EP1888206A1 - Procede et dispositif pour decomposer des oxydes d'azote dans un flux de gaz d'echappement - Google Patents

Procede et dispositif pour decomposer des oxydes d'azote dans un flux de gaz d'echappement

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Publication number
EP1888206A1
EP1888206A1 EP06741033A EP06741033A EP1888206A1 EP 1888206 A1 EP1888206 A1 EP 1888206A1 EP 06741033 A EP06741033 A EP 06741033A EP 06741033 A EP06741033 A EP 06741033A EP 1888206 A1 EP1888206 A1 EP 1888206A1
Authority
EP
European Patent Office
Prior art keywords
honeycomb body
channels
ceramic
filter arrangement
electrodes
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Withdrawn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
EP06741033A
Other languages
German (de)
English (en)
Inventor
Carl M. Fleck
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.)
Individual
Original Assignee
Individual
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
Priority claimed from AT0096705A external-priority patent/AT501888B1/de
Application filed by Individual filed Critical Individual
Publication of EP1888206A1 publication Critical patent/EP1888206A1/fr
Withdrawn legal-status Critical Current

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/32—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B01D53/9404—Removing only nitrogen compounds
    • B01D53/9409—Nitrogen oxides
    • B01D53/9431—Processes characterised by a specific device
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2259/00—Type of treatment
    • B01D2259/80—Employing electric, magnetic, electromagnetic or wave energy, or particle radiation
    • B01D2259/818—Employing electrical discharges or the generation of a plasma

