WO2014119274A1 - Batterie lithium-ion et séparateur de batterie lithium-ion - Google Patents

Batterie lithium-ion et séparateur de batterie lithium-ion Download PDF

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Publication number
WO2014119274A1
WO2014119274A1 PCT/JP2014/000393 JP2014000393W WO2014119274A1 WO 2014119274 A1 WO2014119274 A1 WO 2014119274A1 JP 2014000393 W JP2014000393 W JP 2014000393W WO 2014119274 A1 WO2014119274 A1 WO 2014119274A1
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WO
WIPO (PCT)
Prior art keywords
lithium
separator
ion battery
negative electrode
lithium ion
Prior art date
Application number
PCT/JP2014/000393
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English (en)
Japanese (ja)
Inventor
樹 平岡
径 小林
岡崎　禎之
匡洋 白神
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三洋電機株式会社
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Filing date
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Application filed by 三洋電機株式会社 filed Critical 三洋電機株式会社
Publication of WO2014119274A1 publication Critical patent/WO2014119274A1/fr

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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
    • 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
    • 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
    • H01M50/411—Organic material
    • H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
    • H01M50/417—Polyolefins
    • 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
    • H01M50/449—Separators, membranes or diaphragms characterised by the material having a layered structure
    • H01M50/451—Separators, membranes or diaphragms characterised by the material having a layered structure comprising layers of only organic material and layers containing inorganic material
    • 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
    • H01M50/449—Separators, membranes or diaphragms characterised by the material having a layered structure
    • H01M50/457—Separators, membranes or diaphragms characterised by the material having a layered structure comprising three or more layers
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a lithium ion battery and a lithium ion battery separator for use in the lithium ion battery.
  • Metal materials that can be alloyed with lithium such as silicon, germanium, tin and zinc instead of carbonaceous materials such as graphite as negative electrode active materials, and these metals for higher energy density and higher output of lithium ion batteries
  • silicon, germanium, tin and zinc instead of carbonaceous materials such as graphite as negative electrode active materials, and these metals for higher energy density and higher output of lithium ion batteries
  • carbonaceous materials such as graphite
  • a negative active material composed of a metal material that forms an alloy with lithium or an oxide of these metals can insert lithium up to the composition of Li 4.4 Si if it is silicon, so that graphite can only insert lithium up to the composition of LiC 6 It has a larger theoretical capacity than other carbonaceous materials. Even if any negative electrode active material is used, lithium from the positive electrode active material is taken into the negative electrode active material at the time of the first charge, but not all of this lithium can be taken out at the time of discharge. The unspecified amount is fixed in the negative electrode active material, resulting in an irreversible capacity. Since the irreversible capacity of the metal material alloyed with lithium and the negative electrode active material made of an oxide of these metals is larger than the irreversible capacity of the carbonaceous material, there is a problem that the battery capacity does not reach a desired value.
  • Patent Document 1 listed below discloses a lithium ion battery separator in which a lithium powder subjected to stabilization treatment is attached to a separator having an average particle size of 20 ⁇ m on a separator mainly composed of polyolefin.
  • the lithium capacity can be supplemented to the irreversible capacity of the negative electrode by the stabilized lithium powder, so that the battery capacity is improved.
  • the deactivation of lithium does not proceed, and it is not necessary to provide an environment in which lithium does not react before the battery group manufacturing process.
  • the lithium ion battery separator disclosed in Patent Document 1 uses a lithium powder that has been subjected to stabilization treatment on the surface, the particle size of the lithium powder varies and is not uniform. Therefore, when a lithium ion battery is manufactured using the lithium ion battery separator disclosed in Patent Document 1, a hole larger than the diameter of a fine hole that the separator itself originally has in the separator after charge and discharge. May open. Since such a hole causes an internal short circuit between the positive electrode and the negative electrode, it is desired to suppress as much as possible.
  • the components formed on the surface of the lithium powder by the stabilization treatment remain on the surface of the separator after the first charge. Therefore, it becomes a resistance component and causes deterioration of battery characteristics.
