CN102527369A - Reduction denitration catalyst for activated carbon loaded rare-earth metal oxide, as well as preparation method and application thereof - Google Patents
Reduction denitration catalyst for activated carbon loaded rare-earth metal oxide, as well as preparation method and application thereof Download PDFInfo
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- CN102527369A CN102527369A CN2011104454156A CN201110445415A CN102527369A CN 102527369 A CN102527369 A CN 102527369A CN 2011104454156 A CN2011104454156 A CN 2011104454156A CN 201110445415 A CN201110445415 A CN 201110445415A CN 102527369 A CN102527369 A CN 102527369A
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Abstract
The invention relates to a reduction denitration catalyst for an activated carbon loaded rare-earth metal oxide, as well as a preparation method and an application thereof and belongs to the technical field of atmospheric pollution treatment. The activated carbon is taken as a carrier of the denitration catalyst; the rare-earth metal cerium or the dual components of lanthanum and cerium are taken as the active components of the catalyst; when the cerium is single loaded, the mass percents of cerium and activated carbon are respectively 3.2-6.5wt%; and when the dual components of lanthanum and cerium are loaded, the mass percents of lanthanum and cerium as well as activated carbon are respectively 0.8-1.6wt% and 1.6-3.2wt%. The reduction denitration catalyst provided by the invention has the beneficial effects that the source of the raw materials of the carrier activated carbon is wide; the preparation process of the catalyst is simple; the reduction gases, such as, NH3, CO, and the like, do not need to be added as a reducing agent in a denitration reaction; the operation safety in a plant workshop is increased; no secondary pollution exists; and the denitration ratio is kept above 95% under a condition of high airspeed.
Description
Technical field
The invention belongs to the air contaminant treatment technical field, relate to a kind of activated carbon supported rare-earth oxide reduction denitrating catalyst, preparation method and application thereof.
Background technology
NO in recent years
XBecome power plant emission pollutant relaying SO
2A large focal spot afterwards, its harm mainly comprise and bring out photochemical fog, acid rain, ozone cavity, cause greenhouse effects etc.China NO
XThe industrial source emission behaviour very serious, these emission sources are concentrated and are distributed in city and areal of industrial concentration territory, floss hole is low, NO
XDense, potential hazard property is big.SO continues
2Afterwards, during the Chinese Ministry of Environmental Protection " 12 " with NO
XAlso include overall control in, formulated concrete reduction of discharging target.
Gas denitrifying technology mainly contains selective catalytic reduction (SCR method), non-selective catalytic reduction and absorption method at present.The SCR method has that reaction temperature is low, purifying rate is high, and process equipment is compact, reliable, advantages such as the nitrogen emptying after the reduction, non-secondary pollution.But the catalyst preparation process of SCR method is complicated, and use cost is high; Unreacted NH in the denitration reaction system
3SO in meeting and the flue gas
2Reaction generates perishable and (NH occluding device
4)
2SO
4And NH
4HSO
4, reduced the utilization rate of ammonia, aggravated equipment corrosion; In addition, the transportation of reducing agent ammonia and use cost be high, have potential safety hazard, hindered the SCR broad application.The reducing agent that non-selective catalytic reduction is commonly used is generally CO, H
2, propane etc., its denitration rate is very high, but reducing agent itself is difficult for transportation and stores, and has potential safety hazard.Absorption method is simple to operate, be easy to control, but adsorbents adsorb capacity commonly used is little, and consumption is big, and equipment is huge, and cost of investment is high.
Active carbon (Ac) unique chemical character makes it under suitable reaction condition, show the favorable denitrification performance, compares with the SCR method, and material source is abundant, easy to operate when using, potential safety hazard is low, convenient transportation.Rare earth metal is a kind of as non-ferrous metal, has a series of properties, and as carbon and oxygen are had extremely strong chemical affinity, heat resistanceheat resistant performance preferably etc., this possibly make it, and reaction has special catalytic effect to C-NO.Active carbon is used for the research of denitrating flue gas very early, but focuses mostly in simple cryogenic absorption denitration or merely as catalyst carrier (need extra interpolation reducing agent), activated carbon supported rare earth metal is less relatively as the report of catalyst carrier and reducing agent.
