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WO2006061639A2 - Pile a combustible - Google Patents

Pile a combustible Download PDF

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Publication number
WO2006061639A2
WO2006061639A2 PCT/GB2005/004744 GB2005004744W WO2006061639A2 WO 2006061639 A2 WO2006061639 A2 WO 2006061639A2 GB 2005004744 W GB2005004744 W GB 2005004744W WO 2006061639 A2 WO2006061639 A2 WO 2006061639A2
Authority
WO
WIPO (PCT)
Prior art keywords
fuel cell
cell according
solid
carbon
electrolyte
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/GB2005/004744
Other languages
English (en)
Other versions
WO2006061639A3 (fr
Inventor
John Thomas Sirr Irvine
John Lewis Bradley
John Barry Lakeman
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.)
UK Secretary of State for Defence
Original Assignee
UK Secretary of State for Defence
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 UK Secretary of State for Defence filed Critical UK Secretary of State for Defence
Publication of WO2006061639A2 publication Critical patent/WO2006061639A2/fr
Publication of WO2006061639A3 publication Critical patent/WO2006061639A3/fr
Anticipated expiration legal-status Critical
Ceased 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
    • H01M8/22—Fuel cells in which the fuel is based on materials comprising carbon or oxygen or hydrogen and other elements; Fuel cells in which the fuel is based on materials comprising only elements other than carbon, oxygen or hydrogen
    • H01M8/225—Fuel cells in which the fuel is based on materials comprising particulate active material in the form of a suspension, a dispersion, a fluidised bed or a paste
    • 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
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M8/1233—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte with one of the reactants being liquid, solid or liquid-charged
    • 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
    • H01M8/14—Fuel cells with fused electrolytes
    • H01M8/143—Fuel cells with fused electrolytes with liquid, solid or electrolyte-charged reactants
    • 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 is generally concerned with a fuel cell comprising a composite anode of a solid fuel material dispersed in a liquid electrolyte.
  • the invention is particularly, although not exclusively, directed to fuel cells in which the composite anode comprises carbon as the solid fuel material.
  • fuel cell also refers to semi-batteries and semi-fuel wherein the fuel is stored.
  • Carbon fuel cells are of interest as portable or compact power sources in that they offer the potential for high energy storage and power efficiencies when compared to alternative fuel cells, for example, those based on hydrogen, methanol and methane fuel.
  • alternative fuel cells for example, those based on hydrogen, methanol and methane fuel.
  • carbon fuel cells comprising a solid carbon anode and molten carbonate or hydroxide electrolytes are well known, the power available from such cells has to date been limited by inherent low current density and problems with corrosion of the cathode or electrolyte poisoning. Recent improvements have sought to address these inefficiencies.
  • US patent application 2002/0106549 discloses a corrosion resistant carbon fuel cell based on molten carbonate electrolyte.
  • the cell uses a highly reactive and expensive form of carbon (pyrolysed carbon) in order to obtain improved current density and power output (-100 mWcm "2 ).
  • acidic oxide is added to a molten hydroxide electrolyte and a humidified air feed is added to the cathode in order to avoid carbonate poisoning of the cell.
  • US patent application 2002/0015877 discloses a carbon fuel cell in which a solid state cathode reduces oxygen to oxygen anions (O 2" ) and passes them to a solid state or a melt electrolyte in contact with a carbon-containing anode.
  • the carbon anode is particulate in form and the electrolyte is a solid metal oxide.
  • the electrolyte comprises molten carbonate, which contacts a solid carbon anode or is admitted to a housing containing particulate carbon.
  • the current density of each arrangement is, however, low (power output ⁇ 1 mWcm "2 ) on account of solid-solid boundary surfaces or sluggish reactivity of carbon with carbonate ion.
  • the present invention therefore, provides an electricity producing fuel cell comprising a cathode, a solid electrolyte and a composite anode, which anode comprises, at an operating temperature of the cell, a dispersion of a solid fuel material in a liquid electrolyte.
