EP2077378A1 - Procédé et dispositif de traitement des gaz d'échappement d'un dispositif de combustion - Google Patents

Procédé et dispositif de traitement des gaz d'échappement d'un dispositif de combustion Download PDF

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Publication number
EP2077378A1
EP2077378A1 EP08100134A EP08100134A EP2077378A1 EP 2077378 A1 EP2077378 A1 EP 2077378A1 EP 08100134 A EP08100134 A EP 08100134A EP 08100134 A EP08100134 A EP 08100134A EP 2077378 A1 EP2077378 A1 EP 2077378A1
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EP
European Patent Office
Prior art keywords
ammonia
exhaust gas
precursor
converter
anyone
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Withdrawn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
EP08100134A
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German (de)
English (en)
Inventor
Brendan Carberry
Albert Chigapov
Alexei Dubkov
Robert Ukropec
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.)
Ford Global Technologies LLC
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Ford Global Technologies LLC
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 Ford Global Technologies LLC filed Critical Ford Global Technologies LLC
Priority to EP08100134A priority Critical patent/EP2077378A1/fr
Publication of EP2077378A1 publication Critical patent/EP2077378A1/fr
Withdrawn legal-status Critical Current

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    • 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 ; Methods of operation or control of catalytic converters
    • 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
    • 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
    • F01N2240/00—Combination or association of two or more different exhaust treating devices, or of at least one such device with an auxiliary device, not covered by indexing codes F01N2230/00 or F01N2250/00, one of the devices being
    • F01N2240/25—Combination or association of two or more different exhaust treating devices, or of at least one such device with an auxiliary device, not covered by indexing codes F01N2230/00 or F01N2250/00, one of the devices being an ammonia generator
    • 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
    • F01N2610/00—Adding substances to exhaust gases
    • F01N2610/02—Adding substances to exhaust gases the substance being ammonia or urea
    • 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
    • F01N2610/00—Adding substances to exhaust gases
    • F01N2610/10—Adding substances to exhaust gases the substance being heated, e.g. by heating tank or supply line of the added substance

