WO2013128563A1 - Nonaqueous electrolyte secondary battery - Google Patents

Nonaqueous electrolyte secondary battery Download PDF

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Publication number
WO2013128563A1
WO2013128563A1 PCT/JP2012/054909 JP2012054909W WO2013128563A1 WO 2013128563 A1 WO2013128563 A1 WO 2013128563A1 JP 2012054909 W JP2012054909 W JP 2012054909W WO 2013128563 A1 WO2013128563 A1 WO 2013128563A1
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positive electrode
negative electrode
electrode
positive
secondary battery
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PCT/JP2012/054909
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French (fr)
Japanese (ja)
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佳樹 宮本
田中　明
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新神戸電機株式会社
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Priority to PCT/JP2012/054909 priority Critical patent/WO2013128563A1/en
Publication of WO2013128563A1 publication Critical patent/WO2013128563A1/en

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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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H01M4/622—Binders being polymers
    • 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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • 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 non-aqueous electrolyte secondary battery, and more particularly to a laminated lithium ion secondary battery.
  • the lithium ion secondary battery Since the lithium ion secondary battery has a high energy density, it is possible to miniaturize and lighten the power supply. Therefore, it began to be put to practical use as a portable power source from the 1990s.
  • power sources for electric vehicles have been developed as large-capacity batteries.
  • developments are being developed for the effective use of natural energy such as solar light and wind power, equalization of power usage, and industrial power supplies for use in uninterruptible power supplies and construction machines.
  • the electrode has a strip shape in which the active material is coated on the metal foil for both the positive electrode and the negative electrode, and the wound structure has a flat structure in which the separator is sandwiched between the positive electrode and the negative electrode. It is taken.
  • it is also a laminated type structure in which a strip of the positive electrode and the negative electrode in which the active material is coated on the metal foil is cut to a certain size and the separator is sandwiched so that the positive electrode and the negative electrode do not contact directly. It is adopted.
  • the electrode group is housed in a rectangular can or a container to be a battery container, and after injecting an electrolytic solution, the electrode group is sealed and initially charged to impart a function as a battery.
  • the main configuration of this lithium ion secondary battery is a metal current collector having a negative electrode active material layer formed on the surface, and a strip-like negative electrode coated with a negative electrode active material capable of containing and releasing lithium ions by charge and discharge. And a separator capable of holding an electrolyte and allowing lithium ions to pass through, and another metal current collector having a positive electrode active material layer formed on the surface, and capable of releasing and storing lithium ions by charge and discharge. It consists of a strip-shaped positive electrode coated.
  • the lithium ion secondary battery is made of a lithium metal oxide for the positive electrode and a carbon material such as graphite for the negative electrode.
  • the battery structure is roughly classified into a strip type negative electrode, a separator, a wound type structure in which a positive electrode is spirally wound, and a stacked type structure in which a strip-like negative electrode, a separator, and a positive electrode are alternately arranged.
  • a laminated structure in which strip-like negative electrodes, separators, and positive electrodes are alternately arranged, as compared to a wound structure having many volume parts that do not participate in power generation such as strip-like negative electrodes, separators, and axial cores for winding the positive electrodes. are generally suitable for high volumetric energy density. This is because the laminated type does not require an axial core for winding, and it is easy to form the positive and negative terminals for external output on the same surface, so the volume other than the part contributing to power generation can be reduced. It is from.
  • the electrode stack group contained in the battery can or container is held down by groove or brazing in the battery can or container to reduce variation in the distance between the positive electrode and the negative electrode.
  • a spacer is provided in the gap between the battery can or container and the electrode laminate group, and the pressing force of the electrode laminate group contained in the battery can or container is increased. doing.
  • the positive electrode, the negative electrode, and the separator are adhered, so the problems described herein can be avoided.
  • Such a secondary battery is sealed by a lid plate having an outer can of the battery assembly and a positive and negative terminals for external output.
  • a secondary battery is assembled by electrically connecting a positive and negative terminals for external output and an electrode group including a negative electrode, a separator, and a positive electrode before sealing with an outer case with a lid plate. Make a connection.
  • the positive and negative terminals for external output include a terminal body and a terminal base portion formed on the base of the terminal body. The portion exposed to the outside of the battery can is called a terminal body, and the portion housed inside the battery can is called a terminal base portion.
  • the terminal base portion is electrically connected to the electrode group.
  • a structure in which the positive and negative terminals for external output and the electrode group are assembled and integrated is attached to the opening of the lid plate via the insulating member.
  • the lid plate and the outer can are sealed.
  • the separator, the positive electrode, and the negative electrode, which are components of the battery assembly are impregnated with the electrolytic solution.
  • this invention mixes powder, such as polyethylene, as a heat absorption material in a positive electrode, and suppressing that the temperature of a battery rises rapidly by Joule heat generated by a short circuit, it does not carry out thermal welding, and a positive electrode , The negative electrode and the separator are not fixed.
  • One of the objects of the present invention is to reduce the variation in discharge characteristics caused by the increase in size of the battery.
  • the present invention uses a positive electrode current collector coated with a positive electrode active material capable of releasing and storing lithium ions by charge and discharge, and a negative electrode current collector stores lithium ions by charge and discharge.
  • a negative electrode coated with a releasable negative electrode active material is provided with an electrode stack group in which lithium ions can pass through a strip-shaped separator, and the electrode stack group is housed in a rectangular battery case and supported in the battery case Or a non-aqueous electrolyte secondary battery having a fixed structure, wherein at least one of the positive electrode and the negative electrode contains a powder resin and a binder, and the powder resin is made of a resin of the same material as the separator; And the separator is fixed.
  • the positive electrode, the negative electrode and the separator be fixed by heat welding.
  • the powder resin is preferably a polyolefin-based powder resin.
  • the polyolefin resin is more preferably polypropylene or polyethylene.
  • the variation in the distance between the electrodes is eliminated, and the discharge characteristics are stabilized.
