CN109794248A - A kind of low cost catalyst for denitrating flue gas and its preparation, application method - Google Patents
A kind of low cost catalyst for denitrating flue gas and its preparation, application method Download PDFInfo
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- CN109794248A CN109794248A CN201910049202.8A CN201910049202A CN109794248A CN 109794248 A CN109794248 A CN 109794248A CN 201910049202 A CN201910049202 A CN 201910049202A CN 109794248 A CN109794248 A CN 109794248A
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Abstract
A kind of low cost catalyst for denitrating flue gas, is the flying dust loaded metal ion catalyst being prepared by metal salt, flying dust；The mass ratio of metal and flying dust is 1:20-1:10 in the catalyst.The present invention by flying ash in electric power plant, active component presoma thermal decomposition and the equally distributed process conformity of active component together.The relatively smooth densification in flying ash in electric power plant surface, keep the hole of flying dust flourishing using autoclave, pore structure is more abundant, steam activation is used simultaneously, be conducive to active component in the more full and uniform distribution of carrier ash surface, active component iron zinc-copper metal oxide in catalyst improves the denitration efficiency of catalyst, effective denitration time extends with the presence of nano-scale particle size；Catalyst has higher denitration efficiency, and denitration precision is high, to the NO in flue gasXRemoving ability is strong；Catalyst carrier flying dust raw material, it is cheap and easy to get, it is without secondary pollution, reduce cost；Apparatus and process is simple, and cost of investment is low.
Description
Technical field
The present invention relates to gas denitrifying technology field more particularly to a kind of inexpensive catalyst for denitrating flue gas and its preparation,
Application method.
Background technique
Coal is currently one of the main energy sources in China, and coal-fired plant boiler discharges a large amount of SO2、NOX, mercury, particle and its
His microelement is discharge SO2And NOXThe main industries of equal pollutants.Especially in recent years, with national wide range of haze day
The formation and diffusion of gas, it is coal-fired caused by the atmosphere polluting problem highest attention by government and the public.At the same time, it is firing
During coal, the solid waste such as a large amount of flyash can be generated, pollute environment.China still falls within the utilization of flyash low
Level, how Efficient Development and using flyash be also deeply hot issue that current insider extremely pays close attention to.Although with height
Development and application based on added value silica aerogel product are one of the directions of flyash future development, but there are secondary pollution,
The problems such as complex process.Therefore, how cost-effective removing coal-fired flue-gas nitrogen oxides and discarded flyash is efficiently utilized
It is China's fire coal industry problem in the urgent need to address.Currently, with NH3It is existing for reduced form Selective Catalytic Reduction of NO x (SCR)
Main denitrating technique used by stage coal-burning power plant, catalyst are the cores of SCR gas denitrifying technology, and the composition of catalyst is straight
Connect the effect for influencing denitrating flue gas.Currently, catalyst, based on V/Ti system, ingredient is all V mostly2O5, such catalyst contains
Severe toxicity is also easy to produce secondary pollution in catalyst production and use process.Patent CN1777477 and patent CN1792431 are
With V2O5-WO3/TiO2For active component, denitration efficiency is high, but there is also co-catalyst WO3And MoO3Cost of material it is high, be added
Measure the problems such as big.Patent CN107335466A is using yttria, tungstic acid, manganese dioxide and titanium dioxide as active group
Point, molecular sieve and activated alumina are complex carrier, which has good denitration effect, high denitrification rate dimension
It is long to hold the time.Used carrier is at high cost, preparation process is more complex, this materially increases operating cost, hinders this
The application of technology.To overcome disadvantages mentioned above, exploitation new type low temperature catalyst for denitrating flue gas is the cutting edge technology of current denitrating flue gas
One of.Flyash is one of biggish industrial residue of the current discharge capacity in China at present, with the development of power industry, coal-burning power plant
Flyash discharge capacity increases year by year.A large amount of flyash is untreated, will generate fugitive dust, pollutes atmosphere；If being discharged into water system meeting
River is caused to silt up, and toxic chemical substance therein can also cause damages to human body and biology.But flyash be again can be with
The resource of exploitation, in terms of being especially used in civil construction material, can not only thoroughly solve to stack land occupation and environmental pollution problem and
And have significant economic benefit and environmental benefit, or even also there is special technical advantage, the performance of these materials can be improved.Cause
This, the recycling of flyash is the key subjects of current economy and society development, and to one that contemporary science and technology proposes
New issue.How efficiently, having developed and utilized to high added value flyash is one of technology for being worth research and discovery.Utilize powder
Coal ash can not only bring huge economic benefits as catalyst for denitrating flue gas carrier, moreover it is possible to reduce environmental pollution, realize fine coal
Grey solid waste and atmosphere pollution comprehensive treatment.
