WO2001097304A1 - Electrode au lithium multicouche, procede de preparation associe et batteries au lithium comprenant cette electrode - Google Patents
Electrode au lithium multicouche, procede de preparation associe et batteries au lithium comprenant cette electrode Download PDFInfo
- Publication number
- WO2001097304A1 WO2001097304A1 PCT/KR2000/000616 KR0000616W WO0197304A1 WO 2001097304 A1 WO2001097304 A1 WO 2001097304A1 KR 0000616 W KR0000616 W KR 0000616W WO 0197304 A1 WO0197304 A1 WO 0197304A1
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- WIPO (PCT)
- Prior art keywords
- lithium
- layer
- porous
- alloy layer
- porous metal
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Classifications
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- 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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
-
- 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
- H01M4/06—Electrodes for primary cells
-
- 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
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- 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
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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- 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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
-
- 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
- H01M4/40—Alloys based on alkali metals
- H01M4/405—Alloys based on lithium
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M6/00—Primary cells; Manufacture thereof
- H01M6/14—Cells with non-aqueous electrolyte
- H01M6/16—Cells with non-aqueous electrolyte with organic electrolyte
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- 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
- lithium or lithium alloy layer and a 1A - 10 ⁇ m thick porous metal or porous
- lithium electrode which is fabricated by in the order
- lithium or a lithium alloy on a Cu- or Ni-current collector forming a 1A - 10 ⁇ m thick porous metal or porous carbon layer by coating a porous metal or porous carbon on the lithium or lithium alloy layer, and coating consecutively a lithium or lithium alloy layer and a porous metal or porous carbon layer on the resulting current collector, and to lithium batteries comprising it.
- Lithium batteries are generally divided into lithium primary batteries and lithium secondary batteries according to whether or not they can be recharged.
- lithium primary batteries lithium is used as a negative electrode material, and Li-MnO 2 , Li-(CF) n , Li-SOCI 2 , etc. are used as a positive electrode material according to the type of cathode. These batteries are presently commercialized. (J. O. Basenhard, Handbook of Battery Materials, Wiley-VCH, Weinheim (1999)).
- the lithium primary batteries are disadvantageous in that non-uniform potential distribution occurrs due to local dissolution of a lithium electrode, resulting in degradation in the utilization of the electrode.
- Figure 1 is a cross-sectional view of a multi-layered lithium electrode of the present invention.
- Figure 2 is a graph illustrating the test results of the capacity and cycle characteristics of an electrode using lithium batteries obtained in Examples 1 - 5 and Comparative Example 1.
- Figure 3 is a graph illustrating the test results of the high-rate charge characteristic of an electrode using lithium batteries obtained in Example 3 and Comparative Example 1.
- the present invention relates to a multi-layered lithium electrode
- a lithium electrode which is fabricated by forming a
- FIG. 1 illustrates a cross-sectional view of a multi-layered lithium electrode of the present invention.
- a lithium or lithium alloy layer 101a is coated on a current collector 103, and the lithium or lithium alloy layer 101 a is in turn coated with a porous metal or porous carbon layer 102a.
- This porous metal or porous carbon layer 102a is coated with a lithium or lithium alloy layer 101 b, and the lithium or lithium alloy layer 101 b is coated with a porous metal or porous carbon layer 102b.
- a multi-layered lithium electrode is formed by sequential stacks of lithium or lithium alloy layers 101 c....101 n and porous metal or porous carbon layers 102c .... 102n.
- 101 c...101 n are stacked at a thickness of 1A - 10 ⁇ m, but they are not limited
- lithium or lithium alloy layers 101 a, 101 b,....101 n become thiner, the number thereof to be coated becomes larger. In this case, the performance of the battery can be improved.
- mtals used for forming a lithium alloy in combination with metallic lithium include Al, Sn, Bi, Si, Sb, B and alloys thereof.
- the porous metal or porous carbon layers 102a, 102b, 102c....102n are coated at a thickness of 1A - 10 ⁇ m, but they are not limited thereto.
- metals used for the porous metal layers include Ni, Cu, Ti, V, Cr, Mn, Fe, Co, Zn, Mo, W, Ag, Au, Ru, Pt, Ir, Al, Sn, Bi, Si, Sb and alloys thereof.
- carbon group materials used for the porous carbon layers includes graphite, cokes, hard carbon, acetylene black, carbon black, and activated carbon.
- the electrical conductivity of the electrode is improved, and accordingly current and potential distribution is made constant, resulting in the suppression of local overcharging.
- the utilization and cycle life of the electrode are increased, and because of their porosity, the porous metal layers do not reduce the transport rate of lithium, in particular, in large-sized batteries.
