CN102489107A - Desulfurization and denitrification process utilizing microwave to intermittently irradiate activated carbon - Google Patents

Desulfurization and denitrification process utilizing microwave to intermittently irradiate activated carbon Download PDF

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Publication number
CN102489107A
CN102489107A CN2011104176288A CN201110417628A CN102489107A CN 102489107 A CN102489107 A CN 102489107A CN 2011104176288 A CN2011104176288 A CN 2011104176288A CN 201110417628 A CN201110417628 A CN 201110417628A CN 102489107 A CN102489107 A CN 102489107A
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activated carbon
microwave
flue gas
desulfurization
adsorbent bed
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CN2011104176288A
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Chinese (zh)
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CN102489107B (en
Inventor
马双忱
姚娟娟
张博
石荣雪
董松
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华北电力大学(保定)
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Abstract

Disclosed is a desulfurization and denitrification process utilizing microwave to intermittently irradiate activated carbon. Two or more adsorption beds filled with activated carbon particles are used for adsorbing or implementing microwave irradiation to flue gas of boilers alternatively. Flue gas is delivered into one of the adsorption beds by an induced draft fan, then the adsorption bed begins to run, and sulfur and nitric oxides in the flue gas are adsorbed by the activated carbon. After the activated carbon in the adsorption bed in running is saturated, the adsorption bed is in a regenerating state so as to be reused. The flue gas is delivered into the other adsorption bed beginning to run so as to be adsorbed, activated carbon particles of the regenerating adsorption bed are irradiated by microwave, sulfur and nitric oxides adsorbed on the surface of the activated carbon are quickly reduced and decomposed into elemental sulfur and nitrogen gas under high temperature, and the different adsorption beds are switched between the running state and the regenerating stage alternatively. Metal oxide is used as a reduction reaction catalyst so as to reduce reduction and decomposition temperature and loss of carbon. By the desulfurization and denitrification process, energy consumption of microwave irradiation can be reduced greatly, loss of carbon can be decreased, and in-situ regeneration of activated carbon is realized. In addition, the desulfurization and denitrification process has the advantages of fine desulfurization and denitrification effect, short time for regeneration of activated carbon, low cost for desulfurization and denitrification, high recovery rate, easiness in industrialized implementing and the like.

