DE4342297C2 - Method and device for reducing the nitrogen oxide content contained in the exhaust gas from combustion plants - Google Patents
Method and device for reducing the nitrogen oxide content contained in the exhaust gas from combustion plantsInfo
- Publication number
- DE4342297C2 DE4342297C2 DE4342297A DE4342297A DE4342297C2 DE 4342297 C2 DE4342297 C2 DE 4342297C2 DE 4342297 A DE4342297 A DE 4342297A DE 4342297 A DE4342297 A DE 4342297A DE 4342297 C2 DE4342297 C2 DE 4342297C2
- Authority
- DE
- Germany
- Prior art keywords
- membrane
- hydrogen
- exhaust gas
- atomic hydrogen
- exhaust
- 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.)
- Expired - Lifetime
Links
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 title claims description 50
- 238000000034 method Methods 0.000 title claims description 14
- 239000007789 gas Substances 0.000 title claims description 13
- 238000002485 combustion reaction Methods 0.000 title claims description 6
- 239000012528 membrane Substances 0.000 claims description 34
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 15
- 239000001257 hydrogen Substances 0.000 claims description 15
- 229910052739 hydrogen Inorganic materials 0.000 claims description 15
- YZCKVEUIGOORGS-UHFFFAOYSA-N Hydrogen atom Chemical compound [H] YZCKVEUIGOORGS-UHFFFAOYSA-N 0.000 claims description 14
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 13
- 150000002431 hydrogen Chemical class 0.000 claims description 9
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 5
- 238000005868 electrolysis reaction Methods 0.000 claims description 5
- 239000001301 oxygen Substances 0.000 claims description 5
- 229910052760 oxygen Inorganic materials 0.000 claims description 5
- 229910021536 Zeolite Inorganic materials 0.000 claims description 3
- 239000002131 composite material Substances 0.000 claims description 3
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 3
- 229910052757 nitrogen Inorganic materials 0.000 claims description 3
- 229910052709 silver Inorganic materials 0.000 claims description 3
- 239000010457 zeolite Substances 0.000 claims description 3
- 229910001252 Pd alloy Inorganic materials 0.000 claims description 2
- 229910001069 Ti alloy Inorganic materials 0.000 claims description 2
- 229910000756 V alloy Inorganic materials 0.000 claims description 2
- 229910001093 Zr alloy Inorganic materials 0.000 claims description 2
- 229910052787 antimony Inorganic materials 0.000 claims description 2
- 229910052802 copper Inorganic materials 0.000 claims description 2
- 238000009792 diffusion process Methods 0.000 claims 1
- 239000002245 particle Substances 0.000 claims 1
- 238000006243 chemical reaction Methods 0.000 description 7
- 239000000463 material Substances 0.000 description 5
- 238000006722 reduction reaction Methods 0.000 description 4
- 239000003054 catalyst Substances 0.000 description 3
- 230000003197 catalytic effect Effects 0.000 description 3
- 230000002860 competitive effect Effects 0.000 description 3
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- 238000010531 catalytic reduction reaction Methods 0.000 description 2
- JEGUKCSWCFPDGT-UHFFFAOYSA-N h2o hydrate Chemical compound O.O JEGUKCSWCFPDGT-UHFFFAOYSA-N 0.000 description 2
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 238000003776 cleavage reaction Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 229910000765 intermetallic Inorganic materials 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910052987 metal hydride Inorganic materials 0.000 description 1
- 150000004681 metal hydrides Chemical class 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 230000007017 scission Effects 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000011144 upstream manufacturing Methods 0.000 description 1
- 239000002912 waste gas Substances 0.000 description 1
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
- B01D53/22—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 diffusion
-
- 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
- B01D53/326—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 in electrochemical cells
-
- 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
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8625—Nitrogen oxides
-
- 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
-
- B01J35/59—
Description
Die Erfindung betrifft ein Verfahren und eine Vorrichtung zur Verminderung der im Abgas von Verbrennungsanlagen enthaltenen Stickoxide gemäß dem Oberbegriff des Hauptanspruchs.The invention relates to a method and an apparatus for Reduction in the waste gas from combustion plants Nitrogen oxides according to the preamble of the main claim.
Aus der US-PS 39 86 350 ist eine Brennkraftmaschine bekannt, in deren Abgasleitung ein Katalysator zur Umwandlung von Stick oxiden angeordnet ist. Stromauf des Katalysators kann mittels einer Leitung zur Bildung einer reduzierenden Atmosphäre Wasser stoffgas in die Abgasleitung eingebracht werden.From US-PS 39 86 350 an internal combustion engine is known in whose exhaust pipe is a catalyst for converting stick oxide is arranged. Upstream of the catalyst can be by means of a pipe to form a reducing atmosphere water Substance gas are introduced into the exhaust pipe.