  • references herein to "liquid” refer to the property of flow or a tendency to flow in response to an applied force, which flow is within a time scale perceptible to the human eye.
  • the cathode and/or solid electrolyte is capable of generating and/or passing a species oxidising the solid fuel material of the composite anode.
  • the fuel cell may, for example, comprise means providing for or supplying a precursor for the species to the cathode.
  • the present invention may provide a fuel cell comprising a cathode capable of generating oxygen anion from an oxygen-containing gas, means providing for or supplying an oxygen-containing gas to the cathode, a solid electrolyte capable of passing oxygen anion and a composite anode which comprises, at an operating temperature of the cell, a dispersion of a solid fuel material in a liquid electrolyte.
  • the fuel cell may use air as a source of the oxygen-containing gas.
  • the fuel cell may, in particular, comprise an oxygen gas permeable cathode, which is simply exposed to air.
  • the solid fuel material may comprise any suitable anode material capable of undergoing oxidation at the operating temperature of the cell.
  • suitable solid fuel materials include, in particular, magnesium, aluminium, carbon, silicon, zinc, iron, sulphur or materials containing these elements.
  • the solid fuel material comprises carbon or a carbon-containing material.
  • the solid fuel material is preferably comprised in a form, such as powder, particulate or shavings, which presents a high surface area.
  • a suitable carbon comprises one or more of graphite, quasi-graphite, coal, coke, fullerenes, carbon black, activated carbon, decolourised carbon and pyrolysed carbon.
  • Commercially available mixtures known as Super-S or Super-P carbon are particularly suitable.
  • the liquid electrolyte of the composite anode comprises a melt electrolyte.
  • Particularly suitable liquid electrolytes include highly conducting, molten metal salts, in particular, molten metal oxides, metal hydroxides, metal carbonates or mixtures thereof.
  • the composite anode generally comprises, at the operating temperature of the cell, a slurry of the solid fuel anode material in the liquid electrolyte.
  • operating temperature refers to a temperature at which the cell produces electricity. It will be appreciated, however, that the cell will produce electricity over a wide temperature range and that there is no requirement to maintain any particular temperature within that range.
  • the minimum operating temperature of the cell is that necessary to achieve, at least in part, a molten electrolyte. In any case, however, it is preferred that the operating temperature or temperature range is such that there is minimum resistance in the fuel cell.
  • the operating temperature lies between about 300 0 C and about 1000 0 C. In particularly preferred embodiments, the operating temperature lies between about 575 0 C and about 75O 0 C.
  • the melt or solid electrolyte may suitably include any of the following metal oxides: lead (II) oxide, bismuth (III) oxide, bismuth (V) oxide, molybdenum oxide, caesium (I) oxide, caesium (III) oxide, antimony (III) oxide, antimony (IV) oxide, antimony (V) oxide, copper (II) oxide, copper (I) oxide, germanium (II) oxide, germanium (IV) oxide, lithium oxide, palladium oxide, potassium (I) oxide, sodium (I) oxide, sodium peroxide, rubidium (II) oxide, rubidium (III) oxide, tin (II) oxide, tin (FV) oxide, tellurium (II) oxide, tellurium (I) oxide, tellurium (I) oxide, tellurium (III) oxide, vanadium pentoxide, arsenic (III) oxide, arsenic (V) oxide, indium (I) oxide, indium (III) oxide, boron oxide
  • the melt electrolyte may suitably include any of the following metal hydroxides: Group IA and Group IIA metal hydroxides, such as potassium hydroxide, sodium hydroxide, lithium hydroxide, strontium hydroxide, calcium hydroxide, magnesium hydroxide and mixtures thereof.
  • Group IA and Group IIA metal hydroxides such as potassium hydroxide, sodium hydroxide, lithium hydroxide, strontium hydroxide, calcium hydroxide, magnesium hydroxide and mixtures thereof.
  • the melt electrolyte includes a metal carbonate such as lithium carbonate, sodium carbonate, potassium carbonate, strontium carbonate, barium carbonate, magnesium carbonate, calcium carbonate, beryllium carbonate, caesium carbonate, rubidium carbonate or mixtures thereof.
