CN102553412A - Method for denitrifying flue gas by using amino reducing agent with high reaction activity - Google Patents

Method for denitrifying flue gas by using amino reducing agent with high reaction activity Download PDF

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Publication number
CN102553412A
CN102553412A CN2012100301086A CN201210030108A CN102553412A CN 102553412 A CN102553412 A CN 102553412A CN 2012100301086 A CN2012100301086 A CN 2012100301086A CN 201210030108 A CN201210030108 A CN 201210030108A CN 102553412 A CN102553412 A CN 102553412A
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reducing agent
flue gas
active amino
reaction
amino reducing
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***
王倩
宋名秀
阿不都拉江·那斯尔
刘晓明
孙洪志
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Shandong University
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Shandong University
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Abstract

The invention relates to a method for denitrifying flue gas by using an amino reducing agent with high reaction activity. The method comprises the following steps of: spraying the amino reducing agent NR3 with high reaction activity into a denitrification reaction zone to ensure that the amino reducing agent and the flue gas are fully mixed, and reacting the amino reducing agent and NOX in the flue gas at the temperature of 350 - 800 DEG C to fulfill the aim of removing the NOX, wherein the denitrification efficiency can reach 70 to 90 percent. By the technology for denitrifying the flue gas by using the active amino reducing agent NR3, the disadvantages of a selective catalytic reduction (SCR) denitrification technology and a selective non-catalytic reduction (SNCR) denitrification technology are overcome, the reaction temperature is moderate, and the reaction selectivity is high. The method is applicable to the flue gas denitrification of multiple kinds of industrial boilers and industrial kilns and the treatment of automobile exhaust.