Weiterhin ist aus der DE 36 44 090 A1 eine Anordnung bekannt, bei der atomarer Wasserstoff durch Elektrolyse von im Abgas enthaltenem Wasserdampf erzeugt und mit den Stickoxiden unter Bildung von Stickstoff und Wasser an einer katalytisch wirkenden Elektrode zur Reaktion gebracht wird.Furthermore, an arrangement is known from DE 36 44 090 A1, in the case of atomic hydrogen by electrolysis from in the exhaust gas Contained water vapor generated and with the nitrogen oxides below Formation of nitrogen and water on a catalytically active Electrode is reacted.
Nachteilig bei diesen Anordnungen ist, daß Konkurrenzreaktionen, beispielsweise mit dem Restsauerstoff im Abgas, nicht verhindert werden können.A disadvantage of these arrangements is that competitive reactions, for example, with the residual oxygen in the exhaust gas, not prevented can be.
Schließlich ist aus der EP 0 566 071 A1 ein gattungsgemäßes Verfahren bekannt, bei dem eine protonenleitende Membran aus Sinterkeramik mit Stickoxide und Wasserdampf enthaltendem Abgas beaufschlagt wird. An den gegenüberliegenden Oberflächen der Membran sind Elektroden vorgesehen, zwischen denen eine Gleichspannung angelegt wird. An der Anode wird hierbei der Wasserdampf elektrolytisch zersetzt. Die dabei erzeugten Protonen werden durch die Membran zur Kathode transportiert, wo die adsorbierten Stickoxide durch den entstehenden Wasserstoff reduziert werden.Finally, EP 0 566 071 A1 is a generic one Process known in which a proton-conducting membrane Sintered ceramic with nitrogen oxides and exhaust gas containing water vapor is applied. On the opposite surfaces of the Membrane electrodes are provided, between which one DC voltage is applied. At the anode, the Water vapor is decomposed electrolytically. The generated Protons are transported through the membrane to the cathode where the adsorbed nitrogen oxides due to the resulting hydrogen be reduced.
Dieses Verfahren weist den Nachteil auf, daß die Membran erst ab Temperaturen von 300°C die notwendige Protonenleitfähigkeit aufweist. Bei niedrigeren Abgastemperaturen kann das Verfahren daher ohne vorheriges Aufheizen nicht verwendet werden.This method has the disadvantage that the membrane is only removed Temperatures of 300 ° C the necessary proton conductivity having. The process can be carried out at lower exhaust gas temperatures therefore not be used without prior heating.
Die Aufgabe der Erfindung besteht darin, ein Verfahren und eine Vorrichtung zu schaffen, mit der die im Abgas enthaltenen Stickoxide mit hoher Selektivität durch den Wasserstoff am Katalysator umgewandelt werden.The object of the invention is a method and To create a device with which the contained in the exhaust gas Nitrogen oxides with high selectivity due to the hydrogen on Catalyst to be converted.
Die Aufgabe wird erfindungsgemäß durch die kennzeichnenden Merkmale des Patentanspruchs 1 gelöst. The object is achieved by the characterizing Features of claim 1 solved.
Dadurch, daß die Stickoxide und der Wasserstoff erst in Gegen wart des katalytischen Materials in Kontakt kommen, können Konkurrenzreaktionen weitestgehend vermieden und somit die Selektivität für die gewünschte Reaktion erheblich verbessert werden. Außerdem liegt der Wasserstoff in der Membran nicht in gasförmiger, sondern in gespaltener Form vor, so daß eine ver besserte Umwandlungsrate erreicht werden kann.Because the nitrogen oxides and the hydrogen only in counter were able to come into contact with the catalytic material Competitive reactions largely avoided and thus the Selectivity for the desired reaction significantly improved will. In addition, the hydrogen is not in the membrane gaseous, but in split form, so that a ver better conversion rate can be achieved.
Weitere Vorteile und Ausgestaltungen gehen aus den Unteran sprüchen und der Beschreibung hervor. Die Erfindung ist nachstehend anhand einer Zeichnung näher beschrieben, wobeiFurther advantages and configurations can be found in the lower sub sayings and the description. The invention is described below with reference to a drawing, wherein
Fig. 1 ein mit Wasserstoffgas beaufschlagter Membranreaktor zur selektiven katalytischen Reduktion von in Abgasen enthaltenen Stickoxiden, Fig. 1 is a acted upon with hydrogen gas membrane reactor for the selective catalytic reduction of nitrogen oxides contained in exhaust gases,
Fig. 2 eine Prinzipdarstellung der beim Ausführungsbeispiel gemäß Fig. 1 ablaufenden Reaktionen, Fig. 2 is a schematic representation of the running in the embodiment of Fig. 1 reactions,
Fig. 3 ein zweites Ausführungsbeispiel eines erfindungsgemäßen Membranreaktors, in dem der zur Reduktion benötigte Wasserstoff durch Elektrolyse aus Wasser gewonnen wird, und Fig. 3 shows a second embodiment in which the need for reduction, hydrogen is produced by electrolysis of water of a membrane reactor according to the invention, and
Fig. 4 eine Prinzipdarstellung der beim Ausführungsbeispiel gemäß Fig. 3 ablaufenden Reaktionen zeigt. FIG. 4 shows a basic illustration of the reactions taking place in the exemplary embodiment according to FIG. 3.
