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WO1991019888A1 - Regeneration d'un convertisseur catalytique d'automobile par oxydation - Google Patents

Regeneration d'un convertisseur catalytique d'automobile par oxydation Download PDF

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Publication number
WO1991019888A1
WO1991019888A1 PCT/US1991/004221 US9104221W WO9119888A1 WO 1991019888 A1 WO1991019888 A1 WO 1991019888A1 US 9104221 W US9104221 W US 9104221W WO 9119888 A1 WO9119888 A1 WO 9119888A1
Authority
WO
WIPO (PCT)
Prior art keywords
oxidizing agent
catalyst
automobile
injection means
oxygen
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.)
Ceased
Application number
PCT/US1991/004221
Other languages
English (en)
Inventor
William A. Colburn
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
CONVERTER SERVICES Corp
Original Assignee
CONVERTER SERVICES Corp
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by CONVERTER SERVICES Corp filed Critical CONVERTER SERVICES Corp
Publication of WO1991019888A1 publication Critical patent/WO1991019888A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

Links

Classifications

    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/18—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control
    • F01N3/22—Control of additional air supply only, e.g. using by-passes or variable air pump drives
    • 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
    • B01J23/90—Regeneration or reactivation
    • B01J23/96—Regeneration or reactivation of catalysts comprising metals, oxides or hydroxides of the noble metals
    • 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
    • B01J38/00—Regeneration or reactivation of catalysts, in general
    • B01J38/04—Gas or vapour treating; Treating by using liquids vaporisable upon contacting spent catalyst
    • B01J38/12—Treating with free oxygen-containing gas
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/18—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control
    • F01N3/20—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control specially adapted for catalytic conversion
    • F01N3/206—Adding periodically or continuously substances to exhaust gases for promoting purification, e.g. catalytic material in liquid form, NOx reducing agents
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
    • F02M25/00—Engine-pertinent apparatus for adding non-fuel substances or small quantities of secondary fuel to combustion-air, main fuel or fuel-air mixture
    • F02M25/10—Engine-pertinent apparatus for adding non-fuel substances or small quantities of secondary fuel to combustion-air, main fuel or fuel-air mixture adding acetylene, non-waterborne hydrogen, non-airborne oxygen, or ozone
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N2260/00—Exhaust treating devices having provisions not otherwise provided for
    • F01N2260/04—Exhaust treating devices having provisions not otherwise provided for for regeneration or reactivation, e.g. of catalyst
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N2430/00—Influencing exhaust purification, e.g. starting of catalytic reaction, filter regeneration, or the like, by controlling engine operating characteristics
    • F01N2430/06—Influencing exhaust purification, e.g. starting of catalytic reaction, filter regeneration, or the like, by controlling engine operating characteristics by varying fuel-air ratio, e.g. by enriching fuel-air mixture
    • 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
    • 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
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/10—Internal combustion engine [ICE] based vehicles
    • Y02T10/12—Improving ICE efficiencies