  • there is no reduction in the energy density of the battery because it is not necessary to groove or braze the battery can or container in order to apply pressure to the electrode stack.
  • the output characteristics are not degraded.
  • Lithium manganate (LiMn 2 O 4 ) powder which is an active material capable of releasing and storing lithium by charge and discharge, flaky graphite as a conductive agent, polyvinylidene fluoride (PVdF) as a binder, and polyethylene as a powder resin
  • the resin powder was mixed in a ratio to be described later, N-methyl-2-pyrrolidone (NMP) as a dispersion solvent was added thereto, and the mixture was kneaded to prepare a slurry. And it apply
  • NMP N-methyl-2-pyrrolidone
  • the strip was dried, pressed, and cut to obtain a strip-shaped positive electrode plate having a width of 230 mm, a predetermined length to be described later, and a predetermined thickness of the positive electrode active material mixture application portion.
  • a notch was made in the slurry uncoated portion of the positive electrode plate, and the notch remaining portion was used as a lead piece.
  • a mixture of polyvinylidene fluoride as a binder and polyethylene resin powder as a powder resin is mixed with an amorphous carbon capable of containing and releasing lithium by charge and discharge so as to have a ratio to be described later, and N-methyl-2 as a dispersion solvent is mixed therewith.
  • -A slurry obtained by adding and kneading pyrrolidone was applied to both sides of a 10 ⁇ m-thick rolled copper foil (negative electrode current collector). At this time, an uncoated portion with a width of 30 mm was left at one side edge in the length direction of the negative electrode plate.
  • the strip was dried, pressed, and cut to obtain a strip-shaped negative electrode plate having a width of 235 mm, a predetermined length described later, and a predetermined thickness of the negative electrode active material coated portion.
  • a notch was made in the slurry uncoated portion of the negative electrode plate in the same manner as the positive electrode plate, and the remaining portion was used as a lead piece.
  • the electrode laminate group was pressed with a heat press at a temperature of 200 ° C. for 1 second to weld the positive electrode, the negative electrode and the separator.
  • lithium hexafluorophosphate LiPF 6
  • LiPF 6 lithium hexafluorophosphate
  • the materials for the positive electrode material, the negative electrode material, and the electrolyte used in the present invention are not particularly limited.
  • the positive electrode plate and the negative electrode plate of this example were produced as follows.
  • a positive electrode active material was lithium manganate, and a positive electrode plate having a thickness of 243 ⁇ m including a positive electrode current collector was produced.
  • a positive electrode plate having a thickness of 243 ⁇ m including a positive electrode current collector was produced.
  • a negative electrode plate having a thickness of 140 ⁇ m including a negative electrode current collector was produced using Carbotron P (registered trademark) made by Toha Chemical Industry Co., Ltd.
  • the positive electrode plate and the negative electrode plate were combined, and 5 cells of each of the batteries having the specifications shown in Table 1 were produced.
  • a battery of a specification in which the polyethylene powder was not mixed with the positive electrode and the negative electrode and a battery with the specification in which the polyethylene powder was mixed with the positive electrode and the negative electrode were not respectively heat-welded.
  • discharge capacity measurement results are shown in Table 1 as Examples and Comparative Examples.
  • FIG. 4 shows the relationship between the amount of total polyethylene powder mixed in the positive electrode and the negative electrode and the average capacity at the time of 6 A discharge in battery specifications 2 to 10 in which polyethylene powder was mixed with the positive electrode and negative electrode and heat welded.
  • Table 2 shows the average capacity and the result of deviation obtained by measuring the discharge capacity of the battery specifications 12 to 17 in which the polyethylene powder was mixed with the positive electrode or the negative electrode and heat-welded.
  • the relationship between the total amount of polyethylene powder and the average capacity at the time of 6 A discharge is shown in FIG.
  • the battery specifications 12 to 17 have the effect of improving the variation of the discharge characteristics lower than the case where the polyethylene powder is mixed in both electrodes, but the battery specification 1 (comparative example 1) in which the polyethylene powder is not mixed in both electrodes Compared with the battery specification 11 (comparative example 2) which is not heat-welded, the effect which improves the dispersion
  • the battery was prepared in the same manner except that the heat welding condition was pressed at a temperature of 200 ° C. for 2 seconds to weld the positive electrode, the negative electrode and the separator.
  • the discharge capacity was measured.
  • Table 3 shows the specifications of the battery manufactured at that time and the results of measurement of discharge capacity. As in the above example, the average capacity when discharged at 6 A is larger than in the battery specification 1 (conventional example 1) and the battery specification 11 (comparative example 2), and the effect of improving the variation in discharge characteristics is obtained. It was done.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Secondary Cells (AREA)

Abstract

Because of irregularities in the flatness of electrodes due to increases in electrode surface area, variations in inter-electrode distances for positive electrodes and negative electrodes that are stacked with separators therebetween arise easily. Therefore, there is the problem of variations in discharge characteristics for batteries arising easily. One purpose of the present invention is to reduce the variations in discharge characteristics that accompany increases in size of batteries. This nonaqueous electrolyte secondary battery has a structure which is provided with an electrode laminate group which is accommodated in a square battery container and supported or affixed within the battery container, said electrode laminate group being formed such that positive electrodes and negative electrodes are stacked with band shaped separators therebetween through which lithium ions can pass, said positive electrodes being formed by coating positive electrode current collectors with a positive electrode active material that can release and store lithium ions upon charging and discharging, and said negative electrodes being formed by coating negative electrode current collectors with a negative electrode active material that can store and release lithium ions upon charging and discharging. The constitution is such that either or both of the positive electrode and negative electrode includes a powdered resin and a binder, the powdered resin is formed from the same resin material as the separators, and the positive electrodes, negative electrodes, and separators are fixed.

Description

非水電解液二次電池Nonaqueous electrolyte secondary battery
　本発明は、非水電解液二次電池に係り、特に積層型リチウムイオン二次電池に関する。 The present invention relates to a non-aqueous electrolyte secondary battery, and more particularly to a laminated lithium ion secondary battery.
