CN106861676A - A kind of anti-sulfur dioxide is suitable to denitrating catalyst that low temperature is used and preparation method thereof - Google Patents

A kind of anti-sulfur dioxide is suitable to denitrating catalyst that low temperature is used and preparation method thereof Download PDF

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CN106861676A
CN106861676A CN201710020835.7A CN201710020835A CN106861676A CN 106861676 A CN106861676 A CN 106861676A CN 201710020835 A CN201710020835 A CN 201710020835A CN 106861676 A CN106861676 A CN 106861676A
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catalyst
content
slurry
tio
powder
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翟燕萍
许壮
姚小强
刘清侠
李晨旭
沈美庆
王军
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CHINA HUADIAN SCIENCE AND TECHNOLOGY INSTITUTE Co Ltd
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Abstract

It is suitable to the denitrating catalyst that low temperature is used, including carrier, active component and catalyst promoter the invention discloses a kind of anti-sulfur dioxide, wherein, the carrier is 70 90% TiO2, the active component is 0.01 10% V2O5, the catalyst promoter include 3 20% WO3The oxide selected from least one of Sc, Cr, Fe, Co, Ni, Ce, Zr, Sb, Pb, Ta, La element with 0.01 10%, percentage is with catalyst weight.Catalyst of the invention can be used under the flue gas condition of coal-burning power plant's underrun, with preferable anti-sulfur dioxide performance, efficient denitration can be realized, and catalyst of the invention preparation method process is simple, substantially waste water,waste gas and industrial residue, environmental protection are not produced.

Description

A kind of anti-sulfur dioxide is suitable to denitrating catalyst that low temperature is used and preparation method thereof
Technical field
The present invention relates to a kind of catalyst, more particularly to a kind of anti-sulfur dioxide is suitable to the denitration catalyst that low temperature is used Agent, the invention further relates to the preparation method of the catalyst.
Background technology
Contain sulfur dioxide (SO in the flue gas of coal-burning power plant2), nitrogen oxides (NOx, mainly NO), dust (PM) and weight Metal (such as mercury) etc. to human health be harmful to material, it is necessary to carry out absorption cleaning after reach national requirements limit value could be to big Gas is discharged.At present, coal-burning power plant is translated into harmless generally using ammonia reducing process removing NOx in Benitration reactor Nitrogen (N2)：
4NH3+4NO+O2→4N2+6H2O
2NH3+NO+NO2→2N2+3H2O
8NH3+6NO2→7N2+12H2O
The above-mentioned intrinsic activation energy of denitration reaction is higher, it is necessary to could occur in the presence of a catalyst.Additionally, coal-fired SO containing higher concentration in power-plant flue gas2, it can occur side reaction generation sulfate and be covered in catalyst surface, lead with ammonia Cause denitrating catalyst poisoning.
2SO2+O2→2SO3
NH3+SO3+H2O→NH4HSO4
2NH3+SO3+H2O→(NH4)2SO4
In order to realize the efficient removal of NOx, the denitrating flue gas reaction temperature general control of coal-burning power plant more than 300 DEG C, As SO in flue gas2When content is higher, in addition it is also necessary to further rise high reaction temperature and avoid catalyst poisoning.
Over nearly 1 year, China Power demand speedup slows down, Thermal generation unit depth peak regulation and underrun pattern The new normality that domestic electrical development occurs under the new situation is turned into.The continuous underrun time increases, and causes Benitration reactor Entrance flue gas temperature is too low, catalytic eliminating NOx efficiency declines, NOx content is exceeded in exiting flue gas, denitrating system compulsory withdrawal, The normal operation of Thermal generation unit is had a strong impact on.Therefore, the denitrating catalyst that be can be used under the conditions of exploitation low-temperature flue gas is compeled In the eyebrows and eyelashes；Further, since SO in coal-fired plant flue gas2Content is (generally higher than 1000ppm) higher, and denitrating catalyst makes in low temperature Anti- SO under the conditions of2Performance is equally most important.
The content of the invention
The technical problem to be solved in the present invention is to provide a kind of anti-sulfur dioxide and is suitable to the denitrating catalyst that low temperature is used, should Catalyst can be used under the flue gas condition of coal-burning power plant's underrun, with preferable anti-sulfur dioxide performance, can Realize efficient denitration.
In order to solve the above technical problems, being suitable to the denitration catalyst that low temperature is used the invention provides a kind of anti-sulfur dioxide Agent, including carrier, active component and catalyst promoter, wherein, the carrier is the TiO of 70-90%2, the active component is The V of 0.01-10%2O5, WO of the catalyst promoter including 3-20%3With 0.01-10% selected from Sc, Cr, Fe, Co, Ni, The oxide of at least one of Ce, Zr, Sb, Pb, Ta, La element, percentage is with catalyst weight.
