CN109225248A - Cellular low-temperature denitration catalyst and its preparation process - Google Patents
Cellular low-temperature denitration catalyst and its preparation process Download PDFInfo
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- CN109225248A CN109225248A CN201810903216.7A CN201810903216A CN109225248A CN 109225248 A CN109225248 A CN 109225248A CN 201810903216 A CN201810903216 A CN 201810903216A CN 109225248 A CN109225248 A CN 109225248A
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- 239000003054 catalyst Substances 0.000 title claims abstract description 82
- 230000001413 cellular effect Effects 0.000 title claims abstract description 24
- 238000002360 preparation method Methods 0.000 title claims abstract description 24
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 27
- 239000011347 resin Substances 0.000 claims description 31
- 229920005989 resin Polymers 0.000 claims description 31
- NBVXSUQYWXRMNV-UHFFFAOYSA-N fluoromethane Chemical compound FC NBVXSUQYWXRMNV-UHFFFAOYSA-N 0.000 claims description 25
- 239000000463 material Substances 0.000 claims description 20
- 230000001376 precipitating effect Effects 0.000 claims description 20
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 18
- 230000032683 aging Effects 0.000 claims description 18
- 239000006210 lotion Substances 0.000 claims description 18
- 239000004033 plastic Substances 0.000 claims description 18
- 239000008367 deionised water Substances 0.000 claims description 16
- 229910021641 deionized water Inorganic materials 0.000 claims description 16
- 239000000243 solution Substances 0.000 claims description 13
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 11
- -1 polytetrafluoroethylene Polymers 0.000 claims description 11
- 239000001099 ammonium carbonate Substances 0.000 claims description 9
- 239000007864 aqueous solution Substances 0.000 claims description 9
- 238000001354 calcination Methods 0.000 claims description 9
- 238000001914 filtration Methods 0.000 claims description 9
- 229910002804 graphite Inorganic materials 0.000 claims description 9
- 239000010439 graphite Substances 0.000 claims description 9
- 239000012535 impurity Substances 0.000 claims description 9
- 239000000377 silicon dioxide Substances 0.000 claims description 9
- 229910001593 boehmite Inorganic materials 0.000 claims description 8
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 claims description 8
- 238000005360 mashing Methods 0.000 claims description 8
- 150000000703 Cerium Chemical class 0.000 claims description 7
- PRKQVKDSMLBJBJ-UHFFFAOYSA-N ammonium carbonate Chemical class N.N.OC(O)=O PRKQVKDSMLBJBJ-UHFFFAOYSA-N 0.000 claims description 7
- 235000011162 ammonium carbonates Nutrition 0.000 claims description 7
- 150000001868 cobalt Chemical class 0.000 claims description 7
- 238000001035 drying Methods 0.000 claims description 7
- 150000002696 manganese Chemical class 0.000 claims description 7
- 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 6
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 claims description 5
- 229910001981 cobalt nitrate Inorganic materials 0.000 claims description 5
- 239000011737 fluorine Substances 0.000 claims description 5
- 229910052731 fluorine Inorganic materials 0.000 claims description 5
- 229920003063 hydroxymethyl cellulose Polymers 0.000 claims description 5
- 229940031574 hydroxymethyl cellulose Drugs 0.000 claims description 5
- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(2+);dinitrate Chemical compound [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 claims description 4
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 4
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 4
- MULYSYXKGICWJF-UHFFFAOYSA-L cobalt(2+);oxalate Chemical compound [Co+2].[O-]C(=O)C([O-])=O MULYSYXKGICWJF-UHFFFAOYSA-L 0.000 claims description 3
- RGVLTEMOWXGQOS-UHFFFAOYSA-L manganese(2+);oxalate Chemical compound [Mn+2].[O-]C(=O)C([O-])=O RGVLTEMOWXGQOS-UHFFFAOYSA-L 0.000 claims description 3
- ATRRKUHOCOJYRX-UHFFFAOYSA-N Ammonium bicarbonate Chemical compound [NH4+].OC([O-])=O ATRRKUHOCOJYRX-UHFFFAOYSA-N 0.000 claims description 2
- 235000012501 ammonium carbonate Nutrition 0.000 claims description 2
- 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 2
- 229940011182 cobalt acetate Drugs 0.000 claims description 2
- QAHREYKOYSIQPH-UHFFFAOYSA-L cobalt(II) acetate Chemical compound [Co+2].CC([O-])=O.CC([O-])=O QAHREYKOYSIQPH-UHFFFAOYSA-L 0.000 claims description 2
- 238000000227 grinding Methods 0.000 claims description 2
- 229940071125 manganese acetate Drugs 0.000 claims description 2
- UOGMEBQRZBEZQT-UHFFFAOYSA-L manganese(2+);diacetate Chemical compound [Mn+2].CC([O-])=O.CC([O-])=O UOGMEBQRZBEZQT-UHFFFAOYSA-L 0.000 claims description 2
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 claims 2