Description

A kind of method of utilizing the high reaction activity amino reductive to carry out denitrating flue gas
Technical field
The present invention relates to a kind of method of utilizing the high reaction activity amino reductive to carry out denitrating flue gas, belong to the gas denitrifying technology field.
Technical background
Along with Chinese economic development, the environmental pollution that mass energy consumption brings is also more and more serious.China is to be the country of main energy sources with coal, and harmful substance such as contained flue dust, sulfur dioxide, nitrogen oxide has caused severe contamination to air in the coal-fired flue-gas.At present, China has carried out large-scale flue gas desulfurization and has obtained good effect; But denitrating flue gas is not also carried out on a large scale.Country strengthens the control dynamics to discharged nitrous oxides during " 12 ", denitrating flue gas is imperative.
The gas denitrifying technology that adopts at present mainly contains selective catalytic reduction (SCR) and SNCR method (SNCR).On using, SCR and SNCR technology respectively have superiority.SCR technology reaction temperature lower (280-400 ℃), the denitration rate can reach more than 90%, but its initial investment expense is high, and catalyst poisons easily, increased operating cost.SNCR technology reaction temperature is 850-1100 ℃, and the denitration rate is medium, but the SNCR method does not need catalyst, and operating cost is lower, and the construction period is short, is fit to the transformation of medium small boiler.No matter its source is liquefied ammonia, ammoniacal liquor and urea to the reducing agent that two kinds of technology of SCR and SNCR adopt at present, with NO XThe compound that redox reaction takes place all is the NH of gaseous state 3The core of SCR denitration technology is to utilize NH 3Under catalytic condition with NOx redox reaction takes place; The SNCR denitration technology is NH 3High temperature 850-1100 ℃ down and NOx redox reaction directly takes place.
Patent CN102247754A (CN201110210353.0) discloses a kind of method that improves the SNCR denitration efficiency; Be included in and spray into the sodalite powder when spraying into reducing agent liquefied ammonia, urea, carbonic hydroammonium or ammonium carbonate in the SNCR system; Sodium element in the sodalite powder and other trace elements have improved the utilization rate of SNCR system reducing agent like nickel, titanium, vanadium, molybdenum, selenium etc.; Increased denitration efficiency; The reaction optimum temperature range expands to 800-1000 ℃, has suppressed the oxidation reaction of reducing agent and nitrogen oxide, has reduced the leakage of system reducing agent.
Chinese patent file CN101555025A (CN200910014992.2) discloses a kind of co-production preparation method of ammonia for coal-fired flue gas desulfurization and denitration; Comprise urea is carried out condensation reaction; The ammonia that reaction is produced is used for desulphurization denitration, and coproduction obtains cyanuric acid, biuret or the triuret chemical products that contract; Perhaps, urea and dihydroxylic alcohols, monohydric alcohol, phenol or amine are carried out substitution reaction, the ammonia that reaction produces is used for desulphurization denitration, and coproduction obtains series chemical product.In urea condensation or substitution reaction process, do not produce carbon dioxide, all elements in the urea molecule is fully used, and improves the utilization rate of urea, eliminates or minimizing CO 2Discharging.Reduce the purchase cost of the out of stock used ammonia of flue gas desulfurization, obtain chemical products with high added-value simultaneously, increase economic benefit.
Aqueous solution of urea is to use denitrification reducing agent more widely, and still, its calorimetric analysis shows that energy that evaporation of water latent heat is consumed is about 2 times of urea decomposition institute energy requirement, not only causes extra energy consumption, and makes reaction complicated.In addition, the non-uniform temperature in the denitration reaction zone, the temperature field inaccuracy of urea decomposition reaction causes product complicated; And denitration reduction reaction temperature influence is big, when temperature is higher, and NH 3Be prone to be oxidized to NOx, offset its denitration efficiency; When temperature was low, reaction rate descended, and reduction reaction is carried out insufficiently, causes NH 3Escape.
In the existing denitration patented technology, still there is not the report that the high reaction activity amino reductive is used for denitrating system.
Summary of the invention
In order to solve problems such as the catalyst input cost is high in selective catalytic reduction (SCR) technology, the regeneration difficulty is big, operating cost is big; And reducing agent (ammonia and urea) reactant aqueous solution energy consumption height in SNCR method (SNCR) technology, reaction temperature field inaccuracy, problem that the reducing agent utilization ratio is low, the present invention provides a kind of method of utilizing the high reaction activity amino reductive to carry out denitrating flue gas.
Summary of the invention