Above-mentioned denitrating catalyst, wherein, the catalyst promoter includes the WO of 3-20%3With 0.01-10% selected from Ce, The oxide of at least one of Zr, Sb, Pb, Ta, La element, catalyst promoter is preferably the WO of 3-20%3With 0.01-10%'s Selected from the oxide of at least one of Ce, Sb, Pb, Ta element, the more preferably WO of 3-10%3With 3-5% selected from Ce, The WO of the oxide of at least one of Sb, Pb, Ta element, most preferably 3-10%3With the Ce of 3-5%2O3、Sb2O3、Ta2O5Or Pb3O4.The carrier is preferably the TiO of 85-90%2, the active component is preferably the V of 0.1-2%2O5。
It is suitable to the preparation method of the denitrating catalyst that low temperature is used present invention also offers a kind of anti-sulfur dioxide, including such as Lower step：
A) by the WO containing design proportioning3Presoma ammonium metatungstate, V2O5Or V2O5Presoma ammonium metavanadate, selected from Sc, Cr, The presoma of the oxide of at least one of Fe, Co, Ni, Ce, Zr, Sb, Pb, Ta, La element be dissolved in water or ethanol or water and In the mixed liquor of ethanol, the solution of clarification is obtained；
B) TiO of proportioning will be designed2Powder is added into the solution of the step a, forms uniform slurry；
C) slurry for obtaining step b is stirred under conditions of temperature is not less than 50 DEG C, evaporated, when slurry is changed into paste When, stop stirring；
D) by the paste that step c is obtained be put into vacuum more than 0.5 drying box in, temperature control at 50-100 DEG C, Dry and obtain drying solid；
E) solid that obtains step d is ground to be calcined 3-5 hour into powder at 300-500 DEG C, prepared catalyst.
It is suitable to the preparation method of the denitrating catalyst that low temperature is used present invention also offers a kind of anti-sulfur dioxide, including such as Lower step：
A) by the WO containing design proportioning3Presoma ammonium metatungstate, V2O5It is dissolved in the mixing of water or ethanol or water and ethanol In liquid, the solution of clarification is obtained；
B) TiO of proportioning will be designed2Powder is added into the solution of the step a, forms uniform slurry；
C) slurry for obtaining step b is stirred under conditions of temperature is not less than 50 DEG C, evaporated, when slurry is changed into paste When, stop stirring；
D) by the paste that step c is obtained be put into vacuum more than 0.5 drying box in, temperature control at 50-100 DEG C, Dry and obtain drying solid；
E) solid for obtaining step d is ground into powder, and the antimony oxide for adding design to match carries out mixing and grinds Mill, is calcined 3-5 hours at 300-500 DEG C, and catalyst is obtained.
Anti- sulfur dioxide of the invention is suitable to the denitrating catalyst that low temperature uses and has the advantages that：
1st, catalyst of the invention can realize efficient denitration under the flue gas condition of coal-burning power plant's underrun, Denitration activity is good under cryogenic conditions, with very strong anti-SO2Poisoning capability；
2nd, catalyst of the invention, when catalyst promoter uses WO3With the oxidation of at least one of Ce, Sb, Pb, Ta element During thing, when flue-gas temperature is not less than 270 DEG C, SO in flue gas2Concentration is more than 1000ppm, spray ammonia ratio (NH3/ NOx mol ratios) no Under the conditions of 0.8, denitration efficiency can reach more than 90%；
3rd, the preparation method process is simple of catalyst of the present invention, does not produce waste water,waste gas and industrial residue, environmental protection substantially.
Specific embodiment
The present invention is described in detail with reference to embodiment.
Embodiment 1
30 weight portion WO will be contained3Presoma ammonium metatungstate, contain 50 weight portion V2O5Presoma ammonium metavanadate, contain There are 20 weight portion scandium oxide (Sc2O3) presoma scandium nitrate and lactic acid solution that 500 weight portion mass concentrations are 50% it is molten In Xie Shui, stirring obtains the solution of clarification, and the TiO of 900 weight portions is added in the solution2Powder, forms uniform slurry, Slurry is stirred 5 hours under conditions of 50 DEG C so that solvent slow evaporation, paste is changed into slurry.The paste that will be obtained Thing is put into the drying box that vacuum is 0.7 and dries 24 hours, and drying box temperature control is 80 DEG C, dries and obtains drying solid, Solid is ground into powder, it is calcined 5 hours at 500 DEG C, catalyst is obtained.In obtained catalyst, TiO2Content is 90%, V2O5Content is 5%, WO3Content is 3%, Sc2O3Content is 2%, and percentage composition is with catalyst weight.
Catalyst obtained in the present embodiment is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 78%.
