CN102407073A - Denitration method for two-section microwave catalytic reaction bed - Google Patents
Denitration method for two-section microwave catalytic reaction bed Download PDFInfo
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- CN102407073A CN102407073A CN2011104512185A CN201110451218A CN102407073A CN 102407073 A CN102407073 A CN 102407073A CN 2011104512185 A CN2011104512185 A CN 2011104512185A CN 201110451218 A CN201110451218 A CN 201110451218A CN 102407073 A CN102407073 A CN 102407073A
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Abstract
The invention relates to a denitration method for a two-section microwave catalytic reaction bed. The method comprises the following steps: filling a catalyst in a reaction tube of a microwave catalytic reactor device, thereby forming a microwave catalytic reaction bed, and then generating a gas-solid reaction by use of a processed gas while passing by the microwave catalytic reaction bed, thereby performing the denitration treatment. The microwave catalytic reaction bed is composed of two independent microwave catalytic reaction beds which are mutually connected in series; Cu-HZSM-5 or Mn/MgFe2O4 catalyst is taken as the catalyst in a first section microwave catalytic reaction bed; activated carbon or activated carbon loaded MnO, CuO or CeO-CuO, MgO-FeOx, CeO-ZrO2 catalyst is taken as the catalyst in a second section microwave catalytic reaction bed; and the processed gas passes by the first and second section microwave catalytic reaction beds in turn and is subjected to a direct decomposition reaction and a selective reduction reaction in turn, thereby removing the nitric oxide. The denitration method has the advantages of being free from secondary pollution and corrosion, high in conversion rate, small in energy consumption, energy-saving, environmentally-friendly, low in running cost, and the like.
Description
Technical field
The present invention relates to a kind of two sections microwave catalysis reaction bed method of denitration.
Background technology
Nitrogen oxide NO
xHealth and ecological environment are all caused very big harm, how to have taked denitration measure efficiently, eliminated NO
xPolluting has become the important topic in the environmental protection.It is to be the SCR technology (NH of reducing agent with ammonia that the technology of using is gone up in industry at present
3-SCR), this technology has been made positive contribution for the Environmental Protection in China cause.NH
3-SCR method is one of method the most ripe in the existing nitrogen oxide treatment technology, and this method can make the removal of nitrogen oxide rate reach 80~90% under lower temperature.Its weak point: the reducing agent consumption is big, and catalyst is prone to poison, and the pipeline equipment requirement is high and denitration efficiency is not high.
Summary of the invention
The objective of the invention is to overcome deficiency of the prior art, provide a kind of conversion ratio two sections microwave catalysis reaction bed method of denitration high, energy-conserving and environment-protective.
The object of the invention is achieved through following technical proposals: said method is included in that catalyst filling forms the microwave catalysis reaction bed in the reaction tube of microwave catalysis reactor assembly, and the gas that is processed gas-solid reaction takes place through the microwave catalysis reaction bed time carries out the denitration processing; Said microwave catalysis reaction bed is two microwave catalysis reaction beds of independently connecting each other, and the catalyst of first section microwave catalysis reaction bed is Cu-ZSM-5 or Mn/MgFe
2O
4Catalyst; The catalyst of second section microwave catalysis reaction bed is active carbon or activated carbon supported MnO, CuO or CeO-CuO, MgO-FeO
x, CeO-ZrO
2Catalyst; Be processed gas in proper order through first section microwave catalysis reaction bed and second section microwave catalysis reaction bed, direct decomposition reaction takes place in first catalyst with first section, reacts with second section catalyst generation selective reduction then, with removal of nitrogen oxide.
250 ℃-550 ℃ of the temperature of said first section microwave catalysis reaction bed, preferred 320 ℃-420 ℃.
The said gas that is processed is 1-5 second through first section microwave catalysis reaction bed reaction time, optimizes 1.5-3.5 second.
300 ℃-600 ℃ of said second section microwave catalysis reaction bed temperature, preferred 420 ℃-550 ℃.
The said gas that is processed is 1-6 second through second section microwave catalysis reaction bed reaction time, optimizes 1.5-3 second.
