EP3972730A1 - Membrane reactor - Google Patents

Membrane reactor

Info

Publication number
EP3972730A1
EP3972730A1 EP20711774.8A EP20711774A EP3972730A1 EP 3972730 A1 EP3972730 A1 EP 3972730A1 EP 20711774 A EP20711774 A EP 20711774A EP 3972730 A1 EP3972730 A1 EP 3972730A1
Authority
EP
European Patent Office
Prior art keywords
housing
membrane
process gas
permeate
flow channel
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.)
Pending
Application number
EP20711774.8A
Other languages
German (de)
French (fr)
Inventor
Roland Kirchberger
Michael Lang
Nicole Wermuth
Igor SAUPERL
Benjamin JÄGER
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.)
Lec GmbH
Original Assignee
Lec GmbH
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Lec GmbH filed Critical Lec GmbH
Publication of EP3972730A1 publication Critical patent/EP3972730A1/en
Pending legal-status Critical Current

Links

Classifications

    • 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
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/2475—Membrane reactors
    • 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
    • B01J8/008—Details of the reactor or of the particulate material; Processes to increase or to retard the rate of reaction
    • B01J8/009—Membranes, e.g. feeding or removing reactants or products to or from the catalyst bed through a membrane
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • 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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • 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
    • C01B3/323—Catalytic reaction of gaseous or liquid organic compounds other than hydrocarbons with gasifying agents
    • 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
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2491—Other constructional details
    • B01J2219/2492—Assembling means
    • B01J2219/2496—Means for assembling modules together, e.g. casings, holders, fluidic connectors
    • 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
    • C01B2203/0405—Purification by membrane separation
    • C01B2203/041—In-situ membrane purification during hydrogen production
    • 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
    • C01B2203/12—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
    • C01B2203/1217—Alcohols
    • C01B2203/1223—Methanol

