CN101869833B - Catalyst for SCR denitration of furnace middle temperature fume and preparation method thereof - Google Patents
Catalyst for SCR denitration of furnace middle temperature fume and preparation method thereof Download PDFInfo
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- CN101869833B CN101869833B CN2010102290087A CN201010229008A CN101869833B CN 101869833 B CN101869833 B CN 101869833B CN 2010102290087 A CN2010102290087 A CN 2010102290087A CN 201010229008 A CN201010229008 A CN 201010229008A CN 101869833 B CN101869833 B CN 101869833B
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Abstract
The invention relates to a catalyst for the SCR denitration of furnace middle temperature fume and a preparation method thereof. The catalyst is an integrated composite catalyst prepared by loading V2O5 and WO3 on a SiO2-TiO2 composite carrier. In the SiO2-TiO2 composite carrier, the SiO2 accounts for 3 to 10 percent of the total mass of the SiO2-TiO2 composite carrier; and in the catalyst, the V2O5 catalyst component accounts for 1 to 2 percent of the total mass of the catalyst including the composite carrier, and the WO3 catalyst component accounts for 5 to 10 percent of the total mass of the catalyst including the composite carrier. The catalyst prepared by the invention uses ammonia as a reducer, can achieve a nitric oxide removal rate of over 90 percent at most, and is widely used in nitric oxide catalytic reduction denitration of furnace fume.
Description
Technical field
The present invention relates to the nitrogen oxide of warm flue gas processing in the boiler in the environmental technology field, particularly a kind of catalyst and preparation method who is used for the SCR denitration of boiler temperature flue gas.
Background technology
The energy resource structure of China is main with coal, and the coal consumption amount is also with sustainable growth.According to statistics, China's capacity of installed generator moderate heat Denso machine capacity accounts for more than 74% at present, and in a very long time in future, the coal-fired nitrogen oxides pollution that is caused is the another important environmental problem after sulfur dioxide pollution." thermal power plant's atmosphere pollutants emission standards (GB13223-2003) " that implements while in January, 2004 has been reduced to 450-1100mg/m to the highest permission concentration of emission of station boiler nitrogen oxide of the 3rd period
3Along with development economic and society, the control criterion of nitrogen oxide will be strict gradually.
At present, to stationary source NO
xControl technology mainly contains two types: one type technological for Combustion Process Control, is characterized in controlling NO in the combustion process
xGeneration, comprise selection, operation adjustment and the low NO of the type of furnace and design parameter
xCombustion technology is controlled the nitrogen oxide of fuel type in the combustion process, heating power type and quick three kinds of mechanism of type with this; Two types are burning back control technology, promptly various flue gas de-NO
xTechnology is characterized in the NO that has generated in the flue gas
xBe fixed up or be reduced to N
2The nitrogen oxide control technology is a cost to reduce boiler heating power efficient generally in the stove; Its denitration efficiency is not high yet; And (the Selective Catalytic Reduction of the selective catalytic reduction in the gas denitrifying technology behind the stove; SCR) have the efficient height, to the little advantage of boiler existing equipment transformation, be a kind of more potential denitration technology.
Reach its maturity with the SCR technology as reducing gas such as ammonia, this technology is to utilize the selectivity of ammonia reducing agent, preferentially reacts with nitrogen oxide, and its is reduced becomes nitrogen and water.
Flue-gas temperature condition stub according to catalyst is suitable for generally uses window can SCR technology can be divided into according to different temperature: high temperature, middle temperature, three kinds of different SCR technologies of low temperature.The Applicable temperature that high temperature SCR generally refers to catalyst 450～600 ℃ and more than, middle temperature SCR is meant the Applicable temperature of catalyst at 320～450 ℃, and the Applicable temperature that low-temperature SCR is meant catalyst is at 120～300 ℃ or low temperature more.Commercial is that running temperature is in 300～450 ℃ middle temperature catalyst more widely at present, and this catalyst is with TiO
2Be carrier, above major catalyst or co-catalyst such as load vanadium, tungsten and molybdenum.
