CN101773780A - Method for depriving nitric oxide by plasma cooperating with low-temperature catalytic oxidation NO - Google Patents
Method for depriving nitric oxide by plasma cooperating with low-temperature catalytic oxidation NO Download PDFInfo
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- CN101773780A CN101773780A CN201010130186A CN201010130186A CN101773780A CN 101773780 A CN101773780 A CN 101773780A CN 201010130186 A CN201010130186 A CN 201010130186A CN 201010130186 A CN201010130186 A CN 201010130186A CN 101773780 A CN101773780 A CN 101773780A
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- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 title claims abstract description 69
- 238000000034 method Methods 0.000 title claims abstract description 26
- 230000003197 catalytic effect Effects 0.000 title claims abstract description 13
- 238000007254 oxidation reaction Methods 0.000 title claims abstract description 12
- 230000003647 oxidation Effects 0.000 title claims abstract description 11
- 239000003054 catalyst Substances 0.000 claims abstract description 15
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 13
- 239000008246 gaseous mixture Substances 0.000 claims description 10
- 229910001220 stainless steel Inorganic materials 0.000 claims description 10
- 239000010935 stainless steel Substances 0.000 claims description 10
- 230000004913 activation Effects 0.000 claims description 8
- 238000006243 chemical reaction Methods 0.000 claims description 7
- 229910000831 Steel Inorganic materials 0.000 claims description 5
- 239000003595 mist Substances 0.000 claims description 5
- 239000010959 steel Substances 0.000 claims description 5
- 238000003780 insertion Methods 0.000 claims description 2
- 230000037431 insertion Effects 0.000 claims description 2
- 230000004888 barrier function Effects 0.000 claims 1
- 238000005265 energy consumption Methods 0.000 abstract description 4
- 230000001590 oxidative effect Effects 0.000 abstract description 4
- 230000000694 effects Effects 0.000 abstract description 3
- 238000012545 processing Methods 0.000 abstract description 3
- 230000002411 adverse Effects 0.000 abstract description 2
- 239000012535 impurity Substances 0.000 abstract description 2
- 230000003213 activating effect Effects 0.000 abstract 1
- 239000007789 gas Substances 0.000 description 15
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 11
- 238000010521 absorption reaction Methods 0.000 description 10
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 9
- 239000012153 distilled water Substances 0.000 description 6
- 238000005516 engineering process Methods 0.000 description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 6
- 229910016978 MnOx Inorganic materials 0.000 description 5
- 125000002924 primary amino group Chemical group [H]N([H])* 0.000 description 5
- 235000011121 sodium hydroxide Nutrition 0.000 description 5
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 4
- 239000003513 alkali Substances 0.000 description 4
- 238000010531 catalytic reduction reaction Methods 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 238000003756 stirring Methods 0.000 description 4
- 238000005303 weighing Methods 0.000 description 4
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 3
- 229910010413 TiO 2 Inorganic materials 0.000 description 3
- 238000002485 combustion reaction Methods 0.000 description 3
- 238000006477 desulfuration reaction Methods 0.000 description 3
- 230000023556 desulfurization Effects 0.000 description 3
- 239000003546 flue gas Substances 0.000 description 3
- 229940071125 manganese acetate Drugs 0.000 description 3
- UOGMEBQRZBEZQT-UHFFFAOYSA-L manganese(2+);diacetate Chemical compound [Mn+2].CC([O-])=O.CC([O-])=O UOGMEBQRZBEZQT-UHFFFAOYSA-L 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- 230000002195 synergetic effect Effects 0.000 description 3
- 229910021529 ammonia Inorganic materials 0.000 description 2
- 238000000975 co-precipitation Methods 0.000 description 2
- 239000003245 coal Substances 0.000 description 2
- 239000013256 coordination polymer Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 238000005406 washing Methods 0.000 description 2
- 235000008733 Citrus aurantifolia Nutrition 0.000 description 1
- 239000002202 Polyethylene glycol Substances 0.000 description 1
- 235000011941 Tilia x europaea Nutrition 0.000 description 1
- 239000002250 absorbent Substances 0.000 description 1
- 230000002745 absorbent Effects 0.000 description 1
- 238000003916 acid precipitation Methods 0.000 description 1
- 235000011114 ammonium hydroxide Nutrition 0.000 description 1
- 239000002585 base Substances 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 229940061631 citric acid acetate Drugs 0.000 description 1
- 230000002153 concerted effect Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 230000003009 desulfurizing effect Effects 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 230000005284 excitation Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000003500 flue dust Substances 0.000 description 1