- 229910052799 carbon Inorganic materials 0.000 claims 2
- 229910001868 water Inorganic materials 0.000 abstract description 10
- 239000003513 alkali Substances 0.000 abstract description 8
- 229910052717 sulfur Inorganic materials 0.000 abstract description 7
- 239000011593 sulfur Substances 0.000 abstract description 7
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 abstract description 6
- 230000000694 effects Effects 0.000 abstract description 6
- 239000002689 soil Substances 0.000 abstract description 6
- 206010027439 Metal poisoning Diseases 0.000 abstract description 5
- 239000002994 raw material Substances 0.000 abstract description 3
- 239000002585 base Substances 0.000 description 15
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 9
- 239000000523 sample Substances 0.000 description 5
- 229920002678 cellulose Polymers 0.000 description 4
- 235000010980 cellulose Nutrition 0.000 description 4
- 239000002244 precipitate Substances 0.000 description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 description 3
- VQWQYXBWRCCZGX-UHFFFAOYSA-N acetic acid;manganese Chemical compound [Mn].CC(O)=O.CC(O)=O VQWQYXBWRCCZGX-UHFFFAOYSA-N 0.000 description 3
- 239000001913 cellulose Substances 0.000 description 3
- 239000003795 chemical substances by application Substances 0.000 description 3
- 229910052802 copper Inorganic materials 0.000 description 3
- 239000010949 copper Substances 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 239000011572 manganese Substances 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 229910052751 metal Inorganic materials 0.000 description 3
- 239000002184 metal Substances 0.000 description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- 229910052723 transition metal Inorganic materials 0.000 description 3
- 150000003624 transition metals Chemical class 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- ZMZNLKYXLARXFY-UHFFFAOYSA-H cerium(3+);oxalate Chemical class [Ce+3].[Ce+3].[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O ZMZNLKYXLARXFY-UHFFFAOYSA-H 0.000 description 2
- 239000003610 charcoal Substances 0.000 description 2
- 235000013495 cobalt Nutrition 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 239000003546 flue gas Substances 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 229910052700 potassium Inorganic materials 0.000 description 2
- 239000011591 potassium Substances 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
- 206010006966 Calcium intoxication Diseases 0.000 description 1
- 229910052684 Cerium Inorganic materials 0.000 description 1
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 150000001340 alkali metals Chemical class 0.000 description 1
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- 150000001342 alkaline earth metals Chemical class 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000012752 auxiliary agent Substances 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000011575 calcium Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 238000010531 catalytic reduction reaction Methods 0.000 description 1
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 238000000975 co-precipitation Methods 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 229910052878 cordierite Inorganic materials 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 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 1
- 239000012153 distilled water Substances 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 230000002779 inactivation Effects 0.000 description 1
- 230000008595 infiltration Effects 0.000 description 1
- 238000001764 infiltration Methods 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 230000035987 intoxication Effects 0.000 description 1
- 231100000566 intoxication Toxicity 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 description 1
- 239000006101 laboratory sample Substances 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- IPJKJLXEVHOKSE-UHFFFAOYSA-L manganese dihydroxide Chemical compound [OH-].[OH-].[Mn+2] IPJKJLXEVHOKSE-UHFFFAOYSA-L 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 231100000572 poisoning Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- FGIUAXJPYTZDNR-UHFFFAOYSA-N potassium nitrate Chemical compound [K+].[O-][N+]([O-])=O FGIUAXJPYTZDNR-UHFFFAOYSA-N 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000006722 reduction reaction Methods 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
- 239000004408 titanium dioxide Substances 0.000 description 1
- MEYZYGMYMLNUHJ-UHFFFAOYSA-N tunicamycin Natural products CC(C)CCCCCCCCCC=CC(=O)NC1C(O)C(O)C(CC(O)C2OC(C(O)C2O)N3C=CC(=O)NC3=O)OC1OC4OC(CO)C(O)C(O)C4NC(=O)C MEYZYGMYMLNUHJ-UHFFFAOYSA-N 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
- B01J23/002—Mixed oxides other than spinels, e.g. perovskite
-
- 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
-
