CN103100294A - Method for removing oxynitride from flue gas through ozone oxidation method - Google Patents
Method for removing oxynitride from flue gas through ozone oxidation method Download PDFInfo
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- CN103100294A CN103100294A CN2011103607027A CN201110360702A CN103100294A CN 103100294 A CN103100294 A CN 103100294A CN 2011103607027 A CN2011103607027 A CN 2011103607027A CN 201110360702 A CN201110360702 A CN 201110360702A CN 103100294 A CN103100294 A CN 103100294A
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- absorption tower
- flue gas
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- ozone
- alkali lye
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Abstract
The invention discloses a method for removing oxynitride from flue gas through an ozone oxidation method. The method comprises the following steps of: cooling the flue gas to 30-110 DEG C; introducing ozone into the cooled flue gas to react for 0 to 10 seconds; introducing the gas after the reaction into an absorbing tower; and spraying alkali liquor into the absorbing tower to absorb the gas after the reaction, wherein the gas after absorption can be discharged into air or put into other devices, and the alkali liquor after the absorption is reused. By adopting the method, the oxynitride in the flue gas can be efficiently and highly-selectively removed, so that the method can be used on industrial devices generating a lot of flue gas, such as the industrial devices of coal-fired power plants, cement plants, oil refineries and steel works.
Description
Technical field
The invention belongs to environmental protection technical field, particularly a kind of Ozonation removes the method for oxynitrides in flue gas.
Background technology
As everyone knows, environmental protection has become the hot issue that the world today pays close attention to, and the control level of environmental quality becomes the criterion of a national development degree.NOx is in rising trend year by year as the aerial content of a kind of dusty gas, and this is mainly that waste gas due to moving source dischargings such as the stationary source such as coal-fired power plant and oil-refining chemical factory's catalytic cracking (FCC) device and automobile, trains causes.Wherein, NO easily forms acid rain, photochemical fog, the respiratory system of serious harm human body under effect of sunlight; And N
2O energy strong absorption infra-red radiation helps the reinforcement of greenhouse effects.Therefore, eliminating NOx has very important significance to the environmental protection tool.Many countries have formulated strict NOx discharge standard.
At present, carried out a large amount of research work in gas denitrifying technology field Chinese scholars, the measure of controlling at present the NOx discharging roughly is divided into two classes, and a class is flue gases purification, removes the NOx in flue gas; Another kind of is low NOx combusting technology, and by various technological means, the NOx in inhibition or reduction combustion process reaches the purpose that reduces the NOx discharging.The selective catalytic reduction of wet method denitride technology (Selective Catalytic Reduction, abbreviation SCR) method, SNCR (Selective Non-Catalytic Reduction is called for short SNCR) method, wet type Absorption via Chemical Complexation etc.SNCR uses NH
3, in the injection of reducing agent people stove such as urea and NO
xCarry out selective reaction, without catalyst, therefore must add reducing agent in the high-temperature region.It is between 900 ℃～1200 ℃ that reducing agent sprays into fire box temperature, and the rapid thermal decomposition of this reducing agent becomes NH
3And with flue gas in NO
xCarry out the SNCR reaction and generate N
2These method characteristics are not need catalyst, and the rebuilding old equipment amount is little, invest littlely than the SCR method, but the ammoniacal liquor consumption is than the SCR fado.The SCR method refers to the selective catalytic reduction process of nitrogen oxide (NOx), is under the effect of catalyst, by ammonification (NH
3) can change into nitrogen (N to NOx
2) and water, due to NH
3Can " optionally " and NOx reaction rather than by oxygen (O
2) oxidation, therefore reaction is called as and has " selectively ".Reaction can be carried out between 280～450 ℃.The advantage of this method is: reaction temperature is lower, and purifying rate is high, and process equipment is compact, and is reliable, the nitrogen emptying after reduction, non-secondary pollution.But also have some obvious shortcomings: smoke components is complicated, and some pollutant can make catalyst poisoning; But the surface of the dust particle covering catalyst of high dispersive makes its active decline; Investment is higher with operating cost, NH
3Easily leak, operation and storage difficulty, and easily form (NH
4)
2SO
4
