DE2412290A1 - Catalyst for oxidizing carbon monoxide and hydrocarbons - comprising aluminates of copper, manganese, nickel, and opt. cerium on alumina - Google Patents
Catalyst for oxidizing carbon monoxide and hydrocarbons - comprising aluminates of copper, manganese, nickel, and opt. cerium on aluminaInfo
- Publication number
- DE2412290A1 DE2412290A1 DE2412290A DE2412290A DE2412290A1 DE 2412290 A1 DE2412290 A1 DE 2412290A1 DE 2412290 A DE2412290 A DE 2412290A DE 2412290 A DE2412290 A DE 2412290A DE 2412290 A1 DE2412290 A1 DE 2412290A1
- Authority
- DE
- Germany
- Prior art keywords
- cerium
- temperatures
- moldings
- manganese
- oxide
- 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.)
- Granted
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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
- B01J23/70—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
- 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
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
- B01D53/944—Simultaneously removing carbon monoxide, hydrocarbons or carbon making use of oxidation catalysts
-
- 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
-
- 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
- B01J37/0009—Use of binding agents; Moulding; Pressing; Powdering; Granulating; Addition of materials ameliorating the mechanical properties of the product catalyst
- B01J37/0018—Addition of a binding agent or of material, later completely removed among others as result of heat treatment, leaching or washing,(e.g. forming of pores; protective layer, desintegrating by heat)
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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
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Combustion & Propulsion (AREA)
- Biomedical Technology (AREA)
- Environmental & Geological Engineering (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Catalysts (AREA)
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
Abstract
Description
Verfahren zur Oxidation von Kohlenmonoxid und Kohlenwasserstoffen (Zusatz zu Patent ..... (Aktenzeichen P 23 23 251. 1)) Gegenstand der Hauptpatentanmeldung P 23 23 251. 1 ist ein Verfahren zur Oxidation von Kohlenmonoxid und Kohlenwasserstoffen, insbesondere aus Abgasen von Verbrennungsmotoren, mit sauerstoffhaltigen Gasen zu Kohlendioxid und Wasser, wobei man die Oxidation bei Temperaturen von 150 bis 800 0C in Gegenwart eines Trägerkatalysators durchführt, welcher aus einem Gemisch von Aluminaten des Kupfers, Mangans und Nickels als aktive Bestandteile und aus reinem Aluminiumoxid als Trägerstoff besteht und wobei die Summe der Aluminate 10 bis 45 GeWichts% beträgt.Process for the oxidation of carbon monoxide and hydrocarbons (Addition to patent ..... (file number P 23 23 251. 1)) Subject of the main patent application P 23 23 251. 1 is a process for the oxidation of carbon monoxide and hydrocarbons, in particular from exhaust gases from internal combustion engines, with gases containing oxygen Carbon dioxide and water, the oxidation being carried out at temperatures of 150 to 800 Carries out 0C in the presence of a supported catalyst, which consists of a mixture of Aluminates of copper, manganese and nickel as active ingredients and of pure There is aluminum oxide as a carrier and the sum of the aluminates 10 to 45 Weight% is.
Die Hauptpatentanmeldung betrifft weiterhin ein Verfahren zur Herstellung des Trägerkatalysators.The main patent application also relates to a method of manufacture of the supported catalyst.
Es ist Aufgabe der vorliegenden Erfindung, ein Verfahren zur Oxidation von Kohlenmonoxid und Kohlenwasserstoffen mit sauerstoffhaltigen Gasen zu Kohlendioxid und Wasser unter Verwendung eines solchen Trägerkatalysators zu schaffen, dessen Aktivität unabhängig von der Sauerstoffkonzentration des mit ihm in Kontakt gebrachten Gasgemisches ist und welcher bei hoher mechanischer Festigkeit niedrigere Anspringtemperaturen insbesondere für die Oxidation von Kohlenmonoxid aufweist.It is the object of the present invention to provide a method for oxidation from carbon monoxide and hydrocarbons with oxygen-containing gases to carbon dioxide and to provide water using such a supported catalyst, the Activity regardless of the oxygen concentration of what is in contact with it Is a gas mixture and which has lower light-off temperatures with high mechanical strength in particular for the oxidation of carbon monoxide.
