EP1974413A1 - Cellule a combustible a oxydation directe dotee d'un apport passif de combustible et procede pour son utilisation - Google Patents

Cellule a combustible a oxydation directe dotee d'un apport passif de combustible et procede pour son utilisation

Info

Publication number
EP1974413A1
EP1974413A1 EP07702934A EP07702934A EP1974413A1 EP 1974413 A1 EP1974413 A1 EP 1974413A1 EP 07702934 A EP07702934 A EP 07702934A EP 07702934 A EP07702934 A EP 07702934A EP 1974413 A1 EP1974413 A1 EP 1974413A1
Authority
EP
European Patent Office
Prior art keywords
fuel
fuel cell
membrane
distribution structure
direct oxidation
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.)
Withdrawn
Application number
EP07702934A
Other languages
German (de)
English (en)
Inventor
Steffen Eccarius
Christian Litterst
Peter Koltay
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.)
Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV
Albert Ludwigs Universitaet Freiburg
Original Assignee
Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV
Albert Ludwigs Universitaet Freiburg
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 Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV, Albert Ludwigs Universitaet Freiburg filed Critical Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV
Publication of EP1974413A1 publication Critical patent/EP1974413A1/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • 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
    • H01M8/04291—Arrangements for managing water in solid electrolyte fuel cell systems
    • 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
    • H01M8/04186—Arrangements for control of reactant parameters, e.g. pressure or concentration of liquid-charged or electrolyte-charged 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
    • H01M8/04—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
    • H01M8/04186—Arrangements for control of reactant parameters, e.g. pressure or concentration of liquid-charged or electrolyte-charged reactants
    • H01M8/04194—Concentration measuring cells
    • 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
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/1009—Fuel cells with solid electrolytes with one of the reactants being liquid, solid or liquid-charged
    • H01M8/1011—Direct alcohol fuel cells [DAFC], e.g. direct methanol fuel cells [DMFC]
    • 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

