DE10132441A1 - Mixed oxide catalysts and their use for catalytic combustion - Google Patents
Mixed oxide catalysts and their use for catalytic combustionInfo
- Publication number
- DE10132441A1 DE10132441A1 DE2001132441 DE10132441A DE10132441A1 DE 10132441 A1 DE10132441 A1 DE 10132441A1 DE 2001132441 DE2001132441 DE 2001132441 DE 10132441 A DE10132441 A DE 10132441A DE 10132441 A1 DE10132441 A1 DE 10132441A1
- Authority
- DE
- Germany
- Prior art keywords
- mol
- catalysts
- metals
- oxide
- aluminum
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- 239000003054 catalyst Substances 0.000 title claims abstract description 34
- 238000007084 catalytic combustion reaction Methods 0.000 title claims description 7
- 229910052751 metal Inorganic materials 0.000 claims abstract description 13
- 239000002184 metal Substances 0.000 claims abstract description 13
- 238000000034 method Methods 0.000 claims abstract description 9
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims abstract description 6
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229910001928 zirconium oxide Inorganic materials 0.000 claims abstract description 6
- 229910052782 aluminium Inorganic materials 0.000 claims description 11
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 10
- 229910052748 manganese Inorganic materials 0.000 claims description 10
- 229910052697 platinum Inorganic materials 0.000 claims description 10
- 150000002739 metals Chemical class 0.000 claims description 9
- 238000006243 chemical reaction Methods 0.000 claims description 8
- 229910052745 lead Inorganic materials 0.000 claims description 8
- 229910052720 vanadium Inorganic materials 0.000 claims description 8
- 229910052727 yttrium Inorganic materials 0.000 claims description 8
- 229910052684 Cerium Inorganic materials 0.000 claims description 7
- 238000002485 combustion reaction Methods 0.000 claims description 7
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims description 6
- 229910052763 palladium Inorganic materials 0.000 claims description 5
- 238000002360 preparation method Methods 0.000 claims description 5
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 4
- 150000003755 zirconium compounds Chemical class 0.000 claims description 4
- 150000004703 alkoxides Chemical class 0.000 claims description 3
- 150000007942 carboxylates Chemical class 0.000 claims description 3
- 229910052741 iridium Inorganic materials 0.000 claims description 3
- 229910052703 rhodium Inorganic materials 0.000 claims description 3
- 229910052707 ruthenium Inorganic materials 0.000 claims description 3
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 2
- 125000005595 acetylacetonate group Chemical group 0.000 claims description 2
- 239000000446 fuel Substances 0.000 claims description 2
- 150000003839 salts Chemical class 0.000 claims description 2
- 239000002253 acid Substances 0.000 claims 1
- 238000003915 air pollution Methods 0.000 claims 1
- 230000005611 electricity Effects 0.000 claims 1
- 239000003960 organic solvent Substances 0.000 claims 1
- 229930195733 hydrocarbon Natural products 0.000 abstract description 5
- 150000002430 hydrocarbons Chemical class 0.000 abstract description 5
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 2
- 239000001301 oxygen Substances 0.000 abstract description 2
- 229910052760 oxygen Inorganic materials 0.000 abstract description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 34
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Substances [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 22
- 239000007789 gas Substances 0.000 description 9
- 239000000203 mixture Substances 0.000 description 7
- 229910052726 zirconium Inorganic materials 0.000 description 5
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 4
- 239000001273 butane Substances 0.000 description 4
- IJDNQMDRQITEOD-UHFFFAOYSA-N n-butane Chemical compound CCCC IJDNQMDRQITEOD-UHFFFAOYSA-N 0.000 description 4
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 4
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 3
- 230000003647 oxidation Effects 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- 229910052783 alkali metal Inorganic materials 0.000 description 2
- 150000001340 alkali metals Chemical class 0.000 description 2
- 238000004140 cleaning Methods 0.000 description 2
- SWXVUIWOUIDPGS-UHFFFAOYSA-N diacetone alcohol Chemical compound CC(=O)CC(C)(C)O SWXVUIWOUIDPGS-UHFFFAOYSA-N 0.000 description 2
- 229910052737 gold Inorganic materials 0.000 description 2
- 229960005235 piperonyl butoxide Drugs 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 229910052761 rare earth metal Inorganic materials 0.000 description 2
- 239000006104 solid solution Substances 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- POILWHVDKZOXJZ-ARJAWSKDSA-M (z)-4-oxopent-2-en-2-olate Chemical compound C\C([O-])=C\C(C)=O POILWHVDKZOXJZ-ARJAWSKDSA-M 0.000 description 1
- 229910018131 Al-Mn Inorganic materials 0.000 description 1
- 229910018125 Al-Si Inorganic materials 0.000 description 1
- 229910018461 Al—Mn Inorganic materials 0.000 description 1
- 229910018520 Al—Si Inorganic materials 0.000 description 1
- 229910018580 Al—Zr Inorganic materials 0.000 description 1
- FIPWRIJSWJWJAI-UHFFFAOYSA-N Butyl carbitol 6-propylpiperonyl ether Chemical compound C1=C(CCC)C(COCCOCCOCCCC)=CC2=C1OCO2 FIPWRIJSWJWJAI-UHFFFAOYSA-N 0.000 description 1
- 229910018921 CoO 3 Inorganic materials 0.000 description 1
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical class [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 description 1
