CN106076305B - A kind of grade spheric catalyst and preparation method thereof and its application in denitrating flue gas - Google Patents
A kind of grade spheric catalyst and preparation method thereof and its application in denitrating flue gas Download PDFInfo
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- CN106076305B CN106076305B CN201610414362.4A CN201610414362A CN106076305B CN 106076305 B CN106076305 B CN 106076305B CN 201610414362 A CN201610414362 A CN 201610414362A CN 106076305 B CN106076305 B CN 106076305B
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- flue gas
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- spheric catalyst
- denitrating flue
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- 239000003054 catalyst Substances 0.000 title claims abstract description 53
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 26
- 239000003546 flue gas Substances 0.000 title claims abstract description 26
- 238000002360 preparation method Methods 0.000 title claims abstract description 25
- IXPNQXFRVYWDDI-UHFFFAOYSA-N 1-methyl-2,4-dioxo-1,3-diazinane-5-carboximidamide Chemical compound CN1CC(C(N)=N)C(=O)NC1=O IXPNQXFRVYWDDI-UHFFFAOYSA-N 0.000 claims abstract description 18
- 238000001035 drying Methods 0.000 claims abstract description 18
- 235000010413 sodium alginate Nutrition 0.000 claims abstract description 18
- 239000000661 sodium alginate Substances 0.000 claims abstract description 18
- 229940005550 sodium alginate Drugs 0.000 claims abstract description 18
- 239000002002 slurry Substances 0.000 claims abstract description 14
- 238000003837 high-temperature calcination Methods 0.000 claims abstract description 13
- 238000003756 stirring Methods 0.000 claims abstract description 12
- 239000000843 powder Substances 0.000 claims abstract description 10
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 claims abstract description 9
- 229910052751 metal Inorganic materials 0.000 claims abstract description 6
- 239000002184 metal Substances 0.000 claims abstract description 6
- 229910044991 metal oxide Inorganic materials 0.000 claims abstract description 6
- 150000004706 metal oxides Chemical class 0.000 claims abstract description 6
- 150000003839 salts Chemical class 0.000 claims abstract description 6
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 16
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical group [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims description 13
- 230000002572 peristaltic effect Effects 0.000 claims description 9
- 239000000395 magnesium oxide Substances 0.000 claims description 7
- 239000011787 zinc oxide Substances 0.000 claims description 6
- 238000010907 mechanical stirring Methods 0.000 claims description 5
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical group [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 claims description 4
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 4
- 238000001354 calcination Methods 0.000 claims description 4
- 239000003795 chemical substances by application Substances 0.000 claims description 4
- 229910000019 calcium carbonate Inorganic materials 0.000 claims description 2
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 claims description 2
- 239000001095 magnesium carbonate Substances 0.000 claims description 2
- 229910000021 magnesium carbonate Inorganic materials 0.000 claims description 2
- 239000004408 titanium dioxide Substances 0.000 claims description 2
- 238000000034 method Methods 0.000 abstract description 16
- 230000000694 effects Effects 0.000 abstract description 4
- 230000008901 benefit Effects 0.000 abstract description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 13
- 229910052878 cordierite Inorganic materials 0.000 description 6
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 6
- 239000002245 particle Substances 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 230000004913 activation Effects 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 230000005284 excitation Effects 0.000 description 1
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 238000001179 sorption measurement Methods 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/06—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of zinc, cadmium or mercury
-
- 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
-
- 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
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/10—Magnesium; Oxides or hydroxides thereof
-
- 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
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/16—Clays or other mineral silicates
-
- B01J35/40—
-
- B01J35/51—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/02—Other waste gases
- B01D2258/0283—Flue gases
Abstract
Application the invention discloses a kind of grade spheric catalyst and preparation method thereof and its in denitrating flue gas, is related to field of catalyst preparation, solves the problems, such as preparation method complexity and at high cost.The method of the present invention obtains presoma slurries the following steps are included: by metal-oxide powder or metal salt powder addition sodium alginate soln after stirring;The presoma slurries are added dropwise in calcium chloride solution, millimeter ball presoma is obtained;High-temperature calcination will be carried out again after millimeter ball presoma drying, grade spheric catalyst is obtained after high-temperature calcination.The method of the present invention has the advantages that preparation process is simple, grade spheric catalyst denitration effect at low cost and preparation is good.
Description
Technical field
The method of the present invention is related to field of catalyst preparation more particularly to a kind of grade spheric catalyst and preparation method thereof
And its application in denitrating flue gas.