Definitions

  • the invention relates to a method for the operation of a filter arrangement for the decomposition of nitrogen oxides from an exhaust gas stream, wherein the exhaust gas stream is passed through extending in the longitudinal direction of a ceramic honeycomb body, open on both sides channels of the ceramic honeycomb body, and at parallel to the channels extending electrodes to a voltage the honeycomb body for generating an electric field in the channels of the honeycomb body, which is oriented in each case transversely to the longitudinal axis of the channels, is applied, according to the preamble of claim 1.
  • the invention further relates to a filter arrangement for the decomposition of nitrogen oxides from an exhaust gas flow with a ceramic honeycomb body with exhaust gas flowing through and in the longitudinal direction of the honeycomb body, open on both sides channels, which are separated from each other by webs, wherein the honeycomb body electrodes for generating an electric field in the channels of the honeycomb body, which is oriented in each case transversely to the axis of the channels, are arranged, according to the preamble of claim 6.
  • EP 0 885 647 discloses an apparatus for the dissociation of nitrogen oxides in an exhaust stream, which provides a ceramic honeycomb body in whose channels a DC electric field is generated.
  • the electrons for the dissociation of nitrogen oxides are generated in such a filter arrangement in the channels on the negative wall at a sufficiently high field strength by field emission from the rough ceramic surface, and at higher temperatures also by thermally induced emissions (Richardson effect). Further electron emission from the ceramic can be triggered by quanta generated by inelastic collisions or bremsstrahlung.
  • honeycomb body initially allows the application of higher field strengths than would be possible with a discharge space not subdivided into channels, without the formation of a preliminary spark ("streamer") and, as a consequence, sparking through of a spark Channels of the honeycomb body rather act like a plurality of series connected barriers, which complicate the formation of a streamer.
  • streamer preliminary spark
  • Another disadvantage of the known methods or filter arrangements is the energy requirement and the degree of denitration.
  • SCR Selective Catalytic Reduction by Urea or AdBlue, which also suggested an acceleration of the SCR with the aid of plasma
  • both energy demand and the degree of denitration in all known processes for industrial application are considered as unacceptable.
  • Both disadvantages result from plasma reactions that are high-energy enough to high levels of oxygen and To dissociate nitrogen. This leads to a formation of secondary NO x , and thus to a reduction of the efficiency. Since a significant proportion of the energy in the plasma is bound by these dissociation processes, the energy consumption of the plasma increases at the same time and the whole process becomes extremely uneconomical.
  • Claim 1 relates to a method for operating a filter assembly for the decomposition of nitrogen oxides from an exhaust gas stream, wherein the exhaust gas stream is passed through extending in the longitudinal direction of a ceramic honeycomb body, open on both sides channels of the ceramic honeycomb body, and at parallel to the channels extending electrodes Voltage is applied to the honeycomb body for generating an electric field in the channels of the honeycomb body, which is oriented in each case transversely to the longitudinal axis of the channels.
  • the voltage applied to the electrodes is voltage pulses for generating an electric field within the channels with field strength amplitudes U ⁇ ron at least 5 kV / cm, preferably at least 10 kV / cm, and the product of the field strength amplitude U in V / cm and pulse duration B in seconds (s) is between 0.01 and 0.1 V. s / cm, preferably between 0.04 and 0.1 V. s / cm, wherein as wall material of the ceramic honeycomb body one with a work function below 2 electron volts, preferably less than 1 electron volts, so that the plasma thus formed is formed predominantly of Richardson electrons, secondary electrons and photoelectrons.
  • the choice of the interval for the product of the field strength amplitude U and the pulse duration B on the one hand optimizes the number of excited molecules for an efficient decomposition of nitrogen oxides by means of a sufficiently high field strength, and on the other hand the suppression of Vorfunken using a sufficiently short pulse duration.
  • the Richardson electrons, secondary electrons and photoelectrons released at the delimiting walls of the channels of the honeycomb body are accelerated by the high-frequency pulse field established in the channels of the honeycomb body.
  • the plasma then consists of electrons with energies around 1.25 eV, 1.75 eV, 2.0 and 2.5 eV, a small proportion of electrons with energies around 5 eV and a negligible proportion of electrons with energies around 9 eV or about that. These energies up to 2.5 eV are also sufficient for the triggering of secondary electrons and for the generation of quantum radiation, which significantly increase the plasma density via the release of photoelectrons.
  • the electrons pass solely from the walls of the discharge Needless and are not generated by impact ionization, so there is a need for the economic reduction of NO 2 and sufficient limitation of the electron energy as the one hand, the nitrogen dioxide are dissociated must, on the other hand not the predominant part of of the exhaust gas making up nitrogen molecules. This will be explained in more detail below.
  • the field strength amplitude U is between 5 kV / cm and 25 kV / cm, preferably between 10 kV / cm and 15 kV / cm.
  • the duty cycle of the voltage pulses should be chosen so that the pulse duration is short enough to prevent spark ignition, and the interval between the pulses is sufficiently long to ensure sufficient diffusion of the formed charge carriers.
  • the individual pulses of the electric field strength within the channels have a half-width (half-height) of at most 10 ⁇ s, and a 90% width (duration in 90% of the pulse height) of at most 1 ⁇ s, and pulse pauses of at least 50 microseconds, preferably at least 100 microseconds are provided.
  • the voltage pulses are alternating voltage pulses.
  • Claim 6 finally relates to a filter assembly for the decomposition of nitrogen oxides from an exhaust gas stream with a ceramic honeycomb body with flowed through by the exhaust and extending in the longitudinal direction of the honeycomb body, open on both sides channels, • which are each separated by webs from each other, wherein the honeycomb body with electrodes for generating an electric field in the channels of the honeycomb body, which is respectively oriented transversely to the axis of the channels, is provided.
