DE10240953A1 - Device for producing hydrogen has conversion stages and fine purification stage formed as hollow bodies having an annular chamber for receiving corresponding catalysts - Google Patents

Device for producing hydrogen has conversion stages and fine purification stage formed as hollow bodies having an annular chamber for receiving corresponding catalysts Download PDF

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Publication number
DE10240953A1
DE10240953A1 DE2002140953 DE10240953A DE10240953A1 DE 10240953 A1 DE10240953 A1 DE 10240953A1 DE 2002140953 DE2002140953 DE 2002140953 DE 10240953 A DE10240953 A DE 10240953A DE 10240953 A1 DE10240953 A1 DE 10240953A1
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Prior art keywords
reformer
hydrogen
carbon monoxide
cooling medium
stage
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DE2002140953
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German (de)
Inventor
Nicolas Zartenar
Peter Dr. Britz
Klaus Dr. Wanninger
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Viessmann Werke GmbH and Co KG
Sued Chemie AG
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Viessmann Werke GmbH and Co KG
Sued Chemie AG
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Application filed by Viessmann Werke GmbH and Co KG, Sued Chemie AG filed Critical Viessmann Werke GmbH and Co KG
Priority to DE2002140953 priority Critical patent/DE10240953A1/en
Priority to US10/508,881 priority patent/US20050172553A1/en
Priority to EP03744764A priority patent/EP1427668B9/en
Priority to DE50305340T priority patent/DE50305340D1/en
Priority to DE20321332U priority patent/DE20321332U1/en
Priority to JP2003578275A priority patent/JP4288179B2/en
Priority to AT03744764T priority patent/ATE342227T1/en
Priority to AU2003232582A priority patent/AU2003232582A1/en
Priority to PCT/DE2003/000968 priority patent/WO2003080505A1/en
Publication of DE10240953A1 publication Critical patent/DE10240953A1/en
Ceased legal-status Critical Current

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    • C—CHEMISTRY; METALLURGY
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    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C01B3/384—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts the catalyst being continuously externally heated
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B01J8/0446—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical
    • B01J8/0461—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical annular shaped beds
    • B01J8/0469—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical annular shaped beds the beds being superimposed one above the other
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B01J8/0496—Heating or cooling the reactor
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    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/48—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents followed by reaction of water vapour with carbon monoxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00106—Controlling the temperature by indirect heat exchange
    • B01J2208/00115—Controlling the temperature by indirect heat exchange with heat exchange elements inside the bed of solid particles
    • B01J2208/0015—Plates; Cylinders
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00106—Controlling the temperature by indirect heat exchange
    • B01J2208/00168—Controlling the temperature by indirect heat exchange with heat exchange elements outside the bed of solid particles
    • B01J2208/00203—Coils
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00106—Controlling the temperature by indirect heat exchange
    • B01J2208/00309—Controlling the temperature by indirect heat exchange with two or more reactions in heat exchange with each other, such as an endothermic reaction in heat exchange with an exothermic reaction
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00504—Controlling the temperature by means of a burner
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/0053—Controlling multiple zones along the direction of flow, e.g. pre-heating and after-cooling
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
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    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0283—Processes for making hydrogen or synthesis gas containing a CO-shift step, i.e. a water gas shift step
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    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0435—Catalytic purification
    • C01B2203/044—Selective oxidation of carbon monoxide
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0435—Catalytic purification
    • C01B2203/0445—Selective methanation
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0465—Composition of the impurity
    • C01B2203/047—Composition of the impurity the impurity being carbon monoxide
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0811—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel
    • C01B2203/0816—Heating by flames
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0838—Methods of heating the process for making hydrogen or synthesis gas by heat exchange with exothermic reactions, other than by combustion of fuel
    • C01B2203/0844—Methods of heating the process for making hydrogen or synthesis gas by heat exchange with exothermic reactions, other than by combustion of fuel the non-combustive exothermic reaction being another reforming reaction as defined in groups C01B2203/02 - C01B2203/0294
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    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • C01B2203/1241—Natural gas or methane
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    • C01B2203/80—Aspect of integrated processes for the production of hydrogen or synthesis gas not covered by groups C01B2203/02 - C01B2203/1695
    • C01B2203/82—Several process steps of C01B2203/02 - C01B2203/08 integrated into a single apparatus