The present invention provides a kind of high reaction activity amino reductive NR 3Carry out the method for denitrating flue gas, with the active amino reducing agent NR of amino substance heating generation 3Spray in the denitration reaction district, at a certain temperature with flue gas in oxynitrides NO XAbundant hybrid reaction reaches and removes NO in the flue gas XPurpose.NR 3With NOx the redox chemistry reactive activity taking place compares NH 3Height, can under the catalyst-free condition with 350-800 ℃ of lower temperature under reductive NO X
Detailed Description Of The Invention
A kind of method of utilizing the active amino reducing agent to carry out denitrating flue gas comprises that step is following:
(1) the active amino raw material is heated the active amino reducing agent (NR that produces gaseous state under 100-500 ℃ of condition 3);
Said active amino raw material is one of following:
A. acid amides, preferred formamide or acetamide;
B. hexa (C 6H 12N 4);
C. alkylamine, preferred methylamine or ethamine;
D. can produce the raw material of above-mentioned active amino thing or the salt of its raw material;
E. cyanic acid and/or isocyanic acid perhaps can produce the raw material cyanuric acid and the analog thereof of cyanic acid, isocyanic acid;
F. urea.
(2) the active amino reducing agent (NR that step (1) is made 3) inject in the denitration reaction district, under 350-800 ℃ temperature, NR 3Fully mix NR with flue gas 3With the NO in the flue gas XReaction generates N 2And H 2O.
Described NO XMainly be NO and NO 2Mixing, perhaps also have minor N 2O 3
The active amino raw material is solid, liquid or the aqueous solution in the said step (1).
Active amino reducing agent (NR in the said step (2) 3) with flue gas in NO XThe reaction consumption can be according to specifically the controlling of denitration degree, preferred, NR 3With NO XMol ratio is (0.1-1.5): 1; Further preferred, NR 3With NO XMol ratio is (0.2-1): 1
Have high reaction activity and high owing to the active amino reducing agent in the said step (2), so and NO XBe swift in response, be reflected in the 5s and accomplish.Preferably, the reaction time is 0.1-4.5s.The most preferred reaction time is 1s.
Preferably, active amino reducing agent NR in the said step (2) 3With NO XOptimal reaction temperature 450-650 ℃, loss that all can cause reducing agent too high or too low for temperature and NOx removal efficiency descend.
Reaction pressure is not done particular determination in the said step (2), and pressure limit is generally at 0.1-10 atmospheric pressure.
Active amino reducing agent NR in the said step (2) 3With NO XReaction do not need catalyst, practiced thrift denitrating system investment and operating cost.
Active ammonia NR of the present invention 3Method of denitration can use separately, also can unite use with selective catalytic reduction (SCR).Unite active amino reducing agent NR of the present invention when using 3With NH 3As combined reducing agent, can reduce the use amount of catalyst in the SCR denitrating system jointly, reduce departmental cost, improve whole denitration efficiency.
In view of active ammonia NR of the present invention 3Method of denitration and selective catalytic reduction (SCR) are having or not the difference of using on the catalyst, for reducing the use amount of catalyst in the SCR denitrification process, and the compound mode that also can adopt described two kinds of methods series connection to use.
Active amino reducing agent NR of the present invention 3Method of denitration and selective catalytic reduction (SCR) are united the method for use, and step is following:
Earlier carry out denitrating flue gas by the method for the invention described above, the flue gas that removes behind the part NOx gets into the SCR denitrating system again, feeds NH 3, the amount of institute's bringing Selection In property catalyst is the 1/3-1/4 of the technological catalyst amount of existing SCR in this moment SCR denitrification apparatus.
Said catalyst gets final product by prior art.For example Datang environmental science and technology Engineering Co., Ltd catalyst is with TiO 2Be main and interpolation V 2O 5And WO 3.It mainly is to add FeSO that Hebei Elite Ceramics Industrial Co., Ltd. produces its composition of SCR Faveolate denitration catalyst of selling 4TiO 2, its preparation technology is referring to CN102266777A.
Active ammonia NR of the present invention 3Denitration technology can wholely replace existing SCR denitrating system or SNCR denitration technology.
Active ammonia denitration technology realizability of the present invention is good, applied widely; Need not catalyst; As long as under 350-800 ℃ temperature window, can accomplish denitration, applicable to the flue gas or the vent gas treatment of multiple Industrial Boiler, Industrial Stoves, the denitration that also can be used for vehicle exhaust is handled.
The high reaction activity amino reductive gas denitrifying technology that the present invention relates to, different activity ammonia reducing agent NR 3With NO XThe product of reaction is different, and its primary product is N 2, also have H 2O, CO, CO 2Deng.
NR 3With NO XNH is compared in reaction 3Have higher chemical reactivity, can be under the process conditions of catalyst-free, reaction temperature (350-800 ℃) and NO XCarry out chemical reaction rapidly, denitration efficiency is high.
