EP1204458A1 - Method for removing nitrogen oxides from an oxygen-containing gas stream - Google Patents

Method for removing nitrogen oxides from an oxygen-containing gas stream

Info

Publication number
EP1204458A1
EP1204458A1 EP00941030A EP00941030A EP1204458A1 EP 1204458 A1 EP1204458 A1 EP 1204458A1 EP 00941030 A EP00941030 A EP 00941030A EP 00941030 A EP00941030 A EP 00941030A EP 1204458 A1 EP1204458 A1 EP 1204458A1
Authority
EP
European Patent Office
Prior art keywords
stream
oxygen
hydrocarbons
gas stream
catalyst
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Withdrawn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
EP00941030A
Other languages
German (de)
English (en)
French (fr)
Inventor
Sytse Jelle Jelles
Willem Hendrik Bouwman
Petrus Franciscus M. Th. Van Nisselrooij
Renee Van Yperen
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.)
Gastec NV
Original Assignee
Gastec NV
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 Gastec NV filed Critical Gastec NV
Publication of EP1204458A1 publication Critical patent/EP1204458A1/en
Withdrawn legal-status Critical Current

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Classifications

    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10Exhaust 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
    • F01N3/18Exhaust 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
    • F01N3/20Exhaust 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
    • F01N3/2066Selective catalytic reduction [SCR]
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D53/00Separation 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
    • B01D53/34Chemical or biological purification of waste gases
    • B01D53/74General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86Catalytic processes
    • B01D53/8621Removing nitrogen compounds
    • B01D53/8625Nitrogen oxides
    • B01D53/8631Processes characterised by a specific device
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D53/00Separation 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
    • B01D53/34Chemical or biological purification of waste gases
    • B01D53/92Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B01D53/9404Removing only nitrogen compounds
    • B01D53/9409Nitrogen oxides
    • B01D53/9431Processes characterised by a specific device
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/0807Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by using absorbents or adsorbents
    • F01N3/0871Regulation of absorbents or adsorbents, e.g. purging
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/38Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
    • B01J23/40Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/74Iron group metals
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2240/00Combination 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
    • F01N2240/25Combination 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
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2240/00Combination 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
    • F01N2240/30Combination 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 a fuel reformer
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2610/00Adding substances to exhaust gases
    • F01N2610/02Adding substances to exhaust gases the substance being ammonia or urea
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2610/00Adding substances to exhaust gases
    • F01N2610/03Adding substances to exhaust gases the substance being hydrocarbons, e.g. engine fuel
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01NGAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2610/00Adding substances to exhaust gases
    • F01N2610/04Adding substances to exhaust gases the substance being hydrogen
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02TCLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00Road transport of goods or passengers
    • Y02T10/10Internal combustion engine [ICE] based vehicles
    • Y02T10/12Improving ICE efficiencies

