CN102240500A - System and process for desulfuration and denitration by pure oxygen dielectric barrier discharge in flue - Google Patents
System and process for desulfuration and denitration by pure oxygen dielectric barrier discharge in flue Download PDFInfo
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- CN102240500A CN102240500A CN2011101772176A CN201110177217A CN102240500A CN 102240500 A CN102240500 A CN 102240500A CN 2011101772176 A CN2011101772176 A CN 2011101772176A CN 201110177217 A CN201110177217 A CN 201110177217A CN 102240500 A CN102240500 A CN 102240500A
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Abstract
The invention relates to a system and a process for desulfuration and denitration by pure oxygen dielectric barrier discharge in a flue, and belongs to the technical field of the desulfuration and denitration of flue gas in heat-engine plants. In the process, air is separated by an air separator, and separated oxygen enters a dielectric barrier discharge reactor; O2 molecules are activated, cracked or ionized in the reactor to form free radicals O or O3 and the like which have high oxidability; the oxidizing gas which is subjected to discharging is mixed with the flue gas quickly and fully through a spray device to be subjected to reaction, so that NO and SO2 in the flue gas are oxidized to form high-valence nitric oxides and high-valence sulfur oxides; and the oxidized flue gas enters an alkali liquor absorption tower, and is washed by alkali liquor to fulfill the aims of removing the nitric oxides and the sulfur oxides. In the process, due to pure oxygen discharging, the cost of producing the free radicals is low, the free radicals and the flue gas are mixed early, the removal efficiency of pollutants is high, the economic benefit is higher, and nitrates, nitrites, sulfates and the like are used as products to be recovered to realize the environment-friendly recycling of the pollutants.
Description
Technical field
The invention belongs to flue gas desulphurization denitration technology field, pure oxygen dielectric barrier discharge system for desulfuration and denitration and technology in particularly a kind of flue.
Background technology
SO in the flue gas of thermal power plant
2With NOx be gas pollutant main in the atmosphere, it not only brings various harm to human body, and can produce very big influence to vegeto-animal growth and to weather and weather, therefore must take measures to be controlled.And outstanding flue gases purification not only needs to satisfy removal efficiency efficiently, but also will consider the simple operability of technical economy and system, and at present numerous researchers is consistent, and that admit is SO
2Remove with the integrated of NOx.
And thermal power plant generally adopts two covering devices respectively flue gas to be carried out the desulphurization denitration processing at present, and that flue gas desulfurization is mainly adopted is wet fuel gas desulfurizing technology (Wet-FGD), and what denitrating flue gas then adopted is with NH
3Be the SCR technology (SCR) of reducing agent, wherein wet fuel gas desulfurizing technology is done desulfurization absorbent with lime stone or lime, mixes with water behind the limestone crushing, and pulverize is made the absorption slurries.In the absorption tower, the SO in the flue gas
2With the CaCO in the slurries
3And the oxidation air that blasts carries out chemical reaction to generate calcium sulphate dihydrate is gypsum, makes the SO in the flue gas
2Removed.Key reaction equation in the wet desulfurizing process process is:
2CaCO
3+H
2O+2SO
2→2CaSO
3·1/2H
2O+2CO
2↑
2CaCO
3·1/2H
2O+O
2+3H
2O→2CaSO
4·2H
2O
The SCR technology is meant at O
2Under the condition that exists with heterogeneous catalysis, with NH
3As reducing agent, under the flue-gas temperature between economizer and the air preheater, NOx is reduced to harmless nitrogen G﹠W.Main reaction equation is as follows:
4NO+4NH
3+O
2→4N
2+6H
2O
2NO
2+4NH
3+O
2→3N
2+6H
2O
NO+NO
2+2NH
3+O
2→2N
2+3H
2O
Publication number is that the patent of invention of CN1768902 and CN1923341 has been introduced a kind of method of boiler smoke oxidizing and denitrating ozone and the devices and methods therefor of coal-burning boiler fume ozone oxidation and simultaneous desulfurization denitration respectively, ozone generator places the low temperature flue outside in the patent, the ozone that generates sprays in the flue and mixes with flue gas, make nitrogen oxide and oxidize sulfur oxides, afterbody adopts alkali lye to absorb, this flow process can obtain more satisfactory removal efficiency, but in the commercial Application process, the ozone that produces will react apart from mixing with flue gas through long, cause the ozone depletion amount more, increase the cost of desulphurization denitration.
