CN104043322A - Method for denitrifying coal-fired flue gas through synergy of plasma and complex catalysis - Google Patents
Method for denitrifying coal-fired flue gas through synergy of plasma and complex catalysis Download PDFInfo
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Abstract
The invention discloses a method for denitrifying coal-fired flue gas through synergy of plasma and complex catalysis. According to the method, four plasma reactors, a high-voltage power supply system, a mixer, three water treatment systems, a neutralizing agent, two spraying water electrode formation circulatory systems and catalytic complexing absorption liquid are included. The method comprises the following steps that coal-fired flue gas to be treated is introduced into inlets of the plasma reactors firstly and is treated by the mixer and then the treated coal-fired flue gas enters electric fields of the plasma reactors, part of NO in flue gas is oxidized into NO2 by free radicals and active substances generated by high-voltage corona discharge, NO2 and unoxidized NO are migrated into liquid of spraying water electrodes in the reactors under the combined action of the electric fields and diffusion, NO2 is absorbed by the liquid to form acids, and NO is subjected to complexation and catalytic oxidation by triethylenediamine cobalt in the presence of oxygen so as to form acids finally. Waste water generated by denitrification reaction of flue gas can be recycled by being processed by the water treatment systems, and part of nitrate can be recycled from waste water.
Description
Technical field
The present invention relates to a kind of plasma and the collaborative coal-fired flue gas denitration method of complex catalysis of filed of flue gas purification.
Background technology
Industrial expansion promotes advancing of society's science and technology, and the mankind, when enjoying scientific and technological achievement, are also bearing environmental problem.Nitrogen oxide be one of main source of atmosphere pollution, be also one of main matter forming acid rain, according to statistics, the annual emissions of China's nitrogen oxide is 2,400 ten thousand tons, and wherein nitrogen oxide 67% comes from coal-fired flue-gas.
Within 2011, coal-fired consumption the in the whole nation is 37.96 hundred million tons, increases by 17% than last year, accounts for 50% of global total amount, and National Development and Reform Committee estimates, to the year two thousand twenty whole nation coal consumption, will reach 6,200,000,000 tons.Energy resources conditional decision China take coal and be that main energy consumption structure is difficult to change in a short time, following coal will be brought into play irreplaceable effect in whole energy processes.Cause thus pollutant emission occupy high-leveled and difficult under: from the statistics of relevant department, the pollutant emission of nitrogen oxide in energy-consuming process, the energy is in exploitation, in refining and supply process, also can produce a large amount of pernicious gases, having a strong impact on atmosphere quality, according to relevant department, estimate, the disease that the year two thousand twenty coal-smoke pollution causes need pay economic cost and reach 3,900 hundred million dollars, account for 13% of GDP, the appearance that developed country has emerged rapidly in large numbersBamboo shoots after a spring rain in China in the environmental pollution public hazards that the industrialization middle and later periods occurs, it causes polarization between the rich and the poor aggravation, social contradications intensify, Acid Rain Pollution is serious, therefore in the urgent need to further developing more advanced flue-gas denitration process technology.
Recent two decades is gas denitrifying technology period with fastest developing speed, and the new technology of research and development reaches tens kinds, but wherein majority still mediates test or laboratory research stage.These technology are roughly divided into five classes.1) electron beam irradiation method.Its principle is to utilize electron accelerator to produce electron beam irradiation flue gas, thereby excites the molecule of the gas in flue gas to produce high mars free radical, by NO oxidation, then generates ammonium sulfate and ammonium nitrate with the ammonia react adding.This technique denitration efficiency is higher, is dry way process, without waste water, produces, and system is simple, easy to operate, but exists byproduct hygroscopicity strong, the problems such as ammonia leakage.2) pulse plasma method.Its principle is to utilize pulsed electron that gas molecule is ionized, thereby produces a large amount of high energy electrons and oxyradical, by NO in flue gas
xoxidation, utilizes NH
3carry out the recovery of product, mainly generate ammonium sulfate and ammonium nitrate etc.Its cost is low, pollutes little.3) solid phase adsorption regeneration techniques.Its principle is by the NO in solid absorbent and flue gas
xreaction generates salts substances, and then under certain condition, passes through various distinct methods by NO
xdesorption out transforms again.Advantage removal efficiency is high, and the consumption that shortcoming is sorbing material is large, and needs regeneration to process.4) SNO
xtechnique.SNO
xits main method is to utilize sack cleaner to remove after the flue dust in flue gas, and in A reactor, the flue gas after heating enters catalytic reactor, the ammonia passing through and NO
xreact, its primary product is ammonia G&W.The method advantage is that operating cost is low, and waste water and refuse produce few, and denitration efficiency can reach 90%.5) SCR method.Its principle is under catalyst action, reducing agent NH
3at 290-400 ℃ by NO and NO
2be reduced into N
2, and there is hardly NH
3oxidation reaction, thereby improved N
2selective, reduced NH
3consumption.SCR method now worldwide becomes the main flow technique of large scale industry denitration of boiler smoke, shortcoming is that catalyst price is high, needs periodic replacement, high-temperature catalytic, the problems such as the easy poisoning and deactivation of catalyst and ammonia escape, the problems such as simultaneously floor space is large, flow process is complicated, investment and operating cost height.Therefore there is compact conformation, low expense, investment and operating cost is few, removal efficiency is high, denitration technology is subject to increasing attention when low power consumption and other advantages, is the important development trend of gas denitrifying technology from now on.