  • a lithium ion battery includes a positive electrode plate including a positive electrode active material layer capable of reversibly occluding and releasing lithium, and a negative electrode plate including a negative electrode active material layer capable of reversibly occluding and releasing lithium.
  • the separator used in the lithium ion battery of one aspect of the present invention is provided with a lithium metal film on one surface of the separator base material, and this lithium metal film is homogeneous and has an extra component. Not. According to the lithium ion battery of one aspect of the present invention, lithium from the lithium metal film is taken into the negative electrode active material during the first charge, but a hole may be formed in the separator base material or internal resistance may increase. A lithium ion battery that is suppressed, has high initial charge / discharge efficiency, and excellent cycle characteristics can be obtained.
  • FIG. 2A is a schematic front view of a flat lithium ion battery according to one aspect of the present invention
  • FIG. 2B is a cross-sectional view taken along the line IIB-IIB in FIG. 2A
  • 3A to 3D are schematic cross-sectional views of the separators of Experimental Examples 1 to 4, respectively. It is a figure which shows the scanning electron microscope (SEM) photograph of the separator surface of Experimental example 4.
  • FIG. 5A is an enlarged SEM photograph of the VA portion of FIG. 4
  • FIG. 5B is an enlarged SEM photograph of the VB portion of FIG.
  • a lithium ion battery according to one aspect of the present invention and a lithium ion battery separator for use in the lithium ion battery will be described in detail using various experimental examples.
  • the following experimental examples are illustrated for explaining an example of a lithium ion battery for embodying the technical idea of the present invention and a separator for a lithium ion battery for use in the present invention. Is not intended to be limited to any of these experimental examples.
  • the present invention can be equally applied to those in which various modifications are made to those shown in these experimental examples without departing from the technical idea shown in the claims.
  • This negative electrode mixture slurry was applied to both surfaces of a negative electrode current collector sheet made of a copper foil having a thickness of 10 ⁇ m, dried, cut into a size corresponding to a battery case made of a predetermined laminate material after rolling, and Experimental Example 1
  • the negative electrode used with a lithium ion battery was obtained.
  • the charge capacity of this negative electrode was 5.0 mAh / cm 2 .
  • a ceramic layer made of inorganic particles is formed on one surface of the microporous membrane base material as follows, and homogeneous lithium is formed on the other surface. A metal film was formed.
  • the inorganic particles alumina powder having an average particle diameter (D 50 ) of 0.7 ⁇ m manufactured by Sumitomo Chemical Co., Ltd. was used.
  • this alumina powder 100 parts by weight of this alumina powder was mixed with 3 parts by weight of polyvinylidene fluoride (PVdF) as a binder and an appropriate amount of NMP to prepare a slurry which is a precursor of the porous heat-resistant layer.
  • PVdF polyvinylidene fluoride
  • This slurry was applied to one side of a microporous membrane substrate using a doctor blade and dried in a drier maintained at 60 ° C. to form a porous heat-resistant layer having a thickness of 4 ⁇ m on the microporous membrane substrate.
  • an aluminum laminate film material was previously molded into a container so as to accommodate the flat wound electrode group 13 produced as described above. A thing was used. Then, the flat wound electrode group 13 and the non-aqueous electrolyte prepared as described above are inserted into the outer package 14 in a carbon dioxide atmosphere at 25 ° C. and 1 atm, and the end of the aluminum laminate material is inserted. The closed part 35 was formed by heat-sealing the parts, and the flat lithium secondary battery 10 according to Experimental Example 1 having the structure shown in FIGS. 2A and 2B was produced.
  • Example 2 The lithium ion battery of Experimental Example 2 is an experiment except that only a porous heat-resistant layer is formed on one surface of the microporous membrane substrate as a separator, but a lithium metal membrane is not formed. A device having the same configuration as in Example 1 was produced.
  • Example 3 As the lithium ion battery of Experimental Example 3, a porous heat-resistant layer is formed on one surface of a microporous membrane substrate as a separator, and a lithium metal film formed on the porous heat-resistant layer is used. Were manufactured in the same configuration as in Experimental Example 1.
  • FIG. 3A to 3D show schematic cross-sectional views of the separators of Experimental Examples 1 to 4.
  • FIG. 1 the porous heat-resistant layer 18b is formed on one surface of the separator substrate 18a, and the homogeneous lithium metal layer 18c is formed on the other surface.
  • the separator 18B of Experimental Example 2 only the porous heat-resistant layer 18b is formed on one surface of the separator substrate 18a, and no lithium metal layer is formed.