CN1597095A relates to a kind of catalyst that is used to remove flue gas nitrogen oxide, and this catalyst consists of 90～99.9% active carbon and 0.1～10% vanadic anhydride, adopts equi-volume impregnating, makes through dipping, dry, calcining and oxidation.This invention has higher removal of nitrogen oxide rate under the ammonia existence condition, can overcome dust blockage problem in the flue gas, and bed pressure drop is little, is fit to industrial applications.But use NH
3Make reducing agent, equipment investment and cost of transportation are high, and security of operation hidden danger is high.
People such as Wang Xiaolei (Wang Xiaolei, Piao Guilin, Xie Hao, Zhao Xiaoyuan. the active carbon Selective Catalytic Reduction of NO
X[J], Southeast China University's journal, 2011 (41): 145-149) adopt carbon compositing catalyst, NH
3Be reducing agent, carried out active carbon denitration Experimental Study of Mechanism, the result shows that its denitration efficiency is merely 50～88%, and efficient is low, and removal efficiency is unstable, and with ammonia as reducing agent.
People such as Chu heroes (Chu heroes, Liu Chao, Song Peng, Yin Huaqiang, Guo Jiaxiu. preparation condition is to Ce/Ac catalyst low temperature C
3H
6The influence of Selective Catalytic Reduction of NO [J], Sichuan University's journal, 2011 (43): a series of Ce/Ac catalyst that 160-164.) adopted immersion process for preparing, with C
3H
6Be reducing agent, in 270 ℃ to 330 ℃ temperature range, denitration efficiency is 70%.Compare other non-selective catalytic reduction methods, this catalyst operating temperature decreases, but the Preparation of catalysts process need carries out high-temperature roasting under nitrogen protection, and energy consumption is high, and to adopt methane be reducing agent, and cost is high.
Wan Xiankai et al. (Wan Xiankai, Zou Xuequan, Shi Huixiang, Wang Dahui.Nitrogen doping of activated carbon loading Fe
2O
3And activity in carbon-nitric oxide reaction [J] .Journal of Zhejiang University Science A, 2007,8 (5): 707-711.) with the load Fe of immersion process for preparing
2O
3People (Zhou Weiming such as activated-carbon catalyst and Zhou Weiming; Du Lizhen, Shi Huixiang, Wang is dizzy greatly. the research [J] of the active carbon reductive NO of lanthanum oxide-carrying; Environmental pollution and improvement; 2006 (28): the 676-679) activated carbon granule of the lanthanum oxide-carrying of employing immersion process for preparing, all adopt active carbon to carry out denitration reaction as carrier and reducing agent, overcome other reducing agents of extra use (CO, NH
3, propane etc.) problem, the security that has improved denitrification process has reduced factory management and operation risk.But load Fe
2O
3Activated-carbon catalyst, require the denitration temperature higher, when temperature reached more than 700 ℃, the denitration rate was 95%; And when temperature was between 500～600 ℃, its denitration rate was merely 50～75%.The activated-carbon catalyst of lanthanum oxide-carrying needs higher denitration temperature equally, and only when temperature reached 800 ℃, the denitration rate just rose to 99%; And the denitration rate is merely 50～80% in the time of 500 ℃.And the preparation process of the activated-carbon catalyst of lanthanum oxide-carrying not only needs also need under the protection of argon gas, carry out drying and high-temperature roasting with activated carbon modified preparation condition harshness, complex process, energy consumption height.
