CN103157371B - A kind of coal tar reduces the method for oxynitride discharge - Google Patents
A kind of coal tar reduces the method for oxynitride discharge Download PDFInfo
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- CN103157371B CN103157371B CN201110437093.0A CN201110437093A CN103157371B CN 103157371 B CN103157371 B CN 103157371B CN 201110437093 A CN201110437093 A CN 201110437093A CN 103157371 B CN103157371 B CN 103157371B
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Abstract
The invention discloses a kind of method that coal tar reduces oxynitride discharge, with the problem such as solve that fluctuation of service existing for existing minimizing oxynitride discharge, catalyst cost be high and oxynitride removal efficiency is low.The method of minimizing oxynitride discharge of the present invention is that coke powder is broken to the granule of 75～5000 μm; again after carbonization and activation; it is placed under nitrogen protection in fluid bed or fixed bed reactors; under the temperature conditions of 300～800 DEG C, by the flue gas containing nitrogen oxides by this fluid bed or fixed bed bed.The coal tar reacted is converted into flyash, carries out settling, getting rid of by reactor bed, adds fresh coal tar in fluid bed or fixed bed reactors simultaneously.
Description
Technical field
The invention belongs to environmental protection technical field, the technique reducing oxynitride discharge particularly to a kind of coal tar.
Background technology
Oxynitride mainly includes NO, NO2And a small amount of N2O etc., are referred to as NOx.NOx emission can cause environmental pollution, cause acid rain, generates the ground level ozone (smog) to human health and bad environmental under the effect of sunlight.According to National Environmental publication statistical data, the NOx discharge of the current coal fired thermal power plant of China is estimated as about 5,000,000 t/a.
It is an object of the invention to use coal tar to react as the oxynitride in reactant, with flue gas, make oxynitride be converted into nitrogen and other innocuous substances are discharged, this method has higher removal efficiency, and fixed investment is less simultaneously, it is easy to operation, cost is relatively low.Described coal tar is that main component is carbon, ash and volatile matter by the solid product of coal low temperature distillation gained, darkish complexion porous.
The technology reducing oxynitride discharge outside Present Domestic is a lot.The most ripe technology includes the technology such as SNCR denitration (SNCR), selective catalytic reduction (SCR).SNCR is to use NH3, in the reducing agent such as carbamide spray people's stove and NOxCarry out selective reaction, without catalyst, it is therefore necessary to add reducing agent in high-temperature region.It is between 900 DEG C～1200 DEG C that reducing agent sprays into fire box temperature, and this reducing agent rapid thermal decomposition becomes NH3And with the NO in flue gasxCarry out SNCR reaction and generate N2.This method feature is to be not required to catalyst, and rebuilding old equipment amount is little, invests little compared with SCR method, but ammoniacal liquor consumption relatively SCR fado.
SCR method refers to the selective catalytic reduction process of nitrogen oxides (NOx), is under the effect of catalyst, by ammonification (NH3) NOx conversion can be become nitrogen (N2) and water, due to NH3Can " optionally " and NOx reaction rather than by oxygen (O2) oxidation, therefore reaction is referred to as having " selectivity ".Reaction can be carried out between 280～450 DEG C.The advantage of this method is: reaction temperature is relatively low, and purifying rate is high, and process equipment is compact, reliable, the nitrogen emptying after reduction, non-secondary pollution.But there is also some obvious shortcomings: smoke components is complicated, and some pollutant can make catalyst poisoning；The dust particle of high dispersive can the surface of covering catalyst so that it is activity decrease；Investment is higher with operating cost, NH3Easily leakage, operates and stores difficulty, and be easily formed (NH4)2SO4。
United States Patent (USP) US7,591,986 discloses a kind of exhaust emission control device.But this device contains the catalyst of nitrogen oxides, catalyst amount in this device, and the actual conditions that operation temperature is required for according to flue gas is set, particularly in flue gas, the content of oxygen is bigger on its impact, the key factors such as the replacing of catalyst and operation temperature are required for being determined in advance, and this operation having resulted in device is relatively difficult, and different flue gases needs different operation schemes, this is industrially infeasible, and its catalyst is relatively costly simultaneously.