Definitions

  • the invention relates to a method of operating a direct oxidation fuel cell in which at least one fluid fuel from a fuel reservoir is transported via a fluid distribution structure to a membrane-electrode assembly, the transport of the fuel being passive, i. without convection. Furthermore, the invention relates to a corresponding direct oxidation fuel cell.
  • direct oxidation fuel cells for example, direct methanol fuel cells
  • direct oxidation fuel cells are considered to be particularly promising mobile energy sources, since the liquid fuel is comparatively easy to handle and as a rule has a much higher energy density than batteries or rechargeable batteries.
  • a pump which supplies the direct oxidation fuel cell with liquid fuel is operated continuously.
  • the gas bubbles are dissolved with the most over-stoichiometric volume flow in liquid or flushed out with the liquid from the fuel cell and separated from the liquid fuel in a subsequent step.
  • This requires continuous operation of the pump, which results in greater pump power inputs and consequently decreases the system efficiency of the entire fuel cell system.
  • a method for operating a direct oxidation fuel cell, in which at least one fluid fuel from a fuel reservoir is transported via a fluid distribution structure to a membrane-electrode unit.
  • the present invention is characterized in that the transport of the at least one fluidic fluid takes place convection-free, by the transport being based solely on the diffusion of the fuel and at least one further fluid.
  • the optimum fuel concentration can be adjusted on the membrane. In this way, the so-called. Crossover of fuel, ie the passage of unused fuel through the membrane minimize. Due to the fact that up an active component, such as a pump can be omitted, the inventive method has the significant advantage that the efficiency of Trimoxidationsbrennstoffzelle compared to the known from the prior art method can be significantly increased.
  • the at least one further fluid in the process according to the invention is at least partially recycled electrochemically.
  • methanol is converted with water to CO 2 .
  • the used water is then recycled electrochemically.
  • a preferred variant of the method according to the invention provides that the fuel cell has a pinhole and / or porous membrane, which is in communication with a fuel reservoir.
  • the fuel cell has a pinhole and / or porous membrane, which is in communication with a fuel reservoir.
  • all structures with regularly arranged openings can also be used here. So can the
  • the diameter of the holes and / or pores is chosen so that a sufficient for the electrochemical reaction diffusion and thus a transport of the fuel to the membrane-electrode unit is ensured.
  • the passive fuel supply ie a supply without convective transport, depends on various parameters.
  • concentration of fuel prevailing at a specific location can be calculated by means of a diffusion equation. This will be illustrated using the example of a direct methanol fuel cell (DMFC), which uses methanol as fuel.
  • DMFC direct methanol fuel cell
  • the fuel cell has a pinhole or porous Membrane at a distance d to the membrane-electrode unit on.
  • the basis for the calculation is a one-dimensional stationary diffusion model, which is based on a point source and a sink at a distance d. This will be clarified with reference to FIG. 6.
  • ⁇ fuel consumption of the fuel cell
  • C A concentration of the fuel at the membrane-electrode unit
  • C a concentration of the fuel to the
  • the membrane-electrode assembly has the construction known from the prior art.
  • this comprises a proton-conducting membrane, e.g. from Nafion, as well as in each case anode-side and cathode-side catalyst and diffusion layers.
  • the proton-conducting membrane should be impermeable to the fuel and the reaction products.
  • catalyst layers preference is given to those materials which have a large active surface, a resistance to carbon monoxide and preferably no side reactions or by-products.
  • Particularly preferred catalyst layers include platinum, ruthenium and / or their alloys.
  • the diffusion layers are to allow the transport of the fuel to the anodic catalyst layer and the further reactant to the cathodic catalyst layer.
  • the diffusion layer must make it possible to transport the gaseous reaction products from the anodic catalyst layer or the reaction products from the cathodic catalyst layer.
  • Another requirement for the diffusion layer relates to its property for electron management .
  • a further preferred variant of the method according to the invention provides that degassing of the liquid fuel additionally takes place in the fuel cell.
  • a variant of this provides for a microstructuring of the fluid distribution structure by which the removal of gaseous media from the fluid distribution structure is favored. With regard to this variant, reference is made to Figures 1 to 4.
  • the fuel cell on the anode side has at least one for gases and liquids impermeable barrier.
  • the liquids can be held in the fluid distribution structure and the gases are transported away from the fluid distribution structure.
  • the barrier layer is preferably an oleophobic membrane.
  • microstructures or ceramics can also be used as a barrier layer.
  • a first preferred variant provides that it is arranged between the anode-side end plate, which is located on the side of the fluid distribution structure facing away from the MEA, and the anode-side fluid distribution structure.
  • barrier layer is arranged on the side of the anode-side end plate facing away from the anode-side fluid distribution structure.
  • the end plate preferably has relief holes.
  • FIG. 1 is a perspective view of a channel portion of a device for removing gaseous components in the form of a microstructure with an inclusion at four successive times
  • FIG. 2 shows a cross-section through a channel in another embodiment of the microstructure with inclusions at six successive points in time as well as a side view of the same channel with an inclusion at two successive points in time
  • Fig. 4 in turn in each case a longitudinal section through two channels of further embodiments.
  • Fig. 5 shows schematically the structure of a variant according to the invention relating to the degassing of the fuel cell.
  • DMFC directme ethanol fuel cell
  • FIG. 8 schematically shows the structure of a fuel cell according to the invention with the values derived from the diffusion models.
  • FIG. 1 four times the same channel 1 is shown, which is integrated into a self not shown chemical microreactor and is arranged there adjacent to a lying in the figure side surface 2 on a catalytic membrane.
