CN108236960A - A kind of TiO2-SO42-High resistant to sulfur ceria-based denitration catalyst of load and preparation method thereof - Google Patents
A kind of TiO2-SO42-High resistant to sulfur ceria-based denitration catalyst of load and preparation method thereof Download PDFInfo
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- 239000003054 catalyst Substances 0.000 title claims abstract description 105
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 title claims abstract description 43
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 title claims abstract description 39
- 238000002360 preparation method Methods 0.000 title claims abstract description 35
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 title claims abstract description 31
- 229910052717 sulfur Inorganic materials 0.000 title claims abstract description 31
- 239000011593 sulfur Substances 0.000 title claims abstract description 31
- 238000001354 calcination Methods 0.000 claims abstract description 37
- 239000007864 aqueous solution Substances 0.000 claims abstract description 30
- ADCOVFLJGNWWNZ-UHFFFAOYSA-N antimony trioxide Inorganic materials O=[Sb]O[Sb]=O ADCOVFLJGNWWNZ-UHFFFAOYSA-N 0.000 claims abstract description 17
- 238000001125 extrusion Methods 0.000 claims abstract description 17
- 238000000034 method Methods 0.000 claims abstract description 16
- 238000001035 drying Methods 0.000 claims abstract description 15
- 239000012752 auxiliary agent Substances 0.000 claims abstract description 9
- YEAUATLBSVJFOY-UHFFFAOYSA-N tetraantimony hexaoxide Chemical compound O1[Sb](O2)O[Sb]3O[Sb]1O[Sb]2O3 YEAUATLBSVJFOY-UHFFFAOYSA-N 0.000 claims abstract description 8
- 239000000243 solution Substances 0.000 claims description 38
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 33
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 27
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims description 24
- 239000002253 acid Substances 0.000 claims description 22
- 239000011230 binding agent Substances 0.000 claims description 22
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 22
- 239000000314 lubricant Substances 0.000 claims description 21
- 239000000463 material Substances 0.000 claims description 21
- 239000011148 porous material Substances 0.000 claims description 21
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 18
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 16
- 239000003365 glass fiber Substances 0.000 claims description 15
- 210000001161 mammalian embryo Anatomy 0.000 claims description 15
- 239000008367 deionised water Substances 0.000 claims description 14
- 229910021641 deionized water Inorganic materials 0.000 claims description 14
- -1 extrusion aid Substances 0.000 claims description 14
- JVTAAEKCZFNVCJ-UHFFFAOYSA-N lactic acid Chemical compound CC(O)C(O)=O JVTAAEKCZFNVCJ-UHFFFAOYSA-N 0.000 claims description 14
- 238000003756 stirring Methods 0.000 claims description 14
- 229910001868 water Inorganic materials 0.000 claims description 13
- HZAXFHJVJLSVMW-UHFFFAOYSA-N 2-Aminoethan-1-ol Chemical compound NCCO HZAXFHJVJLSVMW-UHFFFAOYSA-N 0.000 claims description 12
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 claims description 10
- 230000032683 aging Effects 0.000 claims description 9
- 238000002156 mixing Methods 0.000 claims description 9
- FPCJKVGGYOAWIZ-UHFFFAOYSA-N butan-1-ol;titanium Chemical compound [Ti].CCCCO.CCCCO.CCCCO.CCCCO FPCJKVGGYOAWIZ-UHFFFAOYSA-N 0.000 claims description 8
- XAYGUHUYDMLJJV-UHFFFAOYSA-Z decaazanium;dioxido(dioxo)tungsten;hydron;trioxotungsten Chemical compound [H+].[H+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].[NH4+].O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.[O-][W]([O-])(=O)=O.[O-][W]([O-])(=O)=O.[O-][W]([O-])(=O)=O.[O-][W]([O-])(=O)=O.[O-][W]([O-])(=O)=O.[O-][W]([O-])(=O)=O XAYGUHUYDMLJJV-UHFFFAOYSA-Z 0.000 claims description 8
- 235000019441 ethanol Nutrition 0.000 claims description 8
- 239000004408 titanium dioxide Substances 0.000 claims description 8
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 7
- 229920000742 Cotton Polymers 0.000 claims description 7
- 229920001131 Pulp (paper) Polymers 0.000 claims description 7
- 239000000908 ammonium hydroxide Substances 0.000 claims description 7
- 239000004310 lactic acid Substances 0.000 claims description 7
- 235000014655 lactic acid Nutrition 0.000 claims description 7
- 229920003171 Poly (ethylene oxide) Polymers 0.000 claims description 6
- WBJXZTQXFVDYIZ-UHFFFAOYSA-N [Sb].[N+](=O)(O)[O-] Chemical compound [Sb].[N+](=O)(O)[O-] WBJXZTQXFVDYIZ-UHFFFAOYSA-N 0.000 claims description 6
- VGBWDOLBWVJTRZ-UHFFFAOYSA-K cerium(3+);triacetate Chemical compound [Ce+3].CC([O-])=O.CC([O-])=O.CC([O-])=O VGBWDOLBWVJTRZ-UHFFFAOYSA-K 0.000 claims description 6
- 229940031098 ethanolamine Drugs 0.000 claims description 6
- 150000000703 Cerium Chemical class 0.000 claims description 5
- 235000021355 Stearic acid Nutrition 0.000 claims description 5
- HSJPMRKMPBAUAU-UHFFFAOYSA-N cerium(3+);trinitrate Chemical compound [Ce+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O HSJPMRKMPBAUAU-UHFFFAOYSA-N 0.000 claims description 5
