CN101632897B - Method for simultaneously removing sulfur oxides and nitric oxides in flue gas - Google Patents
Method for simultaneously removing sulfur oxides and nitric oxides in flue gas Download PDFInfo
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- CN101632897B CN101632897B CN2009100907408A CN200910090740A CN101632897B CN 101632897 B CN101632897 B CN 101632897B CN 2009100907408 A CN2009100907408 A CN 2009100907408A CN 200910090740 A CN200910090740 A CN 200910090740A CN 101632897 B CN101632897 B CN 101632897B
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Abstract
The present invention relates to a method for simultaneously removing sulfur oxides and nitric oxides in flue gas, which belongs to the technical field of flue gas purification. The method comprises the following steps: spraying water or steam into a flue before flue gas from burning equipment enters a fluidized bed reactor through the flue and controlling the temperature of the flue gas within a range of 90-200 DEG C, wherein the flue gas in the flue contains gas components of O2, H2O, SO2 and NOx; directly jetting CaO and/or Ca(OH)2 into the flue to oxidize NO; and controlling the temperature of the fluidized bed reactor to be between 50 DEG C and 90 DEG C for the flue gas to desulfurize and denitrate in the fluidized bed reactor. In the method, desulfurization and denitration can be simultaneously realized in the same system by adjusting processing steps and controlling a reaction condition. When a molar ratio Ca/(S+0.5N) of calcium to sulfur to nitrogen is 1.3, the removal rate of the SO2 can reach over 85 percent, and the removal rate of the NO can reach over 60 percent.
Description
Technical field
The present invention relates to a kind of desulfurization denitration method of combustion of fossil fuel flue gas, belong to the flue gases purification field.
Background technology
Current because the extensive fossil fuel that uses has oxysulfide more than 20,000,000 tons every year (with SO
2Be main) and the nitrogen oxide more than 10,000,000 tons (based on NO) enter atmosphere, cause serious acid rain to pollute within the border in China.Carried out at present the technology of the control sulfur dioxide (SO2) emissions of large-scale commercial applications application, comprised limestone-gypsum method and half in method flue gas desulfurization technique (spray drying process and flue gas circulating fluidized bed method), their characteristics are desulfuration efficiency height, but can't denitration.Especially for the semi-dry process flue gas desulphurization technology, when with CaO or Ca (OH)
2As absorbent, though absorbent granules is thin more, reactivity is high more, and calcium to sulphur mole ratio is (with respect to the SO in the inlet flue gas
2) in fact surpass 1.3, just can reach higher desulfuration efficiency.And the technology of discharged nitrous oxides has SCR (SCR) and SNCR (SNCR) in the ripe reduction flue gas, the two discharges after all adopting ammonia or urea that the nitrogen oxide in the flue gas is reduced to harmless nitrogen again, the advantage of SCR is the denitration efficiency height, shortcoming is the cost height, especially catalyst cost, make the user beyond affordability, and operation maintenance is required high, and the cost of SNCR is relatively low, but denitration efficiency is also low, and to the strictness of spray site temperature requirement, the two all requires reducing agent and flue gas to mix, otherwise partial reduction agent meeting is escaped away, causes secondary pollution.Above desulphurization denitration technology is implemented control respectively to sulfur dioxide and nitrogen oxide, and equipment investment is bigger.
Summary of the invention
Purpose of the present invention and task are at the deficiencies in the prior art and defective, a kind of method that removes flue gas sulphur oxide and nitrogen oxide simultaneously is provided, under the situation that adopts the calcium to sulphur mole ratio identical with traditional semi-dry process flue gas desulphurization technology, by reasonable control processing step and operational factor, in a system, realize desulphurization denitration simultaneously, thereby further save equipment investment, reach good desulfurization off sulfide effect.
Technical scheme of the present invention is as follows:
A kind of method that removes flue gas sulphur oxide and nitrogen oxide simultaneously is characterized in that this method comprises the steps:
1) enters in the fluidized-bed reactor by flue from the flue gas in the combustion apparatus, before flue gas enters fluidized-bed reactor, water or water vapour are sprayed into the flue gas flue, contain O in the flue gas in the flue
2, H
2O, SO
2With the NOx gas componant, and the control flue-gas temperature is in 90 ℃～200 ℃ scopes; Then with fresh absorbent CaO and Ca (OH)
2In one or both be directly injected in the flue, participate in earlier the oxidizing process of NO in the flue gas, control calcium sulphur nitrogen mol ratio Ca/ (S+0.5N) realizes the desulfurization and the denitration function of part between 1.0～2.5;
2) flue gas carries out desulphurization denitration in fluidized-bed reactor, and by spraying water in fluidized-bed reactor, the temperature of control fluidized-bed reactor is between 50 ℃～90 ℃, and fluidized-bed reactor moves under the temperature conditions that is higher than 5 ℃～25 ℃ of dew points;
3) flue gas behind the desulphurization denitration enters separator by pipeline, a separated solid particle part of getting off is returned fluidized-bed reactor or is sprayed into former flue gas flue and enters fluidized-bed reactor with flue gas again in the separator, another part is discharged from system, to keep the material balance of whole system; Discharge from flue through the flue gas that purifies.
