DE10118618A1 - Catalytic reforming of hydrocarbons or alcohols to produce hydrogen for fuel cells used to power vehicles is carried out as several partial reactions in a network of interconnected microreactors - Google Patents
Catalytic reforming of hydrocarbons or alcohols to produce hydrogen for fuel cells used to power vehicles is carried out as several partial reactions in a network of interconnected microreactorsInfo
- Publication number
- DE10118618A1 DE10118618A1 DE10118618A DE10118618A DE10118618A1 DE 10118618 A1 DE10118618 A1 DE 10118618A1 DE 10118618 A DE10118618 A DE 10118618A DE 10118618 A DE10118618 A DE 10118618A DE 10118618 A1 DE10118618 A1 DE 10118618A1
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- Germany
- Prior art keywords
- reactor
- microreactors
- hydrocarbons
- alcohols
- network
- 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.)
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- B01J19/0093—Microreactors, e.g. miniaturised or microfabricated reactors
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01B—BOILING; BOILING APPARATUS ; EVAPORATION; EVAPORATION APPARATUS
- B01B1/00—Boiling; Boiling apparatus for physical or chemical purposes ; Evaporation in general
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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Abstract
Description
In der deutschen Patentanmeldung Nr. 100 32 059.7 ist eine Vorrichtung zum Ausführen ei ner katalytischen Rohrreaktion beschrieben.In German patent application No. 100 32 059.7 a device for executing egg ner catalytic tube reaction described.
Mit Hilfe einer "modifizierten Vorrichtung zum Ausführen einer katalytischen Rohrreaktion" lässt sich ein mit geringen Mengen Kohlenmonoxid verunreinigter Wasserstoffstrom durch einen stufenweisen katalytischen Oxidationsprozess soweit reinigen, dass der Wasserstoff anschließend als Brennstoff für eine PEM-Brennstoffzelle verwendet werden kann.Using a "Modified Device to Perform a Catalytic Pipe Reaction" a hydrogen stream contaminated with small amounts of carbon monoxide can pass through clean a step-by-step catalytic oxidation process until the hydrogen can then be used as fuel for a PEM fuel cell.
Bei der Gewinnung von Wasserstoff aus Methanol durch katalytische Reformierung sind Spu ren von Kohlenmonoxid im Wasserstoffgas nach dem heutigen Stand der Technik unver meidlich. Zur elektrochemischen Stromerzeugung, vor allem in mobilen Systemen (z. B. Au tos), wird der Wasserstoff in einer PEM-Brennstoffzelle zu Wasser verbrannt.In the production of hydrogen from methanol by catalytic reforming, spu Ren of carbon monoxide in hydrogen gas according to the current state of the art in averting. For electrochemical power generation, especially in mobile systems (e.g. Au tos), the hydrogen is burned to water in a PEM fuel cell.
Eine PEM Brennstoffzelle wird aber in ihrer Wirksamkeit durch Spuren von Kohlenmonoxid beträchtlich herabgesetzt und im Endeffekt vergiftet. Der für eine PEM-Brennstoffzelle er laubte Kohlenmonoxidgehalt muss unter 100 ppm liegen. Zu diesem Zweck wir der mit CO beaufschlagte Wasserstoff in einem sehr engen Temperaturbereich um 100°C katalytisch zu CO2 (Kohlendioxid) oxidiert. Das Problem dabei ist die Aufrechterhaltung einer konstanten Temperatur in einem gegen die Umwelt nur wenig abgeschirmten System wie dem Auto.However, a PEM fuel cell's effectiveness is considerably reduced by traces of carbon monoxide and the result is poisoned. The carbon monoxide content permitted for a PEM fuel cell must be below 100 ppm. For this purpose, the hydrogen charged with CO is catalytically oxidized to CO 2 (carbon dioxide) in a very narrow temperature range around 100 ° C. The problem is maintaining a constant temperature in a system such as the car that is not very well shielded from the environment.
Aufgabe der Erfindung ist es, in einer hochselektiven, mehrstufigen, heterogenen, katalyti schen Oxidation, das in einem Wasserstoffsystem enthaltene Kohlenmonoxid CO in CO2 zu überführen, ohne dabei den Wasserstoff in nennenswertem Umfang ebenfalls zu oxidieren.The object of the invention is to convert the carbon monoxide CO contained in a hydrogen system into CO 2 in a highly selective, multi-stage, heterogeneous, catalytic oxidation, without also oxidizing the hydrogen to any appreciable extent.
