CN116116430A - Catalyst for purifying carbon monoxide and nitrogen oxides simultaneously and preparation method and application thereof - Google Patents
Catalyst for purifying carbon monoxide and nitrogen oxides simultaneously and preparation method and application thereof Download PDFInfo
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- CN116116430A CN116116430A CN202211741400.9A CN202211741400A CN116116430A CN 116116430 A CN116116430 A CN 116116430A CN 202211741400 A CN202211741400 A CN 202211741400A CN 116116430 A CN116116430 A CN 116116430A
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- 239000003054 catalyst Substances 0.000 title claims abstract description 80
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 64
- 229910002091 carbon monoxide Inorganic materials 0.000 title claims abstract description 53
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 title claims description 12
- 238000002360 preparation method Methods 0.000 title claims description 9
- 230000003197 catalytic effect Effects 0.000 claims abstract description 39
- 230000003647 oxidation Effects 0.000 claims abstract description 38
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 38
- 238000000576 coating method Methods 0.000 claims abstract description 36
- 239000011248 coating agent Substances 0.000 claims abstract description 33
- 238000010531 catalytic reduction reaction Methods 0.000 claims abstract description 29
- 229910052878 cordierite Inorganic materials 0.000 claims abstract description 13
- 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 claims abstract description 13
- 239000003546 flue gas Substances 0.000 claims abstract description 13
- 238000000034 method Methods 0.000 claims abstract description 13
- 238000001125 extrusion Methods 0.000 claims abstract description 8
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 22
- 238000001354 calcination Methods 0.000 claims description 22
- 239000002243 precursor Substances 0.000 claims description 22
- 238000001035 drying Methods 0.000 claims description 21
- 239000000654 additive Substances 0.000 claims description 18
- 230000000996 additive effect Effects 0.000 claims description 18
- 239000011230 binding agent Substances 0.000 claims description 17
- 239000000843 powder Substances 0.000 claims description 16
- 239000002002 slurry Substances 0.000 claims description 16
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 claims description 15
- 238000000227 grinding Methods 0.000 claims description 14
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims description 12
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 12
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 12
- 239000004408 titanium dioxide Substances 0.000 claims description 11
- 239000001866 hydroxypropyl methyl cellulose Substances 0.000 claims description 8
- 229920003088 hydroxypropyl methyl cellulose Polymers 0.000 claims description 8
- 235000010979 hydroxypropyl methyl cellulose Nutrition 0.000 claims description 8
- UFVKGYZPFZQRLF-UHFFFAOYSA-N hydroxypropyl methyl cellulose Chemical compound OC1C(O)C(OC)OC(CO)C1OC1C(O)C(O)C(OC2C(C(O)C(OC3C(C(O)C(O)C(CO)O3)O)C(CO)O2)O)C(CO)O1 UFVKGYZPFZQRLF-UHFFFAOYSA-N 0.000 claims description 8
- 239000011148 porous material Substances 0.000 claims description 8
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims description 7
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 7
- 238000005245 sintering Methods 0.000 claims description 7
- 229910052684 Cerium Inorganic materials 0.000 claims description 6
- 229910002651 NO3 Inorganic materials 0.000 claims description 6
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 6
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 6
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 6
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims description 6
- 229910052742 iron Inorganic materials 0.000 claims description 6
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 6
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 5
- 229910052802 copper Inorganic materials 0.000 claims description 5
- 239000010949 copper Substances 0.000 claims description 5
- 238000004519 manufacturing process Methods 0.000 claims description 5
- 239000000203 mixture Substances 0.000 claims description 5
- 239000002808 molecular sieve Substances 0.000 claims description 5
- 235000006408 oxalic acid Nutrition 0.000 claims description 5
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical group O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 claims description 5
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 5
- 238000003756 stirring Methods 0.000 claims description 5
- 229920000663 Hydroxyethyl cellulose Polymers 0.000 claims description 4
- 239000004354 Hydroxyethyl cellulose Substances 0.000 claims description 4
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 4
- 235000019447 hydroxyethyl cellulose Nutrition 0.000 claims description 4
- 238000002156 mixing Methods 0.000 claims description 4
- 229910017604 nitric acid Inorganic materials 0.000 claims description 4
- 229920002401 polyacrylamide Polymers 0.000 claims description 4
