WO2008138923A1 - Pile à combustible pour une utilisation dans la génération d'électricité à partir d'un substrat carboné solide - Google Patents

Pile à combustible pour une utilisation dans la génération d'électricité à partir d'un substrat carboné solide Download PDF

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Publication number
WO2008138923A1
WO2008138923A1 PCT/EP2008/055827 EP2008055827W WO2008138923A1 WO 2008138923 A1 WO2008138923 A1 WO 2008138923A1 EP 2008055827 W EP2008055827 W EP 2008055827W WO 2008138923 A1 WO2008138923 A1 WO 2008138923A1
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WO
WIPO (PCT)
Prior art keywords
fuel cell
oxygen
electrochemical
carbonaceous substrate
anode
Prior art date
Application number
PCT/EP2008/055827
Other languages
English (en)
Inventor
Geoffrey Howard Kelshall
Klaus Hellgardt
Original Assignee
Imperial Innovations Limited
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 Imperial Innovations Limited filed Critical Imperial Innovations Limited
Priority to EP08750259A priority Critical patent/EP2156500A1/fr
Publication of WO2008138923A1 publication Critical patent/WO2008138923A1/fr

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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
    • H01M8/10—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
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/9041—Metals or alloys
    • H01M4/905—Metals or alloys specially used in fuel cell operating at high temperature, e.g. SOFC
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
    • H01M8/0668—Removal of carbon monoxide or carbon dioxide
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
    • H01M8/0675—Removal of sulfur
    • 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
    • H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
    • H01M4/9025—Oxides specially used in fuel cell operating at high temperature, e.g. SOFC
    • H01M4/9033—Complex oxides, optionally doped, of the type M1MeO3, M1 being an alkaline earth metal or a rare earth, Me being a metal, e.g. perovskites
    • 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
    • H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
    • H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
    • H01M8/1253—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides the electrolyte containing zirconium oxide
    • 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
    • H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
    • H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
    • H01M8/126—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides the electrolyte containing cerium oxide
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to an electrochemical fuel cell for generating electricity from a solid carbonaceous substrate, comprising an electrochemical reactor and an oxidation reactor and a method of generating electricity from a solid carbonaceous substrate.
  • the resulting oxide ions are transported under an electric potential and oxygen concentration gradients, through an ionically-conducting electrolyte (e.g. ZrO 2 - Y 2 O 3 yttrium- stabilised zirconia (YSZ) or Ce 09 Gd 0 1 O 1 95 (CGO)) 10s of ⁇ m thick, to an electronically conducting anode, at which those ions oxidise carbon particles, caused to impinge from a molten anolyte onto the anode, evolving CO 2 .
  • an ionically-conducting electrolyte e.g. ZrO 2 - Y 2 O 3 yttrium- stabilised zirconia (YSZ) or Ce 09 Gd 0 1 O 1 95 (CGO)
  • the first aspect of the invention therefore provides an electrochemical fuel cell for generating electricity from a solid carbonaceous substrate, comprising an electrochemical reactor and an oxidation reactor; wherein the electrochemical reactor comprises: a cathode for forming oxygen ions from an oxygen source; an anode for facilitating the dissolution of the oxygen into a liquid; and an ionically conducting electrolyte for transporting the dissolved oxygen to the anode; and wherein the oxidation reactor comprises: an inlet for introduction of the dissolved oxygen from the electrochemical reactor; a bed or slurry of solid carbonaceous substrate; an outlet for removal of the oxidised carbon species generated by oxidation of the carbonaceous substrate by the dissolved oxygen; and a second outlet for re-introduction of the deplenished liquid to the electrochemical reactor.
  • the electrochemical reactor comprises: a cathode for forming oxygen ions from an oxygen source; an anode for facilitating the dissolution of the oxygen into a liquid; and an ionically conducting electrolyte for
  • a particular feature of the first aspect of the invention is the use of a second separate reactor for the oxidation of the carbonaceous fuel.
  • the dissolved oxygen and liquid are therefore transported from the electrochemical reactor to the oxidation reactor and contacted with the carbonaceous substrate.
  • the dissolved oxygen oxidises the carbonaceous substrate resulting in the depletion of the dissolved oxygen from the liquid, evolving oxidised carbon species, in particular CO 2 or other carbon containing gases which can be further modified and/or are removed from the oxidation reactor and can be treated subsequently.