Zur Lösung dieser Aufgabe wird eine modifizierte Verrichtung zum Ausführen einer katalyti schen Rohrreaktion verwendet.To solve this problem, a modified execution for performing a catalytic pipe reaction used.
Der in mehrere Reaktorräume (R1 bis Rn) untergliederte katalytische Rohrreaktor wird von dem Wasserstoff/Kohlenmonoxid-Gemisch durchströmt. Die einzelnen Reaktorräume R1 bis Rn sind untereinander mit einem Kanalsystem verbunden. Die Reaktorräume R1 bis Rn und die einzelnen Kanäle K1 bis Km befinden sich in einem kleinen Heizblock, der auf konstanter Grundtemperatur gehalten wird. Die einzelnen Reaktorräume bestehen aus sehr flachen Hohl räumen, die mit dem Katalysator beschichtet sind. The hydrogen / carbon monoxide mixture flows through the catalytic tubular reactor, which is subdivided into several reactor spaces (R 1 to R n ). The individual reactor rooms R 1 to R n are connected to one another with a channel system. The reactor rooms R 1 to R n and the individual channels K 1 to K m are located in a small heating block which is kept at a constant basic temperature. The individual reactor rooms consist of very flat cavities, which are coated with the catalyst.
Jeder dieser Reaktorräume R1 bis Rn, ist individuell heizbar, so dass sie eine Temperatur er halten, die über der Grundtemperatur des Heizblocks liegt. Gegebenenfalls kann die Tempe ratur eines jeden dieser Reaktorräume gemessen und individuell geregelt werden.Each of these reactor rooms R 1 to R n can be heated individually, so that they maintain a temperature which is above the basic temperature of the heating block. If necessary, the temperature of each of these reactor rooms can be measured and individually controlled.
Die Kanäle K1 bis Kn sind mit eigenen Gaseingängen, G1 bis Gn, verbunden, so dass vor je dem Reaktorraum zusätzlich weitere Gase (z. B. Luft oder das H2/CO-Gemisch) zugeführt werden können.The channels K 1 to K n are connected to their own gas inputs, G 1 to G n , so that additional gases (e.g. air or the H 2 / CO mixture) can be fed in front of the reactor space.
Die Selektivität der katalytischen Oxidation wird dadurch erreicht, dass durch die Aufgliede
rung des Rohrreaktors in sehr kleine Reaktorräume, R1 bis Rn die exothermen Oxidationen
temperaturmäßig beherrschbar werden und, dass das zur selelektiven Oxidation notwendige
Temperaturfenster in jedem Reaktorraum genau eingestellt werden kann. Durch die selektive
Oxidation des CO zu CO2 entsteht ein H2/CO2-Gemisch, das unter Gleichgewichtsbedingun
gen (Wassergasgleichgewicht) der selektiven Oxidation entgegen wirkt
The selectivity of the catalytic oxidation is achieved in that the temperature of the exothermic oxidations can be controlled by dividing the tubular reactor into very small reactor spaces, R 1 to R n , and in that the temperature window required for selective oxidation can be set precisely in each reactor space. The selective oxidation of CO to CO 2 creates an H 2 / CO 2 mixture that counteracts selective oxidation under conditions of equilibrium (water gas balance)
(H2 + CO2 CO + H2O).(H 2 + CO 2 CO + H 2 O).
Die Möglichkeit- über die zwischen den Reaktorräumen R1 bis Rn mittels der Gaseinlässe G1 bis Gk zusätzlich einen Anteil der Gesamtmenge der Reaktionskomponente - einerseits be feuchtete Luft und andererseits das H2/CO-Gemischgas - in die Folge der Reaktoren zu ge ben, entspricht einer gesteuerten Vorwärtsvermischung. Hierin vor allem besteht die Modifi zierung der "Vorrichtung zum Ausführen einer katalytischen Rohrreaktion" (vgl. Patentan meldung Nr. 10032059.7).The possibility - via the between the reactor spaces R 1 to R n by means of the gas inlets G 1 to G k in addition to give a portion of the total amount of the reaction component - on the one hand humidified air and on the other hand the H2 / CO mixture gas - in the sequence of the reactors , corresponds to a controlled forward mixing. This is mainly the modification of the "device for carrying out a catalytic tube reaction" (see. Patent application No. 10032059.7).