  • the channel 1 carries a flowable medium, which in the present case is a liquid.
  • Proper operation of the chemical microreactor is associated with the formation of gas on the catalytic membrane which enters the channel 1 at the side surface 2 and forms bubbles therein.
  • An inclusion 3 formed by such a bubble is in FIG. 1 in the illustrations marked with a), b), c) and d) four successive
  • Figure b) represents a 0.000755 s
  • Figure c) a 0.001175 s
  • Figure d a 0.00301 s after the time shown in Figure a).
  • the inclusions 3 could also be formed by a fluid which is distinguishable from the medium carried by the channel 1. It would also be possible that that flowable medium not as a liquid, but as
  • the flowable medium is a liquid reactant which is supplied to the channel 1 from an end lying in FIG. 1 on the left.
  • the latter has an open-ended channel output 4, through which the inclusion of gas 3 can escape into an environment of the microreactor.
  • the channel 1 has a cross-section which forms a T-profile, wherein the side surface 2 terminates a further beam projecting from a transverse bar of the T-profile. Due to capillary forces which cause a minimization of surface energy of the inclusion 3, the inclusion 3 formed on the side surface 2 first rises to a point where said further beam contacts the transverse beam, whereby the inclusion 3 is separated from that on the side surface 2 adjacent catalytic membrane is removed.
  • the channel 1 now has a geometry which forces the enclosure 3 into a shape in which capillary forces in turn act on it, which move the inlet 3 along the channel 1 towards the channel exit 4.
  • This geometry is characterized in that a ratio A 1 / I 1 and a ratio A / l along the channel 1 towards the channel output 4 towards strictly monotonous and steadily increase, wherein for each on a longitudinal direction of the channel 1 perpendicular cross-section of the channel 1 the Size A is defined as the area and the size 1 as the circumferential length of this cross section, while A 1 denotes a surface area and 1 'a length of a circumferential line of a contiguous area lying within this cross section, this area being defined by A' / l 'assumes a maximum value compared to all other contiguous surfaces lying in the cross-section, where ⁇ is defined as the contact angle which, at the level of the respective cross-section, on the channel wall 5 between that of the channel 1 guided flowable medium and the inclusions 3 forming gas
  • the monotonous increase of the mentioned quantities or ratios along the channel 1 towards the channel exit 4 is realized in the present case by the area A of the cross-section of the channel 1 and thus also the area A 1 of said area lying within the cross-section, which, in a good approximation, corresponds to the area which an enclosure 3 tends to occupy within the cross-section, increasing monotonically along the channel.
  • An increase of those areas A and A 1 along the channel 1 is achieved in that a dimension of the cross section in a direction perpendicular to the crossbar of said T-profile direction along the channel 1 is monotonically increasing, which is a through the channel 1 increasing extension of the cross-beam forming part of the T-profile is realized in the direction perpendicular to the crossbar and an associated profile change.
  • the respective part of the channel 1 forming the transverse bar of the T-profile thereby acquires a wedge shape.
  • Other geometries of the channel 1 would also be conceivable in which a maximum diameter of the cross-section of the channel 1 and / or a dimension of this cross-section increases monotonically in a direction perpendicular to that diameter along the channel 1, thereby causing a movement of inclusions 3 in FIG a preferred direction by Ka induce pillar forces.
  • the channel 1 of FIG. 1 results in the manner described a profile change in which a defined as A / l 2 and A as A 1 / I 12 ratio along the channel 1 to the channel output 4 out steadily and strictly monotone increases.
  • the channel wall 5 of the channel 1 alternatively or in addition to a profile change with surface properties changing along the channel, for example by a location-dependent coating, so that the contact angle ⁇ , which is a function of the gas forming the inclusions 3 , the flowable medium guided by the channel 1 and the surface properties of the channel wall 5, has a value changing along the channel 1 and that the inclusions 3 are thereby brought into a shape which reflects the capillary forces moving the inclusions 3 towards the channel outlet 4 caused or intensified.
  • the channel not shown to scale in FIG. 1 is further dimensioned so that the surface area A of the cross section of the channel 1 at a channel beginning has a value of 25,000 ⁇ m 2 and along a distance of 0, 7 mm along the Channel 1 evenly increases to a value of 95 000 microns 2 at the channel output 4.
  • the channel 1 has a given by a length of the crossbar of said T-profile and in the present case constant width of 500 microns.
  • a corresponding design of a capillary would also be possible, in which a change in cross section is realized by only about 0.001 ° by tilting at least one of the channel walls 5.
  • the gas forming the inclusions 3 forming a gas on the side surface 2 due to the device has a clearly defined chemical composition at the catalytic reaction taking place there. This also determines the contact angle ⁇ previously used to describe properties of the channel 1. Due to the described geometry of the channel 1, the inclusions 3 are now moved to the channel exit 4 only driven by capillary forces.
  • Media-carrying capillaries of the type of the channel 1 described above are also provided in other devices, in particular for the purpose of degassing or removing other inclusions, for example in devices containing refillable liquids and in which refilling is typically associated with bubbling. Refillable ink cartridges are mentioned as an example.
  • the fuel cell stack not shown itself, consists of direct methanol fuel cells, with the channel 1 shown serving primarily for the transport of the reactants forming methanol.
  • the channel 1 again has a cross-section forming a T-shaped profile, wherein a transversal bar of this T-profile lying in each case in FIG. 2 rests against a diffusion layer which serves as a catalyst and in turn bears against an electrolyte membrane.
  • This diffusion layer forms an active surface 6, at which gaseous carbon dioxide is formed during operation of the fuel cell stack, which forms inclusions 3 surrounded by the methanol within the channel 1.
  • the crossbar of the T-profile has a tapered towards two ends shape, wherein centrally of the crossbar from the active surface 6 facing away further beam protrudes.