Summary of the invention
To the deficiency and the defective of prior art, a kind of activated carbon supported rare-earth oxide reduction denitrating catalyst, preparation method have been the object of the present invention is to provide.Active carbon is a catalyst carrier, is again reducing agent, and the source is abundant, industrial applications is safe.The active constituent of load is rare earth metal cerium or cerium and lanthanum bi-component, and catalyst adopts immersion process for preparing, and technology is simple, and is with low cost, and at high-speed 8000～12000h
-1Still can keep high denitration activity, denitration rate to reach more than 95% down, non-secondary pollution.
The object of the invention is realized through following technical scheme:
One side of the present invention is: a kind of activated carbon supported rare-earth oxide reduction denitrating catalyst, and catalyst is made up of as follows carrier active carbon and active constituent by mass percentage:
When described active constituent was cerium, the mass percent of cerium and active carbon was 3.2～6.5% in the catalyst;
When described active constituent was the two component of lanthanum and cerium, the mass percent of lanthanum and active carbon was 0.8～1.6% in the catalyst, and the mass percent of cerium and active carbon is 1.6～3.2%.
Other one side of the present invention is: a kind of preparation method of activated carbon supported rare-earth oxide reduction denitrating catalyst, and it may further comprise the steps:
(a) take by weighing raw material respectively in following ratio, the mass ratio of water and active carbon is 1～4: 1, and the mass ratio of nitrate hydrate crystal and active carbon is 10～20%;
(b) above-mentioned nitrate hydrate crystal is soluble in water, stir it is fully dissolved after, again to wherein adding active carbon and fully stir, in normal temperature dipping 2～3 days;
(c) sample that above-mentioned steps (b) is obtained dries by the fire under 80～120 ℃ to the sample constant weight, promptly gets product catalyst.
Of the present invention more on the one hand: the application of above-mentioned activated carbon supported rare-earth oxide reduction denitrating catalyst aspect denitration reaction, when reaction temperature is 500～600 ℃, air speed is 8000～12000h
-1The time, the denitration rate reaches 95～99%.
Effect of the present invention and benefit are:
Activated carbon supported rare-earth oxide reduction denitrating catalyst of the present invention is a carrier with the active carbon, and raw material sources are extensive, and preparation technology only comprises dipping and dry, and simple to operate, energy consumption is low; Active carbon plays the effect of catalyst carrier and reducing agent simultaneously, and denitration reaction need not to add NH
3, reducing gas such as CO makes reducing agent, improved the security of factory floor operation, the denitrating technique flow process is simple, non-secondary pollution; The denitration reaction air speed is high, and catalyst amount is few; The denitration test result shows under the distribution condition, at 500～600 ℃ of temperature, air speed 8000～12000h
-1The time, the denitration rate reaches 95～99%.
The specific embodiment
Below in conjunction with instance the present invention is further described, following non-limiting example can make those of ordinary skill in the art more fully understand the present invention, but does not limit the present invention in any way.
Active carbon: source water-purifying material factory of Gongyi City, Henan Province section, cas number: 64365-11-3.
Embodiment 1
Accurate weighing 8g Ce (NO
3)
3.6H
2The O crystal is dissolved in the 40ml distilled water, constantly is stirred to dissolving fully, is mixed with the cerous nitrate aqueous solution of 16.7wt%.
Accurately weighing 40g active carbon adds in the cerous nitrate aqueous solution of above-mentioned preparation, and the limit adds the active carbon limit stirs, and normal temperature left standstill 2 days, in 120 ℃ of oven dry down, promptly gets the active carbon of load C e 6.45wt%.
Place fixed bed reactors to carry out denitration experiment above-mentioned catalyst, test result shows, when the NO volumetric concentration is 500ppm, air speed is 10000h
-1, when reaction temperature was 600 ℃, the NO removal efficiency was 99%.
Embodiment 2
Accurate weighing 2g La (NO
3)
3.6H
2The O crystal is dissolved in the 80ml distilled water, is mixed with the lanthanum nitrate aqueous solution of 2.4wt%.
Accurate weighing 2g Ce (NO
3)
3.6H
2The O crystal is dissolved in the lanthanum nitrate aqueous solution of the above-mentioned 80ml that has disposed, 2.4wt%, is mixed with the mixed aqueous solution of 2.4wt% lanthanum nitrate and 2.4wt% cerous nitrate.