  • the separator 18C of Experimental Example 3 the porous heat-resistant layer 18b is formed on one surface of the separator substrate 18a, and the lithium metal layer 18d is further formed on the surface thereof.
  • the porous heat-resistant layer 18b is formed on one surface of the separator substrate 18a, and the lithium metal particle layer 18e whose surface is stabilized similarly is formed on the other surface.
  • the batteries of Experimental Examples 1, 3, and 4 differ in the microstructure of the lithium metal layer based on the difference in the method of forming the lithium metal layer formed on the separator substrate. That is, since the lithium metal layer in the battery of Experimental Example 1 is formed on the separator substrate by a vacuum deposition method, the lithium metal layer is formed to have a uniform thickness. On the other hand, the lithium metal layer in the battery of Experimental Example 3 reacts with the porous heat-resistant layer to consume lithium. Therefore, it is considered that the charge / discharge efficiency of the battery of Experimental Example 3 is lower than that of the battery of Experimental Example 1.
  • the lithium metal layer in the battery of Experimental Example 4 is provided with lithium metal particles whose surface is stabilized on the separator substrate, the lithium metal layer has an uneven structure corresponding to the shape of the lithium metal particles used. Yes.
  • the portion of the lithium metal layer facing the positive electrode and the negative electrode disappears by moving to the negative electrode, but the components used for the lithium stabilization treatment remain on the surface of the negative electrode. ing. Therefore, in the battery of Experimental Example 4, the internal resistance increases due to the components used for the stabilization treatment of lithium, and thus it is considered that the initial charge / discharge efficiency is lower than that of the battery of Experimental Example 1.
  • the capacity retention rate As for the capacity retention rate, almost the same results were obtained for both the batteries of Experimental Example 1 and Experimental Example 3, but the battery of Experimental Example 3 was inferior to the battery of Experimental Example 1, and the battery of Experimental Example 2 was the most. It was inferior.
  • the battery of Experimental Example 2 since the irreversible capacity of the negative electrode is large, it is considered that the capacity retention rate was reduced due to the consumption of lithium in the irreversible capacity supplement during the charge / discharge cycle.
  • the reaction product between the lithium metal and the porous heat-resistant layer such as alumina becomes a resistance component
  • the component used for the lithium stabilization treatment becomes a resistance component. This is thought to have led to a decrease in the maintenance rate.
  • FIG. 4 shows an SEM photograph (50 times) of the surface of the separator of Experimental Example 4 after two charge / discharge cycles
  • FIG. 5A shows enlarged photographs (2000 times) of the VA portion and VB portion of FIG. And shown in FIG. 5B.
  • the separator of Experimental Example 4 was confirmed to have a hole in the separator after a charge / discharge cycle. Around this hole, the fibrous structure of the separator substrate has disappeared, and there is concern about the possibility of thermal damage associated with the charge / discharge cycle. On the other hand, such a hole was not formed in the separator used in the batteries of Experimental Examples 1 to 3 even after the charge / discharge cycle.
  • the thickness of the lithium metal film was 4 ⁇ m, but the thickness of the lithium metal film is not particularly limited. However, the appropriate thickness of the lithium metal film varies depending on the irreversible capacity of the negative electrode active material layer to be used, and needs to be appropriately adjusted. If the thickness of the lithium metal film is too small, the irreversible capacity in the negative electrode active material layer may not be sufficiently compensated, and the initial efficiency and cycle characteristics may not be sufficiently improved. If the thickness of the lithium metal film is too large, lithium is likely to precipitate on the negative electrode, which may reduce safety.
  • the mass ratio of SiO x to the carbon-based active material is 5:95 to 100: 0.
  • the coating amount of the negative electrode mixture is 100 to 300 g / m 2
  • the preferable thickness of the lithium metal film is 1 to 40 ⁇ m.
  • a negative electrode for a lithium ion battery according to one aspect of the present invention and a lithium ion battery using the negative electrode are, for example, a driving power source for a mobile information terminal such as a mobile phone, a notebook personal computer, and a PDA, and particularly required for high energy density Can be applied to.
  • a mobile information terminal such as a mobile phone, a notebook personal computer, and a PDA
  • high energy density Can be applied to.
  • it can be expected to be used for high output applications such as electric vehicles (EV), hybrid electric vehicles (HEV, PHEV) and electric tools.
  • EV electric vehicles
  • HEV hybrid electric vehicles
  • PHEV PHEV