United States Patent (USP) US7,229,597 disclose the smoke processing system in a kind of diesel exhaust gas, including reducing nitrogen oxides (NOx), particulate matter and the multiple technologies of gaseous state hydrocarbon emission.Discharge for oxynitride, it has used the method for SCR (SCR), flue gas processing device covers the active coating containing ammonia, ammonia therein acts primarily as reduction, and combine conventional SCR catalyst, it is used directly for reducing the discharge of the oxynitride of diesel engine exhaust system.But technical costs is higher, temperature is very big on its impact, and the life-span containing ammonia coating is the shortest, does not have dissemination.
The Chinese patent of Publication No. CN1712108A discloses a kind of flue gas desulfurization, method of denitration.The reaction of its desulphurization and denitration is carried out in the desulfurization and denitrification reaction device being made up of two sections of moving-burden bed reactors, and flow process includes: flue gas is introduced into the bottom second segment reactor equipped with the activated coke from first paragraph reactor, the SO in adsorbing and removing flue gas2, then with NH3Or H2After mixing with CO mixed gas, enter the top first paragraph reactor added with activated coke, react removing nitrogen oxides therein with the activated coke in the first paragraph reactor of top, generate gas and enter air.Inventive desulfurization, denitration efficiency are high, low cost, and removal of nitrogen oxide rate is 70～95%, SO2Removal efficiency is up to 90～99%.But this technology needs to use some gases, and including ammonia, hydrogen, carbon monoxide etc., these gases can cause the potential safety hazard that some are unnecessary.The regeneration of activated coke simultaneously can cause intensity to decline, and causes operation pressure drop to increase, can cause the biggest safety problem.
The Chinese patent of Publication No. CN1911491A discloses a kind of moving bed flue gas desulfurization denitration dust-removing technique, and flue gas is vertical with activated coke inversely to be contacted, and flue gas first passes through desulfurization layer flue gas adsorbed removing SO in this layer2, flue gas injects ammonia, the NO in flue gas during continuing up flowingXWith NH3There is redox reaction, generate N2、H2The harmless products such as O are discharged；Activated coke enters regenerating unit after completing desulphurization denitration and heats through air stove so that it is the sulphuric acid in hole and sulphate decomposition desorption, it is achieved physics regenerates, the SO simultaneously generated3React with activated coke internal pore surface, generate surface functional group, it is achieved chemical regeneration.Through test, applying this technical scheme, desulphurization denitration dedusting one step completes, and simplifies operation, achieve automatization to run continuously, improve efficiency, operating cost is low, desulphurization denitration good dedusting effect, system run all right, flue gas can be directly entered desulphurization denitration dust arrester at 100～200 DEG C, it is not necessary to heats again, has saved the energy and water resource.But this technology is SCR technique and adsorption/desorption technique to be combined, needing also exist for ammonia to use as reducing substances, this is a potential safety hazard, and in this process activated coke both as adsorbent, again as catalyst, this dual role will cause operation easier to be greatly increased.
Summary of the invention
The present invention be directed to the shortcomings such as prior art operation instability, catalyst cost height and oxynitride removal efficiency are low, and a kind of coal tar method to reduce oxynitride discharge is provided, use the inventive method to be effectively reduced the emphasis such as power plant, oil plant, steel mill and pollute the oxynitride discharge in unit.And this technology is due to low in raw material price, denitration efficiency is high, it is adaptable to various flue gas conditions, cost is relatively low.
The present invention provides a kind of coal tar method to reduce oxynitride discharge, it is characterised in that comprise the steps:
1) coke powder is broken to 75～5000 μm; the granule of preferably 500～2000 μm; then at 500～700 DEG C; preferably 580～650 DEG C carry out carbonization 2～8 hours; Coal Char Particles after carbonization is 500～900 DEG C in temperature, under conditions of preferably 550～800 DEG C, is passed through steam 10～200 minutes; within preferably 20～100 minutes, activate, after activation, under nitrogen protection coal tar is cooled to room temperature.