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 claims description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 claims description 3
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 3
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims description 3
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims description 3
- VXAUWWUXCIMFIM-UHFFFAOYSA-M aluminum;oxygen(2-);hydroxide Chemical compound [OH-].[O-2].[Al+3] VXAUWWUXCIMFIM-UHFFFAOYSA-M 0.000 claims description 3
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 3
- 229910052737 gold Inorganic materials 0.000 claims description 3
- 239000010931 gold Substances 0.000 claims description 3
- 229910052763 palladium Inorganic materials 0.000 claims description 3
- 229910052697 platinum Inorganic materials 0.000 claims description 3
- 229910052718 tin Inorganic materials 0.000 claims description 3
- PBYZMCDFOULPGH-UHFFFAOYSA-N tungstate Chemical compound [O-][W]([O-])(=O)=O PBYZMCDFOULPGH-UHFFFAOYSA-N 0.000 claims description 3
- LSGOVYNHVSXFFJ-UHFFFAOYSA-N vanadate(3-) Chemical group [O-][V]([O-])([O-])=O LSGOVYNHVSXFFJ-UHFFFAOYSA-N 0.000 claims description 3
- 229910052726 zirconium Inorganic materials 0.000 claims description 3
- 239000002202 Polyethylene glycol Substances 0.000 claims description 2
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 2
- 235000011054 acetic acid Nutrition 0.000 claims description 2
- 229910000278 bentonite Inorganic materials 0.000 claims description 2
- 239000000440 bentonite Substances 0.000 claims description 2
- SVPXDRXYRYOSEX-UHFFFAOYSA-N bentoquatam Chemical compound O.O=[Si]=O.O=[Al]O[Al]=O SVPXDRXYRYOSEX-UHFFFAOYSA-N 0.000 claims description 2
- 229920001223 polyethylene glycol Polymers 0.000 claims description 2
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 2
- 229910052710 silicon Inorganic materials 0.000 claims description 2
- 239000010703 silicon Substances 0.000 claims description 2
- 235000011121 sodium hydroxide Nutrition 0.000 claims description 2
- 238000000746 purification Methods 0.000 claims 1
- 230000008030 elimination Effects 0.000 abstract description 4
- 238000003379 elimination reaction Methods 0.000 abstract description 4
- 229910000831 Steel Inorganic materials 0.000 abstract description 3
- 238000006555 catalytic reaction Methods 0.000 abstract description 3
- 238000013461 design Methods 0.000 abstract description 3
- 239000010959 steel Substances 0.000 abstract description 3
- 238000011217 control strategy Methods 0.000 abstract description 2
- 238000006243 chemical reaction Methods 0.000 description 7
- 229910052783 alkali metal Inorganic materials 0.000 description 4
- 150000001340 alkali metals Chemical class 0.000 description 4
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 4
- 150000001342 alkaline earth metals Chemical class 0.000 description 4
- 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 description 4
- 239000003344 environmental pollutant Substances 0.000 description 4
- 238000011068 loading method Methods 0.000 description 4
- 231100000719 pollutant Toxicity 0.000 description 4
- 229910052723 transition metal Inorganic materials 0.000 description 4
- 150000003624 transition metals Chemical class 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 239000002253 acid Substances 0.000 description 3
- 230000002378 acidificating effect Effects 0.000 description 3
- 229910052782 aluminium Inorganic materials 0.000 description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 238000010276 construction Methods 0.000 description 3
- 239000008367 deionised water Substances 0.000 description 3
- 229910021641 deionized water Inorganic materials 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 229910000281 calcium bentonite Inorganic materials 0.000 description 2
- 125000002091 cationic group Chemical group 0.000 description 2
- 239000006255 coating slurry Substances 0.000 description 2
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- 238000006722 reduction reaction Methods 0.000 description 2
- 238000009628 steelmaking Methods 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- UNTBPXHCXVWYOI-UHFFFAOYSA-O azanium;oxido(dioxo)vanadium Chemical compound [NH4+].[O-][V](=O)=O UNTBPXHCXVWYOI-UHFFFAOYSA-O 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 239000012159 carrier gas Substances 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000006477 desulfuration reaction Methods 0.000 description 1
- 230000023556 desulfurization Effects 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 239000000446 fuel Substances 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
- 239000000126 substance Substances 0.000 description 1
- HPGGPRDJHPYFRM-UHFFFAOYSA-J tin(iv) chloride Chemical compound Cl[Sn](Cl)(Cl)Cl HPGGPRDJHPYFRM-UHFFFAOYSA-J 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
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- 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
- 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
- B01D53/46—Removing components of defined structure
- B01D53/54—Nitrogen compounds
- B01D53/56—Nitrogen oxides
-
- 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
- B01D53/46—Removing components of defined structure
