CN103432877A - Integrated method for wet-process dust removal, desulfurization, denitrification demercuration, dearsenification of complexing ferroporphyrin smoke based on supergravity - Google Patents

Integrated method for wet-process dust removal, desulfurization, denitrification demercuration, dearsenification of complexing ferroporphyrin smoke based on supergravity Download PDF

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CN103432877A
CN103432877A CN2013104036559A CN201310403655A CN103432877A CN 103432877 A CN103432877 A CN 103432877A CN 2013104036559 A CN2013104036559 A CN 2013104036559A CN 201310403655 A CN201310403655 A CN 201310403655A CN 103432877 A CN103432877 A CN 103432877A
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denitration
dust
hypergravity machine
sulfide
desulfurization
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CN103432877B (en
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余国贤
黄泽朔
潘威
李海峰
路平
吴宏观
隋志军
万昆
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余国贤
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Abstract

The invention discloses an integrated method for wet-process dust removal, desulfurization, denitrification demercuration and dearsenification of supergravity complexing ferroporphyrin smoke based on a wet method. The method provided by the invention comprises the following steps of firstly, absorbing SOx by utilizing inorganic sulfide, and meanwhile, trapping dust particles in smoke; reacting inorganic sulfide with poisonous heavy metals such as mercury and arsenic in the smoke to generate an insoluble vulcanized salt; absorbing NOx by utilizing complexing ferroporphyrin; and regenerating an absorber using inorganic sulfide as a reducer. The method provided by the invention has the advantages that a supergravity machine is adopted as gas-liquid mass transfer strengthening equipment, the dust extraction desulfurization and denitrification integrated method is beneficial to removal of toxicants such as SOx, NOx, mercury and arsenic, the process is simple, the absorption efficiency is high, the dust is thoroughly removed, the desulfurization degree is more than 99%, the denitration rate is more than 96%, and the dust, mercury and arsenic in the smoke are fully basically removed.

Description

The integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing

Technical field

The present invention relates to industrial flue gas cleaning, refer to particularly the integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of a kind of hypergravity complexing.

Background technology

The pollution of acid rain and the harm caused thereof have become one of important environmental problem of paying close attention to various countries, the whole world.The country that coal is main energy sources be take in China, statistics according to investigations, the SO of China more than 90% 2, the NO more than 67% x, the flue dust more than 70% discharge capacity all come from burning of coal.And the SO that coal combustion produces 2and NO xthat industrial waste gas pollutes the main source of (acid rain harm).Nitrogen oxide also can form photochemical pollution, produce greenhouse effects, damage the ozone layer, human body is had the harm such as toxic action processed.Nitrogen oxide and oxysulfide also can be converted into PM2.5 and cause haze weather.

The whole world mercury total amount that is discharged in atmosphere in every year has more than 5000 ton, wherein approximately 4000 tons be artificial result, and the mercury emission of coal-fired process accounts for more than 30%.In China's raw coal, the mercury content excursion is at 0.1~5.5mg/Kg, average mercury content 0.22mg/Kg.Because the yearly consumption of China's fire coal is huge, the amount of annual coal fire discharged mercury and pollutant thereof is all very surprising, the current mercury emission of China has surpassed the U.S., and growth rate is very fast, human health and ecological environment have been formed to grave danger, and the discharge capacity of therefore controlling Mercury In Coal Combustion Flue Gas is significant.During coal combustion, the mercury major part enters atmosphere with flue gas, and what enter lime-ash only accounts for fraction, wherein accounts for 23.1%~26.9% in flying dust, accounts for 56.3%~69.7% in flue gas, and the mercury that enters lime-ash only accounts for 2% left and right.Therefore controlling coal-fired mercury pollution key is that the mercury of controlling in flue gas discharges in atmosphere.Stronger oxidant SO in flue gas 2, NO 2, Cl 2deng the simple substance that can obviously affect mercury metal and oxide existence form.Along with the increase of oxidant, also increased the oxide components of mercury, as HgCl 2, HgSO 4deng.

Mercury In Coal Combustion Flue Gas belongs to the trace level pollutant, wherein mainly contains three kinds of forms: gaseous elemental mercury, gaseous oxidation mercury, solid granulates mercury.Wherein gaseous elemental mercury is the main existence form of mercury in flue gas.Mercury in flue gas have the removed material impact of form to mercury.Affect the principal element that there is form in mercury in flue gas coal-fired kind, ignition temperature, smoke components etc. are arranged.Physics, the chemical property of mercury species differ greatly.As soluble in water as gaseous oxidation mercury, and easily by the particle in flue gas, adsorbed, therefore easily by wet desulphurization equipment or cleaner, removed, particle mercury is also easily removed by deduster, contrary atomic state mercury volatility is high, water-soluble low, is difficult to be desulfurized or cleaner is caught, and almost all discharges into the atmosphere, and mean residence time reaches half a year to two year in atmosphere, very easily in atmosphere, the conveying by long distance forms mercury pollution widely.Atomic state mercury is form the most rambunctious, is also the difficult point of coal-fired flue gas mercury removal.

