CN103028313A - 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 PDFInfo
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- CN103028313A CN103028313A CN2012105783085A CN201210578308A CN103028313A CN 103028313 A CN103028313 A CN 103028313A CN 2012105783085 A CN2012105783085 A CN 2012105783085A CN 201210578308 A CN201210578308 A CN 201210578308A CN 103028313 A CN103028313 A CN 103028313A
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
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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
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 sulfur dioxide is arranged in the flue gas that produces during burning, normally the latter's content is greater than the former.The desulphurization denitration technology can be divided into two large classes: the desulphurization denitration technology in the flue gas after desulphurization denitration technology and the burning in the time of the stove combustion process, because there is the burning degree that affects coal in the desulphurization denitration technology in the time of in the combustion process, the problems such as the thermal efficiency of reduction boiler and denitrification efficiency are restricted, thereby flue gas and desulfurizing and denitrifying has become difficult point and the focus of present research after the burning, also is to carry out from now on the emphasis that heavy industrialization is used.Typical technique has two kinds of wet method and dry method.Take electron beam irradiation (ER) though method, charcoal absorption desulphurization denitration, ammonia process etc. have preferably desulphurization and denitration efficient as the dry process of representative, but plant energy consumption greatly and the problem such as follow-up collection accessory substance be the key of its development of puzzlement.And the wet processing take alkali absorption method, oxidation absorption process, iron Cobalt complex complexed absorption etc. as representative, exist equally the recycling of alkali lye, the volatilization of organic solvent and stable and regeneration reducing expensive, catalyst, some difficult problems such as effective disposal of accessory substance.Under this background, the flue gas desulfurization and denitrification that non-secondary pollution, resource consumption are few, operating cost is low that research and development are fit to China's national situation especially simultaneously the desulfurization and denitrification integral technology to solving the SO of 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:
To contain SO
2And NO
XFlue gas passes into acid ferric iron solution or trivalent and ferrous mixed solution, under 0-100 ℃ temperature conditions, absorbs NO
XAnd sulfur dioxide, generate the mixed solution that auburn nitroso-ferrous salt, sulfate and a small amount of nitric acid, nitrous acid form, above-mentioned mixed solution is carried out oxidation processes, and the ferrous ion in the solution is oxidized to ferric while nitric oxide and is released and is oxidized to nitrogen dioxide and emit.
Further, will contain 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 ℃, reaction 0-3h absorbs NO
XAnd sulfur dioxide, SO
2Water-soluble generation sulfite ion is followed and ferric iron generation redox reaction first, and inferior sulfate radical becomes sulfate radical, and ferric iron becomes ferrous iron; The ferrous iron that generates adsorbs the last mixed solution that generates auburn nitroso-ferrous salt, sulfate and a small amount of nitric acid, nitrous acid composition of nitric oxide in the flue gas immediately, above-mentioned mixed solution is carried out oxidation processes, ferrous iron in the solution is oxidized to ferric iron and emits nitric oxide, and nitric oxide is oxidized to again nitrogen dioxide immediately simultaneously.
Further, will contain SO
2And NO
XFlue gas passes into acid ferric iron solution or trivalent and ferrous mixed solution, and under 0-100 ℃ temperature conditions, reaction 0-3h absorbs NO
XAnd sulfur dioxide, SO
2Water-soluble generation sulfite ion is followed and ferric iron generation redox reaction first, and inferior sulfate radical becomes sulfate radical, and ferric iron becomes ferrous iron; The ferrous iron that generates adsorbs the last mixed solution that generates auburn nitroso-ferrous salt, sulfate and a small amount of nitric acid, nitrous acid composition of nitric oxide in the flue gas immediately, above-mentioned mixed solution is carried out oxidation processes, ferrous iron in the solution is oxidized to ferric iron and emits nitric oxide, and nitric oxide is oxidized to again nitrogen dioxide immediately simultaneously.
Further, add oxidant in the mixed solution with above-mentioned nitroso-ferrous salt, nitric acid and nitrous acid, carry out oxidation reaction, ferrous iron is oxidized to ferric iron in the absorption liquid, and gained ferric iron solution circulation is used for containing SO
2And NO
XSmoke absorption is processed, the NO that discharges simultaneously
2Gas makes flue gas reach the recycling purpose through liquid absorption.