  • the electrochemical reactor further comprises an inlet for the introduction of a source of oxygen.
  • the source of oxygen can be any oxygen containing gas including O 2 and air.
  • the source of oxygen can be compressed and provided in a supercritical state (i.e. >50 bar).
  • the lifespan and efficiency of the electrodes is extended in the fuel cell of the present application.
  • the range of substrates available for use in the fuel cell is therefore wider than that available for use in conventional fuel cells, which usually use gaseous (e.g. hydrogen, methane, etc) or liquid (e.g. methanol) fuels.
  • gaseous e.g. hydrogen, methane, etc
  • liquid e.g. methanol
  • the fuel cell of the present application for example allows the use of carbonaceous substrates which comprise heteroatoms and which could not be used in conventional fuel cells. It will be appreciated that the apparatus of the present invention facilitates the subsequent treatment of the resulting CO 2 product by sequestration and sulphur removal.
  • the oxidation reactor therefore provides an inlet for the carbonaceous substrate.
  • the carbonaceous substrate can be provided continuously while the fuel cell is in use or in a batch wise manner.
  • the carbonaceous substrate can be provided to the oxidation reactor continuously in a co-current or counter current flow with the dissolved oxygen.
  • the carbonaceous substrate is provided to the oxidation reactor continuously in a counter current flow with the dissolved oxygen.
  • Electrolyte e.g. YSZ: 2O 2 ⁇ (cathode) >2O 2 ⁇ (anode) (8)
  • the temperature of the electrochemical reactor and the oxidation reactor can be separately controlled and optimised. It will be appreciated that the optimum temperature of the reactors will depend on the melting point of the liquid and the integrity of the reactor compartments.
  • liquid preferably exists in a liquid form at a temperature above 400 0 C.
  • the liquid is preferably a molten metal or alloy in which the oxygen is dissolved.
  • the molten metal is preferably provided as a eutectic material.
  • the molten metal can be selected from one or more of Sn, Pb or Pb-Bi.
  • a particular example of a eutectic material for the present invention is Lead-Bismuth Eutectic (LBE).
  • the anode is a liquid, particularly a molten metal as defined above.
  • the liquid, e.g. the molten metal is provided as a solvent for the oxygen.
  • the amount of oxygen dissolved in the molten metal should preferably not exceed the oxygen solubility of the molten metal. If the dissolved oxygen solubility is exceeded, a metal oxide will form which can be used to oxidise the carbonaceous substrate. For example, if the dissolved oxygen solubility of the molten tin is exceeded then SnO 2 will form which itself could oxidise carbon.
  • the Sn-O phase diagram predicts that two liquids (Sn + SnO 2 ) should co-exist at > 1318 K. After depletion of the dissolved oxygen in the oxidation reaction, the liquid, e.g. the molten metal will then be returned to the electrochemical reactor for further oxygenation.
  • the electrolyte is preferably selected from one or more of ZrO 2 -Y 2 O 3 , yttrium stabilised zirconia and Ce 09 Gd O iOi 95 .
  • the cathode is preferably La 06 Sr 04 Co 02 Fe 0 8 O 3 or La 06 Sr 04 MnO 3 (LSM).
  • the solid carbonaceous substrate can be any material comprising carbon.
  • the solid carbonaceous substrate can be selected from one or more of coal, petroleum derived fuels, petroleum coke, natural gas, naphtha, low/high sulphur fuel oil, hydrocarbons including long chain hydrocarbons, such as methane, ethane, propane etc, acetylene black, furnace black, carbon black, carbon aerogels, graphite, charcoal, carbon-based polymers including plastics such as polyethylene, biomass, pitch, tar, asphalt, wood, waste carbon products etc.
  • the hydrogen content is oxidised to water and at higher temperatures (» 972 K) CO, rather than CO 2 .
  • the carbon monoxide in combination with the H 2 O can be reformed to syngas (CO + H 2 ).
  • This endothermic reforming reaction provides a means of controlling autothermicity in the oxidation reactor.
  • the second aspect of the invention provides a method of generating electricity from a solid carbonaceous substrate, comprising
  • the steps of forming the oxygen ions at a cathode, transporting the oxygen ions to an anode and dissolving the oxygen in a molten metal and the step of oxidising the carbonaceous fuel are carried out in separate reaction vessels.
  • the present invention therefore provides a method of generating electricity from a solid carbonaceous substrate, comprising
  • steps 1), 2) and 3) are carried out in a first reaction vessel and step 4) is carried out in a second reaction vessel.
  • steps 1), 2) and 3) are carried out in an electrochemical reactor and step 4) is carried out in an oxidation reactor as defined in the first aspect of the invention.
  • step 3) of the method of the second aspect involves dissolving the oxygen into a liquid anode, wherein said anode is preferably a molten metal or alloy.