Definitions

  • This invention relates to a method of rejuvenating catalytic materials in an automobile catalytic converter and particularly the rejuvenation of the catalyst using oxidizing agents.
  • Automobile catalytic converters become less effective by contact with lead-containing gasoline, by poorly adjusted ignition systems, by overheating and/or by physical damage.
  • the formation of catalyst alloys or the deposit of carbonaceous or hydrocarbon materials on the catalys can inhibit the catalyst's ability to catalyze the oxidation of hydrocarbons, carbonaceous material or carbon monoxide, or to catalyze the reduction of oxides of nitrogen.
  • Example 1 demonstrates that a mixture of carbon monoxide and chlorine passing through a deactivated catalyst for one hour effects a 98% conversion of a CO at 500°F and 90% conversion of hydrocarbons at 550°F.
  • the catalyst may be removed from the catalytic-converter chamber or applied directly to the chamber without removal from the automobile if the chamber design permits.
  • U.S. Patent Number 3,134,732 describes a method of reactivating a platinum hydroforming catalyst, platinum on alumina, by contact with oxygen to burn off carbonaceous deposits, then to reducing platinum crystallite size with gaseous halogen, followed by a reduction step using hydrogen whereby the catalyst is regenerated.
  • the hydroforming function involves treatment of naphtha stock in the presence of hydrogen.
  • Patent Number 2,906,702 describes another method using a gaseous halogen to reactivate platinum-alumina hydroforming catalyst which comprises the steps of contacting the catalyst with halogen, followed by removal of volatile or soluble halogen derivatives by steam or other aqueous medium.
  • the present invention comprises a method and device for the efficient in situ rejuvenation of the catalyst of automobile catalytic converters by oxidation of hydrocarbons and/or carbonaceous or other matter deposited on the catalyst.
  • the rejuvenation is accomplished by introducing the oxidizing agent upstream or ahead of the catalytic converter in the automobile air stream while the engine is in operation.
  • the duration of treatment of catalyst with oxidizing agent is sufficient to partially or completely . oxidize deposited hydrocarbons and/or carbonaceous or other materials.
  • the oxidizing agent is introduced into the exhaust stream just upstream of the converter.
  • the oxidizing agent is introduced into the intake manifold or carburetor of the internal combustion engine. When the oxidizing agent reaches the catalytic converter, the hydrocarbons and/or carbonaceous material deposited on the catalyst are partially or completely oxidized, rendering the catalyst more effective.
  • the present invention also provides a method for reducing carbon monoxide and hydrocarbon emissions from automobiles by contacting the catalytic converter catalyst with an oxidizing agent under operating conditions for a period of time sufficient to decrease carbon monoxide and hydrocarbon emissions.
  • said method can also increase carbon dioxide emissions.
  • a decrease in carbon monoxide and increase in carbon dioxide emissions can reflect an improvement in gasoline mileage.
  • the device comprises a means for injecting the oxidizing agent into the automobile air stream at a point upstream of the catalytic converter.
  • the oxidizing agent is injected into the exhaust stream just upstream of the converter by way of a fitting inserted into an exhaust line hole.
  • the oxidizing agent is injected by way of a fitting into the intake manifold or into a vacuum line feeding directly into either the intake manifold or the carburetor.
  • the oxidizing agent supply comprises an oxidizing agent in a vessel and a means of delivery of the agent to the fitting or injection means.
  • the present invention provides a simple, inexpensive alternative to replacement of spent automobile catalytic converters. Further, the subject catalyst regeneration process requires only a brief treatment period and uses relatively inexpensive reagents.
  • Figure 1 is a schematic diagram of two embodiments of the method of the subject invention in which the oxidizing agent is injected into the automobile air stream at the exhaust stream or the intake manifold or carburetor.
  • the subject inventive process and device can be used to rejuvenate all automobile catalytic converter catalysts regardless of the composition of the catalyst or the catalyst support or substrate. It is not believed, however, that the subject method can remove lead from lead- contaminated catalytic converter.
  • the subject method for rejuvenation of the catalyst is carried out by the introduction of an oxidizing agent into the automobile air stream, such that the agent contacts and oxidizes the converter catalyst and contaminants (e.g., hydrocarbons and carbonaceous materials) contained thereon.
  • the resulting oxidation products such as carbon dioxide and water, are then exhausted into the atmosphere.
  • the subject method of catalyst regeneration and decrease in carbon monoxide and hydrocarbon emissions is carried out- while the automobile and its converter are in operation and the catalytic converter remains mounted on the automobile (in situ) .
  • the operating temperature inside a catalytic converter can vary substantially, but is at least about 500°F, and typically is between about 800° and 1400°F.
  • the oxidizing agent is introduced into the automobile air stream, wherein the oxidizing agent is heated and dispersed or mixed in said stream prior to entry of the oxidizing agent into the catalytic converter and contact with the catalyst or contaminants thereon.
  • “Automobile air stream” means the flow or stream of air through the air intake manifold, carburetor, vacuum lines, internal combustion engine, exhaust conduits, catalytic converter and any intermediate conduit, device or apparatus.
  • the oxidizing agent is a material which rapidly oxidizes the deposited contaminants under typical catalytic converter operating conditions.
  • Such agents include, but are not limited to substantially pure oxygen or oxygen- enriched air.
  • Oxygen-enriched air means air having an oxygen concentration greater than about 30% (v/v) . It is increasingly preferred that the oxygen-enriched air contain 50%, 70%, 80% and 90% (v/v) oxygen.
