CN101972603A - Method for removing nitrogen oxides from waste gas - Google Patents
Method for removing nitrogen oxides from waste gas Download PDFInfo
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- CN101972603A CN101972603A CN 201010517329 CN201010517329A CN101972603A CN 101972603 A CN101972603 A CN 101972603A CN 201010517329 CN201010517329 CN 201010517329 CN 201010517329 A CN201010517329 A CN 201010517329A CN 101972603 A CN101972603 A CN 101972603A
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Abstract
The invention discloses a method for removing nitrogen oxides from a waste gas, which comprises the process of causing the waste gas to flow past a catalyst bed in a microwave field for treatment, wherein the catalyst bed is a microwave catalyst bed comprising a microwave catalyst and a reducing agent; the microwave catalyst may be activated carbon, activated carbon-supported metals or activated carbon-supported metallic oxides; the reducing agent is the activated carbon; hydroxyl groups on the surface of the activated carbon are activated by utilizing the microwave field, and gas-solid catalytic reduction action is performed to remove the nitrogen oxides; the microwave frequency of the microwave field may be 500 to 3,000MHz, 500 to 2,350MHz or 865 to 965MHz; the working temperature of the microwave catalyst bed may be 200 to 600 DEG C, 250 to 340 DEG C or 360 to 600 DEG C; and the airspeed of the waste gas is 500 to 8,000h<-1>. The method has the advantages of no secondary pollution, simple process, high efficiency, energy saving, low running cost and the like.
Description
Technical field
The present invention relates to green technology, a kind of method that removes nitrogen oxides of exhaust gas is provided.
Background technology
Comprise in the tail gas of waste gas that metallurgy, thermoelectricity etc. produce and motor vehicle emission at modern industry, comprised a large amount of nitrogen oxide.As everyone knows, nitrogen oxide very harmful to health and ecological environment.Along with improving constantly of human living standard, all pay much attention to containing research, the promotion and application that nitrogen oxides emissions is administered countries in the world.
As with ammoniacal liquor NH
3NH for reducing agent
3-SCR SCR technology, though denitration effect is pretty good, its weak point: (1) is because NH
3Have corrosivity, leakage accident takes place in transportation, storage process easily, increase plant maintenance expense and operating cost; (2) content of processed continuously nitrogen oxides of exhaust gas changes, and the NH that adds
3Amount and the amount of nitrogen oxides of exhaust gas be not to mate excessive N H in real time fully
3Be discharged away, cause secondary pollution.Replace can reducing secondary pollution behind the ammonia though use urea instead in the SCR technology, equipment investment is big, energy utilization rate is low, operating cost is high.
And for example: Chinese patent application number is 200510110314.8, the applying date is 2005-11-11, the application people is an East China University of Science, publication number be CN1824371A's " a kind of micro ware auxiliary catalysis removes the method for sulfur dioxide and nitrogen oxide ", its disclosed technical scheme is: new catalyst with metal oxide as the main active of catalyst and the wave absorbing agent of microwave, with active carbon as catalyst carrier, under the simulated flue gas condition, catalyst is catalytic oxidation of sulphur dioxide and nitrogen oxide under microwave field, and catalysate obtains the composite fertilizer of ammonium sulfate and ammonium nitrate again with steam and ammonia absorption reaction.This method can remove sulfur dioxide and nitrogen oxide preferably.Its weak point: in removing sulfur dioxide and nitrogen oxide process, complex technical process, removal efficiency are not high, and wherein as long as removal efficiency of nitrogen oxides is the highest also 94%.
Summary of the invention
The objective of the invention is to overcome deficiency of the prior art, a kind of method that removes nitrogen oxides of exhaust gas simple for process, that removal efficiency of nitrogen oxides is higher, economical and practical is provided.
