CN103203176A - Method for flue gas desulfurization, denitrification and demercuration by semidry method - Google Patents

Method for flue gas desulfurization, denitrification and demercuration by semidry method Download PDF

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Publication number
CN103203176A
CN103203176A CN2013101355016A CN201310135501A CN103203176A CN 103203176 A CN103203176 A CN 103203176A CN 2013101355016 A CN2013101355016 A CN 2013101355016A CN 201310135501 A CN201310135501 A CN 201310135501A CN 103203176 A CN103203176 A CN 103203176A
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China
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flue gas
demercuration
composite oxidant
additive
semi
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CN2013101355016A
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Chinese (zh)
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CN103203176B (en
Inventor
王涵
赵毅
郝润龙
郝思琪
王莉
郭青
杜磊霞
崔帅
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华北电力大学(保定)
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    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02ATECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
    • Y02A50/00TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
    • Y02A50/20Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters

Abstract

The invention discloses a method for flue gas desulfurization, denitrification and demercuration by a semidry method, belonging to the technical field of flue gas purification. The method comprises the following steps of: (1) spraying a composite oxidant from the bottom of a circulating fluidized bed to oxidize NO and HgO, wherein the composite oxidant is an aqueous solution containing hydrogen peroxide, an additive and a stabilizer; the additive is one or more of sodium perborate, sodium persulfate and potassium pyrosulfate; and the stabilizer is one of hydrochloric acid, sulfuric acid and perchloric acid; and (2) absorbing and removing an oxidative product and SO2 by using a calcium-based sorbent. According to the method, the composite oxidant is firstly used for oxidizing NO and HgO in flue gas, and then SO2, NO and HgO are simultaneously removed to realize integration of desulfurization, denitrification and demercuration, thus the removal rate is greatly improved, the cost is greatly reduced, and the method has high economic and environmental benefits.

