CN102389791A - Desulfurization and denitrification catalyst taking kaolin as carrier and preparation method thereof - Google Patents
Desulfurization and denitrification catalyst taking kaolin as carrier and preparation method thereof Download PDFInfo
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- CN102389791A CN102389791A CN2011102846849A CN201110284684A CN102389791A CN 102389791 A CN102389791 A CN 102389791A CN 2011102846849 A CN2011102846849 A CN 2011102846849A CN 201110284684 A CN201110284684 A CN 201110284684A CN 102389791 A CN102389791 A CN 102389791A
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Abstract
The invention relates to a desulfurization and denitrification catalyst taking kaolin as a carrier and a preparation method thereof, belonging to the technical field of atmospheric pollution control. The desulfurization and denitrification catalyst is characterized in that the catalyst takes the kaolin as the carrier and takes one component or two components of rare earth oxides, namely, lanthanum oxide and cerium oxide as active components, wherein the mass percentage of the lanthanum oxide and the mass percentage of the cerium oxide in the catalyst are respectively 2.5%-30% and 1%-20%, and the mass percentage of the kaolin in the catalyst is 70%-95%. In the catalyst, when two active components are adopted, the mass ratio of two metal elements, namely, lanthanum to cerium, is 2:1 to 1:2. The catalyst and the preparation method have the effects and benefits that: the preparation method of the catalyst is simple, and the raw materials are easy to get, so that the cost of the catalyst is greatly lowered, and the desulfurization and the denitrification can be synchronously realized; proved by a simulated flue gas test, when the temperature is 300-600 DEG C and the air speed is 12500-25000 h<-1>, the desulfurization rate of the catalyst is over 95%, and the denitrification rate of the catalyst is over 98%; and moreover, the desulphurisation byproduct elemental sulfur can be recycled in a resourcing manner so as to avoid secondary pollution.
Description
Technical field
The invention belongs to the air contaminant treatment technical field, relating to a kind of is the desulphurization denitration Catalysts and its preparation method of carrier with kaolin.
Background technology
The kaolin resource of China is abundant, relative low price, has been widely used in fields such as rubber, plastics, coating, papermaking and PETROLEUM PROCESSING at present.Kaolin also more and more comes into one's own in the application in environmental improvement field in recent years, and main research relates to the absorption and the degraded of poisonous and harmful substance in the sewage, but kaolin is still few in the application of air contaminant treatment technical field.
China is to be the coal-fired big country of energy-consuming main body with coal, and coal fired power generation can cause serious air environmental pollution, especially SO
2And NO
xExcessive emissions, can form acid rain under certain condition, serious threat ecological environment and health of human body.Flue gas desulfurization (FGD) and selective reduction denitration (SCR) technology that adopts gone up in industry at present, is two independently technical process, and wherein wet desulfurizing process is comparatively ripe; Flue gas desulfurization unit total capacity has been installed according to statistics up to 81.8%; But exist equipment huge, floor space is wide, and water consumption is big; The perishable pipeline of sulfuric acid, shortcoming such as the utilization rate of accessory substance gypsum is low.The denitrating flue gas field, the SCR technical application is the widest, but the catalyst use amount is big, the regeneration difficulty, and cost is higher.Independent desulfurization or denitration technology can not satisfy the current environmental protection requirement of China, and catalytic reduction synchronized desulfuring and denitrifying technology receives publicity day by day.
CN1288774 relates to a kind of catalyst of eliminating sulfur dioxide and nitrogen oxide in the gaseous mixture simultaneously, and described catalyst carrier is TiO
2, metal oxide cobalt oxide and nickel oxide are active component, said Preparation of catalysts process is that carrier, active component and ammoniacal liquor are obtained TiO through coprecipitation
2-CoS catalyst carries out the desulphurization denitration experiment under the CO effect, obtained certain effect, but because coprecipitation process is loaded down with trivial details, needs multistep washing and filtration, and TiO
2Cost is expensive, is unfavorable for the industrialization use.