- JVLRYPRBKSMEBF-UHFFFAOYSA-K diacetyloxystibanyl acetate Chemical compound [Sb+3].CC([O-])=O.CC([O-])=O.CC([O-])=O JVLRYPRBKSMEBF-UHFFFAOYSA-K 0.000 claims description 5
- 235000011187 glycerol Nutrition 0.000 claims description 5
- 229920000609 methyl cellulose Polymers 0.000 claims description 5
- 239000001923 methylcellulose Substances 0.000 claims description 5
- QIQXTHQIDYTFRH-UHFFFAOYSA-N octadecanoic acid Chemical compound CCCCCCCCCCCCCCCCCC(O)=O QIQXTHQIDYTFRH-UHFFFAOYSA-N 0.000 claims description 5
- OQCDKBAXFALNLD-UHFFFAOYSA-N octadecanoic acid Natural products CCCCCCCC(C)CCCCCCCCC(O)=O OQCDKBAXFALNLD-UHFFFAOYSA-N 0.000 claims description 5
- 229920002401 polyacrylamide Polymers 0.000 claims description 5
- 239000008117 stearic acid Substances 0.000 claims description 5
- 240000008415 Lactuca sativa Species 0.000 claims description 4
- DPXJVFZANSGRMM-UHFFFAOYSA-N acetic acid;2,3,4,5,6-pentahydroxyhexanal;sodium Chemical compound [Na].CC(O)=O.OCC(O)C(O)C(O)C(O)C=O DPXJVFZANSGRMM-UHFFFAOYSA-N 0.000 claims description 4
- 239000001768 carboxy methyl cellulose Substances 0.000 claims description 4
- 235000012045 salad Nutrition 0.000 claims description 4
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 claims description 4
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 claims description 4
- 150000001462 antimony Chemical class 0.000 claims description 3
- 150000003839 salts Chemical class 0.000 claims description 2
- 238000002604 ultrasonography Methods 0.000 claims 1
- 230000002378 acidificating effect Effects 0.000 abstract description 4
- 238000010521 absorption reaction Methods 0.000 abstract description 3
- 239000003795 chemical substances by application Substances 0.000 description 9
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 9
- 239000007788 liquid Substances 0.000 description 7
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 5
- 239000001301 oxygen Substances 0.000 description 5
- 229910052760 oxygen Inorganic materials 0.000 description 5
- 230000000694 effects Effects 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 238000004090 dissolution Methods 0.000 description 3
- 239000003546 flue gas Substances 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 238000006722 reduction reaction Methods 0.000 description 2
- 238000003860 storage Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 231100000331 toxic Toxicity 0.000 description 2
- 230000002588 toxic effect Effects 0.000 description 2
- 229910052684 Cerium Inorganic materials 0.000 description 1
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
- 238000003916 acid precipitation Methods 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- XKMRRTOUMJRJIA-UHFFFAOYSA-N ammonia nh3 Chemical compound N.N XKMRRTOUMJRJIA-UHFFFAOYSA-N 0.000 description 1
- 229910052787 antimony Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000010531 catalytic reduction reaction Methods 0.000 description 1
- 230000001413 cellular effect Effects 0.000 description 1
- 229910000421 cerium(III) oxide Inorganic materials 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000002242 deionisation method Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 239000003517 fume Substances 0.000 description 1
- 238000004868 gas analysis Methods 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 238000005461 lubrication Methods 0.000 description 1
- JKQOBWVOAYFWKG-UHFFFAOYSA-N molybdenum trioxide Inorganic materials O=[Mo](=O)=O JKQOBWVOAYFWKG-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000002574 poison Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 230000002265 prevention Effects 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 238000007493 shaping process Methods 0.000 description 1
- 238000005486 sulfidation Methods 0.000 description 1
- 230000002195 synergetic effect Effects 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/02—Sulfur, selenium or tellurium; Compounds thereof
- B01J27/053—Sulfates
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8625—Nitrogen oxides
- B01D53/8628—Processes characterised by a specific catalyst
-
- B01J35/60—
-
- B01J35/61—
Abstract
The present invention carries a kind of TiO2‑SO4 2‑The high resistant to sulfur ceria-based denitration catalyst of load, the catalyst components mass percentage content are as follows：Active component：10wt% to 20wt%CeO2；Auxiliary agent：8wt% to 15wt%WO3, 1wt% to 5wt%Sb2O3；Carrier：65wt% to 80wt%TiO2‑SO4 2‑.The preparation method of above-mentioned denitrating catalyst is additionally provided, this method comprises the following steps：1)TiO2‑SO4 2‑The preparation of carrier；2) preparation of aqueous solution；3) preparation of catalyst pug；4) extrusion molding；5)；Drying and calcining.The present invention uses TiO2‑SO4 2‑For carrier, have the characteristics that large specific surface area, intensity are high and acidic site is more, larger specific surface area and more acidic site are conducive to catalyst to gaseous state NH3Absorption, so as to promote SCR react progress, higher intensity be conducive to improve catalyst service life.