- the multi-layered lithium electrode of this invention is fabricated by thin film fabrication techniques and certain pressing techniques commonly employed in an electrode fabrication process.
- thin film fabrication techniques refers to techniques for physical deposition under a non-aqueous atmosphere. These thin film fabrication techniques include thermal deposition, electron beam deposition, ion beam deposition, sputtering, arc deposition, laser ablation deposition methods, and the like. These deposition methods are advantageous in that a desired single metal or alloy can be freely coated, a pure porous metal or porous carbon can be coated without external contamination, the uniformity of coatings can be achieved, and the deposition thickness and time can be controlled by adjusting the rate of deposition freely.
- the lithium or lithium alloy layers and porous metal or porous carbon layers which form the lithium electrode are pressed.
- pressing refers to densification of the layers by applying pressure.
- Means for pressing includes a roll press and plate press. The pressure applied at this time is usually 10kg/cm 2 - 100 ton/cm 2 .
- the method of preparing a multi-layered lithium electrode according to the present invention will now be described more specifically.
- the multi- layered lithium electrode is fabricated as follows: a) Coating lithium or a lithium alloy on a copper or nickel current
- lithium or lithium alloys used for fabricating the above-described lithium or lithium alloy layer include a thin plate made of lithium or a lithium alloy and fine particles thereof.
- the multi- layered lithium electrode fabricated with sequential stacks of a lithium or lithium alloy layer and a porous metal or porous carbon layer, increases the utilization and cycle life of the lithium electrode and improves the high-rate charge and discharge characteristics by increasing the conductivity of the lithium electrode and by keeping potential distribution constant on the surface of the electrode.
- the multi-layered lithium electrode of the present invention can be widely used to fabricate a variety of lithium batteries including lithium primary batteries and lithium secondary batteries.
- lithium primary batteries using the lithium electrode of the present invention and MnO 2 , (DF) n or SOCI 2 as a cathode
- lithium secondary batteries using the lithium electrode of the present invention and LiCoO 2 , LiNiO 2l LiNiCoO 2 , LiMn2O 4 , V 2 O 5 , or V 6 O 13 as a cathode.
- the lithium electrode of the present invention is advantageous in that it can be used as an anode material of a lithium ion battery using a separator such as PP (polypropylene), PE (polyethylene), etc., a lithium polymer battery using a polymer electrolyte, and a complete solid-type lithium battery using a solid electrolyte, among the lithium secondary batteries.
- a separator such as PP (polypropylene), PE (polyethylene), etc.
- Example 1 1 -1 Preparation of a multi-layered lithium anode used for lithium batteries.
- lithium anode with a thickness of 80 ⁇ m.
- LiCoO 2 cathode After mixing a composition of 5.7g of LiCoO 2 , 0.6g of AB (acetylene black), and 0.4g of PVdF(polyvinylidenefluoride) with an appropriate amount of NMP (1-methyl-2-pyrrolidon) and acetone, the mixture was cast onto an aluminum thin plate when an appropriate viscosity was obtained and then dried, and thereafter rolled to prepare a LiCoO 2 cathode.
- LiCoO 2 cathode After mixing a composition of 5.7g of LiCoO 2 , 0.6g of AB (acetylene black), and 4.0g of PVdF (polyvinylidenefluohde) with an appropriate amount of NMP (1-methyl-2-pyrrolidon) and acetone, the mixture was cast onto an aluminum thin plate when an appropriate viscosity was obtained and then dried, and thereafter rolled to prepare a LiCoO 2 cathode.
- AB acetylene black
- PVdF polyvinylidenefluohde
- Example 2-1 After stacking the multi-layered lithium anode obtained in Example 2-1 , a PP separator, and the LiCoO 2 cathode obtained in Example 2-2, injected 1 M UPF 6 solution in PC:EMC, and then sealed to prepare a lithium battery.
- resulting plate at a thickness of 1000A by a vacuum deposition method.
- a further 15 layers were coated to prepare a multi-layered lithium anode of about 80 ⁇ m thick.
- LiCoO 2 cathode After mixing a composition of 5.7g of LiCoO 2 , 0.6g of AB (acetylene black), and 0.4g of PVdF (polyvinylidenefluohde) with an appropriate amount of NMP (1-methyl-2-pyrrolidon) and acetone, the mixture was cast onto an aluminum thin plate when an appropriate viscosity was obtained and then dried, and thereafter rolled to prepare a LiCoO 2 cathode.
- AB acetylene black
- PVdF polyvinylidenefluohde
- Example 3-1 After stacking the multi-layered lithium anode obtained in Example 3-1 , a PP separator, and the LiCoO 2 cathode obtained in Example 3-2, injected 1 M LiPF 6 solution in PC:EMC, and then sealed to prepare a lithium battery.