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  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Abstract

Hydrogen production device comprises heated steam reforming stage with reforming catalyst to convert gaseous hydrocarbons and water into hydrogen, carbon monoxide and further reformer products, conversion stages to catalytically convert hydrogen, carbon monoxide and steam mixture leaving reforming stage, and fine purification stage to catalytically reduce residual carbon monoxide in conversion products. Device for producing hydrogen comprises heated steam reforming stage (1) with reforming catalyst to convert gaseous or vaporizable hydrocarbons and water into hydrogen, carbon monoxide and further reformer products, conversion stages (2a, 2b) connected to reforming stage to catalytically convert mixture of hydrogen, carbon monoxide and excess steam leaving reforming stage, and fine purification stage (3) connected to conversion stages to catalytically reduce residual carbon monoxide content of conversion products. Conversion stages and purification stage are each formed as hollow bodies having annular chamber for receiving corresponding catalysts.

Description

Die Erfindung betrifft einen Apparat zur Erzeugung von Wasserstoff gemäß dem Oberbegriff des Anspruchs 1.The invention relates to an apparatus for the production of hydrogen according to the preamble of the claim 1.

Ein gattungsgemäßer Apparat ist beispielsweise aus der (noch nicht veröffentlichten) DE 102 13 326.3 bekannt. Mit diesem Apparat wird Wasserstoff vorzugsweise zum Betrieb einer Polymermembran-Brennstoffzelle erzeugt, wobei das gesamte Gaserzeugungs- und Brennstoffzellensystem als Hausenergieversorgungsanlage zur Erzeugung von Strom und Wärme eingesetzbar ist.A generic apparatus is, for example, from the (not yet published) DE 102 13 326.3 known. With this apparatus, hydrogen is preferably generated for the operation of a polymer membrane fuel cell, the entire gas generation and fuel cell system being usable as a domestic energy supply system for generating electricity and heat.

Bei diesem Apparat weist die mindestens eine dem Reformer nachgeschaltete Katalysatorstufe eine im wesentlichen hohlzylindrisch ausgebildete Form auf, was den Vorteil hat, dass die radiale, Temperaturverteilung wesentlich gleichmäßiger als bei einer zylindrischen Katalysatorstufe ausgebildet ist. Die Temperaturverteilung ist dabei deshalb für den Reformerprozess von besonderer Bedeutung, da sie unmittelbaren Einfluss auf die Gleichgewichtsreaktion bei der Umwandlung von Kohlendioxid in Kohlenmonoxid hat. Betrachtet man beispielsweise eine üblicherweise verwendete zylindrische Shiftstufe, so führen die radialbezogen unterschiedlichen Temperaturen zu unterschiedlichen Kohlenmonoxid-Anteilen im Produktgas, was, da der Einsatz der Katalysatorstufen ja auf einen möglichst geringen Kohlenmonoxidanteil im Produktgases abzielt, keine optimalen Ergebnisse zur Folge hat.In this apparatus, the at least one the catalyst stage downstream of the reformer is essentially one hollow cylindrical shape, which has the advantage that the radial, temperature distribution much more even than is formed in a cylindrical catalyst stage. The temperature distribution is therefore for the reform process of particular importance as it is immediate Influence on the equilibrium reaction in the conversion of carbon dioxide in carbon monoxide. For example, consider one usually used cylindrical shift stage, so lead radially different Temperatures at different carbon monoxide proportions in the product gas, what, because the use of the catalyst stages on a possible low carbon monoxide content in the product gas, no optimal results has the consequence.

