CN106268207A - The device of gas-liquid two-phase dielectric barrier discharge removing nitrogen oxides and application thereof - Google Patents
The device of gas-liquid two-phase dielectric barrier discharge removing nitrogen oxides and application thereof Download PDFInfo
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- CN106268207A CN106268207A CN201610648049.7A CN201610648049A CN106268207A CN 106268207 A CN106268207 A CN 106268207A CN 201610648049 A CN201610648049 A CN 201610648049A CN 106268207 A CN106268207 A CN 106268207A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/32—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/40—Nitrogen compounds
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/02—Other waste gases
- B01D2258/0283—Flue gases
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2259/00—Type of treatment
- B01D2259/80—Employing electric, magnetic, electromagnetic or wave energy, or particle radiation
- B01D2259/818—Employing electrical discharges or the generation of a plasma
Abstract
The device of gas-liquid two-phase dielectric barrier discharge disclosed by the invention removing nitrogen oxides and application thereof, including plasma reactor, plasma reactor has a column copper electrode and a liquid phase water electrode；Liquid phase water electrode connects ground connection stainless steel bar；The welded top of column copper electrode has stainless steel bar to connect low temperature plasma experimental power supply, and low temperature plasma experimental power supply connects oscillograph, pressure regulator；Oscillograph, pressure regulator are connected with power supply；Forming region of discharge between column copper electrode and liquid phase water electrode, there is the fibre-optical probe of spectrogrph region of discharge side, and spectrogrph is connected with computer；Plasma reactor is connected with surge flask by gas conduit a, and gas introduction tube a connects flue gas analyzer by gas introduction tube b；Surge flask connects air accumulator by trachea；Plasma reactor is connected with gas introduction tube b by fume pipe.The low temperature plasma that assembly of the invention uses gas-liquid two-phase dielectric barrier discharge to produce is made a return journey denitrification.
Description
Technical field
The invention belongs to thermal power generating technology field, be specifically related to a kind of vapor-liquid two phases dielectric barrier discharge removing nitrogen oxygen
The device of compound, the invention still further relates to utilize the device of vapor-liquid two phases dielectric barrier discharge removing nitrogen oxides to carry out removing nitrogen
The method of oxide.
Background technology
Thermal power generation is important energy industry and basic industry, to national economy, social development and people's lives water
Flat raising all has very important effect；Thermal power generation simultaneously is also main emission industry, according to statistics, and thermal power generation row
In industry, nitrogen oxide emission accounts for more than the 40% of whole nation total emission volumn.Therefore, the row of thermal power plant pollutant is effectively controlled
It is rivals in a contest the sustainable development important in inhibiting of thermal power industry.
At present, widely used remove denitrification (NOx) method be selective catalytic reduction (be called for short:
SCR).But, there are some defects, such as in catalytic reduction method in actual application: high cost and easily cause secondary pollution
And NH_3 leakage etc..
In recent years, Low Temperature Plasma Treating nitrogen oxides (NOx) is study hotspot, and the most frequently used generation low temperature etc. from
The method of daughter is dielectric barrier discharge.Dielectric barrier discharge is a kind of strong ionization discharge, and it is uniform and stable, easy that it has electric discharge
Control, utilization rate is high and is applicable to the advantage of chemical reaction, is therefore applicable to exhaust-gas treatment.
Summary of the invention
It is an object of the invention to provide the device of a kind of vapor-liquid two phases dielectric barrier discharge removing nitrogen oxides, use
The low temperature plasma that vapor-liquid two phases dielectric barrier discharge produces is made a return journey denitrification (NOx), and the method is to low-temperature plasma
The application processing nitrogen oxides (NOx) has certain directive significance.
Another object of the present invention is to provide the device utilizing vapor-liquid two phases dielectric barrier discharge removing nitrogen oxides to take off
The method of denitrification.