- B01D53/62—Carbon oxides
-
- 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
- B01D53/864—Removing carbon monoxide or hydrocarbons
-
- 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
- B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
- B01J23/8933—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals also combined with metals, or metal oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/8993—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals also combined with metals, or metal oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with chromium, molybdenum or tungsten
-
- 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
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/40—Nitrogen compounds
- B01D2257/404—Nitrogen oxides other than dinitrogen oxide
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/50—Carbon oxides
- B01D2257/502—Carbon monoxide
-
- 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
-
- 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
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- 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
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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Abstract
The invention relates to the technical field of flue gas treatment in the steel industry, in particular to a method for simultaneously treating CO and NO x Is prepared from the catalyst, its preparing process and application. The catalyst of the invention can be prepared in two ways: (1) For a pair with NO x The extrusion type honeycomb catalyst carrier with the selective catalytic reduction function is coated with a CO oxidation catalytic active layer; (2) Staged coating of NO on honeycomb cordierite x A selective catalytic reduction active layer and a CO oxidation catalytic active layer. The invention uses NO x And CO elimination function organically combined into a catalystThe front-back stage catalysis of the same catalyst is realized, so that the design pressure can be relieved, the occupied area of equipment is reduced, the use cost is greatly reduced, the use amount of the catalyst can be saved, and the control strategy of the catalyst is simpler and more efficient.
Description
Technical Field
The invention relates to the technical field of flue gas treatment in the steel industry, in particular to a method for simultaneously treating CO and NO x Is prepared from the catalyst, its preparing process and application.
Background
Sintering is an indispensable ring in the long-flow steelmaking process as a production means of sinter. During sintering, the fuel reacts with oxygen in the air, and carbon and nitrogen are converted at high temperature into carbon monoxide (CO) and nitrogen oxides (NO x ) Both types of atmospheric pollutants. Statistically, CO and NO generated during sintering x Respectively occupy 15 percent and 48 percent of the long-flow steelmaking process, and is the first pollution load of the steel production process.
CO and NO in sintering flue gas x Catalytic chemical reactions (CO oxidation catalysis and NO) essentially relying on honeycomb catalysts x Selective catalytic reduction) to effect elimination. The conventional honeycomb catalyst includes two types, one obtained by extruding a catalytically active component into a honeycomb shape by an extruder and the other obtained by coating a catalytically active component on a honeycomb-shaped carrier by a coater. In practical industrial application, CO oxidation catalyst and NO x The selective reduction catalysts are respectively filled in different reactors and are arranged in the later use of dust removal and desulfurization equipment of the flue gas. The treatment mode can ensure the performance of the catalyst, but the two reactors are required to be simultaneously installed, so that the occupied area of equipment is increased, and the process design difficulty in a compact space environment is improved. In addition, the additional catalyst usage and the high equipment construction costs also greatly increase the operating and construction costs.
Disclosure of Invention
The invention aims at solving the technical problems of CO and NO in the existing sintering flue gas x The defect of treatment is that an extrusion type honeycomb catalyst or honeycomb cordierite is used as a carrier to simultaneously purify CO and NO x The catalyst not only has better CO and NO x The catalyst consumption and the reactor construction cost can be reduced, and the economy of sintering flue gas treatment is obviously improved.
The invention simultaneously purifies CO and NO x The two-stage catalyst is characterized in that two parts on the surface of a carrier are respectively different catalytic active layers, wherein the proportion of the two catalytic active layers and/or the coating amount of the catalytic active layers are different. The front-back section proportion and the coating amount can be flexibly modulated according to the concentration of pollutant components in the flue gas and the control requirement on pollutants, and completely different formula schemes are adopted to realize the simultaneous control of two pollutants by a single catalyst.