Description

The method of a kind of microwave intermitant irradiation active carbon desulfurization denitration
Technical field
The present invention relates to a kind of flue gas purifying method, particularly adopt the method and the device of microwave intermitant irradiation active carbon desulfurization denitration, belong to the flue gases purification field.
Background technology
For environmental protection and sustainable development, strict day by day standard has all been formulated to the discharging of sulfur dioxide and nitrogen oxide in countries in the world, to the SO of thermal power plant 2, NO XEmission request has increased significantly.Through continuous technological innovation, realize smoke pollution control efficient, low consumption, be the important channel that solves flue gas pollutant control problem.Flue gas desulfurization is to control acid rain and SO at present in the world 2The most effective and major technology means of polluting.Its mainstream technology is a lime stone gypsum washing method, this technology comparative maturity, removal efficiency height, but shortcoming is that investment is high, complex process.In addition, be easy to generate problems such as equipment obstruction, burn into leakage and desulfurated plaster are difficult to utilize again.SO 2Though be polluter, also be valuable sulphur resource, directly with SO 2Be reduced to callable elemental sulfur another promising fume desulphurization method is provided.In the selection of reducing agent, the raw material of wood-charcoal material is than CO, H 2And CH 4Deng, have characteristics such as low price, source abundance, production and transportation facility.Therefore, utilize the raw material of wood-charcoal material as SO 2Reducing agent will be environmental friendliness and cheaply.But under the traditional heating method, SO 2And the reaction between the carbon often requires high temperature, such as adopting the oil-sand coke to be used for SO as reducing agent 2Reduction, find just can reach effective SO more than 600 ℃ 2Reduction temperature, thus make this technology in industry, be difficult to realize.So reducing reduction reaction temperature is the key of reducing process flue gas sulfur recovery.
Removing SO in a large number 2After, at the higher area of environmental requirement, NO xJust become the major control target that the acid rain precursor reduces discharging.At present, in practical application in industry, the NO that is extensively adopted xControl technology mainly contains two types: burning NO xControl and gas denitrifying technology.Burning NO xControl technology reduces NO through the optimized combustion process xGeneration, this technology installation and operation cost is cheap relatively, but the denitration rate is lower, is generally 30% ~ 40%.Therefore, when to NO xWhen emission request is higher (such as aforementioned new standard), adopt combustion control technology often can not reach emission request merely, just need to adopt the tail flue gas denitration technology to come further to reduce NO xDischarging.The more gas denitrifying technology of domestic and international application is selective catalytic reduction (SCR) at present, and the SCR law technology is ripe relatively, and reliability is high; The denitration rate can reach more than 90%; But invest hugely, catalyst is expensive and consume a large amount of ammonias or urea, and operating cost is higher.
Microwave is the electromagnetic wave of a kind of frequency range from 0.3 ~ 300GHz, and corresponding wavelength range is 1mm ~ 1m, and in electromagnetic spectrum, the microwave region is between infrared ray and radio wave frequency.Microwave heating technique is an a kind of brand-new heat energy technology, and the applied microwave heating object can be rapidly heated, because " focus " effect occurs in heat medium a plurality of " thermals source ", and abundant heat medium not only, and can quicken chemical reaction rate.The These characteristics of heating using microwave makes it can be applied to the regeneration of active carbon.Patent CN2680343, CN101249412 and CN101693162A relate to the microwave desulfurization denitration technology, utilize the unique selectivity heating properties of microwave, in conjunction with charcoal to SO 2And NO xReducing power, improved the efficient of desulfurization simultaneously, denitration greatly.But the existing common problem of above-mentioned microwave desulfurization denitration technology is following: 1. microwave continuous irradiation active carbons, and active carbon is continuous firing at high temperature, and the charcoal loss is serious; 2. microwave generator belongs to high-energy equipment, microwave continuous irradiation makes desulfurization, denitration operating cost higher, influenced should technology industrializing implementation; 3. catalyst is selected to have much room for improvement; As adopting CuCl in the patent CN101693162A public technology is catalyst; Have that CuCl preparation difficulty, chemical characteristic are unstable, there is oxidation in the oxygen in the flue gas, itself is easy to absorb water vapour and problems such as deliquescence CuCl, these have all damaged its catalytic activity in various degree; 4, under the hot conditions, continuous microwave irradiation can make oxygen meeting lot of consumption active carbon in the flue gas, thereby makes process economy become relatively poor.
Summary of the invention
Problem to be solved by this invention provides the method for the microwave intermitant irradiation active carbon desulfurization denitration of a kind of low energy consumption, high removal efficiency.
The alleged problem of the present invention is solved by following technical scheme:
The method of a kind of microwave intermitant irradiation active carbon desulfurization denitration, its special feature is: it is alternately adsorbed boiler smoke or the microwave irradiation processing by two or many adsorbent beds that activated carbon granule is housed, wherein; Flue gas is sent into an adsorbent bed by air-introduced machine behind the high-effective dust-removing; This adsorbent bed gets into duty, by the sulphur nitrogen oxide in the charcoal absorption flue gas, treat that the charcoal absorption of duty adsorbent bed is saturated after; This adsorbent bed gets into reproduced state; Flue gas is switched to another adsorbent bed that gets into duty carry out flue gas absorption, under the subsequent use bed of the microwave irradiation situation, the at high temperature isolated flue gas of sulphur nitrogen oxide that is adsorbed on activated carbon surface is elemental sulfur and nitrogen by the charcoal reduction decomposition; Each adsorbent bed duty and reproduced state alternate cycles are carried out, and realize the flue gas continuous purification.
The microwave irradiation frequency is 2.45GHz when the method for above-mentioned microwave intermitant irradiation active carbon desulfurization denitration, said regeneration of adsorbent beds state, makes active carbon microwave radiation under 300~600 ℃ of temperature conditions 15-30min
The method of above-mentioned microwave intermitant irradiation active carbon desulfurization denitration; Add metal oxides such as cupric oxide, manganese oxide in the said active carbon as catalyst; The catalyst adition process is carried out according to following step: a. removes the impurity on surface with activated carbon granule with the abundant cleaning and removing of deionized water, fully soaks the foreign ion that 2 ~ 6h removes charcoal absorption with deionized water again; B. take by weighing corresponding to quality of activated carbon 0.5% ~ 5%Metallic catalyst be carried on the active carbon with equi-volume impregnating; C. will contain activity of such catalysts charcoal particle at 65 ~ 100 ℃ of vacuum drying 4h, continue then at 100 ~ 120 ℃ of vacuum drying 5 ~ 10h.
The method of above-mentioned microwave intermitant irradiation active carbon desulfurization denitration, said reproduced state adsorbent bed microwave irradiation heating process, gas that comes out through the microwave irradiation desorption in the active carbon and sulfur vapor get into the sulfur recovery pond and reclaim elemental sulfur, and the flue gas of cleaning is discharged.
The present invention is directed to problems such as existing microwave desulfurization denitration technology high energy consumption, charcoal loss are big improves; Provide a kind of effective catalyst of selecting for use to combine the active-carbon bed while desulfurization denitration method of microwave intermitant irradiation; This method belongs to the category of microwave induction catalytic reduced oxide; It has effectively utilized the absorption of active carbon and the efficient degradation characteristic of microwave; Be the flue gas pollutant removal methods of a kind of high efficiency, high-adsorption-capacity, high catalytic activity, adopt this method can reduce the microwave irradiation energy consumption greatly, reduce the charcoal loss; Realize the in-situ regeneration of active carbon, have simple to operate flexibly, removal effect is good, the regeneration of activated carbon time short, remove that cost is low, the rate of recovery is high, be easy to characteristics such as industrializing implementation.
Description of drawings
Fig. 1 is a process chart of the present invention;
Fig. 2 is the following two kinds of active carbon denitration efficiency graphs of a relation of different temperatures.
The label implication is following among the figure: 1. first valve; 2. second valve; 3. the 3rd valve; 4. the 4th valve; 5. the 5th valve; 6. the 6th valve; 7. the 7th valve; 8. air-introduced machine; , 9-1, first adsorbent bed; 9-2.Second adsorbent bed; 10-1. first microwave generator, 10-2. second microwave generator; 11-1. the first sulfur recovery pond; 11-2. the second sulfur recovery pond.
The specific embodiment
The inventive method adopts two or many adsorbent beds that activated carbon granule is housed alternately boiler smoke to be carried out adsorption treatment, and technical essential is to adopt the microwave intermitant irradiation, is removing SO in the flue gas continuously 2, NO xProcess in can reduce the energy consumption of microwave irradiation greatly, and reduce the charcoal loss.Said method implementation process is following: flue gas is introduced the duty adsorbent bed; By the sulphur nitrogen oxide in the absorption of the granular activated carbon in this adsorbent bed flue gas; When the exit concentration of treating duty adsorbent bed flue gas is about to exceed national atmosphere pollution control criterion; It is saturated that the activated carbon granule that this duty adsorbent bed is described has reached absorption, flue gas switched to another adsorbent bed carry out flue gas absorption, and the adsorbent bed that arrives the absorption saturation state gets into reproduced state.Active carbon to said reproduced state adsorbent bed adopts microwave irradiation; Make the sulphur nitrogen oxide that is adsorbed on activated carbon surface at high temperature be decomposed into elemental sulfur and nitrogen by carbon reduction; In the microwave heating process; Gas that desorption comes out and sulfur vapor reclaim elemental sulfur through the sulfur recovery pond, the flue gas of cleaning is discharged.After the active carbon in-situ regeneration of reproduced state adsorbent bed finishes, prepare to get into next duty.Two or many adsorbent bed duties, reproduced state alternate cycles are carried out, and make flue gas be able to continuous processing.
During the regeneration of adsorbent beds state, the microwave irradiation frequency is 2.45GHz, makes active carbon microwave radiation under 300~600 ℃ of temperature conditions 15-30min.Under hot conditions, SO 2And NO XUnder microwave irradiation, take place to reduce to react through active-carbon bed, equation is following:
(1)
(2)