Background technique
Environmental problem has become most one of severe challenge that China faces 21 century, and fast-developing is economical and increasingly prominent
The contradiction between environmental problem out, has been to be concerned by more and more people.Wherein, nitrogen oxides (NOx) is that main atmosphere is dirty
Contaminate one of object.
Plasma is a kind of state existing for substance, is by largely interacting but still under non-bound state
The meta system of charged particle composition, is the 4th state of substance that same level is in solid-state, liquid, gaseous state.In numerous low temperature
In the method for plasma, dielectric barrier discharge has stable discharge, and the opposite low advantage that consumes energy has good industrial application
Prospect.
Plasma and catalyst cooperation-removal nitrogen oxides remove NO because having energy consumption smallXTemperature is low and removal is imitated
The advantages that rate is high has been increasingly becoming NOXOne of novel method of pollution control.In dielectric impedance (DBD) low temperature plasma
Preparing for middle catalyst is most important, especially grade spheric catalyst wherein served it is critically important.
Discharge of plasma in low temperature generate high energy active particle and simulated flue gas in NOx molecular collision, activate, reach
Excitation state, meanwhile, high energy active particle bombards catalyst particle surface, enhances the dispersibility at catalyst surface active center;It urges
Agent has certain adsorption capacity to NO gas, easily forms gas source molecule enrichment region in catalyst surface, reaction can break through tradition
All kinds of physical-chemical reaction removing NO occur rapidly for chemical reaction, in addition, some studies pointed out that in plasma body cooperative catalytic denitration
Catalyst can not only accelerate to react, moreover it is possible to selectively generate product.
Therefore, grade spheric catalyst is prepared, using plasma technique, denitrating flue gas efficiency, drop can be improved
Low cost plays critically important effect;It now urgently develops a kind of simple process and at low cost prepares grade spheric catalyst
Method.
Summary of the invention
In view of this, the embodiment of the invention provides a kind of grade spheric catalyst and preparation method thereof and its in flue gas
Application in denitration, main purpose are to provide a kind of simple process and the lower-cost side for preparing grade spheric catalyst
Method.
In order to achieve the above objectives, the embodiment of the present invention mainly provides following technical solution:
On the one hand, the embodiment of the invention provides a kind of preparation methods of grade spheric catalyst, which comprises
Metal-oxide powder or metal salt powder are added in sodium alginate soln, presoma slurries are obtained after stirring;
The presoma slurries are added dropwise in calcium chloride solution, millimeter ball presoma is obtained;
High-temperature calcination will be carried out again after millimeter ball presoma drying, grade spherical shape is obtained after high-temperature calcination and is urged
Agent.
Preferably, the metal oxide is magnesia, zinc oxide or titanium dioxide;The metal salt be calcium carbonate,
Magnesium carbonate or cordierite.
Preferably, the mass percentage concentration of the sodium alginate soln is 1.5%-3%.
Preferably, the stirring is mechanical stirring, the churned mechanically rate is 300r/min-1500r/min.
Preferably, the equipment of the dropwise addition is peristaltic pump tube, the caliber of the peristaltic pump tube is 1mm-5mm;Before described
Driving flow velocity of the somaplasm liquid in peristaltic pump tube is 50mL/min-500mL/min.
Preferably, the mass percentage concentration of the calcium chloride solution is 4%-8%.
Preferably, the drying is carried out in drying box, drying temperature is 80 DEG C -200 DEG C, drying time 3h-
48h。
Preferably, the high-temperature calcination is carried out in Muffle furnace, calcination temperature is 400 DEG C -1200 DEG C, calcination time
For 2h-48h.
On the other hand, a kind of grade spheric catalyst is prepared using the above method in the embodiment of the present invention.
In another aspect, the application the embodiment of the invention provides above-mentioned grade spheric catalyst in denitrating flue gas.
Compared with prior art, the beneficial effects of the present invention are:
The present invention is for the technical issues of grade spheric catalyst preparation process is complicated and higher cost, using by metal
Oxide powder or metal salt powder are added in sodium alginate soln, and presoma slurries are obtained after stirring;By forerunner's somaplasm
Drop adds in calcium chloride solution, obtains millimeter ball presoma;High-temperature calcination will be carried out again after millimeter ball presoma drying,
The method that grade spheric catalyst is obtained after high-temperature calcination keeps whole preparation process process simple, at low cost, production effect
Rate is high, can largely improve denitration efficiency of the catalyst in flue gas under condition of plasma.