Definitions

  • This invention relates to a catalytic conversion of nitrogen oxides to molecular nitrogen, which nitrogen oxides are formed upon combustion of hydrocarbons and/or synthesis gas (H2/CO). More particularly, it relates to the conversion of nitrogen oxides in the presence of oxygen such as these are formed, for instance, in the operation of units such as combustion engines under so-called poor or 'lean-burn' conditions, that is: under combustion conditions where an excess of oxygen is present.
  • the invention further relates to the conversion of nitrogen oxides which may be formed in industrial processes, such as nitric acid production. In the combustion of hydrocarbons with molecular oxygen (for instance originating from air), oxides of nitrogen may be formed due to the prevailing temperature and pressure during the combustion process. These nitrogen oxides, among which NO and NO 2 (usually denoted by NOx) are very harmful to the environment. Nitrogen oxides are held responsible inter alia for the formation of acid rain and photochemical smog.
  • Reducing NO x emission in stoichiometrically running engines is often accomplished by making use of a so-called three-way catalyst system.
  • the NOx conversion catalyst in such systems is capable of converting nitrogen oxides to harmless compounds by reacting them with the reducing combustion products present in the exhaust gas, such as hydrocarbons and CO, to form N 2 .
  • reductants for the SCR reaction are ammonia and urea.
  • hydrocarbons such as ethylene, propylene and propane as reductant (see, for instance, G.P. Ansell et al, 'Mechanism of the lean NOx reaction over Cu/ZSM-5', Appl. Catal. B, 2 (1993), pp. 81-100).
  • Other possible reductants are, for instance, CO, H2 and CH , ethanol, hydrocarbons, in particular fuels such as gasoline and diesel oil.
  • DE-A-44 04 617 a technique is described whereby, using an electrically heated reactor, a hydrocarbon-containing fuel is catalytically cracked at 200 to 700°C and the cracking products are further activated with air before they are added as reducing agent to the exhaust gas, whereupon the total gas stream is passed over an SCR catalyst.
  • cracked hydrocarbons are used as reducing agent. These hydrocarbons have been obtained from diesel.
  • hydrogen is added to the exhaust gas to reduce NOx over the SCR catalyst where the cracked hydrocarbons are not sufficiently active.
  • the hydrogen originates from a storage tank or is made through electrolysis or methanol reforming.
  • hydrocarbons are converted to a reductant stream under suitable conditions, optionally by contacting them with a reductant forming catalyst.
  • the hydrocarbons in the product stream of the reductant forming step can be unreacted hydrocarbons from the feedstock of this step, but may also be smaller hydrocarbons which have been formed by cracking reactions during the reductant forming step.
  • the reductants can be prepared, by the use of a reductant forming catalyst, from, for instance, residues of hydrocarbons which are contained in the exhaust gas of the unit in which the combustion takes place. It is also possible to draw these hydrocarbons from a different source, for instance the fuel for the combustion unit, which is already available in situ. Combinations of effluent and such a different source are naturally also possible.
  • the oxygen needed for this step at least partly originates from the off-gas to be treated, i.e., the nitrogen oxide- and oxygen-containing gas. Preferably, substantially all oxygen present in the part of the off-gas used for the reductant formation is used for forming the reducing gas stream.
  • the hydrocarbons present in this portion of the off-gas can also be converted to reducing compounds in this step.
  • the hydrocarbons present in the off-gas can then also be converted to reducing compounds in this step.
  • the reductants necessary for the catalytic reduction of NOx in the form of CO and/or H2, optionally supplemented with hydrocarbons, can be prepared from hydrocarbons in situ, so that the above-outlined drawbacks in removing NOx under oxygen-rich conditions can be eliminated at least partly.
  • ammonia can be formed in the presence of hydrogen and nitrogen, under suitable process conditions, because of the position of the chemical equilibrium
  • Another advantage is that no pure H 2 or H 2 with small amounts of carbon monoxide needs to be produced. As a consequence, it is possible to omit shift reactors and membrane technology.
  • the reductant forming step can be a partial oxidation step, in which use can be made of a partial oxidation catalyst.
  • the reductant forming step can be a steam reforming step in which use is made of a steam reforming catalyst.
