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WO1999053560A1 - Pile à combustible non susceptible d'empoisonnement, procédés de fonctionnement de ladite pile avec des combustibles carbonés - Google Patents

Pile à combustible non susceptible d'empoisonnement, procédés de fonctionnement de ladite pile avec des combustibles carbonés Download PDF

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Publication number
WO1999053560A1
WO1999053560A1 PCT/US1998/007373 US9807373W WO9953560A1 WO 1999053560 A1 WO1999053560 A1 WO 1999053560A1 US 9807373 W US9807373 W US 9807373W WO 9953560 A1 WO9953560 A1 WO 9953560A1
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WO
WIPO (PCT)
Prior art keywords
hydrogen
membrane
fuel
cell
fuel cell
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/US1998/007373
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English (en)
Inventor
Omar Yepez
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.)
Westfield Trading Corp
Original Assignee
Westfield Trading Corp
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 Westfield Trading Corp filed Critical Westfield Trading Corp
Priority to PCT/US1998/007373 priority Critical patent/WO1999053560A1/fr
Priority to AU71126/98A priority patent/AU7112698A/en
Publication of WO1999053560A1 publication Critical patent/WO1999053560A1/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
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8605—Porous electrodes
    • 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
    • H01M8/08—Fuel cells with aqueous electrolytes
    • 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
    • H01M8/1007—Fuel cells with solid electrolytes with both reactants being gaseous or vaporised
    • 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