The present invention is used the technical scheme of the first to be that vapor-liquid two phases dielectric barrier discharge removes the dress of nitrogen oxides
Putting, include plasma reactor, plasma reactor is provided with two sparking electrodes, and a sparking electrode is column copper
Electrode, another sparking electrode is liquid phase water electrode；Liquid phase water electrode outer wall is pasted with silk screen, and liquid phase water electrode connects ground connection
Stainless steel bar, to ensure liquid phase ground connection in experimentation；It is pasted with block media on column copper electrode outer wall, and block media is
Quartz plate, the welded top of column copper electrode has stainless steel bar, in order to connect low temperature plasma experimental power supply, low-temperature plasma
Body experimental power supply connects oscillograph, pressure regulator respectively, and oscillograph is used for measuring crest voltage, current signal, pressure regulator
It is used for regulating crest voltage；Oscillograph, pressure regulator are all connected with power supply；Formed between column copper electrode and liquid phase water electrode and put
Electricity region, region of discharge side is provided with the fibre-optical probe of spectrogrph, and spectrogrph is connected with computer；Plasma reactor leads to
Crossing gas conduit a to be connected with surge flask, gas introduction tube a connects flue gas analyzer, and gas introduction tube by gas introduction tube b
It is provided with valve aF on a, gas introduction tube b is provided with valve bF；Surge flask connects two gas storage respectively by two tracheas
One effusion meter is set on tank, and every trachea；Plasma reactor is connected with gas introduction tube b also by fume pipe, and
Fume pipe is provided with circulating pump.
The feature of the first technical scheme of the present invention also resides in:
Morpho2011 software it is preset with in computer.
The parameter of spectrogrph is: FX400+, CCD:TCD1304DG-UV, grating: 600L/250nm.
The thickness of quartz plate is 0.5mm～1.5mm.
The model of low temperature plasma experimental power supply is CTP-2000K.
Oscillograph uses ADS1102 numeric type oscillograph.
The second technical scheme of the present invention is the side of vapor-liquid two phases dielectric barrier discharge removing nitrogen oxides
Method, specifically implements according to following steps:
Step 1, open two air accumulators, make N2, NO and O2, dampness mix homogeneously in surge flask, formed mixed gas；
Opening valve a and valve b, the mixed gas in surge flask, in gas introduction tube a flows into plasma reactor, is delayed simultaneously
Rush the mixed gas in bottle also in gas introduction tube b enters flue gas analyzer, flue gas analyzer observe mixed gas composition,
Effusion meter to be regulated also observes the data variation that flue gas analyzer shows, to obtain rising of nitrogen oxide NOx
Beginning concentration；
Step 2, after step 1 completes, close valve a and valve b, open circulating pump, make mix homogeneously in surge flask
Mixed gas flow in plasma reactor, and make it keep flow regime in plasma reactor；
Step 3, after step 1 and step 2 complete, open low temperature plasma experimental power supply and oscillograph, by regulation
Pressure regulator, crest voltage numerical value shown on oscillograph, also in change, stops regulation when reaching required crest voltage,
Crest voltage is 18kV～21kV, and observation oscilloscope video data；
Timing is proceeded by, in order to observe different discharge times to treatment effect while obtaining crest voltage
Impact, will control at 30s～60s the time；
Step 4, after step 3 completes, utilize spectrogrph fibre-optical probe observation OH free radical spectral intensity, and will
To the spectral intensity of OH free radical be transmitted in computer；Utilize the embedded Morpho2011 software of computer to OH free radical
Spectral intensity process, can obtain during discharging, the change of the spectral intensity of OH free radical.
Step 5, through step 4, after gas treatment 30s, open valve b；
By the concentration change of flue gas analyzer sampling analysis NO and NO2, with the gas componant after being processed；
Step 6, the data obtained through step 5 and the initial concentration of the nitrogen oxide NOx obtained through step 1 are carried out right
Ratio, after being computed, i.e. obtains nitrogen oxide NOx treatment effeciency, and specific algorithm is as follows:
In formula: C (NOX0) for processing front NO and NO2Total volume concentration, C (NOX) it is NO and NO after process2Cumulative volume dense
Degree.
In the present invention second, the feature of technical scheme also resides in:
In step 2, mixed gas flow velocity in plasma reactor is mainly controlled by circulating pump, by flow velocity control
It is made as 1L/min～4L/min.
The invention has the beneficial effects as follows:
(1) apparatus structure of vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides simply and readily operates, non-
Often it is suitable for promoting the use of.
(2) device of vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides in the application, uses solution-air two
The low temperature plasma that phase medium barrier discharge produces removes denitrification (NOx), and low-temperature plasma is processed by this achievement in research
The application of nitrogen oxides (NOx) has certain directive significance.