  • Substantially pure oxygen means at least about 95% (v/v) oxygen. The use of substantially pure oxygen in the subject methods is most preferred.
  • substantially pure oxygen The advantages of using substantially pure oxygen include: (1) less than 5% (v/v) nitrogen is introduced into the converter; (2) the use of substantially pure oxygen reduces the catalyst treatment time; and (3) substantially pure oxygen is less expensive per mole and less hazardous than halide oxidizing agents such as chlorine.
  • the duration of treatment is determined by the type and concentration of oxidizing agent used, the flow or feed rate of oxidizing agent into the automobile air stream, the operating temperature of the automobile and other factors.
  • the duration of treatment is sufficient to partially or completely regenerate the catalyst or to cause a positive reduction in the emission of carbon monoxide and/or hydrocarbons.
  • the duration of treatment is typically between about 2 and 30 minutes, and preferably between about 5 and 15 minutes.
  • a "partial regeneration" of the catalyst means a reduction of the carbon monoxide and/or hydrocarbon emission by at least about 5%.
  • a "positive reduction" in the emission of carbon monoxide and/or hydrocarbons means a reduction of either or both emissions by at least about 5%. It is increasingly preferred that the reduction in said emissions be at least about 10%, 25%, 50%, 75%, 90% and 95%.
  • Such reductions in emissions can be measured, for example, by a Sun Modular Engine Analyzer (MEA) . -1-
  • the subject invention does not require or involve any modification to or tampering with the catalytic converter itself.
  • FIG. 1 schematically illustrates two embodiments of the subject invention.
  • the oxidizing agent (6) can be introduced into the automobile air stream at the intake manifold or carburetor (1) or in the exhaust stream (3) upstream of the converter (4) .
  • the oxidizing agent can be introduced by an injection means into a vacuum line that feeds into the intake manifold or into the carburetor.
  • Such injection means can be a plastic fitting.
  • a hole or tap is drilled into the exhaust conduit and the oxidizing agent is introduced by an injection means, such as a stainless steel fitting, into the exhaust conduit.
  • a 1/8 inch fitting has been found to be suitable.
  • the oxidizing agent be introduced into the carburetor or intake manifold or vacuum lines which feed directly thereto. This embodiment is preferred because it is not necessary to hoist the automobile to gain access to the air stream; it does not require the drilling and repair of a hole or tap in the exhaust conduit or introduce the possibility of an exhaust leak; and it provides for more complete heating of the oxidizing agent prior to contact with the catalyst or contaminants thereon.
  • the subject device used in catalyst rejuvenation or in carbon monoxide and hydrocarbon emission reduction comprises an oxidizing agent supply and an injection means for introducing the supply's oxidizing agent to the automobile's air stream.
  • the point of injection into the air stream can be at a number of locations along the automobile air stream.
  • plastic or stainless steel fittings can be used as the injection means.
  • the oxidizing agent supply is a vessel that contains oxidizing agent and is capable of delivering the agent to the injection means.
  • a 95% (v/v) compressed oxygen tank or an oxygen concentrator can supply a stream of substantially pure oxygen to the injection means.
  • the means of delivery of the oxidizing agent by the supply vessel can be by any means known in the art including mechanical pumping or channeling of compressed oxidizing agent.
  • the oxidizing agent supply can be constructed to provide an appropriate flow rate of oxidizing agent that efficiently rejuvenates the converter catalyst or reduces emissions.
  • the oxidizing agent supply can provide means of selecting flow rate according to the engine size, number of cylinders of the automobile to be treated, the condition of the catalyst as reflected by the total mileage of the automobile, or other factors. It is a matter of experimentation to determine an appropriate flow rate of a particular oxidizing agent to provide for an efficient regeneration of the converter catalyst or reduction in hydrocarbon and carbon monoxide emissions.
  • a tap was drilled into each exhaust pipe of about 50 automobiles between the engine and the catalytic converter. After each engine had run for fifteen minutes and had heated the catalyst, 95% (v/v) oxygen was injected into the tap at a rate of about 13 liters/minute for five minutes while the engine was still in operation. Gases passed out through the exhaust into the atmosphere. The emissions were tested before and after the oxygen injection, and all catalytic converters tested showed a minimum of 25% improvement in the standard hydrocarbon and carbon monoxide State of Colorado Vehicle Emissions Control System Tests.
  • HC refers to hydrocarbons
  • Example 1 The procedure of Example 1 was followed with the exception that the 95% oxygen was introduced into the intake manifold of a 1985 Mercedes (8 cylinders). The flow rate of oxygen provided by the oxygen concentrator was between about 8 and 18 liters/minute through the 1/8 inch fitting.
  • the treatment procedure was as follows: 5 minutes of oxygen at elevated rpm (about 2500 rp ) , 5 minutes of oxygen at idle, followed by 5 minutes of oxygen at elevated rpm (about 2500 rpm) .
  • the following results were measured using a Sun Modular Engine Analyzer.
  • Example 3 The procedure of Example 3 was used on a 1981 Jeep and the following results were obtained.
  • Example 3 The procedure of Example 3 was used on a 1990 Ford Econoline and the following results were obtained.
  • Example 3 The procedure of Example 3 was used on a 1982 Mitsubishi Cordia (4 cylinders) and the following results were obtained.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Combustion & Propulsion (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Health & Medical Sciences (AREA)
  • Toxicology (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Exhaust Gas After Treatment (AREA)
  • Exhaust Gas Treatment By Means Of Catalyst (AREA)

