WO2012106468A2 - Pile hybride au nickel-hydrure métallique/hydrogène faisant appel à un séparateur conducteur d'ions alcalins - Google Patents

Pile hybride au nickel-hydrure métallique/hydrogène faisant appel à un séparateur conducteur d'ions alcalins Download PDF

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Publication number
WO2012106468A2
WO2012106468A2 PCT/US2012/023541 US2012023541W WO2012106468A2 WO 2012106468 A2 WO2012106468 A2 WO 2012106468A2 US 2012023541 W US2012023541 W US 2012023541W WO 2012106468 A2 WO2012106468 A2 WO 2012106468A2
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WO
WIPO (PCT)
Prior art keywords
hydrogen
nickel
electrode
metal hydride
hybrid battery
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/US2012/023541
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English (en)
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WO2012106468A3 (fr
Inventor
Ashok Joshi
John Gordon
Sai Bhavaraju
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Ceramatec Inc
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Ceramatec Inc
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Filing date
Publication date
Priority claimed from US13/189,177 external-priority patent/US8722221B2/en
Application filed by Ceramatec Inc filed Critical Ceramatec Inc
Publication of WO2012106468A2 publication Critical patent/WO2012106468A2/fr
Publication of WO2012106468A3 publication Critical patent/WO2012106468A3/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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/24—Alkaline accumulators
    • H01M10/30—Nickel accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/431—Inorganic material
    • H01M50/434—Ceramics
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/34—Gastight accumulators
    • H01M10/345—Gastight metal hydride accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M12/00—Hybrid cells; Manufacture thereof
    • H01M12/08—Hybrid cells; Manufacture thereof composed of a half-cell of a fuel-cell type and a half-cell of the secondary-cell type
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/446—Composite material consisting of a mixture of organic and inorganic materials
    • 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
    • Y02E60/10—Energy storage using batteries