Summary of the invention
The invention provides a kind of collaborative coal-fired flue gas denitration method of plasma and complex catalysis, first pending coal-fired flue-gas is passed into plasma reactor entrance, after blender is processed, enter in corona discharge reactor electric field, the free radical of high-voltage corona electric field discharge generation and active material are oxidized respectively NO by part NO in flue gas
2, under the acting in conjunction by electric field and diffusion, NO
2and not oxidized NO migration enters in the liquid of shower water shape electrode in reactor, NO
2further by liquid phase, absorbed and form NO
3 -, triethylenediamine cobalt carries out complexing and catalytic oxidation to not oxidized NO under oxygen exists, and forms acid, thereby reaches the object that purifies coal-fired flue-gas.Under excessive ethylenediamine and highly basic, triethylenediamine cobalt can be regenerated voluntarily, keeps long-time NO_x Reduction by Effective efficiency simultaneously.
The inventive method can realize by plasma reactor, the center of plasma reactor arranges discharge electrode, 1-3 is set with one heart again and arranges annular cage and put body electrode, shower water shape electrode looped pipeline system is set between discharge electrode, and pass into wherein solution and form cascade as flowing water pole plate; Discharge electrode connects negative pulse high pressure, and flowing water pole plate connects positive pulse high pressure, between discharge electrode and flowing water pole plate, forms strong impulse electric corona, and now, the steam in flue gas and oxygen are activated under electric discharge, produce O, OH, O
3, OH
2deng oxidative free radical, part NO is oxidized to NO
2.Under acting in conjunction by electric field and diffusion, NO
2and not oxidized SO
2, NO migration enters in the liquid of shower water shape electrode in reactor, NO
2further by liquid phase, absorbed and form NO
3 -, triethylenediamine cobalt carries out complexing and catalytic oxidation to not oxidized NO under oxygen exists, and reaches the object that purifies coal-fired flue-gas; Under excessive ethylenediamine and highly basic, triethylenediamine cobalt can be regenerated voluntarily, keeps long-time NO_x Reduction by Effective efficiency simultaneously.The inventive method has realized NO
xremove, there is removal efficiency high, do not produce the features such as secondary pollution, there is wide prospects for commercial application.
Described plasma reactor is mainly comprised of reactor tower body, shower water shape electrode looped pipeline system, discharge electrode, fume-dehydrating device.Reactor tower body is made by stainless steel or the mixed earth of reinforcing bar, tower body internal diameter 4200-5500mm, the long 7500-8500mm of tower body; Shower water shape electrode looped pipeline system 2 is processed into circulating line by diameter 2 '-3 ' stainless steel tube, arc opening spray groove in the vertical downward direction of annular shaft spool wall surface every 15mm disposed at equal distance arc length * groove width=100mm * 10mm, circulating line quantity 3-4(is specifically determined by reaction tower internal diameter size), circulating line and circulation solution system are connected; Discharge electrode is large carrying food-basket type discharge electrode, by many barb type discharge electrodes are equidistant, forms, and barb type discharge electrode adopts the stainless steel tube that external diameter is 25-36mm, and its length and reactor tower body match, the long 10-15mm of prickle, and spacing is 50-60mm.Fume-dehydrating device is baffling chip dehydrator, is vertically mounted on reaction tower exit.
Described high voltage source electric power system is comprised of high pressure tumour power supply, intelligent controller (ESPC-III type), and rated output voltage is 100kV, output-current rating 300-500mA, controller adjustable output voltage parameter and pulse power supply mode.
Described blender can be by NO
xthe plasma reactor of entering after mixing with additional air.The Main Function of additional air is that part NO in flue gas is oxidized to NO
2, additional MAF is 1%-5% of smoke treatment quality.
Described water treatment system is comprised of wastewater collection neutralization pond, condensing crystallizing pond, circulation fluid Buffer Pool, and wastewater collection neutralization pond, condensing crystallizing pond, circulation fluid Buffer Pool connect by pipeline or overflow irrigation canals and ditches.
Described nertralizer is to adopt industrial limestone particle or lime or alkaline flushing cinder water, and the particle size range of industrial limestone particle is 2mm-5mm.