Chinese patent CN1923341A discloses a kind of coal-burning boiler fume ozone oxidation and simultaneous desulfurization denitrification apparatus and method thereof.Its method comprises the following steps: 1) 110～150 ℃ of low-temperature zone before or after the electrostatic precipitator of boiler flue spray into ozone O
3The nitrogen oxide molar ratio that sprays in ozone and boiler smoke is 0.5～1.5, water-fast lower valency nitrogen oxide in boiler smoke is oxidized into high valence state nitrogen oxide soluble in water, and oxidizing sulfur dioxide generates sulfur trioxide, and the reaction time is at least 0.5 second; 2) will send into the alkali liquid washing tower through the boiler smoke that previous step is processed, in the alkali liquid washing tower, flue gas be washed, absorb simultaneously high valence state nitrogen oxide and oxysulfide in flue gas.But ozone approximately just was decomposed into oxygen at normal temperatures and pressures daytime in 3 minutes fully, it is very violent that temperature reaches 100 ℃ of decomposition, and this technology points out that reaction temperature is between 110～150 ℃, ozone moment just becomes oxygen at this temperature, also do not react with oxynitrides and just no longer have strong oxidizing property, so this technology is difficult to the effect that reaches good under practical situations.
Chinese patent CN101485957A discloses a kind of fire coal boiler fume treatment technology, aims to provide a kind of using ozone oxygenation combined with double-tower washing to the device and method of the flue gas and desulfurizing and denitrifying of coal-burning boiler.This device comprises flue, and flue is connected with heat exchanger, alkali liquid washing tower A, alkali liquid washing tower B successively; In alkali liquid washing tower A and alkali liquid washing tower B, circulating sprayer A and circulating sprayer B are set respectively, ozone generator respectively with alkali liquid washing tower A bottom liquid phase region with enter alkali liquid washing tower B before pipeline be connected.Use this technology can reach denitration efficiency and 95% above desulfuration efficiency more than 80%.First carry out desulfurization and carry out again the order of denitration but this technology adopts, in fact oxynitrides than oxygen sulfur compound easier and ozone reaction, so the process route of this patent is put upside down just; Simultaneously general sulfureous in flue gas content is greater than oxynitrides content, adopts the ozone desulfurization to need a large amount of ozone, and the incurred cost of ozone not only is the oxygen source, and be that its power consumption is higher, so for desulfurization, seldom adopt ozone oxidation, be exactly because its cost is too high.
Chinese patent CN101259369A discloses a kind of flue gas desulfurization denitration dust-removing integrated technique, and it is that flue gas is carried out desulphurization denitration by reactor generation oxidation reaction and acid-base neutralization reaction, and the flue gas after processing obtains pure flue gas through dedusting.A whole set of process unit comprises ozone generator, and the water of generation is supplied with molten mechanism of qi and made the oxygen enrichment absorption liquid, sends into reactor and mixes with flue gas and carry out oxidation reaction.Reactor comprises Venturi tube, elbow, white lime distribution grid, straight tube and perpendicular type deflector.The present invention is that brand-new technique, efficient are high, small investment, operating cost are low.This technology is first reacted with flue gas ozone is soluble in water again, because seldom there is the composition energy soluble in water in flue gas except steam, ozone namely enables soluble in water, and ozone also needs first to break gas-liquid interface and reacts, increase the reaction resistance, reduced the touch opportunity of reactant.
Summary of the invention
The purpose of this invention is to provide a kind of method that Ozonation removes oxynitrides in flue gas, to overcome the shortcomings such as prior art reaction temperature height and cost are higher.Use the inventive method can remove efficiently oxynitrides in flue gas, and the cost of the inventive method is lower, selectively good.The inventive method can be used for the commercial plant that coal-burning power plant, cement plant, oil plant, steel mill etc. have a large amount of flue gases to produce.
The invention provides a kind of method that Ozonation removes oxynitrides in flue gas, it is characterized in that comprising the steps:
1) between flue gas cool-down to 30～110 ℃, between preferred 40～90 ℃, then ozone is passed in the flue gas after cooling and react, very little owing to reacting liberated heat in this reaction, so reaction temperature remains unchanged substantially, the reaction time is between 0～10 second, between preferred 2～8 seconds; The ozone amount that passes into and oxynitrides mol ratio be 0.5～2: between 1, preferred 1.2～1.8: 1.