The position that middle temperature catalyst is laid according to the SCR device is different, is divided into high ash section, low ash section and afterbody and arranges three types.Particular location promptly is installed on air preheater and ESP (electric precipitation) is preceding, before the air preheater but behind the high temperature ESP, FGD (desulfurization) three kinds of forms afterwards.Be arranged in the preceding high ash section of air preheater and ESP (electric precipitation), catalyst requires that stronger antiblocking ability is arranged, and stronger alkali resistant metal toxicity, anti-SO are arranged
2Toxicity etc.Be arranged in before the air preheater but behind the high temperature ESP, catalyst can be avoided the side effect of high dust, but still need stronger anti-SO
2Toxicity requires ESP to possess the high-temperature behavior of restraining oneself simultaneously.Be arranged in FGD middle temperature catalyst afterwards, need a large amount of flue gas reheat energy consumptions.
Traditional SCR catalyst carrier all is TiO
2, cost is high.
Summary of the invention
The objective of the invention is to overcome the deficiency of prior art, a kind of catalyst and preparation method who is used for the SCR denitration of boiler temperature flue gas is provided, this catalyst utilizes SiO
2And TiO
2Constitute complex carrier, substantially improve the performance of catalyst carrier; Utilize SiO simultaneously
2Substitute part TiO
2, to reduce the catalyst cost.
The technical solution adopted for the present invention to solve the technical problems is:
A kind of catalyst that is used for the SCR denitration of boiler temperature flue gas is characterized in that: be to adopt sol-gel method to prepare SiO simultaneously
2And TiO
2The complex carrier that constitutes, the temperature that is suitable for boiler smoke is 320～450 ℃, is at SiO
2-TiO
2Supported V on the complex carrier
2O
5And WO
3The integrant composite catalyst of oxide; Said at SiO
2-TiO
2In the complex carrier that constitutes, SiO
2Account for by SiO
2-TiO
2The mass percent of the complex carrier that constitutes is 3%-10%; In the said catalyst, V
2O
5The catalyst component percentage that accounts for the catalyst total quality that comprises complex carrier be 1%～2%; WO
3The catalyst component percentage that accounts for the catalyst total quality that comprises complex carrier be 5%～10%.
A kind of Preparation of catalysts method that is used for the SCR denitration of boiler temperature flue gas, it is characterized in that: preparation method's step is:
(1) preparation of complex carrier: measure a certain amount of butyl titanate, slowly splash in the absolute ethyl alcohol of 2-6 times of volume,, mix, form yellow settled solution A with the powerful 10min that stirs of magnetic stirring apparatus; To be added in the absolute ethyl alcohol of other 2-6 times of volume with the ultra-pure water and the silester of the same volume of butyl titanate, and obtain solution B, this silester is pressed SiO
2/ (SiO
2-TiO
2)=3-10% calculates; Add nitre acid for adjusting pH value≤3; Under vigorous stirring, solution B is slowly splashed in the solution A, gel is placed 80 ℃ of dry 20h down, get crystal; This crystal respectively at Muffle furnace 400-750 ℃ of heat treatment 2h, is promptly obtained SiO
2-TiO
2Complex carrier;
(2) load of catalyst: according to V
2O
5The load capacity mass percent is 1%-2%, WO
3The mass percent load capacity be 5-10%, respectively with NH
4VO
3And N
5H
37W6024H
2O is a predecessor, calculates the quality of required predecessor, and under 60 ℃ of conditions of water-bath, the aqueous solution with the predecessor preparation certain volume that measures adopts infusion process, with SiO
2-TiO
2Complex carrier impregnated in the solution of the ammonium metavanadate prepared and ammonium paratungstate, concussion 24h, and 105 ℃ of dry 6h at 450 ℃ of calcinings of Muffle furnace 3h, obtain required catalyst then.