Beneficial effect of the present invention
High reaction activity amino reductive NR of the present invention 3Gas denitrifying technology and existing SNCR technology are not used catalyst, and the active ammonia gas denitrifying technology has overcome the shortcoming that the SNCR reaction temperature is high, denitration efficiency is low, and its main feature is and NO XThat react is not NH 3, but the active amino reducing agent, like HNCO, CH 3NH 2Equimolecular.Compare with the SNCR denitration technology; The reaction temperature of active ammonia denitration technology of the present invention is low; Good reaction selectivity, denitration efficiency is high, and the reaction temperature of having avoided existing in the SNCR technology is high, reducing agent and a series of shortcomings such as the flue gas mixability is poor, denitration efficiency is low, the ammonia escaped quantity is big.Application advantages such as the construction costs that the active ammonia denitration technology not only has the SNCR denitration technology is low, layout is simple and easy, floor space is little, and easy and simple to handle, applicability is wide, and operating cost is low.In addition, high reaction activity amino reductive NR of the present invention 3Gas denitrifying technology is compared without catalyst with the SCR denitration technology, has overcome the difficult problem that the catalyst investment is big, product quality is wayward, operating cost is high.Applicable to the denitrating flue gas of multiple Industrial Boiler and Industrial Stoves, and the processing of vehicle exhaust.
The specific embodiment
Below in conjunction with embodiment the present invention is further specified, but be not limited thereto.
Embodiment 1: coal steam-electric plant smoke denitration, NO XBe about 500ppmv.
NO in the coal steam-electric plant smoke XMain component is NO, accounts for NO XMore than 95%, all the other are NO 2
The 34.5g cyanuric acid is added in the reactor, and temperature is controlled at about 350 ℃, and heating produces active ammonia reducing agent cyanic acid and isocyanic acid, through injection grid with contain NO XFlue gas fully be mixed into the denitration reaction district, with NO XMol ratio reacted by 0.8: 1, behind about 550 ℃ of temperature reaction 1s, reaction effluent gets into nitrogen-oxide analyzer.Analyze and purify NO in the flue gas of front and back XConcentration, the clearance of nitrogen oxide reaches 86%.
Embodiment 2.
Of embodiment 1, different is:
(1) raw material predecomposition: 48g urea is cyanuric acid and ammonia in 250 ℃ of following heating and decomposition;
(2) the gained cyanuric acid carries out denitrating flue gas by the method for embodiment 1 again as the raw material of active amino reducing agent.Analyze and purify NO in the flue gas of front and back XConcentration, the clearance of nitrogen oxide reaches 86%.
It is catalytic-reduction denitrified that the ammonia of step (1) is used for the SCR system in 350 ℃.
Embodiment 3.
Of embodiment 1, different is: the 18.6g methylamine is added in the reactor, and temperature is controlled at about 100 ℃, and the active ammonia reducing agent gaseous state methylamine that heating produces is with NO XMol ratio reacted by 0.6: 1, keep reaction temperature after 540-580 ℃ of reaction stops 1s, reaction effluent gets into nitrogen-oxide analyzer.Warp is to NO in the flue gas before and after purifying XConcentration analysis, the clearance of nitrogen oxide reaches 75%.
Embodiment 4.
Of embodiment 1, different is: the 21g hexa is added in the reactor, and temperature is controlled at about 260-280 ℃, heating make its distil the gaseous state hexa, through injection grid with contain NO XFlue gas fully be mixed into the denitration reaction district, control itself and NO XMol ratio reacted by 0.2: 1, keep reaction temperature after 540-580 ℃ of reaction stops 1s, reaction effluent gets into nitrogen-oxide analyzer.NO in the flue gas before and after purifying XConcentration analysis, the clearance of nitrogen oxide reaches 76%.
Embodiment 5.
Of embodiment 1, different is: the 27g formamide is added in the reactor, and temperature is controlled at 170-200 ℃, the active ammonia reducing agent gaseous formamide that heating produces, through injection grid with contain NO XFlue gas fully be mixed into the denitration reaction district, control itself and NO XThe reaction mol ratio reacted by 0.6: 1, keep reaction temperature after 540-580 ℃ of reaction stops 1s, reaction effluent gets into nitrogen-oxide analyzer.Warp is to NO in the flue gas before and after purifying XConcentration analysis, the clearance of nitrogen oxide reaches 75%.
Embodiment 6. vehicle exhaust denitrations
The NO of motor vehicle exhaust emission XBe NO, NO 2, N 2O 3Deng mixture, wherein NO accounts for 90%.
Of embodiment 1, different is: the 32.7g cyanuric acid is added in the reactor, and temperature is controlled at about 350 ℃, and heating produces active ammonia reducing agent cyanic acid and isocyanic acid, controls itself and NO XReaction mol ratio 0.8: 1 get into the denitration reaction district and react, behind about 550 ℃ reactions of temperature 1s, reaction effluent gets into nitrogen-oxide analyzer.Analyze and purify NO in the tail gas of front and back XConcentration, the clearance of nitrogen oxide reaches 85%.