Definitions

  • the invention relates to a method and a device for treating an exhaust gas of a combustion device.
  • the invention relates to a device and method for producing ammonia and controlled delivering thereof to an exhaust gas flow, particularly but not exclusively to an exhaust gas flow of an internal combustion engine (ICE) for reducing NOx contained in this exhaust gas flow, in particularly on a SCR-catalyst.
  • ICE internal combustion engine
  • the invention is particularly applied to automotive applications, in particular diesel engines, the invention can also be applied to stationary diesel engines as well as in industry, power plants and fuel cell applications which are using ammonia.
  • Ammonia is known as a selective and effective reduction agent for the selective catalytic reduction (SCR) of nitrogen oxides in oxygen-containing exhaust gases from burners in power plants, from internal combustion engines etc.
  • SCR selective catalytic reduction
  • ammonia is generated on-board as a reduction agent by hydrolysis of urea.
  • EP 0 487 886 B1 discloses a method of quantitative hydrolysis of urea, wherein an aqueous urea solution is sprayed onto an evaporator and forwarded via a hydrolysis catalyst at the surface of the evaporator, and a hydrolysis catalyst being coated with active components catalyzing the quantitative hydrolysis of urea into ammonia and CO 2 and inhibiting the formation of solid urea reaction by-products.
  • a urea-using procedure causes large equipment costs due to the hydrolysis catalyst, the energy supply for urea decomposition and hydrolysis, as well as due to the transportation of urea and its introduction, which must be uniform over the cross section of the flow.
  • a further disadvantage is the formation of undesirable by-products such as, for example isocyanic acid, and cyanuric acid, and in addition the formation of polymeric products blocking urea converter and catalyst.
  • DE 34 22 175 A1 and DE 42 00 514 A1 disclose processes related to the "just-in-time" production of NH 3 for the reduction of NO x .
  • the concept comprises using specific substances which hydro-thermally decompose to NH 3 , the handling and toxicity of which being quite safe, in order to release the required quantity of NH 3 in accordance with the particular requirements and to inject the same into the exhaust gas flow.
  • the generation of NH 3 takes place by heating ammonia generating compounds as e. g. ammonium carbamate.
  • the adaptation to the particular operating state of the motor, as described in DE 34 22 175 A1 takes place by controlling the calorific power which e.g. acts on the carbamate.
  • the NH 3 generation and thus the NH 3 quantity added to the exhaust gas flow can be regulated.
  • US 6 399 034 B1 discloses a process and device for NO x -reduction of exhaust gases of an internal combustion engine using a SCR-catalyst, wherein substances are used which are decomposing to NH 3 substantially free of residues under hydrothermal conditions, such as e.g. ammonium carbamate (NH 2 CO 2 NH 4 ), as well as substances which are able to reversibly NH 3 -absorb/desorb and thus splitting off NH 3 , such as e.g. iron (II) ammine sulphate.
  • substances are used which are decomposing to NH 3 substantially free of residues under hydrothermal conditions, such as e.g. ammonium carbamate (NH 2 CO 2 NH 4 ), as well as substances which are able to reversibly NH 3 -absorb/desorb and thus splitting off NH 3 , such as e.g. iron (II) ammine sulphate.
  • EP 1 263 520 B1 discloses the use of solid reducing agent as ammonium carbamate and for example ammonium salts as ammonium carbonate, ammonium formate for thermolysis into ammonia in SCR-applications.
  • the reducing agent is brought into physical contact with a hot liquid heat transfer agent.
  • the gas After gas formation, the gas is held in a gas collecting chamber and is fed in a controlled manner into the exhaust gas flow. Furthermore, the pumping power and/or the heating power and/or the amount of reduction agent fed into the exhaust gas are controlled by virtue of a controller.
  • EP 1 323 903 B1 also discloses the use of ammonium carbonate in order to produce ammonia in the same field of use, but as a solid mixture with heat carrier substance. Using such carrier substances can create problems like depositions or blockage. Vapours of these carrier substances could deposit on the SCR catalyst, which could have influence on the SCR catalyst activity and seriously decrease activity of SCR catalyst.
  • a method of treating an exhaust gas of a combustion device, wherein the exhaust gas is treated with ammonia (NH 3 ) which is produced by decomposition of a precursor comprising ammonium carbonate (NH 4 ) 2 CO 3 ), comprises the steps of:
  • a flow through pressure-tight converter (which could be heated if needed) is provided as a NH 3 source, wherein a precursor comprising ammonium carbonate being located in said converter produces ammonia via maintaining equilibrium gas composition in the converter with gas flow.