Summary of the invention
The present invention is at high cost in order to solve catalyst in existing denitration technology, and the stronger problem of active component toxicity provides
A kind of inexpensive catalyst for denitrating flue gas and its preparation, application method.The present invention selects flying ash in electric power plant as catalyst carrier
Active component iron zinc-copper is added, the catalyst of flying dust load iron zinc-copper ternary metal oxide is prepared and constructs makes accordingly
Use method.Catalyst of the invention can reduce denitration cost, without secondary pollution, while catalyst catalysis with higher is also
Former denitration performance can be widely used in the large-scale flue gas emission such as iron and steel enterprise, coal-burning power plant, Industrial Stoves, metallurgy industry enterprise
Catalytic denitration, be suitable for from high NO concentration to low NO concentration enterprise denitrating flue gas, reach discharge standard.
To achieve the above object, the present invention is implemented with the following technical solutions:
A kind of low cost catalyst for denitrating flue gas, is the flying dust supported nano-gold category oxygen being prepared by metal salt, flying dust
Compound catalyst；The mass ratio of metal and flying dust is 1:20-1:10 in the catalyst.
The metal salt is one or more of molysite, zinc salt, mantoquita.
The metal salt is the mixture of molysite, zinc salt, mantoquita, metal iron ion and gold in preparation-obtained catalyst
Belong to zinc ion, the mass ratio of metal copper ion is 18:1:1~9:1:1.
The flying dust is flying ash in electric power plant.
A kind of preparation method of low cost catalyst for denitrating flue gas, includes the following steps:
1) by flying dust, drying to constant weight；
2) solid metal salt is dissolved into deionized water, obtains metal salt solution, by flying dust and metal salt solution in height
It presses in kettle and is uniformly mixed, impregnate 20-40min at pressure 3-6MPa, 40-60 DEG C of temperature, mixture is cooled to room temperature, instill
Ammonium hydroxide continues mechanical stirring 0.5-1h until pH value of solution is 9-10, and mixture is taken out and is filtered, drying to constant weight again；
3) drying object for obtaining step 2) is put into fixed bed reactors, under nitrogen atmosphere protection, in crucible furnace
It is warming up to 600-700 DEG C and is passed through vapor and calcined and gasified 15-30min, be down to room temperature, obtain catalyst.
In the metal salt solution, the ratio of the quality and volume of metal ion and deionized water is 1:20-1:10.
A kind of application method of low cost catalyst for denitrating flue gas, includes the following steps:
1) NO will be containedXFlue gas be passed through in catalyst, carry out catalysis reduction removing flue gas in NO；
2) flue gas is 3~6s by the residence time of catalyst in fixed bed denitrating tower；
3) the denitration temperature of catalyst is 200~400 DEG C.
Compared with prior art, the beneficial effects of the present invention are:
1) by flying ash in electric power plant, the thermal decomposition of active component presoma and the equally distributed process conformity of active component one
It rises.The relatively smooth densification in flying ash in electric power plant surface keeps the hole of flying dust flourishing using autoclave, and pore structure is more abundant,
Steam activation is used simultaneously, is conducive to work of the active component in the more full and uniform distribution of carrier ash surface, catalyst
Property component of iron zinc-copper metal oxide with the presence of nano-scale particle size, the denitration efficiency of catalyst is improved, when effective denitration
Between extend；
2) catalyst has higher denitration efficiency, and denitration precision is high, to the NO in flue gasXRemoving ability is strong；
3) catalyst carrier flying dust raw material, it is cheap and easy to get, it is without secondary pollution, reduce cost；
4) apparatus and process is simple, and cost of investment is low.