  • a suitable reductant forming catalyst is, for instance, a partial oxidation catalyst. In the presence of such a catalyst, the partial oxidation of hydrocarbons takes place.
  • the oxygen needed for this partial oxidation is derived from the effluent of the combustion unit, optionally supplemented with oxygen obtained from elsewhere, coming, for instance, from added air.
  • the product stream of the partial oxidation step is highly suitable for use as reductant stream.
  • steam reforming in addition to hydrocarbons, water is to be added to the steam reforming step. This water may originate from the effluent of the combustion engine, from a separate stock, or from a combination of these two sources.
  • hydrocarbons are converted with water (steam) to a mixture of hydrocarbons, such as methane, and/or H2 and CO2.
  • hydrocarbons such as methane, and/or H2 and CO2.
  • CO may also be present.
  • the mixture thus formed is very suitable to be used as a reductant stream.
  • the reductant stream together with the effluent of the combustion unit, is contacted with a deNOx catalyst so that the desired conversion of nitrogen oxides takes place.
  • the in situ production of the reductant offers a number of important advantages.
  • the supply of reductants can take place continuously, in the case of natural gas, or in any case simultaneously with the supply of the fuel for the combustion unit, and it is no longer necessary to have and maintain a separate stock thereof.
  • This can be practical, for instance, when used in mobile combustion units, such as trucks or passenger cars, because then no separate storage tanks for the reducing agent need to be present.
  • This may also be an important advantage in stationary units.
  • the fact that no ammonia and urea (whether or not as a urea solution) are used, at least do not need to be drawn from elsewhere, is also an advantage because the above-outlined disadvantages associated with the use of these reductants no longer occur.
  • Another advantage of the invention arises if hydrocarbons from the effluent of the combustion unit are used as feedstock for the reductant forming step, as a result of which the amounts of hydrocarbons in the exhaust gas will then be lowered in that they are used for the reaction with NOx. Such a reduction is favorable, since the emission of hydrocarbons is undesirable from an environmental point of view.
  • Another advantage of the use of the effluent of the combustion unit for the formation of the reducing gas is the decrease of the amount of hydrocarbons needed for the reductant formation.
  • the present invention is characterized by a method for reducing the content of nitrogen oxides in a nitrogen oxide- and oxygen- containing gas stream by contacting this gas stream in the presence of a deNOx catalyst with a reducing gas stream, which comprises CO, H 2 and possibly NH3 and which reducing gas stream has been obtained by converting hydrocarbons with the oxygen from the nitrogen oxide- and oxygen-containing gas stream, optionally in the presence of a reductant forming catalyst.
  • the nitrogen oxide- and oxygen-containing gas stream is the effluent of a step for combusting fuels, which comprises the steps of feeding at least a stream a) comprising one or more fuels and a stream b) containing excess oxygen with respect to the fuel, which further comprises nitrogen, wherein the effluent, together with the reducing gas stream c) which further optionally comprises one or more hydrocarbons, is contacted with the deNOx catalyst, wherein to stream c) no ammonia and no urea is added and wherein stream c) has been substantially obtained by contacting streams d) and e) with the reductant forming catalyst, stream d) comprising one or more hydrocarbons and stream e) comprising oxygen and water.
  • the combustion unit is suitable for generating heat, and optionally energy.
  • the combustion unit can work on the basis of a flame, but the combustion in the combustion unit can also proceed by catalytic route.
  • the combustion unit is a gas engine, gas turbine, diesel engine or gasoline engine.
  • a stream c) which is substantially free from externally added ammonia and urea is understood to mean that to this stream, in accordance with the invention, no reductants of this type need to be added. Still, ammonia and possibly compounds derived therefrom, such as urea, can be present as a result of the above-mentioned equilibrium reaction of N2 and H 2 .
  • the NO x is reduced with a mixture of H 2> CO and possibly NH3.
  • hydrocarbons which have not been (entirely) converted can be present in the reducing gas stream. These hydrocarbons also work as reductants.
