WO2003030282A2 - Couche electriquement conductrice d'une electrode positive - Google Patents

Couche electriquement conductrice d'une electrode positive Download PDF

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Publication number
WO2003030282A2
WO2003030282A2 PCT/AT2002/000280 AT0200280W WO03030282A2 WO 2003030282 A2 WO2003030282 A2 WO 2003030282A2 AT 0200280 W AT0200280 W AT 0200280W WO 03030282 A2 WO03030282 A2 WO 03030282A2
Authority
WO
WIPO (PCT)
Prior art keywords
electrically conductive
conducting layer
flexible current
layer according
conductive coating
Prior art date
Application number
PCT/AT2002/000280
Other languages
German (de)
English (en)
Other versions
WO2003030282A3 (fr
Inventor
Martha Maly-Schreiber
Adam Whitehead
Original Assignee
Funktionswerkstoffe Forschungs- Und Entwicklungs Gmbh
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 Funktionswerkstoffe Forschungs- Und Entwicklungs Gmbh filed Critical Funktionswerkstoffe Forschungs- Und Entwicklungs Gmbh
Priority to AU2002340614A priority Critical patent/AU2002340614A1/en
Publication of WO2003030282A2 publication Critical patent/WO2003030282A2/fr
Publication of WO2003030282A3 publication Critical patent/WO2003030282A3/fr