In weiterer Ausgestaltung des in der Hauptanmeldung angegebenen Verfahrens betrifft die vorliegende Erfindung ein Verfahren zur Oxidation von Kohlenmonoxic und Kohlenwasserstoffen, insbesondere aus Abgasen von Verbrennungsmotoren, mit sauerstoffhaltigen Gasen zu Kohlendioxid und Wasser, wobei man die Oxidation bei Temperaturen von 150 bis 800°C in Gegenwart eines Trägerkatalysators durchführt, welcher aus einem Gemisch von Aluminaten des Kupfers, Mangans und Nickels als aktive Bestandteile und aus reinem Aluminiumoxid als Trägerstoff besteht und wobei die Summe der Aluminate 10 bis 45 Gewichts beträgt, nach Patent ..... (Aktenzeichen P 23 23 251. 1), welches dadurch gekennzeichnet ist, daß auf den Trägerkatalysator zusätzlich 0,5 bis 10 Gewicht Cer als Oxid aufgebracht sind.In a further embodiment of the procedure specified in the main application The present invention relates to a method for the oxidation of carbon monoxic and hydrocarbons, in particular from exhaust gases from internal combustion engines, with oxygen-containing Gases to carbon dioxide and water, the oxidation being carried out at temperatures of 150 Carries out up to 800 ° C in the presence of a supported catalyst which consists of a mixture of aluminates of copper, manganese and nickel as active ingredients and from pure aluminum oxide as a carrier and where the sum of the aluminates 10 up to 45 weight, according to patent ..... (file number P 23 23 251. 1), which is characterized in that an additional 0.5 to 10 Weight of cerium are applied as oxide.
Weiterhin kann das erfindungsgemäße Verfahren wahlweise noch dadurch gekennzeichnet sein, daß a) auf den Trägerkatalysator zusätzlich 1 bis 7 Gewichts% Cer als Oxid aufgebracht sind; b) man zur Herstellung des Trägerkatalysators reines Aluminiumoxid zu Formkörpern verpreßt; daß man die Formkörper bei Temperaturen von 1000 bis 12000 glüht; daß man die geglühten Formkörper mit einer wäßrigen Lösung von Salzen leicht zersetzbarer Säuren des Kupfers, Mangans und Nickels tränkt; daß man die auf die Formkörper aufgezogenen Metallsalze bei Temperaturen von 300 bis 6000G zersetzt, daß man die metalloxidhaltigen Formkörper bei Temperaturen von 800 bis 1200 0C glüht; daß man die geglühten Formkörper mit einer wäßrigen Lösung eines Cersalzes einer leicht zersetzbaren Säure tränkt; daß man das auf die Formkörper aufgezogene Cersalz bei 130 bis 1#00C trocknet; daß man das getrocknete Cersalz auf den Formkörpern durch stufenweises Erhitzen auf Temperaturen von 200 bis 300 0C und 450 bis 550°C zersetzt und daß man anschließend die ceroxidhaltigen Formkörper bei Temperaturen von 700 bis 9000C glüht; c) die Kupfer-, Mangan-, Nickel- und Cersalze leicht zersetzbarer Säuren Nitrate sind.Furthermore, the method according to the invention can optionally also thereby be characterized in that a) an additional 1 to 7% by weight of the supported catalyst Cerium are applied as oxide; b) one pure for the preparation of the supported catalyst Alumina pressed to form shaped bodies; that the moldings at temperatures of 1000 to 12000 glow; that the annealed shaped body with an aqueous solution soaked in salts of easily decomposable acids of copper, manganese and nickel; that the metal salts drawn onto the shaped bodies at temperatures of 300 to 6000G decomposes that the metal oxide-containing moldings at temperatures of 800 glows up to 1200 0C; that the annealed shaped body with an aqueous solution of a Cerium salt of an easily decomposable acid soaks; that you can do that on the moldings raised Cerium salt dries at 130 to 1 # 00C; that one the dried cerium salt on the moldings by gradually heating to temperatures of 200 to 300 ° C and 450 to 550 ° C decomposed and that you then the cerium oxide-containing moldings at temperatures glows from 700 to 9000C; c) the copper, manganese, nickel and cerium salts are easily decomposable Acids are nitrates.
Das Verfahren gemäß der Erfindung erlaubt insbesondere die Oxidation von Kohlenmonoxid und Kohlenwasserstoffen mit überschüssigem Sauerstoff, wodurch eine vollständige Verbrennung der genannten Stoffe erreicht wird.The method according to the invention allows in particular oxidation of carbon monoxide and hydrocarbons with excess oxygen, causing complete combustion of the substances mentioned is achieved.
Der beim erfindungsgemäßen Verfahren verwendete Trägerkatalysator ist abriebfest und weist eine hohe Druckfestigkeit auf. Er zeichnet sich weiterhin durch niedrige Anspringtemperaturen, insbesondere für die Oxidation von Kohlenmonoxid, aus.The supported catalyst used in the process according to the invention is abrasion-resistant and has a high compressive strength. He continues to stand out due to low light-off temperatures, especially for the oxidation of carbon monoxide, the end.
