WO2014111273A1 - Accumulateur d'énergie électrique rechargeable - Google Patents

Accumulateur d'énergie électrique rechargeable Download PDF

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Publication number
WO2014111273A1
WO2014111273A1 PCT/EP2014/050020 EP2014050020W WO2014111273A1 WO 2014111273 A1 WO2014111273 A1 WO 2014111273A1 EP 2014050020 W EP2014050020 W EP 2014050020W WO 2014111273 A1 WO2014111273 A1 WO 2014111273A1
Authority
WO
WIPO (PCT)
Prior art keywords
oxide
storage
electrical energy
wettable
rechargeable
Prior art date
Application number
PCT/EP2014/050020
Other languages
German (de)
English (en)
Inventor
Carsten Schuh
Thomas Soller
Original Assignee
Siemens Aktiengesellschaft
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 Siemens Aktiengesellschaft filed Critical Siemens Aktiengesellschaft
Publication of WO2014111273A1 publication Critical patent/WO2014111273A1/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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/362—Composites
    • H01M4/366—Composites as layered products
    • 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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • 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
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • 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
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • 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
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • 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

  • the invention relates to a rechargeable electrical energy storage, in particular a metal oxide-air energy storage, with at least one storage element for storing electrical energy, wherein the storage element comprises a reducible in the charging operation of the energy storage and oxidizable in the discharge operation of the energy storage memory material.
  • a new example of a storage option for excess electrical energy is the use of rechargeable electrical energy absorbers in the form of metal-air energy storage devices or metal-air batteries.
  • Energy stores are based essentially on the principle of electrochemical cells, d. H . the redox-based conversion of chemical into electrical energy or vice versa.
  • oxidizing agents for example oxygen ions obtained from atmospheric oxygen, are usually formed on a positively charged (air) electrode and are arranged by means of a between the positive and a negative electrode and for the oxidizing agent, ie. H . for example B.
  • the oxygen ions formed according to permeable electrolyte fed to the negative electrode. Conversely, it is possible that the oxygen ions migrate from the negative electrode through the electrolyte to the positive (air) electrode ⁇ charging process).
  • a reaction of the oxygen ions with a gaseous redox couple ("redox shuttle"), in particular a hydrogen Water vapor mixture, instead, wherein the oxygen taken up or released by the gaseous redox pair is transferred by diffusion of the redox couple to a porous or particulate, in the charging mode of the energy storage reducible and oxidizable in the discharge operation of the energy storage memory material of a storage element.
  • Generic energy storage require for operation high temperatures in the range between 600 and 900 ° C, since only at sufficiently high temperatures, a sufficient activity or ionic conductivity of the materials used is given.
  • the problem is that the mentioned high operating temperatures as well as the repeated oxidation or reduction of the storage material favor a successive coarsening of the storage material, in particular by grain growth and sintering, which causes a noticeable aging of the power output or power consumption of the energy store.
  • the oxidation mechanism of the storage material present on the shelf as metal (reduced form) or metal oxide (oxidized form) is often based primarily on cationic diffusion.
  • the oxidation mechanism based on cationic diffusion causes a mass flow of the storage material out of the storage element Towards an oxidation source and thus contributes to a continuous change in the structure of the memory element, which manifests itself in a deterioration of the charging and discharging characteristics and the useful capacity of the energy storage.
  • the invention is therefore based on the problem to provide an improved rechargeable electrical energy storage.
  • the problem is solved by a rechargeable electrical energy store of the type mentioned above, which is characterized in that the storage element comprises a material wettable at least in sections by the reduced form of the storage material.