- 238000005187 foaming Methods 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 238000007654 immersion Methods 0.000 description 1
- 239000002440 industrial waste Substances 0.000 description 1
- 238000009434 installation Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 239000004571 lime Substances 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 239000011572 manganese Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000002574 poison Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 229920001223 polyethylene glycol Polymers 0.000 description 1
- 239000012286 potassium permanganate Substances 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 150000003254 radicals Chemical class 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 238000006722 reduction reaction Methods 0.000 description 1
- 230000002829 reductive effect Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000000967 suction filtration Methods 0.000 description 1
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Classifications
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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- Exhaust Gas Treatment By Means Of Catalyst (AREA)
Abstract
The invention relates to a method for depriving nitric oxide by plasma cooperating with low-temperature catalytic oxidation NO, which is characterized by comprising the following steps of: controlling the airspeed of a mixed gas which contains NO and O2 and is to be processed between 10,000 h<-1> and 60,000 h<-1>; activating through a plasma reactor; and quantificationally oxidizing NOx contained in the activated mixed gas into NO2 at 50-150 DEG C through a fixed bed reactor containing a manganese-base oxide catalyst. Compared with the prior art, the invention has simple process, less adverse effects of CO, CO2 and SO2 impurity components contained in the gas and wide NOX processing concentration range, quantificationally coverts the NO into the NO2 at lower temperature and further absorbs and utilizes the NO2, thereby achieving the resource processing; in addition, the invention has low energy consumption, simple process, small occupying area, no secondary pollution, and the like.
Description
Technical field
The present invention relates to atmosphere pollution purification techniques field, specifically a kind of low-temperature plasma synergistic catalytic oxidation NO that utilizes under normal temperature condition removes the method for nitrogen oxide.
Background technology
Nitrogen oxide (NOx) is one of main atmosphere pollution, is the important presoma that brings out photochemical fog and acid rain.Now the NO discharge capacity in the whole world has reached 35~58Mt/a, wherein more than 95% from the combustion process of fossil fuel.NO accounts for 90%~95% of NOx total amount in the combustion product gases.China NOx is mainly derived from industrial combustion process and vehicle motor.Because the energy resource structure of China is still based on coal, and the directly burning of most of genus, the NOx that burning produces is a kind of important dusty gas.
Many at present employing ammine selectivity catalytic reduction methods are carried out purified treatment to the stationary source nitrogen oxides from exhaust gas, though the ammine selectivity catalytic reduction method is the nitrogen oxide that is used to remove stationary source (as thermal power plant) discharging of success, but ammonia used in amounts accurate measurement control, and ammonia has very strong corrosivity, easily reveal and cause secondary pollution, the operating cost height, and reaction temperature must be more than 350 ℃, and catalyst is subjected to washing away of high concentration flue dust easily and poisons; The economizer of China's boiler and air preheater are assembled into one in addition, are unfavorable for the installation of SCR reactor, and therefore existing SCR technology is difficult to directly use on China's boiler.
Disclosing a kind of among the Chinese patent CN 1803257A is that reducing agent is used for the method that coal fired power plant removes nitrogen oxide with amino material, this method is to spray into amino material and nitrogen oxide partial reaction in the coal-burning boiler upper furnace to remove in the flue gas 35~40% nitrogen oxide, the amino completely material of unreacted enters reactor with flue gas, at catalyst surface, amino material again with reaction of nitrogen oxides, the nitrogen oxide percent reduction can reach more than 90%, but this method reaction temperature is higher, introduce amino reductive, exist and reveal and the equipment corrosion problem.Disclose a kind of plasma among the Chinese patent CN 1613544A and strengthened the method that methane is selected catalyzing and reducing nitrogen oxides, realized ℃ utilizing the plasma body cooperative catalytic reduction in room temperature to 350, only utilize catalytic reduction when surpassing 350 ℃, though this method input power is lower, but still must heat up, energy consumption is higher.
