CN103028313B - Integrated desulfuration and denitration method for wet oxidation of flue gas - Google Patents

Integrated desulfuration and denitration method for wet oxidation of flue gas Download PDF

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CN103028313B
CN103028313B CN201210578308.5A CN201210578308A CN103028313B CN 103028313 B CN103028313 B CN 103028313B CN 201210578308 A CN201210578308 A CN 201210578308A CN 103028313 B CN103028313 B CN 103028313B
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solution
ferrous
iron
flue gas
ferric iron
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CN103028313A (en
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田文学
贾汉东
李慧
陈晨
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HENAN LVDIAN ENVIRONMENTAL PROTECTION ENERGY SAVING TECHNOLOGY Co Ltd
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HENAN LVDIAN ENVIRONMENTAL PROTECTION ENERGY SAVING TECHNOLOGY Co Ltd
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/46—Removing components of defined structure
    • B01D53/60—Simultaneously removing sulfur oxides and nitrogen oxides
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
    • Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
    • Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Biomedical Technology (AREA)
  • Environmental & Geological Engineering (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
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Abstract

The invention discloses an integrated desulfuration and denitration method for wet oxidation of flue gas. The method comprises the steps that the flue gas containing SO2 and NOX are supplied to an acid ferric iron solution or a ferric iron and ferrous iron mixed solution; NOX and sulfur dioxide are absorbed at 0-100 DEG C; a mixed solution consisting of puce nitroso ferrite, sulfate and a little nitric acid and nitrous acid is generated; then desulfuration and denitration treatment on the flue gas is achieved; the mixed solution is supplied to an oxidant for oxidation desorption treatment, so that nitrogen dioxide is released and dissolved in an aqueous solution, an ammonia aqueous solution, a potassium hydroxide solution or a sodium hydroxide solution; nitric acid, ammonium nitrate, potassium nitrate, sodium nitrate, and the like are generated; and then resource utilization is achieved.

Description

A kind of fume wet-type integration desulfurization denitration method
Technical field
The present invention relates to the purification techniques field of flue gas, particularly a kind of fume wet-type integration desulfurization denitration method.
Background technology
Because some propellant compositions are different, not only comprise nitrogen oxide but also have sulfur dioxide in the flue gas produced during burning, normally the content of the latter is greater than the former.Desulphurization denitration technology can be divided into two large classes: the simultaneous SO_2 and NO removal technology of stove combustion process and the desulphurization denitration technology after burning in flue gas, because the simultaneous SO_2 and NO removal technology in combustion process exists the burning degree affecting coal, the problem such as reduce the thermal efficiency of boiler and denitrification efficiency is restricted, thus after burning, flue gas and desulfurizing and denitrifying has become difficult point and the focus of current research, is also the emphasis that may carry out heavy industrialization application from now on.Typical technique has wet method and dry method two kinds.With electron beam irradiation (ER) though the dry process that method, charcoal absorption desulphurization denitration, ammonia process etc. are representative has good desulphurization and denitration efficiency, but plant energy consumption is large and the problem such as later collection accessory substance is key of its development of puzzlement.And with the wet processing that complex complexed absorption of alkali absorption method, oxidative absorption method, iron cobalt etc. is representative, there is the recycling of alkali lye equally, stable and the regeneration reducing of the volatilization of organic solvent and high cost, catalyst, some difficult problems such as effective disposal of accessory substance.Under this background, research and development be applicable to the non-secondary pollution of China's national situation, resource consumption is few, operating cost is low flue gas desulfurization and denitrification especially simultaneous SO_2 and NO removal integrated technique to the SO solving China 2, NOx pollution problem tool is of great significance.
Summary of the invention
The object of the invention is to provide a kind of fume wet-type integration desulfurization denitration method.