Mit dem Einsatz der hohlzylindrisch ausgebildeten Katalysatorstufe nach der DE 102 13 326.3 ist das Problem der radial ungleichmäßigen Temperaturverteilung im wesentlichen gelöst. Als problematisch hat sich darüber hinaus aber auch noch herausgestellt, dass innerhalb der Katalysatorstufe in axialer Richtung aufgrund der exothermen Reaktion bei der Umwandlung von Kohlendioxid in Kohlenmonoxid ebenfalls eine Verungleichmäßigung des Temperaturprofils und damit eine Verschlechterung der Gasqualität resultiert.With the use of the hollow cylindrical catalyst stage after the DE 102 13 326.3 the problem of radially uneven temperature distribution is essentially solved. In addition, it has also proven to be problematic that within the catalyst stage in the axial direction, due to the exothermic reaction during the conversion of carbon dioxide to carbon monoxide, the temperature profile also becomes uneven and thus the gas quality deteriorates.

Der Erfindung liegt demgemäß die Aufgabe zugrunde, bei einem Apparat der eingangs genannten Art durch möglichst einfache technische Mittel, eine Vergleichmäßigung des Temperaturprofils in axialer Richtung der Katalysatorstufe zu realisieren.The invention is accordingly based on the object in the case of an apparatus of the type mentioned at the beginning, if possible simple technical means, an equalization of the temperature profile to realize in the axial direction of the catalyst stage.

Diese Aufgabe ist mit einem Apparat der eingangs genannten Art durch die im Kennzeichen des Anspruchs 1 genannten Merkmale gelöst.This task is with an apparatus of the type mentioned in the characterizing part of the claim 1 mentioned features solved.

Nach der Erfindung ist also vorgesehen, die mindestens eine Shiftstufe mit einem Umschließungsgehäuse zu versehen, durch das ein Kühlmedium gefördert wird, um die bei der Umwandlung von Kohlendioxid in Kohlenmonoxid entstehende Wärme abzutransportieren. Wie später noch ausführlich beschrieben wird, bilden also einerseits die Oberfläche des Shiftstufenkatalysators (bzw. eine entsprechende Ummantelung) und andererseits die Wand des Umschließungsgehäuses die Flankierungen des erfindungsgemäßen Kühlkanals, der gleichzeitig noch den Vorteil mit sich bringt, dass die in der Shiftstufe anfallende Wärme gezielt abgeführt werden kann und nicht nutzlos an die Umgebung des Apparats abgegeben wird. Aufgrund der Außenmantelkühlung ergibt sich eine erhebliche Vergleichmäßigung des axialen Temperaturprofils, d. h. durch die Kombination aus Außenmantelkühlung und Ausbildung des Katalysators als Hohlzylinder wird an jeder Stelle der Shiftstufe im gleichen Maße Kohlendioxid in Kohlenmonoxid umgewandelt.According to the invention it is therefore provided to provide the at least one shift stage with an enclosure, through which a cooling medium promoted is used to converting carbon dioxide to carbon monoxide to remove the heat generated. How later still detailed is described, on the one hand, form the surface of the Shift stage catalyst (or a corresponding casing) and on the other hand, the wall of the enclosure housing the flanks of the cooling duct according to the invention, which also has the advantage that those in the Shift level heat deliberately dissipated can be released and not useless to the environment of the apparatus becomes. Due to the outer jacket cooling results a considerable equalization of the axial temperature profile, d. H. through the combination of outer jacket cooling and Training of the catalyst as a hollow cylinder is at every point the shift level to the same extent Carbon dioxide converted to carbon monoxide.

Nach einer vorteilhaften Weiterbildung ist vorgesehen, dass das Strömungsführungsgehäuse Zu- und Abfuhranschlüsse für das Kühlmedium aufweist und wahlweise im Gleich- oder Gegenstrom zur Durchströmungsrichtung innerhalb der Katalysatorstufe durchströmbar ausgebildet ist. Ist dabei auf der Reaktionsseite am Katalysatoreintritt mit einer starken Wärmeentwicklung zu rechnen, begünstigt ein Gleichstrombetrieb auf Grund des grösseren thermodynamischen Temperaturabstandes der beteiligten Medien die Kühlwirkung und somit einen Betrieb in Richtung Isometrie, d. h. hin zu einer gleichmäßigen Temperaturverteilung in der Shiftstufe. Entsprechendes gilt für den umgekehrten Fall des Gegenstroms.After an advantageous further education it is provided that the flow guide housing and drain connections for the cooling medium has and optionally in cocurrent or countercurrent to the flow direction is designed to flow through within the catalyst stage. Is in on the reaction side at the catalyst inlet with a strong heat generation to count, favors DC operation due to the larger thermodynamic temperature difference the cooling effect of the media involved and thus an operation in the direction of isometry, d. H. towards one even temperature distribution in the shift stage. The same applies to the reverse case of Counter current.

