CN101306308A - Method for synchronously treating the combined pollution exhaust gas containing nitric oxide and sulfur dioxide - Google Patents
Method for synchronously treating the combined pollution exhaust gas containing nitric oxide and sulfur dioxide Download PDFInfo
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- CN101306308A CN101306308A CNA2008100329390A CN200810032939A CN101306308A CN 101306308 A CN101306308 A CN 101306308A CN A2008100329390 A CNA2008100329390 A CN A2008100329390A CN 200810032939 A CN200810032939 A CN 200810032939A CN 101306308 A CN101306308 A CN 101306308A
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Abstract
The invention relates to a method for simultaneous treatment of mixed pollutant exhaust gas containing NOx and SO2. Absorption liquid of ferrous salt, ethylenediaminetetraacetic acid disodium and a desulphurization agent and waste gas containing SO2 and NO are introduced into a conventional reactor to carry out the reaction, thereby realizing the simultaneous absorption of NO and SO2. The absorption liquid after the reaction can be introduced in a liquid-solid reactor which takes activated carbon as a catalyst for regeneration. The method is a low-cost wet desulphurization and denitrification technique with market competitiveness.
Description
Technical field
The present invention relates to a kind of improvement simultaneously and contain NO
XAnd SO
2The method of mixed pollutants waste gas especially relates to NO and SO in the power-plant flue gas
2The time removal methods.
Background technology
The pollution of acid rain and the harm that causes thereof have become one of environmental problem of paying close attention to countries in the world.SO
2And NO
XBeing two kinds of dusty gas that discharge capacity is maximum, harmfulness is maximum, also is the main matter that forms acid rain.With the coal country of main energy sources, the SO that coal combustion produces
2(1000~4000ppm) and NO
X(300~800ppm), be that industrial waste gas pollutes the main root of (acid rain harm).
NO
XBe the general designation of nitrogen oxide, comprise N
2O, NO, N
2O
3, NO
2, N
2O
5Deng.NO
XHarmfulness be that not only it is an acid rain gas, and NO is the same with fluorochlorohydrocarbon can significantly damage the ozone layer NO and N
2O also is greenhouse gases simultaneously, and NO energy and hydrocarbon react in the sun and cause photochemical pollution.
NO in the atmosphere more than 95%
XBe NO, NO
2Only account for seldom amount, the NO in the flue gas
XAlso NO more than 90%.Because the NO respond is relatively poor, is insoluble in water again, therefore, it removes also just quite difficult technically.Developed multiple method of denitration through years of researches.What at present, industrial employing was more is catalytic reduction method.As patent USP:4,221,768, Swedish Patent 8404840-4, USP:4,101,238, US:4,048,112 disclosed method, but the reaction of this method needs to consume a large amount of reducing agents, and the nitrogen in the flue gas can not recycle, and causes the valuable wasting of resources.
Japan Patent P1659565j (1976), P181759c (1976), P63100918, A2 (1988) remove NO when proposing
XAnd SO
2Oxidant that method adopts, as chloric acid, potassium permanganate, hydrogen peroxide, ozone etc., liquid phase oxidation NO
XDeng because cost height etc. is former thereby fail to promote and come.The yellow phosphorus method that California, USA university Berkeley laboratory proposes (is seen document Nature, 1990,343 (11): 151-153), can remove the NO in the flue gas simultaneously
XAnd SO
2, but belong to the method for abandoning entirely.This method will consume a large amount of phosphor resources, and its toxicity is big, and operation is had relatively high expectations.
The early 1970s people propose to adopt Fe (II)-EDTA (EDTA represents disodium ethylene diamine tetraacetate) to remove NO in the waste gas, and the reaction equation of Fe (II)-EDTA and NO is as follows:
In nearly three ten years afterwards, many scholars have carried out comparatively systematic research to this reaction, but do not see the industrialization report at present yet, main cause is that (document sees reference: Bull.of theChem.Soc.of Jpn. because Fe (II)-EDTA easily is oxidized to Fe (III)-EDTA, 1968,41:2234-2239.Ind.Eng.Chem.Res., 1987,26:1468-1472.Inorg.Chem., 1990,29:1705-1711.Ind.Eng.Chem.Res., 1993,32:2580-2594.), and Fe (III)-EDTA can not complexing NO, and absorption efficiency is descended rapidly.People propose to regenerate with the living things catalysis reducing process, and (Fe (II) sees reference document: UnitedStates Patent US5891408.Biotechnol.Prog., 2003,19:1323-1328.J Chem Technol Biotechnol, 2004,79:835-841.Biotechnology and Bio engineering, 2005,90:433-441.Environ Sci Technol, 2005,39:2616-2623.J of Chem Technol and Biotechnol, 2006,81:306-311.), but this method just is in the exploratory stage at present, obtain large-scale application and also have many problems to need to solve in the waste gas pollution control and treatment process.
