DE10216361A1 - Increasing the efficiency of and reducing exhaust gases in fuel cell systems, comprises increasing the oxygen amount of the air introduced and/or the hydrogen amount of the fuel gas using a gas enriching process - Google Patents

Increasing the efficiency of and reducing exhaust gases in fuel cell systems, comprises increasing the oxygen amount of the air introduced and/or the hydrogen amount of the fuel gas using a gas enriching process

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DE10216361A1
DE10216361A1 DE10216361A DE10216361A DE10216361A1 DE 10216361 A1 DE10216361 A1 DE 10216361A1 DE 10216361 A DE10216361 A DE 10216361A DE 10216361 A DE10216361 A DE 10216361A DE 10216361 A1 DE10216361 A1 DE 10216361A1
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fuel cell
water
temperature fuel
hydrogen
air
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DE10216361B4 (en
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Claus Hoffjann
Hans-Juergen Heinrich
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Airbus Operations GmbH
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Airbus Operations GmbH
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Priority to EP03008227A priority patent/EP1357625B1/en
Priority to DE50313459T priority patent/DE50313459D1/en
Priority to AT03008227T priority patent/ATE498211T1/en
Priority to JP2003108032A priority patent/JP4596745B2/en
Priority to US10/414,418 priority patent/US7208239B2/en
Publication of DE10216361A1 publication Critical patent/DE10216361A1/en
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/249—Grouping of fuel cells, e.g. stacking of fuel cells comprising two or more groupings of fuel cells, e.g. modular assemblies
    • H01M8/2495—Grouping of fuel cells, e.g. stacking of fuel cells comprising two or more groupings of fuel cells, e.g. modular assemblies of fuel cells of different types
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B64—AIRCRAFT; AVIATION; COSMONAUTICS
    • B64D—EQUIPMENT FOR FITTING IN OR TO AIRCRAFT; FLIGHT SUITS; PARACHUTES; ARRANGEMENT OR MOUNTING OF POWER PLANTS OR PROPULSION TRANSMISSIONS IN AIRCRAFT
    • B64D11/00—Passenger or crew accommodation; Flight-deck installations not otherwise provided for
    • B64D11/02—Toilet fittings
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B64—AIRCRAFT; AVIATION; COSMONAUTICS
    • B64D—EQUIPMENT FOR FITTING IN OR TO AIRCRAFT; FLIGHT SUITS; PARACHUTES; ARRANGEMENT OR MOUNTING OF POWER PLANTS OR PROPULSION TRANSMISSIONS IN AIRCRAFT
    • B64D41/00—Power installations for auxiliary purposes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B64—AIRCRAFT; AVIATION; COSMONAUTICS
    • B64D—EQUIPMENT FOR FITTING IN OR TO AIRCRAFT; FLIGHT SUITS; PARACHUTES; ARRANGEMENT OR MOUNTING OF POWER PLANTS OR PROPULSION TRANSMISSIONS IN AIRCRAFT
    • B64D41/00—Power installations for auxiliary purposes
    • B64D2041/005—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
    • Y02C20/00—Capture or disposal of greenhouse gases
    • Y02C20/40—Capture or disposal of greenhouse gases of CO2
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T50/00—Aeronautics or air transport
    • Y02T50/40—Weight reduction
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T90/00—Enabling technologies or technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02T90/40—Application of hydrogen technology to transportation, e.g. using fuel cells

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Electrochemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Aviation & Aerospace Engineering (AREA)
  • Analytical Chemistry (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Fuel Cell (AREA)

Abstract

Process for increasing the efficiency of and reducing exhaust gases in fuel cell systems comprises increasing the oxygen amount of the air introduced for fuel cells operating with atmospheric oxygen on the cathode side and/or the hydrogen amount of the fuel gas for fuel cells operating with hydrocarbons on the anode side, using a gas enriching process coupled to a reforming process using a high temperature fuel cell. The reforming process uses a high temperature fuel cell (3), in which reaction gases (hydrogen, hydrocarbons, water, carbon monoxide and carbon dioxide) are removed and re-used. The hydrogen is fed to one or more low temperature fuel cells (4) and water and hydrocarbons are condensed out and re-introduced to the reforming process. The carbon dioxide and carbon monoxide are fed to an exhaust gas catalyst (14). Preferred Features: Hydrogen obtained by the internal reformer process of a high temperature fuel cell is cooled to less than 80 deg C and is removed using a molecular sieve and fed to one or more low temperature fuel cells.