  • the rechargeable electrical energy store according to the invention has in the storage element, in addition to the storage material, a material that is at least partially wettable even by the form of the storage material that is reduced during the charging operation of the energy store. Consequently, the reduced form of the storage material and the material wettable by it or their surfaces interact with one another in such a way that the reduced form of the storage material wets or wets the surface of the wettable material at least in sections, preferably completely. Accordingly, during the charging process of the energy storage, d. H. upon reduction of the storage material from its oxidized to its reduced form, wetting of the wettable material with the reduced form of the storage material.
  • the storage material is usually iron or iron oxide or a mixture of iron and iron oxide.
  • the reduced form of the storage material is here elementary iron.
  • the process of wetting can be at least partially reversible. If the energy storage is thus operated in the unloading operation, d. H. As the storage material transitions from its reduced to its oxidized form, the bond formed by the wetting of the wettable material with the reduced form of the storage material can be solved. If the energy store is then operated again in the loading mode, the storage material again assumes its reduced form and the processes described above can take place again.
  • a coating or coating of the surface of the wettable material with the reduced form of the storage material results.
  • core-shell particles are formed.
  • the wettable material wetted or surrounded by the reduced form of the storage material may be regarded as a core component and the reduced form of the storage material as a shell or shell component.
  • the good wettability of the wettable material with the reduced form of the storage material is reflected by a comparatively small wetting angle.
  • the wetting angle (hereinafter also referred to as the contact angle) between two solid phases is to be understood as meaning the angle which forms a drop-shaped structure of the wetting material on the surface of the material to be wetted in thermodynamic equilibrium.
  • the size of the wetting angle depends in particular on the strength of the interactions between the surfaces or the respective surface energies of the substances. The smaller the wetting angle, the stronger the interactions.
  • the wetting angle of the reduced form of the storage material on the surface of the wettable material is below 90 °, in particular in the range of 1 to 75 °, in particular 1 to 35 °.
  • the wettable material is expediently formed from a material which has an electrically conductive or semiconducting surface and thus with the electron gas of the reduced form of the storage material, which is present in particular as a metallic form of the storage material, forming attraction or. Adhesion forces can change. This requires the good wettability of the wettable material with the reduced form of the storage material.
  • the wettable material is preferably made of an oxide-ceramic material based on cerium oxide, chromium oxide, gadolinium oxide, copper oxide, manganese oxide, titanium oxide, or a rowskit compound, preferably of the general form (RE,
  • the wettable material may in principle be formed from all, letting to be wet of the reduced form of the memory material letting materials. The selection of the wettable material is therefore expediently to be selected as a function of the specific storage material in question and its reduced form.
  • the wettable material is preferably particulate.
  • the particle-shaped, d. H . Wettable material formed from individual particles and / or particle aggregates is distributed in the matrix of the storage element in which the storage material is also distributed.
  • the wettable material obtains a particle shape in that it is shaped as a coating on a particle
  • Carrier material is applied.
  • the carrier material can be formed, for example, from a particulate, oxide-ceramic material based on aluminum oxide, calcium oxide, lanthanum oxide, magnesium oxide, ioboxide, tantalum oxide, yttrium oxide, zirconium oxide or mixtures of the aforementioned. It is crucial that between the carrier material and the enveloping this or. enclosing wettable material a stable, especially chemical, bond is ensured.
  • the carrier material may have a porous structure.
  • the storage element additionally comprises a spacer material.
  • the spacer material is not or only slightly wettable due to the reduced form of the storage material.
  • the wetting angle 1 between the reduced shape of the storage material and the surface of the spacer material is typically greater than 90 °.
  • the spacer material serves to store the storage material, i. H . in particular the reduced form of the wettable material Storage material respectively the aforementioned, formed by the wetting of the wettable material with the reduced form of the storage material core-shell particles, to separate and a Agg1ome at ion or. Coarsening or Prevent sintering of the storage material.