Diese Vorwärtsvermischung hat ein klassisches Analogon in der Menge der Reaktionspartner, die an dem Katalysator ohne zu reagieren vorbei strömen. Die Vorwärtsvermischung wird gemäß dieses Patentes hier bewusst dazu genutzt, das gesamte System der katalytischen Re aktoren in einem Zustand fern von Gleichgewicht zu halten und somit die Selektivität der katalytischen Oxidation von CO zu CO2 in Gegenwart von Wasserstoff H2 beträchtlich zu steigern. Durch Zugabe befeuchteter Luft über die Gaseingänge G1 bis Gk und eine geeignete Strömungsgeschwindigkeit kann die Einstellung des Wassergasgleichgewichts vermieden werden.This forward mixing has a classic analogue in the amount of reactants that flow past the catalyst without reacting. According to this patent, the forward mixing is consciously used here to keep the entire system of catalytic reactors in a state away from equilibrium and thus to considerably increase the selectivity of the catalytic oxidation of CO to CO 2 in the presence of hydrogen H 2 . By adding humidified air via the gas inlets G 1 to G k and a suitable flow rate, the adjustment of the water gas equilibrium can be avoided.
In einer über einen Heizdraht H elektrisch beheizbaren Grundplatte befinden sich die einzel nen Reaktorräume R1 bis Rn (vgl. Fig. 1) als flache Zylinder (∅ ≦ 2 cm, Tiefe ≦ 5 mm). Die se sind durch Kanäle K1 bis Km (Breite ≦ 3 mm, Tiefe ≦ 3 mm) linear miteinander verbunden. Die Kanäle durchlaufen kleine Einlasszylinder, G1 bis Gk, (∅ ≦ 5 mm, Tiefe ≦ 3 mm) für die zusätzlichen Gaszuführungen.The individual reactor spaces R 1 to R n (see FIG. 1) are located as flat cylinders (elektrisch ≦ 2 cm, depth ≦ 5 mm) in a base plate which can be electrically heated via a heating wire H. These are connected linearly by channels K 1 to K m (width ≦ 3 mm, depth ≦ 3 mm). The channels pass through small inlet cylinders, G 1 to G k , (∅ ≦ 5 mm, depth ≦ 3 mm) for the additional gas feeds.
Das Gemisch der Reaktionsgase H2/CO und befeuchtete Luft strömt über den Gaseinlass G0 in die Reaktoranlage ein. Das Reaktionsprodukt - Gas H2/CO2 sowie die Restluft - verlassen die Anlage über den Gasauslasskanal Gk+1.The mixture of reaction gases H 2 / CO and humidified air flows through the gas inlet G 0 into the reactor system. The reaction product - gas H 2 / CO 2 and the residual air - leave the system via the gas outlet duct G k + 1 .
Die Grundflächen der einzelnen Reaktoren R1 bis Rn, sind mit dem Katalysator beschichtet. Zwischen den Katalysatoren besteht keine elektrische Verbindung. Die einzelnen Katalysato ren bzw. Reaktorräume können individuell beheizt werden. Die Regelung der Heizleistung wird über eine Temperaturmessung in der jeweiligen Katalysatorschicht gewährleistet. Die Gesamtgröße der Mini-Reaktoranlage ist bereits im Prototyp kleiner als 10 × 10 × 5 cm (L × B × H). Der Gasdurchsatz beträgt ca.? l/k.The bases of the individual reactors R 1 to R n are coated with the catalyst. There is no electrical connection between the catalysts. The individual catalysts or reactor rooms can be heated individually. The regulation of the heating power is guaranteed by a temperature measurement in the respective catalyst layer. The overall size of the mini-reactor plant is smaller than 10 × 10 × 5 cm (L × W × H) in the prototype. The gas throughput is approx.? l / k.