Dedusting refers to the separation operation process of the multiphase mixture of gas and dust particle.As the grit diameter of dedusting object, the general grit at 0.01~100 μ m.Grit more than 100 μ m is because sedimentation falls in Action of Gravity Field very soon; And the above grit of 10 μ m is easy to separate, problem is little; 0.1 the following grit of the grit of~10 μ m, particularly 1 μ m separates comparatively difficulty, also is harmful to human body, is current main research range.From the angle of environmental protection, dust is the formidable enemy of health.Especially the floating dust of particle diameter between 0.5~5 μ m (dust even floated in several years in atmosphere for a long time), to people's harm maximum.Be greater than the grit of 5 μ m, due to effect of inertia, can be got rid of by vibrissa and respiratory mucus, be less than the floating dust of 0.5 μ m, also can discharge with phlegm because the gas diffusion is adhered to upper respiratory tract surface.The floating dust of 0.5~5 μ m can directly arrive lung by respiratory tract and deposits only, harmful to human.

At present, what industrial employing was more is selective catalytic reduction, adopt ammonia or urea to make reducing agent NO is reduced to nitrogen, as patent US Patent4,221,768, Swedish Patent8404840-4, US Patent4,101,238, US Patent4,048,112 disclosed method.But said method need (350 ℃ of left and right) just can carry out under higher temperature, and the catalyst price is higher, easily poisoning and deactivation can not be realized desulphurization denitration simultaneously.Japan Patent P1659565j (1976), P181759c (1976), P63100918, A2 (1988) removes NO when proposing xand SO 2method adopt oxidant that NO is oxidized to NO soluble in water 2, as chloric acid, potassium permanganate, hydrogen peroxide, ozone etc., but liquid phase oxidation is former thereby fail to promote and come due to high in cost of production.The yellow phosphorus method that the Berkeley of California, USA university laboratory proposes (is shown in document Nature, 1990,343 (11): 151-153), can remove the NO in flue gas simultaneously xand SO 2, but belong to the method for entirely abandoning.This method will consume a large amount of phosphor resources, and its toxicity is large, and operation requirements is higher.

Adopt Fe (II)-EDTA (EDTA means disodium ethylene diamine tetraacetate) to remove NO in waste gas.The reaction equation of Fe (II) EDTA and NO is as follows:

Fe(II)EDTA+NO→Fe(II)EDTA(NO)????(1)

In nearly three ten years afterwards, many scholars have carried out comparatively systematic research to this reaction, but have not yet to see the industrialization report, and the greatest problem that affects the wet process complex denitration application is the cycle applications of absorption liquid.

The circulation regeneration method of absorption liquid mainly contains bioanalysis, improves the three major types such as absorbent absorbability and electrolysis, wherein to improve the absorbent absorbability, applies the most extensively.Fe (II) EDTA easily is oxidized to Fe (III) EDTA, and Fe (III) EDTA can not complexing NO, and absorption efficiency is descended rapidly.With the living things catalysis reducing process Fe (II) that regenerates, but this method will obtain large-scale application and also have many problems to need to solve at present just in the exploratory stage in the waste gas pollution control and treatment process.In the application of reducing agent, hydrazine and H 2s reduction Fe (III) EDTA, the assimilation effect of enhancing EDTA Fe, but due to H 2s and hydrazine are all poisonous, are difficult in industrial application.Someone adopts tannic acid, pyrogaelol and gallic acid to be the absorptive capacity that the second additive strengthens Fe (II) EDTA, NO in two hours xremoval efficiency remain on 60~65% always, effectively improved the reduction effect of poly-phenol mixture.Also someone has reported dithionic acid sodium reduction Fe (III) EDTA, and reduction effect is better.Domestic scholars has been reported reducing/regenerating Fe (III) EDTA such as iron filings, malic acid, vitamin C, but that the key issue of this technology is operating cost is high, and the process route complexity, also need further research.

Summary of the invention

Purpose of the present invention will overcome the existing deficiency of prior art exactly, provides the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of a kind of hypergravity complexing integrated method.

The integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing of the present invention comprises the following steps:

1) by temperature be 40 ℃~120 ℃ and send into the dust-removal and desulfurizing hypergravity machine containing SOx, NOx, mercury, arsenic flue gas, with be 0.01~4.0mol/L sulfide solution counter current contacting in dust-removal and desulfurizing hypergravity machine rotor packing layer, dedusting, desulfurization, demercuration, the dearsenification of the temperature that enters the dust-removal and desulfurizing hypergravity machine concentration that is 0 ℃~40 ℃; Described sulfide is selected from vulcanized sodium, NaHS, ammonium sulfide, ammonium hydro sulfide, potassium sulfide or potassium bisulfide;

2) enter the denitration hypergravity machine with the reacted flue gas of sulfide solution from dust-removal and desulfurizing hypergravity machine gaseous phase outlet, again with the temperature that enters the denitration hypergravity machine be 0 ℃~55 ℃ absorbent counter current contacting in denitration hypergravity machine rotor packing layer, reaction denitration; Wherein, described absorbent contains complexing ferrous iron and sulfide reducing agent, the complexing agent of described complexing ferrous iron is selected from ethylenediamine tetra-acetic acid (EDTA), N-(2-ethoxy) ethylenediamine-N, N', the mixture of one or both in N'-triacetic acid (HEDTA), nitrilotriacetic acid (NTA), diethylene triamine pentacetic acid (DTPA) (DTPA), citric acid, described sulfide reducing agent is selected from vulcanized sodium, NaHS, ammonium sulfide, ammonium hydro sulfide, potassium sulfide or potassium bisulfide; Reacted purified gas enters demister from denitration hypergravity machine gaseous phase outlet, enters subsequently exhaust system;