Definitions

  • This invention relates to a nickel-metal hydride/Hydrogen hybrid battery that includes a non-porous, alkali ion conducting separator.
  • Nickel-metal hydride storage batteries are widely used for the power sources of cordless electronic equipment, power tools, electric vehicles and the like.
  • Conventional nickel-metal hydride batteries are composed of a positive electrode containing nickel hydroxide, a negative electrode containing a hydrogen-absorbing metal alloy, a microporous separator interposed between the positive and negative electrodes, and an electrolyte.
  • Nickel hydrogen battery (Ni-H 2 ) is a choice battery in many aerospace applications, especially geo- synchronous (GEO) and low earth-orbit (LEO) satellites. Recently, nickel-hydrogen batteries have also been used in terrestrial applications. The difference with a nickel-metal hydride battery is the use of hydrogen in a pressurized cell of up to 1200 psi (82.7 bar).
  • the Ni-H 2 battery comprises a positive electrode containing nickel hydroxide, a negative hydrogen electrode utilizes a teflon-bonded platinum black catalyst, and a zirconia cloth separator. This battery has a long cycle life, high specific energy, high power density, and also exhibits tolerance for overcharge.
  • Self-discharge is a phenomenon in many rechargeable batteries in which internal chemical reactions reduce the stored charge of the battery without any connection between the electrodes. Self-discharge decreases the shelf-life of batteries and causes them to have less charge than expected when actually put to use. How fast self-discharge in a battery occurs is dependent on the type of battery and temperature. Nickel-based batteries typically are significantly affected by self-discharge (nickel cadmium, 15-20% per month; nickel metal hydride, 30% per month; nickel hydrogen proportional to hydrogen pressure). Self-discharge is a chemical reaction and tends to occur more quickly at higher temperatures. Storing batteries at lower temperatures may reduce the rate of self-discharge and preserve the initial energy stored in the battery.
  • a nickel-metal hydride (hydrogen) hybrid battery that contains a positive electrode containing nickel hydroxide and a negative electrode containing a reversible hydrogen electrode.
  • the negative electrode is a combination electrode containing a hydrogen storage alloy electrode.
  • the battery also contains a separator having a substantially non-porous alkali ion conducting material disposed between the positive electrode and the negative electrode.
  • the method includes the steps of applying an electric charging potential to the positive and negative electrodes to cause the following reaction to occur at the positive electrode:
  • H 2 0 + e " + Me + ⁇ l/2H 2 + MeOH M in the forgoing reactions may be a hydrogen absorbing alloy, H a may be absorbed hydrogen, and Me may be an alkali metal.
  • the method may also include the step of conducting Me + ions across the alkali ion conducting separator from the positive electrode to the negative electrode.
  • the positive electrode is the electrode bearing a positive charge on discharge and the negative electrode bears a negative charge on discharge.
  • a method of discharging a nickel-metal (hydrogen) hybrid battery having a positive electrode containing nickel hydroxide, a combination negative electrode containing a hydrogen storage alloy electrode and a reversible hydrogen electrode, an alkaline electrolyte, and a separator comprising a substantially non-porous alkali ion conducting material.
  • the method includes the step of generating an electric potential between the positive and negative electrodes due in part to the following reaction occurring at the positive electrode:
  • M is a hydrogen absorbing alloy
  • 3 ⁇ 4 is absorbed hydrogen
  • Me is an alkali metal.
  • the method includes the step of conducting Me + ions across the alkali ion conducting separator from the negative electrode to the positive electrode.
  • Figure 1 is a schematic representation of one embodiment of a Ni-MH/H 2 hybrid battery within the scope of the invention.
  • Figure 2 is a schematic representation of another embodiment of a Ni-MH/H 2 hybrid battery within the scope of the invention.
  • battery includes a positive nickel hydroxide electrode, a negative electrode, and an alkali ion conducting separator.
  • the battery also includes an alkaline electrolyte, such as an alkali metal hydroxide.
  • the electrolyte may contain other minor constituents to enhance cell performance.
  • the alkaline electrolytes may include by way of non-limiting example, sodium hydroxide, lithium hydroxide, sodium carbonate, lithium carbonate, and the like. In one embodiment, alkaline electrolytes may be positioned on either side of the separator and may be different from one another.
  • the substantially non-porous nature of the separator allows for different electrolytes having different enhancers or constituents to be used on one side of the separator without effecting electrode performance on the other side of separator.
  • different alkaline electrolytes having different alkalinities may be either side of the separator.
  • the positive electrode may comprise nickel hydroxide (Ni(OH) 2 ) or other materials used in conventional nickel-metal hydride batteries.
  • the positive electrode may be a pasted or sintered-type material.
  • the negative electrode in the present invention may contain a reversible hydrogen electrode.
  • the negative electrode is a combination of MH and H 2 electrodes, wherein different charge/discharge reactions happen at the respective electrodes.
  • Figure 1 shows a combination cathode.
  • the MH cathode is same as or similar to traditional Ni-MH battery cathode and the hydrogen cathode is a gas diffusion type of cathode.
  • the MH negative electrode may comprise a hydrogen-absorbing alloy.