Purpose of the present invention is achieved by following technical proposals: this method comprises makes waste gas flow through the process that the beds in the microwave field is handled; Described beds is the microwave catalyst bed, comprise microwave catalyst and reducing agent, described microwave catalyst is active carbon, activated carbon supported metal or activated carbon supported metal oxide, described reducing agent is an active carbon, utilize microwave field to make the surface hydroxyl activation of active carbon, carry out gas-solid catalytic reduction reaction and remove nitrogen oxide.
The microwave frequency of described microwave field is 500-3000MHz, 500-2350MHz or 865-965MHz.
The operating temperature of described microwave catalyst bed is 200-600 Celsius, 250-340,360-600 degree.
The air speed of described waste gas is 500～8000h
-1
Compared with prior art, the present invention has the following advantages: the gas-solid catalytic reduction reaction of microwave does not have secondary pollution, and technology is simple, and easy to operate being easy to controlled, and energy-efficient, operating cost is low.
The specific embodiment
The invention will be further described below in conjunction with embodiment:
Method of the present invention comprises makes waste gas flow through the process that the beds in the microwave field is handled; Described beds is the microwave catalyst bed, comprise microwave catalyst and reducing agent, described microwave catalyst is active carbon, activated carbon supported metal or activated carbon supported metal oxide, described reducing agent is an active carbon, utilize microwave field to make the surface hydroxyl activation of active carbon, carry out gas-solid catalytic reduction reaction and remove nitrogen oxide.
The microwave frequency of described microwave field is 500-3000MHz, 500-2350MHz or 865-965MHz.Preferred 915MHz, 2450MHz.
The operating temperature of described microwave catalyst bed is 200-600 Celsius, 250-340 or 360-600 degree.Preferred 360-600 degree Celsius.
The air speed of described waste gas is 500～8000h
-1
Active carbon is the product of prior art.
Can having of the activated carbon supported metal or the metal of metal oxide: one or more in the group that the metal oxide of Mn, Cu, Ni, Fe, V, Co is formed.
Embodiment 1:
In the laboratory, adopt the specific practice of this method, the be N of described waste gas for providing by Dalian Da Te gas Co., Ltd
2The gaseous mixture that gas and NO form, wherein NO gas content is 1000ppm,
Gas analyzer is Americanized 42C NO-NO
2-NOx Analyzer.
The power 0-1000W of microwave field is adjustable continuously, and frequency is 2400-2500MHz.Quartz tube reactor is WG1/2.45-Φ 5.4 * 54.
Catalyst is filled in forms the microwave catalyst bed in the quartz tube reactor, the waste gas of above-mentioned test usefulness carries out gas-solid catalytic reduction reaction through the microwave catalyst bed and removes nitrogen oxide.
The amount of fill of catalyst all is 10ml, and the mass fraction of Mn is 3%, and the mass fraction of Cu is 5%.Air inlet content is 1000ppm, flow-control 160ml/min, and air speed is 1020h
-1, oxygen content is 5.88%, and microwave power is selected automatic transmission control, and temperature of reaction system is arranged on 400 ℃, and reaction pressure is a normal pressure.Carry out microwave catalysis and remove nitrogen oxide experiment, with the testing result such as the table 1 of three kinds of catalyst:
Table 1.
| Catalyst | Active carbon | Activated carbon supported manganese oxide | Cu/ZSM-5 |
| NO removal efficiency (%) | 99.2 | 99.65 | 68.7 |
In modified activated carbon, the NO removal effect of activated carbon supported manganese oxide is best.
Embodiment 2:
In the laboratory, adopt the specific practice of this method, the be N of described waste gas for providing by Dalian Da Te gas Co., Ltd
2The gaseous mixture that gas and NO form, wherein NO gas content is 1000ppm,
Gas analyzer is Americanized 42C NO-NO
2-NOx Analyzer.