  • the figures marked with a) to f) in FIG. 2 illustrate that this shape of the T-profile results in the growing inclusions 3 moving towards the said further beam due to capillary forces, larger inclusions 3 moving on the way absorb small impurities 3 in it.
  • the mentioned further beam which attaches centrally to the crossbar of the T-profile widened away from the crossbar, causing a movement of the inclusions 3 due to capillary forces in the other beams of the T-profile and thus induce it away from the active surface 6.
  • the channel 1 could also be made with an L-profile (which would result from omitting one-half of the cross-bar) with a leg resting against the active surface 6.
  • the channel 1 depicted in FIG. 2 also has a continuous and strictly monotone along the channel 1 to a channel output 4.
  • Noton increasing cross-section A wherein also defined as A / l ratio to the channel output 4 toward steadily and strictly monotonically increases, where 1 is defined as the circumferential length of the cross-section of the channel 1.
  • the inclusions 3 form with a channel wall 5 a contact angle or angle ⁇ with a small value of between 0 and ⁇ / 2, which is why the mentioned increase in the ratio A / l and the associated increase in the ratio A 1 / I 1 (A 1 and 1 'are defined as previously explained in connection with FIG. 1) has the result that the capillaries act on the inclusions 3 to move them towards the channel exit 4.
  • the increase of the cross-section A and an induced induced movement of an inclusion 3 towards the channel exit 4 is illustrated in figures g) and h), which represent two consecutive times. There, the edge angle ⁇ is also located at one point.
  • a coolant channel can also be embodied that leads a liquid coolant and in which vapor bubbles of the coolant can form during operation of the fuel cell stack or another chemical microreactor.
  • corresponding channels 1 may be arranged not only in bipolar plates, but also in other current collectors, for example of fuel cells.
  • FIG. 3 in which recurring features are again identified by the same reference numerals, illustrate once again the described effects of a due to capillary forces bubble transport.
  • Fig. 3 on the left is a channel 1 with an enclosure 3 of a fluid, which is enclosed on the right and left of a flowable medium ge, shows.
  • the contact angle ⁇ which is defined as lying completely outside the confinement 3 in the flowable medium, is here smaller than ⁇ / 2, so that an increase of A / l (and A '/ l') to the channel output 4 (here to the left) causes a bubble transport in this direction.
  • FIG. 3 on the left is a channel 1 with an enclosure 3 of a fluid, which is enclosed on the right and left of a flowable medium ge, shows.
  • the contact angle ⁇ which is defined as lying completely outside the confinement 3 in the flowable medium, is here smaller than ⁇ / 2, so that an increase of A / l (and A '/ l') to the channel output 4 (here to
  • FIG. 3 another channel 1 from another device is depicted on the right, in which inclusions 3 are formed in a similar manner, but in which a contact angle ⁇ which is greater than ⁇ / 2 is established.
  • a decrease in A / l (and A '/ l') to the channel exit 4 (now right) causes the inclusions 3 to be moved there.
  • FIG. 4 illustrates two examples, left for ⁇ > ⁇ / 2 and right for ⁇ ⁇ / 2, how a corresponding effect is achieved even if the channel cross-section remains the same by location-dependent values of ⁇ .
  • an increase of ⁇ to the channel output 4 causes a force acting on the respective enclosure 3, which moves it toward the channel exit 4.
  • the movement takes place through different capillary pressures at the two opposite ends of the respective enclosure 3, which is reflected in different curvatures of the menisci delimiting the inclusions.
  • This effect is caused in the examples of FIG. 3 by the channel geometry, in the examples of FIG.
  • Typical reactors which are suitable for use of such structures. are suitable, catalytic reactors such as fuel cells with catalytic membranes, which continuously produce gas bubbles. Rapid removal of the gas bubbles thus prevents the blocking of an active membrane surface by emptying this membrane surface.
  • the resulting gas bubbles independently provide for typically periodic cleaning of the membrane surface of gas bubbles. This method ensures a maximum free reaction area, ensures an automatic refilling of the reactor with the appropriate reactants and thus offers great advantages over the prior art.
  • the geometric structures which produce the desired capillary forces for passively transporting the bubble forming phase may also include or be realized by ridges and constrictions.
  • the geometry should be such that the bubble-forming phase moves in a preferred direction due to the geometry and due to surface properties of the geometric structures - driven by a surface tension of the resulting BIAS - a
  • Transport of bubbles typically only passive, i. driven only by the capillary forces at phase boundaries.
  • Fig. 5 the structure of a variant according to the invention concerning the degassing of the fuel cell is shown schematically.
  • This is based on a membrane-electrode unit (MEA) with a proton-conducting membrane 7, to which anode-side and cathode-side catalyst layers 8 and 8 'and gas diffusion layers 9 and 9' are connected.
  • MEA membrane-electrode unit
  • On the Anode side is in the connection a Fluidvertei- ment structure 10 with associated current collectors 11 is arranged.
  • the cathode side has a fluid distribution structure 10 'with current collectors 11'.
  • FIG. 6 schematically shows how the area of the source, ie of the holes or pores, has to be selected in order to ensure the desired concentration C A at a distance d from the source.
  • the area of the portion of the membrane-electrode assembly to be supplied as a sink with a spherical cap A 2 ⁇ d 2 approximated.
  • FIG. 7 shows the concept according to the invention by means of a direct methanol fuel cell (DMFC).
  • the fuel cell in this case has a structure 13, for example in the form of a membrane, with a multiplicity of openings 14, 14 'and 14 ".
  • the structure is in communication with a fuel reservoir so that the fuel can diffuse through the openings 14, 14 'and 14''into the fluid distribution structure, which in the present case is filled with water.
  • the diffusion is now adjusted so that at the membrane electrode assembly 15, the desired fuel concentration is ensured.
  • FIG. 8 schematically shows the structure of a fuel cell according to the invention.
  • Openings 14 to 14 '' '' provided structure is arranged at a distance d to the membrane-electrode unit 15.
  • the distance between the individual openings is 2d.
  • the diameter of the openings is 2r.

