EP0668471A2 - Katalytisches Verfahren - Google Patents

Katalytisches Verfahren Download PDF

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Publication number
EP0668471A2
EP0668471A2 EP94115017A EP94115017A EP0668471A2 EP 0668471 A2 EP0668471 A2 EP 0668471A2 EP 94115017 A EP94115017 A EP 94115017A EP 94115017 A EP94115017 A EP 94115017A EP 0668471 A2 EP0668471 A2 EP 0668471A2
Authority
EP
European Patent Office
Prior art keywords
catalyst
combustion
kelvin
fuel
admixture
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.)
Withdrawn
Application number
EP94115017A
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English (en)
French (fr)
Other versions
EP0668471A3 (de
Inventor
William C. Pfefferle
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Individual
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Individual
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Filing date
Publication date
Priority claimed from US08/197,890 external-priority patent/US5437152A/en
Priority claimed from US08/197,931 external-priority patent/US5593299A/en
Application filed by Individual filed Critical Individual
Publication of EP0668471A2 publication Critical patent/EP0668471A2/de
Publication of EP0668471A3 publication Critical patent/EP0668471A3/de
Withdrawn legal-status Critical Current

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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
    • 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
    • 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
    • F01N3/24—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 constructional aspects of converting apparatus
    • F01N3/26—Construction of thermal reactors
    • 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
    • F01N3/24—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 constructional aspects of converting apparatus
    • F01N3/28—Construction of catalytic reactors
    • F01N3/2882—Catalytic reactors combined or associated with other devices, e.g. exhaust silencers or other exhaust purification devices
    • 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 
    • F23C9/00—Combustion apparatus characterised by arrangements for returning combustion products or flue gases to the combustion chamber
    • F23C9/006—Combustion apparatus characterised by arrangements for returning combustion products or flue gases to the combustion chamber the recirculation taking place in the combustion chamber
    • 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
    • F01N2250/00—Combinations of different methods of purification
    • F01N2250/04—Combinations of different methods of purification afterburning and catalytic conversion
    • 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
    • F01N3/24—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 constructional aspects of converting apparatus
    • F01N3/30—Arrangements for supply of additional air
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02B—INTERNAL-COMBUSTION PISTON ENGINES; COMBUSTION ENGINES IN GENERAL
    • F02B1/00—Engines characterised by fuel-air mixture compression
    • F02B1/02—Engines characterised by fuel-air mixture compression with positive ignition
    • F02B1/04—Engines characterised by fuel-air mixture compression with positive ignition with fuel-air mixture admission into cylinder
    • 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 
    • F23C2900/00—Special features of, or arrangements for combustion apparatus using fluid fuels or solid fuels suspended in air; Combustion processes therefor
    • F23C2900/13002—Catalytic combustion followed by a homogeneous combustion phase or stabilizing a homogeneous combustion phase