  • a metal carbonate such as lithium carbonate, sodium carbonate, potassium carbonate, strontium carbonate, barium carbonate, magnesium carbonate, calcium carbonate, beryllium carbonate, caesium carbonate, rubidium carbonate or mixtures thereof.
  • the composite anode comprises a melt electrolyte of about 62% lithium carbonate and about 38% potassium carbonate.
  • the composite anode will at some point contain carbonate anion.
  • the maintenance of carbonate, oxide or hydroxide anion levels is not a requirement for functioning of the fuel cell.
  • the fuel cell may be provided with a current collector comprising one or more of a wire, mesh, filings or powder.
  • the current collector is resistant to corrosion by the action of carbonate.
  • the current collector material may also be chosen to catalyse the anode reaction.
  • the composite anode may also comprise a catalyst which catalyses the anode reaction and/or improves conductivity of the electrolyte.
  • Preferred collector materials and catalysts include nickel or precious metals such as platinum or palladium, metal alloys such as FeCrAlY or certain metal oxides and others known to those skilled in the art of molten carbonate fuel cells.
  • the solid electrolyte may comprise a solid state metal oxide. It may, in particular, comprise a solid state electrolyte, such as those based on doped ceramic materials of general formula (ZrO 2 )(HfO 2 )a(TiO 2 ) b (Al 2 O 3 ) c (Y 2 O 3 ) d (M x O y )e where a is about 0 to 0.2, b is about 0 to 0.5, c is about 0 to 0.5, d is about 0 to 0.5, e is about 0 to 0.15 and M is a divalent or trivalent metal such as manganese, iron, cobalt, nickel, copper or zinc.
  • a is about 0 to 0.2
  • b is about 0 to 0.5
  • c is about 0 to 0.5
  • d is about 0 to 0.5
  • e is about 0 to 0.15
  • M is a divalent or trivalent metal such as manganese, iron, cobalt
  • the solid state electrolyte comprises an yttrium stabilised zirconia (YSZ).
  • YSZ yttrium stabilised zirconia
  • zirconias doped with lanthanides such as gadolinium, ytterbium, praeseodymium and cerium ion are also suitable.
  • a lanthanide-doped ceria for example, GdCeo.sO t .g may be particularly suitable in that it is very stable to lithium carbonate.
  • Other suitable solid electrolytes may be based on lanthanum gallate, lanthanum aluminate, ABO 3 perovskites, calcium aluminate (C 12 Al 14 O 33 ) and La 9J3 SiOO 26 type apatites.
  • the resistivity of the solid electrolyte which should have substantially zero continuous porosity, is largely a function of its thickness (the distance between a surface contacting the cathode and a surface contacting the anode).
  • the solid electrolyte may, in particular, have thickness from about 10 ⁇ m to about 4 mm. In one embodiment of the present invention, the solid electrolyte is tubular and has thickness of about 3 mm.
  • a preferred cathode arrangement comprises a porous platinum paste sintered to the inner surface of a tubular solid electrolyte, which is open, at one end, to the atmosphere.
  • the cathode material may comprise a complex ceramic oxide, such as those known to the art under the formula (La 1-x Sr x ) 1-y BO 3 . ⁇ , where B is manganese, iron, cobalt or a combination thereof.
  • the composite anode may be contained within a compartment of the cell such that it is out of contact with the cathode surfaces of the cell.
  • the compartment is defined by the inner surfaces of a tubular nickel body and the outer surface of the tubular solid electrolyte referred to above.
  • the present invention also provides for a method of producing electricity comprising i) supplying an oxygen-containing gas to a cathode of a fuel cell comprising a solid electrolyte capable of passing oxygen anion and a composite anode, which anode comprises, at an operating temperature of the cell, a dispersion of a solid fuel material in a liquid electrolyte and ii) heating the fuel cell to the operating temperature.
  • the solid fuel material may comprise carbon or a carbon-containing material.
  • the solid fuel material may, in particular, comprise carbon in one or more of the forms referred to above.
  • the heating of the fuel cell should achieve a molten electrolyte.
  • the fuel cell is heated to the minimum operating temperature necessary to ensure a molten electrolyte.
  • the fuel cell is preferably heated to an operating temperature at which the resistance of the solid electrolyte is a minimum.
  • the fuel cell is heated to an operating temperature lying between about 300 0 C and about 1000 0 C.