Advantage of the present invention and good effect are:
1, the present invention adopts SiO
2-TiO
2Complex carrier is a carrier, has the high characteristics in the big and sour site of specific area, to gaseous material NH
3High adsorption capacity, help the carrying out of denitration; While SiO
2Cost be significantly less than TiO
2Cost, have economic advantages.
In the gas-solid heterogeneous catalytic reaction, gaseous material at first is attracted to catalyst surface, accomplishes catalytic process then.In the SCR catalytic reaction process, generally believe it is reducing agent NH
3At first being adsorbed on catalyst surface becomes the important step that SCR reacts, so the specific area of catalyst is big more, surface acidity is high more, and its catalytic capability is strong more.
2, the present invention adopts the infusion process supported catalyst on carrier, and it is simple to compare with coprecipitation method, infusion process can convenient catalyst load on the carrier of arbitrary shape V
2O
5And WO
3Be the main active substances of SCR catalysis, V among the present invention
2O
5Load capacity be 1%-2%, WO
3Load capacity be 5%-10%; Overcome when load capacity bigger particularly when the specific area of carrier is little catalyst pile up and bad phenomenon such as sintering, reunion at high temperature appear in catalyst easily that cause at carrier surface easily, effectively satisfy the requirement of this load.
3, the present invention adopts sol-gel method to prepare SiO simultaneously in the preparation process of carrier
2And TiO
2The complex carrier that constitutes is because SiO
2Show solid acid, the sour site of having improved catalyst surface helps in the course of reaction absorption of reducing agent ammonia is improved catalytic activity, has also improved the alkali-metal mithridatism of catalyst to existing in the flue gas simultaneously.
The specific embodiment
Through specific embodiment the present invention is made further detailed description below, following examples are descriptive, are not determinate, can not limit protection scope of the present invention with this.
A kind of catalyst that is used for the SCR denitration of boiler temperature flue gas is at SiO with infusion process
2-TiO
2Supported V on the complex carrier
2O
5And WO
3Oxide, integrant composite catalyst, wherein: at SiO
2-TiO
2In the complex carrier that constitutes, SiO
2Account for by SiO
2-TiO
2The mass percent of the complex carrier that constitutes is 3%-10%.This infusion process is the current techique of this area, repeats no more at this.
Catalyst component is V in the catalyst
2O
5And WO
3, V wherein
2O
5The catalyst component percentage that accounts for the catalyst total quality that comprises complex carrier be 1%～2%; WO
3The catalyst component percentage that accounts for the catalyst total quality that comprises complex carrier be 5%～10%.
Narrate preparation method of the present invention through four embodiment below:
Embodiment 1:
A kind of Preparation of catalysts method that is used for the SCR denitration of boiler temperature flue gas is with V
2O
5-WO
3Be major catalyst, adopt infusion process, through suitable immersion, oven dry and calcine technology, through conditions such as control load amount, calcining heats, preparation the application's catalyst.Concrete steps are:
(1) preparation of complex carrier: measure a certain amount of butyl titanate, slowly splash in the absolute ethyl alcohol of 6 times of volumes,, mix, form yellow settled solution A with the powerful 10min that stirs of magnetic stirring apparatus; To (press SiO with the ultra-pure water and the ethyl silicate of the same volume of butyl titanate
2/ (SiO
2-TiO
2)=5% calculates) be added in the absolute ethyl alcohol of other 6 times of volumes, obtain solution B; Add nitre acid for adjusting pH value≤3.
Under vigorous stirring, solution B is slowly splashed in the solution A, gel is placed 80 ℃ of dry down approximately 20h, get crystal; This crystal respectively at 450 ℃ of heat treatment 2h of Muffle furnace, is promptly obtained SiO
2-TiO
2Complex carrier.