- 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
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/889—Manganese, technetium or rhenium
- B01J23/8892—Manganese
-
- 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
- B01J33/00—Protection of catalysts, e.g. by coating
-
- 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
- B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
-
- 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
- B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/30—Capture or disposal of greenhouse gases of perfluorocarbons [PFC], hydrofluorocarbons [HFC] or sulfur hexafluoride [SF6]
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
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- Organic Chemistry (AREA)
- Environmental & Geological Engineering (AREA)
- Health & Medical Sciences (AREA)
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- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
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Abstract
The invention discloses a kind of cellular low-temperature denitration catalyst and its preparation processes, the preparation process of catalyst of the present invention is simple, it is easy to form, and the catalyst low-temperature activity of preparation is high, water resistant sulfur resistive alkali resistant (soil) metal poisoning ability is strong, and the present invention is using useless SCR catalyst as raw material, low in cost, resource utilization can be achieved and give up SCR catalyst, it can be achieved that useless SCR catalyst recycles.
Description
Technical field
The present invention relates to a kind of cellular low-temperature denitration catalyst and its preparation processes.
Background technique
In nitrogen oxides pollution control field, selective catalytic reduction (SCR, selective catalytic
It reduction) is the gas denitrifying technology being most widely used.SCR denitration is with NH3As reducing agent, by catalysis
Oxynitrides harmful in flue gas is reduced into harmless nitrogen by effect.Currently, low-temperature denitration catalyst has become SCR
One hot research topic of catalyst field.
For the active component for the low-temperature SCR catalyst studied at present based on transition metal, Mn member procatarxis has a variety of valence states,
And activation energy required for changing between valence state is lower, has excellent denitration performance at low temperature, is generally acknowledged low-temperature denitration
Catalyst activity component, but its water resistant resistance to SO_2 is poor, and in process of production either with manganese nitrate or manganous hydroxide,
Will (200 DEG C) low due to decomposition temperature cause the product of production to burst, bad mechanical strength causes formed honeycomb difficult,
High production cost.
Patent CN 201610056551.9 discloses a kind of honeycomb monolith low-temperature denitration catalyst and its preparation process,
It immerses transition metal (iron, cobalt, copper, nickel, manganese, cerium) salt in titanium dioxide, forms suspension, then matches with other auxiliary agents and is slurried
Material is coated on honeycomb cordierite carrier, and then drying and calcining obtains honeycomb monolith low-temperature denitration catalyst, but the low temperature is de-
Denox catalyst active component in the high cloud of dust gas of low temperature is prone to wear, it is difficult to industrial applications, and the preparation process of catalyst
Complexity, higher cost.
Patent CN 201611002394.X discloses a kind of preparation process of honeycomb Mn based low-temperature denitration catalyst,
It calcines carrier and active component manganese, cerium and molysite to form powder material, then extrusion molding obtains manganese base honeycomb low temperature
Denitrating catalyst, but the resistance to SO_2 of the low-temperature denitration catalyst is poor, also without investigating influence of the water to catalyst, is easy inactivation.
Patent 201711195037.4 discloses a kind of alkali resistant and is poisoned the preparation work of copper-based spinelle low-temperature denitration catalyst
Mantoquita and metal salt, metal salt, distilled water and mixed acid solution are formed solution, then dried, in oxygen-enriched atmosphere condition by skill
Under, calcining obtains the copper-based spinelle low-temperature denitration catalyst of alkali resistant poisoning, but the low-temperature denitration catalyst is powder sample, is not had
Molding, and also catalyst is influenced without investigating water, it is difficult to industrial applications.
It is urged as it can be seen that needing to research and develop one kind the cellular low-temperature denitration for having water resistant sulfur resistive alkali resistant (soil) metal poisoning ability strong
Agent.