Ferner ist, was noch näher beschrieben wird, vorgesehen, dass wahlweise zum Vorheizen des dem Reformer zugeführten Wassers und/oder Kohlenwasserstoffgas diese bzw. dieses als Kühlmedium dem Strömungsführungsgehäuse zuführbar ist bzw. sind, wozu das Strömungsführungsgehäuse vorzugsweise abfuhranschlussseitig hydraulisch mit dem Edukteingang des Reformers verbunden ist.Furthermore, what is described in more detail is provided that optionally for preheating the reformer supplied Water and / or hydrocarbon gas this or this as the cooling medium Flow guide housing can be fed or are, for which purpose the flow guide housing is preferred on the discharge connection side hydraulically with the educt input of the reformer connected is.

Eine andere vorteilhafte Weiterbildung des erfindungsgemäßen Apparats besteht darin, dass wahlweise an den Zu- und/oder Abfuhranschlüssen des Strömungsführungsgehäuses ein Regelventil zur Massenstromeinstellung des Kühlmediums vorgesehen ist. Zusammen mit einem nach der mindestens einen Katalysatorstufe im Strömungsweg des Wasserstoffs und der übrigen Reformer-Produkte angeordneten Temperatursensor und einer übergeordneten Regeleinrichtung ist eine an der Katalysatorstufenaustrittstemperatur orientierte Massenstromeinstellung des Kühlmediums, das, wie gesagt, auch aus den Reformer-Edukten gebildet sein kann, möglich.Another advantageous training of the apparatus according to the invention consists in the fact that optionally at the inlet and / or outlet connections of the Flow guide housing Control valve for mass flow adjustment of the cooling medium is provided. Together with one after the at least one catalyst stage in the flow path of hydrogen and the rest Reformer products arranged temperature sensor and a parent The control device is at the catalyst stage outlet temperature oriented mass flow setting of the cooling medium, which, as I said, can also be formed from the reformer starting materials, possible.

Andere vorteilhafte Weiterbildungen ergeben sich aus den abhängigen Ansprüchen.Other advantageous developments result from the dependent Claims.

Der erfindungsgemäße Apparat sowie seine vorteilhaften Weiterbildungen gemäß der abhängigen Ansprüche werden nachfolgend anhand der zeichnerischen Darstellung eines Ausführungsbeispiels näher erläutert.The apparatus of the invention and its advantageous Developments according to the dependent claims in the following with the aid of the drawing of an embodiment explained in more detail.

Es zeigt schematischIt shows schematically

1 im Schnitt den erfindungsgemäßen Apparat mit einem Strömungsführungsgehäuse zur Außenmantelkühlung der Shiftstufe; und 1 on average the apparatus according to the invention with a flow guide housing for cooling the outer casing of the shift stage; and

2 einen Schnitt durch den Apparat gemäß 1 entlang der Linie A-A. 2 a section through the apparatus according to 1 along the line AA.