- 241000196324 Embryophyta Species 0.000 description 1
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 1
- 229910002845 Pt–Ni Inorganic materials 0.000 description 1
- 229910018879 Pt—Pd Inorganic materials 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 229910006404 SnO 2 Inorganic materials 0.000 description 1
- 238000003917 TEM image Methods 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- GEIAQOFPUVMAGM-UHFFFAOYSA-N ZrO Inorganic materials [Zr]=O GEIAQOFPUVMAGM-UHFFFAOYSA-N 0.000 description 1
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- 150000001342 alkaline earth metals Chemical class 0.000 description 1
- 239000004411 aluminium Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 229910021472 group 8 element Inorganic materials 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 229910052747 lanthanoid Inorganic materials 0.000 description 1
- 150000002602 lanthanoids Chemical class 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- CLSUSRZJUQMOHH-UHFFFAOYSA-L platinum dichloride Chemical compound Cl[Pt]Cl CLSUSRZJUQMOHH-UHFFFAOYSA-L 0.000 description 1
- 239000002574 poison Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- XPGAWFIWCWKDDL-UHFFFAOYSA-N propan-1-olate;zirconium(4+) Chemical compound [Zr+4].CCC[O-].CCC[O-].CCC[O-].CCC[O-] XPGAWFIWCWKDDL-UHFFFAOYSA-N 0.000 description 1
- OGHBATFHNDZKSO-UHFFFAOYSA-N propan-2-olate Chemical compound CC(C)[O-] OGHBATFHNDZKSO-UHFFFAOYSA-N 0.000 description 1
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 1
- 150000002910 rare earth metals Chemical class 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 238000003980 solgel method Methods 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- WOZZOSDBXABUFO-UHFFFAOYSA-N tri(butan-2-yloxy)alumane Chemical compound [Al+3].CCC(C)[O-].CCC(C)[O-].CCC(C)[O-] WOZZOSDBXABUFO-UHFFFAOYSA-N 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
Classifications
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23G—CREMATION FURNACES; CONSUMING WASTE PRODUCTS BY COMBUSTION
- F23G7/00—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals
- F23G7/06—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases
- F23G7/07—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases in which combustion takes place in the presence of catalytic material
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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
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
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- 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
- B01J21/06—Silicon, titanium, zirconium or hafnium; Oxides or hydroxides thereof
- B01J21/066—Zirconium or hafnium; 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/10—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of rare earths
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- 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
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
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- 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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
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- 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
- B01J23/74—Iron group metals
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- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/03—Precipitation; Co-precipitation
- B01J37/031—Precipitation
- B01J37/033—Using Hydrolysis
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- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/03—Precipitation; Co-precipitation
- B01J37/036—Precipitation; Co-precipitation to form a gel or a cogel
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23C—METHODS OR APPARATUS FOR COMBUSTION USING FLUID FUEL OR SOLID FUEL SUSPENDED IN A CARRIER GAS OR AIR
- F23C13/00—Apparatus in which combustion takes place in the presence of catalytic material
- F23C13/08—Apparatus in which combustion takes place in the presence of catalytic material characterised by the catalytic material
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- 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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/42—Platinum
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- 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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/46—Ruthenium, rhodium, osmium or iridium
- B01J23/464—Rhodium
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- 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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/56—Platinum group metals
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Environmental & Geological Engineering (AREA)
- General Engineering & Computer Science (AREA)
- Mechanical Engineering (AREA)
- Dispersion Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Combustion & Propulsion (AREA)
- Catalysts (AREA)
Abstract
Description
Die Erfindung betrifft Mischoxid-Katalysatoren aus Aluminium- und Zirkonoxid und einem Element der Gruppe VIII oder den Elementen Mn, Y, V, Pb, Ce sowie Verfahren zu ihrer Hestellung. Solche Katalysatoren eignen sich zur katalytischen Verbrennung von Kohlenwasserstoffen und CO mit Luft oder Sauerstoff. The invention relates to mixed oxide catalysts made of aluminum and zirconium oxide and an element from group VIII or the elements Mn, Y, V, Pb, Ce and Process for their preparation. Such catalysts are suitable for catalytic Combustion of hydrocarbons and CO with air or oxygen.