Description

The method of semi-dry process flue gas desulphurization denitration demercuration
Technical field
The present invention relates to the flue gases purification field.
Background technology
SO in the coal-fired flue-gas 2, NO and Hg 0Life and health and ecological sustainable development to the mankind have brought serious threat.SO 2Be the main cause that produces acid rain, NO is the principal element of bringing out photochemical fog, greenhouse effects and depletion of the ozone layer, and by SO 2The aerosol that forms with NOx is to form China's major reason of haze weather on a large scale.Hg 0Have strong toxicity, volatile, difficult degradation, the aerial holdup time is long and the characteristics of long-distance migration, it has grievous injury to the human nervous system, is one of the most serious heavy metal pollution.Mercury content is higher in the used coal of China's thermoelectricity industry, and therefore, China is extremely urgent to the control of mercury in the coal-fired flue-gas.
Wet desulfurization system is to control SO at present 2Comparatively effective way, but there are shortcomings such as the big and secondary wastewater processing of floor space in it.Control to NOx then mainly utilizes SCR (SCR) denitrating system, after it is arranged in economizer.NH under the effect of catalyst 3Carry out reduction reaction with NOx, NOx is reduced to N 2And water.SCR has the high advantage of denitration efficiency, but has shortcomings such as operating cost height, ammonia leakage, catalyst poisoning and generation solid waste simultaneously.The form that exists of mercury mainly contains three kinds in the coal-fired flue-gas: simple substance attitude mercury (Hg 0), oxidation state mercury (Hg 2+) and particle mercury (Hg p).External is active carbon injection technique (ACI) than ripe demercuration technology at present, but because active carbon is on the high side, has increased operating cost greatly, and discarded active carbon needs further the disposal.The collaborative demercuration technology of existing pollutant control appliance is present comparatively feasible way, as wet desulfurization system oxidation state mercury had removal effect preferably, electric cleaner or sack cleaner have very high capture rate to particle mercury, but above-mentioned two kinds of equipment almost do not have removal effect to simple substance mercury.
Because NO and Hg 0Dissolving hardly in the aqueous solution, and be gaseous state.Therefore, be difficult to be removed by wet desulfurization system and cleaner.And NO is about the 90-95% of NOx, Hg in the coal-fired flue-gas 0How the 30-80% that is about total mercury is with NO and Hg 0Be converted into NO 2And Hg 2+Then being absorbed in desulphurization system, is to realize the two and SO 2The key that removes simultaneously.
Summary of the invention
The invention provides a kind of method of semi-dry process flue gas desulphurization denitration demercuration, this method utilizes composite oxidant at first to the NO in the flue gas and Hg 0Carry out oxidation, realize SO then 2, NO and Hg 0Remove simultaneously, realize that desulfurization denitration demercuration is integrated, not only improved removal efficiency greatly, and greatly reduced cost, have higher economy and environmental benefit.
The technical solution used in the present invention is:
A kind of method of semi-dry process flue gas desulphurization denitration demercuration, it comprises:
(1) composite oxidant is sprayed into from the recirculating fluidized bed bottom, to NO and Hg 0Carry out oxidation; Described composite oxidant is the aqueous solution that comprises hydrogen peroxide, additive and stabilizing agent; Described additive is one or more in sodium perborate, sodium peroxydisulfate, the potassium pyrosulfate, and described stabilizing agent is a kind of in hydrochloric acid, sulfuric acid and the perchloric acid.
(2) with calcium-base absorbing agent to oxidation product and SO 2Absorb and remove.
Preferably, the concentration of primary oxidant is 3-5 mol/L in the composite oxidant, and the concentration of additive is 0.1-2 mol/L, and the concentration of stabilizing agent is 0.0001-0.005 mol/L;
The pH value of composite oxidant is 0.5-2;
Temperature in the recirculating fluidized bed is 60-120 ℃;
The flow velocity of flue gas is 1-5 L/min;
The speed of spraying into of composite oxidant is 0.5-2.0 ml/min.
This composite oxidant preparation process is: measure 3-5 mol hydrogen peroxide, 0.1-2 mol additive and 0.0001-0.005 mol stabilizing agent, additive and stabilizing agent are added in the aqueous hydrogen peroxide solution, concussion shakes up, and is diluted with water to 1L then.This composite oxidant has stronger stability, under the lucifuge condition of 24-48h, can keep higher oxidability, and the composite oxidant after the placement is to NO and Hg 0Removal efficient can reach 88% and 85%.
Technical process of the present invention is: composite oxidant sprayed into from the recirculating fluidized bed bottom, it fully mixed with flue gas, and to NO and Hg 0Carry out oxidation, the subsequent section oxidant is subjected to thermal evaporation, react with liquid and gas dual mode and gaseous contaminant, then with calcium-base absorbing agent to oxidation product and SO 2Absorb fixing.
The present invention is applicable to the polytype boiler, and can realize removing simultaneously to multiple flue gas pollutant, so this invention has good benefits in environment and economic benefit, has broad application prospects.
Hydrogen peroxide, hydroxyl radical free radical, over cure acid group, perboric acid root are the core oxides of this composite oxidant, NO, Hg in its main and flue gas 0Carry out oxidation reaction.The over cure acid group then can generate the sulfate radical free radical with hydrogen peroxide, perboric acid root and H 2Chain reaction takes place in O in course of reaction, product is hydrogen peroxide, and the generation of hydrogen peroxide can promote the generation of hydroxyl radical free radical, and the adding of stabilizing agent inorganic acid can slow down the quick decomposition of hydrogen peroxide, and promotes the generation of chain reaction.
The mechanism of action of the present invention is to utilize composite oxidant with the Hg in the flue gas 0Be oxidized to divalence mercury, NO is oxidized to NO 2, its oxidation product and SO 2Absorbed by calcium-base absorbing agent.
The concrete mechanism of action is as follows:
Adopt composite oxidant of the present invention that flue gas is carried out the desulfuration demercuration denitration and handle, treatment effect is as shown in table 1:
Table 1 desulfuration demercuration denitration effect
Project Before the processing After the processing Removal efficiency
Hg 0Concentration 40 3.7 90.8%
NO concentration 500ppm 42ppm 91.6%
SO 2Concentration 2000ppm 0ppm 100%
The time of staying of flue gas, between second, absorbing fully, the pH value of back absorption liquid was 8-10 at 3-4.
Method of the present invention can have higher removal efficiency fast with the pollutant oxidation, and desulfuration efficiency can reach 100%, and denitration and demercuration efficient can reach more than 90%.
The beneficial effect that adopts technique scheme to produce is:
1, the inventive method uniqueness utilizes composite oxidant at first to the NO in the flue gas and Hg 0Carry out oxidation, realize SO then 2, NO and Hg 0Remove simultaneously, thereby realize that desulfurization denitration demercuration is integrated, greatly reduce cost and improved removal efficiency.Thereby solved that the people that exist for a long time want to solve always and a unsolved difficult problem always.Have higher economy and environmental benefit.
2, because can be fast with the pollutant oxidation, so have higher removal efficiency.As long as operation suitably, desulfuration efficiency can reach 100%, and denitration and demercuration efficient can reach more than 90%.
The specific embodiment
Embodiment 1
The configuration composite oxidant: measure 3 mol hydrogen peroxide, 1 mol sodium perborate, 0.5 mol potassium pyrosulfate and 0.0001 mol hydrochloric acid, additive and stabilizing agent are added in the aqueous hydrogen peroxide solution, concussion shakes up, and is diluted with water to 1L then.
Above-mentioned composite oxidant is sprayed into from the recirculating fluidized bed bottom, to NO and Hg 0Carry out oxidation, then with calcium-base absorbing agent to oxidation product and SO 2Absorb fixingly, reaction condition sees Table 2.
Table 2 recirculating fluidized bed reaction condition
Condition Scope
Reaction temperature 120℃
Oxidant sample introduction speed 0.5ml/min
The flue gas intake velocity 3L/min
Composite oxidant pH value 0.5-2
By above-mentioned condition flue gas is carried out the desulfuration demercuration denitration and handle, detection obtains: SO 2Removal efficiency be 100%, denitration efficiency is 91.7%, demercuration efficient is more than 90.8%.
Embodiment 2
The configuration composite oxidant: measure 5 mol hydrogen peroxide, 1mol sodium perborate, 0.5mol sodium peroxydisulfate, 0.5mol potassium pyrosulfate and 0.005 mol sulfuric acid, additive and stabilizing agent are added in the aqueous hydrogen peroxide solution, concussion shakes up, and is diluted with water to 1L then.
Above-mentioned composite oxidant is sprayed into from the recirculating fluidized bed bottom, to NO and Hg 0Carry out oxidation, then with calcium-base absorbing agent to oxidation product and SO 2Absorb fixingly, reaction condition sees Table 3.
Table 3 recirculating fluidized bed reaction condition
Condition Scope
Reaction temperature 90℃
Oxidant sample introduction speed 1.0 ml/min
The flue gas intake velocity 4 L/min
Composite oxidant pH value 0.5-2
By above-mentioned condition flue gas is carried out the desulfuration demercuration denitration and handle, detection obtains: SO 2Removal efficiency be 100%, denitration efficiency is 93.0%, demercuration efficient is more than 91.2%.
Embodiment 3
The configuration composite oxidant: measure 4 mol hydrogen peroxide, 0.5mol sodium peroxydisulfate, 0.5mol potassium pyrosulfate and 0.001 mol perchloric acid, additive and stabilizing agent are added in the aqueous hydrogen peroxide solution, concussion shakes up, and is diluted with water to 1L then.
Above-mentioned composite oxidant is sprayed into from the recirculating fluidized bed bottom, to NO and Hg 0Carry out oxidation, then with calcium-base absorbing agent to oxidation product and SO 2Absorb fixingly, reaction condition sees Table 4.
Table 4 recirculating fluidized bed reaction condition
Condition Scope
Reaction temperature 100℃
Oxidant sample introduction speed 1.5 ml/min
The flue gas intake velocity 5 L/min
Composite oxidant pH value 0.5-2
By above-mentioned condition flue gas is carried out the desulfuration demercuration denitration and handle, detection obtains: SO 2Removal efficiency be 100%, denitration efficiency is 92.3%, demercuration efficient is more than 90.6%.
Embodiment 4
The configuration composite oxidant: measure 3.5mol hydrogen peroxide, 0.5 mol potassium pyrosulfate and 0.003 mol sulfuric acid, additive and stabilizing agent are added in the aqueous hydrogen peroxide solution, concussion shakes up, and is diluted with water to 1L then.
Above-mentioned composite oxidant is sprayed into from the recirculating fluidized bed bottom, to NO and Hg 0Carry out oxidation, then with calcium-base absorbing agent to oxidation product and SO 2Absorb fixingly, reaction condition sees Table 5.
Table 5 recirculating fluidized bed reaction condition
Condition Scope
Reaction temperature 80℃
Oxidant sample introduction speed 2.0 ml/min
The flue gas intake velocity 1 L/min
Composite oxidant pH value 0.5-2
By above-mentioned condition flue gas is carried out the desulfuration demercuration denitration and handle, detection obtains: SO 2Removal efficiency be 100%, denitration efficiency is 92.8%, demercuration efficient is more than 91.1%.
Embodiment 5
The configuration composite oxidant: measure 4.5mol hydrogen peroxide, 0.1 mol sodium peroxydisulfate and 0.004mol hydrochloric acid, additive and stabilizing agent are added in the aqueous hydrogen peroxide solution, concussion shakes up, and is diluted with water to 1L then.
Above-mentioned composite oxidant is sprayed into from the recirculating fluidized bed bottom, to NO and Hg 0Carry out oxidation, then with calcium-base absorbing agent to oxidation product and SO 2Absorb fixingly, reaction condition sees Table 6.
Table 6 recirculating fluidized bed reaction condition
Condition Scope
Reaction temperature 60℃
Oxidant sample introduction speed 0.9 ml/min
The flue gas intake velocity 2 L/min
Composite oxidant pH value 0.5-2
By above-mentioned condition flue gas is carried out the desulfuration demercuration denitration and handle, detection obtains: SO 2Removal efficiency be 100%, denitration efficiency is 91.4%, demercuration efficient is more than 91.3%.