  • This invention relates to an anode for fuel cells, which are able, by the use of hydrogen permeation, to electroxidize carbon compounds continuously at room temperature.
  • a Nonpoisoning fuel cells driven by hydrogen and carbonaceous fuels and methods of operating them is described.
  • Fuel cells have long been regarded as a useful future source of electric power. However, near room temperature commercial fuel cells heretofore have had to run only with hydrogen and have to use platinum as electrocatalyst. The need to use only pure hydrogen has driven the research of fuel cell to consider carbonaceous fuel processing in order to produce pure hydrogen.
  • simple organic compounds such as methanol, formaldehyde or formic acid, as direct fuel cells fuels , presents several advantages. They are relatively non- toxic, easy to store and handle and they possess a high energy density of the order of 1 W/Kg. Also, theoretically, fuel cells which burn carbonaceous fuels directly with air as oxidant have higher efficiencies than hydrogen fuel cells.
  • a new process has been developed which combines electrochemical reactions and the chemical reaction between occluded hydrogen and the carbon monoxide, formed during the electroxidation of a carbonaceous fuel at room temperature.
  • One of the possible reduction reaction paths for CO 2 involves carbon monoxide, CO, which has been designated as the poison in the electrochemical oxidation of carbonaceous compound.
  • the hydrogen permeation should assist the complete electrochemical oxidation of a carbonaceous compound towards CO 2 .
  • the hydrogen permeation should assist the complete electrochemical oxidation of a carbonaceous compound towards CO 2 .
  • a novel fuel cell which uses, as a fuel, a carbon compound which undergoes a direct electrochemical oxidation in the fuel cell at room temperature.
  • This cell comprises: a cathode, an electrolyte, and an anode.
  • the anode, of the present invention has three faces: a first face that is fluid permeable, a second face which is in contact with the electrolyte, and also serves as the reaction insertion face and a third face, which is in contact with hydrogen, is designated as the hydrogen absorption face.
  • the second and the third faces when considered together comprise an atomic hydrogen transmissive membrane which store and diffuses hydrogen in atomic form.
  • the hydrogen absorbed at the third face diffuses through the membrane and appears at the second face, where the direct electrochemical oxidation 3 of a carbonaceous compound and the poisoning of the anode both take place. Then, the occluded hydrogen reacts with the poisons, the product of this reaction undergoes an electrochemical oxidation and, as a consequence, the surface is cleaned, presenting new reaction sites for the continuous electrochemical oxidation of said carbonaceous compound.
  • the membrane material is selected from the group of metals consisting of Pd, Ni, Ti, Fe, V, Ta, Cu, Ag, Au, and the alloys and mixtures thereof.
  • the insertion reaction side of the membrane comprises electrocatalytic particles, which are suitably selected from the group of metals consisting of Pt, Pd, Ni, Ti, Fe, V, Cu, and alloys thereof, and hydrogen permeation nickel alloys. It is furthermore desirable that the insertion reaction side is in contact with colloidal polytetrafluorethylene and with an electrolyte capable of tolerating carbonation.
  • an electrolyte is selected from the group consisting of aqueous sodium bicarbonate, phosphoric acid and solid electrolytes, such as Nation ® .
  • This method comprises the sequential steps of: a. absorbing hydrogen from a source thereof on the absorption side of the atomic hydrogen transmissive membrane, b. passing hydrogen in atomic form, through the membrane to the opposite insertion reaction side of this membrane, c. providing a carbon compound to this insertion reaction side, d. allowing the direct electrochemical oxidation reaction of the carbon compound on the insertion reaction side to give an electrochemical oxidation product, 4 e. chemically reacting this product with the hydrogen passed through the membrane to give a reduction reaction product, f.
  • step (e) further electrochemically oxidizing this reduction reaction products of step (e) to provide carbon dioxide, as the principal product of the complete electrochemical oxidation of the carbon compound; and g. reducing air oxygen to air at the cathode, and drawing electricity generated thereby in said fuel cell from the cathode and anode thereof.
  • the fuel may be a fossil fuel, such as gasoline, kerosene or gas oil. It may also be a C-1 to C-6 alkane, such as methane, ethane, propane or butane. It may also be a C-1 to C-6 alcoh. ' . such as methanol, ethanol, propanol or butanol. It may also be carbon monoxide (CO).
  • the hydrogen containing medium may be hydrogen gas, hydrogen containing gas or hydrogen containing vapor.