  • a hydrogen-absorbing alloy Such alloys are known in the art. Examples of early hydrogen-absorbing alloys include NiFe, Mg 2 Ni, and LaNis. These hydrogen-absorbing alloys combine metal (A) whose hydrides generate heat exothermically with metal (B) whose hydrides generate heat endothermically to produce the suitable binding energy so that hydrogen can be absorbed and released at or around normal temperature and pressure levels. Depending on how metals A and B are combined, the alloys are classified into the following types: AB (TiFe, etc.), AB 2 (ZnMn 2 , etc.), AB 5 (LaNi 5 , etc.) and A 2 B (Mg 2 Ni, etc.).
  • the reversible hydrogen electrode comprises a catalyst comprising platinum dispersed on a carbon in the form of a gas diffusion electrode.
  • the catalyst may be a platinum-type electro catalyst.
  • Gas diffusion electrodes are used in chlor-alkali electrolysis, metal-air batteries, and fuel cells.
  • the reversible hydrogen may be a gas diffusion electrode that interfaces with an alkaline electrolyte and a gaseous phase for electrochemical oxidation of hydrogen, the gas diffusion electrode comprising at least one reaction layer having dispersed therein a platinum-type catalyst, wherein the reaction layer is in fluid communication with the alkaline electrolyte and wherein the gas diffusion layer is in fluid communication with a gas comprising hydrogen.
  • a gas diffusion electrode has a multilayer structure composed of a gas diffusion layer, a reaction layer, and a current collector for electrical connection. Gas phase hydrogen is exposed to the gas diffusion layer.
  • the reaction layer resides between the gas diffusion layer and the electrolyte. After passing through the gas diffusion layer, hydrogen is consumed through a reduction reaction (on discharge) on an hydrogen reduction catalyst in the reaction layer.
  • the gas diffusion layer is required to allow the hydrogen to pass there through rapidly and to diffuse uniformly into the entire reaction layer.
  • the gas diffusion layer is also required to prevent the electrolyte from permeating to the gas phase.
  • the gas diffusion layer is comprised of a material formed of carbon particles bonded to each other with a material, such as polytetrafluoroethylene, having high water repellent properties.
  • the gas diffusion layer must also conduct electrons from the current collector to the reaction layer.
  • the reaction layer contains uniformly dispersed hydrogen reduction catalyst particles in electronic continuity with the gas diffusion layer and current collector.
  • a large interface area is formed among the oxygen, electrolyte, electrons, and the oxygen reduction catalyst.
  • the current collector may be, for example, a wire mesh or a foam material, which is composed of nickel, silver, or the like.
  • Figure 1 shows that the negative electrode is made by placing the reversible hydrogen electrode adjacent to the hydrogen storage alloy electrode such that the reaction layer of the reversible hydrogen electrode is facing the hydrogen storage alloy electrode and the gas diffusion layer is facing the hydrogen gas.
  • Figure 2 shows a second embodiment where the hydrogen absorbing alloy electrode material is combined with the reversible hydrogen electrode material to form the combination negative electrode.
  • One way to form the combination negative electrode is to mix hydrogen absorbing alloy electrode material (mischmetal) with the platinum black catalyst (for reversible hydrogen reaction) and the alkaline electrolyte to form the combination negative electrode or anode as a unitary component.
  • the platinum black and/or the alkaline electrolyte may be dispersed on the hydrogen absorbing alloy electrode material (mischmetal) itself.
  • the combination negative electrode comprises hydrogen storage alloy material, an alkaline electrolyte, and the reaction layer material of the reversible hydrogen electrode.
  • the combination negative electrode includes the hydrogen storage alloy material, the alkaline electrolyte and the materials from both gas diffusion and reaction layers of the reversible hydrogen electrode mixed and formed into a single component.
  • Another way to form the combination negative electrode is to mix hydrogen absorbing alloy electrode material (mischmetal) with the reaction layer material of the gas diffusion electrode (for reversible hydrogen reaction) and the alkaline electrolyte to form the combined anode.
  • the mixtures or combinations of these embodiments may be homogeneous or nonhomogeneous.
  • the hydrogen storage alloy electrode reversibly absorbs hydrogen.
  • the terms hydrogen storage alloy electrode and hydrogen absorbing alloy electrode may be used interchangeably herein throughout as context permits.
  • Negative electrode M + H 2 0 + e " + Na + ⁇ MH ab + NaOH
  • Negative electrode H 2 0 + e " + Na + ⁇ 1/2H 2 + NaOH
  • M is a hydrogen absorbing alloy and H a is absorbed hydrogen.
  • the reversible hydrogen anode oxidizes hydrogen to water during charge and reduces water back to hydrogen during discharge.
  • the capacity distribution between the two negative electrodes may be adjusted so that the either of the charge/discharge reactions for Ni-MH or Ni-H 2 are predominant. This means that one of the negative electrode possesses a greater capacity than the other. It may be that one of the negative electrode will reach full capacity first as the cell is charged/discharged before the other one.
  • the hydrogen storage alloy electrode and the reversible hydrogen electrode have different charge storage capacities.
  • a nickel-metal hydride (hydrogen) hybrid battery that contains an alkali ion conducting separator configured to selectively transport alkali ions.
  • the nickel-metal hydride (hydrogen) combination battery is structurally similar to conventional nickel-metal hydride and nickel-hydrogen batteries and contains a positive electrode and a negative electrode.