(2) load of catalyst: according to V
2O
5Load capacity is 2% (mass percent), WO
3Load capacity be 10% (mass percent), respectively with NH
4VO
3And N
5H
37W6024H
2O is a predecessor, calculates the quality (amount of predecessor when account form is a routine techniques) of required predecessor, under 60 ℃ of conditions of water-bath, prepares the aqueous solution of certain volume with the predecessor of metering.Adopt infusion process, with SiO
2-TiO
2Complex carrier impregnated in the solution of the ammonium metavanadate prepared and ammonium tungstate, concussion 24h, and 105 ℃ of dry 6h at 450 ℃ of calcinings of Muffle furnace 3h, obtain required catalyst then.
Detect: prepared catalyst is 900ppm in the NO volumetric concentration, and temperature is under 300 ℃, and oxygen concentration is 5%, NH
3Under/NO=1.0 the situation, the removal efficiency of NO is more than 90%; In the NO volumetric concentration is 900ppm, and temperature is under 420 ℃, and oxygen concentration is 5%, NH
3Under/NO=1.0 the situation, the removal efficiency of NO is more than 95%.
Embodiment 2:
(1) preparation of complex carrier: measure a certain amount of butyl titanate, slowly splash in the absolute ethyl alcohol of 2 times of volumes,, mix, form yellow settled solution A with the powerful 10min that stirs of magnetic stirring apparatus; To (press SiO with the ultra-pure water and the ethyl silicate of the same volume of butyl titanate
2/ (SiO
2-TiO
2)=10% calculates) be added in the absolute ethyl alcohol of other 2 times of volumes, obtain solution B; Add nitre acid for adjusting pH value≤3.
Under vigorous stirring, solution B is slowly splashed in the solution A, gel is placed 80 ℃ of dry down approximately 20h, get crystal; This crystal respectively at 450 ℃ of heat treatment 2h of Muffle furnace, is promptly obtained SiO
2-TiO
2Complex carrier.
(2) load of catalyst: according to V
2O
5Load capacity is 1% (mass percent), WO
3Load capacity be 5% (mass percent), respectively with NH
4VO
3And N
5H
37W6024H
2O is a predecessor, calculates the quality of required predecessor, under 60 ℃ of conditions of water-bath, prepares the aqueous solution of certain volume with the predecessor of metering.Adopt infusion process, with SiO
2-TiO
2Complex carrier impregnated in the solution of the ammonium metavanadate prepared and ammonium tungstate, concussion 24h, and 105 ℃ of dry 6h at 450 ℃ of calcinings of Muffle furnace 3h, obtain required catalyst then.
Detect: prepared catalyst is 900ppm in the NO volumetric concentration, and temperature is under 300 ℃, and oxygen concentration is 5%, NH
3Under/NO=1.0 the situation, the removal efficiency of NO is more than 83%; In the NO volumetric concentration is 900ppm, and temperature is under 380 ℃, and oxygen concentration is 5%, NH
3Under/NO=1.0 the situation, the removal efficiency of NO is more than 86%.
Embodiment 3:
(1) preparation of complex carrier: measure a certain amount of butyl titanate, slowly splash in the absolute ethyl alcohol of 3 times of volumes,, mix, form yellow settled solution A with the powerful 10min that stirs of magnetic stirring apparatus; To (press SiO with the ultra-pure water and the ethyl silicate of the same volume of butyl titanate
2/ (SiO
2-TiO
2)=5% calculates) be added in the absolute ethyl alcohol of other 3 times of volumes, obtain solution B; Add nitre acid for adjusting pH value≤3.
Under vigorous stirring, solution B is slowly splashed in the solution A, gel is placed 80 ℃ of dry down approximately 20h, get crystal; This crystal respectively at 550 ℃ of heat treatment 2h of Muffle furnace, is promptly obtained SiO
2-TiO
2Complex carrier.