- Example 5 After stacking the multi-layered lithium anode obtained in Example 4-1 , a PP separator, and the LiCoO 2 cathode obtained in Example 4-2, injected 1 M LiPF 6 solution in PC:EMC, and then sealed to prepare a lithium battery.
- Example 5 After stacking the multi-layered lithium anode obtained in Example 4-1 , a PP separator, and the LiCoO 2 cathode obtained in Example 4-2, injected 1 M LiPF 6 solution in PC:EMC, and then sealed to prepare a lithium battery.
- lithium anode of about 80 ⁇ m thick.
- LiCoO 2 cathode After mixing a composition of 5.7g of LiCoO 2 , 0.6g of AB (acetylene black), and 0.4g of PVdF (polyvinylidenefluoride) with an appropriate amount of NMP (1 -methyl-2-pyrrolidon) and acetone, the mixture was cast onto an aluminum thin plate when an appropriate viscosity was obtained and then dried, and thereafter rolled to prepare a LiCoO 2 cathode.
- AB acetylene black
- PVdF polyvinylidenefluoride
- LiCoO 2 cathode After mixing a composition of 5.7g of LiCoO 2 , 0.6g of AB (acetylene black), and 0.4g of PVdF (polyvinylidenefluoride) with an appropriate amount of NMP (1-methyl-2-pyrrolidon) and acetone, the mixture was cast onto an aluminum thin plate when an appropriate viscosity was obtained and then dried, and thereafter rolled to prepare a LiCoO 2 cathode.
- AB acetylene black
- PVdF polyvinylidenefluoride
- Example 6-1 After stacking the multi-layered lithium anode obtained in Example 6-1, a PP separator, and the LiCoO 2 cathode obtained in Example 6-2, injected 1 M LiPF 6 solution in PC:EMC, and then sealed to prepare a lithium battery.
- LiCoO 2 cathode After mixing a composition of 5.7g of LiCoO 2 , 0.6g of AB (acetylene black), and 0.4g of PVdF (polyvinylidenefluoride) with an appropriate amount of NMP (1-methyl-2-pyrrolidon) and acetone, the mixture was cast onto an aluminum thin plate when an appropriate viscosity was obtained and then dried, and thereafter rolled to prepare a LiCoO 2 cathode.
- AB acetylene black
- PVdF polyvinylidenefluoride
- Example 7-1 After stacking the multi-layered lithium anode obtained in Example 7-1 , a PP separator, and the LiCoO 2 cathode obtained in Example 7-2, injected 1 M LiPF 6 solution in PC:EMC, and then sealed to prepare a lithium battery.
- a high-rate discharge characteristic was tested using the lithium battery obtained in Example 3 and the lithium battery obtained in Comparative Example 1. The results thereof are illustrated in Figure 3. As illustrated therein, it is shown that the lithium battery obtained in Example 3 has a more excellent high-rate charge and discharge characteristic than the lithium battery obtained in Comparative Example 1.
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- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Composite Materials (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Battery Electrode And Active Subsutance (AREA)
- Secondary Cells (AREA)
Abstract
La présente invention concerne une électrode au lithium multicouche formée sur un collecteur de courant avec des piles successives d'une couche de lithium ou d'alliage de lithium de 10Å à 100νm d'épaisseur et d'une couche de métal poreux ou de carbone poreux de 1Å à 10νm d'épaisseur. L'invention se rapporte également au procédé de fabrication de cette électrode, ainsi qu'à des batteries au lithium comprenant ladite électrode. Plus particulièrement, la présente invention concerne une électrode au lithium fabriquée par formation successive d'une couche de lithium ou d'alliage de lithium de 10Å à 100νm d'épaisseur sur un collecteur de courant de Cu ou de Ni et d'une couche de métal poreux ou de carbone poreux de 1Å à 10νm d'épaisseur. Elle porte enfin sur des batteries au lithium comprenant cette électrode.
