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WO2005078846A1 - Pile a combustible et electroreformeur jumeles - Google Patents

Pile a combustible et electroreformeur jumeles Download PDF

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Publication number
WO2005078846A1
WO2005078846A1 PCT/US2005/002631 US2005002631W WO2005078846A1 WO 2005078846 A1 WO2005078846 A1 WO 2005078846A1 US 2005002631 W US2005002631 W US 2005002631W WO 2005078846 A1 WO2005078846 A1 WO 2005078846A1
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WO
WIPO (PCT)
Prior art keywords
hydrogen
cell
barrier layer
fuel
dual
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.)
Ceased
Application number
PCT/US2005/002631
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English (en)
Inventor
Mahlon S. Wilson
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.)
University of California Berkeley
University of California San Diego UCSD
Original Assignee
University of California Berkeley
University of California San Diego UCSD
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 University of California Berkeley, University of California San Diego UCSD filed Critical University of California Berkeley
Publication of WO2005078846A1 publication Critical patent/WO2005078846A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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
    • H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
    • H01M8/184—Regeneration by electrochemical means
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/92—Metals of platinum group
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/94—Non-porous diffusion electrodes, e.g. palladium membranes, ion exchange membranes
    • 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
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/023—Porous and characterised by the material
    • 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
    • H01M8/04197—Preventing means for fuel crossover
    • 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 present invention relates generally to fuel cell technology, and, more particularly, to the use of an electroreformer with a fuel cell.
  • a reformer is a device for converting hydrocarbon fuels, such as methanol, into free hydrogen, carbon dioxide, and water.
  • the present invention comprises back-to-back electrochemical cells separated by an electronically conductive hydrogen permselective barrier layer that altogether form a "dual" cell: Cell One and Cell Two.
  • Cell One is employed as an electrochemical reformer (electroreformer) that oxidizes a fuel (such as methanol) at the anode and provides hydrogen to the permselective barrier layer in the cathode reaction. The hydrogen then traverses the permselective barrier layer, the other side of which serves as the anode of Cell Two.
  • Cell Two is effectively a hydrogen fuel cell that provides power for the electroreformer and an attached load.
  • the present invention provides a supplemental current to the electroreformer that assists in maintaining a hydrogen content of the permselective barrier layer that is sufficiently high to sustain performance of the overall dual-cell.
  • the use of the permselective barrier layer allows for a fuel cell system that reduces the difficulties with water balance and fuel cross-over to Cell Two cathode, both of which cause losses in efficiency, stability, and cathode performance.
  • the benefits provided by the efficiency, stability, and improve performance are particularly relevant for low-power (e.g., cellular phone) types of methanol fuel cell power systems.
  • One of the earliest uses of a permselective membrane in an electrochemical cell was taught in U.S. Patent no.
  • Ayers further describes fuel cell examples, whereby the dehydrogenation of a reactant on one side of the hydrogen permeable barrier layer supplies hydrogen that diffuses through the barrier layer to the other side to supply a fuel cell.
  • a "potentiostat" power source
  • a fuel cell power load is connected between the barrier layer and the oxygen reduction electrode. While the present invention also uses a power source and a power load, the electrical connections and current flows are different, and the power sources serve different functions.
  • the power source induces a chemical dehydrogenation reaction to supply the permselective barrier layer with hydrogen
  • the power source drives an electrochemical process to supply supplemental hydrogen.
  • the chemical dehydrogenation reaction is lethargic.
  • Ayers reports a current through the fuel cell circuit of 40 microamps/cm 2 when the cell is operated at 80°C.
  • the dual-cell of the present invention achieves current densities a thousand times higher at 80°C.
  • a methanol dual-cell with a permselective barrier layer was investigated in "A Methanol Impermeable Proton Conducting Composite Electrolyte System," J. Electrochem. Soc, Vol.