At present the power plants system for desulfuration and denitration adopts substantially be wet desulfurizing process in conjunction with the SCR denitration, guarantee to some extent though install on denitrification efficiency two cover systems the time, also brought inevitable shortcoming:
(1) system complex, the operation maintenance amount is big;
(2) initial investment expense height, equipment manufacturing cost is high;
(3) since in China's fire coal sulphur content content higher, easily cause the dust stratification and the obstruction of catalyst poisoning in the SCR system and air preheater;
(4) be unfavorable for the transformation of old power plant.
Though the desulfurizing and denitrifying process removal efficiency of ozone is higher, but because ozone generator is arranged on outside the flue, after ozone takes place, experiencing a segment distance just can enter flue and mix with flue gas, and the ozone with strong oxidizing property with the flue gas hybrid reaction before will part and other substance reaction, ozone self also can partly decompose, and has caused the unnecessary consumption of ozone, caused equipment and corrosive pipeline simultaneously, operating cost is high.
Summary of the invention
The invention provides a kind of recycling that can realize nitrogen oxide, oxysulfide, improve the interior pure oxygen dielectric barrier discharge system for desulfuration and denitration of flue and the technology of the economic benefit of desulphurization denitration.
The structure of system of the present invention is: the arrival end of electric cleaner is connected with exhanst gas outlet, the port of export of electric cleaner is connected by the former fume side inlet of flue and gas-gas heater, and the former fume side outlet of gas-gas heater is connected by the smoke inlet of smokejack with bottom, alkali lye absorption tower; The dielectric barrier discharge reactor is arranged in described flue or the smokejack, and the arrival end of dielectric barrier discharge reactor is connected with air separator; The bottom on alkali lye absorption tower is communicated with the alkali lye liquid storage tank by pipeline, and the top on alkali lye absorption tower is provided with spray equipment, and the liquid outlet of alkali lye liquid storage tank is communicated with described spray equipment by pipeline and peristaltic pump; The top on alkali lye absorption tower sets out gas port, is connected by the clean smoke inlet end of pipeline and gas-gas heater, and the port of export of the clean flue gas of gas-gas heater is connected with chimney.
In the described alkali lye absorption tower, the top of spray equipment is provided with demister.
The outlet of described dielectric barrier discharge reactor is connected with nozzle by Venturi tube, this nozzle is the flaring structure along axis direction, the spout head is a spherical cap structure, evenly distribute on the spherical crown 5 by " ten " font arrange, respectively perpendicular to the playpipe that reduces to Way out of spherical crown surface, 5 playpipes lay respectively at four end points and the center of " ten " word.
The flaring angle [alpha] of described outlet nozzle is 25 °-60 °, and axial length L is 30-50mm.
The length of described playpipe is 10-20mm, and the diameter of " ten " word central-injection pipe outlet is 8-15mm, and four playpipe outlet diameters are 5-10mm all around.
The present invention also provides a kind of flue gas desulfurization and denitration technique based on described system, is divided into following steps:
(1) enters flue after the dedusting of flue gas process electric cleaner; After the pure qi (oxygen) of the flue gas of handling after gas-gas heater and alkali lye absorb carries out heat exchange, reduce temperature to 40～60 ℃, enter the alkali lye absorption tower by smokejack then;
(2) after air separates through air separator, oxygen enters the dielectric barrier discharge reactor that is placed in described flue or the smokejack, by the voltage of regulating high voltage source, the discharge power in the FREQUENCY CONTROL reactor, even, stable discharge takes place in reactor, wherein the voltage-regulation scope is 6～20kV, frequency-tuning range is 7～15kHz, and velocity ratio flue gas flow velocity flue in the high 20%-60% of oxygen in the dielectric barrier discharge reactor; The high energy electron that discharge generation is a large amount of, and from the ejection of the nozzle of dielectric barrier discharge reactor;
(3) under the effect of high energy electron, O
2, H
2The O molecule is activated, cracking or ionization, produces to comprise O, O
3, OH, HO
2Highly active oxidisability particle interior makes NO, SO in the flue gas
2Oxidation, the oxidation product of NO is mainly NO
2And a spot of HNO
3, HNO
2With the nitrogen oxide of other high valence states, SO
2Oxidation product be mainly SO
3, under the water vapour content condition with higher, can further generate sulfuric acid;
(4) configuration alkali lye, alkali lye by peristaltic pump by top, absorption tower in spray equipment enters the alkali lye absorption tower, in the alkali lye absorption tower with behind the smoke reaction, discharge by the tower bottom, enter the alkali lye reservoir; Flue gas through the dielectric barrier discharge reactor for treatment is entered by bottom, alkali lye absorption tower, and is discharged by top, alkali lye absorption tower behind the alkaline reaction;
(5) low-temperature flue gas of discharging from the alkali lye absorption tower is sent in the gas-gas heater, and delivers to chimney after the high-temperature flue gas heat exchange and discharges.