  • the process includes a further step of supplying electrolytically formed hydrogen at the hydrogen absorbing surface of the membrane. It is preferred to supply hydrogen to the hydrogen absorbing membrane at a rate sufficient to establish a concentration gradient across said membrane which drives the hydrogen through it.
  • This molecular hydrogen is absorbed at the steam reforming side of a hydrogen permeable membrane, 5 4 H 2 ⁇ 8 H*
  • H* The occluded atomic hydrogen, H*, passes through the membrane to the fuel cell side, where it undergoes an electrochemical oxidation in accordance with the equation 8 H* ⁇ 8 H + + 8 e
  • each methane molecule produces 8 electrons, and the potential at zero current of this cell is 1 ,09 Volts.
  • the present invention provides a path around this problem: 6
  • the atomic hydrogen (H*) chemically reacts with the carbon monoxide adsorbed on the anode and transforms it into formaldehyde which then desorbs from the anode:
  • Figure 1 is a schematic representation of a non-poisoning fuel cell of the present invention.
  • Figure 2 is an schematic cross view of the non-poisoning anode.
  • Figure 3 is a diagrammatic representation of the chemical and electrochemical processes occurring at the inside of the anode of figure 1 .
  • Figure 4 is a schematic diagram showing the details of a compact electrodes test fuel cell, together with an ampermeter used to test its operation.
  • Figure 5 is a cyclic voltammetry of a palladium wire electrode, with no initially occluded hydrogen in NaOH 0.5 M.
  • Figure 6 is a cyclic voltammetry of a palladium wire electrode of Figure 5, deliberately loaded with hydrogen, in NaOH 0.5 M.
  • Figure 7 is a cyclic voltammetry of a palladium wire electrode of Figure 6, without occluded hydrogen in an aqueous 0.26 M NaHCOO and 0.24 M NaOH.
  • Figure 8 is a cyclic voltammetry of a palladium wire electrode of Figure 7 after 50 Coulombs of hydrogen were deliberately occluded .
  • Figure 9 shows the comparison between different current transitories obtained when a + 300 mV (SCE) potential pulse is applied on: 2.1 ) electroxidation of 2 Coulombs of occluded hydrogen in 0.5 M NaOH. 2.2) electroxidation of formate (HCOO ) on a palladium wire without occluded hydrogen and 2.3) electroxidation of formate (HCOO ) on a palladium wire with 2 Coulombs of occluded hydrogen.
  • Figure 10 is a cyclic voltammetry of a palladium wire electrode, without occluded hydrogen in an aqueous 0.5 M NaOH and 0.2 M methanol. 8
  • Figure 1 1 is a cyclic voltammetry of a palladium wire electrode of Figure 10, with 50 C of occluded hydrogen.
  • Figures 1 2 through 1 3 show current (I in milliamps) transitories (t in minutes) for different fuels in the compact electrodes fuel cell described in Figure 4.
  • Figure 1 0.2 molar methanol and a saturated bicarbonate solution on palladium loaded with hydrogen.
  • Figure 1 0.2 molar ethanol and a saturated bicarbonate solution on palladium loaded with hydrogen.
  • Figure 14 0.2 molar sucrose and a saturated bicarbonate solution on palladium loaded with hydrogen.
  • FIG. 1 is an schematic representation of the fuel cell arrangement of the present invention.
  • This comprises a cathode 1 provided with oxygen or air input means 2 and water output means 3.
  • the cell further comprises a non-poisoning anode 4, which comprises a net of capillaries 5, surrounded by a hydrogen supply line 6, originating in the catalytic steam reformer 7.
  • the cell has a primary carbonaceous fuel input means 8 and a carbon dioxide output means 9.
  • the electrolyte 10 is sandwiched between cathode 1 and anode 4.
  • Hydrogen may be supplied by any source of hydrogen, however, it has been found useful to utilize a catalytic steam reformer 7 which is provided with a hydrogen source fuel through conduit 1 1 and carbon dioxide generated in said reformed exits through exit port 1 2. Alternatively the hydrogen may be electrolytically generated.
  • the electricity generated by the system is taken off via cathode conduit 13 and anode conduit 14.
  • FIG 2 a transverse view of the non-poisoning anode 4 is diagrammatically illustrated.
  • the first face of the anode is a fluid permeable face 1 5
  • the body of the anode itself is made of a net of low thickness tubes or capillaries 5 made of a hydrogen permeation nickel 9 alloy or the like. This provides a holed structure to enable the molecular hydrogen to go into the third face 16 and diffuses through the tube wall 17 to the second face 18 of the anode.
  • the outside of the tubes can be coated with platinum, palladium or similarly active particles 19 and with polytetrafluorethylene particles 20 or the like. The spaces between tubes act as meniscus areas .
  • the hydrogen which passes through the capillaries 5 of the anode can react at the outside of the tubes or be ad/absorbed by the electrocatalytic particles 19 to react at their surfaces.
  • a flat screen made of a porous hydrogen storing material such as nickel alloys or the like. Since the hydrogen goes into the anode material through its side, however, in the later case hydrogen diffusion will be less than in the net of tubes or capillaries.