  • the barrier layer is replenished by hydrogen diffusing in through the electrolyte from the fuel anode.
  • the permselective barrier layer becomes depleted.
  • conservation of charge dictates that for every proton that becomes hydrogen on one side of the barrier layer, a hydrogen must leave the opposite side of the barrier layer. Consequently, the net addition is zero and performance dies as hydrogen is lost to scavenging mechanisms.
  • the solution provided by the present invention is to provide supplemental hydrogen directly to the permselective barrier layer, while keeping the supplemental hydrogen separate from the fuel feed.
  • the separation is important, as supplemental hydrogen in the fuel feed would preferably oxidize at the anode instead of traversing the electrolyte to the barrier layer.
  • the present invention includes a fuel cell system using an electrochemical dual-cell configuration.
  • Each dual-cell includes a catalyzed fuel oxidation electrode on one end, followed by an electrolyte separator, a hydrogen permselective barrier layer, another electrolyte separator, and finally a catalyzed oxidant reduction electrode on the other end.
  • a power supply is electrically connected to the hydrogen permselective barrier layer and the catalyzed fuel oxidation electrode to provide a supplemental current to the hydrogen permselective barrier layer.
  • Figure 1 is a pictorial illustration of a hydrogen permselective barrier layer dual cell.
  • Figure 2 is a pictorial illustration displaying the reactions and transport species within a typical dual-cell configuration using acidic electrolytes.
  • Figure 3 is a pictorial illustration of one embodiment of the present invention dual-cell electroreformer.
  • Figure 4 graphically displays the present invention total dual-cell polarization and resistance curves using hydrogen gas as a fuel.
  • Figure 5 graphically displays the present invention total dual-cell polarization and resistance curves using methanol as a fuel.
  • Figure 6 graphically displays the Cell Two polarization curves constructed from the methanol and hydrogen test runs displayed in Figures 4 and 5.
  • Figure 7 is a schematic of a bipolar circuit used with the present invention.
  • Figure 8 is a schematic of a monopolar circuit configuration used with the present invention.
  • Figure 9 is a schematic of a monopolar circuit configuration, including MOSFET switches, used with the present invention.
  • DMFCs DETAILED DESCRIPTION Direct Methanol Fuel Cells
  • PEFCs polymer electrolyte fuel cell
  • Foremost of the identified difficulties is the permeation of the fuel across the polymer electrolyte membrane (PEM), also referred to as fuel cross-over, which results in both fuel loss (with corresponding decrease in efficiency) and negative effects on the air electrode, such as mixed electrochemical potential and electrode flooding.
  • PEM polymer electrolyte fuel cell
  • a popular strategy to minimize fuel cross-over is to provide a lean feed of methanol fuel (e.g., 0.5 M methanol in water), so that the majority of fuel is consumed and/or the amount that permeates the PEM is minimized because of the dilute source.
  • methanol fuel e.g., 0.5 M methanol in water
  • the cross-over flux can be as great as the fuel usage at the anode, resulting in a substantial decrease in overall efficiency.
  • the cross-over methanol causes problems with cathode stability, as the presence of the methanol at the cathode causes a mixed potential (i.e., competes with the oxygen reduction reaction), and longevity, as the methanol causes problems by wetting out otherwise hydrophobic structures and thus interfering with oxygen access and transport (i.e., "flooding" of the electrode).
  • An alternative approach, provided by the present invention is to "electrochemically reform” or “electroreform” the fuel in a separate "first" cell (Cell One) to form protons at the anode, that are then evolved as hydrogen at the cathode of Cell One.
  • the evolved hydrogen is separated from the fuel and introduced to the anode of a "conventional" hydrogen fuel cell (Cell Two).
  • Cell Two a hydrogen permeable separator, hereinafter referred to as a permselective barrier layer, between the two separate cells that allows hydrogen to pass through while blocking other chemical species.
  • the surfaces of the permselective barrier layer preferably treated with a catalyst, serves the electrochemical functions of directly converting protons from Cell One to (monatomic) hydrogen dissolved within the permselective barrier layer on one side and at the other side forming protons for the second cell from the monatomic hydrogen within the barrier layer.
  • Transport of the monatomic hydrogen through the barrier layer proceeds by diffusion of the uncharged species, and, hence, is a function of hydrogen content, which can be increased or maintained by the addition of a supplemental electric current.