The selective catalytic oxidation method be meant earlier with NO partly selective catalytic oxidation be NO
2, use the absorbent (as lime, NaOH and ammoniacal liquor etc.) of wet desulphurization to absorb again, realize wet method desulfurization removing nitric simultaneously.The absorption techniques in present second step is ripe, and the NO of the first step is converted into NO
2The catalytic oxidation technology be key and difficult point.Therefore, how research is converted into NO with NO
2And carry out efficient absorption, to reach simultanously desulfurizing and denitrification, have important practical significance.
Summary of the invention
The purpose of this invention is to provide a kind of low-temperature plasma synergistic selective catalytic oxidation (SCO) technology of utilizing, with the method for the quantitative catalytic oxidative desulfurization NOx of NO low temperature.
Utilize a large amount of as lively as a cricket high activity species (as ion, electronics, the atom and molecule of excitation state and free radical etc.) of plasma space enrichment, the concerted catalysis oxidation reaction reduces the activation energy that reacts, and quantitatively the part NO in the flue gas is oxidized to NO
2, make the NO oxidizability reach 50%~60%, this moment, the absorption reaction of NOx will be by NO and NO
2Equimolecular absorbs, and is the equal of absorption of N
2O
3, at this moment absorption rate and absorption efficiency are the highest, and corresponding required oxidizing reaction temperature is not high yet, realize easily, and energy consumption is lower.This method is mainly used in the NOx that removes in the industrial waste gas, i.e. stationary source institute exhaust gas discharged such as steam power plant, smeltery, oil plant, chemical plant.
Technical scheme of the present invention is (technological process): will contain NO 0.02~0.05%, O
22~6% mist (pending gas), air speed is at 10000~60000h
-1Between, by plasma reactor activation, the gaseous mixture after the activation is by being equipped with the fixed bed reactors of catalyst, makes NOx in the gaseous mixture quantitative NO that is oxidized under 50~150 ℃ of conditions
2, gas enters the alkali lye absorption bottle and absorbs subsequently.Low temperature plasma adopts coaxial-type dielectric impedance reactor plasma reactor, external diameter is respectively the stainless steel electrode of the diameter 10mm of alundum tube center insertion of 20mm and 25mm, the alundum tube outer wall twines as high-field electrode with stainless (steel) wire, the stainless steel wallboard is as low-field electrode, the plasma input voltage is controlled between 10~70V, and Current Control is between 0.2~1.5A.
The present invention compared with prior art, its technology is succinct, CO, CO in the gas
2, SO
2The adverse effect of impurity composition is little, handles NO
XConcentration range wide.Be NO with the NO quantitative conversion under the lower temperature
2, further absorb, accomplished recycling treatment, and the present invention has characteristics such as energy consumption is low, technology is succinct, floor space is little, non-secondary pollution.
Description of drawings
The experiment flow figure of nitrogen oxide in Fig. 1 low-temperature plasma synergistic catalytic oxidative desulfurization of the present invention tail gas.
The specific embodiment
The inside and outside footpath of coaxial-type dielectric impedance reactor plasma reactor is respectively the alundum tube of 20mm and 25mm, the stainless steel electrode of a diameter 10mm is inserted at the alundum tube center, the alundum tube outer wall twines as high-field electrode with stainless (steel) wire, the stainless steel wallboard is as low-field electrode, the plasma input voltage is 10V, and electric current is 0.2A; The NO volume fraction is 5 * 10
-4, O
2Be 3%, N
2Be balance gas, the mist total flow is 200ml/min, and air speed is 51000h
-1Pending gaseous mixture is activated by plasma reactor, and the gaseous mixture after the activation utilizes the temperature control layer to be heated to 250 ℃ and comes the quantitative NO that is oxidized to by the fixed bed reactors of MnOx-CP catalyst (0.2 gram) are housed
2, gas enters the alkali lye absorption bottle and absorbs subsequently.The clearance of NO has reached 82% at 150 ℃.