In 1 ist der erfindungsgemäße Apparat zur Erzeugung von Wasserstoff in einem Längsschnitt dargestellt. Dieser Apparat umfasst einen Reformer 1 zur Umwandlung von Kohlenwasserstoffgas (vorzugsweise Erdgas) und Wasser in Wasserstoff und weitere Reformer-Produkte wie Kohlendioxid und Kohlenmonoxid. Beim dargestellten Ausführungsbeispiel ist der Reformer 1 als hohlzylindrischer Körper ausgebildet, in dessen freien Zentrum ein Gasbrenner (vorzugsweise ein sogenannter Strahlungsbrenner) 10 zur Erzeugung der für die Reformierung erforderlichen Wärme angeordnet ist. Dem Reformer 1 ist zur Verringerung des Kohlenmonoxidanteils eine (es könnten auch mehrere sein – Hochtemperatur- und Niedertemperaturshiftstufe, sowie SelOx- oder Methanisierungsstufe) hohlzylindrisch ausgebildete Katalysatorstufe 2 nachgeschaltet. Unter "hohlzylindrisch" sind dabei natürlich auch beispielsweise mehreckige Hohlkörper zu verstehen, die zur Gewährleistung eines gleichmäßigen Temperaturprofils entsprechend dünnwandig ausgebildet sind. Die Wasserstofferzeugung geschieht somit gemäß folgender Schritte: Zunächst wird dem Reformer Kohlenwasserstoffgas und Wasserdampf zugeführt und dort mit Hilfe der Wärme des Gasbrenners (Temperatur etwa 800°C) in Wasserstoff, Kohlendioxid und Kohlenmonoxid umgewandelt. Am Reformerausgang wird das Produktgas mittels eines dort angeordneten Wärmetauschers 13 auf eine für den katalytischen Prozess zur Reduzierung des Kohlenmonoxidanteils geeignete Temperatur abgekühlt. In der Katalysatorstufe 2 erfolgt anschließend die Umwandlung des Kohlendioxids in Kohlenmonoxids bei einem Temperaturniveau von etwa 250°C bis 300°C. Nach der Shiftstufe, der, wie erwähnt, je nach erforderlicher Reinheit des Produktgases auch noch weitere, eventuell ebenfalls hohlzylindrische Stufen, wie zum Beispiel Methanisierungs- oder SelOx-Stufe nachgeschaltet sein können, gelangt das im wesentlichen kohlenmonoxidfreie Gas über die Produktgasleitung 12 zur Brennstoffzelle.In 1 the apparatus for generating hydrogen according to the invention is shown in a longitudinal section. This apparatus includes a reformer 1 for converting hydrocarbon gas (preferably natural gas) and water into hydrogen and other reformer products such as carbon dioxide and carbon monoxide. In the illustrated embodiment, the reformer 1 formed as a hollow cylindrical body, in the free center of which a gas burner (preferably a so-called radiation burner) 10 is arranged to generate the heat required for the reforming. The reformer 1 is a hollow cylindrical catalyst stage to reduce the carbon monoxide content (there could also be several - high-temperature and low-temperature shift stage, as well as SelOx or methanation stage) 2 downstream. “Hollow cylindrical” is of course also to be understood to mean, for example, polygonal hollow bodies which are designed to be thin-walled to ensure a uniform temperature profile. Hydrogen production is thus carried out according to the following steps: First, hydrocarbon gas and water vapor are fed to the reformer, where they are converted into hydrogen, carbon dioxide and carbon monoxide using the heat of the gas burner (temperature about 800 ° C.). At the reformer outlet, the product gas is generated by means of a heat exchanger located there 13 cooled to a temperature suitable for the catalytic process to reduce the carbon monoxide content. In the catalyst stage 2 the carbon dioxide is then converted into carbon monoxide at a temperature level of approximately 250 ° C. to 300 ° C. After the shift stage, which, as mentioned, depending on the required purity of the product gas, further, possibly also hollow cylindrical stages, such as, for example, methanation or SelOx stage, can follow, the essentially carbon monoxide-free gas passes through the product gas line 12 to the fuel cell.