The invention provides a kind of fume wet-type integration desulfurization denitration method, comprising:
Will containing SO 2and NO xflue gas passes into acid ferric iron solution or trivalent and ferrous mixed solution, under the temperature conditions of 0-100 DEG C, absorbs NO xand sulfur dioxide, generate the mixed solution of auburn nitroso-ferrous salt, sulfate and a small amount of nitric acid, nitrous acid composition, above-mentioned mixed solution is carried out oxidation processes, and the while that the ferrous ion in solution being oxidized to ferric, nitric oxide is released and is oxidized to nitrogen dioxide and releases.
Further, will containing SO 2and NO xflue gas passes into acid ferric iron solution or trivalent and ferrous mixed solution, and under the temperature conditions of an atmospheric pressure, 0-100 DEG C, reaction 0-3h, absorbs NO xand sulfur dioxide, SO 2first water-soluble generation sulfite ion, then with ferric iron generation redox reaction, inferior sulfate radical becomes sulfate radical, and ferric iron becomes ferrous iron; The ferrous iron nitric oxide adsorbed immediately in flue gas generated finally generates the mixed solution of auburn nitroso-ferrous salt, sulfate and a small amount of nitric acid, nitrous acid composition, above-mentioned mixed solution is carried out oxidation processes, ferrous iron in solution is oxidized to ferric iron and releases nitric oxide, and nitric oxide is oxidized to nitrogen dioxide again immediately simultaneously.
Further, will containing SO 2and NO xflue gas passes into acid ferric iron solution or trivalent and ferrous mixed solution, and under the temperature conditions of 0-100 DEG C, reaction 0-3h, absorbs NO xand sulfur dioxide, SO 2first water-soluble generation sulfite ion, then with ferric iron generation redox reaction, inferior sulfate radical becomes sulfate radical, and ferric iron becomes ferrous iron; The ferrous iron nitric oxide adsorbed immediately in flue gas generated finally generates the mixed solution of auburn nitroso-ferrous salt, sulfate and a small amount of nitric acid, nitrous acid composition, above-mentioned mixed solution is carried out oxidation processes, ferrous iron in solution is oxidized to ferric iron and releases nitric oxide, and nitric oxide is oxidized to nitrogen dioxide again immediately simultaneously.
Further, add oxidant by the mixed solution of above-mentioned nitroso-ferrous salt, nitric acid and nitrous acid, carry out oxidation reaction, in absorbing liquid, ferrous iron is oxidized to ferric iron, and gained ferric iron solution circulation is used for containing SO 2and NO xsmoke absorption process, the NO simultaneously discharged 2gas, through liquid absorption, makes flue gas reach recycling object.
Further, also comprise and being separated by the smoke absorption liquid of recycled for multiple times, purifying, crystallization obtains ferric sulfate or iron chloride, realizes the recycling of flue gas desulfurization and denitrification mixed liquor.
Further, also comprise described nitrogen dioxide collection storage;
Collecting the water-soluble or alkali lye of nitrogen dioxide stored, respectively nitric acid or nitrate products, realize recycling while pending flue gas being reached clean.
Further, the NO that discharges of described oxidation reaction 2gas is absorbed by water, ammoniacal liquor, potassium hydroxide or sodium hydroxide solution; The gas discharged is only absorbed by the water and reclaims nitric acid, the gas that discharges is reclaimed ammonium nitrate, the gas that discharges by ammonia absorption and to be absorbed by potassium hydroxide solution and reclaim potassium nitrate, the gas that discharges and to be absorbed by sodium hydroxide solution and reclaim sodium nitrate.
Further, described acid ferric iron solution is: iron chloride and/or ferric sulfate; Described acid ferrous solution is: frerrous chloride and/or ferrous sulfate.
Further, in described trivalent and ferrous mixed solution, ferric iron solution with the ratio of the molal quantity of ferrous solution is: 10:1-5.
Further, in the ferric iron solution that passes into of described flue gas or ferric iron and ferrous mixed solution, total concentration of iron is 1-3mol/L.
Further, in described acid ferric iron solution or trivalent and ferrous mixed solution, initial hydrogen ion concentration is 0.6-1mol/L.
Further, in described acid ferric iron solution or trivalent and ferrous mixed solution, hydrogen ion concentration is 0.3-2mol/L.