3) from the dust-removal and desulfurizing hypergravity machine, liquid out enters the desulfurization subsider after compensator, and sulphur wherein, insoluble sulfuration salt, ash fall, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the desulfurization subsider;

4) clear liquid on desulfurization subsider top is extracted out and is sent to the dust-removal and desulfurizing hypergravity machine, and with after supplementary sulfide on-line mixing, flowing to together the dust-removal and desulfurizing hypergravity machine, Absorption Desulfurization is circulated;

5) from the denitration hypergravity machine, liquid out enters the denitration subsider after compensator, and sulphur wherein, insoluble sulfuration salt settling, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the denitration subsider;

(6) clear liquid on denitration subsider top is extracted out and is sent to the denitration hypergravity machine, with after supplementary sulfide reducing agent on-line mixing, flowing to together the denitration hypergravity machine, circulates and absorbs denitration.

In the present invention, in described absorbent, total Fe concentration is 0.01mol/L~0.5mol/L, and sulfide is 3:1~5:1 with the mol ratio of total Fe, and described complexing agent is 1.02:1~2:1 with the mol ratio of total Fe, and described total Fe refers to Fe 2+and Fe 3+sum.Described sulfide is preferably ammonium sulfide or ammonium hydro sulfide.

In the present invention, the complexing agent of described complexing ferrous iron is preferably the mixture of EDTA and citric acid, the mixture of HEDTA and citric acid, the mixture of the mixture of EDTA and HEDTA or NTA and DTPA.EDTA is 1:2~1:4 with citric acid mixing optimum weight ratio, and HEDTA is 1:3~1:6 with citric acid mixing optimum weight ratio, and EDTA is 1:1~1:3 with HEDTA mixing optimum weight ratio, and NTA is 1:1~1:3 with DTPA mixing optimum weight ratio.

Beneficial effect of the present invention is: first utilize inorganic sulphide to absorb SOx, simultaneously, grit more than 99% in flue gas is trapped, inorganic sulphide is given birth to insoluble one-tenth sulphurizing salt with the reaction of the toxic heavy metals such as the mercury in flue gas, arsenic, then utilize the ferrous NOx of absorption of complexing, inorganic sulphide is as the reducing agent absorbent regeneration.The present invention adopts hypergravity machine as the gas-liquid mass transfer strengthening device, is conducive to removing of the Toxics such as dust, SOx, NOx, mercury, arsenic.

The present invention is in desulfurization, adopt inorganic sulphide to absorb SOx, not only can obtain sulphur, the heavy metals such as mercury, arsenic and lead are converted into to insoluble sulfide precipitation simultaneously and trap from flue gas, the sulphite produced in desulfurization and thiosulfate can be for the production of the sulfide as reducing agent.

The present invention, in denitration, adopts cheap inorganic sulphide, Complexing Iron can not only be reduced to the complexing ferrous iron, and the NO of complexed absorption can be reduced to nitrogen, and the regeneration efficiency of absorbent is high, absorption liquid application capable of circulation.The product sulphur of the oxidized generation of reducing agent inorganic sulphide, can reclaim, and is processed as the high-quality sulfur product, can not produce secondary pollution.Reducing agent is cheap and easy to get, and can to utilize the sulphite high temperature reduction of producing in desulfurization be sulphurizing salt.

Can be by under most dust arrestments in sweetening process, after the hypergravity denitration, the pollutant in flue gas substantially all removes, and the degree of purification of flue gas is high.The sulfureous in flue gas oxygenate conversion is sulphite and thiosulfate, can also further produce thiosulfate, as accessory substance, sells.

Technique of the present invention is simple, and absorption efficiency is high, and dedusting is thorough, and desulfurization degree is more than 99%, and the denitration rate, more than 96%, can remove dust, mercury and the arsenic in flue gas substantially fully.

The accompanying drawing explanation

Fig. 1 is the integrated process chart of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing of the present invention.

The specific embodiment

In order to explain better the present invention, below in conjunction with the drawings and specific embodiments, the present invention is described in further detail, but they do not form restriction to the present invention.

The size of two hypergravity machines of the present invention's test: rotor interior diameter 250mm, rotor overall diameter 600mm, rotor height 100mm.

Embodiment 1

The integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing as shown in Figure 1, comprises the following steps:

1) flue gas that is 120 ℃ by the dedusting temperature is with 400Nm 3the flow velocity of/h is sent into the dust-removal and desulfurizing hypergravity machine, SO in flue gas 2concentration is that 600~1000ppmv, NO concentration are 500~800ppmv, dust content 700~1100mg/Nm 3, arsenic content 6~20 μ g/Nm 3, mercury content 9~17 μ g/Nm 3, oxygen concentration 2%v, flue gas with squeeze into sodium sulfide solution counter current contacting in hypergravity machine rotor packing layer that in the dust-removal and desulfurizing hypergravity, temperature is 20 ℃ by storage tank through pump, dedusting, desulfurization, demercuration, dearsenification, flue gas and sodium sulfide solution volume ratio are 50:1, and the concentration of sodium sulfide solution is 0.01mol/L;