  • the electrolyte can be , for example, sodium bicarbonate, phosphoric acid or a room temperature solid electrolyte.
  • Hydrogen from an appropriate source is continuously pumped into the net of capillaries 5 of the anode 4 , to keep the outside of the capillaries and/or the electrocatalytic particles 19 saturated with it.
  • hydrogen is not used up in the subsequent electrochemical reactions, the hydrogen that does not reacts with the poisons, will electrochemically oxidize to protons, so a continuous hydrogen feed is needed.
  • Air or a similar source of oxygen is then supplied, via conduit 2, to cathode 1 which should, preferably, be made of the state of the art gas diffusion porous electrode, and simultaneously therewith the primary fuel which can be in gaseous or liquid form, is applied through conduit 8 to anode 4.
  • cathode 1 which should, preferably, be made of the state of the art gas diffusion porous electrode, and simultaneously therewith the primary fuel which can be in gaseous or liquid form, is applied through conduit 8 to anode 4.
  • the potential in the cell generated in accordance with the equations set forth above are then taken off from the anode via conduit 14 and the cathode via conduit 13.
  • SCE 242 mV vs. Normal Hydrogen Electrode
  • Cyclic voltammetry consists in measuring the current that floes through the working electrode, while a continuous positive and negative voltage ramps are applied on it. This is done by a potentiostat, and in this experiments, a voltage speed of 50 mV/s was used.
  • Q nF
  • Figure 5 is a cyclic voltammetry of a palladium wire electrode, with no initially occluded hydrogen in NaOH 0.5 M. It shows the formation of palladium oxide pick (a),
  • Control 2 Hartner (US patent 3393098) Process Example Figure 6 shows the cyclic voltammetry of the palladium electrode of Control 1 after initial occlusion of 50 C of hydrogen in the metal. Between 0 and + 300 mV (SCE), there is an oxidation wave diminishing in each potential cycle, which is due to hydrogen, coming from the inside of the electrode, and undergoes an electrochemical oxidation.
  • SCE + 300 mV
  • Figure 7 is a cyclic voltammetry of the palladium electrode of Control 1 , without occluded hydrogen in an aqueous 0.26 M NaHCOO + 0.24 M NaOH.
  • Peak (a) is due to the formate oxidation to CO 2 .
  • the current increases with potential.
  • CO is being generated, it strongly adsorbs on the electrode surface and poisons it.
  • the current no longer increases and falls to almost zero, generating peak (a), HCOO • + OH ⁇ CO 2 + H 2 O + 2 e ' HCOO ⁇ CO + OH
  • palladium oxide is formed and the strongly adsorbed CO is also oxidized
  • Example 2 The Process of the Present Invention Figure 8 is a cyclic voltammetry of the palladium wire of Example 1 , after 50 C of hydrogen were deliberately occluded. The current continuosly increases with the potential, the peak (a) (observed in Figure 7) has disappeared, because the non-poisoning reaction, already described is taking place,
  • FIG. 10 Electroxichemical Oxidation of Methanol (Poisoning Effect Example)
  • Figure 10 is a cyclic voltammetry of the palladium electrode of Control 1 , without occluded hydrogen in an aqueous 0.2 M CH 3 OH (methanol) + 0.5 M NaOH. 15
  • Peak (a) is due to the methanol oxidation to CO 2 .
  • the current increases with potential.
  • CO in this process CO is being generated, it strongly adsorbs on the electrode surface and poisons it. The current no longer increases and falls to almost zero, generating peak
  • Example 4 The Process of the Present Invention with methanol as a fuel
  • Figure 1 1 is a cyclic voltammetry of the palladium wire of Example 3, after 50 C of hydrogen were deliberately occluded. The current continuosly increases with the potential, the peak (a) (observed in Figure 10) has disappeared, because the non-poisoning reaction, is taking place,
  • FIG. 4 An apparatus that simulate a fuel cell, for carrying out test experiments which are set forth in the examples 5 through 7 (below), regarding to the process of the present invention.
  • This apparatus comprises a two-part cell having an anode sector 21 and a cathode sector 22.
  • the cathode sector 22 is further provided with oxygen input means 23.
  • the two sectors are separated by a sintered glass barrier 24 permeable to ion flow.
  • An anode of palladium 25 is provided in sector 21 and a platinum cathode 26 is provided in sector 22.
  • An ammeter 27 is connected to anode 25 via conduit 28 and to cathode 26 via conduit 29.
  • a 1 cm 2 area palladium electrode 25 was occluded with hydrogen up to 1 50 C, at constant current, in a two electrodes electrochemical cell, using perchloric acid 0.5 M as electrolyte. Then the palladium electrode was transferred to the compact electrode fuel cell of Figure 4, where, as the non-poisoning effect of the occluded hydrogen is taking place, an spontaneous flow of current is expected and measured by the ammeter. This experiment were performed at room temperature.