Alkali lye in the described step (2) is for comprising KOH, Na
2CO
3, Ca (OH)
2, CaCO
3NaOH solution, wherein NaOH in the alkali lye, KOH's and with flue gas in SO
2With NO after the oxidation
2And the mole value ratio be 1.8～2.6, Na
2CO
3, Ca (OH)
2, CaCO
3And with flue gas in SO
2With NO after the oxidation
2And the mole value ratio be 0.9～1.3.
Behind described alkali lye and the smoke reaction, flow in the alkali lye reservoir, obtain nitrate, nitrite, sulfate mixed solution,, obtain corresponding nitrate, nitrite and sulfate through pervaporation, crystallization, separation circuit.
Beneficial effect of the present invention is:
(1) desulphurization denitration equipment and technological process have been simplified;
Can not cause the wearing and tearing of back-end ductwork and the dust stratification and the blockage problem of air preheater when (2) burning sulphur coal;
(3) sulfate, nitrate and nitrite reclaim as product, have realized that the green of resource is recycled, and have increased economic benefit simultaneously;
(4) discharge at pure oxygen, the cost that produces free radical is low; The DBD reactor places flue, and free radical can be fast by injection apparatus and the flue gas hybrid reaction, improved removal efficiency.
Description of drawings
Fig. 1 is the structural representation of dielectric barrier discharge reactor at gas-solid/liquid/gas reactions device gas approach;
Fig. 2 is the structural representation of dielectric barrier discharge reactor at gas-solid/liquid/gas reactions device exhaust pass;
Fig. 3 is the sectional view of dielectric barrier discharge reactor outlet nozzle;
Fig. 4 is the playpipe distribution schematic diagram of nozzle.
Number in the figure:
The 1-electric cleaner; 2-dielectric barrier discharge reactor; The 3-air separator; The 4-flue; The 5-gas-gas heater; The 6-smokejack; 7-alkali lye absorption tower; 8-alkali lye liquid storage tank; The 9-demister; The 10-chimney.
The specific embodiment
The invention provides pure oxygen dielectric barrier discharge system for desulfuration and denitration and technology in a kind of flue, the present invention will be further described below in conjunction with the drawings and specific embodiments.
As Fig. 1 or shown in Figure 2, the arrival end of electric cleaner 1 is connected with exhanst gas outlet, the port of export of electric cleaner 1 is connected with gas-gas heater 5 former smoke inlet ends by flue 4, and gas-gas heater 5 former smoke outlets are connected with the smoke inlet of 7 bottoms, alkali lye absorption tower by smokejack 6; Dielectric barrier discharge reactor 2 is arranged in described flue 4 or the smokejack 6, and the arrival end of dielectric barrier discharge reactor 2 is connected with air separator 3; The bottom on alkali lye absorption tower 7 is communicated with alkali lye liquid storage tank 8 by pipeline, and the top on alkali lye absorption tower 8 is provided with spray equipment, and the top of spray equipment is provided with demister 9; The liquid outlet of alkali lye liquid storage tank 8 is communicated with described spray equipment by pipeline and peristaltic pump; The top on alkali lye absorption tower 7 sets out gas port, is connected by the arrival end of pipeline with gas-gas heater 5 clean flue gases, and the port of export of gas-gas heater 5 clean flue gases is connected with chimney 10.