Description

Die Erfindung betrifft ein Verfahren zur Effizienzsteigerung und zur Verminderung von Abgasen bei Brennstoffzellensystemen, insbesondere für die Energieerzeugung sowie für Wassergenerierungssystame auf Brennstoffzellen-Basis. The invention relates to a method for increasing efficiency and reducing exhaust gases Fuel cell systems, in particular for energy generation and for Water generation system based on fuel cells.

Für den Betrieb von Brennstoffzellen werden im Allgemeinen zwei gasförmig vorliegende Ausgangsstoffe benötigt: Wasserstoff (H2) anodenseitig und Sauerstoff (O2) kathodenseitig. Two gaseous starting materials are generally required for the operation of fuel cells: hydrogen (H 2 ) on the anode side and oxygen (O 2 ) on the cathode side.

Diese Gase können, je nach Brennstoffzellentyp, entweder als reine Gase in molekularer Form vorliegen, Bestandteil von Gasgemischen sein oder in sogenannten Reformerprozessen aus anderen chemischen Verbindungen (z. B. Wasserstoff aus Kohlenwasserstoffen) gewonnen werden. Depending on the type of fuel cell, these gases can either be pure gases in molecular form exist, be part of gas mixtures or in so-called reformer processes from others chemical compounds (e.g. hydrogen from hydrocarbons).

In verschiedenen Anwendungsfällen, wie z. B. für den mobilen Einsatz, wird der von der Brennstoffzelle benötigte Sauerstoffanteil aus der Umgebungsluft gewonnen, die in einem Mischungsverhältnis von ca. 18% Sauerstoff (O2), 78% Stickstoff (N2) und 4% anderen Gasen (CO2 und Spurengase) vorliegt. Dies bedeutet, daß ca. 82% der sauerstoffseitig durch die Brennstoffzelle geleiteten Gase für den Reaktionsprozess nicht nutzbar sind. Im Falle von Hochtemperatur-Brennstoffzellen, die bei Temperaturen von ca. 600°C bis 1000°C arbeiten, kommt es zudem zu unerwünschten thermochemischen Reaktionen, wie beispielsweise der Bildung von Stickoxiden NOx. In various applications, such as. B. for mobile use, the proportion of oxygen required by the fuel cell is obtained from the ambient air, which in a mixing ratio of approx. 18% oxygen (O 2 ), 78% nitrogen (N 2 ) and 4% other gases (CO 2 and Trace gases) is present. This means that approx. 82% of the gases passed through the fuel cell on the oxygen side cannot be used for the reaction process. In the case of high-temperature fuel cells that operate at temperatures of approximately 600 ° C to 1000 ° C, there are also undesirable thermochemical reactions, such as the formation of nitrogen oxides NO x .

Bei der Verwendung von Kohlenwasserstoffen, z. B. aus Mineralöl, zur Gewinnung von Wasserstoff (H2) für die Brennstoffzelle, entstehen ebenfalls im Reformerprozess Gase, die für die Brennstoffzelle nicht nutzbar sind und als Abgase anfallen (CO, CO2, CXHY). When using hydrocarbons, e.g. B. from mineral oil for the production of hydrogen (H 2 ) for the fuel cell, gases also arise in the reformer process, which cannot be used for the fuel cell and are produced as exhaust gases (CO, CO 2 , C X H Y ).

Der Erfindung liegt die Aufgabe zugrunde, ein Verfahren zur Effizienzsteigerung aller mit Luftsauerstoff und/oder Kohlenwasserstoffen betriebenen Brennstoffzellen und zur Reduktion von unerwünschten Abgasen bei Hochtemperatur-Brennstoffzellen zu schaffen und somit beispielsweise den Einsatz in Luftfahrzeugen zu ermöglichen. The invention has for its object to provide a method for increasing the efficiency of all Atmospheric oxygen and / or hydrocarbon fuel cells and for the reduction of to create undesirable exhaust gases in high-temperature fuel cells and thus, for example, use to enable in aircraft.

Die Aufgabe wird erfindungsgemäß durch die kennzeichnenden Verfahrensmerkmale von Anspruch 1 gelöst. The object is achieved by the characterizing method features of claim 1 solved.