The power 0-1000W of microwave field is adjustable continuously, selects automatic transmission control, makes the microwave catalyst bed temperature maintain 250 ℃, 400 ℃, 500 ℃, 600 ℃ respectively, and frequency is 2400-2500MHz.Quartz tube reactor is WG1/2.45-Φ 5.4 * 54.This tests used quartzy pipe range 535mm, internal diameter 10mm,
Catalyst is filled in forms the microwave catalyst bed in the quartz tube reactor, the waste gas of above-mentioned test usefulness carries out gas-solid catalytic reduction reaction through the microwave catalyst bed and removes nitrogen oxide.
The amount of fill of catalyst all is 5ml, and air inlet content is 1000ppm, flow-control 160ml/min, and air speed is 1920h
-1, oxygen content is 5.88%, and microwave power is selected automatic transmission control, and temperature of reaction system is arranged on 400 ℃, and reaction pressure is a normal pressure.Carry out microwave catalysis and remove nitrogen oxide experiment, with the testing result such as the table 2 of three kinds of catalyst:
Table 2
| Sequence number | Reaction temperature (℃) | Outlet NO content (ppm) | Conversion ratio (%) |
| 1 | 250 | 371 | 62.9 |
| 2 | 400 | 75.0 | 92.5 |
| 3 | 500 | 2.16 | 99.78 |
| 4 | 600 | 1.81 | 99.82 |
Wherein, import NO content is 1000ppm, and temperature removal efficiency when Celsius 500,600 spend is higher than 99.7%.
Embodiment 3
Substantially with embodiment 2, wherein, reaction temperature is set in 400 ℃, examination table 3.
Table 3
| Sequence number | Oxygen flow (ml/min) | Oxygen content (%) | Outlet NO content (ppm) | Conversion ratio (%) |
| 1 | 10 | 5.8 | ?75.0 | 92.5 |
| 2 | 16 | 9.41 | ?4.37 | 99.56 |
| 3 | 25 | 13.51 | ?3.21 | 99.67 |
| 4 | 35 | 17.95 | ?2.15 | 99.79 |
Wherein, import NO content is 1000ppm, oxygen flow the time 35ml/min, removal efficiency is higher than 99.7%.
Embodiment 4:
Substantially with embodiment 2, the power that changes microwave field is 300,520,800W, examination table 4.
Table 4
| Sequence number | Microwave power | The beds equilibrium temperature | Outlet NO content | Conversion ratio (%) |
| 1 | 300 | 167 | 614 | 38.6 |
| 2 | 520 | 282 | 56.0 | 94.4 |
| 3 | 800 | 424 | 11.6 | 98.8 |
Wherein, import NO content is 1000ppm, and the unit of microwave power is watt, and the unit of beds equilibrium temperature is ℃ that the unit of outlet NO content is ppm.Microwave power is 800 watt-hours, and removal efficiency reaches 98.8%.
Comparative Examples 1
In the active carbon amount of fill is 5ml, and the NO gas flow is 160ml/min, and air speed is 1920h
-1Oxygen content is 5.88%, and air inlet NO content is 1000ppm, selects conventional Electric heating to prepare in the glad boat shield in Beijing company and carries out the experiment of catalytic eliminating nitrogen oxide on the MRT-6123 minisize reaction experimental provision.Reaction temperature is respectively 250 ℃, 400 ℃, 500 ℃, 600 ℃.Gained experimental result such as table 5:
Table 5
| Sequence number | Reaction temperature (℃) | Outlet NO content (ppm) | Conversion ratio (%) |
| 1 | 250 | 528 | 47.2 |
| 2 | 400 | 343 | 65.7 |
| 3 | 500 | 134 | 86.6 |
| 4 | 600 | 61.8 | 93.82 |
Wherein, import NO content is 1000ppm, and the removal efficiency that Electric heating is the highest is 93.82%.
Comparative Examples 2:
The disclosed data of background technology, its best removal efficiency is 94.3%.
From top 2 Comparative Examples as seen.The removal efficiency of method of the present invention is 99.82%.Removal efficiency height than prior art.