Embodiment 2
100 weight portion WO will be contained3Presoma ammonium metatungstate, contain 10 weight portion V2O5Presoma ammonium metavanadate, contain There are 40 weight portion chromated oxide (Cr2O3) presoma chromic nitrate and 25 weight portion dissolving oxalic acids in water, 50 DEG C stirring 0.5 Hour, add the TiO of 850 weight portions in the solution afterwards2Powder, stirring forms uniform slurry, the bar by slurry at 70 DEG C Continue to stir 2 hours under part so that solvent slow evaporation, paste is changed into slurry.The paste that will be obtained is put into vacuum For in 0.7 drying box dry 3 hours, drying box temperature control be 90 DEG C, dry obtain drying solid, by solid it is ground into Powder, is calcined 3 hours in 500 DEG C of air, and catalyst is obtained.In obtained catalyst, TiO2Content is 85%, V2O5Contain It is 1%, WO to measure3Content is 10%, Cr2O3Content is 4%, and percentage composition is with catalyst weight.
Catalyst obtained in the present embodiment is in 270 DEG C, SO2Content 1000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 76%.
Embodiment 3
150 weight portion WO will be contained3Presoma ammonium metatungstate, contain 50 weight portion V2O5Presoma ammonium metavanadate, contain There are 100 weight portion ferriferous oxide (Fe2O3) presoma ferric nitrate and lactic acid solution that 500 weight portion mass concentrations are 50% It is dissolved in water, stirs 0.5 hour, adds the TiO of 700 weight portions in the solution afterwards2Powder, continues to stir formation uniformly Slurry, slurry is continued stirring 5 hours under conditions of 50 DEG C so that solvent slow evaporation, and paste is changed into slurry.Will To paste be put into the drying box that vacuum is 0.7 dry 24 hours, drying box temperature control be 50 DEG C, drying dried Dry solid, solid is ground into powder, it is calcined 5 hours in 500 DEG C of air, catalyst is obtained.In obtained catalyst, TiO2Content is 70%, V2O5Content is 5%, WO3Content is 15%, Fe2O3Content is 10%, and percentage composition is with catalyst weight Meter.
Catalyst obtained in the present embodiment is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 70%.
Embodiment 4
69.9 weight portion WO will be contained3Presoma ammonium metatungstate, contain 0.1 weight portion V2O5Presoma ammonium metavanadate, Contain 30 weight portion cobalt/cobalt oxide (Co2O3) presoma cobalt nitrate and 0.25 weight portion dissolving oxalic acid in water, stirred at 50 DEG C Mix 0.5 hour, add the TiO of 900 weight portions in the solution afterwards2Powder, continues stirring and forms uniform slurry, and slurry is existed Continue to stir 2 hours under conditions of 70 DEG C so that solvent slow evaporation, paste is changed into slurry.The paste that will be obtained is put Enter in the drying box that vacuum is 0.7 and dry 2 hours, drying box temperature control is 100 DEG C, dry and obtain drying solid, will be solid Body is ground into powder, is calcined 5 hours in 300 DEG C of air, and catalyst is obtained.In obtained catalyst, TiO2Content is 90%, V2O5Content is 0.01%, WO3Content is 6.99%, Co2O3Content is 3%, and percentage composition is with catalyst weight.
Catalyst obtained in the present embodiment is in 270 DEG C, SO2Content 1000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 70%.
Embodiment 5
200 weight portion WO will be contained3Presoma ammonium metatungstate, contain 49.9 weight portion V2O5Presoma ammonium metavanadate, Contain 0.1 weight portion nickel oxide (Ni2O3) presoma nickel nitrate and 125 weight portion dissolving oxalic acids in water, stirred at 50 DEG C Mix 0.5 hour, add the TiO of 750 weight portions in the solution afterwards2Powder, continues stirring and forms uniform slurry, and slurry is existed Continue to stir 2 hours under conditions of 70 DEG C so that solvent slow evaporation, paste is changed into slurry.The paste that will be obtained is put Enter in the drying box that vacuum is 0.7 and dry 3 hours, drying box temperature control is 90 DEG C, dry and obtain drying solid, by solid It is ground to be calcined 4.5 hours in 400 DEG C of air into powder, catalyst is obtained.In obtained catalyst, TiO2Content is 75%, V2O5Content is 4.99%, WO3Content is 20%, Ni2O3Content is 0.01%, and percentage composition is with catalyst weight.
Catalyst obtained in the present embodiment is in 270 DEG C, SO2Content 1000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 71%.
Embodiment 6
100 weight portion WO will be contained3Presoma ammonium metatungstate, contain 1 weight portion V2O5Presoma ammonium metavanadate, contain There are 49 weight portion Zirconium oxide (ZrO2) presoma zirconium nitrate and 2.5 weight portion dissolving oxalic acids in water, at 50 DEG C stir 0.5 hour, add the TiO of 850 weight portions in the solution afterwards2Powder, continues stirring and forms uniform slurry, by slurry 70 Continue to stir 2 hours under conditions of DEG C so that solvent slow evaporation, paste is changed into slurry.The paste that will be obtained is put into Vacuum be 0.7 drying box in dry 3 hours, drying box temperature control be 90 DEG C, dry obtain drying solid, solid is passed through Grind into powder, is calcined 3 hours in 500 DEG C of air, and catalyst is obtained.In obtained catalyst, TiO2Content is 85%, V2O5Content is 0.1%, WO3Content is 10%, ZrO2Content is 4.9%, and percentage composition is with catalyst weight.