  • ammonium carbonate (NH 4 ) 2 CO 3 ), according to the present invention, as precursor for ammonia (NH 3 ) can be summarized as follows:
  • the flow through pressure tight converter does not need to be heated, but could be slightly heated, if needed, with heating coils being placed around the converter and/or inside the converter. Principally, the relatively low temperature range of the ammonium carbonate equilibrium decomposition makes it possible to use just the part of the exhausted gas flow, or if needed use also heat sources attributed to the engine. Although the electrical heating is not necessary, it is advantageous in situations where a faster ammonia release at start or cold start conditions is required.
  • the ammonia being produced from said precursor is subsequently placed and stored in a reservoir such as a storage vessel.
  • a reservoir such as a storage vessel.
  • the ammonium storage vessel enables to have gaseous ammonia available even during conditions of intermittent engine operation and/or during start phases, regardless of a possible heating phase of the converter (when there is insufficient energy for heating the precursor).
  • the intermediate amount of ammonia prepared and stored in a compensation vessel or more vessels may be small such, that it cannot create any harmful emissions in case of a hypothetical destruction of the device due to an accident.
  • the production of ammonia and/or the injection of ammonia into the exhaust flow is controlled depending on the engine operating characteristics and/or depending on a NO x -concentration in the exhaust gas, such that a specific quantity of ammonia required for an appropriate reduction of NO x -gases in the exhaust gases may be injected and such that the production/injection may be timely terminated if necessary.
  • the storage vessel preferably acts as a dosing device.
  • the dosing may be performed based upon control signals from a control unit processing in dependence on the engine characteristics, the NO x -gases concentration in the exhaust gas and the NO x -output exhaust concentration, its temperature and the temperature of converter.
  • the inventive method in order to supply a sufficient amount of ammonia as reducing agent for oxides of nitrogen, comprises maintaining a certain sufficient flow of the part of exhaust gas, pressure in the reactor chamber for ammonium carbonate decomposition and/or additional buffer chamber by controlling gas flow and additional amount of ammonium carbonate on demand of required amount of ammonia, and controlling temperature of converter.
  • Evolved gaseous NH 3 is produced at the rate essentially balanced to the amount of nitrogen oxides in the gas stream and in accordance with system strategy requirements.
  • the heat generated during the operation of the internal combustion engine can be additionally used for the process of decomposition to ammonia by making use of the heat of cooling water or oil. Additionally the electrical heating can be used especially for a cold start.
  • the intermediate storage of ammonia can be realized in the decomposition reactor vessel itself or in a separate vessel with specific volume, pressure and temperature accommodating the sufficient amount of ammonia able to support efficient NOx removal.
  • the supply of the part of exhaust gas to converter, and the dosing device can be equipped with valves allowing reduction of the pressure and supplying a required dosing quantity of ammonia.
  • the dosing is preferably controlled according to a given strategy by a programmed unit. Preferably such a strategy does not allow an injection of high quantities of ammonia which would lead to the slip of unconsumed ammonia out of the catalyst.
  • the converter allows easy addition of new substance or mixture of substances, when a part or almost all previous charge is consumed.
  • the converter is preferably equipped and fitted with quick fasteners allowing its quick recharge with fresh substance or its removal or replacement.
  • the amount of the heat supply (only when needed) is regulated according to amount of ammonia needed and in line with a strategy for removal of NO x -gases from engine exhaust gas.
  • the method according to the present invention with the features of the main claim has the advantage over the related art that a gaseous reduction agent is provided which can be accurately metered, and does not cause the freezing problems in winter operation. It does not cool exhaust gas and therefore does not require minimal temperature limit to avoid formation of deposits and to prevent the poor low-temperature performance of SCR-catalyst.
  • the invention also relates to a device for treating an exhaust flow of a combustion device, wherein the exhaust gas is treated with ammonia (NH 3 ) which is produced by decomposition of a precursor comprising ammonium carbonate ((NH 4 ) 2 CO 3 ), wherein said device is adapted to perform a method as described above.
  • ammonia NH 3
  • ammonium carbonate (NH 4 ) 2 CO 3 )
  • Fig. 1 shows a schematic diagram of a preferred embodiment of a device according to the present invention, wherein the principle of producing ammonia and injecting said ammonia into the exhaust stream of a diesel engine is illustrated.