2) by step 1) coal tar made is placed in fluid bed or fixed bed reactors, controlling temperature is 300～800 DEG C, preferably 380～650 DEG C, response time is 0.2～25s, the preferably time is 0.5～5s, by the flue gas containing nitrogen oxides by this fluid bed or fixed bed bed, the oxynitride in removing flue gas.
3) flue gas being stripped of oxynitride enters air, and the coal tar reacted is converted into flyash, carries out settling, getting rid of by reactor bed, adds fresh coal tar in fluid bed or fixed bed reactors simultaneously.
The amount placing coal tar in fixed bed of the present invention or fluid bed generally determines with the content of oxynitride in flue gas, and generally, oxynitride and the mass ratio of coal tar in flue gas are between 0.01～1.5, between preferably 0.5～1.
The present invention is to use coal tar to react as the reducing agent of oxynitride, oxynitride is converted in the range of 300～800 DEG C nitrogen, and generates carbon dioxide and carbon monoxide, which reduces the discharge of oxynitride.Oxynitride therein will react with carbon, and concrete reaction equation is as follows:
2NO+C→CO2+N2
2NO+2C→2CO+N2
SNCR and SCR method use the materials such as liquefied ammonia react as reducing agent and oxynitride, but the transportation safety of the materials such as liquefied ammonia requires higher, according to the definition of standard GB/T 18218-2000 Major Hazard Installations Identifying, belong to major hazard source by the liquefied ammonia storing more than 100 tons as noxious substance.And coal tar is not belonging to dangerous substance, and it is prone to preserve.SNCR and SCR method are desirable that and liquefied ammonia and oxynitride are carried out a certain proportion of proportioning simultaneously, once liquefied ammonia ratio height will result in the leakage of liquefied ammonia, environment being caused secondary pollution, will result in denitration effect when ratio is too low and decline, the operation easier that this also illustrates both approaches is higher.The catalyst cost simultaneously used in SCR method is high, causes factory burden heavier.Activated coke adsorption/desorption technology is the dry desulfurization based on physical-chemical absorption principle, de-NOx technology.SO in flue gas2Generating sulphuric acid under the adsoption catalysis effect of activated charcoal micropore, after reheating, desorption changes into sulfur, liquid SO2Deng product, the NOx in flue gas through activated coke catalysis reduction, generates water and nitrogen under the conditions of ammonification.The method is serious due to equipment corrosion, and the Sulphur ressource response rate is low, simultaneously because the mechanical strength of activated coke itself is the highest, it is easy to abrasion condition occur, reduces the service life of activated coke.
The present invention compared with prior art has the advantage that
1, due to the fact that employing coal tar, it is cheap and easily-available, reduces the cost of investment.
2, due to the fact that coal tar and oxynitride carry out reduction reaction, denitrification effect is high, because the carbon monoxide of the carbon in coal tar and generation is respectively provided with the strongest reducing property, its activity is better than the NH in common SCR device3, the reducing agent such as carbamide, there is from kinetics good respond.
3, due to the fact that and do not use the dangerous materials such as liquefied ammonia to use as reducing agent, the risk factor of the present invention is reduced.
4, the present invention is respectively provided with the effect reducing oxynitride to different types of flue gas, so adaptability is wider.
5, the present invention uses fixed bed or fluid bed to operate, and operating condition is fairly simple, is similar to the technology such as common boiler combustion and recirculating fluidized bed desulfurization, and the coal ash of generation may be used for construction material without causing secondary pollution.
6, the fixed investment of the present invention is less, and floor space is little, has good economic benefit.
Below in conjunction with specific embodiment, the present invention is further detailed explanation.But embodiment is not limiting as the scope of protection of present invention.