Summary of the invention
The objective of the invention is to propose a kind of improvement simultaneously and contain NO
XAnd SO
2The method of mixed pollutants waste gas.
The technical issues that need to address of the present invention provide and a kind ofly remove NO and SO in the waste gas with Fe (II)-EDTA solution
2Method, make NO and SO
2Absorption carry out simultaneously, overcoming the above-mentioned defective that prior art exists, reduce the treatment cost of wet desulphurization denitration, improve the market competitiveness of wet desulphurization denitration technology.
Design of the present invention is such:
Utilization contains the absorption liquid while absorption of N O and the SO of Fe (II)-EDTA and desulfurizing agent composition
2, the Fe (III) that Fe (II)-EDTA oxidation generates-EDTA employing active carbon is made catalyst and is come catalytic reduction to be regenerated as Fe (II)-EDTA, and the basic principle of Fe (II)-EDTA catalytic regeneration is as follows:
Because of impelling Fe (III)-EDTA, acidic-groups such as the carbonyl on the activated carbon, carboxyl, phenolic group dissociate into Fe (III) and EDTA (reaction (2)):
Fe (III) has stronger oxidability, and the pi-electron structure of activated carbon had both had the ability of transmitting electronics, can become the center of Fe (III) ion reduction, SO
2Be dissolved in the inferior sulfate radical that produces in the absorbent solution as reducing agent, Fe (III) reducing/regenerating is become Fe (II) (reaction (3)), inferior sulfate radical is oxidized to sulfate radical.
Fe (II) combines with EDTA in solution again and generates Fe (II)-EDTA (reaction (4)), and absorbent is regenerated, and the ability that absorption liquid removes NO can keep for a long time.
Fe(II)+EDTA→Fe(II)-EDTA (4)
Method of the present invention realizes by the while desulfurization and denitrification reaction: in the reactor of routine, ferrous salt, disodium ethylene diamine tetraacetate (EDTA) and desulfurizing agent be dissolved in be used as absorption liquid in the aqueous solution, will contain NO and SO
2Waste gas feed, realize NO and SO
2Carry out when absorbing.
Described desulfurizing agent is bivalent metal oxide, oxyhydroxide or carbonate etc., can be calcium oxide (lime), magnesia, Mg (OH)
2Or calcium carbonate (lime stone) etc.
The NO concentration range is in the described waste gas: 100~1000ppm; SO
2Concentration range be 500~3000ppm.
Usually can contain oxygen, O in the waste gas
2Concentration be 0~20%.
Operating pressure is a normal pressure, and temperature range is: 10~90 ℃, optimum value is: 30~60 ℃.
The pH scope of solution is generally: 1~9, and optimum value is: 4~7.
The concentration range of ferrous salt is: 0.005~0.1mol l
-1, be preferably 0.02~0.06mol l
-1
The concentration range of EDTA is: 0.01~0.2mol l
-1, be preferably 0.04~0.15mol l
-1
The concentration of desulfurizing agent is 0~0.3mol l
-1Be preferably 0.005~0.3mol l
-1For example the concentration range of calcium oxide is: 0.005~0.3mol l
-1, be recommended as 0.01~0.1mol l
-1Magnesian concentration range is: 0.005~0.3mol l
-1, be recommended as 0.01~0.1mol l
-1The concentration range of calcium carbonate is: 0.005~0.3mol l
-1, be recommended as 0.01~0.1mol l
-1
Common gas liquid ratio (volume flow ratio, M
3) be 10~300: 1, recommending gas liquid ratio is 200: 1.
Ferrous salt can be chosen any one kind of them from ferrous sulfate commonly used, frerrous chloride, ferrous nitrate, and preferably sulfuric acid is ferrous.
The present invention is to NO
XAnd SO
2The reactor of Xi Shouing does not have special requirement simultaneously, NO
XAnd SO
2Remove and can in common gas-liquid reactor such as packed tower, plate column or bubble tower etc., carry out.