2) enter the denitration hypergravity machine with the reacted flue gas of sodium sulfide solution from dust-removal and desulfurizing hypergravity machine gaseous phase outlet, then with the temperature that enters the denitration hypergravity machine be 20 ℃ absorbent counter current contacting in denitration hypergravity machine rotor packing layer, reaction denitration; Wherein, absorbent consists of vulcanized sodium, HEDTA complexing ferrous iron, and total Fe concentration is 0.01mol/L, the mol ratio 1.02:1 of HEDTA and total Fe, and vulcanized sodium is 5:1 with the mol ratio of total iron, the volume ratio of flue gas and absorbent is 100:1; Reacted purified gas enters demister from denitration hypergravity machine gaseous phase outlet, enters subsequently exhaust system; Purified gas adopts infrared spectrometer to detect, SO in purified gas 2concentration is 5ppmv, and NO concentration is 7ppmv, dust content<1mg/Nm 3, adopt atomic absorption spectrography (AAS) to detect heavy metal, can't detect arsenic, mercury;

3) from the dust-removal and desulfurizing hypergravity machine, liquid out enters the desulfurization subsider after compensator, and sulphur wherein, insoluble sulfuration salt, ash fall, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the desulfurization subsider;

4) clear liquid on desulfurization subsider top is extracted out and is sent to the dust-removal and desulfurizing hypergravity machine, and with after supplementary sulfide on-line mixing, flowing to together the dust-removal and desulfurizing hypergravity machine, Absorption Desulfurization is circulated;

5) from the denitration hypergravity machine, liquid out enters the denitration subsider after compensator, and sulphur wherein, insoluble sulfuration salt settling, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the denitration subsider;

(6) clear liquid on denitration subsider top is extracted out and is sent to the denitration hypergravity machine, with after supplementary sulfide reducing agent on-line mixing, flowing to together the denitration hypergravity machine, circulates and absorbs denitration.

Embodiment 2

The integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing as shown in Figure 1, comprises the following steps:

1) by temperature, be that 40 ℃ of flue gases are with 400Nm 3the flow velocity of/h is sent into the dust-removal and desulfurizing hypergravity machine, SO in flue gas 2concentration is that 1400~2000ppmv, NO concentration are 500~800ppmv, dust content 700~1100mg/Nm 3, arsenic content 6~20 μ g/Nm 3, mercury content 9~17 μ g/Nm 3, oxygen concentration 3%v, flue gas with squeeze into NaHS aqueous solution counter current contacting in hypergravity machine rotor packing layer that in the dust-removal and desulfurizing hypergravity, temperature is 0 ℃ by storage tank through pump, dedusting, desulfurization, demercuration, dearsenification, the volume ratio of flue gas and the NaHS aqueous solution is 700:1, and the concentration of the NaHS aqueous solution is 1.0mol/L;

2) with the NaHS reactant aqueous solution after flue gas enter the denitration hypergravity machine from dust-removal and desulfurizing hypergravity machine gaseous phase outlet, then with the temperature that enters the denitration hypergravity machine be 0 ℃ absorbent counter current contacting in denitration hypergravity machine rotor packing layer, reaction denitration; Wherein, absorbent consists of NaHS, EDTA complexing ferrous iron, and total Fe concentration is 0.5mol/L, the mol ratio 1.5:1 of EDTA and total Fe, and NaHS is 4:1 with the mol ratio of total iron, the volume ratio of flue gas and absorbent is 500:1; Reacted purified gas enters demister from denitration hypergravity machine gaseous phase outlet, enters subsequently exhaust system; Purified gas adopts infrared spectrometer to detect, SO in purified gas 2concentration is 10ppmv, and NO concentration is 17ppmv, dust content<1mg/Nm 3, adopt atomic absorption spectrography (AAS) to detect heavy metal, can't detect arsenic, mercury;

3) from the dust-removal and desulfurizing hypergravity machine, liquid out enters the desulfurization subsider after compensator, and sulphur wherein, insoluble sulfuration salt, ash fall, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the desulfurization subsider;

4) clear liquid on desulfurization subsider top is extracted out and is sent to the dust-removal and desulfurizing hypergravity machine, and with after supplementary sulfide on-line mixing, flowing to together the dust-removal and desulfurizing hypergravity machine, Absorption Desulfurization is circulated;

5) from the denitration hypergravity machine, liquid out enters the denitration subsider after compensator, and sulphur wherein, insoluble sulfuration salt settling, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the denitration subsider;

(6) clear liquid on denitration subsider top is extracted out and is sent to the denitration hypergravity machine, with after supplementary sulfide reducing agent on-line mixing, flowing to together the denitration hypergravity machine, circulates and absorbs denitration.