Catalyst obtained in the present embodiment is in 270 DEG C, SO2Content 1000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 86%.
Embodiment 7
50 weight portion WO will be contained3Presoma ammonium metatungstate, contain 7 weight portion V2O5Presoma ammonium metavanadate, contain 43 weight portion lead oxides (Pb3O4) presoma plumbi nitras and the dissolving of lactic acid solution that 70 weight portion mass concentrations are 50% In water, stir 0.5 hour, add the TiO of 900 weight portions in the solution afterwards2Powder, continues to stir to be formed and uniformly starches Material, slurry is continued stirring 5 hours under conditions of 50 DEG C so that solvent slow evaporation, and paste is changed into slurry.To obtain Paste be put into the drying box that vacuum is 0.7 dry 24 hours, drying box temperature control be 60 DEG C, drying dried Solid, solid is ground into powder, it is calcined 5 hours in 500 DEG C of air, catalyst is obtained.In obtained catalyst, TiO2Content is 90%, V2O5Content is 0.7%, WO3Content is 5%, Pb3O4Content is 4.3%, and percentage composition is with catalyst weight Gauge.
Catalyst obtained in the present embodiment is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 93%.
Embodiment 8
100 weight portion WO will be contained3Presoma ammonium metatungstate, contain 10 weight portion V2O5Presoma ammonium metavanadate, contain There are 30 weight portion lead oxides (Pb3O4) presoma plumbi nitras and lactic acid solution that 100 weight portion mass concentrations are 50% it is molten In Xie Shui, stir 0.5 hour, add the TiO of 860 weight portions in the solution afterwards2Powder, continues to stir to be formed and uniformly starches Material, slurry is continued stirring 5 hours under conditions of 50 DEG C so that solvent slow evaporation, and paste is changed into slurry.To obtain Paste be put into the drying box that vacuum is 0.7 dry 24 hours, drying box temperature control be 60 DEG C, drying dried Solid, solid is ground into powder, it is calcined 5 hours in 500 DEG C of air, catalyst is obtained.In obtained catalyst, TiO2Content is 86%, V2O5Content is 1%, WO3Content is 10%, Pb3O4Content is 3%, and percentage composition is with catalyst weight Meter.
Catalyst obtained in the present embodiment is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 93%.
Embodiment 9
30 weight portion WO will be contained3Presoma ammonium metatungstate, contain 20 weight portion V2O5Presoma ammonium metavanadate, contain There are 50 weight portion lead oxides (Pb3O4) presoma plumbi nitras and lactic acid solution that 200 weight portion mass concentrations are 50% it is molten In Xie Shui, stir 0.5 hour, add the TiO of 900 weight portions in the solution afterwards2Powder, continues to stir to be formed and uniformly starches Material, slurry is continued stirring 5 hours under conditions of 50 DEG C so that solvent slow evaporation, and paste is changed into slurry.To obtain Paste be put into the drying box that vacuum is 0.7 dry 24 hours, drying box temperature control be 60 DEG C, drying dried Solid, solid is ground into powder, it is calcined 5 hours in 500 DEG C of air, catalyst is obtained.In obtained catalyst, TiO2Content is 90%, V2O5Content is 2%, WO3Content is 3%, Pb3O4Content is 5%, and percentage composition is with catalyst weight Meter.
Catalyst obtained in the present embodiment is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 92%.
Embodiment 10
50 weight portion WO will be contained3Presoma ammonium metatungstate, 10 weight portion V2O5And 25 weight portion dissolving oxalic acid in water In, stirred 0.5 hour at 50 DEG C, add the TiO of 900 weight portions in the solution afterwards2Powder, continues to stir to be formed and uniformly starches Material, slurry is continued stirring 2 hours under conditions of 70 DEG C so that solvent slow evaporation, and paste is changed into slurry.To obtain Paste be put into the drying box that vacuum is 0.7 dry 3 hours, drying box temperature control be 90 DEG C, drying dried Solid, solid is ground into powder, add 40 weight portion antimony oxide (Sb2O3) mixed grinding into powder is carried out, at 500 DEG C Air in be calcined 3 hours, be obtained catalyst.In obtained catalyst, TiO2Content is 90%, V2O5Content is 1%, WO3Contain It is 5%, Sb to measure2O3Content is 4%, and percentage composition is with catalyst weight.
Catalyst obtained in the present embodiment is in 270 DEG C, SO2Content 1000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 91%.