Mixed oxidization copper in said first section microwave catalysis reaction bed, the mass ratio of the addition of cupric oxide is 10-70%, preferred 30-45%.
Compared with prior art, the present invention has the following advantages: non-secondary pollution, high, little, the energy-conserving and environment-protective of energy consumption of no burn into conversion ratio, and also production cost is low.
The specific embodiment
Following embodiment is described further the present invention:
Said method is included in that catalyst filling forms the microwave catalysis reaction bed in the reaction tube of microwave catalysis reactor assembly, and the gas that is processed gas-solid reaction takes place through the microwave catalysis reaction bed time carries out the denitration processing; Said microwave catalysis reaction bed is two microwave catalysis reaction beds of independently connecting each other, and the catalyst of first section microwave catalysis reaction bed is Cu-ZSM-5 or Mn/MgFe
2O
4Catalyst; The catalyst of second section microwave catalysis reaction bed is active carbon or activated carbon supported MnO, CuO or CeO-CuO, MgO-FeO
x, CeO-ZrO
2Catalyst; Be processed gas in proper order through first section microwave catalysis reaction bed and second section microwave catalysis reaction bed, direct decomposition reaction takes place in first catalyst with first section, reacts with second section catalyst generation selective reduction then, with removal of nitrogen oxide.
250 ℃-550 ℃ of the temperature of said first section microwave catalysis reaction bed, preferred 320 ℃-420 ℃.
The said gas that is processed is 1-5 second through first section microwave catalysis reaction bed reaction time, optimizes 1.5-3.5 second.
300 ℃-600 ℃ of said second section microwave catalysis reaction bed temperature, preferred 420 ℃-550 ℃.
The said gas that is processed is 1-6 second through second section microwave catalysis reaction bed reaction time, optimizes 1.5-3 second.
Mixed oxidization copper in said first section microwave catalysis reaction bed, the mass ratio of the addition of cupric oxide is 10-70%, preferred 30-45%.
Embodiment is from the laboratory.
In the laboratory, waste gas be Dalian Da Te gas Co., Ltd provide for N
2With the gaseous mixture that NO forms, wherein NO concentration is 1000ppm.
Gas analyzer is Americanized 42C NO-NO
2-NO
xAnalyzer.
The power 0-1000w of microwave field is adjustable continuously, and frequency is 2400-2500MHz.The quartz ampoule reaction tube is WG1/2.45-Φ 5.4 * 54.Quartzy pipe range 535mm, internal diameter 10mm.
AC represents active carbon.
Embodiment 1:
First section direct decomposing N O reaction of microwave catalysis reaction bed microwave catalysis.
The catalyst of loading is the CuO-Cu-ZSM-5 of 5g, and the mass fraction of Cu is 5% among the Cu-ZSM-5, and the mass fraction of CuO is 40% among the CuO-Cu-ZSM-5.
Air inlet NO flow-control is at 160ml/min, and oxygen content is 5.88%,
To the control of microwave power automatic catch, make reaction bed temperature maintain 180 ℃, 300 ℃, 380 ℃ respectively, reaction pressure is a normal pressure.
Result such as table 1:
The reaction result of table 1. different catalysts bed temperature
Sequence number | Reaction bed temperature | The NO conversion ratio |
1 | 180℃ | 87.60% |
2 | 300℃ | 97.95% |
3 | 380℃ | 98.93% |
Conclusion: when 380 ℃ of reaction bed temperatures, CuO-Cu-ZSM-5 has the effect of significant decomposing N O in the microwave catalysis reactor, and the NO conversion ratio reaches 98.93%.
Embodiment 2:
Oxygen content is to the influence of microwave catalysis decomposing N O.
Basically with embodiment 1, different is that reaction bed temperature maintains 300 ℃, changes oxygen flow and content, investigates the antioxygen property of this catalyst when microwave catalysis decomposing N O.Result such as table 2.
Table 2. oxygen content is to the influence of microwave catalysis decomposing N O
Wherein, import NO content is 1000ppm, and when oxygen existed, NO almost all was converted into safe N
2, reaction bed temperature is controlled at 300 ℃, and the NO conversion ratio is all more than 98%; Oxygen content does not have influence to microwave catalysis decomposing N O conversion ratio, and catalyst has good antioxygen property during microwave catalysis.