  • the device 1 comprises from a converter 2, a line 11 for a part of exhaust gas, equipped with a valve 14 for controlling gas flow, a supply line 3 for introducing NH 3 into and exhaust gas flow 4 of a diesel engine 5, a valve 6 provided as a dosing device as well as a SCR catalyst 7 being arranged in said exhaust gas flow 4 downstream of the diesel engine 5.
  • the converter 2 is filled with sufficient amount of ammonium carbonate (NH 4 ) 2 CO 3 ) or with a mixture of ammonium carbonate with ammonium hydrogen carbonate and/or ammonium carbamate from a reservoir 8.
  • the reservoir 8 may be selectively isolated from or connected to the converter 2 via a valve 10.
  • the converter 2 usually operates at ambient temperature, but is equipped with heating coils 12, being placed around the converter 2 and/or inside the converter 2, as well as an additional electrical heater 13, to proper adjust temperature of the converter 2 if needed, in order to liberate a sufficient amount of ammonia from the ammonium precursor or the mixture of precursors until the gas equilibrium and pressure inside the converter 2 and/or the additional storage reservoir (or reservoirs) reaches a level which is needed to supply required amount of ammonia to the exhaust gas flow 4 in order to achieve an efficient catalytic removal of nitrogen oxides.
  • the process is controlled by a processing unit 9.
  • the processing unit 9 particularly controls the introduction of part of exhaust gas to the converter and the gaseous ammonia into the exhaust gas flow 4 using the valve 6.
  • the process control can be based on the performance of the engine 5 and/or the measured level of nitrogen oxides (NO x ) exiting the SCR-catalyst 7. In case that an additional amount of precursor is needed, such an additional amount of precursor can be introduced from the reservoir 8 via (opened) valve 10 to the converter 2.
  • the control of the part of the exhaust gas flow and pressure control is allowing also safety control of the system, providing the control to stop an overproduction of ammonia. Under idle engine conditions, i. e. when an ammonia supply is not required, the part of the exhaust gas flow will be shut down and valve 6 can be in its closed position.
  • ammonia from the ammonium carbonate precursor is to spray or dose small particles or dust of ammonium carbonate from the reservoir 8 into the preheated converter 2 (or more than one converter 2 used alone or subsequently), such that all precursor material will decompose and will release ammonia, which can subsequently be dosed into the exhaust stream by the dosing valve 6 as already described above.
  • the electrical heating is not necessary, it is advantageous in situations where a more quick ammonia release during cold start conditions is required.
  • the relatively low temperature range of the ammonium carbonate equilibrium decomposition makes it also possible to use just the part of the exhausted gas flow, or if needed use heat sources attributed to the engine such as cooling water and/or oil.
  • an advantage of using ammonium carbonate ((NH 4 ) 2 CO 3 ) and/or its mixtures compared to ammonium carbamate (NH 2 CO 2 NH 4 ) is that the temperature range of decomposition of ammonium carbonate ((NH 4 ) 2 CO 3 ) to ammonia starts approximately at 50°C, which is higher by (10-15)°C compared to ammonium carbamate decomposition, and finishes approximately at a temperature higher by 30°C (almost at 170°C) if compared to the ammonium carbamate (see Fig.
  • ammonium carbamate starts to decompose at 30°C with peak at 80°C (see dashed line in Fig. 3 ) This makes it potentially risky to use a source of ammonia because of stability at rather lower temperatures. Furthermore, the decomposition of ammonium carbamate produces small amounts of by-products, as can be seen in Fig. 2 from the tailing of ammonium carbamate decomposition curve (though much less pronounced compared e. g. with urea). By using ammonium carbonate ((NH 4 ) 2 CO 3 ), the weight loss is complete, which evidences a complete decomposition without the formation of additional side products.
  • ammonium carbonate at room temperature by flow of gas via the converter filled with adequate amount of ammonium carbonate.
  • ammonium carbonate is proportional to certain extend with amount of ammonium carbonate (as shown in Fig. 5 ).
  • ammonium salts such as ammonium hydrogen carbonate, ammonium carbamate, ammonium formate, and their mixtures.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • Toxicology (AREA)
  • Combustion & Propulsion (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Exhaust Gas After Treatment (AREA)
EP08100134A 2008-01-07 2008-01-07 Procédé et dispositif de traitement des gaz d'échappement d'un dispositif de combustion Withdrawn EP2077378A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP08100134A EP2077378A1 (fr) 2008-01-07 2008-01-07 Procédé et dispositif de traitement des gaz d'échappement d'un dispositif de combustion