  • a portion of the power produced by Cell Two may be used to provide the supplemental current that drives the methanol oxidation/ hydrogen formation in Cell One.
  • the supplemental current drives the electrochemical oxidation of a small amount of fuel to generate a slight excess of protons that conduct across the Cell One electrolyte to introduce the supplemental hydrogen to the permselective barrier layer. Consequently, the net effect is to increase the total current flow through Cell One, somewhat higher than the current provided by Cell Two.
  • permselective barrier layer 10 was "blackened” (electrochemically coated with high surface area platinum to facilitate the hydrogen interfacial reactions) pure palladium and was placed between two electrolyte separators 20, 25 in a fuel cell configuration that comprised: fuel flow field 30, catalyzed fuel oxidation electrode (Cell One anode) 40, air flow field 50, catalyzed oxidant reduction electrode (Cell Two cathode) 60, and electric load 70.
  • Figure 2 portrays the reactions and transport processes within an ideal dual-cell fuel cell.
  • permselective barrier layer 10 must be electrically conductive to shuttle electrons between the interfacial processes since the hydrogen transported through permselective barrier layer 10 is as an uncharged species.
  • Fuel reacts with water at Cell One anode 40 releasing protons that travel through first electrolyte separator 20, creating an ionic current to Cell One cathode 45, which is located on the Cell One side of permselective barrier layer 10.
  • Cell One cathode 45 the protons and combine with electrons, creating non-charged hydrogen that travel through permselective barrier layer 10 to Cell Two anode 65 (the opposite side of barrier layer 10).
  • Protons are again formed with the release of an electron and travel through second electrolyte separator 25, creating an ionic current to Cell Two oxidant reduction cathode 60, where the protons combine with oxygen and electrons to form water.
  • the processes described in Figure 2 are for acidic electrolytes, however, alkaline electrolytes may also be used.
  • the dual-cell was operated with hydrogen as the feed in Cell One, the configuration behaved as a regular fuel cell, but at somewhat diminished currents, due to the hydrogen transport and interfacial limitations of permselective barrier layer 10. Introducing methanol along with the hydrogen had little or no effect on dual-cell performance because permselective barrier layer 10 prevented any methanol access to Cell Two cathode 60.
  • any inefficiencies with the hydrogen transport into permselective barrier layer 10 or the presence of any mechanism that scavenges hydrogen from permselective barrier layer 10, decreases the amount of hydrogen within permselective barrier layer 10. Since lowering hydrogen content within permselective barrier layer 10 lowers the hydrogen flux (permeability concentration x diffusivity), less hydrogen is available to Cell Two, resulting in an increased overpotential condition at Cell Two anode 65 causing overall fuel cell performance to drop.
  • One mechanism that results in the loss of hydrogen from permselective barrier layer 10 is the escape of hydrogen gas through electrolyte separators 20, 25.
  • FIG. 3 Another mechanism that results in the loss of hydrogen is that oxygen can diffuse in from Cell Two cathode 60 to permselective barrier layer 10, scavenging hydrogen to form water.
  • power supply 80 attached to permselective barrier layer 10, to electrochemically charge permselective barrier layer 10 with hydrogen.
  • Cell One anode 40 is used as the necessary counter-electrode for power supply 80.
  • a 4 cm 2 active area dual-cell utilizes a 50 micron thick Ta foil vacuum-coated on either side with 5,000 A of Pd as permselective barrier layer 10, with polymer electrolyte and catalyst inks painted onto both sides.
  • a preferred polymer electrolyte is NationalTM.
  • the Pd-coated Ta foil is highly permeable to hydrogen. However, hydrogen embrittlement may crack the tantalum under certain conditions. Therefore, the cell components are tightly swaged together, helping to keep any cracks formed in permselective barrier layer 10 closed. Because methanol seepage through the cracks could occur, the fuel cell cathode performances were compared with and without methanol in the fuel feed in order to determine if any evidence of methanol cross-over was apparent. 6.45 cm 2 square permselective barrier layer 10 was sandwiched between two electrolyte separators 20, 25.
  • Cell One anode 40 comprised 2.4 mg/cm 2 of Pt- RuOx mixed with a solid polymer electrolyte solution to form an ink and painted onto an uncatalyzed gas diffusion backing.
  • a preferred gas diffusion backing is ELAT®, manufactured by E-TEK, Inc.
  • Cell Two cathode 60 comprised a 0.5 mg Pt/cm 2 catalyzed ELAT® gas diffusion electrode impregnated with a solid polymer electrolyte.
  • a preferred polyester film is Mylar®.