Claims (10)
1. method that removes nitrogen oxides of exhaust gas, this method comprises makes waste gas flow through the process that the catalytic reaction bed in the microwave field is handled; It is characterized in that: contain the microwave catalysis reducing agent in the described catalytic reaction bed, described microwave catalysis reducing agent is the active carbon that active carbon, load have metal or metal oxide, utilize microwave field to make the surface hydroxyl activation of active carbon, carry out gas-solid catalytic reduction reaction and remove nitrogen oxide.
2. the method that removes nitrogen oxides of exhaust gas according to claim 1 is characterized in that: the microwave frequency of described microwave field is 500-3000MHz.To be active carbon reduce the expense 1.5-20 of institute with nitrogen oxides of exhaust gas to the amount of described active carbon fully.
3. the method that removes nitrogen oxides of exhaust gas according to claim 1 is characterized in that: the microwave frequency of described microwave field is 500-2350MHz.
4. the method that removes nitrogen oxides of exhaust gas according to claim 1 is characterized in that: the microwave frequency of described microwave field is 865-965MHz.
5. according to the optional described method that removes nitrogen oxides of exhaust gas of claim 1-4, it is characterized in that: the operating temperature of described microwave catalyst bed is a 200-600 degree Celsius.
6. according to the optional described method that removes nitrogen oxides of exhaust gas of claim 1-4, it is characterized in that: the operating temperature of described microwave catalyst bed is a 250-340 degree Celsius.
7. according to the optional described method that removes nitrogen oxides of exhaust gas of claim 1-4, it is characterized in that: the operating temperature of described microwave catalyst bed is a 360-600 degree Celsius.
8. according to the optional described method that removes nitrogen oxides of exhaust gas of claim 1-4, it is characterized in that: the air speed of described waste gas is 500～8000h
-1
9. the method that removes nitrogen oxides of exhaust gas according to claim 5 is characterized in that: the air speed of described waste gas is 500～8000h
-1
10. according to described method that removes nitrogen oxides of exhaust gas of claim 6, it is characterized in that: the air speed of described waste gas is 500～8000h
-1
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Cited By (14)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102407073A (en) * | 2011-12-30 | 2012-04-11 | 湘潭大学 | Denitration method for two-section microwave catalytic reaction bed |
| CN102407071A (en) * | 2011-12-30 | 2012-04-11 | 湘潭大学 | Denitration method utilizing microwave catalytic selective reduction reaction |
| CN102407072A (en) * | 2011-12-30 | 2012-04-11 | 湘潭大学 | Method for denitrating by utilizing microwave catalytic reaction |
| CN102407113A (en) * | 2011-12-30 | 2012-04-11 | 湘潭大学 | Microwave catalyst and application method thereof |
| CN102489152A (en) * | 2011-12-30 | 2012-06-13 | 湘潭大学 | Denitration method by microwave catalytic reaction for direct decomposition of NO |
| CN102580525A (en) * | 2012-03-21 | 2012-07-18 | 河北工业大学 | Method for using activated carbon load copper oxide composite catalyst to absorb nitrogenous oxide |
| WO2013097676A1 (en) * | 2011-12-30 | 2013-07-04 | 湘潭大学 | Process for removing nitrogen oxides by microwave catalysis |
| WO2013097677A1 (en) * | 2011-12-30 | 2013-07-04 | 湘潭大学 | Microwave catalyst and preparation process and use thereof |