The method of fume wet-type integration desulfurization denitration provided by the invention, can reach the object of gas cleaning, the sulfur dioxide in flue gas, nitrogen oxide finally as Sulphur ressource and nitrogen resource reclaim, really realizes energy-saving and emission-reduction, recycling economy, turn waste into wealth, potential economic benefit is huge.
Accompanying drawing explanation
Fig. 1 is the schematic flow sheet of the fume wet-type integration desulfurization denitration method that the embodiment of the present invention provides.
Detailed description of the invention
Shown in Figure 1, the present invention adopts ferric iron solution or does absorbing liquid containing sulfur dioxide and nitrogen oxide containing gas by the ferric iron of proper proportion mixing and ferrous solution, total concentration of iron controls at 1-3mol/L, be in the acid medium of 0.6-1mol/L in hydrogen ion concentration, under the temperature conditions of 0-100 DEG C, sulfur dioxide absorption and nitrogen oxide, reach the object of gas cleaning through post processing.Wherein ferric iron solution comprises: iron chloride, ferric sulfate etc.; Two valency ferrous solutions comprise: frerrous chloride and/or ferrous sulfate etc.; The ratio of the molal quantity that in mixed solution, ferric iron mixes with ferrous iron is 10:1-5, and concrete selection need be determined by the content ratio of actual sulfureous in flue gas oxide with nitrogen oxide; The kind of the acid in acid medium comprises: hydrochloric acid and/or sulfuric acid.
After passing into absorbing liquid containing the flue gas of sulfur dioxide and nitrogen oxide, sulfur dioxide can generate sulfurous acid and hydration sulfur dioxide and is then oxidized by ferric iron and generate sulphur aqueous acid, and ferric iron becomes ferrous iron simultaneously; Then ferrous iron can absorb the nitric oxide in flue gas, generates nitroso-ferrous salting liquid, thus makes mixed solution show dark brown.Have the of short duration gathering of sulfurous acid and hydration sulfur dioxide in solution, but when ferric iron is excessive, nitroso-ferrously can not to be reduced, comparatively stable existence.
The auburn nitroso-ferrous salt of gained after process, sulfate and a small amount of nitric acid, the mixed liquor of nitrous acid composition, by oxidizing process post processing, makes absorbed flue gas realize innoxious object.Get the absorbing liquid determining volume, pass into or add the one of following oxidant, oxidant comprises: oxygen, ozone etc.In absorbing liquid, ferrous iron is oxidized to trivalent, discharge nitric oxide simultaneously, this nitric oxide is soon oxidized to nitrogen dioxide, enters in suitable absorbing liquid and absorbs, realize the recycling of nitrogen oxide after the excess air blowout that wherein most of nitrogen dioxide is passed into.
Desulphurization denitration black liquor is after oxidation processes, and the suitable absorbing liquid of the nitrogen dioxide blown out by excess air comprises: water, ammoniacal liquor, potassium hydroxide solution, sodium hydroxide solution etc.The recyclable nitric acid of absorbing liquid is done with water; Take ammoniacal liquor as the recyclable ammonium nitrate of absorbing liquid; With potassium hydroxide, the solution such as NaOH do the recyclable potassium nitrate of absorbing liquid, sodium nitrate etc.
Sulfur dioxide is soluble in water, afterwards rapidly be oxidized by ferric iron and generate sulphur aqueous acid.This aqueous solution is when carrying out oxidizing process and removing the nitrogen oxide in solution, and ferrous iron is oxidized to trivalent, so this solution is ferric sulfate, and the acid mixed solution of ferric trichloride and ferric nitrate, this mixed liquor, reusable edible.Repeatedly after circulation, when sulfate radical reaches higher concentration, solution is through concentrated, and be separated, purifying, crystallization obtains ferric sulfate, iron chloride, ferric nitrate etc., realizes the recycling of sulfur dioxide.