Technical characterictic of the present invention also is: absorbent sprays into the volume fraction of steam in the flue gas between 5～25%, O
2Volume fraction between 1～15%.Control calcium sulphur nitrogen mol ratio Ca/ (S+0.5N) is between 1.0～2.5.The flue-gas temperature that preferred absorbent sprays into a little is controlled between 100～150 ℃.The average grain diameter d of absorbent
50Be preferably 2 μ m～50 μ m, R
90Less than 10%.Gas flow rate is controlled to be 3m/s～10m/s in fluidized-bed reactor, and the average content of particle is controlled to be 1kg/m
3～10kg/m
3Described separator adopts inertia separator, electric cleaner or sack cleaner.
The present invention compared with prior art has the following advantages and the high-lighting effect:
When sorbent injection point temperature during at 100～150 ℃, in the flue gas oxygen volume fraction in 1～15% (dry flue gas) scope, the volume fraction of steam between 5～30%, calcium sulphur nitrogen mol ratio Ca/ (S+0.5N) 1.3 o'clock, SO
2Removal efficiency can reach more than 85%, and the NO removal efficiency can reach more than 60%.Under situation about adopting with the identical calcium to sulphur mole ratio of traditional semi-dry process flue gas desulphurization technology, its desulfurized effect obviously improves, when realizing high-efficiency desulfurization, also can remove the NO in the flue gas, make that oxysulfide and discharged nitrous oxides can satisfy national requirements for environmental protection in the SO 2 from fume concentration and nitrous oxides concentration scope of routine.
Another outstanding effect of the present invention is to have realized the purpose of while desulphurization denitration in a system.According to the characteristics of smoke components, by reasonable control processing step and operational factor, elder generation is absorbed agent Ca (OH) with sulfur dioxide after the nitric oxide catalytic oxidation is nitrogen dioxide again
2Or the CaO absorption, realize reaching good desulfurization off sulfide effect, thereby saved equipment investment greatly, needn't set up two cover control device because oxysulfide is different with nitrogen oxide, effectively reduce controlling cost of flue gas pollutant discharging.
Description of drawings
Fig. 1 is a process chart of the present invention.
The former flue gas flue of 1-; The 2-fluidized-bed reactor; 3-steam or water spray injection pipe; 4-absorbent material storing box; The 5-water pipeline; 6-fluidized-bed reactor exhaust pass; The 7-separator; 8-feed back pipeline; The 9-ash discharging hole; The clean flue gas flue of 10-
The specific embodiment
By means of accompanying drawing principle of the present invention, technical process are further described below.
Fig. 1 is a process chart of the present invention.Enter in the fluidized-bed reactor 2 by former flue gas flue 1 from the flue gas in the combustion apparatus, before flue gas enters fluidized-bed reactor, water or water vapour are sprayed into the flue gas flue by steam or water spray injection pipe 3, contain O in the flue gas in the flue
2, H
2O, SO
2With the NOx gas componant, and control flue-gas temperature in 90 ℃～200 ℃ scopes, the volume fraction that guarantees water vapour in the flue gas simultaneously is between 5%～25%.Then with fresh absorbent CaO and Ca (OH)
2In one or both be directly injected in the flue from material storing box 4 roads, fully mix with flue gas, participate in earlier the oxidizing process of NO in the flue gas, control calcium sulphur nitrogen mol ratio Ca/ (S+0.5N) is between 1.0～2.5; Participate on the one hand desulphurization reaction, on the other hand and SO
2, water vapour, oxygen be NO with the NO catalytic oxidation together
2, NO
2With the absorbent reaction, reach the purpose of denitration again.Because part SO
2In time be not removed in flue with NOx, enter after the fluidized-bed reactor 2, further with unreacted absorbent quick lime CaO or white lime Ca (OH) completely
2Reaction makes most of SO
2And NOx is hunted down.For guaranteeing to reach higher denitrification efficiency in the fluidized-bed reactor,, guarantee that temperature in the fluidized-bed reactor is between 50 ℃～90 ℃ and be higher than the scope work of 5 ℃～15 ℃ of dew points by water pipeline 5 control injection flow rates.Flue gas behind the desulphurization denitration carries and removes product and enter separator 7 through fluidized-bed reactor exhaust pass 6, and the solid material that separated device separates mainly contains CaO or Ca (OH)
2And desulfurization product CaSO
4, CaSO
3, denitration product C a (NO
3)
2, Ca (NO
2)
2Deng material, for improving the utilization rate of absorbent, the separated part solid material that gets off is recycled, directly return fluidized-bed reactor through feed back pipeline 8, participate in the chemical reaction process of desulphurization denitration simultaneously again.The part solid material is discharged from ash discharging hole 9, to keep the solid material balance of whole system, discharges from clean flue gas flue 10 through the flue gas after the dedusting.