  • the present invention therefore provides a method of generating electricity from a solid carbonaceous substrate, comprising 1) forming oxygen ions from an oxygen source at a cathode; 2) transporting the oxygen ions to an anode via an ionically conducting electrolyte;
  • steps 1), 2) and 3) are preferably carried out in a first reaction vessel and step 4) is preferably carried out in a second reaction vessel.
  • the resulting oxidised carbon species is preferably a carbon containing gas or a mixture of carbon containing gases, more preferably carbon dioxide.
  • Electrolyte e.g. YSZ: 2O 2 ⁇ (cathode) >2O 2 ⁇ (anode) (14) Anode: Ae ⁇ + 2[O ⁇ ⁇ 2O 2 ⁇ (15)
  • the method of the second aspect of the invention can be carried out at a temperature of 400 to 2000 0 C, preferably 400 to 1200 0 C.
  • the electrochemical reaction can be carried out at a temperature of 400 to 1200 0 C, depending on the combination of electrolyte, cathode and anode employed.
  • the oxidation reaction can preferably be carried out at a temperature of 400 to 1200 0 C, depending on the desired product gas composition.
  • the solid carbonaceous substrate can be any material comprising carbon. Improved oxidation of the carbonaceous substrate can be obtained when the substrate is provided as solid particulate matter with a high surface area.
  • the carbonaceous substrate can therefore be pretreated prior to oxidation to form particles of the substrate by for example, pyrolysis, partial oxidation, grinding, mechanical size reduction, etc.
  • the method of the second aspect therefore provides the step of converting the carbonaceous substrate into particulate material prior to its contact with the dissolved oxygen. It will be appreciated that the smaller the size of the particles, the more surface area is available for reaction with the dissolved oxygen.
  • the particles of the solid carbonaceous substrate are therefore preferably from 1 to 100,000 micrometres, more preferably 10 to 10,000 micrometres, alternatively 10 to 1000 micrometres or 100 to 1000 micrometres in diameter.
  • the solid carbonaceous substrate can additionally or alternatively be pretreated to modify the carbon/hydrogen ratio of the substrate, for example using high temperature pyrolysis. This pre-treatment will allow manipulation of the composition of the resulting oxidised carbon species. Hydrogen generated during the high temperature pyrolysis step can be collected and used for example as a fuel for fuel cells.
  • the CO 2 produced by the method of the second aspect can be further treated for example by sequestration and/or sulphur removal. Sequestration can be carried out by compression and condensation (wherein the pressure can be derived from the continuous evolution of CO 2 ). Alternatively, the CO 2 may be dissolved for example in DEA and separated through absorption.
  • the fuel cell and method of the present application provides a number of advantages over the use of fuel cells currently known in the art.
  • the fuel cell and method of the present invention provides improved efficiency (i.e. less CO 2 emitted per kW) compared with electrical power generation by convention fossil fuel combustion.
  • the generation of electricity from substrates such as coal and/or waste carbon products overcomes problems associated with the security and reliability of energy conversion as it allows the use of indigenous coal and/or waste carbon products.
  • the fuel cell and method of the present application further obviates problems of gasification and gaseous fuel purification associated with conventional fuel cells.
  • the third aspect of the invention provides a use of an electrochemical fuel cell of the first aspect of the invention for generating electricity from a carbonaceous substrate.
  • Figure. 1 shows a schematic of carbon-air fuel cell, coupled to a combustion reactor in which carbon particles are oxidised to CO 2 by dissolved oxygen in molten metal or alloy;
  • Figure 2 shows the predicted temperature dependences of Gibbs energy and enthalpy changes (line (a)), and reversible cell voltage (line (b)), for molten tin oxidation by oxygen, assuming the worst case of SnO 2 as the (unwanted) product, as the oxygen solubility (predicted as ca. 0.32 at.% at 1170 K and 1.6 at.% at 1320 K) in molten tin is exceeded; and
  • FIG 3. shows a further schematic of a fuel cell of the invention comprising an electrochemical reactor (1) and an oxidation reactor (6).
  • the electrochemical reactor comprises a cathode (2) and an anode (4) linked via an electrolyte (3).
  • Oxygen is provided to the electrochemical reactor via inlet (5).
  • the dissolved oxygen in the liquid anode is transported to the oxidation reactor (6) via an outlet (7) and passes over a bed (8).
  • Carbonaceous substrate is supplied to the bed via inlet (9) to flow counter current to the dissolved oxygen flow.
  • the resulting carbon dioxide is removed from the oxidation reactor via outlet (11) and the deplenished liquid anode is recycled to the electrochemical reactor and more specifically to the anode via outlet (10).
  • By-products, including ash are removed from the oxidation reactor via outlet (12).