People such as the Hu Hui of the Central China University of Science and Technology (Hu Hui, Li Jing, Zhang Shunxi, Li Shengli .CeO
2-La
2O
3/ γ-Al
2O
3Rare earth oxide mixture through catalytic reduction SO
2Experimental study [J] environmental science, 2004, (02) .), the series of rare earth catalyst that utilized immersion process for preparing, catalyst carrier is γ-Al
2O
3, active component is rare-earth oxide La
2O
3And CeO
2, the preparation process comprises technologies such as dipping, drying and roasting, this catalyst is under the CO effect, when reaction temperature is that 500～600 ℃, air speed are 2000h
-1The time denitrification efficiency reach 90%.But, catalyst consumption and running cost have been increased because reaction velocity is lower.
The Jia Lishan of University Of Tianjin (Jia Li mountain .O
2There is CO reduction SO down
2Catalyst research [D] for elemental sulfur. University Of Tianjin, 2004), utilize a series of catalyst such as the nitrate of Co, Ni, Fe, Mn and CoS that ammonium sulfate makes, NiS, FeS, MnS, catalytic reduction SO under the CO effect
2, desulfurization degree is higher.Shortcoming is that this catalyst does not have supported cheaply, the desulphurization reaction large usage quantity, and this catalyst does not relate to the Research on degradation to NO.
People such as Zhuang (S.-X.Zhuang, M.Yamazaki, K.Omata.Catalytic conversion ofCO, NO and SO
2On supported sulfide catalysts II.Catalytic reduction of NO and SO
2By CO.Applied Catalysis B:Environmental 31 (2001) 133-143) with γ-Al
2O
3For carrier, with CoMo, FeMo, Mo and Co are active component, the CoMo/Al of preparation
2O
3And FeMo/Al
2O
3Catalyst is at 500 ℃ of reaction temperatures, air speed 9000～36000h
-1Down, the removal efficiency of NO is up to 98%, and SO
2Removal efficiency only have 70%.
People such as Sun Fan (Sun Fan, Zhu Tao, Wang Lei, Ma Jianxin. SO on the rare earth oxide
2Desulfurization and denitrogenation research [J] with the perofskite type oxide catalyst of the catalytic reduction IV. doped Ce of NO. chemistry world, 2005 (7): 389-396) a kind of perovskite type catalyst by the preparation of nitrate mixed grinding method of research and development, preparation technology is with La
2O
3And Co (NO
3)
26H
2O obtains LaCoO through technologies such as grinding, roastings
3Catalyst, this catalyst have denitrification efficiency preferably under the CO effect.Shortcoming is that the catalyst carrier-free supports, and used metal oxide cost is very high.
Summary of the invention
Having the object of the present invention is to provide a kind of is the desulphurization denitration catalyst of carrier with kaolin, and this catalyst is made up of carrier and active component, and wherein carrier is a kaolin, and raw material is easy to get and low price.
Another object of the present invention is to provide that a kind of to be used to prepare above-mentioned be the method for the desulphurization denitration catalyst of carrier with kaolin, catalyst preparation process only relates to dipping and dry, has omitted roasting process, and preparation technology is simple, and energy consumption is low; Catalyst is at high-speed 10000～25000h
-1The time still keep very high desulphurization denitration active, desulfurization degree reaches more than 95%, the denitration rate reaches more than 98%, the accessory substance elemental sulfur has to recycle and is worth non-secondary pollution.
The objective of the invention is to realize through following technical scheme:
Desulphurization denitration catalyst of the present invention is made up of carrier and active constituent; With kaolin as catalyst carrier; Be the activity of such catalysts component with lanthana, cerium oxide one-component or two component respectively, wherein lanthana and the cerium oxide mass percent that accounts for catalyst is respectively 2.5～30% and 1～20%.The shared mass percent of kaolin is 70～95%.In above-mentioned catalyst, when adopting dual-active property component, the mass ratio of two kinds of metallic element lanthanums and cerium is 2: 1～1: 2.