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  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Fuel Cell (AREA)
  • Inert Electrodes (AREA)

Abstract

L'invention concerne un procédé d'utilisation d'une cellule à combustible à oxydation directe dans lequel au moins un combustible fluide est transporté depuis un réservoir à combustible jusque dans une unité à électrodes et membrane par l'intermédiaire d'une structure de répartition de fluide. Le transport du combustible s'effectue passivement, c'est-à-dire sans convection. L'invention concerne en outre une cellule à combustible à oxydation directe de ce type.
EP07702934A 2006-01-20 2007-01-22 Cellule a combustible a oxydation directe dotee d'un apport passif de combustible et procede pour son utilisation Withdrawn EP1974413A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102006002926A DE102006002926A1 (de) 2006-01-20 2006-01-20 Direktoxidationsbrennstoffzelle und Verfahren zu deren Betreiben
PCT/EP2007/000518 WO2007085402A1 (fr) 2006-01-20 2007-01-22 Cellule a combustible a oxydation directe dotee d'un apport passif de combustible et procede pour son utilisation

Publications (1)

Publication Number Publication Date
EP1974413A1 true EP1974413A1 (fr) 2008-10-01

Family

ID=38268046

Family Applications (1)

Application Number Title Priority Date Filing Date
EP07702934A Withdrawn EP1974413A1 (fr) 2006-01-20 2007-01-22 Cellule a combustible a oxydation directe dotee d'un apport passif de combustible et procede pour son utilisation

Country Status (5)

Country Link
US (1) US7927753B2 (fr)
EP (1) EP1974413A1 (fr)
JP (1) JP2009524184A (fr)
DE (1) DE102006002926A1 (fr)
WO (1) WO2007085402A1 (fr)

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US20090017357A1 (en) 2009-01-15
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US7927753B2 (en) 2011-04-19
WO2007085402A1 (fr) 2007-08-02

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