Definitions

  • This invention relates to improved systems for combustion of fuels and to methods for catalytic promotion of fuel combustion.
  • Gas turbine combustors require the capability for good combustion stability over a wide range of operating conditions. To achieve low NO X operation with variations of conventional combustors has required operating so close to the stability limit that not only is turndown compromised , but combustion stability as well. Although emissions can be controlled by use of the catalytic combustors of U.S. Patent #3.928,961, such combustors typically also have a much lower turndown ratio than conventional combustors with efficient operation limited to temperatures above about 1400 Kelvin with an upper temperature limited not only by NO X formation kinetics but by catalyst materials survivability, thus limiting use in some applications.
  • the present invention meets the need for reduced emissions by providing a system for the combustion of fuel lean fuel-air mixtures, even those having exceptionally low adiabatic flame temperatures such as admixtures of air with the exhaust gases from small internal combustion engines.
  • monolith and “monolith catalyst” refer not only to conventional monolithic structures and catalysts such as employed in conventional catalytic converters but also to any equivalent unitary structure such as an assembly or roll of interlocking sheets or the like.
  • microlith and “microlith catalyst” refer to high open area monolith catalyst elements with flow paths so short that reaction rate per unit length per channel is at least fifty percent higher than for the same diameter channel with a fully developed boundary layer in laminar flow, i.e. a flow path of less than about two mm in length, preferably less than one mm or even less than 0.5 mm and having flow channels with a ratio of channel flow length to channel diameter less than about two to one, but preferably less than one to one and more preferably less than about 0.5 to one.
  • Channel diameter is defined as the diameter of the largest circle which will fit within the given flow channel and is preferably less than one mm or more preferably less than 0.5 mm.
  • fuel and hydrocarbon as used in the present invention not only refer to organic compounds, including conventional liquid and gaseous fuels, but also to gas streams containing fuel values in the form of compounds such as carbon monoxide, organic compounds or partial oxidation products of carbon containing compounds.
  • the present invention makes possible practical ultra low emissions catalytic combustors.
  • the low minimum operating temperatures of the method of this invention make possible catalytically stabilized combustors for gas turbines, havng a large turndown ratio without the use of variable geometry and often even the need for dilution air to achieve the low turbine inlet temperatures required for idle and low power operation.
  • the present invention also makes possible ultra low emission automotive exhaust combustors as much as ten fold smaller in catalyst mass than the much lower conversion catalytic converters presently in use.
  • a fuel-air mixture is contacted with an ignition source to produce heat and reactive intermediates for continuous stabilization of combustion in a thermal reaction zone at temperatures not only well below a temperature resulting in significant formation of nitrogen oxides from molecular nitrogen and oxygen but even below the minimum temperatures of prior art catalytic combustors. Combustion can be stabilized in the thermal reaction zone even at temperatures as low as 1000° Kelvin or below. Catalytic surfaces have been found to be especially effective for ignition of such fuel-air mixtures.
  • the efficient, rapid thermal combustion which occurs in the presence of a catalyst, even with lean fuel-air mixtures outside the normal flammable limits, is believed to result from the injection of heat and free radicals produced by the catalyst surface reactions at a rate sufficient to counter the quenching of free radicals which otherwise minimize thermal reaction even at combustion temperatures much higher than those feasible in the method of the present invention.
  • the catalyst may be in the form of a monolith, a microlith or even a combustion wall coating, the latter allowing higher maximum operating temperatures than might be tolerated by a catalyst operating at or close to the adiabatic combustion temperature.
  • the thermal reaction zone is well mixed, especially in reacting engine exhaust gases for emissions control. Plug flow operation is possible provided the thermal zone inlet temperature is above the spontaneous ignition temperature of the given fuel, typically less than about 700 Kelvin for most fuels but around 900 ° Kelvin for methane and about 750 ° Kelvin for ethane.
  • a fuel-air mixture is contacted with an ignition source to produce combustion products, at least a portion of which are mixed with a fuel-air mixture in a well mixed thermal reaction zone.
  • engine exhaust gas is mixed with air in sufficient quantity to consume at least a major portion of the combustibles present and passed to a recirculating flow in a thermal reaction zone.
  • Effluent from the thermal zone exits through a monolithic catalyst, preferably a microlith. Pulsation of the exhaust flow draws sufficient reaction products from contact with the catalyst back into the thermal zone to ignite and stabilize gas phase combustion in the thermal zone.
  • engine exhaust temperature is high enough to achieve thermal combustion light-off within seconds of engine starting, especially with use of low thermal mass microlith igniter catalysts. Hot combustion gases exiting the thermal reaction zone contact the catalyst providing enhanced conversion, particularly at marginal temperature levels for thermal reaction.
  • the catalyst may be placed at the reactor inlet, as typically would be the case for furnace combustors, or even applied as a coating to the thermal zone walls in a manner such as to contact recirculating gases.
  • Wall coated catalysts are especially effective with fuel-air mixtures at thermal reaction zone inlet temperatures in excess of about 700 ° Kelvin such as is often the case with exhaust gases from internal combustion engines.