Das erfindungsgemäße Verfahren beruht auf der Anreicherung der für die Brennstoffzelle nutzbaren Gase bei gleichzeitiger Reduzierung aller anderen nicht am Prozess beteiligten Gase bzw. der Vermeidung unerwünschter chemothermischen Umwandlung. Hierbei erfolgt eine Gliederung in zwei Bereiche, und zwar in den Bereich der Sauerstoffanreicherung bzw. der Brennstoffanreicherung. The method according to the invention is based on the enrichment of those that can be used for the fuel cell Gases while reducing all other gases not involved in the process or the Avoiding unwanted chemothermal conversion. This is divided into two Areas, namely in the area of oxygen enrichment or fuel enrichment.

Erfindungsgemäße Ausgestaltungen des Verfahrens sind in den Unteransprüchen 2 bis 17 beschrieben. Embodiments of the method according to the invention are in subclaims 2 to 17 described.

In der Zeichnung ist ein Ausführungsbeispiel nach der Erfindung beschrieben, und zwar zeigt: In the drawing, an embodiment according to the invention is described, which shows:

Fig. 1 eine Sauerstoff- und Wasserstoffanreicherung für ein kombiniertes Brennstoffzellensystem aus PEMFC-Niedrigtemperatur- und SOFC-Hochtemperatur-Brennstoffzelle zur Wassergenerierung in einem Luftfahrzeug, und Fig. 1 is an oxygen and hydrogen enrichment for a combined fuel cell system from PEMFC low-temperature and SOFC high-temperature fuel cell for water generation in an aircraft, and

Fig. 2 eine Sauerstoffanreicherung für ein Brennstoffzellensystem mit Niedrigtemperatur-Brennstoffzelle für Luftfahrzeuge. Fig. 2 is an oxygen enrichment of a fuel cell system with low temperature fuel cell for aircraft.

Sauerstoffanreicherungoxygenation

Zur Sauerstoffanreicherung lassen sich unterschiedliche Verfahren anwenden. Üblicherweise lässt sich das Gas mit den geometrisch kleineren Molekülen durch ein sogenanntes Molekularsieb von den grösseren Molekülen der anderen vorhandenen Gase trennen. Im vorliegenden Fall sind die Moleküle des Sauerstoffs geometrisch kleiner als die des Stickstoffes und des Kohlendioxids in der Luft, so dass der Sauerstoff durch das Molekularsieb dringt, Stickstoff und Kohlendioxid jedoch nicht. Auf der abgewandten Seite des Siebes entsteht somit eine Sauerstoffanreicherung. Different methods can be used for oxygenation. Usually leaves the gas with the geometrically smaller molecules separates itself through a so-called molecular sieve separate larger molecules of the other gases present. In the present case, the molecules are the oxygen is geometrically smaller than that of nitrogen and carbon dioxide in the air, see above that oxygen passes through the molecular sieve, but nitrogen and carbon dioxide do not. On the Oxygen enrichment thus occurs on the side of the screen facing away.

Bekannt sind Verfahren aus der Luftfahrt bei denen mittels zweier, sich in einem Behälter gegenüberliegender Molekularsiebe und einem wechselseitigen Betrieb der Durchströmrichtung innerhalb dieses Behälters eine Anreicherung von Sauerstoff zur Sauerstoffversorgung von Passagieren vorgenommen wird (OBOGS). Auch Verfahren auf keramischer Grundlage und unter Einfluss elektrostatischer Ladungen sind bekannt. Methods from aviation are known in which two are located in one container opposite molecular sieves and a mutual operation of the flow direction within this Container made an enrichment of oxygen to supply passengers with oxygen will (OBOGS). Also processes based on ceramic and under the influence of electrostatic Charges are known.

Unabhängig vom Sauerstoff-Anreicherungsverfahren besteht die Neuerung des Systems in der Verbindung eines dieser Verfahren oder einer Kombination dieser Verfahren mit einer oder mehreren Brennstoffzellen. Regardless of the oxygen enrichment process, the innovation of the system is that Combining one of these methods or a combination of these methods with one or more Fuel cells.

Hierzu wird das System zuführseitig druckbeaufschlagt und Luft durch ein Sauerstoff- Anreicherungssystem (z. B. einem Molekularsieb) gedrückt wobei Stickstoff- und Kohlendioxidmoleküle zurückgehalten werden. Die sauerstoffangereicherte Luft hinter dem Anreicherungssystem wird direkt der Brennstoffzelle zugeführt. For this purpose, the system is pressurized on the supply side and air through an oxygen Enrichment system (e.g. a molecular sieve) pressed with nitrogen and carbon dioxide molecules be held back. The oxygen-enriched air behind the enrichment system becomes direct fed to the fuel cell.