Further, comprise that also the smoke absorption liquid with recycled for multiple times separates, purifying, crystallization gets 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 that stores, get respectively nitric acid or nitrate product, pending flue gas is reached realize recycling when cleaning.
Further, the NO that discharges of described oxidation reaction
2Gas is absorbed by water, ammoniacal liquor, potassium hydroxide or sodium hydroxide solution; The gas that discharges by water absorb to reclaim nitric acid, the gas that discharges by ammonia absorption reclaim ammonium nitrate, the gas that discharges absorbs the gas that reclaims potassium nitrate, discharges and absorbed by sodium hydroxide solution and reclaim sodium nitrate by potassium hydroxide solution.
Further, described acid ferric iron solution is: iron chloride and/or ferric sulfate; Described acid ferrous iron solution is: frerrous chloride and/or ferrous sulfate.
Further, the ratio of ferric iron solution and the molal quantity of ferrous iron solution is in described trivalent and the ferrous mixed solution: 10:1-5.
Further, total concentration of iron is 1-3mol/L in the ferric iron solution that passes into of described flue gas or ferric iron and the ferrous mixed solution.
Further, the initial hydrogen ion concentration is 0.6-1mol/L in described acid ferric iron solution or trivalent and the ferrous mixed solution.
Further, hydrogen ion concentration is 0.3-2mol/L in described acid ferric iron solution or trivalent and the ferrous mixed solution.
The method of fume wet-type integration desulfurization denitration provided by the invention can reach the purpose of gas cleaning, the sulfur dioxide in the flue gas, nitrogen oxide finally reclaims as sulphur resource and nitrogen resource, really realizes energy-saving and emission-reduction, recycling economy, turn waste into wealth, potential economic benefit is huge.
Description of drawings
Fig. 1 is the schematic flow sheet of the fume wet-type integration desulfurization denitration method that provides of the embodiment of the invention.
The specific embodiment
Referring to shown in Figure 1, the present invention adopts ferric iron solution or does the absorption liquid that contains sulfur dioxide and nitrogen oxide containing gas by ferric iron and ferrous iron solution that proper proportion is mixed, total concentration of iron is controlled at 1-3mol/L, be in the acid medium of 0.6-1mol/L in hydrogen ion concentration, under 0-100 ℃ temperature conditions, sulfur dioxide absorption and nitrogen oxide reach the purpose 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 ferric iron mixes with ferrous iron in the mixed solution is 10:1-5, and the concrete content of selecting to need to press actual sulfureous in flue gas oxide and nitrogen oxide is recently determined; The kind of the acid in the acid medium comprises: hydrochloric acid and/or sulfuric acid.
After the flue gas that contains sulfur dioxide and nitrogen oxide passed into absorption liquid, sulfur dioxide can generate sulfurous acid and hydration sulfur dioxide are then generated sulfuric acid by the ferric iron oxidation the aqueous solution, and ferric iron becomes ferrous iron simultaneously; Then ferrous iron can absorb the nitric oxide in the flue gas, generates nitroso-ferrous salting liquid, thereby makes mixed solution show dark brown.Have the of short duration gathering of sulfurous acid and hydration sulfur dioxide in the solution, but in the excessive situation of ferric iron, nitroso-ferrously can not be reduced, than stable existence.
The auburn nitroso-ferrous salt of gained after processing, sulfate and a small amount of nitric acid, the mixed liquor that nitrous acid forms can pass through the oxidizing process post processing, makes the flue gas that absorbs realize innoxious purpose.Get the absorption liquid of determining volume, pass into or add a kind of of following oxidant, oxidant comprises: oxygen, ozone etc.Ferrous iron is oxidized to trivalent in the absorption liquid, discharge simultaneously nitric oxide, this nitric oxide soon is oxidized to nitrogen dioxide, enters in the suitable absorption liquid after wherein the excess air that is passed into of most of nitrogen dioxide blows out to absorb, and realizes the recycling of nitrogen oxide.
The desulphurization denitration black liquor is after oxidation processes, and the suitable absorption liquid of the nitrogen dioxide that is blown out by excess air comprises: water, ammoniacal liquor, potassium hydroxide solution, sodium hydroxide solution etc.Do the recyclable nitric acid of absorption liquid with water; The recyclable ammonium nitrate take ammoniacal liquor as absorption liquid; With potassium hydroxide, the solution such as NaOH are done the recyclable potassium nitrate of absorption liquid, sodium nitrate etc.