Above-mentioned desulphurization denitration catalyst adopts infusion process to make, and concrete steps are following:
Step 1. preparation maceration extract: the solubility precursor of active constituent is water-soluble, be made into maceration extract;
Step 2. is got kaolin and is dissolved in the maceration extract that step 1 obtains, and is stirred well to even white suspension, normal temperature dipping 2～3d;
The dry moisture of removing of the suspension that step 3. obtains step 2, product through grind white powder;
With the rare nitric acid and the sesbania powder of the above-mentioned sample adding 9～10% that obtains, machine-shaping gets the catalyst finished product after the air dry.
Effect of the present invention and benefit are:
Catalyst according to the invention is a carrier with kaolin, and raw material sources are extensive, obtain easily, and cost is lower; The preparation method is simple, need not roasting, and the production process energy-saving effect is obvious; This catalyst can be realized synchronized desulfuring and denitrifying, and the simulated flue gas test shows is when temperature is that 300～600 ℃, air speed are 12500～25000h
-1The time, its desulfurization degree is more than 95%, and the denitration rate is more than 98%, but secondary pollution is avoided in the recycling of desulfurizing byproduct elemental sulfur resource.
The specific embodiment
Be described in detail specific embodiment of the present invention below in conjunction with technical scheme.
Embodiment 1
Accurate weighing 4g La (NO
3)
3.6H
2O is dissolved in the 100ml distilled water, constantly is stirred to dissolving fully, is mixed with the lanthanum nitrate aqueous solution of 4% (w/v).
With the dried kaolin of the accurate weighing 20g of assay balance, add in the lanthanum nitrate aqueous solution of above-mentioned preparation, while need adding kaolin, this process stirs simultaneously, obtain the lanthanum load capacity and be 20% white suspension.Above-mentioned white suspension is stirred 5h in 1400r/min, 60 ℃ of constant temperature, and products obtained therefrom still is white suspension.This white suspension normal temperature is left standstill 3d, and the moisture meeting natural evaporation in this process mixed liquor obtains white pasty solid.
With above-mentioned formation pasty solid dry 10h under 80 ℃ of dryings, obtain white blocks of solid, be ground into white powder.
(quality/g): 10 (volume/ml): 0.5 (ratio of quality/g) is evenly mixed extruded moulding with 15 with above-mentioned white powder and rare nitric acid of 9%, sesbania powder.Promptly get mass percent and be 15% La
2O
3-kaolin desulphurization denitration catalyst.
Test result shows in the simulated flue gas, works as SO
2Volumetric concentration is 1000ppm, and the NO volumetric concentration is 500ppm, and reducing gases CO volumetric concentration is 3000ppm, and air speed is 12500h
-1, reaction temperature is 500 ℃, SO
2Removal efficiency is 96%, and the NO removal efficiency is 98%.
Embodiment 2
Accurate weighing 4g Ce (NO
3)
3.6H
2O is dissolved in the 100ml distilled water, constantly is stirred to dissolving fully, is mixed with the cerous nitrate aqueous solution of 4% (w/v).
Accurately the dried kaolin of weighing 20g adds in the cerous nitrate aqueous solution of above-mentioned preparation, stirs simultaneously while this process need add kaolin, obtains the cerium load capacity and be 20% white suspension.Above-mentioned white suspension is stirred 5h in 1400r/min, 60 ℃ of constant temperature, and products obtained therefrom still is white suspension.This white suspension normal temperature is left standstill 3d, and the moisture meeting natural evaporation in this process mixed liquor obtains white paste matter.
With the dry 10h under 120 ℃ of the above-mentioned white paste matter after leaving standstill.Obtain white blocks of solid, be ground into white powder.
(quality/g): 10 (volume/ml): 0.5 (ratio of quality/g) is evenly mixed extruded moulding with 15 with above-mentioned white powder and rare nitric acid of 9%, sesbania powder.Promptly get mass percent and be 8% CeO
2-kaolin desulphurization denitration catalyst.
Test result shows in the simulated flue gas, works as SO
2Volumetric concentration is 1000ppm, and the NO volumetric concentration is 500ppm, and reducing gases CO volumetric concentration is 3000ppm, and air speed is 25000h
-1, reaction temperature is 600 ℃, SO
2Removal efficiency is 99%, and the NO removal efficiency is 98%.