Für den erfindungsgemäße Apparat ist nun zur Vergleichmäßigung des axialen Temperaturprofils innerhalb der Katalysatorstufe 2 wesentlich, dass ein diese von aussen umschließendes Strömungsführungsgehäuse 3 für ein Kühlmedium zur Kühlung der Katalysatorstufe 2 vorgesehen ist. Wie insbesondere aus 2 ersichtlich, ist beim dargestellten Ausführungsbeispiel dieses Strömungsführungsgehäuse 3 gewissermassen wie ein die Katalysatorstufe 2 umschließender, zylindrischer Mantel ausgebildet, der einen vom Kühlmedium durchströmten, konzentrischen Ringspalt begrenzt. Selbstverständlich sind aber auch andere Gestaltungen des Gehäuses realisierbar: wesentlich ist, dass eine ausreichende Wärmeabfuhr von der äusseren Peripherie der Katalysatorstufe gewährleistet ist. Hierzu ist beispielsweise sogar eine die Katalysatorstufe umschließende Rohrwendel geeignet, die allgemein ausgedrückt, auch nichts anderes als das beanspruchte Strömungsführungsgehäuse 3 ist.For the apparatus according to the invention, the axial temperature profile is now made uniform within the catalyst stage 2 essential that a flow guide housing enclosing this from the outside 3 for a cooling medium for cooling the catalyst stage 2 is provided. How especially out 2 can be seen in the illustrated embodiment, this flow guide housing 3 sort of like the catalyst stage 2 enclosing cylindrical jacket formed, which delimits a concentric annular gap through which the cooling medium flows. Of course, other designs of the housing can also be implemented: it is essential that sufficient heat dissipation from the outer periphery of the catalyst stage is ensured. For this purpose, for example, even a coiled tubing enclosing the catalyst stage is suitable, which, in general terms, is nothing other than the claimed flow guide housing 3 is.

Wie weiterhin in 1 dargestellt, ist bei dieser bevorzugten Ausführungsform vorgesehen, dass das Strömungsführungsgehäuse 3 Zu- 4 und Abfuhranschlüsse 5 für das Kühlmedium aufweist und vom Kühlmittel im Gegenstrom zur Durchströmungsrichtung innerhalb der Katalysatorstufe 2 durchströmbar ausgebildet ist. Als Kühlmedium wird dabei vorzugsweise das für den Reformerprozess ohnehin erforderlich Wasser verwendet, das aufgrund des erfindungsgemäßen Strömungsführungsgehäuses 3 vorteilhaft gleich vorgeheizt zum Reformereingang gelangt. Bei Bedarf kann aber auch das für den Reformerprozess erforderliche Kohlenwasserstoffgas zusammen mit dem Wasser über den Zufuhranschluss 4 dem Strömungsführungsgehäuse 3 zugeführt und dort vorgeheizt werden.As continues in 1 shown, it is provided in this preferred embodiment that the flow guide housing 3 Supply and drain connections 5 for the cooling medium and from the coolant in countercurrent to the flow direction within the catalyst stage 2 is designed to flow through. As the cooling medium, the water that is required for the reformer process is preferably used, which is due to the flow guide housing according to the invention 3 advantageously comes preheated to the reformer entrance. If necessary, however, the hydrocarbon gas required for the reformer process can also be supplied together with the water via the supply connection 4 the flow guide housing 3 fed and preheated there.

Zur Massenstromeinstellung des Kühlmediums ist beim dargestellten Ausführungsbeispiel vorzugsweise am Zufuhranschluss 4 ein Regelventil 6 vorgesehen, das über eine Leitung mit einer übergeordneten Regeleinrichtung 8 in Verbindung steht. Gleichzeitig ist vorzugsweise nach der Katalysatorstufe 2 im Strömungsweg des Wasserstoffs und der übrigen Reformer-Produkte ein Temperatursensor 7 angeordnet ist, der seinerseits zur Massenstromeinstellung des Kühlmediums über die übergeordnete Regeleinrichtung 8 mit dem Regelventil 6 verbunden ist. Auf diese Weise kann also in Abhängigkeit von der Produktgasaustrittstemperatur die Kühlleistung an der Mantelfläche der Katalysatorstufe 2 in gewissen Grenzen variiert werden.For setting the mass flow of the cooling medium, it is preferably in the exemplary embodiment shown at the supply connection 4 a control valve 6 provided that via a line with a higher-level control device 8th communicates. At the same time is preferably after the catalyst stage 2 A temperature sensor in the flow path of the hydrogen and the other reformer products 7 is arranged, which in turn for mass flow adjustment of the cooling medium via the higher-level control device 8th with the control valve 6 connected is. In this way, depending on the product gas outlet temperature, the cooling capacity on the outer surface of the catalyst stage 2 can be varied within certain limits.