2) with step 1) middle gas introducing absorption tower of having reacted, top, absorption tower sprays into alkali lye, with alkali lye, the gas that has reacted is absorbed, gas after absorption can be discharged in air or enter other device, reacted alkali lye recycles, keeping the pH value of alkali lye is between 6.5～8, between preferred 6.8～7.5; The mol ratio that sprays into the complete gas of alkali lye amount in the absorption tower and absorption tower internal reaction is 20～1: between 1, and preferred 5～1.5: between 1.
3) according to step 2) in the absorption tower situation of change of pH value introduce fresh alkali lye, and discharge a part of crystallized stock bottom the absorption tower.
The further technical characterictic of the present invention is: the reaction of described ozone and flue gas is carried out in reactor, and ozone enters reactor from the reactor middle and upper part, and flue gas enters reactor from reactor bottom.
The further technical characterictic of the present invention is: the gas that has reacted described step 1) is introduced the middle and lower part on absorption tower.
The required ozone of the inventive method mainly prepares by source of oxygen or air-source.
Nitrogen in the inventive method in ozone and flue gas reacts, and its key reaction is as follows:
NO+O
3→NO
2+O
2
2NO
2+O
3→N
2O
5+O
2
N
2O
5+H
2O→2HNO
3
HNO
3+NaOH→NaNO
3+H
2O
Alkali lye described in the inventive method in the absorption tower can be more than one in NaOH, calcium hydroxide, ammoniacal liquor and calcium carbonate etc.
The present invention compared with prior art has fabulous selective and reactivity because it adopts Ozonation, can react rapidly with oxynitrides, and the N that generates
2O
5Very easily soluble in water, therefore reaction is very rapid quick, is suitable for the larger commercial plant of exhaust gas volumn; And the inventive method denitration efficiency is high.This has investment lower than the SCR method of routine etc. in addition, and there is no the phenomenon such as the escaping of ammonia, is conducive to aftertreatment technology.In addition, O
3Have selfdecomposition, catabolite is nontoxic O
2, non-secondary pollution.The inventive method denitration efficiency is high, and cost is low.
Specific embodiment below in conjunction with accompanying drawing is described in further detail the present invention, but does not limit the scope of the invention.
Description of drawings
Figure is a kind of simple flow chart of the present invention.
In figure: the 1-reactor, 2-ozone, the 3-flue gas, the 5-pump,
6-alkali lye, the 7-absorption tower, the fresh alkali lye of 8-,
9-removes the flue gas after nitrogen oxide.
As shown in the figure, be 30～110 ℃ with temperature, the flue gas 3 of preferred 40～90 ℃ passes into from the bottom of reactor 1, ozone 2 passes into from the middle and upper part of reactor 1, flue gas 3 and ozone 2 these two strands of gases react in reactor 1 inside, and the reaction time is 0～10 second, preferred 2～8 seconds; The ozone amount that passes into and oxynitrides mol ratio be 0.5～2: 1, preferred 1.2～1.8: 1.Because the reaction liberated heat is very little, so reaction temperature remains unchanged.
The gas that has reacted in reactor 1 enters the middle and lower part on absorption tower 7, the top on absorption tower 7 sprays into alkali lye 6, the gas that has reacted is absorbed, gas after absorption is the flue gas 9 that removes after nitrogen oxide, the flue gas 9 that removes after nitrogen oxide can be discharged in air or enter other device, reacted alkali lye is pumped into absorption tower 7 through pump 5 and recycles, and keeping the pH value of alkali lye is 6.5～8, between preferred 6.8～7.5; The mol ratio that sprays into the complete gas of alkali lye amount in the absorption tower and absorption tower internal reaction is 20～1: between 1, and preferred 5～1.5: between 1.7 top introduce fresh alkali lye 8 according to the situation of change of absorption tower 7 interior pH values from the absorption tower; Along with the alkali lye that absorbs increases, can the crystallization of some salts appear in the bottom, absorption tower, these crystallizations can be taken out, the limpid alkali lye in upper strata still can recycle.Mainly contain the materials such as sodium nitrate, sodium sulphate, calcium nitrate, calcium sulfate, sodium sulfite in these crystallizations, these materials can use as the raw material of industry after purifying.