In der Brennstoffzelle selbst verbindet sich der Sauerstoff mit Wasserstoffatomen zu H2O - Wasser. Dieses Wasser wird abgeschieden und kann anderweitigen Nutzungen wie z. B. einem Brennstoff- Reformerprozess und/oder einem Wassersystem zugeführt werden. Da nicht der gesamte enthaltene Sauerstoff durch die Brennstoffzelle genutzt wird, d. h. dass die mengenmässige Durchströmung höher ist als der tatsächliche Verbrauch, wird der Restsauerstoff eingangsseitig wieder dem Anreicherungssystem zugeführt. Die Druckbeaufschlagung des Anreicherungssystems und der Brennstoffzeile wird mittels eines Kompressors realisiert, der entweder mit elektrischer Energie aus der Brennstoffzelle betrieben wird oder, bei Verwendung einer Hochtemperatur-Brennstoffzelle, mittels der aus einer Abgas-Turbine gewonnenen mechanischen Energie. In the fuel cell itself, oxygen combines with hydrogen atoms to form H 2 O water. This water is separated and can be used for other purposes such. B. a fuel reformer process and / or a water system. Since not all of the oxygen contained is used by the fuel cell, ie the volume flow is higher than the actual consumption, the residual oxygen is fed back to the enrichment system on the inlet side. The pressurization of the enrichment system and the fuel line is realized by means of a compressor which is either operated with electrical energy from the fuel cell or, when using a high-temperature fuel cell, by means of the mechanical energy obtained from an exhaust gas turbine.

Brennstoffanreicherungfuel enrichment

Bei den Verfahren zur Brennstoffanreicherung aus Kohlenwasserstoffen muss man in der Anordnung zwischen Hochtemperatur- und Niedrigtemperatur-Brennstoffzellen unterscheiden. In beiden Fällen wird in einem Reformerprozess Wasserstoff durch die Aufspaltung von Kohlenwasserstoff- und Wassermolekülen gewonnen. Hierbei entstehen neben atomarem- und molekularem Wasserstoff auch verschiedene weitere Reaktionsgase, die in der Brennstoffzelle keine Verwendung finden. In the process of fuel enrichment from hydrocarbons, one must in the arrangement distinguish between high-temperature and low-temperature fuel cells. In both cases becomes in a reformer process hydrogen by the splitting of hydrocarbon and Water molecules won. In addition to atomic and molecular hydrogen, this also produces various other reaction gases that are not used in the fuel cell.

Findet bei Hochtemperatur-Brennstoffzellen der Reformerprozess intern statt, bei welchem eine Wasserstoffanreicherung innerhalb der Brennstoffzelle selbst erfolgt, so muss der Niedrigtemperatur-Brennstoffzelle ein externer Reformer vorgeschaltet werden. Der interne Reformerprozess von Hochtemperatur-Brennstoffzellen soll hier keine Berücksichtigung finden, da er für diesen Brennstoffzellentyp verfahrenstypisch ist. For high-temperature fuel cells, the reformer process takes place internally, in which one Hydrogen enrichment takes place within the fuel cell itself, so the Low temperature fuel cell can be connected upstream of an external reformer. The internal reform process of High-temperature fuel cells should not be taken into account here as it is for this Fuel cell type is typical of the process.

Niedrigtemperatur Brennstoffzellen sind in der Regel äusserst empfindlich gegen Verunreinigungen des Brenngases, so dass eine vorherige Anreicherung des Brenngases mit Wasserstoff und damit eine prozentuale Herabsetzung der Verunreinigungen geboten ist. Low-temperature fuel cells are usually extremely sensitive to contamination of the fuel gas, so that a prior enrichment of the fuel gas with hydrogen and thus a percentage reduction in impurities is required.

