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WO1990014694A1 - Cellule electrochimique muni d'un recipient a combustible - Google Patents

Cellule electrochimique muni d'un recipient a combustible Download PDF

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Publication number
WO1990014694A1
WO1990014694A1 PCT/SE1990/000319 SE9000319W WO9014694A1 WO 1990014694 A1 WO1990014694 A1 WO 1990014694A1 SE 9000319 W SE9000319 W SE 9000319W WO 9014694 A1 WO9014694 A1 WO 9014694A1
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WO
WIPO (PCT)
Prior art keywords
fuel
cell
chemoelectric
cell according
anode
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Ceased
Application number
PCT/SE1990/000319
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English (en)
Inventor
Olle LINDSTRÖM
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Olle Lindstrom AB
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Olle Lindstrom AB
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Filing date
Publication date
Application filed by Olle Lindstrom AB filed Critical Olle Lindstrom AB
Publication of WO1990014694A1 publication Critical patent/WO1990014694A1/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
    • H01M8/08—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
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2455—Grouping of fuel cells, e.g. stacking of fuel cells 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

  • Liquid fuels being considered as reactants for the cathode reaction in chemoelectric cells, have a high columbic activity.
  • the capacity density of methanol is as an example gravimetrically 5.02 kAh/kg and volumetrically 3.98 kAh /dm 3 .
  • Corresponding figures for zinc at 50 % initial porosity is 0.82 kAh/kg and 2.93 kAh/dm 3 .
  • Liquid fuels are furthermore easy to handle and store compared with for instance hydrogen.
  • Fuel cells for tractionary applications for direct or indirect use of liquid fuels in particular methanol have been subjected to strong development efforts. Carbon dioxide formed in the cold combustion process evaporates from cells with acid electrolyte and is fixed in cells with alkaline electrolyte which therefore are destroyed or consumed. For these reasons these development efforts have been concentrated on cells with acid electrolyte in spite of the fact that the performance at least initially for the corresponding alkaline systems is very much hihger than for the acid systems.
  • the present invention is primarily due to the need to eliminate this problem.
  • the invention is, however, not limited to chemoelectric cells in which carbondioxide is formed.
  • One embodiment is thus concerned with a cell for cold combustion of glycol in an alkaline cell with formation of another reaction product with acid properties like carbondioxide, that is oxalic acid which is also impairing the function of the alkaline electrolyte.
  • Second purpose is to broaden the field of application for these chemoelectric cells so as to make them suitable for light applications as so called consumer products competing with the small primary and secondary cells which are used in these applications for instance those of the standard size R6.
  • a third purpose is to make available a power source in particular for consumer applications with high energy density, with good environmental properties and with a high safety for the user with no risk for leakage, knallgas-explosions etc.
  • this invention satisfies these desiderata in a very efficient manner. It exhibits also other advantages as will be evident from the following description.
  • the spirit of the invention is surprisingly simple and it may in after sight look obvious. This could, however, not be the case since the elements which are combined in the invention have been known and available to the artisan during a very long time.
  • the characteristic feature of the invention is thus that it refers to a chemoelectric cell cold combustion of a fuel in an aqueous phase, the cell comprising an air cathode (2), an electrolyte and a fuel anode (4) characterized in that the air cathode is hydrophobic, that the electrolyte consists of an alkali hydroxide in aqueous solution contained in a micro-porous separator (3) and that at this part of the fuel anode (4) is disposed in direct contact with the separator (3) so as to cover said separator practically completely whereby the aqueous phase with the fuel contains a base for neutralization of acid reaction products formed during the cold combustion of the fuel, said aqueous phase being disposed in a container (5) which is separated from the separator (3) by the part of the fuel anode (4) which is covering the separator (3).
  • Figure 1 illustrates the principle.
  • Figure 2 shows the principle for an embodiment with a so called double-cell.
  • Figure 3 shows an embodiment with a larger fuel anode than the air cathode.
  • Figure 4 shows an embodiment for high powers.