  • the spacer material is expediently formed from an oxide-ceramic material based on zirconium oxide, yttrium oxide and / or yttrium compounds.
  • the ⁇ bstandshaltematerial is preferably present particulate.
  • the particulate d. H . from individual particles and / or
  • Particle aggregates formed, ⁇ bstandshaltem material is distributed in the matrix of the memory element, in which the memory material and the wettable material is distributed, included.
  • the spacer material that at least a part of the spacer material obtains a particle shape in that it is applied as a coating on a particulate carrier material.
  • the carrier material can be formed, for example, from a particulate, oxide-ceramic material based on aluminum oxide, calcium oxide, lanthanum oxide, magnesium oxide, niobium oxide, tantalum oxide, yttrium oxide, zirconium oxide or mixtures of the aforementioned.
  • it is crucial that between the carrier material and the enveloping this or. enclosing ⁇ bstandshaltem material is a stable, in particular chemical, binding geric.
  • the inertial material may also have a horrorant structure here.
  • the proportion of wettable material is advantageously in the range of 30 to 10 Vo1. -%, in particular in the range of 25 to 15 Vo1. -%. In exceptional cases, the proportion of wettable material may also be lower or higher.
  • the proportion of spoke material is in the range of 30 to 90 Vo1. -%, especially above 40 vol. -%, preferably above 50 Vo1. -%.
  • the proportion of memory material may also be lower or higher.
  • the proportion of storage material essentially determines the storage capacity of the storage element and is therefore generally to be set high.
  • spacer material is also contained in the storage element in addition to the storage material and the wettable material, its proportion is in the range from 10 to 30 Vo.sub.1. %, in particular in the range of 15 to 25 vol. -%.
  • the proportion of spacer material may also be lower or higher.
  • the total amount of wettable material and spacer material should total in the range of 2 to 40 Vo1. -%, in particular in the range of 5 to 15 Vo1. -% , lie .
  • a volume fraction of open porosity must also be present in the storage element, which is in the range of 10 to 50 Vo1. -%, preferably in the range of 25 to 40 Vo1. -% should be in order to ensure the unimpeded diffusion of the redox shuttle in the storage material.
  • Energy storage arrangement be summarized. This is done in particular by a stack-like arrangement of several Energypeieher one above the other. A corresponding energy storage arrangement can be referred to as a "stack".
  • FIG. 1 is a schematic diagram of an energy storage device according to an exemplary embodiment of the invention
  • FIG. 2 is an enlarged view of that in FIG. 1
  • Fig. 1 shows a P inzipda position of an energy storage 1 according to an exemplary embodiment of the invention.
  • the energy storage 1 is designed as a metal oxide-air Ene giespeieher. Based on Fig. 1, the structure or the mode of operation of the energy storage 1 will first be described.
  • Viewed from bottom to top of the Ene gie prayer 1 comprises an interconnector plate 2, the contact webs 3 has on its underside. Through the formed by the contact webs 3 comb-like structure of the interconnector plate 2 air channels 4 are formed.
  • de interconnector plate 2 At the top of de interconnector plate 2 is connected to the contact webs 3 of the Inte konnektorplatte 2 adjacent positive electrode 5, a trained in particular as a solid electrolyte electrolyte 6 and a negative electrode 7 at.
  • the positive electrode 5 may be referred to as the air electrode, the negative electrode 7 as the storage electrode.
  • Adjacent to the top of the negative electrode 7 is a storage element 8 for storing electrical energy.
  • an interconector plate 2 again connects.
  • the structure of the energy storage 1 is repeated.
  • Via a gas supply 9 an oxygen-containing process gas, in particular air, is supplied.
  • the oxygen contained in the process gas is converted into oxygen ions (O 2 ⁇ ions) and travels from the positive electrode 5 through the electrolyte 6 to the negative electrode 7.
  • the negative electrode 7 is connected via a redox couple in the form of a gaseous hydrogen-steam mixture
  • H2 / H2O mixture with a redox-active storage material 10, such as an iron-iron oxide mixture, having memory element 8 for storing electrical energy in combination.
  • a redox-active storage material 10 such as an iron-iron oxide mixture
  • the migrated through the electrolyte 6 oxygen ions are bound to the de negative electrode 7 in steam guided through the storage element 8 after the discharge.
  • the storage material 10 is oxidized or reduced, wherein the optionally necessary oxygen can be provided by serving as a redox couple hydrogen-water vapor mixture.