Detailed description of the invention
Fig. 1 is denitration efficiency of the zinc oxide grade spheric catalyst of the preparation of the embodiment of the present invention 1 in flue gas;
Fig. 2 is denitration efficiency of the magnesia grade spheric catalyst of the preparation of the embodiment of the present invention 2 in flue gas;
Fig. 3 is denitration efficiency of the cordierite grade spheric catalyst of the preparation of the embodiment of the present invention 3 in flue gas.
Specific embodiment
It is of the invention to reach the technical means and efficacy that predetermined goal of the invention is taken further to illustrate, below in conjunction with
Preferred embodiment, to specific embodiment, technical solution, feature and its effect applied according to the present invention, detailed description is as follows.
The special characteristic, structure or feature in multiple embodiments in following the description can be combined by any suitable form.
Embodiment 1
Preparation weighs 2.0174g sodium alginate, is slowly added in 98ml pure water while using mechanical stirring, passes through machine
Tool stirring obtains sodium alginate soln after being completely dissolved sodium alginate;
Preparation weighs 40.31g Zinc oxide powder, and above-mentioned Zinc oxide powder is slowly added in above-mentioned sodium alginate soln,
The revolving speed of blender is adjusted after adding to 700r/min, continues to obtain presoma slurries after stirring two hours;
By above-mentioned presoma slurries with the flow velocity of 400mL/min, sucked by the peristaltic pump tube that caliber is 2mm, dropwise plus
Enter in the calcium chloride solution for being 7% to prepared mass percentage concentration in advance, obtains millimeter ball presoma;
Above-mentioned millimeter ball presoma is put into drying box and dries 3h at being 90 DEG C in temperature;
It is 600 DEG C that sample after drying, which is put into Muffle furnace in temperature, and heating rate is 10 DEG C/min, high-temperature calcination 3h
Afterwards, the zinc oxide grade spheric catalyst that diameter is 2mm is obtained.
Embodiment 2
Preparation weighs 1.81g sodium alginate, is slowly added in 98ml pure water while using mechanical stirring, passes through machinery
Stirring obtains sodium alginate soln after being completely dissolved sodium alginate;
Preparation weighs 40.15g magnesium oxide powder, and above-mentioned Zinc oxide powder is slowly added in above-mentioned sodium alginate soln,
The revolving speed of blender is adjusted after adding to 600r/min, continues to obtain presoma slurries after stirring a hour;
By above-mentioned presoma slurries with the flow velocity of 200mL/min, sucked by the peristaltic pump tube that caliber is 3mm, dropwise plus
Enter in the calcium chloride solution for being 6% to prepared mass percentage concentration in advance, obtains millimeter ball presoma;
Above-mentioned millimeter ball presoma is put into drying box and dries 4h at being 100 DEG C in temperature;
It is 650 DEG C that sample after drying, which is put into Muffle furnace in temperature, and heating rate is 10 DEG C/min, high-temperature calcination 5h
Afterwards, the magnesia grade spheric catalyst that diameter is 3mm is obtained.
Embodiment 3
Preparation weighs 2.25g sodium alginate, is slowly added in 98ml pure water while using mechanical stirring, passes through machinery
Stirring obtains sodium alginate soln after being completely dissolved sodium alginate;
Preparation weighs 40.02g cordierite powder, and above-mentioned Zinc oxide powder is slowly added in above-mentioned sodium alginate soln,
The revolving speed of blender is adjusted after adding to 750r/min, continues to obtain presoma slurries after stirring two hours;
By above-mentioned presoma slurries with the flow velocity of 200mL/min, sucked by the peristaltic pump tube that caliber is 4mm, dropwise plus
Enter in the calcium chloride solution for being 6% to prepared mass percentage concentration in advance, obtains millimeter ball presoma;
Above-mentioned millimeter ball presoma is put into drying box and dries 3h at being 110 DEG C in temperature;
It is 550 DEG C that sample after drying, which is put into Muffle furnace in temperature, and heating rate is 10 DEG C/min, high-temperature calcination 5h
Afterwards, the cordierite grade spheric catalyst that diameter is 3mm is obtained.