Definitions

  • the invention relates to a membrane reactor with a housing penetrating, a catalyst receiving flow channel for a process gas and with a flow path for a permeate, which is separated from the flow channel for the process gas by a permeate membrane.
  • methanol which has a high energy density and unlimited storage without losses, be used as a liquid, easily manageable hydrogen storage device.
  • a vaporized methanol-water mixture is converted as a process gas in a catalytic reaction essentially into hydrogen and carbon dioxide, the hydrogen being the main component of the permeate and the carbon monoxide being the main component of the retentate.
  • the process gas which is essentially made up of methanol and water, is passed through a tubular duct equipped with a catalyst, the jacket of which serves as a porous support for the membrane.
  • the permeate formed by the hydrogen penetrating the membrane is withdrawn in countercurrent to the process gas through the annular gap between the pipe channel and the reactor housing enclosing the pipe channel at a distance.
  • the invention is therefore based on the object of designing a membrane reactor in such a way that over the entire local and temporal course of the reaction, favorable parameters for the catalytic conversion of a process gas into a permeate, in particular for the production of hydrogen from methanol, can be guaranteed.
  • the invention solves the problem in that the housing is composed of individual housing modules that form the flow channel for the process gas that runs from housing module to housing module and that are connected to a collecting line for the permeate, transversely have hollow bodies aligned with the flow channel as a carrier for the membrane.
  • housing modules form housing rings which are flanged together between two end caps provided on the one hand with an inlet for the process gas and on the other hand with an outlet for the retentate, so that between the two end caps they differ in their structure and number Housing modules can be combined into a membrane reactor adapted to the respective requirements.
  • the individual housing rings can be sealed against one another in a simple manner with the aid of ring seals.
  • housing modules for permeate discharge on the flow inlet side can be provided with appropriate catalysts, there are advantages in terms of freedom of design if the catalyst and the hollow body provided with the membrane are provided in separate housing modules.
  • the aligned transversely to the flow channel, enclosed with a membrane for Permeatab conduction hollow bodies can be formed in a simple manner from porous tubes which open into collecting spaces provided on the outside of the housing modules and connected to the collecting line. With the number and the diameter of these tubes carrying the membrane, the ratio of the membrane area to the cross section of the flow channel for the process gas or the reaction gas can easily be determined.
  • At least one housing module can have a heat exchanger.
  • heat exchanger modules heat can both be supplied and removed as required in order to be able to set the most favorable process temperature in each case.
  • Show it 1 shows a membrane reactor according to the invention in a schematic longitudinal section
  • FIGS. 1 and 2 shows a section along the line II-II in FIGS. 1 and
  • FIG. 3 shows an embodiment variant of a membrane reactor according to the invention in a schematic section corresponding to FIG. 1.
  • a membrane reactor according to the invention has a housing 1, which is composed of individual, preferably housing rings forming housing modules 2, 3 and 4, which are flanged together sealingly between two end caps 5, 6.
  • the flanged housing modules 2, 3 and 4 form a continuous flow channel 7, which is exposed to a process gas 9 through an inlet 8 of the end cap 5 and opens into an outlet 10 for the retentate 11 in the area of the opposite end cap 6.
  • the housing modules 2 have hollow bodies 12 running transversely to the flow channel 7 in the form of porous tubes as supports for a membrane 13. These hollow bodies 12 open into a collecting space 16 provided on the outside of the housing modules 2 and connected to a collecting line 14 for the permeate 15.
  • the housing modules 2 for permeate discharge are provided in the flow direction of the process gas 9 with a catalyst 17 housing modules 3 vorgela.
  • the catalytic conversion of the process gas 9 into a permeate 15 and a retentate 11 takes place.
  • the permeate that forms is deposited in the respective subsequent housing module 2 via the membrane 13 and discharged through the hollow body 12.
  • the process gas portion is catalytically converted again in a subsequent flow section in order to be able to remove a largely process gas-free retentate 11 from the membrane reactor after a multistage catalytic conversion with subsequent permeate discharge.
  • the influence of temperature on the catalytic reaction can be taken into account by housing modules 4 which accommodate a heat exchanger 18, for example in the form of coiled tubes for a heat carrier, with the help of which heat can either be introduced or removed as required.
  • a membrane reactor according to FIG. 1 is charged with a methanol-water vapor mixture as process gas 9 for hydrogen production, a partially catalytic conversion of the process gas 9 into the main components carbon dioxide and hydrogen takes place first in a housing module 3, which in the following housing module 2 via the Membrane 13 is derived through the hollow body 12.
  • the remaining reaction gas from process gas enriched with carbon dioxide is heated to a process temperature favorable for the subsequent catalytic reaction by supplying heat in the subsequent heat exchanger 18 of a housing module 4 in order to be able to divert the hydrogen converted from the process gas into a housing module 2.
  • the hydrogen deposited in the individual housing modules 2 is drawn off for further use through a collecting line 14 common to these housing modules 2.
  • FIG. 3 shows a membrane reactor whose inlet side catalyst section has been extended compared to the exemplary embodiment according to FIG. 1 by connecting two housing modules 3 accommodating a catalyst 17 in series.
  • the process temperature in this extended catalyst section is influenced by an upstream heat exchanger 18 of a housing module 4.
  • the subsequent implementation of the process gas remaining in the reaction gas is optimized according to FIG.
  • the modular structure of the membrane reactor can be optimally adapted to different requirements of the conversion and separation processes, because the arrangement and properties of catalysts, heat exchangers and membranes can be changed as required and to the respective reaction as well as initially unknown boundary conditions and component properties can be coordinated so that all housing modules can work in an optimal range of the parameters relevant for the conversion.

Abstract

The invention relates to a membrane reactor comprising a flow channel (7), which passes through a housing (1) and receives a catalyst (17), for a process gas (9) and comprising a flow path for a permeate (15), said flow path being separated from the flow channel (7) for the process gas (9) by a membrane (13) which is permeable to the permeate (15). The aim of the invention is to achieve advantageous structural conditions. This is achieved in that the housing (1) is assembled from individual housing modules (2, 3, 4) that form the flow channel (7), which passes through the housing modules (2, 3, 4) one after the other, for the process gas (9) and have hollow bodies (12), which are connected to a collection line (14) for the permeate (15) and are aligned transversely to the flow channel (7), as supports for the membrane (13).