The CO oxidation catalytic active component is one or more of titanium dioxide loaded alkali metal, alkaline earth metal, carbon metal and transition metal, or one or more of alumina loaded alkali metal, alkaline earth metal, carbon metal and transition metal; NO (NO) x The selective catalytic reduction active component is one or more of titanium dioxide loaded alkali metal, alkaline earth metal and transition metal, or one or more of ZSM-5, MOR, SSZ-13, SAPO-34, SSZ-39 and SAPO-18 molecular sieve loaded alkali metal, alkaline earth metal and transition metal.
When the extrusion type honeycomb catalyst is used as a carrier, the carrier is NO x The selective catalytic reduction active component is mainly. The active component precursor, the binder and the additive are uniformly mixed and stirred, extruded by a honeycomb catalyst vacuum extruder, and the extrudate is dried and calcined to obtain the extruded honeycomb catalyst carrier. The extrusion type honeycomb catalyst carrier simultaneously plays roles of carrier and eliminating NO in flue gas x Is effective in (1). After the preparation of the extrusion honeycomb catalyst carrier is finished, uniformly mixing the precursor of the CO oxidation catalytic active component with the binder, grinding (the grinding speed is 600-1000 r/min and the time is 0.5-3 h), and adding the additive after finishing grinding to obtain the catalyst for coatingThe slurry is coated (the coating amount is 60-180 g/L) on a part of the area of the honeycomb catalyst carrier by using a coating machine, and then the CO oxidation catalyst active layer is obtained by drying and calcining. The coating length of the CO oxidation catalytic active layer occupies 1/3 to 2/3 of the carrier.
Further, the number of holes of the extruded honeycomb catalyst carrier is 25 to 50.
Further, the NO x The precursor of the selective catalytic reduction active component is vanadate, tungstate, or one or more of nitrate, sulfate and acetate of copper, cerium, zirconium and iron, and is combined with one or more of titanium dioxide powder, ZSM-5, MOR, SSZ-13, SAPO-34, SSZ-39 and SAPO-18 molecular sieve powder.
Further, the precursor of the CO oxidation catalytic active component is one or more of chloride, nitrate and sulfate of platinum, palladium, gold, copper, cerium, tin or iron, and is combined with one or more of pseudo-boehmite, titanium dioxide powder and active alumina powder.
Further, the binder is silica sol or alumina sol.
Further, the additive is one or more of hydroxyethyl cellulose, hydroxypropyl methylcellulose, polyethylene glycol, polyvinyl alcohol, organic silicon, polyacrylamide, bentonite, sodium hydroxide, oxalic acid, acetic acid and nitric acid.
Further, during the preparation of the extruded honeycomb catalyst carrier, the NO x The mass ratio of the precursor of the selective catalytic reduction active component to the binder to the additive is 1-10:1-20:0-5.
Further, in the process of coating the CO oxidation catalytic active layer, the mass ratio of the precursor of the CO oxidation catalytic active component to the binder to the additive is 1-25:5-20:0-5.
Further, the drying temperature of the extruded honeycomb catalyst carrier is 80-120 ℃ and the drying time is 2-5 hours.
Further, the calcination temperature of the extruded honeycomb catalyst carrier is 400-600 ℃ and the calcination time is 2-5 hours.
Further, the drying temperature of the CO oxidation catalytic active layer is 80-120 ℃ and the drying time is 0.5-1 hour.
Further, the calcination temperature of the CO oxidation catalytic active layer is 350-550 ℃ and the calcination time is 1-3 hours.
When the honeycomb cordierite is used as a carrier, NO is generated x The precursor of the selective catalytic reduction active component and the precursor of the CO oxidation catalytic active component are respectively and uniformly mixed with the binder and then ground (the grinding rotating speed is 600-1000 r/min and the time is 0.5-3 h), the slurry for coating is obtained by adding the additive after the grinding is finished, and the two slurries are respectively coated (NO x The coating amount of the selective catalytic reduction active component is 100g/L, and the coating amount of the CO oxidation catalytic active component is 80 g/L) on different areas of the carrier, and then the corresponding active layer is obtained through drying and calcining. NO (NO) x The coated lengths of the selective catalytic reduction active layer and the CO oxidation catalytic active layer can be modulated according to practical requirements.