Embodiment 3:
Second section microwave catalysis reaction bed microwave catalysis reductive NO reaction.
Load the 10ml active carbon in the crystal reaction tube of novel microwave catalytic reactor, investigate the performance of oxygen content test Mn modified activated carbon Reduction of NO under microwave.Oxygen content to Mn/AC catalyst microwave catalysis reductive NO result referring to table 3.
Reaction condition: 3%Mn/AC amount of fill 10ml, gas flow 160ml/min, nitric oxide production air inlet content 1000ppm, 400 ℃ of temperature.
Table 3. oxygen content is to the influence of Mn modified activated carbon Reduction of NO under microwave
Sequence number | Oxygen flow | Oxygen content | Nitric oxide outlet content | Conversion ratio |
1 | 0ml.min-1 | 0% | 7.5ppm | 99.25% |
2 | 10ml.min-1 | 4% | 3.5ppm | 99.65% |
3 | 15ml.min-1 | 6% | 2.8ppm | 99.72% |
4 | 20ml.min-1 | 8% | 3.3ppm | 99.67% |
Conclusion: oxygen content does not have obvious influence to Mn/AC catalyst microwave catalysis reductive NO conversion ratio.Carry out microwave catalysis reductive NO reaction through second section microwave catalysis reaction bed, the NO conversion ratio can be up to 99.72%.
Embodiment 4
Microwave catalysis reaction bed temperature is to the influence of NO conversion ratio.
Load the 10ml active carbon in crystal reaction tube, investigate reaction temperature, the performance of test Mn modified activated carbon Reduction of NO under microwave.
Reaction condition: 3%Mn/AC amount of fill 10ml, gas flow 160ml/min, 400 ℃ of nitric oxide production air inlet content 1000ppm. temperature.
The result is referring to table 4.
Table 4 reaction bed temperature is to the influence of NO conversion ratio
Sequence number | The reaction bed temperature | 3%Mn/AC catalyst conversion ratio | AC catalyst conversion ratio |
1 | 250℃ | 76.96% | 62.90% |
2 | 300℃ | 84.08% | 75.70% |
3 | 350℃ | 91.03% | ---- |
4 | 380℃ | 99.12% | ---- |
5 | 400℃ | 99.65% | 92.50% |
Conclusion: the reaction bed temperature to Mn/AC catalyst microwave catalysis reduction reaction influence significantly, using the Mn carrying capacity is 3% activated carbon supported catalyst, the NO conversion ratio is respectively 99.12%, 99.65% during 380 ℃, 400 ℃ of reaction bed temperature; Use the AC catalyst not reach high conversion ratio.
Embodiment 5
The result of microwave catalysis activated-carbon catalyst reduction denitration is referring to table 5.
Reaction condition: active carbon amount of fill 10ml, gas flow 160ml/min, air speed is 1920h
-1Oxygen flow 10ml/min, oxygen content is 5.88%.
Table 5 reaction temperature is to the active influence of microwave catalysis active carbon reductive NO
Sequence number | Reaction temperature | The nitric oxide exit concentration | Conversion ratio | Remarks |
1 | 250℃ | 371ppm | 62.9% | |
2 | 400℃ | 75.0ppm | 92.5% | |
3 | 500℃ | 2.16ppm | 99.78% | |
4 | 600℃ | 1.81ppm | 99.82% | |
5 | 27℃ | 890ppm | 11% | Remarks 1 |
Remarks 1: the nitric oxide of minimizing is by charcoal absorption.
Conclusion: with the rising of temperature, nitric oxide production conversion ratio increases.
Embodiment 6
First section microwave catalysis reaction bed uses Cu-ZSM-5 copper zeolite catalyst, and the catalyst of filling is 5g CuO-Cu-ZSM-5, and the mass fraction of Cu is 5% among the Cu-ZSM-5, and the mass fraction of CuO is 40% among the CuO-Cu-ZSM-5.To the control of microwave power automatic catch, make reaction bed temperature maintain 300 ℃,
Second section microwave catalysis reaction bed microwave catalysis 3%Mn/AC catalyst reduction denitration reaction.