Mögliche Einsatzgebiete sind die katalytische Verbrennung zur Abgasreinigung in Kraftwerken und Industrieanlagen, die katalytische Verbrennung von Kraftstoffen (Erdgas, Erdöl) für die Energiegewinnung in Kraftwerken bei hohen Temperaturen, die Reinigung von Küchenluft in Backöfen und über Kochstellen, die Geruchsentfernung aus Innenluft und der Einsatz als Sensoren von zu verbrennenden Stoffen, wie Methan, Kohlenwasserstoffen oder CO. Insbesondere bei den letzteren Beispielen sind niedrige Betriebstemperaturen, hohe Temperatur- und Langzeitstabilität sowie Vergiftungsfestigkeit wesentlich. Possible areas of application are catalytic combustion for exhaust gas cleaning in Power plants and industrial plants, the catalytic combustion of fuels (Natural gas, petroleum) for energy generation in power plants at high Temperatures, the cleaning of kitchen air in ovens and over hobs, odor removal from indoor air and use as sensors from burning substances such as methane, hydrocarbons or CO. In particular in the latter examples, low operating temperatures, high temperature and long-term stability as well as poison resistance.
In der Vergangenheit wurden bereits unterschiedlichste Katalysatoren für diese Anwendungen erprobt und patentiert, wobei in allen Fällen die Verbrennung von Methan Temperaturen über 450°C erfordert, so z. B. ein temperaturstabiles Substrat, auf dem sich ein mit Pd getränktes Mischoxid aus Al2O3, SiO2, TiO2, ZrO2 sowie ein Seltenerdoxid befindet (JP 09262472); Oxide der Form AB1-xCxO3 (wobei A = Seltenerdmetalle oder Alkalimetalle, B = Mn, Co, oder Cr; C = Nb oder Ta, 0,1 < x < 1) (JP 08012334); ein mit In beladener ZSM 5 (JP 06262039); ein mit Co, Mg, Rh, Pd und Pt geträgerter Zeolith vom Mordanit-Typ (JP 5115751); ein Mischoxid aus MgO, Kupferoxiden und Metallen der Pt- Gruppe (JP 03238048); ein Katalysator, der sowohl Pd als auch Al-Mn-Mischoxid enthält (JP 01139911, JP 08020054); ein temperaturstabiler Träger, der mit Al-Si- Mischoxiden beschichtet ist und Pd und/oder PdO als Aktivkomponente enthält (JP 63175638, JP 08008992); ein kombiniertes System aus 1. einem Pd-Pt-Ni- Oxid als Aktivkomponente und 2. Pt oder Pt-Pd als Aktivkomponente auf einem monolitischen Aluminiumoxidträger (JP 63080849, JP 05045295). Des weiteren werden verschiedene Perowskite beschrieben, zum einen vom Typ A1-xA1xM1-yM1yO3 (es bedeuten: A = Seltenerdelement; A1 = Ag, Au; M = M1 = Übergangsmetall; x, y = 0-0,9) (JP 61011149, JP 05043416) und zum anderen vom Typ La1-xCexCoO3 (x = 0-0,2). Im Patent BO 096A000063 werden Katalysatoren des Typs A2B3O6±d beschrieben, wobei A ein Erdalkali-, ein Alkalimetall, ein Lanthanoid oder eine feste Lösung von ihnen, B ein Übergangsmetall, ein Element der Gruppe III oder eine feste Lösung von ihnen ist. Der Wert für d liegt zwischen 0 und 1. Mit diesen Katalysatoren ist die Verbrennung von Methan ab einer Temperatur von 450°C möglich. Umsätze über 50% bei der Niedertemperaturverbrennung von Methan werden mit Mn, Fe oder Co-stabilisierten ZrO2 erst bei Temperaturen über 450°C beobachtet (V. S. Choudhary, B. S. Uphade, S. G. Pataskar, A. Keshavaraja, Angew. Chem. 108 (1996) 2538). 