Schließlich ist vorteilhaft vorgesehen, dass im Innern der hohlzylindrisch ausgebildeten Katalysatorstufe 2 ein weiterer Kühlmediumkanal 9 angeordnet ist, der vorzugs- und wahlweise vom Wasser und/oder vom Kohlenwasserstoffgas durchströmbar ist. Die Zuführung des Kühlmediums erfolgt dabei über die Anschlussleitung 11; die Abfuhrleitung ist, da ohne weiteres vorstellbar, nicht dargestellt.Finally, it is advantageously provided that inside the hollow cylindrical catalyst stage 2 another cooling medium channel 9 is arranged, through which water and / or hydrocarbon gas can flow, preferably. The cooling medium is supplied via the connection line 11 ; the discharge line is not shown since it is easily conceivable.

11
Reformerreformer
22
Katalysatorstufecatalyst stage
33
StrömungsführungsgehäuseFlow guidance housing
44
Zufuhranschlusssupply port
55
Abfuhranschlusswithdrawal connection
66
Regelventilcontrol valve
77
Temperatursensortemperature sensor
88th
Regeleinrichtungcontrol device
99
KühlmediumkanalCoolant channel
1010
Gasbrennergas burner
1111
Anschlussleitungconnecting cable
1212
ProduktgasleitungProduct gas line
1313
Wärmetauscherheat exchangers

Claims (8)