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PCT/KR2000/000616 WO2001097304A1 (fr) | 2000-06-12 | 2000-06-12 | Electrode au lithium multicouche, procede de preparation associe et batteries au lithium comprenant cette electrode |
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PCT/KR2000/000616 WO2001097304A1 (fr) | 2000-06-12 | 2000-06-12 | Electrode au lithium multicouche, procede de preparation associe et batteries au lithium comprenant cette electrode |
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Cited By (37)
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EP1562248A3 (fr) * | 2004-01-13 | 2005-08-17 | Hitachi, Ltd. | Dispositif pour le stockage d'énergie électrique |
GB2412484A (en) * | 2004-07-27 | 2005-09-28 | Intellikraft Ltd | Improvements relating to electron structures in batteries |
FR2873854A1 (fr) * | 2004-07-30 | 2006-02-03 | Commissariat Energie Atomique | Procede de fabrication d'une electrode lithiee, electrode lithiee susceptible d'etre obtenue par ce procede et ses utilisations |
EP1271675A3 (fr) * | 2001-06-20 | 2006-03-08 | Sanyo Electric Co., Ltd. | Méthode de fabrication d'une électrode pour accumulateur au lithium |
WO2006057110A1 (fr) | 2004-11-26 | 2006-06-01 | Matsushita Electric Industrial Co., Ltd. | Batterie primaire au lithium et procédé de fabrication idoine |
JP2007122992A (ja) * | 2005-10-27 | 2007-05-17 | Matsushita Electric Ind Co Ltd | リチウム二次電池用負極およびリチウム二次電池の製造方法 |
WO2007111901A2 (fr) * | 2006-03-22 | 2007-10-04 | Sion Power Corporation | Protection d'electrode dans des piles electrochimiques aqueuses et non aqueuses, comprenant des batteries rechargeables au lithium |
WO2007127636A2 (fr) * | 2006-04-26 | 2007-11-08 | Medtronic, Inc. | Collecteur de courant |
US7695861B2 (en) | 2005-03-22 | 2010-04-13 | Oxis Energy Limited | Lithium sulphide battery and method of producing the same |
US7771870B2 (en) | 2006-03-22 | 2010-08-10 | Sion Power Corporation | Electrode protection in both aqueous and non-aqueous electrochemical cells, including rechargeable lithium batteries |
US8105717B2 (en) | 1999-11-23 | 2012-01-31 | Sion Power Corporation | Lithium anodes for electrochemical cells |
US8679684B2 (en) | 2004-12-02 | 2014-03-25 | Oxis Energy, Ltd. | Electrolyte for lithium-sulphur batteries and lithium-sulphur batteries using the same |
US20140106223A1 (en) * | 2012-10-12 | 2014-04-17 | Hefei Guoxuan High-Tech Power Energy Co., Ltd. | METHODS FOR SURFACE COATING OF CATHODE MATERIAL LiNi0.5-XMn1.5MXO4 FOR LITHIUM-ION BATTERIES |
US8936870B2 (en) | 2011-10-13 | 2015-01-20 | Sion Power Corporation | Electrode structure and method for making the same |
EP2843733A1 (fr) * | 2013-09-03 | 2015-03-04 | Samsung SDI Co., Ltd. | Électrode pour batterie rechargeable au lithium-ion et batterie rechargeable au lithium-ion l'incluant |
US9005311B2 (en) | 2012-11-02 | 2015-04-14 | Sion Power Corporation | Electrode active surface pretreatment |
US9196929B2 (en) | 2005-01-18 | 2015-11-24 | Oxis Energy Limited | Electrolyte compositions for batteries using sulphur or sulphur compounds |
US9219271B2 (en) | 2004-07-27 | 2015-12-22 | Oxis Energy Limited | Battery electrode structure |
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EP1562248A3 (fr) * | 2004-01-13 | 2005-08-17 | Hitachi, Ltd. | Dispositif pour le stockage d'énergie électrique |
US9219271B2 (en) | 2004-07-27 | 2015-12-22 | Oxis Energy Limited | Battery electrode structure |
GB2412484A (en) * | 2004-07-27 | 2005-09-28 | Intellikraft Ltd | Improvements relating to electron structures in batteries |
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US8697287B2 (en) | 2004-07-30 | 2014-04-15 | Commissariat A L'energie Atomique | Process for manufacturing a lithiated electrode, lithiated electrode that can be obtained by this process, and its uses |
JP2008508671A (ja) * | 2004-07-30 | 2008-03-21 | コミツサリア タ レネルジー アトミーク | リチウム化電極製造方法、本方法により得られるリチウム化電極、ならびに、この使用 |
FR2873854A1 (fr) * | 2004-07-30 | 2006-02-03 | Commissariat Energie Atomique | Procede de fabrication d'une electrode lithiee, electrode lithiee susceptible d'etre obtenue par ce procede et ses utilisations |
WO2006021718A1 (fr) * | 2004-07-30 | 2006-03-02 | Commissariat A L'energie Atomique | Procede de fabrication d'une electrode lithiee, electrode lithiee susceptible d'etre obtenue par ce procede et ses utilisations |
EP1801901A1 (fr) * | 2004-11-26 | 2007-06-27 | Matsushita Electric Industrial Co., Ltd. | Batterie primaire au lithium et procede de fabrication idoine |
EP1801901A4 (fr) * | 2004-11-26 | 2012-08-29 | Panasonic Corp | Batterie primaire au lithium et procede de fabrication idoine |
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