Erfindungsgemäss werden hierbei die in einem Reformer erzeugten Reaktionsgase durch ein Molekularsieb getrennt. Im Reformerprozess entstehen aus Kohlenwasserstoffen (CXHY) und Wasser (H2O) die Reaktionsgase Wasserstoff (H2), Kohlenmonoxid (CO), Kohlendioxid (CO2) und Wasserdampf (H2O). Das für die Niedrigtemperatur-Brennstoffzelle (z. B. PEMFC-Protonenaustauschmembran Brennstoffzelle) nutzbare Gas ist der Wasserstoff. Dieser wird mit einem Verfahren, analog zu denen auf der Sauerstoffseite, über ein Molekularsieb abgeschieden bzw. vor der Membran der Brennstoffzelle angereichert. Die anderen Gase werden in einen weiteren den Reformerprozess geführt, wo sie weiter aufgespalten werden und erneut Wasserstoff gewonnen wird, bevor sie als Abgas abgeführt werden. According to the invention, the reaction gases generated in a reformer are separated by a molecular sieve. In the reformer process, hydrocarbons (C X H Y ) and water (H 2 O) produce the reaction gases hydrogen (H 2 ), carbon monoxide (CO), carbon dioxide (CO 2 ) and water vapor (H 2 O). The gas that can be used for the low-temperature fuel cell (e.g. PEMFC proton exchange membrane fuel cell) is hydrogen. This is separated using a process analogous to that on the oxygen side, via a molecular sieve or enriched in front of the membrane of the fuel cell. The other gases are fed into another reforming process, where they are further broken down and hydrogen is recovered before they are discharged as exhaust gas.

Besonderer Anwendungsfall WassergenerierungssystemeSpecial application case water generation systems

Ein besonderer Anwendungsfall sind Wassergenerierungssysteme auf der Basis von Brennstoffzellen. Das zu erzeugende Wasser soll einen möglichst hohen Reinheitsgrad aufweisen und insbesondere frei sein von Kohlenwasserstoffen, Alkoholen etc. wie auch anderen potentiell gesundheitsgefährdenden Inhaltsstoffen. A special application is water generation systems based on fuel cells. The water to be generated should have the highest possible degree of purity and in particular potentially free of hydrocarbons, alcohols etc. as well as others ingredients hazardous to health.

Bei der Verwendung von Hochtemperatur-Brennstoffzellen fällt das nutzbare Wasser anodenseitig an, d. h. auf der Seite der Brennstoffzufuhr. Bei Kohlenwasserstoffen als Brenngas kommt es bei der Kondensation von Wasserdampf aus dem Brennstoffzellenabgas zu einer Vermischung von Wasser und Kohlenwasserstoffmolekülen, eventuell auch Russpartikeln und anderen gesundheitsschädlichen Inhaltsstoffen. Bei Niedrigtemperatur-Brennstoffzellen wird das Wasser auf der Sauerstoff- bzw. Luftseite erzeugt und besitzt dadurch von vornherein einen weit höheren Reinheitsgrad. Jedoch ist bei mobilen Anwendungen, wie z. B. in der Luftfahrt, aus Effizienzgründen ein Hochtemperatur- Brennstoffzellensystem wie z. B. Oxidkeramik-Brennstoffzellen, kombiniert mit Gasturbinen (SOFC + GT) wünschenswert. Beim in Hochtemperatur-Brennstoffzellen intern stattfindenden Reformerprozess kann genügend Wasserstoff abgespalten werden um einerseits die Hochtemperatur- Brennstoffzelle selbst, wie auch zusätzliche Niedrigtemperatur-Brennstoffzellen zu versorgen. When using high-temperature fuel cells, the usable water is produced on the anode side, d. H. on the side of the fuel supply. When using hydrocarbons as fuel gas, Condensation of water vapor from the fuel cell exhaust gas to a mixture of water and Hydrocarbon molecules, possibly also soot particles and other harmful substances Ingredients. With low-temperature fuel cells, the water on the oxygen or Air side generates and therefore has a much higher degree of purity from the outset. However, at mobile applications, such as B. in aviation, for efficiency reasons a high temperature Fuel cell system such as B. oxide ceramic fuel cells combined with gas turbines (SOFC + GT) desirable. With the reformer process taking place internally in high-temperature fuel cells, enough hydrogen can be split off to Fuel cell itself, as well as additional low-temperature fuel cells.

Erfindungsgemäss wird das Verfahren zur Brennstoffanreicherung (H2-Anreicherung) zwischen die Brennstoffseite der Hochtemperatur-Brennstoffzelle und die Brennstoffseite (Wasserstoffseite) der Niedrigtemperatur-Brennstoffzelle geschaltet. According to the invention, the method for fuel enrichment (H 2 enrichment) is switched between the fuel side of the high-temperature fuel cell and the fuel side (hydrogen side) of the low-temperature fuel cell.