Apparat zur Erzeugung von Wasserstoff, umfassend einen Reformer (1) zur Umwandlung von Kohlenwasserstoffgas und Wasser in Wasserstoff und weitere Reformer-Produkte wie Kohlendioxid und Kohlenmonoxid, wobei dem Reformer (1) zur Verringerung des Kohlenmonoxidanteils mindestens eine hohlzylindrisch ausgebildete Katalysatorstufe (2) nachgeschaltet ist, dadurch gekennzeichnet, dass ein die Katalysatorstufe (2) von aussen umschließendes Strömungsführungsgehäuse (3) für ein Kühlmedium zur Kühlung der Katalysatorstufe (2) vorgesehen ist.Apparatus for generating hydrogen in order capturing a reformer ( 1 ) for converting hydrocarbon gas and water into hydrogen and other reformer products such as carbon dioxide and carbon monoxide, the reformer ( 1 ) to reduce the carbon monoxide content at least one hollow cylindrical catalyst stage ( 2 ) is connected downstream, characterized in that the catalyst stage ( 2 ) surrounding flow guide housing ( 3 ) for a cooling medium for cooling the catalyst stage ( 2 ) is provided. Apparat nach Anspruch 1, dadurch gekennzeichnet, dass das Strömungsführungsgehäuse (3) Zu- (4) und Abfuhranschlüsse (5) für das Kühlmedium aufweist und wahlweise im Gleich- oder Gegenstrom zur Durchströmungsrichtung innerhalb der Katalysatorstufe (2) durchströmbar ausgebildet ist.Apparatus according to claim 1, characterized in that the flow guide housing ( 3 ) To- ( 4 ) and drain connections ( 5 ) for the cooling medium and optionally in cocurrent or countercurrent to the direction of flow within the catalyst stage ( 2 ) is designed to flow through. Apparat nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass zum Vorheizen des dem Reformer (1) zugeführten Wassers dieses als Kühlmedium dem Strömungsführungsgehäuse (3) zuführbar ist.Apparatus according to claim 1 or 2, characterized in that for preheating the reformer ( 1 ) water supplied to the flow guide housing as a cooling medium ( 3 ) can be fed. Apparat nach einem der Ansprüche 1 bis 3, dadurch gekennzeichnet, dass zum Vorheizen des dem Reformer (1) zugeführten Kohlenwasserstoffgases dieses als Kühlmedium dem Strömungsführungsgehäuse (3) zuführbar ist.Apparatus according to one of Claims 1 to 3, characterized in that for preheating the reformer ( 1 ) supplied hydrocarbon gas this as a cooling medium to the flow guide housing ( 3 ) can be fed. Apparat nach einem der Ansprüche 2 bis 4, dadurch gekennzeichnet, dass das Strömungsführungsgehäuse (3) abfuhranschlussseitig hydraulisch mit dem Reformer (1) edukteingangsseitig verbunden ist.Apparatus according to one of claims 2 to 4, characterized in that the flow guide housing ( 3 ) hydraulically with the reformer on the discharge connection side ( 1 ) is connected on the educt input side. Apparat nach einem der Ansprüche 2 bis 5, dadurch gekennzeichnet, dass wahlweise an den Zu- (4) und/oder Abfuhranschlüssen (5) des Strömungsführungsgehäuses (3) ein Regelventil (6) zur Massenstromeinstellung des Kühlmediums vorgesehen ist.Apparatus according to one of claims 2 to 5, characterized in that optionally at the inlet (4) and / or outlet connections ( 5 ) of the flow guide housing ( 3 ) a control valve ( 6 ) is provided for setting the mass flow of the cooling medium. Apparat nach Anspruch 6, dadurch gekennzeichnet, dass nach der mindestens einen Katalysatorstufe (2) im Strömungsweg des Wasserstoffs und der übrigen Reformer-Produkte ein Temperatursensor (7) angeordnet ist, der zur Massenstromeinstellung des Kühlmediums über eine übergeordnete Regeleinrichtung (8) mit dem Regelventil (6) verbunden ist.Apparatus according to claim 6, characterized in that after the at least one catalyst stage ( 2 ) a temperature sensor in the flow path of the hydrogen and the other reformer products ( 7 ) is arranged, which is used to set the mass flow of the cooling medium via a higher-level control device ( 8th ) with the control valve ( 6 ) connected is. Apparat nach einem der Ansprüche 1 bis 7, dadurch gekennzeichnet, dass im Innern der hohlzylindrisch ausgebildeten Katalysatorstufe (2) ein weiterer Kühlmediumkanal (9) angeordnet ist, der vorzugs- und wahlweise vom Wasser und/oder vom Kohlenwasserstoffgas durchströmbar ist.Apparatus according to one of claims 1 to 7, characterized in that in the interior of the hollow cylindrical catalyst stage ( 2 ) another cooling medium channel ( 9 ) is arranged, which can be flowed through and preferably by water and / or by hydrocarbon gas.
DE2002140953 1987-11-20 2002-09-02 Device for producing hydrogen has conversion stages and fine purification stage formed as hollow bodies having an annular chamber for receiving corresponding catalysts Ceased DE10240953A1 (en)

Priority Applications (9)

Application Number Priority Date Filing Date Title
DE2002140953 DE10240953A1 (en) 2002-09-02 2002-09-02 Device for producing hydrogen has conversion stages and fine purification stage formed as hollow bodies having an annular chamber for receiving corresponding catalysts
US10/508,881 US20050172553A1 (en) 2002-03-25 2003-03-24 Device for the generation of hydrogen
EP03744764A EP1427668B9 (en) 2002-03-25 2003-03-24 Device for the generation of hydrogen
DE50305340T DE50305340D1 (en) 2002-03-25 2003-03-24 DEVICE FOR PRODUCING HYDROGEN
DE20321332U DE20321332U1 (en) 1987-11-20 2003-03-24 Device for producing hydrogen has conversion stages and fine purification stage formed as hollow bodies having an annular chamber for receiving corresponding catalysts
JP2003578275A JP4288179B2 (en) 2002-03-25 2003-03-24 Hydrogen generator
AT03744764T ATE342227T1 (en) 2002-03-25 2003-03-24 DEVICE FOR GENERATING HYDROGEN
AU2003232582A AU2003232582A1 (en) 2002-03-25 2003-03-24 Device for the generation of hydrogen
PCT/DE2003/000968 WO2003080505A1 (en) 2002-03-25 2003-03-24 Device for the generation of hydrogen

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