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

Abstract

L'invention concerne une nouvelle pile à combustible telle que celles utilisant un composé carboné qui effectue l'électro-oxydation dans ladite pile à combustible. Cette pile comprend une cathode (1), un électrolyte (10), et une anode (4). L'anode possède une première face constituée d'un fluide perméable et une seconde face en contact avec l'électrolyte. La seconde face comprend une membrane perméable à l'hydrogène atomique, constituée d'un élément métallique électro-catalytique qui stocke et diffuse l'hydrogène sous forme atomique. Cette membrane possède un côté d'absorption et un côté opposé de réaction d'insertion. L'invention concerne également un procédé de production d'électricité dans une pile à combustible, tel que spécifié dans la description générale et dans l'une des formes d'exécution spécifique donnée dans ladite description. Ce procédé consiste à absorber un milieu contenant de l'hydrogène du côté absorption de la membrane perméable à l'hydrogène atomique; à faire passer l'hydrogène sous une forme atomique, à travers la membrane, vers le côté opposé de réaction d'insertion de ladite membrane; à fournir un composé carboné audit côté de réaction d'insertion; à permettre la réaction directe d'électro-oxydation du composé carboné sur le côté de réaction d'insertion, de façon à obtenir un produit d'électro-oxydation; à le faire réagir chimiquement avec l'hydrogène qui a traversé la membrane, de façon à obtenir un produit de réaction de réduction; puis à électro-oxyder ce produit de façon à obtenir un dioxyde de carbone comme produit principal de l'oxydation électrochimique complète du composé carboné; et à utiliser l'électricité ainsi produite dans la pile à combustible à partir de la cathode et de l'anode.
PCT/US1998/007373 1998-04-08 1998-04-08 Pile à combustible non susceptible d'empoisonnement, procédés de fonctionnement de ladite pile avec des combustibles carbonés Ceased WO1999053560A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
PCT/US1998/007373 WO1999053560A1 (fr) 1998-04-08 1998-04-08 Pile à combustible non susceptible d'empoisonnement, procédés de fonctionnement de ladite pile avec des combustibles carbonés
AU71126/98A AU7112698A (en) 1998-04-08 1998-04-08 Nonpoisoning fuel cell and methods of operating the same with carbonaceous fuels

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
PCT/US1998/007373 WO1999053560A1 (fr) 1998-04-08 1998-04-08 Pile à combustible non susceptible d'empoisonnement, procédés de fonctionnement de ladite pile avec des combustibles carbonés

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WO1999053560A1 true WO1999053560A1 (fr) 1999-10-21

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7289826B1 (en) 2002-04-16 2007-10-30 Faulkner Interstices, Llc Method and apparatus for beam selection in a smart antenna system
US7349721B2 (en) 2002-04-16 2008-03-25 Faulkner Interstices, Llc System and apparatus for collecting information for use in a smart antenna system
US7418271B2 (en) 2002-04-16 2008-08-26 Faulkner Interstices Llc Smart antenna apparatus
US7463906B2 (en) 2002-04-16 2008-12-09 Faulkner Interstices Llc Method and apparatus for collecting information for use in a smart antenna system

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR1403195A (fr) * 1963-06-20 1965-06-18 Tokyo Shibaura Electric Co Piles à combustible
FR1417112A (fr) * 1962-08-04 1965-11-12 Siemens Ag Procédé de transformation électrochimique de composés dissous, liquides ou gazeux contenant de l'hydrogène
US3337369A (en) * 1960-09-29 1967-08-22 Leesona Corp Non-porous diffusion membrane fuel cell
US3470026A (en) * 1965-03-03 1969-09-30 Prototech Inc Method of operating fuel cell with carbon-containing fuel
GB1449233A (en) * 1973-10-31 1976-09-15 Exxon Research Engineering Co Buffer electrolyte fuel cell with low cost electrodes

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3337369A (en) * 1960-09-29 1967-08-22 Leesona Corp Non-porous diffusion membrane fuel cell
FR1417112A (fr) * 1962-08-04 1965-11-12 Siemens Ag Procédé de transformation électrochimique de composés dissous, liquides ou gazeux contenant de l'hydrogène
FR1403195A (fr) * 1963-06-20 1965-06-18 Tokyo Shibaura Electric Co Piles à combustible
US3470026A (en) * 1965-03-03 1969-09-30 Prototech Inc Method of operating fuel cell with carbon-containing fuel
GB1449233A (en) * 1973-10-31 1976-09-15 Exxon Research Engineering Co Buffer electrolyte fuel cell with low cost electrodes

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7289826B1 (en) 2002-04-16 2007-10-30 Faulkner Interstices, Llc Method and apparatus for beam selection in a smart antenna system
US7349721B2 (en) 2002-04-16 2008-03-25 Faulkner Interstices, Llc System and apparatus for collecting information for use in a smart antenna system
US7418271B2 (en) 2002-04-16 2008-08-26 Faulkner Interstices Llc Smart antenna apparatus
US7444157B2 (en) 2002-04-16 2008-10-28 Faulkner Interstices Llc Method and apparatus for beam selection in a smart antenna system
US7463906B2 (en) 2002-04-16 2008-12-09 Faulkner Interstices Llc Method and apparatus for collecting information for use in a smart antenna system

Also Published As

Publication number Publication date
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