Described shower water electrode forms the circulatory system and is comprised of circulating water pool, water circulating pump.Water circulating pump, circulating water pool and annular spray pipe are connected by pipeline, and the capacity of circulating water chennel and water pump size need to be selected according to smoke treatment amount, and circulating water flow volume is 5-8L/m with the ratio of smoke treatment volume flow
3, the pH value of circulation solution is controlled at 8-9 left and right.
Described complex catalysis absorption liquid is a kind of triethylenediamine cobalt solution, and solution quality percent concentration is 0.5% to 2%.
advantage of the present invention:
The abundant sharp plasma denitrating flue gas of the inventive method, liquid complexing catalytic oxidation denitrating flue gas, chemical oxidation denitration advantage separately, three's advantage is combined, be different from the simple combination of corona discharge denitrating flue gas, liquid phase catalytic oxidation, chemical oxidation denitrating flue gas.The corona wind that it produces by electric field can promote NO
xabsorption, increase electromigration effect, improved capacity usage ratio; The free radical producing by corona discharge, liquid phase catalytic oxidation absorbent have strengthened NO
xoxidation effect, by triethylenediamine cobalt, under oxygen exists, not oxidized NO is carried out to complexing and catalytic oxidation, reach denitrating flue gas effect.The inventive method is used integral type to deal with NO
xremove, in mixed solution actual mechanical process, can reuse, reduced cost of investment, have simple in structurely, denitration efficiency is high, and corona discharge capacity usage ratio is high, the features such as solution circulation utilizes, and investment operating cost is low, have great practical value and wide application prospect.
Accompanying drawing explanation
Fig. 1 is structural representation of the present invention.
Icon: 1-reactor tower body, 2-shower water shape electrode looped pipeline system, 3-discharge electrode; 4-fume-dehydrating device, 5-high voltage source electric power system, 6-blender, 7-wastewater collection neutralization pond, 8-condensing crystallizing pond, 9-circulation fluid Buffer Pool, 10-circulating water pool, 11-nertralizer, 12-water circulating pump, 13-complex catalysis absorption liquid.
specific embodiments:
Coal-fired flue gas denitration method is worked in coordination with in a kind of plasma and complex catalysis.It combines the feature of corona discharge, liquid phase catalytic oxidation and chemical oxidation technology.Its basic thought is: first pending coal-fired flue-gas is passed into corona discharge reactor entrance, after pre-oxidation spray system is processed, enter in corona discharge reactor electric field, the free radical of high-voltage corona electric field discharge generation and active material are oxidized respectively NO by part NO in flue gas
2, under the acting in conjunction by electric field and diffusion, NO
2and not oxidized NO migration enters in the liquid of shower water shape electrode in reactor, triethylenediamine cobalt to NO complexing and catalytic oxidation, reaches the object that purifies coal-fired flue-gas under oxygen exists; The waste water producing after denitrating flue gas reaction can recycle after water treatment system is processed in reuse, can be from waste water recovery section nitrate.
Embodiment 1
Certain company provides 15 tons of coal-fired fluidized bed furnaces for oneself, coal-fired flue-gas amount 49000m
3/ h, flue gas NO
xconcentration is 360mg/m
3, former employing concentration 12% lime pulp-water and spray column carry out flue-gas dust-removing and desulfurization denitration, and actual motion WGR is large, reaches 12L/m
3, denitration efficiency 26.2%.Flue gas denitrification system exists the problems such as lime white blocking pipe, fouling to have a strong impact on denitrating system and normally moves, and has the problems such as desulfurization operation expense height.After transformation, retain original tower body, coal-fired flue gas denitration technique is worked in coordination with in using plasma and complex catalysis, and operation WGR is 5.7L/m
3, triethylenediamine cobalt solution concentration 1%, the pH value of circulation solution is controlled at about 8-9, improves in right amount pH value of solution and makes triethylenediamine cobalt solution renewable and reuse.Through environment monitoring department, detect, denitration efficiency reaches 73.3%, and system is reliable, and removal effect is good, has reduced denitration operating cost.
Embodiment 2
Certain company provides 10 tons of spreader stoker boilers for oneself, coal-fired flue-gas amount 37500m
3/ h, flue gas NO
xconcentration is 410mg/m
3, former employing concentration 18% lime pulp-water and spray column carry out flue-gas dust-removing and desulfurization denitration, and actual motion WGR is large, reaches 13L/m
3, denitration efficiency 27.5%.There is lime white blocking pipe and have the problems such as desulfurization operation expense height in flue gas denitrification system.After transformation, retain original tower body, coal-fired flue gas denitration technique is worked in coordination with in using plasma and complex catalysis, and operation WGR is 7.4L/m
3, triethylenediamine cobalt solution concentration 1.5%, the pH value of circulation solution is controlled at about 8-9, improves in right amount pH value of solution, and triethylenediamine cobalt solution is renewable and reuse.Through environment monitoring department, detect, denitration efficiency reaches 74.5%, and system is reliable, and removal effect is good, has reduced denitration operating cost, has reached the relevant discharge standard requirement of flue gas.