Da die Niedrigtemperatur-Brennstoffzelle, insbesondere die Membran der Brennstoffzeile, empfindlich gegenüber thermischer Belastung ist, muss das Brenngas (H2) auf dem Weg von Hochtemperatur- zu Niedrigtemperatur-Brennstoffzelle abgekühlt werden. Hierfür kann beispielsweise eine Turbine mit nachgeschaltetem Kühler eingesetzt werden. Since the low-temperature fuel cell, in particular the membrane of the fuel line, is sensitive to thermal stress, the fuel gas (H 2 ) must be cooled on the way from the high-temperature to the low-temperature fuel cell. For example, a turbine with a downstream cooler can be used for this.

Claims (17)

1. Verfahren zur Effizienzsteigerung und Verminderung von Abgasen bei Brennstoffzellensystemen, insbesondere für die Energieerzeugung sowie für Wassergenerierungssysteme auf Brennstoffzellen-Basis, dadurch gekennzeichnet, dass bei kathodenseitig Luftsauerstoff (O2) (1, 124) betriebenen Brennstoffzellen (3, 4, 101) der Sauerstoffanteil der zugeführten Luft und/oder bei anodenseitig Kohlenwasserstoff (CXHY) (2, 110) betriebenen Brennstoffzellen der Wasserstoffanteil des Brenngases, durch Anreicherung, unter jeweiliger Verwendung eines Gasanreicherungsverfahrens (z. B. mit Molekularsieben), erhöht wird, wobei das brennstoffseitige Anreicherungsverfahren (H2-Seite) mit einem Reformerprozess gekoppelt ist, der beispielsweise durch eine Hochtemperatur-Brennstoffzelle (3) dargestellt wird, deren Reaktionsgase (H2, CXHY, H2O, CO, CO2) getrennt werden und unterschiedlich weiterverwendet werden, dergestalt, dass der Wasserstoff (H2) einer oder mehreren Niedrigtemperatur- Brennstoffzellen (4) zugeführt wird, Wasser (H2O) auskondensiert wird (9, 114), Kohlenwasserstoffe (CXHY) auskondensiert (9, 114) und in den Reformerprozess zurückgeführt werden sowie Kohlendioxid (CO2) und Kohlenmonoxid (CO) einem Abgaskatalysator (14) zugeführt werden, welcher ebenfalls mit den luftseitig an der Hochtemperatur-Brennstoffzelle (3) anfallenden Stickoxiden (NOx) beaufschlagt wird und diese Gase in Kohlendioxid (CO2) und molekularen Stickstoff (N2) wandelt und an die Atmosphäre/Luft (1) abgibt. 1. A method for increasing efficiency and reducing exhaust gases in fuel cell systems, in particular for energy generation and for water generation systems based on fuel cells, characterized in that in the case of fuel cells ( 3 , 4 , 101 ) operated with atmospheric oxygen (O 2 ) ( 1 , 124 ) on the cathode side Oxygen content of the supplied air and / or in the case of fuel cells operated on the anode-side hydrocarbon (C X H Y ) ( 2 , 110 ), the hydrogen content of the fuel gas is increased by enrichment using a gas enrichment process (e.g. with molecular sieves), the fuel-side enrichment process (H 2 side) is coupled with a reformer process, which is represented for example by a high-temperature fuel cell ( 3 ), the reaction gases (H 2 , C X H Y , H 2 O, CO, CO 2 ) are separated and be used differently, such that the hydrogen (H 2 ) one or more low g-temperature fuel cells ( 4 ) is supplied, water (H 2 O) is condensed out ( 9 , 114 ), hydrocarbons (C X H Y ) are condensed out ( 9 , 114 ) and returned to the reformer process, as well as carbon dioxide (CO 2 ) and carbon monoxide (CO) are supplied to an exhaust gas catalytic converter ( 14 ), which is also charged with the nitrogen oxides (NO x ) accumulating on the air side of the high-temperature fuel cell ( 3 ) and converts these gases into carbon dioxide (CO 2 ) and molecular nitrogen (N 2 ) and releases to the atmosphere / air ( 1 ). 2. Verfahren nach Anspruch 1, dadurch gekennzeichnet, dass durch den internen Reformerprozess einer Hochtemperatur-Brennstoffzelle (z. B. SOFC - Solid Oxide Fuel Cell oder MCFC - Molten Carbonate Fuel Cell) (3) gewonnener Wasserstoff auf t < 80°C gekühlt (10, 108) und beispielsweise über ein Molekularsieb (5) abgeschieden und einer oder mehreren Niedrigtemperatur-Brennstoffzellen (PEMFC - Proton Exchange Fuel Cell) (4, 101) zugeführt wird. 2. The method according to claim 1, characterized in that hydrogen obtained by the internal reformer process of a high-temperature fuel cell (z. B. SOFC - Solid Oxide Fuel Cell or MCFC - Molten Carbonate Fuel Cell) ( 3 ) cooled to t <80 ° C. ( 10 , 108 ) and, for example, deposited over a molecular sieve ( 5 ) and fed to one or more low-temperature fuel cells (PEMFC - Proton Exchange Fuel Cell) ( 4 , 101 ). 