In den folgenden Beispielen wurden jeweils Trägerkatalysatoren in Form von zylindrischen Formkörpern von 3 mm Durchmesser und 3 mm Länge verwendet, an welchen 17 Nl Je ml Katalysator und Stunde eines Testgasgemisches mit 3 Volumen% 02> 2 Volumen% CO, 1000 ppm n-Hexan, 2,5 Volumen% Wasserdampf, Rest N2 oxidiert wurden, wobei der Testgasstrom unter Berücksichtigung der jeweils vorgesehenen Meßtemperatur vorgeheizt war. Im oxidierten Gas wurde der Restgehalt an CO und n-Hexan ermittelt und daraus der prozentuale Umsatz dieser beiden Komponenten errechnet.In each of the following examples, supported catalysts were used in Form of cylindrical moldings of 3 mm diameter and 3 mm length used, at which 17 Nl per ml of catalyst and hour of a test gas mixture with 3 volume% 02> 2 volume% CO, 1000 ppm n-hexane, 2.5 volume% water vapor, remainder N2 oxidized were, the test gas flow taking into account the respective intended measuring temperature was preheated. The residual CO and n-hexane content in the oxidized gas was determined and from this the percentage conversion of these two components is calculated.
Als Maß für die Aktivität des Katalysators wurden die Temperaturen herangezogen, bei welchen 50 bzw. 90 % des CO und des n-Hexans zu C02 und H20 umgesetzt waren (U50 CO; Ugo U90 U50 Hex; U90 Hex# Die Druckfestigkeit der Katalysatoren wurde in Längsrichtung der Formkörper zwischen planparallelen Platten gemessen.As a measure of the activity of the catalyst, the Temperatures used, in which 50 or 90% of the CO and n-hexane converted to CO 2 and H 2 O were (U50 CO; Ugo U90 U50 Hex; U90 Hex # The compressive strength of the catalysts was measured in the longitudinal direction of the moldings between plane-parallel plates.
Beispiel 1 (Vergleichsbeispiel) Ce(N03)3 6H20 wurde bis zur beginnenden Nitratzersetzung getrocknet und zu Formkörpern verpreßt. Die Preßlinge wurden nacheinander je 10 Stunden lang unter Luftzutritt auf 500 bzw. 800 0C erhitzt. Die Aktivitätsbestimmung ergab: U50 CO =430 0C U5o Hex 560°C U90 CO =540°C U90 Hex = 6600C.Example 1 (comparative example) Ce (N03) 3 6H20 was used up to the beginning Dried nitrate decomposition and pressed into molded articles. The compacts were one by one Heated for 10 hours each with access to air to 500 or 800 ° C. The activity determination resulted in: U50 CO = 430 0C U5o Hex 560 ° C U90 CO = 540 ° C U90 Hex = 6600C.
Der Katalysator hatte eine Druckfestigkeit von 0,8 kg/mm.The catalyst had a compressive strength of 0.8 kg / mm.
Beispiel 2 (Vergleichsbeispiel) Alkali- und silikatfreies Aluminiumoxid wurde in Wasser eingerührt und die erhaltene Paste bei 1000C getrocknet.Example 2 (comparative example) Alkali and silicate-free aluminum oxide was stirred into water and the paste obtained was dried at 1000C.
Die trockene Masse wurde vermahlen und nach Zusatz von 5 Gewichts% Graphit in zylindrische Formkörper von 3 mm Durchmesser und 5 mm Länge verpreßt. Nach Abbrennen des als Preßhilfe zugesetzten Graphits bei 650°C wurden die Formkörper 20 Stunden bei 1000°C geglüht. Durch Tränken mit einer wäßrigen Metallnitratlösung wurden auf die Formkörper 5,1 % Cu, 2,94 % Mn und 1,57 % Ni aufgetragen. Die aufgetragenen Metallnitrate wurden durch Erhitzen auf 4000C in die Oxide umgesetzt. Die metalloxidhaltigen Formkörper wurden 18 Stunden bei 1000 0C geglüht. Die Aktivitätsbestimmung ergab: U50 CO =2000 C UgO CO = 285°C U50 Hex= 360°C Der Katalysator hatte eine Druckfestigkeit von 5,0 kg/mm.The dry mass was ground and, after adding 5% by weight Graphite pressed into cylindrical moldings 3 mm in diameter and 5 mm in length. After the graphite added as a pressing aid had burned off at 650.degree. C., the moldings became Annealed for 20 hours at 1000 ° C. By soaking with an aqueous metal nitrate solution 5.1% Cu, 2.94% Mn and 1.57% Ni were applied to the shaped bodies. The applied Metal nitrates were converted into the oxides by heating to 4000C. The ones containing metal oxides Shaped bodies were annealed at 1000 ° C. for 18 hours. the Activity determination resulted in: U50 CO = 2000 C UgO CO = 285 ° C U50 Hex = 360 ° C The catalyst had compressive strength of 5.0 kg / mm.