  • an alkali ion conducting separator is disposed between the positive and negative electrodes.
  • the separator may be substantially non-porous.
  • the separator in one embodiment is an alkali ion conducting solid electrolyte configured to selectively transport alkali ions. It may be a specific alkali ion conductor.
  • the separator may be a solid MeSICON (Metal Super Ion CONducting) material, where Me is Na, K, Li or a combination thereof.
  • the alkali ion conducting separator may comprise a material having the formula Mei +x Zr 2 Si x P 3 _ x Oi2 where 0 ⁇ x ⁇ 3, and where Me is Na, K, Li or a combination thereof.
  • alkali ion conducting solid electrolytes may comprise a material having the formula MesRL ⁇ O ⁇ where Me is Na, K, Li or combinations thereof, and where RE is Y, Nd, Dy, Sm, or any mixture thereof.
  • the alkali ion conducting separator may comprise a non- stoichiometric alkali-deficient material having the formula (Me5RESi40i2)i-5(RE2C>3.2SiC>2)5, where Me is Na, K, Li, or a combination thereof, where RE is Nd, Dy, Sm, or any mixture thereof, and where ⁇ is the measure of deviation from stoichiometry.
  • the separator comprises a material having the formula Nai +x 3 ⁇ 4Si x P 3 - x Oi2 where 0 ⁇ x ⁇ 3.
  • the alkali ion conducting separator may also be beta- alumina.
  • the alkali ion conducting separator may be configured in the form of a monolithic flat plate, a monolithic tube, a monolithic honeycomb, or supported structures of the foregoing.
  • the alkali ion conducting separator may be a flexible sheet of the polymer configured in various forms applicable to the intended application.
  • the alkali ion conducting separator may be a flexible sheet composed of a mixture of polymer and ceramic and configured in a variety of forms.
  • the alkali ion conducting separator may be configured as a layered alkali ion conducting ceramic-polymer composite membrane comprising alkali ion selective polymers layered on alkali ion conducting ceramic solid electrolyte materials.
  • the current carrying species in the electrolyte are exclusively alkali metal ions.
  • concentrations of the electrolyte change at both electrodes during battery operation because the non porous separator prevents mixing of electrolyte from both the compartments. This advantageously prevents transport of unwanted species from one electrode to the other and substantially eliminates capacity loss and self discharge.
  • the separator is a substantially non-porous ceramic separator material.
  • the substantially non- porous ceramic separator material may include pockets of porosity, but it should not have "through-porosity.” "Substantially non-porous" in some embodiments, means less than or equal to 5% porosity.
  • the substantially non-porous separator is preferably hermetic or gas- impermeable.
  • the substantially non-porous separator used within the scope of the present invention may possess a trace amount of through porosity and/or gas permeability.
  • the term substantially non-porous is intended to differentiate the prior art separators that are substantially porous.
  • the separator conducts alkali ions, but is substantially impermeable to hydrogen.
  • substantially impermeable to hydrogen means that the separator is greater than or equal to 95% impermeable to hydrogen.
  • self-discharge of the nickel-metal hydride and nickel-hydrogen batteries may be substantially reduced or eliminated by preventing hydrogen from passing from the negative electrode to the positive electrode.
  • the solid electrolyte separator being non porous prevents any hydrogen transport to the positive electrode while the polymer separator will allow some diffusion of hydrogen although lower than a microporous separator commonly used in the prior art.
  • the Ni-MH/H 2 hybrid battery within the scope of the present invention can be stored and used at higher temperature than the prior art because of the minimal self discharge.
  • the nickel-metal hydride battery may be operated at temperatures from about -40 °C to about 120°C.
  • a method of charging a nickel-metal hydride (hydrogen) hybrid battery having a positive electrode containing nickel hydroxide, a combination negative electrode containing a hydrogen storage alloy electrode and a reversible hydrogen electrode, an alkaline electrolyte, and a separator comprising a substantially non-porous alkali ion conducting material includes the steps of applying an electric charging potential to the positive and negative electrodes to cause the following reaction to occur at the positive electrode:
  • M in the forgoing reactions may be a hydrogen absorbing alloy
  • H ab may be absorbed hydrogen
  • Me may be an alkali metal
  • the method may also include the step of conducting Me + ions across the alkali ion conducting separator from the positive electrode to the negative electrode.
  • the positive electrode is the electrode bearing a positive charge on discharge and the negative electrode bears a negative charge on discharge.
  • a method of discharging a nickel-metal (hydrogen) hybrid battery having a positive electrode containing nickel hydroxide, a combination negative electrode containing a hydrogen storage alloy electrode and a reversible hydrogen electrode, an alkaline electrolyte, and a separator comprising a substantially non-porous alkali ion conducting material includes the step of generating an electric potential between the positive and negative electrodes due in part to the following reaction occurring at the positive electrode:
  • M is a hydrogen absorbing alloy
  • 3 ⁇ 4 is absorbed hydrogen
  • Me is an alkali metal.
  • the method includes the step of conducting Me + ions across the alkali ion conducting separator from the negative electrode to the positive electrode.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Inorganic Chemistry (AREA)
  • Ceramic Engineering (AREA)
  • Composite Materials (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)