3%Mn/AC amount of fill 10ml controls 500 ℃ of microwave catalysis reaction bed temperature in the crystal reaction tube of novel microwave catalytic reactor.
Reaction condition: gas flow 160ml/min, air speed is 1920h
-1Oxygen flow 10ml/min, oxygen content is that 5.88%, the first section nitric oxide production air inlet content is 1000ppm.
Two sections microwave catalysis reaction beds of table 6. reaction result
Sequence number | First section NO exit concentration | Conversion ratio | Second section NO exit concentration | Total conversion |
1 | 37.1ppm | 96.29% | 3.21ppm | 99.68% |
2 | 25.0ppm | 97.50% | 1.65ppm | 99.84% |
3 | 31.0ppm | 96.90% | 2.32ppm | 99.78% |
4 | 22.5ppm | 97.75% | 1.81ppm | 99.82% |
5 | 28.0ppm | 97.20% | 1.16ppm | 99.88% |
Conclusion: two sections microwave catalysis reaction beds can the treatment of high concentration nitrous oxides exhaust gas, and first section microwave catalysis reaction bed can be handled the NO more than 95%, and after handling through second section microwave catalysis reaction bed, the NO total conversion is more than 99% again.Therefore first section direct catalytic decomposition NO of microwave catalysis reaction bed need not consume reducing agent, and second section microwave catalysis reaction bed only need consume seldom reducing agent and just can reach and remove nitrogen oxide more than 99%.
Above embodiment shows:
(1) adopt the novel microwave catalytic reactor device, the microwave catalysis reaction bed that uses the inventive method is two microwave catalysis reaction beds of independently connecting each other, and the catalyst of first section microwave catalysis reaction bed is Cu-HZSM-5 or Mn/MgFe
2O
4Catalyst; The catalyst of second section microwave catalysis reaction bed is activated carbon supported MnO, CuO or CeO-CuO, MgO-FeO
x, CeO-ZrO
2Catalyst; Be processed gas in proper order through first section and second section microwave catalysis reaction bed, direct decomposition reaction and selective reduction reaction successively take place, removal of nitrogen oxide.Two sections microwave catalysis reaction beds of the present invention can the treatment of high concentration nitrous oxides exhaust gas, and first section microwave catalysis reaction bed can be handled the NO more than 95%; After handling through second section microwave catalysis reaction bed, the NO total conversion is more than 99% again.Therefore first section direct catalytic decomposition NO of microwave catalysis reaction bed need not consume reducing agent, and second section microwave catalysis reaction bed only need consume seldom reducing agent and just can reach and remove nitrogen oxide more than 99%.The present invention has that non-secondary pollution, no burn into conversion ratio are high, little, the energy-conserving and environment-protective of energy consumption, and advantage such as operating cost is low.
(2) second section microwave catalysis reaction bed of the inventive method uses a year Mn active carbon to be catalyst, the reaction of microwave selective Reduction of NO, or use active carbon to be catalyst, the reaction of microwave catalysis reductive NO; The NO conversion ratio can be near 99.9%, and the removal of nitrogen oxide rate is high.
(3) use active carbon to be reducing agent simultaneously, eliminated and used the secondary pollution of ammonia as reducing agent.
Claims (9)
1. one kind two sections microwave catalysis reaction bed method of denitration; Said method is included in that catalyst filling forms the microwave catalysis reaction bed in the reaction tube of microwave catalysis reactor assembly, and the gas that is processed gas-solid reaction takes place through the microwave catalysis reaction bed time carries out the denitration processing; It is characterized in that said microwave catalysis reaction bed is two microwave catalysis reaction beds of independently connecting each other, the catalyst of first section microwave catalysis reaction bed is Cu-HZSM-5 or Mn/MgFe
2O
4Catalyst; The catalyst of second section microwave catalysis reaction bed is active carbon or activated carbon supported MnO, CuO or CeO-CuO, MgO-FeO
x, CeO-ZrO
2Catalyst; Be processed gas in proper order through first section microwave catalysis reaction bed and second section microwave catalysis reaction bed, direct decomposition reaction takes place in first catalyst with first section, reacts with second section catalyst generation selective reduction then, with removal of nitrogen oxide.