Embodiment 11
45 weight portion WO will be contained3Presoma ammonium metatungstate, contain 8 weight portion V2O5Presoma ammonium metavanadate, contain 47 weight portion cerium oxide (Ce2O3) presoma cerous nitrate and the dissolving of lactic acid solution that 80 weight portion mass concentrations are 50% In water, stir 0.5 hour, add the TiO of 900 weight portions in the solution afterwards2Powder, continues to stir to be formed and uniformly starches Material, slurry is continued stirring 5 hours under conditions of 50 DEG C so that solvent slow evaporation, and paste is changed into slurry.To obtain Paste be put into the drying box that vacuum is 0.7 dry 24 hours, drying box temperature control be 65 DEG C, drying dried Solid, solid is ground into powder, it is calcined 5 hours in 500 DEG C of air, catalyst is obtained.In obtained catalyst, TiO2Content is 90%, V2O5Content is 0.8%, WO3Content is 4.5%, Ce2O3Content is 4.7%, and percentage composition is with catalyst Weight meter.
The catalyst is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2Content 12%, water Under the flue gas condition of vapor content 4%, denitration conversion ratio reaches 94%.
Embodiment 12
50 weight portion WO will be contained3Presoma ammonium metatungstate, contain 6 weight portion V2O5Presoma ammonium metavanadate, contain 44 weight portion tantalum pentoxide (Ta2O5) presoma nitric acid tantalum and the dissolving of lactic acid solution that 60 weight portion mass concentrations are 50% In water, stir 0.5 hour, add the TiO of 900 weight portions in the solution afterwards2Powder, continues to stir to be formed and uniformly starches Material, slurry is continued stirring 5 hours under conditions of 50 DEG C so that solvent slow evaporation, and paste is changed into slurry.To obtain Paste be put into the drying box that vacuum is 0.7 dry 24 hours, drying box temperature control be 65 DEG C, drying dried Solid, solid is ground into powder, it is calcined 5 hours in 500 DEG C of air, catalyst is obtained.In obtained catalyst, TiO2Content is 90%, V2O5Content is 0.6%, WO3Content is 5%, Ta2O5Content is 4.4%, and percentage composition is with catalyst weight Gauge.
Catalyst obtained in the present embodiment is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 91%.
Embodiment 13
30 weight portion WO will be contained3Presoma ammonium metatungstate, contain 20 weight portion V2O5Presoma ammonium metavanadate, contain There are 50 weight portion tantalum pentoxide (Ta2O5) presoma nitric acid tantalum and lactic acid solution that 200 weight portion mass concentrations are 50% it is molten In Xie Shui, stir 0.5 hour, add the TiO of 900 weight portions in the solution afterwards2Powder, continues to stir to be formed and uniformly starches Material, slurry is continued stirring 5 hours under conditions of 50 DEG C so that solvent slow evaporation, and paste is changed into slurry.To obtain Paste be put into the drying box that vacuum is 0.7 dry 24 hours, drying box temperature control be 65 DEG C, drying dried Solid, solid is ground into powder, it is calcined 5 hours in 500 DEG C of air, catalyst is obtained.In obtained catalyst, TiO2Content is 90%, V2O5Content is 2%, WO3Content is 3%, Ta2O5Content is 5%, and percentage composition is with catalyst weight Meter.
Catalyst obtained in the present embodiment is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 91%.
Embodiment 14
99 weight portion WO will be contained3Presoma ammonium metatungstate, contain 1 weight portion V2O5Presoma ammonium metavanadate, contain 30 weight portion tantalum pentoxide (Ta2O5) presoma nitric acid tantalum and the dissolving of lactic acid solution that 10 weight portion mass concentrations are 50% In water, stir 0.5 hour, add the TiO of 870 weight portions in the solution afterwards2Powder, continues to stir to be formed and uniformly starches Material, slurry is continued stirring 5 hours under conditions of 50 DEG C so that solvent slow evaporation, and paste is changed into slurry.To obtain Paste be put into the drying box that vacuum is 0.7 dry 24 hours, drying box temperature control be 65 DEG C, drying dried Solid, solid is ground into powder, it is calcined 5 hours in 500 DEG C of air, catalyst is obtained.In obtained catalyst, TiO2Content is 87%, V2O5Content is 0.1%, WO3Content is 9.9%, Ta2O5Content is 3%, and percentage composition is with catalyst weight Gauge.
Catalyst obtained in the present embodiment is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 91%.
Embodiment 15
35 weight portion WO will be contained3Presoma ammonium metatungstate, contain 7 weight portion V2O5Presoma ammonium metavanadate, contain 58 weight portion lanthanum-oxides (La2O3) presoma lanthanum nitrate and the dissolving of lactic acid solution that 70 weight portion mass concentrations are 50% In water, stirred 0.5 hour at 50 DEG C, add the TiO of 900 weight portions in the solution afterwards2Powder, continues to stir formation uniformly Slurry, slurry is continued under conditions of 70 DEG C stirring 2 hours so that solvent slow evaporation, be changed into paste to slurry.Will The paste for obtaining is put into the drying box that vacuum is 0.7 and dries 3 hours, and drying box temperature control is 90 DEG C, dries and obtains Drying solid, solid is ground into powder, it is calcined 5 hours in 500 DEG C of air, catalyst is obtained.Obtained catalyst In, TiO2Content is 90%, V2O5Content is 0.7%, WO3Content is 3.5%, La2O3Content is 5.8%, and percentage composition is urging Agent weight meter.