Summary of the invention
The purpose of the present invention is to provide a kind of cellular low-temperature denitration catalyst and its preparation process, catalyst of the present invention
Preparation process it is simple, it is easy to form, and the catalyst low-temperature activity prepared is high, water resistant sulfur resistive alkali resistant (soil) metal poisoning ability
By force, and the present invention is using useless SCR catalyst as raw material, and the SCR catalyst low in cost, it can be achieved that resource utilization is given up is, it can be achieved that useless
SCR catalyst recycles.
To achieve the above object, the present invention provides a kind of preparation process of cellular low-temperature denitration catalyst, including as follows
Step:
1) by after the grinding of the useless SCR catalyst of cleaning-drying, investment is furnished in the aqueous solution of cobalt salt, cerium salt and manganese salt,
80~100 DEG C of mashing are added ammonium carbonate and generate precipitating, 4~6h of aging, and filtering is precipitated and is cleaned and dried；
2) will precipitating obtained by step 1) and boehmite, silica solution, hydroxymethyl cellulose, graphite and deionized water be kneaded at
Plastic mud material；
3) impurity, pugging are filtered to plastic mud material obtained by step 2, it is aging；
4) by pug vacuum extruding form obtained by step 3), the wet base of honeycomb is obtained；
5) fluorocarbon resin lotion will be immersed after the wet base drying of honeycomb obtained by step 4), is dried after taking-up, is then forged again
It is burnt into cellular low-temperature denitration catalyst.
Preferably, in step 1), cobalt salt is selected from one of cobalt nitrate, cobalt oxalate, cobalt acetate；Cerium salt be selected from cerous nitrate,
One of cerous nitrate, cerous acetate；Manganese salt is selected from one of manganese nitrate, manganese acetate, manganese oxalate.
Preferably, in step 5), fluorocarbon resin in fluorocarbon resin lotion be selected from polytetrafluoroethylene (PTFE), polytrifluorochloroethylene,
One of polyfluoroethylene resin.
Preferably, the preparation process of above-mentioned cellular low-temperature denitration catalyst, includes the following steps:
1) useless SCR catalyst of 100 parts by weight after being cleaned and dried is ground to granularity d50 is 3~5 μm, and then investment is matched
Have 2~6 parts by weight cobalt salts, 9~50 parts by weight cerium salts, 25~70 parts by weight manganese salts 350~500 parts by weight aqueous solutions in,
80~100 DEG C of 30~60min of mashing are added 20~60 parts by weight ammonium carbonates and generate precipitating, 4~6h of aging, and filtering precipitating is used in combination
Deionized water is cleaned 2~4 times, in 90~110 DEG C of dry 2~4h；
2) by precipitating obtained by step 1) and 0.8~1.5 parts by weight boehmite, 3~5 parts by weight silica solution, 0.8~1.2 weight
Part hydroxymethyl cellulose, 0.5~0.8 parts by weight of graphite and 80~200 parts by weight of deionized water are measured to be kneaded into plastic mud material；
3) impurity, pugging are filtered to plastic mud material obtained by step 2, it is aging；
4) by pug vacuum extruding form obtained by step 3), the wet base of honeycomb is obtained；
5) fluorocarbon resin lotion will be immersed after the wet base drying of honeycomb obtained by step 4), 80~100 DEG C is carried out at after taking-up again
Cellular low-temperature denitration catalyst is made then in 350~450 DEG C of 6~8h of calcining in dry 6~8h.
Preferably, in step 5), the mass concentration of fluorocarbon resin is 0.1%~0.3% in fluorocarbon resin lotion.
The present invention also provides cellular low-temperature denitration catalysts obtained by above-mentioned preparation process.
Advantages and advantages of the present invention are to provide a kind of honeycomb fashion low-temperature denitration catalyst and its preparation process,
The preparation process of catalyst of the present invention is simple, easy to form, and the catalyst low-temperature activity prepared is high, water resistant sulfur resistive alkali resistant (soil)
Metal poisoning ability is strong, and the present invention, using useless SCR catalyst as raw material, the SCR low in cost, it can be achieved that resource utilization is given up is catalyzed
Agent is, it can be achieved that useless SCR catalyst recycles.
Cobalt salt, manganese salt and cerium salt are precipitated into carbonate by the present invention, and the temperature that carbonate decomposition becomes oxide is high, can
Slow release gas, be not in honeycomb catalyst burst, bad mechanical strength the problem of, active component presoma, carrier and heavy
Shallow lake agent coprecipitation, together, so that the dispersibility of active component is more preferable, more stable, low temperature is de- for active component and carrier interaction
Nitre activity is high.