Embodiment 3

The integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing as shown in Figure 1, comprises the following steps:

1) by temperature, be that 80 ℃ of flue gases are with 400Nm 3the flow velocity of/h is sent into the dust-removal and desulfurizing hypergravity machine, SO in flue gas 2concentration is that 1600~2400ppmv, NO concentration are 500~800ppmv, dust content 700~1100mg/Nm 3, arsenic content 6~20 μ g/Nm 3, mercury content 9~17 μ g/Nm 3, oxygen concentration 5%v, flue gas with squeeze into ammonium sulfide solution counter current contacting in hypergravity machine rotor packing layer that in the dust-removal and desulfurizing hypergravity, temperature is 35 ℃ by storage tank through pump, dedusting, desulfurization, demercuration, dearsenification, the volume ratio of flue gas and ammonium sulfide solution is 800:1, and the concentration of ammonium sulfide solution is 2.0mol/L;

2) enter the denitration hypergravity machine with the reacted flue gas of ammonium sulfide solution from dust-removal and desulfurizing hypergravity machine gaseous phase outlet, then with the temperature that enters the denitration hypergravity machine be 55 ℃ absorbent counter current contacting in denitration hypergravity machine rotor packing layer, reaction denitration; Wherein, absorbent consists of ammonium sulfide, NTA complexing ferrous iron, and total Fe concentration is 0.3mol/L, the mol ratio 2:1 of NTA and total Fe, and ammonium sulfide is 3:1 with the mol ratio of total iron, the volume ratio of flue gas and absorbent is 1000:1; Reacted purified gas enters demister from denitration hypergravity machine gaseous phase outlet, enters subsequently exhaust system; Purified gas adopts infrared spectrometer to detect, SO in purified gas 2concentration is 12ppmv, and NO concentration is 15ppmv, dust content<1mg/Nm 3, adopt atomic absorption spectrography (AAS) to detect heavy metal, can't detect arsenic, mercury;

3) from the dust-removal and desulfurizing hypergravity machine, liquid out enters the desulfurization subsider after compensator, and sulphur wherein, insoluble sulfuration salt, ash fall, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the desulfurization subsider;

4) clear liquid on desulfurization subsider top is extracted out and is sent to the dust-removal and desulfurizing hypergravity machine, and with after supplementary sulfide on-line mixing, flowing to together the dust-removal and desulfurizing hypergravity machine, Absorption Desulfurization is circulated;

5) from the denitration hypergravity machine, liquid out enters the denitration subsider after compensator, and sulphur wherein, insoluble sulfuration salt settling, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the denitration subsider;

(6) clear liquid on denitration subsider top is extracted out and is sent to the denitration hypergravity machine, with after supplementary sulfide reducing agent on-line mixing, flowing to together the denitration hypergravity machine, circulates and absorbs denitration.

Embodiment 4

The integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing as shown in Figure 1, comprises the following steps:

1) by the temperature after dedusting, be that 60 ℃ of flue gases are with 400Nm 3the flow velocity of/h is sent into the dust-removal and desulfurizing hypergravity machine, SO in flue gas 2concentration is that 600~1000ppmv, NO concentration are 800~1200ppmv, dust content 700~1100mg/Nm 3, arsenic content 6~20 μ g/Nm 3, mercury content 9~17 μ g/Nm 3, oxygen concentration 6%v, flue gas with squeeze into ammonium hydro sulfide aqueous solution counter current contacting in hypergravity machine rotor packing layer that in the desulfurization hypergravity, temperature is 40 ℃ by storage tank through pump, dedusting, desulfurization, demercuration, dearsenification, the volume ratio of flue gas and the ammonium hydro sulfide aqueous solution is 800:1, and the concentration of the ammonium hydro sulfide aqueous solution is 3.0mol/L;

2) with the ammonium hydro sulfide reactant aqueous solution after flue gas enter the denitration hypergravity machine from dust-removal and desulfurizing hypergravity machine gaseous phase outlet, again with the temperature that enters the denitration hypergravity machine be 45 ℃ absorbent counter current contacting in denitration hypergravity machine rotor packing layer, reaction denitration; Wherein, absorbent consists of ammonium hydro sulfide, DTPA complexing ferrous iron, and total Fe concentration is 0.3mol/L, the mol ratio 1.2:1 of DTPA and total Fe, and ammonium hydro sulfide is 3:1 with the mol ratio of total iron, the volume ratio of flue gas and absorbent is 800:1; Reacted purified gas enters demister from denitration hypergravity machine gaseous phase outlet, enters subsequently exhaust system; Purified gas adopts infrared spectrometer to detect, SO in purified gas 2concentration is 5ppmv, and NO concentration is 20ppmv, dust content<1mg/Nm 3, adopt atomic absorption spectrography (AAS) to detect heavy metal, can't detect arsenic, mercury;

3) from the dust-removal and desulfurizing hypergravity machine, liquid out enters the desulfurization subsider after compensator, and sulphur wherein, insoluble sulfuration salt, ash fall, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the desulfurization subsider;

4) clear liquid on desulfurization subsider top is extracted out and is sent to the dust-removal and desulfurizing hypergravity machine, and with after supplementary sulfide on-line mixing, flowing to together the dust-removal and desulfurizing hypergravity machine, Absorption Desulfurization is circulated;

5) from the denitration hypergravity machine, liquid out enters the denitration subsider after compensator, and sulphur wherein, insoluble sulfuration salt settling, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the denitration subsider;

(6) clear liquid on denitration subsider top is extracted out and is sent to the denitration hypergravity machine, with after supplementary sulfide reducing agent on-line mixing, flowing to together the denitration hypergravity machine, circulates and absorbs denitration.