50% Methan-Verbrennung wurde mit Pd/Al2O3-Katalyatoren bereits bei 300°C beobachtet (D. ROth, P. Gélin, M. Primet, E. Tena, Appl. Catal. A, General 203 (2000) 37). Mit Ce-stabilisierten Pd/Al2O3-Katalysatoren benötigt die Methan-Verbrennung immer noch Temperaturen über 350°C (G. Groppi, C. Cristiani, L. Lietti, C. Ramella, M. Valentini, P. Forzatti, Catalysis Today, 50 (1999) 399). Ähnliche Temperaturen werden auch für die katalytische Niedertemperatur-Methanverbrennung mit Pd/SnO2-Katalysatoren benötigt (K. Sekizawa, H. Widjaja, S. Maeda, Y. Ozawa, K. Eguchi, Appl. Catal. A, General 200 (2000) 211). Baerns und Mitarbeiter berichteten kürzlich, dass es bisher keine Katalysatoren gibt, die Kohlenwasserstoffe bereits bei Temperaturen unter 150°C katalytisch verbrennen (U. Rodemerck, D. Wolf, O. V. Buyeskaya, P. Claus, S. Senkan, M. Baerns, Chem. Eng. J. 82 (2001) 3). In the past, a wide variety of catalysts for these applications have already been tested and patented. In all cases, the combustion of methane requires temperatures above 450 ° C. B. a temperature-stable substrate on which there is a mixed oxide impregnated with Pd made of Al 2 O 3 , SiO 2 , TiO 2 , ZrO 2 and a rare earth oxide (JP 09262472); Oxides of the form AB 1-x C x O 3 (where A = rare earth metals or alkali metals, B = Mn, Co, or Cr; C = Nb or Ta, 0.1 <x <1) (JP 08012334); a ZSM 5 loaded with In (JP 06262039); a mordanite-type zeolite supported with Co, Mg, Rh, Pd and Pt (JP 5115751); a mixed oxide of MgO, copper oxides and metals of the Pt group (JP 03238048); a catalyst containing both Pd and Al-Mn mixed oxide (JP 01139911, JP 08020054); a temperature-stable carrier which is coated with Al-Si mixed oxides and contains Pd and / or PdO as active component (JP 63175638, JP 08008992); a combined system of 1. a Pd-Pt-Ni oxide as an active component and 2. Pt or Pt-Pd as an active component on a monolithic aluminum oxide support (JP 63080849, JP 05045295). Furthermore, various perovskites are described, on the one hand of the type A 1-x A1 x M 1-y M1 y O 3 (meaning: A = rare earth element; A1 = Ag, Au; M = M1 = transition metal; x, y = 0 -0.9) (JP 61011149, JP 05043416) and secondly of the type La 1-x Ce x CoO 3 (x = 0-0.2). Patent BO 096A000063 describes catalysts of the type A 2 B 3 O 6 ± d , where A is an alkaline earth metal, an alkali metal, a lanthanoid or a solid solution thereof, B is a transition metal, an element of group III or a solid solution of them is. The value for d is between 0 and 1. With these catalysts, the combustion of methane is possible from a temperature of 450 ° C. Sales of more than 50% in the low-temperature combustion of methane are only observed with Mn, Fe or Co-stabilized ZrO 2 at temperatures above 450 ° C (VS Choudhary, BS Uphade, SG Pataskar, A. Keshavaraja, Angew. Chem. 108 (1996) 2538). 50% methane combustion was already observed with Pd / Al 2 O 3 catalysts at 300 ° C (D. ROth, P. Gélin, M. Primet, E. Tena, Appl. Catal. A, General 203 (2000) 37 ). With Ce-stabilized Pd / Al 2 O 3 catalysts, methane combustion still requires temperatures above 350 ° C (G. Groppi, C. Cristiani, L. Lietti, C. Ramella, M. Valentini, P. Forzatti, Catalysis Today, 50 (1999) 399). Similar temperatures are also required for catalytic low-temperature methane combustion with Pd / SnO 2 catalysts (K. Sekizawa, H. Widjaja, S. Maeda, Y. Ozawa, K. Eguchi, Appl. Catal. A, General 200 (2000) 211). Baerns and co-workers recently reported that to date there have been no catalysts that catalytically burn hydrocarbons at temperatures below 150 ° C (U. Rodemerck, D. Wolf, OV Buyeskaya, P. Claus, S. Senkan, M. Baerns, Chem. Eng. J. 82 (2001) 3).