Description
Technical field
The present invention relates to field of denitration catalyst, more particularly to a kind of high resistant to sulfur ceria-based denitration of TiO2-SO42- loads is urged
Agent and preparation method thereof.
Background technology
Nitrogen oxides (NOx) belongs to a kind of main atmosphere pollution, not only causes a series of ecological environment problems, such as light
Chemical fumes, acid rain, depletion of the ozone layer, greenhouse effects etc., and mankind itself's health can be caused great harm.Nitrogen oxidation
The emission reduction and control of object have become the research hotspot and emphasis in global atmosphere prevention and cure of pollution field.
Core for the ammonia selective catalytic reduction (SCR) of the stationary sources mainstream denitration technology such as thermal power plant exists
There is ripe and efficient catalyst in it.At present, the NH of industrial applications3SCR catalyst, mostly with TiO2For carrier, then bear
Carry a certain amount of V2O5、WO3Or MoO3Etc. components, such catalyst have good resistance to SO_2 while high-efficient purification NOx
Energy.But there are still problems with for the catalyst：First, cost is higher；Second is that active component V2O5Presoma toxicity very
Greatly, easy harmful to human and to environment generate pollution.Therefore, catalyst cost how is reduced, and is keeping high activity of catalyst
While with high sulfidation resistance energy, catalyst preparation and the safety during use are improved, decides that can above-mentioned denitration technology
It is widely used in China's stationary source denitration.
Invention content
In order to solve the above technical problems, the invention is realized in this way：
A kind of TiO2-SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, expression formula CeO2-WO3-Sb2O3/TiO2-
SO4 2-, the catalyst components mass percentage content is as follows：
Active component：10wt% to 20wt%CeO2；
Auxiliary agent：8wt% to 15wt%WO3, 1wt% to 5wt%Sb2O3；
Carrier：65wt% to 80wt%TiO2-SO4 2-。
Wt% is mass percentage, above-mentioned each to be molded later catalyst gross mass as 100wt%
When component meets said ratio, catalyst performance is best.
TiO as described above2-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, this method include as follows
Step：
1)TiO2-SO4 2-The preparation of carrier：Take butyl titanate, acetic acid and ethyl alcohol in molar ratio 1:6:10 stir to get it is molten
Liquid A；The sulfuric acid solution of 60% concentrations above is added in into solution A, the wherein molar ratio of sulfate radical and titanium dioxide is SO4 2-：
TiO2=1:4, it is vigorously stirred to obtain colloidal sol, is placed at room temperature for obtain gel to be placed in drying box and dry, be placed in Muffle furnace
Calcining obtains TiO2-SO4 2-Carrier；
Acetic acid and ethyl alcohol can be suitably excessive with respect to butyl titanate, in order to the colloidal sol that forming properties are stablized.This
Invention limits the solubility of sulfuric acid, and the too low sulfuric acid of solubility is unfavorable for forming colloidal sol.Sulfate radical and titanium dioxide rub
You are than being SO4 2-：TiO2=1:4 can be judged according to element conservation.Numberical range above is only one of the present invention
Preferred scope can according to actual needs be extended it.
2) preparation of aqueous solution：Soluble cerium salt, ammonium paratungstate and soluble antimony salt is taken to be dissolved in deionized water respectively, is surpassed
Sound dissolves, and respectively obtains its aqueous solution；
Soluble cerium salt, ammonium paratungstate and soluble antimony salt are dissolved in deionized water respectively, and the molten of solubility is respectively prepared
Liquid, the purpose for the arrangement is that in order to enable mixing in next step more uniformly, fully.
3) TiO obtained by step 1) is taken2-SO4 2-Carrier, step 2) respectively aqueous solution obtained, glass fibre, binding agent, help
Agent, lubricant, pore creating material, acid solution mixing are squeezed, ammonium hydroxide and deionized water is added in and stirs evenly and aging, obtain pH value and contain for 8 to 9
The catalyst pug of water 20% to 30%, wherein TiO2-SO4 2-The addition of aqueous solution made from carrier, difference, should be according to member
Plain conserva-tion principle meets them and is molded later catalyst components mass percentage content；
Catalyst pug pH value and water content control are in above range so that shaping of catalyst handling ease, and be molded with
The performance of rear catalyst is best.