Detailed description of the invention
Fig. 1 is flying dust load active component metal oxide catalyst preparation method flow chart of the present invention；
The denitration efficiency curve of flying dust load Fe-Zn-Cu catalyst at different temperatures in Fig. 2 embodiment of the present invention 3
Variation diagram；
Denitration efficiency curvilinear motion figure of the different catalysts at 350 DEG C in Fig. 3 embodiment of the present invention 1-4.
Specific embodiment
It elaborates below to the present invention, but practical range of the invention is not limited only to embodiment disclosed below.
A kind of low cost catalyst for denitrating flue gas, is the flying dust supported nano-gold category oxygen being prepared by metal salt, flying dust
Compound catalyst；The mass ratio of metal and flying dust is 1:20-1:10 in the catalyst.
The metal salt is one or more of molysite, zinc salt, mantoquita.
The metal salt is the mixture of molysite, zinc salt, mantoquita, metal iron ion and gold in preparation-obtained catalyst
Belong to zinc ion, the mass ratio of metal copper ion is 18:1:1~9:1:1.
The flying dust is flying ash in electric power plant.
A kind of preparation method of low cost catalyst for denitrating flue gas, includes the following steps:
1) by flying dust, drying to constant weight；
2) solid metal salt is dissolved into deionized water, obtains metal salt solution, by flying dust and metal salt solution in height
It presses in kettle and is uniformly mixed, impregnate 20-40min at pressure 3-6MPa, 40-60 DEG C of temperature, mixture is cooled to room temperature, instill
Ammonium hydroxide continues mechanical stirring 0.5-1h until pH value of solution is 9-10, and mixture is taken out and is filtered, drying to constant weight again；
3) drying object for obtaining step 2) is put into fixed bed reactors, under nitrogen atmosphere protection, in crucible furnace
It is warming up to 600-700 DEG C and is passed through vapor and calcined and gasified 15-30min, be down to room temperature, obtain catalyst.
In the metal salt solution, the ratio of the quality and volume of metal ion and deionized water is 1:20-1:10.
A kind of application method of low cost catalyst for denitrating flue gas, includes the following steps:
1) NO will be containedXFlue gas be passed through in catalyst, carry out catalysis reduction removing flue gas in NO；
2) flue gas is 3~6s by the residence time of catalyst in fixed bed denitrating tower；
3) the denitration temperature of catalyst is 200~400 DEG C.
Embodiment 1
Pure Fe (the NO of analysis is weighed respectively3)2·9H2O is added in 100ml deionized water, is uniformly dissolved, and obtains Fe content point
Not Wei 10g/100ml water iron nitrate solution.The flying dust that granularity is 120-200 mesh is put into vacuum drying oven, in 105 DEG C of vacuum
Drying to constant weight.The dry flying dust of 100g is weighed, is put into autoclave simultaneously with above-mentioned iron nitrate solution, in pressure
5MPa impregnates 0.5h under temperature 50 C, sample is cooled to room temperature, a certain amount of ammonium hydroxide is added, until solution ph continues to 9-10
Ultrasonic immersing 1h, later cooled to room temperature are taken out, and filter, and in vacuum drying oven 105 DEG C drying to constant weight again.It will
The catalyst precursor sample 10g of drying is put into fixed-bed reactor, and under nitrogen atmosphere protection, fixed bed reaction is filled
It sets and is heated to 700 DEG C, then pass to the vapor of 0.015ml/min, isothermal pyrolysis gasifies after 30min in N2It is cooled under atmosphere
Room temperature obtains the metal oxide-loaded denitrating catalyst A of flying dust.