3. Verfahren nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass die Abkühlung über die Entspannung in einer oder mehreren Turbinen (6, 104) mit einer oder mehreren Turbinenstufen durchgeführt wird. 3. The method according to claim 1 or 2, characterized in that the cooling is carried out via the expansion in one or more turbines ( 6 , 104 ) with one or more turbine stages. 4. Verfahren nach Anspruch 1, dadurch gekennzeichnet, dass die einer Niedrigtemperatur-Brennstoffzelle (4, 101) zugeführte Luft der Temperatur des Wasserstoffs dadurch angeglichen wird, dass komprimierte Luft aus dem Sauerstoff-Anreicherungsverfahren auf t < 80°C abgekühlt wird. 4. The method according to claim 1, characterized in that the air supplied to a low-temperature fuel cell ( 4 , 101 ) is adjusted to the temperature of the hydrogen by cooling compressed air from the oxygen enrichment process to t <80 ° C. 5. Verfahren nach Anspruch 1 oder 4, dadurch gekennzeichnet, dass die Abkühlung über die Entspannung in einer oder mehreren Turbinen mit einer oder mehreren Turbinenstufen durchgeführt wird. 5. The method according to claim 1 or 4, characterized in that the cooling over the Relaxation in one or more turbines with one or more turbine stages is carried out. 6. Verfahren nach Anspruch 1, 3 oder 5, dadurch gekennzeichnet, dass zur Abkühlung ein Wärmetauscher nachgeschaltet wird, der z. B. mit Außenluft als Kühlmedium betrieben wird. 6. The method according to claim 1, 3 or 5, characterized in that for cooling Heat exchanger is connected downstream, the z. B. is operated with outside air as a cooling medium. 7. Verfahren und Anordnung nach Anspruch 1, dadurch gekennzeichnet, dass alternativ zur Hochtemperatur-Brennstoffzelle ein Reformer (105) für die Erzeugung von Wasserstoff verwendet wird, dem ein Molekularsieb und ein Wasserstoff-Pufferbehälter (107) nachgeschaltet ist, wobei Molekularsieb und Pufferbehälter getrennt oder in die Brennstoffzelle integriert sind. 7. The method and arrangement according to claim 1, characterized in that, alternatively to the high-temperature fuel cell, a reformer ( 105 ) is used for the production of hydrogen, which is followed by a molecular sieve and a hydrogen buffer container ( 107 ), the molecular sieve and buffer container being separated or are integrated in the fuel cell. 8. Verfahren nach Anspruch 1, dadurch gekennzeichnet, dass das System luftsauerstoffseitig druckbeaufschlagt wird, wobei in Luftfahrzeugen in Flughöhe auch der Differenzdruck zwischen Außenluft (1, 124) und Kabinenluft (28, 125) als Druckbeaufschlagung gilt. 8. The method according to claim 1, characterized in that the system is pressurized on the air-oxygen side, the difference in pressure between outside air ( 1 , 124 ) and cabin air ( 28 , 125 ) also being considered as pressurization in aircraft at flight altitude. 9. Verfahren nach Anspruch 1, dadurch gekennzeichnet, dass das System brennstoffseitig druckbeaufschlagt wird. 9. The method according to claim 1, characterized in that the system on the fuel side is pressurized. 10. Verfahren nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass aus der Hochtemperatur- Brennstoffzelle (3) anodenseitig und/oder der Niedrigtemperaturbrennstoffzelle (4, 101) kathodenseitig Wasser (H2O) gewonnen und abgeführt wird. 10. The method according to claim 1 or 2, characterized in that from the high-temperature fuel cell ( 3 ) on the anode side and / or the low-temperature fuel cell ( 4 , 101 ) on the cathode side water (H 2 O) is obtained and removed. 