  • Polyester film 90 served to prevent ionic conductivity and fuel transport between membrane 20 in the area not occluded by Pd/Ta permselective barrier layer 10.
  • the dual-cell assembly was inserted into standard single-cell testing hardware that included machined graphite flow-fields. Aside from the electrical connection to Pd/Ta permselective barrier layer 10, all other elements and connections were identical to any conventional fuel cell.
  • the hydrogen and air feeds used in the tests were pressurized to 3 bar (30 psig) and sparged through humidifier bottles at or above the fuel cell temperature of 80°C. Methanol/ water mixtures were introduced with a liquid feed pump at near ambient pressure.
  • the dual-cell was connected to load 70 to control total-cell voltages or current.
  • the barrier layer becomes depleted of hydrogen on the fuel cell side as current density increases.
  • the polarization curves show that the current densities increase unambiguously with the barrier layer charging current, particularly with increasing current. This suggests that some of the inefficiencies of the hydrogen injection process can be partially overcome by additional charging current.
  • the extraneous charging current increases polarization of Cell One anode 40, which is shown in the anode - barrier layer curves, the lowest set of curves in the figure. A roughly 10 mV increase is obtained per 5 mA/cm 2 of extraneous charging current at any given total cell current. The penalty is more severe than a simple superimposition of currents would anticipate.
  • the anode-barrier layer electroreformer voltage curves suggest that Cell One anode 40 is polarized 300 - 400 mV more than when hydrogen is used, as expected.
  • the supplemental charging current had a greater than anticipated effect on voltage between Cell One anode 40 and cathode 45.
  • the 10 mA/cm 2 anode barrier layer curve was about 30 mV higher than the 5 mA/cm 2 .
  • the total dual-cell polarization curves were not much different at lower current densities, although the 10 mA/cm 2 run attained the higher current densities of the two curves.
  • FIG. 6 graphically portrays five test runs, three with hydrogen feed and two with methanol feed.
  • the Cell Two (fuel cell side) polarization curves were constructed for both the hydrogen and methanol experiments by adding the anode-barrier layer voltages to the total dual cell voltages in the polarization curves in Figures 4 and 5.
  • Review of the results indicates that at the higher currents, the hydrogen-fed cells provided higher performances.
  • permselective barrier layer 10 in the methanol feed configuration is somewhat more hydrogen starved than permselective barrier layer 10 in the hydrogen feed configuration.
  • Load 70 is placed in parallel with energy storage device 100.
  • energy storage device 100 may be a battery or a capacitor.
  • DC-DC converter 110 is also connected in parallel with both load 70 and energy storage device 100, and supplies regulated power to multiplexer 120.
  • Multiplexer 120 provides supplemental current to each dual-cell barrier layer 10 in turn.
  • DC-DC converter 110 must include electrically floating outputs that are multiplexed to each individual barrier layer 10, in order to account for the step changes in voltages across the dual-cell stack.
  • the dual-cell voltages may be monitored through logic circuitry (not shown) that provides extra current to dual-cells that are underperforming.
  • a dual-cell system utilizes power switches 130 between dual-cells 5, and supplemental current switches 140 between barrier layer 10 and Cell One anode 40 of adjacent dual-cells 5.
  • the dual-cells cannot be stacked in the conventional sense using bipolar plates, and, thus, a monopolar configuration is used. In a monopolar configuration, the cells do not share components as in a bipolar plate stack ( Figure 7).
  • the dual-cell system is providing a power output to load 70 or energy storage device 100, power switches 130 are closed and supplemental current switches 140 are open.
  • supplemental current switches 140 close as power switches 130 open, allowing barrier layers 10 to recharge using power from energy storage device 100 that also supplies load 70 while in this mode.
  • the total dual-cell voltage is roughly equal to that of the electroreformer, although opposite in sign. Consequently, a series of cells provides a charging voltage for a battery that is roughly equal to the voltage necessary to charge the permselective barrier layers, although at a slightly higher current density. A charge duty cycle of about 5% suffices in keeping the permselective barrier layers charged to the same degree as the constant current experiments.
  • 2n+2 switches/ relays are then needed to accomplish both modes. While Figure 8 shows a simple configuration to achieve the power/ charge circuits, some of the power switches may see a reverse voltage equivalent to the open-circuit voltage of Cell Two (fuel cell) side during the charge phase.