  • the reducing gas mixture is obtained by converting the hydrocarbons from a part of the exhaust gas stream with optionally extra added hydrocarbons, by means of (catalytic) partial oxidation, steam reforming or a combination of both technologies by means of the oxygen and water vapor present in the same part of the exhaust gas stream and optionally externally added air and/or water vapor.
  • extra reducing agent such as hydrogen can be added to the reducing gas mixture obtained.
  • the method and the apparatus suitable therefor according to the invention wherein the engine comprises a heat exchanger, such that at least a portion of the heat released upon the combustion can be usefully employed, for instance for heating, as of greenhouses or other spaces.
  • Such units in which at the same time both heat and energy are generated, the energy being typically in the form of electrical power, are also referred to as combined heat and power units or total energy plants.
  • the invention can also be applied in various means of transport such as vessels, airplanes, trucks and passenger cars and trains provided with a hydrocarbon-fired locomotive engine.
  • the method according to the invention and the apparatuses suitable therefor is suitable in particular for operating combustion units under so-called lean-burn conditions, i.e., conditions where the ratio between the streams a) and b) is selected such that the amount of oxygen is at least the amount needed for the complete combustion of the fuels in stream a).
  • lean-burn conditions i.e., conditions where the ratio between the streams a) and b) is selected such that the amount of oxygen is at least the amount needed for the complete combustion of the fuels in stream a).
  • Suitable fuels for the feedstock a) are hydrocarbons and/or synthesis gas (CO/H2 mixture).
  • the hydrocarbons for the reductant forming step are at least partly drawn from the same source as the fuel for the combustion unit.
  • stream a) and stream d) comprise the same components.
  • the hydrocarbons that are present in the effluent of the combustion unit are at least partly used as feedstock for the reductant forming step, which may or may not be supplemented with a hydrocarbon stream drawn from elsewhere.
  • the effluent of the combustion unit is used as oxygen source, which may or may not be supplemented with an oxygen stream drawn from elsewhere.
  • hydrocarbons suitable therefor can be used. It is practically preferred, however, when the hydrocarbons from stream a) and d) are selected independently from the group consisting of natural gas (which comprises substantially methane), methane, diesel oil, gasoline, fuel oil, methanol, ethanol, naphtha, kerosene, ethane, propane, butane, LPG, derivatives and mixtures thereof.
  • the catalyst for converting nitrogen oxides can be selected from the group of catalysts which catalyze the reduction of NOx, such as the conventional catalysts for removal of NOx.
  • these are selected from the group comprising zeolites, metal-exchanged zeolites, such as Co-, Cu- and/or Ce-exchanged zeolites, Pt, Rh and/or Ir catalyst, optionally provided on a support such as a washcoat which may further comprise Ba, La, Y, Sr, Pr, Ce, Si, Ti, Al and/or Zr.
  • metal-exchanged zeolites such as Co-, Cu- and/or Ce-exchanged zeolites, Pt, Rh and/or Ir catalyst
  • a support such as a washcoat which may further comprise Ba, La, Y, Sr, Pr, Ce, Si, Ti, Al and/or Zr.
  • the catalyst for the partial oxidation of hydrocarbons can be selected from the group consisting of Pt, Rh, Ru, Pd, Co and Ni, if desired provided on suitable supports such as AI2O3, SiO 2 , TiO 2 , Zr ⁇ 2, silica/alumina-zeolites and mixtures thereof, optionally stabilized with, for instance, Si, La, Ba or Y and mixtures thereof.
  • the steam reforming catalyst which is capable of converting a mixture of hydrocarbons and water to a mixture of H2, CO, CO2 and/or hydrocarbons can be any conventional steam reforming catalyst, which may or may not be supported, according to conventional techniques, as known to the skilled person.
  • the steam reforming catalyst is a supported catalyst comprising Ni, Rh and/or Pt.
  • factors such as hydrocarbon/oxygen ratio, temperature, pressure, residence time and/or amount of catalyst for the partial oxidation of hydrocarbons should be selected such that no complete oxidation takes place.
  • ⁇ po ⁇ 1.
  • ⁇ po is controllable by adjusting the air/fuel amount and is dependent on the hydrocarbons used.
  • the temperature for the reductant forming step is generally between 250 and 1100°C.
  • the residence time for the reductant forming step is generally between 200 en 150,000 h 1 .
  • the pressure will also have an influence, it is generally dictated by the other process conditions. In general, the pressure will be atmospheric or slightly higher and not higher than 50 bars.