embodiment 1
Getting hydrogen ion concentration is 1mol/L, and ferric iron concentration is the liquor ferri trichloridi 1L of 1.66mol/L, in 30 DEG C, pass into sulfur dioxide, nitric oxide gas under an atmospheric pressure, intake is respectively 0.84mol simultaneously, 1.66mol, reaction time is 0-3h, becomes dark brown stop, after leaving standstill 1h to absorbing liquid, this absorbing liquid passes into 0.83mol oxygen, reaction time is 0-5h, and the nitrogen dioxide gas discharged is absorbed by 1L distilled water, without nitrogen dioxide to the residue gas of releasing.Recording contained concentration of nitric acid in absorbing liquid is 0.78mol/L.
In the absorbing liquid after above-mentioned oxidation processes, pass into appropriate oxygen, make ferrous iron in solution all be converted into ferric iron.Gained solution is concentrated, recrystallization, the ferric sulfate product 138g of the crystallization water must be contained, containing iron chloride 114g and a small amount of sodium chloride crystallization of the crystallization water.
embodiment 2
Getting hydrogen ion concentration is 0.6mol/L, ferric iron concentration is 1.66mol/L, ferrous solution concentration is the ferric trichloride of 0.54mol/L and the mixed solution 1L of frerrous chloride, in 30 DEG C, pass into sulfur dioxide under an atmospheric pressure simultaneously, nitric oxide gas, intake is respectively 0.84mol, 2.2mol, and the reaction time is 0-3h, become dark brown to absorbing liquid to stop, after leaving standstill 1h, this absorbing liquid passes into 1.1mol oxygen, and the reaction time is 0-5h, the nitrogen dioxide gas discharged is absorbed by 1L distilled water, without nitrogen dioxide to the residue gas of releasing.Recording contained concentration of nitric acid in absorbing liquid is 0.88mol/L.
In the absorbing liquid after above-mentioned oxidation processes, pass into appropriate oxygen, make ferrous iron in solution all be converted into ferric iron.Gained solution is concentrated, recrystallization, the ferric sulfate product 158g of the crystallization water must be contained, containing iron chloride 122g and a small amount of sodium chloride crystallization of the crystallization water.
The present invention has following beneficial effect:
1, change existing treatment process, remove while realizing sulfur dioxide and nitrogen oxide, decrease cost of investment and unit scale, reduce operating cost, be an important breakthrough to flue gas desulfurization and denitrification technology, really achieve social benefit, the organic unity of economic benefit and environmental benefit.
2, the present invention opens the once technical revolution of desulphurization denitration industry, has good future in engineering applications.Technological precedence, belongs to domestic initiation, and will fill up international blank.Its Transformation Application will have far-reaching social value.
3, this technology is used for the iron system absorbing liquid in fume treatment, can regenerate, can realize recycling, thus reduces the operating cost of system.Sulfur dioxide in flue gas, nitrogen oxide finally as Sulphur ressource and nitrogen resource reclaim, really realizes energy-saving and emission-reduction, recycling economy, turns waste into wealth, and potential economic benefit is huge.
4, in the processing procedure run of this technology and recycling process, non-secondary pollution, realize the innoxious of flue gas and clean discharge, environmental benefit is obvious.
5, realize flue gas and desulfurizing and denitrifying in same system, have equipment and simplify, take up an area few, throw and economize, operating cost is low, and denitrification efficiency is stablized, and operation is simple and reliable, the feature of convenient management.
It should be noted last that, above detailed description of the invention is only in order to illustrate technical scheme of the present invention and unrestricted, although with reference to example to invention has been detailed description, those of ordinary skill in the art is to be understood that, can modify to technical scheme of the present invention or equivalent replacement, and not departing from the spirit and scope of technical solution of the present invention, it all should be encompassed in the middle of right of the present invention.