Embodiment 5

The integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing as shown in Figure 1, comprises the following steps:

1) by the temperature after dedusting, be that 75 ℃ of flue gases are with 400Nm 3the flow velocity of/h is sent into the dust-removal and desulfurizing hypergravity machine, SO in flue gas 2concentration is that 2300~3100ppmv, NO concentration are 800~1200ppmv, dust content 700~1100mg/Nm 3, arsenic content 6~20 μ g/Nm 3, mercury content 9~17 μ g/Nm 3, oxygen concentration 6%v, flue gas with squeeze into potassium sulfide aqueous solution counter current contacting in hypergravity machine rotor packing layer that in the desulfurization hypergravity, temperature is 30 ℃ by storage tank through pump, dedusting, desulfurization, demercuration, dearsenification, the volume ratio of flue gas and potassium sulfide aqueous solution is 800:1, and the concentration of potassium sulfide aqueous solution is 3.0mol/L;

2) enter the denitration hypergravity machine with the reacted flue gas of potassium sulfide aqueous solution from dust-removal and desulfurizing hypergravity machine gaseous phase outlet, then with the temperature that enters the denitration hypergravity machine be 50 ℃ absorbent counter current contacting in denitration hypergravity machine rotor packing layer, reaction denitration; Wherein, absorbent consists of potassium sulfide, EDTA+ citric acid complex ferrous iron, total Fe concentration is 0.2mol/L, the mol ratio 1.3:1 of EDTA+ citric acid and total Fe, EDTA is 1:3 with citric acid mixing optimum weight ratio, potassium sulfide is 3:1 with the mol ratio of total iron, and the volume ratio of flue gas and absorbent is 800:1; Reacted purified gas enters demister from denitration hypergravity machine gaseous phase outlet, enters subsequently exhaust system; Purified gas adopts infrared spectrometer to detect, SO in purified gas 2concentration is 6ppmv, and NO concentration is 6ppmv, dust content<1mg/Nm 3, adopt atomic absorption spectrography (AAS) to detect heavy metal, can't detect arsenic, mercury;

3) from the dust-removal and desulfurizing hypergravity machine, liquid out enters the desulfurization subsider after compensator, and sulphur wherein, insoluble sulfuration salt, ash fall, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the desulfurization subsider;

4) clear liquid on desulfurization subsider top is extracted out and is sent to the dust-removal and desulfurizing hypergravity machine, and with after supplementary sulfide on-line mixing, flowing to together the dust-removal and desulfurizing hypergravity machine, Absorption Desulfurization is circulated;

5) from the denitration hypergravity machine, liquid out enters the denitration subsider after compensator, and sulphur wherein, insoluble sulfuration salt settling, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the denitration subsider;

(6) clear liquid on denitration subsider top is extracted out and is sent to the denitration hypergravity machine, with after supplementary sulfide reducing agent on-line mixing, flowing to together the denitration hypergravity machine, circulates and absorbs denitration.

Embodiment 6

The integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing as shown in Figure 1, comprises the following steps:

1) by the temperature after dedusting, be that 90 ℃ of flue gases are with 400Nm 3the flow velocity of/h is sent into the dust-removal and desulfurizing hypergravity machine, SO in flue gas 2concentration is that 2300~3100ppmv, NO concentration are 800~1200ppmv, dust content 700~1100mg/Nm 3, arsenic content 6~20 μ g/Nm 3, mercury content 9~17 μ g/Nm 3oxygen concentration 7%v, flue gas with squeeze into potassium bisulfide aqueous solution counter current contacting in hypergravity machine rotor packing layer that in the desulfurization hypergravity, temperature is 20 ℃ by storage tank through pump, dedusting, desulfurization, demercuration, dearsenification, the volume ratio of flue gas and the potassium bisulfide aqueous solution is 1000:1, and the concentration of the potassium bisulfide aqueous solution is 4.0mol/L;

2) with the potassium bisulfide reactant aqueous solution after flue gas enter the denitration hypergravity machine from dust-removal and desulfurizing hypergravity machine gaseous phase outlet, then with the temperature that enters the denitration hypergravity machine be 50 ℃ absorbent counter current contacting in denitration hypergravity machine rotor packing layer, reaction denitration; Wherein, absorbent consists of potassium bisulfide, HEDTA+ citric acid complex ferrous iron, total Fe concentration is 0.4mol/L, the mol ratio 1.2:1 of HEDTA+ citric acid and total Fe, HEDTA is 1:5 with citric acid mixing optimum weight ratio, potassium bisulfide is 4:1 with the mol ratio of total iron, and the volume ratio of flue gas and absorbent is 800:1; Reacted purified gas enters demister from denitration hypergravity machine gaseous phase outlet, enters subsequently exhaust system; Purified gas adopts infrared spectrometer to detect, SO in purified gas 2concentration is 5ppmv, and NO concentration is 5ppmv, dust content<1mg/Nm 3, adopt atomic absorption spectrography (AAS) to detect heavy metal, can't detect arsenic, mercury;

3) from the dust-removal and desulfurizing hypergravity machine, liquid out enters the desulfurization subsider after compensator, and sulphur wherein, insoluble sulfuration salt, ash fall, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the desulfurization subsider;

4) clear liquid on desulfurization subsider top is extracted out and is sent to the dust-removal and desulfurizing hypergravity machine, and with after supplementary sulfide on-line mixing, flowing to together the dust-removal and desulfurizing hypergravity machine, Absorption Desulfurization is circulated;

5) from the denitration hypergravity machine, liquid out enters the denitration subsider after compensator, and sulphur wherein, insoluble sulfuration salt settling, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the denitration subsider;

(6) clear liquid on denitration subsider top is extracted out and is sent to the denitration hypergravity machine, with after supplementary sulfide reducing agent on-line mixing, flowing to together the denitration hypergravity machine, circulates and absorbs denitration.