It can be by TiO2-SO4 2-Aqueous solution, glass fibre, binding agent, extrusion aid, profit made from carrier, step 2) difference
Lubrication prescription, pore creating material, acid solution mixing are placed in batch mixer and are uniformly mixed.
It is aging：Refer to and the pug mixed is placed a period of time, make fully to react and be uniformly mixed between pug, also cry old
Change；Aging preferably 12 hours to 36 hours.
4) take catalyst pug obtained by step 3) is filtered to obtain Faveolate denitration catalyst wet embryo with expressing technique；
Can catalyst be made to desired shape according to actual needs, be not limited to cellular.
5) it takes to calcine after the drying of Faveolate denitration catalyst wet embryo is less than 1% to water content obtained by step 4) and obtains TiO2-
SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load.
Faveolate denitration catalyst wet embryo is dried under slow humiture change condition.Calcining can be in Muffle furnace
It carries out.
Preferably, the calcination temperature described in step 1) is 500 DEG C to 600 DEG C, and calcination time is 3 hours to 5 hours.
Preferably, the soluble cerium salt described in step 2) is at least one of selected from cerous nitrate, cerous acetate, soluble antimonic salt
It is at least one of selected from nitric acid antimony, antimony acetate.
Preferably, the TiO described in step 3)2-SO4 2-Carrier, glass fibre, binding agent, extrusion aid, lubricant, pore-creating
The mass ratio that agent, acid solution add in is 65~80：4~5：0.4~0.6：0.4~0.6：0.2：0.4~0.6：0.6~0.8.
Preferably, the step 3) binding agent includes one kind of polyacrylamide, methylcellulose, sodium carboxymethylcellulose
It is or a variety of；The extrusion aid includes polyoxyethylene or ethanol amine；The lubricant includes one kind of stearic acid, glycerine, salad oil
It is or a variety of；The pore creating material includes paper pulp cotton；The acid solution includes lactic acid.
Preferably, TiO as claimed in claim 22-SO4 2-The preparation side of the high resistant to sulfur ceria-based denitration catalyst of load
Method, the temperature of step 5) calcining is 450 DEG C to 600 DEG C, and calcination time is 4 hours to 6 hours.
The beneficial effects of the present invention are：
The present invention uses TiO2-SO4 2-For carrier, have the characteristics that large specific surface area, intensity are high and acidic site is more, compared with
Big specific surface area and more acidic site are conducive to catalyst to gaseous state NH3Absorption, so as to promote SCR react into
Row, higher intensity are conducive to improve the service life of catalyst.
The present invention uses CeO2For main active component, instead of the vanadium sub-group compound of traditional, toxic effect so that urge
Agent is there is no toxic action, and CeO2It is greatly paid close attention to due to its outstanding oxygen storage capacity and redox ability,
Under conditions of oxidation and reduction, Ce2O3And CeO2Between redox conversion can form unstable Lacking oxygen and mobility
Good Lattice Oxygen species, therefore, CeO2It is used as the active component of SCR reactions, and with good catalytic activity.It adds simultaneously
WO3And Sb2O3To play the auxiliary agent of synergistic effect, WO3Addition effectively reduce catalyst particle diameter, improve particle
Dispersibility reduces the crystallinity of Ce and Ti in catalyst；Mix Sb2O3The catalytic activity of catalyst, Er Qieneng can not only be enhanced
Significantly improve the anti-SO of catalyst2And H2O poisons performance.There are strong interaction between Ce, W and Sb, catalyst is promoted
Middle Ce3+The increase of concentration and chemical absorption of surface oxygen concentration improves the oxygen storage capacity and redox ability of catalyst, from
And effectively increase catalyst SCR activity.
Feasibility of the present invention is strong, the characteristics of being easy to amplificationization, meet Green Chemistry, is promoted conducive to the marketization.
Specific embodiment
In order to describe the technical content, the structural feature, the achieved object and the effect of this invention in detail, below in conjunction with embodiment
It is explained in detail.