Abstract

La présente invention concerne un accumulateur hybride au nickel-hydrure métallique (hydrogène) comprenant une électrode positive contenant de l'hydroxyde de nickel, une électrode négative combinée comportant une électrode à base d'un alliage de stockage d'hydrogène et une électrode réversible à hydrogène, un électrolyte alcalin et un séparateur conducteur d'alcalin disposé entre l'électrode positive et l'électrode négative. Le séparateur conducteur d'alcalin peut être un matériau conducteur d'ions essentiellement non poreux, l'alcalin conduit étant Na, K ou Li. L'invention concerne également un procédé de chargement et de déchargement de ladite pile hybride.
PCT/US2012/023541 2011-02-01 2012-02-01 Pile hybride au nickel-hydrure métallique/hydrogène faisant appel à un séparateur conducteur d'ions alcalins Ceased WO2012106468A2 (fr)

Applications Claiming Priority (6)

Application Number Priority Date Filing Date Title
US201161438328P 2011-02-01 2011-02-01
US61/438,328 2011-02-01
US13/189,177 US8722221B2 (en) 2007-11-26 2011-07-22 Method of discharging a nickel-metal hydride battery
US13/189,177 2011-07-22
US13/189,176 2011-07-22
US13/189,176 US8159192B2 (en) 2007-11-26 2011-07-22 Method for charging a nickel-metal hydride battery

Publications (2)

Publication Number Publication Date
WO2012106468A2 true WO2012106468A2 (fr) 2012-08-09
WO2012106468A3 WO2012106468A3 (fr) 2012-11-01

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9343735B2 (en) 2014-04-14 2016-05-17 Ovonic Battery Company, Inc. Shared electrode hybrid battery-fuel cell system

Family Cites Families (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2655810B2 (ja) * 1994-04-08 1997-09-24 工業技術院長 アルカリ二次電池及び触媒性電極体の製造法
US7727662B2 (en) * 2003-04-01 2010-06-01 Ovonic Battery Company, Inc. Low temperature alkaline fuel cell
US7029600B2 (en) * 2003-09-10 2006-04-18 Ovonie Fuel Cell Llc High capacity hydrogen storage material based on catalyzed alanates
US8012621B2 (en) * 2007-11-26 2011-09-06 Ceramatec, Inc. Nickel-metal hydride battery using alkali ion conducting separator

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9343735B2 (en) 2014-04-14 2016-05-17 Ovonic Battery Company, Inc. Shared electrode hybrid battery-fuel cell system

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Publication number Publication date
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