Reaction solution in the inventive method can be regenerated: above-mentioned reacted solution is fed to make in the reactor of catalyst of activated carbon regenerate, this reactor is liquid-solid reactor commonly used, as fixed bed, slurry bed etc., activated carbon can be cocos active carbon commonly used, wood chip activated carbon, ature of coal activated carbon etc., regeneration temperature is 20~90 ℃, optimum temperature is 50~80 ℃, and regeneration pH is 1~9, and best pH is 3~7.Reaction solution can continue to use after the regeneration.
In other words, method of the present invention can be carried out so continuously: above-mentioned absorption liquid imports from the top or the upper lateral part of reactor, and contains NO
XAnd SO
2Waste gas from the bottom of reactor or the following side import and continue reaction, the gas that reacts later is said from the top or the upper lateral part of reactor continuously, and absorption liquid flows out from the bottom or the following side of reactor on the contrary, and importing contains in the liquid-solid reactor of activated carbon continuation use behind the process activating and regenerating.
The present invention makees absorbent by adopting Fe-EDTA solution, and activated carbon is made catalyst, sulphite is done the method that reducing agent regeneration NO absorbs active component Fe (II)-EDTA, realizes recycling of NO absorbent, realizes NO and SO
2Remove simultaneously and carry out, the cost that nitrogen oxide and sulfur dioxide are administered simultaneously descends greatly.
Description of drawings
Fig. 1 is a kind of flow chart of the present invention.
Symbol description.
In the accompanying drawing: the 1-reactor, the 2-liquid-solid reactor, the 3-absorption liquid, 4-contains NO
XAnd SO
2Waste gas, 5-activated carbon, 6-circulating slot.
The specific embodiment
The present invention is further elaborated below in conjunction with embodiment, but can not limit of the present invention in.
Absorption experiment is carried out in the packed tower of diameter 2cm, high 100cm, the gas-liquid two-phase adverse current, and empty tower gas velocity is 0.1m/s, liquid spraying density is 5m
3/ m
2.hr, absorption liquid 500ml.
Wherein: ferrous sulfate concentration is 0.02mol l
-1, EDTA concentration is 0.04mol l
-1, the pH value is 6,
Gas flow is 200ml/minute, and temperature is 50 ℃;
Gas feed consists of NO:480ppm, SO
2: 1500ppm, O
2: 5.2%, all the other are nitrogen.
Absorption liquid enters packed tower absorption of N O and SO by cat head
2In tower bottom flow is gone into circulating slot, enter the fixed bed reactors that high 50cm, diameter 2cm be equipped with cocos active carbon from circulating slot again and carry out catalyst regeneration, reaction temperature is that 80 ℃, the liquid speed with 25ml min-1 in regenerator flows from lower to upper, and the absorption liquid that leaves regenerator directly enters absorption of N O and SO in the packed tower
2Gas vent concentration is carried out on-line analysis by infrared spectrometer, per two minutes automatically sampling once reach when stablizing in operation, gas vent concentration is NO:30ppm, SO
2: 150ppm.The flow chart of logistics as shown in Figure 1.
Embodiment 2
Reactor and operating condition be with embodiment 1, but also have 0.03mol l in the absorption liquid
-1Calcium oxide, reach when stablizing in operation, gas vent concentration is NO:30ppm, SO
2: 40ppm.
Reactor and operating condition be with embodiment 1, but also have 0.03mol l in the absorption liquid
-1Magnesia, reach when stablizing in operation, gas vent concentration is NO:30ppm, SO
2: 40ppm.
Reactor and operating condition be with embodiment 1, but also have 0.03mol l in the absorption liquid
-1Lime stone, reach when stablizing in operation, gas vent concentration is NO:30ppm, SO
2: 40ppm.
Claims (9)
1. one kind removes SO in the waste gas simultaneously with Fe-EDTA solution
2With the method for NO, it is characterized in that in the reactor of routine, when normal pressure and 10~90 ℃, feed absorption liquid and contain SO
2React the volume flow ratio M of gas-liquid with the waste gas of NO
3Be 10~300: 1;
Described absorption liquid is the aqueous solution of pH1~9 of containing ferrous salt, disodium ethylene diamine tetraacetate and desulfurizing agent; Wherein, the concentration range of ferrous salt is 0.005~0.1mol l
-1The disodium ethylene diamine tetraacetate concentration range is 0.01~0.2mol l
-1The concentration of desulfurizing agent is 0~0.3mol l
-1
Described desulfurizing agent is bivalent metal oxide, oxyhydroxide or carbonate.