Embodiment 3
Accurate weighing 1g La (NO
3)
3.6H
2O is dissolved in the 100ml distilled water, is mixed with the lanthanum nitrate aqueous solution of 4% (w/v).
Accurate weighing 1g Ce (NO
3)
3.6H
2O is dissolved in the above-mentioned 100ml that has disposed, 4% the lanthanum nitrate aqueous solution, is mixed with the aqueous solution that contains lanthanum nitrate and cerous nitrate each 4% (w/v).
Accurately the dried kaolin of weighing 20g adds in the above-mentioned 100ml mixed solution of having prepared, stirs simultaneously while this process need add kaolin, obtains white suspension.Place 1400r/min, 60 ℃ of constant temperature to stir 5h above-mentioned suspension, product still is white suspension.This white suspension normal temperature is left standstill 3d, and the moisture meeting natural evaporation in this process mixed liquor obtains white paste matter.
With above-mentioned white paste matter dry 12h under 120 ℃, obtain white blocks of solid.
To powder, (quality/g): 10 (volume/ml): 0.5 (ratio of quality/g) is evenly mixed, and extruded moulding promptly gets mass percent 3.75%-La with 15 with rare nitric acid of 9%, sesbania powder with the block solid abrasive of above-mentioned white
2O
3-2%CeO
2-kaolin desulphurization denitration catalyst.
Test result shows in the simulated flue gas, works as SO
2Volumetric concentration is 1000ppm, and the NO volumetric concentration is 500ppm, and reducing gases CO volumetric concentration is 3000ppm, and air speed is 25000h
-1, reaction temperature is 600 ℃, SO
2Removal efficiency is 99%, and the NO removal efficiency is 99%.
Claims (2)
1. one kind is the desulphurization denitration catalyst of carrier with kaolin, it is characterized in that described carrier is a kaolin, and active constituent is lanthanum, cerium or the two mixing; The mass percent of active constituent and carrier is 2.5～30% lanthana and/or 1～20% cerium oxide; When adopting dual-active property component, the mass ratio of two kinds of metallic element lanthanums and cerium is 2: 1～1: 2.
2. one kind is the desulphurization denitration Preparation of catalysts method of carrier with kaolin, it is characterized in that step is following:
Step 1. preparation maceration extract: the solubility precursor of active constituent is water-soluble, be made into maceration extract;
Step 2. is dissolved in kaolin in the maceration extract that above-mentioned steps 1 obtains, and is stirred to even white suspension, the suspension normal temperature dipping 2～3d of gained;
The dry moisture of removing of the suspension that step 3. obtains above-mentioned steps 2, product through grind white powder.
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Cited By (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103272618A (en) * | 2013-05-20 | 2013-09-04 | 大连理工大学 | Denitrating catalyst and preparation method thereof |
| CN105107493A (en) * | 2015-09-28 | 2015-12-02 | 江苏振宇环保科技有限公司 | Lanthanum and cerium compound desulfurization and denitrification catalyst |
| CN106975474A (en) * | 2017-03-10 | 2017-07-25 | 华南师范大学 | A kind of Ce based composite catalysts for being applied to vulcanization hydrogen catalysis reduction and desulfurization denitrating technique and preparation method thereof |
| CN108404651A (en) * | 2018-02-01 | 2018-08-17 | 中海油天津化工研究设计院有限公司 | A kind of desulfurizing agent for new dry process rotary kiln smoke catalytic desulfurization |
| CN110314681A (en) * | 2019-07-24 | 2019-10-11 | 华中科技大学 | One kind is based on kaolinic low temperature SCR denitration 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 |
| CN110813070A (en) * | 2019-11-15 | 2020-02-21 | 中国神华能源股份有限公司萨拉齐电厂 | Carbide slag modifier for desulfurization of circulating fluidized bed boiler, modified carbide slag and preparation method thereof |