  • the solid electrolyte comprises YSZ
  • the fuel cell is heated to an operating temperature lying between about 575 0 C and about 700 0 C.
  • the present invention provides a composite anode which imparts a liquid character to a solid fuel anode material so minimising solid-solid boundaries between the anode material and a solid electrolyte and improving current densities.
  • the carbon fuel cell of the present invention offers other significant advantages over, in particular, molten carbonate based carbon fuel cells.
  • the avoidance of a requirement for circulation of carbon dioxide means that the oxygen-containing gas flow remains undiluted by carbon dioxide thereby increasing the available cell potential.
  • a lighter and more compact design is available.
  • a suitable cathode material is not limited by a necessity for corrosion resistance since it is never in contact with molten carbonate.
  • the solid electrolyte avoids the need for regulation of a carbonate electrolyte level and allows a less complicated cathode reaction in which oxygen is directly reduced to oxygen anion. In other words, there is no requirement for the delivery of carbon dioxide before conversion of carbon can commence.
  • the fuel cell of the present invention may be provided with an interconnect allowing it to be used in a series-parallel stack with other fuel cells according to the present invention.
  • the stack may, in particular, be used to recharge a battery such as a lithium ion rechargeable battery.
  • the present invention also provides for a hybrid battery device, comprising one or more fuel cells according to the present invention and one or more lithium ion rechargeable batteries.
  • the device comprises one or more carbon fuel cells according to the present invention.
  • Figures 1 (a) and (b) are section perspective views of a fuel cell according to one embodiment of the present invention
  • Figure 2 is a plan view of the embodiment of Figure 1 adapted for inclusion in a stack;
  • Figure 3 is a graph showing the open circuit voltage of the embodiment of Figure 1 at two operating temperatures
  • Figures 4 (a) and (b) are graphs showing the impedance characteristics of the embodiment of Figure 1;
  • Figures 5 (a) and (b) are graphs showing the current developed by the embodiment of Figure 1 at two operating temperatures.
  • a fuel cell 11 comprises a half-closed cylinder container 12.
  • the cylinder 12 which comprises a corrosion resistant nickel body, contains a 8:1 (w/w) solid mixture of carbonate salt (62% lithium carbonate 38 % potassium carbonate) and Super-S carbon powder 13.
  • a tube, comprising YSZ ceramic 14, is maintained immersed in the solid mixture 13.
  • the ceramic 14 may include an interconnecting portion 15 which projects beyond an aperture in provided in the cylinder 12.
  • the tube is open to the atmosphere and its wall (3 mm thickness) carries a sintered coating of a porous platinum paste 22 across the whole of its inner surface 16 (35 cm 2 ).
  • a nickel mesh 19 (1 cm 2 ) is arranged in the solid mixture so that it contacts the outer surface 20 of the ceramic tube.
  • a gold, current collecting, wire 21 is connected to the mesh.
  • oxygen is
  • the nickel mesh allows free circulation of the carbon containing carbonate melt and a series of reactions occur which directly convert carbon to carbon dioxide.
  • the reactions at the anode include inter alia C + 2O 2" -» CO 2 + 4e and C + 2CO 3 2' ->
  • reaction 2CO 3 2" -> O 2 + 2CO 2 + 4e may be suppressed at least whilst
  • the cell is operated at a potential of 500 mV and ran over successive periods of 24 h at temperatures between 600 0 C and 725 0 C.
  • the cell develops an electrical power output of about lOmWcm "2 .
  • the specific resistance resistance per cm 2 of anode
  • the open circuit potential of the fuel cell at 625 0 C is about 700 to 800 mV and increases with run number.
  • the potential is constant at 850 mV with run number.
  • Figures 4 (a) and (b) show the impedance characteristics of the fuel cell with run number at a number of temperatures. As may be seen the impedance of the cell is initially diffusion controlled. However, the change in line shape in Figure 4 (b) at 665 0 C of the second run suggests that deposited nickel on the solid electrolyte inhibits the diffusion of oxygen anions to the mesh. After the second run, the build up of nickel becomes sufficient for efficient current collection and the resistance of the cell has dropped to its original value.