Embodiment 1
A kind of TiO2-SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, expression formula CeO2-WO3-Sb2O3/TiO2-
SO4 2-, the catalyst components mass percentage content is as follows：
Active component：10wt%CeO2；
Auxiliary agent：9wt%WO3, 1wt%Sb2O3；
Carrier：80wt%TiO2-SO4 2-。
TiO as described above2-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, this method include as follows
Step：
1)TiO2-SO4 2-The preparation of carrier：Take butyl titanate, acetic acid and ethyl alcohol in molar ratio 1:6:10 stir to get it is molten
Liquid A；The sulfuric acid solution of 60% concentrations above is added in into solution A, the wherein molar ratio of sulfate radical and titanium dioxide is SO4 2-：
TiO2=1:4, it is vigorously stirred to obtain colloidal sol, is placed at room temperature for obtain gel to be placed in drying box and dry, be placed in Muffle furnace
Calcining obtains TiO2-SO4 2-Carrier, calcination temperature are 500 DEG C, and calcination time is 5 hours；
2) preparation of aqueous solution：Cerous nitrate, ammonium paratungstate and nitric acid antimony is taken to be dissolved in deionized water respectively, ultrasonic dissolution,
Respectively obtain its aqueous solution；
3) TiO obtained by step 1) is taken2-SO4 2-Carrier, step 2) respectively aqueous solution obtained, glass fibre, binding agent, help
Agent, lubricant, pore creating material, acid solution mixing are squeezed, ammonium hydroxide and deionized water is added in and stirs evenly and aging, it is aqueous for 8 to obtain pH value
20% catalyst pug,
Wherein TiO2-SO4 2-The addition of aqueous solution, should make them according to element conservation principle made from carrier, difference
Meet and be molded later catalyst components mass percentage content；
Wherein TiO2-SO4 2-The quality that carrier, glass fibre, binding agent, extrusion aid, lubricant, pore creating material, acid solution add in
Than being 80：5：0.6：0.6：0.2：0.6：0.8.
The binding agent includes polyacrylamide；The extrusion aid includes polyoxyethylene；The lubricant includes stearic acid；
The pore creating material includes paper pulp cotton；The acid solution includes lactic acid；
4) take catalyst pug obtained by step 3) is filtered to obtain Faveolate denitration catalyst wet embryo with expressing technique；
5) it takes to calcine after the drying of Faveolate denitration catalyst wet embryo is less than 1% to water content obtained by step 4) and obtains TiO2-
SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, the temperature of calcining is 450 DEG C, and calcination time is 6 hours.
Embodiment 2
A kind of TiO2-SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, expression formula CeO2-WO3-Sb2O3/TiO2-
SO4 2-, the catalyst components mass percentage content is as follows：
Active component：12wt%CeO2；
Auxiliary agent：13wt%WO3, 4wt%Sb2O3；
Carrier：71wt%TiO2-SO4 2-。
TiO as described above2-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, this method include as follows
Step：
1)TiO2-SO4 2-The preparation of carrier：Take butyl titanate, acetic acid and ethyl alcohol in molar ratio 1:6:10 stir to get it is molten
Liquid A；The sulfuric acid solution of 60% concentrations above is added in into solution A, the wherein molar ratio of sulfate radical and titanium dioxide is SO4 2-：
TiO2=1:4, it is vigorously stirred to obtain colloidal sol, is placed at room temperature for obtain gel to be placed in drying box and dry, be placed in Muffle furnace
Calcining obtains TiO2-SO4 2-Carrier, calcination temperature are 600 DEG C, and calcination time is 3 hours；
2) preparation of aqueous solution：Cerous acetate, ammonium paratungstate and antimony acetate is taken to be dissolved in deionized water respectively, ultrasonic dissolution,
Respectively obtain its aqueous solution；
3) TiO obtained by step 1) is taken2-SO4 2-Carrier, step 2) respectively aqueous solution obtained, glass fibre, binding agent, help
Agent, lubricant, pore creating material, acid solution mixing are squeezed, ammonium hydroxide and deionized water is added in and stirs evenly and aging, it is aqueous for 9 to obtain pH value
30% catalyst pug,
Wherein TiO2-SO4 2-The addition of aqueous solution, should make them according to element conservation principle made from carrier, difference
Meet and be molded later catalyst components mass percentage content；
Wherein TiO2-SO4 2-The quality that carrier, glass fibre, binding agent, extrusion aid, lubricant, pore creating material, acid solution add in
Than being 71：4：0.4：0.4：0.2：0.4：0.6.
The binding agent includes methylcellulose；The extrusion aid includes ethanol amine；The lubricant includes glycerine；It is described
Pore creating material includes paper pulp cotton；The acid solution includes lactic acid；
4) take catalyst pug obtained by step 3) is filtered to obtain Faveolate denitration catalyst wet embryo with expressing technique；
5) it takes to calcine after the drying of Faveolate denitration catalyst wet embryo is less than 1% to water content obtained by step 4) and obtains TiO2-
SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, the temperature of calcining is 600 DEG C, and calcination time is 4 hours.
