps:
Pyrolysis manganese nitrate；Heating manganese nitrate generates nitrogen dioxide gas and manganese dioxide solid；
Denitration: pass into nitrogen dioxide gas in the flue gas after desulfurization, uses the SO in alkaline absorbent Absorption Desulfurization flue gas2And NOxGas, generates sulfate and nitrite；
Secondary denitration: use the acid solution containing manganese dioxide as absorbent, absorb NO that is in a denitration rear pass gas and that artificially add together with manganese dioxide solidxGas, generates manganese nitrate.
2. according to claim 1 a kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, it is characterised in that manganese nitrate in described pyrolysis manganese nitrate step adopts the manganese nitrate generated in secondary denitration.
3. according to claim 1 a kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, it is characterised in that nitrogen dioxide gas in a described denitrification step adopts the nitrogen dioxide gas that pyrolysis manganese nitrate obtains.
4. according to claim 1 or 3 a kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, it is characterised in that the nitrogen dioxide gas passed in a described denitrification step is to make its NO carried out before a denitration in mixing gas2/ NO mol ratio≤1.
5. according to claim 1 a kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, it is characterised in that the sulfate generated in a described denitrification step and nitrite, filter out solid phase, evaporation liquid phase makes nitrite product.
6. according to claim 1 a kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, it is characterized in that, in described pyrolysis manganese nitrate step, manganese nitrate aqueous solution it is injected directly in side line temperature flue gas or adds in hot-air so that it is decomposing between 200-350 DEG C and produce nitrogen dioxide and manganese dioxide.
7. according to claim 1 a kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, it is characterised in that the alkaline absorbent in a described denitrification step is set to NaOH, Mg (OH)2、Fe(OH)3, CaO or Ca (OH)2In any one.
8. according to claim 1 a kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, it is characterized in that, in described secondary denitrification step, the acid solution of manganese dioxide adopts the mixed solution containing manganese dioxide and nitric acid, wherein, manganese dioxide concentration is 0.1%-5%, concentration of nitric acid is 0-10%, and operation temperature is set to 15-60 DEG C.
9. according to claim 8 a kind of be cyclic absorption medium with manganese oxide flue gas method of denitration, it is characterised in that described operation temperature is set to 30-55 DEG C.
10. according to claim 1 a kind of be cyclic absorption medium with manganese oxide the denitrification apparatus that adopts of flue gas method of denitration, it is characterised in that include manganese nitrate pyrolysis apparatus, denitration one tower and denitration two tower:
Manganese nitrate pyrolysis apparatus: top passes into temperature flue gas in side line, and bottom connects gas solid separation assembly, and the portion gas of this gas solid separation assembly passes in denitration one tower by gas mixer, remaining gas and solid are entered in denitration two tower by gas solid separation module outlet；
Denitration one tower: top passes into the alkaline absorbent in alkali circulating slot, the SO in Absorption Desulfurization flue gas2With NOx gas, bottom passes into the mixing gas come in gas mixer, passes into the part nitrogen dioxide gas that gas solid separation components apart goes out in gas mixer, and the exit gas of denitration one tower is passed directly into denitration two tower bottom；
Denitration two tower: top passes into the acid solution in manganese circulating slot containing manganese dioxide, bottom passes into out remaining another part nitrogen dioxide gas and manganese dioxide solid in the flue gas of denitration one tower and gas-solid separation assembly, described manganese circulating slot and manganese nitrate pyrolysis apparatus and connects.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN106861410A (en) * | 2017-01-13 | 2017-06-20 | 青岛科技大学 | A kind of take manganous hydroxide as the flue gas deep desulfuration denitration dry type integral method for circulating working media |
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| CN115253671A (en) * | 2022-08-13 | 2022-11-01 | 嘉兴复翼环保科技有限公司 | NO capable of assisting power by utilizing 2 Method for realizing SCR (selective catalytic reduction) efficient denitration by using generated additive |
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