The outlet of dielectric barrier discharge reactor 2 is connected with nozzle by Venturi tube.As shown in Figure 3 and Figure 4, this nozzle is the flaring structure along axis direction, the spout head is a spherical cap structure, evenly distribute on the spherical crown 5 by " ten " font arrange, respectively perpendicular to the playpipe that reduces to Way out of spherical crown surface, 5 playpipes lay respectively at four end points and the center of " ten " word.The flaring angle [alpha] of outlet nozzle is 25 °-60 °, and axial length L is 30-50mm.The length of playpipe is 10-20mm, and the diameter of " ten " word central-injection pipe outlet is 8-15mm, and four playpipe outlet diameters are 5-10mm all around.
The flow process of this system is as follows: at first isolate airborne nitrogen through air separator, remaining oxygen is introduced the dielectric barrier discharge reactor that is put in the flue, by regulating power source voltage (adjustable range 6～20kV), the frequency (discharge power in adjustable range 7～15kHz) the control reactors, make it that more even, stable discharge take place in reactor, the high energy electron that discharge generation is a large amount of, under the effect of high energy electron, oxygen molecule in the reactor is activated, cracking or ionization, produces highly active oxidisability particle such as O, O
3Mix with flue gas in the flue Deng rapidly flowing out spout, reduced, make NO and SO partly in the flue gas along the loss of active group in the journey
2Oxidation, the oxidation product of NO is mainly NO
2, NO
3And a spot of other high valence state nitrogen oxide, SO
2Oxidation product be mainly SO
3, under the water vapour content condition with higher, can further generate sulfuric acid.Dielectric barrier discharge reactor outside parcel Antiwear casing, oxygen gas flow rate should be selected OK range in it, the too high meeting of flow velocity reduces the productive rate of high mars free radical, flow velocity is crossed the low disturbance that can weaken exit and flue gas, influence the mixing of two strands of gases, therefore oxygen gas flow rate is crossed and is exceeded the low removal efficiency that all can influence nitrogen oxide and oxysulfide, and the interior flue gas flow rate of oxygen gas flow rate flue is high by 20%～60% in the regulation dielectric barrier discharge reactor.Relevant reaction equation is as follows:
NO+O+M→NO
2+M，
O
3+NO→NO
2+O
2，
O
3+NO
2→NO
3+O
2，
NO
3+NO→2NO
2，
SO
2+O+O
2→SO
3+O
2，
O
3+SO
2→O
2+SO
3，
H
2O+SO
3→H
2SO
4，
Abundant reacted flue gas is introduced into the alkali lye absorption tower.Configuration comprises KOH, Na
2CO
3, Ca (OH)
2, CaCO
3NaOH solution as the alkali lye of smoke treatment, wherein NaOH in the alkali lye, KOH's and with flue gas in SO
2With NO after the oxidation
2And the mole value ratio be 1.8～2.6, Na
2CO
3, Ca (OH)
2, CaCO
3And with flue gas in SO
2With NO after the oxidation
2And the mole value ratio be 0.9～1.3.Alkali lye by peristaltic pump by top, absorption tower in spray equipment enters tower, behind Ta Nei and smoke reaction, discharge by the tower bottom, enter reservoir.The flue gas of handling through oxidizing gas is entered by the tower bottom, fully reacting the back by absorption tower and alkali lye is discharged by cat head, absorb solution such as nitrate that the back generated, sulfate through alkali lye and produce qualified product through operations such as pervaporation, crystallization, separation and be installed into to be on sale throughout through bag again and sell, created the recycling that economic benefit has realized resource.
Oxygen mixes with flue gas then at first through the low temperature plasma oxidation processes in this combined desulfurization and denitrification process, and the flue gas after the oxidation is done further to absorb by alkali lye, and the flue gas after handling at last enters atmosphere, and wherein the removal efficiency of NOx can reach more than 80%, SO
2Removal efficiency can reach more than 90%.