Embodiment
The flue gas of 500ppmvNOx is reduced the temperature to below 90 ℃, passing into ozone concentration is 500ppmv, 5 seconds reaction time, then flue gas is sent in the absorption tower, passes into 4% sodium hydroxide solution and absorb, liquid-gas ratio is 3: 1, can be directly emptying with the flue gas after absorbing, wherein the concentration of NOx is 10ppmv, and denitration efficiency is 98%, and alkali lye can continue to recycle.Whole flue gas flow is constant, and NOx discharges minimizing.Experimental results show that the oxynitrides major part is converted into nitrate ion, reached the purpose that reduces discharging.
The flue gas of 300ppmvNOx is reduced the temperature to below 80 ℃, passing into ozone concentration is 500ppmv, 3 seconds reaction time, then flue gas is sent in the absorption tower, passes into 4% sodium hydroxide solution and absorb, liquid-gas ratio is 4: 1, can be directly emptying with the flue gas after absorbing, wherein the concentration of NOx is 10ppmv, and denitration efficiency is 97%, and alkali lye can continue to recycle.Whole flue gas flow is constant, and NOx discharges minimizing.Experimental results show that the oxynitrides major part is converted into nitrate ion, reached the purpose that reduces discharging.
The flue gas of 200ppmvNOx is reduced the temperature to 60 ℃, passing into ozone concentration is 300ppmv, 5 seconds reaction time, then flue gas is sent in the absorption tower, passes into 4% aqua calcis and absorb, liquid-gas ratio is 3.5: 1, can be directly emptying with the flue gas after absorbing, wherein the concentration of NOx is 0ppmv, and denitration efficiency is 100%, and alkali lye can continue to recycle.Whole flue gas flow is constant, and NOx discharges minimizing.Experimental results show that the oxynitrides major part is converted into nitrate ion, reached the purpose that reduces discharging.
Embodiment 4
The flue gas of 420ppmvNOx is reduced the temperature to 40 ℃, passing into ozone concentration is 600ppmv, 5 seconds reaction time, then flue gas is sent in the absorption tower, passes into 4% aqua calcis and absorb, liquid-gas ratio is 5: 1, can be directly emptying with the flue gas after absorbing, wherein the concentration of NOx is 0ppmv, and denitration efficiency is 100%, and alkali lye can continue to recycle.Whole flue gas flow is constant, and NOx discharges minimizing.Experimental results show that the oxynitrides major part is converted into nitrate ion, reached the purpose that reduces discharging.
The flue gas of 180ppmvNOx is reduced the temperature to 40 ℃, passing into ozone concentration is 300ppmv, 4 seconds reaction time, then flue gas is sent in the absorption tower, passes into 4% calcium carbonate soln and absorb, liquid-gas ratio is 2.5: 1, can be directly emptying with the flue gas after absorbing, wherein the concentration of NOx is 0ppmv, and denitration efficiency is 100%, and alkali lye can continue to recycle.Whole flue gas flow is constant, and NOx discharges minimizing.Experimental results show that the oxynitrides major part is converted into nitrate ion, reached the purpose that reduces discharging.
Claims (10)
1. an Ozonation removes the method for oxynitrides in flue gas, it is characterized in that comprising the steps:
1) between flue gas cool-down to 30～110 ℃, then ozone is passed in the flue gas after cooling and react, the reaction time is 0～10 second, and the ozone amount that passes into and the mol ratio of oxynitrides are 0.5～2: 1;
2) with step 1) middle gas introducing absorption tower of having reacted, top, absorption tower sprays into alkali lye, with alkali lye, the gas that has reacted is absorbed, gas discharging after absorption is in air or enter other device, alkali lye after absorption recycles, in the absorption tower, the pH value of alkali lye is 6.5～8, and the mol ratio that sprays into the complete gas of alkali lye amount in the absorption tower and absorption tower internal reaction is 20～1: 1;
3) according to step 2) in the absorption tower situation of change of pH value introduce fresh alkali lye, and discharge a part of crystallized stock bottom the absorption tower.