For further improving denitrification efficiency, in activated carbon granule, add metal oxides such as cupric oxide, manganese oxide and make catalyst, to reduce reaction temperature, promote the selectivity that target contaminant is removed.Said active carbon adds the process of catalyst to carry out according to following step: Activated carbon granule is removed the impurity on surface with the abundant cleaning and removing of deionized water, fully soak the foreign ion that 2 ~ 6 h remove charcoal absorption with deionized water again; 2. take by weighing corresponding to quality of activated carbon 0.5% ~ 5%Metallic catalyst be carried on the active carbon with equi-volume impregnating; 3.. at 65 ~ 100 ℃ of vacuum drying 4 h; 4.. continue 100 ~ 120 ℃ of vacuum drying 5 ~ 10 h.
The inventive method experimental result to the simulated flue gas denitration under laboratory condition is following: take by weighing the active carbon and each 15g of basic charcoal that does not have supported catalyst of a certain amount of copper-based catalysts of load, regulate flue gas flow rate 0.08m 3/ h, NO concentration 650 mg/m 3, regulate microwave power and change reaction temperature, adopt the denitration effect of two kinds of different activities charcoals under the contrast condition of different temperatures, as shown in Figure 1.
Provide the embodiment of the invention below in conjunction with accompanying drawing:
Embodiment 1: Activated carbon granule is removed the impurity on surface with the abundant cleaning and removing of deionized water, fully soak the foreign ion that 6h removes charcoal absorption with deionized water again; 2. take by weighing corresponding to quality of activated carbon 0.5%Cupric oxide be carried on the active carbon with equi-volume impregnating; 3.. at 100 ℃ of vacuum drying 4h; 4.. continue 120 ℃ of vacuum drying 5h;
Embodiment 2: Activated carbon granule is removed the impurity on surface with the abundant cleaning and removing of deionized water, fully soak the foreign ion that 2h removes charcoal absorption with deionized water again; 2. take by weighing corresponding to quality of activated carbon 1%Cupric oxide be carried on the active carbon with equi-volume impregnating; 3.. at 100 ℃ of vacuum drying 4h; 4.. continue 120 ℃ of vacuum drying 5h;
Embodiment 3: Activated carbon granule is removed the impurity on surface with the abundant cleaning and removing of deionized water, fully soak the foreign ion that 4h removes charcoal absorption with deionized water again; 2. take by weighing corresponding to quality of activated carbon 5%Manganese oxide be carried on the active carbon with equi-volume impregnating; 3.. at 85 ℃ of vacuum drying 4h; 4.. continue 110 ℃ of vacuum drying 8h.
Referring to Fig. 1, the device of embodiment of the present invention method comprises that two are set up the activated carbon adsorption bed of microwave generator, two sulphur absorption cells, connecting line and several triple valves.Insert the activated carbon granule of the foregoing description supported catalyst in each adsorbent bed.Be provided with the first microwave generator 10-1 on first adsorbent bed 9-1 side, and set up the first sulfur recovery pond 11-1; Be provided with the second microwave generator 10-2 on second adsorbent bed side, and set up the second sulfur recovery pond 11-2.The device course of work is following: flue gas is sent into the first adsorbent bed 9-1 by air-introduced machine 8 through the c-a mouth of first valve 1; This adsorbent bed gets into duty; By the sulphur nitrogen oxide in the charcoal absorption flue gas, discharge through the c-b mouth of the 3rd valve 3, a – b mouth of the 7th valve 7 through the flue gas of adsorption cleaning.During the work of first adsorbent bed, second adsorbent bed is a reproduced state.Treat that the first adsorbent bed 9-1 discharges the SO in the flue gas 2And NO XWhen concentration exceeds national atmosphere pollution control criterion; The first adsorbent bed 9-1 gets into reproduced state; The second adsorbent bed 9-2 gets into duty, switches first valve 1, send c-b mouth to send into the second adsorbent bed 9-2 through first valve flue gas; By the sulphur nitrogen oxide in the charcoal absorption flue gas, discharge through the c-b mouth of the 5th valve 5, the c-b mouth of the 7th valve 7 through the flue gas of adsorption cleaning.Meanwhile, open the power supply of microwave generator 10-1, the activated carbon granule of the first adsorbent bed 9-1 is carried out microwave irradiation, the microwave irradiation frequency is 2.45GHz, makes active carbon microwave radiation under 300~600 ℃ of temperature conditions 15-30min, the sulphur nitrogen oxide that is adsorbed on activated carbon surface at high temperature is decomposed into elemental sulfur and nitrogen by carbon reduction.In the microwave irradiation process; The c-a of the 3rd valve 3 is communicated with; Be interrupted the b-c mouth and the b-a mouth that switch second valve 2; When second valve switches to during b-c mouth position, the come out gas of part of desorption gets into the first sulfur recovery pond 11-1 with sulfur vapor and reclaims elemental sulfur, and the flue gas of cleaning is through the a-c mouth discharge of the 6th valve 6; During b-a mouth position, the gas that desorption comes out returns first adsorbent bed when second valve switches to, and said process finishes until microwave irradiation, and first regeneration of adsorbent beds is accomplished.After treating that the charcoal absorption of second adsorbent bed is saturated, first adsorbent bed of regeneration activating becomes operation bed once more, and second adsorbent bed gets into reproduced state, and its process is identical with the above-mentioned first adsorbent bed irradiation process, repeats no more here.Above-mentioned two adsorbent bed work and irradiation reproduced state alternate cycles are carried out.
The present invention also can be provided with many adsorbent beds, and several adsorbent beds are worked simultaneously, and several adsorbent beds are regenerated simultaneously in addition, to satisfy big flow, high concentration gas cleaning requirement.