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

Abstract

L'invention concerne un système de pile à combustible faisant appel à des piles électrochimiques jumelées. Chaque pile jumelée comprend une électrode d'oxydation de combustible catalysé (40) à une extrémité, suivie d'un séparateur électrolytique (20), une couche d'arrêt permsélective à l'hydrogène (10), un autre séparateur électrolytique (25), et enfin une électrode de réduction d'oxydant catalysé (60) à l'autre extrémité. Un bloc d'alimentation (80) est électriquement connecté à la couche d'arrêt permsélective à l'hydrogène (10) et à l'électrode d'oxydation de combustible catalysé (40) qui fournit un courant supplémentaire à la couche d'arrêt permsélective à l'hydrogène.
PCT/US2005/002631 2004-02-03 2005-01-31 Pile a combustible et electroreformeur jumeles Ceased WO2005078846A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US77119404A 2004-02-03 2004-02-03
US10/771,194 2004-02-03

Publications (1)

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WO2005078846A1 true WO2005078846A1 (fr) 2005-08-25

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Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3446674A (en) * 1965-07-07 1969-05-27 United Aircraft Corp Method and apparatus for converting hydrogen-containing feedstocks
US3467551A (en) * 1965-09-30 1969-09-16 Leesona Corp Method of operating fuel cell
US5738708A (en) * 1995-06-07 1998-04-14 The Regents Of The University Of California Office Of Technology Transfer Composite metal membrane
US6242122B1 (en) * 1996-11-11 2001-06-05 Forschungszentrum Julich Gmbh Fuel cell electrode-electrolyte unit
US6428918B1 (en) * 2000-04-07 2002-08-06 Avista Laboratories, Inc. Fuel cell power systems, direct current voltage converters, fuel cell power generation methods, power conditioning methods and direct current power conditioning methods
US6696382B1 (en) * 2000-11-14 2004-02-24 The Regents Of The University Of California Catalyst inks and method of application for direct methanol fuel cells
US6866952B2 (en) * 2001-04-18 2005-03-15 Mti Microfuel Cells Inc. Apparatus and method for controlling undesired water and fuel transport in a fuel cell
US6884530B2 (en) * 2001-05-31 2005-04-26 Sfc, Smart Fuel Cell Ag Method of improving the performance of a direct feed fuel cell

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3446674A (en) * 1965-07-07 1969-05-27 United Aircraft Corp Method and apparatus for converting hydrogen-containing feedstocks
US3467551A (en) * 1965-09-30 1969-09-16 Leesona Corp Method of operating fuel cell
US5738708A (en) * 1995-06-07 1998-04-14 The Regents Of The University Of California Office Of Technology Transfer Composite metal membrane
US6242122B1 (en) * 1996-11-11 2001-06-05 Forschungszentrum Julich Gmbh Fuel cell electrode-electrolyte unit
US6428918B1 (en) * 2000-04-07 2002-08-06 Avista Laboratories, Inc. Fuel cell power systems, direct current voltage converters, fuel cell power generation methods, power conditioning methods and direct current power conditioning methods
US6696382B1 (en) * 2000-11-14 2004-02-24 The Regents Of The University Of California Catalyst inks and method of application for direct methanol fuel cells
US6866952B2 (en) * 2001-04-18 2005-03-15 Mti Microfuel Cells Inc. Apparatus and method for controlling undesired water and fuel transport in a fuel cell
US6884530B2 (en) * 2001-05-31 2005-04-26 Sfc, Smart Fuel Cell Ag Method of improving the performance of a direct feed fuel cell

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