The inside and outside footpath of coaxial-type dielectric impedance reactor plasma reactor is respectively the alundum tube of 20mm and 25mm, the stainless steel electrode of a diameter 10mm is inserted at the alundum tube center, the alundum tube outer wall twines as high-field electrode with stainless (steel) wire, the stainless steel wallboard is as low-field electrode, the plasma input voltage is 22V, and electric current is 0.5A.The NO volume fraction is 5 * 10
-4, O
2Be 3%, N
2Be balance gas, the mist total flow is 200ml/min, and air speed is 12000h
-1Pending gaseous mixture is activated by plasma reactor, and the gaseous mixture after the activation utilizes the temperature control layer to be heated to 250 ℃ and comes the quantitative NO that is oxidized to by the fixed bed reactors of MnOx-CA-400 catalyst (0.6 gram) are housed
2, gas enters the alkali lye absorption bottle and absorbs subsequently.The clearance of NO has reached 41% in the time of 50 ℃.
Embodiment 3
The inside and outside footpath of coaxial-type dielectric impedance reactor plasma reactor is respectively the alundum tube of 20mm and 25mm, the stainless steel electrode of a diameter 10mm is inserted at the alundum tube center, the alundum tube outer wall twines as high-field electrode with stainless (steel) wire, the stainless steel wallboard is as low-field electrode, the plasma input voltage is 70V, and electric current is 1.5A; The NO volume fraction is 5 * 10
-4, O
2Be 3%, N
2Be balance gas, the mist total flow is 200ml/min, and air speed is 60000h
-1Pending gaseous mixture is activated by plasma reactor, and the gaseous mixture after the activation is by being equipped with MA-MnOx/TiO
2The fixed bed reactors of catalyst (0.15 gram) utilize the temperature control layer to be heated to 250 ℃ and come the quantitative NO that is oxidized to
2, gas enters the alkali lye absorption bottle and absorbs subsequently.The clearance of NO has reached 56% in the time of 100 ℃.
Preparation of catalysts: adopt the liquid phase coprecipitation method to prepare catalyst (Co-precipitation method), respectively obtain solution I, II and III; Solution I: take by weighing the 7.4g manganese acetate and be dissolved in the 200ml distilled water; Solution II: take by weighing the 2.62g polyethylene glycol and be dissolved in the 100ml distilled water; Solution III: take by weighing 5.2g potassium permanganate and be dissolved in the 200ml distilled water; Under the room temperature condition, solution II is poured in the solution I, the limit bevelling stirs; Subsequently, in above-mentioned solution, add solution III, last continuous stirring 6h; Filter, collect the solids on the filter paper, spend distilled water washing 3~4 times, suction filtration, dry 10h under 70 ℃ again; With dry gained solids through compressing tablet, grind, sieve and make 40~60 purpose particles, be designated as MnOx-CP.
Adopt citric acid method (Citric Acid Method) preparation catalyst, took by weighing a certain amount of citric acid and manganese acetate in 2: 3 in molar ratio, use the 60ml dissolved in distilled water, fully stir about 4h; Stirred and be placed on the processing of foaming in the Rotary Evaporators, handled 8h for 70 ℃; When occurring the foam-like solid in the flask, take out, put into baking oven in 100 ℃ of dry 10h, place the roasting temperature 6h of Muffle furnace at last in setting, can make black MnOx catalyst; Through compressing tablet, grind, sieve and make 40~60 purpose particles, the manganese-base oxide catalyst, and, be designated as MnOx-CA-400 400 ℃ of following roastings 6 hours.
Perhaps adopt the MnOx/TiO of excessive immersion process for preparing 10%Mn load capacity
2Catalyst.In 100ml distilled water, add 10gTiO
2, mix (mass ratio) manganese acetate of back adding 20%, and stir, at room temperature flood 2h after the dissolving fully; Put into baking oven afterwards, at 110 ℃ of dry 10h; Then at 300 ℃ of following roasting 2h; After compressing tablet, grind, sieve 40~60 purpose MnOx/TiO
2Catalyst is designated as: MA-MnOx/TiO
2
Among Fig. 1, V-magnetic valve, I-mass flowmenter.
Claims (3)
1. the method for a depriving nitric oxide by plasma cooperating with low-temperature catalytic oxidation NO is characterized in that and will contain NO, O
2Pending mist, air speed is controlled at 10000~60000h
-1Between, by plasma reactor activation, the gaseous mixture after the activation is by being equipped with the fixed bed reactors of manganese-base oxide catalyst, makes NOx in the gaseous mixture quantitative NO that is oxidized under 50~150 ℃ of conditions
2
2. the method for depriving nitric oxide by plasma cooperating with low-temperature catalytic oxidation NO according to claim 1, it is characterized in that the reaction of low temperature plasma device that adopts is the dielectric barrier discharge device, it is configured to the stainless steel electrode that external diameter is respectively the diameter 10mm of alundum tube center insertion of 20mm and 25mm, the alundum tube outer wall twines as high-field electrode with stainless (steel) wire, and the stainless steel wallboard is as low-field electrode.