Abstract

On décrit un procédé et un dispositif pour la régénération rapide in situ d'un catalyseur de convertisseur catalytique d'automobile par oxydation. Le procédé comprend l'injection de l'oxydant (6) dans le circuit d'alimentation en air de l'automobile à un point situé en amont du convertisseur catalytique (4), de préférence dans le collecteur d'admission (1), et pendant que le convertisseur (4) est à la température de fonctionnement. L'oxydant (6) est de préférence de l'air enrichi en oxygène ou de l'oxygène sensiblement purifié. Le dispositif comprend des éléments d'amenée et d'injection de l'oxydant.
PCT/US1991/004221 1990-06-13 1991-06-13 Regeneration d'un convertisseur catalytique d'automobile par oxydation Ceased WO1991019888A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US53791790A 1990-06-13 1990-06-13
US537,917 1990-06-13

Publications (1)

Publication Number Publication Date
WO1991019888A1 true WO1991019888A1 (fr) 1991-12-26

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Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/US1991/004221 Ceased WO1991019888A1 (fr) 1990-06-13 1991-06-13 Regeneration d'un convertisseur catalytique d'automobile par oxydation

Country Status (3)

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AU (1) AU8231291A (fr)
CA (1) CA2064843A1 (fr)
WO (1) WO1991019888A1 (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0650978A1 (fr) * 1993-11-03 1995-05-03 BASF Aktiengesellschaft Copolymères réticulables par radicaux
US6878471B1 (en) 1999-06-24 2005-04-12 Johnson Matthey Public Limited Company Process for the regeneration of reforming catalysts

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3826089A (en) * 1971-07-07 1974-07-30 Nissan Motor Air-pollution preventive arrangement
US3979185A (en) * 1974-01-21 1976-09-07 The Lubrizol Corporation Catalytic converter having plural reaction stages with temperature-comparing means therein
US4331454A (en) * 1979-03-15 1982-05-25 Texaco Inc. Exhaust filter rejuvenation method
US4372111A (en) * 1980-03-03 1983-02-08 Texaco Inc. Method for cyclic rejuvenation of an exhaust gas filter and apparatus

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3826089A (en) * 1971-07-07 1974-07-30 Nissan Motor Air-pollution preventive arrangement
US3979185A (en) * 1974-01-21 1976-09-07 The Lubrizol Corporation Catalytic converter having plural reaction stages with temperature-comparing means therein
US4331454A (en) * 1979-03-15 1982-05-25 Texaco Inc. Exhaust filter rejuvenation method
US4372111A (en) * 1980-03-03 1983-02-08 Texaco Inc. Method for cyclic rejuvenation of an exhaust gas filter and apparatus

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0650978A1 (fr) * 1993-11-03 1995-05-03 BASF Aktiengesellschaft Copolymères réticulables par radicaux
US6878471B1 (en) 1999-06-24 2005-04-12 Johnson Matthey Public Limited Company Process for the regeneration of reforming catalysts

Also Published As

Publication number Publication date
CA2064843A1 (fr) 1991-12-14
AU8231291A (en) 1992-01-07

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