Claims (4)

1. the method for microwave intermitant irradiation active carbon desulfurization denitration; It is characterized in that: it is alternately adsorbed boiler smoke or the microwave irradiation processing by two or many adsorbent beds that activated carbon granule is housed; Wherein, flue gas is sent into an adsorbent bed by air-introduced machine after the dedusting, and this adsorbent bed gets into duty; By the sulphur nitrogen oxide in the charcoal absorption flue gas; After treating that the charcoal absorption of duty adsorbent bed is saturated, it is elemental sulfur and nitrogen regeneration state by the charcoal reduction decomposition that this adsorbent bed gets into isolated flue gas, flue gas is switched to another adsorbent bed that gets into duty carry out flue gas and adsorb; Said reproduced state adsorbent bed adopts the microwave irradiation activated carbon granule; The at high temperature isolated flue gas of sulphur nitrogen oxide that is adsorbed on activated carbon surface is elemental sulfur and nitrogen by the charcoal reduction decomposition, and each adsorbent bed duty and reproduced state alternate cycles are carried out, and realize the continuous purification flue gas.
2. the method for microwave intermitant irradiation active carbon desulfurization according to claim 1 denitration is characterized in that: the microwave irradiation frequency is 2.45GHz during said regeneration of adsorbent beds state, makes active carbon microwave radiation under 300~600 ℃ of temperature conditions 15-30min
3. the method for microwave intermitant irradiation active carbon desulfurization according to claim 2 denitration; It is characterized in that: add metal oxides such as cupric oxide, manganese oxide in the said active carbon as catalyst; The catalyst adition process is carried out according to following step: a. removes the impurity on surface with activated carbon granule with the abundant cleaning and removing of deionized water, fully soaks the foreign ion that 2 ~ 6h removes charcoal absorption with deionized water again; B. take by weighing corresponding to quality of activated carbon 0.5% ~ 5%Metallic catalyst be carried on the active carbon with equi-volume impregnating; C. will contain activity of such catalysts charcoal particle at 65 ~ 100 ℃ of vacuum drying 4h, continue then at 100 ~ 120 ℃ of vacuum drying 5 ~ 10h.
4. the method for microwave intermitant irradiation active carbon desulfurization according to claim 3 denitration; It is characterized in that: in the said reproduced state adsorbent bed microwave irradiation heating process; Gas that comes out through the microwave irradiation desorption in the active carbon and sulfur vapor get into the sulfur recovery pond and reclaim elemental sulfur, and cleaning flue gases is discharged.
CN201110417628.8A 2011-12-14 2011-12-14 Desulfurization and denitrification process utilizing microwave to intermittently irradiate activated carbon CN102489107B (en)

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CN111185068A (en) * 2020-01-15 2020-05-22 昆明理工大学 Method and device for removing sulfur dioxide in electrolytic aluminum flue gas by adsorption regeneration method

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CN104525116A (en) * 2014-12-31 2015-04-22 上海克硫环保科技股份有限公司 Desulfurization and denitrification modified active coke and preparation method thereof
CN106512686A (en) * 2016-11-24 2017-03-22 华中科技大学 Thermal desorption tail gas treatment system for organic contaminated soil
CN106512686B (en) * 2016-11-24 2019-03-08 华中科技大学 A kind of organic polluted soil Thermal desorption exhaust treatment system
CN110479026A (en) * 2019-07-29 2019-11-22 昆明理工大学 A kind of method and system that the hydrogen sulfide for handling arsenic-containing waste water is prepared in situ
CN111185068A (en) * 2020-01-15 2020-05-22 昆明理工大学 Method and device for removing sulfur dioxide in electrolytic aluminum flue gas by adsorption regeneration method

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