Description

Membranreaktor Membrane reactor
Technisches Gebiet Technical area
Die Erfindung bezieht sich auf einen Membranreaktor mit einem ein Gehäuse durchsetzenden, einen Katalysator aufnehmenden Strömungskanal für ein Pro zessgas und mit einem Strömungsweg für ein Permeat, der vom Strömungskanal für das Prozessgas durch eine für das Permeat durchlässige Membran getrennt ist. The invention relates to a membrane reactor with a housing penetrating, a catalyst receiving flow channel for a process gas and with a flow path for a permeate, which is separated from the flow channel for the process gas by a permeate membrane.
Stand der Technik State of the art
Um die mit der Lagerung von Wasserstoff beispielsweise als Treibstoff für Schiffs antriebe verbundenen Schwierigkeiten zu vermeiden, wurde bereits vorgeschla gen, Methanol, das eine hohe Energiedichte besitzt und eine unbegrenzte Lage rung ohne Verluste erlaubt, als flüssigen, gut handhabbaren Wasserstoffspeicher einzusetzen. In einem Membranreaktor wird ein verdampftes Methanol- Wassergemisch als Prozessgas in einer katalytischen Reaktion im Wesentlichen in Wasserstoff und Kohlendioxid umgesetzt, wobei der Wasserstoff die Haupt komponente des Permeats und das Kohlenmonoxid die Hauptkomponente des Retentats bilden. Das im Wesentlichen aus Methanol und Wasser gebildete Pro zessgas wird durch einen mit einem Katalysator bestückten Rohrkanal geleitet, dessen Mantel als poröser Träger für die Membran dient. Das durch den die Membran durchsetzenden Wasserstoff gebildete Permeat wird im Gegenstrom zum Prozessgas durch den Ringspalt zwischen dem Rohrkanal und dem den Rohrkanal mit Abstand umschließenden Reaktorgehäuse abgezogen. In order to avoid the difficulties associated with the storage of hydrogen, for example as a fuel for ship propulsion, it has already been proposed that methanol, which has a high energy density and unlimited storage without losses, be used as a liquid, easily manageable hydrogen storage device. In a membrane reactor, a vaporized methanol-water mixture is converted as a process gas in a catalytic reaction essentially into hydrogen and carbon dioxide, the hydrogen being the main component of the permeate and the carbon monoxide being the main component of the retentate. The process gas, which is essentially made up of methanol and water, is passed through a tubular duct equipped with a catalyst, the jacket of which serves as a porous support for the membrane. The permeate formed by the hydrogen penetrating the membrane is withdrawn in countercurrent to the process gas through the annular gap between the pipe channel and the reactor housing enclosing the pipe channel at a distance.
Nachteilig bei diesen Membranreaktoren ist, dass sich entlang des axialen Strö mungswegs des Prozessgases durch den Rohrkanal die für die katalytische Reak tion bestimmenden Parameter, wie Druck, Temperatur und chem ische Zusam- mensetzung, ändern, sodass sich hinsichtlich der Optimierung des Umsetzungs prozesses Schwierigkeiten ergeben, die zu ungünstigen Wirkungsgraden führen. The disadvantage of these membrane reactors is that the parameters that determine the catalytic reaction, such as pressure, temperature and chemical combination, vary along the axial flow path of the process gas through the pipe channel. composition, so that difficulties arise with regard to the optimization of the implementation process, which lead to unfavorable levels of efficiency.
Darstellung der Erfindung Presentation of the invention
Der Erfindung liegt somit die Aufgabe zugrunde, einen Membranreaktor so auszu gestalten, dass über den gesamten örtlichen und zeitlichen Reaktionsverlauf vor teilhafte Parameter für die katalytische Umsetzung eines Prozessgases in ein Permeat, insbesondere zur Gewinnung von Wasserstoff aus Methanol, gewähr leistet werden können. The invention is therefore based on the object of designing a membrane reactor in such a way that over the entire local and temporal course of the reaction, favorable parameters for the catalytic conversion of a process gas into a permeate, in particular for the production of hydrogen from methanol, can be guaranteed.