Embodiment 3
A kind of TiO2-SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, expression formula CeO2-WO3-Sb2O3/TiO2-
SO4 2-, the catalyst components mass percentage content is as follows：
Active component：15wt%CeO2；
Auxiliary agent：15wt%WO3, 3wt%Sb2O3；
Carrier：67wt%TiO2-SO4 2-。
TiO as described above2-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, this method include as follows
Step：
1)TiO2-SO4 2-The preparation of carrier：Take butyl titanate, acetic acid and ethyl alcohol in molar ratio 1:6:10 stir to get it is molten
Liquid A；The sulfuric acid solution of 60% concentrations above is added in into solution A, the wherein molar ratio of sulfate radical and titanium dioxide is SO4 2-：
TiO2=1:4, it is vigorously stirred to obtain colloidal sol, is placed at room temperature for obtain gel to be placed in drying box and dry, be placed in Muffle furnace
Calcining obtains TiO2-SO4 2-Carrier, calcination temperature are 520 DEG C, and calcination time is 3.5 hours；
2) preparation of aqueous solution：Cerous nitrate, cerous acetate, ammonium paratungstate and nitric acid antimony, antimony acetate is taken to be dissolved in deionization respectively
In water, ultrasonic dissolution respectively obtains its aqueous solution；
3) TiO obtained by step 1) is taken2-SO4 2-Carrier, step 2) respectively aqueous solution obtained, glass fibre, binding agent, help
Agent, lubricant, pore creating material, acid solution mixing are squeezed, ammonium hydroxide and deionized water is added in and stirs evenly and aging, obtain pH value and contain for 8.5
The catalyst pug of water 23%,
Wherein TiO2-SO4 2-The addition of aqueous solution, should make them according to element conservation principle made from carrier, difference
Meet and be molded later catalyst components mass percentage content；
Wherein TiO2-SO4 2-The quality that carrier, glass fibre, binding agent, extrusion aid, lubricant, pore creating material, acid solution add in
Than being 67：4：0.4：0.4：0.2：0.4：0.6.
The binding agent includes sodium carboxymethylcellulose；The extrusion aid includes polyoxyethylene and ethanol amine；The lubrication
Agent includes salad oil；The pore creating material includes paper pulp cotton；The acid solution includes lactic acid；
4) take catalyst pug obtained by step 3) is filtered to obtain Faveolate denitration catalyst wet embryo with expressing technique；
5) it takes to calcine after the drying of Faveolate denitration catalyst wet embryo is less than 1% to water content obtained by step 4) and obtains TiO2-
SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, the temperature of calcining is 500 DEG C, and calcination time is 5 hours.
The performance of catalyst obtained by the present embodiment is evaluated using simulated flue gas condition, is filled in continuous flow fixed bed
In putting, under normal pressure, with NH3To restore its body, typical flue gas operating mode：NO is 1000ppm, O2For 5%, SO2For 250ppm, H2O is
10%, ammonia nitrogen ratio is 1:1, N2For Balance Air, air speed 5000h-1The performance of the catalyst is evaluated, uses flue gas analysis
The NOx concentration of instrument detection reactor inlet and outlet calculates the denitration efficiency of catalyst.Reaction temperature for 300 DEG C, 400 DEG C, 500
DEG C when catalyst denitration efficiency be respectively 85.2%, 99.6%, 91.8%.
Embodiment 4
A kind of TiO2-SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, expression formula CeO2-WO3-Sb2O3/TiO2-
SO4 2-, the catalyst components mass percentage content is as follows：
Active component：17wt%CeO2；
Auxiliary agent：8wt%WO3, 2wt%Sb2O3；
Carrier：71wt%TiO2-SO4 2-。
TiO as described above2-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, this method include as follows
Step：
1)TiO2-SO4 2-The preparation of carrier：Take butyl titanate, acetic acid and ethyl alcohol in molar ratio 1:6:10 stir to get it is molten
Liquid A；The sulfuric acid solution of 60% concentrations above is added in into solution A, the wherein molar ratio of sulfate radical and titanium dioxide is SO4 2-：
TiO2=1:4, it is vigorously stirred to obtain colloidal sol, is placed at room temperature for obtain gel to be placed in drying box and dry, be placed in Muffle furnace
Calcining obtains TiO2-SO4 2-Carrier, calcination temperature are 550 DEG C, and calcination time is 4 hours；
2) preparation of aqueous solution：Cerous nitrate, cerous acetate, ammonium paratungstate and nitric acid antimony is taken to be dissolved in deionized water respectively, is surpassed
Sound dissolves, and respectively obtains its aqueous solution；
3) TiO obtained by step 1) is taken2-SO4 2-Carrier, step 2) respectively aqueous solution obtained, glass fibre, binding agent, help
Agent, lubricant, pore creating material, acid solution mixing are squeezed, ammonium hydroxide and deionized water is added in and stirs evenly and aging, it is aqueous for 9 to obtain pH value
25% catalyst pug,
Wherein TiO2-SO4 2-The addition of aqueous solution, should make them according to element conservation principle made from carrier, difference
Meet and be molded later catalyst components mass percentage content；
Wherein TiO2-SO4 2-The quality that carrier, glass fibre, binding agent, extrusion aid, lubricant, pore creating material, acid solution add in
Than being 71：4.5：0.5：0.5：0.2：0.5：0.7.