Beispiel 3 (Gemäß der Erfindung) Auf den nach Beispiel 2 hergestellten
Katalysator wurde durch Tränken mit einer wäßrigen Cernitratlösung jeweils 2, 4
oder 6 % Ce aufgetragen. Das aufgetragene Cersalz wurde 32 Stunden bei 1400C getrocknet
und dann durch dreistündiges Erhitzen auf 250°C und durch 10 stündiges Erhitzen
auf #000C zersetzt. Anschließend wurde 10 Stun#den bei 800 0C geglüht. Aktivität
und Druckfestigkeit der so hergestellten Katalysatoren ergeben sich aus der folgenden
Tabelle:
Claims (4)
Priority Applications (16)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE2412290A DE2412290C3 (en) | 1974-03-14 | 1974-03-14 | Process for the oxidation of carbon monoxide and hydrocarbons |
DE19742462792 DE2462792C2 (en) | 1973-05-09 | 1974-03-14 | Process for the production of a supported catalyst |
CS2625A CS169764B2 (en) | 1973-05-09 | 1974-04-11 | |
IL44734A IL44734A (en) | 1973-05-09 | 1974-04-29 | Oxidation of carbon monoxide and hydrocarbons |
GB1856874A GB1462469A (en) | 1973-05-09 | 1974-04-29 | Oxidation of carbon monoxide and hydrocarbons |
NLAANVRAGE7405849,A NL179789C (en) | 1973-05-09 | 1974-05-01 | PROCESS FOR THE OXIDATION OF CARBON MONOXIDE AND HYDROGEN OXYGEN-CONTAINING GASES IN THE PRESENCE OF A CARRIER CATALYST. |
SE7406031A SE403642B (en) | 1973-05-09 | 1974-05-06 | KIT AND CATALYST OXIDATION CATALYTER, PREFERABLY IN EXHAUST ENGINE EXHAUST |
DD178343A DD110916A5 (en) | 1973-05-09 | 1974-05-07 | |
PL1974170878A PL96886B1 (en) | 1973-05-09 | 1974-05-07 | METHOD OF OXIDATION OF CARBON MONOXIDE AND HYDROCARBONES |
IT50815/74A IT1011403B (en) | 1973-05-09 | 1974-05-07 | PROCEDURE FOR THE OXIDATION OF CARBON OXIDE AND HYDROCARBONS |
RO7478699A RO71029A (en) | 1973-05-09 | 1974-05-07 | CATALYST FOR CARBON MONOXIDE AND HYDROCARBURYLOCATALIZER FOR OXIDATION OF CARBON MONOXIDE AND HYDROCARBONS AND PROCESS FOR THE OBTAINING THEM |
AT376774A AT359983B (en) | 1973-05-09 | 1974-05-07 | METHOD FOR THE OXIDATION OF CARBON MONOXIDE AND HYDROCARBONS |
CH629374A CH603994A5 (en) | 1973-05-09 | 1974-05-08 | |
CA199,243A CA1013547A (en) | 1973-05-09 | 1974-05-08 | Oxidation of carbon monoxide and hydrocarbons |
SU742024139A SU1102483A3 (en) | 1974-03-14 | 1974-05-08 | Catalyst of purification of exhaust gases of internal combustion engines |
FR7416081A FR2228720B1 (en) | 1973-05-09 | 1974-05-09 |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE2412290A DE2412290C3 (en) | 1974-03-14 | 1974-03-14 | Process for the oxidation of carbon monoxide and hydrocarbons |
Publications (3)
Publication Number | Publication Date |
---|---|
DE2412290A1 true DE2412290A1 (en) | 1975-10-02 |
DE2412290B2 DE2412290B2 (en) | 1979-01-25 |
DE2412290C3 DE2412290C3 (en) | 1980-11-06 |
Family
ID=5910084
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
DE2412290A Expired DE2412290C3 (en) | 1973-05-09 | 1974-03-14 | Process for the oxidation of carbon monoxide and hydrocarbons |
Country Status (2)
Country | Link |
---|---|
DE (1) | DE2412290C3 (en) |
SU (1) | SU1102483A3 (en) |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE3103533A1 (en) * | 1981-02-03 | 1982-08-05 | Battelle-Institut E.V., 6000 Frankfurt | ZEOLITHIC MOLECULAR SCREEN, ADSORBER AND CATALYST SYSTEM |
-
1974
- 1974-03-14 DE DE2412290A patent/DE2412290C3/en not_active Expired
- 1974-05-08 SU SU742024139A patent/SU1102483A3/en active
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE3103533A1 (en) * | 1981-02-03 | 1982-08-05 | Battelle-Institut E.V., 6000 Frankfurt | ZEOLITHIC MOLECULAR SCREEN, ADSORBER AND CATALYST SYSTEM |
Also Published As
Publication number | Publication date |
---|---|
DE2412290C3 (en) | 1980-11-06 |
SU1102483A3 (en) | 1984-07-07 |
DE2412290B2 (en) | 1979-01-25 |
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