Catalyst soak in fluorine charcoal resin, can be such that fluorine charcoal resin penetrates into the inside and outside wall of catalyst by the present invention, filling
Catalyst inside and outside wall wall surface micropore forms fine and close hole wall infiltration tunic, and high temperature fluorine can be reacted with transition metal generates table
Face fluorinated oxide makes catalyst have water resistant sulfur resistive ability, and increases catalyst strength, make catalyst have it is high-intensitive and
Alkali resistant (soil) metal ability.
The present invention, which can be used, cleans thoroughly dry useless SCR catalyst as carrier, and abundance is low in cost, can provide
Sourceization realizes useless SCR catalyst and recycles using useless SCR catalyst.The preparation time of catalyst of the present invention is short, for industry
Change practical application to lay the foundation.
Specific embodiment
With reference to embodiment, the specific embodiment of the present invention is further described.Following embodiment is only used for more
Add and clearly demonstrate technical solution of the present invention, and not intended to limit the protection scope of the present invention.
The technical solution that the present invention embodies is:
Embodiment 1
1) useless SCR catalyst of 100 parts by weight after being cleaned and dried is ground to granularity d50 is 3~5 μm, and then investment is matched
In the 350 parts by weight aqueous solutions for having 4.35 parts by weight cobalt nitrates, 9.1 parts by weight of cerium nitrate, 69 parts by weight manganese nitrates, beaten at 80 DEG C
60min is starched, 22.8 parts by weight ammonium carbonates are added and generate precipitating, aging 4h, filtering is precipitated and cleaned 2 times with deionized water, 90
DEG C dry 4h；
2) by precipitating obtained by step 1) and 0.8 parts by weight boehmite, 3 parts by weight silica solution, 0.8 parts by weight hydroxylmethyl cellulose
Element, 0.5 parts by weight of graphite and 80 parts by weight of deionized water are kneaded into plastic mud material；
3) impurity, pugging are filtered to plastic mud material obtained by step 2, it is aging；
4) by pug vacuum extruding form obtained by step 3), the wet base of honeycomb is obtained；
5) will the wet base of honeycomb obtained by step 4) it is dry after immerse the fluorocarbon resin lotion (matter of fluorocarbon resin in fluorocarbon resin lotion
Amount concentration is 0.1%), after taking-up to be carried out at 80 DEG C and dry 8h again then in 350 DEG C of calcining 8h cellular low-temperature denitration to be made
Catalyst.
Embodiment 2
1) useless SCR catalyst of 100 parts by weight after being cleaned and dried is ground to granularity d50 is 3~5 μm, and then investment is matched
In the 500 parts by weight aqueous solutions for having 5.43 parts by weight cobalt oxalates, 45.2 parts by weight cerium oxalates, 44.12 parts by weight manganese oxalates,
100 DEG C of mashing 30min are added 55.52 parts by weight ammonium carbonates and generate precipitating, aging 6h, and filtering precipitates and cleans 4 with deionized water
It is secondary, in 110 DEG C of dry 2h；
2) by precipitating obtained by step 1) and 1.5 parts by weight boehmites, 5 parts by weight silica solution, 1.2 parts by weight hydroxylmethyl celluloses
Element, 0.8 parts by weight of graphite and 100 parts by weight of deionized water are kneaded into plastic mud material；
3) impurity, pugging are filtered to plastic mud material obtained by step 2, it is aging；
4) by pug vacuum extruding form obtained by step 3), the wet base of honeycomb is obtained；
5) will the wet base of honeycomb obtained by step 4) it is dry after immerse the fluorocarbon resin lotion (matter of fluorocarbon resin in fluorocarbon resin lotion
Amount concentration is 0.3%), after taking-up to be carried out at 100 DEG C to dry 6h again, and then in 450 DEG C of calcining 6h, it is de- that cellular low temperature is made
Denox catalyst.