Links

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
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/665—Composites
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/665—Composites
    • H01M4/667—Composites in the form of layers, e.g. coatings
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/668—Composites of electroconductive material and synthetic resins
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/72—Grids
    • H01M4/74—Meshes or woven material; Expanded metal
    • H01M4/747—Woven material
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/80—Porous plates, e.g. sintered carriers
    • H01M4/806—Nonwoven fibrous fabric containing only fibres
    • 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
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • 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
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/028—Positive electrodes
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/661—Metal or alloys, e.g. alloy coatings
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/663—Selection of materials containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres
    • 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 flexible current-conducting layer of a flat positive electrode of an alkali or alkali ion battery, in particular a Li or Li ion battery, consisting of a carrier with an at least partially electrically coated surface. Furthermore, the invention also relates to a method for producing such a current-conducting layer.
  • Primary batteries which receive the energy through the manufacturing process and cannot be recharged because the electrolyte decomposes the negative pole, have been known for a long time and are used for a wide variety of applications.
  • primary Li cells and primary Li-ion cells are mainly used in small portable electronic devices, such as watches, hearing aids, cameras and the like, owing to their high gravimetric and volumetric energy density.
  • Secondary batteries which receive the energy only after production by formatting or charging and represent reversible systems that are reversible in their charging / discharging behavior with regard to both their electrochemistry and the structure of their electrodes, have only slowly become available to them in recent years Primary batteries coming up, so far always comparably lower gravimetric and volumetric energy densities also used for small, portable electronic devices of the type mentioned, since they can usually be recharged in the range of a thousand times and more often and are therefore, in spite of the initially higher costs, altogether much cheaper than primary batteries. Secondary batteries can also contain alkali metals, alkali alloys or alkali ions (such as in particular lithium).
  • the positive electroactive material of alkaline batteries or alkaline ion batteries can consist of various compounds which react with the alkali metal or lithium to provide an acceptable voltage - see see for example J. Desilvestro and O. Haas, J. Electrochem. Soc, 137 (1), 5C (1990) or S. Megahed, J. Power Sources, 51, 79 (1994) or M. Winter, JO Besenhard, ME Spahr and P. Noväk, Adv. Mater., 10 (10 ), 725 (1998).
  • the reactions taking place on the positive and negative electrodes must, as mentioned, be at least largely reversible.
  • positive electrode materials such as LiMnO 2 , LiNiO 2 , LiCoO 2 and Li The like is becoming increasingly important.
  • Such positive electrodes reversibly store lithium at 4.2 V compared to Li / Li + .
  • experiments with positive electrodes with even higher positive potentials are already being carried out in research and development.
  • cathodes are produced by attaching electroactive material in powder form with suitable additives which increase the conductivity (for example carbon black, graphite powder, metal powder and the like) by means of a polymer binder (for example PVDF, EPDM, PTFE and the like) on an electrical conductor.
  • suitable additives for example carbon black, graphite powder, metal powder and the like
  • a polymer binder for example PVDF, EPDM, PTFE and the like
  • the current conductor nowadays usually consists of an aluminum foil, since only a few materials are stable at such electrode voltages.
  • these include, for example, Au, Ti, Mo, W, Pt or stainless steel of certain types. Au and Pt are too expensive for common uses and the other examples mentioned are not suitable for simple application in a sufficient layer thickness (for example from aqueous solutions).
  • the coating of layer-wise and / or locally processed with different weave density, also used as a current-conducting layer, polymer materials with different metal coatings and other conductive substances, such as carbon, is known, but it is specifically about locally different storage densities of the electroactive material including any additives and the coating applied to the conductivity on the non-conductive plastic threads of the polymer fabric consists only of the known materials according to the prior art, which have already been mentioned above.
  • the object of the present invention is to improve a flexible current-conducting layer of the type mentioned at the outset in such a way that the disadvantages mentioned are avoided and in particular that it is an easy-to-install, inexpensive electrically conductive layer Coating for the surface of the support can be specified, which is particularly stable even at high electrode potentials (for example in the range of 4 V and above against Li / Li + ).
  • the actual cell voltage can also be ⁇ 3.5 V, for example, while the positive electrode is nevertheless at a correspondingly high potential compared to, for example, Li / Li + .
  • a negative electrode that works at a potential> 1 V compared to Li / Li + (for example, some called “high capacity carbons") and this is used together with a LiMn 2 O 4 cathode (with about 4 to 4.2 V compared to Li / Li + ), the cell voltage is less than 3.2 V compared to Li / Li + - Nevertheless, the potential prevailing at the positive electrode is above 4 V, which in the manner described makes difficulties with the current-conducting layers according to the prior art.
  • the above-mentioned object is achieved in the case of a current-conducting layer of the type mentioned in the introduction in that the electrically conductive coating of the surface of the carrier essentially consists of an alloy of the composition NiM y P ⁇ - with: y ⁇ 0.3
  • M consists of the group: Mo, W, Cr, V, Sn, Co. This alloy can also contain inevitable impurities in trace form during production, without significant effects on the positive behavior being ascertainable.
  • Ni, Co, Ag and most other metallic elements show strong ones Oxidation currents at high potentials compared to Li / Li + in non-aqueous electrolytes. In principle, these currents can result from the oxidation of the electrolytes or the oxidation of the metal.
  • Electrodes made of aluminum foils are stable in a wide variety of Li-battery electrolytes, since there is a very thin oxide film on the aluminum surface. The thin oxide film is thick enough around one Preventing further oxidation of the aluminum is insoluble in the electrolyte and does not require an excessively high additional electrical resistance.