11. Verfahren nach Anspruch 1, 2 oder 10, dadurch gekennzeichnet, dass das gewonnene Wasser der Niedrigtemperatur-Brennstoffzelle (4, 101) ganz oder teilweise für die Nutzung als Trinkwasser aufbereitet wird (17, 19, 21), und dass das gewonnene Wasser der Hochtemperatur-Brennstoffzelle (3) als Brauchwasser (WC-Spülung) (18, 20) verwendet wird. 11. The method according to claim 1, 2 or 10, characterized in that the water obtained from the low-temperature fuel cell ( 4 , 101 ) is wholly or partly prepared for use as drinking water ( 17 , 19 , 21 ), and that the water obtained the high-temperature fuel cell ( 3 ) is used as process water (toilet flushing) ( 18 , 20 ). 12. Verfahren nach Anspruch 1, 2 oder 10, dadurch gekennzeichnet, dass das gewonnene Wasser der Niedrigtemperatur-Brennstoffzelle (4, 101) ganz oder teilweise für die Luftbefeuchtung in einer Klimaanlage (21) verwendet wird. 12. The method according to claim 1, 2 or 10, characterized in that the water obtained from the low-temperature fuel cell ( 4 , 101 ) is used in whole or in part for air humidification in an air conditioning system ( 21 ). 13. Verfahren nach Anspruch 1, 2 oder 10, dadurch gekennzeichnet, dass generiertes Wasser aus Hochtemperatur- und Niedrigtemperatur-Brennstoffzelle (3, 4, 101) getrennt zwischengespeichert (gepuffert) wird. 13. The method according to claim 1, 2 or 10, characterized in that generated water from the high-temperature and low-temperature fuel cell ( 3 , 4 , 101 ) is buffered separately. 14. Verfahren nach Anspruch 1, 2, 10 oder 13, dadurch gekennzeichnet, dass der Füllstand der Puffermengen von einer Steuerungseinheit erfasst wird. 14. The method according to claim 1, 2, 10 or 13, characterized in that the fill level of the Buffer quantities are recorded by a control unit. 15. Verfahren nach Anspruch 1, 2, 11, 12 oder 13, dadurch gekennzeichnet, dass der Brennstoffverbrauch der unterschiedlichen Brennstoffzellen verbrauchsabhängig von der Steuereinheit gegeneinander geregelt wird. 15. The method according to claim 1, 2, 11, 12 or 13, characterized in that the The fuel consumption of the different fuel cells depends on the consumption of the control unit is regulated against each other. 16. Verfahren nach Anspruch 1, 10 oder 11, dadurch gekennzeichnet, dass anfallendes Grauwasser (23) zu einer Nutzung im Reformerprozess (3, 11) rückgeführt wird und überschüssige Wassermengen drainiert werden (24). 16. The method according to claim 1, 10 or 11, characterized in that accumulating gray water ( 23 ) for use in the reformer process ( 3 , 11 ) is returned and excess amounts of water are drained ( 24 ). 17. Verfahren nach Anspruch 1 oder 11, dadurch gekennzeichnet, dass anfallendes Schwarzwasser (22, 23) dehydriert und gereinigt wird und dass das so gewonnene Wasser zu einer Nutzung im Reformerprozess (3, 11) rückgeführt wird und überschüssige Wassermengen drainiert werden (24). 17. The method according to claim 1 or 11, characterized in that accumulating black water ( 22 , 23 ) is dehydrated and purified and that the water thus obtained is returned to use in the reformer process ( 3 , 11 ) and excess water quantities are drained ( 24 ) ,
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DE10216361A DE10216361B4 (en) 2001-10-11 2002-04-13 Process for increasing efficiency and reducing exhaust gases in fuel cell systems
EP03008227A EP1357625B1 (en) 2002-04-13 2003-04-09 Process to increase efficiency and decrease the exhaust gases from fuel cell system
DE50313459T DE50313459D1 (en) 2002-04-13 2003-04-09 Method for increasing efficiency and reducing exhaust gases in fuel cell systems
AT03008227T ATE498211T1 (en) 2002-04-13 2003-04-09 METHOD FOR INCREASE EFFICIENCY AND REDUCING EXHAUST GASES IN FUEL CELL SYSTEMS
JP2003108032A JP4596745B2 (en) 2002-04-13 2003-04-11 Method for improving efficiency and reducing exhaust gas in a fuel cell system
US10/414,418 US7208239B2 (en) 2001-10-11 2003-04-14 Fuel cell system and method with increased efficiency and reduced exhaust emissions

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