　近年、環境問題を背景にして、ハイブリッド電気自動車（ＨＥＶ）、電気自動車（ＥＶ）、フォークリフト、ショベルカー等の移動体のみならず、ＵＰＳ（無停電電源装置）、太陽光発電の電力貯蔵などの産業用用途にも、リチウムイオン電池を代表とする二次電池の適用が図られている。 In recent years, against the background of environmental problems, not only moving objects such as hybrid electric vehicles (HEVs), electric vehicles (EVs), forklifts, and shovels but also UPS (uninterruptible power supply), power storage of solar power generation, etc. Application to secondary batteries typified by lithium ion batteries is also attempted in industrial applications.
　リチウムイオン二次電池はエネルギー密度が高いため、電源の小型化と軽量化が可能である。そのため、１９９０年代から携帯用の電源として実用化され始めた。また、大容量の電池として、電気自動車用の電源が開発されている。さらに、太陽光や風力などの自然エネルギーの有効活用、電力使用の平準化、無停電電源装置および建設機械に用いる産業用の電源についても開発が展開されている。 Since the lithium ion secondary battery has a high energy density, it is possible to miniaturize and lighten the power supply. Therefore, it began to be put to practical use as a portable power source from the 1990s. In addition, power sources for electric vehicles have been developed as large-capacity batteries. In addition, developments are being developed for the effective use of natural energy such as solar light and wind power, equalization of power usage, and industrial power supplies for use in uninterruptible power supplies and construction machines.
　実装した場合の体積効率が高い角形電池の内部は、主に二種の方式が採用されている。一つには、電極は正極、負極共に活物質が金属箔に塗着された帯状であり、正極、負極が直接接触しないようにセパレータを挟んで扁平状に捲回された捲回式構造が採られている。一方、電極が正極、負極共に活物質が金属箔に塗着された帯状のものを、一定の寸法に切断し、正極、負極が直接接触しないようにセパレータを挟んで積層された積層式構造も採用されている。電極群は電池容器となる角形の缶又は容器に収納され、電解液を注入後、封口し、初充電することで電池としての機能が付与される。 Two types of methods are mainly adopted in the interior of a square battery having high volumetric efficiency when mounted. For example, the electrode has a strip shape in which the active material is coated on the metal foil for both the positive electrode and the negative electrode, and the wound structure has a flat structure in which the separator is sandwiched between the positive electrode and the negative electrode. It is taken. On the other hand, it is also a laminated type structure in which a strip of the positive electrode and the negative electrode in which the active material is coated on the metal foil is cut to a certain size and the separator is sandwiched so that the positive electrode and the negative electrode do not contact directly. It is adopted. The electrode group is housed in a rectangular can or a container to be a battery container, and after injecting an electrolytic solution, the electrode group is sealed and initially charged to impart a function as a battery.
　このリチウムイオン二次電池の主要な構成は、表面に負極活物質層を形成した金属集電体であって、充放電によりリチウムイオンを収容・放出可能な負極活物質を塗着した帯状の負極と、電解質を保持し、リチウムイオンが通過可能なセパレータと、表面に正極活物質層を形成した他の金属集電体であって、充放電によりリチウムイオンを放出・収容可能な正極活物質を塗着した帯状の正極とから成っている。また、リチウムイオン二次電池は、正極にリチウム金属酸化物、負極に黒鉛などのカーボン材料から成っている。 The main configuration of this lithium ion secondary battery is a metal current collector having a negative electrode active material layer formed on the surface, and a strip-like negative electrode coated with a negative electrode active material capable of containing and releasing lithium ions by charge and discharge. And a separator capable of holding an electrolyte and allowing lithium ions to pass through, and another metal current collector having a positive electrode active material layer formed on the surface, and capable of releasing and storing lithium ions by charge and discharge. It consists of a strip-shaped positive electrode coated. In addition, the lithium ion secondary battery is made of a lithium metal oxide for the positive electrode and a carbon material such as graphite for the negative electrode.
　電池構造としては、帯状の負極、セパレータ、正極を渦巻き状に巻いた捲回型構造と、短冊状の負極、セパレータ、正極を交互に配置した積層型構造とに大別される。帯状の負極、セパレータ、正極を巻き取るための軸芯等の発電に関与しない体積部分が多くある捲回型構造よりも、短冊状の負極、セパレータ、正極を交互に配置した積層型構造の方が、一般的に高体積エネルギー密度化に適している。これは、積層型は、巻取りのための軸芯が不要であることや、外部出力用の正極及び負極端子を同一面に形成し易いことから、発電に寄与する部分以外の体積を少なくできるからである。 The battery structure is roughly classified into a strip type negative electrode, a separator, a wound type structure in which a positive electrode is spirally wound, and a stacked type structure in which a strip-like negative electrode, a separator, and a positive electrode are alternately arranged. A laminated structure in which strip-like negative electrodes, separators, and positive electrodes are alternately arranged, as compared to a wound structure having many volume parts that do not participate in power generation such as strip-like negative electrodes, separators, and axial cores for winding the positive electrodes. Are generally suitable for high volumetric energy density. This is because the laminated type does not require an axial core for winding, and it is easy to form the positive and negative terminals for external output on the same surface, so the volume other than the part contributing to power generation can be reduced. It is from.
　産業用途に適した概ね容量３０Ａｈ以上の高容量かつ高出力の積層型リチウムイオン二次電池においては、電極面積が大きくなることによる電極の平坦性の乱れから、セパレータを介して積層された正極、負極の極間距離にばらつきを生じ易くなる。そのため、電池の放電特性にばらつきが生じ易いという課題がある。 In a high capacity and high power laminated lithium ion secondary battery having a capacity of about 30 Ah or more suitable for industrial applications, a positive electrode laminated via a separator from the disorder of the flatness of the electrode due to the increase of the electrode area, The distance between the negative electrodes is likely to vary. Therefore, there is a problem that the discharge characteristics of the battery are likely to vary.