Embodiment 7

The integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing as shown in Figure 1, comprises the following steps:

1) by the temperature after dedusting, be that 85 ℃ of flue gases are with 400Nm 3the flow velocity of/h is sent into the dust-removal and desulfurizing hypergravity machine, SO in flue gas 2concentration is that 2300~3100ppmv, NO concentration are 1000~1500ppmv, dust content 700~1100mg/Nm 3, arsenic content 6~20 μ g/Nm 3, mercury content 9~17 μ g/Nm 3, oxygen concentration 7%v, flue gas with squeeze into sodium sulfide solution counter current contacting in hypergravity machine rotor packing layer that in the desulfurization hypergravity, temperature is 25 ℃ by storage tank through pump, dedusting, desulfurization, demercuration, dearsenification, the volume ratio of flue gas and sodium sulfide solution is 1000:1, and the concentration of sodium sulfide solution is 1.0mol/L;

2) enter the denitration hypergravity machine with the reacted flue gas of sodium sulfide solution from dust-removal and desulfurizing hypergravity machine gaseous phase outlet, then with the temperature that enters the denitration hypergravity machine be 40 ℃ absorbent counter current contacting in denitration hypergravity machine rotor packing layer, reaction denitration; Wherein, absorbent consists of vulcanized sodium, EDTA+HEDTA complexing ferrous iron, total Fe concentration is 0.15mol/L, the mol ratio 1.2:1 of EDTA+HEDTA and total Fe, EDTA is 1:2 with HEDTA mixing optimum weight ratio, vulcanized sodium is 3:1 with the mol ratio of total iron, and the volume ratio of flue gas and absorbent is 800:1; Reacted purified gas enters demister from denitration hypergravity machine gaseous phase outlet, enters subsequently exhaust system; Purified gas adopts infrared spectrometer to detect, SO in purified gas 2concentration is 7ppmv, and NO concentration is 9ppmv, dust content<1mg/Nm 3, adopt atomic absorption spectrography (AAS) to detect heavy metal, can't detect arsenic, mercury;

3) from the dust-removal and desulfurizing hypergravity machine, liquid out enters the desulfurization subsider after compensator, and sulphur wherein, insoluble sulfuration salt, ash fall, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the desulfurization subsider;

4) clear liquid on desulfurization subsider top is extracted out and is sent to the dust-removal and desulfurizing hypergravity machine, and with after supplementary sulfide on-line mixing, flowing to together the dust-removal and desulfurizing hypergravity machine, Absorption Desulfurization is circulated;

5) from the denitration hypergravity machine, liquid out enters the denitration subsider after compensator, and sulphur wherein, insoluble sulfuration salt settling, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the denitration subsider;

(6) clear liquid on denitration subsider top is extracted out and is sent to the denitration hypergravity machine, with after supplementary sulfide reducing agent on-line mixing, flowing to together the denitration hypergravity machine, circulates and absorbs denitration.

Embodiment 8

The integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing as shown in Figure 1, comprises the following steps:

1) by the temperature after dedusting, be that 50 ℃ of flue gases are with 400Nm 3the flow velocity of/h is sent into the dust-removal and desulfurizing hypergravity machine, SO in flue gas 2concentration is that 2300~3100ppmv, NO concentration are 800~1200ppmv, dust content 700~1100mg/Nm 3, arsenic content 6~20 μ g/Nm 3, mercury content 9~17 μ g/Nm 3, oxygen concentration 8%v, flue gas with squeeze into potassium bisulfide aqueous solution counter current contacting in hypergravity machine rotor packing layer that in the desulfurization hypergravity, temperature is 35 ℃ by storage tank through pump, dedusting, desulfurization, demercuration, dearsenification, the volume ratio of flue gas and the potassium bisulfide aqueous solution is 1000:1, and the concentration of the potassium bisulfide aqueous solution is 3.5mol/L;

2) enter the denitration hypergravity machine with the reacted flue gas of sodium sulfide solution from dust-removal and desulfurizing hypergravity machine gaseous phase outlet, then with the temperature that enters the denitration hypergravity machine be 40 ℃ absorbent counter current contacting in denitration hypergravity machine rotor packing layer, reaction denitration; Wherein, absorbent consists of vulcanized sodium, DTPA+NTA complexing ferrous iron, and total Fe concentration is 0.25mol/L, the mol ratio 1.3:1 of DTPA+NTA and total Fe, NTA is 1:1 with DTPA mixing optimum weight ratio, and vulcanized sodium is 3:1 with the mol ratio of total iron, and the volume ratio of flue gas and absorbent is 800:1; Reacted purified gas enters demister from denitration hypergravity machine gaseous phase outlet, enters subsequently exhaust system; Purified gas adopts infrared spectrometer to detect, SO in purified gas 2concentration is 5ppmv, and NO concentration is 7ppmv, dust content<1mg/Nm 3, adopt atomic absorption spectrography (AAS) to detect heavy metal, can't detect arsenic, mercury;