Embodiment 2
Weigh analytically pure Fe (NO3)2·9H2O and Cu (NO3)2·5H2O is added in 100ml deionized water, and dissolution is equal
It is even, obtain the mixed nitrate solution that Fe and Cu content is respectively 9.5g/100ml and 0.5g/100ml water.120- will be sized to
The flying dust of 200 mesh is put into vacuum drying oven, in 105 DEG C of vacuum dryings to constant weight.The dry flying dust of 100g is weighed, with above-mentioned nitric acid
Mixed salt solution is put into autoclave simultaneously, impregnates 0.5h at pressure 5MPa, temperature 50 C, and sample is cooled to room
A certain amount of ammonium hydroxide is added in temperature, until solution ph continues ultrasonic immersing 1h, later cooled to room temperature, take out, take out to 9-10
Filter, and in vacuum drying oven 105 DEG C drying to constant weight again.It is anti-that the catalyst precursor sample 10g of drying is put into fixed bed
It answers in device, under nitrogen atmosphere protection, fixed-bed reactor is heated to 700 DEG C, then passes to the water of 0.015ml/min
Steam, isothermal pyrolysis gasify 30min after in N2It is cooled to room temperature under atmosphere, obtains the metal oxide-loaded denitrating catalyst of flying dust
B。
Embodiment 3
Weigh analytically pure Fe (NO3)2·9H2O、Zn(NO3)2·6H2O and Cu (NO3)2·5H2O, be added 100ml go from
It in sub- water, is uniformly dissolved, obtains the nitrate mixed solution that Fe, Zn and Cu content are respectively 8g, 1.5g and 0.5g/100ml water.
The flying dust for being sized to 120-200 mesh is put into vacuum drying oven, in 105 DEG C of vacuum dryings to constant weight.Weigh flying for 100g drying
Ash is put into autoclave simultaneously with above-mentioned nitrate mixed solution, and 0.5h is impregnated at pressure 5MPa, temperature 50 C, will
Sample is cooled to room temperature, and a certain amount of ammonium hydroxide is added, until solution ph continues ultrasonic immersing 1h, naturally cool to later to 9-10
Room temperature, take out, filter, and in vacuum drying oven 105 DEG C drying to constant weight again.By the catalyst precursor sample 10g of drying
It is put into fixed-bed reactor, under nitrogen atmosphere protection, fixed-bed reactor is heated to 700 DEG C, is then passed to
The vapor of 0.015ml/min, isothermal pyrolysis gasify 30min after in N2It is cooled to room temperature under atmosphere, obtains flying dust carried metal
Oxide denitrating catalyst C.
Embodiment 4
The pretreatment of flying ash in electric power plant is the same as embodiment 1.
Dry flying ash in electric power plant sample 100g is put into the fixed-bed reactor of embodiment 1, under nitrogen atmosphere protection,
Fixed-bed reactor is heated to 700 DEG C, then passes to the vapor of 0.015ml/min, isothermal pyrolysis gasify after 30min
N2It is cooled to room temperature under atmosphere, obtains flying dust catalyst D.
The metal oxide-loaded each 10g of denitrating catalyst A, B, C, D of flying dust is measured, is carried out respectively in fixed bed denitrating tower
The metal oxide-loaded denitrating flue gas experiment of flying dust, specific experiment condition are as follows: NO concentration 2500mg/Nm3, air speed 5000h-1, oxygen
Gas content O25%, vapor 5%.As shown in Fig. 2, the catalyst of the preparation of example 3 is 200-400 DEG C of Shi Junneng in reaction temperature
NO in enough effectively removing flue gasesX.It can be found that catalyst C of the present invention has best denitrating flue gas effect by Fig. 3 simultaneously, takes off
Nitre efficiency is up to 95% or more, and nontoxic, without secondary pollution, preparation method is simple, and preparation cost is low.
Claims (7)
1. a kind of low cost catalyst for denitrating flue gas, which is characterized in that be that the flying dust load being prepared by metal salt, flying dust is received
Rice metal oxide catalyst；The mass ratio of metal and flying dust is 1:20-1:10 in the catalyst.