The binding agent includes polyacrylamide, methylcellulose；The extrusion aid includes polyoxyethylene and ethanol amine；Institute
It states lubricant and includes stearic acid, glycerine；The pore creating material includes paper pulp cotton；The acid solution includes lactic acid；
4) take catalyst pug obtained by step 3) is filtered to obtain Faveolate denitration catalyst wet embryo with expressing technique；
5) it takes to calcine after the drying of Faveolate denitration catalyst wet embryo is less than 1% to water content obtained by step 4) and obtains TiO2-
SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, the temperature of calcining is 520 DEG C, and calcination time is 5 hours.
Embodiment 5
A kind of TiO2-SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, expression formula CeO2-WO3-Sb2O3/TiO2-
SO4 2-, the catalyst components mass percentage content is as follows：
Active component：20wt%CeO2；
Auxiliary agent：10wt%WO3, 5wt%Sb2O3；
Carrier：65wt%TiO2-SO4 2-。
TiO as described above2-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, this method include as follows
Step：
1)TiO2-SO4 2-The preparation of carrier：Take butyl titanate, acetic acid and ethyl alcohol in molar ratio 1:6:10 stir to get it is molten
Liquid A；The sulfuric acid solution of 60% concentrations above is added in into solution A, the wherein molar ratio of sulfate radical and titanium dioxide is SO4 2-：
TiO2=1:4, it is vigorously stirred to obtain colloidal sol, is placed at room temperature for obtain gel to be placed in drying box and dry, be placed in Muffle furnace
Calcining obtains TiO2-SO4 2-Carrier, calcination temperature are 500 DEG C to 600 DEG C, and calcination time is 3 hours to 5 hours；
2) preparation of aqueous solution：Cerous acetate, ammonium paratungstate and nitric acid antimony, antimony acetate is taken to be dissolved in deionized water respectively, is surpassed
Sound dissolves, and respectively obtains its aqueous solution；
3) TiO obtained by step 1) is taken2-SO4 2-Carrier, step 2) respectively aqueous solution obtained, glass fibre, binding agent, help
Agent, lubricant, pore creating material, acid solution mixing are squeezed, ammonium hydroxide and deionized water is added in and stirs evenly and aging, it is aqueous for 8 to obtain pH value
28% catalyst pug,
Wherein TiO2-SO4 2-The addition of aqueous solution, should make them according to element conservation principle made from carrier, difference
Meet and be molded later catalyst components mass percentage content；
Wherein TiO2-SO4 2-The quality that carrier, glass fibre, binding agent, extrusion aid, lubricant, pore creating material, acid solution add in
Than being 65：4：0.4：0.4：0.2：0.4：0.6.
The binding agent includes polyacrylamide, methylcellulose, sodium carboxymethylcellulose；The extrusion aid includes polyoxy
Ethylene and ethanol amine；The lubricant includes stearic acid, glycerine, salad oil；The pore creating material includes paper pulp cotton；The acid solution packet
Include lactic acid；
4) take catalyst pug obtained by step 3) is filtered to obtain Faveolate denitration catalyst wet embryo with expressing technique；
5) it takes to calcine after the drying of Faveolate denitration catalyst wet embryo is less than 1% to water content obtained by step 4) and obtains TiO2-
SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, the temperature of calcining is 550 DEG C, and calcination time is 5.5 hours.
The foregoing is merely the embodiment of the present invention, not thereby limit the scope of patent protection of the present invention, every utilization
The equivalent structure or equivalent flow shift that present specification is made directly or indirectly is used in other relevant technologies
Field is included within the scope of the present invention.
Claims (7)
1. a kind of TiO2-SO4 2-The high resistant to sulfur ceria-based denitration catalyst of load, expression formula CeO2-WO3-Sb2O3/TiO2-SO4 2-,
It is characterized in that, the catalyst components mass percentage content is as follows：
Active component：10wt% to 20wt%CeO2；
Auxiliary agent：8wt% to 15wt%WO3, 1wt% to 5wt%Sb2O3；
Carrier：65wt% to 80wt%TiO2-SO4 2-。
2. TiO as described in claim 12-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, feature exist
In this method comprises the following steps：
1)TiO2-SO4 2-The preparation of carrier：Take butyl titanate, acetic acid and ethyl alcohol in molar ratio 1:6:10 stir to get solution A；
The sulfuric acid solution of 60% concentrations above is added in into solution A, the wherein molar ratio of sulfate radical and titanium dioxide is SO4 2-：TiO2=
1:4, it is vigorously stirred to obtain colloidal sol, is placed at room temperature for obtain gel to be placed in drying box and dry, be placed in calcining in Muffle furnace
To TiO2-SO4 2-Carrier；
2) preparation of aqueous solution：Soluble cerium salt, ammonium paratungstate and soluble antimony salt is taken to be dissolved in deionized water respectively, ultrasound is molten
Solution, respectively obtains its aqueous solution；
3) TiO obtained by step 1) is taken2-SO4 2-Carrier, step 2) respectively made from aqueous solution, glass fibre, binding agent, extrusion aid,
Lubricant, pore creating material, acid solution mixing add in ammonium hydroxide and deionized water and stir evenly and aging, it is aqueous for 8 to 9 to obtain pH value
20% to 30% catalyst pug, wherein TiO2-SO4 2-The addition of aqueous solution, should keep according to element made from carrier, difference
Permanent principle meets them and is molded later catalyst components mass percentage content；
4) take catalyst pug obtained by step 3) is filtered to obtain Faveolate denitration catalyst wet embryo with expressing technique；
5) it takes to calcine after the drying of Faveolate denitration catalyst wet embryo is less than 1% to water content obtained by step 4) and obtains TiO2-SO4 2-It is negative
The high resistant to sulfur ceria-based denitration catalyst carried.