  • Figure 5 shows finally in more detail the design of an single cell for glycol.
  • FIG. 1 illustrates the spirit of the invention.
  • the new cell has been given a shape with an exterior which reminds of a conventional primary cell with cylindrical design for instance a so called alkaline cell of the standard size R6.
  • the chemoelectric energy conversion is taking place in the "cell sandwich" (1) comprising the hydrophobic air cathode (2), the electrolyte layer which consists of an alkaline solution contained in a micro-porous separator (3) and the fuel anode (4).
  • the fuel anode (4) is in direct contact with the liquid in the fuel container (5).
  • the fuel is typically methanol in aqueous solution.
  • the solution also contains a base for reaction with carbon dioxide which is formed during the cold combustion of the methanol.
  • a suitable base is calcium oxide which is converted to calcium carbonate in the reaction with the formed carbon dioxide.
  • the fuel is in general water soluble but it may also be present as a stable emulsion in water.
  • the fuel is oxidized at the anode whereby electrons are given to the anode.
  • This is taking place in the container (5) and therefore the conditions for the cold combustion in the "cell sandwich" (1) are not disturbed by the products of the reaction.
  • Figure 1 shows furthermore how the positive air cathode (2) is disposed in contact with a current conductor (6) with holes (7) so as to permit ambient air to enter into the gas pores of the air electrode.
  • the current conductor (6) is also furnished with a pole-knob (8) in the same way as the conventional R6-cell.
  • the current conduction from the negative fuel anode is taking place by means of the conductor (9) which is connected to the pole-plate (10).
  • the cell is completely enclosed in an electrically insulating envelop (11) with the gables free for the pole-plate (10) and the current conductor (6) with the pole-knob (8).
  • Figure 1 is primarily intended to describe the principle for the invention it shows at the time how it is possible to shape this cell as for instance a conventional R6-cell to be used in the same way as such a cell.
  • the interior of the new cell differs most considerably from the established cell. Its interior is dominated by the fuel container (5) in the same way as for instance a cigarette lighter which is very much a gas container.
  • One end of the cigarette lighter is equiped with means for control combustion of the fuel contained in the gas container with ambient air.
  • Similarily one end of the chemoelectric cell according to the invention is equiped with means for controlled "cold combustion" of fuel contained in the fuel container for conversion to electrical energy instead of thermal energy.
  • Alkaline fuel cells for direct oxidation of for instance methanol have the fuel dissolved in the electrolyte arranged between the two electrodes.
  • Such fuel cell systems frequently are furnished with a separate tank for the main bulk of the fuel electrolyte mixture.
  • the fuel electrolyte mixture is circulating between the electrolyte spaces of the fuel cell and this tank.
  • the electrolyte has been carbonized it is replaced by fresh electrolyte.
  • the performance of the fuel cells deteriorates successively during the operation.
  • electrolyte and fuel are separated by the anode according to my invention.
  • the resistance in the electrolyte layer is therefore an order of magnitude smaller than with cells with fuel and electrolyte between the electrodes.
  • Hydroxyl ions are produced continuously at the cathode due to the reduction of the oxygen of the air. These hydroxyl ions migrate to the anode and are consumed there during the oxidation of the fuel. Therefore water soluble bases may also be used for the neutralization of the acid reaction products for instance soudium hydroxide since the carbonate ions do not diffuse through the fuel anode because of the opposite transport of hydroxyl ions in the electrolyte layer.
  • the invention is thus a surprising and a very simple solution to the problem of carbonatization occuring with methanol fuel thanks to the separation of the spaces for the electrolyte and the fuel. It is surprising that nobody else has arrived to this solution earlier inspite of the fact that there are some designs of direct methanol air fuel cells with acid electrolyte which exhibit in a sense a design simularity, see for instance US Patent 4,262,063. Carbon dioxide is evaporating from the acid electrolyte in this acid cell to the atmosphere.
  • a chemoelectric cell according to my invention may be conceived by replacing the acid electrolyte containing the methanol fuel with an alkaline fuel solution containing a base and a proton conducting membrane with an alkaline electrolyte layer contained in a microporous matrix.
  • Such a change give several times higher power density and makes it possible to produce completely sealed power sources to be used in consumer products.