Abstract

La présente invention concerne une pile à combustible électrochimique pour générer de l'électricité à partir d'un substrat carboné solide, comprenant un réacteur électrochimique pour la préparation d'oxygène dissous et un réacteur d'oxydation pour la réaction dudit oxygène dissous avec le substrat carboné solide. L'invention concerne en outre un procédé de génération d'électricité à partir d'un substrat carboné solide.
PCT/EP2008/055827 2007-05-14 2008-05-13 Pile à combustible pour une utilisation dans la génération d'électricité à partir d'un substrat carboné solide WO2008138923A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP08750259A EP2156500A1 (fr) 2007-05-14 2008-05-13 Pile à combustible pour une utilisation dans la génération d'électricité à partir d'un substrat carboné solide

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB0709244.8 2007-05-14
GBGB0709244.8A GB0709244D0 (en) 2007-05-14 2007-05-14 Fuel cells

Publications (1)

Publication Number Publication Date
WO2008138923A1 true WO2008138923A1 (fr) 2008-11-20

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EP (1) EP2156500A1 (fr)
GB (1) GB0709244D0 (fr)
WO (1) WO2008138923A1 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2023057383A1 (fr) 2021-10-07 2023-04-13 Sangle Ferriere Bruno Système de pile à combustible

Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4826740A (en) * 1986-09-15 1989-05-02 Bruno Costa Process for generating electrical energy by oxidation of a solid fuel in liquid metal
EP0333261A2 (fr) * 1988-03-14 1989-09-20 Bruno Costa Méthode et installation pour la production d'énergie électrique et de gaz pour des synthèses chimiques au moyen d'oxydation dans des bains métalliques fondus
US5376469A (en) * 1993-09-30 1994-12-27 The Board Of Trustees Of The Leland Stanford Junior University Direct electrochemical conversion of carbon to electrical energy in a high temperature fuel cell
WO1999045607A1 (fr) * 1998-03-03 1999-09-10 Celltech Power, Llc Groupe electrogene a carbone-oxygene
WO2003001617A2 (fr) * 2001-06-25 2003-01-03 Celltech Power, Inc. Arrangement de couches d'electrodes dans un dispositif electrochimique
US20060019132A1 (en) * 2004-05-19 2006-01-26 Lipilin Alexander S Liquid anode electrochemical cell
US20060257702A1 (en) * 2005-05-16 2006-11-16 Clean Coal Energy, Llc High temperature direct coal fuel cell

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4826740A (en) * 1986-09-15 1989-05-02 Bruno Costa Process for generating electrical energy by oxidation of a solid fuel in liquid metal
EP0333261A2 (fr) * 1988-03-14 1989-09-20 Bruno Costa Méthode et installation pour la production d'énergie électrique et de gaz pour des synthèses chimiques au moyen d'oxydation dans des bains métalliques fondus
US5376469A (en) * 1993-09-30 1994-12-27 The Board Of Trustees Of The Leland Stanford Junior University Direct electrochemical conversion of carbon to electrical energy in a high temperature fuel cell
WO1999045607A1 (fr) * 1998-03-03 1999-09-10 Celltech Power, Llc Groupe electrogene a carbone-oxygene
WO2003001617A2 (fr) * 2001-06-25 2003-01-03 Celltech Power, Inc. Arrangement de couches d'electrodes dans un dispositif electrochimique
US20060019132A1 (en) * 2004-05-19 2006-01-26 Lipilin Alexander S Liquid anode electrochemical cell
US20060257702A1 (en) * 2005-05-16 2006-11-16 Clean Coal Energy, Llc High temperature direct coal fuel cell

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2023057383A1 (fr) 2021-10-07 2023-04-13 Sangle Ferriere Bruno Système de pile à combustible
FR3128064A1 (fr) * 2021-10-07 2023-04-14 Bruno SANGLE-FERRIERE Système de pile à combustible

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Publication number Publication date
EP2156500A1 (fr) 2010-02-24
GB0709244D0 (en) 2007-06-20

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