  • the electrodes are connected to a voltage source for generating voltage pulses, and the wall material of the ceramic Honeycomb body has a work function below 2 electron volts, preferably below 1 electron volt.
  • the honeycomb body consists of an oxide ceramic, preferably of densely burnished cordierite, wherein the oxide ceramic according to claim 8 is doped with vanadium and / or cesium.
  • the oxide ceramic may also be coated or volume-doped with a non-conductive oxide catalyst, preferably a peroskite or iron oxide.
  • the honeycomb body has an annular cross-section, wherein the pulse field supplying electrode is disposed on the inner circumferential surface, and the enclosed by the inner circumferential surface cavity is closed by a ceramic plug.
  • the honeycomb body can also have an elliptical ring-shaped cross section.
  • the electrode of the inner circumferential surface in the direction of the longitudinal axis of the honeycomb body has a smaller extent than the honeycomb body itself, wherein it is arranged in the middle of the axial extent of the honeycomb body.
  • the electrode of the inner circumferential surface in the direction of the longitudinal axis of the honeycomb body have a length of 30 mm to 50 mm.
  • the electrodes are conceivable. Particularly in the case of geometries of the honeycomb body which deviate from the cylindrical shape, that is to say in the case of an elliptical or trapezoidal cross section of the honeycomb body, it may be advantageous, instead of the arrangement of the electrodes described in claims 10 to 13, to arrange an arrangement within the honeycomb body outside the honeycomb body. This can be done, for example, by according to claim 14, the electrodes in each case by a group of channels are formed within the honeycomb body, in which at least partially along its axial extent an electrical conductor is introduced. The introduction of a conductor can be done in principle in different ways.
  • the channels of a group of channels representing one electrode can be filled with an electrical conductor over its entire cross-section and over much of its axial extent.
  • electrically conductive wires, flat strips or flat iron can be inserted into the channels, which thus extend only partially over the cross section of the channels.
  • the electrodes can each also be formed by a group of channels whose inner walls are each provided along the axial extent of the channels at least partially with a metallic coating. The electrical contacting of a group of channels takes place at the one end side of the honeycomb body, and the electrical contacting of the respectively adjacent group of channels at the opposite end side of the honeycomb body - If the channels of a group in each case next to each other, an approximately planar electrode is formed.
  • the electrodes By this design of the electrodes, a significant enlargement of the honeycomb body is possible, as is necessary for large-volume diesel engines, in particular diesel engines for trucks, construction machinery, marine engines and the like.
  • An enlargement of the cross section of the honeycomb body is in fact made more difficult by the fact that the maximum electrode spacing can amount to only a few centimeters, in particular when pulsed electric fields are used. This maximum possible electrode spacing limits the executable size of the honeycomb bodies if the electrodes are placed outside the honeycomb body.
  • the electrode spacing can be selected independently of the size of the honeycomb body. In particular, the electrode spacing can be chosen small enough to even at To achieve lower voltages very well defined field strengths.
  • the field strength can be made very homogeneous by the use of planar electrodes.
  • the field can be shaped, such as in pulse fields, the decrease of the electrical propagation of the pulse can be compensated by a geometric focus, in particular a cylindrical larger, the high voltage pulses emitting electrode of a smaller, concentrically mounted grounding electrode lie opposite.
  • the two electrodes thus constitute a segment of a circular ring cylinder, in which the high-voltage electrode can also be arranged externally, which would not be possible for reasons of isolation technology in an arrangement of the electrodes outside of the honeycomb body.
  • FIG. 1 shows a longitudinal section through an embodiment of a filter arrangement according to the invention with a cylindrical shape in a cylindrical metal housing
  • FIG. 2 shows calculations which indicate the distribution of the electron energies in the plasma, which is dependent on the respective plasma field strength
  • Fig. 3 Denoxing measurements as a function of plasma field strength on a diesel test rig.
  • Fig. 1 shows a longitudinal section through a filter arrangement according to the invention for the decomposition of nitrogen oxides from an exhaust stream, which consists of a cylindrical ceramic honeycomb body 1 with annular cross-section in the longitudinal direction of the honeycomb body 1 open on both sides open channels 16, which are separated from each other by webs ,
  • the honeycomb body 1 is with corresponding swelling mats 2 and net-shaped end grille 3 is embedded from a steel mesh in a cylindrical metal housing 15.
  • the cylindrical interior of the ceramic body 1 is formed by a conductive K ⁇ ntakttechnik as a high voltage electrode, whereas the outer cylindrical surface of the ceramic body 1 represents by a similar contacting the electrode connected to the ground potential.
  • the upstream entrance of the cavity formed by the inner cylinder jacket is closed by a ceramic plug 5 fastened in this cavity by means of ceramic cement 6.
  • the downstream end of the cavity is closed with a ceramic plug 7 having a bore into which a ceramic tube 8 is secured by means of ceramic cement.
  • the passage of the tube 8 through the metal housing 15 is gas-tight by O-ring seals 12.
  • the supply of the electrical voltage to the four electrode segments 9a to 9d is made by steel wires 10a to 10d for each electrode part individually, wherein the steel wires are held by four perforated ceramic discs (not visible in the drawing) at a distance.
  • the closed interior of the honeycomb body 1, the gastight supply of the power supply 10a to 10d to the high voltage electrode parts 9a to 9d and the extension of the honeycomb body 1 with annular lugs 11 prevent the very high operating voltages across the inlet surface 17 and the exit surface 18 of the honeycomb body beat against earth.