(3) utilizing the device of vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides, its result shows: solution-air
The OH free radical spectral intensity that two-phase medium barrier discharge produces is far longer than plate plate electrode, is more beneficial for nitrogen oxides
(NOx) removal；Improve crest voltage, gas residence time, the beneficially removing of nitrogen oxides (NOx)；Increase gas flow rate
Removal with nitrogen oxides (NOx) initial concentration suppression nitrogen oxides (NOx).
(4) device of vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides is in actual applications, for firepower
Nitrogen oxides (NOx) in power plant tail gas can effectively be removed, and alleviates thermal power plant to a certain extent dirty
Contaminate big defect, there is preferable application prospect.
Accompanying drawing explanation
Fig. 1 is the structural representation of the device of vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides；
Fig. 2 is through measuring the plate plate electrode DBD and vapor-liquid two phases DBD spectrum character diagram obtained；
Fig. 3 is the relation map of nitrogen oxides (NOx) clearance and crest voltage；
Fig. 4 is the relation map of nitrogen oxides (NOx) clearance and gas residence time；
Fig. 5 is the relation map of nitrogen oxides (NOx) clearance and gas flow rate；
Fig. 6 is the relation map of nitrogen oxides (NOx) clearance and initial concentration.
In figure, 1. effusion meter, 2. surge flask, 3. computer, 4. spectrogrph, 5. flue gas analyzer, 6. pilot plasma
Power supply, 7. oscillograph, 8. pressure regulator, 9. power supply, 10. circulating pump, 11. gas conduit a, 12. silk screens, 13. ground connection stainless steel bars,
14. block medias, 15. column copper electrodes, 16. region of discharges, 17. liquid phase water electrodes, 18. air accumulators, 19. gas conduit b,
20. fibre-optical probes, F1. valve a, F2. valve b.
Detailed description of the invention
The present invention is described in detail with detailed description of the invention below in conjunction with the accompanying drawings.
Utilizing Cement Composite Treated by Plasma waste gas, its mechanism is: comprise substantial amounts of high energy electron in plasma, they and enter
Enter the portion molecule to discharge space, hydrone collides the reactions such as combination, energy during this reaction is carried out
Generate substantial amounts of OH free radical, HO2, O isoreactivity free radical and there is the ozone O of strong oxidizing property3, they can divide with harmful gas
There is redox chemistry reaction in son, ultimately produces harmless small-molecule substance, as a example by NO, and the chemical equation tool being directed to
Body is as follows:
O2+e→e+O+O (1)；
O+O2→O3(2)；
O+HO→2OH (3)；
H2O+e→e+H+OH (4)；
NO+O→NO2(5)；
NO+O3→NO2+O2(6)；
NO+2OH→NO2+H2O (7)；
NO+HO2→NO2+OH (8)；
By above-mentioned reaction equation (1)～reaction equation (8) it can be seen that NO is at OH free radical, HO2, O isoreactivity free radical and tool
There is the ozone O of Strong oxdiative characteristic3Effect under be oxidized to NO2, it is then dissolved in water and generates nitric acid, then carry out soda acid combination generation
Corresponding salt is to reach the purpose of denitration.As can be seen here: OH free radical goes a good appetite suddenly appearing in a serious disease to play important work at nitrogen oxides (NOx)
With.
In the method for vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides, use and have liquid phase to participate in electric discharge
The device of movable vapor-liquid two phases dielectric barrier discharge removing nitrogen oxides, can draw crest voltage, gas in this course
The impact on processing nitrogen oxides (NOx) efficiency of the time of staying, gas flow rate and nitrogen oxides (NOx) initial concentration, and energy
Analyze the optical characteristics of vapor-liquid two phases dielectric barrier discharge.
The method of vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides have employed the resistance of vapor-liquid two phases medium
The device of gear electric discharge removing nitrogen oxides.