Ausgehend von einem Membranreaktor der eingangs geschilderten Art löst die Er findung die gestellte Aufgabe dadurch, dass das Gehäuse aus einzelnen Gehäu semodulen zusammengesetzt ist, die den von Gehäusemodul zu Gehäusemodul durchgehenden Strömungskanal für das Prozessgas bilden und an eine Sammel leitung für das Permeat angeschlossene, quer zum Strömungskanal ausgerichtete Hohlkörper als Träger für die Membran aufweisen. Based on a membrane reactor of the type described above, the invention solves the problem in that the housing is composed of individual housing modules that form the flow channel for the process gas that runs from housing module to housing module and that are connected to a collecting line for the permeate, transversely have hollow bodies aligned with the flow channel as a carrier for the membrane.
Aufgrund der Zusammensetzung des Gehäuses des Membranreaktors aus ein zelnen Gehäusemodulen, die je einen Strömungskanalabschnitt bilden, können für jeden Strömungsabschnitt des Prozessgases bzw. des Reaktionsgases, das sich aus dem Prozessgas und dem Retentat aus dem bereits umgesetzten Prozessgas zusammensetzt, jeweils vorteilhafte Parameter für die katalytische Umsetzung und die Abscheidung des Permeats vorgegeben werden, weil die einzelnen Gehäuse- module entsprechend gestaltet werden können. Mit dem Vorsehen von einzelnen Gehäusemodulen zur Permeatableitung entlang des Strömungskanals für das Produktgas und von diesen Gehäusemodulen zugeordneten Katalysatoren, die gegebenenfalls die sich aufgrund der Permeatableitung und der chemischen Re aktionen ändernde Zusammensetzung des Reaktionsgases berücksichtigen, kön nen im Bereich jeder dieser voneinander gesonderten Abschnitte für die katalyti schen Reaktionen vorteilhafte, weitgehend konstante Umsetzungsparameter ge währleistet werden. Besonders einfache Konstruktionsverhältnisse ergeben sich, wenn die Gehäuse- module Gehäuseringe bilden, die zwischen zwei einerseits mit einem Zulauf für das Prozessgas und anderseits mit einem Ablauf für das Retentat versehenen Endkappen zusammengeflanscht sind, sodass zwischen den beiden Endkappen in ihrem Aufbau und in ihrer Anzahl unterschiedliche Gehäusemodule zu einem an die jeweiligen Anforderungen angepassten Membranreaktor zusammengefasst werden können. Die einzelnen Gehäuseringe können dabei in einfacher Weise mithilfe von Ringdichtungen gegeneinander abgedichtet werden. Due to the composition of the housing of the membrane reactor from individual housing modules that each form a flow channel section, advantageous parameters for the catalytic can be set for each flow section of the process gas or the reaction gas, which is composed of the process gas and the retentate from the process gas that has already been converted Implementation and separation of the permeate are specified because the individual housing modules can be designed accordingly. With the provision of individual housing modules for permeate discharge along the flow channel for the product gas and catalysts assigned to these housing modules, which may take into account the changes in the composition of the reaction gas due to the permeate discharge and the chemical reactions, each of these separate sections for the catalytic reactions advantageous, largely constant implementation parameters are guaranteed. Particularly simple construction conditions result when the housing modules form housing rings which are flanged together between two end caps provided on the one hand with an inlet for the process gas and on the other hand with an outlet for the retentate, so that between the two end caps they differ in their structure and number Housing modules can be combined into a membrane reactor adapted to the respective requirements. The individual housing rings can be sealed against one another in a simple manner with the aid of ring seals.