　このような課題を回避するために、電池の缶又は容器に溝あるいは癖付けにより、電池の缶又は容器に内蔵する電極積層群を押え付け、正極、負極の極間距離のばらつきを小さくしている。さらに、電池の缶又は容器と電極積層群の隙間にスペーサを具備し、電池の缶又は容器に内蔵する電極積層群の押え付ける力を大きくするなど、正極、負極の極間距離のばらつきを小さくしている。しかしながら、これらの方法では、電極面積の大きな大型電池において、十分な効果を得るためには電池の缶又は容器の溝や癖付けを大きくしなければならない。そのため、それらのスペースを確保するために電池のエネルギー密度が低下してしまう。一方、ゲル電解質を用いた電池であれば、正極、負極とセパレータとが接着されるため、ここに述べた課題を回避できる。 In order to avoid such problems, the electrode stack group contained in the battery can or container is held down by groove or brazing in the battery can or container to reduce variation in the distance between the positive electrode and the negative electrode. There is. Furthermore, a spacer is provided in the gap between the battery can or container and the electrode laminate group, and the pressing force of the electrode laminate group contained in the battery can or container is increased. doing. However, in these methods, in a large battery with a large electrode area, in order to obtain a sufficient effect, it is necessary to increase the groove or brazing of the battery can or container. Therefore, the energy density of the battery is reduced to secure those spaces. On the other hand, in the case of a battery using a gel electrolyte, the positive electrode, the negative electrode, and the separator are adhered, so the problems described herein can be avoided.
　しかしながら、ゲル電解質を用いた電池は、電解液を用いた電池に比べ出力特性が低下してしまう。このような二次電池は、この電池構造体の外装缶と外部出力用の正極及び負極端子とを有する蓋板で密閉されている。従来、一般的にこのような二次電池の組立は、外装缶に蓋板で封止する前に、外部出力用の正極及び負極端子と、負極、セパレータ、正極からなる電極群との電気的接続を行う。外部出力用の正極及び負極端子は、端子本体と端子本体の基部に形成された端子基体部とを備えている。電池缶外部に露出している部分を端子本体と呼び、電池缶内部に納まっている部分を端子基体部と呼ぶ。通常、この端子基体部において、電極群との電気接続を行う。その後、外部出力用の正極及び負極端子と電極群とが組みつけられ一体となった構造体を蓋板の開口部に絶縁性部材を介して取り付けられる。この蓋板付きの構造体を外装缶の開口部に挿入後、蓋板と外装缶を封止する。外装缶の中では、電池構造体の構成要素であるセパレータ、正極、負極が電解液で含浸されている。 However, in the battery using the gel electrolyte, the output characteristics are degraded as compared with the battery using the electrolytic solution. Such a secondary battery is sealed by a lid plate having an outer can of the battery assembly and a positive and negative terminals for external output. Conventionally, in general, such a secondary battery is assembled by electrically connecting a positive and negative terminals for external output and an electrode group including a negative electrode, a separator, and a positive electrode before sealing with an outer case with a lid plate. Make a connection. The positive and negative terminals for external output include a terminal body and a terminal base portion formed on the base of the terminal body. The portion exposed to the outside of the battery can is called a terminal body, and the portion housed inside the battery can is called a terminal base portion. Usually, the terminal base portion is electrically connected to the electrode group. Thereafter, a structure in which the positive and negative terminals for external output and the electrode group are assembled and integrated is attached to the opening of the lid plate via the insulating member. After the structure with the lid plate is inserted into the opening of the outer can, the lid plate and the outer can are sealed. In the outer can, the separator, the positive electrode, and the negative electrode, which are components of the battery assembly, are impregnated with the electrolytic solution.
　前記課題を解決することと目的を異としているが、短絡で発生するジュール熱により電池の温度が急激に上昇をするのを抑制するために、正極中に熱吸収材を混合する発明が、特許文献１に提案されている。 Although the purpose of the invention is different from that of solving the above-mentioned problems, the invention of mixing the heat absorbing material in the positive electrode in order to suppress the rapid rise of the battery temperature due to the Joule heat generated by the short circuit is a patent. It is proposed in reference 1.
　この発明は、正極中に熱吸収材としてポリエチレンなどの粉末を混合し、短絡で発生するジュール熱により電池の温度が急激に上昇をするのを抑制しているため、熱溶着することなく、正極、負極、セパレータが固定化されたものではない。 Since this invention mixes powder, such as polyethylene, as a heat absorption material in a positive electrode, and suppressing that the temperature of a battery rises rapidly by Joule heat generated by a short circuit, it does not carry out thermal welding, and a positive electrode , The negative electrode and the separator are not fixed.
特開平１０－６４５４９号公報JP 10-64549 A
　産業用リチウムイオン電池においては、高容量化の開発が進められている。その結果、電極面積が増大する。電極面積が大きくなることによる電極の平坦性の乱れから、セパレータを介して積層された正極、負極の極間距離にばらつきが生じ易くなる。そのため、電池の放電特性にばらつきが生じ易いという課題がある。本発明の目的の一つは、電池の大型化に伴う放電特性のばらつき小さくすることである。 Development of higher capacity is being promoted for industrial lithium ion batteries. As a result, the electrode area is increased. From the disturbance of the flatness of the electrode due to the increase of the electrode area, the distance between the positive electrode and the negative electrode stacked via the separator tends to vary. Therefore, there is a problem that the discharge characteristics of the battery are likely to vary. One of the objects of the present invention is to reduce the variation in discharge characteristics caused by the increase in size of the battery.