Die Mini-Reaktor-Anlage mit Vorvermischung zur katalytischen Reinigung eines Wasser
stoffsystems von in ihm enthaltenen Kohlenmonoxid mittels selektiver Oxidation bietet vor
allem folgende Vorteile:
Hohe Selektivität der katalytischen Oxidation von Kohlenmonoxid in Gegenwart großer
Mengen von Wasserstoff.The mini-reactor system with premixing for the catalytic purification of a hydrogen system from carbon monoxide contained in it by means of selective oxidation offers the following advantages in particular:
High selectivity of the catalytic oxidation of carbon monoxide in the presence of large amounts of hydrogen.
Verwendbarkeit des gereinigten Wasserstoffes als Brennstoff in der PEM-Brennstoffzelle, da der Kohlenmonoxid-Gehalt in dem verbleibenden Gas unter 100 ppm liegt.Usability of the purified hydrogen as a fuel in the PEM fuel cell, because the carbon monoxide content in the remaining gas is below 100 ppm.
Einhaltung der für die Reaktion erforderlichen Reaktortemperatur ist auf Grund der Kleinheit der Gesamtanlage und insbesondere der einzelnen Reaktorräume leicht möglich.Compliance with the reactor temperature required for the reaction is due to the small size the entire plant and in particular the individual reactor rooms easily possible.
Gewichtseinsparung durch Verwendung von Al-basierten Metallen für die Herstellung des Heizblockes.Weight saving by using Al-based metals for the production of the Heating block.
Geringer Energieverbrauch (elektrische Energie) für die Aufrechterhaltung der notwendigen Betriebstemperatur wegen der Kleinheit der Anlage und der Reaktionsräume.Low energy consumption (electrical energy) for maintaining the necessary Operating temperature due to the small size of the plant and the reaction rooms.
Große Platzersparnis auf Grund der äußeren Abmessungen der Gesamtanlage (bereits ein Protoyp realisiert), so dass ein Einsatz für mobile Brennstoffzellaggregate (z. B. Auto) mög lich ist.Large space saving due to the external dimensions of the entire system (already one Protoyp realized), so that it can be used for mobile fuel cell units (e.g. car) is.
Claims (1)
Priority Applications (8)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE10118618A DE10118618A1 (en) | 2001-04-12 | 2001-04-12 | Catalytic reforming of hydrocarbons or alcohols to produce hydrogen for fuel cells used to power vehicles is carried out as several partial reactions in a network of interconnected microreactors |
DE10291574T DE10291574D2 (en) | 2001-04-12 | 2002-04-02 | Apparatus and method for the catalytic reforming of hydrocarbons or alcohols |
CA002444201A CA2444201A1 (en) | 2001-04-12 | 2002-04-02 | Device and method for the catalytic reformation of hydrocarbons or alcohols |
PCT/DE2002/001184 WO2002083291A1 (en) | 2001-04-12 | 2002-04-02 | Device and method for the catalytic reformation of hydrocarbons or alcohols |
US10/474,649 US20040136902A1 (en) | 2001-04-12 | 2002-04-02 | Device and method for the catalytic reformation of hydrocarbons or alcohols |
JP2002581088A JP2004535347A (en) | 2001-04-12 | 2002-04-02 | Apparatus and method for catalytic reforming of hydrocarbons or alcohols |
CNB028107519A CN1289181C (en) | 2001-04-12 | 2002-04-02 | Device and method for the catalytic reformation of hydrocarbons or alcohols |
EP02729840A EP1377370A1 (en) | 2001-04-12 | 2002-04-02 | Device and method for the catalytic reformation of hydrocarbons or alcohols |
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DE10118618A DE10118618A1 (en) | 2001-04-12 | 2001-04-12 | Catalytic reforming of hydrocarbons or alcohols to produce hydrogen for fuel cells used to power vehicles is carried out as several partial reactions in a network of interconnected microreactors |
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US7851098B2 (en) | 2005-03-16 | 2010-12-14 | Truma Geratetechnik Gmbh & Co. Kg | Reformer fuel cell system with external burner |
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2001
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Cited By (1)
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US7851098B2 (en) | 2005-03-16 | 2010-12-14 | Truma Geratetechnik Gmbh & Co. Kg | Reformer fuel cell system with external burner |
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