2. method according to claim 1, it is characterized in that: the reaction of described ozone and flue gas is carried out in reactor, and ozone enters reactor from the reactor middle and upper part, and flue gas enters reactor from reactor bottom.
3. method according to claim 1 is characterized in that: the middle and lower part on the gas introducing absorption tower of react described step 1).
4. method according to claim 1, it is characterized in that: the alkali lye in described absorption tower is more than one in NaOH, calcium hydroxide, ammoniacal liquor and calcium carbonate.
5. method according to claim 1, it is characterized in that: described flue-gas temperature is 40～90 ℃.
6. method according to claim 1, is characterized in that: described ozone employing oxygen source or the preparation of air source of the gas.
7. method according to claim 1, it is characterized in that: the described reaction time is 2～8 seconds.
8. method according to claim 1, it is characterized in that: the mol ratio of described ozone amount and oxynitrides is 1.2～1.8: 1.
9. method according to claim 1, it is characterized in that: described step 2) in the absorption tower, pH value is 6.8～7.5.
10. method according to claim 1 is characterized in that: the mol ratio that described step 2) sprays into the complete gas of alkali lye amount in the absorption tower and absorption tower internal reaction in the absorption tower is 5～1.5: 1.
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|---|---|---|---|
| CN2011103607027A CN103100294A (en) | 2011-11-15 | 2011-11-15 | Method for removing oxynitride from flue gas through ozone oxidation method |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103435019A (en) * | 2013-08-28 | 2013-12-11 | 阎君 | Method for preparing calcium nitrite by using nitric oxide in smoke |
| CN104607031A (en) * | 2015-02-12 | 2015-05-13 | 巨石集团有限公司 | Waste gas denitration treatment method and device thereof |
| CN104941410A (en) * | 2015-06-03 | 2015-09-30 | 浙江大学 | Flue gas desulfurization and denitrification integrated method and device based on two-step oxidation process of active molecules O3 at low temperature |
| CN105270772A (en) * | 2014-07-07 | 2016-01-27 | 中石化洛阳工程有限公司 | Ethylene spherical tank cooling depressurizing method |
| CN105597502A (en) * | 2016-01-14 | 2016-05-25 | 董海威 | Low-temperature ozone oxidation denitration system |
| CN110180348A (en) * | 2019-06-17 | 2019-08-30 | 中国华能集团有限公司 | A kind of flue gas nitrogen oxide oxidation unit and technique |
| WO2020083170A1 (en) * | 2018-10-22 | 2020-04-30 | 上海必修福企业管理有限公司 | Ozone purification system and method for engine exhaust gas |
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| CN1923341A (en) * | 2006-08-23 | 2007-03-07 | 浙江大学 | Device and method for coal-burning boiler fume ozone oxidation and simultaneous desulfurization and denitrification |
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| CN101485957A (en) * | 2009-01-08 | 2009-07-22 | 浙江大学 | Device and method of simultaneous desulfuration and denitration for flue gas using ozone oxygenation combined with double-tower washing |
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2011
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103435019A (en) * | 2013-08-28 | 2013-12-11 | 阎君 | Method for preparing calcium nitrite by using nitric oxide in smoke |
| CN105270772A (en) * | 2014-07-07 | 2016-01-27 | 中石化洛阳工程有限公司 | Ethylene spherical tank cooling depressurizing method |
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| CN104941410A (en) * | 2015-06-03 | 2015-09-30 | 浙江大学 | Flue gas desulfurization and denitrification integrated method and device based on two-step oxidation process of active molecules O3 at low temperature |
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| WO2020083170A1 (en) * | 2018-10-22 | 2020-04-30 | 上海必修福企业管理有限公司 | Ozone purification system and method for engine exhaust gas |
| CN110180348A (en) * | 2019-06-17 | 2019-08-30 | 中国华能集团有限公司 | A kind of flue gas nitrogen oxide oxidation unit and technique |
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Application publication date: 20130515 |