(2) load of catalyst: according to V
2O
5Load capacity is 1.5% (mass percent), WO
3Load capacity be 7% (mass percent), respectively with NH
4VO
3And N
5H
37W6024H
2O is a predecessor, calculates the quality of required predecessor, under 60 ℃ of conditions of water-bath, prepares the aqueous solution of certain volume with the predecessor of metering.Adopt infusion process, with SiO
2-TiO
2Complex carrier impregnated in the solution of the ammonium metavanadate prepared and ammonium tungstate, concussion 24h, and 105 ℃ of dry 6h at 450 ℃ of calcinings of Muffle furnace 3h, obtain required catalyst then.
Detect: prepared catalyst is 900ppm in the NO volumetric concentration, and temperature is under 300 ℃, and oxygen concentration is 5%, NH
3Under/NO=1.0 the situation, the removal efficiency of NO is 85%; In the NO volumetric concentration is 900ppm, and temperature is under 150 ℃, and oxygen concentration is 5%, NH
3Under/NO=1.0 the situation, the removal efficiency of NO is 90%.
Embodiment 4:
(1) preparation of complex carrier: measure a certain amount of butyl titanate, slowly splash in the absolute ethyl alcohol of 4 times of volumes,, mix, form yellow settled solution A with the powerful 10min that stirs of magnetic stirring apparatus; To (press SiO with the ultra-pure water and the ethyl silicate of the same volume of butyl titanate
2/ (SiO
2-TiO
2)=5% calculates) be added in the absolute ethyl alcohol of other 4 times of volumes, obtain solution B; Add nitre acid for adjusting pH value≤3.
Under vigorous stirring, solution B is slowly splashed in the solution A, gel is placed 80 ℃ of dry down approximately 20h, get crystal; This crystal respectively at 550 ℃ of heat treatment 2h of Muffle furnace, is promptly obtained SiO
2-TiO
2Complex carrier.
(2) load of catalyst: according to V
2O
5Load capacity is 1% (mass percent), WO
3Load capacity be 6% (mass percent), respectively with NH
4VO
3(NH
4) 6Mo70244H
2O is a predecessor, calculates the quality of required predecessor, under 60 ℃ of conditions of water-bath, prepares the aqueous solution of certain volume with the predecessor of metering.Adopt infusion process, with SiO
2-TiO
2Complex carrier impregnated in the solution of the ammonium metavanadate prepared and ammonium tungstate, concussion 24h, and 105 ℃ of dry 6h at 450 ℃ of calcinings of Muffle furnace 3h, obtain required catalyst then.
Detect: prepared catalyst is 900ppm in the NO volumetric concentration, and temperature is under 300 ℃, and oxygen concentration is 5%, NH
3Under/NO=1.0 the situation, the removal efficiency of NO is 86%; In the NO volumetric concentration is 900ppm, and temperature is under 380 ℃, and oxygen concentration is 5%, NH
3Under/NO=1.0 the situation, SO
2Concentration be 1500ppm, H
2O concentration is under 6% situation, and the removal efficiency of NO is 75%.
Claims (2)
1. a catalyst that is used for the SCR denitration of boiler temperature flue gas is characterized in that: be to adopt sol-gel method to prepare SiO simultaneously
2And TiO
2The complex carrier that constitutes, the temperature that is suitable for boiler smoke is 320～450 ℃, is at SiO
2-TiO
2Supported V on the complex carrier
2O
5And WO
3The integrant composite catalyst of oxide; Said at SiO
2-TiO
2In the complex carrier that constitutes, SiO
2Account for by SiO
2-TiO
2The mass percent of the complex carrier that constitutes is 3%-10%; In the said catalyst, V
2O
5The catalyst component percentage that accounts for the catalyst total quality that comprises complex carrier be 1%～2%; WO
3The catalyst component percentage that accounts for the catalyst total quality that comprises complex carrier be 5%～10%.