Claims (8)

1. method of utilizing the active amino reducing agent to carry out denitrating flue gas comprises that step is following:
(1) with the active amino reducing agent (NR of active amino raw material in the following generation of 100-500 ℃ of heating condition gaseous state 3);
Said active amino raw material is one of following:
A. acid amides, preferred formamide or acetamide;
B. hexa (C 6H 12N 4);
C. alkylamine, preferred methylamine or ethamine;
D. can produce the raw material of above-mentioned active amino thing or the salt of its raw material;
E. cyanic acid and/or isocyanic acid perhaps can produce the raw material cyanuric acid and the analog thereof of cyanic acid, isocyanic acid;
F. urea;
(2) the active amino reducing agent (NR that step (1) is made 3) inject in the denitration reaction district, under 350-800 ℃ temperature, NR 3Fully mix NR with flue gas 3With the NO in the flue gas XReaction generates N 2And H 2O.
2. the method for utilizing the active amino reducing agent to carry out denitrating flue gas as claimed in claim 1 is characterized in that active amino reducing agent (NR in the step (2) 3) with flue gas in NO XReaction consumption mol ratio be (0.1-1.5): 1.
3. the method for utilizing the active amino reducing agent to carry out denitrating flue gas as claimed in claim 1 is characterized in that active amino reducing agent (NR in the step (2) 3) with flue gas in NO XReaction consumption mol ratio be (0.2-1): 1.
4. the method for utilizing the active amino reducing agent to carry out denitrating flue gas as claimed in claim 1 is characterized in that active amino reducing agent and NO XBe reflected in the 5s and accomplish.
5. the method for utilizing the active amino reducing agent to carry out denitrating flue gas as claimed in claim 1 is characterized in that active amino reducing agent and NO XReaction time be 0.1-4.5s.
6. the method for utilizing the active amino reducing agent to carry out denitrating flue gas as claimed in claim 1 is characterized in that active amino reducing agent and NO in the step (2) XReaction temperature be 450-650 ℃.
7. the method for utilizing the active amino reducing agent to carry out denitrating flue gas as claimed in claim 1 is characterized in that reaction pressure in the step (2), and pressure limit is at 0.1-10 atmospheric pressure.
8. the method for utilizing the active amino reducing agent to carry out denitrating flue gas as claimed in claim 1; It is characterized in that uniting use with selective catalytic reduction (SCR); Earlier carry out denitrating flue gas by the described method of claim 1, the flue gas after the denitration gets into the SCR denitrating system again, feeds NH 3, the amount of institute's bringing Selection In property catalyst is the 1/3-1/4 of the technological catalyst amount of existing SCR in this moment SCR denitrification apparatus.
CN2012100301086A 2012-02-10 2012-02-10 Method for denitrifying flue gas by using amino reducing agent with high reaction activity Pending CN102553412A (en)

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Cited By (12)