Wir haben nun überraschenderweise gefunden, dass Katalysatoren, die Mischoxide aus 60 bis 90 Mol-% Aluminiumoxid und 10 bis 40 Mol-% Zirkonoxid und zu maximal 10 Mol-% ein oder mehrere Metalle, ausgewählt aus den Elementen der Gruppe VIII und den Elementen Mn, Y, V, Pb, Ce, enthalten, die katalytische Verbrennung von CO, Methan und anderen Kohlenwasserstoffen bei Temperaturen zwischen Raumtemperatur und 250°C katalysieren. We have now surprisingly found that catalysts that Mixed oxides of 60 to 90 mol% aluminum oxide and 10 to 40 mol% zirconium oxide and a maximum of 10 mol% of one or more metals selected from the Group VIII elements and elements Mn, Y, V, Pb, Ce, contain the catalytic combustion of CO, methane and other hydrocarbons Catalyze temperatures between room temperature and 250 ° C.
Ein erfindungsgemäßer Katalysator umfasst also
- a) einen oxidischen Träger, bestehend aus einem Aluminium/Zirkonium- Mischoxid, der beispielsweise poröse, inerte, feste, widerstandsfähige, amorphe oder kristalline Struktur aufweisen kann, und
- b) ein oder mehrere Elemente, ausgewählt aus der VIII. Gruppe und den Elementen Mn, Y, V, Pb, Ce.
- a) an oxidic carrier consisting of an aluminum / zirconium mixed oxide, which can have, for example, porous, inert, solid, resistant, amorphous or crystalline structure, and
- b) one or more elements selected from the VIII. Group and the elements Mn, Y, V, Pb, Ce.
Als Metalle der Gruppe VIII kommen Pt, Pd, Rh, Ir, Ru, und Au in Frage. Ein erfindungsgemäßer Katalysator ist z. B. ein Pt-haltiges Al-Zr-Mischoxid, enthaltend 1 bis 3 Mol-% Pt, 15 bis 30 Mol-% Zr-oxid und 70 bis 85 Mol-% Al- oxid, womit die katalytische Verbrennung ab 60°C möglich ist. Group VIII metals include Pt, Pd, Rh, Ir, Ru, and Au. On inventive catalyst is, for. B. a Pt-containing Al-Zr mixed oxide, containing 1 to 3 mol% Pt, 15 to 30 mol% Zr oxide and 70 to 85 mol% Al oxide, which enables catalytic combustion from 60 ° C.
Für Hochtemperaturanwendungen erwiesen sich insbesondere die Elemente Fe, Mn, Y, V, und Pb als geeignet. For high temperature applications, the elements Fe, Mn, Y, V, and Pb as suitable.
Die erfindungsgemäßen Katalysatoren können mit unterschiedlichen Methoden
hergestellt werden:
- 1. durch Imprägnieren des Mischoxids mit einem oder mehreren Elementen entsprechend der Aufzählung unter (b);
- 2. über eine Sol-Gel-Methode, bei der aus einer organischen Lösung von
Metallsalzen von Metallen entsprechend der Aufzählung unter (b) mit
Aluminium- und Zirkonverbindungen unter Zusatz von Wasser und eines
Reaktionsbeschleunigers ein Gel gebildet wird, das anschließend kalziniert
wird. Als Aluminium- und Zirkonverbindungen eignen sich vor allem die
Alkoxide, Carboxylate, Acetylacetonate und Dioalte, vorzugsweise die n-
und iso-propoxide und -butoxide. Die Kalzinierung erfolgt beispielweise
über ein Temperaturprogramm:
kalziniert wird.