Catalyst obtained in the present embodiment is in 270 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio reaches 90%.
Embodiment 16
42 weight portion WO will be contained3Presoma ammonium metatungstate, contain 8 weight portion V2O5Presoma ammonium metavanadate, contain 30 weight portion lanthanum-oxides (La2O3) presoma lanthanum nitrate, contain 20 weight portion cerium oxide (Ce2O3) presoma nitric acid Cerium and the lactic acid solution that 80 weight portion mass concentrations are 50% are dissolved in water, and are stirred 0.5 hour at 50 DEG C, afterwards in solution The TiO of 900 weight portions of middle addition2Powder, continues stirring and forms uniform slurry, and slurry is continued stirring under conditions of 70 DEG C 2 hours so that solvent slow evaporation, paste is changed into slurry.The paste that will be obtained is put into the drying box that vacuum is 0.7 Interior drying 3 hours, drying box temperature control is 90 DEG C, dries and obtains drying solid, and solid is ground into powder, at 500 DEG C Air in be calcined 3 hours, be obtained catalyst.In obtained catalyst, TiO2Content is 90%, V2O5Content is 0.8%, WO3 Content is 4.2%, La2O3Content is 3%, Ce2O3Content is 2%, and percentage composition is with catalyst weight.
The catalyst is in 270 DEG C, SO2Content 1000ppm, NOx content 500ppm, O2Content 6%, CO2Content 12%, water Under the flue gas condition of vapor content 4%, denitration conversion ratio reaches 91%.
The catalyst promoter of comparative example 1 is WO3
93 weight portion WO will be contained3Presoma ammonium metatungstate, contain 7 weight portion V2O5Presoma ammonium metavanadate and 70 weight portion mass concentrations are that 50% lactic acid solution is dissolved in water, and are stirred 0.5 hour, add 900 weights in the solution afterwards Measure the TiO of part2Powder, continues stirring and forms uniform slurry, and slurry is continued stirring 5 hours under conditions of 50 DEG C so that Solvent slow evaporation, paste is changed into slurry.It is small that the paste that will be obtained is put into the drying box that vacuum is 0.7 dry 24 When, drying box temperature control is 60 DEG C, dries and obtains drying solid, and solid is ground into powder, is roasted in 500 DEG C of air Burn 5 hours, catalyst is obtained.In obtained catalyst, TiO2Content is 90%, V2O5Content is 0.7%, WO3Content is 9.3%, percentage composition is with catalyst weight.
Comparative example 1 is with catalyst obtained in embodiment 7 in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Contain Amount 6%, CO2Denitration efficiency under content 12%, the flue gas condition of water vapour content 4% is shown in Table 1.
Table 1
Embodiment 7 and the difference of catalyst obtained in comparative example 1 be different catalyst promoter, and embodiment 7 is urged Agent auxiliary agent is WO3And lead oxides, the catalyst promoter of comparative example 1 is WO3.Be can be seen that from the denitration conversion ratio in table 1 When reacting 30 minutes, denitration conversion ratio is 40% to comparative example 1, when reacting 1 hour, catalyst sulfur poisoning, inactivation.Can See, only with WO3During as catalyst promoter, there is SO in catalyst quickly2It is poisoned and inactivates, it is impossible to realizes denitration, and it is real Apply in example 7, lead oxides, WO are added in catalyst promoter3And Pb3O4Collective effect, makes denitrating catalyst of the invention exist There is good anti-SO under low temperature2Poisoning capability, when reacting 30 minutes, denitration conversion ratio can reach 85%, reaction 4 After hour, denitration conversion ratio has reached 93%.
The catalyst promoter of comparative example 2 is lead oxides (Pb3O4)
7 weight portion V will be contained2O5Presoma ammonium metavanadate, contain 93 weight portion lead oxides (Pb3O4) presoma Plumbi nitras and the lactic acid solution that 70 weight portion mass concentrations are 50% are dissolved in water, stirring 0.5 hour, afterwards in the solution Add the TiO of 900 weight portions2Powder, continues stirring and forms uniform slurry, and slurry is continued stirring 5 under conditions of 50 DEG C Hour so that solvent slow evaporation, it is changed into paste to slurry.The paste that will be obtained is put into the drying box that vacuum is 0.7 Interior drying 24 hours, drying box temperature control is 60 DEG C, dries and obtains drying solid, and solid is ground into powder, at 500 DEG C Air in be calcined 5 hours, be obtained catalyst.In obtained catalyst, TiO2Content is 90%, V2O5Content is 0.7%, Pb3O4Content is 9.3%, and percentage composition is with catalyst weight.