3) from the dust-removal and desulfurizing hypergravity machine, liquid out enters the desulfurization subsider after compensator, and sulphur wherein, insoluble sulfuration salt, ash fall, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the desulfurization subsider;

4) clear liquid on desulfurization subsider top is extracted out and is sent to the dust-removal and desulfurizing hypergravity machine, and with after supplementary sulfide on-line mixing, flowing to together the dust-removal and desulfurizing hypergravity machine, Absorption Desulfurization is circulated;

5) from the denitration hypergravity machine, liquid out enters the denitration subsider after compensator, and sulphur wherein, insoluble sulfuration salt settling, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the denitration subsider;

(6) clear liquid on denitration subsider top is extracted out and is sent to the denitration hypergravity machine, with after supplementary sulfide reducing agent on-line mixing, flowing to together the denitration hypergravity machine, circulates and absorbs denitration.

Claims (3)

1. the integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing, is characterized in that, comprises the following steps:
1) by temperature be 40 ℃~120 ℃ and send into the dust-removal and desulfurizing hypergravity machine containing SOx, NOx, mercury, arsenic flue gas, with be 0.01~4.0mol/L sulfide solution counter current contacting in dust-removal and desulfurizing hypergravity machine rotor packing layer, dedusting, desulfurization, demercuration, the dearsenification of the temperature that enters the dust-removal and desulfurizing hypergravity machine concentration that is 0 ℃~40 ℃; Described sulfide is selected from vulcanized sodium, NaHS, ammonium sulfide, ammonium hydro sulfide, potassium sulfide or potassium bisulfide;
2) enter the denitration hypergravity machine with the reacted flue gas of sulfide solution from dust-removal and desulfurizing hypergravity machine gaseous phase outlet, again with the temperature that enters the denitration hypergravity machine be 0 ℃~55 ℃ absorbent counter current contacting in denitration hypergravity machine rotor packing layer, reaction denitration; Wherein, described absorbent contains complexing ferrous iron and sulfide reducing agent, the complexing agent of described complexing ferrous iron is selected from ethylenediamine tetra-acetic acid, N-(2-ethoxy) ethylenediamine-N, N', the mixture of one or both in N'-triacetic acid, nitrilotriacetic acid, diethylene triamine pentacetic acid (DTPA), citric acid, described sulfide reducing agent is selected from vulcanized sodium, NaHS, ammonium sulfide, ammonium hydro sulfide, potassium sulfide or potassium bisulfide; Reacted purified gas enters demister from denitration hypergravity machine gaseous phase outlet, enters subsequently exhaust system;
3) from the dust-removal and desulfurizing hypergravity machine, liquid out enters the desulfurization subsider after compensator, and sulphur wherein, insoluble sulfuration salt, ash fall, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the desulfurization subsider;
4) clear liquid on desulfurization subsider top is extracted out and is sent to the dust-removal and desulfurizing hypergravity machine, and with after supplementary sulfide on-line mixing, flowing to together the dust-removal and desulfurizing hypergravity machine, Absorption Desulfurization is circulated;
5) from the denitration hypergravity machine, liquid out enters the denitration subsider after compensator, and sulphur wherein, insoluble sulfuration salt settling, to bottom, are reclaimed to solid after filter filters, and filtrate is returned the denitration subsider;
(6) clear liquid on denitration subsider top is extracted out and is sent to the denitration hypergravity machine, with after supplementary sulfide reducing agent on-line mixing, flowing to together the denitration hypergravity machine, circulates and absorbs denitration.
2. the integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing according to claim 1, it is characterized in that: in described absorbent, total Fe concentration is 0.01mol/L~0.5mol/L, sulfide is 3:1~5:1 with the mol ratio of total Fe, described complexing agent is 1.02:1~2:1 with the mol ratio of total Fe, and described total Fe refers to Fe 2+and Fe 3+sum.
3. the integrated method of the ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification of hypergravity complexing according to claim 1, it is characterized in that: the complexing agent of described complexing ferrous iron is selected from the mixture of ethylenediamine tetra-acetic acid and citric acid, N-(2-ethoxy) ethylenediamine-N, N', the mixture of N'-triacetic acid and citric acid, ethylenediamine tetra-acetic acid and N-(2-ethoxy) ethylenediamine-N, N', the mixture of the mixture of N'-triacetic acid or nitrilotriacetic acid and diethylene triamine pentacetic acid (DTPA).
CN201310403655.9A 2013-09-06 2013-09-06 The method of hypergravity complexing ferrous flue-gas wet dust removal desulfurization denitration demercuration dearsenification integration CN103432877B (en)

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CN103768910A (en) * 2014-01-16 2014-05-07 昆明理工大学 Synergetic purification method and device for SO2 and heavy metals in smelting flue gas
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CN105233647A (en) * 2015-09-17 2016-01-13 昆明理工大学 Desulphurization denitration method for ammonium sulfide solution
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CN105311947A (en) * 2015-12-08 2016-02-10 济南乾坤环保设备有限公司 Boiler fume denitration and desulfuration dedusting device and process
CN106474905A (en) * 2016-12-29 2017-03-08 焦作和信冶金科技有限责任公司 A kind of calcining fume desulfurizing and dedusting technology

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