Obwohl die Gehäusemodule zur Permeatableitung auf der Strömungszulaufseite mit entsprechenden Katalysatoren versehen sein können, ergeben sich hinsicht lich der Gestaltungsfreiheit Vorteile, wenn der Katalysator und die mit der Memb ran versehenen Hohlkörper in gesonderten Gehäusemodulen vorgesehen sind. Although the housing modules for permeate discharge on the flow inlet side can be provided with appropriate catalysts, there are advantages in terms of freedom of design if the catalyst and the hollow body provided with the membrane are provided in separate housing modules.
Die quer zum Strömungskanal ausgerichteten, mit einer Membran zur Permeatab leitung umschlossenen Hohlkörper können in einfacher Weise aus porösen Roh ren gebildet werden, die in außen an den Gehäusemodulen vorgesehene, an die Sammelleitung angeschlossene Sammelräume münden. Mit der Anzahl und dem Durchmesser dieser die Membran tragenden Rohre lässt sich das Verhältnis der Membranfläche zum Querschnitt des Strömungskanals für das Prozessgas bzw. das Reaktionsgas einfach festlegen. The aligned transversely to the flow channel, enclosed with a membrane for Permeatab conduction hollow bodies can be formed in a simple manner from porous tubes which open into collecting spaces provided on the outside of the housing modules and connected to the collecting line. With the number and the diameter of these tubes carrying the membrane, the ratio of the membrane area to the cross section of the flow channel for the process gas or the reaction gas can easily be determined.
Um Einfluss auf die Temperatur nehmen zu können, kann zumindest ein Gehäu semodul einen Wärmetauscher aufweisen. Mit solchen Wärmetauschermodulen kann je nach Bedarf Wärme sowohl zugeführt als auch abgeführt werden, um die jeweils günstigste Prozesstemperatur einstellen zu können. In order to be able to influence the temperature, at least one housing module can have a heat exchanger. With such heat exchanger modules, heat can both be supplied and removed as required in order to be able to set the most favorable process temperature in each case.
Kurze Beschreibung der Erfindung Brief description of the invention
In der Zeichnung ist der Erfindungsgegenstand beispielsweise dargestellt. Es zei gen Fig. 1 einen erfindungsgemäßen Membranreaktor in einem schematischen Längsschnitt, The subject matter of the invention is shown in the drawing, for example. Show it 1 shows a membrane reactor according to the invention in a schematic longitudinal section,
Fig. 2 einen Schnitt nach der Linie ll-ll der Fig. 1 und 2 shows a section along the line II-II in FIGS. 1 and
Fig. 3 eine Ausführungsvariante eines erfindungsgemäßen Membranreaktors in einem der Fig. 1 entsprechenden, schematischen Schnitt. 3 shows an embodiment variant of a membrane reactor according to the invention in a schematic section corresponding to FIG. 1.
Wege zur Ausführung der Erfindung Ways of Carrying Out the Invention
Ein erfindungsgemäßer Membranreaktor weist ein Gehäuse 1 auf, das sich aus einzelnen, vorzugsweise Gehäuseringe bildenden Gehäusemodulen 2, 3 und 4 zusammensetzt, die zwischen zwei Endkappen 5, 6 dichtend zusammenge flanscht sind. Die zusammengeflanschten Gehäusemodule 2, 3 und 4 bilden einen durchgehenden Strömungskanal 7, der durch einen Zulauf 8 der Endkappe 5 mit einem Prozessgas 9 beaufschlagt wird und im Bereich der gegenüberliegenden Endkappe 6 in einen Ablauf 10 für das Retentat 1 1 mündet. A membrane reactor according to the invention has a housing 1, which is composed of individual, preferably housing rings forming housing modules 2, 3 and 4, which are flanged together sealingly between two end caps 5, 6. The flanged housing modules 2, 3 and 4 form a continuous flow channel 7, which is exposed to a process gas 9 through an inlet 8 of the end cap 5 and opens into an outlet 10 for the retentate 11 in the area of the opposite end cap 6.