3. the method for depriving nitric oxide by plasma cooperating with low-temperature catalytic oxidation NO according to claim 1 is characterized in that the operational factor control range of plasma is: input voltage: 10~70V, electric current: 0.2~1.5A.
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Cited By (11)
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CN102487880A (en) * | 2011-12-14 | 2012-06-13 | 苏州超等环保科技有限公司 | Method of preparing plasma aquaculture water |
CN102716647A (en) * | 2012-07-09 | 2012-10-10 | 上海万强科技开发有限公司 | Method for treating NOx-containing waste gas and system thereof |
CN105163476A (en) * | 2015-08-21 | 2015-12-16 | 厦门大学 | Plasma discharge device |
CN105457488A (en) * | 2015-12-24 | 2016-04-06 | 华北电力大学 | Catalyst unified plasma nitric oxide removing device and method |
CN105833718A (en) * | 2016-04-14 | 2016-08-10 | 中国石油大学(北京) | Denitration system and denitration processing method of plasma synergistic catalyst |
CN106268207A (en) * | 2016-08-09 | 2017-01-04 | 西安理工大学 | The device of gas-liquid two-phase dielectric barrier discharge removing nitrogen oxides and application thereof |
CN106268222A (en) * | 2016-09-30 | 2017-01-04 | 成都信息工程大学 | Ammonia spray photocatalyst dielectric barrier discharge method simultaneous SO_2 and NO removal the method for resource |
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CN113350985A (en) * | 2021-06-04 | 2021-09-07 | 北京化工大学 | Plasma-based denitration device and method |
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CN102716647A (en) * | 2012-07-09 | 2012-10-10 | 上海万强科技开发有限公司 | Method for treating NOx-containing waste gas and system thereof |
WO2014008702A1 (en) * | 2012-07-09 | 2014-01-16 | Hang Pengzhi | Method for treating nox-containing waste gas and system thereof |
CN105163476A (en) * | 2015-08-21 | 2015-12-16 | 厦门大学 | Plasma discharge device |
CN105163476B (en) * | 2015-08-21 | 2017-05-03 | 厦门大学 | Plasma discharge device |
CN105457488A (en) * | 2015-12-24 | 2016-04-06 | 华北电力大学 | Catalyst unified plasma nitric oxide removing device and method |
CN105833718A (en) * | 2016-04-14 | 2016-08-10 | 中国石油大学(北京) | Denitration system and denitration processing method of plasma synergistic catalyst |
CN105833718B (en) * | 2016-04-14 | 2019-12-03 | 中国石油大学(北京) | A kind of denitrating system and its processing method of plasma body cooperative catalyst |
CN107398144A (en) * | 2016-06-08 | 2017-11-28 | 黄华丽 | A kind of gas discharge collaboration solution absorbs the method and apparatus for removing removing and harmful gas |
CN107398144B (en) * | 2016-06-08 | 2020-10-09 | 黄华丽 | Method and device for removing harmful gas by gas discharge in cooperation with solution absorption |
CN106268207A (en) * | 2016-08-09 | 2017-01-04 | 西安理工大学 | The device of gas-liquid two-phase dielectric barrier discharge removing nitrogen oxides and application thereof |
CN106268222A (en) * | 2016-09-30 | 2017-01-04 | 成都信息工程大学 | Ammonia spray photocatalyst dielectric barrier discharge method simultaneous SO_2 and NO removal the method for resource |
CN106955654A (en) * | 2017-05-09 | 2017-07-18 | 杭州三得农业科技有限公司 | A kind of powder enabling apparatus |
CN108786393A (en) * | 2018-06-12 | 2018-11-13 | 河北工业大学 | A kind of room temperature decomposition method of carbon dioxide |
CN113350985A (en) * | 2021-06-04 | 2021-09-07 | 北京化工大学 | Plasma-based denitration device and method |
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Application publication date: 20100714 |