  • placement of the catalyst at the inlet to the thermal reaction zone allows operation of the catalyst at a temperature below that of the thermal combustion region.
  • Such placement permits operation of the combustor at temperatures well above the temperature of the catalyst as is the case for a combustor wall coated catalyst.
  • Use of electrically heatable catalysts provides both ease of light-off and ready relight in case of a flameout. This also permits use of less costly catalyst materials inasmuch as the lowest possible lightoff temperature is not required with an electrically heated catalyst.
  • near instantaneous light-off of combustion is important. This is especially true of auxilliary power units which must be started in flight, typically at high altitude low temperature conditions.
  • microlith catalyst elements can be so low that it is feasible to electrically preheat the catalyst to an effective operating temperature in less than about 0.50 seconds.
  • the low thermal mass of "microlith" catalysts makes it possible to bring an electrically conductive combustor catalyst up to a light-off temperature as high as 1000 or even 1500 degrees Kelvin or more in less than about five seconds, often in less than about one or two seconds with modest power useage.
  • Such rapid heating is allowable for microlith catalysts because sufficiently short flow paths permit rapid heating without destructive stresses from consequent thermal expansion.
  • the microlith catalyst elements preferrably have an open area in the direction of flow of at least about 65%, and more preferrably at least about 70%.
  • lower open area catalysts may be desireable for low flow placements and use of wall coated catalysts are especially advantageous in certain applications.
  • flow channel diameter should preferably be large enough to allow unrestricted passage of the largest expected fuel droplet. Therefore in catalytic combustor applications flow channels may be as large as 1.0 millimeters in diameter or more.
  • operation with fuel droplets entering the catalyst allows plug flow operation in a downsteam thermal combustion zone even at the very low temperatures otherwise achievable only in a well mixed thermal reaction zone.
  • wall coated catalysts offer not only very high maximum operating temperatures but very low pressure drop capabilities. No obstruction in the flow path is required. Thus, wall coated catalysts are especially advantageous for very high flow velocity combustors and particularly at supersonic flow velocities.
  • the exhaust from a single cylinder gasoline engine 1 passes through exhaust line 2 into which is injected air through line 3.
  • the exhaust gas and the added air pass from line 2 into vessel 4 where swirler 5 creates strong recirculation in thermal reaction zone 7.
  • Gases exiting vessel 4 pass through catalytic element 8 into vent line 9. Reactions occurring on catalyst 8 ignite and stabilize gas phase combustion in reaction zone 7 resulting in very low emissions of carbonaceous pollutants. Gas phase reaction is stabilized even at temperatures as low as 800° Kelvin.
  • catalytic baffle plate surfaces 12 of exhaust muffler 10 promote gas phase thermal reactions in muffler 10.
  • Fuel rich exhaust gas from a small single cylinder gasoline powered spark ignition engine was passed into a thermal reactor through a swirler thereby inducing recirculation within the thermal reactor.
  • the gases exiting the thermal reactor passed through a bed comprising ten microlith catalyst elements having a platinum containing coating. Exhaust pulsations resulted in backflow surges through the catalyst back into the thermal reaction zone.
  • Addition of sufficient air to the exhaust gases for combustion of the hydrocarbons and carbon monoxide in the hot 800 ° Kelvin exhaust gases before the exhaust gases entered the thermal reactor resulted in better than 90 percent destruction of the hydrocarbons present and a carbon monoxide concentration of less than 0.5 percent in the effluent from the thermal reactor entering the catalyst bed.
  • the temperature rise in the thermal reactor was greater than 200 ° Kelvin.
  • Example II Using the same system as in Example I, tests were run in the absence of the microlith catalyst bed. Addition of air to the hot exhaust gases yielded essentially no conversion of hydrocarbons or carbon monoxide. Reactor exit temperature was lower than the 800° Kelvin engine exhaust temperature.
  • Example II In place of the reaction system of Example I, tests were run with the same engine in which a coating of platinum metal catalyst was applied to the internal walls of the engine muffler with the muffler serving as a stirred thermal reactor. As in example I, addition of sufficient air for combustion resulted in stable thermal combustion. With sufficient air for complete combustion of all fuel values, the measured exhaust emis- sisions as a function of engine load were:
  • Lean gas phase combustion of Jet-A fuel is stabilized by spraying the fuel into flowing air at a temperature of 750 ° Kelvin and passing the resulting fuel-air mixture through a platinum activated microlith catalyst.
  • the fuel-air mixture is ignited by contact with the catalyst, passed to a plug flow thermal reactor and reacts to produce carbon dioxide and water with release of heat.
  • the catalyst typically operates at a temperature in the range of about 100 Kelvin or more lower than the adiabatic flame temperature of the inlet fuel-air mixture. Efficient combustion is obtained over range of temperatures as high 2000 ° Kelvin and as low as 1100 ° Kelvin, a turndown ratio higher than existing conventional gas turbine combustors and much higher than catalytic combustors.
  • Premixed fuel and air may be added to the thermal reactor downstream of the catalyst to reduce the flow through the catalyst. If the added fuel-air mixture has an adiabatic flame temperature higher than that of the mixture contacting the catalyst, outlet temperatures at full load much higher than 2000 ° Kelvin can be obtained with operation of the catalyst maintained at a temperature lower than 1200 ° Kelvin.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Combustion & Propulsion (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Health & Medical Sciences (AREA)
  • Toxicology (AREA)
  • Exhaust Gas After Treatment (AREA)
EP94115017A 1994-02-17 1994-09-23 Katalytisches Verfahren. Withdrawn EP0668471A3 (de)