Further, the honeycomb cordierite carrier has a pore number of 40-70.
Further, the NO x The precursor of the selective catalytic reduction active component is vanadate, tungstate, or one or more of nitrate, sulfate and acetate of copper, cerium, zirconium and iron, and is combined with one or more of titanium dioxide powder, ZSM-5, MOR, SSZ-13, SAPO-34, SSZ-39 and SAPO-18 molecular sieve powder.
Further, the precursor of the CO oxidation catalytic active component is one or more of chloride, nitrate and sulfate of platinum, palladium, gold, copper, cerium, tin or iron, and is combined with one or more of pseudo-boehmite, titanium dioxide powder and active alumina powder.
Further, the binder is one of silica sol or alumina sol.
Further, the additive is one or more of hydroxyethyl cellulose, hydroxypropyl methylcellulose, sodium hydroxide, oxalic acid, acetic acid, nitric acid, isopropanol and n-propanol.
Further toIn the form of the NO x The mass ratio of the precursor of the selective catalytic reduction active component to the binder to the additive is 1-15:5-20:0-5.
Further, the mass ratio of the precursor of the CO oxidation catalytic active component to the binder to the additive is 1-25:5-20:0-5.
Further, NO x The drying temperature of the selective catalytic reduction active layer is 80-120 ℃ and the drying time is 0.5-1 hour.
Further, NO x The calcination temperature of the selective catalytic reduction active layer is 500-600 ℃ and the calcination time is 1-3 hours.
Further, the drying temperature of the CO oxidation catalytic active layer is 80-120 ℃ and the drying time is 0.5-1 hour.
Further, the calcination temperature of the CO oxidation catalytic active layer is 350-550 ℃ and the calcination time is 1-3 hours.
By adopting the scheme, the invention has the following advantages compared with the prior art:
by having NO x Extrusion type honeycomb catalyst carrier with selective catalytic reduction function is coated with CO oxidation catalytic active layer or NO is coated on cordierite in a segmented way x Selective catalytic reduction active layer and CO oxidation catalytic active layer capable of converting NO x And the CO elimination function is organically combined on one catalyst, so that the front-stage and back-stage catalysis of the same catalyst is realized, the design pressure can be relieved, the occupied area of equipment is reduced, the use cost is greatly reduced, the use amount of the catalyst can be saved, and the catalyst control strategy is simpler and more efficient.
Drawings
FIG. 1 is a graph of CO and NO produced in example 1 using an extruded honeycomb catalyst as a support x Simultaneously processing a structural schematic diagram of the catalyst A;
FIG. 2 is a graph of CO and NO produced in example 2 using honeycomb cordierite as a carrier x Simultaneously processing a structural schematic diagram of the catalyst B;
FIG. 3 is a graph of the performance of catalyst A prepared in example 1 under simulated flue gas conditions;
FIG. 4 is a graph of the performance of catalyst B prepared in example 2 under simulated flue gas conditions.
Detailed Description
The technical scheme of the invention is specifically described below through specific embodiments and with reference to the accompanying drawings. The experimental methods used in the following examples are all conventional methods unless otherwise specified; materials, reagents and the like used, unless otherwise indicated, are all commercially available.
Titanium dioxide powder is provided by DuPont, hydroxypropyl methylcellulose, cationic polyacrylamide, calcium bentonite is provided by Shandong Ruitai chemical industry Co., ltd, acidic silica sol is provided by Qingdao microphone silica gel desiccant Co., ltd, acidic nano aluminum sol is provided by Texas crystal fire technology glass Co., ltd, and ZSM-5 is provided by Nanka university catalyst plant.