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

Abstract

Cette invention concerne une pile à combustible productrice d'électricité comprenant une cathode, un électrolyte solide et une anode composite, laquelle anode présente, à une température de fonctionnement de la pile, une dispersion d'un matériau combustible solide dans un électrolyte liquide.
PCT/GB2005/004744 2004-12-08 2005-12-08 Pile a combustible Ceased WO2006061639A2 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GBGB0426879.3A GB0426879D0 (en) 2004-12-08 2004-12-08 A fuel cell
GB0426879.3 2004-12-08

Publications (2)

Publication Number Publication Date
WO2006061639A2 true WO2006061639A2 (fr) 2006-06-15
WO2006061639A3 WO2006061639A3 (fr) 2006-09-28

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Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/GB2005/004744 Ceased WO2006061639A2 (fr) 2004-12-08 2005-12-08 Pile a combustible

Country Status (2)

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GB (1) GB0426879D0 (fr)
WO (1) WO2006061639A2 (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2013061067A1 (fr) 2011-10-28 2013-05-02 University Court Of The University Of St Andrews Cellule électrochimique au carbone direct
CN114361533A (zh) * 2022-01-10 2022-04-15 华北科技学院(中国煤矿安全技术培训中心) 一种具备三电极结构的碳燃料电池系统的测试方法

Family Cites Families (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1997013288A1 (fr) * 1995-10-06 1997-04-10 Hitachi, Ltd. Systeme faisant appel a des batteries auxiliaires
WO1999045607A1 (fr) * 1998-03-03 1999-09-10 Celltech Power, Llc Groupe electrogene a carbone-oxygene
NL1008832C2 (nl) * 1998-04-07 1999-10-08 Univ Delft Tech Werkwijze voor het omzetten van een koolstofomvattend materiaal, een werkwijze voor het bedrijven van een brandstofcel en een werkwijze voor het bedrijven van een brandstofcelstapel.
US6815105B2 (en) * 2000-10-23 2004-11-09 The Regents Of The University Of California Fuel cell apparatus and method thereof

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2013061067A1 (fr) 2011-10-28 2013-05-02 University Court Of The University Of St Andrews Cellule électrochimique au carbone direct
GB2496110A (en) * 2011-10-28 2013-05-08 Univ St Andrews Electrochemical Cell
CN104011932A (zh) * 2011-10-28 2014-08-27 圣安德鲁斯大学董事会 直接碳电化学电池
US9917321B2 (en) 2011-10-28 2018-03-13 University Court Of The University Of St Andrews Direct carbon electrochemical cell
KR102061645B1 (ko) * 2011-10-28 2020-01-02 유니버시티 코트 오브 더 유니버시티 오브 세인트 앤드류스 직접 탄소 전지화학 전지
CN114361533A (zh) * 2022-01-10 2022-04-15 华北科技学院(中国煤矿安全技术培训中心) 一种具备三电极结构的碳燃料电池系统的测试方法
CN114361533B (zh) * 2022-01-10 2024-01-30 华北科技学院(中国煤矿安全技术培训中心) 一种具备三电极结构的碳燃料电池系统的测试方法

Also Published As

Publication number Publication date
GB0426879D0 (en) 2005-01-12
WO2006061639A3 (fr) 2006-09-28

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