  • Some types of stainless steel are highly stable, but pure iron and pure chrome are relatively unstable.
  • the stainless steel apparently also forms a protective layer in the electrolyte by partially dissolving the more soluble components and reacting them with the electrolyte (the reaction of stainless steel with water typically leaves a chromium and oxygen-rich surface layer). Accordingly, the introduction of the phosphorus portion described into the alloy can obviously promote the corrosion resistance by forming a similar “passivation layer” at elevated potentials.
  • a low current flow can be expected in accordance with the solution of some nickel on the surface and oxidation of the remaining phosphorus, according to which the layer of oxidized phosphorus or the oxidized phosphorus-nickel layer on the surface is much more resistant to further oxidation than the underlying alloy, which prevents further reaction with the electrolyte mentioned elements such as W and Mo, which can also form or support such a passivation layer.
  • This passivation process is also favored by the stability of W and Mo, for example, at high potentials (the pure metals are reactive and cannot be obtained from aqueous solution) en coated, but are easily passivated - similar to aluminum - in the described manner).
  • At least one further conductive layer preferably made of graphite, conductive carbon black or another carbon compound or of Au or Pt, is arranged between the carrier surface and the electrically conductive coating.
  • These layers serve mainly to facilitate the production or to improve and simplify the actual coating and can be applied in a very thin form as a starting layer in a variety of suitable ways.
  • This starting layer should also be stable with respect to the potentials to be expected, so that damage to the actual conductive layer above it cannot lead to oxidation and / or dissolution of the starting layer.
  • a further cover layer made of non-porous carbon is applied over the electrically conductive coating, which offers an additional protective function - after the actual power conduction takes place in the alloy layer, this carbon layer is not thick and actual closed critical.
  • the actual carrier consists of a three-dimensionally woven or knitted polymer material, the fibers of which have an electrically conductive coating (as is known per se in general form from AT 408.288 B mentioned at the beginning).
  • the woven threads of this polymeric material preferably consist of fibers of a polymer from the following group: polyester, silicone rubber, polyethylene, polypropylene, ethylene-tetrafluoroethylene copolymer, polytetrafluoroethylene len and polyvinylidene fluoride. This results in a flexible, particularly light, flat support which has an advantageous large surface area with easy penetrability for the electrolyte or other electroactive materials and additives.
  • Such materials are inexpensive to manufacture and can be cut into various shapes and sizes without any problems, so that the electrodes can be used for a wide variety of batteries.
  • so-called randomly woven mats non-woven fiber fabrics made of polymer fibers of random orientation or thin polymer films with perforations or similar flat structures can also be used for this purpose, which also applies, for example, to the use of such current-conducting layers for extremely thin, flat batteries tailored to the respective application.
  • the method according to the invention which is particularly advantageous for producing a flexible current-conducting layer of the type described above is characterized in that the electrically conductive coating is carried out chemically or electrochemically or by a combination of these two process steps, which enables simple and inexpensive production, which also enables the use of the invention of mass products makes it economical.
  • FIG. 1 shows the first cycle of an aluminum foil current arrester according to the prior art and of a current collector fabric coated with nickel alloy according to Example 1 according to the present invention in an electrolyte composed of 1 mol dm "3 LiCF 3 SO 3 / ethylene carbonate / Diethyl carbonate at a scanning speed of 0.2 mV s "1 and FIG. 2 shows a corresponding second cycle, FIGS. 3 and 4 show the same for example 2 with a different electrolyte at different current densities.
  • a polyester fabric was cleaned with an alkaline solution using a palladium-based activator and then rinsed. Then the active fourth fabric, through 600 s immersion in a bath at 65-70 ° C with the following composition, chemically coated with an alloy.
  • a pH of 6 was adjusted by adding sodium hydroxide.
  • button cells were produced using electrodes from the coated fabric ( ⁇ 1 cm “2 geometrical area), lithium as counterelectrode and an inert separator.
  • the electrodes were examined at 30 ° C. by means of cyclic voltammetry Scanning speed was 0.2 mV s "1 from the quiescent voltage to 4.3 V vs. Li / Li + and then repetitively between 2.3 V and 4.3 V vs. Li / Li + .
  • FIGS. 1 and 2 With an electrolyte of 1 mol dm "3 LiCF 3 SO 3 in ethylene carbonate / diethyl carbonate, electrodes made of aluminum foil showed a behavior which is illustrated in FIGS. 1 and 2 is.
  • Fig. 1 it can be seen that the aluminum foil was “activated , ⁇ (eg: passivating film was removed) when the potential was reduced to 4.3 V vs. Li / Li rose. This led to a high current flow until the passivating film regressed at low potentials.
  • the nickel phosphorus alloy showed a permanent passivating behavior.
  • a polyester fabric was coated with an alloy after activation with a palladium-based activator (as in Example 1).
  • the activated tissue was immersed in a bath of the following composition at 60 ° C. for 1,800 seconds
  • a pH of 9 was set by adding sodium hydroxide.
  • a silver-colored metallic film on the fabric was then visually detectable. Corresponding measurements confirmed the electrical conductivity of the surface.
  • An atomic ratio of the elements Ni: P: W of 82: 14: 4 was determined by EDX analysis, which corresponds to an alloy composition NiW 0 , osPo.i7.
  • FIGS. 3 and 4 show different current density scales from FIGS. 1 and 2.
  • Aluminum foil is much more stable in this electrolyte than that discussed in Example 1. Both the Ni-W-P alloy and the aluminum foil showed irreversible currents. It should be noted here that the surface of the Ni-WP alloy (applied to the plastic fabric in the manner described) was very much larger than that of the aluminum foil, so that it can be assumed that, based on the "electrochemical surface” instead of the " geometric surface "the alloy is more stable than the aluminum foil.
  • Example 2 The added come in the Example 2 "M ⁇ component increases while costs and complexity of the coating process, reduces the deposition rate and increases the electrical resistance, but offers the advantage of increasing the stability of the current-conducting layer under the given conditions (voltage, electrolyte composition ... .).