Fig. 1 zeigt eine Abgasleitung 1 einer nicht dargestellten Ver brennungsanlage, beispielsweise einer Diesel-Brennkraftmaschine. In der Abgasleitung 1 ist ein Membranreaktor 2 angeordnet. Der aus einer Membran 3 gebildete Membranreaktor 2 weist eine ge schlossene zylindrische Form auf und wird über eine Zuleitung 4 mit Wasserstoffgas H₂ beaufschlagt. Die Membran 3 besteht aus einem für Wasserstoff H durchlässigen Material, welches für die Reduktion der Stickoxide NOx mittels Wasserstoff H eine kataly tische Wirkung besitzt. Beispielsweise kann hierzu eine Legie rung aus Palladium mit 25 atomprozenten Silber verwendet werden. Denkbar ist aber auch die Verwendung anderer Pd-Legierungen mit Ag, Cu oder Sb oder auch von V-, Ti- oder Zr-Legierungen. Grund sätzlich kann hierbei auch auf andere Werkstoffe, die bei der Speicherung von Wasserstoff in Metallhydriden Verwendung finden, zurückgegriffen werden. Da die Membran 3 aber auch die Fähigkeit besitzen muß, Stickoxide NOx zu adsorbieren, wird vorzugsweise ein Composite aus den genannten Materialien und einem Zeolith, das diese Fähigkeit besitzt, verwendet. Fig. 1 shows an exhaust pipe 1 of a combustion system, not shown, for example a diesel internal combustion engine. A membrane reactor 2 is arranged in the exhaust line 1 . The membrane reactor 2 formed from a membrane 3 has a closed cylindrical shape and is supplied with hydrogen gas H₂ via a feed line 4 . The membrane 3 consists of a material permeable to hydrogen H, which has a catalytic effect for the reduction of nitrogen oxides NO x by means of hydrogen H. For example, an alloy made of palladium with 25 atomic percent silver can be used. However, it is also conceivable to use other Pd alloys with Ag, Cu or Sb or also V, Ti or Zr alloys. In principle, other materials that are used in the storage of hydrogen in metal hydrides can also be used. However, since the membrane 3 must also have the ability to adsorb nitrogen oxides NO x , a composite of the materials mentioned and a zeolite which has this ability is preferably used.
In Fig. 2 ist die Funktion der Membran 3 schematisch darge stellt. Das Wasserstoffgas H₂ trifft auf eine Grenzfläche B der Membran 3. Die Membran 3 enthält Metalle oder intermetallische Verbindungen, die in der Lage sind, die Spaltung und anschließende Adsorption des Wasserstoffs H durch die Membran katalytisch zu beschleunigen. An der anderen Grenzfläche A der Membran 3 werden Stickoxide NOx aus dem Abgas adsorbiert. Der aktive Wasserstoff H diffundiert aufgrund des Konzentrations gradienten durch die Membran 3 und trifft im Bereich der Grenz fläche A auf die adsorbierten Stickoxide NOx. Dort werden die Stickoxide NOx durch den Wasserstoff H nach einer bekannten SCR-Methode (Selective Catalytic Reduction) zu Stickstoff N₂ und Wasserdampf H₂O reduziert, wobei die Endprodukte in den vorbei strömenden Abgasstrom entweichen. Dieses Verfahren hat den Vor teil, daß die Stickoxide NOx erst unmittelbar in der Nähe des katalytischen Materials mit dem Reduktionsmittel Wasserstoff H in Kontakt kommen. Dadurch können Konkurrenzreaktionen des Wasserstoffs H, beispielsweise mit dem Restsauerstoff in den Abgasen, weitestgehend vermieden und eine besonders hohe Selektivität für die NOx-Reduktion erreicht werden.In Fig. 2 the function of the membrane 3 is shown schematically Darge. The hydrogen gas H₂ meets an interface B of the membrane 3rd The membrane 3 contains metals or intermetallic compounds which are able to catalytically accelerate the cleavage and subsequent adsorption of the hydrogen H through the membrane. At the other interface A of the membrane 3 , nitrogen oxides NO x are adsorbed from the exhaust gas. The active hydrogen H diffuses through the concentration gradient through the membrane 3 and hits the adsorbed nitrogen oxides NO x in the area of the interface A. There, the nitrogen oxides NO x are reduced by the hydrogen H according to a known SCR method (Selective Catalytic Reduction) to nitrogen N₂ and water vapor H₂O, the end products escaping into the exhaust gas stream flowing past. This method has the part before that the nitrogen oxides NO x come only in the vicinity of the catalytic material with the reducing agent hydrogen H in contact. As a result, competitive reactions of the hydrogen H, for example with the residual oxygen in the exhaust gases, can be largely avoided and a particularly high selectivity for the NO x reduction can be achieved.