Embodiment 1
By the coal of 1000～5000 μm 650 DEG C of carbonizations 4 hours, it is then fed in activation furnace, is warmed up to 800 DEG C, be passed through steam and nitrogen activates for 20 minutes.Under nitrogen protection Coal Char Particles is cooled to room temperature after activation, Coal Char Particles is positioned in fixed bed reactors.The composition (listing according to the percentage by volume of every kind of gas in flue gas) of laboratory flue gas is as follows: flow be 100L/h, NOx be 1000ppmv, oxygen is 3.5% (gas volume percent), and remaining is nitrogen.Flue-gas temperature is 500 DEG C, and the response time is 0.8s, and oxynitride is 0.5 with the mass ratio of coal tar, is introduced in reactor by flue gas, and at the gas composition of reactor outlet detection outlet, it consists of accordingly；Flow be 100L/h, NOx be 0ppm, CO be 2010ppm, oxygen is 0.5% (percentage by volume), and carbon dioxide is 2.7% (percentage by volume), and remaining is nitrogen.Experiment proves that oxynitride is converted into nitrogen completely, has reached the purpose reduced discharging.
Embodiment 2
By the coal of 500～3000 μm 580 DEG C of carbonizations 3 hours, it is then fed in activation furnace, is warmed up to 550 DEG C, be passed through steam and nitrogen activates for 100 minutes.Under nitrogen protection Coal Char Particles is cooled to room temperature after activation, Coal Char Particles is positioned in fixed bed reactors.The composition (listing according to the percentage by volume of every kind of gas in flue gas) of laboratory flue gas is as follows: flow be 100L/h, NOx be 800ppm, oxygen is 4.1% (percentage by volume), and remaining is nitrogen.Flue-gas temperature is 550 DEG C, and the response time is 2s, and oxynitride is 1 with the mass ratio of coal tar.Flue gas is introduced in reactor, and at the gas composition of reactor outlet detection outlet, it consists of accordingly；Flow be 100L/h, NOx be 0ppm, CO be 5000ppm, oxygen is 0.5% (percentage by volume), and carbon dioxide is 3.1% (percentage by volume), and remaining is nitrogen.Experiment proves that oxynitride is converted into nitrogen completely, has reached the purpose reduced discharging.
Embodiment 3
By the coal of 1000～2000 μm 600 DEG C of carbonizations 8 hours, it is then fed in activation furnace, is warmed up to 650 DEG C, be passed through steam and nitrogen activates for 40 minutes.Under nitrogen protection Coal Char Particles is cooled to room temperature after activation, Coal Char Particles is positioned in fixed bed reactors.The composition (listing according to the percentage by volume of every kind of gas in flue gas) of laboratory flue gas is as follows: flow be 200L/h, NOx be 500ppm, oxygen is 4.0% (percentage by volume), and remaining is nitrogen.Flue-gas temperature is 500 DEG C, and the response time is 5s, and oxynitride is 0.8 with the mass ratio of coal tar.Flue gas is introduced in reactor, and at the gas composition of reactor outlet detection outlet, it consists of accordingly；Flow be 200L/h, NOx be 0ppm, CO be 3000ppm, oxygen is 0.2% (percentage by volume), and carbon dioxide is 2.9% (percentage by volume), and remaining is nitrogen.Experiment proves that oxynitride is converted into nitrogen completely, has reached the purpose reduced discharging.
Embodiment 4
By the coal of 1000～3000 μm 600 DEG C of carbonizations 2 hours, it is then fed in activation furnace, is warmed up to 700 DEG C, be passed through steam and nitrogen activates for 60 minutes.Under nitrogen protection Coal Char Particles is cooled to room temperature after activation, Coal Char Particles is positioned in fluidized-bed reactor.The composition (listing according to the percentage by volume of every kind of gas in flue gas) of laboratory flue gas is as follows: flow be 200L/h, NOx be 2500ppm, oxygen is 1.0% (percentage by volume), and remaining is nitrogen.Flue-gas temperature is 500 DEG C, and the response time is 4s, and oxynitride is 0.95 with the mass ratio of coal tar.Flue gas is introduced in reactor, and at the gas composition of reactor outlet detection outlet, it consists of accordingly；Flow be 200L/h, NOx be 0ppm, CO be 3000ppm, oxygen is 0.2% (percentage by volume), and carbon dioxide is 0.7% (percentage by volume), and remaining is nitrogen.Experiment proves that oxynitride is converted into nitrogen completely, has reached the purpose reduced discharging.