The device of vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides, its structure is as it is shown in figure 1, include
Plasma reactor, plasma reactor is provided with two sparking electrodes, and a sparking electrode is column copper electrode 15, separately
One sparking electrode is liquid phase water electrode 17；Liquid phase water electrode 17 outer wall is pasted with silk screen 12, and liquid phase water electrode 17 connects
Ground stainless steel bar 13, to ensure liquid phase ground connection in experimentation；Block media 14, and resistance it is pasted with on column copper electrode 15 outer wall
Gear medium 14 is quartz plate, and the welded top of column copper electrode 15 has stainless steel bar, in order to connect low temperature plasma experiment electricity
Source 6, low temperature plasma experimental power supply 6 connects oscillograph 7, pressure regulator 8 respectively, and oscillograph 7 is used for crest voltage, electric current letter
Number measuring, pressure regulator 8 is used for regulating crest voltage；Oscillograph 7, pressure regulator 8 are all connected with power supply 9；At column copper electrode
Forming region of discharge 16 between 15 and liquid phase water electrode 17, region of discharge 16 side is provided with the fibre-optical probe 20 of spectrogrph 4, light
Spectrometer 4 is connected with computer 3；Plasma reactor is connected with surge flask 2 by gas conduit a11, and gas introduction tube a11 leads to
Cross and be provided with valve aF1, on gas introduction tube b19 on gas introduction tube b19 connection flue gas analyzer 5, and gas introduction tube a11
It is provided with valve bF2 (gas introduction tube a11 therein and gas introduction tube b19 is used for transmitting gas)；Surge flask 2 is by two
Root trachea connects two air accumulators 18 respectively, and arranges an effusion meter 1 on every trachea；Plasma reactor is also by gas
Body canal is connected with gas introduction tube b19, and is provided with circulating pump 10 on gas conduit.
Being preset with Morpho2011 software in computer 3, this software mainly coordinates spectrogrph 4 to use, and is gathered by spectrogrph 4
To the curve of spectrum show on computers, in order to observe.
The parameter of spectrogrph 4 is: FX400+, CCD:TCD1304DG-UV, grating: 600L/250nm.
The thickness of quartz plate is 0.5mm～1.5mm.
The model of low temperature plasma experimental power supply 6 is: CTP-2000K.
Oscillograph 7 uses ADS1102 numeric type oscillograph.
The method of vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides, specifically implements according to following steps:
Step 1, open two air accumulators 18, make N2, NO and O2, dampness mix homogeneously in surge flask 2, form gaseous mixture
Body；Opening valve aF1 and valve bF2, the mixed gas in surge flask 2 flows into plasma reaction through gas introduction tube a11
In device, the mixed gas in simultaneous buffering bottle 2 is also in gas introduction tube b19 enters flue gas analyzer 5, by flue gas analyzer 5
Observing mixed gas composition, the data variation of flue gas analyzer 5 display also observed by effusion meter 1 to be regulated, with
Obtain the initial concentration of nitrogen oxide NOx.
Step 2, after step 1 completes, close valve aF1 and valve bF2, open circulating pump 10, make in surge flask 2 mixed
Close uniform mixed gas to flow in plasma reactor, and make it keep flow regime in plasma reactor；
Wherein, mixed gas flow velocity in plasma reactor is mainly controlled by circulating pump 10, preferably by flow velocity
Control as 1.5L/min～2.5L/min.
Step 3, after step 1 and step 2 complete, open low temperature plasma experimental power supply 6 and oscillograph 7, by adjust
Joint pressure regulator 8 observation oscilloscope 7 video data, just can obtain required crest voltage, preferably control crest voltage at 18kV
～21kV；(by regulation pressure regulator 8, crest voltage numerical value shown on oscillograph 7 is also in change, needed for reaching experiment
Regulation is stopped) during crest voltage；
While obtaining testing required crest voltage, when proceeding by timing in order to observe different electric discharges
Between impact on treatment effect, preferably will control at 30s～60s the time.
Step 4, after step 3 completes, utilize the fibre-optical probe 20 of spectrogrph 4 to observe spectral intensity (its of OH free radical
Middle fibre-optical probe 20 is positioned at plasma reactor region of discharge 16 side), and the spectral intensity of OH free radical that will obtain
Being transmitted in computer 3, the spectral intensity of OH free radical is processed by the Morpho2011 software utilizing computer 3 embedded,
Can obtain during discharging, the spectral intensity change of OH free radical.
Step 5, through step 4, after the required process time to be achieved (30s), open valve bF2；
By the concentration change of flue gas analyzer 5 sampling analysis NO and NO2, with the gas componant after being processed.
Step 6, the data obtained through step 5 and the initial concentration of the nitrogen oxide NOx obtained through step 1 are carried out right
Ratio, obtains nitrogen oxide NOx treatment effeciency after being computed, specific algorithm is as follows:
In above formula: C (NOX0) for processing front NO and NO2Total volume concentration, C (NOX) it is NO and NO after process2Overall
Volume concentrations.