Catalyst obtained in comparative example 2 is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Denitration conversion ratio under content 12%, the flue gas condition of water vapour content 4% is 40%.Embodiment 7 is obtained with comparative example 2 to urge The difference of agent is different catalyst promoter, and the catalyst promoter of embodiment 7 is WO3And lead oxides, comparative example 2 makes In the catalyst for obtaining, catalyst promoter is only Pb3O4, do not contain WO3.Under identical flue gas condition, the denitration of embodiment 7 Conversion ratio can reach 93%, and comparative example 2 is only 40%, and the denitration conversion ratio of embodiment 7 is apparently higher than in comparative example 2 Denitration conversion ratio, it is seen that use WO3There is good anti-SO at low ambient temperatures as catalyst promoter with lead oxides combination2 Poisoning capability, greatly improves the denitration conversion ratio of catalyst.
The catalyst promoter of comparative example 3 is tantalum pentoxide (Ta2O5)
6 weight portion V will be contained2O5Presoma ammonium metavanadate, contain 94 weight portion tantalum pentoxide (Ta2O5) presoma Nitric acid tantalum and the lactic acid solution that 60 weight portion mass concentrations are 50% are dissolved in water, stirring 0.5 hour, afterwards in the solution Add the TiO of 900 weight portions2Powder, continues stirring and forms uniform slurry, and slurry is continued stirring 5 under conditions of 50 DEG C Hour so that solvent slow evaporation, it is changed into paste to slurry.The paste that will be obtained is put into the drying box that vacuum is 0.7 Interior drying 24 hours, drying box temperature control is 65 DEG C, dries and obtains drying solid, and solid is ground into powder, at 500 DEG C Air in be calcined 5 hours, be obtained catalyst.In obtained catalyst, TiO2Content is 90%, V2O5Content 0.6%, Ta2O5 Content is 9.4%, and percentage composition is with catalyst weight.
Catalyst obtained in comparative example 3 is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio is 50%.
Embodiment 12 is different catalyst promoter from the difference of catalyst obtained in comparative example 3, embodiment 12 Catalyst promoter is WO3And tantalum pentoxide, in catalyst obtained in comparative example 3, catalyst promoter is only Ta2O5, do not contain WO3.Under identical flue gas condition, the denitration conversion ratio of embodiment 12 can reach 91%, and comparative example 3 is only 50%, The denitration conversion ratio of embodiment 12 is apparently higher than the denitration conversion ratio in comparative example 3, it is seen that use WO3Combined with tantalum pentoxide and made There is good anti-SO at low ambient temperatures for catalyst promoter2Poisoning capability, greatly improves the denitration conversion ratio of catalyst.
The catalyst promoter of comparative example 4 is sb oxide (Sb2O3)
By 10 weight portion V2O5, 25 weight portion dissolving oxalic acids in water, at 50 DEG C stir 0.5 hour, afterwards in the solution plus Enter the TiO of 900 weight portions2Powder, continues stirring and forms uniform slurry, and slurry is continued under conditions of 70 DEG C to stir 2 small When so that solvent slow evaporation, it is changed into paste to slurry.The paste that will be obtained is put into the drying box that vacuum is 0.7 Dry 3 hours, drying box temperature control is 90 DEG C, dry and obtain drying solid, solid is ground into powder, add 90 weight Part antimony oxide (Sb2O3) mixed grinding into powder is carried out, it is calcined 3 hours in 500 DEG C of air, catalyst is obtained.It is obtained In catalyst, TiO2Content is 90%, V2O5Content is 1%, Sb2O3Content is 9%, and percentage composition is with catalyst weight.
Catalyst obtained in comparative example 4 is in 270 DEG C, SO2Content 1000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio is 40%.Embodiment 10 is obtained with comparative example 4 to urge The difference of agent is different catalyst promoter, and the catalyst promoter of embodiment 10 is WO3And sb oxide, comparative example 4 In obtained catalyst, catalyst promoter is only Sb2O3, do not contain WO3.Under identical flue gas condition, embodiment 10 it is de- Nitre conversion ratio can reach 91%, and comparative example 4 is only 40%, and the denitration conversion ratio of embodiment 10 is apparently higher than comparative example 4 In denitration conversion ratio, it is seen that use WO3Have at low ambient temperatures well as catalyst promoter with sb oxide combination Anti- SO2Poisoning capability, greatly improves the denitration conversion ratio of catalyst.
The catalyst promoter of comparative example 5 is cerium oxide (Ce2O3)
8 weight portion V will be contained2O5Presoma ammonium metavanadate, contain 92 weight portion cerium oxide (Ce2O3) presoma Cerous nitrate and the lactic acid solution that 80 weight portion mass concentrations are 50% are dissolved in water, stirring 0.5 hour, afterwards in the solution Add the TiO of 900 weight portions2Powder, continues stirring and forms uniform slurry, and slurry is continued stirring 5 under conditions of 50 DEG C Hour so that solvent slow evaporation, it is changed into paste to slurry.The paste that will be obtained is put into the drying box that vacuum is 0.7 Interior drying 24 hours, drying box temperature control is 65 DEG C, dries and obtains drying solid, and solid is ground into powder, at 500 DEG C Air in be calcined 5 hours, be obtained catalyst.In obtained catalyst, TiO2Content is 90%, V2O5Content 0.8%, Ce2O3 Content is 9.2%, and percentage composition is with catalyst weight.