Case study on implementation one: as shown in Figure 1, the dielectric barrier discharge reactor places in the electric cleaner flue afterwards, according to different unit loads with choose the number of dielectric barrier discharge reactor monomer and the flow velocity by oxygen in the reactor, reactor is evenly arranged in flue, is made the oxidizing gas of ejection fully mix, to react with flue gas.Alkali lye adopts NaOH, KOH, Na in the absorption tower
2CO
3, Ca (OH)
2, CaCO
3Wherein a kind of or wherein several mixed liquor.
Case study on implementation two: as shown in Figure 2, the dielectric barrier discharge reactor places in the smokejack between the inlet of gas-gas heater and alkali lye absorption tower, and the reduction of flue-gas temperature is beneficial to the oxidation of NO.Choose the number of dielectric barrier discharge reactor monomer and the flow velocity that passes through oxygen in the reactor according to the unit different load, reactor is evenly arranged in flue, is made the oxidizing gas of ejection fully mix, to react with flue gas.Alkali lye adopts NaOH, KOH, Na in the absorption tower
2CO
3, Ca (OH)
2, CaCO
3Wherein a kind of or wherein several mixed liquor.
Claims (8)
1. pure oxygen dielectric barrier discharge system for desulfuration and denitration in the flue, it is characterized in that, the arrival end of electric cleaner is connected with exhanst gas outlet, the port of export of electric cleaner is connected by the former fume side inlet of flue and gas-gas heater, and the former fume side outlet of gas-gas heater is connected by the smoke inlet of smokejack with bottom, alkali lye absorption tower; The dielectric barrier discharge reactor is arranged in described flue or the smokejack, and the arrival end of dielectric barrier discharge reactor is connected with air separator; The bottom on alkali lye absorption tower is communicated with the alkali lye liquid storage tank by pipeline, and the top on alkali lye absorption tower is provided with spray equipment, and the liquid outlet of alkali lye liquid storage tank is communicated with described spray equipment by pipeline and peristaltic pump; The top on alkali lye absorption tower sets out gas port, is connected by the clean smoke inlet end of pipeline and gas-gas heater, and the clean smoke outlet of gas-gas heater is connected with chimney.
2. pure oxygen dielectric barrier discharge system for desulfuration and denitration in the flue according to claim 1 is characterized in that in the described alkali lye absorption tower, the top of spray equipment is provided with demister.
3. pure oxygen dielectric barrier discharge system for desulfuration and denitration in the flue according to claim 1, it is characterized in that, the outlet of described dielectric barrier discharge reactor is connected with nozzle by Venturi tube, this nozzle is the flaring structure along axis direction, the spout head is a spherical cap structure, evenly distribute on the spherical crown 5 by " ten " font arrange, respectively perpendicular to the playpipe that reduces to Way out of spherical crown surface, 5 playpipes lay respectively at four end points and the center of " ten " word.
4. pure oxygen dielectric barrier discharge system for desulfuration and denitration in the flue according to claim 3 is characterized in that the flaring angle [alpha] of described outlet nozzle is 25 °-60 °, and axial length L is 30-50mm.
5. pure oxygen dielectric barrier discharge system for desulfuration and denitration in the flue according to claim 3, it is characterized in that, the length of described playpipe is 10-20mm, and the diameter of " ten " word central-injection pipe outlet is 8-15mm, and four playpipe outlet diameters are 5-10mm all around.