Wie insbesondere der Fig. 2 entnommen werden kann, weisen die Gehäusemodu le 2 quer zum Strömungskanal 7 verlaufende Hohlkörper 12 in Form von porösen Rohren als Träger für eine Membran 13 auf. Diese Hohlkörper 12 münden in einen außen an den Gehäusemodulen 2 vorgesehenen, an eine Sammelleitung 14 für das Permeat 15 angeschlossenen Sammelraum 16. As can be seen in particular from FIG. 2, the housing modules 2 have hollow bodies 12 running transversely to the flow channel 7 in the form of porous tubes as supports for a membrane 13. These hollow bodies 12 open into a collecting space 16 provided on the outside of the housing modules 2 and connected to a collecting line 14 for the permeate 15.
Den Gehäusemodulen 2 zur Permeatableitung sind in Strömungsrichtung des Prozessgases 9 mit einem Katalysator 17 versehene Gehäusemodule 3 vorgela gert. In diesen Katalysatoren 17 findet die katalytische Umsetzung des Prozess gases 9 in ein Permeat 15 und ein Retentat 1 1 statt. Das sich bildende Permeat wird in dem jeweils nachfolgenden Gehäusemodul 2 über die Membran 13 abge schieden und durch die Hohlkörper 12 ausgetragen. Von dem Reaktionsgas ver bleibenden, wird der Prozessgasanteil in einem nachfolgenden Strömungsab schnitt wieder katalytisch umgewandelt, um gegebenenfalls nach einer mehrstufi gen katalytischen Umwandlung mit nachfolgender Permeatableitung ein weitge hend prozessgasfreies Retentat 1 1 aus dem Membranreaktor abführen zu kön- nen. Der Temperatureinfluss auf die katalytische Reaktion kann durch Gehäusemodule 4 berücksichtigt werden, die einen Wärmetauscher 18 aufnehmen, beispielsweise in Form von in Windungen verlegte Rohrschlangen für einen Wärmeträger, mit dessen Hilfe je nach Bedarf entweder Wärme eingebracht oder abgeführt werden kann. The housing modules 2 for permeate discharge are provided in the flow direction of the process gas 9 with a catalyst 17 housing modules 3 vorgela. In these catalysts 17, the catalytic conversion of the process gas 9 into a permeate 15 and a retentate 11 takes place. The permeate that forms is deposited in the respective subsequent housing module 2 via the membrane 13 and discharged through the hollow body 12. Of the remaining reaction gas, the process gas portion is catalytically converted again in a subsequent flow section in order to be able to remove a largely process gas-free retentate 11 from the membrane reactor after a multistage catalytic conversion with subsequent permeate discharge. The influence of temperature on the catalytic reaction can be taken into account by housing modules 4 which accommodate a heat exchanger 18, for example in the form of coiled tubes for a heat carrier, with the help of which heat can either be introduced or removed as required.
Wird ein Membranreaktor gemäß der Fig. 1 zur Wasserstoffgewinnung mit einem Methanol-Wasserdampfgemisch als Prozessgas 9 beaufschlagt, so erfolgt zu nächst in einem Gehäusemodul 3 eine teilweise katalytische Umsetzung des Pro zessgases 9 in die Hauptkomponenten Kohlendioxid und Wasserstoff, der im nachfolgenden Gehäusemodul 2 über die Membran 13 durch die Hohlkörper 12 abgeleitet wird. Das verbleibende Reaktionsgas aus mit Kohlendioxid angereicher tem Prozessgas wird durch Wärmezufuhr im anschließenden Wärmetauscher 18 eines Gehäusemoduls 4 auf eine für die nachfolgende katalytische Reaktion güns tige Prozesstemperatur erwärmt, um im Anschluss den aus dem Prozessgas um gesetzten Wasserstoff in einem Gehäusemodul 2 ableiten zu können. Der in den einzelnen Gehäusemodulen 2 abgeschiedene Wasserstoff wird durch eine diesen Gehäusemodulen 2 gemeinsame Sammelleitung 14 zur weiteren Verwendung ab gezogen. Das Rententat 1 1 , im Wesentlichen Kohlendioxid und Wasser, verlässt den Membranreaktor durch den Ablauf 10 der Endkappe 6. If a membrane reactor according to FIG. 1 is charged with a methanol-water vapor mixture as process gas 9 for hydrogen