  • the generation of free carbon dioxide with the acid cell does not permit a sealed cell design.
  • the cell sandwich can have many different appearences.
  • the new chemoelectric cell has in a preferred embodiment several things in common with the zinc/air cell.
  • the zinc/air cell is a hybride between a fuel cell of the alkaline type (AFC, Alkaline Fuel Cell) and an alkaline zinc cell.
  • AFC Alkaline Fuel Cell
  • the air electrode (2) and the electrolyte layer (3) can be designed in identically the same way as in a zinc/air cell, see for instance D. Linden, "Handbook of batteries and fuel cells", McGraw-Hill 1984, chap. 10.
  • the negative part of the new chemoelectric cell is, however, completely different.
  • the zinc electrode has been replaced by the fuel anode (4) and by a fuel solution.
  • a very large part of the inner volume of the new chemoelectric cell is taking up by active electrode material in the form of a liquid fuel.
  • the second electrode material, the oxygen of the air, is available in unlimited quantity.
  • the capacity of the cell is governed by the amount of fuel in the container (5). This will be exemplified with a comparison with the standard cell R6. Such a cell has a length of 4.8 cm and a diameter of 1.4 cm.
  • the inner volume in the container (5) disposed in an R6-cylinder gets a volume of 6 cm 3 which corresponds to 80 % of the total volume.
  • the capacity is 4.8 Ah for methanol concentration of 5-M. At the working voltage of 0.7 V this is equivalent to 3.4 Wh, that is a volumetric energy density of 460 Wh/dm 3 .
  • the volumetric energy density for zinc/manganese dioxide cells of different types is typically 150-300 Wh/dm 3 and rechargeable nickel/cadmium cells 75-90 Wh/dm 3 .
  • the volumetric energy density for the new cell is thus in the "battery range”.
  • the fuel solution may in this case besides 5-M CH 3 OH contain 9-M KOH or, as an alternative, 2-M KOH + 6-M CaO as a powder. In the former case produced CO 2 is neutralized to K 2 CO 3 , in the latter case to insoluble CaCO 3 . 6H 2 O.
  • the cell voltage is an important property in the relation between the power source and the power consumer.
  • Various primary cells based on the system zinc/manganese dioxide give open voltages of 1.5 V, the zinc/air cell 1.4 V and the rechargeable nickel/cadmium cell 1.2 V.
  • the open voltage for the chemoelectric cells according to the invention is on the level around 1 V or slight below depending on the actual reactant system.
  • Figure 2 shows a so called double cell which will match a zinc/manganese dioxide cell with respect to cell voltage.
  • the conductor (9) from the one fuel anode (4) is connected to the air cathode (12) of the other cell.
  • the fuel anode (13) of the other cell is connected to the pole-plate (10) by means of the conductor (14).
  • the pole-plate (10), which is perforated in the same way as the current conductor (6), is electrically insulated from the air electrode (12) with a layer of a porous polymer, for instance porous polyethylene (15).
  • the two cells have separate fuel containers (5) separated by the wall (16). (A common fuel container would cause internal short-circuit between the two fuel anodes).
  • the anode has in general higher polarization than the cathode.
  • Figure 3 shows an embodiment where the fuel anode has been elongated into the fuel container.
  • the cylindrical part of the anode (17) is essentially the same properties as the part of the anode (4) which is covering the separator (3).
  • Figure 4 shows a high power design of a single cell where a large part of the mantle surface of the cell is disposed for the electrode functions.
  • the cell sandwich (1) is here the mantle surface of the cell.
  • the air cathode (2) is connected to the current conductor (18) with the pole-knob (8).
  • the separator (3) is disposed as a layer between the cathode (2) and the fuel anode (4) which is connected to the pole-plate (10).
  • Insulating plastic rings (19) and (20) support and seal at the two gables of the cell.
  • a thin plastic net (21) furnishes space for supply of air from the holes (22) in the envelop of the cell (11). Powers increase with the factor of ten with this cell design compared to the design according to Figure 1 for cells of R6-size.
  • Bipolar cell assemblies may be used for connecting cells in series.
  • the bipolar collectors which are made of for instance graphite or nickel coated steel, are shaped so that they provide channels for the air on one side with the air being supplied by openings in the insulating envelop of the stack.
  • the opposite sides of the collectors face the associated fuel containers.
  • the ribbs are in electrical contact witht the fuel anode and the air cathode respectively.
  • This stack arrangement is based on the technology which has been developed for bipolar stacks for fuel cells of phosphoric acid type (PAFC) and molten carbonate type (MCFC) which is described in detail in Appleby, A.J. & Foulkes, F.R., "Fuel Cell Handbook", Van Nostrand Reinhold, N.Y., 1988.