　上記課題を解決するために、本発明は、正極集電体に充放電によりリチウムイオンを放出・収容可能な正極活物質を塗布した正極と、負極集電体に充放電によりリチウムイオンを収容・放出可能な負極活物質を塗布した負極とが、リチウムイオンが通過可能な帯状のセパレータを介して積層された電極積層群を備え、電極積層群は角形電池容器に収納され、電池容器内で支持または固定された構造の非水電解液二次電池であって、正極および負極の少なくとも一方に粉末樹脂と結着剤とが含有され、粉末樹脂はセパレータと同じ材質の樹脂からなり、正極、負極およびセパレータが固定されている構成とする。 In order to solve the above problems, the present invention uses a positive electrode current collector coated with a positive electrode active material capable of releasing and storing lithium ions by charge and discharge, and a negative electrode current collector stores lithium ions by charge and discharge. A negative electrode coated with a releasable negative electrode active material is provided with an electrode stack group in which lithium ions can pass through a strip-shaped separator, and the electrode stack group is housed in a rectangular battery case and supported in the battery case Or a non-aqueous electrolyte secondary battery having a fixed structure, wherein at least one of the positive electrode and the negative electrode contains a powder resin and a binder, and the powder resin is made of a resin of the same material as the separator; And the separator is fixed.
　また正極、負極およびセパレータが熱溶着により固定されていれば望ましい。 It is preferable that the positive electrode, the negative electrode and the separator be fixed by heat welding.
　粉末樹脂については、ポリオレフィン系粉末樹脂であることが好ましい。 The powder resin is preferably a polyolefin-based powder resin.
　あるいはポリオレフィン系樹脂が、ポリプロピレンまたはポリエチレンであればさらに好ましい。 Alternatively, the polyolefin resin is more preferably polypropylene or polyethylene.
　一方、粉末樹脂は、正極合剤部体積および負極合剤部体積の合計の０．４～２５ｗｔ％であることで顕著な効果が見られた。 On the other hand, a significant effect was observed when the powder resin was 0.4 to 25 wt% of the sum of the positive electrode mixture portion volume and the negative electrode mixture portion volume.
　さらに正極合剤部体積および負極合剤部体積の合計の１．０～１０ｗｔ％であることで、より顕著な効果が見られた。 Furthermore, a more remarkable effect was observed when the total volume of the positive electrode mixture portion volume and the negative electrode mixture portion volume was 1.0 to 10 wt%.
　本発明の構成を採用することにより、電極間距離のばらつきはなくなり、放電特性が安定化する。また、電極積層群に圧力を加えるために、電池の缶又は容器の溝や癖付けをする必要がないため、電池のエネルギー密度の低下はない。また、ゲル電解質を用いないため、出力特性も低下しない。 By adopting the configuration of the present invention, the variation in the distance between the electrodes is eliminated, and the discharge characteristics are stabilized. In addition, there is no reduction in the energy density of the battery because it is not necessary to groove or braze the battery can or container in order to apply pressure to the electrode stack. In addition, since no gel electrolyte is used, the output characteristics are not degraded.
本発明の一実施例を説明する電極を積層した状態図である。It is the state figure which laminated | stacked the electrode which demonstrates one Example of this invention. 本発明の一実施例を説明する電極積層群とポリプロピレン付き外部端子の接続図である。It is a connection diagram of the electrode laminated group and the external terminal with polypropylene which demonstrate one Example of this invention. 本発明の一実施例を説明する袋状に熱溶着した後のアルミラミネートフィルム状態図である。It is the aluminum laminate film state figure after heat-welding in the shape of a bag explaining one example of the present invention. 本発明の一実施例を説明するポリエチレン粉末量と６Ａ放電時の平均容量の関係図である。It is a related figure of the amount of polyethylene powder and the average capacity at the time of 6A discharge explaining one example of the present invention.
　以下、図面を参照して、本発明の積層型リチウムイオン電池の実施の形態について説明する。 Hereinafter, with reference to the drawings, an embodiment of a laminated lithium ion battery of the present invention will be described.
　充放電によりリチウムを放出・収容可能な活物質であるマンガン酸リチウム（ＬｉＭｎ２Ｏ４）粉末と、導電剤として鱗片状黒鉛と、結着剤としてポリフッ化ビニリデン（ＰＶｄＦ）と、粉末樹脂としてポリエチレン樹脂粉末とを、後述する割合になるように混合し、これに分散溶媒のＮ－メチル－２－ピロリドン（ＮＭＰ）を添加、混練してスラリを作製した。そして厚さ２０μｍのアルミニウム箔（正極集電体）の両面に塗布した。このとき、正極板長寸方向の一方の側縁に幅３０ｍｍの未塗布部を残した。その後乾燥、プレス、裁断して幅２３０ｍｍ、後述する所定長さ及び正極活物質合剤塗布部所定厚さの帯状の正極板を得た。正極板のスラリ未塗布部に切り欠きを入れ、切り欠き残部をリード片とした。次に、長さが３００ｍｍとなるように裁断し、正極板とした。 Lithium manganate (LiMn 2 O 4 ) powder which is an active material capable of releasing and storing lithium by charge and discharge, flaky graphite as a conductive agent, polyvinylidene fluoride (PVdF) as a binder, and polyethylene as a powder resin The resin powder was mixed in a ratio to be described later, N-methyl-2-pyrrolidone (NMP) as a dispersion solvent was added thereto, and the mixture was kneaded to prepare a slurry. And it apply | coated to the both surfaces of 20-micrometer-thick aluminum foil (positive electrode collector). At this time, an uncoated portion with a width of 30 mm was left on one side edge in the positive electrode plate length direction. Thereafter, the strip was dried, pressed, and cut to obtain a strip-shaped positive electrode plate having a width of 230 mm, a predetermined length to be described later, and a predetermined thickness of the positive electrode active material mixture application portion. A notch was made in the slurry uncoated portion of the positive electrode plate, and the notch remaining portion was used as a lead piece. Next, it cut | judged so that length might be set to 300 mm, and it was set as the positive electrode plate.
　以下、本発明の実施形態について図面を参照して詳細に説明する。 Hereinafter, embodiments of the present invention will be described in detail with reference to the drawings.