Sulfur dioxide is soluble in water, is generated rapidly afterwards the aqueous solution of sulfuric acid by the oxidation of ferric iron institute.This aqueous solution is when carrying out oxidizing process and remove nitrogen oxide in the solution, and ferrous iron has been 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 the circulation, when sulfate radical reached higher concentration, solution separated through concentrated, purifying, and crystallization makes ferric sulfate, iron chloride, ferric nitrate etc., the recycling of realization 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 ℃, pass into simultaneously sulfur dioxide under the atmospheric pressure, nitric oxide gas, intake is respectively 0.84mol, 1.66mol, reaction time is 0-3h, becomes dark brown to absorption liquid and stops, leaving standstill 1h after, this absorption liquid passes into 0.83mol oxygen, reaction time is 0-5h, and the nitrogen dioxide gas that discharges is absorbed by 1L distilled water, to the residue gas of emitting without till the nitrogen dioxide.Record that contained concentration of nitric acid is 0.78mol/L in the absorption liquid.
Pass into an amount of oxygen in the absorption liquid after the above-mentioned oxidation processes, make that ferrous iron all is converted into ferric iron in the solution.Gained solution is concentrated, be recrystallized, must contain the ferric sulfate product 138g of the crystallization water, contain 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, the ferrous iron solution concentration is the ferric trichloride of 0.54mol/L and the mixed solution 1L of frerrous chloride, in 30 ℃, pass into simultaneously sulfur dioxide under the atmospheric pressure, nitric oxide gas, intake is respectively 0.84mol, 2.2mol, and the reaction time is 0-3h, becoming dark brown to absorption liquid stops, after leaving standstill 1h, this absorption liquid passes into 1.1mol oxygen, and the reaction time is 0-5h, the nitrogen dioxide gas that discharges is absorbed by 1L distilled water, to the residue gas of emitting without till the nitrogen dioxide.Record that contained concentration of nitric acid is 0.88mol/L in the absorption liquid.
Pass into an amount of oxygen in the absorption liquid after the above-mentioned oxidation processes, make that ferrous iron all is converted into ferric iron in the solution.Gained solution is concentrated, be recrystallized, must contain the ferric sulfate product 158g of the crystallization water, contain iron chloride 122g and a small amount of sodium chloride crystallization of the crystallization water.
The present invention has following beneficial effect:
1, changes existing treatment process, remove when realizing sulfur dioxide and nitrogen oxide, reduced cost of investment and unit scale, reduced operating cost, be an important breakthrough to the flue gas desulfurization and denitrification technology, really realized social benefit, the organic unity of economic benefit and environmental benefit.
2, the present invention has opened 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, to be used for the iron that flue gas processes be absorption liquid to this technology, can regenerate, can realize recycling, thereby reduce the operating cost of system.Sulfur dioxide in the flue gas, nitrogen oxide finally reclaim as sulphur resource and nitrogen resource, really realize energy-saving and emission-reduction, and recycling economy turns waste into wealth, and potential economic benefit is huge.
4, in the processing procedure and recycling process of this technology operation, non-secondary pollution is realized the innoxious of flue gas and cleans discharging that environmental benefit is obvious.
5, realize flue gas and desulfurizing and denitrifying in the same system, have equipment and simplify, take up an area and lack that throw and economize, operating cost is low, denitrification efficiency is stable, and operation is simple and reliable, the characteristics of convenient management.
It should be noted last that, the above specific embodiment is only unrestricted in order to technical scheme of the present invention to be described, although with reference to example the present invention is had been described in detail, those of ordinary skill in the art is to be understood that, can make amendment or be equal to replacement technical scheme of the present invention, and not breaking away from the spirit and scope of technical solution of the present invention, it all should be encompassed in the middle of the claim scope of the present invention.
Claims (13)
1. fume wet-type integration desulfurization denitration method is characterized in that:
To contain SO
2And NO
XFlue gas passes into acid ferric iron solution or trivalent and ferrous mixed solution, under 0-100 ℃ temperature conditions, absorbs NO
XAnd sulfur dioxide, generate the mixed solution that auburn nitroso-ferrous salt, sulfate and a small amount of nitric acid, nitrous acid form, above-mentioned mixed solution is carried out oxidation processes, and the ferrous ion in the solution is oxidized to ferric while nitric oxide and is released and is oxidized to nitrogen dioxide and emit.