In addition, the part solid material that returns in feed back pipeline 8 also can be directly injected in the former flue gas flue 1, enters circulating fluid bed reactor with flue gas, thus extension of absorbent and pollutant SO
2With the time of contact of NOx, improve nitric oxide production oxygenation efficiency, strengthen desulfurization off sulfide effect.Gas velocity is about 3m/s to 5m/s in fluidized-bed reactor 7, solid material quality average out to 6kg/m in fluidized-bed reactor 7
3, gaseous contaminant SO
2, SO
3, NO, NO
2Absorbed by fine grain active absorbent largely in fluidized-bed reactor 7 with HCl.This kind method also can remove the HCl in the flue gas, the CaCl of the moisture absorption that it forms with the absorbent reaction
2, help to improve denitrification efficiency.
Simultaneously the principle of desulphurization denitration is: in the flue gas except containing pollutant SO
2Outside NO, absorbent sprays in a little the flue gas must contain the oxygen of volume fraction 1%～15% and 5～30% water vapour, the SO in the flue gas simultaneously
2Can be directly and CaO and (or) Ca (OH)
2Outside reaction was removed, oxygen, water vapour that it can also be in flue gas were at absorbent quick lime CaO or white lime Ca (OH)
2Under the situation about existing, catalyzing N O is oxidized into NO
2, the latter again with CaO or Ca (OH)
2Reaction reduces SO in the flue gas thereby reach
2Purpose with NOx.In temperature range of the present invention, when absorbent is CaO or Ca (OH)
2The time, the SO in the flue gas
2Can be directly be removed, simultaneously water vapour, oxygen, SO in flue gas with the form of sulfate or sulphite
2And Ca (OH)
2Or under the acting in conjunction of CaO, the NOx in the flue gas can nitrate or the form of nitrite be removed.Main desulfurization and denitrification reaction equation is:
Ca(OH)
2+SO
2→CaSO
3+H
2O (1)
CaO+SO
2→CaSO
3 (2)
At SO
2, O
2, steam and CaO or Ca (OH)
2Under the common catalytic action, the reaction that NO is oxidized to NO2 is:
NO+1/2O
2←→NO
2 (3)
In addition, also comprise following reaction
2NO
2(g)←→N
2O
4(g) (4)
NO(g)+NO
2(g)←→N
2O
3(g) (5)
N
2O
3(g)+H
2O←→2HNO
2(g) (6)
N
2O
4(g)+H
2O(g)←→HNO
2(g)+HNO
3(g) (7)
HNO
2(g)+Ca(OH)
2←→Ca(NO
2)
2+H
2O (8)
HNO
3(g)+Ca(OH)
2←→Ca(NO
3)
2+H
2O (9)
HNO
2(g)+CaO←→Ca(NO
2)
2 (10)
HNO
3(g)+CaO←→Ca(NO
3)
2 (11)
Except above independent desulfurization and denitrification reaction, also there is the chemical reaction of mutually promoting of desulfurization and denitration, thereby significantly improved desulfurization degree and denitration rate, concrete overall budget reaction equation is as follows:
2NO
2+ CaSO
3→ Ca (NO
2)
2+ CaSO
4(12) make desulphurization reaction (1) and (2) carry out to the right, thereby can guarantee that the conventional semi-dry desulfurizing process of this desulfurizing and denitrifying process has higher desulfuration efficiency.And, as absorbent average grain diameter d
50Effect is fine when being 2 μ m～20 μ m.Fluidized-bed reactor moves under the temperature conditions that is higher than 5 ℃～25 ℃ of dew points, and gas velocity is controlled at 4m/s～6m/s in the fluidized-bed reactor, and average solid retention time is controlled at 30min, and average solids content is controlled at 6kg/m
3The time, use by method of the present invention to keep high denitrification efficiency reliably.Under these conditions, even if SO in the waste gas
2The content height also can keep SO in the flue gas reliably
2Removal efficiency is greater than 85%, and the NOx removal efficiency is greater than 60%.