　充放電によりリチウムを収容・放出可能な非晶質炭素に結着剤としてポリフッ化ビニリデンと粉末樹脂としてポリエチレン樹脂粉末を後述する割合になるように混合し、これに分散溶媒のＮ－メチル－２－ピロリドンを添加、混練したスラリを、厚さ１０μｍの圧延銅箔（負極集電体）の両面に塗布した。このとき、負極板長寸方向の一方の側縁に幅３０ｍｍの未塗布部を残した。その後乾燥、プレス、裁断して幅２３５ｍｍ、後述する所定長さ及び負極活物質塗布部所定厚さの帯状の負極板を得た。負極板のスラリ未塗布部に正極板と同様に切り欠きを入れ、切り欠き残部をリード片とした。次に、長さが３０５ｍｍとなるように裁断し、負極板とした。 A mixture of polyvinylidene fluoride as a binder and polyethylene resin powder as a powder resin is mixed with an amorphous carbon capable of containing and releasing lithium by charge and discharge so as to have a ratio to be described later, and N-methyl-2 as a dispersion solvent is mixed therewith. -A slurry obtained by adding and kneading pyrrolidone was applied to both sides of a 10 μm-thick rolled copper foil (negative electrode current collector). At this time, an uncoated portion with a width of 30 mm was left at one side edge in the length direction of the negative electrode plate. Thereafter, the strip was dried, pressed, and cut to obtain a strip-shaped negative electrode plate having a width of 235 mm, a predetermined length described later, and a predetermined thickness of the negative electrode active material coated portion. A notch was made in the slurry uncoated portion of the negative electrode plate in the same manner as the positive electrode plate, and the remaining portion was used as a lead piece. Next, it cut | judged so that length might be set to 305 mm, and it was set as the negative electrode plate.
　上述したように作製した正極板１を１枚と負極板２を２枚とをこれら両極板が直接接触しないように厚さ４０μｍ、幅２１５ｍｍ、長さ３０５のポリエチレン製セパレータ３を２枚使用し、図１に示すように積層した。その後、電極積層群を熱プレス機で、２００℃の温度で１秒間プレスし、正極、負極、セパレータを溶着した。 Using two pieces of polyethylene separator 3 with a thickness of 40 μm, a width of 215 mm, and a length of 305 so that the bipolar plates do not directly contact one positive plate 1 and two negative plates 2 prepared as described above , As shown in FIG. Thereafter, the electrode laminate group was pressed with a heat press at a temperature of 200 ° C. for 1 second to weld the positive electrode, the negative electrode and the separator.
　次に、図２に示すように、正極板から導出されているリード片４とポリプロピレン付き正極外部端子６とを超音波溶接し固定した。また、負極板から導出されているリード片５とポリプロピレン付き負極外部端子７との接続操作も同様に行った。 Next, as shown in FIG. 2, ultrasonic welding was performed to fix the lead piece 4 derived from the positive electrode plate and the positive electrode external terminal 6 with polypropylene. Moreover, the connection operation between the lead piece 5 led out from the negative electrode plate and the negative electrode external terminal 7 with polypropylene was similarly performed.
　その後、予め筒状に熱溶着したアルミラミネートフィルム８に挿入し、図３に示すように、ポリエチレン付き正極外部端６およびポリエチレン付き負極外部端子７がアルミラミネートフィルム８で袋状になるように熱溶着した。 After that, it is inserted into the aluminum laminate film 8 heat-welded in a tubular shape in advance, and as shown in FIG. 3, the heat is applied so that the positive electrode external end 6 with polyethylene and the negative electrode external terminal 7 with polyethylene become bag-like with the aluminum laminate film 8 It was welded.
　そして、アルミラミネートフィルム８の開口部９から電解液を所定量注入し、開口部を熱溶着することにより積層型リチウムイオン電池を完成させた。 Then, a predetermined amount of electrolytic solution was injected from the opening 9 of the aluminum laminate film 8 and the opening was heat-welded to complete a laminated lithium ion battery.
　電解液には、エチレンカーボネートとジメチルカーボネートの混合溶液中へ電解質として６フッ化リン酸リチウム（ＬｉＰＦ６）を溶解したものを用いた。 As the electrolytic solution, one in which lithium hexafluorophosphate (LiPF 6 ) was dissolved in a mixed solution of ethylene carbonate and dimethyl carbonate as an electrolyte was used.
　なお、本発明に用いた正極材料、負極材料、電解液は、前記の材料を特に限定するものではない。 The materials for the positive electrode material, the negative electrode material, and the electrolyte used in the present invention are not particularly limited.
　本実施形態に従って作製した積層型リチウムイオン電池６の実施例について説明する。まず、本実施例の正極板及び負極板を次のように作製した。正極活物質をマンガン酸リチウムとし、正極集電体を含んだ電極厚さ２４３μｍの正極板を作製した。非晶質炭素として、呉羽化学製カーボトロンＰ（登録商標）を用い、負極集電体を含んだ電極厚さ１４０μｍの負極板を作製した。正極板と負極板とを組み合わせ、表１に示した仕様の電池をそれぞれ５セルずつ作製した。比較例として正極、負極にポリエチレン粉末を混合していない仕様の電池および正極、負極にポリエチレン粉末を混合しているが、熱溶着しなかった仕様の電池を同様にそれぞれ５セルずつ作製した。 An example of the stacked lithium ion battery 6 manufactured according to the present embodiment will be described. First, the positive electrode plate and the negative electrode plate of this example were produced as follows. A positive electrode active material was lithium manganate, and a positive electrode plate having a thickness of 243 μm including a positive electrode current collector was produced. As an amorphous carbon, a negative electrode plate having a thickness of 140 μm including a negative electrode current collector was produced using Carbotron P (registered trademark) made by Toha Chemical Industry Co., Ltd. The positive electrode plate and the negative electrode plate were combined, and 5 cells of each of the batteries having the specifications shown in Table 1 were produced. As a comparative example, a battery of a specification in which the polyethylene powder was not mixed with the positive electrode and the negative electrode, and a battery with the specification in which the polyethylene powder was mixed with the positive electrode and the negative electrode were not respectively heat-welded.