2. fume wet-type integration desulfurization denitration method according to claim 1 is characterized in that:
To contain 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 ℃, reaction 0-3h absorbs NO
XAnd sulfur dioxide, SO
2Water-soluble generation sulfite ion is followed and ferric iron generation redox reaction first, and inferior sulfate radical becomes sulfate radical, and ferric iron becomes ferrous iron; The ferrous iron that generates adsorbs the last mixed solution that generates auburn nitroso-ferrous salt, sulfate and a small amount of nitric acid, nitrous acid composition of nitric oxide in the flue gas immediately, above-mentioned mixed solution is carried out oxidation processes, ferrous iron in the solution is oxidized to ferric iron and emits nitric oxide, and nitric oxide is oxidized to again nitrogen dioxide immediately simultaneously.
3. fume wet-type integration desulfurization denitration method according to claim 1 is characterized in that,
To contain SO
2And NO
XFlue gas passes into acid ferric iron solution or trivalent and ferrous mixed solution, and under 0-100 ℃ temperature conditions, reaction 0-3h absorbs NO
XAnd sulfur dioxide, SO
2Water-soluble generation sulfite ion is followed and ferric iron generation redox reaction first, and inferior sulfate radical becomes sulfate radical, and ferric iron becomes ferrous iron; The ferrous iron that generates adsorbs the last mixed solution that generates auburn nitroso-ferrous salt, sulfate and a small amount of nitric acid, nitrous acid composition of nitric oxide in the flue gas immediately, above-mentioned mixed solution is carried out oxidation processes, ferrous iron in the solution is oxidized to ferric iron and emits nitric oxide, and nitric oxide is oxidized to again nitrogen dioxide immediately simultaneously.
4. each described fume wet-type integration desulfurization denitration method according to claim 1-3 is characterized in that:
Add oxidant in the mixed solution with above-mentioned nitroso-ferrous salt, nitric acid and nitrous acid, carry out oxidation reaction, ferrous iron is oxidized to ferric iron in the absorption liquid, and gained ferric iron solution circulation is used for containing SO
2And NO
XSmoke absorption is processed, the NO that discharges simultaneously
2Gas makes flue gas reach the recycling purpose through liquid absorption.
5. by the described fume wet-type integration desulfurization denitration of claim 4 and resource utilization method, it is characterized in that, also comprise:
The smoke absorption liquid of recycled for multiple times is separated, purifying, crystallization gets ferric sulfate or iron chloride, realizes the recycling of flue gas desulfurization and denitrification mixed liquor.
6. each described fume wet-type integration desulfurization denitration method is characterized in that according to claim 1-3, also comprises:
Described nitrogen dioxide is collected storage;
Collecting the water-soluble or alkali lye of nitrogen dioxide that stores, get respectively nitric acid or nitrate product, pending flue gas is reached realize recycling when cleaning.
7. fume wet-type integration desulfurization denitration method according to claim 6 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 that discharges by water absorb to reclaim nitric acid, the gas that discharges by ammonia absorption reclaim ammonium nitrate, the gas that discharges absorbs the gas that reclaims potassium nitrate, discharges and absorbed by sodium hydroxide solution and reclaim sodium nitrate by potassium hydroxide solution.
8. each described fume wet-type integration desulfurization denitration method according to claim 1-3 is characterized in that:
Described flue gas comprises: all high temp. combustion of fuels produce contains SO
2And NO
XGas.
9. each described fume wet-type integration desulfurization denitration method according to claim 1-3 is characterized in that:
Described acid ferric iron solution is: iron chloride and/or ferric sulfate; Described acid ferrous iron solution is: frerrous chloride and/or ferrous sulfate.
10. each described fume wet-type integration desulfurization denitration method according to claim 1-3 is characterized in that:
Ferric iron solution with the ratio of the molal quantity of ferrous iron solution is in described trivalent and the ferrous mixed solution: 10:1-5.
11. each described fume wet-type integration desulfurization denitration method according to claim 1-3 is characterized in that:
Total concentration of iron is 1-3mol/L in the ferric iron solution that described flue gas passes into or ferric iron and the ferrous mixed solution.