Embodiment 5
By the coal of 1500～3500 μm 600 DEG C of carbonizations 5 hours, it is then fed in activation furnace, is warmed up to 600 DEG C, be passed through steam and nitrogen activates for 25 minutes.Under nitrogen protection Coal Char Particles is cooled to room temperature after activation, Coal Char Particles is positioned in fluidized-bed reactor.The composition (listing according to the percentage by volume of every kind of gas in flue gas) of laboratory flue gas is as follows: flow be 200L/h, NOx be 3000ppm, oxygen is 1.5% (percentage by volume), and remaining is nitrogen.Flue-gas temperature is 550 DEG C, and the response time is 1s, and oxynitride is 0.91 with the mass ratio of coal tar.Flue gas is introduced in reactor, and at the gas composition of reactor outlet detection outlet, it consists of accordingly；Flow be 200L/h, NOx be 0ppm, CO be 3500ppm, oxygen is 0.5% (percentage by volume), and carbon dioxide is 0.9% (percentage by volume), and remaining is nitrogen.Experiment proves that oxynitride is converted into nitrogen completely, has reached the purpose reduced discharging.
Claims (9)
1. the method reducing oxynitride discharge with coal tar, it is characterised in that comprise the steps:
1) coke powder is broken to the granule of 75～5000 μm; then carbonization 2～8 hours are carried out at 500～700 DEG C; Coal Char Particles after carbonization, under conditions of temperature is 500～900 DEG C, is passed through steam 10～activates for 200 minutes, under nitrogen protection coal tar being cooled to room temperature after activation；
2) by step 1) coal tar made places in a fluidized bed reactor, by the flue gas containing oxynitride by this fluid bed bed, controlling reaction temperature is 300～800 DEG C, response time is 0.2～25s, making flue gas containing oxynitride and step 1) coal tar made carries out the oxynitride in reaction removing flue gas, and described oxynitride is 0.01～1.5 with the mass ratio of coal tar；
3) flue gas being stripped of oxynitride enters air, and the coal tar reacted is converted into flyash, carries out settling, getting rid of by reactor bed, adds fresh coal tar in fluidized-bed reactor simultaneously.
The method reducing oxynitride discharge with coal tar the most according to claim 1, it is characterised in that: described coke powder is broken to the granule of 500～2000 μm.
Coal tar the most according to claim 1 or claim 2 reduces the method for oxynitride discharge, it is characterised in that: described carbonization temperature is 580～650 DEG C.
The method reducing oxynitride discharge with coal tar the most according to claim 1, it is characterised in that: described activation temperature is 550～800 DEG C.
5. according to the method reducing oxynitride discharge with coal tar described in claim 1 or 4, it is characterised in that: described soak time is 20～100 minutes.
Coal tar the most according to claim 1 or claim 2 reduces the method for oxynitride discharge, it is characterised in that: described carbonization temperature is 580～650 DEG C, and activation temperature is 550～800 DEG C, and soak time is 20～100 minutes.
The most according to claim 1 with coal tar reduce oxynitride discharge method, it is characterised in that: described step 2) reaction temperature be 380～650 DEG C.
8. according to the method reducing oxynitride discharge with coal tar described in claim 1 or 7, it is characterised in that: described step 2) in the mass ratio of oxynitride and coal tar be 0.5～1.
9. according to described in claim 1 or 7 with coal tar reduce oxynitride discharge method, it is characterised in that: described step 2) in response time be 0.5～5s.
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| CN103877856B (en) * | 2014-03-27 | 2016-01-06 | 中冶焦耐工程技术有限公司 | A kind of method of coke oven flue waste gas heat utilization and purification |
| CN105396460B (en) * | 2015-12-25 | 2019-12-24 | 华烁科技股份有限公司 | High-efficiency combined removal of N2O and NOxMethod (2) |
| CN105854541A (en) * | 2016-05-20 | 2016-08-17 | 武汉理工大学 | Method for reducing and removing nitrogen oxide by adsorption-oxidation and liquid phase absorption |
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