Example 1
After adding 30g of ammonium metavanadate, 7.5g of ammonium tungstate and 30g of oxalic acid into 200g of deionized water, the mixture was stirred for half an hour until the solution was mixed uniformly. 500g of titanium dioxide powder, 100g of a 7.5wt% aqueous solution of hydroxypropyl methylcellulose, 100g of a 20wt% acidic silica sol, 30g of cationic polyacrylamide and 30g of calcium bentonite were added to an electric mixer, and stirred (stirring speed: 50r/min, stirring time: 3 h) to a dough state. The stirred solution was then poured into a mixer and stirred for 30 minutes. The stirred dough material was placed in a honeycomb catalyst vacuum extruder and a 30-hole honeycomb extrudate having a length of 9cm and a width and height of 3cm was extruded under a pressure of 10 MPa. The extrudate is dried for 4 hours at the temperature of 100 ℃ in an oven, and then calcined for 4 hours at the temperature of 500 ℃ in a muffle furnace to obtain the final extruded honeycomb catalyst carrier for standby.
30g of cerium nitrate, 20g of copper nitrate, 10g of tin chloride and 100g of 15wt% of acid nano aluminum sol are added into 200g of deionized water, and after stirring for 30 minutes until the mixture is uniform, 300g of titanium dioxide powder is added to form slurry. The slurry was put into a grinder and ground (rotational speed 800r/min, grinding time 2 h) until D90 was 1.2-1.8 μm, and 50g of 7.5wt% aqueous hydroxypropyl methylcellulose was added to the slurry after the grinding was completedAnd 1.5g of chloroplatinic acid to give a coating slurry. The slurry was coated into the channels of the honeycomb catalyst carrier prepared in this example using a coater, and then dried at 100 c hot air for 0.5 hours, followed by calcination at 400 c in a muffle furnace for 3 hours to obtain CO and NO x Catalyst a was treated simultaneously. The loading of the CO catalytic oxidation coating is 80g/L, and the coating length occupies the position from the front end to one half of the length of the carrier (the length direction of the carrier is symmetrically divided into two halves, and one half of the carrier is coated). The structural schematic diagram of the catalyst A is shown in FIG. 1.
Example 2
Honeycomb cordierite with a pore number of 50 and a size of 150 x 500mm was selected as a carrier. To 200g of deionized water, 20g of copper nitrate, 10g of cerium nitrate and 80g of 15wt% acid nano aluminum sol were added, and after stirring for 30 minutes until the mixture was uniform, 200g of ZSM-5 powder was added to form a slurry. The slurry was put in a grinder to grind (rotation speed 1000r/min, grinding time 2 h) until D90 was 1.2-1.8 μm, and 40g of 7.5wt% aqueous hydroxypropyl methylcellulose solution and 0.5g of isopropyl alcohol were added to the slurry after grinding was completed to obtain a coating slurry. The slurry is coated into the pore canal of honeycomb cordierite by a coating machine, then dried for 0.5 hours under 100 ℃ hot air, and then calcined for 3 hours under 550 ℃ in a muffle furnace to obtain NO x A selective catalytic reduction coating. NO (NO) x The loading of the catalytic reduction coating is 100g/L, and the coating length occupies the position from the front end to one half of the length of the carrier (the length direction of the carrier is symmetrically divided into two halves, and one half of the carrier is coated).
A CO catalytic oxidation coating was prepared in the same formulation and method as in example 1, with a loading of 80g/L, and a coating length occupying one half of the length of the support from the rear end (the support being divided into two halves symmetrically in the length direction, the other half being coated) to give CO and NO x Simultaneously treated catalyst B. The schematic structure of the catalyst B is shown in FIG. 2.
FIGS. 1 and 2 are schematic views of the structures of the catalysts prepared in example 1 and example 2, respectively. The main difference between the two catalysts is the different supports of the catalysts. The catalyst of example 1 was in the form of extruded honeycomb NO x Selective catalytic reduction catalystAs carrier, the carrier can eliminate NO in flue gas x The CO catalytic oxidation coating is impregnated in the pore canal by a coating method. Example 2 honeycomb cordierite was used directly as a carrier, which did not have contaminant removal capability. NO by coating method x The selective catalytic reduction coating and the CO catalytic oxidation coating are coated inside the carrier pore canal in a segmented way. Example 1 is more advantageous in terms of cost of the catalyst than example 2 because more expensive cordierite is not used as the carrier.