- 1. by impregnating the mixed oxide with one or more elements in accordance with the list under (b);
- 2. Using a sol-gel method in which a gel is formed from an organic solution of metal salts of metals according to the list under (b) with aluminum and zirconium compounds with the addition of water and a reaction accelerator, which is then calcined. Particularly suitable as aluminum and zirconium compounds are the alkoxides, carboxylates, acetylacetonates and dioalts, preferably the n- and iso-propoxides and butoxide. The calcination is carried out, for example, using a temperature program:
is calcined.
Die Komponente(n) entsprechend der Aufzählung unter (b) liegen zweckmäßigerweise in einer Gesamtkonzentration von 0,1-10 Mol-Prozent vor. Component (s) are listed under (b) expediently in a total concentration of 0.1-10 mol percent.
80 mg Platin(II)chlorid (0,3 mmol) wurden in 50 ml (0,65 mol) Isopropanol
gelöst, anschließend wurden 3,7 ml (30 mmol) 4-Hydroxy-4-methyl-2-pentanon,
0,62 ml (2,2 mmol) Zirkon-n-propoxid, 1,98 ml (7,2 mmol) Aluminium-sec-
butoxid, sowie 0,18 ml (10 mmol) dest. Wasser und 21,6 µl (0,6 mmol)
konzentrierte Salzsäure zugegeben. Die erhaltene Lösung wurde bis zum Gelieren
gerührt und das erhaltene Gel anschließend über die
Temperaturrampe:
kalziniert.
80 mg of platinum (II) chloride (0.3 mmol) were dissolved in 50 ml (0.65 mol) of isopropanol, then 3.7 ml (30 mmol) of 4-hydroxy-4-methyl-2-pentanone, 0, 62 ml (2.2 mmol) of zirconium n-propoxide, 1.98 ml (7.2 mmol) of aluminum sec-butoxide, and 0.18 ml (10 mmol) of dist. Water and 21.6 µl (0.6 mmol) concentrated hydrochloric acid were added. The solution obtained was stirred until it gelled, and the gel obtained then on the temperature ramp:
calcined.
Man erhielt somit einen Katalysator der ungefähren Zusammensetzung Pt3Zr20Al77O158,5. A catalyst with the approximate composition Pt 3 Zr 20 Al 77 O 158.5 was thus obtained.
Der Platingehalt des erfindungsgemäßen Katalysators beträgt etwa 3 Mol-Prozent, die Oberfläche beträgt 146 m2/g. Das Material weist eine mesoporöse Struktur auf, am häufigsten findet man Poren der Größe 4,62 nm, 88% der Poren weisen eine Größe zwischen 2 und 8 nm auf. TEM-Aufnahmen zeigen, dass das Platin in überwiegend 5-50 nm großen, kristallinen Domänen vorliegt. Bei EDX-Analysen dieser Domänen findet man neben Pt auch Aluminium, jedoch kein Zirkonium. Die Matrix aus Zirkonium und Aluminium ist weitgehend amorph, Platin findet man bei diesen EDX-Analysen überall in Spuren, was auf atomare Verteilung hinweist. Das Zirkonium zu Aluminium-Verhältnis zeigt eine gute Übereinstimmung mit dem theoretischen Wert. The platinum content of the catalyst according to the invention is about 3 mol percent, the surface is 146 m 2 / g. The material has a mesoporous structure, the most common are pores of 4.62 nm in size, 88% of the pores are between 2 and 8 nm in size. TEM images show that the platinum is present in predominantly 5-50 nm large, crystalline domains. In EDX analyzes of these domains, aluminum is found in addition to Pt, but no zirconium. The matrix of zirconium and aluminum is largely amorphous, platinum can be found everywhere in these EDX analyzes, which indicates atomic distribution. The zirconium to aluminum ratio shows a good agreement with the theoretical value.
100 mg des oben beschriebenen Pt-Katalysators, der zuvor 15 min in einer
Kugelmühle gemahlen wurde, wurden in einen Gasphasenreaktor eingebracht und
mit einem Gemisch aus Methan und synthetischer Luft durchströmt. Es wurden
folgende Parameter verwendet: 40 ml/min Methan und 26 ml/min synthetische
Luft. Die nachfolgende Tabelle gibt den CO2-Gehalt des Produktgasstroms sowie
die O2-Umsätze (als Indikator für die Methanumsätze) bei den verschiedenen
Temperaturen an.