  • PAFC phosphoric acid type
  • MCFC molten carbonate type
  • State of art anodes with noble metal catalysts may be used for the oxidation of the fuel in the alkaline environment.
  • Such catalysts are platinum on carbon support in the concentration of 10-20 % per weight or Raneynickel.
  • the catalyst may be bonded to a fine nickel wire mesh or graphite paper by state of art binders like sintered PTFE etc.
  • a suitable catalyst for the fuel anode is 20 % platinum black on active carbon in a concentration of 2 mg Pt/cm 2 .
  • the air cathode can be built in a similar way and contain a noble metal catalyst.
  • Alternatives to the noble metal catalyst are silver, perovskites and manganese dioxide.
  • a very suitable catalyst for the air cathode is described in the Swedish patent application 8801325-5.
  • the air electrode may also be identical to the air electrodes which are used in commercial zinc/air cells. Many different fuels can be used. Water soluble fuels like methyl alcohol, ethyl alcohol, s isopropyl alcohol, ethylene diglycol, water soluble carbons like saccharous constitute obvious candidates. The water soluble salts of the former acid are particularly reactive fuels. It is desired that the fuel should have a low vapour pressure and a not too high diffusion coefficient in order to reduce losses and transport through the electrolyte matrix to the air electrode. Ethylene diglycol is a particularly suitable fuel considering these requirements.
  • Calcium oxide is a given candidate for this function.
  • Calcium oxide is, as is well known, also used on an industrial scale for causticising of alkali carbonates to alkali hydroxide.
  • the technical effect can also be obtained by means of other bases which form insoluble carbonates, for instance oxides and hydroxides of for instance magnesium, zinc and barium just to take a few examples.
  • Calcined dolomite which is a mixture of calcium oxide and mangnesium oxide is particularly suitable for fixation of the carbon dioxide. These oxides are also used for elimination of carbon dixode in atmospheric air.
  • a fuel composition containing glycol, alkali hydroxide and calcium oxide, "lime", is very suitable for the chemoelectric cell according to the invention. Even if there are many other formulations within the frame of the invention glycol formulations are perhaps the best options of the many alternatives considering the complete map of properties. The invention will therefore be exemplified with this particular embodiment.
  • the embodiment of the new power source shown as an example in Figure 5 is related to the principle design according to Figure 1.
  • the cell sandwich (1) is contained in a plastic frame with a metal plate with holes as support and current conductor (23) for the fuel anode (4).
  • the supply of air to the hydrophobic air cathode is taking place through small air holes (7) and gas diffusion channels on the side of the current conductor (6) facing the air electrode which is shaped with a so called waffle pattern as described in the European patent 84107200-2.
  • the air cathode has to be hydrophobic since otherwise means would be necessary for pressurization of the surrounding air which would not be feasible in this case.
  • the electrolyte layer (3) consists of an asbestos sheet soaked with 7-N potassium hydroxide.
  • the contact between the fuel electrode (4) and the electrolyte layer (3) is secured with a compressible expansion element (24) according to the Swedish patent 7607608-2.
  • This element is at the same time serving as a current conductor for the fuel anode.
  • the conductor (9) is in this example an electrical wire which is connecting the element (24) with the pole-plate (10).
  • the protrusion (25) through the gable of the container (5) has been used for filling the fuel mixture and has then been sealed with for instance a fast curing epoxy resin.
  • the volume available for the fuel mixture is 6 cm 3 .
  • the fuel mixture for this R6-cell contains 3 g ethylene glycol, 2 g water, 4 g calcium oxide and 1 g potassium hydroxide.
  • the air electrode is manufactured according to the Swedish patent application 8801325-5.
  • the fuel anode contains 4 mg (PtPd)Bi/cm 2 which has been deposited galvanically on a nickel wire mesh (see Frensh patent 2336808).
  • the cell has an open voltage of about 1 V and can be charged at 0.7 V with 0.02 A during 500 hours.
  • the capacity is 10 Ah which corresponds to an energy density at 0.02 A of 460 Wh/kg or 900 Wh/dm 3 . This is well above what can be obtained with the corresponding manganese dioxide batteries.
  • the cell contains very small quantities of metal compounds compared to the consumer batteries and is therefore completely acceptable from an environmental point of view.
  • the cell may then deliver in the neighbourhood of 5 W at a cell voltage of 0.5 V.