  • the PTK resistor 13 on the grounded side of the honeycomb body 1 also contributes to the uniform distribution of the current flowing through the honeycomb body 1 in that regions with increased current also have an increased ohmic power in the PTK resistor 13 and thus have a higher temperature
  • the current is regulated off via the positive temperature characteristic of the PTK resistor 13.
  • the plasma is formed predominantly of Richardson electrons, secondary electrons and photoelectrons, and
  • the product of the field strength amplitude U in V / cm and pulse duration B in seconds (s) is between 0.01 and 0.1 V. s / cm, preferably between 0.04 and 0.1 V. s / cm.
  • the electrical pulse field is preferably 5 kV / cm and 25 kV / cm, preferably between 10 kV / cm and 15 kV / cm, and is predominantly perpendicular to the surfaces dominating the discharge space.
  • the pulse field strength and the corresponding pulse duration it is ensured that, in particular, the following method steps take place in the resulting plasma which, although not exclusively, but in a decisive manner, are involved in the degradation of nitrogen oxides:
  • Plasma Reaction It generates excited oxygen molecules via collisions with excited nitrogen molecules, which are or are formed by trapping electrons with kinetic energies 1.25 eV in a virtual excited state N 2 * (Volume II of the Electronic and Ionic Impact Phenomena)
  • Plasma reaction Ib Part of the excited oxygen molecules is also obtained via second-type collisions with excited nitrogen dioxide from the oxidation reaction of NO to NO 2 * described in "Process Step 3";
  • Plasma reaction 2a Dissociative trapping of electrons with
  • Plasma reaction 2b Dissociative capture of electrons with energies around or above IeV by the oxygen molecule excited with about 2 eV and an electron affinity (EA) of 2 eV for the atomic oxygen:
  • Plasma reaction 4 Dissociative electron capture on excited nitrogen dioxide with electrons around or above 1.25 eV:
  • NO 2 can be dissociated with electron energies of only 1.25 eV to 2.5 eV, since a larger number of gas molecules in the same time is due to the electric pulse field between 5 kV / cm and 25.Z 7 "'kV / cm Higher electron energies occur only to a negligible extent due to the rapidly increasing cross sections for inelastic collisions, and the higher field strength only generates excited states of the gas molecules to an increasing extent.
  • this unipolar plasma according to the invention which thus consists predominantly of only electrons, has the advantage of saving energy in that there is no electrical energy transmission of the field to atomic hulls consume the vast majority of energy from the field by the large mass of atomic hulls compared to the electron masses.
  • the limitation of the electron energy below 5 eV is particularly important because otherwise dissociation of nitrogen lead to the formation of secondary nitrogen oxides and thus to a limitation of the possible degree of denitration. While at least 12.5 eV (first ionization potential for molecular oxygen) and nitrogen at least 15.5 eV (first ionization potential for molecular nitrogen) are required for an impact ionization of oxygen, the dissociation energies from the ground state are already considerably lower: 9.1 eV for nitrogen and 5.1 eV for oxygen.
  • the lifetime of these excited nitrogen molecules can be up to 50 ms, and due to the high number of gases, they can also excite their excitation energy to other gases, e.g. give off nitrogen oxides or molecular oxygen, which are present only in low concentration. If nitrogen dioxide is excited by such plasma reactions, dissociated electron capture with electrons of energy around or above 1.25 eV can take place at this excited nitrogen dioxide.
  • the ratio value for plasma-induced oxidation of soot is between 4.6 and 5.3 V / cm.torr, for the plasma-induced selective dissociation of NO 2 between 8.8 and 17.5 V / cm.torr.
  • rotational excitations start at about 6 meV and have a cross section of about 10 meV of about 4.10 "18 cm 2
  • the vibrational excitations start at about 0.3 eV, reach about 10 -18 cm 2 at 1 eV, at 2 eV about 10 cm 2 and are at 3 eV over
  • the high-frequency pulse field in the pulse peaks a Field strength of 5 kV / cm to 25 kV / cm, preferably reached 10 kV / cm.
  • the second table shows which field strengths are necessary, so that the reaction energy for disturbing reactions can be recorded with very little probability, ie on the six times ( ⁇ s ) or four times ( ⁇ 4 ) free path length occurring very rarely within the distribution of the free path lengths :
  • the individual pulses of this high-frequency pulse field have a half-width (half-height) of 10 ⁇ s, preferably 7 ⁇ s and a 90% width (duration in 90% of the pulse height) of 2 ⁇ s, preferably 1 ⁇ s, and each packet of these pulses is followed by a pause of at least 50 ⁇ s duration, preferably at least 100 ⁇ s.
  • the electrons In addition to the suppression of streamer according to the invention in the reaction space, the electrons must not be allowed to ionize either be generated on the walls by means of tips and the like, as this always ion species both show signs that are torn by the high-frequency field in the reaction space. Since according to the invention only those electrons are to form the plasma, which emerge from the walls by thermal processes (Richardson electrons) collision processes (secondary electrons) or quantum processes (photoelectrons), wall materials must be used according to the invention for the honeycomb body whose work function for electrons below 2 eV, preferably below 1 eV.
  • This inventive method is best implemented by a cylindrical honeycomb body 1 having a circular cross-section, wherein the high-frequency pulse field supplying electrode 9 is mounted on the inner circumferential surface, and this cavity is closed by a ceramic plug 5, 7. If the space for the installation of such a "denoxing device" under the vehicle requires an elliptical honeycomb body 1, then this method according to the invention can also be carried out for such a honeycomb body 1 with an elliptical-annular cross-section The electrode 9 supplying the high-frequency impulse field is in turn attached to the mounted inside the shell, and the cavity is also closed by a ceramic plug 6, 7.
  • FIG. 2 shows calculations which indicate the distribution of the electron energies in the plasma, which is dependent on the respective plasma field strength.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Health & Medical Sciences (AREA)
  • Biomedical Technology (AREA)
  • Environmental & Geological Engineering (AREA)
  • Combustion & Propulsion (AREA)
  • Exhaust Gas After Treatment (AREA)
  • Treating Waste Gases (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)