Accurately weighing 40g active carbon adds in the mixed liquor of above-mentioned cerous nitrate and lanthanum nitrate, and the limit adds the active carbon limit stirs, and normal temperature left standstill 2 days, in 120 ℃ of oven dry down, promptly gets the active carbon of load La 1.6wt% and Ce 1.6wt%.
Place fixed bed reactors to carry out denitration experiment above-mentioned catalyst, test result shows, when the NO volumetric concentration is 500ppm, air speed is 8000h
-1, when reaction temperature was 550 ℃, the NO removal efficiency was 98%.
Embodiment 3
Accurate weighing 2g Ce (NO
3)
3.6H
2The O crystal is dissolved in the 20ml distilled water, constantly is stirred to dissolving fully, is mixed with the cerous nitrate aqueous solution of 9.1wt%.
Accurately weighing 20g active carbon adds in the cerous nitrate aqueous solution of above-mentioned preparation, and the limit adds the active carbon limit stirs, and normal temperature left standstill 3 days, in 80 ℃ of oven dry down, promptly gets the active carbon of load C e 3.2wt%.
Place fixed bed reactors to carry out denitration experiment above-mentioned catalyst, test result shows, when the NO volumetric concentration is 500ppm, air speed is 12000h
-1, when reaction temperature was 600 ℃, the NO removal efficiency was 99%.
Embodiment 4
Accurate weighing 1gLa (NO
3)
3.6H
2The O crystal is dissolved in the 40ml distilled water, is mixed with the lanthanum nitrate aqueous solution of 2.4wt%.
Accurate weighing 2g Ce (NO
3)
3.6H
2The O crystal is dissolved in the lanthanum nitrate aqueous solution of the above-mentioned 40ml that has disposed, 2.4wt%, is mixed with the aqueous solution of 2.4wt% lanthanum nitrate and 4.6wt% cerous nitrate.
Accurately weighing 20g active carbon adds in the mixed liquor of above-mentioned cerous nitrate and lanthanum nitrate, and the limit adds the active carbon limit stirs, and normal temperature left standstill 2 days, in 120 ℃ of oven dry down, promptly gets the active carbon of load La 1.6wt% and Ce3.2wt%.
Place fixed bed reactors to carry out denitration experiment above-mentioned catalyst, test result shows, when the NO volumetric concentration is 500ppm, air speed is 8000h
-1, when reaction temperature was 500 ℃, the NO removal efficiency was 96%.
Embodiment 5
Accurate weighing 3g Ce (NO
3)
3.6H
2The O crystal is dissolved in the 80ml distilled water, constantly is stirred to dissolving fully, is mixed with the cerous nitrate aqueous solution of 3.6wt%.
Accurately weighing 20g active carbon adds in the cerous nitrate aqueous solution of above-mentioned preparation, and the limit adds the active carbon limit stirs, and normal temperature left standstill 3 days, in 100 ℃ of oven dry down, promptly gets the active carbon of load C e 4.8wt%.
Place fixed bed reactors to carry out denitration experiment above-mentioned catalyst, test result shows, when the NO volumetric concentration is 500ppm, air speed is 10000h
-1, when reaction temperature was 500 ℃, the NO removal efficiency was 95%.
Embodiment 6
Accurate weighing 0.5g La (NO
3)
3.6H
2The O crystal is dissolved in the 80ml distilled water, is mixed with the lanthanum nitrate aqueous solution of 0.6wt%.
Accurate weighing 2g Ce (NO
3)
3.6H
2The O crystal is dissolved in the lanthanum nitrate aqueous solution of the above-mentioned 80ml that has disposed, 0.6wt%, is mixed with the aqueous solution of 0.6wt% lanthanum nitrate and 2.4wt% cerous nitrate.