100 mg of the Pt catalyst described above, which had previously been ground in a ball mill for 15 minutes, were introduced into a gas phase reactor and a mixture of methane and synthetic air was passed through. The following parameters were used: 40 ml / min methane and 26 ml / min synthetic air. The following table shows the CO 2 content of the product gas flow and the O 2 conversions (as an indicator for the methane conversions) at the different temperatures.
100 mg eines erfindungsgemäßen Pt-Katalysators der ungefähren
Zusammensetzung Pt6Zr20Al73O149,5 (Synthese analog zum oben beschriebenen
Pt-Katalysator), der zuvor 15 min in einer Kugelmühle gemahlen wurde, wurden
in einen Gasphasenreaktor eingebracht und mit einem Gemisch aus Methan und
synthetischer Luft durchströmt. Es wurden folgende Parameter verwendet: 40
ml/min Methan und 26 ml/min synthetische Luft. Die nachfolgende Tabelle gibt
den CO2-Gehalt des Produktgasstroms sowie die O2-Umsätze bei den
verschiedenen Temperaturen an.
100 mg of a Pt catalyst according to the invention of the approximate composition Pt 6 Zr 20 Al 73 O 149.5 (synthesis analogous to the Pt catalyst described above), which had previously been ground in a ball mill for 15 minutes, were introduced into a gas phase reactor and mixed made of methane and synthetic air. The following parameters were used: 40 ml / min methane and 26 ml / min synthetic air. The following table shows the CO 2 content of the product gas flow and the O 2 conversions at the different temperatures.
100 mg des Pt-Katalysators aus Beispiel 1, der zuvor 15 min in einer Kugelmühle
gemahlen wurde, wurden in einen Gasphasenreaktor eingebracht und mit einem
Gemisch aus Butan und synthetischer Luft durchströmt. Es wurden folgende
Parameter verwendet: 1 ml/min Butan und 99 ml/min synthetische Luft. Die
nachfolgende Tabelle gibt den CO2-Gehalt des Produktgasstroms sowie die
Butan-Umsätze bei den verschiedenen Temperaturen an.
100 mg of the Pt catalyst from Example 1, which had previously been ground in a ball mill for 15 minutes, were introduced into a gas phase reactor and a mixture of butane and synthetic air was passed through. The following parameters were used: 1 ml / min butane and 99 ml / min synthetic air. The table below shows the CO 2 content of the product gas flow and the butane conversions at the different temperatures.
Analog Beispiel 4 wurde ein Gemisch aus CO und Luft (1 : 100, 100 ml/min) bei unterschiedlichen Temperaturen über den Katalysator (100 mg) geleitet. Die Zusammensetzung des Produktgases wurde mit Sensoren (O2, CO, CO2) kontinuierlich analysiert. Bei Temperaturen ab 150°C wurde quantitativer Umsatz erzielt. Analogously to Example 4, a mixture of CO and air (1: 100, 100 ml / min) was passed over the catalyst (100 mg) at different temperatures. The composition of the product gas was continuously analyzed with sensors (O 2 , CO, CO 2 ). Quantitative conversion was achieved at temperatures above 150 ° C.