2. a kind of inexpensive catalyst for denitrating flue gas according to claim 1, which is characterized in that the metal salt is iron
One or more of salt, zinc salt, mantoquita.
3. a kind of inexpensive catalyst for denitrating flue gas according to claim 1, which is characterized in that the metal salt is iron
Salt, zinc salt, mantoquita mixture, metal iron ion and metal zinc ion in preparation-obtained catalyst, metal copper ion
Mass ratio is 18:1:1~9:1:1.
4. a kind of inexpensive catalyst for denitrating flue gas according to claim 1, which is characterized in that the flying dust flies for power plant
Ash.
5. a kind of preparation method of inexpensive catalyst for denitrating flue gas as described in claim 1, which is characterized in that including as follows
Step:
1) by flying dust, drying to constant weight；
2) solid metal salt is dissolved into deionized water, obtains metal salt solution, by flying dust and metal salt solution in autoclave
It is interior to be uniformly mixed, 20-40min is impregnated at pressure 3-6MPa, 40-60 DEG C of temperature, mixture is cooled to room temperature, instills ammonia
Water continues mechanical stirring 0.5-1h until pH value of solution is 9-10, and mixture is taken out and is filtered, drying to constant weight again；
3) drying object for obtaining step 2) is put into fixed bed reactors, under nitrogen atmosphere protection, is heated up in crucible furnace
Vapor is passed through to 600-700 DEG C and is calcined and gasified 15-30min, is down to room temperature, is obtained catalyst.
6. a kind of preparation method of inexpensive catalyst for denitrating flue gas according to claim 5, which is characterized in that the gold
Belong in salting liquid, the ratio of the quality and volume of metal ion and deionized water is 1:20-1:10.
7. a kind of application method of inexpensive catalyst for denitrating flue gas as described in claim 1, which is characterized in that including as follows
Step:
1) NO will be containedXFlue gas be passed through in catalyst, carry out catalysis reduction removing flue gas in NO；
2) flue gas is 3~6s by the residence time of catalyst in fixed bed denitrating tower；
3) the denitration temperature of catalyst is 200~400 DEG C.
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| CN112094073A (en) * | 2020-05-11 | 2020-12-18 | 清华大学 | Ammonia curing agent for fly ash and ammonia fixing method thereof |
| CN112604694A (en) * | 2020-12-16 | 2021-04-06 | 辽宁科技大学 | Novel low-temperature water-resistant sulfur-resistant NH taking low-cost fly ash as carrier3-SCR catalyst |
| CN114032391A (en) * | 2021-10-29 | 2022-02-11 | 天津城建大学 | High-value utilization method of waste incineration fly ash prepared based on catalyst |
| CN114160122A (en) * | 2021-11-29 | 2022-03-11 | 长沙理工大学 | Wide-temperature-zone SCR catalyst with fly ash as matrix and capable of preventing ammonium bisulfate poisoning and preparation method and application thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN109433236A (en) * | 2018-11-27 | 2019-03-08 | 辽宁科技大学 | Porous carbon material loads zeroth order Fe-Fe3The denitrating catalyst of C and its preparation, application method |
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| CN112604694A (en) * | 2020-12-16 | 2021-04-06 | 辽宁科技大学 | Novel low-temperature water-resistant sulfur-resistant NH taking low-cost fly ash as carrier3-SCR catalyst |
| CN114032391A (en) * | 2021-10-29 | 2022-02-11 | 天津城建大学 | High-value utilization method of waste incineration fly ash prepared based on catalyst |
| CN114160122A (en) * | 2021-11-29 | 2022-03-11 | 长沙理工大学 | Wide-temperature-zone SCR catalyst with fly ash as matrix and capable of preventing ammonium bisulfate poisoning and preparation method and application thereof |
| CN114160122B (en) * | 2021-11-29 | 2023-12-01 | 长沙理工大学 | Ammonium bisulfate poisoning prevention wide-temperature-zone SCR catalyst taking fly ash as matrix and preparation method and application thereof |
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