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Composite Materials (AREA)
  • Manufacturing & Machinery (AREA)
  • Secondary Cells (AREA)
  • Cell Electrode Carriers And Collectors (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

L'invention concerne une couche électriquement conductrice et flexible d'une électrode positive plate, notamment sur une batterie Li ou à ions Li. Selon l'invention, cette couche comporte un support pourvu d'une couche conductrice composée d'un alliage de la composition suivante : NiMyPx, où y = 0,3, 0,01 = x = 0,5 et M est sélectionné dans le groupe comprenant Mo, W, Cr, V, Sn, Co. Cette invention permet une fabrication et une utilisation aisées et peu onéreuses, même pour des potentiels électriques de 4V et plus (par rapport à Li/Li+).
PCT/AT2002/000280 2001-09-28 2002-09-25 Couche electriquement conductrice d'une electrode positive WO2003030282A2 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AU2002340614A AU2002340614A1 (en) 2001-09-28 2002-09-25 Electrically conductive layer of a positive electrode

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
ATA1543/2001 2001-09-28
AT0154301A AT409973B (de) 2001-09-28 2001-09-28 Strom-leitschicht einer positiven elektrode

Publications (2)

Publication Number Publication Date
WO2003030282A2 true WO2003030282A2 (fr) 2003-04-10
WO2003030282A3 WO2003030282A3 (fr) 2003-12-11

Family

ID=3688335

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/AT2002/000280 WO2003030282A2 (fr) 2001-09-28 2002-09-25 Couche electriquement conductrice d'une electrode positive

Country Status (3)

Country Link
AT (1) AT409973B (fr)
AU (1) AU2002340614A1 (fr)
WO (1) WO2003030282A2 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1675656B (zh) * 2002-08-06 2010-08-18 皇家飞利浦电子股份有限公司 倾斜台架计算层析x射线摄影法的重建方法和设备

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CA2643789A1 (fr) 2006-04-18 2007-10-25 Commonwealth Scientific And Industrial Research Organisation Dispositifs flexibles pour le stockage d'energie

Family Cites Families (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH10241697A (ja) * 1997-02-21 1998-09-11 Matsushita Electric Ind Co Ltd アルカリ蓄電池用電極及びその製造法
AT408288B (de) * 2000-05-10 2001-10-25 Funktionswerkstoffe Forschungs Mehrschichtige elektrode
EP1299916B1 (fr) * 2000-06-29 2004-07-07 Wolfgang Kollmann Procede de production de materiau metallise et pile et pile a combustible contenant ce materiau

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
None

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1675656B (zh) * 2002-08-06 2010-08-18 皇家飞利浦电子股份有限公司 倾斜台架计算层析x射线摄影法的重建方法和设备

Also Published As

Publication number Publication date
AU2002340614A1 (en) 2003-04-14
ATA15432001A (de) 2002-05-15
AT409973B (de) 2002-12-27
WO2003030282A3 (fr) 2003-12-11

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