Accurately weighing 20g active carbon adds in the cerous nitrate and lanthanum nitrate mixed liquor of above-mentioned preparation, and the limit adds the active carbon limit stirs, and normal temperature left standstill 3 days, in 120 ℃ of oven dry down, promptly gets the active carbon of load La 0.8wt% and Ce 3.2wt%.
Place fixed bed reactors to carry out denitration experiment above-mentioned catalyst, test result shows, when the NO volumetric concentration is 500ppm, air speed is 12000h
-1, when reaction temperature was 600 ℃, the NO removal efficiency was 99%.
The comparative example 1
Accurately weighing 7.5g active carbon places fixed bed reactors, carries out the denitration experiment, and test result shows that the NO volumetric concentration is 500ppm, and air speed is 8000h
-1, when reaction temperature is 600 ℃, NO removal efficiency 20%.
The comparative example 2
Accurately weighing 5g active carbon places fixed bed reactors, carries out the denitration experiment, and test result shows that the NO volumetric concentration is 500ppm, and air speed is 12000h
-1, when reaction temperature was 500 ℃, the NO removal efficiency was 8%.
Claims (3)
1. activated carbon supported rare-earth oxide reduction denitrating catalyst is characterized in that catalyst is made up of as follows carrier active carbon and active constituent by mass percentage:
When described active constituent was cerium, the mass percent of cerium and active carbon was 3.2～6.5% in the catalyst;
When described active constituent was the two component of lanthanum and cerium, the mass percent of lanthanum and active carbon was 0.8～1.6% in the catalyst, and the mass percent of cerium and active carbon is 1.6～3.2%.
2. the preparation method of a kind of activated carbon supported rare-earth oxide reduction denitrating catalyst as claimed in claim 1 is characterized in that, may further comprise the steps:
(a) take by weighing raw material respectively in following ratio, the mass ratio of water and active carbon is 1～4: 1, and the mass ratio of nitrate hydrate crystal and active carbon is 10～20%;
(b) above-mentioned nitrate hydrate crystal is soluble in water, stir it is fully dissolved after, again to wherein adding active carbon and fully stir, in normal temperature dipping 2～3 days;
(c) sample that above-mentioned steps (b) is obtained dries by the fire under 80～120 ℃ to the sample constant weight, promptly gets product catalyst.
3. the application of a kind of activated carbon supported rare-earth oxide reduction denitrating catalyst as claimed in claim 1 aspect denitration reaction is characterized in that, when reaction temperature is 500～600 ℃, air speed is 8000～12000h
-1The time, its denitration rate reaches 95～99%.
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|---|---|---|---|---|
| CN103191710A (en) * | 2013-03-15 | 2013-07-10 | 大连理工大学 | Denitrifying catalyst preparation method and application of denitrifying catalyst prepared by same in denitration |
| CN105170150A (en) * | 2015-10-12 | 2015-12-23 | 重庆科技学院 | Supported metallic oxide catalyst for assisting microwave denitration and preparation method and using method thereof |
| CN105170131A (en) * | 2015-09-10 | 2015-12-23 | 广州中国科学院先进技术研究所 | Preparation method of novel sludge carbon-based desulfurization and denitrification catalyst |
| CN106345453A (en) * | 2016-08-26 | 2017-01-25 | 成都国化环保科技有限公司 | Carbon-based material low-temperature denitrification catalyst and preparation method thereof |
| CN106391041A (en) * | 2015-07-28 | 2017-02-15 | 江苏吉华化工有限公司 | Catalyst for treating chemical industry organic wastewater |
| CN106669673A (en) * | 2015-11-11 | 2017-05-17 | 中国石油化工股份有限公司 | Method for preparing CO (Carbon Monoxide) reduction denitration catalyst |