Concrete processing step: contain SO
2, NO, water vapour, oxygen, carbon dioxide and nitrogen combustion product gases enter in the fluidized-bed reactor from former flue gas flue, by spraying into water or water vapour, control flue-gas temperature in 90 ℃～200 ℃ scopes on the one hand, the volume fraction that guarantees water vapour in the flue gas simultaneously is between 5%～25%.Then, fresh absorbent CaO and Ca (OH)
2In the flue of 90 ℃～200 ℃ of one or both be directly injected to flue-gas temperatures in and flue gas fully mix absorbent and SO
2, water vapour, oxygen be NO with the NO catalytic oxidation together
2, NO
2And SO
2Being absorbed agent simultaneously absorbs.The gaseous contaminant SO that in time is not removed
2Enter in the circulating bed reactor further and the absorbent reaction with flue gas with NOx, make most of SO
2Be hunted down with NOx.For guaranteeing to reach higher denitrification efficiency in the fluidized-bed reactor,, guarantee that temperature in the fluidized-bed reactor is between 50 ℃～90 ℃ and be higher than the scope work of 5 ℃～25 ℃ of dew points by water pipeline 5 control injection flow rates.Flue gas behind the desulphurization denitration carries and removes product and enter separator, and the separated part solid material that gets off is discharged from ash discharging hole, to keep the solid material balance of whole system, discharges from clean flue gas flue 10 through the flue gas after the dedusting.The material that separated device separates mainly contains CaO or Ca (OH)
2And desulfurization product CaSO
4, CaSO
3, denitration product C a (NO
3)
2And Ca (NO
2)
2Deng material.For improving the utilization rate of absorbent, the separated material that gets off of part is recycled, directly return fluidized-bed reactor through the feed back pipeline, participate in the chemical reaction process of desulphurization denitration simultaneously again.In addition, the part solid material that returns in the feed back pipeline also can be directly injected in the former flue gas flue, enters circulating fluid bed reactor with flue gas, thus extension of absorbent and pollutant SO
2With the time of contact of NOx, improve nitric oxide production oxygenation efficiency, strengthen desulfurization off sulfide effect.Gaseous contaminant SO
2, SO
3, NO, NO
2Being absorbed the agent efficient absorption in flue and fluidized-bed reactor absorbs.This kind method also can remove the HCl in the flue gas, and it forms hygroscopic CaCl with the absorbent reaction
2, help to improve denitrification efficiency.The absorbent particle diameter is thin more, and the once desulfurization denitration effect is good more, the average grain particle diameter d of absorbent
50Quick lime (CaO) or white lime (Ca (OH) less than 100 μ m
2) desulfurized effect is good.The product of discharging from flue gas purification system can be recycled.
With several specific embodiments the present invention is described below:
Embodiment 1: and employing white lime (as absorbent, average grain particle diameter d
50Be 20 μ m, R
90Less than 10%, calcium sulphur nitrogen mol ratio (Ca/ (S+0.5N)) is 1.3, light a cigarette 110 ℃ of temperature degree of sorbent injection, temperature is 80 ℃ in the fluidized-bed reactor, is higher than dew-point temperature and differs from 20 ℃, oxygen volume fraction 5% in the flue gas, water vapour volume fraction 20%, NO is 400ppm, SO
2Be 800ppm, desulfuration efficiency 85%, denitration efficiency 60%.
Embodiment 2: adopt quick lime as absorbent, the average grain diameter d of absorbent
50Be 50 μ m, R
90Less than 10%, calcium sulphur nitrogen mol ratio Ca/ (S+0.5N) is 1.1, light a cigarette 150 ℃ of temperature degree of sorbent injection, oxygen volume fraction 3% in the flue gas, water vapour volume fraction 20%, temperature is 60 ℃ in the fluidized-bed reactor, be higher than dew-point temperature and differ from 15 ℃, NO is 400ppm, SO
2Be 800ppm, desulfuration efficiency 80%, denitration efficiency 50%.
Embodiment 3: adopt quick lime as absorbent, average grain particle diameter d
50Be 20 μ m, R
90Less than 10%, calcium sulphur nitrogen mol ratio (Ca/ (S+0.5N)) is 2.5, light a cigarette 120 ℃ of temperature degree of sorbent injection, oxygen volume fraction 8% in the flue gas, water vapour volume fraction 30%, temperature is 70 ℃ in the fluidized-bed reactor, be higher than dew-point temperature and differ from 15 ℃, NO is 400ppm, SO
2Be 800ppm, desulfuration efficiency 95%, denitration efficiency 75%.