3. TiO as claimed in claim 22-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, feature exist
In the calcination temperature described in step 1) is 500 DEG C to 600 DEG C, and calcination time is 3 hours to 5 hours.
4. TiO as claimed in claim 22-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, feature exist
It is at least one of to be selected from cerous nitrate, cerous acetate in, soluble cerium salt described in step 2), soluble antimonic salt be selected from nitric acid antimony,
Antimony acetate is at least one of.
5. TiO as claimed in claim 22-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, feature exist
In the TiO described in step 3)2-SO4 2-The matter that carrier, glass fibre, binding agent, extrusion aid, lubricant, pore creating material, acid solution add in
Amount is than being 65~80：4~5：0.4~0.6：0.4~0.6：0.2：0.4~0.6：0.6~0.8.
6. TiO as claimed in claim 52-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, feature exist
In, the step 3) binding agent include polyacrylamide, methylcellulose, sodium carboxymethylcellulose it is one or more；It is described
Extrusion aid includes polyoxyethylene or ethanol amine；The lubricant include stearic acid, glycerine, salad oil it is one or more；It is described
Pore creating material includes paper pulp cotton；The acid solution includes lactic acid.
7. TiO as claimed in claim 22-SO4 2-The preparation method of the high resistant to sulfur ceria-based denitration catalyst of load, feature exist
In the temperature of step 5) calcining is 450 DEG C to 600 DEG C, and calcination time is 4 hours to 6 hours.
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| CN109126807A (en) * | 2018-10-12 | 2019-01-04 | 安徽建筑大学 | A kind of copper containing mixed oxides high/low temperature denitrating catalyst and preparation method thereof |
| CN110368925A (en) * | 2019-04-04 | 2019-10-25 | 上海大学 | The preparation method of the modified cerium tungsten oxide carried titanium dioxide denitrating catalyst of Sb doped |
| CN111195524A (en) * | 2020-01-17 | 2020-05-26 | 中国科学院重庆绿色智能技术研究院 | Tubular S-CT/TNT denitration catalyst with strong alkali metal poisoning resistance and preparation method thereof |
| CN112844482A (en) * | 2021-01-14 | 2021-05-28 | 万华化学集团股份有限公司 | Acid-base dual-function heterogeneous catalyst with core-shell structure, preparation method thereof and method for cracking and recycling butyl acrylate heavy component |
| CN115155607A (en) * | 2022-07-12 | 2022-10-11 | 中晶环境科技股份有限公司 | Solid catalyst, process for producing the same and use thereof |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109126807A (en) * | 2018-10-12 | 2019-01-04 | 安徽建筑大学 | A kind of copper containing mixed oxides high/low temperature denitrating catalyst and preparation method thereof |
| CN110368925A (en) * | 2019-04-04 | 2019-10-25 | 上海大学 | The preparation method of the modified cerium tungsten oxide carried titanium dioxide denitrating catalyst of Sb doped |
| CN111195524A (en) * | 2020-01-17 | 2020-05-26 | 中国科学院重庆绿色智能技术研究院 | Tubular S-CT/TNT denitration catalyst with strong alkali metal poisoning resistance and preparation method thereof |
| CN112844482A (en) * | 2021-01-14 | 2021-05-28 | 万华化学集团股份有限公司 | Acid-base dual-function heterogeneous catalyst with core-shell structure, preparation method thereof and method for cracking and recycling butyl acrylate heavy component |
| CN112844482B (en) * | 2021-01-14 | 2022-04-22 | 万华化学集团股份有限公司 | Acid-base dual-function heterogeneous catalyst with core-shell structure, preparation method thereof and method for cracking and recycling butyl acrylate heavy component |
| CN115155607A (en) * | 2022-07-12 | 2022-10-11 | 中晶环境科技股份有限公司 | Solid catalyst, process for producing the same and use thereof |
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