Embodiment 4
The grade magnesia spherical shape of the grade zinc oxide spheric catalyst, the preparation of embodiment 2 that prepare to embodiment 1 is urged
Grade cordierite spheric catalyst prepared by agent and embodiment 3 carries out the experiment of denitrating flue gas;
Specific experiment method are as follows: utilize the denitration situation of simulated flue gas test grade sphere catalyst;
Simulated flue gas composition are as follows: NO:500ppm, O2: 5%vol, N2For Balance Air;
Flue gas total flow is 100mL/min, wherein NO flow is 40mL/min, O2Flow be 5mL/min, nitrogen stream
Amount is 55mL/min;
Above-mentioned three kinds of grade spheric catalysts are put into dielectric impedance pipe, carry out the suction of nitrogen oxides at normal temperatures and pressures
Attached, activation, decomposition reaction;Using the concentration of flue gas analyzer detection reactor exit NO;Wherein, the calculation formula of denitrification rate
Are as follows:
Denitration efficiency of the above-mentioned three kinds of grade spheric catalysts in flue gas has been obtained by calculating analysis, wherein such as
Shown in Fig. 1, the denitration efficiency of grade zinc oxide spheric catalyst prepared by embodiment 1 is 96.4%;As shown in Fig. 2, implementing
The denitration efficiency of grade magnesia spheric catalyst prepared by example 2 is 98.7%;As shown in figure 3, millimeter prepared by embodiment 3
The denitration efficiency of grade cordierite spheric catalyst is 99.3%;The grade spheric catalyst of preparation of the embodiment of the present invention is compared to same
The catalyst denitration efficiency of type is higher.
The method that the embodiment of the present invention prepares grade spheric catalyst is simple, high production efficiency, consume energy it is low, it is at low cost and
Denitration efficiency of the grade spheric catalyst prepared in flue gas is higher.
Place, those skilled in the art can not select from the prior art to the greatest extent in the embodiment of the present invention.
Disclosed above is only a specific embodiment of the invention, but scope of protection of the present invention is not limited thereto, is appointed
What those familiar with the art in the technical scope disclosed by the present invention, can easily think of the change or the replacement, answer
It is included within the scope of the present invention.Therefore, protection scope of the present invention should be with above-mentioned scope of protection of the claims.
Claims (7)
1. a kind of application of grade spheric catalyst in denitrating flue gas, which is characterized in that the catalyst is in plasma item
Applied under part, the preparation method of the catalyst the following steps are included:
Metal-oxide powder or metal salt powder are added in sodium alginate soln, presoma slurries are obtained after stirring;Wherein,
The metal oxide is magnesia, zinc oxide or titanium dioxide;The metal salt is calcium carbonate, magnesium carbonate;
The presoma slurries are added dropwise in calcium chloride solution, millimeter ball presoma is obtained;
High-temperature calcination will be carried out again after millimeter ball presoma drying, grade spherical catalyst is obtained after high-temperature calcination
Agent.
2. a kind of application of the grade spheric catalyst according to claim 1 in denitrating flue gas, which is characterized in that institute
The mass percentage concentration for stating sodium alginate soln is 1.5%-3%.
3. a kind of application of the grade spheric catalyst according to claim 1 in denitrating flue gas, which is characterized in that institute
Stating stirring is mechanical stirring, and the churned mechanically rate is 300r/min-1500r/min.
4. a kind of application of the grade spheric catalyst according to claim 1 in denitrating flue gas, which is characterized in that institute
The equipment for stating dropwise addition is peristaltic pump tube, and the caliber of the peristaltic pump tube is 1mm-5mm;The presoma slurries are in peristaltic pump tube
Flow velocity be 50mL/min-500mL/min.
5. a kind of application of the grade spheric catalyst according to claim 1 in denitrating flue gas, which is characterized in that institute
The mass percentage concentration for stating calcium chloride solution is 4%-8%.
6. a kind of application of the grade spheric catalyst according to claim 1 in denitrating flue gas, which is characterized in that institute
Stating drying is carried out in drying box, and drying temperature is 80 DEG C -200 DEG C, drying time 3h-48h.
7. a kind of application of the grade spheric catalyst according to claim 1 in denitrating flue gas, which is characterized in that institute
Stating high-temperature calcination is carried out in Muffle furnace, and calcination temperature is 400 DEG C -1200 DEG C, calcination time 2h-48h.
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Citations (2)
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CN102718241A (en) * | 2012-06-28 | 2012-10-10 | 天津大学 | Method for preparing spherical alumina particles by alginic acid auxiliary forming method |
CN103055694A (en) * | 2011-10-21 | 2013-04-24 | 中国石油化工股份有限公司 | Method for flue gas denitrification by organic waste gas |
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CN103055694A (en) * | 2011-10-21 | 2013-04-24 | 中国石油化工股份有限公司 | Method for flue gas denitrification by organic waste gas |
CN102718241A (en) * | 2012-06-28 | 2012-10-10 | 天津大学 | Method for preparing spherical alumina particles by alginic acid auxiliary forming method |
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