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

Abstract

L'invention concerne une batterie lithium-ion ayant non seulement un séparateur protégé contre les perforations après des cycles de charge et de décharge mais aussi une efficacité de charge et de décharge initiales, des caractéristiques de cycle et des caractéristiques de débit excellentes, et l'invention concerne aussi un séparateur de batterie lithium-ion utilisé dans la batterie lithium-ion. Selon un aspect de la présente invention, un séparateur utilisé dans la batterie lithium-ion a une pellicule de lithium métallique uniforme disposée sur une surface d'un substrat de séparateur constitué principalement d'une polyoléfine. Une couche résistante à la chaleur poreuse peut être formée sur l'autre surface de ce substrat de séparateur, et la pellicule de lithium métallique est disposée sur le côté faisant face à l'électrode négative.
PCT/JP2014/000393 2013-01-31 2014-01-27 Batterie lithium-ion et séparateur de batterie lithium-ion WO2014119274A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2013017127A JP2016058129A (ja) 2013-01-31 2013-01-31 リチウムイオン電池及びリチウムイオン電池用セパレータ
JP2013-017127 2013-01-31

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WO2014119274A1 true WO2014119274A1 (fr) 2014-08-07

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Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2016194589A1 (fr) * 2015-05-29 2016-12-08 日立マクセル株式会社 Batterie secondaire au lithium-ion
US9954213B2 (en) 2011-07-11 2018-04-24 California Institute Of Technology Electrochemical systems with at least one electronically and ionically conductive layer
US9991492B2 (en) 2013-11-18 2018-06-05 California Institute Of Technology Separator enclosures for electrodes and electrochemical cells
US10158110B2 (en) 2011-07-11 2018-12-18 California Institute Of Technology Separators for electrochemical systems
US10714724B2 (en) 2013-11-18 2020-07-14 California Institute Of Technology Membranes for electrochemical cells
US11271214B2 (en) 2015-12-02 2022-03-08 California Institute Of Technology Three-dimensional ion transport networks and current collectors for electrochemical cells

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2020149921A (ja) * 2019-03-15 2020-09-17 Tdk株式会社 非水電解質二次電池用負極及びこれを用いた非水電解質二次電池

Citations (6)

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JP2003197198A (ja) * 2001-12-26 2003-07-11 Kakogawa Plastic Kk 非水系電池ならびにこれを構成する電極フィルムおよび電池素子
JP2003524857A (ja) * 1997-07-21 2003-08-19 デュラセル インコーポレイテッド リチウムイオン電気化学電池
WO2007072713A1 (fr) * 2005-12-22 2007-06-28 Fuji Jukogyo Kabushiki Kaisha Feuille metallique au lithium pour batterie ou condensateur
JP2007220452A (ja) * 2006-02-16 2007-08-30 Matsushita Electric Ind Co Ltd 非水電解液二次電池用セパレータおよび非水電解液二次電池
JP2008084842A (ja) * 2006-08-30 2008-04-10 Shin Etsu Chem Co Ltd 非水系二次電池用セパレータ及びその製造方法並びに非水電解質二次電池
JP2011216600A (ja) * 2010-03-31 2011-10-27 Jm Energy Corp 蓄電デバイス

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2003524857A (ja) * 1997-07-21 2003-08-19 デュラセル インコーポレイテッド リチウムイオン電気化学電池
JP2003197198A (ja) * 2001-12-26 2003-07-11 Kakogawa Plastic Kk 非水系電池ならびにこれを構成する電極フィルムおよび電池素子
WO2007072713A1 (fr) * 2005-12-22 2007-06-28 Fuji Jukogyo Kabushiki Kaisha Feuille metallique au lithium pour batterie ou condensateur
JP2007220452A (ja) * 2006-02-16 2007-08-30 Matsushita Electric Ind Co Ltd 非水電解液二次電池用セパレータおよび非水電解液二次電池
JP2008084842A (ja) * 2006-08-30 2008-04-10 Shin Etsu Chem Co Ltd 非水系二次電池用セパレータ及びその製造方法並びに非水電解質二次電池
JP2011216600A (ja) * 2010-03-31 2011-10-27 Jm Energy Corp 蓄電デバイス

Cited By (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9954213B2 (en) 2011-07-11 2018-04-24 California Institute Of Technology Electrochemical systems with at least one electronically and ionically conductive layer
US10158110B2 (en) 2011-07-11 2018-12-18 California Institute Of Technology Separators for electrochemical systems
US10693117B2 (en) 2011-07-11 2020-06-23 California Institute Of Technology Electrochemical systems with ionically conductive and electronically insulating separator
US11527802B2 (en) 2011-07-11 2022-12-13 California Institute Of Technology Electrochemical systems with ionically conductive and electronically insulating separator
US9991492B2 (en) 2013-11-18 2018-06-05 California Institute Of Technology Separator enclosures for electrodes and electrochemical cells
US10714724B2 (en) 2013-11-18 2020-07-14 California Institute Of Technology Membranes for electrochemical cells
US11177537B2 (en) 2013-11-18 2021-11-16 California Institute Of Technology Separator enclosures for electrodes and electrochemical cells
WO2016194589A1 (fr) * 2015-05-29 2016-12-08 日立マクセル株式会社 Batterie secondaire au lithium-ion
US11271214B2 (en) 2015-12-02 2022-03-08 California Institute Of Technology Three-dimensional ion transport networks and current collectors for electrochemical cells
US11894562B2 (en) 2015-12-02 2024-02-06 California Institute Of Technology Three-dimensional ion transport networks and current collectors for electrochemical cells

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