Claims (7)

1. a fume wet-type integration desulfurization denitration method, is characterized in that:
Will containing SO 2and NO xflue gas passes into acid ferric iron solution or trivalent and ferrous mixed solution, and under the temperature conditions of an atmospheric pressure, 0-100 DEG C, reaction 0-3h, absorbs NO xand sulfur dioxide, SO 2first water-soluble generation sulfite ion, then with ferric iron generation redox reaction, inferior sulfate radical becomes sulfate radical, and ferric iron becomes ferrous iron; The ferrous iron nitric oxide adsorbed immediately in flue gas generated finally generates the mixed solution of auburn nitroso-ferrous salt, sulfate and a small amount of nitric acid, nitrous acid composition, above-mentioned mixed solution is carried out oxidation processes, ferrous iron in solution is oxidized to ferric iron and releases nitric oxide, and nitric oxide is oxidized to nitrogen dioxide again immediately simultaneously;
In described trivalent and ferrous mixed solution, ferric iron solution with the ratio of the molal quantity of ferrous solution is: 10: 1-5; In described acid ferric iron solution or trivalent and ferrous mixed solution, initial hydrogen ion concentration is 0.6-1mol/L; In the ferric iron solution that described flue gas passes into or ferric iron and ferrous mixed solution, total concentration of iron is 1-3mol/L.
2. fume wet-type integration desulfurization denitration method according to claim 1, is characterized in that:
Add oxidant by the mixed solution of above-mentioned nitroso-ferrous salt, nitric acid and nitrous acid, carry out oxidation reaction, in absorbing liquid, ferrous iron is oxidized to ferric iron, and gained ferric iron solution circulation is used for containing SO 2and NO xsmoke absorption process, the NO simultaneously discharged 2gas, through liquid absorption, makes flue gas reach recycling object.
3. fume wet-type integration desulfurization denitration and resource utilization method according to claim 1, is characterized in that, also comprise:
Be separated by the smoke absorption liquid of recycled for multiple times, purifying, crystallization obtains ferric sulfate or iron chloride, realizes the recycling of flue gas desulfurization and denitrification mixed liquor.
4. fume wet-type integration desulfurization denitration method according to claim 1, is characterized in that, also comprise:
Described nitrogen dioxide is collected and stores;
Collecting the water-soluble or alkali lye of nitrogen dioxide stored, respectively nitric acid or nitrate products, realize recycling while pending flue gas being reached clean.
5. fume wet-type integration desulfurization denitration method according to claim 4, is characterized in that:
The NO that described oxidation reaction discharges 2gas is absorbed by water, ammoniacal liquor, potassium hydroxide or sodium hydroxide solution; The gas discharged is only absorbed by the water and reclaims nitric acid, the gas that discharges is reclaimed ammonium nitrate, the gas that discharges by ammonia absorption and to be absorbed by potassium hydroxide solution and reclaim potassium nitrate, the gas that discharges and to be absorbed by sodium hydroxide solution and reclaim sodium nitrate.
6. fume wet-type integration desulfurization denitration method according to claim 1, is characterized in that:
Described flue gas comprises: what all high temp. combustion of fuels produced contains SO 2and NO xgas
7. fume wet-type integration desulfurization denitration method according to claim 1, is characterized in that:
Described acid ferric iron solution is: iron chloride and/or ferric sulfate; Described acid ferrous solution is: frerrous chloride and/or ferrous sulfate.
CN201210578308.5A 2012-09-12 2012-12-27 Integrated desulfuration and denitration method for wet oxidation of flue gas Expired - Fee Related CN103028313B (en)

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CN104353347A (en) * 2014-10-11 2015-02-18 黄立维 Method and device for simultaneous reduction and oxidation of nitrogen oxides from airflow
CN109715269B (en) * 2016-10-14 2022-03-08 黄华丽 Harmful gas purifying agent for adsorbing and removing nitrogen oxides in gas flow within temperature range of 60-500 DEG C
CN111167263B (en) * 2018-11-13 2021-04-13 黄华丽 Nitrogen oxide absorbent slurry and preparation and use methods thereof
CN110075677A (en) * 2019-04-09 2019-08-02 苏州华加星光环保工程技术有限公司 A kind of desulfuring and denitrifying apparatus and method
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