  • the mechanism of oxygen transport through a redox pair is called a shuttle mechanism.
  • Oxidation process in about the same resting voltage of about 1 V has, as serving as a redox couple hydrogen-steam mixture at a partial pressure ratio of 1, otherwise there is an increased resistance to the oxygen transport through the components of the redox couple, d. H . of the hydrogen-steam mixture.
  • the diffusion of the oxygen ions through the electrolyte 6 requires a Radiotempe nature of the energy storage device 1 600-900 "C.
  • temperatures of 600 to 900 ° C for optimum composition of the hydrogen-steam mixture in equilibrium with the storage material 10 are advantageous the high operating temperatures of the Energy storage 1 are all components of the energy storage device 1, ie in particular the electrodes 5, 7 and the electrolyte 6, as well as the storage element 8 exposed to high thermal loads.
  • FIG. 2 shows an enlarged view of the storage element 8 associated with the energy store 1 shown in FIG. 1.
  • the storage element 8 has a cuboid, porous storage element body.
  • the memory element 8 represents a matrix in which a storage material 10 which can be reduced during charging operation of the energy store 1 and oxidizable in the discharge operation of the energy store 1 is contained in the form of a particulate iron-iron oxide mixture.
  • the reduced form of the storage material 10 present in the charging operation of the energy store 1 is therefore elemental iron, which in the discharge operation of the energy store 1 present oxidized form of the storage material 10 consists of at least one iron oxide compound.
  • particulate storage material 10 is in the matrix a wettable by the reduced form of the memory material 10 material 11, which z. B. from a particulate oxide ceramic based on cerium oxide, gadolinium oxide, chromium oxide, copper oxide, manganese oxide, titanium oxide or a perovskite compound, preferably of the general form (RE,
  • the wettable material 11 in FIG. 2 is wetted with the storage material 10, that is to say the wettable material 11 in FIG. H .
  • the storage material 10 encloses the wettable material 11 to form so-called core-shell particles.
  • the wettable material 11 surrounded by the reduced shape of the storage material 10 as the core component ("core") and the reduced form of the storage material 10 as a shell or shell component
  • FIG. 2 shows the state of charge or charged state of the energy store 1.
  • the wetting of the wettable material 11 with the reduced shape of the storage material 10 is possible because the wetting angle between the reduced shape of the storage material 10 and the wettable material 11 is less than 90 °.
  • the wetting angle between the reduced shape of the storage material 10 and the wettable material 11 is in the range of 5 to 75 °.
  • the process of wetting the wettable material 11 with the storage material 10 in its reduced form may be reversible so that the bond formed by wetting the reduced form of the storage material 10 on the surface of the wettable material 11 in a discharge of the Energy storage 1 can solve.
  • the spacer material 12 is z. B. in the form of particles based on yttrium oxide or yttrium-containing oxidic compounds.
  • the spacer material 12 serves to prevent the formation of particle-particle contacts of the memory material 10 and thus a possible sintering at the high temperatures required for the operation of the energy store 1. Coarsening of the memory material 10 to prevent.
  • wetting of the spacer material 12 with the storage material 10 is neither in its reduced nor oxidized form against the wetting of the wettable material 11 by the storage ial 10 favors.
  • the wetting angle between the spacer material 12 and the memory material 10 is greater than 90 °.
  • the wettable material 11 differs from the spacer material 12 substantially in terms of their Benet tion angle relative to the memory material 10 and. its reduced form.
  • Both the wettable material 11 and the ⁇ bstandshalte- material 12 may be applied in addition to the described possibility that it is itself particulate or granular, as a coating on a particulate, porous carrier material.
  • the carrier material may, for.
  • Example be formed from an oxide ceramic material based on calcium oxide, magnesium oxide, zirconium oxide, aluminum oxide, lanthanum oxide, niobium oxide or tantalum oxide or mixtures of the above.
  • the proportion of memory material 10 in the matrix of the memory element 8 is z. In the range of 30 to 90 Vo1. -%, especially above 40 Vo1. -%, preferably above 50 vol. -%.
  • the total amount of wettable material 11 and spacer material 12 is in the range of 2 to 40 Vo1 in total. -%, in particular in the range of 5 to 15 Vo1. -% , lie .
  • a volume fraction of open porosity in Speicherelement 8 is also present in the range of 10 to 50 Vo1. -%, preferably in the range of 25 to 40 vol. -%, lies.