2. Preparation of catalysts method that is used for the SCR denitration of boiler temperature flue gas as claimed in claim 1, it is characterized in that: preparation method's step is:
(1) preparation of complex carrier: measure a certain amount of butyl titanate, slowly splash in the absolute ethyl alcohol of 2-6 times of volume,, mix, form yellow settled solution A with the powerful 10min that stirs of magnetic stirring apparatus; To be added in the absolute ethyl alcohol of other 2-6 times of volume with the ultra-pure water and the silester of the same volume of butyl titanate, and obtain solution B, this silester is pressed SiO
2/ (SiO
2-TiO
2)=3-10% calculates; Add nitre acid for adjusting pH value≤3; Under vigorous stirring, solution B is slowly splashed in the solution A, gel is placed 80 ℃ of dry 20h down, get crystal; This crystal respectively at Muffle furnace 400-750 ℃ of heat treatment 2h, is promptly obtained SiO
2-TiO
2Complex carrier;
(2) load of catalyst: according to V
2O
5The load capacity mass percent is 1%-2%, WO
3The mass percent load capacity be 5-10%, respectively with NH
4VO
3And N
5H
37W6024H
2O is a predecessor, calculates the quality of required predecessor, and under 60 ℃ of conditions of water-bath, the aqueous solution with the predecessor preparation certain volume that measures adopts infusion process, with SiO
2-TiO
2Complex carrier impregnated in the solution of the ammonium metavanadate prepared and ammonium paratungstate, concussion 24h, and 105 ℃ of dry 6h at 450 ℃ of calcinings of Muffle furnace 3h, obtain required catalyst then.
Priority Applications (1)
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|---|---|---|---|
| CN2010102290087A CN101869833B (en) | 2010-07-16 | 2010-07-16 | Catalyst for SCR denitration of furnace middle temperature fume and preparation method thereof |
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|---|---|---|---|
| CN2010102290087A CN101869833B (en) | 2010-07-16 | 2010-07-16 | Catalyst for SCR denitration of furnace middle temperature fume and preparation method thereof |
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| CN101869833A CN101869833A (en) | 2010-10-27 |
| CN101869833B true CN101869833B (en) | 2012-01-11 |
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Families Citing this family (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102921405B (en) * | 2012-09-29 | 2014-10-08 | 重庆大学 | SiO2-containing denitration catalyst and preparation method thereof |
| CN103920503B (en) * | 2013-12-03 | 2016-04-13 | 华南理工大学 | A kind of modification regeneration SCR denitration and preparation method thereof |
| CN103623808A (en) * | 2013-12-10 | 2014-03-12 | 柳景惠 | Selective catalytic reduction (SCR) catalyst and preparation method thereof |
| CN105289580A (en) * | 2015-10-12 | 2016-02-03 | 安徽迪诺环保新材料科技有限公司 | Soaking type low-temperature honeycomb flue gas catalyst and preparation method thereof |
| CN106423139A (en) * | 2016-11-14 | 2017-02-22 | 包头稀土研究院 | Rare-earth-based SCR denitration catalyst and preparation method thereof |
| CN106799224A (en) * | 2017-01-03 | 2017-06-06 | 广西大学 | A kind of preparation method of sol-gel-dip method SCR denitration |
| CN109126841B (en) * | 2018-08-10 | 2020-08-14 | 太原理工大学 | Preparation of core-shell VPO @ SiO2Method for preparing catalyst |
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| CN1792431A (en) * | 2006-01-13 | 2006-06-28 | 清华大学 | Integral denitration catalyst using double-oxide as composite carrier and its prepn. method |
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Patent Citations (2)
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| CN1792431A (en) * | 2006-01-13 | 2006-06-28 | 清华大学 | Integral denitration catalyst using double-oxide as composite carrier and its prepn. method |
| CN101011659A (en) * | 2007-02-07 | 2007-08-08 | 南开大学 | Catalyst for SCR denitration in boiler low-temperature fume and preparation method thereof |
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| Title |
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