Embodiment 3
1) useless SCR catalyst of 100 parts by weight after being cleaned and dried is ground to granularity d50 is 3~5 μm, and then investment is matched
In the 400 parts by weight aqueous solutions for having 5.07 parts by weight acetic acid cobalts, 42.2 parts by weight acetic acid ceriums, 27.5 parts by weight acetic acid manganese, 90
DEG C mashing 45min, be added 56.2 parts by weight ammonium carbonates generate precipitating, aging 5h, filtering precipitate simultaneously cleaned 3 times with deionized water,
In 100 DEG C of dry 3h；
2) will precipitating obtained by step 1) and 1 parts by weight boehmite, 4 parts by weight silica solution, 1 parts by weight hydroxymethyl cellulose,
0.7 parts by weight of graphite and 90 parts by weight of deionized water are kneaded into plastic mud material；
3) impurity, pugging are filtered to plastic mud material obtained by step 2, it is aging；
4) by pug vacuum extruding form obtained by step 3), the wet base of honeycomb is obtained；
5) will the wet base of honeycomb obtained by step 4) it is dry after immerse the fluorocarbon resin lotion (matter of fluorocarbon resin in fluorocarbon resin lotion
Amount concentration is 0.2%), after taking-up to be carried out at 80 DEG C and dry 8h again then in 350 DEG C of calcining 8h cellular low-temperature denitration to be made
Catalyst.
Embodiment 4
1) useless SCR catalyst of 100 parts by weight after being cleaned and dried is ground to granularity d50 is 3~5 μm, and then investment is matched
In the 450 parts by weight aqueous solutions for having 2.89 parts by weight cobalt nitrates, 12.05 parts by weight cerium oxalates, 39.1 parts by weight acetic acid manganese,
100 DEG C of mashing 45min are added 24.95 parts by weight ammonium carbonates and generate precipitating, aging 5h, and filtering precipitates and cleans 2 with deionized water
It is secondary, in 90 DEG C of dry 4h；
2) by precipitating obtained by step 1) and 0.8 parts by weight boehmite, 3 parts by weight silica solution, 0.8 parts by weight hydroxylmethyl cellulose
Element, 0.5 parts by weight of graphite and 200 parts by weight of deionized water are kneaded into plastic mud material；
3) impurity, pugging are filtered to plastic mud material obtained by step 2, it is aging；
4) by pug vacuum extruding form obtained by step 3), the wet base of honeycomb is obtained；
5) will the wet base of honeycomb obtained by step 4) it is dry after immerse the fluorocarbon resin lotion (matter of fluorocarbon resin in fluorocarbon resin lotion
Amount concentration is 0.3%), after taking-up to be carried out at 80 DEG C and dry 8h again then in 400 DEG C of calcining 8h cellular low-temperature denitration to be made
Catalyst.
Embodiment 5
1) useless SCR catalyst of 100 parts by weight after being cleaned and dried is ground to granularity d50 is 3~5 μm, and then investment is matched
In the 500 parts by weight aqueous solutions for having 4.76 parts by weight cobalt nitrates, 19.8 parts by weight acetic acid ceriums, 25.77 parts by weight acetic acid manganese,
100 DEG C of mashing 60min are added 32.65 parts by weight ammonium carbonates and generate precipitating, aging 4h, and filtering precipitates and cleans 2 with deionized water
It is secondary, in 90 DEG C of dry 4h；
2) by precipitating obtained by step 1) and 0.8 parts by weight boehmite, 3 parts by weight silica solution, 0.8 parts by weight hydroxylmethyl cellulose
Element, 0.5 parts by weight of graphite and 200 parts by weight of deionized water are kneaded into plastic mud material；
3) impurity, pugging are filtered to plastic mud material obtained by step 2, it is aging；
4) by pug vacuum extruding form obtained by step 3), the wet base of honeycomb is obtained；
5) will the wet base of honeycomb obtained by step 4) it is dry after immerse the fluorocarbon resin lotion (matter of fluorocarbon resin in fluorocarbon resin lotion
Amount concentration is 0.25%), after taking-up to be carried out at 80 DEG C to dry 8h again, and then in 350 DEG C of calcining 8h, it is de- that cellular low temperature is made
Denox catalyst.
Denitration experiment
Prepare three laboratory samples:
Sample 1: denitrating catalyst made from embodiment 1, as fresh catalyst；
Sample 2: the K of 1.0wt% is loaded on the denitrating catalyst made from embodiment 12O carries out potassium intoxication experiment；
Sample 3: loading the CaO of 2.5wt% on the denitrating catalyst made from embodiment 1, carries out calcium intoxication experiment；
Then with the denitration efficiency of flue gas analyzer detection each sample；Test condition are as follows: NO 500ppm, NH3500ppm,
O210%, SO2500ppm, 10%H2O, N2For Balance Air, air speed 5000h-1, 150~250 DEG C of temperature are detected, catalyst 20 × 20
Hole, length 500mm.Testing result is as shown in table 1.