Emission spectrographic analysis is specific as follows:
The internal active particle kind produced of vapor-liquid two phases dielectric barrier discharge plasma and relevant parameter thereof, to it
It is applied to exhaust-gas treatment field have an impact, specific as follows:
During operation, as it is shown in figure 1, the fibre-optical probe 20 of spectrogrph 4 to be arranged on the side of plasma reactor, it is used for
Measure emission spectrum.Fig. 2 gives and measures that obtain is plate plate electrode DBD during 21kV and vapor-liquid two phases DBD at applied voltage
Spectrum character diagram, as can be seen from Figure 2: obvious OH free radical can be found in the range of 309nm～313nm wavelength spectral line to compose
Tape, and under the same conditions, the OH free radical spectral intensity of vapor-liquid two phases DBD has reached about 14000, is far longer than
Plate plate electrode DBD, it is possible to draw: vapor-liquid two phases DBD having liquid phase to participate in is more suitable for the process of nitrogen oxides (NOx).
The crest voltage impact on nitrogen oxides (NOx) clearance:
The electric discharge of crest voltage plasma has critically important impact；Under normal temperature and pressure, at N2/O2/ NO/ dampness atmosphere
Under, gas flow rate is 2.5L/min, and gas residence time is 30 seconds, and gas relative humidity is 36%, and supply frequency is 11kHz,
The relation of nitrogen oxides (NOx) clearance and crest voltage is as shown in Figure 3；As shown in Figure 3: initial dense with nitrogen oxides (NOx)
Degree is for as a example by 150ppm, when crest voltage is less than 21kV, with crest voltage rising nitrogen oxides (NOx) clearance amplification relatively
Greatly, after crest voltage is more than 21kV, nitrogen oxides (NOx) clearance is close to 90%, and then crest voltage is to nitrogen oxides
(NOx) impact of clearance is little；This is because along with the rising of crest voltage, OH free radical, HO2, O isoreactivity particle and O3
Concentration increase, the reaction more promoting reaction equation (5), reaction equation (6), reaction equation (7) and reaction equation (8) is carried out, base
Whole NO is oxidized to NO by instinct2, so clearance is constant afterwards.
The gas residence time impact on nitrogen oxide removal efficiency:
Under normal temperature and pressure, at N2/O2Under/NO/ dampness atmosphere, gas flow rate is 2.5L/min, and gas relative humidity is
36%, supply frequency is 11kHz, and crest voltage is 21kV, NOx clearance with the relation of gas residence time as shown in Figure 4；By
Fig. 4 understands: as a example by 150ppm: when gas processing time is less than 30s, and nitrogen oxides (NOx) clearance has significantly increase,
When gas residence time is more than 30s, nitrogen oxides (NOx) clearance is close to 90%, and without significant change.This is because nitrogen
Oxide (NOx) gas time of staying in plasma reactor is the longest, and gas is by high energy electron, OH free radical, O and smelly
The action time of oxygen is the longest, and reaction equation (5), reaction equation (6), reaction equation (7) and reaction equation (8) are carried out time of reacting also
The longest, and make NO be oxidized to NO2Efficiency improve.After the time of staying is more than the 30s second, nitrogen oxides (NOx) and active particle
Reaction be in poised state, so the clearance change of nitrogen oxides (NOx) is little.
The gas flow rate impact on nitrogen oxides (NOx) clearance:
At N2/O2Under/NO/ dampness atmosphere, gas residence time is 30 seconds, and gas relative humidity is 36%, and supply frequency is
11kHz, when crest voltage is 21kV, the relation of nitrogen oxides (NOx) clearance and gas flow rate is as shown in Figure 5；As shown in Figure 5,
As a example by 150ppm: when gas flow rate is less than 2.5L/min, the impact of nitrogen oxides (NOx) clearance is compared by gas flow rate
Greatly；When gas flow rate is more than 2.5L/min, gas flow rate is smaller on the impact of nitrogen oxides (NOx) clearance.This is because
The little then NO of gas flow rate just increases with the collision probability of active particle in reactor, reaction equation (5), reaction equation (6), reaction equation
(7), the reaction that carried out of reaction equation (8) the most abundant, NO oxygenation efficiency is the highest, so nitrogen oxides (NOx) clearance liter
High.But when gas flow rate is excessive, on the one hand because the active particle number being activated in unit volume declines, on the other hand it is
NO reduces, so causing nitrogen oxides (NOx) clearance to reduce with the collision probability of active particle in reactor.