　次に、以上のように作製した実施例および比較例の各電池について、２５°Ｃの温度下にて、４．２Ｖ定電圧、電流制限（上限）１．５Ａ、５時間の充電、３Ａ定電流、終止電圧２．５Ｖまでの放電を２回繰り返した後、同条件で充電し、０．６Ａおよび６Ａ定電流の放電を行い、放電容量を計測した。充電と放電、放電と充電の切り替え時に、１５分間の休止期間を設けた。 Next, about each battery of the Example and comparative example which were produced as mentioned above, under the temperature of 25 ° C, 4.2V constant voltage, current limit (upper limit) 1.5A, charge for 5 hours, 3A fixed After the current and the discharge to the final voltage 2.5 V were repeated twice, charging was performed under the same conditions, discharging at a constant current of 0.6 A and 6 A was performed, and the discharge capacity was measured. When switching between charge and discharge and between discharge and charge, a 15-minute rest period was provided.
Figure JPOXMLDOC01-appb-T000001
Figure JPOXMLDOC01-appb-T000001
　各種電池仕様に応じて、放電容量測定結果（平均容量と偏差の結果）を実施例および比較例として表１に示す。 According to various battery specifications, discharge capacity measurement results (results of average capacity and deviation) are shown in Table 1 as Examples and Comparative Examples.
　電池仕様１（従来例１）は、０．６Ａ放電容量の平均値は２．８０Ａｈで、それらの偏差が０．０９４Ａｈとばらつきが大きく、６Ａ放電時の偏差は０．２３２Ａｈで、さらにばらつきは大きな結果となった。正極、負極にポリエチレン粉末を混合し、熱溶着した電池仕様２～１０で、正極および負極に混合した総ポリエチレン粉末量と６Ａ放電時の平均容量の関係について図４に示す。正極および負極にポリエチレン粉末の量を増加させると、放電容量のばらつきが小さくなり、ポリエチレン粉末の量が５ｗｔ％まで、６Ａで放電時の平均容量は増加した。その後、ポリエチレン粉末の量を増加させると、平均容量は低下した。これは、電池容量に関係のないポリエチレン粉末が増加したためである。 In Battery Specification 1 (Conventional Example 1), the average value of the 0.6A discharge capacity is 2.80Ah, their deviation is large with 0.094Ah, the deviation at 6A discharge is 0.232Ah, and the dispersion is more The result was great. FIG. 4 shows the relationship between the amount of total polyethylene powder mixed in the positive electrode and the negative electrode and the average capacity at the time of 6 A discharge in battery specifications 2 to 10 in which polyethylene powder was mixed with the positive electrode and negative electrode and heat welded. When the amount of polyethylene powder was increased in the positive electrode and the negative electrode, the variation in discharge capacity decreased, and the amount of polyethylene powder increased to 5 wt%, and the average capacity at the time of discharge increased at 6A. The average volume then decreased as the amount of polyethylene powder was increased. This is because polyethylene powder not related to battery capacity has increased.
　この結果より、正極および負極のポリエチレン粉末の合計量を０．４ｗｔ％から２５ｗｔ％混合することで、混合しない電池（従来例１）よりも平均容量が大きくなった。また、電池容量のばらつきも小さくすることが可能であった。さらに、ポリエチレン粉末の合計量を１．０ｗｔ％から１０ｗｔ％混合することで、その効果はさらに顕著であった。一方、電池仕様１０（比較例３）は、正極および負極にポリエチレン粉末を混合しているが、熱溶着していないため、電池容量のばらつきを改善する効果は得られなかった。 From this result, by mixing the total amount of the positive electrode and the negative electrode polyethylene powder from 0.4 wt% to 25 wt%, the average capacity was larger than that of the non-mixed battery (conventional example 1). In addition, it was possible to reduce the variation in battery capacity. Furthermore, the effect was further remarkable by mixing the total amount of polyethylene powder with 1.0 wt% to 10 wt%. On the other hand, in the battery specification 10 (comparative example 3), although polyethylene powder was mixed to the positive electrode and the negative electrode, since heat welding was not performed, the effect of improving the variation of the battery capacity was not obtained.
Figure JPOXMLDOC01-appb-T000002
Figure JPOXMLDOC01-appb-T000002
　次に、正極あるいは負極にポリエチレン粉末を混合し、熱溶着した電池仕様１２～１７の電池の放電容量計測にて得られた平均容量と偏差の結果を表２に示す。また、総ポリエチレン粉末量と６Ａ放電時の平均容量の関係について図４に示す。電池仕様１２～１７の電池は、両極にポリエチレン粉末を混合した場合よりも放電特性のばらつきを改善する効果は低下するが、両極にポリエチレン粉末を混合していない電池仕様１（比較例１）および熱溶着をしていない電池仕様１１（比較例２）に比べ、放電特性のばらつきを改善する効果が得られた。 Next, Table 2 shows the average capacity and the result of deviation obtained by measuring the discharge capacity of the battery specifications 12 to 17 in which the polyethylene powder was mixed with the positive electrode or the negative electrode and heat-welded. The relationship between the total amount of polyethylene powder and the average capacity at the time of 6 A discharge is shown in FIG. The battery specifications 12 to 17 have the effect of improving the variation of the discharge characteristics lower than the case where the polyethylene powder is mixed in both electrodes, but the battery specification 1 (comparative example 1) in which the polyethylene powder is not mixed in both electrodes Compared with the battery specification 11 (comparative example 2) which is not heat-welded, the effect which improves the dispersion | variation in discharge characteristics was acquired.