  • a conversion curve of NO x as a function of the temperature is given, in which a conversion of 40% is achieved.
  • This is typical of SCR systems that do not work with NH3 or urea as reducing agent. Selecting the process conditions of the reductant forming step such that also NH3 is generated is therefore advantageous because then a higher NO x conversion can be achieved.
  • NO x storage system also referred to as NO x Storage and Reduction Catalyst, NSR
  • NSR NO x Storage and Reduction Catalyst
  • nitrogen oxides are absorbed from the nitrogen oxide- and oxygen-containing gas stream to a suitable absorbent and subsequently, for instance by switching, the reducing gas stream is contacted with the absorbent.
  • the deNOx step is thus operated discontinuously.
  • a very effective NOx removal can thus be obtained.
  • the catalyst in the NOx storage system can very suitably consist of platinum provided on a barium-containing and/or zeolite-comprising alumina washcoat.
  • the barium present can react with NOx to barium nitrate. This nitrate salt decomposes in a reducing medium to barium and N2.
  • the NOx storage system can be operated according to the invention by passing the exhaust gases through the NOx storage system until the system is saturated with NOx. Thereafter, regeneration can be done with a reducing agent which has been obtained as described above. Optionally, this reducing agent can be supplemented with a reduction agent drawn from elsewhere.
  • this NOx storage system is designed with minimally two parallel beds.
  • One bed is used to absorb NOx, while the other bed is regenerated.
  • the streams are switched, so that the regenerated bed can proceed to absorb NOx and the loaded NOx bed is regenerated in that the absorbed NOx is converted to nitrogen.
  • the effluent of the regeneration step of the NOx storage bed can be recirculated with advantage and, together with the inlet air, be passed to the inlet of the combustion unit (for instance a gas engine).
  • the combustion unit for instance a gas engine.
  • Both the deNOx catalyst and the reductant forming catalyst can be present in the method according to the invention in the forms known to those skilled in the art, as in the form of a bed of granules, extrusions, granules, and/or pellets, or provided on ceramic or so-called metal monoliths, or differently structured forms.
  • the use of the catalyst in structured form is preferred because this allows other relevant factors for the method, such as pressure drop, mixing, contact time, heat management, mechanical strength and life, to be tailored to the prevailing conditions through suitable choices, and the method can thereby be optimized.
  • the invention is therefore characterized by the use of a catalyst suitable for converting nitrogen oxides in combination with either a catalyst suitable for the partial oxidation of hydrocarbons, or a catalyst suitable for steam reforming, for converting nitrogen oxides in generating heat and optionally energy from hydrocarbons, without this requiring ammonia or urea to be added externally.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Environmental & Geological Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Biomedical Technology (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • General Chemical & Material Sciences (AREA)
  • Analytical Chemistry (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Toxicology (AREA)
  • Exhaust Gas After Treatment (AREA)
  • Exhaust Gas Treatment By Means Of Catalyst (AREA)
EP00941030A 1999-06-11 2000-06-13 Method for removing nitrogen oxides from an oxygen-containing gas stream Withdrawn EP1204458A1 (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
NL1012296 1999-06-11
NL1012296A NL1012296C2 (nl) 1999-06-11 1999-06-11 Werkwijze voor het verwijderen van stikstofoxiden.
PCT/NL2000/000404 WO2000076637A1 (en) 1999-06-11 2000-06-13 Method for removing nitrogen oxides from an oxygen-containing gas stream

Publications (1)

Publication Number Publication Date
EP1204458A1 true EP1204458A1 (en) 2002-05-15

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EP00941030A Withdrawn EP1204458A1 (en) 1999-06-11 2000-06-13 Method for removing nitrogen oxides from an oxygen-containing gas stream

Country Status (7)

Country Link
EP (1) EP1204458A1 (nl)
JP (1) JP2003530982A (nl)
CN (1) CN1355721A (nl)
AU (1) AU5579600A (nl)
CA (1) CA2374647A1 (nl)
NL (1) NL1012296C2 (nl)
WO (1) WO2000076637A1 (nl)

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CN102162389B (zh) * 2011-03-30 2013-03-13 北京工业大学 一种基于重整气净化发动机尾气的装置及方法
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CA2374647A1 (en) 2000-12-21
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