| CN106794442A (en) * | 2014-07-22 | 2017-05-31 | 康宁股份有限公司 | The method of the nano particle based on transition metal that manufacture activated carbon is carried |
| CN108283883A (en) * | 2017-01-09 | 2018-07-17 | 青州日新特种材料有限公司 | NO in a kind of removing flue gasxMethod |
| CN108283920A (en) * | 2017-01-09 | 2018-07-17 | 青州日新特种材料有限公司 | A kind of de- NOx catalyst and preparation method thereof |
| CN110354839A (en) * | 2019-08-20 | 2019-10-22 | 北京晨晰环保工程有限公司 | A kind of cerium based composite metal oxidate nanometer floral material and the preparation method and application thereof |
| US11058993B2 (en) | 2017-09-30 | 2021-07-13 | Environment Sustainable System Engineering Technology Co., Ltd. | Dry desulfurizing and denitrificating agent, and its preparation method and applications |
| CN114849687A (en) * | 2022-03-24 | 2022-08-05 | 山东亮剑环保新材料有限公司 | Preparation method of rare earth modified composite activated carbon-based catalyst |
| WO2023020295A1 (en) * | 2021-08-19 | 2023-02-23 | 南京工业大学 | Difunctional powder, and preparation method therefor and use thereof |
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| CN103191710A (en) * | 2013-03-15 | 2013-07-10 | 大连理工大学 | Denitrifying catalyst preparation method and application of denitrifying catalyst prepared by same in denitration |
| CN106794442A (en) * | 2014-07-22 | 2017-05-31 | 康宁股份有限公司 | The method of the nano particle based on transition metal that manufacture activated carbon is carried |
| CN106391041A (en) * | 2015-07-28 | 2017-02-15 | 江苏吉华化工有限公司 | Catalyst for treating chemical industry organic wastewater |
| CN105170131A (en) * | 2015-09-10 | 2015-12-23 | 广州中国科学院先进技术研究所 | Preparation method of novel sludge carbon-based desulfurization and denitrification catalyst |
| CN105170150A (en) * | 2015-10-12 | 2015-12-23 | 重庆科技学院 | Supported metallic oxide catalyst for assisting microwave denitration and preparation method and using method thereof |
| CN106669673A (en) * | 2015-11-11 | 2017-05-17 | 中国石油化工股份有限公司 | Method for preparing CO (Carbon Monoxide) reduction denitration catalyst |
| CN106669673B (en) * | 2015-11-11 | 2019-05-21 | 中国石油化工股份有限公司 | A kind of preparation method of CO reduction denitrating catalyst |
| CN106345453A (en) * | 2016-08-26 | 2017-01-25 | 成都国化环保科技有限公司 | Carbon-based material low-temperature denitrification catalyst and preparation method thereof |
| CN108283920A (en) * | 2017-01-09 | 2018-07-17 | 青州日新特种材料有限公司 | A kind of de- NOx catalyst and preparation method thereof |
| CN108283883A (en) * | 2017-01-09 | 2018-07-17 | 青州日新特种材料有限公司 | NO in a kind of removing flue gasxMethod |
| CN108283920B (en) * | 2017-01-09 | 2021-07-27 | 青州日新特种材料有限公司 | NOx removal catalyst and preparation method thereof |
| US11058993B2 (en) | 2017-09-30 | 2021-07-13 | Environment Sustainable System Engineering Technology Co., Ltd. | Dry desulfurizing and denitrificating agent, and its preparation method and applications |
| CN110354839A (en) * | 2019-08-20 | 2019-10-22 | 北京晨晰环保工程有限公司 | A kind of cerium based composite metal oxidate nanometer floral material and the preparation method and application thereof |
| CN110354839B (en) * | 2019-08-20 | 2022-11-18 | 北京晨晰环保工程有限公司 | Cerium-based composite metal oxide nanoflower material and preparation method and application thereof |
| WO2023020295A1 (en) * | 2021-08-19 | 2023-02-23 | 南京工业大学 | Difunctional powder, and preparation method therefor and use thereof |
| CN114849687A (en) * | 2022-03-24 | 2022-08-05 | 山东亮剑环保新材料有限公司 | Preparation method of rare earth modified composite activated carbon-based catalyst |
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Application publication date: 20120704 |