Example 3
The catalysts a and B prepared in examples 1, 2 were evaluated for their performance in a fixed bed. Test conditions of O 2 Concentration 16% (volume percent), NO concentration 800ppm, NH 3 Concentration 800ppm, CO concentration 5000ppm, CO 2 Concentration 5% (volume percent), H 2 O content 15% (volume percent), SO 2 Concentration of 35ppm, N 2 As a carrier gas, the flow rate was 900ml/min and the reaction temperature was 280 ℃. The length and width Gao Jun of the two catalysts were 9cm, 3cm and 3cm, respectively (catalyst B prepared in example 2 was cut to size before activity testing), and NO was then added x The selective catalytic reduction section is used as the upper end of the catalyst, and is contacted with the flue gas firstly.
From the test results of FIGS. 3 and 4, the two-stage NO prepared according to the present invention x The catalyst for purifying CO simultaneously has good NO x And CO elimination performance in H-containing 2 O and SO 2 During 48 hours of reaction, NO of catalyst a x And CO conversion rates of 91% and 85% respectively, NO of catalyst B x And CO conversion rates of 96% and 90% respectively. The calculation formula is as follows: conversion (CO,%) = (inlet CO concentration-outlet CO concentration)/inlet CO concentration 100%, conversion (NO x ,%) = (inlet NO concentration-outlet NO concentration)/inlet NO concentration x 100%. Catalyst B shows performance advantages mainly due to NO x The selective reduction catalytic coating adopts a molecular sieve catalyst with better activity, and the number of pores of the carrier is larger, and the loading capacity of the catalytic coating is higher under the same carrier volume.
Claims (10)
1. Simultaneously purifying CO and NO x Wherein the catalyst is an extruded honeycomb catalyst or honeycomb cordierite as a carrier;
the surface of the carrier is divided into two parts, namely NO x A selective catalytic reduction active layer and a CO oxidation catalytic active layer.
2. A method of preparing the catalyst of claim 1, comprising the steps of:
(1) When the catalyst takes an extrusion type honeycomb catalyst as a carrier, NO is firstly added into the catalyst x The preparation method comprises the steps of mixing and stirring a precursor of a selective catalytic reduction active component, a binder and an additive uniformly, extruding the mixture through an extruder, and drying and calcining the extrudate to obtain an extruded honeycomb catalyst carrier; after the preparation of the extrusion type honeycomb catalyst carrier is finished, uniformly mixing a precursor of a CO oxidation catalytic active component with a binder, grinding, adding an additive after finishing grinding to obtain slurry for coating, coating the slurry on a part of the area of the honeycomb catalyst carrier by using a coating machine, and drying and calcining to obtain a CO oxidation catalytic active layer;
(2) When the catalyst takes honeycomb cordierite as a carrier, NO is added x The preparation method comprises the steps of uniformly mixing a selective catalytic reduction active component precursor and a CO oxidation catalytic active component precursor with a binder, grinding, adding an additive to obtain slurry for coating, respectively coating the two slurries on different areas of a carrier by using a coating machine, and drying and calcining to obtain a corresponding active layer.
3. The method of claim 2, wherein the extruded honeycomb catalyst support has a pore number of 25 to 50 and the honeycomb cordierite support has a pore number of 40 to 70.
4. The method of claim 2, wherein NO x The precursor of the selective catalytic reduction active component is vanadate, tungstate or copperOne or more of nitrate, sulfate and acetate of cerium, zirconium and iron, and one or more of titanium dioxide powder, ZSM-5, MOR, SSZ-13, SAPO-34, SSZ-39 and SAPO-18 molecular sieve powder;
the precursor of the CO oxidation catalytic active component is one or more of chloride, nitrate and sulfate of platinum, palladium, gold, copper, cerium, tin or iron, and is combined with one or more of pseudo-boehmite, titanium dioxide powder and active alumina powder.
5. The method according to claim 2, 3 or 4, wherein the binder is silica sol or alumina sol;
the additive in the mode (1) is one or more of hydroxyethyl cellulose, hydroxypropyl methyl cellulose, polyethylene glycol, polyvinyl alcohol, organic silicon, polyacrylamide, bentonite, sodium hydroxide, oxalic acid, acetic acid and nitric acid;
the additive in the mode (2) is one or more of hydroxyethyl cellulose, hydroxypropyl methyl cellulose, sodium hydroxide, oxalic acid, acetic acid, nitric acid, isopropanol and n-propanol.