Claims (6)

1. the method for a semi-dry process flue gas desulphurization denitration demercuration is characterized in that comprising the steps:
(1) composite oxidant is sprayed into from the recirculating fluidized bed bottom, to NO and Hg 0Carry out oxidation; Described composite oxidant is the aqueous solution that comprises hydrogen peroxide, additive and stabilizing agent; Described additive is one or more in sodium perborate, sodium peroxydisulfate, the potassium pyrosulfate, and described stabilizing agent is a kind of in hydrochloric acid, sulfuric acid and the perchloric acid;
(2) with calcium-base absorbing agent to oxidation product and SO 2Absorb and remove.
2. the method for semi-dry process flue gas desulphurization denitration demercuration according to claim 1, the concentration that it is characterized in that hydrogen peroxide in the described composite oxidant is 3-5mol/L, the concentration of additive is 0.1-2 mol/L, and the concentration of stabilizing agent is 0.0001-0.005 mol/L.
3. the method for semi-dry process flue gas desulphurization denitration demercuration according to claim 1 is characterized in that the pH value of described composite oxidant is 0.5-2.
4. according to the method for claim 1,2 or 3 described semi-dry process flue gas desulphurization denitration demercurations, it is characterized in that the temperature in the described recirculating fluidized bed is 60-120 ℃.
5. the method for semi-dry process flue gas desulphurization denitration demercuration according to claim 4, the flow velocity that it is characterized in that described flue gas is 1-5 L/min.
6. the method for semi-dry process flue gas desulphurization denitration demercuration according to claim 5, the speed of spraying into that it is characterized in that described composite oxidant is 0.5-2.0 ml/min.
CN201310135501.6A 2013-04-18 2013-04-18 Method for flue gas desulfurization, denitrification and demercuration by semidry method CN103203176B (en)

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Cited By (5)

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Publication number Priority date Publication date Assignee Title
CN103691267A (en) * 2013-12-19 2014-04-02 海南中航特玻材料有限公司 Low-temperature synchronous denitration and desulfurization equipment and process for flue gas
CN105233687A (en) * 2015-10-21 2016-01-13 华北电力大学(保定) Method for removing elemental mercury in coal-fired flue gas
CN105903329A (en) * 2016-06-14 2016-08-31 东莞市联洲知识产权运营管理有限公司 Novel flue gas desulfurization and denitrification technology
CN106268293A (en) * 2015-05-14 2017-01-04 王立群 A kind of wet desulphurization denitration synergist for coal-burning boiler
CN109865415A (en) * 2019-04-08 2019-06-11 福建省特种设备检验研究院 CFB boiler, which is mixed, burns anthracite and sawdust sludge gas mercury oxidation control technique

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CN1962034A (en) * 2006-10-25 2007-05-16 华北电力大学 Method and apparatus for removing sulfur, nitrate and mercury simultaneously from boiler flue gas
CN101337153A (en) * 2008-08-12 2009-01-07 东南大学 Ultrasonic integration desulfurization denitration demercuration method and device thereof

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JP2002361034A (en) * 2001-06-01 2002-12-17 Japan Science & Technology Corp Oxidation treatment method and equipment for so2 in waste gas of making ho2 radical into oh forming reaction species in radical chain reaction of so2 oxidation
CN1950139A (en) * 2004-05-11 2007-04-18 国家航空和宇宙航行局 Method and apparatus utilising hydrogen peroxyde to reduce SOx, NOx and heavy metal emissions
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Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN103691267A (en) * 2013-12-19 2014-04-02 海南中航特玻材料有限公司 Low-temperature synchronous denitration and desulfurization equipment and process for flue gas
CN103691267B (en) * 2013-12-19 2016-09-07 海南中航特玻材料有限公司 A kind of flue gas low-temperature synchronizes denitration desulphurization plant and technique
CN106268293A (en) * 2015-05-14 2017-01-04 王立群 A kind of wet desulphurization denitration synergist for coal-burning boiler
CN105233687A (en) * 2015-10-21 2016-01-13 华北电力大学(保定) Method for removing elemental mercury in coal-fired flue gas
CN105233687B (en) * 2015-10-21 2018-01-02 华北电力大学(保定) A kind of method of elemental mercury in removing coal-fired flue-gas
CN105903329A (en) * 2016-06-14 2016-08-31 东莞市联洲知识产权运营管理有限公司 Novel flue gas desulfurization and denitrification technology
CN105903329B (en) * 2016-06-14 2018-06-29 广东万引科技发展有限公司 A kind of flue gas desulfurization and denitration technique
CN109865415A (en) * 2019-04-08 2019-06-11 福建省特种设备检验研究院 CFB boiler, which is mixed, burns anthracite and sawdust sludge gas mercury oxidation control technique

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