Claims (8)
1.
a coal-fired flue gas denitration method is worked in coordination with in plasma and complex catalysis,it is to form the circulatory system, complex catalysis absorption liquid by four plasma reactors, high voltage source electric power system, blender, three water treatment systems, nertralizer, two shower water electrodes, first pending coal-fired flue-gas is passed into plasma reactor entrance, after blender is processed, enter in plasma reactor electric field, free radical and active material that high-voltage corona discharge produces are oxidized to NO by part NO in flue gas
2, under the acting in conjunction by electric field and diffusion, NO
2and not oxidized NO migration enters in the liquid of shower water shape electrode in reactor, NO
2through liquid absorption, form acids, and triethylenediamine cobalt carries out complexing and catalytic oxidation to NO under oxygen exists, finally also form acids, in solution, triethylenediamine cobalt solution can be recycled, the waste water producing after denitrating flue gas reaction can recycle after water treatment system is processed in reuse, can be from waste water recovery section nitrate.
2. according to claim 1
coal-fired flue gas denitration method is worked in coordination with in a kind of plasma and complex catalysisit is characterized in that described plasma reactor is mainly comprised of reactor tower body, shower water shape electrode looped pipeline system, discharge electrode, fume-dehydrating device, reactor tower body is made by stainless steel or armored concrete cast, tower body internal diameter 4200-5500mm, the long 7500-8500mm of tower body; Shower water shape electrode looped pipeline system 2 is processed into circulating line by diameter 2 '-3 ' stainless steel tube, arc opening spray groove in the vertical downward direction of annular shaft spool wall surface every 15mm disposed at equal distance arc length * groove width=100mm * 10mm, circulating line quantity 3-4, circulating line and circulation solution system are connected; Discharge electrode is large carrying food-basket type discharge electrode, by many barb type discharge electrodes are equidistant, forms, and barb type discharge electrode adopts the stainless steel tube that external diameter is 25-36mm, and its length and reactor tower body match, the long 10-12mm of prickle, and spacing is 70-80mm; Fume-dehydrating device 4 is baffling chip dehydrators, is vertically mounted on reaction tower exit.
3. according to claim 1
coal-fired flue gas denitration method is worked in coordination with in a kind of plasma and complex catalysis, it is characterized in that described high voltage source electric power system is comprised of high pressure tumour power supply, intelligent controller, rated output voltage is 100kV, output-current rating 300-500mA, controller adjustable output voltage parameter and pulse power supply mode.
4. according to claim 1
coal-fired flue gas denitration method is worked in coordination with in a kind of plasma and complex catalysis, it is characterized in that described blender can be by NO
xthe plasma reactor of entering after mixing with additional air, the Main Function of additional air is that part NO in flue gas is oxidized to NO
2, additional MAF is 1%-5% of smoke treatment quality.
5. according to claim 1
coal-fired flue gas denitration method is worked in coordination with in a kind of plasma and complex catalysis, it is characterized in that described nertralizer is to adopt industrial limestone particle or lime or alkaline flushing cinder water, the particle size range of industrial limestone particle is 2 mm-5mm.
6. according to claim 1
coal-fired flue gas denitration method is worked in coordination with in a kind of plasma and complex catalysis, it is characterized in that described water treatment system is comprised of wastewater collection neutralization pond, condensing crystallizing pond, circulation fluid Buffer Pool, wastewater collection neutralization pond, condensing crystallizing pond, circulation fluid Buffer Pool connect by pipeline or overflow irrigation canals and ditches.
7. according to claim 1
coal-fired flue gas denitration method is worked in coordination with in a kind of plasma and complex catalysisit is characterized in that described shower water electrode forms the circulatory system and is comprised of circulating water pool, water circulating pump, water circulating pump, circulating water pool and annular spray pipe are connected by pipeline, the capacity of circulating water chennel and water pump size need to be selected according to smoke treatment amount, and circulating water flow volume is 5-8L/m with the ratio of smoke treatment volume flow
3, the pH value of circulation solution is controlled at 8-9 left and right.
8. according to claim 1
coal-fired flue gas denitration method is worked in coordination with in a kind of plasma and complex catalysis, it is characterized in that described complex catalysis absorption liquid is a kind of triethylenediamine cobalt solution, solution quality percent concentration is 0.5% to 2%.
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| CN109351151A (en) * | 2018-12-12 | 2019-02-19 | 山西晋浙环保科技有限公司 | Denitration reaction of low temperature plasma device |
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Application publication date: 20140917 |