production, a partially catalytic conversion of the process gas 9 into the main components carbon dioxide and hydrogen takes place first in a housing module 3, which in the following housing module 2 via the Membrane 13 is derived through the hollow body 12. The remaining reaction gas from process gas enriched with carbon dioxide is heated to a process temperature favorable for the subsequent catalytic reaction by supplying heat in the subsequent heat exchanger 18 of a housing module 4 in order to be able to divert the hydrogen converted from the process gas into a housing module 2. The hydrogen deposited in the individual housing modules 2 is drawn off for further use through a collecting line 14 common to these housing modules 2. The rent act 11, essentially carbon dioxide and water, leaves the membrane reactor through the outlet 10 of the end cap 6.
Durch unterschiedliche Kombinationen der Gehäusemodule 2, 3 und 4 lässt sich der Membranreaktor in einfacher Art an unterschiedliche Anforderungen anpas sen. So zeigt die Fig. 3 beispielsweise einen Membranreaktor, dessen zulaufseiti ger Katalysatorabschnitt gegenüber dem Ausführungsbeispiel nach der Fig. 1 durch das Hintereinanderschalten von zwei einen Katalysator 17 aufnehmenden Gehäusemodulen 3 verlängert wurde. Außerdem wird auf die Prozesstemperatur in diesem verlängerten Katalysatorabschnitt durch einen vorgelagerten Wärme tauscher 18 eines Gehäusemoduls 4 Einfluss genommen. Die nachfolgende Um setzung des im Reaktionsgas verbleibenden Prozessgases wird entsprechend der Fig. 1 optimiert, indem zunächst nach dem Ableiten des Permeats das verbleiben de Gasgemisch im Wärmetauscher 18 eines nachfolgenden Gehäusemoduls 4 auf die gewünschte Prozesstemperatur gebracht und dann das restliche Prozessgas in einem Gehäusemodul 3 in ein Permeat und ein Retentat umgesetzt wird, bevor das Permeat in einem abschließenden Gehäusemodul 2 aus dem Gasgemisch abgeleitet wird. The membrane reactor can be easily adapted to different requirements by different combinations of the housing modules 2, 3 and 4. For example, FIG. 3 shows a membrane reactor whose inlet side catalyst section has been extended compared to the exemplary embodiment according to FIG. 1 by connecting two housing modules 3 accommodating a catalyst 17 in series. In addition, the process temperature in this extended catalyst section is influenced by an upstream heat exchanger 18 of a housing module 4. The subsequent implementation of the process gas remaining in the reaction gas is optimized according to FIG. 1 by first bringing the remaining gas mixture in the heat exchanger 18 of a subsequent housing module 4 to the desired process temperature after the permeate has been discharged, and then the remaining process gas is converted into a permeate and a retentate in a housing module 3 before the permeate is derived from the gas mixture in a final housing module 2.
Es zeigt sich somit, dass durch den modulartigen Aufbau der Membranreaktor in optimaler Art an unterschiedliche Anforderungen der Umwandlungs- und Abschei devorgänge angepasst werden kann, weil die Anordnung und Eigenschaften von Katalysatoren, Wärmetauschern und Membranen beliebig verändert werden und auf die jeweilige Reaktion sowie auf anfangs unbekannte Randbedingungen und Komponenteneigenschaften abgestimmt werden können, sodass sämtliche Ge- häusemodule in einem optimalen Bereich der für die Umwandlung maßgebenden Parameter arbeiten können. It thus shows that the modular structure of the membrane reactor can be optimally adapted to different requirements of the conversion and separation processes, because the arrangement and properties of catalysts, heat exchangers and membranes can be changed as required and to the respective reaction as well as initially unknown boundary conditions and component properties can be coordinated so that all housing modules can work in an optimal range of the parameters relevant for the conversion.