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CN103638805A (en) * 2013-12-16 2014-03-19 东方电气集团东方锅炉股份有限公司 SNCR (selective non-catalytic reduction) smoke denitration method of double-reductant CFB (circulating fluidized bed) boiler
CN104014232A (en) * 2014-06-24 2014-09-03 山东大学 Method for performing smoke desulfurization and denitrification by using urea co-production preparation technology
CN104874270A (en) * 2015-05-05 2015-09-02 北京环科腾越环保工程有限公司 Method and system for denitration by adopting isocyanic acid gas
CN105854548A (en) * 2016-04-15 2016-08-17 廖引家 Cement denitration method
CN106524205A (en) * 2016-09-14 2017-03-22 科林环保技术有限责任公司 Smoke ultra-low emission purification equipment of coal-fired industrial boiler
CN106621782A (en) * 2016-12-30 2017-05-10 深圳市唯有新材料有限公司 High-polymer denitration agent and preparation method thereof
CN106807201A (en) * 2017-02-07 2017-06-09 济南利鸿环保科技有限公司 A kind of denitration method for flue gas of coproduction cyanuric acid
CN107149867A (en) * 2017-06-07 2017-09-12 四川施利旺农业科技开发有限公司 Combustion product gases environment-friendly low-temperature composite denitration agent and preparation method thereof
CN107281915A (en) * 2017-07-19 2017-10-24 中国科学院过程工程研究所 SNCR and SCR the combination denitrating system and method for denitration of a kind of aluminium oxide calcining flue gas
CN108905595A (en) * 2018-09-20 2018-11-30 北京英斯派克科技有限公司 A kind of flue gas in power station boiler Dry denitration method
CN109107373A (en) * 2018-08-16 2019-01-01 西安热工研究院有限公司 A kind of denitrfying agent and preparation method thereof can be used for coal-fired flue gas denitration
CN110898647A (en) * 2019-11-19 2020-03-24 上海众仕环境科技股份有限公司 Hydrophobic powder denitration agent for thermally controlled release of ammonia, preparation method and application

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CN103638805A (en) * 2013-12-16 2014-03-19 东方电气集团东方锅炉股份有限公司 SNCR (selective non-catalytic reduction) smoke denitration method of double-reductant CFB (circulating fluidized bed) boiler
CN103638805B (en) * 2013-12-16 2016-03-30 东方电气集团东方锅炉股份有限公司 A kind of CFB boiler SNCR denitration method for flue gas of dual reducting agents
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CN104874270A (en) * 2015-05-05 2015-09-02 北京环科腾越环保工程有限公司 Method and system for denitration by adopting isocyanic acid gas
CN105854548A (en) * 2016-04-15 2016-08-17 廖引家 Cement denitration method
CN106524205A (en) * 2016-09-14 2017-03-22 科林环保技术有限责任公司 Smoke ultra-low emission purification equipment of coal-fired industrial boiler
CN106524205B (en) * 2016-09-14 2021-04-02 科林环保技术有限责任公司 Ultra-low emission purification equipment for flue gas of coal-fired industrial furnace
CN106621782B (en) * 2016-12-30 2019-04-16 深圳华明环保科技有限公司 A kind of macromolecule denitrfying agent and preparation method thereof
CN106621782A (en) * 2016-12-30 2017-05-10 深圳市唯有新材料有限公司 High-polymer denitration agent and preparation method thereof
CN106807201A (en) * 2017-02-07 2017-06-09 济南利鸿环保科技有限公司 A kind of denitration method for flue gas of coproduction cyanuric acid
CN107149867A (en) * 2017-06-07 2017-09-12 四川施利旺农业科技开发有限公司 Combustion product gases environment-friendly low-temperature composite denitration agent and preparation method thereof
CN107281915A (en) * 2017-07-19 2017-10-24 中国科学院过程工程研究所 SNCR and SCR the combination denitrating system and method for denitration of a kind of aluminium oxide calcining flue gas
CN109107373A (en) * 2018-08-16 2019-01-01 西安热工研究院有限公司 A kind of denitrfying agent and preparation method thereof can be used for coal-fired flue gas denitration
CN109107373B (en) * 2018-08-16 2020-12-11 西安热工研究院有限公司 Denitration agent for coal-fired flue gas denitration and preparation method thereof
CN108905595A (en) * 2018-09-20 2018-11-30 北京英斯派克科技有限公司 A kind of flue gas in power station boiler Dry denitration method
CN110898647A (en) * 2019-11-19 2020-03-24 上海众仕环境科技股份有限公司 Hydrophobic powder denitration agent for thermally controlled release of ammonia, preparation method and application

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Application publication date: 20120711