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
US197890 1989-01-13
US08/197,890 US5437152A (en) 1991-01-09 1994-02-17 Catalytic method
US08/197,931 US5593299A (en) 1991-01-09 1994-02-17 Catalytic method
US197931 1994-02-17

Publications (2)

Publication Number Publication Date
EP0668471A2 true EP0668471A2 (de) 1995-08-23
EP0668471A3 EP0668471A3 (de) 1997-06-11

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Family Applications (1)

Application Number Title Priority Date Filing Date
EP94115017A Withdrawn EP0668471A3 (de) 1994-02-17 1994-09-23 Katalytisches Verfahren.

Country Status (2)

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EP (1) EP0668471A3 (de)
JP (1) JPH07243325A (de)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP2947290A1 (de) * 2014-05-20 2015-11-25 GE Jenbacher GmbH & Co. OG Verfahren zur abgasnachbehandlung
US9771892B2 (en) 2014-05-20 2017-09-26 Ge Jenbacher Gmbh & Co Og Method of starting up a thermoreactor
US10801381B2 (en) 2015-09-04 2020-10-13 Innio Jenbacher Gmbh & Co Og Exhaust gas after treatment device

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1476475A1 (de) * 1964-07-10 1969-05-08 Allan Aronsohn Abgasverbrenner
US3976432A (en) * 1972-08-22 1976-08-24 Osterreichische Mineralolverwaltung Aktiengesellschaft Reactor having an austenite steel catalyst for purifying flue gas
JPH02238206A (ja) * 1989-03-10 1990-09-20 Sakai Chem Ind Co Ltd 接触燃焼方法とその燃焼装置
US5051241A (en) * 1988-11-18 1991-09-24 Pfefferle William C Microlith catalytic reaction system
JPH0415410A (ja) * 1990-05-09 1992-01-20 Central Res Inst Of Electric Power Ind 触媒燃焼器
JPH062849A (ja) * 1992-06-22 1994-01-11 Central Res Inst Of Electric Power Ind 触媒燃焼器

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1476475A1 (de) * 1964-07-10 1969-05-08 Allan Aronsohn Abgasverbrenner
US3976432A (en) * 1972-08-22 1976-08-24 Osterreichische Mineralolverwaltung Aktiengesellschaft Reactor having an austenite steel catalyst for purifying flue gas
US5051241A (en) * 1988-11-18 1991-09-24 Pfefferle William C Microlith catalytic reaction system
JPH02238206A (ja) * 1989-03-10 1990-09-20 Sakai Chem Ind Co Ltd 接触燃焼方法とその燃焼装置
JPH0415410A (ja) * 1990-05-09 1992-01-20 Central Res Inst Of Electric Power Ind 触媒燃焼器
JPH062849A (ja) * 1992-06-22 1994-01-11 Central Res Inst Of Electric Power Ind 触媒燃焼器

Non-Patent Citations (3)

* Cited by examiner, † Cited by third party
Title
PATENT ABSTRACTS OF JAPAN vol. 014, no. 556 (M-1057), 11 December 1990 & JP 02 238206 A (SAKAI CHEM IND CO LTD), 20 September 1990, *
PATENT ABSTRACTS OF JAPAN vol. 016, no. 169 (M-1239), 23 April 1992 & JP 04 015410 A (CENTRAL RES INST OF ELECTRIC POWER IND;OTHERS: 01), 20 January 1992, *
PATENT ABSTRACTS OF JAPAN vol. 018, no. 196 (M-1589), 6 April 1994 & JP 06 002849 A (CENTRAL RES INST OF ELECTRIC POWER IND;OTHERS: 01), 11 January 1994, *

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP2947290A1 (de) * 2014-05-20 2015-11-25 GE Jenbacher GmbH & Co. OG Verfahren zur abgasnachbehandlung
US9657619B2 (en) 2014-05-20 2017-05-23 Ge Jenbacher Gmbh & Co Og Method of exhaust gas aftertreatment
US9771892B2 (en) 2014-05-20 2017-09-26 Ge Jenbacher Gmbh & Co Og Method of starting up a thermoreactor
US10801381B2 (en) 2015-09-04 2020-10-13 Innio Jenbacher Gmbh & Co Og Exhaust gas after treatment device

Also Published As

Publication number Publication date
JPH07243325A (ja) 1995-09-19
EP0668471A3 (de) 1997-06-11

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