Claims

Patentansprüche Claims
1. Membranreaktor mit einem ein Gehäuse (1 ) durchsetzenden, einen Kataly sator (17) aufnehmenden Strömungskanal (7) für ein Prozessgas (9) und mit ei nem Strömungsweg für ein Permeat (15), der vom Strömungskanal (7) für das Prozessgas (9) durch eine für das Permeat (15) durchlässige Membran (13) ge trennt ist, dadurch gekennzeichnet, dass das Gehäuse (1 ) aus einzelnen Gehäu semodulen (2, 3, 4) zusammengesetzt ist, die den von Gehäusemodul (2, 3, 4) zu Gehäusemodul (2, 3, 4) durchgehenden Strömungskanal (7) für das Prozessgas (9) bilden und an eine Sammelleitung (14) für das Permeat (15) angeschlossene, quer zum Strömungskanal (7) ausgerichtete Hohlkörper (12) als Träger für die Membran (13) aufweisen. 1. Membrane reactor with a housing (1) penetrating a catalyzer (17) receiving flow channel (7) for a process gas (9) and with egg nem flow path for a permeate (15) from the flow channel (7) for the process gas (9) is separated by a membrane (13) which is permeable to the permeate (15), characterized in that the housing (1) is composed of individual housing modules (2, 3, 4) which correspond to the housing module (2, 3, 4) to form the housing module (2, 3, 4) continuous flow channel (7) for the process gas (9) and to a collecting line (14) for the permeate (15) connected, transverse to the flow channel (7) aligned hollow body (12 ) as a carrier for the membrane (13).
2. Membranreaktor nach Anspruch 1 , dadurch gekennzeichnet, dass die Ge- häusemodule (2, 3, 4) Gehäuseringe bilden, die zwischen zwei einerseits mit ei nem Zulauf (8) für das Prozessgas (9) und anderseits mit einem Ablauf (10) für das Retentat (11 ) versehenen Endkappen (5, 6) zusammengeflanscht sind. 2. Membrane reactor according to claim 1, characterized in that the housing modules (2, 3, 4) form housing rings which between two on the one hand with an inlet (8) for the process gas (9) and on the other hand with an outlet (10) end caps (5, 6) provided for the retentate (11) are flanged together.
3. Membranreaktor nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass der Katalysator (17) und die mit der Membran (13) versehenen Hohlkörper (12) in gesonderten Gehäusemodulen (2, 3) vorgesehen sind. 3. Membrane reactor according to claim 1 or 2, characterized in that the catalyst (17) and the hollow bodies (12) provided with the membrane (13) are provided in separate housing modules (2, 3).
4. Membranreaktor nach einem der Ansprüche 1 bis 3, dadurch gekennzeich- net, dass die die Membran (13) tragenden Hohlkörper (12) Rohre bilden, die in außen an den Gehäusemodulen (2) vorgesehene, an die Sammelleitung (14) an geschlossene Sammelräume (16) münden. 4. Membrane reactor according to one of claims 1 to 3, characterized in that the hollow bodies (12) carrying the membrane (13) form tubes which are provided on the outside of the housing modules (2) and are closed on the collecting line (14) Open collecting spaces (16).
5. Membranreaktor nach einem der Ansprüche 1 bis 4, dadurch gekennzeich net, dass zumindest ein Gehäusemodul (4) einen Wärmetauscher (18) aufweist. 5. Membrane reactor according to one of claims 1 to 4, characterized in that at least one housing module (4) has a heat exchanger (18).
EP20711774.8A 2019-05-21 2020-03-05 Membrane reactor Pending EP3972730A1 (en)

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PL163570B1 (en) * 1990-05-18 1994-04-29 Inst Chemii Nieorganicznej Fixed catalyst reactor with internal heat exchange
JP3898892B2 (en) * 1998-10-14 2007-03-28 アイダテック・エルエルシー Reformer
MXPA03004997A (en) * 2000-12-05 2003-09-05 Texaco Development Corp Apparatus and method for heating catalyst for start-up of a compact fuel processor.
US20030039601A1 (en) * 2001-08-10 2003-02-27 Halvorson Thomas Gilbert Oxygen ion transport membrane apparatus and process for use in syngas production
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NL2006245C2 (en) * 2011-02-18 2012-08-21 Stichting Energie MEMBRANE REACTOR AND PROCESS FOR THE PRODUCTION OF A GASEOUS PRODUCT WITH SUCH REACTOR.

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