2. method according to claim 1 is characterized in that, 250 ℃-550 ℃ of the temperature of said first section microwave catalysis reaction bed.
3. method according to claim 1 and 2 is characterized in that, the said gas that is processed is 1-5 second through first section microwave catalysis reaction bed reaction time.
4. method according to claim 1 and 2 is characterized in that, 300 ℃-600 ℃ of said second section microwave catalysis reaction bed temperature.
5. method according to claim 3 is characterized in that, the said gas that is processed is 1-6 second through second section microwave catalysis reaction bed reaction time.
6. method according to claim 1 and 2 is characterized in that: mixed oxidization copper in said first section microwave catalysis reaction bed, the mass ratio of the addition of cupric oxide is 10-70%.
7. method according to claim 3 is characterized in that: mixed oxidization copper in said first section microwave catalysis reaction bed, the mass ratio of the addition of cupric oxide is 10-70%.
8. method according to claim 4 is characterized in that: mixed oxidization copper in said first section microwave catalysis reaction bed, the mass ratio of the addition of cupric oxide is 10-70%.
9. method according to claim 5 is characterized in that: mixed oxidization copper in said first section microwave catalysis reaction bed, the mass ratio of the addition of cupric oxide is 10-70%.
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CN2011104512185A CN102407073B (en) | 2011-12-30 | 2011-12-30 | Denitration method for two-section microwave catalytic reaction bed |
PCT/CN2012/087342 WO2013097676A1 (en) | 2011-12-30 | 2012-12-24 | Process for removing nitrogen oxides by microwave catalysis |
US14/318,740 US9199196B2 (en) | 2011-12-30 | 2014-06-30 | Process for removing nitrogen oxides from gas using microwave catalytic reaction by microwave catalysis |
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CN103011333A (en) * | 2012-12-25 | 2013-04-03 | 湘潭大学 | Method for degrading organic wastewater by using ferrite microwave catalyst |
WO2013097676A1 (en) * | 2011-12-30 | 2013-07-04 | 湘潭大学 | Process for removing nitrogen oxides by microwave catalysis |
CN104437080A (en) * | 2014-12-29 | 2015-03-25 | 湘潭大学 | Denitration method for microwave catalytic decomposition of NO and method of preparing Cu-ZSM-11 |
WO2016065600A1 (en) * | 2014-10-31 | 2016-05-06 | 云南创森环保科技有限公司 | Nitrogen oxide ammonia-free low-temperature selective reduction catalyst, preparation method therefor, and uses thereof |
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CN1824372A (en) * | 2006-01-23 | 2006-08-30 | 华东理工大学 | Method of desulfurizing and denitrate simultaneously of exhaust gas by micro wave catalysis |
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Cited By (8)
Publication number | Priority date | Publication date | Assignee | Title |
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WO2013097676A1 (en) * | 2011-12-30 | 2013-07-04 | 湘潭大学 | Process for removing nitrogen oxides by microwave catalysis |
CN103011333A (en) * | 2012-12-25 | 2013-04-03 | 湘潭大学 | Method for degrading organic wastewater by using ferrite microwave catalyst |
CN103011333B (en) * | 2012-12-25 | 2014-06-18 | 湘潭大学 | Method for degrading organic wastewater by using ferrite microwave catalyst |
WO2016065600A1 (en) * | 2014-10-31 | 2016-05-06 | 云南创森环保科技有限公司 | Nitrogen oxide ammonia-free low-temperature selective reduction catalyst, preparation method therefor, and uses thereof |
CN104437080A (en) * | 2014-12-29 | 2015-03-25 | 湘潭大学 | Denitration method for microwave catalytic decomposition of NO and method of preparing Cu-ZSM-11 |
CN106268225A (en) * | 2016-08-04 | 2017-01-04 | 李祖良 | A kind of microwave purifying device |
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 |
CN114471148A (en) * | 2022-03-01 | 2022-05-13 | 浙江浩普环保工程有限公司 | Microwave heating dissociation denitration method for flue gas of thermal power plant |
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