100 mg des mit 6 Mol-% M dotierten Katalysators (Herstellung analog Beispiel 1)
wurden in einem Gasphasenreaktor eingebracht und mit einem Gemisch aus
Methan und synthetischer Luft durchströmt (40 ml/min Methan, 26 ml/min
synthetische Luft) bei einer Temperatur von 800°C verbrannt. Während der
Umsatz anfänglich schwach abfiel, war er danach über 24 h konstant. Es ergaben
sich folgende Umsätze:
100 mg of the catalyst doped with 6 mol% M (preparation analogous to Example 1) were introduced into a gas phase reactor and a mixture of methane and synthetic air was passed through (40 ml / min methane, 26 ml / min synthetic air) at a temperature of 800 ° C burned. While sales initially fell slightly, they remained constant over 24 hours. The following sales resulted:
Claims (11)
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DE2001132441 DE10132441A1 (en) | 2001-07-04 | 2001-07-04 | Mixed oxide catalysts and their use for catalytic combustion |
PCT/EP2002/007361 WO2003004152A2 (en) | 2001-07-04 | 2002-07-03 | Mixed oxide catalysts based on zr02.al203 and their use for catalytic combustion |
AU2002345082A AU2002345082A1 (en) | 2001-07-04 | 2002-07-03 | Mixed oxide catalysts based on zr02.al203 and their use for catalytic combustion |
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DE2001132441 DE10132441A1 (en) | 2001-07-04 | 2001-07-04 | Mixed oxide catalysts and their use for catalytic combustion |
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Cited By (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2005123594A2 (en) | 2004-06-21 | 2005-12-29 | Johnson Matthey Public Limited Company | Sols comprising mixed transitional metal oxide nanoparticles |
WO2006077256A1 (en) * | 2005-01-24 | 2006-07-27 | Cinvention Ag | Metal containing composite materials |
US7780875B2 (en) | 2005-01-13 | 2010-08-24 | Cinvention Ag | Composite materials containing carbon nanoparticles |
US9126192B2 (en) | 2004-06-21 | 2015-09-08 | Johnson Matthey Public Limited Company | Platinum group metal oxide sols |
Families Citing this family (1)
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CN108435163A (en) * | 2018-02-10 | 2018-08-24 | 普利飞尔环保科技(上海)有限公司 | One kind is for VOCs waste gas catalytic combustion Pd base monolithic catalysts and preparation method thereof |
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DE69324201T2 (en) * | 1992-08-31 | 1999-11-25 | Norton Chemical Process Products Corp., Stow | Catalyst carrier |
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JPH04330940A (en) * | 1991-05-01 | 1992-11-18 | Mitsubishi Heavy Ind Ltd | Oxidation catalyst |
JPH06319995A (en) * | 1993-05-07 | 1994-11-22 | Mitsubishi Heavy Ind Ltd | Oxidation catalyst |
-
2001
- 2001-07-04 DE DE2001132441 patent/DE10132441A1/en not_active Withdrawn
-
2002
- 2002-07-03 WO PCT/EP2002/007361 patent/WO2003004152A2/en not_active Application Discontinuation
- 2002-07-03 AU AU2002345082A patent/AU2002345082A1/en not_active Abandoned
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DE3823239A1 (en) * | 1987-07-09 | 1989-01-26 | Toyota Motor Co Ltd | CATALYST FOR PURIFYING EXHAUST GAS AND CATALYST CARRIER DAFUER |
DE68903953T2 (en) * | 1988-06-01 | 1993-04-22 | Allied Signal Inc | CATALYTIC LAYERED BODY FOR VEHICLES. |
DE69326659T2 (en) * | 1992-08-28 | 2000-05-18 | Union Carbide Chemicals & Plastics Technology Corp., Danbury | Catalysts for the treatment of exhaust gases from internal combustion engines and fixed engines |
DE69324201T2 (en) * | 1992-08-31 | 1999-11-25 | Norton Chemical Process Products Corp., Stow | Catalyst carrier |
DE19918956A1 (en) * | 1999-04-27 | 2000-11-02 | Studiengesellschaft Kohle Mbh | Process for the automated investigation of catalytic and spectroscopic properties of the components of combinatorial libraries |
Cited By (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2005123594A2 (en) | 2004-06-21 | 2005-12-29 | Johnson Matthey Public Limited Company | Sols comprising mixed transitional metal oxide nanoparticles |
WO2005123594A3 (en) * | 2004-06-21 | 2006-03-16 | Johnson Matthey Plc | Sols comprising mixed transitional metal oxide nanoparticles |
CN1980736B (en) * | 2004-06-21 | 2010-05-05 | 约翰森·马瑟公开有限公司 | A sol comprising hybrid transition metal oxide nanoparticles |
US8173572B2 (en) | 2004-06-21 | 2012-05-08 | Johnson Matthey Plc | Metal oxide sols |
US9126192B2 (en) | 2004-06-21 | 2015-09-08 | Johnson Matthey Public Limited Company | Platinum group metal oxide sols |
US7780875B2 (en) | 2005-01-13 | 2010-08-24 | Cinvention Ag | Composite materials containing carbon nanoparticles |
WO2006077256A1 (en) * | 2005-01-24 | 2006-07-27 | Cinvention Ag | Metal containing composite materials |
EA012114B1 (en) * | 2005-01-24 | 2009-08-28 | Синвеншен Аг | Process for manufacturing of metal containing composite material and material therefrom |
Also Published As
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AU2002345082A1 (en) | 2003-01-21 |
WO2003004152A2 (en) | 2003-01-16 |
WO2003004152A3 (en) | 2003-04-24 |
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