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
EP08100134A EP2077378A1 (fr) 2008-01-07 2008-01-07 Procédé et dispositif de traitement des gaz d'échappement d'un dispositif de combustion

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102817681A (zh) * 2012-07-26 2012-12-12 北京理工大学 柴油机固体scr控制系统
CN103437866A (zh) * 2013-07-25 2013-12-11 吉林大学 为车用选择性催化还原系统全工况提供还原剂方法及装置

Citations (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE3422175A1 (de) 1984-06-04 1985-12-19 Julius Dr. 8000 München Kern Verfahren zur beimischung von ammoniak zu saure schadstoffe enthaltenden abgasen oder luft
JPS62262729A (ja) * 1986-05-09 1987-11-14 Mitsubishi Heavy Ind Ltd 排ガス中の窒素酸化物の除去方法
DE4200514A1 (de) 1992-01-11 1993-07-15 Asea Brown Boveri Verfahren zur katalytischen entstickung von abgasen
JPH05272331A (ja) * 1992-03-25 1993-10-19 Hino Motors Ltd 排ガス浄化装置およびその排ガス浄化装置に使用される還元剤供給方法および装置
EP0487886B1 (fr) 1990-11-29 1994-04-13 MAN Nutzfahrzeuge Aktiengesellschaft Procédé et installation pour la réduction catalytique sélective de NOx des gaz d'échappement contenant de l'oxygène
JP2001157822A (ja) * 1999-12-03 2001-06-12 Mitsui Chemicals Inc 燃焼排ガス中の窒素酸化物の除去方法
US6399034B1 (en) 1997-05-14 2002-06-04 Hjs Fahrzeugtechnik Gmbh & Co. Process for reducing nitrogen oxides on SCR catalyst
EP1323903B1 (fr) 2001-12-29 2005-08-10 Robert Bosch Gmbh Dispositif de traitement des gaz d'échappement d'un dispositif de combustion
EP1263520B1 (fr) 2001-01-13 2007-01-03 FEV Motorentechnik GmbH Procede permettant de transformer un agent de reduction azote solide en phase gazeuse pour reduire les oxydes d'azote des gaz d'echappement

Patent Citations (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE3422175A1 (de) 1984-06-04 1985-12-19 Julius Dr. 8000 München Kern Verfahren zur beimischung von ammoniak zu saure schadstoffe enthaltenden abgasen oder luft
JPS62262729A (ja) * 1986-05-09 1987-11-14 Mitsubishi Heavy Ind Ltd 排ガス中の窒素酸化物の除去方法
EP0487886B1 (fr) 1990-11-29 1994-04-13 MAN Nutzfahrzeuge Aktiengesellschaft Procédé et installation pour la réduction catalytique sélective de NOx des gaz d'échappement contenant de l'oxygène
DE4200514A1 (de) 1992-01-11 1993-07-15 Asea Brown Boveri Verfahren zur katalytischen entstickung von abgasen
JPH05272331A (ja) * 1992-03-25 1993-10-19 Hino Motors Ltd 排ガス浄化装置およびその排ガス浄化装置に使用される還元剤供給方法および装置
US6399034B1 (en) 1997-05-14 2002-06-04 Hjs Fahrzeugtechnik Gmbh & Co. Process for reducing nitrogen oxides on SCR catalyst
JP2001157822A (ja) * 1999-12-03 2001-06-12 Mitsui Chemicals Inc 燃焼排ガス中の窒素酸化物の除去方法
EP1263520B1 (fr) 2001-01-13 2007-01-03 FEV Motorentechnik GmbH Procede permettant de transformer un agent de reduction azote solide en phase gazeuse pour reduire les oxydes d'azote des gaz d'echappement
EP1323903B1 (fr) 2001-12-29 2005-08-10 Robert Bosch Gmbh Dispositif de traitement des gaz d'échappement d'un dispositif de combustion

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102817681A (zh) * 2012-07-26 2012-12-12 北京理工大学 柴油机固体scr控制系统
CN103437866A (zh) * 2013-07-25 2013-12-11 吉林大学 为车用选择性催化还原系统全工况提供还原剂方法及装置

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