Embodiment 4: adopt white lime as absorbent, average grain particle diameter d
50Be 80 μ m, R
90Less than 20%, calcium sulphur nitrogen mol ratio (Ca/ (S+0.5N)) is 1.2, light a cigarette 100 ℃ of temperature degree of sorbent injection, oxygen volume fraction 3% in the flue gas, water vapour volume fraction 5%, temperature is 90 ℃ in the fluidized-bed reactor, be higher than dew-point temperature and differ from 25 ℃, NO is 400ppm, SO
2Be 800ppm, desulfuration efficiency 70%, denitration efficiency 45%.
Claims (6)
1. a method that removes flue gas sulphur oxide and nitrogen oxide simultaneously is characterized in that this method comprises the steps:
1) enters in the fluidized-bed reactor by flue from the flue gas in the combustion apparatus, before flue gas enters fluidized-bed reactor, water or water vapour are sprayed into the flue gas flue, contain O in the flue gas in the flue
2, H
2O, SO
2With the NOx gas componant, and the control flue-gas temperature is in 90 ℃～200 ℃ scopes; Then with fresh absorbent CaO and Ca (OH)
2In one or both be directly injected in the flue, participate in earlier the oxidizing process of NO in the flue gas, control calcium sulphur nitrogen mol ratio Ca/ (S+0.5N) realizes the desulfurization and the denitration function of part between 1.0～2.5;
2) flue gas carries out desulphurization denitration in fluidized-bed reactor, and by spraying water in fluidized-bed reactor, the temperature of control fluidized-bed reactor is between 50 ℃～90 ℃, and fluidized-bed reactor moves under the temperature conditions that is higher than 5 ℃～25 ℃ of dew points;
3) flue gas behind the desulphurization denitration enters separator by pipeline, a separated solid particle part of getting off is returned fluidized-bed reactor or is sprayed into flue and enters fluidized-bed reactor with flue gas again in the separator, another part is discharged from system, to keep the material balance of whole system; Discharge from the flue pipeline through the flue gas that purifies.
2. according to the described a kind of method that removes flue gas sulphur oxide and nitrogen oxide simultaneously of claim 1, it is characterized in that: absorbent sprays into the volume fraction of steam in the flue gas between 5～25%, O
2Volume fraction between 1～15%.
3. according to claim 1 or 2 described a kind of methods that remove flue gas sulphur oxide and nitrogen oxide simultaneously, it is characterized in that: the flue-gas temperature in the described flue is controlled between 100～150 ℃.
4. according to the described a kind of method that removes flue gas sulphur oxide and nitrogen oxide simultaneously of claim 3, it is characterized in that: the average grain diameter d of absorbent
50Be 2 μ m～100 μ m, R
200Less than 10%.
5. according to the described a kind of method that removes flue gas sulphur oxide and nitrogen oxide simultaneously of claim 1, it is characterized in that: gas flow rate is controlled to be 3m/s～10m/s in fluidized-bed reactor, and the average content of particle is controlled to be 1kg/m
3～10kg/m
3
6. according to the described a kind of method that removes flue gas sulphur oxide and nitrogen oxide simultaneously of claim 1, it is characterized in that: described separator adopts inertia separator, electric cleaner or sack cleaner.
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| CN102512921A (en) * | 2011-12-06 | 2012-06-27 | 清华大学 | Method and system for integrated removal of a plurality of flue gas pollutants in circulating fluidized bed |
| CN102836634B (en) * | 2012-09-11 | 2015-01-14 | 北京世能中晶能源科技有限公司 | Desulfurization denitration method |
| CN102836636B (en) * | 2012-09-11 | 2015-01-14 | 北京世能中晶能源科技有限公司 | Desulfurization denitration composition, preparation method and application thereof |
| CN105056749A (en) * | 2015-07-20 | 2015-11-18 | 清华大学 | System and method for removing nitric oxides and sulfur oxides in flue gas simultaneously |
| CN113117492A (en) * | 2019-12-31 | 2021-07-16 | 中晶环境科技股份有限公司 | Semi-dry integrated process for flue gas desulfurization and denitrification |
| CN113559693A (en) * | 2020-04-29 | 2021-10-29 | 国家电投集团远达环保工程有限公司重庆科技分公司 | Apparatus and method for removing pollutants from flue gas flowing through flue |
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