1 catalyst denitration efficiency testing result of table
As it can be seen from table 1 the low temperature active of denitrating catalyst of the present invention is high, denitration efficiency under the conditions of high-sulfur Gao Shui compares
Height, and the denitration efficiency after carrying alkali metal potassium and alkaline earth metals calcium is also relatively high.As it can be seen that present invention honeycomb fashion low-temperature denitration
Water resistant sulfur resistive alkali resistant (soil) metal poisoning ability of catalyst is stronger.
The above is only a preferred embodiment of the present invention, it is noted that for the ordinary skill people of the art
For member, without departing from the technical principles of the invention, several improvements and modifications can also be made, these improvements and modifications
Also it should be regarded as protection scope of the present invention.
Claims (6)
1. the preparation process of cellular low-temperature denitration catalyst, which comprises the steps of:
1) by after the grinding of the useless SCR catalyst of cleaning-drying, investment is furnished in the aqueous solution of cobalt salt, cerium salt and manganese salt,
80~100 DEG C of mashing are added ammonium carbonate and generate precipitating, 4~6h of aging, and filtering is precipitated and is cleaned and dried；
2) will precipitating obtained by step 1) and boehmite, silica solution, hydroxymethyl cellulose, graphite and deionized water be kneaded at
Plastic mud material；
3) impurity, pugging are filtered to plastic mud material obtained by step 2, it is aging；
4) by pug vacuum extruding form obtained by step 3), the wet base of honeycomb is obtained；
5) fluorocarbon resin lotion will be immersed after the wet base drying of honeycomb obtained by step 4), is dried after taking-up, is then forged again
It is burnt into cellular low-temperature denitration catalyst.
2. the preparation process of cellular low-temperature denitration catalyst according to claim 1, which is characterized in that in step 1), cobalt
Salt is selected from one of cobalt nitrate, cobalt oxalate, cobalt acetate；Cerium salt is selected from one of cerous nitrate, cerous nitrate, cerous acetate；Manganese salt
Selected from one of manganese nitrate, manganese acetate, manganese oxalate.
3. the preparation process of cellular low-temperature denitration catalyst according to claim 1, which is characterized in that in step 5), fluorine
Fluorocarbon resin in carbon resin lotion is selected from one of polytetrafluoroethylene (PTFE), polytrifluorochloroethylene, polyfluoroethylene resin.
4. the according to claim 1, preparation process of the 2 or 3 cellular low-temperature denitration catalysts, which is characterized in that including such as
Lower step:
1) useless SCR catalyst of 100 parts by weight after being cleaned and dried is ground to granularity d50 is 3~5 μm, and then investment is matched
Have 2~6 parts by weight cobalt salts, 9~50 parts by weight cerium salts, 25~70 parts by weight manganese salts 350~500 parts by weight aqueous solutions in,
80~100 DEG C of 30~60min of mashing are added 20~60 parts by weight ammonium carbonates and generate precipitating, 4~6h of aging, and filtering precipitating is used in combination
Deionized water is cleaned 2~4 times, in 90~110 DEG C of dry 2~4h；
2) by precipitating obtained by step 1) and 0.8~1.5 parts by weight boehmite, 3~5 parts by weight silica solution, 0.8~1.2 weight
Part hydroxymethyl cellulose, 0.5~0.8 parts by weight of graphite and 80~200 parts by weight of deionized water are measured to be kneaded into plastic mud material；
3) impurity, pugging are filtered to plastic mud material obtained by step 2, it is aging；
4) by pug vacuum extruding form obtained by step 3), the wet base of honeycomb is obtained；
5) fluorocarbon resin lotion will be immersed after the wet base drying of honeycomb obtained by step 4), 80~100 DEG C is carried out at after taking-up again
Cellular low-temperature denitration catalyst is made then in 350~450 DEG C of 6~8h of calcining in dry 6~8h.
5. the preparation process of cellular low-temperature denitration catalyst according to claim 4, which is characterized in that in step 5), fluorine
The mass concentration of fluorocarbon resin is 0.1%~0.3% in carbon resin lotion.
6. cellular low-temperature denitration catalyst obtained by preparation process described in any one of claims 1 to 5.
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