Im zweiten Ausführungsbeispiel, welches in Fig. 3 und 4 darge stellt ist, wird der atomare Wasserstoff H durch Elektrolyse aus Wasser H₂O gewonnen. Der Membranreaktor 2 ist als Wasser reservoir 5 ausgeführt, dem über die Zuleitung 4 Wasser H₂O zugeführt wird. Im Bereich der Längsachse des Membranreaktors 2 ist eine Elektrode 6 angeordnet. Die Membran 2 wird gegenüber der Elektrode 6 auf ein negatives Potential gelegt. Durch die angelegte Spannung wird das Wasser H₂O elektrolytisch zersetzt, wobei der Wasserstoff H an der auf negativem Potential liegenden Membran 2 absorbiert und der Sauerstoff O₂ an der Anode 6 abge schieden wird. Zur Abfuhr des Sauerstoffs O₂ ist eine Abström leitung 7 vorgesehen. Die Reduktion der Stickoxide NOx erfolgt entsprechend dem ersten Ausführungsbeispiel in der Membran 3.In the second embodiment, which is shown in Fig. 3 and 4 Darge, the atomic hydrogen H is obtained by electrolysis from water H₂O. The membrane reactor 2 is designed as a water reservoir 5 , to which water H 2 O is supplied via the feed line 4 . An electrode 6 is arranged in the region of the longitudinal axis of the membrane reactor 2 . The membrane 2 is placed at a negative potential with respect to the electrode 6 . Due to the applied voltage, the water H₂O is decomposed electrolytically, the hydrogen H being absorbed on the membrane 2 lying at negative potential and the oxygen O₂ being separated on the anode 6 . To discharge the oxygen O₂ an outflow line 7 is provided. The nitrogen oxides NO x are reduced in the membrane 3 in accordance with the first exemplary embodiment.
Claims (8)
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE4342297A DE4342297C2 (en) | 1993-12-11 | 1993-12-11 | Method and device for reducing the nitrogen oxide content contained in the exhaust gas from combustion plants |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE4342297A DE4342297C2 (en) | 1993-12-11 | 1993-12-11 | Method and device for reducing the nitrogen oxide content contained in the exhaust gas from combustion plants |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| DE4342297A1 DE4342297A1 (en) | 1995-06-22 |
| DE4342297C2 true DE4342297C2 (en) | 1998-01-29 |
Family
ID=6504757
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| DE4342297A Expired - Lifetime DE4342297C2 (en) | 1993-12-11 | 1993-12-11 | Method and device for reducing the nitrogen oxide content contained in the exhaust gas from combustion plants |
Country Status (1)
| Country | Link |
|---|---|
| DE (1) | DE4342297C2 (en) |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE19527693C1 (en) * | 1995-07-28 | 1996-10-10 | Dornier Gmbh | Nitrogen oxide redn. from vehicle exhaust gases without use of ammonia |
| SE523342C2 (en) | 2000-05-02 | 2004-04-13 | Volvo Teknisk Utveckling Ab | Apparatus and method for reducing a gas component in an exhaust gas stream from an internal combustion engine |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE3644090A1 (en) * | 1986-12-23 | 1988-07-07 | Bbc Brown Boveri & Cie | Process and apparatus for purifying exhaust gases |
| EP0566071A1 (en) * | 1992-04-14 | 1993-10-20 | Kabushiki Kaisha Toyota Chuo Kenkyusho | Method for reducing nitrogen oxides |
-
1993
- 1993-12-11 DE DE4342297A patent/DE4342297C2/en not_active Expired - Lifetime
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE3644090A1 (en) * | 1986-12-23 | 1988-07-07 | Bbc Brown Boveri & Cie | Process and apparatus for purifying exhaust gases |
| EP0566071A1 (en) * | 1992-04-14 | 1993-10-20 | Kabushiki Kaisha Toyota Chuo Kenkyusho | Method for reducing nitrogen oxides |
Also Published As
| Publication number | Publication date |
|---|---|
| DE4342297A1 (en) | 1995-06-22 |
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Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| OP8 | Request for examination as to paragraph 44 patent law | ||
| D2 | Grant after examination | ||
| 8364 | No opposition during term of opposition | ||
| 8327 | Change in the person/name/address of the patent owner |
Owner name: DAIMLERCHRYSLER AG, 70567 STUTTGART, DE |
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| 8330 | Complete renunciation |