12. each described fume wet-type integration desulfurization denitration method according to claim 1-3 is characterized in that:
The initial hydrogen ion concentration is 0.6-1mol/L in described acid ferric iron solution or trivalent and the ferrous mixed solution.
13. each described fume wet-type integration desulfurization denitration method according to claim 1-3 is characterized in that:
Hydrogen ion concentration is 0.3-2mol/L in described acid ferric iron solution or trivalent and the ferrous mixed solution.
Priority Applications (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201210578308.5A CN103028313B (en) | 2012-09-12 | 2012-12-27 | Integrated desulfuration and denitration method for wet oxidation of flue gas |
| PCT/CN2013/083353 WO2014040541A1 (en) | 2012-09-12 | 2013-09-12 | Flue gas wet oxidation integrated desulfurization and denitration method |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201210336226.X | 2012-09-12 | ||
| CN201210336226XA CN102824836A (en) | 2012-09-12 | 2012-09-12 | Integrated wet-type oxidation, desulfurization, denitration and recycling method for smoke |
| CN201210578308.5A CN103028313B (en) | 2012-09-12 | 2012-12-27 | Integrated desulfuration and denitration method for wet oxidation of flue gas |
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| Publication Number | Publication Date |
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| CN103028313A true CN103028313A (en) | 2013-04-10 |
| CN103028313B CN103028313B (en) | 2015-01-21 |
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| CN201210336226XA Withdrawn CN102824836A (en) | 2012-09-12 | 2012-09-12 | Integrated wet-type oxidation, desulfurization, denitration and recycling method for smoke |
| CN201210581309.5A Expired - Fee Related CN102989303B (en) | 2012-09-12 | 2012-12-27 | Smoke wet-type oxidation integral desulfuration denitration and energy using method |
| CN201210578308.5A Expired - Fee Related CN103028313B (en) | 2012-09-12 | 2012-12-27 | Integrated desulfuration and denitration method for wet oxidation of flue gas |
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| CN201210581309.5A Expired - Fee Related CN102989303B (en) | 2012-09-12 | 2012-12-27 | Smoke wet-type oxidation integral desulfuration denitration and energy using method |
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| WO (2) | WO2014040539A1 (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2014040541A1 (en) * | 2012-09-12 | 2014-03-20 | 河南绿典环保节能科技有限公司 | Flue gas wet oxidation integrated desulfurization and denitration method |
| CN105080327A (en) * | 2014-05-05 | 2015-11-25 | 淮南市明月环保科技有限责任公司 | Method for desulfurizing and recovering NOx with alkali liquor |
| CN105126567A (en) * | 2014-10-11 | 2015-12-09 | 黄立维 | Method and device for removing nitric oxide and sulfur oxide from gas flow |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| 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 |
| WO2022135223A1 (en) * | 2020-12-26 | 2022-06-30 | 黄立维 | Device and process for removing nitric oxide in gas flow |
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| CN102824836A (en) * | 2012-09-12 | 2012-12-19 | 河南绿典环保节能科技有限公司 | Integrated wet-type oxidation, desulfurization, denitration and recycling method for smoke |
Cited By (4)
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| WO2014040541A1 (en) * | 2012-09-12 | 2014-03-20 | 河南绿典环保节能科技有限公司 | Flue gas wet oxidation integrated desulfurization and denitration method |
| CN105080327A (en) * | 2014-05-05 | 2015-11-25 | 淮南市明月环保科技有限责任公司 | Method for desulfurizing and recovering NOx with alkali liquor |
| CN105126567A (en) * | 2014-10-11 | 2015-12-09 | 黄立维 | Method and device for removing nitric oxide and sulfur oxide from gas flow |
| CN105126567B (en) * | 2014-10-11 | 2019-08-20 | 黄立维 | A kind of method and device thereof for removing denitrification and oxysulfide from air-flow |
Also Published As
| Publication number | Publication date |
|---|---|
| CN103028313B (en) | 2015-01-21 |
| WO2014040541A1 (en) | 2014-03-20 |
| WO2014040539A1 (en) | 2014-03-20 |
| CN102989303A (en) | 2013-03-27 |
| CN102989303B (en) | 2014-10-08 |
| CN102824836A (en) | 2012-12-19 |
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