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

Abstract

Les cellules électrochimiques pourvues d'électrolyte alcalin peuvent soumettre les combustibles liquides, tels que le méthanol et le glycol, à une ''combustion froide'' à des densités énergétiques relativement élevées. Néanmoins, les produits de réaction d'acide provenant du combustible dissous dans l'électrolyte neutralisent l'électrolyte de manière à entraver son fonctionnement. Selon l'invention, la cellule est pourvue d'un récipient séparé (5) pour la phase aqueuse contenant le combustible. Ladite phase aqueuse comprend également une base pour la neutralisation des products de réaction d'acide. La combustion froide s'effectue dans un ''sandwich de cellules'' (1) comprenant une cathode à air hydrophobe, un électrolyte constitué par un hydroxyde alcalin dans une solution aqueuse contenue dans un separateur microporeux (3), et l'anode du combustible (4). Une surface de l'anode (4) est en contact direct avec le séparateur (3), l'autre étant en contact direct avec la phase aqueuse contenue dans le récipient (5).
PCT/SE1990/000319 1989-05-16 1990-05-14 Cellule electrochimique muni d'un recipient a combustible Ceased WO1990014694A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
SE8901750-3 1989-05-16
SE8901750A SE8901750L (sv) 1989-05-16 1989-05-16 Kemoelektrisk cell med braenslebehaallare

Publications (1)

Publication Number Publication Date
WO1990014694A1 true WO1990014694A1 (fr) 1990-11-29

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SE (1) SE8901750L (fr)
WO (1) WO1990014694A1 (fr)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
ES2247928A1 (es) * 2004-06-03 2006-03-01 Celaya Emparanza Y Galdos, S.A. (Cegasa) Pila de consumo con tecnologia de pila de combustible.
EP1930976A1 (fr) * 2006-11-23 2008-06-11 Celaya, Emparanza Y Galdos S.A. (Cegasa) Batterie de consommateur comportant une pile à combustible
WO2011073621A1 (fr) * 2009-12-15 2011-06-23 Michael Alexander Priestnall Système de pile à combustible

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2047688A1 (de) * 1969-09-29 1971-04-01 Comp Generale Electricite Brennstoffzelle mit alkalischem Elektrolyten und insbesondere kohlen wasserstoffhaltigem Brennstoff
US4262063A (en) * 1978-05-26 1981-04-14 Hitachi, Ltd. Fuel cell using electrolyte-soluble fuels
EP0098376A2 (fr) * 1982-06-30 1984-01-18 International Business Machines Corporation Système électrolytique pour piles à combustible et autres cellules électrolytiques

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2047688A1 (de) * 1969-09-29 1971-04-01 Comp Generale Electricite Brennstoffzelle mit alkalischem Elektrolyten und insbesondere kohlen wasserstoffhaltigem Brennstoff
US4262063A (en) * 1978-05-26 1981-04-14 Hitachi, Ltd. Fuel cell using electrolyte-soluble fuels
EP0098376A2 (fr) * 1982-06-30 1984-01-18 International Business Machines Corporation Système électrolytique pour piles à combustible et autres cellules électrolytiques

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
ES2247928A1 (es) * 2004-06-03 2006-03-01 Celaya Emparanza Y Galdos, S.A. (Cegasa) Pila de consumo con tecnologia de pila de combustible.
ES2247928B1 (es) * 2004-06-03 2007-06-01 Celaya Emparanza Y Galdos, S.A. (Cegasa) Pila de consumo con tecnologia de pila de combustible.
EP1930976A1 (fr) * 2006-11-23 2008-06-11 Celaya, Emparanza Y Galdos S.A. (Cegasa) Batterie de consommateur comportant une pile à combustible
WO2011073621A1 (fr) * 2009-12-15 2011-06-23 Michael Alexander Priestnall Système de pile à combustible

Also Published As

Publication number Publication date
AU5733790A (en) 1990-12-18
SE8901750L (sv) 1990-11-17
SE8901750D0 (sv) 1989-05-16

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