Abstract

L'invention concerne un accumulateur d'énergie électrique rechargeable (1), notamment un accumulateur d'énergie à oxyde métallique-air, comportant au moins un élément accumulateur (8) pour accumuler de l'énergie électrique, l'élément accumulateur (8) contenant un matériau accumulateur (10) pouvant être réduit en mode de charge de l'accumulateur d'énergie (1) et pouvant être oxydé en mode de décharge de l'accumulateur d'énergie (1), l'élément accumulateur (8) contenant un matériau (11) pouvant être mouillé au moins par endroits par la forme réduite du matériau accumulateur (10).
PCT/EP2014/050020 2013-01-16 2014-01-02 Accumulateur d'énergie électrique rechargeable WO2014111273A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102013200582.2 2013-01-16
DE102013200582.2A DE102013200582A1 (de) 2013-01-16 2013-01-16 Wiederaufladbarer elektrischer Energiespeicher

Publications (1)

Publication Number Publication Date
WO2014111273A1 true WO2014111273A1 (fr) 2014-07-24

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PCT/EP2014/050020 WO2014111273A1 (fr) 2013-01-16 2014-01-02 Accumulateur d'énergie électrique rechargeable

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DE (1) DE102013200582A1 (fr)
WO (1) WO2014111273A1 (fr)

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2003001617A2 (fr) * 2001-06-25 2003-01-03 Celltech Power, Inc. Arrangement de couches d'electrodes dans un dispositif electrochimique
EP1513214A1 (fr) * 2003-09-05 2005-03-09 Sulzer Hexis AG Pile à combustible haute température ayant une structure cermet stabilisée
US20120034520A1 (en) * 2010-08-09 2012-02-09 Chun Lu Self-sealed metal electrode for rechargeable oxide-ion battery cells
US20120058396A1 (en) * 2010-09-07 2012-03-08 Chun Lu Oxidation-resistant metal supported rechargeable oxide-ion battery cells and methods to produce the same
WO2012038312A1 (fr) * 2010-09-20 2012-03-29 Siemens Aktiengesellschaft Unité d'accumulation d'énergie rechargeable
DE102011017594A1 (de) * 2011-04-27 2012-10-31 Siemens Aktiengesellschaft Verfahren zur Herstellung eines porösen Körpers und Zelle einer wieder aufladbaren Oxidbatterie

Family Cites Families (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP3717085B2 (ja) * 1994-10-21 2005-11-16 キヤノン株式会社 二次電池用負極、該負極を有する二次電池及び電極の作製方法
DE102011004183A1 (de) * 2011-02-16 2012-08-16 Siemens Aktiengesellschaft Wiederaufladbare Energiespeichereinheit

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2003001617A2 (fr) * 2001-06-25 2003-01-03 Celltech Power, Inc. Arrangement de couches d'electrodes dans un dispositif electrochimique
EP1513214A1 (fr) * 2003-09-05 2005-03-09 Sulzer Hexis AG Pile à combustible haute température ayant une structure cermet stabilisée
US20120034520A1 (en) * 2010-08-09 2012-02-09 Chun Lu Self-sealed metal electrode for rechargeable oxide-ion battery cells
US20120058396A1 (en) * 2010-09-07 2012-03-08 Chun Lu Oxidation-resistant metal supported rechargeable oxide-ion battery cells and methods to produce the same
WO2012038312A1 (fr) * 2010-09-20 2012-03-29 Siemens Aktiengesellschaft Unité d'accumulation d'énergie rechargeable
DE102011017594A1 (de) * 2011-04-27 2012-10-31 Siemens Aktiengesellschaft Verfahren zur Herstellung eines porösen Körpers und Zelle einer wieder aufladbaren Oxidbatterie

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