The initial concentration impact on nitrogen oxides (NOx) clearance:
At N2/O2Under/NO/ dampness atmosphere, gas residence time is 30 seconds, and gas relative humidity is 36%, and supply frequency is
11kHz, when crest voltage is 21kV, the relation of nitrogen oxides (NOx) clearance and initial concentration is as shown in Figure 6；During operation, point
Not taking gas flow rate is that 1L/min, 2L/min, 3L/min contrast；As shown in Figure 6: the clearance of nitrogen oxides (NOx) with
The increase of nitrogen oxides (NOx) initial concentration first to increase and reduce afterwards；As a example by gas flow rate is as 1L/min: work as nitrogen oxides
(NOx), when initial concentration is less than 150ppm, nitrogen oxides (NOx) clearance is in increasing trend and close to 90%, when nitrogen aoxidizes
When thing (NOx) initial concentration is more than 150ppm, nitrogen oxides (NOx) clearance is in reducing trend.This is because certain defeated
Enter and a certain amount of active particle under power, can only be produced, and a certain amount of NO is oxidized to NO2.As can be seen here: select suitably
Nitrogen oxides (NOx) initial concentration is conducive to the removal of nitrogen oxides (NOx).
Vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides method show: vapor-liquid two phases DBD compared to
Plate plate electrode DBD can produce more OH free radical, is more suitable for the removal of nitrogen oxides (NOx).It addition, solution-air of the present invention
The method of two-phase medium barrier discharge removing nitrogen oxides also utilize vapor-liquid two phases DBD reactor to investigate reaction condition pair
The impact of nitrogen oxides (NOx) clearance: nitrogen oxides (NOx) clearance raises with the rising of voltage peak；Stop with gas
The increase staying the time first increases and then tends to be steady；Reduce with the increase of gas flow rate；First increase with the increase of NOx initial concentration
Reduce after adding.As can be seen here: vapor-liquid two phases dielectric barrier discharge plasma is for the nitrogen oxides in thermal power plant's tail gas
(NOx) can effectively remove, there is preferable application prospect.
Plasma collides at discharge space and portion molecule, hydrone the reactions such as combination, generates substantial amounts of
OH free radical, HO2, O isoreactivity free radical and there is the O of strong oxidizing property3, they occur redox chemistry to react generation with NO
NO2, NO2Generate nitric acid after being dissolved in water, then carry out soda acid and combine the corresponding salt of generation to reach the purpose of denitration.
The device utilizing vapor-liquid two phases dielectric barrier discharge of the present invention removing nitrogen oxides carries out removing the side of nitrogen oxides
Method has that low cost, plant area area be little and the advantage of non-secondary pollution.And the more important thing is: vapor-liquid two phases dielectric impedance
The produced OH free radical isoreactivity number of free radical of electric discharge is significantly larger than produced by conventional panels plate electrode dielectric barrier discharge,
Therefore the removing of nitrogen oxides (NOx) it is more beneficial for.
Claims (8)
1. the device of vapor-liquid two phases dielectric barrier discharge removing nitrogen oxides, it is characterised in that include plasma reaction
Device, described plasma reactor is provided with two sparking electrodes, and a sparking electrode is column copper electrode (15), and another is put
Electricity electrode is liquid phase water electrode (17)；Described liquid phase water electrode (17) outer wall is pasted with silk screen (12), and liquid phase water electrode (17)
Connect ground connection stainless steel bar (13), to ensure liquid phase ground connection in experimentation；It is pasted with on described column copper electrode (15) outer wall
Block media (14), and block media (14) is quartz plate, the welded top of described column copper electrode (15) has stainless steel bar, uses
To connect low temperature plasma experimental power supply (6), described low temperature plasma experimental power supply (6) connects oscillograph (7) respectively, adjusts
Depressor (8), described oscillograph (7) is used for measuring crest voltage, current signal, and described pressure regulator (8) is used for regulating peak
Threshold voltage；Described oscillograph (7), pressure regulator (8) are all connected with power supply (9)；
Region of discharge (16), described region of discharge (16) is formed between described column copper electrode (15) and liquid phase water electrode (17)
Side is provided with the fibre-optical probe (20) of spectrogrph (4), and described spectrogrph (4) is connected with computer (3)；
Described plasma reactor is connected with surge flask (2) by gas conduit a (11), and described gas introduction tube a (11) is led to
Cross gas introduction tube b (19) and connect flue gas analyzer (5), and on described gas introduction tube a (11), be provided with valve a (F1), gas
Valve b (F2) it is provided with on body ingress pipe b (19)；
Described surge flask (2) connects two air accumulators (18) respectively by two tracheas, and arranges a flow on every trachea
Meter (1)；Described plasma reactor is connected with gas introduction tube b (19) also by fume pipe, and is provided with on fume pipe
Circulating pump (10).