6. The method according to claim 2, 3 or 4, wherein during the preparation of the extruded honeycomb catalyst support according to mode (1), the NO x The mass ratio of the precursor of the selective catalytic reduction active component to the binder and the additive is 1-10:1-20:0-5, and in the CO oxidation catalytic active layer coating process of the mode (1), the mass ratio of the precursor of the CO oxidation catalytic active component to the binder and the additive is 1-25:5-20:0-5;
in the mode (2), the NO x The mass ratio of the precursor of the selective catalytic reduction active component to the binder and the additive is 1-15:5-20:0-5, and the mass ratio of the precursor of the CO oxidation catalytic active component to the binder and the additive is 1-25:5-20:0-5.
7. The production method according to claim 2, 3 or 4, wherein the drying temperature of the extruded honeycomb catalyst carrier in the mode (1) is 80 to 120 ℃, the drying time is 2 to 5 hours, the calcining temperature is 400 to 600 ℃, the calcining time is 2 to 5 hours, the drying temperature of the CO oxidation catalyst active layer is 80 to 120 ℃, the drying time is 0.5 to 1 hour, the calcining temperature is 350 to 550 ℃, and the calcining time is 1 to 3 hours;
the NO described in the mode (2) x The drying temperature of the selective catalytic reduction active layer is 80-120 ℃, the drying time is 0.5-1 hour, the calcining temperature is 500-600 ℃, the calcining time is 1-3 hours, the drying temperature of the CO oxidation catalytic active layer is 80-120 ℃, the drying time is 0.5-1 hour, the calcining temperature is 350-550 ℃, and the calcining time is 1-3 hours.
8. The method according to claim 2, 3 or 4, wherein the grinding speed is 600-1000 r/min and the time is 0.5-3 h during the grinding process for preparing the slurry.
9. The production method according to claim 2, 3 or 4, wherein in the mode (1), the CO oxidation catalyst active layer is coated in an amount of 60 to 180g/L, and the coating length occupies 1/3 to 2/3 of the carrier;
in the mode (2), NO x The coating amount of the selective catalytic reduction active layer was 100g/L, and the coating amount of the CO oxidation catalytic active layer was 80g/L.
10. Use of the catalyst of claim 1 or the catalyst prepared according to the preparation method of any one of claims 2-9 for simultaneous purification of carbon monoxide and nitrogen oxides in sintering flue gas.
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| CN117504857A (en) * | 2023-10-30 | 2024-02-06 | 浙江德创环保科技股份有限公司 | Preparation method of catalyst suitable for CO catalytic combustion treatment of steel sintering flue gas |
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| US5120695A (en) * | 1989-07-28 | 1992-06-09 | Degusaa Aktiengesellschaft (Degussa Ag) | Catalyst for purifying exhaust gases from internal combustion engines and gas turbines operated at above the stoichiometric ratio |
| CN104759281A (en) * | 2015-03-11 | 2015-07-08 | 江苏大学 | Preparation method of composite oxide catalyst used for purifying diesel engine |
| CN109261220A (en) * | 2018-09-28 | 2019-01-25 | 昆明贵研催化剂有限责任公司 | A kind of preparation method and application of non-homogeneous coating tai-gas clean-up catalyst |
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| US5120695A (en) * | 1989-07-28 | 1992-06-09 | Degusaa Aktiengesellschaft (Degussa Ag) | Catalyst for purifying exhaust gases from internal combustion engines and gas turbines operated at above the stoichiometric ratio |
| CN104759281A (en) * | 2015-03-11 | 2015-07-08 | 江苏大学 | Preparation method of composite oxide catalyst used for purifying diesel engine |
| CN109261220A (en) * | 2018-09-28 | 2019-01-25 | 昆明贵研催化剂有限责任公司 | A kind of preparation method and application of non-homogeneous coating tai-gas clean-up catalyst |
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| CN117504857A (en) * | 2023-10-30 | 2024-02-06 | 浙江德创环保科技股份有限公司 | Preparation method of catalyst suitable for CO catalytic combustion treatment of steel sintering flue gas |
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