Catalyst obtained in comparative example 5 is in 280 DEG C, SO2Content 2000ppm, NOx content 500ppm, O2Content 6%, CO2 Under content 12%, the flue gas condition of water vapour content 4%, denitration conversion ratio is 40%.Embodiment 11 is obtained with comparative example 5 to urge The difference of agent is different catalyst promoter, and the catalyst promoter of embodiment 11 is WO3And cerium oxide, comparative example 5 In obtained catalyst, catalyst promoter is only Ce2O3, do not contain WO3.Under identical flue gas condition, embodiment 11 it is de- Nitre conversion ratio can reach 94%, and comparative example 5 is only 40%, and the denitration conversion ratio of embodiment 11 is apparently higher than comparative example 5 In denitration conversion ratio, it is seen that use WO3Have at low ambient temperatures well as catalyst promoter with cerium oxide combination Anti- SO2Poisoning capability, greatly improves the denitration conversion ratio of catalyst.

Claims (10)

1. a kind of anti-sulfur dioxide is suitable to the denitrating catalyst that low temperature is used, including carrier, active component and catalyst promoter, its In, the carrier is the TiO of 70-90%2, the active component is the V of 0.01-5%2O5, the catalyst promoter include 3- 20% WO3With the oxygen selected from least one of Sc, Cr, Fe, Co, Ni, Ce, Zr, Sb, Pb, Ta, La element of 0.01-10% Compound, percentage is with catalyst weight.
2. denitrating catalyst as claimed in claim 1, wherein, the catalyst promoter includes the WO of 3-20%3And 0.01- 10% oxide selected from least one of Ce, Zr, Sb, Pb, Ta, La element.
3. the denitrating catalyst as described in right wants 2, wherein, the catalyst promoter includes the WO of 3-20%3And 0.01-10% The oxide selected from least one of Ce, Sb, Pb, Ta element.
4. denitrating catalyst as claimed in claim 3, wherein, the carrier is the TiO of 85-90%2, the active component is The V of 0.1-2%2O5, WO of the catalyst promoter including 3-10%3With 3-5% selected from least one of Ce, Sb, Pb, Ta The oxide of element.
5. denitrating catalyst as claimed in claim 4, wherein, the catalyst promoter is the WO of 3-10%3With 3-5%'s Ce2O3。
6. denitrating catalyst as claimed in claim 4, wherein, the catalyst promoter is the WO of 3-10%3With 3-5%'s Sb2O3。
7. denitrating catalyst as claimed in claim 4, wherein, the catalyst promoter is the WO of 3-10%3With 3-5%'s Ta2O5。
8. denitrating catalyst as claimed in claim 4, wherein, the catalyst promoter is the WO of 3-10%3With 3-5%'s Pb3O4。
9. a kind of preparation method of the denitrating catalyst described in claim 1, comprises the following steps：
A) by the WO containing design proportioning3Presoma ammonium metatungstate, V2O5Or V2O5Presoma ammonium metavanadate, selected from Sc, Cr, Fe, The presoma of the oxide of at least one of Co, Ni, Ce, Zr, Sb, Pb, Ta, La element is dissolved in water or ethanol or water and ethanol Mixed liquor in, obtain clarification solution；
B) TiO of proportioning will be designed2Powder is added into the solution of the step a, forms uniform slurry；
C) slurry for obtaining step b is stirred under conditions of temperature is not less than 50 DEG C, evaporated, when slurry is changed into paste, Stop stirring；
D) paste that step c is obtained is put into drying box of the vacuum more than 0.5, temperature control is dried at 50-100 DEG C Obtain drying solid；
E) solid that obtains step d is ground to be calcined 3-5 hour into powder at 300-500 DEG C, prepared catalyst.
10. a kind of preparation method of the denitrating catalyst described in claim 6, comprises the following steps：
A) by the WO containing design proportioning3Presoma ammonium metatungstate, V2O5It is dissolved in the mixed liquor of water or ethanol or water and ethanol In, obtain the solution of clarification；
B) TiO of proportioning will be designed2Powder is added into the solution of the step a, forms uniform slurry；
C) slurry for obtaining step b is stirred under conditions of temperature is not less than 50 DEG C, evaporated, when slurry is changed into paste, Stop stirring；
D) paste that step c is obtained is put into drying box of the vacuum more than 0.5, temperature control is dried at 50-100 DEG C Obtain drying solid；
E) solid for obtaining step d is ground into powder, and the antimony oxide for adding design to match carries out mixed grinding, 300-500 DEG C is calcined 3-5 hours, and catalyst is obtained.
CN201710020835.7A 2017-01-11 2017-01-11 A kind of anti-sulfur dioxide is suitable to denitrating catalyst that low temperature is used and preparation method thereof Pending CN106861676A (en)

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Application publication date: 20170620