The device of vapor-liquid two phases dielectric barrier discharge the most according to claim 1 removing nitrogen oxides, it is characterised in that
Described computer is preset with Morpho2011 software in (3).
The device of vapor-liquid two phases dielectric barrier discharge the most according to claim 1 removing nitrogen oxides, it is characterised in that
The parameter of described spectrogrph (4) is: FX400+, CCD:TCD1304DG-UV, grating: 600L/250nm.
The device of vapor-liquid two phases dielectric barrier discharge the most according to claim 1 removing nitrogen oxides, it is characterised in that
The thickness of quartz plate is 0.5mm～1.5mm.
The device of vapor-liquid two phases dielectric barrier discharge the most according to claim 1 removing nitrogen oxides, it is characterised in that
The model of described low temperature plasma experimental power supply (6) is CTP-2000K.
The device of vapor-liquid two phases dielectric barrier discharge the most according to claim 1 removing nitrogen oxides, it is characterised in that
Described oscillograph (7) uses ADS1102 numeric type oscillograph.
7. the method for vapor-liquid two phases dielectric barrier discharge removing nitrogen oxides, it is characterised in that the method depends on claim
The device of the vapor-liquid two phases dielectric barrier discharge removing nitrogen oxides described in 1, specifically implements according to following steps:
Step 1, open two air accumulators (18), make N2, NO and O2, dampness mix homogeneously in surge flask (2), form gaseous mixture
Body；Open valve a (F1) and valve b (F2), the mixed gas in surge flask (2) through gas introduction tube a (11) flow into wait from
In daughter reactor, the mixed gas in simultaneous buffering bottle (2) also in gas introduction tube b (19) enters flue gas analyzer (5),
Being observed mixed gas composition by flue gas analyzer (5), effusion meter to be regulated (1) also observes flue gas analyzer
(5) data variation shown, to obtain the initial concentration of nitrogen oxide NOx；
Step 2, after step 1 completes, close valve a (F1) and valve b (F2), open circulating pump (10), make surge flask (2)
The mixed gas of interior mix homogeneously flows in plasma reactor, and makes it keep the shape that flows in plasma reactor
State；
Step 3, after step 1 and step 2 complete, open low temperature plasma experimental power supply (6) and oscillograph (7), by adjust
Joint pressure regulator (8), the upper shown crest voltage numerical value of oscillograph (7) is also in change, when reaching required crest voltage
Stopping regulation, crest voltage is 18kV～21kV, and observation oscilloscope (7) video data；
Timing is proceeded by, in order to observe the different discharge times of the shadow to treatment effect while obtaining crest voltage
Ring, will control at 30s～60s the time；
Step 4, after step 3 completes, utilize spectrogrph (4) fibre-optical probe (20) observation OH free radical spectral intensity, and
The spectral intensity of the OH free radical obtained is transmitted in computer (3)；Utilize the Morpho2011 software that computer (3) is embedded
The spectral intensity of OH free radical is processed, can obtain during discharging, the spectral intensity change of OH free radical；
Step 5, through step 4, after gas treatment 30s, open valve b (F2)；
By the concentration change of flue gas analyzer (5) sampling analysis NO and NO2, with the gas componant after being processed；
Step 6, the initial concentration of the data obtained through step 5 with the nitrogen oxide NOx obtained through step 1 is contrasted, warp
After calculating, i.e. obtaining nitrogen oxide NOx treatment effeciency, specific algorithm is as follows:
In formula: C (NOX0) for processing front NO and NO2Total volume concentration, C (NOX) it is NO and NO after process2Total volume concentration.
The method of vapor-liquid two phases dielectric barrier discharge the most according to claim 7 removing nitrogen oxides, it is characterised in that
In described step 2, mixed gas flow velocity in plasma reactor is mainly controlled by circulating pump (10), by flow velocity control
It is made as 1.5L/min～2.5L/min.
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