6. the flue gas desulfurization and denitration technique based on the described system of claim 1 is characterized in that, is divided into following steps:
(1) enters flue after the dedusting of flue gas process electric cleaner; After the pure qi (oxygen) of the flue gas of handling after gas-gas heater and alkali lye absorb carries out heat exchange, reduce temperature to 40～60 ℃, enter the alkali lye absorption tower by smokejack then;
(2) after air separates through air separator, oxygen enters the dielectric barrier discharge reactor that is placed in described flue or the smokejack, by the voltage of regulating high voltage source, the discharge power in the FREQUENCY CONTROL reactor, even, stable discharge takes place in reactor, wherein the voltage-regulation scope is 6～20kV, frequency-tuning range is 7～15kHz, and velocity ratio flue gas flow velocity flue in the high 20%-60% of oxygen in the dielectric barrier discharge reactor; The high energy electron that discharge generation is a large amount of, and from the ejection of the nozzle of dielectric barrier discharge reactor;
(3) under the effect of high energy electron, O
2, H
2The O molecule is activated, cracking or ionization, produces to comprise O, O
3, OH, HO
2Highly active oxidisability particle interior makes NO, SO in the flue gas
2Oxidation, the oxidation product of NO is mainly NO
2And a spot of HNO
3, HNO
2With the nitrogen oxide of other high valence states, SO
2Oxidation product be mainly SO
3, under the water vapour content condition with higher, can further generate sulfuric acid;
(4) configuration alkali lye, alkali lye by peristaltic pump by top, absorption tower in spray equipment enters the alkali lye absorption tower, in the alkali lye absorption tower with behind the smoke reaction, discharge by the tower bottom, enter the alkali lye reservoir; Flue gas through the dielectric barrier discharge reactor for treatment is entered by bottom, alkali lye absorption tower, and is discharged by top, alkali lye absorption tower behind the alkaline reaction;
(5) low-temperature flue gas of discharging from the alkali lye absorption tower is sent in the gas-gas heater, and delivers to chimney after the high-temperature flue gas heat exchange and discharges.
7. flue gas desulfurization and denitration technique according to claim 6 is characterized in that, the alkali lye in the described step (2) is for comprising KOH, Na
2CO
3, Ca (OH)
2, CaCO
3NaOH solution, wherein NaOH in the alkali lye, KOH's and with flue gas in SO
2With NO after the oxidation
2And the mole value ratio be 1.8～2.6, Na
2CO
3, Ca (OH)
2, CaCO
3And with flue gas in SO
2With NO after the oxidation
2And the mole value ratio be 0.9～1.3.
8. flue gas desulfurization and denitration technique according to claim 6, it is characterized in that, behind described alkali lye and the smoke reaction, flow in the alkali lye reservoir, obtain nitrate, nitrite, sulfate mixed solution, through pervaporation, crystallization, separation circuit, obtain corresponding nitrate, nitrite and sulfate.
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| CN102500210A (en) * | 2012-01-04 | 2012-06-20 | 山东电力研究院 | System for removing elementary mercury from smoke by adopting injection type discharging activation method |
| CN103950907A (en) * | 2014-05-05 | 2014-07-30 | 李治 | Method for converting nitric oxides to nitric acid |
| CN106064017A (en) * | 2016-08-08 | 2016-11-02 | 辽宁信威环保科技有限公司 | Oxidoreduction is with journey desulfuring and denitrifying apparatus |
| CN106422715A (en) * | 2016-07-12 | 2017-02-22 | 湖南商学院 | Integrated wet-process flue gas purifying system and flue gas purifying method |
| CN107131517A (en) * | 2016-02-26 | 2017-09-05 | 杭州中兵环保股份有限公司 | A kind of ozone oxidation lifts the device and method of SNCR denitration efficiency |
| CN107921166A (en) * | 2015-06-09 | 2018-04-17 | 约翰·斯斐恩 | Plasma jet air filtration and sterilization system |
| WO2018068548A1 (en) * | 2016-10-12 | 2018-04-19 | 广东佳德环保科技有限公司 | Oxidation method for sintering flue gas denitrification and system |
| CN108246071A (en) * | 2018-03-28 | 2018-07-06 | 昆明理工大学 | A kind of adjustable throat inlet Venturi tube strong ionization discharge desulfuring and denitrifying apparatus |
| CN108636085A (en) * | 2018-04-24 | 2018-10-12 | 北京宜泽环保科技有限责任公司 | A kind of high-pressure discharging device and exhaust treatment system |
| CN110302623A (en) * | 2019-04-15 | 2019-10-08 | 杭州双良中荷环保科技有限公司 | A kind of technique of flue gas of refuse burning plasma cooperation-removal pollutant |
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| CN102500210B (en) * | 2012-01-04 | 2014-12-10 | 国家电网公司 | System for removing elementary mercury from smoke by adopting injection type discharging activation method |
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| WO2018068548A1 (en) * | 2016-10-12 | 2018-04-19 | 广东佳德环保科技有限公司 | Oxidation method for sintering flue gas denitrification and system |
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Application publication date: 20111116 |