Abstract

L'invention concerne un procédé permettant d'exploiter un système filtrant pour décomposer des oxydes d'azote provenant d'un flux de gaz d'échappement, selon lequel le flux de gaz d'échappement est guidé à travers les canaux (16), ouverts des deux côtés, d'un corps alvéolaire céramique (1), qui s'étendent dans le sens longitudinal dudit corps alvéolaire (1), et une tension est appliquée audit corps alvéolaire (1), au niveau d'électrodes (9) parallèles aux canaux (16), pour produire un champ électrique dans les canaux (16) du corps alvéolaire (1). Selon l'invention, il est prévu, pour ce qui est de la tension appliquée aux électrodes, qu'il s'agisse d'impulsions de tension, pour produire un champ électrique à l'intérieur des canaux (16) avec des amplitudes d'intensité de champ U d'au moins 5 kV/cm, et que le produit de l'amplitude d'intensité de champ U exprimée en V/cm et la durée d'impulsion B exprimée en seconde (s) se situe entre 0,01 et 0,1 V. s/cm. Le matériau de la paroi du corps alvéolaire céramique (1) présente un travail de sortie inférieur à 2 électrons-volts, de sorte que le plasma ainsi produit se compose essentiellement d'électrons de type Richardson, d'électrons secondaires et de photoélectrons.
EP06741033A 2005-06-08 2006-06-08 Procede et dispositif pour decomposer des oxydes d'azote dans un flux de gaz d'echappement Withdrawn EP1888206A1 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
AT0096705A AT501888B1 (de) 2005-06-08 2005-06-08 Wabenfilter mit planaren elektroden
AT11512005A AT501876B1 (de) 2005-06-08 2005-07-07 Verfahren und vorrichtung zum abbau von stickstoffoxiden in einem abgasstrom
PCT/AT2006/000234 WO2006130895A1 (fr) 2005-06-08 2006-06-08 Procede et dispositif pour decomposer des oxydes d'azote dans un flux de gaz d'echappement

Publications (1)

Publication Number Publication Date
EP1888206A1 true EP1888206A1 (fr) 2008-02-20

Family

ID=37114475

Family Applications (1)

Application Number Title Priority Date Filing Date
EP06741033A Withdrawn EP1888206A1 (fr) 2005-06-08 2006-06-08 Procede et dispositif pour decomposer des oxydes d'azote dans un flux de gaz d'echappement

Country Status (3)

Country Link
EP (1) EP1888206A1 (fr)
AT (1) AT501876B1 (fr)
WO (1) WO2006130895A1 (fr)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102016203997A1 (de) * 2016-03-11 2017-09-14 Robert Bosch Gmbh Filtervorrichtung

Family Cites Families (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1997002410A1 (fr) * 1995-07-06 1997-01-23 Fleck Carl M Filtre a suie, notamment pour gaz d'echappement de moteurs diesel
AU6347696A (en) * 1995-07-27 1997-02-26 Carl Maria Fleck Process and device for decompositing nitrogen oxides in internal combustion engine exhaust gases
AT2330U1 (de) * 1997-06-17 1998-08-25 Fleck Carl M Dr Vorrichtung zur dissoziation von im abgas von verbrennungskraftmaschinen enthaltenen stickstoffoxiden
GB9803817D0 (en) * 1998-02-25 1998-04-22 Aea Technology Plc A component for gas treatment
FR2818558B1 (fr) * 2000-12-21 2003-10-24 Brandt Cooking Dispositif de traitement par catalyse des odeurs et hotte de filtration equipee d'un tel dispositif
US20040208804A1 (en) * 2001-08-25 2004-10-21 Hall Stephen Ivor Non-thermal plasma reactor

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
See references of WO2006130895A1 *

Also Published As

Publication number Publication date
AT501876B1 (de) 2008-10-15
AT501876A1 (de) 2006-12-15
WO2006130895A1 (fr) 2006-12-14

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