2. the method for claim 1 is characterized in that described temperature range is 30~60 ℃; Gas-liquid volume flow M
3It is 200: 1.
3. the method for claim 1 is characterized in that the NO concentration range is 100~1000ppm in the described waste gas; SO
2Concentration range be 500~3000ppm; Containing concentration of oxygen in the waste gas is 0~20%.
4. the method for claim 1 is characterized in that the pH scope of described absorption liquid is: 4~7.
5 the method for claim 1, the concentration that it is characterized in that described molysite is 0.02~0.06mol l
-1The concentration of described disodium ethylene diamine tetraacetate is 0.04~0.15mol l
-1The concentration of described desulfurizing agent is 0.005~0.3mol l
-1
6. the method for claim 1 is characterized in that described bivalent metal oxide is calcium oxide, magnesia or calcium carbonate; The concentration range of described calcium oxide is 0.005~0.3mol l
-1Described magnesian concentration range is 0.005~0.3moll
-1The concentration range of described calcium carbonate is 0.005~0.3mol l
-1
7. the method for claim 1 is characterized in that described ferrous salt is ferrous sulfate, frerrous chloride or ferrous nitrate.
8. the method for claim 1 is characterized in that described reaction back absorption liquid is to feed in the liquid-solid reactor of making catalyst of activated carbon to regenerate at 20~90 ℃ and pH at 1~9 o'clock.
9. the method for claim 1 is characterized in that described activated carbon is cocos active carbon, wood chip activated carbon or the ature of coal activated carbon of using always etc., and regeneration temperature is 50~80 ℃; PH is 3~7.
10. as claim 1 and 8 described methods, it is characterized in that describedly importing in the liquid-solid reactor as claimed in claim 8 at the absorption liquid that from the reactor of routine, flows out.
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CN101785965A (en) * | 2010-03-02 | 2010-07-28 | 浙江菲达环保科技股份有限公司 | Complex absorption cycle semi-dry desulfurization and denitrification integral process and device |
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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 |
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CN105536493A (en) * | 2015-12-28 | 2016-05-04 | 昆明理工大学 | Method for removing SO2 and NOX from flue gas of coal-fired boiler by virtue of phosphoric ore pulp and phosphorus sludge |
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CN115738599A (en) * | 2022-11-23 | 2023-03-07 | 攀钢集团攀枝花钢铁研究院有限公司 | Simultaneous absorption of NO x And preparation method of CO complexing denitration liquid |
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CN104084025A (en) * | 2014-07-17 | 2014-10-08 | 湖南平安环保有限责任公司 | Method for removing nitric oxides from boiler smoke |
CN105536493B (en) * | 2015-12-28 | 2018-04-06 | 昆明理工大学 | One kind utilizes SO in phosphate ore pulp and mud phosphorus removing fire coal boiler fume2And NOXMethod |
CN105536493A (en) * | 2015-12-28 | 2016-05-04 | 昆明理工大学 | Method for removing SO2 and NOX from flue gas of coal-fired boiler by virtue of phosphoric ore pulp and phosphorus sludge |
CN106621808A (en) * | 2017-01-03 | 2017-05-10 | 北京清新环境技术股份有限公司 | Wet type integrated purification system and method for recovery of residual heat in flue gas |
CN107308783A (en) * | 2017-08-31 | 2017-11-03 | 山东瑞嘉通风环保科技有限公司 | A kind of simultaneous desulfuration and denitration technique by wet flue gas method |
CN109825338A (en) * | 2019-01-30 | 2019-05-31 | 维珂瑞(北京)环境科技有限公司 | H in a kind of removal biogas2The LO-CAT system of S |
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CN110124451B (en) * | 2019-05-13 | 2021-11-05 | 上海大学 | Wet-type step-by-step SO removal in flue gas2And NO process |
CN114432869A (en) * | 2020-10-31 | 2022-05-06 | 中国石油化工股份有限公司 | Coal-fired flue gas treatment method and device |
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CN115738599A (en) * | 2022-11-23 | 2023-03-07 | 攀钢集团攀枝花钢铁研究院有限公司 | Simultaneous absorption of NO x And preparation method of CO complexing denitration liquid |
CN115738599B (en) * | 2022-11-23 | 2024-06-04 | 攀钢集团攀枝花钢铁研究院有限公司 | At the same time absorb NOxPreparation method of complexing denitration liquid of CO |
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