| CN103990361A (en) * | 2014-05-29 | 2014-08-20 | 徐州工程学院 | Device and process for removing nitrogen oxides under synergistic effect of heteropolyacid and microwave irradiation |
| CN104984761A (en) * | 2015-06-30 | 2015-10-21 | 苏州博利迈新材料科技有限公司 | Nitric oxide catalysis nanometer film and preparation method thereof |
| CN105727745A (en) * | 2016-03-29 | 2016-07-06 | 北京工业大学 | Microwave reaction system device for SCR denitration |
| CN106582642A (en) * | 2016-12-14 | 2017-04-26 | 湘潭大学 | Novel combined catalyst and method for selective catalytic reduction of NO by using same |
| CN112569768A (en) * | 2020-12-06 | 2021-03-30 | 贵州福泉川东化工有限公司 | Yellow phosphorus tail gas purification and absorption method |
| CN115957619A (en) * | 2021-10-11 | 2023-04-14 | 华北电力大学（保定） | Microwave catalytic oxidation denitration method for ferro-manganese based molecular sieve |
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| CN102489152B (en) * | 2011-12-30 | 2014-05-21 | 湘潭大学 | Denitration method by microwave catalytic reaction for direct decomposition of NO |
| CN102407071B (en) * | 2011-12-30 | 2014-10-22 | 湘潭大学 | Denitration method utilizing microwave catalytic selective reduction reaction |
| CN102407073A (en) * | 2011-12-30 | 2012-04-11 | 湘潭大学 | Denitration method for two-section microwave catalytic reaction bed |
| CN102407113A (en) * | 2011-12-30 | 2012-04-11 | 湘潭大学 | Microwave catalyst and application method thereof |
| CN102489152A (en) * | 2011-12-30 | 2012-06-13 | 湘潭大学 | Denitration method by microwave catalytic reaction for direct decomposition of NO |
| WO2013097676A1 (en) * | 2011-12-30 | 2013-07-04 | 湘潭大学 | Process for removing nitrogen oxides by microwave catalysis |
| WO2013097677A1 (en) * | 2011-12-30 | 2013-07-04 | 湘潭大学 | Microwave catalyst and preparation process and use thereof |
| CN102407072A (en) * | 2011-12-30 | 2012-04-11 | 湘潭大学 | Method for denitrating by utilizing microwave catalytic reaction |
| CN102407071A (en) * | 2011-12-30 | 2012-04-11 | 湘潭大学 | Denitration method utilizing microwave catalytic selective reduction reaction |
| US9168514B2 (en) | 2011-12-30 | 2015-10-27 | Xiangtan University | Microwave catalyst and preparation process and use thereof |
| CN102580525A (en) * | 2012-03-21 | 2012-07-18 | 河北工业大学 | Method for using activated carbon load copper oxide composite catalyst to absorb nitrogenous oxide |
| CN103990361B (en) * | 2014-05-29 | 2016-05-18 | 徐州工程学院 | Heteropoly acid and microwave irradiation synergy are removed device and the technique thereof of nitrogen oxide |
| CN103990361A (en) * | 2014-05-29 | 2014-08-20 | 徐州工程学院 | Device and process for removing nitrogen oxides under synergistic effect of heteropolyacid and microwave irradiation |
| CN104984761A (en) * | 2015-06-30 | 2015-10-21 | 苏州博利迈新材料科技有限公司 | Nitric oxide catalysis nanometer film and preparation method thereof |
| CN105727745A (en) * | 2016-03-29 | 2016-07-06 | 北京工业大学 | Microwave reaction system device for SCR denitration |
| CN106582642A (en) * | 2016-12-14 | 2017-04-26 | 湘潭大学 | Novel combined catalyst and method for selective catalytic reduction of NO by using same |
| CN106582642B (en) * | 2016-12-14 | 2019-09-27 | 湘潭大学 | A kind of method of novel compositions catalyst and its Selective Catalytic Reduction of NO |
| CN112569768A (en) * | 2020-12-06 | 2021-03-30 | 贵州福泉川东化工有限公司 | Yellow phosphorus tail gas purification and absorption method |
| CN115957619A (en) * | 2021-10-11 | 2023-04-14 | 华北电力大学（保定） | Microwave catalytic oxidation denitration method for ferro-manganese based molecular sieve |
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Application publication date: 20110216 |