Figure JPOXMLDOC01-appb-T000003
Figure JPOXMLDOC01-appb-T000003
　さらに、上記の実施例で用いたセパレータの材質および粉末樹脂をポリプロピレンとし、熱溶着の条件を２００℃の温度で２秒間プレスし、正極、負極、セパレータを溶着した以外は、同様に電池を作製し、放電容量計測を行った。そのときに作製した電池の仕様および放電容量計測の結果を表３に示す。上記の実施例と同様に、６Ａで放電したときの平均容量は、電池仕様１（従来例１）および電池仕様１１（比較例２）に比べ大きくなり、放電特性のばらつきを改善する効果が得られた。 Furthermore, using the material of the separator and the powder resin used in the above example as polypropylene, the battery was prepared in the same manner except that the heat welding condition was pressed at a temperature of 200 ° C. for 2 seconds to weld the positive electrode, the negative electrode and the separator. The discharge capacity was measured. Table 3 shows the specifications of the battery manufactured at that time and the results of measurement of discharge capacity. As in the above example, the average capacity when discharged at 6 A is larger than in the battery specification 1 (conventional example 1) and the battery specification 11 (comparative example 2), and the effect of improving the variation in discharge characteristics is obtained. It was done.
　１…正極板、２…負極板、３…セパレータ、４…正極リード片、５…負極リード片、６…ポリプロピレン付き正極外部端子、７…ポリプロピレン付き負極外部端子、８…アルミラミネートフィルム、９…アルミラミネートフィルム開口部、１０…アルミラミネートフィルム熱溶着部。 DESCRIPTION OF SYMBOLS 1 ... positive electrode plate, 2 ... negative electrode plate, 3 ... separator, 4 ... positive electrode lead piece, 5 ... negative electrode lead piece, 6 ... positive electrode external terminal with polypropylene, 7 ... negative electrode external terminal with polypropylene, 8 ... aluminum laminated film, 9 ... Aluminum laminate film opening, 10 ... aluminum laminate film heat weld.

Claims (6)

  1. 　正極集電体に充放電によりリチウムイオンを放出・収容可能な正極活物質を塗布した正極と、負極集電体に充放電によりリチウムイオンを収容・放出可能な負極活物質を塗布した負極とが、リチウムイオンが通過可能な帯状のセパレータを介して積層された電極積層群を備え、前記電極積層群は角形電池容器に収容され、前記電池容器内で支持または固定された構造の非水電解液二次電池であって、
    　前記正極および負極の少なくとも一方に粉末樹脂と結着剤とが含有され、前記粉末樹脂は前記セパレータと同じ材質の樹脂からなり、前記正極、負極およびセパレータが固定されていることを特徴とする非水電解液二次電池。     The positive electrode collector is a positive electrode coated with a positive electrode active material capable of releasing and storing lithium ions by charge and discharge, and the negative electrode is a negative electrode collector coated with a negative electrode active material capable of storing and releasing lithium ions by charge and discharge. And a non-aqueous electrolyte solution having a structure in which an electrode stack group is stacked via a strip-shaped separator through which lithium ions can pass, and the electrode stack group is accommodated in a rectangular battery container and supported or fixed in the battery container. A secondary battery,
    A powder resin and a binder are contained in at least one of the positive electrode and the negative electrode, the powder resin is made of a resin of the same material as the separator, and the positive electrode, the negative electrode and the separator are fixed. Water electrolyte secondary battery.
  2. 　前記正極、負極およびセパレータが熱溶着により固定されていることを特徴とする請求項１に記載の非水電解液二次電池。 The non-aqueous electrolyte secondary battery according to claim 1, wherein the positive electrode, the negative electrode, and the separator are fixed by heat welding.
  3. 　前記粉末樹脂が、ポリオレフィン系粉末樹脂であることを特徴とする請求項１に記載の非水電解液二次電池。 The non-aqueous electrolyte secondary battery according to claim 1, wherein the powder resin is a polyolefin-based powder resin.
  4. 　前記ポリオレフィン系樹脂が、ポリプロピレンまたはポリエチレンであることを特徴とする請求項３に記載の非水電解液二次電池。 The non-aqueous electrolyte secondary battery according to claim 3, wherein the polyolefin resin is polypropylene or polyethylene.
  5. 　前記粉末樹脂は、正極合剤部体積および負極合剤部体積の合計体積の０．４～２５ｗｔ％であることを特徴とする請求項１記載の非水電解液二次電池。 The non-aqueous electrolyte secondary battery according to claim 1, wherein the powder resin is 0.4 to 25 wt% of the total volume of the positive electrode mixture portion volume and the negative electrode mixture portion volume.
  6. 　前記粉末樹脂は、正極合剤部体積および負極合剤部体積の合計体積の１．０～１０ｗｔ％であることを特徴とする請求項５記載の非水電解液二次電池。 6. The non-aqueous electrolyte secondary battery according to claim 5, wherein the powder resin is 1.0 to 10 wt% of the total volume of the positive electrode mixture portion volume and the negative electrode mixture portion volume.
PCT/JP2012/054909 2012-02-28 2012-02-28 Nonaqueous electrolyte secondary battery WO2013128563A1 (en)

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2003151558A (en) * 2001-11-14 2003-05-23 Matsushita Electric Ind Co Ltd Non-aqueous electrolyte secondary battery
JP2007311057A (en) * 2006-05-16 2007-11-29 Nissan Motor Co Ltd Electrode for battery
JP2008546135A (en) * 2005-05-17 2008-12-18 エルジー・ケム・リミテッド Binder for electrochemical devices including multiple stacked electrochemical cells
JP2011029079A (en) * 2009-07-28 2011-02-10 Sharp Corp Nonaqueous electrolyte secondary battery

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2003151558A (en) * 2001-11-14 2003-05-23 Matsushita Electric Ind Co Ltd Non-aqueous electrolyte secondary battery
JP2008546135A (en) * 2005-05-17 2008-12-18 エルジー・ケム・リミテッド Binder for electrochemical devices including multiple stacked electrochemical cells
JP2007311057A (en) * 2006-05-16 2007-11-29 Nissan Motor Co Ltd Electrode for battery
JP2011029079A (en) * 2009-07-28 2011-02-10 Sharp Corp Nonaqueous electrolyte secondary battery

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