| CN111346495A (en) * | 2020-03-31 | 2020-06-30 | 内蒙古包钢和发稀土有限公司 | Preparation method of metakaolin-based flue gas denitration agent |
| CN111450841A (en) * | 2020-05-22 | 2020-07-28 | 福州大学 | Reduction method simultaneous desulfurization and denitrification catalyst prepared from red mud and preparation method thereof |
| CN111715234A (en) * | 2020-07-24 | 2020-09-29 | 北京贞吉环保科技有限公司 | Can simultaneously remove CO and SO2And NOxCatalyst of (2) |
| CN111822009A (en) * | 2020-07-24 | 2020-10-27 | 北京贞吉环保科技有限公司 | Low-temperature desulfurization and denitrification catalyst and preparation method thereof |
| CN115532261A (en) * | 2021-06-29 | 2022-12-30 | 中国石油化工股份有限公司 | Heterogeneous Fenton catalyst and preparation method and application thereof |
| CN115672306A (en) * | 2022-11-01 | 2023-02-03 | 广东韩研活性炭科技股份有限公司 | Modified activated carbon for desulfurization and denitrification and preparation process thereof |
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Cited By (19)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103272618A (en) * | 2013-05-20 | 2013-09-04 | 大连理工大学 | Denitrating catalyst and preparation method thereof |
| CN105107493A (en) * | 2015-09-28 | 2015-12-02 | 江苏振宇环保科技有限公司 | Lanthanum and cerium compound desulfurization and denitrification catalyst |
| CN106975474B (en) * | 2017-03-10 | 2020-06-09 | 华南师范大学 | Ce-based composite catalyst suitable for hydrogen sulfide catalytic reduction desulfurization and denitrification process and preparation method thereof |
| CN106975474A (en) * | 2017-03-10 | 2017-07-25 | 华南师范大学 | A kind of Ce based composite catalysts for being applied to vulcanization hydrogen catalysis reduction and desulfurization denitrating technique and preparation method thereof |
| CN108404651A (en) * | 2018-02-01 | 2018-08-17 | 中海油天津化工研究设计院有限公司 | A kind of desulfurizing agent for new dry process rotary kiln smoke catalytic desulfurization |
| CN108404651B (en) * | 2018-02-01 | 2021-04-30 | 中海油天津化工研究设计院有限公司 | Desulfurizing agent for novel dry-process cement kiln flue gas catalytic desulfurization |
| CN110314681A (en) * | 2019-07-24 | 2019-10-11 | 华中科技大学 | One kind is based on kaolinic low temperature SCR denitration 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 |
| 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 |
| CN110813070A (en) * | 2019-11-15 | 2020-02-21 | 中国神华能源股份有限公司萨拉齐电厂 | Carbide slag modifier for desulfurization of circulating fluidized bed boiler, modified carbide slag and preparation method thereof |
| CN111346495A (en) * | 2020-03-31 | 2020-06-30 | 内蒙古包钢和发稀土有限公司 | Preparation method of metakaolin-based flue gas denitration agent |
| CN111346495B (en) * | 2020-03-31 | 2022-04-22 | 内蒙古包钢和发稀土有限公司 | Preparation method of metakaolin-based flue gas denitration agent |
| CN111450841A (en) * | 2020-05-22 | 2020-07-28 | 福州大学 | Reduction method simultaneous desulfurization and denitrification catalyst prepared from red mud and preparation method thereof |
| CN111715234A (en) * | 2020-07-24 | 2020-09-29 | 北京贞吉环保科技有限公司 | Can simultaneously remove CO and SO2And NOxCatalyst of (2) |
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| CN115532261A (en) * | 2021-06-29 | 2022-12-30 | 中国石油化工股份有限公司 | Heterogeneous Fenton catalyst and preparation method and application thereof |
| CN115532261B (en) * | 2021-06-29 | 2024-01-12 | 中国石油化工股份有限公司 | Heterogeneous Fenton catalyst and preparation method and application thereof |
| CN115672306A (en) * | 2022-11-01 | 2023-02-03 | 广东韩研活性炭科技股份有限公司 | Modified activated carbon for desulfurization and denitrification and preparation process thereof |
| CN115672306B (en) * | 2022-11-01 | 2023-08-22 | 广东韩研活性炭科技股份有限公司 | Modified activated carbon for desulfurization and denitrification and preparation process thereof |
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Application publication date: 20120328 |